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• W2105514771 endingPage "7135" @default.
• W2105514771 startingPage "7123" @default.
• W2105514771 abstract "K+-exchanged, Ru(bpy)32+-encapsulating zeolite-Y [K+-Ru(bpy)32+Y] and N-[3-(dicyclohexylmethyl)oxypropyl-N‘-methyl-4,4‘-bipyridinium [DCH-MV2+] were prepared, and visible light-induced electron transfer from the zeolite-encapsulated Ru(II) complex to the size-excluded viologen was studied in acetonitrile. Addition of a series of crown ethers (CEs) into the heterogeneous solution leads to over a 10-fold increase in the yield of DCH-MV•+, where the yield linearly increases as the formation constant of CE with K+ [Kf(K+)CE] increases. The following two sequential events are attributed to be responsible for the above novel phenomenon. First, K+ ions are liberated from the zeolite to solution during interfacial electron transfer from the photoexcited Ru(II) complexes to DCH-MV2+. Second, the liberated K+ ions form strong host−guest complexes with the added CE molecules, which leads to retardation of the reverse flow of the cations, hence the charge-balancing electrons, from the solution to the zeolite. Surprisingly, the yield of DCH-MV•+ reaches more than ∼50 times the amount of Ru(bpy)32+ situated in the outermost supercages, despite the absence of electron relay in the zeolite. This is attributed to photosensitized electron pumping from the zeolite framework to viologen by the outermost Ru(bpy)32+ ions. In support of the above conclusion, Ru(bpy)33+ does not accumulate in the zeolite host while DCH-MV•+ accumulates in the supernatant solution. Consistent with the above, the independently prepared hexafluorophosphate salt of Ru(bpy)33+ is reduced to Ru(bpy)32+ in acetonitrile upon contact with Ru(bpy)32+-free M+Y (M+ = Li+, Na+, K+, Rb+, and Cs+), where the yield increases as the donor strength of the framework oxygen increases. Although small, thermal electron transfer also takes place from the zeolite framework to DCH-MV2+, where the yield increases upon increasing the donor strength of the framework, concentration of DCH-MV2+, temperature, and Kf(K+)CE (when K+Y is the zeolite host). The photoyield is always higher than the thermal yield by 4−30 times, confirming that the zeolite-encapsulated Ru(bpy)32+ serves as the photosensitized electron pump." @default.
• W2105514771 created "2016-06-24" @default.
• W2105514771 creator A5003029603 @default.
• W2105514771 creator A5009735236 @default.
• W2105514771 creator A5011601556 @default.
• W2105514771 creator A5075291156 @default.
• W2105514771 creator A5082030061 @default.
• W2105514771 date "2002-05-23" @default.
• W2105514771 modified "2023-09-24" @default.
• W2105514771 title "Long-Lived Charge-Separation by Retarding Reverse Flow of Charge-Balancing Cation and Zeolite-Encapsulated Ru(bpy)₃²⁺as Photosensitized Electron Pump from Zeolite Framework to Externally Placed Viologen" @default.
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• W2105514771 doi "https://doi.org/10.1021/ja020446a" @default.
• W2105514771 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/12059238" @default.
• W2105514771 hasPublicationYear "2002" @default.
• W2105514771 type Work @default.

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