催化作用
电化学
吸附
密度泛函理论
拉曼光谱
金属
化学
法拉第效率
过渡金属
多孔性
氧化还原
材料科学
无机化学
化学工程
物理化学
电极
计算化学
冶金
光学
物理
工程类
复合材料
生物化学
作者
Jiaqi Sang,Pengfei Wei,Tianfu Liu,Houfu Lv,Xingming Ni,Dunfeng Gao,Jiangwei Zhang,Hefei Li,Yipeng Zang,Fan Yang,Zhi Liu,Guoxiong Wang,Xinhe Bao
标识
DOI:10.1002/anie.202114238
摘要
The electrochemical CO2 reduction reaction (CO2 RR) over Cu-based catalysts shows great potential for converting CO2 into multicarbon (C2+ ) fuels and chemicals. Herein, we introduce an A2 M2 O7 structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu2 P2 O7 catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO2 RR conditions. The reconstructed Cu2 P2 O7 catalyst achieves a Faradaic efficiency of 73.6 % for C2+ products at an applied current density of 350 mA cm-2 , remarkably higher than the CuO counterparts. The reconstructed Cu2 P2 O7 catalyst has a high electrochemically active surface area, abundant defects, and low-coordinated sites. In situ Raman spectroscopy and density functional theory calculations reveal that CO adsorption with bridge and atop configurations is largely improved on Cu with defects and low-coordinated sites, which decreased the energy barrier of the C-C coupling reaction for C2+ products.
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