A QM/MM study of the initial steps of catalytic mechanism of nitrile hydratase

被引：7

作者：

Kayanuma, Megumi ^{[1
]}

Hanaoka, Kyohei ^{[2
]}

Shoji, Mitsuo ^{[2
]}

Shigeta, Yasuteru ^{[2
]}

机构：

[1] Univ Tsukuba, Grad Sch Syst & Informat Engn, Tsukuba, Ibaraki 3058573, Japan

[2] Univ Tsukuba, Grad Sch Pure & Appl Sci, Tsukuba, Ibaraki 3058571, Japan

来源：

CHEMICAL PHYSICS LETTERS | 2015年 / 623卷

基金：

日本学术振兴会;

关键词：

MOLECULAR-ORBITAL METHODS; NONHEME IRON; ELECTRONIC-STRUCTURE; SULFENIC ACIDS; ENZYME;

D O I：

10.1016/j.cplett.2015.01.039

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Four possible reaction paths of an Fe-containing nitrile hydratase (NHase) are examined using the method of hybrid quantum mechanics/molecular mechanics (QM/MM) to reveal the initial steps of the catalytic mechanism of NHases. The reaction barrier for a nucleophilic attack of the sulfenic oxygen of alpha Cys114-SO- to the substrate is the lowest among the four paths, though another path, in which a water molecule activated by alpha Cys114-SO- attacks the substrate, also has a low enough barrier. Under the protein environment, beta Arg56 has weaker proton donor ability and shows no proton transfer to alpha Cys114-SO-, which was reported in model clusters. (C) 2015 Elsevier B.V. All rights reserved.

引用

页码：8 / 13

页数：6

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