Aqueous FeIV=O:: Spectroscopic identification and oxo-group exchange

被引:324
作者
Pestovsky, O
Stoian, S
Bominaar, EL
Shan, XP
Münck, E
Que, L
Bakac, A
机构
[1] Carnegie Mellon Univ, Dept Chem, Pittsburgh, PA 15213 USA
[2] Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA
[3] Univ Minnesota, Ctr Met Biocatalysis, Minneapolis, MN 55455 USA
[4] Iowa State Univ, Ames Lab, Ames, IA 50011 USA
关键词
Fenton reaction; iron; Mossbauer spectroscopy; oxygen; X-ray absorption spectroscopy;
D O I
10.1002/anie.200502686
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
(Figure Presented) A combination of techniques (Mössbauer and X-ray absorption spectroscopy, H218O exchange experiments, and DFT calculations) has shown that the reaction of [Fe(H2O) 6]2+ with ozone generates [(H2O) 5FeIV=O]2+ (see calculated structure). The oxidation of selected substrates with [(H2O)5Fe IV=O]2+ yields unique products that are different from those generated in the Fenton reaction or derived from HO• radicals. © 2005 Wiley-VCH Verlag GmbH & Co. KGaA.
引用
收藏
页码:6871 / 6874
页数:4
相关论文
共 27 条
[1]   Ferryl ion, a compound of tetravalent iron [J].
Bray, WC ;
Gorin, MH .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1932, 54 :2124-2125
[2]   O2 evolution in the Fenton reaction [J].
Buda, F ;
Ensing, B ;
Gribnau, MCM ;
Baerends, EJ .
CHEMISTRY-A EUROPEAN JOURNAL, 2003, 9 (14) :3436-3444
[3]   FORMATION OF IRON(4) IN OXIDATION OF IRON(2) [J].
CONOCCHIOLI, TJ ;
HAMILTON, EJ ;
SUTIN, N .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1965, 87 (04) :926-+
[4]   Comparison of FeIV=O heme and non-heme species:: Electronic structures, bonding, and reactivities [J].
Decker, A ;
Solomon, EI .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (15) :2252-2255
[5]  
DECKER A, 2005, ANGEW CHEM, V44, P2292
[6]  
EBERHARDT MK, 1988, J ORG CHEM, P53
[7]  
Fenton H. J. H., 1894, J CHEM SOC, V65, P899, DOI DOI 10.1039/CT8946500899
[8]   ELECTRON-SPIN RESONANCE STUDIES .43. REACTION OF DIMETHYL-SULFOXIDE WITH HYDROXYL RADICAL [J].
GILBERT, BC ;
NORMAN, ROC ;
SEALY, RC .
JOURNAL OF THE CHEMICAL SOCIETY-PERKIN TRANSACTIONS 2, 1975, (04) :303-308
[9]   STEREOSPECIFIC ALIPHATIC HYDROXYLATION BY AN IRON-BASED OXIDANT [J].
GROVES, JT ;
VANDERPU.M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1974, 96 (16) :5274-5275
[10]   ALIPHATIC HYDROXYLATION VIA OXYGEN REBOUND - OXYGEN-TRANSFER CATALYZED BY IRON [J].
GROVES, JT ;
MCCLUSKY, GA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1976, 98 (03) :859-861