A Metal-Organic Frameworks Derived 1T-MoS₂ with Expanded Layer Spacing for Enhanced Electrocatalytic Hydrogen...

Metal phase molybdenum disulfide (1T-MoS₂ ) is considered a promising electrocatalyst for hydrogen evolution reaction (HER) due to its activated basal and superior electrical conductivity. Here, a one-step solvothermal route is developed to prepare 1T-MoS₂ with expanded layer spacing through the derivatization of a Mo-based organic framework (Mo-MOFs). Benefiting from N,N-dimethylformamide oxide as external stress, the interplanar spacing of (002) of the MoS₂ catalyst is extended to 10.87 Å, which represents the largest one for the 1T-MoS₂ catalyst prepared by the bottom-up approach. Theoretical calculations reveal that the expanded crystal planes alter the electronic structure of 1T-MoS₂ , lower the adsorption-desorption potentials of protons, and thus, trigger efficient catalytic activity for HER. The optimal 1T-MoS₂ catalyst exhibits an overpotential of 98 mV at 10 mA cm^-2 for HER, corresponding to a Tafel slope of 52 mV dec^-1 . This Mo-MOFs-derived strategy provides a potential way to design high-performance catalysts by adjusting the layer spacing of 2D materials.