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Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO(2)/CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm(−2)...

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Detalles Bibliográficos
Autores principales: Li, Jun, Xu, Aoni, Li, Fengwang, Wang, Ziyun, Zou, Chengqin, Gabardo, Christine M., Wang, Yuhang, Ozden, Adnan, Xu, Yi, Nam, Dae-Hyun, Lum, Yanwei, Wicks, Joshua, Chen, Bin, Wang, Zhiqiang, Chen, Jiatang, Wen, Yunzhou, Zhuang, Taotao, Luo, Mingchuan, Du, Xiwen, Sham, Tsun-Kong, Zhang, Bo, Sargent, Edward H., Sinton, David
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7378828/
https://www.ncbi.nlm.nih.gov/pubmed/32703956
http://dx.doi.org/10.1038/s41467-020-17499-5
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author Li, Jun
Xu, Aoni
Li, Fengwang
Wang, Ziyun
Zou, Chengqin
Gabardo, Christine M.
Wang, Yuhang
Ozden, Adnan
Xu, Yi
Nam, Dae-Hyun
Lum, Yanwei
Wicks, Joshua
Chen, Bin
Wang, Zhiqiang
Chen, Jiatang
Wen, Yunzhou
Zhuang, Taotao
Luo, Mingchuan
Du, Xiwen
Sham, Tsun-Kong
Zhang, Bo
Sargent, Edward H.
Sinton, David
author_facet Li, Jun
Xu, Aoni
Li, Fengwang
Wang, Ziyun
Zou, Chengqin
Gabardo, Christine M.
Wang, Yuhang
Ozden, Adnan
Xu, Yi
Nam, Dae-Hyun
Lum, Yanwei
Wicks, Joshua
Chen, Bin
Wang, Zhiqiang
Chen, Jiatang
Wen, Yunzhou
Zhuang, Taotao
Luo, Mingchuan
Du, Xiwen
Sham, Tsun-Kong
Zhang, Bo
Sargent, Edward H.
Sinton, David
author_sort Li, Jun
collection PubMed
description Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO(2)/CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm(−2)). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C(2) intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm(−2) from CO electroreduction. The activity exceeds that of prior reports by a factor of 2.
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spelling pubmed-73788282020-07-28 Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption Li, Jun Xu, Aoni Li, Fengwang Wang, Ziyun Zou, Chengqin Gabardo, Christine M. Wang, Yuhang Ozden, Adnan Xu, Yi Nam, Dae-Hyun Lum, Yanwei Wicks, Joshua Chen, Bin Wang, Zhiqiang Chen, Jiatang Wen, Yunzhou Zhuang, Taotao Luo, Mingchuan Du, Xiwen Sham, Tsun-Kong Zhang, Bo Sargent, Edward H. Sinton, David Nat Commun Article Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO(2)/CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm(−2)). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C(2) intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm(−2) from CO electroreduction. The activity exceeds that of prior reports by a factor of 2. Nature Publishing Group UK 2020-07-23 /pmc/articles/PMC7378828/ /pubmed/32703956 http://dx.doi.org/10.1038/s41467-020-17499-5 Text en © The Author(s) 2020 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Li, Jun
Xu, Aoni
Li, Fengwang
Wang, Ziyun
Zou, Chengqin
Gabardo, Christine M.
Wang, Yuhang
Ozden, Adnan
Xu, Yi
Nam, Dae-Hyun
Lum, Yanwei
Wicks, Joshua
Chen, Bin
Wang, Zhiqiang
Chen, Jiatang
Wen, Yunzhou
Zhuang, Taotao
Luo, Mingchuan
Du, Xiwen
Sham, Tsun-Kong
Zhang, Bo
Sargent, Edward H.
Sinton, David
Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
title Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
title_full Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
title_fullStr Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
title_full_unstemmed Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
title_short Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
title_sort enhanced multi-carbon alcohol electroproduction from co via modulated hydrogen adsorption
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7378828/
https://www.ncbi.nlm.nih.gov/pubmed/32703956
http://dx.doi.org/10.1038/s41467-020-17499-5
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