Activating a [FeFe] Hydrogenase Mimic for Hydrogen Evolution under Visible Light

in: Angewandte Chemie-International Edition (2022)
Buday, Philipp; Kasahara, Chizuru; Hofmeister, Elisabeth; Kowalczyk, Daniel; Farh, Micheal K.; Riediger, Saskia; Schulz, Martin; Wächtler, Maria; Furukawa, Shunsuke; Saito, Masaichi; Ziegenbalg, Dirk; Gräfe, Stefanie; Bäuerle, Peter; Kupfer, Stephan; Dietzek-Ivanšić, Benjamin; Weigand, Wolfgang
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 -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 [FeIFe0] species – in accordance with theoretical calculations – presumably driving photocatalysis effectively (TON ≈ 210).

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