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Molecular Design Strategies toward Binary (Ge; Mo; Sn; Ti; V)S2 High-Entropy Sulfide
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DOI：10.1021/acs.chemmater.6c00951.png)
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Abstract
En 中文
Metal dichalcogenides (MDCs) of the type MS2 have emerged as promising electrocatalysts for the hydrogen evolution reaction (HER) due to their earth abundance, tunable electronic properties, and distinctive layered structures, which provide a high density of active edge sites and enable efficient interlayer charge transport. However, the controlled incorporation of multiple metal species into a single-phase MS2 framework remains challenging, particularly in the context of high-entropy design principles. In this study, we present a molecular precursor strategy for the controlled synthesis of tetravalent high-entropy sulfides using metal tert-butyl thiolates of the general formula [M(StBu)4] with M = Mo, Sn, Ti, V, and the germanium alkoxide [Ge(OEt)4]. Through partial thiolysis of an equimolar mixture of five precursors resulting in gel formation, a homogeneous network and preorganization of high-entropy elements is formed at the molecular level, allowing precise composition control. Subsequent thermal treatment yielded crystalline MS2-type high-entropy sulfides with a uniform elemental distribution. These materials exhibit significantly enhanced electrocatalytic activity toward HER when compared with their lower-entropy analogues. Overall, this study highlights thiolate-based sol–gel chemistry as a versatile and scalable route for synthesizing compositionally complex sulfide electrocatalysts.
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