Biotransformation of 6:2/4:2 fluorotelomer alcohols by Dietzia aurantiaca J3: Enzymes and proteomics.

Journal of hazardous materials Pub Date : 2024-10-05 Epub Date: 2024-08-13 DOI:10.1016/j.jhazmat.2024.135510
Shefali Bhardwaj, Matthew Lee, Denis O'Carroll, James McDonald, Keith Osborne, Stuart Khan, Russell Pickford, Nicholas Coleman, Casey O'Farrell, Sarah Richards, Michael J Manefield
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Abstract

Per- and polyfluoroalkyl substances (PFAS) are recalcitrant synthetic organohalides known to negatively impact human health. Short-chain fluorotelomer alcohols are considered the precursor of various perfluorocarboxylic acids (PFCAs) in the environment. Their ongoing production and widespread detection motivate investigations of their biological transformation. Dietzia aurantiaca strain J3 was isolated from PFAS-contaminated landfill leachate using 6:2 fluorotelomer sulphonate (6:2 FTS) as a sulphur source. Resting cell experiments were used to test if strain J3 could transform fluorotelomer alcohols (6:2 and 4:2 FTOH). Strain J3 transformed fluorotelomer alcohols into PFCAs, polyfluorocarboxylic acids and transient intermediates. Over 6 days, 80 % and 58 % of 6:2 FTOH (0.1 mM) and 4:2 FTOH (0.12 mM) were degraded with 6.4 % and 14 % fluoride recovery respectively. Fluorotelomer unsaturated carboxylic acid (6:2 FTUCA) was the most abundant metabolite, accounting for 21 to 30 mol% of 6:2 FTOH (0.015 mM) applied on day zero. Glutathione (GSH) conjugates of 6:2/4:2 FTOH and 5:3 FTCA adducts were also structurally identified. Proteomics studies conducted to identify enzymes in the biotransformation pathway have revealed the role of various enzymes involved in β oxidation. This is the first report of 6:2/4:2 FTOH glutathione conjugates and 5:3 FTCA adducts in prokaryotes, and the first study to explore the biotransformation of 4:2 FTOH by pure bacterial strain.

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Dietzia aurantiaca J3 对 6:2/4:2 氟代醇的生物转化:酶和蛋白质组学。
全氟烷基和多氟烷基物质(PFAS)是一种难降解的合成有机卤化物,已知会对人类健康产生负面影响。短链氟代醇被认为是环境中各种全氟羧酸(PFCAs)的前体。它们的持续生产和广泛检测促使人们对其生物转化进行研究。以 6:2 氟代苯磺酸酯(6:2 FTS)为硫源,从受 PFAS 污染的垃圾填埋场渗滤液中分离出 Dietzia aurantiaca 菌株 J3。静止细胞实验用于检测菌株 J3 能否转化氟代醇(6:2 和 4:2 FTOH)。菌株 J3 将氟代醇转化为全氟羧酸、多氟羧酸和瞬时中间产物。6 天内,6:2 FTOH(0.1 mM)和 4:2 FTOH(0.12 mM)分别降解了 80% 和 58%,氟回收率分别为 6.4% 和 14%。氟代不饱和羧酸(6:2 FTUCA)是最丰富的代谢物,占第零天施用的 6:2 FTOH(0.015 mM)的 21 至 30 摩尔%。还从结构上确定了 6:2/4:2 FTOH 和 5:3 FTCA 加合物的谷胱甘肽(GSH)共轭物。为确定生物转化途径中的酶而进行的蛋白质组学研究揭示了参与 β 氧化的各种酶的作用。这是首次报道原核生物中的 6:2/4:2 FTOH 谷胱甘肽共轭物和 5:3 FTCA 加合物,也是首次探讨纯细菌菌株对 4:2 FTOH 的生物转化的研究。
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