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

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

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Publication Details

Journal
ACS Nano
Published
2024-11-12
DOI
https://doi.org/10.1021/acsnano.4c10085
Citations
17
Primary Topic
2D Materials and Applications
Type
article
Field-Weighted Citation Impact
1.99

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article

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

Fangfei Ming, Xiao Hai, Nan Xu, Tao Sun et al.
17 citations
ACS Nano
2D Materials and Applications
1.99
article

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

Fangfei Ming, Xiao Hai, Nan Xu, Tao Sun, Xin Xu, Ping Cui, Jiong Lu, Yaping Ma, Jing Li, Hao Li, Chenhui Wang, Xue Liu, Ying Zhang, Zhenyu Zhang, Quan Zhang, Weifeng Zhang, Lei Li, Guowei Liu, Shuming Yu, Kedong Wang, Jiangang Yang, Xudong Xiao, Xuechun Wang
article en
17 citations

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

ACS NanoVol. 18(47)
University of Science and Technology of China (CN), Anhui University (CN), Sun Yat-sen University (CN), National University of Singapore (SG), Southern University of Science and Technology (CN), Henan University of Technology (CN), Wuhan University (CN), Northwest University (CN), Henan Academy of Sciences (CN), Hubei Normal University (CN), Beihang University (CN)
National Natural Science Foundation of China, Chinese Academy of Sciences, Sun Yat-sen University, Ministry of Science and Technology of the People's Republic of China, Henan University, Natural Science Foundation of Henan Province, Wuhan University, Basic and Applied Basic Research Foundation of Guangdong Province
Industry, innovation and infrastructure
Openalex Percentile: Top 9%
2D Materials and Applications
1.99
DOISourceOpenAlex
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