Jens Norskov
Leland T. Edwards Professor in the School of Engineering and Professor of Photon Science and Senior Fellow at the Precourt Institute for Energy
Chemical Engineering
Academic Appointments
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Professor, Chemical Engineering
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Professor, Photon Science Directorate
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Senior Fellow, Precourt Institute for Energy
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Affiliate, Precourt Institute for Energy
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Affiliate, Stanford Woods Institute for the Environment
Administrative Appointments
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Director, Chemical Science Division, SLAC National Accelerator Laboratory (2011 - 2014)
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Director, SUNCAT Center for Interface Science and Catalysis, SLAC and Stanford University (2010 - Present)
Honors & Awards
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Michel Boudart Award for the Advancement of Catalysis, North American Catalysis Society and the European Federation of Catalysis Societies (2013)
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Hagemann Medal, Technical University of Denmark (2013)
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Dr. Honoris Causa, Norwegian University of Science and Technology (2012)
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The Giuseppe Parravano Award, The Giuseppe Parravano Award (2011)
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The Science of Hydrogen and Energy Award, EMPA, Switzerland (2009)
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The Alwin Mittasch Award, The Alwin Mittasch Award (2009)
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The Gabor A. Somorjai Award, ACS (2009)
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The Gerhard Ertl Lecture Award, The Gerhard Ertl Lecture Award (2009)
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The Grundfos Prize, Copenhagen, The Grundfos Prize, Copenhagen (2007)
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The Mulliken Medal, University of Chicago, Illinois (2007)
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Dr. Honoris Causa, Technical University of Eindhoven, The Netherlands (2006)
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The Innovation Prize, DTU (2005)
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The Richard A. Glenn Award, ACS (2003)
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Fellow, American Physical Society (2003)
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Member, Royal Danish Academy of Science and Letters (1996)
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The Villum Kann Rasmussens Award, The Villum Kann Rasmussens Award (1991)
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The Danish Physical Society's Prize, Danish Physical Society (1990)
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The Samuel Friedman (Rescue) Award, University of California Los Angeles (1989)
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Member, Danish Academy of Engineering (ATV) (1987)
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The Reinholdt W. Jorch's Award, The Reinholdt W. Jorch's Award (1987)
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The ECOSS prize, Cambridge, UK (1979)
Boards, Advisory Committees, Professional Organizations
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Member, International Advisory Board of the State Key Laboratory of Catalysis (SKLC), Dalian Institute of Chemical Physics, Chinese Academy of Sciences (2014 - Present)
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Member, Scientific Advisory Board for the Max-Planck-Institute for Chemical Energy Conversion (2014 - Present)
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Elected Member, Royal Danish Academy of Science and Letters (1996 - Present)
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Elected Member, Danish Academy of Engineering (ATV) (1987 - Present)
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Member, Condensed Matter and Materials Research Committee, Board on Physics and Astronomy, National Academies (2013 - Present)
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Member, Advisory Board, Innovation Center Denmark, Silicon Valley (2012 - Present)
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Member, Board of Directors, Haldor Topsøe A/S (2010 - Present)
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Member, Board of Directors, Topsøe Fuel Cells A/S (2009 - Present)
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Member, Advisory Board and Scientific Committee of the State Key Laboratory for Surface Physics (SKLSP), Chinese Academy of Sciences & Division of Surface Physics, Beijing National Lab for Condensed Matter Physics (2006 - Present)
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Member, International Advisory Board, The Partnership for International Research and Education, University of California, Santa Barbara (2005 - Present)
Professional Education
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PhD, Aarhus University, Physics (1979)
2014-15 Courses
- Basic Principles of Heterogeneous Catalysis with Applications in Energy Transformations
CHEMENG 142, CHEMENG 242 (Spr) - Electronic Structure Theory and Applications to Chemical Kinetics
CHEMENG 444, ENERGY 256 (Win) - Special Topics in Interface Science and Catalysis
CHEMENG 519 (Aut, Win, Spr, Sum) -
Independent Studies (4)
- Graduate Research Rotation in Chemical Engineering
CHEMENG 399 (Aut, Win, Sum) - Graduate Research in Chemical Engineering
CHEMENG 600 (Aut, Win, Spr, Sum) - Undergraduate Honors Research in Chemical Engineering
CHEMENG 190H (Aut, Win, Spr) - Undergraduate Research in Chemical Engineering
CHEMENG 190 (Aut, Win, Spr)
- Graduate Research Rotation in Chemical Engineering
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Prior Year Courses
2013-14 Courses
- Basic Principles of Heterogeneous Catalysis with Applications in Energy Transformations
CHEMENG 142, CHEMENG 242 (Spr) - Special Topics in Interface Science and Catalysis
CHEMENG 519 (Aut, Win, Spr, Sum)
2012-13 Courses
- Basic Principles of Heterogeneous Catalysis with Applications in Energy Transformations
CHEMENG 142, CHEMENG 242 (Spr) - Electronic Structure Theory and Applications to Chemical Kinetics
CHEMENG 444, ENERGY 256 (Win) - Special Topics in Interface Science and Catalysis
CHEMENG 519 (Aut, Win, Spr, Sum)
2011-12 Courses
- Catalysis
CHEMENG 124, CHEMENG 224 (Spr) - Special Topics in Interface Science and Catalysis
CHEMENG 519 (Aut, Win, Spr, Sum)
- Basic Principles of Heterogeneous Catalysis with Applications in Energy Transformations
Journal Articles
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Exploring the limits: A low-pressure, low-temperature Haber-Bosch process
CHEMICAL PHYSICS LETTERS
2014; 598: 108-112
View details for DOI 10.1016/j.cplett.2014.03.003
View details for Web of Science ID 000334294900021
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Discovery of a Ni-Ga catalyst for carbon dioxide reduction to methanol
NATURE CHEMISTRY
2014; 6 (4): 320-324
Abstract
The use of methanol as a fuel and chemical feedstock could become very important in the development of a more sustainable society if methanol could be efficiently obtained from the direct reduction of CO2 using solar-generated hydrogen. If hydrogen production is to be decentralized, small-scale CO2 reduction devices are required that operate at low pressures. Here, we report the discovery of a Ni-Ga catalyst that reduces CO2 to methanol at ambient pressure. The catalyst was identified through a descriptor-based analysis of the process and the use of computational methods to identify Ni-Ga intermetallic compounds as stable candidates with good activity. We synthesized and tested a series of catalysts and found that Ni5Ga3 is particularly active and selective. Comparison with conventional Cu/ZnO/Al2O3 catalysts revealed the same or better methanol synthesis activity, as well as considerably lower production of CO. We suggest that this is a first step towards the development of small-scale low-pressure devices for CO2 reduction to methanol.
View details for DOI 10.1038/NCHEM.1873
View details for Web of Science ID 000333396200022
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Effects of d-band shape on the surface reactivity of transition-metal alloys
PHYSICAL REVIEW B
2014; 89 (11)
View details for DOI 10.1103/PhysRevB.89.115114
View details for Web of Science ID 000332705300001
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Electronic Structure Effects in Transition Metal Surface Chemistry
TOPICS IN CATALYSIS
2014; 57 (1-4): 25-32
View details for DOI 10.1007/s11244-013-0159-2
View details for Web of Science ID 000330829600004
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Direct observation of the oxygenated species during oxygen reduction on a platinum fuel cell cathode
NATURE COMMUNICATIONS
2013; 4
Abstract
The performance of polymer electrolyte membrane fuel cells is limited by the reduction at the cathode of various oxygenated intermediates in the four-electron pathway of the oxygen reduction reaction. Here we use ambient pressure X-ray photoelectron spectroscopy, and directly probe the correlation between the adsorbed species on the surface and the electrochemical potential. We demonstrate that, during the oxygen reduction reaction, hydroxyl intermediates on the cathode surface occur in several configurations with significantly different structures and reactivities. In particular, we find that near the open-circuit potential, non-hydrated hydroxyl is the dominant surface species. On the basis of density functional theory calculations, we show that the removal of hydration enhances the reactivity of oxygen species. Tuning the hydration of hydroxyl near the triple phase boundary will be crucial for designing more active fuel cell cathodes.
View details for DOI 10.1038/ncomms3817
View details for Web of Science ID 000329392900001
View details for PubMedID 24346299
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Theoretical Investigation of the Activity of Cobalt Oxides for the Electrochemical Oxidation of Water
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2013; 135 (36): 13521-13530
Abstract
The presence of layered cobalt oxides has been identified experimentally in Co-based anodes under oxygen-evolving conditions. In this work, we report the results of theoretical investigations of the relative stability of layered and spinel bulk phases of Co oxides, as well as the stability of selected surfaces as a function of applied potential and pH. We then study the oxygen evolution reaction (OER) on these surfaces and obtain activity trends at experimentally relevant electro-chemical conditions. Our calculated volume Pourbaix diagram shows that β-CoOOH is the active phase where the OER occurs in alkaline media. We calculate relative surface stabilities and adsorbate coverages of the most stable low-index surfaces of β-CoOOH: (0001), (0112), and (1014). We find that at low applied potentials, the (1014) surface is the most stable, while the (0112) surface is the more stable at higher potentials. Next, we compare the theoretical overpotentials for all three surfaces and find that the (1014) surface is the most active one as characterized by an overpotential of η = 0.48 V. The high activity of the (1014) surface can be attributed to the observation that the resting state of Co in the active site is Co(3+) during the OER, whereas Co is in the Co(4+) state in the less active surfaces. Lastly, we demonstrate that the overpotential of the (1014) surface can be lowered further by surface substitution of Co by Ni. This finding could explain the experimentally observed enhancement in the OER activity of Ni(y)Co(1-y)O(x) thin films with increasing Ni content. All energetics in this work were obtained from density functional theory using the Hubbard-U correction.
View details for DOI 10.1021/ja405997s
View details for Web of Science ID 000330163200050
View details for PubMedID 23944254
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Methanol to Dimethyl Ether over ZSM-22: A Periodic Density Functional Theory Study
ACS CATALYSIS
2013; 3 (4): 735-745
View details for DOI 10.1021/cs300722w
View details for Web of Science ID 000317328000037
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Real-Time Observation of Surface Bond Breaking with an X-ray Laser
SCIENCE
2013; 339 (6125): 1302-1305
View details for DOI 10.1126/science.1231711
View details for Web of Science ID 000316053400033
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Electronic Origin of the Surface Reactivity of Transition-Metal-Doped TiO2(110)
JOURNAL OF PHYSICAL CHEMISTRY C
2013; 117 (1): 460-465
View details for DOI 10.1021/jp310667r
View details for Web of Science ID 000313220700059
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Electronic Structure Effects in Transition Metal Surface Chemistry
Topics in Catalysis
2013; 53
View details for DOI 10.1007/s11244-013-0159-2
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Finite-Size Effects in O and CO Adsorption for the Late Transition Metals
TOPICS IN CATALYSIS
2012; 55 (19-20): 1276-1282
View details for DOI 10.1007/s11244-012-9908-x
View details for Web of Science ID 000312074600003
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Unifying the 2e(-) and 4e(-) Reduction of Oxygen on Metal Surfaces
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2012; 3 (20): 2948-2951
View details for DOI 10.1021/jz301476w
View details for Web of Science ID 000310177200005
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Modeling van der Waals Interactions in Zeolites with Periodic DFT: Physisorption of n-Alkanes in ZSM-22
CATALYSIS LETTERS
2012; 142 (9): 1057-1060
View details for DOI 10.1007/s10562-012-0870-9
View details for Web of Science ID 000307511800003
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Density functionals for surface science: Exchange-correlation model development with Bayesian error estimation
PHYSICAL REVIEW B
2012; 85 (23)
View details for DOI 10.1103/PhysRevB.85.235149
View details for Web of Science ID 000305739800001
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Balance of Nanostructure and Bimetallic Interactions in Pt Model Fuel Cell Catalysts: In Situ XAS and DFT Study
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2012; 134 (23): 9664-9671
Abstract
We have studied the effect of nanostructuring in Pt monolayer model electrocatalysts on a Rh(111) single-crystal substrate on the adsorption strength of chemisorbed species. In situ high energy resolution fluorescence detection X-ray absorption spectroscopy at the Pt L(3) edge reveals characteristic changes of the shape and intensity of the "white-line" due to chemisorption of atomic hydrogen (H(ad)) at low potentials and oxygen-containing species (O/OH(ad)) at high potentials. On a uniform, two-dimensional Pt monolayer grown by Pt evaporation in ultrahigh vacuum, we observe a significant destabilization of both H(ad) and O/OH(ad) due to strain and ligand effects induced by the underlying Rh(111) substrate. When Pt is deposited via a wet-chemical route, by contrast, three-dimensional Pt islands are formed. In this case, strain and Rh ligand effects are balanced with higher local thickness of the Pt islands as well as higher defect density, shifting H and OH adsorption energies back toward pure Pt. Using density functional theory, we calculate O adsorption energies and corresponding local ORR activities for fcc 3-fold hollow sites with various local geometries that are present in the three-dimensional Pt islands.
View details for DOI 10.1021/ja3003765
View details for Web of Science ID 000305107800025
View details for PubMedID 22616917
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The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts
SCIENCE
2012; 336 (6083): 893-897
Abstract
One of the main stumbling blocks in developing rational design strategies for heterogeneous catalysis is that the complexity of the catalysts impairs efforts to characterize their active sites. We show how to identify the crucial atomic structure motif for the industrial Cu/ZnO/Al(2)O(3) methanol synthesis catalyst by using a combination of experimental evidence from bulk, surface-sensitive, and imaging methods collected on real high-performance catalytic systems in combination with density functional theory calculations. The active site consists of Cu steps decorated with Zn atoms, all stabilized by a series of well-defined bulk defects and surface species that need to be present jointly for the system to work.
View details for DOI 10.1126/science.1219831
View details for Web of Science ID 000304145600059
View details for PubMedID 22517324
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CatApp: A Web Application for Surface Chemistry and Heterogeneous Catalysis
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2012; 51 (1): 272-274
View details for DOI 10.1002/anie.201107947
View details for Web of Science ID 000298598500049
View details for PubMedID 22162297
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Electrical conductivity in Li2O2 and its role in determining capacity limitations in non-aqueous Li-O-2 batteries
JOURNAL OF CHEMICAL PHYSICS
2011; 135 (21)
Abstract
Non-aqueous Li-air or Li-O(2) cells show considerable promise as a very high energy density battery couple. Such cells, however, show sudden death at capacities far below their theoretical capacity and this, among other problems, limits their practicality. In this paper, we show that this sudden death arises from limited charge transport through the growing Li(2)O(2) film to the Li(2)O(2)-electrolyte interface, and this limitation defines a critical film thickness, above which it is not possible to support electrochemistry at the Li(2)O(2)-electrolyte interface. We report both electrochemical experiments using a reversible internal redox couple and a first principles metal-insulator-metal charge transport model to probe the electrical conductivity through Li(2)O(2) films produced during Li-O(2) discharge. Both experiment and theory show a "sudden death" in charge transport when film thickness is ~5 to 10 nm. The theoretical model shows that this occurs when the tunneling current through the film can no longer support the electrochemical current. Thus, engineering charge transport through Li(2)O(2) is a serious challenge if Li-O(2) batteries are ever to reach their potential.
View details for DOI 10.1063/1.3663385
View details for Web of Science ID 000298490700036
View details for PubMedID 22149808
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On the behavior of Bronsted-Evans-Polanyi relations for transition metal oxides
JOURNAL OF CHEMICAL PHYSICS
2011; 134 (24)
Abstract
Versatile Brønsted-Evans-Polanyi (BEP) relations are found from density functional theory for a wide range of transition metal oxides including rutiles and perovskites. For oxides, the relation depends on the type of oxide, the active site, and the dissociating molecule. The slope of the BEP relation is strongly coupled to the adsorbate geometry in the transition state. If it is final state-like the dissociative chemisorption energy can be considered as a descriptor for the dissociation. If it is initial state-like, on the other hand, the dissociative chemisorption energy is not suitable as descriptor for the dissociation. Dissociation of molecules with strong intramolecular bonds belong to the former and molecules with weak intramolecular bonds to the latter group. We show, for the prototype system La-perovskites, that there is a "cyclic" behavior in the transition state characteristics upon change of the active transition metal of the oxide.
View details for DOI 10.1063/1.3602323
View details for Web of Science ID 000292331900043
View details for PubMedID 21721645
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Bioinspired molecular co-catalysts bonded to a silicon photocathode for solar hydrogen evolution
NATURE MATERIALS
2011; 10 (6): 434-438
Abstract
The production of fuels from sunlight represents one of the main challenges in the development of a sustainable energy system. Hydrogen is the simplest fuel to produce and although platinum and other noble metals are efficient catalysts for photoelectrochemical hydrogen evolution, earth-abundant alternatives are needed for large-scale use. We show that bioinspired molecular clusters based on molybdenum and sulphur evolve hydrogen at rates comparable to that of platinum. The incomplete cubane-like clusters (Mo(3)S(4)) efficiently catalyse the evolution of hydrogen when coupled to a p-type Si semiconductor that harvests red photons in the solar spectrum. The current densities at the reversible potential match the requirement of a photoelectrochemical hydrogen production system with a solar-to-hydrogen efficiency in excess of 10%. The experimental observations are supported by density functional theory calculations of the Mo(3)S(4) clusters adsorbed on the hydrogen-terminated Si(100) surface, providing insights into the nature of the active site.
View details for DOI 10.1038/NMAT3008
View details for Web of Science ID 000290855100017
View details for PubMedID 21516095
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Trends in Metal Oxide Stability for Nanorods, Nanotubes, and Surfaces
JOURNAL OF PHYSICAL CHEMISTRY C
2011; 115 (5): 2244-2252
View details for DOI 10.1021/jp110489u
View details for Web of Science ID 000286868600107
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Density functional theory in surface chemistry and catalysis
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
2011; 108 (3): 937-943
Abstract
Recent advances in the understanding of reactivity trends for chemistry at transition-metal surfaces have enabled in silico design of heterogeneous catalysts in a few cases. The current status of the field is discussed with an emphasis on the role of coupling theory and experiment and future challenges.
View details for DOI 10.1073/pnas.1006652108
View details for Web of Science ID 000286310300013
View details for PubMedID 21220337
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How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
ENERGY & ENVIRONMENTAL SCIENCE
2010; 3 (9): 1311-1315
View details for DOI 10.1039/c0ee00071j
View details for Web of Science ID 000282334000016
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Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method
JOURNAL OF PHYSICS-CONDENSED MATTER
2010; 22 (25)
Abstract
Electronic structure calculations have become an indispensable tool in many areas of materials science and quantum chemistry. Even though the Kohn-Sham formulation of the density-functional theory (DFT) simplifies the many-body problem significantly, one is still confronted with several numerical challenges. In this article we present the projector augmented-wave (PAW) method as implemented in the GPAW program package (https://wiki.fysik.dtu.dk/gpaw) using a uniform real-space grid representation of the electronic wavefunctions. Compared to more traditional plane wave or localized basis set approaches, real-space grids offer several advantages, most notably good computational scalability and systematic convergence properties. However, as a unique feature GPAW also facilitates a localized atomic-orbital basis set in addition to the grid. The efficient atomic basis set is complementary to the more accurate grid, and the possibility to seamlessly switch between the two representations provides great flexibility. While DFT allows one to study ground state properties, time-dependent density-functional theory (TDDFT) provides access to the excited states. We have implemented the two common formulations of TDDFT, namely the linear-response and the time propagation schemes. Electron transport calculations under finite-bias conditions can be performed with GPAW using non-equilibrium Green functions and the localized basis set. In addition to the basic features of the real-space PAW method, we also describe the implementation of selected exchange-correlation functionals, parallelization schemes, ΔSCF-method, x-ray absorption spectra, and maximally localized Wannier orbitals.
View details for DOI 10.1088/0953-8984/22/25/253202
View details for Web of Science ID 000278613100002
View details for PubMedID 21393795
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Communications: Elementary oxygen electrode reactions in the aprotic Li-air battery
JOURNAL OF CHEMICAL PHYSICS
2010; 132 (7)
Abstract
We discuss the electrochemical reactions at the oxygen electrode of an aprotic Li-air battery. Using density functional theory to estimate the free energy of intermediates during the discharge and charge of the battery, we introduce a reaction free energy diagram and identify possible origins of the overpotential for both processes. We also address the question of electron conductivity through the Li(2)O(2) electrode and show that in the presence of Li vacancies Li(2)O(2) becomes a conductor.
