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Published on: October 5, 2019
Activating a [FeFe] Hydrogenase Mimic for Hydrogen Evolution under Visible Light
Philipp Buday1, Chizuru Kasahara1,2, Elisabeth Hofmeister3
1Institute of Inorganic and Analytical Chemistry, Friedrich Schiller University Jena, Humboldtstraße 8, 07743, Jena, Germany.
Abstract:
Inspired by the active center of the natural [FeFe] hydrogenases, we designed a compact and precious metal-free photosensitizer-catalyst dyad (PS-CAT) for photocatalytic hydrogen evolution under visible light irradiation. PS-CAT represents a prototype dyad comprising π-conjugated oligothiophenes as light absorbers. PS-CAT and its interaction with the sacrificial donor 1,3-dimethyl-2-phenylbenzimidazoline were studied by steady-state and time-resolved spectroscopy coupled with electrochemical techniques and visible light-driven photocatalytic investigations. Operando EPR spectroscopy revealed the formation of an active [FeI Fe0 ] species-in accordance with theoretical calculations-presumably driving photocatalysis effectively (TON≈210).
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