On the structure of a proposed mixed-valent analogue of the diiron subsite of [FeFe]-hydrogenase

被引:57
作者
Best, Stephen P. [1 ]
Borg, Stacey J.
White, Jonathan M.
Razavet, Mathieu
Pickett, Christopher J.
机构
[1] Univ Melbourne, Sch Chem, Melbourne, Vic, Australia
[2] Univ E Anglia, Sch Chem & Pharm, Norwich NR4 7TJ, Norfolk, England
关键词
D O I
10.1039/b712758h
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We show that a dinuclear assembly apparently providing the first example of a synthetic molecule exhibiting key features of the diiron subsite of [FeFe] hydrogenase, viz. CO-bridging of a coordinatively unsaturated, dithiolate- bridged mixed-valence diiron centre, is in fact a diamagnetic tetranuclear complex.
引用
收藏
页码:4348 / 4350
页数:3
相关论文
共 22 条
[1]   Integration of EXAFS, spectroscopic, and DFT techniques for elucidation of the structure of reactive diiron compounds [J].
Bondin, MI ;
Borg, SJ ;
Cheah, MH ;
Foran, G ;
Best, SP .
AUSTRALIAN JOURNAL OF CHEMISTRY, 2006, 59 (04) :263-272
[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]   Assignment of molecular structures to the electrochemical reduction products of diiron compounds related to [Fe-Fe] hydrogenase: A combined experimental and density functional theory study [J].
Borg, Stacey J. ;
Tye, Jesse W. ;
Hall, Michael B. ;
Best, Stephen P. .
INORGANIC CHEMISTRY, 2007, 46 (02) :384-394
[4]  
CAO WM, 2007, INORG CHEM, V46, P1981
[5]   Electrochemical and theoretical investigations of the reduction of [Fe2(CO)5L{μ-SCH2XCH2S}] complexes related to [FeFe] hydrogenase [J].
Capon, Jean-Francois ;
Ezzaher, Salah ;
Gloaguen, Frederic ;
Petillon, Francois Y. ;
Schollhammer, Philippe ;
Talarmin, Jean ;
Davin, Thomas J. ;
McGrady, John E. ;
Muir, Kenneth W. .
NEW JOURNAL OF CHEMISTRY, 2007, 31 (12) :2052-2064
[6]   Modeling [Fe-Fe] hydrogenase: evidence for bridging carbonyl and distal iron coordination vacancy in an electrocatalytically competent proton reduction by an iron thiolate assembly that operates through Fe(0)-Fe(II) levels [J].
Cheah, Mun Hon ;
Tard, Cedric ;
Borg, Stacey J. ;
Liu, Xiaoming ;
Ibrahim, Saad K. ;
Pickett, Christopher J. ;
Best, Stephen P. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (36) :11085-11092
[7]   Steps along the path to dihydrogen activation at [FeFe] hydrogenase structural models: Dependence of the core geometry on electrocatalytic proton reduction [J].
Cheah, Mun Hon ;
Borg, Stacey J. ;
Best, Stephen P. .
INORGANIC CHEMISTRY, 2007, 46 (05) :1741-1750
[8]   Active-site models for iron hydrogenases: Reduction chemistry of dinuclear iron complexes [J].
de Carcer, Inigo Aguirre ;
DiPasquale, Antonio ;
Rheingold, Arnold L. ;
Heinekey, D. Michael .
INORGANIC CHEMISTRY, 2006, 45 (20) :8000-8002
[9]   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
[10]   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