Marine bacteria-mediated abiotic-biotic coupling degradation mechanism of ibuprofen.
Marine bacteria-mediated abiotic-biotic coupling degradation mechanism of ibuprofen.
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海洋细菌介导的布洛芬非生物 - 生物耦合降解机制
DOI：
10.2139/ssrn.4034386
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发表时间：
2022-04
影响因子：
13.6
通讯作者：
Zelong Li;Jing Wang;C. Gu;Yali Guo;Shuo Wu
中科院分区：
文献类型：
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作者：
Zelong Li;Jing Wang;C. Gu;Yali Guo;Shuo Wu
关于药物和个人护理产品（PPCPs）在海洋无光环境中的行为和归宿的知识很少。本研究基于转录组和关键酶分析，研究了一种海洋泛生假交替单胞菌对典型PPCPs-布洛芬（IBP）的降解机制。更重要的是，首次发现了一种新的酶-非酶耦合降解机制，即IBP的降解首先由胞外活性氧（ROS）引发，然后中间产物（如4-乙基间苯二酚）被胞内酶进一步降解。结果表明，胞外非酶降解主要是生物源·OH、O2·-和H2 O2的作用，其中IBP通过氢化、异丁基裂解、氧化和脱羧等反应降解为4-乙基间苯二酚。4-羟苯丙酮酸双加氧酶、尿黑酸1，2-双加氧酶、长链酰基辅酶A合成酶、乙酰辅酶A酰基转移酶和烯酰辅酶A水合酶参与细胞内降解，导致4-乙基间苯二酚裂解并最终矿化。最终，这种新的降解机制被证明是氨基酸驱动，通过KEGG富集分析和实验数据。总之，本研究揭示了PPCPs生物转化过程中一种尚未被发现的非生物-生物耦合降解机制，从而更新了传统的污染物转化仅由酶或非酶完成的概念，也为PPCPs的环境行为和归宿提供了新的见解。
Knowledge on the behavior and fate of pharmaceuticals and personal care products (PPCPs) is poorly explored in marine aphotic environment. In this study, the degradation mechanism of a typical PPCPs-ibuprofen (IBP) by a ubiquitous marine Pseudoalteromonas sp. was investigated based on transcriptome and key enzymes analysis. More importantly, a novel enzymatic-nonenzymatic coupling degradation mechanism was uncovered for the first time, namely, the degradation of IBP was firstly initiated by extracellular reactive oxygen species (ROS), then the intermediate (e.g.4-ethylresorcinol) was further degraded by intracellular enzymes. It was showed that biogenic •OH, O2•-and H2O2 were responsible for extracellular nonenzymatic degradation, in which IBP was degraded to 4-ethylresorcinol through hydrogenation, isobutyl moiety cleavage, oxidation and decarboxylation. 4-Hydroxyphenylpyruvate dioxygenase, homogentisate 1,2-dioxygenase, long-chain acyl-CoA synthetase, acetyl-CoA acyltransferase and enoyl-CoA hydratase were identified to be involved in intracellular degradation, leading 4-ethylresorcinol cracked and eventually mineralized. Ultimately, this novel degradation mechanism was demonstrated to be amino acids-driven through KEGG enrichment analysis and experimental data. Overall, our work uncovered a yet undiscovered abiotic-biotic coupling degradation mechanism in PPCPs biotransformation, thereby updating the conventional concept that contaminants transformation is solely accomplished by enzymes or non-enzymes, which can also provide new insights into PPCPs environmental behavior and fate.