Simultaneous Determination of 5 PBT Substances in Toys by High Performance Liquid Chromatography-Tandem Mass Spectrometry
摘 要
提出了高效液相色谱-串联质谱法同时测定玩具中5种持久性、生物累积性和毒性(PBT)物质含量的方法。按照ISO 8124-3:2020对玩具中的涂层、塑料及纺织物进行取样和处理,分取1 g,加入10 mL甲苯。密封,于常温超声萃取30 min。取上层清液过0.45 μm滤膜,滤液用高效液相色谱-串联质谱仪分析。在色谱分析中,以Agilent Poroshell HPH-C18色谱柱为固定相,以不同体积比的甲醇-0.1%(体积分数)乙酸溶液的混合溶液为流动相进行梯度洗脱分离。在质谱分析中,采用电喷雾离子源正离子(ESI+)模式和多反应监测(MRM)模式扫描,外标法定量。结果显示,5种PBT物质的质量浓度在0.005~0.2 mg·L-1内和峰面积呈线性关系,检出限(3S/N)为0.010~0.078 mg·kg-1。按照标准加入法进行回收试验,回收率为85.7%~105%,测定值的相对标准偏差(n=6)均不大于7.0%。
Abstract
A method of high performance liquid chromatography-tandem mass spectrometry was proposed for the simultaneous determination of 5 persistent, bioaccumulative and toxic (PBT) substances in toys. The coatings, plastics, and textiles of toys were collected and treated in accordance with ISO 8124-3:2020, and an aliquot (1 g) was taken, and mixed with 10 mL of toluene. After sealing, ultrasonic extraction was performed at room temperature for 30 min. The supernatant was taken and passed through a 0.45 μm filter membrane, and the filtrate was analyzed by high performance liquid chromatograph-tandem mass spectrometer. In the chromatography analysis, Agilent Poroshell HPH-C18 column was used as the stationary phase, and mixed solutions composed of methanol and 0.1% (volume fraction) acetic acid solution at different volume ratios were used as the mobile phase for gradient elution separation. In the mass spectrometry analysis, ESI+ and MRM modes were used for scanning, and external standard method was used for quantification. It was shown that linear relationships between values of the mass concentration of 5 PBT substances and the peak area were kept in the range of 0.005-0.2 mg·L-1, with detection limits (3S/N) in the range of 0.010-0.078 mg·kg-1. Test for recovery was made according to the standard addition method, giving recoveries in the range of 85.7%-105%, and RSDs (n=6) of the determined values were not greater than 7.0%.
中图分类号 O657.63 DOI 10.11973/lhjy-hx202311013
所属栏目 工作简报
基金项目 海关总署科研项目(2019HK069)
收稿日期 2022/2/1
修改稿日期
网络出版日期
作者单位点击查看
备注巫珊珊,工程师,博士,主要从事婴童用品中有害物质检测工作
引用该论文: WU Shanshan,ZHENG Jianguo,LIU Chonghua,LIN Shaopeng,YI Lezhou. Simultaneous Determination of 5 PBT Substances in Toys by High Performance Liquid Chromatography-Tandem Mass Spectrometry[J]. Physical Testing and Chemical Analysis part B:Chemical Analysis, 2023, 59(11): 1321~1326
巫珊珊,郑建国,刘崇华,林绍鹏,蚁乐洲. 高效液相色谱-串联质谱法同时测定玩具中5种PBT物质的含量[J]. 理化检验-化学分册, 2023, 59(11): 1321~1326
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【2】ZHANG R, ZHANG X S, SHI J Q, et al. Polychlorinated diphenyl sulfides:An emerging class of persistent, bioaccumulative, and toxic substances in the environment[J]. Environmental Toxicology and Chemistry, 2021,40(10):2657-2666.
【3】MATTHIES M, SOLOMON K, VIGHI M, et al. The origin and evolution of assessment criteria for persistent, bioaccumulative and toxic (PBT) chemicals and persistent organic pollutants (POPs)[J]. Environmental Science:Processes & Impacts, 2016,18(9):1114-1128.
【4】DU J, LI H X, XU S D, et al. A review of organophosphorus flame retardants (OPFRs):Occurrence, bioaccumulation, toxicity, and organism exposure[J]. Environmental Science and Pollution Research, 2019,26(22):22126-22136.
【5】张其才,饶钦雄,王献礼,等.固相萃取净化-气相色谱法测定食用菌及其栽培基质中26种多溴联苯醚[J].分析试验室, 2022(5):558-563.
