土壤中全氟化合物的生物可利用性研究
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摘要
全氟化合物(perfluoroalkyl substances, PFASs)因其独特的疏水和疏油特性而被广泛应用于工业和日常生活产品中,如表面活性剂、制冷剂、润滑剂、涂料、泡沫灭火剂和化妆品等。含有PFASs及其前体化合物的产品在生产、应用、运输和处置过程中会释放到环境介质大气、水、土壤和沉积物中。PFASs具有较强的蛋白质结合能力,能在发生生物富集和生物放大效应,从而对生物和人体健康等产生不利影响。因此,近年来关于PFASs在生物体内的富集研究一直是环境科学研究领域的热点问题。
以蚯蚓(Eisenia fetida)为受试生物,通过10个PFASs(7个全氟羧酸(PFCAs)和3个全氟磺酸(PFSAs))在人工染毒土壤中的富集与清除实验,研究土壤中PFASs的生物可利用性。所有测试PFASs都可以被蚯蚓吸收。PFASs在蚯蚓体内的富集与清除动力常数与全氟碳链的长度密切相关。蚯蚓对PFASs的吸收速率常数(ku)为0.016(全氟己酸,PFHxA)～0.102d-1(全氟十二酸,PFDoA)和0.003(全氟丁烷磺酸,PFBS)～0.030d-1(全氟己烷磺酸,PFOS)。清除速率常数(ku)为0.030(PFDoA)～0.187(PFHxA) d-1和0.039(PFOS)～0.072d-1(PFBS)。长碳链的PFASs显示出较高的吸收速率常数(ku),较高的半衰期(t1/2),达到吸收平衡所需要的时间(tss)也较长,但是其清除速率常数(ke)却较低。并且,全氟磺酸(PFSAs)的ku,t1/2,和tss值要比相同全氟碳链长度的全氟羧酸(PFCAs)的高,而ke值却较低。说明蚯蚓更易于吸收长碳链的PFASs,同等全氟碳链长度时,更易于吸收PFSAs,清除规律则恰好相反,即短碳链的PFASs更易于从蚯蚓体内排除,相同全氟碳链长度的PFASs, PFCAs比PFSAs更易清除。蚯蚓能从染毒土壤中高效富集PFASs,即使是全氟碳链长度小于等于7的PFHxA、全氟庚酸(PFHpA)、全氟辛酸(PFOA)、PFBS和全氟己烷磺酸(PFHxS)等,均有很好的生物富集效应。PFASs在蚯蚓从土壤中的富集因子(BSAFs)与全氟碳链长度呈现显著的正线性相关性。并且,相同全氟碳链长度的PFSAs比PFCAs具有更高的BSAFs,说明蚯蚓更容易从土壤中富集长碳链的PFASs,相较于PFCAs也更易于富集PFSAs。蚯蚓从土壤中富集PFASs的BSAFs具有浓度依赖性,BSAFs随着土壤中暴露浓度的增加而降低。
以小麦(Triticum aestivum)为受试生物,通过温室培养盆栽实验研究了11个PFASs(8个PFCAs和3个PFSAs)在小麦中的吸收累积。PFASs能被小麦根从土壤中吸收富集,并且发生根部向茎叶部分的迁移。PFASs在小麦根中的富集因子(RCFs)以及在整个小麦中的富集因子(BCF)均随着全氟碳链长度增加而降低,呈现负线性相关性,并且RCFs随土壤—水分配系数(Koc)的增加而降低。PFASs在小麦中从根到茎叶的传输因子(TFs)以PFHxA为界限,先增加后再指数降低。在三个PFSAs中,PFHxS显示最高的TF。小麦从土壤中富集PFASs的趋势与蚯蚓从土壤中富集PFASs'恰好相反,而PFHpA在植物体内的BCFs与在蚯蚓体内的BSAF非常相似。以PFHpA为界限,当全氟碳链长度≥7时,PFASs在蚯蚓体内的BSAFs值大于在植物体内的BCFs,而当全氟碳链长度<7时,蚯蚓的富集因子(BSAFs)小于植物的富集因子(BCFs). PFASs在植物体内的富集受其在土壤—土壤孔隙水中的分配能力、穿透植物表皮的能力及其水溶解度和疏水性的影响。
通过实验室盆栽培养实验,模拟动物—植物联合生境,研究蚯蚓与小麦共存时对PFASs的生物富集的相互影响。当蚯蚓与小麦联合时,蚯蚓对所有供试PFASs的富集能力都显著增强,而小麦对PFASs富集变化表现为,短碳链(≤7) PFCAs的富集能力提高,而长碳链(>7) PFCAs以及PFSAs的富集能力均减弱。但是,总体来说,蚯蚓与小麦共存时土壤中PFASs总的生物可利用性都有所提高。
通过对蚯蚓在N-乙基全氟辛基磺酰胺基乙醇(N-EtFOSE)与氟调醇(FTOHs,8:2FTOH(2-全氟辛基乙醇),10:2FTOH(2-全氟癸基乙醇))染毒土壤中暴露实验,研究了PFASs前体物质在蚯蚓体内的富集及清除动力学,以及可能发生的生物转化,并且测定了降解产物。N-EtFOSE与FTOHs及其代谢产物在蚯蚓体内富集效果显著,并且能够发生生物转化和降解。N-EtFOSE在土壤—蚯蚓系统能够降解成其它中间代谢产物,如N-EtFOSE^N-乙基全氟辛基磺酰胺乙酸(N-EtFOSAA,52.4%)→全氟磺酰胺乙酸(FOSAA,2.0%)→全氟辛基磺酰胺(FOSA,22.4%),并最终降解成稳定的PFOS (23.3%),主要代谢产物为N-EtFOSAA。8:2FTOH在土壤—蚯蚓系统主要的最终代谢产物为全氟辛酸(PFOA),10:2FTOH在土壤—蚯蚓系统主要的最终代谢产物为全氟癸酸(PFDA)。研究结果说明全氟前体物质的降解是环境中的PFSAs和PFCAs一个重要来源。
