电催化剂
催化作用
热液循环
价(化学)
化学
选择性
傅里叶变换红外光谱
化学工程
材料科学
无机化学
纳米技术
电化学
电极
物理化学
有机化学
工程类
作者
Huan Liu,Cheng‐Han Yang,Tong Bian,Huijun Yu,Yuming Zhou,Yiwei Zhang
标识
DOI:10.1002/anie.202404123
摘要
One challenge confronting the Cu2O catalysts in the electrocatalysis of carbon dioxide reduction reaction (CO2RR) is the reduction of active Cu(I) species, resulting in low selectivity and quick deactivation. In this study, we for the first time introduce a bottom‐up growth of convex sphere with adjustable Cu(0)/Cu(I) interfaces (Cux@Cu2O convex spheres). Interestingly, the interfaces are dynamically modulated by varying hydrothermal time, thus regulating the conversion of C1 and C2 products. In particular, the 4 h hydrothermal treatment applied to Cu0.25@Cu2O convex sphere with the favorable Cu(0)/Cu(I) interface results in the highest selectivity for C2 products (90.5%). In situ Fourier‐transform infrared spectroscopy measurements and density functional theory calculations reveal that the Cu(0)/Cu(I) interface lowers the energy barrier for the production of ethylene and ethanol while increasing the coverage of localized *CO adsorbate for increased dimerization. This work establishes a novel approach for transforming the state of valence‐sensitive electrocatalysts into high‐value energy‐related engineering products.
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