A Reconstructed Cu2P2O7 Catalyst for Selective CO2 Electroreduction to Multicarbon Products

被引:130
作者
Sang, Jiaqi [1 ,2 ]
Wei, Pengfei [1 ,2 ]
Liu, Tianfu [1 ]
Lv, Houfu [1 ]
Ni, Xingming [3 ]
Gao, Dunfeng [1 ]
Zhang, Jiangwei [1 ]
Li, Hefei [1 ,2 ]
Zang, Yipeng [1 ]
Yang, Fan [3 ]
Liu, Zhi [3 ]
Wang, Guoxiong [1 ]
Bao, Xinhe [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100039, Peoples R China
[3] Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
基金
国家重点研发计划; 中国博士后科学基金; 中国国家自然科学基金;
关键词
CO2; electroreduction; Cu2P2O7; Electrochemical in situ reconstruction; Multicarbon products; REDUCTION; EFFICIENCY; ELECTRODES; MECHANISM; COVERAGE; STATE;
D O I
10.1002/anie.202114238
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The electrochemical CO2 reduction reaction (CO2RR) over Cu-based catalysts shows great potential for converting CO2 into multicarbon (C2+) fuels and chemicals. Herein, we introduce an A(2)M(2)O(7) structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu2P2O7 catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO2RR conditions. The reconstructed Cu2P2O7 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 Cu2P2O7 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.
引用
收藏
页数:7
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