Three-Dimensional Ternary Hybrid Architectures Constructed from Graphene, MoS₂, and Graphitic Carbon Nitride Nanosheets as Efficient Electrocatalysts for Hydrogen Evolution

Electrocatalytic materials for hydrogen production through water splitting are becoming a hotspot in the renewable energy field. In this work, we present a bottom-up approach to the large-scale synthesis of three-dimensional (3D) ternary hybrid architectures constructed from graphene, MoS2, and graphitic carbon nitride nanosheets (MoS2-CN/G) by a facile self-assembly method. Benefiting from their distinct architectural features including 3D interconnected porous networks, large specific surface areas, ultrathin walls, and low charge-transfer resistance, the as-prepared MoS2-CN/G catalysts exhibit superior hydrogen evolution reaction (HER) performance with a low onset potential of 140 mV, a small Tafel slope of 79 mV dec–1, and reliable long-term durability, markedly outperforming those of bare graphene, MoS2, and graphitic carbon nitride catalysts. DFT calculations further reveal an optimized band structure and numerous efficient electrocatalytic sites for the MoS2-CN/G architectures, both of which are very conducive to boosting the HER kinetics.