Mechanistic Insights Into Selective CO2-to-Fuels Catalysis
Yogesh Surendranath a, Anna Wuttig a, Youngmin Yoon a, Sahr Khan a
a Massachusetts Institute of Technology (MIT), Massachusetts Avenue, 77, Cambridge, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe September Meeting 2017 (NFM17)
SF1: Material and Device Innovations for the Practical Implementation of Solar Fuels (SolarFuel17)
Barcelona, Spain, 2017 September 4th - 9th
Organizers: Wilson Smith and Ki Tae Nam
Invited Speaker, Yogesh Surendranath, presentation 088
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.

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