Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.230
Publication date: 28th August 2024
Proton exchange membrane water electrolysis (PEMWE) demands a highly active and stable bifunctional electrocatalyst for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in acidic electrolytes. In this study, we present a high entropy alloy (HEA) ZnNiCoIrMn as an effective bifunctional electrocatalyst for HER and OER under acidic conditions. A nanoporous structure was obtained by facile dealloying method in a vacuum system using Zn as a sacrificial element. In particular, the electronic structure of Ir was modified by incorporating Mn. The downshift of the d-band center separates the d-band center of Ir away from the Fermi level, weakening the adsorption energy with reaction intermediates. The result is that weaker adsorption energy is beneficial for the catalytic reaction. The electronic structure of Ir can be further tailored by composition control, resulting in optimized adsorption energies that are required not only to improve catalytic activity but also to prevent the dissolution of the metal atoms. The diffusion of elements in ZnNiCoIrMn is limited by high entropy effects, which also contributes to prohibiting the loss of elements during electrolysis. A low overpotential of 29 mV and 242 mV was required for HER and OER to generate the current density of 10 mA cm-2 despite low Ir content in ZnNiCoIrMn. Furthermore, ZnNiCoIrMn shows high stability for HER and OER over 200 h. It demonstrates that weak adsorption energy of HEA induced by compositional engineering suppress solvation of elements, which is responsible for the enhanced durability of OER and HER under acidic conditions.
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