期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 28, 期 18, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202103882
关键词
Artificial Photosynthesis; Multielectron Storage; Ruthenium Photosensitizer; Computational Chemistry; Time-Resolved Spectroscopy
资金
- French National Research Agency [ANR-11-LABX-0003-01, ANR-17-EURE-0003, ANR-19-CE05-0044-01]
- CEA DRF Impulsion Program
- German Research Foundation (DFG) [TRR234, 364549901, KU 3933/2-1]
- Projekt DEAL
- Agence Nationale de la Recherche (ANR) [ANR-19-CE05-0044] Funding Source: Agence Nationale de la Recherche (ANR)
This study investigates the photo-physical properties of a ruthenium photosensitizer capable of storing and relaying multiple electrons. The results provide insights on the impact of protonation or multiple reducing equivalents on reactive excited states.
The design of photoactive systems capable of storing and relaying multiple electrons is highly demanded in the field of artificial photosynthesis, where transformations of interest rely on multielectronic redox processes. The photo-physical properties of the ruthenium photosensitizer [(bpy)(2)Ru(oxim-dppqp)](2+) (Ru), storing two electrons coupled to two protons on the pi-extended oxim-dppqp ligand under light-driven conditions, are investigated by means of excitation wavelength-dependent resonance Raman and transient absorption spectroscopies, in combination with time-dependent density functional theory; the results are discussed in comparison to the parent [(bpy)(2)Ru(dppz)](2+) and [(bpy)(2)Ru(oxo-dppqp)](2+) complexes. In addition, this study provides in-depth insights on the impact of protonation or of accumulation of multiple reducing equivalents on the reactive excited states.
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