Highly durable nanoporous Cu2-xS films for efficient hydrogen evolution electrocatalysis under mild pH conditions

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 Cu2-xS electroca...

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Detalhes bibliográficos
Autores: Fernández-Climent, Roser, Redondo, Jesús, García-Tecedor, Miguel, Spadaro, Maria Chiara, Li, Junnan, Chartrand, Daniel, Schiller, Frederik, Pazos, Jhon, Hurtado, Mikel F., Peña O'Shea, Victor de la, Kornienko, Nikolay, Arbiol, Jordi, Barja, Sara, Mesa, Camilo A., Giménez, Sixto
Formato: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Recursos:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/342429
Acesso em linha:http://hdl.handle.net/10261/342429
Access Level:acceso abierto
Palavra-chave:Green hydrogen
Mechanistic analysis
Hydrogen evolution reaction
Operando ECSA increase
Electrocatalysis
Cu-based electrodes
Descrição
Resumo: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 Cu2-xS electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our Cu2-xS 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 Cu2-xS 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 Cu2-xS electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions.