Defect engineering to activate the basal planes of transition metal
dichalcogenides (TMDs) is critical for the development of TMD-based
electrocatalysts as the chemical inertness of basal planes restrict their
potential applications in hydrogen evolution reaction (HER). Here, we report
the synthesis and evaluation of few-layer (7x7)-PtTe2-x with an ordered,
well-defined and high-density Te vacancy superlattice. Compared with pristine
PtTe2, (2x2)-PtTe2-x and Pt(111), (7x7)-PtTe2-x exhibits superior HER
activities in both acidic and alkaline electrolytes due to its rich structures
of undercoordinated Pt sites. Furthermore, the (7x7)-PtTe2-x sample features
outstanding catalytic stability even compared to the state-of-the-art Pt/C
catalyst. Theoretical calculations reveal that the interactions between various
undercoordinated Pt sites due to proximity effect can provide superior
undercoordinated Pt sites for hydrogen adsorption and water dissociation. This
work will enrich the understanding of the relationship between defect
structures and electrocatalytic activities and provide a promising route to
develop efficient Pt-based TMD electrocatalysts