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

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. Furthermore, 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.

Authors:
ORCiD logo; ; ; ; ; ; ; ORCiD logo; ; ;
Publication Date:
Research Org.:
Univ. of Central Florida Research Foundation, Orlando, FL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1310260
Alternate Identifier(s):
OSTI ID: 1336136
Report Number(s):
BNL-112610-2016-JA
Journal ID: ISSN 2041-1723; ncomms12123
Grant/Contract Number:  
FG02-08ER15995; SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; Catalysis; plasma processing; ethylene; carbon dioxide; Center for Functional Nanomaterials

Citation Formats

Mistry, Hemma, Varela, Ana Sofia, Bonifacio, Cecile S., Zegkinoglou, Ioannis, Sinev, Ilya, Choi, Yong-Wook, Kisslinger, Kim, Stach, Eric A., Yang, Judith C., Strasser, Peter, and Cuenya, Beatriz Roldan. Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene. United States: N. p., 2016. Web. doi:10.1038/ncomms12123.
Mistry, Hemma, Varela, Ana Sofia, Bonifacio, Cecile S., Zegkinoglou, Ioannis, Sinev, Ilya, Choi, Yong-Wook, Kisslinger, Kim, Stach, Eric A., Yang, Judith C., Strasser, Peter, & Cuenya, Beatriz Roldan. Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene. United States. doi:10.1038/ncomms12123.
Mistry, Hemma, Varela, Ana Sofia, Bonifacio, Cecile S., Zegkinoglou, Ioannis, Sinev, Ilya, Choi, Yong-Wook, Kisslinger, Kim, Stach, Eric A., Yang, Judith C., Strasser, Peter, and Cuenya, Beatriz Roldan. Thu . "Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene". United States. doi:10.1038/ncomms12123. https://www.osti.gov/servlets/purl/1310260.
@article{osti_1310260,
title = {Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene},
author = {Mistry, Hemma and Varela, Ana Sofia and Bonifacio, Cecile S. and Zegkinoglou, Ioannis and Sinev, Ilya and Choi, Yong-Wook and Kisslinger, Kim and Stach, Eric A. and Yang, Judith C. and Strasser, Peter and Cuenya, Beatriz Roldan},
abstractNote = {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. Furthermore, 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.},
doi = {10.1038/ncomms12123},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {6}
}

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    Works referencing / citing this record:

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