View details for DOI 10.1063/1.3298994
View details for Web of Science ID 000274756000001
View details for PubMedID 20170208
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The effect of Co-promotion on MoS2 catalysts for hydrodesulfurization of thiophene: A density functional study
JOURNAL OF CATALYSIS
2009; 268 (2): 201-208
View details for DOI 10.1016/j.jcat.2009.09.016
View details for Web of Science ID 000272899900003
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Trends in CO Oxidation Rates for Metal Nanoparticles and Close-Packed, Stepped, and Kinked Surfaces
JOURNAL OF PHYSICAL CHEMISTRY C
2009; 113 (24): 10548-10553
View details for DOI 10.1021/jp811185g
View details for Web of Science ID 000266930400038
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Towards the computational design of solid catalysts
NATURE CHEMISTRY
2009; 1 (1): 37-46
Abstract
Over the past decade the theoretical description of surface reactions has undergone a radical development. Advances in density functional theory mean it is now possible to describe catalytic reactions at surfaces with the detail and accuracy required for computational results to compare favourably with experiments. Theoretical methods can be used to describe surface chemical reactions in detail and to understand variations in catalytic activity from one catalyst to another. Here, we review the first steps towards using computational methods to design new catalysts. Examples include screening for catalysts with increased activity and catalysts with improved selectivity. We discuss how, in the future, such methods may be used to engineer the electronic structure of the active surface by changing its composition and structure.
View details for DOI 10.1038/NCHEM.121
View details for Web of Science ID 000268913800021
View details for PubMedID 21378799
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The nature of the active site in heterogeneous metal catalysis
CHEMICAL SOCIETY REVIEWS
2008; 37 (10): 2163-2171
Abstract
This tutorial review, of relevance for the surface science and heterogeneous catalysis communities, provides a molecular-level discussion of the nature of the active sites in metal catalysis. Fundamental concepts such as "Brønsted-Evans-Polanyi relations" and "volcano curves" are introduced, and are used to establish a strict partitioning between the so-called "electronic" and "geometrical" effects. This partitioning is subsequently employed as the basis for defining the concept "degree of structure sensitivity" which can be used when analyzing the structure sensitivity of catalytic reactions.
View details for DOI 10.1039/b800260f
View details for Web of Science ID 000259505600003
View details for PubMedID 18818819
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First principles calculations and experimental insight into methane steam reforming over transition metal catalysts
JOURNAL OF CATALYSIS
2008; 259 (1): 147-160
View details for DOI 10.1016/j.jcat.2008.08.003
View details for Web of Science ID 000260267900017
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Indirect, reversible high-density hydrogen storage in compact metal ammine salts
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2008; 130 (27): 8660-8668
Abstract
The indirect hydrogen storage capabilities of Mg(NH 3) 6Cl 2, Ca(NH 3) 8Cl 2, Mn(NH 3) 6Cl 2, and Ni(NH 3) 6Cl 2 are investigated. All four metal ammine chlorides can be compacted to solid tablets with densities of at least 95% of the crystal density. This gives very high indirect hydrogen densities both gravimetrically and volumetrically. Upon heating, NH 3 is released from the salts, and by employing an appropriate catalyst, H 2 can be released corresponding to up to 9.78 wt % H and 0.116 kg H/L for the Ca(NH 3) 8Cl 2 salt. The NH 3 release from all four salts is investigated using temperature-programmed desorption employing different heating rates. The desorption is found mainly to be limited by heat transfer, indicating that the desorption kinetics are extremely fast for all steps. During desorption from solid tablets of Mg(NH 3) 6Cl 2, Mn(NH 3) 6Cl 2, and Ni(NH 3) 6Cl 2, nanoporous structures develop, which facilitates desorption from the interior of large, compact tablets. Density functional theory calculations reproduce trends in desorption enthalpies for the systems studied, and a mechanism in which individual chains of the ammines are released from the surface of the crystal is proposed to explain the fast absorption/desorption processes.
View details for DOI 10.1021/ja076762c
View details for Web of Science ID 000257358300029
View details for PubMedID 18549216
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Identification of non-precious metal alloy catalysts for selective hydrogenation of acetylene
SCIENCE
2008; 320 (5881): 1320-1322
Abstract
The removal of trace acetylene from ethylene is performed industrially by palladium hydrogenation catalysts (often modified with silver) that avoid the hydrogenation of ethylene to ethane. In an effort to identify catalysts based on less expensive and more available metals, density functional calculations were performed that identified relations in heats of adsorption of hydrocarbon molecules and fragments on metal surfaces. This analysis not only verified the facility of known catalysts but identified nickel-zinc alloys as alternatives. Experimental studies demonstrated that these alloys dispersed on an oxide support were selective for acetylene hydrogenation at low pressures.
View details for DOI 10.1126/science.1156660
View details for Web of Science ID 000256441100039
View details for PubMedID 18535238
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Scaling relationships for adsorption energies on transition metal oxide, sulfide, and nitride surfaces
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2008; 47 (25): 4683-4686
View details for DOI 10.1002/anie.200705739
View details for Web of Science ID 000256894600012
View details for PubMedID 18484577
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Comparing electrochemical and biological water splitting
JOURNAL OF PHYSICAL CHEMISTRY C
2007; 111 (51): 18821-18823
View details for DOI 10.1021/jp077210j
View details for Web of Science ID 000251830200001
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Scaling properties of adsorption energies for hydrogen-containing molecules on transition-metal surfaces
PHYSICAL REVIEW LETTERS
2007; 99 (1)
Abstract
Density functional theory calculations are presented for CHx, x=0,1,2,3, NHx, x=0,1,2, OHx, x=0,1, and SHx, x=0,1 adsorption on a range of close-packed and stepped transition-metal surfaces. We find that the adsorption energy of any of the molecules considered scales approximately with the adsorption energy of the central, C, N, O, or S atom, the scaling constant depending only on x. A model is proposed to understand this behavior. The scaling model is developed into a general framework for estimating the reaction energies for hydrogenation and dehydrogenation reactions.
View details for DOI 10.1103/PhysRevLett.99.016105
View details for Web of Science ID 000247819900029
View details for PubMedID 17678168
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Electrochemical dissolution of surface alloys in acids: Thermodynamic trends from first-principles calculations
ELECTROCHIMICA ACTA
2007; 52 (19): 5829-5836
View details for DOI 10.1016/j.electacta.2007.02.082
View details for Web of Science ID 000246978800008
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Calculated phase diagrams for the electrochemical oxidation and reduction of water over Pt(111)
JOURNAL OF PHYSICAL CHEMISTRY B
2006; 110 (43): 21833-21839
Abstract
Ab initio density functional theory is used to calculate the electrochemical phase diagram for the oxidation and reduction of water over the Pt(111) surface. Three different schemes proposed in the literature are used to calculate the potential-dependent free energy of hydrogen, water, hydroxyl, and oxygen species adsorbed to the surface. Despite the different foundations for the models and their different complexity, they can be directly related to one another through a systematic Taylor series expansion of the Nernst equation. The simplest model, which includes the potential only as a shift in the chemical potential of the electrons, accounts very well for the thermochemical features determining the phase-diagram.
View details for DOI 10.1021/jp0631735
View details for Web of Science ID 000241553500066
View details for PubMedID 17064147
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Computational high-throughput screening of electrocatalytic materials for hydrogen evolution
NATURE MATERIALS
2006; 5 (11): 909-913
Abstract
The pace of materials discovery for heterogeneous catalysts and electrocatalysts could, in principle, be accelerated by the development of efficient computational screening methods. This would require an integrated approach, where the catalytic activity and stability of new materials are evaluated and where predictions are benchmarked by careful synthesis and experimental tests. In this contribution, we present a density functional theory-based, high-throughput screening scheme that successfully uses these strategies to identify a new electrocatalyst for the hydrogen evolution reaction (HER). The activity of over 700 binary surface alloys is evaluated theoretically; the stability of each alloy in electrochemical environments is also estimated. BiPt is found to have a predicted activity comparable to, or even better than, pure Pt, the archetypical HER catalyst. This alloy is synthesized and tested experimentally and shows improved HER performance compared with pure Pt, in agreement with the computational screening results.
View details for DOI 10.1038/nmat1752
View details for Web of Science ID 000241732000026
View details for PubMedID 17041585
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Step sites in syngas catalysis
TOPICS IN CATALYSIS
2006; 40 (1-4): 45-48
View details for DOI 10.1007/s11244-006-0107-5
View details for Web of Science ID 000242689200005
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Toward computational screening in heterogeneous catalysis: Pareto-optimal methanation catalysts
JOURNAL OF CATALYSIS
2006; 239 (2): 501-506
View details for DOI 10.1016/j.jcat.2006.02.016
View details for Web of Science ID 000236890200027
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Changing the activity of electrocatalysts for oxygen reduction by tuning the surface electronic structure
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2006; 45 (18): 2897-2901
View details for DOI 10.1002/anie.200504386
View details for Web of Science ID 000237518600015
View details for PubMedID 16596688
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Understanding the effect of steps, strain, poisons, and alloying: Methane activation on Ni surfaces
CATALYSIS LETTERS
2005; 105 (1-2): 9-13
View details for DOI 10.1007/s10562-005-7998-9
View details for Web of Science ID 000232697100002
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Biornimetic hydrogen evolution: MoS2 nanoparticles as catalyst for hydrogen evolution
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2005; 127 (15): 5308-5309
Abstract
The electrochemical hydrogen evolution reaction is catalyzed most effectively by the Pt group metals. As H2 is considered as a future energy carrier, the need for these catalysts will increase and alternatives to the scarce and expensive Pt group catalysts will be needed. We analyze the ability of different metal surfaces and of the enzymes nitrogenase and hydrogenase to catalyze the hydrogen evolution reaction and find a necessary criterion for high catalytic activity. The necessary criterion is that the binding free energy of atomic hydrogen to the catalyst is close to zero. The criterion enables us to search for new catalysts, and inspired by the nitrogenase active site, we find that MoS2 nanoparticles supported on graphite are a promising catalyst. They catalyze electrochemical hydrogen evolution at a moderate overpotential of 0.1-0.2 V.
View details for DOI 10.1021/ja0504690
View details for Web of Science ID 000228408300018
View details for PubMedID 15826154
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The electronic structure effect in heterogeneous catalysis
CATALYSIS LETTERS
2005; 100 (3-4): 111-114
View details for DOI 10.1007/s10562-004-3434-9
View details for Web of Science ID 000228226800001
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A density functional study of the chemical differences between type I and type II MOS2-based structures in hydrotreating catalysts
JOURNAL OF PHYSICAL CHEMISTRY B
2005; 109 (6): 2245-2253
Abstract
Density functional theory is used to investigate the origin of the activity differences between Type I and Type II MoS2-based structures in hydrotreating catalysts. It is well known that the Type II structures, where only weak interactions with the support exist, have a higher catalytic activity than Type I structures, where Mo-O linkages to the alumina are present. The present results show that the differences in activities for MoS2 and Co-Mo-S structures can be attributed to the electronic and bonding differences introduced by the bridging O bonds. We find that the Mo-O linkages are most probably located on the (1010) S edge. The presence of oxygen linkages increases the energy required to form sulfur vacancies significantly so that almost no vacancies can be formed at these and neighboring sites. In this way, the reactivity of the S edge is reduced. In addition, the studies also show that the linkages introduce changes in the one-dimensional metallic-like brim states. Furthermore, the presence of oxygen linkages also changes the energetics of hydrogen adsorption, which becomes less exothermic on sulfur sites directly above linkages and more exothermic on sulfur sites adjacent to linkages. The present results explain previously observed differences in Type I-Type II transition temperatures for Co-Mo-S structures with different Co contents.
View details for DOI 10.1021/jp048842y
View details for Web of Science ID 000226956300025
View details for PubMedID 16851217
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Controlling the catalytic bond-breaking selectivity of Ni surfaces by step blocking
NATURE MATERIALS
2005; 4 (2): 160-162
Abstract
The reactivity of catalytic surfaces is often dominated by very reactive low-coordinated atoms such as step-edge sites. However, very little knowledge exists concerning the influence of step edges on the selectivity in reactions involving multiple reaction pathways. Such detailed information could be very valuable in rational design of new catalysts with improved selectivity. Here we show, from an interplay between scanning tunnelling microscopy experiments and density functional theory calculations, that the activation of ethylene on Ni(111) follows the trend of higher reactivity for decomposition at step edges as compared with the higher-coordinated terrace sites. The step-edge effect is considerably more pronounced for the C-C bond breaking than for the C-H bond breaking, and thus steps play an important role in the bond-breaking selectivity. Furthermore, we demonstrate how the number of reactive step sites can be controlled by blocking the steps with Ag. This approach to nanoscale design of catalysts is exploited in the synthesis of a new high-surface-area AgNi alloy catalyst, which is tested in hydrogenolysis experiments.
View details for Web of Science ID 000226749400021
View details for PubMedID 15665835
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Ammonia synthesis from first-principles calculations
SCIENCE
2005; 307 (5709): 555-558
Abstract
The rate of ammonia synthesis over a nanoparticle ruthenium catalyst can be calculated directly on the basis of a quantum chemical treatment of the problem using density functional theory. We compared the results to measured rates over a ruthenium catalyst supported on magnesium aluminum spinel. When the size distribution of ruthenium particles measured by transmission electron microscopy was used as the link between the catalyst material and the theoretical treatment, the calculated rate was within a factor of 3 to 20 of the experimental rate. This offers hope for computer-based methods in the search for catalysts.
View details for DOI 10.1126/science.1106435
View details for Web of Science ID 000226694000040
View details for PubMedID 15681379
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Trends in the exchange current for hydrogen evolution
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
2005; 152 (3): J23-J26
View details for DOI 10.1149/1.1856988
View details for Web of Science ID 000227607300072
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Origin of the overpotential for oxygen reduction at a fuel-cell cathode
JOURNAL OF PHYSICAL CHEMISTRY B
2004; 108 (46): 17886-17892
View details for DOI 10.1021/jp047349j
View details for Web of Science ID 000225079300029
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Elastic effects behind cooperative bonding in beta-sheets
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2004; 126 (40): 13140-13143
Abstract
We present extensive density functional theory calculations of the bonding between strands in beta-sheets. We identify a significant cooperative effect whereby the interaction increases in strength with the number of strands. We show that the effect is related to a coupling between interstrand bonding and intrastrand elastic properties. It is found that a direct consequence of this coupling is that the pitch of beta-sheets should contract with increasing number of strands, and we show that the effect can be observed directly in experimental data from the Protein Data Bank.
View details for DOI 10.1021/ja0490626
View details for Web of Science ID 000224357700083
View details for PubMedID 15469313
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The Bronsted-Evans-Polanyi relation and the volcano curve in heterogeneous catalysis
JOURNAL OF CATALYSIS
2004; 224 (1): 206-217
View details for DOI 10.1016/j.jcat.2004.02.034
View details for Web of Science ID 000221200700023
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On the origin of the catalytic activity of gold nanoparticles for low-temperature CO oxidation
JOURNAL OF CATALYSIS
2004; 223 (1): 232-235
View details for DOI 10.1016/j.jcat.2004.01.001
View details for Web of Science ID 000220726900024
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Atomic-scale imaging of carbon nanofibre growth
NATURE
2004; 427 (6973): 426-429
Abstract
The synthesis of carbon nanotubes with predefined structure and functionality plays a central role in the field of nanotechnology, whereas the inhibition of carbon growth is needed to prevent a breakdown of industrial catalysts for hydrogen and synthesis gas production. The growth of carbon nanotubes and nanofibres has therefore been widely studied. Recent advances in in situ techniques now open up the possibility of studying gas-solid interactions at the atomic level. Here we present time-resolved, high-resolution in situ transmission electron microscope observations of the formation of carbon nanofibres from methane decomposition over supported nickel nanocrystals. Carbon nanofibres are observed to develop through a reaction-induced reshaping of the nickel nanocrystals. Specifically, the nucleation and growth of graphene layers are found to be assisted by a dynamic formation and restructuring of mono-atomic step edges at the nickel surface. Density-functional theory calculations indicate that the observations are consistent with a growth mechanism involving surface diffusion of carbon and nickel atoms. The finding that metallic step edges act as spatiotemporal dynamic growth sites may be important for understanding other types of catalytic reactions and nanomaterial syntheses.
View details for DOI 10.1038/nature02278
View details for Web of Science ID 000188470500038
View details for PubMedID 14749826
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Atomic and electronic structure of MoS2 nanoparticles
PHYSICAL REVIEW B
2003; 67 (8)
View details for DOI 10.1103/PhysRevB.67.085410
View details for Web of Science ID 000181520100059
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Universality in heterogeneous catalysis
JOURNAL OF CATALYSIS
2002; 209 (2): 275-278
View details for DOI 10.1006/jcat.2002.3615
View details for Web of Science ID 000176916300001
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Combined electronic structure and evolutionary search approach to materials design
PHYSICAL REVIEW LETTERS
2002; 88 (25)
Abstract
We show that density functional theory calculations have reached an accuracy and speed making it possible to use them in conjunction with an evolutionary algorithm to search for materials with specific properties. The approach is illustrated by finding the most stable four component alloys out of the 192 016 possible fcc and bcc alloys that can be constructed out of 32 different metals. A number of well known and new "super alloys" are identified in this way.
View details for DOI 10.1103/PhysRevLett.88.255506
View details for Web of Science ID 000176554800023
View details for PubMedID 12097098
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The surface science of enzymes
SURFACE SCIENCE
2002; 500 (1-3): 678-698
View details for Web of Science ID 000175303400030
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One-dimensional metallic edge states in MoS2
PHYSICAL REVIEW LETTERS
2001; 87 (19)
Abstract
By the use of density functional calculations it is shown that the edges of a two-dimensional slab of insulating MoS2 exhibit several metallic states. These edge states can be viewed as one-dimensional conducting wires, and we show that they can be observed directly using scanning tunneling microscopy for single-layer MoS2 nanoparticles grown on a support.
View details for DOI 10.1103/PhysRevLett.87.196803
View details for Web of Science ID 000172027200043
View details for PubMedID 11690441
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Catalyst design by interpolation in the periodic table: Bimetallic ammonia synthesis catalysts
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2001; 123 (34): 8404-8405
View details for DOI 10.1021/ja010963d
View details for Web of Science ID 000170730000028
View details for PubMedID 11516293
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The Bronsted-Evans-Polanyi relation and the volcano plot for ammonia synthesis over transition metal catalysts
JOURNAL OF CATALYSIS
2001; 197 (2): 229-231
View details for Web of Science ID 000167253600001
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Ammonia synthesis at low temperatures
JOURNAL OF CHEMICAL PHYSICS
2000; 112 (12): 5343-5347
View details for Web of Science ID 000085766100015
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Atomic-scale structure of single-layer MoS2 nanoclusters
PHYSICAL REVIEW LETTERS
2000; 84 (5): 951-954
View details for Web of Science ID 000085005700039
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Theoretical surface science and catalysis - Calculations and concepts
ADVANCES IN CATALYSIS, VOL 45
2000; 45: 71-129
View details for Web of Science ID 000089180200002
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Role of steps in N-2 activation on Ru(0001)
PHYSICAL REVIEW LETTERS
1999; 83 (9): 1814-1817
View details for Web of Science ID 000082242600029
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Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals
PHYSICAL REVIEW B
1999; 59 (11): 7413-7421
View details for Web of Science ID 000079507700036
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Effect of strain on the reactivity of metal surfaces
PHYSICAL REVIEW LETTERS
1998; 81 (13): 2819-2822
View details for Web of Science ID 000076133300050
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Alkali promotion of N-2 dissociation over Ru(0001)
PHYSICAL REVIEW LETTERS
1998; 80 (19): 4333-4336
View details for Web of Science ID 000073550200056
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Design of a surface alloy catalyst for steam reforming
SCIENCE
1998; 279 (5358): 1913-1915
View details for Web of Science ID 000072613300040
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Electronic factors determining the reactivity of metal surfaces
SURFACE SCIENCE
1995; 343 (3): 211-220
View details for Web of Science ID A1995TN95500009
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A KINETIC-MODEL OF METHANOL SYNTHESIS
JOURNAL OF CATALYSIS
1995; 156 (2): 229-242
View details for Web of Science ID A1995RZ09300004
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WHY GOLD IS THE NOBLEST OF ALL THE METALS
NATURE
1995; 376 (6537): 238-240
View details for Web of Science ID A1995RK33100041
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The surface science based ammonia kinetics revisited
TOPICS IN CATALYSIS
1994; 1 (3-4): 253-263
View details for Web of Science ID 000208529500006
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A KINETIC-MODEL OF THE WATER GAS SHIFT REACTION
JOURNAL OF CATALYSIS
1992; 134 (2): 445-468
View details for Web of Science ID A1992HK08500006
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A DESCRIPTION OF THE HIGH-PRESSURE AMMONIA-SYNTHESIS REACTION BASED ON SURFACE SCIENCE
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
1987; 5 (4): 581-585
View details for Web of Science ID A1987J259000048
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INTERATOMIC INTERACTIONS IN THE EFFECTIVE-MEDIUM THEORY
PHYSICAL REVIEW B
1987; 35 (14): 7423-7442
View details for Web of Science ID A1987H364200015
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BRIDGING THE PRESSURE GAP BETWEEN ULTRAHIGH-VACUUM SURFACE PHYSICS AND HIGH-PRESSURE CATALYSIS
PHYSICAL REVIEW LETTERS
1985; 55 (22): 2502-2505
View details for Web of Science ID A1985AUN4900035
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MICROSCOPIC MODEL FOR THE POISONING AND PROMOTION OF ADSORPTION RATES BY ELECTRONEGATIVE AND ELECTROPOSITIVE ATOMS
SURFACE SCIENCE
1984; 137 (1): 65-78
View details for Web of Science ID A1984SE23100006
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EFFECTIVE-MEDIUM THEORY OF CHEMICAL-BINDING - APPLICATION TO CHEMISORPTION
PHYSICAL REVIEW B
1980; 21 (6): 2131-2136
View details for Web of Science ID A1980JL83400013
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Surface energetics of alkaline-earth metal oxides: Trends in stability and adsorption of small molecules
PHYSICAL REVIEW B
2015; 91 (15)
View details for DOI 10.1103/PhysRevB.91.155401
View details for Web of Science ID 000352129200001
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Theoretical evaluation of the surface electrochemistry of perovskites with promising photon absorption properties for solar water splitting.
