Nicholas School of the Environment, Duke University, Durham, NC, United States.
Nicholas School of the Environment, Duke University, Durham, NC, United States.
Environ Int. 2018 Jul;116:176-185. doi: 10.1016/j.envint.2018.04.013. Epub 2018 Apr 21.
Following the phase-out of polybrominated diphenyl ethers (PBDEs), organophosphate esters (OPEs) have been increasingly used in consumer products and building materials for their flame retardant and plasticizing properties. As a result, human exposure to these chemicals is widespread as evidenced by common detection of their metabolites in urine. However, little is known about the major exposure pathways, or factors that influence children's exposure to OPEs. Furthermore, little data is available on exposure to the novel aryl OPEs.
To examine predictors of children's internal exposure, we assessed relationships between OPEs in house dust and on hand wipes and levels of their corresponding metabolites in paired urine samples (n = 181). We also examined associations between urinary metabolites and potential covariates, including child's age and sex, mother's educational attainment and race, and average outdoor air temperature.
Children aged 3 to 6 years provided urine and hand wipe samples. Mothers or legal guardians completed questionnaires, and a house dust sample was taken from the main living area during home visits. Alkyl chlorinated and aryl OPEs were measured in dust and hand wipes, and composite urine samples were analyzed for several metabolites.
Tris(2-chloroethyl) phosphate (TCEP), tris(2-chloroisopropyl) phosphate (TCIPP), tris(1,3-dichloro-2-propyl) phosphate (TDCIPP), 2-ethylhexyl diphenyl phosphate (EHDPHP), triphenyl phosphate (TPHP), and 2-isopropylphenyl diphenyl phosphate (2IPPDPP) were detected frequently in hand wipes and dust (>80%), indicating that these compounds were near-ubiquitous in indoor environments. Additionally, bis(1-chloro-2-propyl) 1-hydroxy-2-propyl phosphate (BCIPHIPP), bis(1,3-dichloro-2-propyl) phosphate (BDCIPP), diphenyl phosphate (DPHP), mono-isopropyl phenyl phenyl phosphate (ip-PPP), and mono-tert-butyl phenyl phenyl phosphate (tb-PPP) were detected in >94% of tested urine samples, signifying that TESIE participants were widely exposed to OPEs. Contrary to PBDEs, house dust OPE concentrations were generally not correlated with urinary OPE metabolite levels; however, hand wipe levels of OPEs were associated with internal dose. For example, children with the highest mass of TDCIPP on hand wipes had BDCIPP levels that were 2.73 times those of participants with the lowest levels (95% CI: 1.67, 4.48, p < 0.0001). Of the variables examined, hand wipe level was the most consistent and strongest predictor of OPE urinary metabolite concentrations. Outdoor air temperature was also a significant predictor of urinary BDCIPP concentrations, with a 1 °C increase in temperature corresponding to a 4% increase in urinary BDCIPP (p < 0.0001).
OPE exposures are highly prevalent, and data provided herein further substantiate hand-to-mouth contact and dermal absorption as important pathways of OPE exposure, especially for young children.
随着多溴二苯醚(PBDEs)的逐步淘汰,有机磷酸酯(OPEs)因其阻燃和增塑性能而在消费品和建筑材料中得到了越来越多的应用。因此,由于这些化学物质在尿液中的代谢物普遍存在,人类接触这些化学物质的情况很普遍。然而,人们对主要暴露途径或影响儿童接触 OPEs 的因素知之甚少。此外,关于新型芳基 OPEs 的暴露数据也很少。
为了研究儿童体内暴露的预测因素,我们评估了房屋灰尘和手上擦拭物中的 OPEs 与配对尿液样本中相应代谢物之间的关系(n=181)。我们还研究了尿液代谢物与潜在混杂因素(包括儿童年龄和性别、母亲的教育程度和种族以及室外平均气温)之间的关联。
3 至 6 岁的儿童提供了尿液和手上擦拭物样本。母亲或法定监护人完成了问卷调查,在家庭访问期间从主要居住区域采集了房屋灰尘样本。对灰尘和手上擦拭物中的烷基氯化和芳基 OPEs 进行了测量,并对复合尿液样本进行了几种代谢物的分析。
三(2-氯乙基)磷酸酯(TCEP)、三(2-氯异丙基)磷酸酯(TCIPP)、三(1,3-二氯-2-丙基)磷酸酯(TDCIPP)、2-乙基己基二苯基磷酸酯(EHDPHP)、磷酸三苯酯(TPHP)和 2-异丙基苯基二苯基磷酸酯(2IPPDPP)在手上擦拭物和灰尘中频繁检测到(>80%),表明这些化合物在室内环境中几乎无处不在。此外,1-羟基-2-丙基双(1-氯-2-丙基)磷酸酯(BCIPHIPP)、双(1,3-二氯-2-丙基)磷酸酯(BDCIPP)、磷酸二苯酯(DPHP)、单异丙基苯基苯基磷酸酯(ip-PPP)和单叔丁基苯基苯基磷酸酯(tb-PPP)在>94%的测试尿液样本中均有检测到,这表明 TESIE 参与者广泛接触了 OPEs。与 PBDEs 不同,房屋灰尘中的 OPE 浓度通常与尿液 OPE 代谢物水平没有相关性;然而,手上擦拭物中的 OPE 水平与体内剂量有关。例如,手上擦拭物中 TDCIPP 含量最高的儿童,其 BDCIPP 水平是含量最低的儿童的 2.73 倍(95%CI:1.67,4.48,p<0.0001)。在所检查的变量中,手上擦拭物水平是 OPE 尿液代谢物浓度最一致和最强的预测因素。室外空气温度也是 BDCIPP 尿液浓度的一个显著预测因素,温度每升高 1°C,尿液中的 BDCIPP 就会增加 4%(p<0.0001)。
OPE 暴露非常普遍,本文提供的数据进一步证实了手口接触和皮肤吸收是 OPE 暴露的重要途径,尤其是对幼儿而言。