Electrochemical CO Reduction Builds Solvent Water into Oxygenate Products

Journal of the American Chemical Society
Yanwei LumJoel W Ager

Abstract

Numerous studies have examined the electrochemical reduction of CO (COR) to oxygenates (e.g., ethanol). None have considered the possibility that oxygen in the product might arise from water rather than from CO. To test this assumption, C16O reduction was performed in H218O electrolyte. Surprisingly, we found that 60-70% of the ethanol contained 18O, which must have originated from the solvent. We extended our previous all-solvent density functional theory metadynamics calculations to consider the possibility of incorporating water, and indeed, we found a new mechanism involving a Grotthuss chain of six water molecules in a concerted reaction with the *C-CH intermediate to form *CH-CH(18OH), subsequently leading to (18O)ethanol. This competes with the formation of ethylene that also arises from *C-CH. These unforeseen results suggest that all previous studies of COR under aqueous conditions must be reexamined.

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Citations

Aug 25, 2019·Nature Chemistry·Matthew JounyFeng Jiao
Feb 27, 2020·Nature Materials·Dae-Hyun NamEdward H Sargent
Nov 30, 2019·Nature Communications·Xue WangEdward H Sargent
Mar 15, 2019·Proceedings of the National Academy of Sciences of the United States of America·Tao ChengWilliam A Goddard
Oct 23, 2020·Angewandte Chemie·Bjorn HasaFeng Jiao
Jan 1, 2021·Proceedings of the National Academy of Sciences of the United States of America·Peng ZhuHaotian Wang
Apr 30, 2021·Advanced Materials·Yuhang WangGengfeng Zheng
May 28, 2021·Physical Chemistry Chemical Physics : PCCP·Kim R Gustavsen, Kaiying Wang
Jul 10, 2021·Small·Bingxing ZhangWenping Sun
May 24, 2019·Chemical Reviews·Stephanie NitopiIb Chorkendorff
Feb 26, 2019·Journal of the American Chemical Society·Ezra L ClarkAlexis T Bell
May 10, 2019·Journal of the American Chemical Society·Yuguang C LiEdward H Sargent

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