Insights into the catalytic mechanism of chlorophenol 4-monooxygenase: a quantum mechanics/molecular mechanics study
文献类型：期刊论文
| 作者 | Li, Yanwei1; Zhang, Ruiming1; Du, Likai2 ; Zhang, Qingzhu1; Wang, Wenxing1
|
| 刊名 | RSC ADVANCES
 |
| 出版日期 | 2015 |
| 卷号 | 5期号:18页码:13871-13877 |
| 英文摘要 | 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. |
| WOS标题词 | Science & Technology ; Physical Sciences |
| 类目[WOS] | Chemistry, Multidisciplinary |
| 研究领域[WOS] | Chemistry |
| 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记录号 | WOS:000349434300076 |
| 公开日期 | 2015-12-24 |
| 源URL | [http://ir.qibebt.ac.cn/handle/337004/6151]  |
| 专题 | 青岛生物能源与过程研究所_仿真模拟团队 |
| 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. |
入库方式： OAI收割
来源：青岛生物能源与过程研究所
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