Coordination of Coenzyme M and Its Derivatives on NiII(tetraazacycle) Complexes: A Model for the Active Site of Methyl Coenzyme M Reductase

被引：10
|
作者：
Nishigaki, Jun-ichi [1 ,2 ]
Matsumoto, Tsuyoshi [1 ,2 ]
Tatsumi, Kazuyuki [1 ,2 ]
机构：
[1] Nagoya Univ, Grad Sch Sci, Res Ctr Mat Sci, Chikusa Ku, Nagoya, Aichi 4648602, Japan
[2] Nagoya Univ, Grad Sch Sci, Dept Chem, Chikusa Ku, Nagoya, Aichi 4648602, Japan
来源：
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY | 2010年 / 31期
关键词：
Enzyme models; Nickel; Tetraazamacrocycle; Methanogenesis; Methane; BIOLOGICAL METHANE FORMATION; METHANOBACTERIUM-THERMOAUTOTROPHICUM; NICKEL(II) COMPLEXES; CRYSTAL-STRUCTURE; MACROCYCLIC LIGANDS; SECONDARY AMINE; METAL-COMPLEXES; EQUILIBRIUM; SOLVENTS; ION;
D O I：
10.1002/ejic.201000801
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
A series of tetraazamacrocyclic nickel(II) complexes coordinated by methyl coenzyme M (MeSCoM), coenzyme M (HSCoM), and 3-methylthiopropionate (Metp) have been synthesized as structural models of the active site of methyl coenzyme M reductase in the oxidized MCRsilent state. They include RSRS-[Ni(tmc)(L)](OTf) {L = MeSCoM (2), HSCoM (4), and Metp (5)} (tmc = 1,4,8,11-tetramethyl- 1,4,8,11-tetraazacyclotetradecane) and [Ni(pyc)(L)](OTf) (L = MeSCoM (6), HSCoM (7), Metp (8), pyc = 5-oxo-7-(2-pyridyl)-1,4,8,11-tetraazacyclotetradecane). The X-ray crystal analysis revealed that MeSCoM, HSCoM, and Metp are bound to Ni in an eta(1) manner through interactions with one O atom of each ligand. The tmc complexes assume a pentacoordinate geometry, which is in between a square pyramid and a trigonal bipyramid, while the pyc complexes are octahedral with coordination of the pendant pyridine at the site trans to the sulfonate or carboxylate ligand.
引用
收藏
页码：5011 / 5017
页数：7
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