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Copper adparticle enabled selective electrosynthesis of n-propanol

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...

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Detalles Bibliográficos
Autores principales: 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
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6218481/
https://www.ncbi.nlm.nih.gov/pubmed/30397203
http://dx.doi.org/10.1038/s41467-018-07032-0
Descripción
Sumario: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).