Collaborative Research: Designing Nitrogen Coordinated Single Atomic Metal Electrocatalysts for Selective CO2 Reduction to CO
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abstract
Fossil fuels (i.e., coal, petroleum, and natural gas) are still today''s primary energy sources, but their utilization increases carbon emissions. Technologies that can convert waste carbon dioxide (CO2) into value-added chemicals have great economic and societal importance for realizing a sustainable energy future. Electricity, generated from sunlight, offers a potential sustainable route for CO2 conversion to chemicals, but present electrochemical approaches require expensive precious metals as catalysts. The project will focus on discovery of cost-effective alternatives to the precious metal catalysts while contributing to U.S. research leadership in energy utilization. The project will impact a broad range of technology related to renewable energy, water usage, transportation, and defense. Moreover, the research results will be incorporated into curriculum development, student mentoring, and educational outreach to high-school teachers and students. This award will also broaden the participation of underrepresented groups in conducting research and will positively impact higher education in science and engineering disciplines. Nitrogen coordinated single atomic metal (e.g. iron, cobalt, or nickel) is a new type of electrocatalyst that has demonstrated impressive activity and relatively high selectivity for electrochemical reduction of CO2 to carbon monoxide (CO) in recent research. However, the chemical nature of the active sites as well as the catalytic mechanisms for CO2 reduction in such complex catalyst systems are not fully understood. In addition, the factors controlling selectivity to CO2 reduction versus the competitive water reduction reaction are not well known. This research aims to provide fundamental understanding of rationally designed nitrogen coordinated single atomic metal sites embedded in a carbon framework and to elucidate the relationship between the synthesis, properties and performance of the catalysts in selective CO2 reduction into CO. The research team will 1) predict the active sites using first-principles calculation methods, 2) synthesize the catalysts containing the predicted active sites and local carbon structures, 3) conduct comprehensive characterization of the chemical properties, structure, and morphology of the synthesized catalysts, and 4) measure the performance of the synthesized catalysts for electrochemical CO2 reduction. This research will provide insights on how to achieve the highest possible activity and selectivity of the catalysts for CO2 reduction to CO through tuning the coordination environment of the central metal-nitrogen atom and the local carbon structure. This award reflects NSF''s statutory mission and has been deemed worthy of support through evaluation using the Foundation''s intellectual merit and broader impacts review criteria.