Physical chemistry chemical physics
2015; 17 (4): 2634-2640
Abstract
In this work, we present first-principles calculations describing the catalytic activity for of a set of photoelectrocatalysts identified as candidates for total water splitting in a previous screening study for bulk stability and bandgap. Our Density Functional Theory (DFT) calculations of the intermediate energetics for hydrogen evolution and oxygen evolution suggest that none of the proposed materials has the ideal combination of bandgap and surface chemical properties that should allow for total water splitting in a single material. This result suggests that co-catalysts are necessary to overcome the kinetic limitations of the both reactions, although some materials may catalyze one half-reaction, as has been observed in experiment.
View details for DOI 10.1039/c4cp05259e
View details for PubMedID 25502921
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Trends in Hydrodesulfurization Catalysis Based on Realistic Surface Models
CATALYSIS LETTERS
2014; 144 (8): 1425-1432
View details for DOI 10.1007/s10562-014-1279-4
View details for Web of Science ID 000339938000010
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Catalysis. Assessing the reliability of calculated catalytic ammonia synthesis rates.
Science
2014; 345 (6193): 197-200
Abstract
We introduce a general method for estimating the uncertainty in calculated materials properties based on density functional theory calculations. We illustrate the approach for a calculation of the catalytic rate of ammonia synthesis over a range of transition-metal catalysts. The correlation between errors in density functional theory calculations is shown to play an important role in reducing the predicted error on calculated rates. Uncertainties depend strongly on reaction conditions and catalyst material, and the relative rates between different catalysts are considerably better described than the absolute rates. We introduce an approach for incorporating uncertainty when searching for improved catalysts by evaluating the probability that a given catalyst is better than a known standard.
View details for DOI 10.1126/science.1253486
View details for PubMedID 25013071
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Reactivity Descriptor in Solid Acid Catalysis: Predicting Turnover Frequencies for Propene Methylation in Zeotypes
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2014; 5 (9): 1516-1521
View details for DOI 10.1021/jz500482z
View details for Web of Science ID 000335432800003
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Theoretical Analysis of Transition-Metal Catalysts for Formic Acid Decomposition
ACS CATALYSIS
2014; 4 (4): 1226-1233
View details for DOI 10.1021/cs400664z
View details for Web of Science ID 000338807100024
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Tuning the MoS2 Edge-Site Activity for Hydrogen Evolution via Support Interactions
NANO LETTERS
2014; 14 (3): 1381-1387
Abstract
The hydrogen evolution reaction (HER) on supported MoS2 catalysts is investigated using periodic density functional theory, employing the new BEEF-vdW functional that explicitly takes long-range van der Waals (vdW) forces into account. We find that the support interactions involving vdW forces leads to significant changes in the hydrogen binding energy, resulting in several orders of magnitude difference in HER activity. It is generally seen for the Mo-edge that strong adhesion of the catalyst onto the support leads to weakening in the hydrogen binding. This presents a way to optimally tune the hydrogen binding on MoS2 and explains the lower than expected exchange current densities of supported MoS2 in electrochemical H2 evolution studies.
View details for DOI 10.1021/nl404444k
View details for Web of Science ID 000335720300044
View details for PubMedID 24499163
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Pt Skin Versus Pt Skeleton Structures of Pt3Sc as Electrocatalysts for Oxygen Reduction
TOPICS IN CATALYSIS
2014; 57 (1-4): 245-254
View details for DOI 10.1007/s11244-013-0179-y
View details for Web of Science ID 000330829600024
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Lithium and oxygen vacancies and their role in Li2O2 charge transport in Li-O-2 batteries
ENERGY & ENVIRONMENTAL SCIENCE
2014; 7 (2): 720-727
View details for DOI 10.1039/c3ee42446d
View details for Web of Science ID 000331413700026
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Activity and Selectivity Trends in Synthesis Gas Conversion to Higher Alcohols
TOPICS IN CATALYSIS
2014; 57 (1-4): 135-142
View details for DOI 10.1007/s11244-013-0169-0
View details for Web of Science ID 000330829600014
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Trends in electrochemical CO2 reduction activity for open and close-packed metal surfaces
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2014; 16 (10): 4720-4727
Abstract
We present a theoretical analysis of trends in overpotentials for electrocatalytic CO2 reduction based on density functional theory calculations. The analysis is based on understanding variations in the free energy of intermediates and mapping out the potential at which different elementary steps are exergonic as a measure of the catalytic activity. We study different surface structures and introduce a simple model for including the effect of adsorbate-adsorbate interactions. We find that high coverages of CO under typical reaction conditions for the more reactive transition metals affect the catalytic activity towards the CO2 reduction reaction, but the ordering of metal activities is not changed. For the hydrogen evolution reaction, a high CO coverage shifts the maximum activity towards more reactive metals than Pt.
View details for DOI 10.1039/c3cp54822h
View details for Web of Science ID 000332393200032
View details for PubMedID 24468980
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Thermochemistry and micro-kinetic analysis of methanol synthesis on ZnO (0001)
JOURNAL OF CATALYSIS
2014; 309: 397-407
View details for DOI 10.1016/j.jcat.2013.10.015
View details for Web of Science ID 000330815400042
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In silico search for novel methane steam reforming catalysts
NEW JOURNAL OF PHYSICS
2013; 15
View details for DOI 10.1088/1367-2630/15/12/125021
View details for Web of Science ID 000329439500001
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On the effect of coverage-dependent adsorbate-adsorbate interactions for CO methanation on transition metal surfaces
JOURNAL OF CATALYSIS
2013; 307: 275-282
View details for DOI 10.1016/j.jcat.2013.08.002
View details for Web of Science ID 000327903900030
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Ni-Fe-S Cubanesin CO2 Reduction Electrocatalysis: A DFT Study
ACS CATALYSIS
2013; 3 (11): 2640-2643
View details for DOI 10.1021/cs4005419
View details for Web of Science ID 000326615200028
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Tunneling and Polaron Charge Transport through Li2O2 in Li-O-2 Batteries
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2013; 4 (20): 3494-3499
View details for DOI 10.1021/jz401926f
View details for Web of Science ID 000326124500021
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Analysis of sulfur-induced selectivity changes for anhydrous methanol dehydrogenation on Ni(100) surfaces
SURFACE SCIENCE
2013; 613: 58-62
View details for DOI 10.1016/j.suse.2013.03.004
View details for Web of Science ID 000319180600010
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Electroreduction of Methanediol on Copper
CATALYSIS LETTERS
2013; 143 (7): 631-635
View details for DOI 10.1007/s10562-013-1023-5
View details for Web of Science ID 000321239300001
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Selective Ultrafast Probing of Transient Hot Chemisorbed and Precursor States of CO on Ru(0001)
PHYSICAL REVIEW LETTERS
2013; 110 (18)
Abstract
We have studied the femtosecond dynamics following optical laser excitation of CO adsorbed on a Ru surface by monitoring changes in the occupied and unoccupied electronic structure using ultrafast soft x-ray absorption and emission. We recently reported [M. Dell'Angela et al. Science 339, 1302 (2013)] a phonon-mediated transition into a weakly adsorbed precursor state occurring on a time scale of >2 ps prior to desorption. Here we focus on processes within the first picosecond after laser excitation and show that the metal-adsorbate coordination is initially increased due to hot-electron-driven vibrational excitations. This process is faster than, but occurs in parallel with, the transition into the precursor state. With resonant x-ray emission spectroscopy, we probe each of these states selectively and determine the respective transient populations depending on optical laser fluence. Ab initio molecular dynamics simulations of CO adsorbed on Ru(0001) were performed at 1500 and 3000 K providing insight into the desorption process.
View details for DOI 10.1103/PhysRevLett.110.186101
View details for Web of Science ID 000319019300011
View details for PubMedID 23683223
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Guest-host interactions of arenes in H-ZSM-5 and their impact on methanol-to-hydrocarbons deactivation processes
JOURNAL OF CATALYSIS
2013; 300: 235-241
View details for DOI 10.1016/j.jcat.2013.01.009
View details for Web of Science ID 000317558000026
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Insights into CC Coupling in CO2 Electroreduction on Copper Electrodes
CHEMCATCHEM
2013; 5 (3): 737-742
View details for DOI 10.1002/cctc.201200564
View details for Web of Science ID 000315416200018
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First-Principles Calculations of FischerTropsch Processes Catalyzed by Nitrogenase Enzymes
CHEMCATCHEM
2013; 5 (3): 732-736
View details for DOI 10.1002/cctc.201200635
View details for Web of Science ID 000315416200017
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Formation energies of group I and II metal oxides using random phase approximation
PHYSICAL REVIEW B
2013; 87 (7)
View details for DOI 10.1103/PhysRevB.87.075207
View details for Web of Science ID 000315374800005
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Li-O-2 Kinetic Overpotentials: Tafel Plots from Experiment and First-Principles Theory
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2013; 4 (4): 556-560
View details for DOI 10.1021/jz400019y
View details for Web of Science ID 000315432000001
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Understanding Trends in the Electrocatalytic Activity of Metals and Enzymes for CO2 Reduction to CO
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2013; 4 (3): 388-392
View details for DOI 10.1021/jz3021155
View details for Web of Science ID 000314907500009
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Theoretical evidence for low kinetic overpotentials in Li-O-2 electrochemistry
JOURNAL OF CHEMICAL PHYSICS
2013; 138 (3)
Abstract
We develop a density functional theory model for the electrochemical growth and dissolution of Li(2)O(2) on various facets, terminations, and sites (terrace, steps, and kinks) of a Li(2)O(2) surface. We argue that this is a reasonable model to describe discharge and charge of Li-O(2) batteries over most of the discharge-charge cycle. Because non-stoichiometric surfaces are potential dependent and since the potential varies during discharge and charge, we study the thermodynamic stability of facets, terminations, and steps as a function of potential. This suggests that different facets, terminations, and sites may dominate in charge relative to those for discharge. We find very low thermodynamic overpotentials (<0.2 V) for both discharge and charge at many sites on the facets studied. These low thermodynamic overpotentials for both discharge and charge are in very good agreement with the low kinetic overpotentials observed in recent experiments. However, there are other predicted paths for discharge/charge that have higher overpotentials, so the phase space available for the electrochemistry opens up with overpotential.
View details for DOI 10.1063/1.4773242
View details for Web of Science ID 000313671700030
View details for PubMedID 23343289
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Investigation of Catalytic Finite-Size-Effects of Platinum Metal Clusters
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2013; 4 (1): 222-226
View details for DOI 10.1021/jz3018286
View details for Web of Science ID 000313142000032
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Modeling CO2 reduction on Pt(111)
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2013; 15 (19): 7114-7122
Abstract
Density functional theory was used to model the electrochemical reduction of CO2 on Pt(111) with an explicit solvation layer and the presence of extra hydrogen atoms to represent a negatively charged electrode. We focused on the electronic energy barriers for the first four lowest energy proton-electron transfer steps for reducing CO2 on Pt(111) beginning with adsorbed *CO2 and continuing with *COOH, *CO + H2O, *COH, and ending with *C + H2O. We find that simple elementary steps in which a proton is transferred to an adsorbate (such as the protonation of *CO to *COH) have small barriers on the order of 0.1 eV. Elementary steps in which a proton is transferred and a C-O bond is simultaneously cleaved show barriers on the order of 0.5 eV. All barriers calculated for these steps show no sign of being insurmountable at room temperature. To explain why these barriers are so small, we analyze the charge density and the density of states plots to see that first, the electron transfer is decoupled from the proton transfer so that in the initial state, the surface and adsorbate are already charged up and can easily accept the proton from solution. Also, we see that in the cases where barriers are on the order of 0.1 eV, electron density in the initial state localizes on the oxygen end of the adsorbate, while electron density is more spread out on the surface for initial states of the C-O bond cleaving elementary steps.
View details for DOI 10.1039/c3cp50645b
View details for Web of Science ID 000317980600016
View details for PubMedID 23552398
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First principles investigation of zinc-anode dissolution in zinc-air batteries
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2013; 15 (17): 6416-6421
Abstract
With surging interest in high energy density batteries, much attention has recently been devoted to metal-air batteries. The zinc-air battery has been known for more than a hundred years and is commercially available as a primary battery, but recharging has remained elusive, in part because the fundamental mechanisms still remain to be fully understood. Here, we present a density functional theory investigation of the zinc dissolution (oxidation) on the anode side in the zinc-air battery. Two models are envisaged, the most stable (0001) surface and a kink surface. The kink model proves to be more accurate as it brings about some important features of bulk dissolution and yields results in good agreement with experiments. From the adsorption energies of hydroxyl species and experimental values, we construct a free energy diagram and confirm that there is a small overpotential associated with the reaction. The applied methodology provides new insight into computational modelling and design of secondary metal-air batteries.
View details for DOI 10.1039/c3cp50349f
View details for Web of Science ID 000317012800033
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CO and CO2 Hydrogenation to Methanol Calculated Using the BEEF-vdW Functional
CATALYSIS LETTERS
2013; 143 (1): 71-73
View details for DOI 10.1007/s10562-012-0947-5
View details for Web of Science ID 000313653600009
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Energetics of Oxygen Adatoms, Hydroxyl Species and Water Dissociation on Pt(111)
JOURNAL OF PHYSICAL CHEMISTRY C
2012; 116 (49): 25772-25776
View details for DOI 10.1021/jp3066794
View details for Web of Science ID 000312176100015
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The Computational Materials Repository
COMPUTING IN SCIENCE & ENGINEERING
2012; 14 (6): 51-57
View details for Web of Science ID 000310221500007
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Importance of Correlation in Determining Electrocatalytic Oxygen Evolution Activity on Cobalt Oxides
JOURNAL OF PHYSICAL CHEMISTRY C
2012; 116 (39): 21077-21082
View details for DOI 10.1021/jp306303y
View details for Web of Science ID 000309375700054
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CO hydrogenation to methanol on Cu-Ni catalysts: Theory and experiment
JOURNAL OF CATALYSIS
2012; 293: 51-60
View details for DOI 10.1016/j.jcat.2012.06.004
View details for Web of Science ID 000308836800005
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Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces
ACS CATALYSIS
2012; 2 (8): 1654-1660
View details for DOI 10.1021/cs300227s
View details for Web of Science ID 000307257800013
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Evidence of Scrambling over Ruthenium-based Catalysts in Supercritical-water Gasification
CHEMCATCHEM
2012; 4 (8): 1185-1189
View details for DOI 10.1002/cctc.201100450
View details for Web of Science ID 000306907700023
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Application of a new informatics tool in heterogeneous catalysis: Analysis of methanol dehydrogenation on transition metal catalysts for the production of anhydrous formaldehyde
JOURNAL OF CATALYSIS
2012; 291: 133-137
View details for DOI 10.1016/j.jcat.2012.04.017
View details for Web of Science ID 000306779600017
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Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters
TOPICS IN CATALYSIS
2012; 55 (5-6): 336-344
View details for DOI 10.1007/s11244-012-9798-y
View details for Web of Science ID 000303883700011
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Elementary steps of syngas reactions on Mo2C(001): Adsorption thermochemistry and bond dissociation
JOURNAL OF CATALYSIS
2012; 290: 108-117
View details for DOI 10.1016/j.jcat.2012.03.007
View details for Web of Science ID 000305098400011
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Twin Problems of Interfacial Carbonate Formation in Nonaqueous Li-O-2 Batteries
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2012; 3 (8): 997-1001
View details for DOI 10.1021/jz300243r
View details for Web of Science ID 000302924500008
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Photoelectrocatalysis and electrocatalysis on silicon electrodes decorated with cubane-like clusters
JOURNAL OF PHOTONICS FOR ENERGY
2012; 2
View details for DOI 10.1117/1.JPE.2.026001
View details for Web of Science ID 000309174400001
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Simulating Linear Sweep Voltammetry from First-Principles: Application to Electrochemical Oxidation of Water on Pt(111) and Pt3Ni(111)
JOURNAL OF PHYSICAL CHEMISTRY C
2012; 116 (7): 4698-4704
View details for DOI 10.1021/jp210802q
View details for Web of Science ID 000301156500043
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A theoretical evaluation of possible transition metal electro-catalysts for N2 reduction.
Physical chemistry chemical physics
2012; 14 (3): 1235-1245
Abstract
Theoretical studies of the possibility of forming ammonia electrochemically at ambient temperature and pressure are presented. Density functional theory calculations were used in combination with the computational standard hydrogen electrode to calculate the free energy profile for the reduction of N(2) admolecules and N adatoms on several close-packed and stepped transition metal surfaces in contact with an acidic electrolyte. Trends in the catalytic activity were calculated for a range of transition metal surfaces and applied potentials under the assumption that the activation energy barrier scales with the free energy difference in each elementary step. The most active surfaces, on top of the volcano diagrams, are Mo, Fe, Rh, and Ru, but hydrogen gas formation will be a competing reaction reducing the faradaic efficiency for ammonia production. Since the early transition metal surfaces such as Sc, Y, Ti, and Zr bind N-adatoms more strongly than H-adatoms, a significant production of ammonia compared with hydrogen gas can be expected on those metal electrodes when a bias of -1 V to -1.5 V vs. SHE is applied. Defect-free surfaces of the early transition metals are catalytically more active than their stepped counterparts.
View details for DOI 10.1039/c1cp22271f
View details for PubMedID 22146855
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Activity Descriptors for CO2 Electroreduction to Methane on Transition-Metal Catalysts
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
2012; 3 (2): 251-258
View details for DOI 10.1021/jz201461p
View details for Web of Science ID 000299365500019
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Identifying active surface phases for metal oxide electrocatalysts: a study of manganese oxide bi-functional catalysts for oxygen reduction and water oxidation catalysis
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2012; 14 (40): 14010-14022
Abstract
Progress in the field of electrocatalysis is often hampered by the difficulty in identifying the active site on an electrode surface. Herein we combine theoretical analysis and electrochemical methods to identify the active surfaces in a manganese oxide bi-functional catalyst for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER). First, we electrochemically characterize the nanostructured ?-Mn(2)O(3) and find that it undergoes oxidation in two potential regions: initially, between 0.5 V and 0.8 V, a potential region relevant to the ORR and, subsequently, between 0.8 V and 1.0 V, a potential region between the ORR and the OER relevant conditions. Next, we perform density function theory (DFT) calculations to understand the changes in the MnO(x) surface as a function of potential and to elucidate reaction mechanisms that lead to high activities observed in the experiments. Using DFT, we construct surface Pourbaix and free energy diagrams of three different MnO(x) surfaces and identify 1/2 ML HO* covered Mn(2)O(3) and O* covered MnO(2), as the active surfaces for the ORR and the OER, respectively. Additionally, we find that the ORR occurs through an associative mechanism and that its overpotential is highly dependent on the stabilization of intermediates through hydrogen bonds with water molecules. We also determine that OER occurs through direct recombination mechanism and that its major source of overpotential is the scaling relationship between HOO* and HO* surface intermediates. Using a previously developed Sabatier model we show that the theoretical predictions of catalytic activities match the experimentally determined onset potentials for the ORR and the OER, both qualitatively and quantitatively. Consequently, the combination of first-principles theoretical analysis and experimental methods offers an understanding of manganese oxide oxygen electrocatalysis at the atomic level, achieving fundamental insight that can potentially be used to design and develop improved electrocatalysts for the ORR and the OER and other important reactions of technological interest.
