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- W2077564863 abstract "Visible light excitation of the ligand-bridged assembly [(bpy) 2 Ru a II (L)Ru b II (bpy)(OH 2 ) 4+ ] (bpy is 2,2′-bipyridine; L is the bridging ligand, 4-phen-tpy) results in emission from the lowest energy, bridge-based metal-to-ligand charge transfer excited state (L −• )Ru b III -OH 2 with an excited-state lifetime of 13 ± 1 ns. Near–diffusion-controlled quenching of the emission occurs with added HPO 4 2− and partial quenching by added acetate anion (OAc − ) in buffered solutions with pH control. A Stern–Volmer analysis of quenching by OAc − gave a quenching rate constant of k q = 4.1 × 10 8 M −1 ⋅s −1 and an estimated pK a * value of ∼5 ± 1 for the [(bpy) 2 Ru a II (L •− )Ru b III (bpy)(OH 2 ) 4+ ]* excited state. Following proton loss and rapid excited-state decay to give [(bpy) 2 Ru a II (L)Ru b II (bpy)(OH) 3+ ] in a H 2 PO 4 − /HPO 4 2− buffer, back proton transfer occurs from H 2 PO 4 − to give [(bpy) 2 Ru a II (L)Ru b (bpy)(OH 2 ) 4+ ] with k PT,2 = 4.4 × 10 8 M −1 ⋅s −1 . From the intercept of a plot of k obs vs. [H 2 PO 4 − ], k = 2.1 × 10 6 s −1 for reprotonation by water providing a dramatic illustration of kinetically limiting, slow proton transfer for acids and bases with pK a values intermediate between pK a (H 3 O + ) = −1.74 and pK a (H 2 O) = 15.7." @default.
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- W2077564863 date "2012-12-31" @default.
- W2077564863 modified "2023-10-17" @default.
- W2077564863 title "Accelerating slow excited state proton transfer" @default.
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- W2077564863 doi "https://doi.org/10.1073/pnas.1220742110" @default.
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