Journal
CHINESE JOURNAL OF CATALYSIS
Volume 39, Issue 3, Pages 401-406Publisher
SCIENCE PRESS
DOI: 10.1016/S1872-2067(17)62945-0
Keywords
Hydrogen evolution reaction; Molybdenum sulfide; Electrocatalyst; In-situ Raman spectroscopy; Artificial photosynthesis; Clean energy
Funding
- JSPS [26288092]
- Grants-in-Aid for Scientific Research [26288092] Funding Source: KAKEN
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Molybdenum sulfides are promising electrocatalysts for the hydrogen evolution reaction (HER). Sand 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 H-2 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, Mo-3-mu S-3, 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 Mo-3-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. (C) 2018, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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