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Pierre Moenne-Loccoz Institute of Environmental Health

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Secondary coordination sphere influence on the reactivity of nonheme iron(II) complexes: An experimental and DFT approach

Sumit Sahu; Leland R. Widger; Matthew G. Quesne; Sam P. De Visser; Hirotoshi Matsumura; Pierre Moënne-Loccoz; Maxime A. Siegler; David P. Goldberg

(Profiled Author: Pierre Moenne-Loccoz)

Journal of the American Chemical Society. 2013;135(29):10590-10593.

Abstract

The new biomimetic ligands N4Py2Ph (1) and N4Py 2Ph,amide (2) were synthesized and yield the iron(II) complexes [FeII(N4Py2Ph)(NCCH3)](BF4) 2 (3) and [FeII(N4Py2Ph,amide)](BF 4)2 (5). Controlled orientation of the Ph substituents in 3 leads to facile triplet spin reactivity for a putative FeIV(O) intermediate, resulting in rapid arene hydroxylation. Addition of a peripheral amide substituent within hydrogen-bond distance of the iron first coordination sphere leads to stabilization of a high-spin FeIIIOOR species which decays without arene hydroxylation. These results provide new insights regarding the impact of secondary coordination sphere effects at nonheme iron centers. © 2013 American Chemical Society.


PMID: 23834409     PMCID: PMC3746373    

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