International Journal of Chemical Kinetics p. 225 - 230 (1997)
Update date:2022-08-11
Topics:
Saha
Dutta
Gangopadhyay
Banerjee
The kinetics of the oxidation of formate, oxalate, and malonate by [NiIII(L1)]2+ (where HL1 = 15-amino-3-methyl-4,7,10,13-tetraazapentadec-3-en-2-one oxime) were carried out over the regions pH 3.0-5.75, 2.80-5.50, and 2.50-7.58, respectively, at constant ionic strength and temperature 40°C. All the reactions are overall second-order with first-order on both the oxidant and reductant. A general rate law is given as - d/dt[NiIII(L1)2+] = kobs[NiIII(L1)2+] = (kd + nks[R])[NiIII(L1)2+], where kd is the auto-decomposition rate constant of the complex, ks is the electron transfer rate constant, n is the stoichiometric factor, and R is either formate, oxalate, or malonate. The reactivity of all the reacting species of the reductants in solution were evaluated choosing suitable pH regions. The reactivity orders are: kHCOOH > kHCOO(-); kH(2)ox > kHox(-) > kox(2-), and kH(2)mal > kHmal(-) < kmal(2-) for the oxidation of formate, oxalate, and malonate, respectively, and these trends were explained considering the effect of hydrogen bonded adduct formation and thermodynamic potential.
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