Catalytic mechanism of C-F bond cleavage: insights from QM/MM analysis of fluoroacetate dehalogenase

doi:10.1039/c5cy00777a

QIBEBT-IR > 蛋白质设计研究组

	Catalytic mechanism of C-F bond cleavage: insights from QM/MM analysis of fluoroacetate dehalogenase
	Li, Yanwei 1; Zhang, Ruiming 1; Du, Likai2 ; Zhang, Qingzhu 1; Wang, Wenxing 1
	2016
发表期刊	CATALYSIS SCIENCE & TECHNOLOGY
卷号	6 期号:1 页码:73-80
摘要	The catalytic mechanisms of fluoroacetate dehalogenase (FAcD) toward substrates fluoroacetate and chloroacetate were studied by a combined quantum mechanics/molecular mechanics (QM/MM) method. There are twenty snapshots considered for each of the three individual systems. By analyzing multiple independent snapshots, positive or negative relationships between energy barriers and structural parameters in defluorination and dechlorination processes were established. We have also shown that conformational variations may cause enzymatic preference differences toward competitive pathways. Besides residues Arg111, Arg114, His155, Trp156, and Tyr219, the importance of residues His109, Asp134, Lys181, and His280 during the defluorination process were also highlighted through electrostatic analysis. These results may provide clues for designing new biomimetic catalysts toward degradation of fluorinated compounds.
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences
DOI	10.1039/c5cy00777a
关键词[WOS]	BURKHOLDERIA SP FA1 ; SINGLE-MOLECULE ; ENZYME CATALYSIS ; DYNAMICS ; REACTIVITY ; PROGRAM ; OXIDATION ; FLUORINE ; CHARMM
收录类别	SCI
语种	英语
WOS研究方向	Chemistry
项目资助者	NSFC (National Natural Science Foundation of China)(21337001 ; SPNSFC (Shandong Provincial Natural Science Foundation, China)(ZR2015PB002) ; FRFSU (Fundamental Research Funds of Shandong University)(2015GN007) ; GFGCPSF (General Financial Grant from the China Postdoctoral Science Foundation)(2015M570594) ; 21577082 ; 21507073 ; 21177077)
WOS类目	Chemistry, Physical
WOS记录号	WOS:000366857300004
引用统计
文献类型	期刊论文
条目标识符	http://ir.qibebt.ac.cn/handle/337004/6850
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. Catalytic mechanism of C-F bond cleavage: insights from QM/MM analysis of fluoroacetate dehalogenase[J]. CATALYSIS SCIENCE & TECHNOLOGY,2016,6(1):73-80.
APA	Li, Yanwei,Zhang, Ruiming,Du, Likai,Zhang, Qingzhu,&Wang, Wenxing.(2016).Catalytic mechanism of C-F bond cleavage: insights from QM/MM analysis of fluoroacetate dehalogenase.CATALYSIS SCIENCE & TECHNOLOGY,6(1),73-80.
MLA	Li, Yanwei,et al."Catalytic mechanism of C-F bond cleavage: insights from QM/MM analysis of fluoroacetate dehalogenase".CATALYSIS SCIENCE & TECHNOLOGY 6.1(2016):73-80.