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全氟辛烷磺酸(PFOS)前体在截然不同的土壤中的好氧生物转化途径的动力学分析

Kinetic analysis of aerobic biotransformation pathways of a perfluorooctane sulfonate (PFOS) precursor in distinctly different soils.

作者信息

Zhang Lilan, Lee Linda S, Niu Junfeng, Liu Jinxia

机构信息

State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, PR China; State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, PR China.

Purdue University, Department of Agronomy, Ecological Science and Engineering, West Lafayette, IN 47907-2054, United States.

出版信息

Environ Pollut. 2017 Oct;229:159-167. doi: 10.1016/j.envpol.2017.05.074. Epub 2017 Jun 5.

Abstract

With the phaseout of perfluorooctane sulfonate (PFOS) production in most countries and its well known recalcitrance, there is a need to quantify the potential release of PFOS from precursors previously or currently being emitted into the environment. Aerobic biodegradation of N-ethyl perfluorooctane sulfonamidoethanol (EtFOSE) was monitored in two soils from Indiana, USA: an acidic forest silt loam (FRST-48, pH = 5.5) and a high pH agricultural loam (PSF-49, pH = 7.8) with similar organic carbon contents (2.4 and 2.6%) for 210 d and 180 d, respectively. At designated times, triplicate samples were sacrificed for which headspace samples were taken followed by three sequential extractions. Extracts were analyzed using HPLC-tandem mass spectrometry. Measured profiles of EtFOSE degradation and generation/degradation of subsequent metabolites were fitted to the Indiana soils data as well as to a previously published data set for a Canadian soil using an R-based model (KinGUII) to explore pathways and estimate half-lives (t) for EtFOSE and metabolites. EtFOSE degradation ranged from a few days to up to a month. PFOS yields ranged form 1.06-5.49 mol% with the alkaline soils being four to five times higher than the acidic soil. In addition, a direct pathway to PFOS had to be invoked to describe the early generation of PFOS in the Canadian soil. Of all metabolites, the sulfonamidoacetic acids were the most persistent (t ≥ 3 months) in all soils. We hypothesized that while pH-pK dependent speciation may have impacted rates, differences in microbial communities between the 3 soils arising from varied soil properties including pH, nutrient levels, soil management, and climatic regions are likely the major factors affecting pathways, rates, and PFOS yields.

摘要

随着大多数国家全氟辛烷磺酸(PFOS)生产的逐步淘汰及其众所周知的难降解性,有必要对以前或目前排放到环境中的前体物质中PFOS的潜在释放量进行量化。在美国印第安纳州的两种土壤中监测了N-乙基全氟辛烷磺酰胺乙醇(EtFOSE)的好氧生物降解:一种酸性森林粉质壤土(FRST-48,pH = 5.5)和一种高pH值的农业壤土(PSF-49,pH = 7.8),它们的有机碳含量相似(分别为2.4%和2.6%),监测时间分别为210天和180天。在指定时间,牺牲三份重复样品,采集顶空样品,然后进行三次连续萃取。提取物使用高效液相色谱-串联质谱法进行分析。使用基于R的模型(KinGUII)将EtFOSE降解以及后续代谢物的生成/降解的测量曲线拟合到印第安纳州土壤数据以及先前发表的加拿大土壤数据集,以探索途径并估计EtFOSE和代谢物的半衰期(t)。EtFOSE的降解时间从几天到长达一个月不等。PFOS的产量范围为1.06 - 5.49 mol%,碱性土壤中的产量比酸性土壤高四到五倍。此外,必须引入一条直接生成PFOS的途径来描述加拿大土壤中PFOS的早期生成。在所有代谢物中,磺基氨基乙酸在所有土壤中最持久(t≥3个月)。我们假设,虽然pH - pK依赖的形态可能影响了速率,但三种土壤之间由于土壤性质(包括pH值、养分水平、土壤管理和气候区域)不同而产生的微生物群落差异可能是影响途径、速率和PFOS产量的主要因素。

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