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• W2008211036 abstract "At low acid concentration, e.g., <4MH2SO4, the cerium(IV) oxidation of the iron(II) complex of the mixed-diimine ligand 2-pyridinal-α-methyl-(methylimine), PMM = C5H4NC(CH3)NCH3, is a very complex reaction in which ligand-oxidized iron(II) and iron(III) complexes are formed and partly dissociated, with a total consumption of 10–11 equivalents of Ce(IV) per mole of Fe(PMM)2+3. The major oxidation product in ∼50% yield is Fe(PO)3+3, where PO = C5H4NC(CHO)NCH3. The oxisation product has the α-methyl group oxidized to an aldehyde group. At the beginning of the reaction (<25% of the total Ce(IV) comsumption) Fe(PMM)2Po2+ was identified as the major reaction product: Ce(IV) + Fe(PMM)2+3 = Ce(III) + Fe(PMM)3+3 → 0.75 Fe- (PMM)2+3 + 0.25 Fe(PMM)2PO2+. At this stage the kinetics of the reaction was analyzed by two potentiometric techniques. From experiments of addition of Fe(PMM)3+3, prepared in 5 M H2SO4, to Fe(PMM)2+3, to a final 1 M H2SO4 concentration, the variation of the potential of the Fe(PMM)3+3/Fe(PMM)2+3 couple is recorded with time. This variation is associated with the rate of disproportionation of Fe(PMM)3+3 yielding Fe(PMM)2PO2+ and the original iron(II) complex. the rate law from these experiments is -d[Fe(PMM)3+3]/dt = k[Fe(PMM)3+3]1.5. From automatic titration experiments, in which CE(IV) is added to Fe(PMM)2+3 solutions at constant rate (ϱ), at high Fe(PMM)3+3 concentration, the rate law is ϱ = k′[Fe(PMM)3+3]. A mechanism, similar to that proposed for the oxidation of the aliphatic diimine complexes, is proposed. The first step is the formation of Fe(PMM)3+3 and Ce(III) with an equilibrium constant of 4.4 × 107. The iron(III) complex undergoes an intramolecular reduction to the iron(II) state with concomitant radical formation at the ligand, in a step assisted by solvent water and retarded by acid. Further oxidation of the iron(II) complex-ligand-radical by Fe(PMM)3+3 to the final production of Fe(PMM)2PO2+ leads to the derivation on the following rate law, (ϱ) - (d[Fe(PMM)3+3]/dt) = (3k3K7[Fe(PMM)3+3]2)/ (k4 + k7 [Fe(PMM)3+3]), which at high [Fe(PMM)3+3] (automatic titrations) reduces to a first order reaction [Fe(PMM)3+3] with k3 = 0.02 s-1. Analysis of the potential variation experiments with time (low [Fe(PMM)3+3]) with the whole kinetic expression above leads to k3 = 0.02 s1-." @default.
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• W2008211036 date "1980-01-01" @default.
• W2008211036 modified "2023-09-27" @default.
• W2008211036 title "Ligand oxidation in iron diimine complexes. V. Kinetics of the oxidation of tris[2-pyridinal-α-methyl-(methylimine)] iron(II) by cerium(IV)" @default.
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• W2008211036 doi "https://doi.org/10.1016/s0020-1693(00)88896-9" @default.
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