Perfluoroalkyl substances (PFASs) are a group of synthetic compounds which have been widely applied in a variety of commercial and industrial products, such as surfactants, refrigerants, lubricants, paints, fire fighting foams, cosmetics and so on. PFASs have unique water and oil repelling characteristics due to the hydrophobic fluorinated carbon chain and hydrophilic sulfonate or carboxylate end groups. PFASs are released into the environment during the production, application, transport and disposal of PFAS containing products or by degradation of their precursors, and they are ubiquitous in environmental matrices such as air, water, soil and sewage sludge. PFASs can be bioaccumulated and biomagnified throughout the food chain due to their strong binding potential to proteins and may have dverse effects to individual organisms, food webs and human health. The bioaccumulation of PFASs has become a major concern of the international community.
Earthworms were exposed to artificially contaminated soils with ten PFASs to investigate the bioaccumulation and bioavailabiliry of PFASs. All the test PFASs in soil are bioaccumulative to earthworms. The uptake rate coefficients () of PFASs in the range of0.016(perfluorohexanoate, PFHxA)-0.102d-1(perfluorododecanoate, PFDoA) for PFCAs and0.003(perfluorobutane sulfonate, PFBS)-0.030d-1(perfluorooctane sulfonate, PFOS) for PFSAs. The elimination rate coefficients (ke) of PFASs in the range of0.030(PFDoA)-0.187d-1(PFHxA) for PFCAs and0.039(PFOS)-0.072d'1(PFBS) for PFSAs. PFASs with longer perfluorinated carbon chain displayed higher uptake rate coefficients (ku), longer half-life (t1/2) and time to steady-state (tss) but lower elimination rate coefficients (ke) than the shorter ones. Similarly, perfiorosulfonates acids (PFSAs) displayed higher ku, longer t1/2and tss but lower ke than perflurocarboxylic acids (PFCAs) with the same perfluorinated chain length. The results indicate that the uptake of PFASs in the earthworms becomes much easier while the elimination becomes more difficult as the perfluorinated chain length increases and PFCAs are much easier to eliminate from earthworm than PFCAs of equivalent perfluorinated chain length. All the studied PFASs, including those with seven or less perfluorinated carbons, such as PFHxA, perfluoroheptanoate (PFHpA), perfluorooctanoate (PFOA), PFBS and perfluorohexane sulfonate (PFHxS), were bioaccumulated in the earthworms and the biota-to-soil accumulation factors (BSAFs) increased with perfluorinated carbon chain length and were greater for PFSAs than for PFCAs of equal perfluoroalkyl chain length. The BSAFs were found to be dependent on the concentrations of PFASs in soil and decreased as the level of PFASs in soil increased.
