Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2
Understanding the reaction mechanism for the catalytic process is essential to the rational design and synthesis of highly efficient catalysts. MoS2 has been reported to be an efficient catalyst toward the electrochemical hydrogen evolution reaction (HER), but it still lacks direct experimental evid...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Online Access: | https://hdl.handle.net/10356/144116 |
| _version_ | 1826123510334881792 |
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| author | Chen, Junze Liu, Guigao Zhu, Yue-zhou Su, Min Yin, Pengfei Wu, Xue-jun Lu, Qipeng Tan, Chaoliang Zhao, Meiting Liu, Zhengqing Yang, Weimin Li, Hai Nam, Gwang-Hyeon Zhang, Liping Chen, Zhenhua Huang, Xiao Radjenovic, Petar M. Huang, Wei Tian, Zhong-qun Li, Jian-feng Zhang, Hua |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Chen, Junze Liu, Guigao Zhu, Yue-zhou Su, Min Yin, Pengfei Wu, Xue-jun Lu, Qipeng Tan, Chaoliang Zhao, Meiting Liu, Zhengqing Yang, Weimin Li, Hai Nam, Gwang-Hyeon Zhang, Liping Chen, Zhenhua Huang, Xiao Radjenovic, Petar M. Huang, Wei Tian, Zhong-qun Li, Jian-feng Zhang, Hua |
| author_sort | Chen, Junze |
| collection | NTU |
| description | Understanding the reaction mechanism for the catalytic process is essential to the rational design and synthesis of highly efficient catalysts. MoS2 has been reported to be an efficient catalyst toward the electrochemical hydrogen evolution reaction (HER), but it still lacks direct experimental evidence to reveal the mechanism for MoS2-catalyzed electrochemical HER process at the atomic level. In this work, we develop a wet-chemical synthetic method to prepare the single-layer MoS2-coated polyhedral Ag core-shell heterostructure (Ag@MoS2) with tunable sizes as efficient catalysts for the electrochemical HER. The Ag@MoS2 core-shell heterostructures are used as ideal platforms for the real-time surface-enhanced Raman spectroscopy (SERS) study owing to the strong electromagnetic field generated in the plasmonic Ag core. The in situ SERS results provide solid Raman spectroscopic evidence proving the S-H bonding formation on the MoS2 surface during the HER process, suggesting that the S atom of MoS2 is the catalytic active site for the electrochemical HER. It paves the way on the design and synthesis of heterostructures for exploring their catalytic mechanism at atomic level based on the in situ SERS measurement. |
| first_indexed | 2024-10-01T06:05:51Z |
| format | Journal Article |
| id | ntu-10356/144116 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:05:51Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1441162023-07-14T15:54:09Z Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 Chen, Junze Liu, Guigao Zhu, Yue-zhou Su, Min Yin, Pengfei Wu, Xue-jun Lu, Qipeng Tan, Chaoliang Zhao, Meiting Liu, Zhengqing Yang, Weimin Li, Hai Nam, Gwang-Hyeon Zhang, Liping Chen, Zhenhua Huang, Xiao Radjenovic, Petar M. Huang, Wei Tian, Zhong-qun Li, Jian-feng Zhang, Hua School of Materials Science and Engineering Department of Chemistry, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong, China. State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, Department of Physics, College of Chemistry and Chemical Engineering, and College of Energy, Xiamen University, Xiamen, China. State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Institute of Advanced Materials (IAM), Nanjing Tech University (NanjingTech) Jinzhou Medical University Key Laboratory for Organic Electronics and Information Displays, Institute of Advanced Materials, Nanjing University of Posts and Telecommunications, Nanjing Shaanxi Institute of Flexible Electronics, Northwestern Polytechnical University, Xi’an, China Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Hong Kong, China Engineering::Materials Core-Shell Heterostructure Single-Layer MoS2 Understanding the reaction mechanism for the catalytic process is essential to the rational design and synthesis of highly efficient catalysts. MoS2 has been reported to be an efficient catalyst toward the electrochemical hydrogen evolution reaction (HER), but it still lacks direct experimental evidence to reveal the mechanism for MoS2-catalyzed electrochemical HER process at the atomic level. In this work, we develop a wet-chemical synthetic method to prepare the single-layer MoS2-coated polyhedral Ag core-shell heterostructure (Ag@MoS2) with tunable sizes as efficient catalysts for the electrochemical HER. The Ag@MoS2 core-shell heterostructures are used as ideal platforms for the real-time surface-enhanced Raman spectroscopy (SERS) study owing to the strong electromagnetic field generated in the plasmonic Ag core. The in situ SERS results provide solid Raman spectroscopic evidence proving the S-H bonding formation on the MoS2 surface during the HER process, suggesting that the S atom of MoS2 is the catalytic active site for the electrochemical HER. It paves the way on the design and synthesis of heterostructures for exploring their catalytic mechanism at atomic level based on the in situ SERS measurement. Ministry of Education (MOE) Accepted version This research was financially supported by MOE under AcRF Tier 1 (Project No. 2017-T1-002-119) and AcRF Tier 2 (Project No. MOE2017-T2-1-162; MOE2016-T2-2-103) in Singapore, NTU’s Start-Up Grant (Project No. M4081296.070.500000), and NSFC (21775127 and 21522508). H.Z. acknowledges the financial sup-port from ITC via the Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), and the grants (Project No. 9380100, 9610478 and 1886921) in the City University of Hong Kong. 2020-10-14T02:16:37Z 2020-10-14T02:16:37Z 2020 Journal Article Chen, J., Liu, G., Zhu, Y.-z., Su, M., Yin, P., Wu, X.-j., ... Zhang, H. (2020). Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2. Journal of the American Chemical Society, 142(15), 7161–7167. doi:10.1021/jacs.0c01649 1520-5126 https://hdl.handle.net/10356/144116 10.1021/jacs.0c01649 32207969 15 142 7161 7167 en AcRF Tier 1 2017-T1-002-119 MOE2017-T2-1-162 MOE2016-T2-2-103 Start-Up Grant No. M4081296.070.500000 NSFC (21775127 and 21522508) Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM) Grant Project No. 9380100, 9610478 and 1886921) in the City University of Hong Kong. Journal of the American Chemical Society This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/jacs.0c01649 application/pdf |
| spellingShingle | Engineering::Materials Core-Shell Heterostructure Single-Layer MoS2 Chen, Junze Liu, Guigao Zhu, Yue-zhou Su, Min Yin, Pengfei Wu, Xue-jun Lu, Qipeng Tan, Chaoliang Zhao, Meiting Liu, Zhengqing Yang, Weimin Li, Hai Nam, Gwang-Hyeon Zhang, Liping Chen, Zhenhua Huang, Xiao Radjenovic, Petar M. Huang, Wei Tian, Zhong-qun Li, Jian-feng Zhang, Hua Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 |
| title | Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 |
| title_full | Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 |
| title_fullStr | Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 |
| title_full_unstemmed | Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 |
| title_short | Ag@MoS2 core-shell heterostructure as SERS platform to reveal the hydrogen evolution active sites of single-layer MoS2 |
| title_sort | ag mos2 core shell heterostructure as sers platform to reveal the hydrogen evolution active sites of single layer mos2 |
| topic | Engineering::Materials Core-Shell Heterostructure Single-Layer MoS2 |
| url | https://hdl.handle.net/10356/144116 |
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