1T/2H Mixed Phase MoS₂ Nanosheets Integrated by a 3D Nitrogen-Doped Graphene Derivative for Enhanced Electrocatalytic Hydrogen Evolution

Molybdenum disulfide (MoS2) has become one of the most promising non-platinum-based electrocatalysts for the hydrogen evolution reaction (HER) because of its unique layered structure. However, the catalytic performance of the thermodynamically stable MoS2 is hindered by its poor conductivity and scarce active sites. We developed a 3D porous N-doped graphene derivative-integrated metal–semiconductor (1T-2H) mixed phase MoS2 (MNG) using urea as a doping reagent. The highly exposed active sites were achieved by inducing the phase transition of MoS2 from 2H phase to 1T phase and the inclusion of highly N-incorporated reduced graphene oxide, both of which were simultaneously realized by optimizing the concentration of the doping reagent. Moreover, the charge/proton transfer was enhanced by the well-designed porous architecture and hydrophilic 1T-MoS2. With these advantages, the optimized MNG-40 catalyst has a small overpotential of 157 mV at a cathodic current density of 10 mA cm–2, a relatively low Tafel slope of 45.8 mV dec–1, and an excellent stability. This work represents a new strategy to design higher-performance HER catalysts and provides new insights into the structural regulation of metal composite transitions.