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- W2023702162 abstract "Dicationic metal superoxo complexes, L(H2O)MOO2+ (M = Rh, Cr; L = (NH3)4, (H2O)5, [14]aneN4) react with rhodium hydrides L‘(H2O)RhH2+ (L‘ = (NH3)4, [14]aneN4, and meso-Me6-[14]aneN4) to yield L(H2O)MOOH2+ and L‘(H2O)2Rh2+. The rhodium(II) product is rapidly converted to L‘(H2O)RhOO2+ in a reaction with molecular oxygen (k ∼ 108 M-1 s-1), or to a binuclear superoxo product in the absence of O2. When the central metal atom and nonparticipating ligands are identical in the two reactants (M = Rh, L = L‘), the O2 insertion into Rh−H bond becomes catalytic, L‘RhH2+ + O2 → L‘RhOOH2+ (L‘RhOO2+ = catalyst). The hydrogen transfer step exhibits a large kinetic isotope effect (kH/kD = 7.6 for the reaction of CraqOO2+ with ([14]aneN4)(H2O)RhH2+, ΔHH⧧ = 20.3 ± 1.8 kJ mol-1, ΔSH⧧ = −136 ± 6 J mol-1 K-1, and ΔHD⧧ = 24.7 ± 4.3 kJ mol-1, ΔSD⧧ = −138 ± 15 J mol-1 K-1), but the isotopic composition of the solvent has no effect on rates, kH2O/kD2O = 1. Steric effects play a major role in the kinetics. From the available therm..." @default.
- W2023702162 created "2016-06-24" @default.
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- W2023702162 date "1997-11-01" @default.
- W2023702162 modified "2023-09-23" @default.
- W2023702162 title "Kinetics and Thermodynamics of Hydrogen Atom Transfer to Superoxometal Complexes" @default.
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- W2023702162 doi "https://doi.org/10.1021/ja971987g" @default.
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