材料科学
质子化
介孔材料
选择性
路易斯酸
兴奋剂
离解(化学)
吸附
Atom(片上系统)
密度泛函理论
电子转移
分子
催化作用
物理化学
无机化学
计算化学
光电子学
离子
有机化学
化学
计算机科学
嵌入式系统
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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