Unsaturated, mixed-valence diiron dithiolate model for the Hox state of the [FeFe] hydrogenase

被引：137

作者：

Justice, Aaron K. ^{[1
]}

Rauchfuss, Thomas B. ^{[1
]}

Wilson, Scott R. ^{[1
]}

机构：

[1] Univ Illinois, Dept Chem, Urbana, IL 61801 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2007年 / 46卷 / 32期

关键词：

hydrogen; hydrogenases; iron; mixed-valent compounds; thiolates;

D O I：

10.1002/anie.200702224

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

(Chemical Equation Presented) Chemists are closing in on functional and structural models for the [FeFe] hydrogenases. Oxidation of [Fe 2(S2C2H4) (CO)3-(PMe 3)(dppv)] (dppv = cis-1,2-C2H2-(PPh 2)2) by one electron affords a mixed-valence model for the Hox state of the active site of the [FeFe] hydrogenases. Like the enzyme, this model exhibits the rotated structure" and binds CO (see scheme). The radical character of the model is confirmed by its ready binding of NO. © 2007 Wiley-VCH Verlag GmbH & Co. KGaA."

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页码：6152 / 6154

页数：3

相关论文

共 21 条

[1] The active site of the [FeFe]-hydrogenase from Desulfovibrio desulfuricans.: 1.: Light sensitivity and magnetic hyperfine interactions as observed by electron paramagnetic resonance [J].

Albracht, SPJ ;

Roseboom, W ;

Hatchikian, EC .

JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 2006, 11 (01) :88-101

[2] Electron transfer at a dithiolate-bridged diiron assembly: Electrocatalytic hydrogen evolution [J].

Borg, SJ ;

Behrsing, T ;

Best, SP ;

Razavet, M ;

Liu, XM ;

Pickett, CJ .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (51) :16988-16999

[3] FTIR characterization of the active site of the Fe-hydrogenase from Desulfovibrio desulfuricans [J].

De Lacey, AL ;

Stadler, C ;

Cavazza, C ;

Hatchikian, EC ;

Fernandez, VM .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (45) :11232-11233

[4] An insight into the protonation property of a diiron azadithiolate complex pertinent to the active site of Fe-only hydirogenases [J].

Dong, WB ;

Wang, M ;

Liu, XY ;

Jin, K ;

Li, GH ;

Wang, FJ ;

Sun, LC .

CHEMICAL COMMUNICATIONS, 2006, (03) :305-307

[5] Bio-inspired, side-on attachment of a ruthenium photosensitizer to an iron hydrogenase active site model [J].

Ekstoem, Jesper ;

Abrahamsson, Maria ;

Olson, Carol ;

Bergquist, Jonas ;

Kaynak, Filiz B. ;

Eriksson, Lars ;

Licheng, Sun ;

Becker, Hans-Christian ;

Akermark, Bjoern ;

Hammarstroem, Leif ;

Ott, Sascha .

DALTON TRANSACTIONS, 2006, (38) :4599-4606

[6] Chemistry and the hydrogenases [J].

Evans, DJ ;

Pickett, CJ .

CHEMICAL SOCIETY REVIEWS, 2003, 32 (05) :268-275

[7] Evidence for the formation of terminal hydrides by protonation of an asymmetric iron hydrogenase active site mimic [J].

Ezzaher, Salah ;

Capon, Jean-Francois ;

Gloaguen, Frederic ;

Petillon, Francois Y. ;

Schollhammer, Philippe ;

Talarmin, Jean .

INORGANIC CHEMISTRY, 2007, 46 (09) :3426-3428

[8]

Frey M, 2002, CHEMBIOCHEM, V3, P153, DOI 10.1002/1439-7633(20020301)3:2/3<153::AID-CBIC153>3.0.CO

[9]

2-B

[10]

Georgekaki I. P., 2004, COMP COORD CHEM 2, VII, P549