CAS: Principles of Cooperativity for the Electrocatalytic Reduction of Carbon Dioxide

点击翻译按钮获取中文摘要

The Chemical Catalysis Program of the Division of Chemistry supports the research program of Professor Craig Grapperhaus and Dr. Joshua Spurgeon of the University of Louisville. This project focuses on the capture and reactivity of carbon dioxide. Generating fuels and chemicals using electricity is one of the most favorable approaches for using intermittent renewables such as wind and solar. Also, making commercial chemicals from electricity may also be more energetically efficient than using current methods which involve heating. This project develops more sustainable systems to capture carbon dioxide and convert it to fuels or other chemical products. The new reactions employ an abundant metal, such as zinc, within a supporting molecular framework synthesized from inexpensive starting materials. The fundamental research could provide a pathway by which renewable electricity and high concentrations carbon dioxide from fossil fuel combustion could be used to form commercially useful materials. The research provides undergraduate and graduate students hands-on interdisciplinary experience in renewable energy research preparing them for careers in science, technology, engineering, and mathematics. High-school student participants in the annual renewable energy workshop at the University of Louisville have the opportunity to participate in the research and develop independent science fair projects.With funding from the Chemical Catalysis Program of the Division of Chemistry, Professor Craig Grapperhaus and Dr. Joshua Spurgeon of the University of Louisville are developing hybrid thiosemicarbazone-pyridylhydrazone metal complexes as co-catalysts for carbon dioxide capture and reduction. The co-catalysts utilize metal-ligand cooperativity through the incorporation of neighboring Lewis acid and Lewis base sites. Reductions will be performed at a variety of electrodes including Cu-Ni alloys. The project will investigate the factors influencing product distribution, reaction mechanism, and reactivity between the co-catalyst and electrode. Projected outcomes include the quantification of the effect of Lewis acidity and Lewis basicity on the binding and catalytic reactivity of carbon dioxide with the metal co-catalyst. The research team will identify of unique C-C coupled products from carbon dioxide reduction at the Cu-Ni alloy and draw mechanistic insights into the C-C coupling process. The group will increase fundamental knowledge of the reactivity of Cu-Ni alloys with varying compositions. High-school student participants in the annual renewable energy workshop at the University of Louisville have the opportunity to participate in the research and develop independent science fair projects.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.