Wheats were exposed to soils contaminated with11PFASs. Wheat could uptake PFASs from soil by wheat root and translocated to wheat shoot with root concentration factors and bioconcentration factors that decreased as the number of perfluorinated carbons in the molecule increased. And the RCFs of PFASs decreased with the distribution coefficient values between soil and interstitial water (Koc) increased. Translocation factors (TF) of PFCAs in wheat peaked at PFHxA and decreased significantly as the number of carbons increased or decreased. PFHxS produced the greatest TF of the threePFSAs examined. Since PFASs displayed opposite accumulation potentials in earthworms compared to wheat, the accumulation factors of PFASs in earthworms and wheat crossed at around PFHpA, which displayed similar BSAFs in earthworms and BCF in wheat. When the number of perfluorinated carbon is>7, the BSAFs of PFASs in earthworms were larger than their BCFs in plants, while the BSAFs in earthworms were lower than plant BCFs if the number of perfluorinated carbons was<7. The bioaccumulation of PFASs in plant was dependent on the distribution coefficients between soil and interstitial water, ability to cross plant membranes and their water solubility and hydrophobicity.
Wheats and earthworms were exposed together to soils contaminated with11PFASs to investigate the mutual impacts of wheat and earthworm on their bioaccumulation of PFASs from soil. Wheat increased the bioaccumulation of all11PFASs in earthworms and earthworms increased the bioaccumulation in wheat of PFCAs containing seven or less perfluorinated carbons, decreased bioaccumulation of PFCAs with more than seven carbons, and decreased bioaccumulation of PFSAs. In general, the co-presence of wheat and earthworms enhanced the bioavailability of PFASs in soil. When earthworms and wheat are both present in soil, they may affect the accumulation of PFASs within each other by competition or by changing the bioavailability of the contaminants.
The bioaccumulation and metabolism of N-ethyl perfluorooctane sulfonamidoethanol (N-EtFOSE) and two fluorotelomer alcohols (FTOH, perfluorooctylethanol,(8:2FTOH), perfluorodecylethanol,(10:2FTOH)) in earthworm from soil were investigated. N-EtFOSE in earthworm could be degraded to PFOS via some stable intermediate metabolites, N-EtFOSE->N-ethylperfluorooctane sulfonamide acetate (N-EtFOSAA,52.4%)→perfluorooctane sulfonamide acetate (FOSAA,2.0%)→perfluorooctane sulfonamide (FOSA,22.4%)→PFOS (23.3%). N-EtFOAA was the major metabolite and PFOS was the terminal product of N-EtFOSE. PFOA was the major terminal metabolitesof8:2FTOH and perfluorodecanoate (PFDA) was the major terminal metabolite of10:2FTOH. The results suggested that the biotic degradation of PFAS precursors is an important source of PFCAs and PFSAs in the environment.
