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Degradation of Diphenyl Ether in Sphingobium phenoxybenzoativorans SC_ 3 Is Initiated by a Novel Ring Cleavage Dioxygenase

文献类型： 外文期刊

作者： Cai, Shu 1 ; Chen, Li-Wei 2 ; Ai, Yu-Chun 3 ; Qiu, Ji-Guo 1 ; Wang, Cheng-Hong 4 ; Shi, Chao 1 ; He, Jian 1 ; Cai, Tian-M 1 ;

作者机构： 1.Nanjing Agr Univ, Coll Life Sci, Minist Agr, Key Lab Agr Environm Microbiol, Nanjing, Jiangsu, Peoples R China

2.Nanjing Agr Univ, Coll Resources & Environm Sci, Nanjing, Jiangsu, Peoples R China

3.Jiangsu Acad Agr Sci, Inst Agr Resources & Environm, Nanjing, Jiangsu, Peoples R China

4.Jiujiang Univ, Coll Basic Med Sci, Jiujiang, Jiangxi, Peoples R China

关键词： 2-carboxydiphenyl ether;Dpe;Sphingobium;angular dioxygenase;diphenyl ether

期刊名称：APPLIED AND ENVIRONMENTAL MICROBIOLOGY （ 影响因子：4.792； 五年影响因子：5.26 ）

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收录情况： SCI

摘要： Sphingobium phenoxybenzoativorans SC_ 3 degrades and utilizes diphenyl ether (DE) or 2-carboxy-DE as its sole carbon and energy source. In this study, we report the degradation of DE and 2-carboxy-DE initiated by a novel ring cleavage angular dioxygenase (diphenyl ether dioxygenase [Dpe]) in the strain. Dpe functions at the angular carbon and its adjacent carbon (C-1a, C-2) of a benzene ring in DE (or the 2-carboxybenzene ring in 2-carboxy-DE) and cleaves the C-1-C-2 bond (decarboxylation occurs simultaneously for 2-carboxy-DE), yielding 2,4-hexadienal phenyl ester, which is subsequently hydrolyzed to muconic acid semialdehyde and phenol. Dpe is a type IV Rieske non-heme iron oxygenase (RHO) and consists of three components: a hetero-oligomer oxygenase, a [2Fe-2S]-type ferredoxin, and a glutathione reductase (GR)type reductase. Genetic analyses revealed that dpeA1A2 plays an essential role in the degradation and utilization of DE and 2-carboxy-DE in S. phenoxybenzoativorans SC_ 3. Enzymatic study showed that transformation of 1 molecule of DE needs two molecules of oxygen and two molecules of NADH, supporting the assumption that the cleavage of DE catalyzed by Dpe is a continuous two-step dioxygenation process: DE is dioxygenated at C-1a and C-2 to form a hemiacetal-like intermediate, which is further deoxygenated, resulting in the cleavage of the C-1-C-2 bond to form one molecule of 2,4-hexadienal phenyl ester and two molecules of H2O. This study extends our knowledge of the mode and mechanism of ring cleavage of aromatic compounds.

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