Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products

Cheng Du, Joel P. Mills, Asfaw G. Yohannes, Wei Wei, Lei Wang, Siyan Lu, Jian-Xiang Lian, Maoyu Wang, Tao Guo, Xiyang Wang, Hua Zhou, Cheng-Jun Sun, John Z. Wen, Brian Kendall, Martin Couillard, Hongsheng Guo, ZhongChao Tan (), Samira Siahrostami () and Yimin A. Wu ()
Additional contact information
Cheng Du: University of Waterloo
Joel P. Mills: University of Waterloo
Asfaw G. Yohannes: University of Calgary
Wei Wei: University of Waterloo
Lei Wang: University of Waterloo
Siyan Lu: University of Waterloo
Jian-Xiang Lian: University of Calgary
Maoyu Wang: X-Ray Science Division, Argonne National Laboratory
Tao Guo: University of Waterloo
Xiyang Wang: University of Waterloo
Hua Zhou: X-Ray Science Division, Argonne National Laboratory
Cheng-Jun Sun: X-Ray Science Division, Argonne National Laboratory
John Z. Wen: University of Waterloo
Brian Kendall: University of Waterloo
Martin Couillard: National Research Council Canada
Hongsheng Guo: National Research Council Canada
ZhongChao Tan: University of Waterloo
Samira Siahrostami: University of Calgary
Yimin A. Wu: University of Waterloo

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Electrocatalytic CO2 reduction into value-added multicarbon products offers a means to close the anthropogenic carbon cycle using renewable electricity. However, the unsatisfactory catalytic selectivity for multicarbon products severely hinders the practical application of this technology. In this paper, we report a cascade AgCu single-atom and nanoparticle electrocatalyst, in which Ag nanoparticles produce CO and AgCu single-atom alloys promote C-C coupling kinetics. As a result, a Faradaic efficiency (FE) of 94 ± 4% toward multicarbon products is achieved with the as-prepared AgCu single-atom and nanoparticle catalyst under ~720 mA cm−2 working current density at −0.65 V in a flow cell with alkaline electrolyte. Density functional theory calculations further demonstrate that the high multicarbon product selectivity results from cooperation between AgCu single-atom alloys and Ag nanoparticles, wherein the Ag single-atom doping of Cu nanoparticles increases the adsorption energy of *CO on Cu sites due to the asymmetric bonding of the Cu atom to the adjacent Ag atom with a compressive strain.

Date: 2023
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DOI: 10.1038/s41467-023-41871-w

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