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美国普通人群中有机磷酸酯阻燃剂化学品的暴露情况:来自2013 - 2014年国家健康与营养检查调查的数据。

Exposure to organophosphate flame retardant chemicals in the U.S. general population: Data from the 2013-2014 National Health and Nutrition Examination Survey.

作者信息

Ospina Maria, Jayatilaka Nayana K, Wong Lee-Yang, Restrepo Paula, Calafat Antonia M

机构信息

Division of Laboratory Sciences, National Center for Environmental Health, Centers for Disease Control and Prevention, 4770 Buford Hwy, MS F17, Atlanta, GA 30341, USA.

Division of Laboratory Sciences, National Center for Environmental Health, Centers for Disease Control and Prevention, 4770 Buford Hwy, MS F17, Atlanta, GA 30341, USA.

出版信息

Environ Int. 2018 Jan;110:32-41. doi: 10.1016/j.envint.2017.10.001. Epub 2017 Nov 6.

Abstract

BACKGROUND

Use of organophosphate flame retardants (OPFRs) including tris(1,3-dichloro-2-propyl) phosphate, triphenyl phosphate, tris(1-chloro-2-propyl) phosphate, and tris-2-chloroethyl phosphate, in consumer products is on the rise because of the recent phase out of polybrominated diphenyl ether (PBDE) flame retardants. Some of these chemicals are also used as plasticizers or lubricants in many consumer products.

OBJECTIVES

To assess human exposure to these chlorinated and non-chlorinated organophosphates, and non-PBDE brominated chemicals in a representative sample of the U.S. general population 6years and older from the 2013-2014 National Health and Nutrition Examination Survey (NHANES).

METHODS

We used solid-phase extraction coupled to isotope dilution high-performance liquid chromatography-tandem mass spectrometry after enzymatic hydrolysis of conjugates to analyze 2666 NHANES urine samples for nine biomarkers: diphenyl phosphate (DPHP), bis(1,3-dichloro-2-propyl) phosphate (BDCIPP), bis-(1-chloro-2-propyl) phosphate (BCIPP), bis-2-chloroethyl phosphate (BCEP), di-n-butyl phosphate (DNBP), di-p-cresylphosphate (DpCP), di-o-cresylphosphate (DoCP), dibenzyl phosphate (DBzP), and 2,3,4,5-tetrabromobenzoic acid (TBBA). We calculated the geometric mean (GM) and distribution percentiles for the urinary concentrations (both in micrograms per liter [μg/L] and in micrograms per gram of creatinine). We only calculated GMs for analytes with an overall weighted frequency of detection >60%. For those analytes, we also a) determined weighted Pearson correlations among the log10-transformed concentrations, and b) used regression models to evaluate associations of various demographic parameters with urinary concentrations of these biomarkers.

RESULTS

We detected BDCIPP and DPHP in approximately 92% of study participants, BCEP in 89%, DNBP in 81%, and BCIPP in 61%. By contrast, we detected the other biomarkers much less frequently: DpCP (13%), DoCP (0.1%), TBBA (5%), and did not detect DBzP in any of the participants. Concentration ranges were highest for DPHP (<0.16-193μg/L), BDCIPP (<0.11-169μg/L), and BCEP (<0.08-110μg/L). Regardless of race/ethnicity, 6-11year old children had significantly higher BCEP adjusted GMs than other age groups. Females had significantly higher DPHP and BDCIPP adjusted GM than males, and were more likely than males to have DPHP concentrations above the 95th percentile (odds ratio=3.61; 95% confidence interval, 2.01-6.48).

CONCLUSIONS

Our results confirm findings from previous studies suggesting human exposure to OPFRs, and demonstrate, for the first time, widespread exposure to several OPFRs among a representative sample of the U.S. general population 6years of age and older. The observed differences in concentrations of certain OPFRs biomarkers by race/ethnicity, in children compared to other age groups, and in females compared to males may reflect differences in lifestyle and exposure patterns. These NHANES data can be used to stablish a nationally representative baseline of exposures to OPFRs and when combined with future 2-year survey data, to evaluate exposure trends.

摘要

背景

由于近期多溴二苯醚(PBDE)阻燃剂逐步淘汰,包括磷酸三(1,3 - 二氯 - 2 - 丙基)酯、磷酸三苯酯、磷酸三(1 - 氯 - 2 - 丙基)酯和磷酸三(2 - 氯乙基)酯在内的有机磷酸酯阻燃剂(OPFRs)在消费品中的使用正在增加。其中一些化学品还在许多消费品中用作增塑剂或润滑剂。

目的

通过2013 - 2014年美国国家健康与营养检查调查(NHANES)中6岁及以上美国普通人群的代表性样本,评估人类对这些氯化和非氯化有机磷酸酯以及非PBDE溴化化学品的暴露情况。

方法

我们采用固相萃取结合同位素稀释高效液相色谱 - 串联质谱法,在对缀合物进行酶水解后,分析2666份NHANES尿液样本中的9种生物标志物:磷酸二苯酯(DPHP)、双(1,3 - 二氯 - 2 - 丙基)磷酸酯(BDCIPP)、双(1 - 氯 - 2 - 丙基)磷酸酯(BCIPP)、双(2 - 氯乙基)磷酸酯(BCEP)、磷酸二正丁酯(DNBP)、磷酸二对甲苯酯(DpCP)、磷酸二邻甲苯酯(DoCP)、磷酸二苄酯(DBzP)和2,3,4,5 - 四溴苯甲酸(TBBA)。我们计算了尿浓度(以每升微克数[μg/L]和每克肌酐微克数表示)的几何均值(GM)和分布百分位数。我们仅对总体加权检测频率>60%的分析物计算GM。对于这些分析物,我们还a)确定了经log10转换后的浓度之间的加权皮尔逊相关性,以及b)使用回归模型评估各种人口统计学参数与这些生物标志物尿浓度之间的关联。

结果

我们在约92%的研究参与者中检测到BDCIPP和DPHP,89%的参与者中检测到BCEP,81%的参与者中检测到DNBP,61%的参与者中检测到BCIPP。相比之下,我们检测到其他生物标志物的频率要低得多:DpCP(13%)、DoCP(0.1%)、TBBA(5%),并且在任何参与者中均未检测到DBzP。DPHP(<0.16 - 193μg/L)、BDCIPP(<0.11 - 169μg/L)和BCEP(<0.08 - 110μg/L)的浓度范围最高。无论种族/民族如何,6 - 11岁儿童经调整后的BCEP几何均值显著高于其他年龄组。女性经调整后的DPHP和BDCIPP几何均值显著高于男性,并且女性DPHP浓度高于第95百分位数的可能性比男性更大(优势比 = 3.61;95%置信区间,2.01 - 6.48)。

结论

我们的结果证实了先前研究的发现,表明人类暴露于OPFRs,并且首次证明在6岁及以上美国普通人群的代表性样本中广泛暴露于几种OPFRs。观察到的某些OPFRs生物标志物浓度在种族/民族、儿童与其他年龄组以及女性与男性之间的差异可能反映了生活方式和暴露模式的差异。这些NHANES数据可用于建立全国代表性的OPFRs暴露基线,并与未来的两年调查数据相结合,以评估暴露趋势。

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