Direct observation of oxygen rebound with an iron-hydroxide complex

Jan Paulo T. Zaragoza; Timothy H. Yosca; Maxime A. Siegler; Pierre Moënne-Loccoz; Michael T. Green; David P. Goldberg

doi:10.1021/jacs.7b07979

Direct observation of oxygen rebound with an iron-hydroxide complex

Jan Paulo T. Zaragoza, Timothy H. Yosca, Maxime A. Siegler, Pierre Moënne-Loccoz, Michael T. Green, David P. Goldberg

Chemical Physiology and Biochemistry

Research output: Contribution to journal › Article › peer-review

76 Scopus citations

Abstract

The rebound mechanism for alkane hydroxylation was invoked over 40 years ago to help explain reactivity patterns in cytochrome P450, and subsequently has been used to provide insight into a range of biological and synthetic systems. Efforts to model the rebound reaction in a synthetic system have been unsuccessful, in part because of the challenge in preparing a suitable metalhydroxide complex at the correct oxidation level. Herein we report the synthesis of such a complex. The reaction of this species with a series of substituted radicals allows for the direct interrogation of the rebound process, providing insight into this uniformly invoked, but previously unobserved process.

Original language	English (US)
Pages (from-to)	13640-13643
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	139
Issue number	39
DOIs	https://doi.org/10.1021/jacs.7b07979
State	Published - Oct 4 2017

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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abstract = "The rebound mechanism for alkane hydroxylation was invoked over 40 years ago to help explain reactivity patterns in cytochrome P450, and subsequently has been used to provide insight into a range of biological and synthetic systems. Efforts to model the rebound reaction in a synthetic system have been unsuccessful, in part because of the challenge in preparing a suitable metalhydroxide complex at the correct oxidation level. Herein we report the synthesis of such a complex. The reaction of this species with a series of substituted radicals allows for the direct interrogation of the rebound process, providing insight into this uniformly invoked, but previously unobserved process.",

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AU - Siegler, Maxime A.

AU - Moënne-Loccoz, Pierre

AU - Green, Michael T.

AU - Goldberg, David P.

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AB - The rebound mechanism for alkane hydroxylation was invoked over 40 years ago to help explain reactivity patterns in cytochrome P450, and subsequently has been used to provide insight into a range of biological and synthetic systems. Efforts to model the rebound reaction in a synthetic system have been unsuccessful, in part because of the challenge in preparing a suitable metalhydroxide complex at the correct oxidation level. Herein we report the synthesis of such a complex. The reaction of this species with a series of substituted radicals allows for the direct interrogation of the rebound process, providing insight into this uniformly invoked, but previously unobserved process.

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Direct observation of oxygen rebound with an iron-hydroxide complex

Abstract

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