Probing the influence of substrate binding on photocatalytic dehalogenation with a heteroleptic supramolecular [M 4 L a 2 L b 2 ] square containing PDI photosensitizers as ligands.

Autor: Nielsen CJ; Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van't Hoff Institute for Molecular Sciences, Faculty of Natural Sciences, University of Amsterdam, P.O. Box 94720, 1090 GS Amsterdam, The Netherlands. s.pullen@uva.nl., Laan PCM; Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van't Hoff Institute for Molecular Sciences, Faculty of Natural Sciences, University of Amsterdam, P.O. Box 94720, 1090 GS Amsterdam, The Netherlands. s.pullen@uva.nl., Plessius R; Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van't Hoff Institute for Molecular Sciences, Faculty of Natural Sciences, University of Amsterdam, P.O. Box 94720, 1090 GS Amsterdam, The Netherlands. s.pullen@uva.nl., Reek JNH; Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van't Hoff Institute for Molecular Sciences, Faculty of Natural Sciences, University of Amsterdam, P.O. Box 94720, 1090 GS Amsterdam, The Netherlands. s.pullen@uva.nl., van der Vlugt JI; Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van't Hoff Institute for Molecular Sciences, Faculty of Natural Sciences, University of Amsterdam, P.O. Box 94720, 1090 GS Amsterdam, The Netherlands. s.pullen@uva.nl.; Bioinspired Coordination Chemistry & Catalysis, Institute of Chemistry, Carl von Ossietzky University Oldenburg, Carl-von-Ossietzky-Strasse 9-11, D-26129 Oldenburg, Germany., Pullen S; Homogeneous, Supramolecular and Bio-Inspired Catalysis, Van't Hoff Institute for Molecular Sciences, Faculty of Natural Sciences, University of Amsterdam, P.O. Box 94720, 1090 GS Amsterdam, The Netherlands. s.pullen@uva.nl.
Jazyk: angličtina
Zdroj: Faraday discussions [Faraday Discuss] 2023 Aug 11; Vol. 244 (0), pp. 199-209. Date of Electronic Publication: 2023 Aug 11.
DOI: 10.1039/d2fd00179a
Abstrakt: Photoredox catalysis is a valuable tool in a large variety of chemical reactions. Main challenges still to be overcome are photodegradation of photocatalysts and substrates, short lifetimes of reactive intermediates, and selectivity issues due to unwanted side reactions. A potential solution to these challenges is the pre-organization of the photosensitizer, substrate and (co)-catalyst in supramolecular self-assembled structures. In such architectures, (organic) dyes can be stabilized, and higher selectivity could potentially be achieved through pre-organizing desired reaction partners via non-covalent interactions. Perylene diimide (PDI) is an organic dye, which can be readily reduced to its mono- and dianion. Excitation of both anions leads to highly reducing excited states, which are able to reduce a variety of substrates via single electron transfer. The incorporation of PDI into a heteroleptic [M 4 L a 2 L b 2 ] supramolecular square has been recently demonstrated. Herein we investigate its photophysical properties and demonstrate that incorporated PDI indeed features photocatalytic activity. Initial results suggest that the pre-organisation by binding positively affects the outcome.
Databáze: MEDLINE