Constructing Sulfur Vacancy-Rich NiCo 2 S 4 @MoS 2 Core@shell Heterostructure via Interface Engineering for Enhanced HER Electrocatalysis

The rational design of heterointerfaces with optimized charge dynamics and defect engineering remains pivotal for developing advanced non-noble metal-based electrocatalysts for water splitting. A comparative study of NiCo₂S₄–MoS₂ heterostructures was conducted to elucidate the impact of interfacial architecture and defect engineering on hydrogen evolution reaction (HER) performance. A core@shell NiCo₂S₄@MoS₂ heterostructure was synthesized via a facile hydrothermal growth method, inducing lattice distortion and strong interfacial coupling, while supported NiCo₂S₄/MoS₂ heterostructures were prepared by ultrasonic-assisted deposition. A detailed structural and spectroscopic characterization and theoretical calculation demonstrated that the core@shell configuration promotes charge redistribution across the NiCo₂S₄–MoS₂ interface and generates abundant sulfur vacancies, thereby increasing the density of electroactive sites. Electrochemical measurements reveal that NiCo₂S₄@MoS₂ markedly outperforms the supported heterostructure, single-component NiCo₂S₄, and MoS₂ when serving as the HER catalyst in acid solution. These findings establish a dual-optimization strategy—combining interfacial design with vacancy modulation—that provides a generalizable paradigm for the deliberate design of high-efficiency non-noble metal-based electrocatalysts for water splitting reactions.

Abstract licence: CC BY

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