1. Metal-Organic Frameworks for Alkane Activation

Heterogeneous catalysis is a key technology in many industrial chemical processes and energy conversion devices. With the recent surge in shale gas production, the catalytic conversion of small alkane molecules (e.g., CH4 and C2H6) to value-added chemicals and liquid fuels could potentially reshape the current chemicals and energy landscape in the US. The direct oxygen insertion into C-H bonds without the energy-intensive steam-reforming intermediate step has proven to be extremely difficult. Metal oxides catalysts, though extensively explored, often suffer from insufficient selectivity due to the close proximity of too many active sites that lead to further oxidation of intermediates and products. One of the strategies to circumvent the over-oxidation problem is to isolate active metal oxides clusters with organic linker molecules in metal-organic frameworks (MOFs). While the concept has been demonstrated in experiments, predictive models are needed to formulate novel MOFs materials with improved catalytic performance. The objective of the proposed research is to develop predictive models for design of active MOFs for partial oxidation of methane to methanol. The fundamental questions to be answered are: 1) “What are the electronic factors that determine the local chemical reactivity of MOFs?”, and 2) “How can we employ those insights to facilitate catalyst design?”. We address these questions by proposing a comprehensive plan that involves electronic structure calculations, kinetic modeling, and data management for powering an integrated descriptor-based molecular design framework. When successfully completed, the project will provide a systematic way to accelerate the discovery of promising MOFs materials for catalytic applications.


2. Single-Atom Catalysis for CO Oxidation Update coming soon.