NDLI: Kinetics of proton-coupled electron-transfer reactions to the manganese-oxo “cubane” complexes containing the $Mn_{4}O$ and $Mn_{4}O$ core types

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Kinetics of proton-coupled electron-transfer reactions to the manganese-oxo “cubane” complexes containing the $Mn_{4}O$ and $Mn_{4}O$ core types

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Ruettinger, Wolfgang F. Mclendon, George L. Dismukes, G. Charles Bourles, Emilie Maneiro, Marcelino
Description	Author Affiliation: Maneiro M ( Department of Chemistry, Hoyt Laboratory, Princeton University, Princeton, NJ 08544, USA.);
Abstract	The kinetics of proton-coupled electron-transfer (pcet) reactions are reported for Mn(4)O(4)(O(2)PPh(2))(6), 1, and [Mn(4)O(4)(O(2)PPh(2))(6)](+), 1(+), with phenothiazine (pzH). Both pcet reactions form 1H, by H transfer to 1 and by hydride transfer to 1(+). Surprisingly, the rate constants differ by only 25% despite large differences in the formal charges and driving force. The driving force is proportional to the difference in the bond-dissociation energies (BDE >94 kcalmol for homolytic, 1H --> H + 1, vs. approximately 127 kcalmol for heterolytic, 1H --> H(-) + 1(+), dissociation of the OH bond in 1H). The enthalpy and entropy of activation for the homolytic reaction (deltaH = -1.2 kcalmol and deltaS= -32 calmol.K; 25-6.7 degrees C) reveal a low activation barrier and an appreciable entropic penalty in the transition state. The rate-limiting step exhibits no HD kinetic isotope effect (k(H)k(D) = 0.96) for the first H atom-transfer step and a small kinetic isotope effect (1.4) for the second step (1H + pzH --> 1H(2) + pz(*)). These lines of evidence indicate that formation of a reactive precursor complex before atom transfer is rate-limiting (conformational gating), and that little or no NH bond cleavage occurs in the transition state. H-atom transfer from pzH to alkyl, alkoxyl, and peroxyl radicals reveals that BDEs are not a good predictor of the rates of this reaction. Hydride transfer to 1(+) provides a concrete example of two-electron pcet that is hypothesized for the OH bond cleavage step during catalysis of photosynthetic water oxidation.
ISSN	00278424
e-ISSN	10916490
Journal	Proceedings of the National Academy of Sciences of the United States of America
Issue Number	7
Volume Number	100
Language	English
Publisher	National Academy of Sciences
Publisher Date	2003-04-01
Publisher Place	United States
Access Restriction	Open
Subject Keyword	Manganese Compounds Chemistry Oxides Calorimetry Electron Transport Protons Spectrophotometry, Infrared Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, P.H.S. Multidisciplinary
Content Type	Text
Resource Type	Article
Subject	Multidisciplinary

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