Abstract
An effective procedure for selective reduction of O2 to H2O2 exploring the use of hydrogen sulfide, an obnoxious industrial pollutant as reductant is reported herein. The reduction of [Ru(III)(EDTA)pz](-) (EDTA(4-) = ethylenediaminetetraacetate; pz = pyrazine) by hydrogen sulfide resulting in the formation of a red [Ru(II)(EDTA)pz](2-) complex (λmax = 462 nm) has been studied spectrophotometrically and kinetically using both rapid scan and stopped-flow techniques. The time course of the reaction was followed as a function of [HS(-)]i, pH (5.5-8.5), and temperature. Alkali metal ions were found to have a positive influence (K(+) > Na(+) > Li(+)) on the reaction rate. Kinetic data and activation parameters are interpreted in terms of a mechanism (admittedly speculative) involving outer-sphere electron transfer between the reaction partners. Reaction of the red [Ru(II)(EDTA)pz](2-) complex with molecular oxygen regenerates the [Ru(III)(EDTA)pz](-) species in the reacting system along with the formation of H2O2, a partially reduced product of dioxygen (O2) reduction. A detailed reaction mechanism in agreement with the spectral and kinetic data is presented.
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