View details for DOI 10.1039/c2cp40841d
View details for Web of Science ID 000309140400036
View details for PubMedID 22990481
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The importance of surface morphology in controlling the selectivity of polycrystalline copper for CO2 electroreduction
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2012; 14 (1): 76-81
Abstract
This communication examines the effect of the surface morphology of polycrystalline copper on electroreduction of CO(2). We find that a copper nanoparticle covered electrode shows better selectivity towards hydrocarbons compared with the two other studied surfaces, an electropolished copper electrode and an argon sputtered copper electrode. Density functional theory calculations provide insight into the surface morphology effect.
View details for DOI 10.1039/c1cp22700a
View details for Web of Science ID 000297593800006
View details for PubMedID 22071504
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Solar hydrogen production with semiconductor metal oxides: new directions in experiment and theory
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2012; 14 (1): 49-70
Abstract
An overview of a collaborative experimental and theoretical effort toward efficient hydrogen production via photoelectrochemical splitting of water into di-hydrogen and di-oxygen is presented here. We present state-of-the-art experimental studies using hematite and TiO(2) functionalized with gold nanoparticles as photoanode materials, and theoretical studies on electro and photo-catalysis of water on a range of metal oxide semiconductor materials, including recently developed implementation of self-interaction corrected energy functionals.
View details for DOI 10.1039/c1cp23212f
View details for Web of Science ID 000297593800004
View details for PubMedID 22083224
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A theoretical evaluation of possible transition metal electro-catalysts for N-2 reduction
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2012; 14 (3): 1235-1245
View details for DOI 10.1039/c1cp22271f
View details for Web of Science ID 000299271800015
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Scaling relationships for adsorption energies of C-2 hydrocarbons on transition metal surfaces
CHEMICAL ENGINEERING SCIENCE
2011; 66 (24): 6318-6323
View details for DOI 10.1016/j.ces.2011.02.050
View details for Web of Science ID 000296568500003
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Electronic shell structure and chemisorption on gold nanoparticles
PHYSICAL REVIEW B
2011; 84 (24)
View details for DOI 10.1103/PhysRevB.84.245429
View details for Web of Science ID 000298116000011
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Optimizing Perovskites for the Water-Splitting Reaction
SCIENCE
2011; 334 (6061): 1355-1356
View details for DOI 10.1126/science.1215081
View details for Web of Science ID 000297787700037
View details for PubMedID 22158809
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Ab Initio van der Waals Interactions in Simulations of Water Alter Structure from Mainly Tetrahedral to High-Density-Like
JOURNAL OF PHYSICAL CHEMISTRY B
2011; 115 (48): 14149-14160
Abstract
The structure of liquid water at ambient conditions is studied in ab initio molecular dynamics simulations in the NVE ensemble using van der Waals (vdW) density-functional theory, i.e., using the new exchange-correlation functionals optPBE-vdW and vdW-DF2, where the latter has softer nonlocal correlation terms. Inclusion of the more isotropic vdW interactions counteracts highly directional hydrogen bonds, which are enhanced by standard functionals. This brings about a softening of the microscopic structure of water, as seen from the broadening of angular distribution functions and, in particular, from the much lower and broader first peak in the oxygen-oxygen pair-correlation function (PCF) and loss of structure in the outer hydration shells. Inclusion of vdW interactions is shown to shift the balance of resulting structures from open tetrahedral to more close-packed. The resulting O-O PCF shows some resemblance with experiment for high-density water (Soper, A. K. and Ricci, M. A. Phys. Rev. Lett. 2000, 84, 2881), but not directly with experiment for ambient water. Considering the accuracy of the new functionals for interaction energies, we investigate whether the simulation protocol could cause the deviation. An O-O PCF consisting of a linear combination of 70% from vdW-DF2 and 30% from low-density liquid water, as extrapolated from experiments, reproduces near-quantitatively the experimental O-O PCF for ambient water. This suggests the possibility that the new functionals may be reliable and that instead larger-scale simulations in the NPT ensemble, where the density is allowed to fluctuate in accordance with proposals for supercooled water, could resolve the apparent discrepancy with the measured PCF.
View details for DOI 10.1021/jp2040345
View details for Web of Science ID 000297446200020
View details for PubMedID 21806000
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Trends in oxygen reduction and methanol activation on transition metal chalcogenides
ELECTROCHIMICA ACTA
2011; 56 (27): 9783-9788
View details for DOI 10.1016/j.electacta.2011.08.045
View details for Web of Science ID 000297399100013
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Tailoring the Activity for Oxygen Evolution Electrocatalysis on Rutile TiO2(110) by Transition-Metal Substitution
CHEMCATCHEM
2011; 3 (10): 1607-1611
View details for DOI 10.1002/cctc.201100160
View details for Web of Science ID 000297111700012
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Finite Size Effects in Chemical Bonding: From Small Clusters to Solids
CATALYSIS LETTERS
2011; 141 (8): 1067-1071
View details for DOI 10.1007/s10562-011-0632-0
View details for Web of Science ID 000293632800002
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Structure effects on the energetics of the electrochemical reduction of CO2 by copper surfaces
SURFACE SCIENCE
2011; 605 (15-16): 1354-1359
View details for DOI 10.1016/j.susc.2011.04.028
View details for Web of Science ID 000293671000006
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Hydrogen evolution on Au(111) covered with submonolayers of Pd
PHYSICAL REVIEW B
2011; 84 (4)
View details for DOI 10.1103/PhysRevB.84.045407
View details for Web of Science ID 000292385000010
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Atomic-Scale Modeling of Particle Size Effects for the Oxygen Reduction Reaction on Pt
CATALYSIS LETTERS
2011; 141 (7): 909-913
View details for DOI 10.1007/s10562-011-0637-8
View details for Web of Science ID 000292652300001
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Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces
CHEMCATCHEM
2011; 3 (7): 1159-1165
View details for DOI 10.1002/cctc.201000397
View details for Web of Science ID 000293384000012
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The role of transition metal interfaces on the electronic transport in lithium-air batteries
CATALYSIS TODAY
2011; 165 (1): 2-9
View details for DOI 10.1016/j.cattod.2010.12.022
View details for Web of Science ID 000289789800002
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Van der Waals effect in weak adsorption affecting trends in adsorption, reactivity, and the view of substrate nobility
PHYSICAL REVIEW B
2011; 83 (11)
View details for DOI 10.1103/PhysRevB.83.113401
View details for Web of Science ID 000288242800001
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Universal Bronsted-Evans-Polanyi Relations for C-C, C-O, C-N, N-O, N-N, and O-O Dissociation Reactions
CATALYSIS LETTERS
2011; 141 (3): 370-373
View details for DOI 10.1007/s10562-010-0477-y
View details for Web of Science ID 000287506800002
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The Pt(111)/Electrolyte Interface under Oxygen Reduction Reaction Conditions: An Electrochemical Impedance Spectroscopy Study
LANGMUIR
2011; 27 (5): 2058-2066
Abstract
The Pt(111)/electrolyte interface has been characterized during the oxygen reduction reaction (ORR) in 0.1 M HClO(4) using electrochemical impedance spectroscopy. The surface was studied within the potential region where adsorption of OH* and O* species occur without significant place exchange between the adsorbate and Pt surface atoms (0.45-1.15 V vs RHE). An equivalent electric circuit is proposed to model the Pt(111)/electrolyte interface under ORR conditions within the selected potential window. This equivalent circuit reflects three processes with different time constants, which occur simultaneously during the ORR at Pt(111). Density functional theory (DFT) calculations were used to correlate and interpret the results of the measurements. The calculations indicate that the coadsorption of ClO(4)* and Cl* with OH* is unlikely. Our analysis suggests that the two-dimensional (2D) structures formed in O(2)-free solution are also formed under ORR conditions.
View details for DOI 10.1021/la1042475
View details for Web of Science ID 000287624700069
View details for PubMedID 21244087
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First-principles investigations of Ni3Al(111) and NiAl(110) surfaces at metal dusting conditions
SURFACE SCIENCE
2011; 605 (5-6): 582-592
View details for DOI 10.1016/j.susc.2010.12.023
View details for Web of Science ID 000287833500019
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Universal transition state scaling relations for (de)hydrogenation over transition metals
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2011; 13 (46): 20760-20765
Abstract
We analyse the transition state energies for 249 hydrogenation/dehydrogenation reactions of atoms and simple molecules over close-packed and stepped surfaces and nanoparticles of transition metals using Density Functional Theory. Linear energy scaling relations are observed for the transition state structures leading to transition state scaling relations for all the investigated reactions. With a suitable choice of reference systems the transition state scaling relations form a universality class that can be approximated with one single linear relation describing the entire range of reactions over all types of surfaces and nanoclusters.
View details for DOI 10.1039/c1cp20547a
View details for Web of Science ID 000297071400029
View details for PubMedID 21996683
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Bio-inspired co-catalysts bonded to a silicon photocathode for solar hydrogen evolution
SOLAR HYDROGEN AND NANOTECHNOLOGY VI
2011; 8109
View details for DOI 10.1117/12.892994
View details for Web of Science ID 000297588100014
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Descriptor-Based Analysis Applied to HCN Synthesis from NH3 and CH4
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2011; 50 (20): 4601-4605
View details for DOI 10.1002/anie.201100353
View details for Web of Science ID 000290663600007
View details for PubMedID 21500324
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A multifaceted approach to hydrogen storage
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2011; 13 (38): 16955-16972
Abstract
The widespread adoption of hydrogen as an energy carrier could bring significant benefits, but only if a number of currently intractable problems can be overcome. Not the least of these is the problem of storage, particularly when aimed at use onboard light-vehicles. The aim of this overview is to look in depth at a number of areas linked by the recently concluded HYDROGEN research network, representing an intentionally multi-faceted selection with the goal of advancing the field on a number of fronts simultaneously. For the general reader we provide a concise outline of the main approaches to storing hydrogen before moving on to detailed reviews of recent research in the solid chemical storage of hydrogen, and so provide an entry point for the interested reader on these diverse topics. The subjects covered include: the mechanisms of Ti catalysis in alanates; the kinetics of the borohydrides and the resulting limitations; novel transition metal catalysts for use with complex hydrides; less common borohydrides; protic-hydridic stores; metal ammines and novel approaches to nano-confined metal hydrides.
View details for DOI 10.1039/c1cp22312g
View details for Web of Science ID 000295128000006
View details for PubMedID 21887432
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Modeling the Electrochemical Hydrogen Oxidation and Evolution Reactions on the Basis of Density Functional Theory Calculations (vol 114, pg 18182, 2010)
JOURNAL OF PHYSICAL CHEMISTRY C
2010; 114 (50): 22374-22374
View details for DOI 10.1021/jp110913n
View details for Web of Science ID 000285236800067
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The oxygen reduction reaction mechanism on Pt(111) from density functional theory calculations
ELECTROCHIMICA ACTA
2010; 55 (27): 7975-7981
View details for DOI 10.1016/j.electacta.2010.02.056
View details for Web of Science ID 000284434700028
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Modeling the Electrochemical Hydrogen Oxidation and Evolution Reactions on the Basis of Density Functional Theory Calculations
JOURNAL OF PHYSICAL CHEMISTRY C
2010; 114 (42): 18182-18197
View details for DOI 10.1021/jp1048887
View details for Web of Science ID 000283110700025
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CO oxidation on PdO surfaces
JOURNAL OF CHEMICAL PHYSICS
2010; 133 (8)
Abstract
Density functional calculations were performed in order to investigate CO oxidation on two of the most stable bulk PdO surfaces. The most stable PdO(100) surface, with oxygen excess, is inert against CO adsorption, whereas strong adsorption on the stoichiometric PdO(101) surface leads to favorable oxidation via the Langmuir-Hinshelwood mechanism. The reaction with a surface oxygen atom has an activation energy of 0.66 eV, which is comparable to the lowest activation energies observed on metallic surfaces. However, the reaction rate may be limited by the coverage of molecular oxygen. Actually, the reaction with the site blocking molecular oxygen is slightly more favorable, enabling also possible formation of carbonate surface species at low temperatures. The extreme activity of strongly bonded surface oxygen atoms is more greatly emphasized on the PdO(100)-O surface. The direct reaction without adsorption, following the Eley-Rideal mechanism and taking advantage of the reaction tunnel provided by the adjacent palladium atom, has an activation energy of only 0.24 eV. The reaction mechanism and activation energy for the palladium activated CO oxidation on the most stable PdO(100)-O surface are in good agreement with experimental observations.
View details for DOI 10.1063/1.3464481
View details for Web of Science ID 000281743800038
View details for PubMedID 20815587
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On the Role of Metal Step-Edges in Graphene Growth
JOURNAL OF PHYSICAL CHEMISTRY C
2010; 114 (25): 11221-11227
View details for DOI 10.1021/jp1033596
View details for Web of Science ID 000278982300031
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Understanding Trends in Catalytic Activity: The Effect of Adsorbate-Adsorbate Interactions for CO Oxidation Over Transition Metals
TOPICS IN CATALYSIS
2010; 53 (5-6): 298-310
View details for DOI 10.1007/s11244-010-9455-2
View details for Web of Science ID 000276979100002
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Self Blocking of CO Dissociation on a Stepped Ruthenium Surface
TOPICS IN CATALYSIS
2010; 53 (5-6): 357-364
View details for DOI 10.1007/s11244-010-9445-4
View details for Web of Science ID 000276979100007
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Enzymatic versus Inorganic Oxygen Reduction Catalysts: Comparison of the Energy Levels in a Free-Energy Scheme
INORGANIC CHEMISTRY
2010; 49 (8): 3567-3572
Abstract
In this paper, we present a method to directly compare the energy levels of intermediates in enzymatic and inorganic oxygen reduction catalysts. We initially describe how the energy levels of a Pt(111) catalyst, operating at pH = 0, are obtained. By a simple procedure, we then convert the energy levels of cytochrome c oxidase (CcO) models obtained at physiological pH = 7 to the energy levels at pH = 0, which allows for comparison. Furthermore, we illustrate how different bias voltages will affect the free-energy landscapes of the catalysts. This allows us to determine the so-called theoretical overpotential of each system, which is shown to be significantly lower for the enzymatic catalysts compared to the inorganic Pt(111) catalyst. Finally, we construct theoretical polarization curves for the CcO models, in order to illustrate the effect of the low overpotentials on turnover rates per site.
View details for DOI 10.1021/ic900798q
View details for Web of Science ID 000276556900003
View details for PubMedID 20380458
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Ammonia dynamics in magnesium ammine from DFT and neutron scattering
ENERGY & ENVIRONMENTAL SCIENCE
2010; 3 (4): 448-456
View details for DOI 10.1039/b921442a
View details for Web of Science ID 000276378000009
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Step Effects on the Dissociation of NO on Close-Packed Rhodium Surfaces
JOURNAL OF PHYSICAL CHEMISTRY C
2009; 113 (48): 20623-20631
View details for DOI 10.1021/jp904108c
View details for Web of Science ID 000272038600017
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Alloys of platinum and early transition metals as oxygen reduction electrocatalysts
NATURE CHEMISTRY
2009; 1 (7): 552-556
Abstract
The widespread use of low-temperature polymer electrolyte membrane fuel cells for mobile applications will require significant reductions in the amount of expensive Pt contained within their cathodes, which drive the oxygen reduction reaction (ORR). Although progress has been made in this respect, further reductions through the development of more active and stable electrocatalysts are still necessary. Here we describe a new set of ORR electrocatalysts consisting of Pd or Pt alloyed with early transition metals such as Sc or Y. They were identified using density functional theory calculations as being the most stable Pt- and Pd-based binary alloys with ORR activity likely to be better than Pt. Electrochemical measurements show that the activity of polycrystalline Pt(3)Sc and Pt(3)Y electrodes is enhanced relative to pure Pt by a factor of 1.5-1.8 and 6-10, respectively, in the range 0.9-0.87 V.
View details for DOI 10.1038/NCHEM.367
View details for Web of Science ID 000270077200014
View details for PubMedID 21378936
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Magnetic edge states in MoS2 characterized using density-functional theory
PHYSICAL REVIEW B
2009; 80 (12)
View details for DOI 10.1103/PhysRevB.80.125416
View details for Web of Science ID 000270383300117
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Density functional for van der Waals forces accounts for hydrogen bond in benchmark set of water hexamers
JOURNAL OF CHEMICAL PHYSICS
2009; 131 (4)
Abstract
A recent extensive study has investigated how various exchange-correlation (XC) functionals treat hydrogen bonds in water hexamers and has shown traditional generalized gradient approximation and hybrid functionals used in density-functional (DF) theory to give the wrong dissociation-energy trend of low-lying isomers and van der Waals (vdW) dispersion forces to give key contributions to the dissociation energy. The question raised whether functionals that incorporate vdW forces implicitly into the XC functional predict the correct lowest-energy structure for the water hexamer and yield accurate total dissociation energy is here answered affirmatively for the vdW-DF [M. Dion et al., Phys. Rev. Lett.92, 246401 (2004)].
View details for DOI 10.1063/1.3193462
View details for Web of Science ID 000268613700100
View details for PubMedID 19655929
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Density functional theory based screening of ternary alkali-transition metal borohydrides: A computational material design project
JOURNAL OF CHEMICAL PHYSICS
2009; 131 (1)
Abstract
We present a computational screening study of ternary metal borohydrides for reversible hydrogen storage based on density functional theory. We investigate the stability and decomposition of alloys containing 1 alkali metal atom, Li, Na, or K (M(1)); and 1 alkali, alkaline earth or 3d/4d transition metal atom (M(2)) plus two to five (BH(4))(-) groups, i.e., M(1)M(2)(BH(4))(2-5), using a number of model structures with trigonal, tetrahedral, octahedral, and free coordination of the metal borohydride complexes. Of the over 700 investigated structures, about 20 were predicted to form potentially stable alloys with promising decomposition energies. The M(1)(Al/Mn/Fe)(BH(4))(4), (Li/Na)Zn(BH(4))(3), and (Na/K)(Ni/Co)(BH(4))(3) alloys are found to be the most promising, followed by selected M(1)(Nb/Rh)(BH(4))(4) alloys.
View details for DOI 10.1063/1.3148892
View details for Web of Science ID 000267799100002
View details for PubMedID 19586090
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Ammonia synthesis and decomposition on a Ru-based catalyst modeled by first-principles
SURFACE SCIENCE
2009; 603 (10-12): 1731-1739
View details for DOI 10.1016/j.susc.2008.10.059
View details for Web of Science ID 000266786500053
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Modeling Ethanol Decomposition on Transition Metals: A Combined Application of Scaling and Bronsted-Evans-Polanyi Relations
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2009; 131 (16): 5809-5815
Abstract
Applying density functional theory (DFT) calculations to the rational design of catalysts for complex reaction networks has been an ongoing challenge, primarily because of the high computational cost of these calculations. Certain correlations can be used to reduce the number and complexity of DFT calculations necessary to describe trends in activity and selectivity across metal and alloy surfaces, thus extending the reach of DFT to more complex systems. In this work, the well-known family of Brønsted-Evans-Polanyi (BEP) correlations, connecting minima with maxima in the potential energy surface of elementary steps, in tandem with a scaling relation, connecting binding energies of complex adsorbates with those of simpler ones (e.g., C, O), is used to develop a potential-energy surface for ethanol decomposition on 10 transition metal surfaces. Using a simple kinetic model, the selectivity and activity on a subset of these surfaces are calculated. Experiments on supported catalysts verify that this simple model is reasonably accurate in describing reactivity trends across metals, suggesting that the combination of BEP and scaling relations may substantially reduce the cost of DFT calculations required for identifying reactivity descriptors of more complex reactions.
