Modeling nickel hydrogenases:: Synthesis and structure of a distorted octahedral complex with an unprecedented [NiS4H2] core

被引:71
作者
Alvarez, HM
Krawiec, M [1 ]
Donovan-Merkert, BT
Fouzi, M
Rabinovich, D
机构
[1] Clemson Univ, Dept Chem, Ctr Mol Struct, Clemson, SC 29634 USA
[2] Univ N Carolina, Dept Chem, Charlotte, NC 28223 USA
关键词
D O I
10.1021/ic0155838
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The homoleptic nickel(H) bis(mereaptoimidazolyl)-borate complex Ni(Bm(Me))(2) has been readily synthesized in good yield and characterized by a combination of analytical and spectroscopic techniques. Its X-ray structure confirmed the presence of a novel [NiS4H2] species having two cis Ni . . .H-B interactions and an overall distorted octahedral geometry, thereby providing an unprecedented structural model compound for the active form of the nickel center in NiFe hydrogenases.
引用
收藏
页码:5736 / +
页数:3
相关论文
共 29 条
  • [1] The synthesis and molecular structure of [TmPh]2Pb:: a complex with an 'inverted' η4-coordination mode for the tris(2-mercapto-1-phenylimidazolyl)hydroborato ligand
    Bridgewater, BM
    Parkin, G
    [J]. INORGANIC CHEMISTRY COMMUNICATIONS, 2000, 3 (10) : 534 - 536
  • [2] CARBORANE COMPLEXES OF NICKEL AND PLATINUM - SYNTHESIS AND PROTONATION REACTIONS OF ANIONIC ALLYL(CARBORANE) SPECIES
    CARR, N
    MULLICA, DF
    SAPPENFIELD, EL
    STONE, FGA
    [J]. INORGANIC CHEMISTRY, 1994, 33 (08) : 1666 - 1673
  • [3] Infrared spectroelectrochemical characterization of the [NiFe] hydrogenase of Desulfovibrio gigas
    deLacey, AL
    Hatchikian, EC
    Volbeda, A
    Frey, M
    FontecillaCamps, JC
    Fernandez, VM
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1997, 119 (31) : 7181 - 7189
  • [4] Nature and electronic structure of the Ni-X dinuclear center of Desulfovibrio gigas hydrogenase. Implications for the enzymatic mechanism
    Dole, F
    Fournel, A
    Magro, V
    Hatchikian, EC
    Bertrand, P
    Guigliarelli, B
    [J]. BIOCHEMISTRY, 1997, 36 (25) : 7847 - 7854
  • [5] THE DETERMINATION OF THE PARAMAGNETIC SUSCEPTIBILITY OF SUBSTANCES IN SOLUTION BY NUCLEAR MAGNETIC RESONANCE
    EVANS, DF
    [J]. JOURNAL OF THE CHEMICAL SOCIETY, 1959, (JUN): : 2003 - 2005
  • [6] Recent theoretical predictions of the active site for the observed forms in the catalytic cycle of Ni-Fe hydrogenase
    Fan, HJ
    Hall, MB
    [J]. JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 2001, 6 (04): : 467 - 473
  • [7] Nickel-iron-sulfur active sites: Hydrogenase and co dehydrogenase
    Fontecilla-Camps, JC
    Ragsdale, SW
    [J]. ADVANCES IN INORGANIC CHEMISTRY, VOL 47, 1999, 47 : 283 - 333
  • [8] Frey M, 1998, STRUCT BOND, V90, P97
  • [9] Re and Tc complexes containing B-H•••M agostic interactions as building blocks for the design of radiopharmaceuticals
    Garcia, R
    Paulo, A
    Domingos, A
    Santos, I
    Ortner, K
    Alberto, R
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (45) : 11240 - 11241
  • [10] Hydrotris(methimazolyl)borate, a soft analogue of hydrotris(pyrazolyl)borate. Preparation and crystal structure of a novel zinc complex
    Garner, M
    Reglinski, J
    Cassidy, I
    Spicer, MD
    Kennedy, AR
    [J]. CHEMICAL COMMUNICATIONS, 1996, (16) : 1975 - 1976