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Theoretical Investigation of the Electron-Transfer Dynamics and Photodegradation Pathways in a Hydrogen-Evolving Ruthenium-Palladium Photocatalyst
Abstrakt
Time-dependent density functional theory calcula- tions combinedwith the Marcus theory of electron transfer (ET) were app lied on the molecular photocatalys t [(tbbpy) 2 Ru(tpph z)PdC l 2 ] 2 + in order to elucidate thelight-in- duced relaxation pathways populated upon excitation in the longer wavelength range of its absorption spectrum. The computational resultsshow that after the initial excitation, metal (Ru) to ligand (tpphz)chargetransfer (MLCT) triplet states are energeticallyaccessible, but that an ET towardthe catalytic center(PdCl 2 )from thesestates is aslow process, with estimated time constantsabove 1ns. Instead, the cal- culations predict that low-lying Pd-centered states are effi- ciently populated—assoc iated to an energy transfer toward the catalytic center.Thus,itispostulated that thesestates lead to the dissociation of aCl @ and are consequently re- sponsible for the experimentally observed degradation of the catalytic center.Following dissociation, it is shown that the ET rates from the MLCT states to the charge separated statesare significantly increased (i.e. 10 4 –10 6 timeslarger). This demonstrates that alteration of the catalytic center gen- eratesefficientchargeseparation.
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Autorzy (3)
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Stephan Kupfer
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Pełna treść
- Wersja publikacji
- Accepted albo Published Version
- DOI:
- Cyfrowy identyfikator dokumentu elektronicznego (otwiera się w nowej karcie) 10.1002/chem.201801698
- Licencja
- Copyright (2018 Wiley-VCHVerlag GmbH & Co. KGaA, Weinheim)
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Informacje szczegółowe
- Kategoria:
- Publikacja w czasopiśmie
- Typ:
- artykuł w czasopiśmie wyróżnionym w JCR
- Opublikowano w:
-
CHEMISTRY-A EUROPEAN JOURNAL
nr 24,
strony 11166 - 11176,
ISSN: 0947-6539 - Język:
- angielski
- Rok wydania:
- 2018
- Opis bibliograficzny:
- Staniszewska M., Kupfer S., Guthmuller J.: Theoretical Investigation of the Electron-Transfer Dynamics and Photodegradation Pathways in a Hydrogen-Evolving Ruthenium-Palladium Photocatalyst// CHEMISTRY-A EUROPEAN JOURNAL. -Vol. 24, (2018), s.11166-11176
- DOI:
- Cyfrowy identyfikator dokumentu elektronicznego (otwiera się w nowej karcie) 10.1002/chem.201801698
- Weryfikacja:
- Politechnika Gdańska
wyświetlono 109 razy
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