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.

Upgrading wasted carbon emissions to high-value, multi-carbon products provides an economic route to reduce carbon dioxide levels, but such conversions have proven challenging. Here, authors explore copper adparticles as highly active surfaces that convert CO to n-propanol with high selectivities.

Details

Title
Copper adparticle enabled selective electrosynthesis of n-propanol
Author
Li, Jun 1   VIAFID ORCID Logo  ; Che Fanglin 2 ; Pang Yuanjie 1 ; Zou Chengqin 3 ; Howe, Jane Y 4 ; Burdyny, Thomas 5   VIAFID ORCID Logo  ; Edwards, Jonathan P 6 ; Wang, Yuhang 2   VIAFID ORCID Logo  ; Li Fengwang 2   VIAFID ORCID Logo  ; Wang Ziyun 2   VIAFID ORCID Logo  ; De Luna Phil 7   VIAFID ORCID Logo  ; Cao-Thang, Dinh 2 ; Tao-Tao, Zhuang 2 ; Saidaminov, Makhsud I 2 ; Cheng, Shaobo 8 ; Wu Tianpin 9 ; Zou, Finfrock Y 10 ; Lu, Ma 9   VIAFID ORCID Logo  ; Hsieh Shang-Hsien 11   VIAFID ORCID Logo  ; Yi-Sheng, Liu 12   VIAFID ORCID Logo  ; Botton, Gianluigi A 8   VIAFID ORCID Logo  ; Way-Faung, Pong 13 ; Du Xiwen 14 ; Guo Jinghua 12   VIAFID ORCID Logo  ; Tsun-Kong, Sham 15 ; Sargent, Edward H 2   VIAFID ORCID Logo  ; Sinton, David 6   VIAFID ORCID Logo 

 University of Toronto, Department of Mechanical and Industrial Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938); University of Toronto, Department of Electrical and Computer Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938) 
 University of Toronto, Department of Electrical and Computer Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938) 
 University of Toronto, Department of Electrical and Computer Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938); Tianjin University, Institute of New-Energy Materials, School of Materials Science and Engineering, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484) 
 Hitachi High Technologies America, Inc., Clarksburg, USA (GRID:grid.33763.32) 
 University of Toronto, Department of Mechanical and Industrial Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938); Delft University of Technology, Materials for Energy Conversion and Storage, Department of Chemical Engineering, Delft, The Netherlands (GRID:grid.5292.c) (ISNI:0000 0001 2097 4740) 
 University of Toronto, Department of Mechanical and Industrial Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938) 
 University of Toronto, Department of Materials Science and Engineering, Toronto, Canada (GRID:grid.17063.33) (ISNI:0000 0001 2157 2938) 
 McMaster University, Canadian Center for Electron Microscopy, Hamilton, Canada (GRID:grid.25073.33) (ISNI:0000 0004 1936 8227) 
 Argonne National Laboratory, Advanced Photon Source, Lemont, USA (GRID:grid.187073.a) (ISNI:0000 0001 1939 4845) 
10  Argonne National Laboratory, Advanced Photon Source, Lemont, USA (GRID:grid.187073.a) (ISNI:0000 0001 1939 4845); Canadian Light Source Inc., Science Division, Saskatoon, Canada (GRID:grid.423571.6) (ISNI:0000 0004 0443 7584) 
11  Lawrence Berkeley National Laboratory, Advanced Light Source, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551); Tamkang University, Department of Physics, New Taipei City, Taiwan, ROC (GRID:grid.264580.d) (ISNI:0000 0004 1937 1055) 
12  Lawrence Berkeley National Laboratory, Advanced Light Source, Berkeley, USA (GRID:grid.184769.5) (ISNI:0000 0001 2231 4551) 
13  Tamkang University, Department of Physics, New Taipei City, Taiwan, ROC (GRID:grid.264580.d) (ISNI:0000 0004 1937 1055) 
14  Tianjin University, Institute of New-Energy Materials, School of Materials Science and Engineering, Tianjin, China (GRID:grid.33763.32) (ISNI:0000 0004 1761 2484) 
15  University of Western Ontario, Department of Chemistry, London, Canada (GRID:grid.39381.30) (ISNI:0000 0004 1936 8884) 
Publication year
2018
Publication date
Dec 2018
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2130053100
Copyright
This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.