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Open AccessFeature PaperArticle

Towards Covalent Photosensitizer-Polyoxometalate Dyads-Bipyridyl-Functionalized Polyoxometalates and Their Transition Metal Complexes

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Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Humboldtstr. 10, 07743 Jena, Germany
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Center for Energy and Environmental Chemistry (CEEC) Jena, Friedrich Schiller University Jena, Philosophenweg 7a, 07743 Jena, Germany
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Institute for Inorganic and Analytical Chemistry (IAAC), Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany
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Institute of Physical Chemistry (ICP), Friedrich Schiller University Jena, Lessingstr. 10, 07743 Jena, Germany
*
Author to whom correspondence should be addressed.
Molecules 2019, 24(24), 4446; https://doi.org/10.3390/molecules24244446
Received: 13 November 2019 / Revised: 27 November 2019 / Accepted: 28 November 2019 / Published: 4 December 2019
(This article belongs to the Special Issue Bipyridines: Synthesis, Functionalization and Applications)
A triol-functionalized 2,2′-bipyridine (bpy) derivative has been synthesized and used for the tris-alkoxylation of polyoxometalate (POM) precursors. The resultant POM-bpy conjugates of the Wells–Dawson- and Anderson-type feature a C–C bond as a linkage between the POM and bpy fragments. This structural motif is expected to increase the hydrolytic stability of the compounds. This is of particular relevance with respect to the application of POM-bpy metal complexes, as photocatalysts, in the hydrogen-evolution reaction (HER) in an aqueous environment. Accordingly, Rh(III) and Ir(III) complexes of the POM-bpy ligands have been prepared and characterized. These catalyst-photosensitizer dyads have been analyzed with respect to their electrochemical and photophysical properties. Cyclic and square-wave voltammetry, as well as UV/vis absorption and emission spectroscopy, indicated a negligible electronic interaction of the POM and metal-complex subunits in the ground state. However, emission–quenching experiments suggested an efficient intramolecular electron-transfer process from the photo-excited metal centers to the POM units to account for the non-emissive nature of the dyads (thus, suggesting a strong interaction of the subunits in the excited state). In-depth photophysical investigations, as well as a functional characterization, i.e., the applicability in the HER reaction, are currently ongoing. View Full-Text
Keywords: hybrid materials; metal complexes; polyoxometalates; photocatalysis hybrid materials; metal complexes; polyoxometalates; photocatalysis
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Winter, A.; Endres, P.; Schröter, E.; Jäger, M.; Görls, H.; Neumann, C.; Turchanin, A.; Schubert, U.S. Towards Covalent Photosensitizer-Polyoxometalate Dyads-Bipyridyl-Functionalized Polyoxometalates and Their Transition Metal Complexes. Molecules 2019, 24, 4446.

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