Sc3+-Triggered Oxoiron(IV) Formation from O-2 and its Non-Heme Iron(II) Precursor via a Sc3+-Peroxo-Fe3+ Intermediate

Feifei Li; Katherine M. Van Heuvelen; Katlyn K. Meier; Eckard Muenck; Lawrence Que

doi:10.1021/ja402645y

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Sc3+-Triggered Oxoiron(IV) Formation from O-2 and its Non-Heme Iron(II) Precursor via a Sc3+-Peroxo-Fe3+ Intermediate

Journal article

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Sc3+-Triggered Oxoiron(IV) Formation from O-2 and its Non-Heme Iron(II) Precursor via a Sc3+-Peroxo-Fe3+ Intermediate

Feifei Li, Katherine M. Van Heuvelen, Katlyn K. Meier, Eckard Muenck and Lawrence Que

Journal of the American Chemical Society, Vol.135(28), pp.10198-10201

2013-07-17

DOI: https://doi.org/10.1021/ja402645y

PMID: 23802702

Abstract

Chemistry

Chemistry, Multidisciplinary

Physical Sciences

Science & Technology

We report that redox-inactive Sc3+ can trigger O-2 activation by the Fe-II(TMC) center (TMC = tetramethylcyclam) to generate the corresponding oxoiron(IV) complex in the presence of BPh4- as an electron donor. To model a possible intermediate in the above reaction, we generated an unprecedented Sc3+ adduct of [Fe-III(eta(2)-O-2)(TMC)](+) by an alternative route, which was found to have an Fe3+-(mu-eta(2):eta(2)-peroxo)-Sc3+ core and to convert to the oxoiron(IV) complex. These results have important implications for the role a Lewis acid can play in facilitating O-O bond deavage during the course of O-2 activation at non-heme iron centers.

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Collaboration types: Domestic collaboration
Citation topics: 2 Chemistry; 2.22 Inorganic & Nuclear Chemistry; 2.22.1421 Hemocyanin
Web Of Science research areas: Chemistry, Multidisciplinary
ESI research areas: Chemistry

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Title: Sc3+-Triggered Oxoiron(IV) Formation from O-2 and its Non-Heme Iron(II) Precursor via a Sc3+-Peroxo-Fe3+ Intermediate
Creators: Feifei Li - University of Minnesota
Katherine M. Van Heuvelen - University of Minnesota
Katlyn K. Meier - Carnegie Mellon University
Eckard Muenck - Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA
Lawrence Que - University of Minnesota
Publication Details: Journal of the American Chemical Society, Vol.135(28), pp.10198-10201
Publisher: Amer Chemical Soc
Number of pages: 4
Grant note: 1058248 / Direct For Mathematical & Physical Scien; National Science Foundation (NSF); NSF - Directorate for Mathematical & Physical Sciences (MPS) R01EB001475 / NATIONAL INSTITUTE OF BIOMEDICAL IMAGING AND BIOENGINEERING; United States Department of Health & Human Services; National Institutes of Health (NIH) - USA; NIH National Institute of Biomedical Imaging & Bioengineering (NIBIB) NIH; United States Department of Health & Human Services; National Institutes of Health (NIH) - USA EB001475; GM093479 / National Institutes of Health; United States Department of Health & Human Services; National Institutes of Health (NIH) - USA University of Minnesota; University of Minnesota System DOE; United States Department of Energy (DOE) F32GM093479 / NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES; United States Department of Health & Human Services; National Institutes of Health (NIH) - USA; NIH National Institute of General Medical Sciences (NIGMS) CHE1058248 / National Science Foundation; National Science Foundation (NSF)
Academic Unit: A&S - Chemistry; College of A&S
Language: English
Resource Type: Journal article
PMID: 23802702
Record Identifier: 991031713544802976