Tailoring electrocatalytic performance of nickel metal-organic framework derivatives for hydrogen evolution reaction

El Hanafi, Morad and El ouardi, Mohamed and Bau, Jeremy and Khossossi, Nabil and Amal, BaQais and Haspel, Henrik and Kónya, Zoltán and Saadi, Mohamed and Rueping, Magnus and Aiz Ahsaine, Hassan (2025) Tailoring electrocatalytic performance of nickel metal-organic framework derivatives for hydrogen evolution reaction. CHEMICAL ENGINEERING JOURNAL, 527. p. 171757. ISSN 1385-8947

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Abstract

Water electrolysis driven by renewable energy generates “green” hydrogen, a carbon neutral energy source and chemical feedstock, and a key component in mitigating the effect of anthropogenic climate change in the near future. To the wide-spread utilization of water electrolyzers, highly active catalysts are required composed of cheap earth-abundant elements. To this end, we constructed a nickel-based metal-organic framework (MOF) and decomposed it by a controlled pyrolysis at different temperatures into a carbon supported nickel electrocatalyst for the alkaline electrochemical hydrogen evolution reaction (HER). The highest electrocatalytic performance of a low overpotential of 90 mV at a current density of −10 mA cm−2, and a Tafel slope of 93 mV·dec−1 was achieved by annealing at 800 °C. The origin of the catalytic activity was discussed in terms of structural properties, and DFT calculations found a delicate balance among the formation of nickel nanoparticles, the graphitization of the MOF structure, and the metal-support interactions at certain pyrolysis conditions. The Ni-MOF-800 showed low charge-transfer resistance along with excellent stability, retaining the catalytic activity over 2000 cycles. The study is a step forward in designing advanced electrocatalysts with tailored structural properties for large-scale water electrolysis.

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