View details for DOI 10.1021/ja8099322
View details for Web of Science ID 000265460200029
View details for PubMedID 19334787
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Experimental and computational studies on structural transitions in the LiBH4-LiI pseudobinary system
APPLIED PHYSICS LETTERS
2009; 94 (14)
View details for DOI 10.1063/1.3117227
View details for Web of Science ID 000265083700025
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Combinatorial Density Functional Theory-Based Screening of Surface Alloys for the Oxygen Reduction Reaction
JOURNAL OF PHYSICAL CHEMISTRY C
2009; 113 (12): 4932-4939
View details for DOI 10.1021/jp808945y
View details for Web of Science ID 000264349100032
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Density functional study of the adsorption and van der Waals binding of aromatic and conjugated compounds on the basal plane of MoS2
JOURNAL OF CHEMICAL PHYSICS
2009; 130 (10)
Abstract
Accurate calculations of adsorption energies of cyclic molecules are of key importance in investigations of, e.g., hydrodesulfurization (HDS) catalysis. The present density functional theory (DFT) study of a set of important reactants, products, and inhibitors in HDS catalysis demonstrates that van der Waals interactions are essential for binding energies on MoS(2) surfaces and that DFT with a recently developed exchange-correlation functional (vdW-DF) accurately calculates the van der Waals energy. Values are calculated for the adsorption energies of butadiene, thiophene, benzothiophene, pyridine, quinoline, benzene, and naphthalene on the basal plane of MoS(2), showing good agreement with available experimental data, and the equilibrium geometry is found as flat at a separation of about 3.5 A for all studied molecules. This adsorption is found to be due to mainly van der Waals interactions. Furthermore, the manifold of adsorption-energy values allows trend analyses to be made, and they are found to have a linear correlation with the number of main atoms.
View details for DOI 10.1063/1.3086040
View details for Web of Science ID 000264281800035
View details for PubMedID 19292551
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First-principles investigations of the Ni3Sn alloy at steam reforming conditions
SURFACE SCIENCE
2009; 603 (5): 762-770
View details for DOI 10.1016/j.susc.2009.01.018
View details for Web of Science ID 000264507600005
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Formation energies of rutile metal dioxides using density functional theory
PHYSICAL REVIEW B
2009; 79 (4)
View details for DOI 10.1103/PhysRevB.79.045120
View details for Web of Science ID 000262978400036
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Modeling the electrified solid-liquid interface
CHEMICAL PHYSICS LETTERS
2008; 466 (1-3): 68-71
View details for DOI 10.1016/j.cplett.2008.10.024
View details for Web of Science ID 000260906100014
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Electrochemistry on the computer: Understanding how to tailor the metal overlayers for the oxygen reduction reaction (A perspective on the article, "Improved oxygen reduction reactivity of platinum monolayers on transition metal surfaces", by AU Nilekar and M. Mavrikakis)
SURFACE SCIENCE
2008; 602 (14): 2337-2338
View details for DOI 10.1016/j.susc.2008.05.015
View details for Web of Science ID 000259062200008
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Oxidation and photo-oxidation of water on TiO2 surface
JOURNAL OF PHYSICAL CHEMISTRY C
2008; 112 (26): 9872-9879
View details for DOI 10.1021/jp711929d
View details for Web of Science ID 000257155200049
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Ammonia for hydrogen storage: challenges and opportunities
JOURNAL OF MATERIALS CHEMISTRY
2008; 18 (20): 2304-2310
View details for DOI 10.1039/b720020j
View details for Web of Science ID 000256353600003
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A molecular view of heterogeneous catalysis
JOURNAL OF CHEMICAL PHYSICS
2008; 128 (18)
Abstract
The establishment of a molecular view of heterogeneous catalysis has been hampered for a number of reasons. There are, however, recent developments, which show that we are now on the way towards reaching a molecular-scale picture of the way solids work as catalysts. By a combination of new theoretical methods, detailed experiments on model systems, and synthesis and in situ characterization of nano-structured catalysts, we are witnessing the first examples of complete atomic-scale insight into the structure and mechanism of surface-catalyzed reactions. This insight has already proven its value by enabling a rational design of new catalysts. We illustrate this important development in heterogeneous catalysis by highlighting recent examples of catalyst systems for which it has been possible to achieve such a detailed understanding. In particular, we emphasize examples where this progress has made it possible to propose entirely new catalysts, which have then been proven experimentally to exhibit improved performance in terms of catalytic activity or selectivity.
View details for DOI 10.1063/1.2839299
View details for Web of Science ID 000255983500003
View details for PubMedID 18532788
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Structure sensitivity of the methanation reaction: H-2-induced CO dissociation on nickel surfaces
JOURNAL OF CATALYSIS
2008; 255 (1): 6-19
View details for DOI 10.1016/j.jcat.2007.12.016
View details for Web of Science ID 000254966500002
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Using scaling relations to understand trends in the catalytic activity of transition metals
JOURNAL OF PHYSICS-CONDENSED MATTER
2008; 20 (6)
Abstract
A method is developed to estimate the potential energy diagram for a full catalytic reaction for a range of late transition metals on the basis of a calculation (or an experimental determination) for a single metal. The method, which employs scaling relations between adsorption energies, is illustrated by calculating the potential energy diagram for the methanation reaction and ammonia synthesis for 11 different metals on the basis of results calculated for Ru. It is also shown that considering the free energy diagram for the reactions, under typical industrial conditions, provides additional insight into reactivity trends.
View details for DOI 10.1088/0953-8984/20/6/064239
View details for Web of Science ID 000252927300040
View details for PubMedID 21693900
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Recent density functional studies of hydrodesulfurization catalysts: insight into structure and mechanism
JOURNAL OF PHYSICS-CONDENSED MATTER
2008; 20 (6)
Abstract
The present article will highlight some recent density functional theory (DFT) studies of hydrodesulfurization (HDS) catalysts. It will be summarized how DFT in combination with experimental studies can give a detailed picture of the structure of the active phase. Furthermore, we have used DFT to investigate the reaction pathway for thiophene HDS, and we find that the reaction entails a complex interplay of different active sites, depending on reaction conditions. An investigation of pyridine inhibition confirmed some of these results. These fundamental insights constitute a basis for rational improvement of HDS catalysts, as they have provided important structure-activity relationships.
View details for DOI 10.1088/0953-8984/20/6/064236
View details for Web of Science ID 000252927300037
View details for PubMedID 21693897
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Recent STM, DFT and HAADF-STEM studies of sulfide-based hydrotreating catalysts: Insight into mechanistic, structural and particle size effects
CATALYSIS TODAY
2008; 130 (1): 86-96
View details for DOI 10.1016/j.cattod.2007.08.009
View details for Web of Science ID 000251685000013
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BEP relations for N-2 dissociation over stepped transition metal and alloy surfaces
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2008; 10 (34): 5202-5206
Abstract
We present density functional theory (DFT) calculations for N2 dissociation on stepped face-centred cubic (211) surface slabs. By using the same crystal structure, the same adsorption site for atomic nitrogen, and the same transition-state bond length of N2 over a range of pure metal surfaces, a perfectly linear Brønsted-Evans-Polanyi (BEP) relation between the transition-state potential energy and the dissociative chemisorption energy is obtained. The perfect BEP relation, which extends over 12 eV in chemisorption energy, suggests that the manifestation of BEP relations for surface reactions is a general electronic structure effect, and that geometric effects are responsible for the scatter which is normally observed around the BEP line. The BEP relation is also shown to be valid for both surface and bulk alloys. The scatter is, however, larger than for the pure elements. This can be understood as a larger geometrical variance. To analyze the accuracy of the DFT calculations a detailed convergence study is performed for several adsorbates on stepped hexagonal close-packed and face-centred cubic Ru slabs.
View details for DOI 10.1039/b720021h
View details for Web of Science ID 000258738200006
View details for PubMedID 18728861
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Steady state oxygen reduction and cyclic voltammetry
FARADAY DISCUSSIONS
2008; 140: 337-346
Abstract
The catalytic activity of Pt and Pt3Ni for the oxygen reduction reaction is investigated by applying a Sabatier model based on density functional calculations. We investigate the role of adsorbed OH on the activity, by comparing cyclic voltammetry obtained from theory with previously published experimental results with and without molecular oxygen present. We find that the simple Sabatier model predicts both the potential dependence of the OH coverage and the measured current densities seen in experiments, and that it offers an understanding of the oxygen reduction reaction (ORR) at the atomic level. To investigate kinetic effects we develop a simple kinetic model for ORR. Whereas kinetic corrections only matter close to the volcano top, an interesting outcome of the kinetic model is a first order dependence on the oxygen pressure. Importantly, the conclusion obtained from the simple Sabatier model still persists: an intermediate binding of OH corresponds to the highest catalytic activity, i.e. Pt is limited by a too strong OH binding and Pt3Ni is limited by a too weak OH binding.
View details for DOI 10.1039/b802129e
View details for Web of Science ID 000260437800023
View details for PubMedID 19213325
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Surface Pourbaix diagrams and oxygen reduction activity of Pt, Ag and Ni(111) surfaces studied by DFT
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2008; 10 (25): 3722-3730
Abstract
Based on density functional theory calculations we investigate the electrochemically most stable surface structures as a function of pH and electrostatic potential for Pt(111), Ag(111) and Ni(111), and we construct surface Pourbaix diagrams. We study the oxygen reduction reaction (ORR) on the different surface structures and calculate the free energy of the intermediates. We estimate their catalytic activity for ORR by determining the highest potential at which all ORR reaction steps reduce the free energy. We obtain self-consistency in the sense that the surface is stable under the potential at which that particular surface can perform ORR. Using the self consistent surfaces, the activity of the very reactive Ni surface changes dramatically, whereas the activity of the more noble catalysts Pt and Ag remains unchanged. The reason for this difference is the oxidation of the reactive surface. Oxygen absorbed on the surface shifts the reactivity towards the weak binding region, which in turn increases the activity. The oxidation state of the surface and the ORR potential are constant versus the reversible hydrogen electrode (RHE). The dissolution potential in acidic solution, on the other hand, is constant vs. the standard hydrogen electrode (SHE). For Ag, this means that where the potential for dissolution and ORR are about the same at pH = 0, Ag becomes more stable relative to RHE as pH is increased. Hence the pH dependent stability offers an explanation for the possible use of Ag in alkaline fuel cell cathodes.
View details for DOI 10.1039/b803956a
View details for Web of Science ID 000256877200014
View details for PubMedID 18563233
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Trends in the catalytic CO oxidation activity of nanoparticles
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2008; 47 (26): 4835-4839
View details for DOI 10.1002/anie.200801479
View details for Web of Science ID 000257040800006
View details for PubMedID 18496809
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On the Role of Surface Modifications of Palladium Catalysts in the Selective Hydrogenation of Acetylene
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2008; 47 (48): 9299-9302
View details for DOI 10.1002/anie.200802844
View details for Web of Science ID 000261445900023
View details for PubMedID 18833559
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Direct NO decomposition over stepped transition-metal surfaces
PURE AND APPLIED CHEMISTRY
2007; 79 (11): 1895-1903
View details for DOI 10.1351/pac200779111895
View details for Web of Science ID 000250863000010
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Size-specific chemistry on bimetallic surfaces: A combined experimental and theoretical study
CHEMPHYSCHEM
2007; 8 (14): 2068-2071
View details for DOI 10.1002/cphc.200700070
View details for Web of Science ID 000250253500004
View details for PubMedID 17806131
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Cyclic voltammograms for H on Pt(111) and Pt(100) from first principles
PHYSICAL REVIEW LETTERS
2007; 99 (12)
Abstract
Cyclic voltammetry is a fundamental experimental method for characterizing electrochemical surfaces. Despite its wide use, a way to quantitatively and directly relate cyclic voltammetry to ab initio calculations has been lacking. We derive the cyclic voltammogram for H on Pt(111) and Pt(100), based solely on density functional theory calculations and standard molecular tables. By relating the gas phase adsorption energy to the electrochemical electrode potential, we provide a direct link between surface science and electrochemistry.
View details for DOI 10.1103/PhysRevLett.99.126101
View details for Web of Science ID 000249668000046
View details for PubMedID 17930522
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Electrolysis of water on oxide surfaces
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
2007; 607 (1-2): 83-89
View details for DOI 10.1016/j.jelechem.2006.11.008
View details for Web of Science ID 000249177100011
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Discovery of technical methanation catalysts based on computational screening
TOPICS IN CATALYSIS
2007; 45 (1-4): 9-13
View details for DOI 10.1007/s11244-007-0232-9
View details for Web of Science ID 000248819800003
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Catalytic activity of Au nanoparticles
NANO TODAY
2007; 2 (4): 14-18
View details for Web of Science ID 000248904900011
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Trends in catalytic NO decomposition over transition metal surfaces
TOPICS IN CATALYSIS
2007; 45 (1-4): 117-120
View details for DOI 10.1007/s11244-007-0250-7
View details for Web of Science ID 000248819800021
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Location and coordination of promoter atoms in Co- and Ni-promoted MoS2-based hydrotreating catalysts
JOURNAL OF CATALYSIS
2007; 249 (2): 220-233
View details for DOI 10.1016/j.jcat.2007.04.013
View details for Web of Science ID 000248397400010
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The hydrogenation and direct desulfurization reaction pathway in thiophene hydrodesulfurization over MoS2 catalysts at realistic conditions: A density functional study
JOURNAL OF CATALYSIS
2007; 248 (2): 188-203
View details for DOI 10.1016/j.jcat.2007.02.028
View details for Web of Science ID 000247327300005
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Insights into the reactivity of supported Au nanoparticles: combining theory and experiments
TOPICS IN CATALYSIS
2007; 44 (1-2): 15-26
View details for DOI 10.1007/s11244-007-0335-3
View details for Web of Science ID 000247310000003
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Ligand effects in heterogeneous catalysis and electrochemistry
ELECTROCHIMICA ACTA
2007; 52 (18): 5512-5516
View details for DOI 10.1016/j.electacta.2007.02.041
View details for Web of Science ID 000246655300002
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CO methanation over supported bimetallic Ni-Fe catalysts: From computational studies towards catalyst optimization
APPLIED CATALYSIS A-GENERAL
2007; 320: 98-104
View details for DOI 10.1016/j.apcata.2006.12.017
View details for Web of Science ID 000245534900012
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Large-scale, density functional theory-based screening of alloys for hydrogen evolution
SURFACE SCIENCE
2007; 601 (6): 1590-1598
View details for DOI 10.1016/j.susc.2007.01.037
View details for Web of Science ID 000245616400022
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Estimations of electric field effects on the oxygen reduction reaction based on the density functional theory
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2007; 9 (37): 5158-5161
Abstract
By varying the external electric field in density functional theory (DFT) calculations we have estimated the impact of the local electric field in the electric double layer on the oxygen reduction reaction (ORR). Potentially, including the local electric field could change adsorption energies and barriers substantially, thereby affecting the reaction mechanism predicted for ORR on different metals. To estimate the effect of local electric fields on ORR we combine the DFT results at various external electric field strengths with a previously developed model of electrochemical reactions which fully accounts for the effect of the electrode potential. We find that the local electric field only slightly affects the output of the model. Hence, the general picture obtained without inclusion of the electric field still persists. However, for accurate predictions at oxygen reduction potentials close to the volcano top local electric field effects may be of importance.
View details for DOI 10.1039/b705938h
View details for Web of Science ID 000249564300012
View details for PubMedID 17878993
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Density functional theory calculations for the hydrogen evolution reaction in an electrochemical double layer on the Pt(111) electrode
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2007; 9 (25): 3241-3250
Abstract
We present results of density functional theory calculations on a Pt(111) slab with a bilayer of water, solvated protons in the water layer, and excess electrons in the metal surface. In this way we model the electrochemical double layer at a platinum electrode. By varying the number of protons/electrons in the double layer we investigate the system as a function of the electrode potential. We study the elementary processes involved in the hydrogen evolution reaction, 2(H(+) + e(-)) --> H(2), and determine the activation energy and predominant reaction mechanism as a function of electrode potential. We confirm by explicit calculations the notion that the variation of the activation barrier with potential can be viewed as a manifestation of the Brønsted-Evans-Polanyi-type relationship between activation energy and reaction energy found throughout surface chemistry.
View details for DOI 10.1039/b700099e
View details for Web of Science ID 000247367200005
View details for PubMedID 17579732
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Theoretical trends in particle size effects for the oxygen reduction reaction
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS
2007; 221 (9-10): 1209-1220
View details for DOI 10.1524/zpch.2007.221.9-10.1209
View details for Web of Science ID 000250768300009
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Electronic-structure-based design of ordered alloys
MRS BULLETIN
2006; 31 (12): 986-990
View details for Web of Science ID 000243162700016
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Reactive and nonreactive scattering of N-2 from Ru(0001): A six-dimensional adiabatic study
JOURNAL OF CHEMICAL PHYSICS
2006; 125 (11)
Abstract
We have studied the dissociative chemisorption and scattering of N(2) on and from Ru(0001), using a six-dimensional quasiclassical trajectory method. The potential energy surface, which depends on all the molecular degrees of freedom, has been built applying a modified Shepard interpolation method to a data set of results from density functional theory, employing the RPBE generalized gradient approximation. The frozen surface and Born-Oppenheimer [Ann. Phys. (Leipzig) 84, 457 (1927)] approximations were used, neglecting phonons and electron-hole pair excitations. Dissociative chemisorption probabilities are found to be very small even for translational energies much higher than the minimum reaction barrier, in good agreement with experiment. A comparison to previous low dimensional calculations shows the importance of taking into account the multidimensional effects of N(2) rotation and translation parallel to the surface. The new calculations strongly suggest a much smaller role of nonadiabatic effects than previously assumed on the basis of a comparison between low dimensional results and experiments [J. Chem. Phys. 115, 9028 (2001)]. Also in agreement with experiment, our theoretical results show a strong dependence of reaction on the initial vibrational state. Computed angular scattering distributions and parallel translation energy distributions are in good agreement with experiments on scattering, but the theory overestimates vibrational and rotational excitations in scattering.
View details for DOI 10.1063/1.2229197
View details for Web of Science ID 000240658700045
View details for PubMedID 16999500
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Insights into ammonia synthesis from first-principles
SURFACE SCIENCE
2006; 600 (18): 4264-4268
View details for DOI 10.1016/j.susc.2005.11.070
View details for Web of Science ID 000241450600150
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Predicting catalysis: Understanding ammonia synthesis from first-principles calculations
JOURNAL OF PHYSICAL CHEMISTRY B
2006; 110 (36): 17719-17735
Abstract
Here, we give a full account of a large collaborative effort toward an atomic-scale understanding of modern industrial ammonia production over ruthenium catalysts. We show that overall rates of ammonia production can be determined by applying various levels of theory (including transition state theory with or without tunneling corrections, and quantum dynamics) to a range of relevant elementary reaction steps, such as N(2) dissociation, H(2) dissociation, and hydrogenation of the intermediate reactants. A complete kinetic model based on the most relevant elementary steps can be established for any given point along an industrial reactor, and the kinetic results can be integrated over the catalyst bed to determine the industrial reactor yield. We find that, given the present uncertainties, the rate of ammonia production is well-determined directly from our atomic-scale calculations. Furthermore, our studies provide new insight into several related fields, for instance, gas-phase and electrochemical ammonia synthesis. The success of predicting the outcome of a catalytic reaction from first-principles calculations supports our point of view that, in the future, theory will be a fully integrated tool in the search for the next generation of catalysts.
View details for DOI 10.1021/jp056982h
View details for Web of Science ID 000240340600006
View details for PubMedID 16956255
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Density functional theory in surface science and heterogeneous catalysis
MRS BULLETIN
2006; 31 (9): 669-674
View details for Web of Science ID 000240745500014
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Hydrogen evolution over bimetallic systems: Understanding the trends
CHEMPHYSCHEM
2006; 7 (5): 1032-1035
View details for DOI 10.1002/cphc.200500663
View details for Web of Science ID 000237836700009
View details for PubMedID 16557633
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A high-density ammonia storage/delivery system based on Mg(NH3)(6)Cl-2 for SCR-DeNO(x) in vehicles
CHEMICAL ENGINEERING SCIENCE
2006; 61 (8): 2618-2625
View details for DOI 10.1016/j.ces.2005.11.038
View details for Web of Science ID 000236191700031
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Multidimensional effects on dissociation of N-2 on Ru(0001)
PHYSICAL REVIEW LETTERS
2006; 96 (9)
Abstract
The applicability of the Born-Oppenheimer approximation to molecule-metal surface reactions is presently a topic of intense debate. We have performed classical trajectory calculations on a prototype activated dissociation reaction, of N2 on Ru(0001), using a potential energy surface based on density functional theory. The computed reaction probabilities are in good agreement with molecular beam experiments. Comparison to previous calculations shows that the rotation of N2 and its motion along the surface affect the reactivity of N2 much more than nonadiabatic effects.
