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. Here, 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. Therein 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. These 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:
- Publication Date:
- Research Org.:
- Univ. of Central Florida Research Foundation, Orlando, FL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- 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. https://doi.org/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. https://doi.org/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. Here, 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. Therein 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. These 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 = {Thu Jun 30 00:00:00 EDT 2016},
month = {Thu Jun 30 00:00:00 EDT 2016}
}
Web of Science
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High efficiency electrochemical reduction of CO 2 beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO 2 nanoparticles
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Cuprous ions embedded in ceria lattice for selective and stable electrochemical reduction of carbon dioxide to ethylene
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Heteroatom-doped carbon materials and their composites as electrocatalysts for CO 2 reduction
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“Hot edges” in an inverse opal structure enable efficient CO 2 electrochemical reduction and sensitive in situ Raman characterization
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Understanding three-dimensionally interconnected porous oxide-derived copper electrocatalyst for selective carbon dioxide reduction
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Current progress in electrocatalytic carbon dioxide reduction to fuels on heterogeneous catalysts
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Application of plasma for efficient H 2 production: A realism of copper electrode in single dielectric barrier discharge reactor
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Full atomistic reaction mechanism with kinetics for CO reduction on Cu(100) from ab initio molecular dynamics free-energy calculations at 298 K
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On the Electrochemical CO 2 Reduction at Copper Sheet Electrodes with Enhanced Long-Term Stability by Pulsed Electrolysis
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A Review of Metal- and Metal-Oxide-Based Heterogeneous Catalysts for Electroreduction of Carbon Dioxide
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Cu 2 O Nanoparticles with Both {100} and {111} Facets for Enhancing the Selectivity and Activity of CO 2 Electroreduction to Ethylene
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Atomic‐Scale Spacing between Copper Facets for the Electrochemical Reduction of Carbon Dioxide
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In-Situ Nanostructuring and Stabilization of Polycrystalline Copper by an Organic Salt Additive Promotes Electrocatalytic CO 2 Reduction to Ethylene
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Insights into Carbon Dioxide Electroreduction in Ionic Liquids: Carbon Dioxide Activation and Selectivity Tailored by Ionic Microhabitat
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Synergistic enhancement of electrocatalytic CO2 reduction to C2 oxygenates at nitrogen-doped nanodiamonds/Cu interface
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Sequential catalysis enables enhanced C–C coupling towards multi-carbon alkenes and alcohols in carbon dioxide reduction: a study on bifunctional Cu/Au electrocatalysts
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Nitride-Derived Copper Modified with Indium as a Selective and Highly Stable Catalyst for the Electroreduction of Carbon Dioxide
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Amorphizing of Cu Nanoparticles toward Highly Efficient and Robust Electrocatalyst for CO 2 Reduction to Liquid Fuels with High Faradaic Efficiencies
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The p‐Orbital Delocalization of Main‐Group Metals to Boost CO 2 Electroreduction
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Dynamic Changes in the Structure, Chemical State and Catalytic Selectivity of Cu Nanocubes during CO 2 Electroreduction: Size and Support Effects
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Morphological and Compositional Design of Pd-Cu Bimetallic Nanocatalysts with Controllable Product Selectivity toward CO 2 Electroreduction
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