A Metal–Organic Frameworks Derived 1T‐MoS2 with Expanded Layer Spacing for Enhanced Electrocatalytic Hydrogen Evolution

Abstract Metal phase molybdenum disulfide (1T‐MoS 2 ) 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‐MoS 2 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 MoS 2 catalyst is extended to 10.87 Å, which represents the largest one for the 1T‐MoS 2 catalyst prepared by the bottom‐up approach. Theoretical calculations reveal that the expanded crystal planes alter the electronic structure of 1T‐MoS 2 , lower the adsorption–desorption potentials of protons, and thus, trigger efficient catalytic activity for HER. The optimal 1T‐MoS 2 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.