Photocatalytic hydrogen evolution from FeMoS-based biomimetic chalcogels

Benjamin D. Yuhas, Amanda L. Smeigh, Alexios P. Douvalis, Michael R. Wasielewski, Mercouri G. Kanatzidis

Research output: Contribution to journalArticle

60 Citations (Scopus)

Abstract

The naturally abundant elements used to catalyze photochemical processes in biology have inspired many research efforts into artificial analogues capable of proton reduction or water oxidation under solar illumination. Most biomimetic systems are isolated molecular units, lacking the protective encapsulation afforded by a protein's tertiary structure. As such, advances in biomimetic catalysis must also be driven by the controlled integration of molecular catalysts into larger superstructures. Here, we present porous chalcogenide framework materials that contain biomimetic catalyst groups immobilized in a chalcogenide network. The chalcogels are formed via metathesis reaction between the clusters [Mo 2Fe 6S 8(SPh) 3Cl 6] 3- and [Sn 2S 6] 4- in solution, yielding an extended, porous framework structure with strong optical absorption, high surface area (up to 150 m 2/g), and excellent aqueous stability. Using [Ru(bpy) 3] 2+ as the light-harvesting antenna, the chalcogels are capable of photocatalytically producing hydrogen from mixed aqueous solutions and are stable under constant illumination over a period of at least 3 weeks. We also present improved hydrogen yields in the context of the energy landscape of the chalcogels.

Original languageEnglish
Pages (from-to)10353-10356
Number of pages4
JournalJournal of the American Chemical Society
Volume134
Issue number25
DOIs
Publication statusPublished - Jun 27 2012

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ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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