A Mononuclear Tungsten Photocatalyst for H2 Production

Aron J. Huckaba, Hunter Shirley, Robert W. Lamb, Steve Guertin, Shane Autry, Hammad Cheema, Kallol Talukdar, Tanya Jones, Jonah W. Jurss, Amala Dass, Nathan I. Hammer, Russell H. Schmehl, Charles Edwin Webster, Jared H. Delcamp

Research output: Contribution to journalArticlepeer-review

24 Scopus citations

Abstract

We report herein a mononuclear, homogeneous photocatalyst for H2 production with sunlight. The synthesis and characterization of a (pyridyl)-N-heterocyclic carbene tungsten tetracarbonyl complex W(pyNHC)(CO)4 is described, and its application as a precatalyst for photocatalytic generation of H2 is evaluated. Electrochemical and photophysical studies were used to characterize and evaluate the precatalyst and in situ generated catalyst [W(pyNHC)(CO)3] for the visible-light-driven production of H2 in the presence of triflic acid and decamethylferrocene without an additional photosensitizer. Under irradiation with a solar-simulated spectrum, a catalyst turnover number (TON) of >17 in 3 h of reaction time is observed for the production of H2 with this system, which compares favorably to a prior reported (multinuclear) homogeneous photocatalyst using visible light (4 TON). Photonic energy was found to be necessary to access the active catalysts from the precatalyst and in the catalytic cycle. A mechanism is detailed on the basis of a combined photophysical and computational approach.

Original languageEnglish
Pages (from-to)4838-4847
Number of pages10
JournalACS Catalysis
Volume8
Issue number6
DOIs
StatePublished - Jun 1 2018

Bibliographical note

Publisher Copyright:
© 2018 American Chemical Society.

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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