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Effective quenching and excited-state relaxation of a Cu(I) photosensitizer addressed by time-resolved spectroscopy and TDDFT calculations
Authors
Beller M.
Bokareva O.
+5 more
Friedrich A.
Junge H.
Kühn O.
Lochbrunner S.
Luo S.
Publication date
1 January 2018
Publisher
Doi
Cite
Abstract
© 2018 Elsevier B.V. Homogenous photocatalytic systems based on copper photosensitizers are promising candidates for noble metal free approaches in solar hydrogen generation. To improve their performance, a detailed understanding of the individual steps is needed. Here, we study the interaction of a heteroleptic copper (I) photosensitizer with an iron catalyst by time-resolved spectroscopy and ab initio calculations. The catalyst leads to rather efficient quenching of the 3MLCT state of the copper complex, with a bimolecular rate being about three times smaller than the collision rate. Using control experiments with methyl viologen, an appearing absorption band is assigned to the oxidized copper complex demonstrating that an electron transfer from the sensitizer to the iron catalyst occurs and the system reacts along an oxidative pathway. However, only about 30% of the quenching events result in an electron transfer while the other 70% experience deactivation indicating that the photocatalytic performance might suffer from geminate recombination
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Kazan Federal University Digital Repository
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oai:dspace.kpfu.ru:net/147958
Last time updated on 07/05/2019
ChemRxiv
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60c73e959abda2ebd3f8b8da
Last time updated on 25/08/2023