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Ordered Clustering of Single Atomic Te Vacancies in Atomically Thin PtTe2 Promotes Hydrogen Evolution Catalysis


Exposing and stabilizing undercoordinated platinum (Pt) sites and therefore optimizing their adsorption to reactive intermediates offers a desirable strategy to develop highly efficient Pt-based electrocatalysts. However, preparation of atomically controllable Pt-based model catalysts to understand the correlation between electronic structure, adsorption energy, and catalytic properties of atomic Pt sites is still challenging. Herein we report the atomically thin two-dimensional PtTe2 nanosheets with well-dispersed single atomic Te vacancies (Te-SAVs) and atomically well-defined undercoordinated Pt sites as a model electrocatalyst. A controlled thermal treatment drives the migration of the Te-SAVs to form thermodynamically stabilized, ordered Te-SAV clusters, which decreases both the density of states of undercoordinated Pt sites around the Fermi level and the interacting orbital volume of Pt sites. As a result, the binding strength of atomically defined Pt active sites to H intermediates is effectively reduced, which renders PtTe2 nanosheets highly active and stable in hydrogen evolution reaction.

Funding source: National Natural Science Foundation of China (21972094 and 22005244), Guangdong Special Support Program, Pengcheng Scholar program, Shenzhen Peacock Plan (KQJSCX20170727100802505 andKQTD2016053112042971), Natural Science Foundation of Ningbo City (202003N4052), the Ministry of Education of Singapore (AcRF Tier 1 M4011021.120, 2015-T1-002-108, R-143-000-A75-114, R-143-000-B47-114, Tier 1: RG4/20 and Tier 2: MOET2EP10120-0002), and Agency for Science, Technology and Research (A*Star IRG: A20E5c0080).
Related subjects: Production & Supply Chain

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