Electron transfer within ruthenium(II) polypyridyl-(salt bridge)-dimethylaniline acceptor-donor complexes
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The modified Q-cycle: A look back at its development and forward to a functional model
2021, Biochimica et Biophysica Acta - BioenergeticsCitation Excerpt :In effect, the rapid rate constant expected from the short distance is slowed by the low probability of finding the proton in the right place. This type of mechanism was first proposed to explain the behavior in chemical models by Nocera et al. [149,150]. Here the value 13 is log10 of the limiting rate constant (1013 s−1) from bond vibrational frequency of a typical H-bond (3.6 Å), and β is an empirically determined slope for dependence of rate on distance from a sampling of measured rates in the context of structural distances (in the seminal work, mainly from bacterial reaction centers).
Dissecting the pattern of proton release from partial process involved in ubihydroquinone oxidation in the Q-cycle
2018, Biochimica et Biophysica Acta - BioenergeticsCitation Excerpt :The electron can transfer only when the H+ is positioned along the H-bond close to Nε of H152 (the acceptor configuration), with a probability of 10−5 that depends on the pK difference between H152 and QH2 (a Brønsted term). Then, the observed rate can be economically explained if the expected rate (of 108 s−1) is lowered by this factor [35,51,52]. However, other factors complicate the picture; notably, the reaction is strongly endergonic, so the reaction is observed to proceed only if the products are rapidly removed.
Proton-coupled electron transfer with photoexcited ruthenium(II), rhenium(I), and iridium(III) complexes
2015, Coordination Chemistry ReviewsCitation Excerpt :Similarly, in symmetric (COOH)2 interfaces formed by carboxylic acid dimers photoinduced electron transfer between Ru(bpy)32+ and 3,5-dinitrobenzene was not coupled to net proton transfer [28]. Attempts to perform reductive 3MLCT excited-state quenching of Ru(bpy)32+ by N,N-dimethylaniline in amidinium-carboxylate bridged adducts did not provide any evidence for PCET either [30]. However, amidinium-carboxylate and amidinium-sulfonate salt-bridged systems involving porphyrin photosensitizers were successfully employed in several PCET studies [32–34].
Ferrocenyl-amidinium compound as building block for aqueous proton-coupled electron transfer studies
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2013, Biochimica et Biophysica Acta - Bioenergetics