山东莱州湾出生队列孕妇及幼儿有机磷农药暴露水平
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摘要
[目的]测定山东莱州湾出生队列中孕妇及24月龄幼儿的有机磷农药(organophosphate pesticides,OPs)暴露水平。[方法]依托于山东莱州湾出生队列研究,对436名孕妇进行问卷调查,收集孕妇产前随机尿,并随访至24个月,收集239份24月龄幼儿的随机尿。采用气相色谱-质谱串联法检测孕妇及幼儿尿液中6种OPs非特异性代谢产物,即二乙基二硫代磷酸酯(diethyldithiophosphate,DEDTP)、二乙基硫代磷酸酯(diethylthiophosphate,DETP)、磷酸二乙酯(diethylphosphate,DEP)、二甲基二硫代磷酸酯(dimethyldithiophosphate,DMDTP)、二甲基硫代磷酸酯(dimethylthiophosphate,DMTP)、磷酸二甲酯(dimethylphosphate,DMP)。采用Spearman相关分析孕妇及幼儿尿液中OPs非特异性代谢产物水平的相关性。[结果]436份孕妇尿样中DEP、DETP、DMP、DMTP的水平分别为11.41、1.93、21.42、2.24μg/g(经尿肌酐校正),239份幼儿尿样中DEP、DETP、DMP、DMTP的水平分别为16.65、3.95、38.68、3.48μg/g(经尿肌酐校正)。仅发现孕妇与幼儿尿液中的DEP水平呈负相关(r=-0.149,P=0.021)。[结论]山东省渤海莱州湾出生队列中的孕妇及幼儿OPs暴露水平较高,应引起重视。
[Objective] To determine the organophosphate pesticides(OPs) exposure levels in pregnant women and children at 24 months of age fromLaizhou Wan(Bay) Birth Cohort(LWBC) in Shandong.[Methods] The present study was a part of a longitudinal birth cohort study in the southern coastal area of Laizhou Wan(Bay) of the Bohai Sea,Shandong Province,China.Pregnant women(n=436) were recruited to complete a questionnaire survey and to collect random spot urine samples.They were followed up until their children were 24 months of age to collect children's urine samples(n=239).Non-specific OPs metabolites,including diethyldithiophosphate(DEDTP),diethylthiophosphate(DETP),diethylphosphate(DEP),dimethyldithiophosphate(DMDTP),dimethylthiophosphate(DMTP),and dimethylphosphate(DMP),in mothers' and children's urine samples were detected by gas chromatography-mass spectrometry.Correlations of the non-specific OPs metabolites mother's and children's urine samples were analyzed by Spearman correlation analysis.[Results] The creatinine-adjusted levels in 436 maternal urine samples were 11.41 μg/g for DEP,1.93 μg/g for DETP,21.42 μg/g for DMP,and 2.24 μg/g for DMTP,respectively.The levels in 239 twenty-four-month-old children's urine samples were 16.65 μg/g for DEP,3.95 μg/g for DETP,38.68 μg/g for DMP,and 3.48 μg/g for DMTP,respectively.A negative correlation was found between DEP levels in maternal and children's urine samples(r=-0.149,P=0.021).[Conclusion] The pregnant women and children from the Laizhou Bay Birth Cohort show high exposure levels of OPs,requiring concerns.
