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 language | English |
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Pages (from-to) | 4838-4847 |
Number of pages | 10 |
Journal | ACS Catalysis |
Volume | 8 |
Issue number | 6 |
DOIs | |
State | Published - Jun 1 2018 |
Bibliographical note
Publisher Copyright:© 2018 American Chemical Society.
ASJC Scopus subject areas
- Catalysis
- General Chemistry