Proceedings of nanoGe September Meeting 2017 (NFM17)
Publication date: 20th June 2016
The widespread utilization of renewable energy will require energy dense and cost-effective methods for storage. This challenge could be met by using renewable electricity to drive the reduction of carbon dioxide to energy dense carbonaceous fuels. However, many fuels are accessible over a narrow range in electrochemical potential, requiring a detailed mechanistic understanding of the key factors that control kinetic branching in these reactions. Using in situ surface-enhanced infrared reflection absorption spectrcopy, we have measured the adsorption isotherms of carbon monoxide on Cu and Au surfaces , revealing how the dynamics of this common intermediate gate the formation of higher order fuel products. Using complementary electrochemical kinetic studies, we have uncovered the disparate proton coupling requirements for hydrogen evolution relative to carbon dioxide reduction and we have applied this understanding to systematically tune product distribution in CO2-to-fuels catalysis by varying the mesostructure of the catalyst. Our latest mechanistic findings in this area will be discussed.