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Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper

The electroreduction of carbon dioxide using renewable electricity is an appealing strategy for the sustainable synthesis of chemicals and fuels. Extensive research has focused on the production of ethylene, ethanol and n‐propanol, but more complex C(4) molecules have been scarcely reported. Herein,...

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Autores principales: Ting, Louisa Rui Lin, García‐Muelas, Rodrigo, Martín, Antonio J., Veenstra, Florentine L. P., Chen, Stuart Tze‐Jin, Peng, Yujie, Per, Edwin Yu Xuan, Pablo‐García, Sergio, López, Núria, Pérez‐Ramírez, Javier, Yeo, Boon Siang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2020
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7693243/
https://www.ncbi.nlm.nih.gov/pubmed/32706141
http://dx.doi.org/10.1002/anie.202008289
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author Ting, Louisa Rui Lin
García‐Muelas, Rodrigo
Martín, Antonio J.
Veenstra, Florentine L. P.
Chen, Stuart Tze‐Jin
Peng, Yujie
Per, Edwin Yu Xuan
Pablo‐García, Sergio
López, Núria
Pérez‐Ramírez, Javier
Yeo, Boon Siang
author_facet Ting, Louisa Rui Lin
García‐Muelas, Rodrigo
Martín, Antonio J.
Veenstra, Florentine L. P.
Chen, Stuart Tze‐Jin
Peng, Yujie
Per, Edwin Yu Xuan
Pablo‐García, Sergio
López, Núria
Pérez‐Ramírez, Javier
Yeo, Boon Siang
author_sort Ting, Louisa Rui Lin
collection PubMed
description The electroreduction of carbon dioxide using renewable electricity is an appealing strategy for the sustainable synthesis of chemicals and fuels. Extensive research has focused on the production of ethylene, ethanol and n‐propanol, but more complex C(4) molecules have been scarcely reported. Herein, we report the first direct electroreduction of CO(2) to 1‐butanol in alkaline electrolyte on Cu gas diffusion electrodes (Faradaic efficiency=0.056 %, j (1‐Butanol)=−0.080 mA cm(−2) at −0.48 V vs. RHE) and elucidate its formation mechanism. Electrolysis of possible molecular intermediates, coupled with density functional theory, led us to propose that CO(2) first electroreduces to acetaldehyde‐a key C(2) intermediate to 1‐butanol. Acetaldehyde then undergoes a base‐catalyzed aldol condensation to give crotonaldehyde via electrochemical promotion by the catalyst surface. Crotonaldehyde is subsequently electroreduced to butanal, and then to 1‐butanol. In a broad context, our results point to the relevance of coupling chemical and electrochemical processes for the synthesis of higher molecular weight products from CO(2).
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spelling pubmed-76932432020-12-11 Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper Ting, Louisa Rui Lin García‐Muelas, Rodrigo Martín, Antonio J. Veenstra, Florentine L. P. Chen, Stuart Tze‐Jin Peng, Yujie Per, Edwin Yu Xuan Pablo‐García, Sergio López, Núria Pérez‐Ramírez, Javier Yeo, Boon Siang Angew Chem Int Ed Engl Research Articles The electroreduction of carbon dioxide using renewable electricity is an appealing strategy for the sustainable synthesis of chemicals and fuels. Extensive research has focused on the production of ethylene, ethanol and n‐propanol, but more complex C(4) molecules have been scarcely reported. Herein, we report the first direct electroreduction of CO(2) to 1‐butanol in alkaline electrolyte on Cu gas diffusion electrodes (Faradaic efficiency=0.056 %, j (1‐Butanol)=−0.080 mA cm(−2) at −0.48 V vs. RHE) and elucidate its formation mechanism. Electrolysis of possible molecular intermediates, coupled with density functional theory, led us to propose that CO(2) first electroreduces to acetaldehyde‐a key C(2) intermediate to 1‐butanol. Acetaldehyde then undergoes a base‐catalyzed aldol condensation to give crotonaldehyde via electrochemical promotion by the catalyst surface. Crotonaldehyde is subsequently electroreduced to butanal, and then to 1‐butanol. In a broad context, our results point to the relevance of coupling chemical and electrochemical processes for the synthesis of higher molecular weight products from CO(2). John Wiley and Sons Inc. 2020-09-09 2020-11-16 /pmc/articles/PMC7693243/ /pubmed/32706141 http://dx.doi.org/10.1002/anie.202008289 Text en © 2020 The Authors. Published by Wiley-VCH GmbH This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Ting, Louisa Rui Lin
García‐Muelas, Rodrigo
Martín, Antonio J.
Veenstra, Florentine L. P.
Chen, Stuart Tze‐Jin
Peng, Yujie
Per, Edwin Yu Xuan
Pablo‐García, Sergio
López, Núria
Pérez‐Ramírez, Javier
Yeo, Boon Siang
Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
title Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
title_full Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
title_fullStr Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
title_full_unstemmed Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
title_short Electrochemical Reduction of Carbon Dioxide to 1‐Butanol on Oxide‐Derived Copper
title_sort electrochemical reduction of carbon dioxide to 1‐butanol on oxide‐derived copper
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7693243/
https://www.ncbi.nlm.nih.gov/pubmed/32706141
http://dx.doi.org/10.1002/anie.202008289
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