Photochemistry and Photobiology · 1978 · 130 citations · 23 references
Natural SciencesChemistryCatalysisEnzyme MechanismRedox BiochemistryCatalytic MechanismsCatalytic Reaction KineticsElimination ReactionsOxidation ReactionsRadical ReactionsReactive Oxygen SpeciesAlcohol OxidationDeuterium Isotope EffectElimination From AlcoholsKinetic Isotope Effects In Reductive EliminationPeroxy Radical ChemistrySolvent Effects In EliminationSolvent PolarityTemperature Dependence
Abstract— In aqueous solutions α‐hydroxyalkylperoxyl radicals undergo a spontaneous and a base catalysed HO 2 elimination. From kinetic deuterium isotope effects, temperature dependence, and the influence of solvent polarity it was concluded that the spontaneous reaction occurs via an HO 2 elimination followed by the dissociation of the latter into H + and O 2 ‐ . The rate constant of the spontaneous HO 2 elimination increases with increasing methyl substitution in α‐position ( k (CH 2 (OH)O 2 ) < 10s ‐1 k (CH 3 CH(OH)O 2 ) = 52s ‐1 k ((CH 3 ) 2 C(OH)O 2 ) = 665 s ‐1 ). The OH ‐ catalysed reaction is somewhat below diffusion controlled. The mixture of peroxyl radicals derived from polyhydric alcohols eliminate HO 2 at two different rates. Possible reasons for this behaviour are discussed. The mixture of the six peroxyl radicals derived from d ‐glucose are observed to eliminate HO 2 with at least three different rates. The fastest rate is attributed to the HO 2 elimination from the peroxyl radical at C‐l ( k > 7000s ‐1 ). Because of the HO 2 eliminations the peroxyl radicals derived from d ‐glucose do not undergo a chain reaction in contrast to peroxyl radicals not containing an α‐OH group. In competition with the first order elimination reactions the α‐hydroxylalkylperoxyl radicals undergo a bimolecular decay. These reactions are briefly discussed.
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