Microbial detoxification of 2,4,6-tribromophenol via a novel process with consecutive oxidative and hydrolytic debromination: Biochemical, genetic and evolutionary characterization
Min, Jun2,3,4; Fang, Suyun4; Peng, Jian4; Lv, Xin4; Xu, Lingxue4; Li, Yan1; Hu, Xiaoke2,3,4
刊名ENVIRONMENTAL RESEARCH
2022-04-01
卷号205页码:10
关键词Brominated flame retardants Comparative genomics Dehalogenation mechanism Cluster evolution (H2O)-O-18-Labeling analysis
ISSN号0013-9351
DOI10.1016/j.envres.2021.112494
通讯作者Hu, Xiaoke(xkhu@yic.ac.cn)
英文摘要As a typical brominated flame retardants (BFRs), 2,4,6-tribromophenol (TBP) has serious hazard to the environmental health and its environmental fate has attracted considerable attention. Dehalogenation reaction plays key role in microbial TBP degradation and detoxification. So far, several halophenols-degrading enzymes have been reported to transform their substrate by oxidative dehalogenation; however, the molecular and biochemistry characterization of microbial hydrolytic dehalogenation is limited. In this study, Cupriavidus sp. CNP-8 with high TBP degradation activity was found to degrade TBP via an obviously differnet pathway as compared to other reported TBP-degraders. The transcription of Imp genes were significantly upregulated with TBP stimulation, indicating their involvment in TBP degradation. Enzymatic assays with O-18-labeling experiments showed that HnpAB, a two-component FAD-dependent monooxygenase, transformed TBP via consecutive oxidative and hydrolytic debromination reactions with the formation of 6-bromo-1,2,4-benzenetriol (BBT) as the ring-cleavage substrate. The function of the BBT ring-cleavage enzyme (HnpC) was also characterized both in vitro and in vivo. This finding provides new molecular mechanism of microbial detoxification of TBP and novel information of the environmental fate of this BFRs. Furthermore, to investigate the frequency of this novel dehalogenation mechanism in microbes, we also analyzed the distribution as well as the genetic structure of the hnpABC cluster by comparative genomics. Although hnpA homolog is distributed in several bacterial genera including Cupriavidus, Paraburkholderia, Variovorax and Streptomyces, the complete hnpABC cluster is only retrieved from Cupriavidus and strictly conservative in the genomes. This indicated that Cupriavidus have unique evolutionary pattern in acquiring the hnpABC to degrade TBP and its analogs, enhancing our understanding of the microbial adaptive evolution in halophenols-contaminated environment.
WOS关键词BROMINATED FLAME RETARDANTS ; REDUCTIVE DEHALOGENATION ; STRAIN ; BIODEGRADATION ; NITROPHENOL ; DEGRADATION ; CATABOLISM ; PATHWAY ; CATALYZES ; 2,4,6-TRICHLOROPHENOL
WOS研究方向Environmental Sciences & Ecology ; Public, Environmental & Occupational Health
语种英语
WOS记录号WOS:000740229100008
资助机构National Natural Science Foundation of China ; Youth Innovation Promotion Association Program of the Chinese Academy of Sciences ; Special Foundation of Science and Technology Resources Survey ; Key project of Center for Ocean Mega-Science, Chinese Academy of Sciences ; Research Fund for the Taishan Scholar Project of Shandong Province of China
内容类型期刊论文
源URL[http://ir.yic.ac.cn/handle/133337/31327]  
专题海岸带生物学与生物资源利用重点实验室
通讯作者Hu, Xiaoke
作者单位1.Yantai Univ, Coll Life Sci, Yantai, Peoples R China
2.Chinese Acad Sci, Ctr Ocean Megasci, Qingdao, Peoples R China
3.Qingdao Natl Lab Marine Sci & Technol, Lab Marine Biol & Biotechnol, Qingdao, Peoples R China
4.Chinese Acad Sci, Yantai Inst Coastal Zone Res, Key Lab Coastal Biol & Bioresource Utilizat, Yantai 264003, Peoples R China
推荐引用方式
GB/T 7714
Min, Jun,Fang, Suyun,Peng, Jian,et al. Microbial detoxification of 2,4,6-tribromophenol via a novel process with consecutive oxidative and hydrolytic debromination: Biochemical, genetic and evolutionary characterization[J]. ENVIRONMENTAL RESEARCH,2022,205:10.
APA Min, Jun.,Fang, Suyun.,Peng, Jian.,Lv, Xin.,Xu, Lingxue.,...&Hu, Xiaoke.(2022).Microbial detoxification of 2,4,6-tribromophenol via a novel process with consecutive oxidative and hydrolytic debromination: Biochemical, genetic and evolutionary characterization.ENVIRONMENTAL RESEARCH,205,10.
MLA Min, Jun,et al."Microbial detoxification of 2,4,6-tribromophenol via a novel process with consecutive oxidative and hydrolytic debromination: Biochemical, genetic and evolutionary characterization".ENVIRONMENTAL RESEARCH 205(2022):10.
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