We seek fundamental level understanding of the physical principles driving thermal catalytic reactions related to methane activation. We use first principle tools based on Density Functional Theory (DFT) and micro-kinetic models to understand these processes at the atomic level. We explore variety of processes from converting methane into a more easily transportable fuel (CH3OH), to converting methane into more valuable chemicals (C2H4/CH2O), as well as catalysts that enable clean and efficient complete combustion of methane. We have successfully reduced the complexity of the first step in methane activation using simple descriptors that universally span many material types. We are leveraging this understanding to design catalysts that can selectively and efficiently activate methane. We couple this design with experimental efforts that involve the use of colloidal nanocrystals as well-defined building blocks to provide further understanding on methane activation reactions. Starting from size-, shape- and composition-controlled materials, we are able to provide systematic structure-property relationships on the role of specific active sites, oxidation states, metal-support interactions in the reactions of interest. We then apply the fundamental understanding gained from combining theory and catalytic studies to prepare more active, selective and stable catalysts.
We also use our base-level understanding of methane chemistry to translate it into larger hydrocarbons, thereby designing new scaling schemes that enable accurate predictions of transition state energy through reduced computational cost. Our studies span many material types including zeolites, transition metals, transition metal oxides, alkaline metal oxides, and many more with the objective of designing the right catalyst for the right application. We want to understand the rationale behind the current limitations of the process and design new methods to circumvent them. For the same reason, we investigate novel materials, including hybrid organic-inorganic catalytic systems and materials with encapsulated metal particles to provide novel ways to perform methane activation reactions.