Ag@MoS 2 Core–Shell Heterostructure as SERS Platform to Reveal the Hydrogen Evolution Active Sites of Single-Layer MoS 2

作者：Junze Chen, Guigao Liu, Yue-Zhou Zhu, Min Su, Pengfei Yin, Xue‐Jun Wu, Qipeng Lu, Chaoliang Tan, Meiting Zhao, Zhengqing Liu, Weimin Yang, Hai Li, Gwang‐Hyeon Nam, Liping Zhang, Zhenhua Chen, Xiao Huang, Petar M. Radjenovic, Wei Huang, Zhong‐Qun Tian, Jian‐Feng Li, Hua Zhang · 发表于：Journal of the American Chemical Society · 年份：2020 · DOI：10.1021/jacs.0c01649 · 被引用次数：281 · 研究领域：Electrocatalysts for Energy Conversion、2D Materials and Applications、Machine Learning in Materials Science

Understanding the reaction mechanism for the catalytic process is essential to the rational design and synthesis of highly efficient catalysts. MoS 2 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 MoS 2 -catalyzed electrochemical HER process at the atomic level. In this work, we develop a wet-chemical synthetic method to prepare the single-layer MoS 2 -coated polyhedral Ag core–shell heterostructure (Ag@MoS 2 ) with tunable sizes as efficient catalysts for the electrochemical HER. The Ag@MoS 2 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 MoS 2 surface during the HER process, suggesting that the S atom of MoS 2 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.