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Title: 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:
ORCiD logo [1];  [1];  [1];  [2];  [3]; ORCiD logo [4];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1];  [5];  [6];  [7]; ORCiD logo [6]; ORCiD logo [8]; ORCiD logo [9] more »; ORCiD logo [5];  [10];  [11]; ORCiD logo [9];  [12]; ORCiD logo [1]; ORCiD logo [1] « less
+ Show Author Affiliations
  1. Univ. of Toronto, Toronto, ON (Canada)
  2. Univ. of Toronto, Toronto, ON (Canada); Tianjin Univ., Tianjin (China)
  3. Hitachi High Technologies America, Inc., Clarksburg, MD (United States)
  4. Univ. of Toronto, Toronto, ON (Canada); Delft Univ. of Technology, Delft (The Netherlands)
  5. McMaster Univ., Hamilton, ON (Canada)
  6. Argonne National Lab. (ANL), Lemont, IL (United States)
  7. Argonne National Lab. (ANL), Lemont, IL (United States); Canadian Light Source Inc., Saskatoon, SK (Canada)
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tamkang Univ., Taiwan (Republic of China)
  9. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  10. Tamkang Univ., Taiwan (Republic of China)
  11. Tianjin Univ., Tianjin (China)
  12. 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.
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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
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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.
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@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}
}
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https://doi.org/10.1038/s41467-018-07032-0
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Figures / Tables:

Fig. 1 Fig. 1: DFT calculations of Cu adparticle effects on CO-RR. a Demonstration of various low-coordinated Cu sites (CN: coordination number) by adding different number of Cu adatoms (ADs) on various Cu slabs. b The adsorption energy of CO. c The reaction energies of *CO dimerization. d, e CO–C2 (i.e., *OCCOH,more » *CCH2) on various modified Cu surfaces (i.e., (111), (100), (211)) in the presence and absence of Cu adparticles« less
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Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction
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Chemical storage of renewable energy
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    • Green Chemistry, Vol. 22, Issue 1
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    • CHIMIA International Journal for Chemistry, Vol. 65, Issue 5
    • DOI: 10.2533/chimia.2011.303

    Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen
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