超高效液相色谱串联质谱法快速测定地下水和含水层介质中16种全氟烷基酸
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摘要
全氟烷基酸(PFAAs)是一种新型的持久有机污染物,在各种环境介质中被频繁检出。目前,PFAAs的检测方法主要包括液相色谱串联质谱法(HPLC-MS/MS)、超高效液相色谱串联质谱法(UPLC-MS/MS)、气相色谱法和光谱类方法。但是,上述方法多存在样品前处理过程复杂、周期长、成本高的问题,不适用于PFAAs的快速检测。为此,本文建立了一种快速测量地下水和含水层介质中16种PFAAs的UPLC-MS/MS方法。水样过0.22μm滤膜后直接测定浓度,土样经过超声离心后,取上清液过滤测量浓度。本方法分别为16种PFAAs建立了低浓度(5～50μg/L)和高浓度(100～500μg/L)两条校准曲线,相关系数R~2>0.99。地下水中16种PFAAs快速检测方法检出限为0.06～1.07μg/L,回收率为75%～120%,精密度(RSD)为2.61%～9.19%(除高浓度时全氟丁烷磺酸和全氟已烷磺酸分别为11.34%和14.70%外)。含水层介质中14种PFAAs(全氟十三酸和全氟十四酸除外)方法检出限为2.69～12.33ng/g,回收率为65%～103%,精密度(RSD)为1.96%～7.22%。
Perfluorinated alkyl acids(PFAAs)are a group of emerging persistent organic pollutant that have received increasing attention due to their global occurrence,accumulation and toxicity.At present,PFAA detection mainly uses high-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS),ultra-performance liquid chromatography-tandem mass spectrometry(UPLC-MS/MS),gas chromatography(GC)and spectroscopy.However,these detection methods often involve complicated sample pretreatment,longer work cycle and higher cost,therefore,they are not suitable for quick PFAA detection.In this study,we developed a method for quick analysis of 16 PFAAs in groundwater and aquifer based on UPLC-MS/MS.In the experiment,the groundwater sample was filtered through 0.22μm membrane and injected directly into the detection instrument;the aquifer sample was prepared by liquid solvent extraction.A good linear calibration using 16 PFAAs standards was achieved(R~2>0.99)in the low and high concentration ranges of 5-50 and 100-500μg/L,respectively.The method's detection limits(MDLs)of 16 PFAAs in groundwater were 0.06-1.07μg/L,and the recovery rates were 75%-120% with relative standard deviations(RSD)at2.61%-9.19%.In aquifer media,MDLs of 14 PFAAs were 2.69-12.33 ng/L,and the recovery rates were65%-103% with RSDs at 1.96%-7.22%.
Perfluorinated alkyl acids(PFAAs)are a group of emerging persistent organic pollutant that have received increasing attention due to their global occurrence,accumulation and toxicity.At present,PFAA detection mainly uses high-performance liquid chromatography-tandem mass spectrometry(HPLC-MS/MS),ultra-performance liquid chromatography-tandem mass spectrometry(UPLC-MS/MS),gas chromatography(GC)and spectroscopy.However,these detection methods often involve complicated sample pretreatment,longer work cycle and higher cost,therefore,they are not suitable for quick PFAA detection.In this study,we developed a method for quick analysis of 16 PFAAs in groundwater and aquifer based on UPLC-MS/MS.In the experiment,the groundwater sample was filtered through 0.22μm membrane and injected directly into the detection instrument;the aquifer sample was prepared by liquid solvent extraction.A good linear calibration using 16 PFAAs standards was achieved(R~2>0.99)in the low and high concentration ranges of 5-50 and 100-500μg/L,respectively.The method's detection limits(MDLs)of 16 PFAAs in groundwater were 0.06-1.07μg/L,and the recovery rates were 75%-120% with relative standard deviations(RSD)at2.61%-9.19%.In aquifer media,MDLs of 14 PFAAs were 2.69-12.33 ng/L,and the recovery rates were65%-103% with RSDs at 1.96%-7.22%.
引文
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[6]王燕,吕达,郭明,等.全氟辛酸与血清蛋白分子间作用的紫外荧光光谱分析法建立及理论模建研究[J].光谱学与光谱分析,2018(2):494-501.
