Two-Dimensional Topological Platinum Telluride Superstructures with Periodic Tellurium Vacancies for Efficient and Robust Catalysis

Abstract

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)-PtTe_2-<i>x</i> superstructure. Compared with pristine Pt(111), PtTe₂, and (2 × 2)-PtTe_2-<i>x</i>, (7 × 7)-PtTe_2-<i>x</i> 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)-PtTe_2-<i>x</i> exhibit favorable hydrogen adsorption Gibbs free energies, and remain active upon increasing hydrogen coverage. Furthermore, (7 × 7)-PtTe_2-<i>x</i> 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.