Coordinated design of cofactor and active site structures in development of new protein catalysts

被引:143
|
作者
Ueno, T
Koshiyama, T
Ohashi, M
Kondo, K
Kono, M
Suzuki, A
Yamane, T
Watanabe, Y [1 ]
机构
[1] Nagoya Univ, Grad Sch Sci, Dept Chem, Nagoya, Aichi 4648602, Japan
[2] Nagoya Univ, Res Ctr Mat Sci, Nagoya, Aichi 4648602, Japan
[3] Grad Univ Adv Studies, Dept Struct Mol Sci, Okazaki, Aichi 4448585, Japan
[4] Nagoya Univ, Grad Sch Engn, Dept Biotechnol & Biomat, Nagoya, Aichi 4648602, Japan
关键词
D O I
10.1021/ja045995q
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
New methods for the synthesis of artificial metalloenzymes are important for the construction of novel biocatalysts and biomaterials. Recently, we reported new methodology for the synthesis of artificial metalloenzymes by reconstituting apo-myoglobin with metal complexes (Ohashi, M. et al., Angew Chem., Int. Ed. 2003, 42, 1005-1008). However, it has been difficult to improve their reactivity, since their crystal structures were not available. In this article, we report the crystal structures of M-III(Schiff base)-apo-A71 GMbs (M = Cr and Mn). The structures suggest that the position of the metal complex in apo-Mb is regulated by (i) noncovalent interaction between the ligand and surrounding peptides and (ii) the ligation of the metal ion to proximal histidine (His93). In addition, it is proposed that specific interactions of lle107 with 3- and T-substituent groups on the salen ligand control the location of the Schiff base ligand in the active site. On the basis of these results, we have successfully controlled the enantioselectivity in the sulfoxidation of thioanisole by changing the size of substituents at the 3 and 3' positions. This is the first example of an enantioselective enzymatic reaction regulated by the design of metal complex in the protein active site.
引用
收藏
页码:6556 / 6562
页数:7
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