以蚯蚓(Eisenia fetida)为受试生物,通过10个PFASs(7个全氟羧酸(PFCAs)和3个全氟磺酸(PFSAs))在人工染毒土壤中的富集与清除实验,研究土壤中PFASs的生物可利用性。所有测试PFASs都可以被蚯蚓吸收。PFASs在蚯蚓体内的富集与清除动力常数与全氟碳链的长度密切相关。蚯蚓对PFASs的吸收速率常数(ku)为0.016(全氟己酸,PFHxA)～0.102d-1(全氟十二酸,PFDoA)和0.003(全氟丁烷磺酸,PFBS)～0.030d-1(全氟己烷磺酸,PFOS)。清除速率常数(ku)为0.030(PFDoA)～0.187(PFHxA) d-1和0.039(PFOS)～0.072d-1(PFBS)。长碳链的PFASs显示出较高的吸收速率常数(ku),较高的半衰期(t1/2),达到吸收平衡所需要的时间(tss)也较长,但是其清除速率常数(ke)却较低。并且,全氟磺酸(PFSAs)的ku,t1/2,和tss值要比相同全氟碳链长度的全氟羧酸(PFCAs)的高,而ke值却较低。说明蚯蚓更易于吸收长碳链的PFASs,同等全氟碳链长度时,更易于吸收PFSAs,清除规律则恰好相反,即短碳链的PFASs更易于从蚯蚓体内排除,相同全氟碳链长度的PFASs, PFCAs比PFSAs更易清除。蚯蚓能从染毒土壤中高效富集PFASs,即使是全氟碳链长度小于等于7的PFHxA、全氟庚酸(PFHpA)、全氟辛酸(PFOA)、PFBS和全氟己烷磺酸(PFHxS)等,均有很好的生物富集效应。PFASs在蚯蚓从土壤中的富集因子(BSAFs)与全氟碳链长度呈现显著的正线性相关性。并且,相同全氟碳链长度的PFSAs比PFCAs具有更高的BSAFs,说明蚯蚓更容易从土壤中富集长碳链的PFASs,相较于PFCAs也更易于富集PFSAs。蚯蚓从土壤中富集PFASs的BSAFs具有浓度依赖性,BSAFs随着土壤中暴露浓度的增加而降低。
以小麦(Triticum aestivum)为受试生物,通过温室培养盆栽实验研究了11个PFASs(8个PFCAs和3个PFSAs)在小麦中的吸收累积。PFASs能被小麦根从土壤中吸收富集,并且发生根部向茎叶部分的迁移。PFASs在小麦根中的富集因子(RCFs)以及在整个小麦中的富集因子(BCF)均随着全氟碳链长度增加而降低,呈现负线性相关性,并且RCFs随土壤—水分配系数(Koc)的增加而降低。PFASs在小麦中从根到茎叶的传输因子(TFs)以PFHxA为界限,先增加后再指数降低。在三个PFSAs中,PFHxS显示最高的TF。小麦从土壤中富集PFASs的趋势与蚯蚓从土壤中富集PFASs'恰好相反,而PFHpA在植物体内的BCFs与在蚯蚓体内的BSAF非常相似。以PFHpA为界限,当全氟碳链长度≥7时,PFASs在蚯蚓体内的BSAFs值大于在植物体内的BCFs,而当全氟碳链长度<7时,蚯蚓的富集因子(BSAFs)小于植物的富集因子(BCFs). PFASs在植物体内的富集受其在土壤—土壤孔隙水中的分配能力、穿透植物表皮的能力及其水溶解度和疏水性的影响。
通过实验室盆栽培养实验,模拟动物—植物联合生境,研究蚯蚓与小麦共存时对PFASs的生物富集的相互影响。当蚯蚓与小麦联合时,蚯蚓对所有供试PFASs的富集能力都显著增强,而小麦对PFASs富集变化表现为,短碳链(≤7) PFCAs的富集能力提高,而长碳链(>7) PFCAs以及PFSAs的富集能力均减弱。但是,总体来说,蚯蚓与小麦共存时土壤中PFASs总的生物可利用性都有所提高。
通过对蚯蚓在N-乙基全氟辛基磺酰胺基乙醇(N-EtFOSE)与氟调醇(FTOHs,8:2FTOH(2-全氟辛基乙醇),10:2FTOH(2-全氟癸基乙醇))染毒土壤中暴露实验,研究了PFASs前体物质在蚯蚓体内的富集及清除动力学,以及可能发生的生物转化,并且测定了降解产物。N-EtFOSE与FTOHs及其代谢产物在蚯蚓体内富集效果显著,并且能够发生生物转化和降解。N-EtFOSE在土壤—蚯蚓系统能够降解成其它中间代谢产物,如N-EtFOSE^N-乙基全氟辛基磺酰胺乙酸(N-EtFOSAA,52.4%)→全氟磺酰胺乙酸(FOSAA,2.0%)→全氟辛基磺酰胺(FOSA,22.4%),并最终降解成稳定的PFOS (23.3%),主要代谢产物为N-EtFOSAA。8:2FTOH在土壤—蚯蚓系统主要的最终代谢产物为全氟辛酸(PFOA),10:2FTOH在土壤—蚯蚓系统主要的最终代谢产物为全氟癸酸(PFDA)。研究结果说明全氟前体物质的降解是环境中的PFSAs和PFCAs一个重要来源。
Perfluoroalkyl substances (PFASs) are a group of synthetic compounds which have been widely applied in a variety of commercial and industrial products, such as surfactants, refrigerants, lubricants, paints, fire fighting foams, cosmetics and so on. PFASs have unique water and oil repelling characteristics due to the hydrophobic fluorinated carbon chain and hydrophilic sulfonate or carboxylate end groups. PFASs are released into the environment during the production, application, transport and disposal of PFAS containing products or by degradation of their precursors, and they are ubiquitous in environmental matrices such as air, water, soil and sewage sludge. PFASs can be bioaccumulated and biomagnified throughout the food chain due to their strong binding potential to proteins and may have dverse effects to individual organisms, food webs and human health. The bioaccumulation of PFASs has become a major concern of the international community.