View details for DOI 10.1103/PhysRevLett.96.096102
View details for Web of Science ID 000235905700038
View details for PubMedID 16606281
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Mechanisms for catalytic carbon nanofiber growth studied by ab initio density functional theory calculations
PHYSICAL REVIEW B
2006; 73 (11)
View details for DOI 10.1103/PhysRevB.73.115419
View details for Web of Science ID 000236467300139
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Predictable reactions
TCE
2006: 44-45
View details for Web of Science ID 000236231900052
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Catalysis by enzymes: The biological ammonia synthesis
TOPICS IN CATALYSIS
2006; 37 (1): 55-70
View details for DOI 10.1007/s11244-006-0002-0
View details for Web of Science ID 000236983700006
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Special Issue - Frontiers in catalysis: A molecular view of industrial catalysis
CATALYSIS TODAY
2006; 111 (1-2): 1-1
View details for DOI 10.1016/j.cattod.2005.10.004
View details for Web of Science ID 000234634100001
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A density functional study of inhibition of the HDS hydrogenation pathway by pyridine, benzene, and H2S on MoS2-based catalysts
CATALYSIS TODAY
2006; 111 (1-2): 44-51
View details for DOI 10.1016/j.cattod.2005.10.018
View details for Web of Science ID 000234634100008
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Towards an ammonia-mediated hydrogen economy?
CATALYSIS TODAY
2006; 111 (1-2): 140-144
View details for DOI 10.1016/j.cattod.2005.10.011
View details for Web of Science ID 000234634100019
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Generation of nanopores during desorption of NH3 from Mg(NH3)(6)Cl-2
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2006; 128 (1): 16-17
Abstract
It is shown that nanopores are formed during desorption of NH3 from Mg(NH3)6Cl2, which has been proposed as a hydrogen storage material. The system of nanopores facilitates the transport of desorbed ammonia away from the interior of large volumes of compacted storage material. DFT calculations show that there exists a continuous path from the initial Mg(NH3)6Cl2 material to MgCl2 that does not involve large-scale material transport. Accordingly, ammonia desorption from this system is facile.
View details for DOI 10.1021/ja0556070
View details for Web of Science ID 000234547700008
View details for PubMedID 16390099
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Response to "comment on 'Trends in the exchange current for hydrogen evolution' [J. Electrochem. Soc., 152, J23 (2005)]"
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
2006; 153 (12): L33-L33
View details for DOI 10.1149/1.2358292
View details for Web of Science ID 000241757400083
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Ethylene dissociation on flat and stepped Ni(111): A combined STM and DFT study
SURFACE SCIENCE
2006; 600 (1): 66-77
View details for DOI 10.1016/j.susc.2005.10.006
View details for Web of Science ID 000234948000010
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Electrolysis of water on (oxidized) metal surfaces
CHEMICAL PHYSICS
2005; 319 (1-3): 178-184
View details for DOI 10.1016/j.chemphys.2005.05.038
View details for Web of Science ID 000233955500017
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The ligand effect: CO desorption from Pt/Ru catalysts
FUEL CELLS
2005; 5 (4): 429-435
View details for DOI 10.1002/fuce.200400076
View details for Web of Science ID 000234363900002
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Bayesian error estimation in density-functional theory
PHYSICAL REVIEW LETTERS
2005; 95 (21)
Abstract
We present a practical scheme for performing error estimates for density-functional theory calculations. The approach, which is based on ideas from Bayesian statistics, involves creating an ensemble of exchange-correlation functionals by comparing with an experimental database of binding energies for molecules and solids. Fluctuations within the ensemble can then be used to estimate errors relative to experiment on calculated quantities such as binding energies, bond lengths, and vibrational frequencies. It is demonstrated that the error bars on energy differences may vary by orders of magnitude for different systems in good agreement with existing experience.
View details for DOI 10.1103/PhysRevLett.95.216401
View details for Web of Science ID 000233362100045
View details for PubMedID 16384163
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A general scheme for the estimation of oxygen binding energies on binary transition metal surface alloys
SURFACE SCIENCE
2005; 592 (1-3): 104-111
View details for DOI 10.1016/j.susc.2005.07.018
View details for Web of Science ID 000232461700013
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The role of reaction pathways and support interactions in the development of high activity hydrotreating catalysts
CATALYSIS TODAY
2005; 107-08: 12-22
View details for DOI 10.1016/j.cattod.2005.07.165
View details for Web of Science ID 000233293600003
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Methane activation on Ni(111): Effects of poisons and step defects
SURFACE SCIENCE
2005; 590 (2-3): 127-137
View details for DOI 10.1016/j.susc.2005.05.057
View details for Web of Science ID 000231657300004
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CO oxidation on gold nanoparticles: Theoretical studies
APPLIED CATALYSIS A-GENERAL
2005; 291 (1-2): 13-20
View details for DOI 10.1016/j.apcata.2005.01.052
View details for Web of Science ID 000231651300004
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Trends in the chemical properties of early transition metal carbide surfaces: A density functional study
CATALYSIS TODAY
2005; 105 (1): 66-73
View details for DOI 10.1016/j.cattod.2005.04.008
View details for Web of Science ID 000230576000006
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The reaction rate for dissociative adsorption of N-2 on stepped Ru(0001): Six-dimensional quantum calculations
JOURNAL OF CHEMICAL PHYSICS
2005; 122 (23)
Abstract
Quantum-mechanical calculations of the reaction rate for dissociative adsorption of N2 on stepped Ru(0001) are presented. Converged six-dimensional quantum calculations for this heavy-atom reaction have been performed using the multiconfiguration time-dependent Hartree method. A potential-energy surface for the transition-state region is constructed from density-functional theory calculations using Shepard interpolation. The quantum results are in very good agreement with the results of the harmonic transition-state theory. In contrast to the findings of previous model calculations on similar systems, the tunneling effect is found to be small.
View details for DOI 10.1063/1.1927513
View details for Web of Science ID 000230091400045
View details for PubMedID 16008468
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Why the optimal ammonia synthesis catalyst is not the optimal ammonia decomposition catalyst
JOURNAL OF CATALYSIS
2005; 230 (2): 309-312
View details for DOI 10.1016/j.jcat.2004.12.013
View details for Web of Science ID 000227565800006
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Trends in hydride formation energies for magnesium-3d transition metal alloys
JOURNAL OF ALLOYS AND COMPOUNDS
2005; 386 (1-2): 1-7
View details for DOI 10.1016/j.jallcom.2004.03.143
View details for Web of Science ID 000226186300002
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Metal ammine complexes for hydrogen storage
JOURNAL OF MATERIALS CHEMISTRY
2005; 15 (38): 4106-4108
View details for DOI 10.1039/b511589b
View details for Web of Science ID 000232206300002
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CO oxidation on rutile-supported Au nanoparticles
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
2005; 44 (12): 1824-1826
View details for DOI 10.1002/anie.200461699
View details for Web of Science ID 000227765600010
View details for PubMedID 15712248
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CO Desorption Rate Dependence on CO Partial Pressure over Platinum Fuel Cell Catalysts
FUEL CELLS
2004; 4 (4): 309-319
View details for DOI 10.1002/fuce.200400046
View details for Web of Science ID 000208115800010
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Role of strain and ligand effects in the modification of the electronic and chemical properties of bimetallic surfaces
PHYSICAL REVIEW LETTERS
2004; 93 (15)
Abstract
Periodic density functional calculations are used to illustrate how the combination of strain and ligand effects modify the electronic and surface chemical properties of Ni, Pd, and Pt monolayers supported on other transition metals. Strain and the ligand effects are shown to change the width of the surface d band, which subsequently moves up or down in energy to maintain a constant band filling. Chemical properties such as the dissociative adsorption energy of hydrogen are controlled by changes induced in the average energy of the d band by modification of the d-band width.
View details for DOI 10.1103/PhysRevLett.93.156801
View details for Web of Science ID 000224341600067
View details for PubMedID 15524919
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DFT study of formaldehyde and methanol synthesis from CO and H-2 on Ni(111)
JOURNAL OF PHYSICAL CHEMISTRY B
2004; 108 (38): 14535-14540
View details for DOI 10.1021/jp0493374
View details for Web of Science ID 000223922500044
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Spectroscopic link between adsorption site occupation and local surface chemical reactivity
PHYSICAL REVIEW LETTERS
2004; 93 (4)
Abstract
In this Letter we show that sequences of adsorbate-induced shifts of surface core level (SCL) x-ray photoelectron spectra contain profound information on surface changes of electronic structure and reactivity. Energy shifts and intensity changes of time-lapsed spectral components follow simple rules, from which adsorption sites are directly determined. Theoretical calculations rationalize the results for transition metal surfaces in terms of the energy shift of the d-band center of mass and this proves that adsorbate-induced SCL shifts provide a spectroscopic measure of local surface reactivity.
View details for DOI 10.1103/PhysRevLett.93.046101
View details for Web of Science ID 000222856400040
View details for PubMedID 15323775
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The adhesion and shape of nanosized Au particles in a Au/TiO2 catalyst
JOURNAL OF CATALYSIS
2004; 225 (1): 86-94
View details for DOI 10.1016/j.jcat.2004.03.036
View details for Web of Science ID 000221966300010
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Nano-scale effects in electrochemistry
CHEMICAL PHYSICS LETTERS
2004; 390 (4-6): 440-444
View details for DOI 10.1016/j.cplett.2004.03.149
View details for Web of Science ID 000221730600024
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Modification of the surface electronic and chemical properties of Pt(111) by subsurface 3d transition metals
JOURNAL OF CHEMICAL PHYSICS
2004; 120 (21): 10240-10246
Abstract
The modification of the electronic and chemical properties of Pt(111) surfaces by subsurface 3d transition metals was studied using density-functional theory. In each case investigated, the Pt surface d-band was broadened and lowered in energy by interactions with the subsurface 3d metals, resulting in weaker dissociative adsorption energies of hydrogen and oxygen on these surfaces. The magnitude of the decrease in adsorption energy was largest for the early 3d transition metals and smallest for the late 3d transition metals. In some cases, dissociative adsorption was calculated to be endothermic. The surfaces investigated in this study had no lateral strain in them, demonstrating that strain is not a necessary factor in the modification of bimetallic surface properties. The implications of these findings are discussed in the context of catalyst design, particularly for fuel cell electrocatalysts.
View details for DOI 10.1063/1.1737365
View details for Web of Science ID 000221404500043
View details for PubMedID 15268048
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Hydrodesulfurization reaction pathways on MoS2 nanoclusters revealed by scanning tunneling microscopy
JOURNAL OF CATALYSIS
2004; 224 (1): 94-106
View details for DOI 10.1016/j.jcat.2004.02.009
View details for Web of Science ID 000221200700011
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A negative surface energy for alumina
NATURE MATERIALS
2004; 3 (5): 289-293
Abstract
The surface energy of a solid measures the energy cost of increasing the surface area. All normal solids therefore have a positive surface energy-if it had been negative, the solid would disintegrate. For this reason it is also generally believed that when certain ceramics can be found in a highly porous form, this is a metastable state, which will eventually sinter into the bulk solid at high temperatures. We present theoretical evidence suggesting that for theta-alumina, the surface energy is strongly dependent on the size of the crystallites, and that for some facets it is negative for thicknesses larger than approximately 1 nm. This suggests a completely new picture of porous alumina in which the high-surface-area, nanocrystalline form is the thermodynamic ground state. The negative surface energy is found to be related to a particularly strongly adsorbed state of dissociated water on some alumina surfaces. We also present new experimental evidence based on infrared spectroscopy, in conjunction with X-ray diffraction and surface-area measurements, that theta-alumina has indeed very stable surface OH groups at high temperatures, and that this form of alumina does not sinter even at temperatures up to 1,300 K.
View details for DOI 10.1038/nmat1106
View details for Web of Science ID 000221322000013
View details for PubMedID 15077105
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Sintering of nickel steam-reforming catalysts: effects of temperature and steam and hydrogen pressures
JOURNAL OF CATALYSIS
2004; 223 (2): 432-443
View details for DOI 10.1016/j.jcat.2004.01.026
View details for Web of Science ID 000220754300020
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Chemical activity of the nitrogenase FeMo cofactor with a central nitrogen ligand: Density functional study
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2004; 126 (12): 3920-3927
Abstract
We investigate the chemical consequences of a central ligand in the nitrogenase FeMo cofactor using density functional calculations. Several studies have shown that the central ligand most probably is a nitrogen atom, but the consequences for the chemical reactivity of the cofactor are unknown. We investigate several possible routes for insertion of the central nitrogen ligand and conclude that all routes involve barriers and intermediate states, which are inaccessible at ambient conditions. On this basis we suggest that the central nitrogen ligand is present at all times during the reaction. Furthermore, we investigate how the FeMoco with the central ligand can interact with N(2) and reduce it.
View details for DOI 10.1021/ja037792s
View details for Web of Science ID 000220440400053
View details for PubMedID 15038746
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Atomic-scale insight into structure and morphology changes of MoS2 nanoclusters in hydrotreating catalysts
JOURNAL OF CATALYSIS
2004; 221 (2): 510-522
View details for DOI 10.1016/j.jcat.2003.09.015
View details for Web of Science ID 000188798400026
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Structure of the FeFe-cofactor of the iron-only nitrogenase and possible mechanism for dinitrogen reduction
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2004; 6 (4): 843-853
View details for DOI 10.1039/b310850c
View details for Web of Science ID 000188894400025
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beta-sheet preferences from first principles
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2003; 125 (52): 16383-16386
Abstract
The natural amino acids have different preferences of occurring in specific types of secondary protein structure. Simulations are performed on periodic model beta-sheets of 14 different amino acids, at the level of density functional theory, employing the generalized gradient approximation. We find that the statistically observed beta-sheet propensities correlate very well with the calculated binding energies. Analysis of the calculations shows that the beta-sheet propensities are determined by the local flexibility of the individual polypeptide strands.
View details for DOI 10.1021/ja0359658
View details for Web of Science ID 000187574800046
View details for PubMedID 14692780
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Ammonia synthesis over a Ru(0001) surface studied by density functional calculations
JOURNAL OF CATALYSIS
2003; 220 (2): 273-279
View details for DOI 10.1016/S0021-9517(03)00156-8
View details for Web of Science ID 000186817800003
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Pareto-optimal alloys
APPLIED PHYSICS LETTERS
2003; 83 (22): 4527-4529
View details for DOI 10.1063/1.1631051
View details for Web of Science ID 000186787100020
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Modeling the electro-oxidation of CO and H-2/CO on Pt, Ru, PtRu and Pt3Sn
ELECTROCHIMICA ACTA
2003; 48 (25-26): 3731-3742
View details for DOI 10.1016/S0013-4686(03)00538-3
View details for Web of Science ID 000186221100003
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High throughput experimental and theoretical predictive screening of materials - A comparative study of search strategies for new fuel cell anode catalysts
JOURNAL OF PHYSICAL CHEMISTRY B
2003; 107 (40): 11013-11021
View details for DOI 10.1021/jp030508z
View details for Web of Science ID 000185756900009
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On the compensation effect in heterogeneous catalysis
JOURNAL OF PHYSICAL CHEMISTRY B
2003; 107 (35): 9325-9331
View details for DOI 10.1021/jp034447g
View details for Web of Science ID 000185034700026
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The stability of the hydroxylated (0001) surface of alpha-Al2O3
JOURNAL OF CHEMICAL PHYSICS
2003; 118 (24): 11179-11188
View details for DOI 10.1063/1.1574798
View details for Web of Science ID 000183402200039
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A simple and realistic model system for studying hydrogen bonds in beta-sheets
JOURNAL OF CHEMICAL PHYSICS
2003; 118 (21): 9783-9794
View details for DOI 10.1063/1.1570395
View details for Web of Science ID 000182890000038
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Atomic and electronic structure of MoS2 nanoparticles (vol B 67, art no 085410, 2003)
PHYSICAL REVIEW B
2003; 67 (12)
View details for DOI 10.1103/PhysRevB.67.129906
View details for Web of Science ID 000182158000113
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Chemistry of one-dimensional metallic edge states in MoS2 nanoclusters
NANOTECHNOLOGY
2003; 14 (3): 385-389
View details for Web of Science ID 000182066500009
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Modeling a central ligand in the nitrogenase FeMo cofactor
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2003; 125 (6): 1466-1467
Abstract
In very recent work by Einsle et al. (Science 2002, 297, 1696), a new X-ray crystallographic structure of the FeMo cofactor of nitrogenase with a central ligand was presented. The central ligand is a light atom (N, O, or C), and Einsle et al. suggest that it is nitrogen. We present density functional calculations on the FeMo cofactor, and we investigate N, O, and C as central ligands. We show that both N and O lead to energetically stable FeMo cofactor structures, whereas C is energetically unfavorable. By comparison of bond geometries with the crystallographically determined values, we show that the central ligand is most likely nitrogen.
View details for DOI 10.1021/ja029041g
View details for Web of Science ID 000180842200012
View details for PubMedID 12568592
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Bonding of gold nanoclusters to oxygen vacancies on rutile TiO2(110)
PHYSICAL REVIEW LETTERS
2003; 90 (2)
Abstract
Through an interplay between scanning tunneling microscopy (STM) and density functional theory (DFT) calculations, we show that bridging oxygen vacancies are the active nucleation sites for Au clusters on the rutile TiO2(110) surface. We find that a direct correlation exists between a decrease in density of vacancies and the amount of Au deposited. From the DFT calculations we find that the oxygen vacancy is indeed the strongest Au binding site. We show both experimentally and theoretically that a single oxygen vacancy can bind 3 Au atoms on average. In view of the presented results, a new growth model for the TiO2(110) system involving vacancy-cluster complex diffusion is presented.
View details for DOI 10.1103/PhysRevLett.90.026101
View details for Web of Science ID 000180444200028
View details for PubMedID 12570557
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Interaction of Pd with steps on alpha-Al2O3(0001)
SURFACE SCIENCE
2002; 518 (1-2): L577-L582
View details for Web of Science ID 000178643200002
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Atomic and molecular adsorption on Rh(111)
JOURNAL OF CHEMICAL PHYSICS
2002; 117 (14): 6737-6744
View details for DOI 10.1063/1.1507104
View details for Web of Science ID 000178256100044
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Catalytic CO oxidation by a gold nanoparticle: A density functional study
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2002; 124 (38): 11262-11263
Abstract
Gold is usually considered very noble. It does not oxidize, and the surface of gold cannot adsorb most molecules from the gas phase. Yet it has been found that nanometer size gold particles on different oxide supports can act as catalysts even at or below room temperature. We present self-consistent density functional calculations showing that even an isolated Au10 cluster should be able to catalyze the CO oxidation reaction even below room temperature. We use the calculations to analyze the origin of this effect and suggest that the extraordinary reactivity can be traced back to special reaction geometries available at small particles in combination with an enhanced ability of low coordinated gold atoms to interact with molecules from the surroundings.
View details for DOI 10.1021/ja026998a
View details for Web of Science ID 000178104600019
View details for PubMedID 12236728
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Theoretical study of the Au/TiO2(110) interface
SURFACE SCIENCE
2002; 515 (1): 175-186
View details for Web of Science ID 000177735900021
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Adsorption-induced restructuring of gold nanochains
PHYSICAL REVIEW B
2002; 66 (8)
View details for DOI 10.1103/PhysRevB.66.081405
View details for Web of Science ID 000177972500027
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Steam reforming and graphite formation on Ni catalysts
JOURNAL OF CATALYSIS
2002; 209 (2): 365-384
View details for DOI 10.1006/jcat.2002.3579
View details for Web of Science ID 000176916300009
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Monte Carlo simulations of adsorption-induced segregation
SURFACE SCIENCE
2002; 505 (1-3): 200-214
View details for Web of Science ID 000175740200021
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Adsorption-induced step formation (vol 87, art no 126102, 2001)
PHYSICAL REVIEW LETTERS
2002; 88 (4)
View details for DOI 10.1103/PhysRevLett.88.049902
View details for Web of Science ID 000173907500087
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Optimal catalyst curves: Connecting density functional theory calculations with industrial reactor design and catalyst selection
JOURNAL OF CATALYSIS
2002; 205 (2): 382-387
View details for DOI 10.1006/jcat.2001.3442
View details for Web of Science ID 000173691900019
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Structure sensitivity of CO dissociation on Rh surfaces
CATALYSIS LETTERS
2002; 81 (3-4): 153-156
View details for Web of Science ID 000176934300004
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Hydrogen and synthesis gas by steam- and CO2 reforming
ADVANCES IN CATALYSIS, VOL 47
2002; 47: 65-139
View details for Web of Science ID 000180211800002
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Electronic structure and catalysis on metal surfaces
ANNUAL REVIEW OF PHYSICAL CHEMISTRY
2002; 53: 319-348
Abstract
The powerful computational resources available to scientists today, together with recent improvements in electronic structure calculation algorithms, are providing important new tools for researchers in the fields of surface science and catalysis. In this review, we discuss first principles calculations that are now capable of providing qualitative and, in many cases, quantitative insights into surface chemistry. The calculations can aid in the establishment of chemisorption trends across the transition metals, in the characterization of reaction pathways on individual metals, and in the design of novel catalysts. First principles studies provide an excellent fundamental complement to experimental investigations of the above phenomena and can often allow the elucidation of important mechanistic details that would be difficult, if not impossible, to determine from experiments alone.
