Kinetics and Mechanisms of the Redox Reactions of µ-Adipato-Di (N,N/ Bis(Salicylidene) Ethylenediaminatoiron (Iii) [(Fe-Salen)2adi] with some Thiols

Description

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Abstract

Electron transfer reactions of Fe₂adi was studied with reductants (L-cysteine (LSH),thiourea(USH), thioglycolic acid(GSH), 2-mecarptobenzothiazole (BTSH) and benzyl mercaptan (BSH)). The stoichiometries of the reactions were 1:1 (oxidant/reductant) for LSH, GSH and BTSH while 1:2 (oxidant/reductant) was obtained for Fe₂adi – USH and Fe₂adi – BSH systems.

The reactions of  LSH, GSH, and BTSH showed direct acid dependence and this was rationalized in terms of the protonation of the iron(III) complex in acid media. The non-acid dependence observed for Fe₂adi – USH and Fe₂adi – BSH systems were rationalized in terms of the deprotonation of the thiols in acid media.

An increase in ionic strength resulted in a decrease in rates of reaction for the five systems. These results suggest that the rate-determining step involved oppositely charged species; thereby signifying the primary salt effect. Added anion (CH₃COO^–) and cation (Mg²⁺) did not affect the rates of reaction for Fe₂adi – LSH, Fe₂adi – USH, Fe₂adi – GSH and Fe₂adi – BTSH systems.

Lack of dependence of the rate of reaction on added ions is likely to result from inner-sphere complex formation in accordance with the results of the ionic strength. Enhanced rates of reaction observed for the anion and cation catalysis of Fe₂adi – BSH system may be attributed to occur as a result of possible electron transfer prior to the formation of the intermediate complex.

Introduction

The electron transfer reactions of binuclear iron (III) complexes have attracted a lot of interest in recent times due to their application as models for the investigation of the physiological role played by iron in biochemical processes ^2, such as hemerythrin ^2,3,4.6 and ferric porphyrin^{7,27,28 47}.

Previously,  the dynamics of electron transfer reactions of dinuclear oxo binged iron(III) complexes of the form   [Fe₂O]⁴⁺with ascorbic acid  ⁴,þ -mercapto acetic  acid⁵  and þ -mercaptoethylamine ⁶ have been investigated. Most of these reactions followed the outer sphere electron transfer route with intervening ion-pair complexes and free radicals.

The behaviour of transition metal ions with respect to their electron transfer and the roles played by bridging ligands in the course of redox reaction formed the bedrock of this study.

^37,39 The main advantage of this research is that the results provide additional insight into the complexities attending reactions of bridged iron(III) complexes and the extent of influence of the bridging ligand on the rate of electron transfer.

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