化学
催化作用
吸附
离解(化学)
路易斯酸
无机化学
密度泛函理论
兴奋剂
选择性
协同催化
联轴节(管道)
组合化学
布朗斯特德-洛瑞酸碱理论
多相催化
拉曼光谱
电化学
化学工程
过渡金属
光化学
作者
Jiahao Wang,Hu Zang,Xin Liu,Changjiang Liu,Haiyan Lu,Nan Yu,Baoyou Geng
出处
期刊:Inorganic Chemistry
[American Chemical Society]
日期:2024-09-21
卷期号:63 (40): 18892-18901
被引量:8
标识
DOI:10.1021/acs.inorgchem.4c03122
摘要
The electroreduction of CO2 to valuable fuels or high-value chemicals by using sustainable electric energy provides a promising strategy for solving environmental problems dominated by the greenhouse effect. Copper-based materials are the only catalysts that can convert CO2 into multicarbon products, but they are plagued by high potential, low selectivity, and poor stability. The key factors to optimize the conversion of CO2 into multicarbon products are to improve the adsorption capacity of intermediates on the catalyst surface, accelerate the hydrogenation step, and improve the C-C coupling efficiency. Herein, we successfully doped Lewis acid Mg into Cu-based materials using a simple liquid-phase chemical method. In situ Raman and FT-IR tracking show that the Mg site enhances the surface coverage of the *CO intermediate, simultaneously promoting water dissociation. Under an industrial current density of 0.7 A cm-2, the FEC2+ reaches 73.9 ± 3.48% with remarkable stability. Density functional theory studies show that doping the Lewis acid Mg site increases the coverage of *CO and accelerates the splitting of water, thus promoting the C-C coupling efficiency, reducing the reaction energy barrier, and greatly improving the selectivity of C2+ products.
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