Synthesis of Metal-Organic Hybrid Thin Films for Hydrogen Storage and Catalytic Applications: Inert, High-Pressure Environment

2D Metal-Organic Chalcogenolates (MOChas) are an emerging class of materials with high potential in hydrogen generation, storage, and catalysis research, particularly demonstrated by their use in photocatalytic and electrocatalytic hydrogen gas production. Among them, mithrene AgSePh based two-dimensional layered structure, holds significant promise as a catalyst for hydrogen gas storage and generation due to its large surface area. However, conventional synthesis methods have been limited in producing high-quality thin films due to difficulties in controlling the reaction rate, chemical contamination from solvents, and poor reproducibility.In this study, we present a novel synthesis strategy for highly crystalline mithrene thin films using a custom-designed stainless steel reaction chamber under an inert, high-pressure, and solvent-free environment. By precisely controlling the internal vapor pressure through the regulation of the reaction temperature, the reaction kinetics were optimized. This resulted in continuous, stoichiometric, and highly oriented thin films. This research establishes a reliable and reproducible pathway for synthesizing high-quality mithrene thin films without the chemical intervention of solvents, suggesting that MOChas-based thin films fabricated via this method can be expanded to next-generation catalysts, and hydrogen gas storage and other related applications.