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DOI | 10.1038/s41467-017-02755-y |
Cobamide-mediated enzymatic reductive dehalogenation via long-range electron transfer | |
Kunze, Cindy1; Bommer, Martin2,4; Hagen, Wilfred R.3; Uksa, Marie1,5; Dobbek, Holger2; Schubert, Torsten1; Diekert, Gabriele1 | |
2017-07-03 | |
发表期刊 | NATURE COMMUNICATIONS
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ISSN | 2041-1723 |
出版年 | 2017 |
卷号 | 8 |
文章类型 | Article |
语种 | 英语 |
国家 | Germany; Netherlands |
英文摘要 | The capacity of metal-containing porphyrinoids to mediate reductive dehalogenation is implemented in cobamide-containing reductive dehalogenases (RDases), which serve as terminal reductases in organohalide-respiring microbes. RDases allow for the exploitation of halogenated compounds as electron acceptors. Their reaction mechanism is under debate. Here we report on substrate-enzyme interactions in a tetrachloroethene RDase (PceA) that also converts aryl halides. The shape of PceA's highly apolar active site directs binding of bromophenols at some distance from the cobalt and with the hydroxyl substituent towards the metal. A close cobalt-substrate interaction is not observed by electron paramagnetic resonance spectroscopy. Nonetheless, a halogen substituent para to the hydroxyl group is reductively eliminated and the path of the leaving halide is traced in the structure. Based on these findings, an enzymatic mechanism relying on a long-range electron transfer is concluded, which is without parallel in vitamin B12-dependent biochemistry and represents an effective mode of RDase catalysis. |
领域 | 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000404575300001 |
WOS关键词 | DEHALOSPIRILLUM-MULTIVORANS ; MACROMOLECULAR CRYSTALLOGRAPHY ; SULFUROSPIRILLUM-MULTIVORANS ; CATALYTIC PATHWAY ; TETRACHLOROETHENE ; PURIFICATION ; CLONING ; HALORESPIRATION ; DECHLORINATION ; BIOSYNTHESIS |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/203637 |
专题 | 资源环境科学 |
作者单位 | 1.Friedrich Schiller Univ, Inst Microbiol, Dept Appl & Ecol Microbiol, Philosophenweg 12, D-07743 Jena, Germany; 2.Humboldt Univ, Inst Biol, Struct Biol Biochem, Philippstr 13, D-10115 Berlin, Germany; 3.Delft Univ Technol, Fac Appl Sci, Dept Biotechnol, Maasweg 9, NL-2629 HZ Delft, Netherlands; 4.Max Delbruck Centrum Mol Med, Robert Roessle Str 10, D-13092 Berlin, Germany; 5.Univ Hohenheim, Inst Soil Sci & Land Evaluat, Emil Wolff Str 27, D-70593 Stuttgart, Germany |
推荐引用方式 GB/T 7714 | Kunze, Cindy,Bommer, Martin,Hagen, Wilfred R.,et al. Cobamide-mediated enzymatic reductive dehalogenation via long-range electron transfer[J]. NATURE COMMUNICATIONS,2017,8. |
APA | Kunze, Cindy.,Bommer, Martin.,Hagen, Wilfred R..,Uksa, Marie.,Dobbek, Holger.,...&Diekert, Gabriele.(2017).Cobamide-mediated enzymatic reductive dehalogenation via long-range electron transfer.NATURE COMMUNICATIONS,8. |
MLA | Kunze, Cindy,et al."Cobamide-mediated enzymatic reductive dehalogenation via long-range electron transfer".NATURE COMMUNICATIONS 8(2017). |
条目包含的文件 | 条目无相关文件。 |
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