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[14] FAGBAYIGBO B O,OPEOLU B O,FATOKI O S,et al.Validation and determination of nine PFCS in surface water and sediment samples using UPLC-QTOF-MS[J].Environmental Monitoring and Assessment,2018,190(6):346.
[15] ZHAO X,XIA X,ZHANG S,et al.Spatial and vertical variations of perfluoroalkyl substances in sediments of the Haihe River,China[J].Journal of Environmental Sciences,2014,26(8):1557-1566.
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[20]范庆,邓述波,周琴,等.城市污水处理厂中全氟化合物的存在及去除效果研究[J].环境污染与防治,2011,33(1):30-35.
[21]王懿,孔德洋,单正军,等.加速溶剂萃取-固相萃取净化-超高效液相色谱串联质谱法测定土壤中11种全氟化合物[J].环境化学,2012,31(1):113-119.
[22]李法松,倪卉,黄涵宇,等.安徽省部分城市土壤中全氟化合物空间分布及来源解析[J].环境科学,2017,38(1):327-332.
[23]章涛,孙红文,ALFREDO C,等.液相萃取-高效液相色谱-串联质谱联用测定污泥中的全氟化合物[J].色谱,2010,28(5):498-502.
[24]刘庆,贺德春,许振成,等.液相色谱-串联质谱法测定水体、沉积物及土壤中全氟化合物[J].中国环境监测,2014(4):134-139.
[25]陈舒.中国东部地区典型全氟化合物污染地理分布特征及来源辨析[D].北京:中国地质科学院,2016.
[26]张晓梅,张竹青,黄文鹏.超声萃取-高效液相色谱法测定土壤中多环芳烃[J].环境科学与管理,2010,35(7):124-127.
[27]张翠华,张菊花,范小振.超声萃取-高效液相色谱法检测土壤中烟嘧磺隆和莠去津的残留量[J].化学研究与应用,2018(1):114-118.
[28]曹攽,李云木子,马军,等.超声波萃取-高效液相色谱法测定土壤中邻苯二甲酸酯[J].岩矿测试,2011,30(2):178-181.
[29]潘媛媛,史亚利,蔡亚岐.土壤、底泥和活性污泥中全氟化合物的高效液相色谱-串联质谱分析方法[J].环境化学,2010,29(3):519-523.
[30]张莉,陈亮,刘菲.快速分光光度法同步测定地下水中赤霉素和草甘膦的相互影响[J].光谱学与光谱分析,2015,35(4):966-970.
[2] CHEN X,ZHU L,PAN X,et al.Isomeric specific partitioning behaviors of perfluoroalkyl substances in water dissolved phase,suspended particulate matters and sediments in Liao River Basin and Taihu Lake,China[J].Water Research,2015,80:235-244.
[3] WANG T,VESTERGREN R,HERZKE D,et al.Levels,isomer profiles,and estimated riverine mass discharges of perfluoroalkyl acids and fluorinated alternatives at the mouths of Chinese Rivers[J].Environmental Science and Technology,2016,50(21):1584.
[4] LOOS R,LOCORO G,COMERO S,et al.Pan-European survey on the occurrence of selected polar organic persistent pollutants in ground water[J].Water Research,2010,44(14):4115-4126.
[5] WANG X,HALSALL C,CODLING G,et al.Accumulation of perfluoroalkyl compounds in Tibetan mountain snow:temporal patterns from 1980to 2010[J].Environmental Science and Technology,2014,48(1):173-181.
[6]王燕,吕达,郭明,等.全氟辛酸与血清蛋白分子间作用的紫外荧光光谱分析法建立及理论模建研究[J].光谱学与光谱分析,2018(2):494-501.
[7]任肖敏,张连营,郭良宏.多溴联苯醚和PFAAs的分子毒理机制研究[J].环境化学,2014,1(10):1662-1671.
[8]王士运.全氟化合物PFOA对雄性黑斑蛙的生殖毒效应及机理研究[D].杭州:杭州师范大学,2017.
[9]叶露,吴玲玲,蒋雨希,等.PFOS/PFOA对斑马鱼(Daniorerio)胚胎致毒效应研究[J].环境科学,2009,30(6):1727-1732.
