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• W2024490080 abstract "The oxidation of sulfite by the two nickel(IV) oxime–imine complexes [NiIVL12+]2 and [NiIVL2]2+(HL1= 6-amino-3-methyl-4-azahex-3-en-2-one oxime and H2L2= 3,14-dimethyl-4,7,10,13-tetra-azahexadeca-3,13-diene-2,1 5-dione dioxime) has been investigated in aqueous medium at 30 °C over the range pH 2.0–8.0. Single-step two-electron transfer reactions were encountered in the regions 2.0 ⩽ pH ⩽ 5.50 for [NiIVL12]2+ and 2.0 ⩽ pH ⩽ 4.25 for [NiIVL2]2+ reductions. A distinct biphasic process with faster initial one-electron reduction of NiIV to NiIII followed by a slower conversion of NiIII into NiII was observed above pH 5.75 and 4.50 for the respective complexes. Attempts were made to evaluate the reactivity of all the reacting species of the complexes as well as of sulfur(IV) by considering suitable pH regions. The stoichiometries of the reactions ([SIV]:[NiIV]) were found to vary within the region ≈2.0–1.0 depending upon the mole ratios of the reactants. At pH 4.50 with an excess of complex over the reductant the ratio [SIV]:[NiIV] is less than 2:1 for both complexes giving a mixture of dithionate and sulfate as the oxidation products of sulfite. However, with an excess of sulfite over the complex this ratio reaches a limiting value of ≈2:1 at [SIV]:[NiIV] > 8 giving dithionate as the major oxidation product. The observed stoichiometric ratios for both complexes are in accord with the distribution of the sulfate and dithionate products. Attempts were made to correlate the experimentally observed rate constants with those obtained from Marcus cross-relation calculations. Calculated rate constants for the oxidation of SO32– by various nickel-(IV) and -(III) species were found to be one to two orders of magnitude lower than the corresponding experimental values. The oxidation of SO2·H2O and HSO3– is proposed to proceed through the formation of a hydrogen-bonded adduct." @default.
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• W2024490080 date "1994-01-01" @default.
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• W2024490080 title "Kinetic studies on the oxidation of sulfur(<scp>IV</scp>) by nickel(<scp>IV</scp>) oxime–lmine complexes" @default.
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• W2024490080 doi "https://doi.org/10.1039/dt9940003733" @default.
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