Citation: Yamei Li, Ryuhei Nakamura. Structural change of molybdenum sulfide facilitates the electrocatalytic hydrogen evolution reaction at neutral pH as revealed by in situ Raman spectroscopy[J]. Chinese Journal of Catalysis, ;2018, 39(3): 401-406. doi: 10.1016/S1872-2067(17)62945-0 shu

Structural change of molybdenum sulfide facilitates the electrocatalytic hydrogen evolution reaction at neutral pH as revealed by in situ Raman spectroscopy

Yamei Li ^a, ,
Ryuhei Nakamura ^a,b

a Biofunctional Catalyst Research Team, RIKEN Center for Sustainable Resource Science(CSRS), 2-1 Hirosawa, Wako, Saitama 351-0198, Japan;
b Earth-Life Science Institute(ELSI), Tokyo Institute of Technology, 2-12-1-I7 E Ookayama, Meguro-ku, Tokyo 152-8550, Japan

Received Date: 27 September 2017
Revised Date: 26 October 2017

Fund Project: This work was supported by a JSPS Grant-in-Aid for Scientific Research (26288092).

Molybdenum sulfides are promising electrocatalysts for the hydrogen evolution reaction (HER). S-and Mo-related species have been proposed as the active site for forming adsorbed hydrogen to initiate the HER; however, the nature of the interaction between Mo centers and S ligands is unclear. Further, the development of cost-effective water-splitting systems using neutral water as a proton source for H₂ evolution is highly desirable, whereas the mechanism of the HER at neutral pH is rarely discussed. Here, the structural change in the Mo-Mo and S-S species in a synthesized molybdenum sulfide was monitored at neutral pH using in situ electrochemical Raman spectroscopy. Analysis of the potential dependent Raman spectra revealed that the band assigned to a terminal S-S species emerged along with synchronized changes in the frequency of the Mo-Mo, Mo₃-μ₃S, and Mo-S vibrational bands. This indicates that Mo-Mo bonds and terminal S-S ligands play synergistic roles in facilitating hydrogen evolution, likely via the internal reorganization of trinuclear Mo₃-thio species. The nature and role of metal-ligand interactions in the HER revealed in this study demonstrated a mechanism that is distinct from those reported previously in which the S or Mo sites function independently.
- Hydrogen evolution reaction,
- Molybdenum sulfide,
- Electrocatalyst,
- In-situ Raman spectroscopy,
- Artificial photosynthesis,
- Clean energy
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