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

Jakob Kibsgaard, Thomas F. Jaramillo, Flemming Besenbacher

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Identifying and understanding the active sites responsible for reaction turnover is critical to developing improved catalysts. For the hydrogen-evolution reaction (HER), MoS 2 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.
Original languageEnglish
JournalNature Chemistry
Volume6
Issue number3
Pages (from-to)248-253
Number of pages6
ISSN1755-4330
DOIs
Publication statusPublished - 2014
Externally publishedYes

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