Edge-Terminated MoS₂ Nanoassembled Electrocatalyst via In Situ Hybridization with 3D Carbon Network

Transition metal dichalcogenides, especially MoS₂ , are considered as promising electrocatalysts for hydrogen evolution reaction (HER). Since the physicochemical properties of MoS₂ and electrode morphology are highly sensitive factor for HER performance, designed synthesis is highly pursued. Here, an in situ method to prepare a 3D carbon/MoS₂ hybrid catalyst, motivated by the graphene ribbon synthesis process, is reported. By rational design strategies, the hybrid electrocatalysts with cross-connected porous structure are obtained, and they show a high HER activity even comparable to the state-of-the-art MoS₂ catalyst without appreciable activity loss in long-term operations. Based on various physicochemical techniques, it is demonstrated that the synthetic procedure can effectively guide the formation of active site and 3D structure with a distinctive feature; increased exposure of active sites by decreased domain size and intrinsically high activity through controlling the number of stacking layers. Moreover, the importance of structural properties of the MoS₂ -based catalysts is verified by controlled experiments, validating the effectiveness of the designed synthesis approach.