Gold-in-copper at low *CO coverage enables efficient electromethanation of CO2

Xue Wang, Pengfei Ou, Joshua Wicks, Yi Xie, Ying Wang, Jun Li, Jason Tam, Dan Ren, Jane Y. Howe, Ziyun Wang, Adnan Ozden, Y. Zou Finfrock, Yi Xu, Yuhang Li, Armin Sedighian Rasouli, Koen Bertens, Alexander H. Ip, Michael Graetzel, David Sinton and Edward H. Sargent ()
Additional contact information
Xue Wang: University of Toronto
Pengfei Ou: University of Toronto
Joshua Wicks: University of Toronto
Yi Xie: The Chinese University of Hong Kong
Ying Wang: The Chinese University of Hong Kong
Jun Li: École Polytechnique Fédérale de Lausanne
Jason Tam: University of Toronto
Dan Ren: École Polytechnique Fédérale de Lausanne
Jane Y. Howe: University of Toronto
Ziyun Wang: University of Toronto
Adnan Ozden: University of Toronto
Y. Zou Finfrock: Canadian Light Source
Yi Xu: University of Toronto
Yuhang Li: University of Toronto
Armin Sedighian Rasouli: University of Toronto
Koen Bertens: University of Toronto
Alexander H. Ip: University of Toronto
Michael Graetzel: École Polytechnique Fédérale de Lausanne
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: Abstract The renewable-electricity-powered CO2 electroreduction reaction provides a promising means to store intermittent renewable energy in the form of valuable chemicals and dispatchable fuels. Renewable methane produced using CO2 electroreduction attracts interest due to the established global distribution network; however, present-day efficiencies and activities remain below those required for practical application. Here we exploit the fact that the suppression of *CO dimerization and hydrogen evolution promotes methane selectivity: we reason that the introduction of Au in Cu favors *CO protonation vs. C−C coupling under low *CO coverage and weakens the *H adsorption energy of the surface, leading to a reduction in hydrogen evolution. We construct experimentally a suite of Au-Cu catalysts and control *CO availability by regulating CO2 concentration and reaction rate. This strategy leads to a 1.6× improvement in the methane:H2 selectivity ratio compared to the best prior reports operating above 100 mA cm−2. We as a result achieve a CO2-to-methane Faradaic efficiency (FE) of (56 ± 2)% at a production rate of (112 ± 4) mA cm−2.

Date: 2021
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DOI: 10.1038/s41467-021-23699-4

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