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

Wang, Xue; Ou, Pengfei; Wicks, Joshua; Xie, Yi; Wang, Ying; Li, Jun; Tam, Jason; Ren, Dan; Howe, Jane Y.; Wang, Ziyun; Ozden, Adnan; Finfrock, Y. Zou; Xu, Yi; Li, Yuhang; Rasouli, Armin Sedighian; Bertens, Koen; Ip, Alexander H.; Graetzel, Michael; Sinton, David; Sargent, Edward H.

doi:10.1038/s41467-021-23699-4

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

Journal Article · Mon Jun 07 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-23699-4· OSTI ID:1815530

^[1]; ^[2]; ^[2]; Xie, Yi ^[3]; ^[3]; ^[4]; Tam, Jason ^[5]; ^[4]; Howe, Jane Y. ^[5]; ^[2]; Ozden, Adnan ^[6]; Finfrock, Y. Zou ^[7]; ^[6]; ^[2]; Rasouli, Armin Sedighian ^[2]; Bertens, Koen ^[2]; Ip, Alexander H. ^[2]; ^[4]; ^[6]; ^[2]

Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering; OSTI
Univ. of Toronto, ON (Canada). Dept. of Electrical and Computer Engineering
The Chinese Univ. of Hong Kong, Hong Kong, S.A.R. (China). Dept. of Chemistry
Ecole Polytechnique Federale Lausanne (Switzerland). Inst. of Chemical Sciences and Engineering
Univ. of Toronto, ON (Canada). Dept. of Materials Science and Engineering
Univ. of Toronto, ON (Canada). Dept. of Mechanical and Industrial Engineering
Canadian Light Sources, Inc., Saskatoon, SK (Canada); Argonne National Lab. (ANL), Argonne, IL (United States). Photon Science Division

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1815530

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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