Control of the evolution of iron peroxide intermediate in superoxide reductase from Desulfoarculus baarsii. Involvement of lysine 48 in protonation

Journal of the American Chemical Society
Florence BonnotVincent Nivière

Abstract

Superoxide reductase is a nonheme iron metalloenzyme that detoxifies superoxide anion radicals O(2)(•-) in some microorganisms. Its catalytic mechanism was previously proposed to involve a single ferric iron (hydro)peroxo intermediate, which is protonated to form the reaction product H(2)O(2). Here, we show by pulse radiolysis that the mutation of the well-conserved lysine 48 into isoleucine in the SOR from Desulfoarculus baarsii dramatically affects its reaction with O(2)(•-). Although the first reaction intermediate and its decay are not affected by the mutation, H(2)O(2) is no longer the reaction product. In addition, in contrast to the wild-type SOR, the lysine mutant catalyzes a two-electron oxidation of an olefin into epoxide in the presence of H(2)O(2), suggesting the formation of iron-oxo intermediate species in this mutant. In agreement with the recent X-ray structures of the peroxide intermediates trapped in a SOR crystal, these data support the involvement of lysine 48 in the specific protonation of the proximal oxygen of the peroxide intermediate to generate H(2)O(2), thus avoiding formation of iron-oxo species, as is observed in cytochrome P450. In addition, we proposed that the first reaction intermediate observed...Continue Reading

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Citations

Oct 1, 2013·Photosynthesis Research·Frank Müh, Athina Zouni
Nov 9, 2012·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Amr Ali Ahmed Ali AttiaRadu Silaghi-Dumitrescu
Aug 7, 2013·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Emilie TremeyVincent Nivière
Jan 1, 2012·Scientifica·Paul R Gardner
Dec 6, 2014·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Ana F PintoMiguel Teixeira
May 28, 2016·Journal of Biological Inorganic Chemistry : JBIC : a Publication of the Society of Biological Inorganic Chemistry·Tibor András RokobLubomír Rulíšek
Mar 10, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Markus R AnneserFritz E Kühn
Aug 14, 2012·Angewandte Chemie·Aidan R McDonaldLawrence Que
Apr 2, 2014·Chemical Reviews·Yuewei ShengJoan Selverstone Valentine
Feb 12, 2019·Chemical Reviews·Kazuo Kobayashi

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