Amorphous MoSx Nanosheets with Abundant Interlayer Dislocations for Enhanced Photolytic Hydrogen Evolution Reaction

Transition metal dichalcogenides (TMSs), exemplified by molybdenum disulfide (MoS2), exhibit significant potential as alternatives to noble metals (e.g., Pt) for the hydrogen evolution reaction (HER). However, conventional synthesis methods of MoSx often suffer from active site loss, harsh reaction conditions, or undesirable oxidation, limiting their practical applicability. The development of MoSx with high-density active sites remains a formidable challenge. Herein, we propose a novel strategy employing [Mo3S13]2− clusters as precursors to construct three-dimensional amorphous MoSx nanosheets through optimized hydrothermal and solvent evaporation-induced self-assembly approaches. Comprehensive characterization confirms the material’s unique amorphous lamellar structure, featuring preserved [Mo3S13]2− units and engineered interlayer dislocations that facilitate enhanced electron transfer and active site exposure. This work not only establishes [Mo3S13]2− clusters as effective building blocks for high-performance MoSx catalysts, but also provides a scalable and environmentally benign synthesis route for the large-scale production of such nanostructured a-MoSx. Our findings facilitate the rational design of non-noble HER catalysts via structural engineering, with broad implications for energy conversion technologies.