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

Sahu, S., Widger, L. R., Quesne, Matthew, De Visser, S. P., Matsumura, H., Moenne-Loccoz, P., Siegler, M. A. and Goldberg, D. P. 2013. Secondary coordination sphere influence on the reactivity of nonheme iron(II) complexes: an experimental and DFT approach. Journal of the American Chemical Society 135 (29) , pp. 10590-10593. 10.1021/ja402688t

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Abstract

The new biomimetic ligands N4Py2Ph (1) and N4Py2Ph,amide (2) were synthesized and yield the iron(II) complexes [FeII(N4Py2Ph)(NCCH3)](BF4)2 (3) and [FeII(N4Py2Ph,amide)](BF4)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.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Publisher: American Chemical Society
ISSN: 0002-7863
Last Modified: 04 Jun 2017 08:58
URI: http://orca-mwe.cf.ac.uk/id/eprint/88636

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