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Titolo:
A polyoxoanion-based iron(II) catechol extradiol dioxygenase: oxygenation of 3,5-di-tert-butylcatechol by the polyoxoanion-supported iron(II) complex(n-Bu4N)(7)[(CH3CN)(x)Fe-II center dot P2W15Nb3O62]
Autore:
Weiner, H; Hayashi, Y; Finke, RG;
Indirizzi:
Colorado State Univ, Dept Chem, Ft Collins, CO 80523 USA Colorado State Univ Ft Collins CO USA 80523 hem, Ft Collins, CO 80523 USA Kanazawa Univ, Dept Chem, Kanazawa, Ishikawa 92011, Japan Kanazawa Univ Kanazawa Ishikawa Japan 92011 nazawa, Ishikawa 92011, Japan
Titolo Testata:
INORGANICA CHIMICA ACTA
fascicolo: 1-2, volume: 291, anno: 1999,
pagine: 426 - 437
SICI:
0020-1693(199908)291:1-2<426:APICED>2.0.ZU;2-Q
Fonte:
ISI
Lingua:
ENG
Soggetto:
METAL-OXIDE ANALOGS; REACTIVE FUNCTIONAL-MODEL; TRISUBSTITUTED HETEROPOLYTUNGSTATES; CATALYST PRECURSORS; ORGANOMETALLIC COMPLEX; HOMOGENEOUS CATALYSIS; MOLECULAR-OXYGEN; ACTIVE-SITES; 1,2-DIOXYGENASE; IRIDIUM(I);
Keywords:
oxygenation; iron complexes; polyoxometalate complexes;
Tipo documento:
Article
Natura:
Periodico
Settore Disciplinare:
Physical, Chemical & Earth Sciences
Citazioni:
65
Recensione:
Indirizzi per estratti:
Indirizzo: Finke, RG Colorado State Univ, Dept Chem, Ft Collins, CO 80523 USA Colorado State Univ Ft Collins CO USA 80523 llins, CO 80523 USA
Citazione:
H. Weiner et al., "A polyoxoanion-based iron(II) catechol extradiol dioxygenase: oxygenation of 3,5-di-tert-butylcatechol by the polyoxoanion-supported iron(II) complex(n-Bu4N)(7)[(CH3CN)(x)Fe-II center dot P2W15Nb3O62]", INORG CHIM, 291(1-2), 1999, pp. 426-437

Abstract

The stoichiometric oxygenation of 3,5-di-tert-butylcatechol (DTBC) with molecular oxygen at 25 degrees C and using the novel polyoxoanion-supported Fe-II complex, (n-Bu4N)(7)[(CH3CN)(x) Fe-II. P2W15Nb3O62] (1), is reported. This is the first report of an iron(II) plus polyoxoanion-based catechol dioxygenase. The catechol oxygenation reaction exhibits a clean, 1:1 DTBC:I stoichiometry to form 1 DTBC; this complex then exhibits a substrate-triggered binding of 1.0 equiv. of O-2 to form a 1:1:1 complex 1 . DTBC . O-2, thereby proving the 1:1 catechol to O-2 stoichiometry which defines a dioxygenase reaction. The overall oxygenation of DTBC proceeds through three distinct reaction stages (A --> B --> C --> D), each stage being slower than the previous stage and of a different absorption maximum. Each intermediate can, therefore, be observed directly, another valuable feature of the present system, and a feature which should allow characterization of reaction intermediates and kinetic and mechanistic studies in a bona fide Fe-II, non-enzymatic dioxygenase system. The observed catechol cleavage products are extradiol ring-cleavage products characteristic of Fe-II extradiol enzymes; the non-ambiguity about the Fe-II oxidation state, and, hence, the ability to correlate unambiguously the Fe-II initial oxidation state with the formationof only extradiol products in a synthetic dioxygenase system is another important feature of the present system. The choice of the all-inorganic, oxidation resistant polyoxoanion ligand system is significant as well en routeto the goal of achieving a long-lived, catalytic dioxygenase system without the need to worry about catalyst lifetime-limiting, ligand-oxidation sidereactions. (C) 1999 Elsevier Science S.A. All rights reserved.

ASDD Area Sistemi Dipartimentali e Documentali, Università di Bologna, Catalogo delle riviste ed altri periodici
Documento generato il 01/12/20 alle ore 10:15:29