Defect engineering in the inherently inert basal planes of transition metal dichalcogenides (TMDs), involving the introduction of chalcogen vacancies, represents a pivotal approach to enhance catalytic activity by exposing high-density catalytic metal single-atom sites. However, achieving a single-atom limit spacing between chalcogen vacancies to form ordered superstructures remains challenging for creating uniformly distributed high-density metal single-atom sites on TMDs comparable to carbon-supported single-atom catalysts (SACs). Here we unveil an efficient TMD-based topological catalyst for hydrogen evolution reaction (HER), featuring high-density single-atom reactive centers on a few-layer (7 × 7)-PtTe2-x superstructure. Compared with pristine Pt(111), PtTe2, and (2 × 2)-PtTe2-x, (7 × 7)-PtTe2-x exhibits superior HER performance owing to its substantially increased density of undercoordinated Pt sites, alongside exceptional catalytic stability when operating at high current densities. First-principles calculations confirm that multiple types of undercoordinated Pt sites on (7 × 7)-PtTe2-x exhibit favorable hydrogen adsorption Gibbs free energies, and remain active upon increasing hydrogen coverage. Furthermore, (7 × 7)-PtTe2-x possesses nontrivial band topologies with robust edge states, suggesting potential enhancements for HER. Our findings are expected to advance TMD-based catalysts and exploration of topological materials in catalysis.
Keywords: few-layer platinum telluride; hydrogen evolution; nontrivial band topology; periodic Te vacancies; precise nanofabrication.