Journal Article

Copper adparticle enabled selective electrosynthesis of n-propanol

Ma, Lu, Saidaminov, Makhsud I., Pang, Yuanjie, Che, Fanglin, Wang, Ziyun, Sinton, David, Cheng, Shaobo, Finfrock, Y. Zou, Wu, Tianpin, Sham, Tsun-Kong, Sargent, Edward H., Li, Fengwang, Howe, Jane Y., Wang, Yuhang, Pong, Way-Faung, De Luna, Phil, Liu, Yi-Sheng, Guo, Jinghua, Du, Xiwen, Zou, Chengqin, Dinh, Cao-Thang, Li, Jun, Edwards, Jonathan P., Hsieh, Shang-Hsien, Botton, Gianluigi A., Burdyny, Thomas, Zhuang, Tao-Tao

2018

Overview

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.

• Publisher: Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
• Subject: 639/301/299/886 / 639/638/675 / 639/638/77/886 / Carbon / Carbon dioxide / Carbon monoxide / Catalysis / Catalysts / Chemical activity / Chemical reduction / Chemisorption / Copper / Density functional theory / Electrochemistry / Humanities and Social Sciences / INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY / Intermediates / Liquid fuels / multidisciplinary / Organic chemistry / Propanol / Science / Science (multidisciplinary) / Selectivity