Collaborative Research: CAS-Climate: Structure, Dynamics, and Reaction Mechanism of Supported Single Atom for Photocatalytic CO2 Reduction

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With support from the Chemical Structure, Dynamics & Mechanisms-B (CSDM-B) Program of the Chemistry Division, Jier Huang of the Department of Chemistry at Marquette University and Jing Gu of the Department of Chemistry and Biochemistry at San Diego State University aim to construct and investigate new generation single atom catalysts for visible light driven carbon dioxide (CO2) reduction to form chemical fuels with high efficiency, selectivity, and stability. Photocatalytic CO2 reduction through the harnessing solar energy represents one of the most attractive strategies that attempts to simultaneously address the greenhouse gas sequestration issue and work toward alternative energy sources for the future. The research will be supplemented by diverse educational and outreach activities, including efforts to encourage graduate and undergraduate students, especially members of underrserved minority groups, to consider pursuing careers in science. The Huang/Gu team will also provide opportunities for students/teachers ranging from elementary to high schools to advance their general understanding of catalysis and renewable energy technologies. Supported single atoms (SAs) have emerged as a novel class of catalysts, offering new promise for light-driven CO2 reduction. The focus of prior research is largely on documenting the efficiency, stability, and the selectivity of the catalysts, not the fundamental mechanistic studies that underlines the correlation of SA structure and their photocatalytic performance. To address such gaps in knowledge, Drs. Gu and Professor Huang are targeting the following objectives by leveraging their complementary expertise in materials design and synthesis with time resolved spectroscopy: 1) to systematically tune the geometric and electronic structures of supported SAs by altering the intrinsic nature of SAs, the metal-support interaction, and by comparing with nanoparticles with various sizes; 2) to examine the charge separation and structural dynamics, and resolving the intermediate structures at catalytic active sites with high temporal and spatial resolution using time resolved optical and X-ray absorption spectroscopy; and 3) to evaluate the direct correlation of the structures of the supported SA catalysts with their photophysical properties and catalytic function to establish structure-property-function relationships for CO2 reduction. Results obtained from these efforts are expected to aid in the development of more effective supported SAs for photocatalytic CO2 reduction, going forward.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.