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Among transition metal dichalcogenides (TMdCs) as alternatives for Pt-basedcatalysts, metallic-TMdCs catalysts have highly reactive basal-plane but areunstable. Meanwhile, chemically stable semiconducting-TMdCs show limitingcatalytic activity due to their inactive basal-plane. Here, we propose metallicvanadium sulfide (VSn) nanodispersed in a semiconducting MoS2 film (V-MoS2) asan efficient catalyst. During synthesis, vanadium atoms are substituted intohexagonal monolayer MoS2 to form randomly distributed VSn units. The V-MoS2film on a Cu electrode exhibits Pt-scalable catalytic performance; currentdensity of 1000 mA cm-2 at 0.6 V, overpotential of -0.06 V at a current densityof 10 mA cm-2 and exchange current density of 0.65 mA cm-2 at 0 V withexcellent cycle stability for hydrogen-evolution-reaction (HER). The highintrinsic HER performance of V-MoS2 is explained by the efficient electrontransfer from the Cu electrode to chalcogen vacancies near vanadium sites withoptimal Gibbs free energy (-0.02 eV). This study adds insight into ways toengineer TMdCs at the atomic-level to boost intrinsic catalytic activity forhydrogen evolution.

Substitutional VSn nanodispersed in MoS$_2$ film for Pt-scalable catalyst