Fine Control of the Redox Reactivity of a Nonheme Iron( III)-Peroxo Complex by Binding Redox-Inactive Metal Ions | |
Department | OSSO国家重点实验室 |
Seong Hee Bae1; Yong-Min Lee1; Shunichi Fukuzumi1,2; Wonwoo Nam1,3 | |
2017 | |
Source Publication | Angewandte Chemie International Edition |
ISSN | 1433-7851 |
Volume | 56Issue:3Pages:801-805 |
Abstract | Redox-inactive metal ions are one of the most important co-factors involved in dioxygen activation and formation reactions by metalloenzymes. In this study, we have shown that the logarithm of the rate constants of electron-transfer and C−H bond activation reactions by nonheme iron(III)–peroxo complexes binding redox-inactive metal ions, [(TMC)FeIII(O2)]+-Mn+ (Mn+=Sc3+, Y3+, Lu3+, and La3+), increases linearly with the increase of the Lewis acidity of the redox-inactive metal ions (ΔE), which is determined from the gzz values of EPR spectra of O2.−-Mn+ complexes. In contrast, the logarithm of the rate constants of the [(TMC)FeIII(O2)]+-Mn+ complexes in nucleophilic reactions with aldehydes decreases linearly as the ΔE value increases. Thus, the Lewis acidity of the redox-inactive metal ions bound to the mononuclear nonheme iron(III)–peroxo complex modulates the reactivity of the [(TMC)FeIII(O2)]+-Mn+ complexes in electron-transfer, electrophilic, and nucleophilic reactions. |
Keyword | Iron-peroxo Intermediates Lewis Acidity Nonheme Iron Enzymes Reactive Species Redox-inactive Metal Ions |
Subject Area | 物理化学与绿色催化 |
DOI | 10.1002/anie.201610828 |
Funding Organization | the NRF of Korea through CRI (NRF-2012R1A3A2048842 to W.N.);GRL (NRF-2010-00353 to W.N.);a Grant-in-Aid (no.16H02268 to S.F.)from the Ministry of Education, Culture,Sports,Science and Technology (MEXT);a SENTAN project (to S.F.)from the Japan Science and Technology Agency, Japan |
Indexed By | SCI |
If | 11.994 |
Language | 英语 |
compositor | 第三作者单位 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/21529 |
Collection | 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Shunichi Fukuzumi; Wonwoo Nam |
Affiliation | 1.Ewha Womans Univ, Dept Chem & Nano Sci, Seoul 03760, South Korea 2.Meijo Univ, Fac Sci & Engn, SENTAN Japan Sci & Technol Agcy JST, Nagoya, Aichi 4688502, Japan 3.Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China |
Recommended Citation GB/T 7714 | Seong Hee Bae,Yong-Min Lee,Shunichi Fukuzumi,et al. Fine Control of the Redox Reactivity of a Nonheme Iron( III)-Peroxo Complex by Binding Redox-Inactive Metal Ions[J]. Angewandte Chemie International Edition,2017,56(3):801-805. |
APA | Seong Hee Bae,Yong-Min Lee,Shunichi Fukuzumi,&Wonwoo Nam.(2017).Fine Control of the Redox Reactivity of a Nonheme Iron( III)-Peroxo Complex by Binding Redox-Inactive Metal Ions.Angewandte Chemie International Edition,56(3),801-805. |
MLA | Seong Hee Bae,et al."Fine Control of the Redox Reactivity of a Nonheme Iron( III)-Peroxo Complex by Binding Redox-Inactive Metal Ions".Angewandte Chemie International Edition 56.3(2017):801-805. |
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