金属间化合物
双金属片
催化作用
选择性
电合成
电解
乙醇
铜
无机化学
密度泛函理论
化学
电化学
物理化学
电解质
电极
有机化学
合金
计算化学
作者
Peng Chen,Jiaxing Ma,Gan Luo,Shuai Yan,Junbo Zhang,Yangshen Chen,Ning Chen,Zhiqiang Wang,Wei Wei,Tsun‐Kong Sham,Yao Zheng,Min Kuang,Gengfeng Zheng
出处
期刊:Angewandte Chemie
[Wiley]
日期:2024-03-04
卷期号:63 (17): e202316907-e202316907
被引量:69
标识
DOI:10.1002/anie.202316907
摘要
The efficient ethanol electrosynthesis from CO2 is challenging with low selectivity at high CO2 electrolysis rates, due to the competition with H2 and other reduction products. Copper-based bimetallic electrocatalysts are potential candidates for the CO2-to-ethanol conversion, but the secondary metal has mainly been focused on active components (such as Ag, Sn) for CO2 electroreduction, which also promote selectivity of ethylene or other reduction products rather than ethanol. Limited attention has been given to alkali-earth metals due to their inherently active chemical property. Herein, we rationally synthesized a (111) facet-oriented nano Cu2Mg (designated as Cu2Mg(111)) intermetallic compound with high-density ordered Cu3-Mg sites. The in situ Raman spectroscopy and density function theory calculations revealed that the Cu3 - δ $_{^{\rm{{\rm \delta} }} }$ --Mg- δ $_{^{\rm{{\rm \delta} }} }$ + active sites allowed to increase *CO surface coverage, decrease reaction energy for *CO-CO coupling, and stabilize *CHCHOH intermediates, thus promoting the ethanol formation pathway. The Cu2Mg(111) catalyst exhibited a high FEC2H5OH of 76.2±4.8 % at 600 mA⋅cm-2, and a peak value of |jC2H5OH| of 720±34 mA⋅cm-2, almost 4 times of that using conventional Cu2Mg with (311) facets, comparable to the best reported values for the CO2-to-ethanol electroreduction.
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