Advances in researches on migration and transformation behavior of per- and polyfluoroalkyl substances precursors in the environment
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摘要:
全氟及多氟烷基化合物（per- and polyfluoroalkyl substances，PFAS）前体物质是环境中许多PFAS的间接来源，广泛应用于食品包装、消防灭火泡沫、金属电镀、纺织涂料及农药等领域。由于PFAS前体物质能够在环境中发生转化以及分析测试方法的限制，其存在往往被忽视。PFAS前体物质自身的生物学毒性已被证实，如干扰母体内胎儿的正常发育、诱导免疫毒性和细胞凋亡等。深入探究PFAS前体物质在不同环境介质中的迁移转化规律是对其进行污染控制的关键。结合近年来国内外研究，对PFAS前体物质的主要来源、赋存特征及在大气、土壤和水体等环境介质中的迁移和转化行为研究进行了综述。结果表明，前体物质在全球范围内的水体、土壤、悬浮颗粒物、沉积物和大气中均有检出。在迁移过程中，水体是PFAS前体物质污染主要的载体，土壤、悬浮颗粒物和沉积物主要起滞留作用，而通过大气进行的长距离迁移是极端地区污染的重要来源。除此之外，PFAS前体物质在环境介质中的滞留和迁移往往伴随转化行为，生成更稳定的PFAS持续危害生态环境和生物健康。文章可以为PFAS前体物质及PFAS的污染防控提供参考和依据。
Abstract:Per- and polyfluoroalkyl substances (PFAS) precursors are indirect sources of many PFAS in the environment, widely utilized in various fields such as food packaging, firefighting foams, metal plating, textile coatings, and pesticides. Due to the transformation of PFAS precursors in the environment and limitations in analytical testing methods, PFAS precursors are often neglected. The biological toxicity of PFAS precursors has been confirmed, including their interference with normal fetal development, induction of immunotoxicity, and cell apoptosis in the mother's body. Moreover, PFAS precursors can transform into stable PFAS, posing sustained hazards to the ecological environment and biological health. Investigating the transport and transformation behavior of PFAS precursors in different environmental media is crucial to their contaminant control. Based on recent researches, this study provides a comprehensive review of the major sources and existence characteristics of PFAS precursors, as well as their transport and transformation behaviors in environmental media such as the atmosphere, soil, and water bodies. The results indicate that PFAS precursors have been widely detected in water bodies, soils, suspended particulate matter (SPM), sediments, and the atmosphere worldwide. During the transport process, water bodies are the main carriers of PFAS precursors, while soils, SPM, and sediments mainly play a role in retention. In addition, long-distance transport through the atmosphere is an important source of pollution in extreme areas. Furthermore, the retention and migration of PFAS precursors in environmental media often accompany transformation, resulting in producing PFAS that endangers the ecological environment and biological health continuously. This article reviews the research progress on the migration and transformation of PFAS precursors in the environment, aiming to provide the basis for the pollution prevention and control of PFAS precursors and PFAS.
