Modeling of the molybdenum center in the nitrogenase FeMo-cofactor

被引:73
作者
Barrière, F [1 ]
机构
[1] Natl Univ Ireland Univ Coll Galway, Dept Chem, Galway, Ireland
关键词
nitrogenase; FeMo-cofactor; molybdenum; sulfur; nitrogen fixation; modeling;
D O I
10.1016/S0010-8545(02)00183-2
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The functional, structural and theoretical chemical approaches to specifically model the molybdenum center of the nitrogenase enzyme are reviewed. We show how dinitrogen can be reduced at monometallic centers and highlight attempts to develop a nitrogenase-relevant dinitrogen reduction chemistry at molybdenum-sulfur complexes and clusters. The theoretical work addressing the molybdenum issue is also reported together with models for nitrogenase function, some of them directly involving the molybdenum atom. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:71 / 89
页数:19
相关论文
共 184 条
[31]   THE REACTIONS OF DINITROGEN IN ITS METAL-COMPLEXES [J].
CHATT, J ;
RICHARDS, RL .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1982, 239 (01) :65-77
[32]   PREPARATION, CRYSTAL AND MOLECULAR-STRUCTURE OF [MOCL2(NH)O(ETPH2PO)2] - EXAMPLE OF TERMINAL, NON-LINEAR IMIDO-COORDINATION [J].
CHATT, J ;
CHOUKROUN, R ;
DILWORTH, JR ;
HYDE, J ;
VELLA, P ;
ZUBIETA, J .
TRANSITION METAL CHEMISTRY, 1979, 4 (01) :59-63
[33]   Mechanistic features of the Mo-containing nitrogenase [J].
Christiansen, J ;
Dean, DR ;
Seefeldt, LC .
ANNUAL REVIEW OF PLANT PHYSIOLOGY AND PLANT MOLECULAR BIOLOGY, 2001, 52 :269-+
[34]   ELECTRONIC-STRUCTURE OF THE MOFE3S4(SH)63- ION [J].
COOK, M ;
KARPLUS, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1985, 107 (01) :257-259
[35]   ELECTRONIC-STRUCTURE OF THE MOFE3S4(SH)3/6-ION - A BROKEN-SYMMETRY METAL SULFUR CLUSTER [J].
COOK, M ;
KARPLUS, M .
JOURNAL OF CHEMICAL PHYSICS, 1985, 83 (12) :6344-6366
[36]   Functional analogs for the reduction of certain nitrogenase substrates. Are multiple sites within the Fe/Mo/S active center involved in the 6e(-) reduction of N-2? [J].
Coucouvanis, D .
JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY, 1996, 1 (06) :594-600
[37]   SYNTHESIS, CHARACTERIZATION, AND REACTIVITY OF NEW CLUSTERS THAT CONTAIN THE [MFE3S4]0 CORE, M = MO, W - A WEAKLY PERTURBED [MFE3S4]0 UNIT STRUCTURALLY AND ELECTRONICALLY ANALOGOUS TO THE REDUCED 3-IRON CENTERS IN FERREDOXINS [J].
COUCOUVANIS, D ;
ALAHMAD, SA ;
SALIFOGLOU, A ;
PAPAEFTHYMIOU, V ;
KOSTIKAS, A ;
SIMOPOULOS, A .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (07) :2472-2482
[38]   Catalytic and stoichiometric multielectron reduction of hydrazine to ammonia and acetylene to ethylene with clusters that contain the MFe(3)S(4) cores (M=Mo, V). Relevance to the function of nitrogenase [J].
Coucouvanis, D ;
Demadis, KD ;
Malinak, SM ;
Mosier, PE ;
Tyson, MA ;
Laughlin, LJ .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1996, 107 (1-3) :123-135
[39]   THE CATALYTIC REDUCTION OF HYDRAZINE TO AMMONIA BY THE MOFE3S4 CUBANES AND IMPLICATIONS REGARDING THE FUNCTION OF NITROGENASE - EVIDENCE FOR DIRECT INVOLVEMENT OF THE MOLYBDENUM ATOM IN SUBSTRATE REDUCTION [J].
COUCOUVANIS, D ;
MOSIER, PE ;
DEMADIS, KD ;
PATTON, S ;
MALINAK, SM ;
KIM, CG ;
TYSON, MA .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1993, 115 (25) :12193-12194
[40]   SINGLE AND DOUBLE MOFE3S4 CUBANES WITH MO-COORDINATED POLYCARBOXYLATE LIGANDS - SYNTHESES AND STRUCTURAL CHARACTERIZATION OF (ET4N)4([MOFE3S4CL4]2(MU-C2O4)) AND (ET4N)3[MOFE3S4CL4(C2O4)] CLUSTERS [J].
COUCOUVANIS, D ;
DEMADIS, KD ;
KIM, CG ;
DUNHAM, RW ;
KAMPF, JW .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1993, 115 (08) :3344-3345