Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene

被引:1090
作者
Mistry, Hemma [1 ,2 ]
Varela, Ana Sofia [3 ]
Bonifacio, Cecile S. [4 ]
Zegkinoglou, Ioannis [2 ]
Sinev, Ilya [2 ]
Choi, Yong-Wook [2 ]
Kisslinger, Kim [5 ]
Stach, Eric A. [5 ]
Yang, Judith C. [4 ]
Strasser, Peter [3 ]
Roldan Cuenya, Beatriz [2 ]
机构
[1] Univ Cent Florida, Dept Phys, Orlando, FL 32816 USA
[2] Ruhr Univ Bochum, Dept Phys, D-44780 Bochum, Germany
[3] Tech Univ Berlin, Div Chem Engn, Dept Chem, D-10623 Berlin, Germany
[4] Univ Pittsburgh, Chem & Petr Engn & Phys, Pittsburgh, PA 15261 USA
[5] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA
基金
美国国家科学基金会;
关键词
ELECTROCHEMICAL REDUCTION; CO2; REDUCTION; TIN ELECTRODES; ELECTROREDUCTION; HYDROCARBONS; INSIGHTS; SIZE; ELECTROCATALYSTS; NANOPARTICLES;
D O I
10.1038/ncomms12123
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
There is an urgent need to develop technologies that use renewable energy to convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon dioxide can be electrochemically reduced to hydrocarbons over copper catalysts, although higher efficiency is required. We have developed oxidized copper catalysts displaying lower overpotentials for carbon dioxide electroreduction and record selectivity towards ethylene (60%) through facile and tunable plasma treatments. Herein we provide insight into the improved performance of these catalysts by combining electrochemical measurements with microscopic and spectroscopic characterization techniques. Operando X-ray absorption spectroscopy and cross-sectional scanning transmission electron microscopy show that copper oxides are surprisingly resistant to reduction and copper(+) species remain on the surface during the reaction. Our results demonstrate that the roughness of oxide-derived copper catalysts plays only a partial role in determining the catalytic performance, while the presence of copper(+) is key for lowering the onset potential and enhancing ethylene selectivity.
引用
收藏
页数:8
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