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The iron-sulfur cluster compounds Fe(4)S(4)(SR)(4) (-2) [where -SR = -SCH(3), -S-C(CH(3))(3), and -S- CH(2)-CH(CH(3))(2)] have been found to represent the base species of weak acids of pK(a) comparable to that of carboxylic acids. The acid species Fe(4)S(4)(SR)(4)H(-) is most subject to reaction with O(2) and to acid-catalyzed solvolysis, while the base species Fe(4)S(4)(SR)(4) (-2) most readily undergoes ligand exchange. The kinetics for hydrolysis of the isobutyl mercaptide cluster salt has been investigated in detail and a mechanism involving the stepwise process [Formula: see text] has been proposed. The importance of the acid-base equilibria in determining the reactivity of the iron-sulfur clusters and its possible importance as a factor in the determination of the potentials of ferredoxins and high potential iron protein are discussed.

proceedings of the national academy of sciences of the united states of america

The Acid-Base Properties, Hydrolytic Mechanism, and Susceptibility to O 2 Oxidation of Fe 4 S 4 (SR) 4 -2 Clusters