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

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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 ( IF 14.4 ) Pub Date : 2020-03-24 , DOI: 10.1021/jacs.0c01649
Junze Chen ₁ , Guigao Liu ₁ , Yue-zhou Zhu ₂ , Min Su ₂ , Pengfei Yin _{1,

3} , Xue-jun Wu ₄ , Qipeng Lu ₁ , Chaoliang Tan ₁ , Meiting Zhao ₁ , Zhengqing Liu ₁ , Weimin Yang ₂ , Hai Li ₅ , Gwang-Hyeon Nam ₁ , Liping Zhang ₁ , Zhenhua Chen ₆ , Xiao Huang ₅ , Petar M. Radjenovic ₂ , Wei Huang _{5,

7,

8} , Zhong-qun Tian ₂ , Jian-feng Li ₂ , Hua Zhang _{3,

9}

Affiliation

Center for Programmable Materials, School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore
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
Department of Chemistry, City University of Hong Kong, Hong Kong, China
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
Institute of Advanced Materials (IAM), Nanjing Tech University (NanjingTech), 30 South Puzhu Road, Nanjing 211816, China
Jinzhou Medical University, Songpo Road, Jinzhou 121001, China
The Key Laboratory for Organic Electronics and Information Displays, Institute of Advanced Materials, Nanjing University of Posts and Telecommunications, Nanjing 211816, China
Shaanxi Institute of Flexible Electronics, Northwestern Polytechnical University, Xi’an 710072, China
Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Hong Kong China

Understanding the reaction mechanism for the catalytic process is essential to rational design and synthesis of the highly efficient catalyst. MoS2 has been reported to be an efficient catalyst towards the electrochemical hydrogen evolution reaction (HER), but it still lacks direct experimental evidence to reveal the mechanism for MoS2-catalyzed electrochemical HER process at atomic level. In this work, we develop a wet-chemical synthetic method to prepare the single-layer MoS2-coated polyhedral Ag core-shell heter-ostructure (Ag@MoS2) with tunable sizes as efficient catalysts for the electrochemical HER. The Ag@MoS2 core-shell hetero-structures are used as ideal platforms for the real-time surface-enhanced Raman spectroscopy (SERS) study owing to the strong electromagnetic field which is 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.

中文翻译：

Ag@MoS2核壳异质结构作为SERS平台揭示单层MoS2的析氢活性位点

了解催化过程的反应机理对于合理设计和合成高效催化剂至关重要。据报道，MoS2 是电化学析氢反应 (HER) 的有效催化剂，但仍缺乏直接的实验证据来揭示 MoS2 催化电化学 HER 过程的原子级机理。在这项工作中，我们开发了一种湿化学合成方法来制备具有可调尺寸的单层 MoS2 涂层多面体 Ag 核壳异质结构 (Ag@MoS2) 作为电化学 HER 的有效催化剂。由于等离子体 Ag 核中产生的强电磁场，Ag@MoS2 核壳异质结构被用作实时表面增强拉曼光谱 (SERS) 研究的理想平台。原位 SERS 结果提供了固体拉曼光谱证据，证明了在 HER 过程中 MoS2 表面上形成了 SH 键，表明 MoS2 的 S 原子是电化学 HER 的催化活性位点。它为基于原位 SERS 测量在原子水平上探索其催化机制的异质结构的设计和合成铺平了道路。

更新日期：2020-03-24

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