Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products
Abstract
Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti3C2Tx MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at -0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O3 sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.
- Authors:
-
[2];
[1];
[4];
[6];
[1];
[9]
- Tianjin Univ. of Technology, Tianjin (China). Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices
- Univ. of Jinan (China). School of Material Science and Engineering,
- Univ. of Science and Technology, Beijing (China). Dept. of Environmental Engineering
- Tianjin Univ. of Technology, Tianjin (China). Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices; Civil Aviation Univ. of China, Tianjin (China). Key Laboratory of Civil Aviation Thermal Hazards Prevention and Emergency Response
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Xi'an Univ. of Technology, Xi'an, Shanxi (China). School of Materials Science and Engineering
- Lanzhou Univ. of Science and Technology, Lanzhou, Gansu (China). State Key Lab of Advanced Processing and Recycling of Nonferrous Metals
- Chinese Academy of Sciences (CAS), Beijing (China). Institute of Coal Chemistry, State Key Laboratory of Coal Conversion
- Univ. of Electronic Science and Technology of China, Chengdu, Sichuan (China). Institute of Fundamental and Frontier Sciences
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC); Tianjin Science Fund
- OSTI Identifier:
- 1811911
- Grant/Contract Number:
- AC02-76SF00515; 2017YFA0700104; 22075211; 51971157; 51808037; 21601136; 51761165012
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Bao, Haihong, Qiu, Yuan, Peng, Xianyun, Wang, Jia-ao, Mi, Yuying, Zhao, Shunzheng, Liu, Xijun, Liu, Yifan, Cao, Rui, Zhuo, Longchao, Ren, Junqiang, Sun, Jiaqiang, Luo, Jun, and Sun, Xuping. Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products. United States: N. p., 2021.
Web. doi:10.1038/s41467-020-20336-4.
Bao, Haihong, Qiu, Yuan, Peng, Xianyun, Wang, Jia-ao, Mi, Yuying, Zhao, Shunzheng, Liu, Xijun, Liu, Yifan, Cao, Rui, Zhuo, Longchao, Ren, Junqiang, Sun, Jiaqiang, Luo, Jun, & Sun, Xuping. Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products. United States. https://doi.org/10.1038/s41467-020-20336-4
Bao, Haihong, Qiu, Yuan, Peng, Xianyun, Wang, Jia-ao, Mi, Yuying, Zhao, Shunzheng, Liu, Xijun, Liu, Yifan, Cao, Rui, Zhuo, Longchao, Ren, Junqiang, Sun, Jiaqiang, Luo, Jun, and Sun, Xuping. Mon .
"Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products". United States. https://doi.org/10.1038/s41467-020-20336-4. https://www.osti.gov/servlets/purl/1811911.
@article{osti_1811911,
title = {Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products},
author = {Bao, Haihong and Qiu, Yuan and Peng, Xianyun and Wang, Jia-ao and Mi, Yuying and Zhao, Shunzheng and Liu, Xijun and Liu, Yifan and Cao, Rui and Zhuo, Longchao and Ren, Junqiang and Sun, Jiaqiang and Luo, Jun and Sun, Xuping},
abstractNote = {Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti3C2Tx MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at -0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O3 sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.},
doi = {10.1038/s41467-020-20336-4},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United States},
year = {Mon Jan 11 00:00:00 EST 2021},
month = {Mon Jan 11 00:00:00 EST 2021}
}
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