Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products

• Published in: Nature communications Vol. 14; no. 1; pp. 4615 - 11
• Main Authors: Feng, Jiaqi, Zhang, Libing, Liu, Shoujie, Xu, Liang, Ma, Xiaodong, Tan, Xingxing, Wu, Limin, Qian, Qingli, Wu, Tianbin, Zhang, Jianling, Sun, Xiaofu, Han, Buxing
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01.08.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/131; 140/133; 140/146; 147/137; 147/143; 639/301/299/886; 639/638/224/685; 639/638/224/909; Carbon; Carbon dioxide; Catalysts; Dimerization; Electrochemistry; Humanities and Social Sciences; multidisciplinary; Nanoparticles; Protonation; Science; Science (multidisciplinary)
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-40412-9

Electrocatalytic CO 2 reduction is a typical reaction involving two reactants (CO 2 and H 2 O). However, the role of H 2 O 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 H 2 O 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. A dual-site catalyst consisting of Cu nanoparticles (NPs) and atomic Cu sites is designed. The atomic Cu boosts H2O dissociation for modulating the *H coverage on Cu NPs, improving the efficiency of CO2 electroreduction to multi-carbon products.