Highly Durable Nanoporous CuS 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 CuS electrocatal...

Descripción completa

Detalles Bibliográficos
Autores: Fernández-Climent, Roser, Redondo, Jesús, García-Tecedor, Miguel|||0000-0002-9664-4665, Spadaro, Maria Chiara|||0000-0002-6540-0377, Li, Junnan, Chartrand, Daniel, Schiller, Frederik|||0000-0003-1727-3542, Pazos, Jhon, Hurtado, Mikel F., de la Peña O'Shea, Victor|||0000-0001-5762-4787, Kornienko, Nikolay|||0000-0001-7193-2428, Arbiol i Cobos, Jordi|||0000-0002-0695-1726, Barja, Sara|||0000-0002-4257-2651, Mesa, Camilo A.|||0000-0002-8450-2563, Giménez, Sixto|||0000-0002-4522-3174
Tipo de recurso: artículo
Fecha de publicación:2023
País:España
Institución:Universitat Autònoma de Barcelona
Repositorio:Dipòsit Digital de Documents de la UAB
Idioma:inglés
OAI Identifier:oai:ddd.uab.cat:287097
Acceso en línea:https://ddd.uab.cat/record/287097
https://dx.doi.org/urn:doi:10.1021/acscatal.3c01673
Access Level:acceso abierto
Palabra clave:Green hydrogen
Hydrogen evolution reaction
Electrocatalysis
Cu-based electrodes
Operando ECSA increase
Mechanistic analysis
Descripción
Sumario: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 CuS electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our CuS 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 CuS 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 CuS electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions.