TY - JOUR
T1 - Direct observation of oxygen rebound with an iron-hydroxide complex
AU - Zaragoza, Jan Paulo T.
AU - Yosca, Timothy H.
AU - Siegler, Maxime A.
AU - Moënne-Loccoz, Pierre
AU - Green, Michael T.
AU - Goldberg, David P.
N1 - Funding Information:
The authors acknowledge support by the NIH (Grant GM101153 to D.P.G. and Grant GM101390 to M.T.G.). J.P.T.Z. thanks JHU for the Glen E. Meyer ’39 Fellowship. We also thank Dr. R. Baglia for helpful discussions, and T. Pangia for the synthesis of some compounds.
Publisher Copyright:
© 2017 American Chemical Society.
PY - 2017/10/4
Y1 - 2017/10/4
N2 - 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.
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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U2 - 10.1021/jacs.7b07979
DO - 10.1021/jacs.7b07979
M3 - Article
C2 - 28930448
AN - SCOPUS:85032629239
SN - 0002-7863
VL - 139
SP - 13640
EP - 13643
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 39
ER -