[Objective] To determine the organophosphate pesticides(OPs) exposure levels in pregnant women and children at 24 months of age fromLaizhou Wan(Bay) Birth Cohort(LWBC) in Shandong.[Methods] The present study was a part of a longitudinal birth cohort study in the southern coastal area of Laizhou Wan(Bay) of the Bohai Sea,Shandong Province,China.Pregnant women(n=436) were recruited to complete a questionnaire survey and to collect random spot urine samples.They were followed up until their children were 24 months of age to collect children's urine samples(n=239).Non-specific OPs metabolites,including diethyldithiophosphate(DEDTP),diethylthiophosphate(DETP),diethylphosphate(DEP),dimethyldithiophosphate(DMDTP),dimethylthiophosphate(DMTP),and dimethylphosphate(DMP),in mothers' and children's urine samples were detected by gas chromatography-mass spectrometry.Correlations of the non-specific OPs metabolites mother's and children's urine samples were analyzed by Spearman correlation analysis.[Results] The creatinine-adjusted levels in 436 maternal urine samples were 11.41 μg/g for DEP,1.93 μg/g for DETP,21.42 μg/g for DMP,and 2.24 μg/g for DMTP,respectively.The levels in 239 twenty-four-month-old children's urine samples were 16.65 μg/g for DEP,3.95 μg/g for DETP,38.68 μg/g for DMP,and 3.48 μg/g for DMTP,respectively.A negative correlation was found between DEP levels in maternal and children's urine samples(r=-0.149,P=0.021).[Conclusion] The pregnant women and children from the Laizhou Bay Birth Cohort show high exposure levels of OPs,requiring concerns.
引文
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[13]YE X,PIERIK F H,HAUSER R,et al.Urinary metabolite concentrations of organophosphorous pesticides,bisphenol A,and phthalates among pregnant women in Rotterdam,the Netherlands:the Generation R study[R].Environ Res,2008,108(2):260-267.
[14]BECKER K,SEIWERT M,ANGERER J,et al.Ger ES IV pilot study:assessment of the exposure of German children to organophosphorus and pyrethroid pesticides[J].Int J Hyg Environ Health,2006,209(3):221-233.
[15]APREA C,STRAMBI M,NOVELLI M T,et al.Biologic monitoring of exposure to organophosphorus pesticides in 195Italian children[J].Environ Health Perspect,2000,108(6):521-525.
[16]ESKENAZI B,MARKS A R,BRADMAN A,et al.Organophosphate pesticide exposure and neurodevelopment in young Mexican-American children[J].Environ Health Perspect,2007,115(5):792-798.
[17]BARR D B,BRAVO R,WEERASEKERA G,et al.Concentrations of dialkyl phosphate metabolites of organophosphorus pesticides in the U.S.population[J].Environ Health Perspect,2004,112(2):186-200.
[18]ATWOOD D,PAISLEY-JONES C.Pesticides industry sales and usage:2008-2012 market estimates[R].Washington,DC:U.S.Environmental Protection Agency,2017.
[19]ROY R R,WILSON P,LASKI R R,et al.Monitoring of domestic and imported apples and rice by the U.S.Food and Drug Administration pesticide program[J].J AOAC Int,1997,80(4):883-894.
[20]BRADMAN A,KOGUT K,EISEN E A,et al.Variability of organophosphorous pesticide metabolite levels in spot and24-hr urine samples collected from young children during1 week[J].Environ Health Perspect,2013,121(1):118-124.
[21]SPAAN S,PRONK A,KOCH H M,et al.Reliability of concentrations of organophosphate pesticide metabolites in serial urine specimens from pregnancy in the Generation R Study[J].J Expo Sci Environ Epidemiol,2015,25(3):286-294.
[22]MEEKER J D,BARR D B,RYAN L,et al.Temporal variability of urinary levels of nonpersistent insecticides in adult men[J].J Expo Anal Environ Epidemiol,2005,15(3):271-281.
[2]CHEN C,LI Y,CHEN M,et al.Organophosphorus pesticide residues in milled rice(Oryza sativa)on the Chinese market and dietary risk assessment[J].Food Addit Contam Part A Chem Anal Control Expo Risk Assess,2009,26(3):340-347.
[3]WANG P,TIAN Y,WANG X J,et al.Organophosphate pesticide exposure and perinatal outcomes in Shanghai,China[J].Environ Int,2012,42:100-104.
[4]DING G,WANG P,TIAN Y,et al.Organophosphate pesticide exposure and neurodevelopment in young Shanghai children[J].Environ Sci Technol,2012,46(5):2911-2917.
