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Rational Design and Operando Characterization of Hierarchical α-FeOOH-FeP/Ni3S2 Catalysts for High-Rate Alkaline Water Electrolysis
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DOI：10.1002/eem2.70187.png)
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Abstract
En 中文
Advancing alkaline water electrolysis for renewable energy technologies requires oxygen evolution reaction electrocatalysts that combine high activity, long-term durability, and mechanistic clarity. Herein, we report a hierarchically engineered α-FeOOH–FeP/Ni3S2 electrocatalyst supported on 3D Ni foam, synthesized via a stepwise hydrothermal sulfidation, gas-phase phosphidation, and chemical impregnation strategy. This integrated multi-phase architecture exhibits strong interfacial coupling, enabling accelerated charge transfer and favorable oxygen evolution reaction kinetics under alkaline conditions. In situ/operando Raman, UV–vis, and electrochemical impedance spectroscopy uncover dynamic surface reconstruction under operating conditions, with reversible Fe3+/Fe4+ redox cycling within the α-FeOOH overlayer, pinpointing transient Fe4+–O species as key catalytic intermediates. The optimized catalyst attains low overpotentials of 223 and 251 mV at 10 and 100 mA cm−2 and sustains industrial-level operation (>500 mA cm−2) with outstanding durability in 1.0 m KOH. When deployed in a symmetric anion exchange membrane water electrolyzer, it delivers a cell voltage of only 1.47 V at 10 mA cm−2, outperforming benchmark noble-metal-based systems. Mechanistic studies including kinetic isotope effect and pH-dependent analysis support a proton-coupled electron transfer mechanism, with O–H bond cleavage as the rate-determining step. These findings elucidate key structure–function relationships and establish a modular design strategy for advanced alkaline oxygen evolution reaction electrocatalysts.
Keywords:
electrocatalysis
oxygen evolution reaction
heterostructured catalysts
oxyhydroxides
transition metal phosphides
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