Copper adparticle enabled selective electrosynthesis of n-propanol
Abstract
The electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products; however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation. Density functional theory calculations suggest that copper adparticles increase CO binding energy and stabilize two-carbon intermediates, facilitating coupling between adsorbed *CO and two-carbon intermediates to form three-carbon products. We form adparticle-covered catalysts in-situ by mediating catalyst growth with strong CO chemisorption. The new catalysts exhibit an n-propanol Faradaic efficiency of 23% from CO reduction at an n-propanol partial current density of 11 mA cm(-2).
- Authors:
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- Univ. of Toronto, Toronto, ON (Canada)
- Univ. of Toronto, Toronto, ON (Canada); Tianjin Univ., Tianjin (China)
- Hitachi High Technologies America, Inc., Clarksburg, MD (United States)
- Univ. of Toronto, Toronto, ON (Canada); Delft Univ. of Technology, Delft (The Netherlands)
- McMaster Univ., Hamilton, ON (Canada)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Canadian Light Source Inc., Saskatoon, SK (Canada)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tamkang Univ., Taiwan (Republic of China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Tamkang Univ., Taiwan (Republic of China)
- Tianjin Univ., Tianjin (China)
- Univ. of Western Ontario, London, ON (Canada)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Sciences and Engineering Research Council of Canada (NSERC); Canadian Institute for Advanced Research (CIFAR); University of Toronto; National Research Council (Canada); University of Saskatchewan
- OSTI Identifier:
- 1493275
- Alternate Identifier(s):
- OSTI ID: 1504772
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Li, Jun, Che, Fanglin, Pang, Yuanjie, Zou, Chengqin, Howe, Jane Y., Burdyny, Thomas, Edwards, Jonathan P., Wang, Yuhang, Li, Fengwang, Wang, Ziyun, De Luna, Phil, Dinh, Cao -Thang, Zhuang, Tao -Tao, Saidaminov, Makhsud I., Cheng, Shaobo, Wu, Tianpin, Finfrock, Y. Zou, Ma, Lu, Hsieh, Shang -Hsien, Liu, Yi -Sheng, Botton, Gianluigi A., Pong, Way -Faung, Du, Xiwen, Guo, Jinghua, Sham, Tsun -Kong, Sargent, Edward H., and Sinton, David. Copper adparticle enabled selective electrosynthesis of n-propanol. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-07032-0.
Li, Jun, Che, Fanglin, Pang, Yuanjie, Zou, Chengqin, Howe, Jane Y., Burdyny, Thomas, Edwards, Jonathan P., Wang, Yuhang, Li, Fengwang, Wang, Ziyun, De Luna, Phil, Dinh, Cao -Thang, Zhuang, Tao -Tao, Saidaminov, Makhsud I., Cheng, Shaobo, Wu, Tianpin, Finfrock, Y. Zou, Ma, Lu, Hsieh, Shang -Hsien, Liu, Yi -Sheng, Botton, Gianluigi A., Pong, Way -Faung, Du, Xiwen, Guo, Jinghua, Sham, Tsun -Kong, Sargent, Edward H., & Sinton, David. Copper adparticle enabled selective electrosynthesis of n-propanol. United States. https://doi.org/10.1038/s41467-018-07032-0
Li, Jun, Che, Fanglin, Pang, Yuanjie, Zou, Chengqin, Howe, Jane Y., Burdyny, Thomas, Edwards, Jonathan P., Wang, Yuhang, Li, Fengwang, Wang, Ziyun, De Luna, Phil, Dinh, Cao -Thang, Zhuang, Tao -Tao, Saidaminov, Makhsud I., Cheng, Shaobo, Wu, Tianpin, Finfrock, Y. Zou, Ma, Lu, Hsieh, Shang -Hsien, Liu, Yi -Sheng, Botton, Gianluigi A., Pong, Way -Faung, Du, Xiwen, Guo, Jinghua, Sham, Tsun -Kong, Sargent, Edward H., and Sinton, David. Mon .
"Copper adparticle enabled selective electrosynthesis of n-propanol". United States. https://doi.org/10.1038/s41467-018-07032-0. https://www.osti.gov/servlets/purl/1493275.
@article{osti_1493275,
title = {Copper adparticle enabled selective electrosynthesis of n-propanol},
author = {Li, Jun and Che, Fanglin and Pang, Yuanjie and Zou, Chengqin and Howe, Jane Y. and Burdyny, Thomas and Edwards, Jonathan P. and Wang, Yuhang and Li, Fengwang and Wang, Ziyun and De Luna, Phil and Dinh, Cao -Thang and Zhuang, Tao -Tao and Saidaminov, Makhsud I. and Cheng, Shaobo and Wu, Tianpin and Finfrock, Y. Zou and Ma, Lu and Hsieh, Shang -Hsien and Liu, Yi -Sheng and Botton, Gianluigi A. and Pong, Way -Faung and Du, Xiwen and Guo, Jinghua and Sham, Tsun -Kong and Sargent, Edward H. and Sinton, David},
abstractNote = {The electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products; however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation. Density functional theory calculations suggest that copper adparticles increase CO binding energy and stabilize two-carbon intermediates, facilitating coupling between adsorbed *CO and two-carbon intermediates to form three-carbon products. We form adparticle-covered catalysts in-situ by mediating catalyst growth with strong CO chemisorption. The new catalysts exhibit an n-propanol Faradaic efficiency of 23% from CO reduction at an n-propanol partial current density of 11 mA cm(-2).},
doi = {10.1038/s41467-018-07032-0},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Mon Nov 05 00:00:00 EST 2018},
month = {Mon Nov 05 00:00:00 EST 2018}
}
Web of Science
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