摘要
有机磷酸酯(Organophosphate Esters,OPEs)作为典型阻燃剂,易吸附于大气细颗粒物(PM_(2.5))表面,对人群健康构成潜在风险。为应对PM_(2.5)复杂基质中多类别OPEs同步精准定量的挑战,建立了一种基于超高效液相色谱-三重四极杆串联质谱(UHPLC-QqQ-MS/MS)的高灵敏度分析方法。结果表明:①通过甲醇超声提取结合ENVI-18固相萃取柱净化,实现了PM_(2.5)中OPEs的高效提取(平均提取率为82.2%)与基质净化(基质效应为0.9%~17.4%);进一步通过Acquity UPLC BEH C_(18)色谱柱,以0.1%甲酸水溶液/甲醇为流动相进行梯度洗脱,结合UHPLC-QqQ-MS/MS实现了对28种烷基、芳基及氯代OPEs的有效分离与检测。②方法学验证显示,该方法在相应浓度范围内线性关系良好(R^(2)>0.999)、灵敏度高(检出限为0.19~0.97 pg/m^(3))、准确度与精密度可靠(加标回收率为70.8%~116.7%,相对标准偏差为2.8%~14.4%)。③该方法应用于北京市PM_(2.5)样本分析,所有目标物均有检出,总浓度范围为2.0×10^(3)~6.4×10^(3)pg/m^(3),磷酸三(1-氯-2-丙基)酯(TCIPP)和磷酸三(2-氯乙基)酯(TCEP)中位数浓度较高,分别为1.3×10^(3)和0.7×10^(3)pg/m^(3)。研究显示,本研究建立的OPEs检测方法操作简便、重现性好,适用于大气PM_(2.5)中多类别OPEs的高通量筛查,可为环境暴露与健康风险评价提供技术支持。
Organophosphate esters(OPEs)are widely used as flame retardants and can readily adsorb onto atmospheric fine particulate matter(PM_(2.5)),posing potential risks to human health.To address the challenge of accurately and simultaneously quantifying multiple categories of OPEs in the complex PM_(2.5)matrix,a highly sensitive analytical method based on ultra-high-performance liquid chromatography-triple quadrupole tandem mass spectrometry(UHPLC-QqQ-MS/MS)was developed.The results indicate that:(1)Efficient extraction and purification of OPEs from PM_(2.5)were achieved through methanol ultrasonic extraction combined with ENVI-18 solid-phase extraction(SPE)column cleanup,resulting in an average extraction efficiency of 82.2%and matrix effects ranging from 0.9%to 17.4%.Using an Acquity UPLC BEH C_(18) chromatographic column,with 0.1%formic acid aqueous solution and methanol as the mobile phase under gradient elution,the UHPLC-QqQ-MS/MS system successfully enabled the effective separation and detection of 28 alkyl,aryl,and chlorinated OPEs.(2)Method validation demonstrated excellent linearity within the tested concentration ranges(R^(2)>0.999),high sensitivity with detection limits of 0.19 to 0.97 pg/m^(3),and reliable accuracy and precision,with spiked recoveries of 70.8%-116.7%and relative standard deviations of 2.8%-14.4%.(3)Application of the method to PM_(2.5)samples in Beijing showed that all target compounds were detected,with total concentrations ranging from 2.0×10^(3)to 6.4×10^(3)pg/m^(3).Among them,tris(2-chloroisopropyl)phosphate(TCIPP)and tris(2-chloroethyl)phosphate(TCEP)exhibited relatively high median concentrations of 1.3×10^(3)pg/m^(3)and 0.7×10^(3)pg/m^(3),respectively.This study demonstrates that the developed method for OPE detection is simple to operate,highly reproducible,and suitable for high-throughput screening of multiple classes of OPEs in atmospheric PM_(2.5),providing technical support for environmental exposure assessment and health risk evaluation.
作者
段舒龄
刘娟
吴非
陈钰瑶
王梦瑶
贝昕玥
赵哲
崔洪洋
顾雯
王超
史亚利
唐宋
DUAN Shuling;LIU Juan;WU Fei;CHEN Yuyao;WANG Mengyao;BEI Xinyue;ZHAO Zhe;CUI Hongyang;GU Wen;WANG Chao;SHI Yali;TANG Song(China CDC Key Laboratory of Environment and Population Health,National Institute of Environmental Health,Chinese Center for Disease Control and Prevention,Beijing 100021,China;Center for Global Health,School of Public Health,Nanjing Medical University,Nanjing 211166,China;State Key Laboratory of Environmental Chemistry and Ecotoxicology,Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing 100085,China)
出处
《环境科学研究》
北大核心
2026年第4期913-923,共11页
Research of Environmental Sciences
基金
国家自然科学基金项目(No.82241091)
国家重点研发计划项目(No.2022YFC3702700)
北京市自然科学基金青年项目(No.7244456)。
关键词
有机磷酸酯
阻燃剂
超高效液相色谱-三重四极杆串联质谱
固相萃取
PM_(2.5)
organophosphate esters
flame retardants
ultra-high-performance liquid chromatography-triple quadrupole tandem mass spectrometry
solid-phase extraction
PM_(2.5)
