Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, PR China.
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, PR China.
Sci Total Environ. 2024 Nov 25;953:176039. doi: 10.1016/j.scitotenv.2024.176039. Epub 2024 Sep 4.
Domoic acid (DA) is a compound generated as a secondary metabolite during harmful algal blooms, has historically received attention as the potent neurotoxicity in marine environment. However, the aerobic degradation mechanism of DA and the DA-degrader remain largely unknown. Here, we revealed the mechanism of aerobic degradation of DA by a ubiquitous marine Pseudoalteromonas sp., and more importantly, we confirmed that the degradation of DA is mediated by biogenic reactive oxygen species (ROS), rather than direct enzyme-mediated as traditionally conceived. Results indicated that DA degradation was caused by biogenic O and OH, where DA underwent reactions of decarboxylation, hydroxylation, and oxidation to yield the detoxification terminal product. Besides, whole genome sequencing and RT-qPCR analysis revealed that the genes conferring to encoding leucine dehydrogenase (ldh) and Na+-translocated NADH-quinone oxidoreductase (nqrA, nqrF) are responsible for biogenic ROS production. Finally, we found through comparative proteomic analysis that biogenic ROS mediated the DA degradation may be prevalent in the environment. Overall, this work not only reveals aerobic biotransformation mechanism of DA, but also identifies a novel mechanism of DA degradation, which provides new perspective into the environmental fate of DA and the artificial bioremediation of DA.
脱羧酸(DA)是一种在有害藻类大量繁殖时作为次生代谢物产生的化合物,在历史上因其在海洋环境中的强烈神经毒性而受到关注。然而,DA 的好氧降解机制和 DA 降解菌在很大程度上仍不清楚。在这里,我们揭示了一种普遍存在的海洋假交替单胞菌(Pseudoalteromonas sp.)对 DA 的好氧降解机制,更重要的是,我们证实了 DA 的降解是由生物产生的活性氧(ROS)介导的,而不是传统上认为的直接酶介导。结果表明,DA 的降解是由生物产生的 O 和 OH 引起的,其中 DA 经历了脱羧、羟化和氧化反应,生成解毒的终产物。此外,全基因组测序和 RT-qPCR 分析表明,编码亮氨酸脱氢酶(ldh)和 Na+-转运 NADH-醌氧化还原酶(nqrA、nqrF)的基因负责生物 ROS 的产生。最后,通过比较蛋白质组学分析发现,生物 ROS 介导的 DA 降解可能在环境中普遍存在。总的来说,这项工作不仅揭示了 DA 的好氧生物转化机制,还确定了一种 DA 降解的新机制,为 DA 的环境归宿和 DA 的人工生物修复提供了新的视角。