Pressure-induced generation of heterogeneous electrocatalytic metal hydride surfaces for sustainable hydrogen transfer.

Autor: Luo L; School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China.; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China., Liu X; Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China., Zhao X; School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China.; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China., Zhang X; School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China.; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China., Peng HJ; Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China.; Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, 313001, Huzhou, Zhejiang, P. R. China., Ye K; Interdisciplinary Research Center, Institute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, 200240, Shanghai, P. R. China., Jiang K; Interdisciplinary Research Center, Institute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, 200240, Shanghai, P. R. China., Jiang Q; School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China., Zeng J; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, 230026, Hefei, Anhui, P. R. China.; School of Chemistry & Chemical Engineering, Anhui University of Technology, 243002, Ma'anshan, Anhui, P. R. China., Zheng T; School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China., Xia C; School of Materials and Energy, University of Electronic Science and Technology of China, 611731, Chengdu, P. R. China. chuan.xia@uestc.edu.cn.; Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, 313001, Huzhou, Zhejiang, P. R. China. chuan.xia@uestc.edu.cn.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2024 Sep 08; Vol. 15 (1), pp. 7845. Date of Electronic Publication: 2024 Sep 08.
DOI: 10.1038/s41467-024-52228-2
Abstrakt: Metal hydrides are crucial intermediates in numerous catalytic reactions. Intensive efforts have been dedicated to constructing molecular metal hydrides, where toxic precursors and delicate mediators are usually involved. Herein, we demonstrate a facile pressure-induced methodology to generate a cost-effective heterogeneous electrocatalytic metal hydride surface for sustainable hydrogen transfer. Taking carbon dioxide (CO 2 ) electroreduction as a model system and zinc (Zn), a well-known carbon monoxide (CO)-selective catalyst, as a model catalyst, we showcase a homogeneous-type hydrogen atom transfer process induced by heterogeneous hydride surfaces, enabling direct hydrogenation pathways traditionally considered "prohibited". Specifically, the maximal Faradaic efficiency for formate is enhanced by ~fivefold to 83% under ambient conditions. Experimental and theoretical analyses reveal that unlike the distal hydrogenation route for CO 2 to CO over pristine Zn, the Zn hydride surface enables direct hydrogenation at the carbon site of CO 2 to form formate. This work provides a promising material platform for sustainable synthesis.
(© 2024. The Author(s).)
Databáze: MEDLINE
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