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Title: Rhenium-Doped and Stabilized MoS 2 Atomic Layers with Basal-Plane Catalytic Activity

Abstract

The development of stable and efficient hydrogen evolution reaction (HER) catalysts is essential for the production of hydrogen as a clean energy resource. A combination of experiment and theory demonstrates that the normally inert basal planes of 2D layers of MoS 2 can be made highly catalytically active for the HER when alloyed with rhenium (Re). The presence of Re at the ≈50% level converts the material to a stable distorted tetragonal (DT) structure that shows enhanced HER activity as compared to most of the MoS 2-based catalysts reported in the literature. More importantly, this new alloy catalyst shows much better stability over time and cycling than lithiated 1T-MoS 2. Density functional theory calculations find that the role of Re is only to stabilize the DT structure, while catalysis occurs primarily in local Mo-rich DT configurations, where the HER catalytic activity is very close to that in Pt. The study provides a new strategy to improve the overall HER performance of MoS 2-based materials via chemical doping.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [6];  [7];  [5];  [1]; ORCiD logo [8]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Rice Univ., Houston, TX (United States); Beihang Univ., Beijing (China)
  3. Vanderbilt Univ., Nashville, TN (United States)
  4. Vanderbilt Univ., Nashville, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)
  5. Rice Univ., Houston, TX (United States)
  6. Univ. of Science and Technology, Hefei Anhui (China)
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Vanderbilt Univ., Nashville, TN (United States)
  8. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1490572
Alternate Identifier(s):
OSTI ID: 1479536
Grant/Contract Number:  
AC05-00OR22725; FG02-09ER46554; AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 51; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Yang, Shi-Ze, Gong, Yongji, Manchanda, Priyanka, Zhang, Yu-Yang, Ye, Gonglan, Chen, Shuangming, Song, Li, Pantelides, Sokrates T., Ajayan, Pulickel M., Chisholm, Matthew F., and Zhou, Wu. Rhenium-Doped and Stabilized MoS2 Atomic Layers with Basal-Plane Catalytic Activity. United States: N. p., 2018. Web. doi:10.1002/adma.201803477.
Yang, Shi-Ze, Gong, Yongji, Manchanda, Priyanka, Zhang, Yu-Yang, Ye, Gonglan, Chen, Shuangming, Song, Li, Pantelides, Sokrates T., Ajayan, Pulickel M., Chisholm, Matthew F., & Zhou, Wu. Rhenium-Doped and Stabilized MoS2 Atomic Layers with Basal-Plane Catalytic Activity. United States. doi:10.1002/adma.201803477.
Yang, Shi-Ze, Gong, Yongji, Manchanda, Priyanka, Zhang, Yu-Yang, Ye, Gonglan, Chen, Shuangming, Song, Li, Pantelides, Sokrates T., Ajayan, Pulickel M., Chisholm, Matthew F., and Zhou, Wu. Thu . "Rhenium-Doped and Stabilized MoS2 Atomic Layers with Basal-Plane Catalytic Activity". United States. doi:10.1002/adma.201803477.
@article{osti_1490572,
title = {Rhenium-Doped and Stabilized MoS2 Atomic Layers with Basal-Plane Catalytic Activity},
author = {Yang, Shi-Ze and Gong, Yongji and Manchanda, Priyanka and Zhang, Yu-Yang and Ye, Gonglan and Chen, Shuangming and Song, Li and Pantelides, Sokrates T. and Ajayan, Pulickel M. and Chisholm, Matthew F. and Zhou, Wu},
abstractNote = {The development of stable and efficient hydrogen evolution reaction (HER) catalysts is essential for the production of hydrogen as a clean energy resource. A combination of experiment and theory demonstrates that the normally inert basal planes of 2D layers of MoS2 can be made highly catalytically active for the HER when alloyed with rhenium (Re). The presence of Re at the ≈50% level converts the material to a stable distorted tetragonal (DT) structure that shows enhanced HER activity as compared to most of the MoS2-based catalysts reported in the literature. More importantly, this new alloy catalyst shows much better stability over time and cycling than lithiated 1T-MoS2. Density functional theory calculations find that the role of Re is only to stabilize the DT structure, while catalysis occurs primarily in local Mo-rich DT configurations, where the HER catalytic activity is very close to that in Pt. The study provides a new strategy to improve the overall HER performance of MoS2-based materials via chemical doping.},
doi = {10.1002/adma.201803477},
journal = {Advanced Materials},
issn = {0935-9648},
number = 51,
volume = 30,
place = {United States},
year = {2018},
month = {10}
}

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Works referenced in this record:

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