Document Type

Article

Publication Date

Fall 9-8-2026

Abstract

Developing efficient, durable, and earth-abundant electrocatalysts for alkaline water electrolysis is critical for sustainable hydrogen production. Transition-metal sulfides have emerged as promising hydrogen evolution reaction (HER) catalysts; however, their catalytic behavior is often governed by dynamic structural transformations occurring under operating conditions. Herein, we report the synthesis of tetra-metallic Ni-Co-Fe-Mn sulfide nanoflowers directly grown on Ni foam via a one-step hydrothermal approach. The as-prepared catalysts underwent significant electrochemical activation, leading to surface reconstruction and enhanced catalytic activity. The optimized catalyst exhibited a remarkable reduction in overpotential from 300 mV to 121 mV at 100 mA cm⁻², further decreasing to 100 mV after prolonged activation. Electrochemical impedance spectroscopy and double-layer capacitance analyses revealed improved charge transfer and increased electrochemically active surface area. Density functional theory (DFT) calculations suggest that electronic structure modulation contributes to the optimized hydrogen adsorption. This work provides fundamental insights into electrochemical reconstruction in multimetal sulfides and establishes a viable strategy for designing high-performance electrocatalysts for alkaline hydrogen evolution

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