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• W2041144869 abstract "Photoinduced electron transfer from sensitizers attached to zeolite surface to electron acceptors within the zeolite provides opportunities for long-lived charge separation, as well as potential utilization of the charge separated species. In this study, the focus is on the ruthenium polypyridyl compound [(bpy)2RuLDQ]4+ (where bpy = bipyridine, and LDQ = 1-[4-(4′-methyl)-2,2′-bipyridyl]-2-[4-(4′-N,N′-tetramethylene-2,2′-bipyridinium)]ethene) and its unquaternized analogue of structural formula [(bpy)2RuL]2+ (L = trans-1,2-bis[4-(4′-methyl)-2,2′-bipyridyl]ethene). Both complexes show strong metal-to-ligand charge-transfer (MLCT) and olefinic ligand based absorption bands. The emission of [(bpy)2RuLDQ]4+ in solution is quenched, whereas the [(bpy)2RuL]2+ complex exhibits emission at 675 nm. The quenching is attributed to the intramolecular electron transfer from the Ru center to the diquat (DQ) moiety upon photoexcitation. The [(bpy)2RuLDQ]4+ complex is stable upon visible light illumination, while [(bpy)2RuL]2+ is photochemically unstable. Nanocrystalline zeolite Y with particle size of ∼80 nm was prepared and characterized by diffraction and electron microscopy. Protonated [(bpy)2RuL]2+ and [(bpy)2RuLDQ]4+ were attached to the surface of the zeolite Y by ion-exchange and permanent incorporation into the supercage, respectively. The zeolite-encapsulated [(bpy)2RuLDQ]4+ species was found to be emissive at 695 nm with at lifetime of 796 ns. Intermolecular electron transfer from photoexcited [(bpy)2RuLDQ]4+ to methylviologen (MV2+) in solution was not observed. However, in the zeolite, ∼40% of the initial MV+• generated via photoinduced electron transfer from surface-bound [(bpy)2RuLLQ]4+ survived for the duration of the experiment (milliseconds). The long-lived viologen radical resulted from a competitive effect between the back electron transfer from MV+• to Ru3+ (kb = 3.0 × 105 s−1) with a self-exchange electron propagation between the densely packed viologens (khop = 2.0 × 105 s−1) that moves the charge away from the surface of the zeolite." @default.
• W2041144869 created "2016-06-24" @default.
• W2041144869 creator A5050225415 @default.
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• W2041144869 date "2009-02-23" @default.
• W2041144869 modified "2023-09-23" @default.
• W2041144869 title "Ruthenium Polypyridyl Complexes Containing a Conjugated Ligand L_DQ (L_DQ = 1-[4-(4′-methyl)-2,2′-bipyridyl]-2-[4-(4′-<i>N</i>,<i>N</i>′-tetramethylene-2,2′-bipyridinum)]ethene): Synthesis, Characterization, and Photoinduced Electron Transfer at Solution−Zeolite Interfaces" @default.
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• W2041144869 doi "https://doi.org/10.1021/jp8061459" @default.
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