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Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction

An overarching challenge of the electrochemical carbon dioxide reduction reaction (eCO(2)RR) is finding an earth-abundant, highly active catalyst that selectively produces hydrocarbons at relatively low overpotentials. Here, we report the eCO(2)RR performance of two-dimensional transition metal carb...

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Autores principales: Esmaeilirad, Mohammadreza, Baskin, Artem, Kondori, Alireza, Sanz-Matias, Ana, Qian, Jin, Song, Boao, Tamadoni Saray, Mahmoud, Kucuk, Kamil, Belmonte, Andres Ruiz, Delgado, Pablo Navarro Munoz, Park, Junwon, Azari, Rahman, Segre, Carlo U., Shahbazian-Yassar, Reza, Prendergast, David, Asadi, Mohammad
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2021
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8379264/
https://www.ncbi.nlm.nih.gov/pubmed/34417447
http://dx.doi.org/10.1038/s41467-021-25295-y
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author Esmaeilirad, Mohammadreza
Baskin, Artem
Kondori, Alireza
Sanz-Matias, Ana
Qian, Jin
Song, Boao
Tamadoni Saray, Mahmoud
Kucuk, Kamil
Belmonte, Andres Ruiz
Delgado, Pablo Navarro Munoz
Park, Junwon
Azari, Rahman
Segre, Carlo U.
Shahbazian-Yassar, Reza
Prendergast, David
Asadi, Mohammad
author_facet Esmaeilirad, Mohammadreza
Baskin, Artem
Kondori, Alireza
Sanz-Matias, Ana
Qian, Jin
Song, Boao
Tamadoni Saray, Mahmoud
Kucuk, Kamil
Belmonte, Andres Ruiz
Delgado, Pablo Navarro Munoz
Park, Junwon
Azari, Rahman
Segre, Carlo U.
Shahbazian-Yassar, Reza
Prendergast, David
Asadi, Mohammad
author_sort Esmaeilirad, Mohammadreza
collection PubMed
description An overarching challenge of the electrochemical carbon dioxide reduction reaction (eCO(2)RR) is finding an earth-abundant, highly active catalyst that selectively produces hydrocarbons at relatively low overpotentials. Here, we report the eCO(2)RR performance of two-dimensional transition metal carbide class of materials. Our results indicate a maximum methane (CH(4)) current density of −421.63 mA/cm(2) and a CH(4) faradic efficiency of 82.7% ± 2% for di-tungsten carbide (W(2)C) nanoflakes in a hybrid electrolyte of 3 M potassium hydroxide and 2 M choline-chloride. Powered by a triple junction photovoltaic cell, we demonstrate a flow electrolyzer that uses humidified CO(2) to produce CH(4) in a 700-h process under one sun illumination with a CO(2)RR energy efficiency of about 62.3% and a solar-to-fuel efficiency of 20.7%. Density functional theory calculations reveal that dissociation of water, chemisorption of CO(2) and cleavage of the C-O bond—the most energy consuming elementary steps in other catalysts such as copper—become nearly spontaneous at the W(2)C surface. This results in instantaneous formation of adsorbed CO—an important reaction intermediate—and an unlimited source of protons near the tungsten surface sites that are the main reasons for the observed superior activity, selectivity, and small potential.
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spelling pubmed-83792642021-09-22 Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction Esmaeilirad, Mohammadreza Baskin, Artem Kondori, Alireza Sanz-Matias, Ana Qian, Jin Song, Boao Tamadoni Saray, Mahmoud Kucuk, Kamil Belmonte, Andres Ruiz Delgado, Pablo Navarro Munoz Park, Junwon Azari, Rahman Segre, Carlo U. Shahbazian-Yassar, Reza Prendergast, David Asadi, Mohammad Nat Commun Article An overarching challenge of the electrochemical carbon dioxide reduction reaction (eCO(2)RR) is finding an earth-abundant, highly active catalyst that selectively produces hydrocarbons at relatively low overpotentials. Here, we report the eCO(2)RR performance of two-dimensional transition metal carbide class of materials. Our results indicate a maximum methane (CH(4)) current density of −421.63 mA/cm(2) and a CH(4) faradic efficiency of 82.7% ± 2% for di-tungsten carbide (W(2)C) nanoflakes in a hybrid electrolyte of 3 M potassium hydroxide and 2 M choline-chloride. Powered by a triple junction photovoltaic cell, we demonstrate a flow electrolyzer that uses humidified CO(2) to produce CH(4) in a 700-h process under one sun illumination with a CO(2)RR energy efficiency of about 62.3% and a solar-to-fuel efficiency of 20.7%. Density functional theory calculations reveal that dissociation of water, chemisorption of CO(2) and cleavage of the C-O bond—the most energy consuming elementary steps in other catalysts such as copper—become nearly spontaneous at the W(2)C surface. This results in instantaneous formation of adsorbed CO—an important reaction intermediate—and an unlimited source of protons near the tungsten surface sites that are the main reasons for the observed superior activity, selectivity, and small potential. Nature Publishing Group UK 2021-08-20 /pmc/articles/PMC8379264/ /pubmed/34417447 http://dx.doi.org/10.1038/s41467-021-25295-y Text en © The Author(s) 2021 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
Esmaeilirad, Mohammadreza
Baskin, Artem
Kondori, Alireza
Sanz-Matias, Ana
Qian, Jin
Song, Boao
Tamadoni Saray, Mahmoud
Kucuk, Kamil
Belmonte, Andres Ruiz
Delgado, Pablo Navarro Munoz
Park, Junwon
Azari, Rahman
Segre, Carlo U.
Shahbazian-Yassar, Reza
Prendergast, David
Asadi, Mohammad
Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
title Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
title_full Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
title_fullStr Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
title_full_unstemmed Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
title_short Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
title_sort gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8379264/
https://www.ncbi.nlm.nih.gov/pubmed/34417447
http://dx.doi.org/10.1038/s41467-021-25295-y
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