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Issue 9, 2007
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Reaction of [RuIII(edta)(H2O)] with H2O2 in aqueous solution. Kinetic and mechanistic investigation

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Abstract

The reaction of [RuIII(edta)(H2O)] (1) (edta = ethylenediaminetetraacetate) with hydrogen peroxide was studied kinetically as a function of [H2O2], temperature (5–35 °C) and pressure (1–1300 atm) at a fixed pH of 5.1 using stopped-flow techniques. The reaction was found to consist of two steps involving the rapid formation of a [RuIII(edta)(OOH)]2− intermediate which subsequently undergoes parallel heterolytic and homolytic cleavage to produce [(edta)RuV[double bond, length as m-dash]O] (45%) and [(edta)RuIV(OH)] (55%), respectively. The water soluble trap, 2,2′-azobis(3-ethylbenzithiazoline-6-sulfonate) (ABTS), was employed to substantiate the mechanistic proposal. Reactions were carried out under pseudo-first conditions for [ABTS] ≫ [HOBr] ≫ [1], and were monitored as a function of time for the formation of the one-electron oxidation product ABTS˙+. A detailed mechanism in agreement with the rate and activation parameters is presented, and the results are discussed with reference to data reported for the corresponding [FeIII(edta)(H2O)]/H2O2 system.

Graphical abstract: Reaction of [RuIII(edta)(H2O)]− with H2O2 in aqueous solution. Kinetic and mechanistic investigation

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Supplementary files

Article information


Submitted
22 Nov 2006
Accepted
04 Jan 2007
First published
30 Jan 2007

Dalton Trans., 2007, 943-948
Article type
Paper

Reaction of [RuIII(edta)(H2O)] with H2O2 in aqueous solution. Kinetic and mechanistic investigation

D. Chatterjee, A. Mitra and R. van Eldik, Dalton Trans., 2007, 943
DOI: 10.1039/B617119M

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