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Title: Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film

Abstract

The catalytic and magnetic properties of molybdenum disulfide (MoS2) are significantly enhanced by the presence of edge sites. One way to obtain a high density of edge sites in a two-dimensional (2D) film is by introducing porosity. However, the large-scale bottom-up synthesis of a porous 2D MoS2 film remains challenging and the correlation of growth conditions to the atomic structures of the edges is not well understood. Here, using molecular beam epitaxy, we prepare wafer-scale nanoporous MoS2 films under conditions of high Mo flux and study their catalytic and magnetic properties. Atomic-resolution electron microscopy imaging of the pores reveals two new types of reconstructed Mo-terminated edges, namely, a distorted 1T (DT) edge and the Mo-Klein edge. Nanoporous MoS2 films are magnetic up to 400 K, which is attributed to the presence of Mo-terminated edges with unpaired electrons, as confirmed by density functional theory calculation. The small hydrogen adsorption free energy at these Mo-terminated edges leads to excellent activity for the hydrogen evolution reaction.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [3];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1];  [1];  [1]; ORCiD logo [4];  [1];  [5];  [1]; ORCiD logo [6]; ORCiD logo [1]
  1. National Univ. of Singapore (Singapore)
  2. National Univ. of Singapore (Singapore); National Research Foundation (Singapore)
  3. Chinese Academy of Sciences (CAS), Beijing (China); Vanderbilt Univ., Nashville, TN (United States)
  4. Agency for Science, Technology and Research (Singapore)
  5. Vanderbilt Univ., Nashville, TN (United States)
  6. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Vanderbilt Univ., Nashville, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1484744
Alternate Identifier(s):
OSTI ID: 1597866
Grant/Contract Number:  
FG02-09ER46554; AC02- 05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Molybdenum disulfide; edge magnetism; hydrogen evolution reactions; transition metal dichalcogenides

Citation Formats

Zhao, Xiaoxu, Fu, Deyi, Ding, Zijing, Zhang, Yu-Yang, Wan, Dongyang, Tan, Sherman J. R., Chen, Zhongxin, Leng, Kai, Dan, Jiadong, Fu, Wei, Geng, Dechao, Song, Peng, Du, Yonghua, Venkatesan, T., Pantelides, Sokrates T., Pennycook, Stephen J., Zhou, Wu, and Loh, Kian Ping. Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film. United States: N. p., 2017. Web. doi:10.1021/acs.nanolett.7b04426.
Zhao, Xiaoxu, Fu, Deyi, Ding, Zijing, Zhang, Yu-Yang, Wan, Dongyang, Tan, Sherman J. R., Chen, Zhongxin, Leng, Kai, Dan, Jiadong, Fu, Wei, Geng, Dechao, Song, Peng, Du, Yonghua, Venkatesan, T., Pantelides, Sokrates T., Pennycook, Stephen J., Zhou, Wu, & Loh, Kian Ping. Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film. United States. doi:10.1021/acs.nanolett.7b04426.
Zhao, Xiaoxu, Fu, Deyi, Ding, Zijing, Zhang, Yu-Yang, Wan, Dongyang, Tan, Sherman J. R., Chen, Zhongxin, Leng, Kai, Dan, Jiadong, Fu, Wei, Geng, Dechao, Song, Peng, Du, Yonghua, Venkatesan, T., Pantelides, Sokrates T., Pennycook, Stephen J., Zhou, Wu, and Loh, Kian Ping. Mon . "Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film". United States. doi:10.1021/acs.nanolett.7b04426. https://www.osti.gov/servlets/purl/1484744.
@article{osti_1484744,
title = {Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film},
author = {Zhao, Xiaoxu and Fu, Deyi and Ding, Zijing and Zhang, Yu-Yang and Wan, Dongyang and Tan, Sherman J. R. and Chen, Zhongxin and Leng, Kai and Dan, Jiadong and Fu, Wei and Geng, Dechao and Song, Peng and Du, Yonghua and Venkatesan, T. and Pantelides, Sokrates T. and Pennycook, Stephen J. and Zhou, Wu and Loh, Kian Ping},
abstractNote = {The catalytic and magnetic properties of molybdenum disulfide (MoS2) are significantly enhanced by the presence of edge sites. One way to obtain a high density of edge sites in a two-dimensional (2D) film is by introducing porosity. However, the large-scale bottom-up synthesis of a porous 2D MoS2 film remains challenging and the correlation of growth conditions to the atomic structures of the edges is not well understood. Here, using molecular beam epitaxy, we prepare wafer-scale nanoporous MoS2 films under conditions of high Mo flux and study their catalytic and magnetic properties. Atomic-resolution electron microscopy imaging of the pores reveals two new types of reconstructed Mo-terminated edges, namely, a distorted 1T (DT) edge and the Mo-Klein edge. Nanoporous MoS2 films are magnetic up to 400 K, which is attributed to the presence of Mo-terminated edges with unpaired electrons, as confirmed by density functional theory calculation. The small hydrogen adsorption free energy at these Mo-terminated edges leads to excellent activity for the hydrogen evolution reaction.},
doi = {10.1021/acs.nanolett.7b04426},
journal = {Nano Letters},
number = 1,
volume = 18,
place = {United States},
year = {2017},
month = {12}
}

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