[FeFe] Hydrogenase based Prototype Photosensitizer-Catalyst Dyad for Hydrogen Generation under Visible Light [post]

Philipp Buday, Chizuru Kasahara, Elisabeth Hofmeister, Daniel Kowalczyk, Michael K. Farh, Saskia Riediger, Martin Schulz, Maria Wächtler, Shunsuke Furukawa, Masaichi Saito, Dirk Ziegenbalg, Stefanie Gräfe (+4 others)
2021 unpublished
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 pi-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
more » ... chniques and visible light-driven photocatalytic investigations. Operando EPR spectroscopy revealed the formation of an active [Fe(I)Fe(0)] species – in accordance with theoretical calculations – presumably driving photocatalysis effectively (TON ≈ 210).
doi:10.33774/chemrxiv-2021-1wh3l fatcat:r723wvk6y5eeffjcluvozvyzxa