铜
法拉第效率
硼
电极
价(化学)
吸附
材料科学
可逆氢电极
无机化学
氢
化学
分析化学(期刊)
冶金
电化学
工作电极
有机化学
物理化学
色谱法
作者
Gangfeng Wu,Chang Zhu,Jianing Mao,Guihua Li,Shoujie Li,Xiao Dong,Aohui Chen,Yanfang Song,Guanghui Feng,Xiaohu Liu,Yiheng Wei,Jiangjiang Wang,Wei Wei,Wei Chen
出处
期刊:ACS energy letters
[American Chemical Society]
日期:2023-10-25
卷期号:8 (11): 4867-4874
被引量:42
标识
DOI:10.1021/acsenergylett.3c01901
摘要
Partial positive valence Cu (Cu δ+ ) sites on Cu-based electrocatalysts are important for C–C coupling to form C 2+ products; however, maintaining the stability of Cu δ+ remains a challenge. Herein, an ultrastable Cu δ+ (0 < δ < 1) site over the copper penetration electrode was constructed using boron to tailor the *CO adsorption strength and configuration for facilitating C–C coupling, which achieves a C 2+ Faradaic efficiency (FE) of 78.9% at −0.91 V (vs reversible hydrogen electrode), of which the ethanol FE reaches 52.4% with an ultrahigh partial current density of 1.25 A cm –2, far outperforming state-of-the-art electrocatalysts, corresponding to the ethanol cathodic energy efficiency (CEE) of 27.7%. Spectroscopy and computation results show that introducing boron to optimize the coordination numbers and oxidation states of surface Cu atoms enables enrichment of locally asymmetric *CO atop and *CHO intermediates to trigger asymmetric C–C coupling to form ethanol.
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