Ordered clustering of single atomic Te vacancies in atomically thin PtTe2 promotes hydrogen evolution catalysis

Xinzhe Li; Yiyun Fang; Jun Wang; Hanyan Fang; Shibo Xi; Xiaoxu Zhao; Danyun Xu; Haomin Xu; Wei Yu; Xiao Hai; Cheng Chen; Chuanhao Yao; Hua Bing Tao; Alexander G. R. Howe; Stephen J. Pennycook; Bin Liu; Jiong Lu; Chenliang Su

doi:10.1038/s41467-021-22681-4

Ordered clustering of single atomic Te vacancies in atomically thin PtTe₂ promotes hydrogen evolution catalysis

Xinzhe Li, Yiyun Fang, Jun Wang, Hanyan Fang, Shibo Xi, Xiaoxu Zhao, Danyun Xu, Haomin Xu, Wei Yu, Xiao Hai, Cheng Chen, Chuanhao Yao, Hua Bing Tao, Alexander G. R. Howe, Stephen J. Pennycook, Bin Liu^*, Jiong Lu^*, Chenliang Su^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

130 Citations (Scopus)

28 Downloads (CityUHK Scholars)

Abstract

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. © 2021, The Author(s).

Original language	English
Article number	2351
Journal	Nature Communications
Volume	12
Online published	21 Apr 2021
DOIs	https://doi.org/10.1038/s41467-021-22681-4
Publication status	Published - 2021
Externally published	Yes

Publisher's Copyright Statement

This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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Li, X., Fang, Y., Wang, J., Fang, H., Xi, S., Zhao, X., Xu, D., Xu, H., Yu, W., Hai, X., Chen, C., Yao, C., Tao, H. B., Howe, A. G. R., Pennycook, S. J., Liu, B., Lu, J., & Su, C. (2021). Ordered clustering of single atomic Te vacancies in atomically thin PtTe₂ promotes hydrogen evolution catalysis. Nature Communications, 12, Article 2351. https://doi.org/10.1038/s41467-021-22681-4

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title = "Ordered clustering of single atomic Te vacancies in atomically thin PtTe2 promotes hydrogen evolution catalysis",

abstract = "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. {\textcopyright} 2021, The Author(s).",

author = "Xinzhe Li and Yiyun Fang and Jun Wang and Hanyan Fang and Shibo Xi and Xiaoxu Zhao and Danyun Xu and Haomin Xu and Wei Yu and Xiao Hai and Cheng Chen and Chuanhao Yao and Tao, {Hua Bing} and Howe, {Alexander G. R.} and Pennycook, {Stephen J.} and Bin Liu and Jiong Lu and Chenliang Su",

year = "2021",

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T1 - Ordered clustering of single atomic Te vacancies in atomically thin PtTe2 promotes hydrogen evolution catalysis

AU - Li, Xinzhe

AU - Fang, Yiyun

AU - Wang, Jun

AU - Fang, Hanyan

AU - Xi, Shibo

AU - Zhao, Xiaoxu

AU - Xu, Danyun

AU - Xu, Haomin

AU - Yu, Wei

AU - Hai, Xiao

AU - Chen, Cheng

AU - Yao, Chuanhao

AU - Tao, Hua Bing

AU - Howe, Alexander G. R.

AU - Pennycook, Stephen J.

AU - Liu, Bin

AU - Lu, Jiong

AU - Su, Chenliang

PY - 2021

Y1 - 2021

N2 - 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. © 2021, The Author(s).

AB - 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. © 2021, The Author(s).

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DO - 10.1038/s41467-021-22681-4

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