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

15 October 2021, Version 2


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 techniques 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).


Photocatalytic hydrogen generation
Quantum Chemistry
[FeFe] hydrogenase mimic
Electron paramagnetic resonance (EPR) spectroscopy
Conjugated oligothiophenes
Photosensitizer-catalyst dyad
Time-resolved spectroscopy

Supplementary materials

Supporting Information
Materials and instrumentation, Synthesis and characterization, NMR spectra, Single crystal X-ray structure determination, Photocatalysis, UV-vis-monitored photocatalysis, Fluorescence quenching in presence of BIH, Time-resolved spectroscopy, EPR spectroscopy, Electrochemical characterization, Computational details, Crystallographic data have been deposited with the Cambridge Crystallographic Data Center as supplementary publication CCDC-2106348


Comments are not moderated before they are posted, but they can be removed by the site moderators if they are found to be in contravention of our Commenting Policy [opens in a new tab] - please read this policy before you post. Comments should be used for scholarly discussion of the content in question. You can find more information about how to use the commenting feature here [opens in a new tab] .
This site is protected by reCAPTCHA and the Google Privacy Policy [opens in a new tab] and Terms of Service [opens in a new tab] apply.