【6】CHUPEAU Z, BONVALLOT N, MERCIER F, et al. Organophosphorus flame retardants:A global review of indoor contamination and human exposure in Europe and epidemiological evidence[J]. International Journal of Environmental Research and Public Health, 2020,17(18):6713.
【7】HOU R, XU Y P, WANG Z J. Review of OPFRs in animals and humans:Absorption, bioaccumulation, metabolism, and internal exposure research[J]. Chemosphere, 2016,153:78-90.
【8】CHECK L, MARTEEL-PARRISH A. The fate and behavior of persistent, bioaccumulative, and toxic (PBT) chemicals:Examining lead (Pb) as a PBT metal[J]. Reviews on Environmental Health, 2013,28(2/3):85-96.
【9】DÓREA J G. Persistent, bioaccumulative and toxic substances in fish:Human health considerations[J]. The Science of the Total Environment, 2008,400(1/2/3):93-114.
【10】GAO X Z, HUANG P, HUANG Q H, et al. Organophosphorus flame retardants and persistent, bioaccumulative, and toxic contaminants in Arctic seawaters:On-board passive sampling coupled with target and non-target analysis[J]. Environmental Pollution, 253(2019):1-10.
【11】SEGEV O, KUSHMARO A, BRENNER A. Environmental impact of flame retardants (persistence and biodegradability)[J]. International Journal of Environmental Research and Public Health, 2009,6(2):478-491.
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【15】LI Y, HASHI Y, LIU Y, et al. Comparison and optimization of several pretreatment techniques for determination of decabrominated diphenyl ether in polymer samples by gas chromatography mass spectrometry[J]. Analytical Sciences, 2009,25(4):523-527.
【16】CEQUIER E, MARCÉ R M, BECHER G, et al. Determination of emerging halogenated flame retardants and polybrominated diphenyl ethers in serum by gas chromatography mass spectrometry[J]. Journal of Chromatography A, 2013,1310:126-132.
【17】CEQUIER E, MARCÉ R M, BECHER G, et al. Determination of emerging halogenated flame retardants and polybrominated diphenyl ethers in serum by gas chromatography mass spectrometry[J]. Journal of Chromatography A, 2013,1310:126-132.
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【19】LI Y Y, WEI G H, WANG X D. Determination of decabromodiphenyl ether in water samples by single-drop microextraction and RP-HPLC[J]. Journal of Separation Science, 2007,30(16):2698-2702.
【20】GHANEM R, BAKER H. Determination of decabromodiphenyl ether in backcoated textile preparation[J]. Journal of Hazardous Materials, 2009,162(1):249-253.
【21】SURMA-ZADORA M, GROCHOWALSKI A. Using a membrane technique (SPM) for high fat food sample preparation in the determination of chlorinated persistent organic pollutants by a GC/ECD method[J]. Food Chemistry, 2008,111(1):230-235.
【22】LEONG M I, HUANG S D. Dispersive liquid-liquid microextraction method based on solidification of floating organic drop combined with gas chromatography with electron-capture or mass spectrometry detection[J]. Journal of Chromatography A, 2008,1211(1/2):8-12.
【23】FANG Y Y, NIE Z Q, DIE Q Q, et al. Organochlorine pesticides in soil, air, and vegetation at and around a contaminated site in southwestern China:Concentration, transmission, and risk evaluation[J]. Chemosphere, 2017,178:340-349.
【24】ZHANG H Y, JIANG L, ZHOU X, et al. Determination of hexachlorobutadiene, pentachlorobenzene, and hexachlorobenzene in waste incineration fly ash using ultrasonic extraction followed by column cleanup and GC-MS analysis[J]. Analytical and Bioanalytical Chemistry, 2018,410(7):1893-1902.
【25】MAJOROS L I, LAVA R, RICCI M, et al. Full method validation for the determination of hexachlorobenzene and hexachlorobutadiene in fish tissue by GC-IDMS[J]. Talanta, 2013,116:251-258.
【26】PILLA D, KAVADI A K M, GURIJALA P, et al. Determination of selected chlorohydrocarbons and polyaromatic hydrocarbons by gas chromatography-mass spectrometry in soils in Southwest Louisiana[J]. Microchemical Journal, 2009,91(1):13-15.
【27】索莉莉,朱群英,胡美华.超声辅助萃取-液相色谱-串联质谱法同时检测水产品中11种有机磷酸酯类阻燃剂[J].食品工业科技, 2018,39(6):210-216.
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