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Nat Chem. 2014 Mar;6(3):248-53. doi: 10.1038/nchem.1853. Epub 2014 Jan 26.

Building an appropriate active-site motif into a hydrogen-evolution catalyst with thiomolybdate [Mo3S13]2- clusters.

Author information

  • 11] Interdisciplinary Nanoscience Center and Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C, Denmark [2] Department of Chemical Engineering, Stanford University, Stanford, California 94305, USA.
  • 2Department of Chemical Engineering, Stanford University, Stanford, California 94305, USA.
  • 3Interdisciplinary Nanoscience Center and Department of Physics and Astronomy, Aarhus University, DK-8000 Aarhus C, Denmark.

Abstract

Identifying and understanding the active sites responsible for reaction turnover is critical to developing improved catalysts. For the hydrogen-evolution reaction (HER), MoS2 has been identified as an active non-noble-metal-based catalyst. However, only edge sites turnover the reaction because the basal planes are catalytically inert. In an effort to develop a scalable HER catalyst with an increased number of active sites, herein we report a Mo-S catalyst (supported thiomolybdate [Mo3S13](2-) nanoclusters) in which most sulfur atoms in the structure exhibit a structural motif similar to that observed at MoS2 edges. Supported sub-monolayers of [Mo3S13](2-) nanoclusters exhibited excellent HER activity and stability in acid. Imaging at the atomic scale with scanning tunnelling microscopy allowed for direct characterization of these supported catalysts. The [Mo3S13](2-) nanoclusters reported herein demonstrated excellent turnover frequencies, higher than those observed for other non-precious metal catalysts synthesized by a scalable route.

PMID:
24557141
DOI:
10.1038/nchem.1853
[PubMed - indexed for MEDLINE]
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