Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products

Jiaqi Feng, Libing Zhang, Shoujie Liu, Liang Xu, Xiaodong Ma, Xingxing Tan, Limin Wu, Qingli Qian, Tianbin Wu, Jianling Zhang, Xiaofu Sun () and Buxing Han ()
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Jiaqi Feng: Chinese Academy of Sciences
Libing Zhang: Chinese Academy of Sciences
Shoujie Liu: Anhui University
Liang Xu: Chinese Academy of Sciences
Xiaodong Ma: Chinese Academy of Sciences
Xingxing Tan: Chinese Academy of Sciences
Limin Wu: Chinese Academy of Sciences
Qingli Qian: Chinese Academy of Sciences
Tianbin Wu: Chinese Academy of Sciences
Jianling Zhang: Chinese Academy of Sciences
Xiaofu Sun: Chinese Academy of Sciences
Buxing Han: Chinese Academy of Sciences

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Electrocatalytic CO2 reduction is a typical reaction involving two reactants (CO2 and H2O). However, the role of H2O dissociation, which provides active *H species to multiple protonation steps, is usually overlooked. Herein, we construct a dual-active sites catalyst comprising atomic Cu sites and Cu nanoparticles supported on N-doped carbon matrix. Efficient electrosynthesis of multi-carbon products is achieved with Faradaic efficiency approaching 75.4% with a partial current density of 289.2 mA cm−2 at −0.6 V. Experimental and theoretical studies reveal that Cu nanoparticles facilitate the C-C coupling step through *CHO dimerization, while the atomic Cu sites boost H2O dissociation to form *H. The generated *H migrate to Cu nanoparticles and modulate the *H coverage on Cu NPs, and thus promote *CO-to-*CHO. The dual-active sites effect of Cu single-sites and Cu nanoparticles gives rise to the catalytic performance.

Date: 2023
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DOI: 10.1038/s41467-023-40412-9

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