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Highly Durable Nanoporous Cu_2-xS Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions.

ABSTRACT: 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-xS electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our Cu_2-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 Cu_2-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 Cu_2-xS electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions.

SUBMITTER: Fernandez-Climent R

PROVIDER: S-EPMC10411506 | biostudies-literature | 2023 Aug

REPOSITORIES: biostudies-literature

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Highly Durable Nanoporous Cu2-xS Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions.

Fernández-Climent Roser R Redondo Jesús J García-Tecedor Miguel M Spadaro Maria Chiara MC Li Junnan J Chartrand Daniel D Schiller Frederik F Pazos Jhon J Hurtado Mikel F MF de la Peña O'Shea Victor V Kornienko Nikolay N Arbiol Jordi J Barja Sara S Mesa Camilo A CA Giménez Sixto S

ACS catalysis 20230726 15

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- ...[more]

PMID: 37564127

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Project description:Efficient and cost-effective electrocatalysts for the hydrogen oxidation/evolution reaction (HOR/HER) are essential for commercializing alkaline fuel cells and electrolyzers. The sluggish HER/HOR reaction kinetics in base is the key issue that requires resolution so that commercialization may proceed. It is also quite challenging to decrease the noble metal loading without sacrificing performance. Herein, we report improved HER/HOR activity as a result of hydrogen spillover on platinum-supported MoO3 (Pt/MoO3-CNx-400) with a Pt loading of 20%. The catalyst exhibited a decreased over-potential of 66.8 mV to reach 10 mA cm-2 current density with a Tafel slope of 41.2 mV dec-1 for the HER in base. The Pt/MoO3-CNx-400 also exhibited satisfactory HOR activity in base. The mass-specific exchange current density of Pt/MoO3-CNx-400 and commercial Pt/C are 505.7 and 245 mA mgPt-1, respectively. The experimental results suggest that the hydrogen binding energy (HBE) is the key descriptor for the HER/HOR. We also demonstrated that the enhanced HER/HOR performance was due to the hydrogen spillover from Pt to MoO3 sites that enhanced the Volmer/Heyrovsky process, which led to high HER/HOR activity and was supported by the experimental and theoretical investigations. The work function value of Pt [Φ = 5.39 eV) is less than that of β-MoO3 (011) [Φ = 7.09 eV], which revealed the charge transfer from Pt to the β-MoO3 (011) surface. This suggested the feasibility of hydrogen spillover, and was further confirmed by the relative hydrogen adsorption energy [ΔGH] at different sites. Based on these findings, we propose that the H2O or H2 dissociation takes place on Pt and interfaces to form Pt-Had or (Pt/MoO3)-Had, and some of the Had shifted to MoO3 sites through hydrogen spillover. Then, Had at the Pt and interface, and MoO3 sites reacted with H2O and HO- to form H2 or H2O molecules, thereby boosting the HER/HOR activity. This work may provide valuable information for the development of hydrogen-spillover-based electrocatalysts for use in various renewable energy devices.

Dataset Information

Highly Durable Nanoporous Cu_2-xS Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions.

Publications

Highly Durable Nanoporous Cu<sub>2-<i>x</i></sub>S Films for Efficient Hydrogen Evolution Electrocatalysis under Mild pH Conditions.

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