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Key words:
- PFAS /
- precursor /
- existence /
- transport /
- transformation /
- environmental media
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表 1 本文出现的PFAS及其前体物质的名称及化学式
Table 1. Information related to PFASs and their precursors appearing in this study
中文名 缩写 英文全称 化学式 全氟丁酸 PFBA perfluorobutanoic acid C3F7COOH 全氟戊酸 PFPeA perfluoropentanoic acid C4F9COOH N-乙基全氟辛烷磺酰胺乙酸 N-EtFOSAA N-ethylperfluorooctane sulfonamidoacetic acid C12H8F17NO4S 全氟辛烷磺酸 PFOS perfluorooctane sulfonic acid C8F17SO3H 6∶2、8∶2氟二胺磺胺烷基甜菜碱 6∶2、8∶2 FTAB 6∶2、8∶2 fluorotelomer sulfonamide alkylbetaine C15H20F13N2SO4+、C17H20F17N2SO4+ 全氟辛烷磺酰胺 PFOSA perfluoroctylsulfonamide C8F17SO2NH2 6∶2、8∶2、10∶2氟调醇 6∶2、8∶2、10∶2 FTOH 6∶2、8∶2、10∶2 fluorotelomer alcohol C8H5F13O、C10H5F17O、C12H5F21O 4∶2、6∶2、8∶2、10∶2氟调磺酸 4∶2、6∶2、8∶2、10∶2 FTS 4∶2、6∶2、8∶2、10∶2 fluorotelomer sulfonate C4F9CH2CH2SO3−、C6F13CH2CH2SO3−、C8F17CH2CH2SO3−、C10F19CH2CH2SO3− N-乙基全氟辛烷磺酰胺 N-EtFOSA N-ethyl perfluorooctane sulfonamide C8F17SO2N（C2H5）H EtFOSA衍生磷酸二酯 di-SAmPAP EtFOSE-based phosphate diester 全氟辛烷磺酰氨基乙酸 FOSAA perfluorooctane sulfonamido acetic acid C8F17SO2NCH2COOH N-乙基全氟辛烷磺酰胺基乙醇 N-EtFOSE N-ethyl perfluorooctane sulfonamide ethanol C12H10F17NO3S 全氟己酸 PFHxA perfluorohexanoic acid C5F11COOH 8∶2氟调醛 8∶2 FTAL 8∶2 fluorotelomer aldehyde C10H5F17O2 8∶2氟调羧酸 8∶2 FTCA 8∶2 fluorotelomer carboxylic acid C10H3F17O2 8∶2氟调不饱和羧酸 8∶2 FTUCA 8∶2 fluorotelomer unsaturated carboxylic acid C10H2F17O2 全氟壬酸 PFNA per-fluorononanoic acid C9F17COOH 全氟烷基磺酰胺衍生物 6∶2、8∶2 diPAP 6∶2、8∶2 polyfluoroalkyl phosphoric acid diester C16F26H9PO4、C18F30H9PO4 N-甲基全氟辛烷磺酰胺乙酸 N-MeFOSAA N-ethylperfluorooctane sulfonamidoacetic acid C12H8F17NO4S 全氟辛酸 PFOA perfluorooctanoic acid C8F15COOH 全氟癸酸 PFUnDA perfluoroundecanoic acid C11F21COOH 全氟庚酸 PFHpA perfluoroheptanoic acid C6F13COOH 全氟-1-丁磺酰胺 FBSA perfluoro-1-butanesulfonamide C4H2F9NO2S 
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表 2 国内外文献报道中PFAS前体物质的检出情况
Table 2. Detection of PFAS precursors reported in the previous studies
环境介质 采样位置 采样时间 样品个数 分析方法 数据意义 单位 检出前体物质种类和浓度 参考文献 水
体地
表
水①渤海海湾（LZB）
②河流入海口2012年4、8和12月 ①LZB： 29
②河流入海口： 7总可氧化前体物质（TOP）、液相色谱质谱联用仪（LC-MS/MS） 浓度范围 ng/L ∆ΣPFCA：
①LZB：3.89～18.1
②河流入海口：10.7～36.7文献[13] 中国天津大港油田地表水 51 TOP、高效液相色谱质谱联用仪（HPLC-MS/MS） 浓度范围 ng/L 未知∆ΣPFCA：0.25～3.47 文献[14] 中国沿海旅游胜地地表水 2021年4、8和12月 20 TOP、HPLC-MS/MS 浓度范围 ng/L ①PFOSA：0.140～1.15
