State Key Laboratory of Microbial Metabolism, Joint International Research Laboratory of Metabolic and Developmental Sciences, and School of Life Sciences and Biotechnology, Shanghai Jiao Tong University, 200240 Shanghai, China.
State Key Laboratory of Microbial Metabolism, Joint International Research Laboratory of Metabolic and Developmental Sciences, and School of Life Sciences and Biotechnology, Shanghai Jiao Tong University, 200240 Shanghai, China.
J Hazard Mater. 2024 Oct 5;478:135511. doi: 10.1016/j.jhazmat.2024.135511. Epub 2024 Aug 13.
Triclosan (TCS), an antimicrobial agent extensively incorporated into pharmaceuticals and personal care products, poses significant environmental risks because of its persistence and ecotoxicity. So far, a few microorganisms were suggested to degrade TCS, but the microbial degradation mechanism remains elusive. Here, a two-component angular dioxygenase (TcsAaAb) responsible for the initial TCS degradation was characterized in Sphingomonas sp. strain YL-JM2C. Whole-cell biotransformation and crude enzyme assays demonstrated that TcsAaAb catalyzed the conversion of TCS to 4-chlorocatechol and 3,5-dichlorocatechol rather than the commonly suggested product 2,4-dichlorophenol. Then two intermediates were catabolized by tcsCDEF cluster via an ortho-cleavage pathway. Critical residues (N262, F279, and F391) for substrate binding were identified via molecular docking and mutagenesis. Further, TcsAaAb showed activity toward methyl triclosan and nitrofen, suggesting its versatile potential for bioremediation. In addition, TCS-degrading genes were also present in diverse bacterial genomes in wastewater, ocean and soil, and a relatively high gene abundance was observed in marine metagenomes, revealing the transformation fate of TCS in environments and the microbial potential in pollutant removal. These findings extend the understanding of the microbe-mediated TCS degradation and contribute to the mining of TCS-degrading strains and enzymes, as well as their application in the bioremediation of contaminated environments.
三氯生(TCS)作为一种广泛应用于医药和个人护理产品的抗菌剂,由于其持久性和生态毒性而带来了重大的环境风险。到目前为止,已经有一些微生物被认为可以降解 TCS,但微生物降解机制仍不清楚。在这里,我们在一株鞘氨醇单胞菌(Sphingomonas sp. strain YL-JM2C)中鉴定出了一种负责 TCS 初始降解的双组分角加氧酶(TcsAaAb)。全细胞生物转化和粗酶分析表明,TcsAaAb 催化 TCS 转化为 4-氯儿茶酚和 3,5-二氯儿茶酚,而不是通常认为的产物 2,4-二氯苯酚。然后,两个中间产物通过 tcsCDEF 簇通过邻位裂解途径进行代谢。通过分子对接和突变分析鉴定出关键残基(N262、F279 和 F391)参与底物结合。此外,TcsAaAb 对甲基三氯生和硝基酚也表现出活性,表明其在生物修复方面具有广泛的应用潜力。此外,TCS 降解基因也存在于废水、海洋和土壤中的多种细菌基因组中,并且在海洋宏基因组中观察到相对较高的基因丰度,这揭示了 TCS 在环境中的转化命运以及微生物在污染物去除方面的潜力。这些发现扩展了对微生物介导的 TCS 降解的理解,并有助于 TCS 降解菌株和酶的挖掘及其在污染环境的生物修复中的应用。