Copper adparticle enabled selective electrosynthesis of n-propanol

被引:0
作者
Jun Li
Fanglin Che
Yuanjie Pang
Chengqin Zou
Jane Y. Howe
Thomas Burdyny
Jonathan P. Edwards
Yuhang Wang
Fengwang Li
Ziyun Wang
Phil De Luna
Cao-Thang Dinh
Tao-Tao Zhuang
Makhsud I. Saidaminov
Shaobo Cheng
Tianpin Wu
Y. Zou Finfrock
Lu Ma
Shang-Hsien Hsieh
Yi-Sheng Liu
Gianluigi A. Botton
Way-Faung Pong
Xiwen Du
Jinghua Guo
Tsun-Kong Sham
Edward H. Sargent
David Sinton
机构
[1] University of Toronto,Department of Mechanical and Industrial Engineering
[2] University of Toronto,Department of Electrical and Computer Engineering
[3] Tianjin University,Institute of New
[4] Hitachi High Technologies America,Energy Materials, School of Materials Science and Engineering
[5] Inc.,Materials for Energy Conversion and Storage, Department of Chemical Engineering
[6] Delft University of Technology,Department of Materials Science and Engineering
[7] University of Toronto,Canadian Center for Electron Microscopy
[8] McMaster University,Advanced Photon Source
[9] Argonne National Laboratory,Science Division
[10] Canadian Light Source Inc.,Advanced Light Source
[11] Lawrence Berkeley National Laboratory,Department of Physics
[12] Tamkang University,Department of Chemistry
[13] University of Western Ontario,undefined
来源
Nature Communications | / 9卷
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摘要
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.
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