View details for DOI 10.1146/annurev.physchem.53.100301.131630
View details for Web of Science ID 000176264900013
View details for PubMedID 11972011
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Oxygen vacancies as active sites for water dissociation on rutile TiO2(110)
PHYSICAL REVIEW LETTERS
2001; 87 (26)
Abstract
Through an interplay between scanning tunneling microscopy experiments and density functional theory calculations, we determine unambiguously the active surface site responsible for the dissociation of water molecules adsorbed on rutile TiO(2)(110). Oxygen vacancies in the surface layer are shown to dissociate H(2)O through the transfer of one proton to a nearby oxygen atom, forming two hydroxyl groups for every vacancy. The amount of water dissociation is limited by the density of oxygen vacancies present on the clean surface exclusively. The dissociation process sets in as soon as molecular water is able to diffuse to the active site.
View details for DOI 10.1103/PhysRevLett.87.266104
View details for Web of Science ID 000172999700019
View details for PubMedID 11800845
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Adsorption of Cu and Pd on alpha-Al2O3(0001) surfaces with different stoichiometries
JOURNAL OF CHEMICAL PHYSICS
2001; 115 (24): 11261-11267
View details for Web of Science ID 000172683200027
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Electronic factors in catalysis: the volcano curve and the effect of promotion in catalytic ammonia synthesis
APPLIED CATALYSIS A-GENERAL
2001; 222 (1-2): 19-29
View details for Web of Science ID 000173425000003
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Kinetics of the Anode Processes in PEM Fuel Cells - The Promoting Effect of Ru in PtRu Anodes
FUEL CELLS
2001; 1 (3-4): 192-201
View details for Web of Science ID 000208113500005
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N-2 dissociation on Fe(110) and Fe/Ru(0001): what is the role of steps?
SURFACE SCIENCE
2001; 491 (1-2): 183-194
View details for Web of Science ID 000171389900022
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Adsorption-induced step formation
PHYSICAL REVIEW LETTERS
2001; 87 (12)
Abstract
Through an interplay between density functional calculations, Monte Carlo simulations and scanning tunneling microscopy experiments, we show that an intermediate coverage of CO on the Pt(110) surface gives rise to a new rough equilibrium structure with more than 50% step atoms. CO is shown to bind so strongly to low-coordinated Pt atoms that it can break Pt-Pt bonds and spontaneously form steps on the surface. It is argued that adsorption-induced step formation may be a general effect, in particular at high gas pressures and temperatures.
View details for DOI 10.1103/PhysRevLett.87.126102
View details for Web of Science ID 000171122700042
View details for PubMedID 11580529
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The effect of strain for N-2 dissociation on Fe surfaces
SURFACE SCIENCE
2001; 489 (1-3): 135-143
View details for Web of Science ID 000170761800014
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Structure and reactivity of Ni-Au nanoparticle catalysts
JOURNAL OF PHYSICAL CHEMISTRY B
2001; 105 (23): 5450-5458
View details for DOI 10.1021/jp0043975
View details for Web of Science ID 000169371400013
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The CO/Pt(111) puzzle
JOURNAL OF PHYSICAL CHEMISTRY B
2001; 105 (18): 4018-4025
View details for Web of Science ID 000168624400047
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Synergetic effects in CO adsorption on Cu-Pd(111) alloys
SURFACE SCIENCE
2001; 477 (1): 59-75
View details for Web of Science ID 000168024000008
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Anode materials for low-temperature fuel cells: A density functional theory study
JOURNAL OF CATALYSIS
2001; 199 (1): 123-131
View details for DOI 10.1006/jcat.2000.3136
View details for Web of Science ID 000168082200013
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Density functional theory studies of the adsorption of ethylene and oxygen on Pt(111) and Pt3Sn(111)
JOURNAL OF CHEMICAL PHYSICS
2001; 114 (10): 4663-4668
View details for Web of Science ID 000167367800035
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Ligand and ensemble effects in adsorption on alloy surfaces
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
2001; 3 (17): 3814-3818
View details for Web of Science ID 000170907800053
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Catalysis from first principles
FOUNDATIONS OF MOLECULAR MODELING AND SIMULATION
2001; 97 (325): 131-134
View details for Web of Science ID 000180146200015
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Modeling the nitrogenase FeMo cofactor
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2000; 122 (51): 12751-12763
View details for DOI 10.1021/ja00163q
View details for Web of Science ID 000166045000018
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Molecular aspects of the H-2 activation on MoS2 based catalysts the role of dynamic surface arrangements
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
2000; 163 (1-2): 117-122
View details for Web of Science ID 000165998600012
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Steps, kinks, and segregation at metallic surfaces
PROGRESS IN SURFACE SCIENCE
2000; 64 (3-8): 193-198
View details for Web of Science ID 000087293800009
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Surface chemistry in three dimensions: CO dissociation between two surfaces
CHEMICAL PHYSICS LETTERS
2000; 322 (5): 307-311
View details for Web of Science ID 000087272100002
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Diffusion of N adatoms on the Fe(100) surface
PHYSICAL REVIEW LETTERS
2000; 84 (21): 4898-4901
View details for Web of Science ID 000087114400029
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A comparative theoretical study of the hydrogen, methyl, and ethyl chemisorption on the Pt(111) surface
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2000; 122 (17): 4129-4144
View details for Web of Science ID 000086950500020
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First principles analysis of hydrogen chemisorption on Pd-Re alloyed overlayers and alloyed surfaces
JOURNAL OF CHEMICAL PHYSICS
2000; 112 (12): 5435-5439
View details for Web of Science ID 000085766100026
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Theoretical studies of stability and reactivity of C-2 hydrocarbon species on Pt clusters, Pt(111), and Pt(211)
JOURNAL OF PHYSICAL CHEMISTRY B
2000; 104 (10): 2299-2310
View details for Web of Science ID 000085902600015
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Making gold less noble
CATALYSIS LETTERS
2000; 64 (2-4): 101-106
View details for Web of Science ID 000085099300005
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Asymmetric pair distribution functions in catalysts
TOPICS IN CATALYSIS
2000; 10 (3-4): 221-230
View details for Web of Science ID 000086446400009
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Edge termination of MoS2 and CoMoS catalyst particles
CATALYSIS LETTERS
2000; 64 (2-4): 95-99
View details for Web of Science ID 000085099300004
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Theoretical studies of stability and reactivity of CHx species on Ni(111)
JOURNAL OF CATALYSIS
2000; 189 (1): 16-30
View details for Web of Science ID 000084796000002
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Molecular N-2 chemisorption-specific adsorption on step defect sites on Pt surfaces
JOURNAL OF CHEMICAL PHYSICS
1999; 111 (18): 8651-8658
View details for Web of Science ID 000083345100046
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Chemisorption of methane on Ni(100) and Ni(111) surfaces with preadsorbed potassium
JOURNAL OF CATALYSIS
1999; 187 (1): 238-244
View details for Web of Science ID 000083018400025
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DFT calculations of unpromoted and promoted MoS2-based hydrodesulfurization catalysts
JOURNAL OF CATALYSIS
1999; 187 (1): 109-122
View details for Web of Science ID 000083018400011
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Mechanisms of self-diffusion on Pt(110)
PHYSICAL REVIEW B
1999; 60 (8): R5149-R5152
View details for Web of Science ID 000082478600015
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Theoretical analysis of hydrogen chemisorption on Pd(111), Re(0001) and Pd-ML/Re(0001), Re-ML/Pd(111) pseudomorphic overlayers
PHYSICAL REVIEW B
1999; 60 (8): 6146-6154
View details for Web of Science ID 000082478600132
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Oxygen adsorption on Pt(110)-(1x2): new high-coverage structures
SURFACE SCIENCE
1999; 430 (1-3): L533-L539
View details for Web of Science ID 000081492000004
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Surface segregation energies in transition-metal alloys
PHYSICAL REVIEW B
1999; 59 (24): 15990-16000
View details for Web of Science ID 000081134700053
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How a gold substrate can increase the reactivity of a Pt overlayer
SURFACE SCIENCE
1999; 426 (3): 395-409
View details for Web of Science ID 000080670000015
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Nitrogen adsorption and hydrogenation on a MoFe6S9 complex
PHYSICAL REVIEW LETTERS
1999; 82 (20): 4054-4057
View details for Web of Science ID 000080319900033
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Enhancement of surface self-diffusion of platinum atoms by adsorbed hydrogen
NATURE
1999; 398 (6723): 134-136
View details for Web of Science ID 000079135200039
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Nitrogen adsorption and dissociation on Fe(111)
JOURNAL OF CATALYSIS
1999; 182 (2): 479-488
View details for Web of Science ID 000079076900020
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Nitrogen adsorption on Fe(111), (100), and (110) surfaces
SURFACE SCIENCE
1999; 422 (1-3): 8-16
View details for Web of Science ID 000078934500007
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Advances in deep desulfurization
SCIENCE AND TECHNOLOGY IN CATALYSIS 1998
1999; 121: 13-22
View details for Web of Science ID 000081933100002
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A theoretical study of adsorbate-adsorbate interactions on Ru(0001)
SURFACE SCIENCE
1998; 414 (3): 315-329
View details for Web of Science ID 000076198900003
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Crystal-structure contribution to the solid solubility in transition metal alloys
PHYSICAL REVIEW LETTERS
1998; 80 (6): 1240-1243
View details for Web of Science ID 000071915900030
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Sulphur bonding in transition metal sulphides and MoS2 based structures
TRANSITIONAL METAL SULPHIDES
1998; 60: 155-168
View details for Web of Science ID 000077552400006
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N-2 interaction with Fe surfaces
ISRAEL JOURNAL OF CHEMISTRY
1998; 38 (4): 279-284
View details for Web of Science ID 000081567400002
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Adsorbate reorganization at steps: NO on Pd(211)
PHYSICAL REVIEW LETTERS
1997; 79 (22): 4441-4444
View details for Web of Science ID A1997YJ38800036
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Growth of Co on Cu(111): subsurface growth of trilayer Co islands
SURFACE SCIENCE
1997; 387 (1-3): 86-101
View details for Web of Science ID A1997YC84800017
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CO adsorption and dissociation on Pt(111) and Ni(111) surfaces
SURFACE SCIENCE
1997; 386 (1-3): 67-72
View details for Web of Science ID A1997YA92500008
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Phase diagrams for surface alloys
PHYSICAL REVIEW B
1997; 56 (10): 5822-5834
View details for Web of Science ID A1997XY59500026
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Density functional calculations of N-2 adsorption and dissociation on a Ru(0001) surface
JOURNAL OF CATALYSIS
1997; 169 (1): 85-92
View details for Web of Science ID A1997XL77900009
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Kinetic implications of dynamical changes in catalyst morphology during methanol synthesis over Cu/ZnO catalysts
JOURNAL OF CATALYSIS
1997; 168 (2): 133-142
View details for Web of Science ID A1997XE03100002
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Surface electronic structure and reactivity of transition and noble metals
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
1997; 115 (3): 421-429
View details for Web of Science ID A1997WG58300005
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Scattering and conductance quantization in three-dimensional metal nanocontacts
PHYSICAL REVIEW B
1997; 55 (4): 2637-2650
View details for Web of Science ID A1997WF12400090
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Cs-induced relaxation of the Cu(110) surface - Comment
PHYSICAL REVIEW LETTERS
1997; 78 (1): 158-158
View details for Web of Science ID A1997WA70900040
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Sulfur bonding in MoS2 and Co-Mo-S structures
CATALYSIS LETTERS
1997; 47 (3-4): 177-182
View details for Web of Science ID A1997YC90000002
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A comparison of N-2 and CO adsorption on Ru(001)
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS
1997; 198: 113-122
View details for Web of Science ID A1997WB57300007
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Structure sensitivity in adsorption: CO interaction with stepped and reconstructed Pt surfaces
CATALYSIS LETTERS
1997; 46 (1-2): 31-35
View details for Web of Science ID A1997XM51300006
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Theory of adsorption and surface reactions
CHEMISORPTION AND REACTIVITY ON SUPPORTED CLUSTERS AND THIN FILMS
1997; 331: 285-351
View details for Web of Science ID A1997BH53Z00011
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Importance of dynamics in real catalyst systems
DYNAMICS OF SURFACES AND REACTION KINETICS IN HETEROGENEOUS CATALYSIS
1997; 109: 121-139
View details for Web of Science ID 000071440800007
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A semi-empirical effective medium theory for metals and alloys
SURFACE SCIENCE
1996; 366 (2): 394-402
View details for Web of Science ID A1996VL93400026
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A theoretical study of CH4 dissociation on pure and gold-alloyed Ni(111) surfaces
JOURNAL OF CHEMICAL PHYSICS
1996; 105 (13): 5595-5604
View details for Web of Science ID A1996VL46900035
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Incomplete melting of the Si(100) surface from molecular-dynamics simulations using the effective-medium tight-binding model
SURFACE SCIENCE
1996; 360 (1-3): 221-228
View details for Web of Science ID A1996UX92300030
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Island shapes in homoepitaxial growth of Pt(111)
SURFACE SCIENCE
1996; 359 (1-3): 37-44
View details for Web of Science ID A1996UW25400009
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Geometric and electronic factors determining the differences in reactivity of H-2 on Cu(100) and Cu(111)
SURFACE SCIENCE
1996; 359 (1-3): 45-53
View details for Web of Science ID A1996UW25400010
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Electronic factors determining the reactivity of metal surfaces (vol 343, pg 211, 1995)
SURFACE SCIENCE
1996; 359 (1-3): 306-306
View details for Web of Science ID A1996UW25400034
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Stability of adsorbed hydrogen on Si(100) under changes of the surface potential
SURFACE REVIEW AND LETTERS
1996; 3 (2): 1227-1233
View details for Web of Science ID A1996VC94800001
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Anisotropic corner diffusion as origin for dendritic growth on hexagonal substrates
SURFACE SCIENCE
1996; 349 (1): L115-L122
View details for Web of Science ID A1996UB58100006
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CO chemisorption at metal surfaces and overlayers
PHYSICAL REVIEW LETTERS
1996; 76 (12): 2141-2144
View details for Web of Science ID A1996TZ98400039
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Microkinetic analysis of the water-gas shift reaction under industrial conditions
JOURNAL OF CATALYSIS
1996; 158 (1): 170-180
View details for Web of Science ID A1996TQ77400016
- Geometric and electronic factors determining the difference in reactivity of H2 on Cu(110) and Cu(111) Surf.Sci. 1996; 359: 45
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Designing surface alloys with specific active sites
CATALYSIS LETTERS
1996; 40 (3-4): 131-135
View details for Web of Science ID A1996VE92300001
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Fractal and dendritic growth of surface aggregates
DISORDERED MATERIALS AND INTERFACES
1996; 407: 379-389
View details for Web of Science ID A1996BF25P00056
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ELECTRONIC-STRUCTURE, TOTAL ENERGIES, AND STM IMAGES OF CLEAN AND OXYGEN-COVERED AL(111)
PHYSICAL REVIEW B
1995; 52 (20): 14954-14962
View details for Web of Science ID A1995TH68200093
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EFFECT OF STRAIN ON SURFACE-DIFFUSION AND NUCLEATION
PHYSICAL REVIEW B
1995; 52 (20): 14380-14383
View details for Web of Science ID A1995TH68200020
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QUANTIZED CONDUCTANCE IN ATOM-SIZED WIRES BETWEEN 2 METALS
PHYSICAL REVIEW B
1995; 52 (11): 8499-8514
View details for Web of Science ID A1995RV81800107
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ATOMIC-SCALE DETERMINATION OF MISFIT DISLOCATION LOOPS AT METAL-METAL INTERFACES
PHYSICAL REVIEW LETTERS
1995; 75 (3): 489-492
View details for Web of Science ID A1995RK33000034
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DIRECT PATHWAY FOR STICKING DESORPTION OF H-2 ON SI(100)
PHYSICAL REVIEW B
1995; 51 (19): 13432-13440
View details for Web of Science ID A1995QZ16500060
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SURFACE STRESS, SURFACE ELASTICITY, AND THE SIZE EFFECT IN SURFACE SEGREGATION
PHYSICAL REVIEW B
1995; 51 (16): 10937-10946
View details for Web of Science ID A1995QW28400074
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THE BOND-ENERGY MODEL FOR HYDROTREATING REACTIONS - THEORETICAL AND EXPERIMENTAL ASPECTS
BULLETIN DES SOCIETES CHIMIQUES BELGES
1995; 104 (4-5): 283-291
View details for Web of Science ID A1995QT07600015
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ISLAND SHAPE-INDUCED TRANSITION FROM 2D TO 3D GROWTH FOR PT/PT(111)
PHYSICAL REVIEW LETTERS
1995; 74 (12): 2295-2298
View details for Web of Science ID A1995QM94300037
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QUANTIZED CONDUCTANCE IN AN ATOM-SIZED POINT-CONTACT - REPLY
PHYSICAL REVIEW LETTERS
1995; 74 (11): 2147-2147
View details for Web of Science ID A1995QL58400064
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DEALLOYING PHASE-SEPARATION DURING GROWTH OF AU ON NI(110)
PHYSICAL REVIEW LETTERS
1995; 74 (7): 1159-1162
View details for Web of Science ID A1995QG47200030
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SIZE DEPENDENCE OF PHASE-SEPARATION IN SMALL BIMETALLIC CLUSTERS
JOURNAL OF PHYSICS-CONDENSED MATTER
1995; 7 (6): 1047-1057
View details for Web of Science ID A1995QH27300008
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THE MOBILITY OF PT ATOMS AND SMALL PT CLUSTERS ON PT(111) AND ITS IMPLICATIONS FOR THE EARLY STAGES OF EPITAXIAL-GROWTH
SURFACE SCIENCE
1994; 321 (1-2): 161-171
View details for Web of Science ID A1994PX99700022
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THE COUPLING BETWEEN ADSORPTION DYNAMICS AND THE SURFACE-STRUCTURE - H-2 ON SI(100)
CHEMICAL PHYSICS LETTERS
1994; 229 (6): 645-649
View details for Web of Science ID A1994PQ55100013
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EFFECTIVE-MEDIUM TIGHT-BINDING MODEL FOR SILICON
PHYSICAL REVIEW B
1994; 50 (15): 10727-10741
View details for Web of Science ID A1994PP12400035
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MULTIDIMENSIONAL POTENTIAL-ENERGY SURFACE FOR H-2 DISSOCIATION OVER CU(111)
PHYSICAL REVIEW LETTERS
1994; 73 (10): 1400-1403
View details for Web of Science ID A1994PE72700023
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Wetting/non-wetting phenomena during catalysis: evidence from in situ on-line EXAFS studies of Cu-based catalysts
TOPICS IN CATALYSIS
1994; 1 (3-4): 367-376
View details for Web of Science ID 000208529500016
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DETERMINATION OF METAL-PARTICLE SIZES FROM EXAFS
CATALYSIS TODAY
1994; 21 (1): 49-55
View details for Web of Science ID A1994PF95200005
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CONSTRUCTION OF TRANSFERABLE SPHERICALLY AVERAGED ELECTRON POTENTIALS
JOURNAL OF PHYSICS-CONDENSED MATTER
1994; 6 (28): 5415-5421
View details for Web of Science ID A1994NW72200016
