CAS: Nitrogen-Coupled Carbon Dioxide Conversion to Methylamine: Molecular Level Understanding and Tailoring of the Electrocatalysis

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With the support of the Chemical Catalysis program in the Division of Chemistry, Hailiang Wang of Yale University and Julien Panetier of Binghamton University are studying chemical reactions that use renewable electricity to transform carbon dioxide and nitrate, both of which are major environmental pollutants, into methylamine, an organic compound that has widespread applications in chemical synthesis, pharmaceuticals, agriculture, and the aerospace industry. This transformation holds promise for recycling environmental wastes into valuable chemical products under mild conditions. In this project, the team will combine experimental and computational research to systematically study the mechanism of the electrocatalytic reaction. With the guidance of fundamental mechanistic understanding, the team will work to develop more selective and active catalysts, as well as optimize the best catalysts to improve reaction performance toward practical applications. This project will also provide educational opportunities in chemistry, with a focus on catalysis and sustainability, via outreach activities, classroom teaching, and research training to a diverse body of students in STEM (science, technology, engineering and mathematics) fields.Under this award, Hailiang Wang of Yale University and Julien Panetier of Binghamton University are studying the electrochemical co-reduction of carbon dioxide and nitrate in aqueous media to methylamine catalyzed by cobalt phthalocyanine molecules supported on carbon nanotubes. The goal of this project is to understand the catalytic mechanism and improve the reaction performance. The team will combine theoretical calculations, kinetic studies, and in situ vibrational spectroscopy measurements to analyze the reaction mechanism. Selectivity- and rate-limiting steps, as well as their contributing factors, will be identified. Key reaction intermediates and the C-N coupling step will be examined. With guidance from enhanced mechanistic understanding, molecular structure tailoring, nanoscale interactions, and microenvironment tuning will be combined to develop the best catalytic systems for the most efficient and sustainable synthetic processes achievable. This project will also provide educational opportunities in chemistry, with a focus on catalysis and sustainability, via outreach activities, classroom teaching, and research training to a diverse body of students in STEM fields.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.