材料科学
介孔材料
路易斯酸
兴奋剂
基础(拓扑)
纳米技术
催化作用
化学工程
结晶学
光电子学
有机化学
化学
数学分析
数学
工程类
作者
Jiahao Wang,Qinyuan Ji,Hu Zang,Yan Zhang,Changjiang Liu,Nan Yu,Baoyou Geng
标识
DOI:10.1002/adfm.202404274
摘要
Abstract Electroreduction of CO 2 into high‐value chemicals and fuels driven is an effective way to alleviate the environmental crisis, but it suffers from poor activity and low selectivity of the catalyst. Single‐atom catalysts have excellent selectivity and the highest atomic efficiency, and are widely used in the 2‐electron transfer to produce CO. However, electroreduction of CO 2 to C 2+ products involves complex processes such as multi‐electron reaction and competitive adsorption, so single‐atom catalysis is often powerless. Herein, a single‐atom Ga‐anchored F‐doped Cu 2 O catalyst with dual active sites is reported. The Lewis acid‐base pairs and Ga single atom sites promote the adsorption/activation of CO 2 and the dissociation of water molecules, respectively, enhance the coverage of *CO and *H, and their synergy optimizes the reaction path. At a high current density of 600 mA cm −2 , the FE C2+ reached 72.8 ± 3.2% with remarkable stability. Experiments and theory calculations demonstrate that the dual sites increase the coverage of *CO and *H, and the key intermediate *CO is transformed into *CHO through protonation reaction, which changes the reaction path from the C─C coupling (*OCCO) to the protonation followed by C─C coupling (*OCCHO) with low energy barrier, greatly improving the selectivity for C 2+ products.
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