Insights into the catalytic mechanism of chlorophenol 4-monooxygenase: a quantum mechanics/molecular mechanics study

doi:10.1039/c4ra16165c

QIBEBT-IR > 蛋白质设计研究组

	Insights into the catalytic mechanism of chlorophenol 4-monooxygenase: a quantum mechanics/molecular mechanics study
	Li, Yanwei 1; Zhang, Ruiming 1; Du, Likai2 ; Zhang, Qingzhu 1; Wang, Wenxing 1
	2015
发表期刊	RSC ADVANCES
卷号	5 期号:18 页码:13871-13877
摘要	The catalytic mechanism of chlorophenol 4-monooxygenase (TftD) toward substrates 2,4,5-trichlorophenol (2,4,5-TCP), 2,4,6-trichlorophenol (2,4,6-TCP), and 2,5-dichloro-p-hydroquinone (2,5-DiCHQ) was studied by quantum mechanical/molecular mechanical (QM/MM) investigations. The hydroxylation rather than dechlorination was found to be the rate determining step for all three substrates. Substantial energy barrier spreads on the hydroxylation steps have been found. The corresponding Boltzmann-weighted average barriers are 16.3, 17.8, and 19.7 kcal mol(-1) for 2,4,5-TCP, 2,4,6-TCP, and 2,5-DiCHQ, in accordance with the experimentally determined reaction rates. A previously unnoticed residue Arg100 was found to be important during the hydroxylation steps. Electrostatic influences of ten active site residues on the hydroxylation step were also investigated. Glu251 and Arg366 were highlighted as candidate residues for future mutation studies. In addition, we have shown that spatial location of 2,6-DiCHQ as well as the hydroxylation barrier are the two possible reasons why 2,6-DiCHQ cannot be further degraded by TftD.
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences
DOI	10.1039/c4ra16165c
关键词[WOS]	BURKHOLDERIA-CEPACIA AC1100 ; MICROBIAL-DEGRADATION ; BACTERIAL-DEGRADATION ; OXIDOREDUCTASE TFTC ; CHLORINATED PHENOLS ; MOLECULAR-DYNAMICS ; SINGLE-MOLECULE ; HYDROXYLATION ; OXIDATION ; PROGRAM
收录类别	SCI
语种	英语
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:000349434300076
引用统计	被引频次：11[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.qibebt.ac.cn/handle/337004/6151
专题	蛋白质设计研究组
作者单位	1.Shandong Univ, Environm Res Inst, Jinan 250100, Peoples R China 2.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Key Lab Biobased Mat, Qingdao 266101, Peoples R China
推荐引用方式 GB/T 7714	Li, Yanwei,Zhang, Ruiming,Du, Likai,et al. Insights into the catalytic mechanism of chlorophenol 4-monooxygenase: a quantum mechanics/molecular mechanics study[J]. RSC ADVANCES,2015,5(18):13871-13877.
APA	Li, Yanwei,Zhang, Ruiming,Du, Likai,Zhang, Qingzhu,&Wang, Wenxing.(2015).Insights into the catalytic mechanism of chlorophenol 4-monooxygenase: a quantum mechanics/molecular mechanics study.RSC ADVANCES,5(18),13871-13877.
MLA	Li, Yanwei,et al."Insights into the catalytic mechanism of chlorophenol 4-monooxygenase: a quantum mechanics/molecular mechanics study".RSC ADVANCES 5.18(2015):13871-13877.