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SURFACE ALLOYING IN METAL-ON-METAL EPITAXIAL-GROWTH
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
1994; 12 (4): 1787-1789
View details for Web of Science ID A1994NZ03200001
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QUANTIZED CONDUCTANCE IN AN ATOM-SIZED POINT-CONTACT
PHYSICAL REVIEW LETTERS
1994; 72 (14): 2251-2254
View details for Web of Science ID A1994NE03000032
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MELTING A COPPER CLUSTER - CRITICAL-DROPLET THEORY
EUROPHYSICS LETTERS
1994; 26 (1): 51-56
View details for Web of Science ID A1994NH19100009
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THE ENERGETICS AND DYNAMICS OF H-2 DISSOCIATION ON AL(110)
SURFACE SCIENCE
1994; 304 (1-2): 131-144
View details for Web of Science ID A1994MZ12200021
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THEORY OF ADSORPTION AND ADSORBATE-INDUCED RECONSTRUCTION
SURFACE SCIENCE
1994; 299 (1-3): 690-705
View details for Web of Science ID A1994MT97800050
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METHANOL SYNTHESIS ON CU(100) FROM A BINARY GAS-MIXTURE OF CO2 AND H2
CATALYSIS LETTERS
1994; 26 (3-4): 373-381
View details for Web of Science ID A1994NR87300017
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MODELING THE POTASSIUM PROMOTION OF CO BONDING TO NI(100)
CHEMICAL PHYSICS LETTERS
1993; 214 (5): 443-446
View details for Web of Science ID A1993MF36200003
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OXYGEN-CHEMISORPTION ON METAL-SURFACES - GENERAL TRENDS FOR CU, NI AND AG
PROGRESS IN SURFACE SCIENCE
1993; 44 (1): 5-66
View details for Web of Science ID A1993LX86500001
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EXPERIMENTAL AND THEORETICAL-STUDIES OF PERIODIC TRENDS AND PROMOTIONAL BEHAVIORS OF HYDROTREATING CATALYSTS
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
1993; 206: 8-PETR
View details for Web of Science ID A1993LP32200629
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IMPROVED METHOD FOR DETERMINATION OF METAL-PARTICLE SIZES FROM EXAFS
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
1993; 206: 64-PETR
View details for Web of Science ID A1993LP32200685
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ACCOMMODATION AND DIFFUSION OF CU DEPOSITED ON FLAT AND STEPPED CU(111) SURFACES
PHYSICAL REVIEW B
1993; 48 (8): 5607-5611
View details for Web of Science ID A1993LV38500069
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INITIAL GROWTH OF AU ON NI(110) - SURFACE ALLOYING OF IMMISCIBLE METALS
PHYSICAL REVIEW LETTERS
1993; 71 (5): 754-757
View details for Web of Science ID A1993LQ10700025
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ROLE OF NONLOCAL EXCHANGE-CORRELATION IN ACTIVATED ADSORPTION
PHYSICAL REVIEW LETTERS
1993; 70 (25): 3971-3974
View details for Web of Science ID A1993LH55400034
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A NEW PROCEDURE FOR PARTICLE-SIZE DETERMINATION BY EXAFS BASED ON MOLECULAR-DYNAMICS SIMULATIONS
JOURNAL OF CATALYSIS
1993; 141 (2): 368-379
View details for Web of Science ID A1993LE31100005
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ACTIVATION FREE-ENERGY AND ENTROPY FOR THE NORMAL AND EXCHANGE SELF-DIFFUSION PROCESSES ON CU(100)
SURFACE SCIENCE
1993; 289 (1-2): 68-74
View details for Web of Science ID A1993LE87300017
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CHEMISORPTION AND VIBRATION OF HYDROGEN ON CU(111)
SURFACE SCIENCE
1993; 285 (1-2): 27-30
View details for Web of Science ID A1993KU65600011
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MANY-ATOM INTERACTIONS IN METALS
SURFACE SCIENCE
1993; 283 (1-3): 277-282
View details for Web of Science ID A1993KM97500043
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THE EFFECT OF ANHARMONICITY ON THE EXAFS COORDINATION-NUMBER IN SMALL METALLIC PARTICLES
JAPANESE JOURNAL OF APPLIED PHYSICS PART 1-REGULAR PAPERS BRIEF COMMUNICATIONS & REVIEW PAPERS
1993; 32: 95-97
View details for Web of Science ID A1993LT05000030
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AB-INITIO EFFECTIVE-MEDIUM THEORY FOR AL
INTERATOMIC POTENTIAL AND STRUCTURAL STABILITY
1993; 114: 15-22
View details for Web of Science ID A1993BA62C00002
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DISSOCIATION PATH FOR H2 ON AL(110)
PHYSICAL REVIEW LETTERS
1992; 69 (13): 1971-1974
View details for Web of Science ID A1992JP85900037
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AN EFFECTIVE-MEDIUM THEORY APPROACH TO ORDERING IN CU-AU ALLOYS
JOURNAL OF PHYSICS-CONDENSED MATTER
1992; 4 (35): 7191-7202
View details for Web of Science ID A1992JM00700005
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ABINITIO POTENTIAL FOR SOLIDS
PHYSICAL REVIEW B
1992; 46 (7): 3798-3809
View details for Web of Science ID A1992JJ84600011
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CHEMISORPTION OF H, O, AND S ON NI(110) - GENERAL TRENDS
SURFACE SCIENCE
1992; 272 (1-3): 334-341
View details for Web of Science ID A1992HZ81900046
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UNDERSTANDING THE TRENDS IN THE HYDRODESULFURIZATION ACTIVITY OF THE TRANSITIN METAL SULFIDES
CATALYSIS LETTERS
1992; 13 (1-2): 1-8
View details for Web of Science ID A1992HL44500001
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ANHARMONICITY AND DISORDER ON THE CU(110) SURFACE
PHYSICAL REVIEW B
1991; 44 (23): 13002-13009
View details for Web of Science ID A1991GV74100044
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SELF-DIFFUSION ON COPPER SURFACES
PHYSICAL REVIEW B
1991; 44 (12): 6523-6526
View details for Web of Science ID A1991GH55300060
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VIBRATIONAL PROPERTIES OF ALUMINUM, NICKEL AND COPPER SURFACES
SURFACE SCIENCE
1991; 254 (1-3): 261-274
View details for Web of Science ID A1991GC42900042
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CU CLUSTER SHELL STRUCTURE AT ELEVATED-TEMPERATURES
PHYSICAL REVIEW LETTERS
1991; 66 (17): 2219-2222
View details for Web of Science ID A1991FJ59800012
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MANY-ATOM INTERACTIONS IN SOLIDS
PHILOSOPHICAL TRANSACTIONS OF THE ROYAL SOCIETY OF LONDON SERIES A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES
1991; 334 (1635): 393-405
View details for Web of Science ID A1991FE32600001
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ELECTRONIC FACTORS IN CATALYSIS
PROGRESS IN SURFACE SCIENCE
1991; 38 (2): 103-144
View details for Web of Science ID A1991GT01500001
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THE REACTIVITY OF METAL-SURFACES
CATALYSIS LETTERS
1991; 9 (3-4): 173-182
View details for Web of Science ID A1991FR65400003
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THE SURFACE PHONONS OF CU(111)
JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA
1990; 54: 237-244
View details for Web of Science ID A1990ET21000023
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OXYGEN-CHEMISORPTION ON CU(110) - A MODEL FOR THE C(6X2) STRUCTURE
PHYSICAL REVIEW LETTERS
1990; 65 (16): 2027-2030
View details for Web of Science ID A1990ED48100016
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THEORY OF THE OXYGEN-INDUCED RESTRUCTURING OF CU(110) AND CU(100) SURFACES
PHYSICAL REVIEW LETTERS
1990; 65 (14): 1788-1791
View details for Web of Science ID A1990EA46200025
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INTERACTION OF HYDROGEN ISOTOPES WITH METALS - DEUTERIUM TRAPPED AT LATTICE-DEFECTS IN PALLADIUM
JOURNAL OF FUSION ENERGY
1990; 9 (3): 257-261
View details for Web of Science ID A1990EQ36700003
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THE DISSOCIATIVE ADSORPTION OF HYDROGEN - 2-DIMENSIONAL, 3-DIMENSIONAL, AND 4-DIMENSIONAL QUANTUM SIMULATIONS
JOURNAL OF CHEMICAL PHYSICS
1990; 93 (4): 2879-2884
View details for Web of Science ID A1990DT88800081
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IS THERE A CONTRACTION OF THE INTERATOMIC DISTANCE IN SMALL METAL PARTICLES
PHYSICAL REVIEW LETTERS
1990; 64 (26): 3155-3158
View details for Web of Science ID A1990DK65900014
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EFFECTIVE-MEDIUM CALCULATIONS FOR HYDROGEN IN NI, PD, AND PT
PHYSICAL REVIEW B
1990; 41 (18): 12413-12423
View details for Web of Science ID A1990DL67200003
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ELECTROSTATIC INTERACTIONS BETWEEN COADSORBED XE AND CO
SURFACE SCIENCE
1990; 226 (1-2): L48-L50
View details for Web of Science ID A1990CU70300002
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THE ONSET OF DISORDER IN AL(110) SURFACES BELOW THE MELTING-POINT
SURFACE SCIENCE
1989; 220 (2-3): L693-L700
View details for Web of Science ID A1989AU63100001
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H-H INTERACTIONS IN PD
PHYSICAL REVIEW B
1989; 40 (3): 1993-1996
View details for Web of Science ID A1989AG98100075
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MULTIPLE DEUTERIUM OCCUPANCY OF VACANCIES IN PD AND RELATED METALS
PHYSICAL REVIEW B
1989; 40 (3): 1990-1992
View details for Web of Science ID A1989AG98100074
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DISORDERING AND MELTING OF ALUMINUM SURFACES
PHYSICAL REVIEW LETTERS
1988; 61 (4): 440-443
View details for Web of Science ID A1988P335500016
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THEORY OF ALKALI-METAL INDUCED RECONSTRUCTION OF FCC (110) SURFACES
PHYSICAL REVIEW LETTERS
1988; 60 (24): 2496-2498
View details for Web of Science ID A1988N799600014
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AN INTERPRETATION OF THE HIGH-PRESSURE KINETICS OF AMMONIA-SYNTHESIS BASED ON A MICROSCOPIC MODEL
JOURNAL OF CATALYSIS
1988; 110 (1): 1-10
View details for Web of Science ID A1988M631300001
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THEORY OF ADSORBATE-INDUCED SURFACE RELAXATIONS - HYDROGEN ON CU(110)
PHYSICAL REVIEW LETTERS
1987; 59 (24): 2764-2767
View details for Web of Science ID A1987L179100014
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THEORETICAL ASPECTS OF SURFACE-REACTIONS
SURFACE SCIENCE
1987; 189: 91-105
View details for Web of Science ID A1987K537200014
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MONTE-CARLO CALCULATION OF THE THERMAL-EXPANSION COEFFICIENT OF AL
PHYSICAL REVIEW B
1987; 36 (9): 5035-5036
View details for Web of Science ID A1987K345400058
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THEORY OF HYDROGEN INTERACTION WITH METALS
JOURNAL OF THE LESS-COMMON METALS
1987; 130: 475-490
View details for Web of Science ID A1987G849400065
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MULTIPLE HYDROGEN OCCUPANCY OF VACANCIES IN FE
JOURNAL OF APPLIED PHYSICS
1987; 61 (5): 1788-1794
View details for Web of Science ID A1987G151000015
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ELECTROSTATIC INTERACTIONS AND THEIR ROLE IN COADSORPTION PHENOMENA
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I
1987; 83: 1935-1943
View details for Web of Science ID A1987J243500003
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TRENDS IN HYDROGEN HEATS OF SOLUTION AND VACANCY TRAPPING ENERGIES IN TRANSITION-METALS
JOURNAL OF PHYSICS F-METAL PHYSICS
1986; 16 (9): 1161-1171
View details for Web of Science ID A1986D850800007
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CALCULATED DIABATIC ATOM-SURFACE POTENTIAL-ENERGY CURVES
PHYSICA SCRIPTA
1986; 34 (1): 77-83
View details for Web of Science ID A1986D386300013
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QUANTUM MOTION OF CHEMISORBED HYDROGEN
JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA
1986; 38 (1-4): 313-315
View details for Web of Science ID A1986A806200039
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A THEORETICAL-STUDY OF CARBON CHEMISORPTION ON NICKEL SURFACES
SURFACE SCIENCE
1986; 166 (2-3): 539-553
View details for Web of Science ID A1986A713800020
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THEORETICAL-EXAMINATION OF THE TRAPPING OF ION-IMPLANTED HYDROGEN IN METALS
PHYSICAL REVIEW B
1986; 33 (2): 854-863
View details for Web of Science ID A1986AXX0400022
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EXCITATION OF HYDROGEN MOTION INSIDE A NICKEL VACANCY
PHYSICAL REVIEW LETTERS
1985; 55 (8): 852-855
View details for Web of Science ID A1985ANX2600023
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ELECTROSTATIC ADSORBATE ADSORBATE INTERACTIONS - THE POISONING AND PROMOTION OF THE MOLECULAR ADSORPTION REACTION
SURFACE SCIENCE
1985; 150 (1): 24-38
View details for Web of Science ID A1985ADN8800012
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ADSORBATE SURFACE AND ADSORBATE ADSORBATE INTERACTIONS AND THEIR ROLE IN SURFACE-REACTIONS
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY A
1985; 3 (3): 1668-1672
View details for Web of Science ID A1985AKX5100183
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IMMOBILIZATION MECHANISMS FOR ION-IMPLANTED DEUTERIUM IN ALUMINUM
JOURNAL OF APPLIED PHYSICS
1985; 58 (5): 1841-1850
View details for Web of Science ID A1985APV4100021
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OXYGEN-CHEMISORPTION AND INCORPORATION ON TRANSITION-METAL SURFACES
SURFACE SCIENCE
1985; 152 (APR): 660-683
View details for Web of Science ID A1985AHV6300006
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INTERACTION OF HYDROGEN WITH DEFECTS IN METALS
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS
1985; 7-8 (MAR): 55-66
View details for Web of Science ID A1985AGM5800010
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ELECTROSTATIC ADSORBATE-ADSORBATE INTERACTIONS - THE POISONING AND PROMOTION OF THE MOLECULAR ADSORPTION REACTION
ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
1985; 190 (SEP): 228-COL
View details for Web of Science ID A1985APH0301171
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INTERACTION OF DEUTERIUM WITH LATTICE-DEFECTS IN NICKEL
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS
1984; 4 (3): 374-387
View details for Web of Science ID A1984TH64700008
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VIBRATIONAL-EXCITATION, HARPOONING, AND STICKING IN MOLECULE SURFACE COLLISIONS
JOURNAL OF CHEMICAL PHYSICS
1984; 81 (6): 2828-2838
View details for Web of Science ID A1984TJ82200040
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THEORY OF CHEMISORPTION AND HETEROGENEOUS CATALYSIS
PHYSICA B & C
1984; 127 (1-3): 193-202
View details for Web of Science ID A1984AAL6400029
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HYDROGEN ADSORPTION ON METAL-SURFACES
SURFACE SCIENCE
1984; 136 (1): 59-81
View details for Web of Science ID A1984SB32900013
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QUANTUM MOTION OF CHEMISORBED HYDROGEN ON NI SURFACES
PHYSICAL REVIEW LETTERS
1983; 51 (12): 1081-1084
View details for Web of Science ID A1983RG66900018
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THEORETICAL-STUDIES OF MOLECULAR ADSORPTION ON METAL-SURFACES
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY
1983; 23 (3): 1083-1090
View details for Web of Science ID A1983QF84100031
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THE THEORY OF IONIZATION PROBABILITY IN SPUTTERING
PHYSICA SCRIPTA
1983; T6: 15-18
View details for Web of Science ID A1983RR84800003
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INTERACTION OF HELIUM WITH A METAL-SURFACE
PHYSICAL REVIEW B
1983; 27 (8): 4612-4616
View details for Web of Science ID A1983QL76000008
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RARE-GAS-METAL PAIR POTENTIAL - HE-VACANCY INTERACTION
JOURNAL OF PHYSICS F-METAL PHYSICS
1982; 12 (2): L7-L11
View details for Web of Science ID A1982NA59300001
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CALCULATION OF THE HELIUM DIFFRACTION FROM THE RECONSTRUCTED AU(110) SURFACE
SURFACE SCIENCE
1982; 119 (2-3): L393-L400
View details for Web of Science ID A1982PF74100005
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INTERACTION OF HYDROGEN WITH DEFECTS IN METALS - INTERPLAY BETWEEN THEORY AND EXPERIMENT
PHYSICAL REVIEW LETTERS
1982; 49 (19): 1420-1423
View details for Web of Science ID A1982PN79200016
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CALCULATED BINDING-PROPERTIES OF HYDROGEN ON NICKEL SURFACES
PHYSICAL REVIEW LETTERS
1982; 48 (23): 1620-1624
View details for Web of Science ID A1982NR77100014
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COVALENT EFFECTS IN THE EFFECTIVE-MEDIUM THEORY OF CHEMICAL-BINDING - HYDROGEN HEATS OF SOLUTION IN THE 3D-METALS
PHYSICAL REVIEW B
1982; 26 (6): 2875-2885
View details for Web of Science ID A1982PH27000016
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DYNAMICAL ASPECTS OF ELECTRONIC-STRUCTURE DURING ADSORPTION
JOURNAL OF VACUUM SCIENCE & TECHNOLOGY
1981; 18 (2): 420-426
View details for Web of Science ID A1981LT55400071
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ADSORPTION AND DISSOCIATION OF H-2 ON MG SURFACES
PHYSICAL REVIEW LETTERS
1981; 46 (4): 257-260
View details for Web of Science ID A1981KZ00700014
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EFFECTIVE-MEDIUM THEORY OF CHEMICAL-BINDING - APPLICATION TO CHEMISORPTION
BULLETIN OF THE AMERICAN PHYSICAL SOCIETY
1980; 25 (3): 192-192
View details for Web of Science ID A1980JG27900208
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VARIATION OF ADATOM VALENCE-LEVEL POSITIONS WITH THE DISTANCE TO A METAL-SURFACE
PHYSICA SCRIPTA
1980; 22 (2): 165-170
View details for Web of Science ID A1980JX73200013
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THEORETICAL DESCRIPTION OF MOLECULE-METAL INTERACTION AND SURFACE-REACTIONS
SURFACE SCIENCE
1979; 89 (1-3): 196-225
View details for Web of Science ID A1979HZ47200023
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CORRELATION BETWEEN STICKING PROBABILITY AND ADSORBATE-INDUCED ELECTRON-STRUCTURE
SURFACE SCIENCE
1979; 89 (1-3): 251-261
View details for Web of Science ID A1979HZ47200026
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PICTURE OF ADSORPTION AND DESORPTION OF HYDROGEN EMERGING FROM SELF-CONSISTENT MODEL CALCULATIONS
SURFACE SCIENCE
1979; 80 (1): 441-449
View details for Web of Science ID A1979GK05400050
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MOLECULAR-ORBITAL DESCRIPTION OF SURFACE CHEMI-LUMINESCENCE
SURFACE SCIENCE
1979; 80 (1): 179-188
View details for Web of Science ID A1979GK05400023
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SELF-CONSISTENT CALCULATION OF MOLECULAR CHEMISORPTION ON METALS
PHYSICA SCRIPTA
1979; 20 (2): 192-201
View details for Web of Science ID A1979HH28700012
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CALCULATED ENERGIES AND GEOMETRIES FOR HYDROGEN IMPURITIES IN AL AND MG
JOURNAL OF PHYSICS F-METAL PHYSICS
1979; 9 (10): 1975-1982
View details for Web of Science ID A1979HR39700008
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PHOTON AND ELECTRON-EMISSION AS INDICATORS OF INTERMEDIATE STATES IN SURFACE-REACTIONS
SURFACE SCIENCE
1979; 89 (1-3): 554-565
View details for Web of Science ID A1979HZ47200052
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SECONDARY-ION EMISSION PROBABILITY IN SPUTTERING
PHYSICAL REVIEW B
1979; 19 (11): 5661-5665
View details for Web of Science ID A1979HD05700019
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CONTRACTION OF DIATOMIC-MOLECULES UPON CHEMISORPTION
SOLID STATE COMMUNICATIONS
1978; 28 (11): 899-902
View details for Web of Science ID A1978GC50700002
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IMPURITY INTERACTIONS AND PSEUDO-MOLECULE FORMATION IN METALS
SOLID STATE COMMUNICATIONS
1978; 25 (12): 995-998
View details for Web of Science ID A1978EW74200007
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ELECTRONIC-STRUCTURE OF H AND HE IN METAL VACANCIES
SOLID STATE COMMUNICATIONS
1977; 24 (9): 691-693
View details for Web of Science ID A1977EB21300025
Books and Book Chapters
- Theory, Fundamentals, and Biocatalysis edited by Wieckowski, A., Nørskov, J., K. Wiley. 2010
- Local equilibrium of metallic surface alloys, Chapter 1 The Chemical Physics of Solid Surfaces: Surface Alloys and Alloy Surfaces edited by Woodruff, D., P. Elsevier. 2002: 1
Conference Proceedings
-
Hydrogen evolution on nano-particulate transition metal sulfides
ROYAL SOC CHEMISTRY. 2008: 219-231
Abstract
The hydrogen evolution reaction (HER) on carbon supported MoS2 nanoparticles is investigated and compared to findings with previously published work on Au(111) supported MoS2. An investigation into MoS2 oxidation is presented and used to quantify the surface concentration of MoS2. Other metal sulfides with morphologies similar to MoS2 such as WS2, cobalt-promoted WS2, and cobalt-promoted MoS2 were also investigated in the search for improved HER activity. Experimental findings are compared to density functional theory (DFT) calculated values for the hydrogen binding energies (deltaGH) on each system.
View details for DOI 10.1039/b803857k
View details for Web of Science ID 000260437800016
View details for PubMedID 19213319