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Coordination polymer structure and revisited hydrogen evolution catalytic mechanism for amorphous molybdenum sulfide
- Source :
- Nature Materials, Nature Materials, Nature Publishing Group, 2016, 15 (6), pp.640-646. ⟨10.1038/nmat4588⟩, Nature Materials, 2016, 15 (6), pp.640-646. ⟨10.1038/nmat4588⟩
- Publication Year :
- 2016
- Publisher :
- HAL CCSD, 2016.
-
Abstract
- International audience; Molybdenum sulfides are very attractive noble-metal-free electrocatalysts for the hydrogen evolution reaction (HER) from water. The atomic structure and identity of the catalytically active sites have been well established for crystalline molybdenum disulfide (c-MoS2) but not for amorphous molybdenum sulfide (a-MoSx), which exhibits significantly higher HER activity compared to its crystalline counterpart. Here we show that HER-active a-MoSx, prepared either as nanoparticles or as films, is a molecular-based coordination polymer consisting of discrete [Mo3S13]2- building blocks. Of the three terminal disulfide (S22-) ligands within these clusters, two are shared to form the polymer chain. The third one remains free and generates molybdenum hydride moieties as the active site under H2 evolution conditions. Such a molecular structure therefore provides a basis for revisiting the mechanism of a-MoSx catalytic activity, as well as explaining some of its special properties such as reductive activation and corrosion. Our findings open up new avenues for the rational optimization of this HER electrocatalyst as an alternative to platinum.
- Subjects :
- Coordination polymer
Inorganic chemistry
chemistry.chemical_element
02 engineering and technology
010402 general chemistry
Electrocatalyst
01 natural sciences
Article
Catalysis
chemistry.chemical_compound
General Materials Science
Molybdenum disulfide
biology
Hydride
Mechanical Engineering
Active site
General Chemistry
[CHIM.CATA]Chemical Sciences/Catalysis
[CHIM.MATE]Chemical Sciences/Material chemistry
021001 nanoscience & nanotechnology
Condensed Matter Physics
0104 chemical sciences
Crystallography
chemistry
Mechanics of Materials
Molybdenum
biology.protein
0210 nano-technology
Platinum
Subjects
Details
- Language :
- English
- ISSN :
- 14761122 and 14764660
- Database :
- OpenAIRE
- Journal :
- Nature Materials, Nature Materials, Nature Publishing Group, 2016, 15 (6), pp.640-646. ⟨10.1038/nmat4588⟩, Nature Materials, 2016, 15 (6), pp.640-646. ⟨10.1038/nmat4588⟩
- Accession number :
- edsair.doi.dedup.....6ba6b24f6733e70e13d9ff73b2b82aaa