Reactions of methane monooxygenase intermediate Q with derivatized methanes

Reactions of methane monooxygenase intermediate Q with derivatized methanes
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DOI:
10.1021/ja0265759
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发表时间:
2002-07-31
影响因子:
15
通讯作者:
Lippard, SJ
Lippard, SJ
中科院分区:
化学1区
文献类型:
--
作者:
Ambundo, EA;Friesner, RA;Lippard, SJ

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描述了荚膜甲基球菌(methylococcus capsulatus, Bath)可溶性甲烷单加氧酶中间Q与一系列通式为CH3−R的衍生甲烷(R = CN、NO2和OH)及其氘化类似物的反应性。尽管反应相对缓慢,但在与乙腈和硝基甲烷的反应中观察到显著的动力学同位素效应(KIEs);但是,用甲醇都不能得到。此外,观察到底物氧化之前发生底物结合步骤的证据。
The reactivity of intermediate Q of soluble methane monooxygenase fromMethylococcus capsulatus(Bath) with a series of derivatized methanes of general formula CH3−R, where R = CN, NO2, and OH, and their deuterated analogues is described. Despite relatively slow reactions, significant kinetic isotope effects, KIEs, are observed in reactions with acetonitrile and nitromethane; however, none is obtained with methanol. In addition, evidence of a substrate-binding step that occurs prior to substrate oxidation is observed.