Sc3+-Triggered Oxoiron(IV) Formation from O2 and its Non-Heme Iron(II) Precursor via a Sc3+-Peroxo-Fe3+ Intermediate

被引：88

作者：

Li, Feifei ^{[1
,2
]}

Van Heuvelen, Katherine M. ^{[1
,2
]}

Meier, Katlyn K. ^{[3
]}

Muenck, Eckard ^{[3
]}

Que, Lawrence, Jr. ^{[1
,2
]}

机构：

[1] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA

[2] Univ Minnesota, Ctr Met Biocatalysis, Minneapolis, MN 55455 USA

[3] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2013年 / 135卷 / 28期

基金：

美国国家科学基金会; 美国国家卫生研究院;

关键词：

COUPLED ELECTRON-TRANSFER; INACTIVE METAL-IONS; DIOXYGEN ACTIVATION; CRYSTAL-STRUCTURE; IRON(IV)-OXO COMPLEX; PEROXO COMPLEXES; HIGH-SPIN; REACTIVITY; PROTON; FE;

D O I：

10.1021/ja402645y

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页码：10198 / 10201

页数：4

共 4 条

[1] The "innocent" role of Sc3+ on a non-heme Fe catalyst in an O2 environment
Poater, Albert
Vummaleti, Sai Vikrama Chaitanya
Cavallo, Luigi
DALTON TRANSACTIONS, 2014, 43 (29) : 11190 - 11194
[2] Sc3+-Promoted O-O Bond Cleavage of a (μ-1,2-Peroxo)diiron(III) Species Formed from an Iron(11) Precursor and O2 to Generate a Complex with an Fe2IV(μ-O)2 Core
Banerjee, Saikat
Draksharapu, Apparao
Crossland, Patrick M.
Fan, Ruixi
Guo, Yisong
Swart, Marcel
Que, Lawrence, Jr.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (09) : 4285 - 4297
[3] An approach to the O2 activating mononuclear non-heme Fe enzymes:: structural characterization of Fe(II)-acetato complex and formation of alkylperoxoiron(III) species with the highly hindered hydrotris(3-tert-butyl-5-isopropyl-1-pyrazolyl)borate
Ogihara, T
Hikichi, S
Akita, M
Uchida, T
Kitagawa, T
Moro-oka, Y
INORGANICA CHIMICA ACTA, 2000, 297 (1-2) : 162 - 170
[4] β-Fe2O3 nanomaterials from an iron(II) diketonate-diamine complex: a study from molecular precursor to growth process
Barreca, Davide
Carraro, Giorgio
Devi, Anjana
Fois, Ettore
Gasparotto, Alberto
Seraglia, Roberta
Maccato, Chiara
Sada, Cinzia
Tabacchi, Gloria
Tondello, Eugenio
Venzo, Alfonso
Winter, Manuela
DALTON TRANSACTIONS, 2012, 41 (01) : 149 - 155

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