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构建用于高效中性CO电还原为CH₄的Ag/CuO界面

Constructing Ag/CuO Interface for Efficient Neutral CO Electroreduction to CH.

作者信息

Wei Zongnan, Wang Wenwen, Shao Tao, Yang Shuaibing, Liu Chang, Si Duanhui, Cao Rong, Cao Minna

机构信息

Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, P.R. China.

出版信息

Angew Chem Int Ed Engl. 2025 Jan 21;64(4):e202417066. doi: 10.1002/anie.202417066. Epub 2024 Nov 14.

Abstract

Neutral CO electroreduction to multi-carbons (C) offers a promising pathway to reduce the CO and energy losses originating from the carbonate formation. However, the sluggish kinetics of C-C coupling brings a significant challenge of achieving high selectivity of a single product (such as ethylene), especially at industrial-relevant current densities (>300 mA cm). Here, we reported an optimized Ag-CuO interfacial catalyst that exhibited C Faradaic efficiency (FE) of 73.6 % at 650 mA cm in a flow cell. Remarkably, it obtained FE of 66.0 % with a partial current density of 429.1 mA cm, making it stand out among the reported Cu-based electrocatalysts. In situ Raman spectra uncovered that the Ag/CuO interfaces enabled a high coverage of *CO around the partially reduced Cu/Cu active sites. Furthermore, theoretical calculations demonstrated the enhanced CO formation and C-C coupling at the Ag/CuO interface. This work reported an unprecedented neutral CO electroreduction to CH performance and provided an in-depth comprehension of the role of the bimetallic interface.

摘要

中性条件下将一氧化碳(CO)电还原为多碳产物(C)为减少因碳酸盐形成导致的CO和能量损失提供了一条有前景的途径。然而,C-C偶联的缓慢动力学给实现单一产物(如乙烯)的高选择性带来了重大挑战,尤其是在与工业相关的电流密度(>300 mA cm)下。在此,我们报道了一种优化的Ag-CuO界面催化剂,在流动池中,该催化剂在650 mA cm下表现出73.6%的C法拉第效率(FE)。值得注意的是,其在429.1 mA cm的分电流密度下获得了66.0%的FE,使其在已报道的铜基电催化剂中脱颖而出。原位拉曼光谱揭示,Ag/CuO界面在部分还原的Cu/Cu活性位点周围实现了*CO的高覆盖。此外,理论计算表明Ag/CuO界面处的CO形成和C-C偶联得到了增强。这项工作报道了前所未有的中性条件下CO电还原为CH的性能,并深入理解了双金属界面的作用。

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