Metal-Organic Layers Leading to Atomically Thin Bismuthene for Efficient Carbon Dioxide Electroreduction to Liquid Fuel

被引:371
作者
Cao, Changsheng [1 ,2 ]
Ma, Dong-Dong [1 ]
Gu, Jia-Fang [3 ]
Xie, Xiuyuan [1 ]
Zeng, Guang [1 ]
Li, Xiaofang [1 ]
Han, Shu-Guo [1 ,2 ]
Zhu, Qi-Long [1 ]
Wu, Xin-Tao [1 ]
Xu, Qiang [4 ,5 ]
机构
[1] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Fuzhou Univ, Dept Chem Engn, Zhicheng Coll, Fuzhou 350002, Peoples R China
[4] Natl Inst Adv Ind Sci & Technol, AIST Kyoto Univ Chem Energy Mat Open Innovat Lab, Sakyo Ku, Kyoto 6068501, Japan
[5] Yangzhou Univ, Sch Chem & Chem Engn, Yangzhou 225009, Jiangsu, Peoples R China
基金
中国国家自然科学基金;
关键词
bismuthene; CO(2)reduction; electrocatalysis; flow cells; metal-organic layers; ELECTROCHEMICAL CO2 REDUCTION; NANOSHEETS; BICARBONATE; SELECTIVITY; FORMATE;
D O I
10.1002/anie.202005577
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical reduction of CO(2)to valuable fuels is appealing for CO(2)fixation and energy storage. However, the development of electrocatalysts with high activity and selectivity in a wide potential window is challenging. Herein, atomically thin bismuthene (Bi-ene) is pioneeringly obtained by an in situ electrochemical transformation from ultrathin bismuth-based metal-organic layers. The few-layer Bi-ene, which possesses a great mass of exposed active sites with high intrinsic activity, has a high selectivity (ca. 100 %), large partial current density, and quite good stability in a potential window exceeding 0.35 V toward formate production. It even deliver current densities that exceed 300.0 mA cm(-2)without compromising selectivity in a flow-cell reactor. Using in situ ATR-IR spectra and DFT analysis, a reaction mechanism involving HCO(3)(-)for formate generation was unveiled, which brings new fundamental understanding of CO(2)reduction.
引用
收藏
页码:15014 / 15020
页数:7
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