②∆ΣPFCAC4～C12：1.51～40.4文献[15] 中国太湖 2015年6月 28 超高效液相色谱质谱联用仪（UPLC-MS/MS） 平均浓度 ng/L ①PFOSA：0.19
②6∶2 diPAP：0.034
③N-EtFOSAA：0.026文献[16] 中国东部城市地表水（浙江、上海和江苏） 2011年 ①河流： 29
②湖泊： 6
③水库： 4HPLC-MS/MS 浓度范围 ng/L ①浙江：<LOD～0.20
②上海：0.13～2.5
③江苏：0.18～0.25文献[17] 波罗的海水样 2013—2014年 4 UPLC-MS/MS 平均浓度 ng/L ①PFOSA：0.06
②MeFOSAA：0.0017
③EtFOSAA：0.0044文献[18] 孟加拉国达卡地表水 2021年 8 LC-MS/MS 浓度范围 ng/L 4∶2、6∶2和8∶2 FTS总浓度：1～5 文献[19] 美国马萨诸塞州科德角沿海海域 2017年8月—2019年7月 ①受AFFF污染：41②未污染：13 TOP、LC-MS/MS 平均浓度 ng/L 受污染/未受污染：
①4∶2 FTS：5.77/3.50
②6∶2 FTS：15.6/1.02
③8∶2 FTS：8.7/0.75
④ΣPFAS前体物质：157/14.5文献[21] 地
下
水美国5个军事基地地下LNAPL 17 ①LC-MS
②气相色谱-质谱联用仪（GC-MS）浓度范围 ng/L ①PFOSA：<LOD～2500
②6∶2 FTS：<LOD～6040
③8∶2 FTS：<LOD～712
④10∶2 FTS：<LOD～141
⑤6∶2 FTOH：<LOD～15000文献[20] 美国马萨诸塞州科德角地下水 2018年9月 13 LC-MS/MS 平均浓度 ng/L ①6∶2 FTS：346.61
②8∶2 FTS：268.67
③PFOSA：32.11文献[22] 中国黄土高原地下水 2019年8月 泉水：22
井水：1TOP、LC-MS/MS 平均浓度 ng/L ①4∶2 FTS：0.38
②6∶2 FTS：2.0
③8∶2 FTS：1.1文献[23] 悬浮颗粒物 德国和荷兰 2021年 ①SPM：116
②沉积物：60TOP、超高效液相色谱-高分辨率质谱仪（UHPLC-HRMS） 最高浓度 ng/g ①6∶2 diPAP：25.377
②8∶2 diPAP：19.944
③FOSAA：2.259
④6∶2 FTS：5.983
⑤8∶2 FTS：0.865
⑥PFOSA：2.259
⑦MeFOSAA：0.995
⑧EtFOSAA：8.896文献[28] 土壤 德国环境样本库 2002—2018年 11 TOP、LC-MS/MS 中位数、
最高浓度ng/g TOP后∆ΣPFAS中位数最多升高72%、最高浓度：0.51 文献[29] 沉积物 黄海、东海 2019年8月 68 UPLC-MS/MS 浓度范围 ng/g ①4∶2 FTS：0.004～0.103
②FBSA：0.001～0.010
③PFOSA：0.002～0.012文献[25] 托多斯桑托斯湾 ①SPM：3
②沉积物：4UPLC-MS/MS 最高浓度 ng/g ①EtFOSAA：0.59
②PFOSA：0.46文献[26] 温哥华福溪 2011年8月3日 11 HPLC-MS/MS 平均浓度 pg/g ①PFOSA：59
②FOSAA：39
③MeFOSAA：240
④EtFOSAA：590
⑤SAmPAP diester：200文献[27] 法国 2018年9—11月 43 TOP、LC-MS/MS 最高浓度 ng/g ∆ΣPFAS：98.5 文献[30] 大气 室内
空气中国香港废物管理设施内或周边 2020年11月—2021年1月 4 气相色谱-质谱/质谱联用技术（GC-MS/MS） 最高浓度 pg/m3 空气/颗粒物：
①6∶2 diPAP：3.39/2.71
②8∶2 diPAP：2.72/—
③6∶2 FTOH：1240/59.5
④8∶2 FTOH：309/21.9
⑤10∶2 FTOH：173/335
⑥N-MeFOSA：18.1/—
⑦N-EtFOSA：40.2/3.0
⑧N-MeFHxSA：4.08/—
⑨N-EtFHxSA：4.16/15.2
⑩N-MeFOSE：3.08/—
⑪N-EtFOSE：5.56/—
⑫N-MeFBSA：352/44.6文献[33] 加州北部幼儿园教室、住宅、户外服装店等 2018—2020年 36 GC-MS 最高浓度 ng/m3 空气：
①6∶2 FTOH：1910
②8∶2 FTOH：270
③10∶2 FTOH：33
④MeFOSA：12
⑤MeFOSE：32
⑥EtFOSE：14.7
⑦ΣPFAS前体物质：2220文献[34] 马萨诸塞州消防站 2018年 39 LC-MS/MS 平均浓度 ng/g 颗粒物：
①4∶2 FTS：1.06
②6∶2 FTS：11.9
③8∶2 FTS：7.55
④PFOSA：0.569
⑤N-MeFOSAA：0.777文献[37] 室外
大气新奥勒松 2011年9月—2012年9月 45 GC-MS 最高浓度 pg/m3 空气：
①6∶2 FTOH：5.1
②8∶2 FTOH：25
③10∶2 FTOH：9.3
④12:2 FTOH：3.3
⑤MeFOSA：0.5
⑥EtFOSA：0.5
⑦MeFBSA：1.8
⑧MeFOSE：0.8
⑨EtFOSE：0.4
⑩MeFOSE：0.2文献[35] 北京西城区 2014年10月 7 HPLC-MS/MS 最高浓度 pg/m3 颗粒物：
①PFOSA：0.2
②N-EtFOSA：0.6文献[36] 注：LOD表示Limit of detection，检出限；—表示未检出。
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