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Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions

[Image: see text] Copper-based hydrogen evolution electrocatalysts are promising materials to scale-up hydrogen production due to their reported high current densities; however, electrode durability remains a challenge. Here, we report a facile, cost-effective, and scalable synthetic route to produc...

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Autores principales: Fernández-Climent, Roser, Redondo, Jesús, García-Tecedor, Miguel, Spadaro, Maria Chiara, Li, Junnan, Chartrand, Daniel, Schiller, Frederik, Pazos, Jhon, Hurtado, Mikel F., de la Peña O’Shea, Victor, Kornienko, Nikolay, Arbiol, Jordi, Barja, Sara, Mesa, Camilo A., Giménez, Sixto
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10411506/
https://www.ncbi.nlm.nih.gov/pubmed/37564127
http://dx.doi.org/10.1021/acscatal.3c01673
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author Fernández-Climent, Roser
Redondo, Jesús
García-Tecedor, Miguel
Spadaro, Maria Chiara
Li, Junnan
Chartrand, Daniel
Schiller, Frederik
Pazos, Jhon
Hurtado, Mikel F.
de la Peña O’Shea, Victor
Kornienko, Nikolay
Arbiol, Jordi
Barja, Sara
Mesa, Camilo A.
Giménez, Sixto
author_facet Fernández-Climent, Roser
Redondo, Jesús
García-Tecedor, Miguel
Spadaro, Maria Chiara
Li, Junnan
Chartrand, Daniel
Schiller, Frederik
Pazos, Jhon
Hurtado, Mikel F.
de la Peña O’Shea, Victor
Kornienko, Nikolay
Arbiol, Jordi
Barja, Sara
Mesa, Camilo A.
Giménez, Sixto
author_sort Fernández-Climent, Roser
collection PubMed
description [Image: see text] Copper-based hydrogen evolution electrocatalysts are promising materials to scale-up hydrogen production due to their reported high current densities; however, electrode durability remains a challenge. Here, we report a facile, cost-effective, and scalable synthetic route to produce Cu(2–x)S electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our Cu(2–x)S electrodes reach a state-of-the-art performance of ∼400 mA cm(–2) at −1 V vs RHE under mild conditions (pH 8.6), with almost 100% Faradaic efficiency for hydrogen evolution. The rise in current density was found to scale with the electrode electrochemically active surface area. The increased performance of our Cu(2–x)S electrodes correlates with a decrease in the Tafel slope, while analyses by X-ray photoemission spectroscopy, operando X-ray diffraction, and in situ spectroelectrochemistry cooperatively revealed the Cu-centered nature of the catalytically active species. These results allowed us to increase fundamental understanding of heterogeneous electrocatalyst transformation and consequent structure–activity relationship. This facile synthesis of highly durable and efficient Cu(2–x)S electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions.
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spelling pubmed-104115062023-08-10 Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions Fernández-Climent, Roser Redondo, Jesús García-Tecedor, Miguel Spadaro, Maria Chiara Li, Junnan Chartrand, Daniel Schiller, Frederik Pazos, Jhon Hurtado, Mikel F. de la Peña O’Shea, Victor Kornienko, Nikolay Arbiol, Jordi Barja, Sara Mesa, Camilo A. Giménez, Sixto ACS Catal [Image: see text] Copper-based hydrogen evolution electrocatalysts are promising materials to scale-up hydrogen production due to their reported high current densities; however, electrode durability remains a challenge. Here, we report a facile, cost-effective, and scalable synthetic route to produce Cu(2–x)S electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our Cu(2–x)S electrodes reach a state-of-the-art performance of ∼400 mA cm(–2) at −1 V vs RHE under mild conditions (pH 8.6), with almost 100% Faradaic efficiency for hydrogen evolution. The rise in current density was found to scale with the electrode electrochemically active surface area. The increased performance of our Cu(2–x)S electrodes correlates with a decrease in the Tafel slope, while analyses by X-ray photoemission spectroscopy, operando X-ray diffraction, and in situ spectroelectrochemistry cooperatively revealed the Cu-centered nature of the catalytically active species. These results allowed us to increase fundamental understanding of heterogeneous electrocatalyst transformation and consequent structure–activity relationship. This facile synthesis of highly durable and efficient Cu(2–x)S electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions. American Chemical Society 2023-07-26 /pmc/articles/PMC10411506/ /pubmed/37564127 http://dx.doi.org/10.1021/acscatal.3c01673 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Fernández-Climent, Roser
Redondo, Jesús
García-Tecedor, Miguel
Spadaro, Maria Chiara
Li, Junnan
Chartrand, Daniel
Schiller, Frederik
Pazos, Jhon
Hurtado, Mikel F.
de la Peña O’Shea, Victor
Kornienko, Nikolay
Arbiol, Jordi
Barja, Sara
Mesa, Camilo A.
Giménez, Sixto
Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions
title Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions
title_full Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions
title_fullStr Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions
title_full_unstemmed Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions
title_short Highly Durable Nanoporous Cu(2–x)S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions
title_sort highly durable nanoporous cu(2–x)s films for efficient hydrogen evolution electrocatalysis under mild ph conditions
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10411506/
https://www.ncbi.nlm.nih.gov/pubmed/37564127
http://dx.doi.org/10.1021/acscatal.3c01673
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