CAREER: Binuclear Chemistry of Heterogenized Molecular Catalysts in Solar CO2 Reduction

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In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Gonghu Li of the University of New Hampshire is investigating recycling carbon dioxide into chemicals, materials and fuels. However, carbon dioxide is thermodynamically stable, and its conversion often requires high energy. This research project constructs innovative catalytic systems to enable carbon dioxide activation via low-energy pathways, in which two metal centers work together to reduce carbon dioxide into fuels under light irradiation. The low-energy pathways will be investigated using both experimental and theoretical methods. This project will also provide excellent opportunities for educating the current and emerging workforce in energy-related fields to increase the national talent pipeline in clean energy, materials and catalysis science. The broader impacts of this project include the development of efficient and robust catalytic systems for carbon dioxide utilization, which will subsequently reduce dependency on fossil fuels and help to mitigate climate change.Dr. Li is investigating cooperative interactions of surface metal centers in photocatalytic carbon dioxide reduction. In particular, heterogenized molecular catalysts will be synthesized by grafting coordination complexes of Rhenium, Manganese, Nickel and Cobalt onto mesoporous silicas via covalent linkers. The linkers and porous surfaces will be optimized to achieve proper intermolecular distances and geometry. Advanced spectroscopic techniques and density functional theory calculations will be employed to investigate low-energy, binuclear pathways in carbon dioxide reduction using the heterogenized molecular catalysts. The proposed research focuses on fundamental issues in surface chemistry and carbon dioxide -reduction photocatalysis in confined environments. This CAREER award also supports educational activities, including annual solar energy workshops, to effectively disseminated sustainability concepts to K-12 students and the public. The broader impacts of this work include potential societal benefits from the development of innovative catalytic systems for efficient solar energy conversion and sustainable carbon dioxide utilization.