Earthworms were exposed to artificially contaminated soils with ten PFASs to investigate the bioaccumulation and bioavailabiliry of PFASs. All the test PFASs in soil are bioaccumulative to earthworms. The uptake rate coefficients () of PFASs in the range of0.016(perfluorohexanoate, PFHxA)-0.102d-1(perfluorododecanoate, PFDoA) for PFCAs and0.003(perfluorobutane sulfonate, PFBS)-0.030d-1(perfluorooctane sulfonate, PFOS) for PFSAs. The elimination rate coefficients (ke) of PFASs in the range of0.030(PFDoA)-0.187d-1(PFHxA) for PFCAs and0.039(PFOS)-0.072d'1(PFBS) for PFSAs. PFASs with longer perfluorinated carbon chain displayed higher uptake rate coefficients (ku), longer half-life (t1/2) and time to steady-state (tss) but lower elimination rate coefficients (ke) than the shorter ones. Similarly, perfiorosulfonates acids (PFSAs) displayed higher ku, longer t1/2and tss but lower ke than perflurocarboxylic acids (PFCAs) with the same perfluorinated chain length. The results indicate that the uptake of PFASs in the earthworms becomes much easier while the elimination becomes more difficult as the perfluorinated chain length increases and PFCAs are much easier to eliminate from earthworm than PFCAs of equivalent perfluorinated chain length. All the studied PFASs, including those with seven or less perfluorinated carbons, such as PFHxA, perfluoroheptanoate (PFHpA), perfluorooctanoate (PFOA), PFBS and perfluorohexane sulfonate (PFHxS), were bioaccumulated in the earthworms and the biota-to-soil accumulation factors (BSAFs) increased with perfluorinated carbon chain length and were greater for PFSAs than for PFCAs of equal perfluoroalkyl chain length. The BSAFs were found to be dependent on the concentrations of PFASs in soil and decreased as the level of PFASs in soil increased.
Wheats were exposed to soils contaminated with11PFASs. Wheat could uptake PFASs from soil by wheat root and translocated to wheat shoot with root concentration factors and bioconcentration factors that decreased as the number of perfluorinated carbons in the molecule increased. And the RCFs of PFASs decreased with the distribution coefficient values between soil and interstitial water (Koc) increased. Translocation factors (TF) of PFCAs in wheat peaked at PFHxA and decreased significantly as the number of carbons increased or decreased. PFHxS produced the greatest TF of the threePFSAs examined. Since PFASs displayed opposite accumulation potentials in earthworms compared to wheat, the accumulation factors of PFASs in earthworms and wheat crossed at around PFHpA, which displayed similar BSAFs in earthworms and BCF in wheat. When the number of perfluorinated carbon is>7, the BSAFs of PFASs in earthworms were larger than their BCFs in plants, while the BSAFs in earthworms were lower than plant BCFs if the number of perfluorinated carbons was<7. The bioaccumulation of PFASs in plant was dependent on the distribution coefficients between soil and interstitial water, ability to cross plant membranes and their water solubility and hydrophobicity.
Wheats and earthworms were exposed together to soils contaminated with11PFASs to investigate the mutual impacts of wheat and earthworm on their bioaccumulation of PFASs from soil. Wheat increased the bioaccumulation of all11PFASs in earthworms and earthworms increased the bioaccumulation in wheat of PFCAs containing seven or less perfluorinated carbons, decreased bioaccumulation of PFCAs with more than seven carbons, and decreased bioaccumulation of PFSAs. In general, the co-presence of wheat and earthworms enhanced the bioavailability of PFASs in soil. When earthworms and wheat are both present in soil, they may affect the accumulation of PFASs within each other by competition or by changing the bioavailability of the contaminants.
The bioaccumulation and metabolism of N-ethyl perfluorooctane sulfonamidoethanol (N-EtFOSE) and two fluorotelomer alcohols (FTOH, perfluorooctylethanol,(8:2FTOH), perfluorodecylethanol,(10:2FTOH)) in earthworm from soil were investigated. N-EtFOSE in earthworm could be degraded to PFOS via some stable intermediate metabolites, N-EtFOSE->N-ethylperfluorooctane sulfonamide acetate (N-EtFOSAA,52.4%)→perfluorooctane sulfonamide acetate (FOSAA,2.0%)→perfluorooctane sulfonamide (FOSA,22.4%)→PFOS (23.3%). N-EtFOAA was the major metabolite and PFOS was the terminal product of N-EtFOSE. PFOA was the major terminal metabolitesof8:2FTOH and perfluorodecanoate (PFDA) was the major terminal metabolite of10:2FTOH. The results suggested that the biotic degradation of PFAS precursors is an important source of PFCAs and PFSAs in the environment.
引文
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