[5]BRADMAN A,BARR D B,CLAUS HENN B G,et al.Measurement of pesticides and other toxicants in amniotic fluid as a potential biomarker of prenatal exposure:a validation study[J].Environ Health Perspect,2003,111(14):1779-1782.
[6]WHYATT R M,BARR D B.Measurement of organ-ophosphate metabolites in postpartum meconium as a potential biomarker of prenatal exposure:a validation study[J].Environ Health Perspect,2001,109(4):417-420.
[7]ZARTARIAN V G,?ZKAYNAK H,BURKE J M,et al.A modeling framework for estimating children’s residential exposure and dose to chlorpyrifos via dermal residue contact and nondietary ingestion[J].Environ Health Perspect,2000,108(6):505-514.
[8]ESKENAZI B,BRADMAN A,CASTORINA R.Exp-osures of children to organophosphate pesticides and their potential adverse health effects[J].Environ Health Perspect,1999,107 Suppl 3:409-419.
[9]姚新民,周志俊.长期接触低剂量有机磷农药对人体健康影响的研究进展[J].环境与职业医学,2008,25(4):409-411.
[10]DING G,CUI C,CHEN L,et al.Prenatal low-level mercury exposure and neonatal anthropometry in rural northern China[J].Chemopshere,2013,92(9):1085-1089.
[11]杨玉林,芮振荣,王宏,等.气相色谱法分析尿样中六种有机磷农药代谢产物[J].中国卫生检验杂志,2003,13(1):24-26.
[12]BRADMAN A,ESKENAZI B,BARR D B,et al.Organophosphate urinary metabolite levels during pregnancy and after delivery in women living in an agricultural community[J].Environ Health Perspect,2005,113(12):1802-1807.
[13]YE X,PIERIK F H,HAUSER R,et al.Urinary metabolite concentrations of organophosphorous pesticides,bisphenol A,and phthalates among pregnant women in Rotterdam,the Netherlands:the Generation R study[R].Environ Res,2008,108(2):260-267.
[14]BECKER K,SEIWERT M,ANGERER J,et al.Ger ES IV pilot study:assessment of the exposure of German children to organophosphorus and pyrethroid pesticides[J].Int J Hyg Environ Health,2006,209(3):221-233.
[15]APREA C,STRAMBI M,NOVELLI M T,et al.Biologic monitoring of exposure to organophosphorus pesticides in 195Italian children[J].Environ Health Perspect,2000,108(6):521-525.
[16]ESKENAZI B,MARKS A R,BRADMAN A,et al.Organophosphate pesticide exposure and neurodevelopment in young Mexican-American children[J].Environ Health Perspect,2007,115(5):792-798.
[17]BARR D B,BRAVO R,WEERASEKERA G,et al.Concentrations of dialkyl phosphate metabolites of organophosphorus pesticides in the U.S.population[J].Environ Health Perspect,2004,112(2):186-200.
[18]ATWOOD D,PAISLEY-JONES C.Pesticides industry sales and usage:2008-2012 market estimates[R].Washington,DC:U.S.Environmental Protection Agency,2017.
[19]ROY R R,WILSON P,LASKI R R,et al.Monitoring of domestic and imported apples and rice by the U.S.Food and Drug Administration pesticide program[J].J AOAC Int,1997,80(4):883-894.
[20]BRADMAN A,KOGUT K,EISEN E A,et al.Variability of organophosphorous pesticide metabolite levels in spot and24-hr urine samples collected from young children during1 week[J].Environ Health Perspect,2013,121(1):118-124.
[21]SPAAN S,PRONK A,KOCH H M,et al.Reliability of concentrations of organophosphate pesticide metabolites in serial urine specimens from pregnancy in the Generation R Study[J].J Expo Sci Environ Epidemiol,2015,25(3):286-294.
[22]MEEKER J D,BARR D B,RYAN L,et al.Temporal variability of urinary levels of nonpersistent insecticides in adult men[J].J Expo Anal Environ Epidemiol,2005,15(3):271-281.