材料科学
电化学
法拉第效率
催化作用
二氧化碳电化学还原
拉曼光谱
密度泛函理论
选择性
化学工程
电流密度
氧化还原
原位
碳纤维
无机化学
电极
纳米技术
物理化学
一氧化碳
化学
有机化学
计算化学
冶金
工程类
物理
量子力学
复合材料
复合数
光学
作者
Lixia Liu,Yanming Cai,Huitong Du,Xuanzhao Lu,Xiang Li,Fuqiang Liu,Jiaju Fu,Jun‐Jie Zhu
标识
DOI:10.1021/acsami.2c21902
摘要
The electrochemical carbon-dioxide reduction reaction (CO2RR) to high-value multi-carbon (C2+) chemicals provides a hopeful approach to store renewable energy and close the carbon cycle. Although copper-based catalysts with a porous architecture are considered potential electrocatalysts for CO2 reduction to C2+ chemicals, challenges remain in achieving high selectivity and partial current density simultaneously for practical application. Here, the porous Cu catalysts with a cavity structure by in situ electrochemical-reducing Cu2O cavities are developed for high-performance conversion of CO2 to C2+ fuels. The as-described catalysts exhibit a high C2+ Faradaic efficiency and partial current density of 75.6 ± 1.8% and 605 ± 14 mA cm-2, respectively, at a low applied potential (-0.59 V vs RHE) in a microfluidic flow cell. Furthermore, in situ Raman tests and finite element simulation indicated that the cavity structure can enrich the local concentration of CO intermediates, thus promoting the C-C coupling process. More importantly, the C-C coupling should be major through the *CO-*CHO pathway as demonstrated by the electrochemical Raman spectra and density functional theory calculations. This work can provide ideas and insights into designing high-performance electrocatalysts for producing C2+ compounds and highlight the important effect of in situ characterization for uncovering the reaction mechanism.
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