International Journal of Hydrogen Energy, cilt.143, ss.1144-1153, 2025 (SCI-Expanded)
Two-dimensional (2D) materials have attracted widespread attention because of their distinctive atomic-scale thicknesses, high surface-to-volume ratios, and remarkable electrocatalytic capabilities. Specifically, 2D molybdenum disulfide (MoS2) nanosheets are particularly notable for their tunable surface characteristics and large electrochemically active areas. However, the naturally semiconducting 2H phase of MoS2 features inactive basal planes, limiting its active sites and efficiency in water electrocatalysis. This study focuses on designing efficient, durable, and cost-effective HER electrocatalysts by incorporating exfoliated MoS2 into a 3D carbon network via an innovative approach. Initially, MoS₂ transformed from the 2H phase to the more conductive and intrinsically active 1T phase. Subsequently, the synthesized 2D layered 1T-MoS₂ structure was interconnected with well-ordered 3D mesoporous CMK-3 to construct a morphological architecture. The assembled catalysts, which possess high surface areas and suitable pore diameters, afford greater accessibility to adsorption sites and enable rapid mass and charge transfer. Thus, not only were rapid HER kinetics achieved, as well as the performance of the 1T-MoS₂ structure was effectively maintained without reverting to the 2H phase. The physicochemical and electrochemical properties of the 1T-MoS2@CMK-3 system were thoroughly examined to determine their synergistic contributions to catalytic performance. This nanostructured catalyst exhibited a low Tafel slope of 65 mV dec⁻1 and an overpotential of 260 mV to reach a current density of 10 mA cm⁻2 in acidic conditions for HER. Compared to pure 1T-MoS2, 1T-MoS2@CMK-3 showed excellent durability in prolonged electrolysis tests. This study introduces a novel strategy for the development of HER catalysts based on 2D/3D composites, in which few-layer MoS2 is dispersed on 3D carbon structures with a high specific surface area, thus offering a promising alternative to expensive metal-based catalysts.