[10]郭睿,蔡亚岐,江桂斌,等.全氟辛烷磺酰基化合物(PFOS)的污染现状与研究趋势[J].化学进展,2006,1(6):808-813.
[11]于茜.全氟壬酸的GC-MS检测及其在沉积物上的吸附特征研究[D].长沙:湖南大学,2012.
[12]陈现平,陶艺,吴飞,等.维多利亚蓝B共振光散射法高灵敏选择性检测全氟辛烷磺酸[J].光谱学与光谱分析,2017,37(3):811-815.
[13] FANG S,ZHAO S,ZHANG Y,et al.Distribution of perfluoroalkyl substances(PFASs)with isomer analysis among the tissues of aquatic organisms in Taihu Lake,China[J].Environmental Pollution,2014,193(10):224-232.
[14] FAGBAYIGBO B O,OPEOLU B O,FATOKI O S,et al.Validation and determination of nine PFCS in surface water and sediment samples using UPLC-QTOF-MS[J].Environmental Monitoring and Assessment,2018,190(6):346.
[15] ZHAO X,XIA X,ZHANG S,et al.Spatial and vertical variations of perfluoroalkyl substances in sediments of the Haihe River,China[J].Journal of Environmental Sciences,2014,26(8):1557-1566.
[16]孟晶,王铁宇,王佩,等.淮河流域土壤中全氟化合物的空间分布及组成特征[J].环境科学,2013,8(8):3188-3194.
[17] CASAL P,GONZLB,ZHANG Y,et al.Accumulation of perfluoroalkylated substances in ceanic plankton[J].Environmental Science and Technology,2017,51(5):2766-2775.
[18] AHRENS L,NORSTR M K,VIKTOR T,et al.Stockholm Arlanda airport as a source of per-and polyfluoroalkyl substances to water,sediment and fish[J].Chemosphere,2015,129(Suppl 1):33-38.
[19] AHRENS L,YAMASHITA N,YEUNG L W Y,et al.Partitioning behavior of per-and polyfluoroalkyl compounds between pore water and sediment in two sediment cores from Tokyo Bay,Japan[J].Environmental Science and Technology,2009,43(18):6969-6975.
[20]范庆,邓述波,周琴,等.城市污水处理厂中全氟化合物的存在及去除效果研究[J].环境污染与防治,2011,33(1):30-35.
[21]王懿,孔德洋,单正军,等.加速溶剂萃取-固相萃取净化-超高效液相色谱串联质谱法测定土壤中11种全氟化合物[J].环境化学,2012,31(1):113-119.
[22]李法松,倪卉,黄涵宇,等.安徽省部分城市土壤中全氟化合物空间分布及来源解析[J].环境科学,2017,38(1):327-332.
[23]章涛,孙红文,ALFREDO C,等.液相萃取-高效液相色谱-串联质谱联用测定污泥中的全氟化合物[J].色谱,2010,28(5):498-502.
[24]刘庆,贺德春,许振成,等.液相色谱-串联质谱法测定水体、沉积物及土壤中全氟化合物[J].中国环境监测,2014(4):134-139.
[25]陈舒.中国东部地区典型全氟化合物污染地理分布特征及来源辨析[D].北京:中国地质科学院,2016.
[26]张晓梅,张竹青,黄文鹏.超声萃取-高效液相色谱法测定土壤中多环芳烃[J].环境科学与管理,2010,35(7):124-127.
[27]张翠华,张菊花,范小振.超声萃取-高效液相色谱法检测土壤中烟嘧磺隆和莠去津的残留量[J].化学研究与应用,2018(1):114-118.
[28]曹攽,李云木子,马军,等.超声波萃取-高效液相色谱法测定土壤中邻苯二甲酸酯[J].岩矿测试,2011,30(2):178-181.
[29]潘媛媛,史亚利,蔡亚岐.土壤、底泥和活性污泥中全氟化合物的高效液相色谱-串联质谱分析方法[J].环境化学,2010,29(3):519-523.
[30]张莉,陈亮,刘菲.快速分光光度法同步测定地下水中赤霉素和草甘膦的相互影响[J].光谱学与光谱分析,2015,35(4):966-970.
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