▎ 摘　　要

Two-dimensional (2D) molybdenum sulfide (MoS2) is an attractive noble-metal-free electrocatalyst for hydrogen evolution (HER) in acids. Tremendous effort has been made to engineer MoS2 catalysts with either more active sites or higher conductivity to enhance their HER activity. However, little attention has been paid to synergistically structural and electronic modulations of MoS2. Herein, 2D hydrogenated graphene (HG) is introduced into MoS2 ultrathin nanosheets for the construction of a highly efficient and stable catalyst for HER Owing to synergistic modulations of both structural and electronic benefits to MoS2 nanosheets via HG support, such a catalyst has improved conductivity, more accessible catalytic active sites, and moderate hydrogen adsorption energy. On the optimized MoS2/HG hybrid catalyst, HER occurs with an overpotential of 124 mV at 10 mA cm(-2), a Tafel slope of 41 mV dec(-1), and a stable durability for 24 h continuous operation at 30 mA cm(-2) without observable fading. The high performance of the optimized MoS2/HG hybrid catalyst for HER was interpreted with density functional theory calculations. The simulation results reveal that the introduction of HG modulates the electronic structure of MoS2 to increase the number of active sites and simultaneously optimizes the hydrogen adsorption energy at S-edge atoms, eventually promoting HER activity. This study thus provides a strategy to design and develop high-performance HER electrocatalysts by employing different 2D materials.