Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film

doi:10.1021/acs.nanolett.7b04426

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

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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:

^[1];

^[2]; Ding, Zijing ^[3]; Zhang, Yu-Yang ^[4]; Wan, Dongyang ^[5];

^[1]; Chen, Zhongxin ^[1];

^[3]; Dan, Jiadong ^[6]; Fu, Wei ^[3]; Geng, Dechao ^[3]; Song, Peng ^[3];

^[7]; Venkatesan, T. ^[8]; Pantelides, Sokrates T. ^[9]; Pennycook, Stephen J. ^[6];

^[10];

^[3]

Department of Chemistry and Centre for Advanced 2D Materials (CA2DM), National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore; NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore, 13 Centre for Life Sciences, #05-01, 28 Medical Drive, Singapore 117456, Singapore
Department of Chemistry and Centre for Advanced 2D Materials (CA2DM), National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore; SinBeRISE CREATE, National Research Foundation, CREATE Tower, 1 Create Way, Singapore 138602, Singapore
Department of Chemistry and Centre for Advanced 2D Materials (CA2DM), National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore
School of Physical Sciences and CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100049, China; Department of Physics and Astronomy and Department of Electrical Engineering and Computer Science, Vanderbilt University, Nashville, Tennessee 37235, United States
NUSNNI-NanoCore, National University of Singapore, 117411, Singapore
NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore, 13 Centre for Life Sciences, #05-01, 28 Medical Drive, Singapore 117456, Singapore; Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, 117575, Singapore
Institute of Chemical and Engineering Sciences, Agency for Science, Technology and Research, 1 Pesek Road, Jurong Island 627833, Singapore
NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore, 13 Centre for Life Sciences, #05-01, 28 Medical Drive, Singapore 117456, Singapore; NUSNNI-NanoCore, National University of Singapore, 117411, Singapore; Department of Materials Science and Engineering, National University of Singapore, 9 Engineering Drive 1, 117575, Singapore; Department of Electrical and Computer Engineering, National University of Singapore, 9 Engineering Drive 1, 117575, Singapore; Department of Physics, National University of Singapore, 2 Science Drive 3, 517551, Singapore
Department of Physics and Astronomy and Department of Electrical Engineering and Computer Science, Vanderbilt University, Nashville, Tennessee 37235, United States
School of Physical Sciences and CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100049, China

Publication Date:: 2017-12-15

Research Org.:: Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1484744

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

Country of Publication:: United States

Language:: English

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.

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                    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.

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                    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. Fri .  
        "Mo-Terminated Edge Reconstructions in Nanoporous Molybdenum Disulfide Film".  United States.  doi:10.1021/acs.nanolett.7b04426.  https://www.osti.gov/servlets/purl/1484744.

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@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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