Pairing of Transition Metal Dichalcogenides and Doped Graphene for Catalytically Dual Active Interfaces for the Hydrogen Evolution Reaction

We screen optimum bilayer pairs of transition metal dichalcogenides (TMDs) and doped graphene (G) for highly active and stable catalysts of the hydrogen evolution reaction (HER). Based on first-principles density functional theory (DFT) calculations and ab initio thermodynamic formalisms, we propose a new design concept for active and durable HER catalysis with cost-effective materials. Specifically, we discover that the dual interfaces of the bilayer in NbS₂ and supported 6% B-doped G systems can be highly activated. The design is especially useful for HER catalysis in a vertically oriented architecture of the material. The Gibbs free energy landscape of the TMD/G pairs for the HER demonstrates that the thermodynamic performance is comparable or superior to conventional platinum on carbon (Pt/C). The stability of the catalyst is evaluated by two descriptors: interface adhesion energy of the pair and defect formation energy of sulfur (S) in the TMD surface. Our results provide new concepts for how to enhance catalytic activity and durability via hybrid interfacing of cost-effective materials, essentially leading to overcoming conventional challenges for Pt-based catalysts.