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

Hemma Mistry, Ana Sofia Varela, Cecile S. Bonifacio, Ioannis Zegkinoglou, Ilya Sinev, Yong-Wook Choi, Kim Kisslinger, Eric A. Stach, Judith C. Yang, Peter Strasser and Beatriz Roldan Cuenya ()
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Hemma Mistry: University of Central Florida
Ana Sofia Varela: Technical University Berlin
Cecile S. Bonifacio: Chemical and Petroleum Engineering and Physics, University of Pittsburgh
Ioannis Zegkinoglou: Ruhr-University Bochum
Ilya Sinev: Ruhr-University Bochum
Yong-Wook Choi: Ruhr-University Bochum
Kim Kisslinger: Center for Functional Nanomaterials, Brookhaven National Laboratory
Eric A. Stach: Center for Functional Nanomaterials, Brookhaven National Laboratory
Judith C. Yang: Chemical and Petroleum Engineering and Physics, University of Pittsburgh
Peter Strasser: Technical University Berlin
Beatriz Roldan Cuenya: Ruhr-University Bochum

Nature Communications, 2016, vol. 7, issue 1, 1-9

Abstract: Abstract 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.

Date: 2016
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DOI: 10.1038/ncomms12123

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