Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts

被引：194

作者：

Mistry, Hemma ^{[1
,2
]}

Choi, Yong-Wook ^{[1
]}

Bagger, Alexander ^{[3
]}

Scholten, Fabian ^{[1
]}

Bonifacio, Cecile S. ^{[4
]}

Sinev, Ilya ^{[1
]}

Divins, Nuria J. ^{[1
]}

Zegkinoglou, Ioannis ^{[1
]}

Jeon, Hyo Sang ^{[1
]}

Kisslinger, Kim ^{[5
]}

Stach, Eric A. ^{[5
]}

Yang, Judith C. ^{[4
]}

Rossmeisl, Jan ^{[3
]}

Roldan Cuenya, Beatriz ^{[1
,6
]}

机构：

[1] Ruhr Univ Bochum, Dept Phys, D-44780 Bochum, Germany

[2] Univ Cent Florida, Dept Phys, Orlando, FL 32816 USA

[3] Univ Copenhagen, Dept Chem, Copenhagen, Denmark

[4] Univ Pittsburgh, Chem & Petr Engn & Phys, Pittsburgh, PA 15261 USA

[5] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA

[6] Fritz Haber Inst Max Planck Soc, Dept Interface Sci, D-14195 Berlin, Germany

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2017年 / 56卷 / 38期

基金：

美国国家科学基金会; 欧洲研究理事会;

关键词：

CO2; reduction; electrocatalysis; nanostructures; silver; CO2; REDUCTION; ELECTROCHEMICAL REDUCTION; AU NANOPARTICLES; ELECTRODES; ELECTROCATALYSTS; INSIGHTS; SURFACES;

D O I：

10.1002/anie.201704613

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Efficient, stable catalysts with high selectivity for a single product are essential if electroreduction of CO2 is to become a viable route to the synthesis of industrial feedstocks and fuels. A plasma oxidation pre-treatment of silver foil enhances the number of low-coordinated catalytically active sites, which dramatically lowers the overpotential and increases the activity of CO2 electroreduction to CO. At -0.6 V versus RHE more than 90% Faradaic efficiency towards CO was achieved on a pre-oxidized silver foil. While transmission electron microscopy (TEM) and operando X-ray absorption spectroscopy showed that oxygen species can survive in the bulk of the catalyst during the reaction, quasi in situ X-ray photoelectron spectroscopy showed that the surface is metallic under reaction conditions. DFT calculations reveal that the defect-rich surface of the plasma-oxidized silver foils in the presence of local electric fields drastically decrease the overpotential of CO2 electroreduction.

引用

页码：11394 / 11398

页数：5

共 31 条

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