Proceedings of nanoGe Fall Meeting19 (NFM19)
Publication date: 18th July 2019
Colloidal semiconductor nanocrystals are excellent light harvesting elements for artificial photocatalysis, due to their high extinction coefficients over a broad spectral region and the possibility to tune the optical and electronic properties by the size of the semiconductor nanocrystals. The tuneable properties of colloidal nanocrystals turn them into interesting candidates as sensitizers in photocatalytic assemblies e.g. for H2 generation. In this respect we want to couple CdSe quantum dots with suited molecular catalytic centers. FeFe-H2ase mimics are able to catalyze the reversible reduction of H2 at overpotentials and catalytic efficiencies that rival platinum electrodes [1], [2]. To reach high turnover numbers the spatial proximity between sensitizer and catalyst needs to be generated as well as a transfer of the catalyst into water. By anchoring the FeFe-H2ase mimics directly to the quantum dot surface via suited coupling groups, both challenges can be addressed. In this contribution the interaction of CdSe quantum dots of different diameters with FeFe-H2ase mimics, possessing different anchoring moieties like carboxyl, amine, disulfide and diselenide groups were followed by steady state and time-resolved emission spectroscopy. The quenching efficiency over time is suggesting a Langmuir adsorption behaviour. Furthermore, to achieve the before mentioned close spatial proximity, different linking strategies like photochemical linking, conversion of amine groups to dithiocarbamate as well as amide linking to the surface ligands of the quantum dots were tested. The results pave the way for a general design principle of anchoring moiety for molecular catalyst and semiconducting nanoparticles.
Financial support is acknowledged by the German Research Foundation (DFG) – project number 364549901 - TRR234 [CataLight, B4)] and the Fonds der Chemischen Industrie (FCI)
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