Cargando…

Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals

The conversion of carbon dioxide to value-added products using renewable electricity would potentially help to address current climate concerns. The electrochemical reduction of carbon dioxide to propylene, a critical feedstock, requires multiple C–C coupling steps with the transfer of 18 electrons...

Descripción completa

Detalles Bibliográficos
Autores principales: Gao, Jing, Bahmanpour, Alimohammad, Kröcher, Oliver, Zakeeruddin, Shaik M., Ren, Dan, Grätzel, Michael
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10159857/
https://www.ncbi.nlm.nih.gov/pubmed/37024716
http://dx.doi.org/10.1038/s41557-023-01163-8
_version_ 1785037183870042112
author Gao, Jing
Bahmanpour, Alimohammad
Kröcher, Oliver
Zakeeruddin, Shaik M.
Ren, Dan
Grätzel, Michael
author_facet Gao, Jing
Bahmanpour, Alimohammad
Kröcher, Oliver
Zakeeruddin, Shaik M.
Ren, Dan
Grätzel, Michael
author_sort Gao, Jing
collection PubMed
description The conversion of carbon dioxide to value-added products using renewable electricity would potentially help to address current climate concerns. The electrochemical reduction of carbon dioxide to propylene, a critical feedstock, requires multiple C–C coupling steps with the transfer of 18 electrons per propylene molecule, and hence is kinetically sluggish. Here we present the electrosynthesis of propylene from carbon dioxide on copper nanocrystals with a peak geometric current density of −5.5 mA cm(−2). The metallic copper nanocrystals formed from CuCl precursor present preponderant Cu(100) and Cu(111) facets, likely to favour the adsorption of key *C(1) and *C(2) intermediates. Strikingly, the production rate of propylene drops substantially when carbon monoxide is used as the reactant. From the electrochemical reduction of isotope-labelled carbon dioxide mixed with carbon monoxide, we infer that the key step for propylene formation is probably the coupling between adsorbed/molecular carbon dioxide or carboxyl with the *C(2) intermediates that are involved in the ethylene pathway. [Image: see text]
format Online
Article
Text
id pubmed-10159857
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-101598572023-05-06 Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals Gao, Jing Bahmanpour, Alimohammad Kröcher, Oliver Zakeeruddin, Shaik M. Ren, Dan Grätzel, Michael Nat Chem Article The conversion of carbon dioxide to value-added products using renewable electricity would potentially help to address current climate concerns. The electrochemical reduction of carbon dioxide to propylene, a critical feedstock, requires multiple C–C coupling steps with the transfer of 18 electrons per propylene molecule, and hence is kinetically sluggish. Here we present the electrosynthesis of propylene from carbon dioxide on copper nanocrystals with a peak geometric current density of −5.5 mA cm(−2). The metallic copper nanocrystals formed from CuCl precursor present preponderant Cu(100) and Cu(111) facets, likely to favour the adsorption of key *C(1) and *C(2) intermediates. Strikingly, the production rate of propylene drops substantially when carbon monoxide is used as the reactant. From the electrochemical reduction of isotope-labelled carbon dioxide mixed with carbon monoxide, we infer that the key step for propylene formation is probably the coupling between adsorbed/molecular carbon dioxide or carboxyl with the *C(2) intermediates that are involved in the ethylene pathway. [Image: see text] Nature Publishing Group UK 2023-04-06 2023 /pmc/articles/PMC10159857/ /pubmed/37024716 http://dx.doi.org/10.1038/s41557-023-01163-8 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/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/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Gao, Jing
Bahmanpour, Alimohammad
Kröcher, Oliver
Zakeeruddin, Shaik M.
Ren, Dan
Grätzel, Michael
Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
title Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
title_full Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
title_fullStr Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
title_full_unstemmed Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
title_short Electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
title_sort electrochemical synthesis of propylene from carbon dioxide on copper nanocrystals
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10159857/
https://www.ncbi.nlm.nih.gov/pubmed/37024716
http://dx.doi.org/10.1038/s41557-023-01163-8
work_keys_str_mv AT gaojing electrochemicalsynthesisofpropylenefromcarbondioxideoncoppernanocrystals
AT bahmanpouralimohammad electrochemicalsynthesisofpropylenefromcarbondioxideoncoppernanocrystals
AT krocheroliver electrochemicalsynthesisofpropylenefromcarbondioxideoncoppernanocrystals
AT zakeeruddinshaikm electrochemicalsynthesisofpropylenefromcarbondioxideoncoppernanocrystals
AT rendan electrochemicalsynthesisofpropylenefromcarbondioxideoncoppernanocrystals
AT gratzelmichael electrochemicalsynthesisofpropylenefromcarbondioxideoncoppernanocrystals