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Ultrafast Electron Transfer from CdSe Quantum Dots to a [FeFe]-Hydrogenase Mimic

preprint
submitted on 29.03.2021, 14:21 and posted on 31.03.2021, 04:49 by Alexander Schleusener, Mathias Micheel, Stefan Benndorf, Markus Rettenmayr, Wolfgang Weigand, Maria Wächtler
The combination of CdSe nanoparticles as photosensitizers and [FeFe]-hydrogenase mimics is known to result in efficient systems for light-driven hydrogen generation. Nevertheless, little is known about the details of the light-induced charge-transfer processes. Here we investigate the timescale of light-induced electron transfer between CdSe quantum dots and a simple [FeFe]-hydrogenase mimic adsorbed on the surface of the quantum dot under non-catalytic conditions. Our time-resolved spectroscopic investigation shows that hot electron transfer on a sub-ps timescale and band-edge electron transfer on a sub-10-ps timescale occurs. Fast recombination is observed in the absence of a sacrificial agent or protons, which under real catalytic conditions would quench remaining holes or could stabilize the charge separation.

Funding

German Research Foundation (DFG)—project number 364549901—TRR234 (CataLight, A2, B4 and Z2)

Inst 275/391-1

Fonds der Chemischen Industrie (FCI)

History

Email Address of Submitting Author

maria.waechtler@leibniz-ipht.de

Institution

Leibniz Institute of Photonic Technology

Country

Germany

ORCID For Submitting Author

0000-0001-6073-1970

Declaration of Conflict of Interest

no conflict of interest

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