Ru(EDTA) mediated partial reduction of O2 by H2S

被引：8
|
作者：
Chatterjee, Debabrata [1 ]
Jaiswal, Namita [1 ]
Sarkar, Papiya [1 ]
机构：
[1] CSIR, Cent Mech Engn Res Inst, Chem & Biomimet Grp, Durgapur 713209, India
来源：
DALTON TRANSACTIONS | 2015年 / 44卷 / 16期
关键词：
ELECTRON-TRANSFER REACTIONS; CYTOCHROME-C-OXIDASE; ETHYLENEDIAMINETETRAACETATE COMPLEXES; OXYGEN REDUCTION; KINETICS; MECHANISM; RUTHENIUM(III); SULFIDE;
D O I：
10.1039/c5dt00472a
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
An effective procedure for selective reduction of O-2 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 (lambda(max) = 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 (O-2) reduction. A detailed reaction mechanism in agreement with the spectral and kinetic data is presented.
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收藏
页码：7613 / 7617
页数：5
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