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1996年至2020年德国人群对紫外线过滤剂二乙氨羟苯甲酰基苯甲酸己酯和水杨酸-2-乙基己酯的暴露增加:德国环境样本库(ESB)24小时尿液样本中的人体生物监测。

Increasing exposure to the UV filters octocrylene and 2-ethylhexyl salicylate in Germany from 1996 to 2020: Human biomonitoring in 24-h urine samples of the German Environmental Specimen Bank (ESB).

作者信息

Bury Daniel, Weber Till, Ebert Katharina E, Zülz Stephanie, Brüning Thomas, Koch Holger M, Kolossa-Gehring Marike

机构信息

Institute for Prevention and Occupational Medicine of the German Social Accident Insurance, Institute of the Ruhr-Universität Bochum (IPA), Bürkle-de-la-Camp-Platz 1, 44789 Bochum, Germany.

German Environment Agency (UBA), Corrensplatz 1, 14195 Berlin, Germany.

出版信息

Environ Int. 2023 Dec;182:108334. doi: 10.1016/j.envint.2023.108334. Epub 2023 Nov 19.

Abstract

The UV filters octocrylene (OC) and 2-ethylhexyl salicylate (EHS) are commonly used in sunscreens and frequently detected in environmental media. However, knowledge on human exposures is scarce. In this human biomonitoring (HBM) study, we analyzed concentrations of exposure biomarkers specific to OC (CPAA, DOCCA, 5OH-OC) and EHS (5OH-EHS, 5oxo-EHS, 5cx-EPS) in 24-h urine samples (n = 420) from the German Environmental Specimen Bank (ESB). These samples were collected from German students (20-29 years; 30 males/30 females per year) between 1996 and 2020 (4-year intervals; collection in winter). We found continuously increasing OC and EHS exposures (Jonckheere-Terpstra; p < 0.001) documented by very few to no samples with concentrations of the most sensitive biomarkers CPAA and 5cx-EPS above the limit of quantification (LOQ) in 1996 (5 % and 0 %, respectively) and reaching 100 % and 93 % above the LOQ in 2016, with median concentrations of 4.79 and 0.071 µg/L, respectively. In 2020, biomarker concentrations slightly decreased to 3.12 µg/L CPAA (97 %>LOQ) and 0.060 µg/L 5cx-EPS (88 %>LOQ). This general trend was confirmed by the other biomarkers, however at lower detection rates. Based on metabolite excretion in the 24-h urine samples and human toxicokinetic data, we calculated maximum daily intakes (DI) of 17 µg/(kg bw * d) OC and 59 µg/(kg bw * d) EHS. Based on a derived no-effect level (DNEL) of 0.8 mg/(kg bw * d), the OC exposures of individuals in our study did not indicate any health risk. Similarly, for EHS all biomarker concentrations were well below the HBM-I values of 12 µg/L 5OH-EHS and 11 µg/L 5cx-EPS. Our data proves the general applicability of specific OC and EHS metabolites for HBM in the general population and shows clearly increasing exposures. Higher (co-)exposures must be expected in populations with increased sunscreen use such as (summer) vacationers, children and outdoor workers.

摘要

紫外线过滤剂二乙氨羟苯甲酰基苯甲酸己酯(OC)和水杨酸2-乙基己酯(EHS)常用于防晒霜中,并且经常在环境介质中被检测到。然而,关于人体暴露的知识却很匮乏。在这项人体生物监测(HBM)研究中,我们分析了德国环境样本库(ESB)提供的24小时尿液样本(n = 420)中特定于OC(CPAA、DOCCA、5OH-OC)和EHS(5OH-EHS、5oxo-EHS、5cx-EPS)的暴露生物标志物的浓度。这些样本采集自1996年至2020年期间(每隔4年;在冬季采集)的德国学生(20 - 29岁;每年30名男性/30名女性)。我们发现OC和EHS的暴露量持续增加(Jonckheere-Terpstra检验;p < 0.001),1996年时,极少有样本(分别为5%和0%)的最敏感生物标志物CPAA和5cx-EPS的浓度高于定量限(LOQ),到2016年,高于LOQ的样本比例分别达到100%和93%,中位数浓度分别为4.79和0.071 μg/L。2020年,生物标志物浓度略有下降,CPAA为3.12 μg/L(97%>LOQ),5cx-EPS为0.060 μg/L(88%>LOQ)。其他生物标志物也证实了这一总体趋势,不过检出率较低。基于24小时尿液样本中的代谢物排泄情况和人体毒代动力学数据,我们计算出OC的最大每日摄入量(DI)为17 μg/(kg bw * d),EHS为59 μg/(kg bw * d)。根据推导的无效应水平(DNEL)为0.8 mg/(kg bw * d),我们研究中个体的OC暴露未显示出任何健康风险。同样,对于EHS,所有生物标志物浓度均远低于HBM - I值,即5OH-EHS为12 μg/L和5cx-EPS为11 μg/L。我们的数据证明了特定的OC和EHS代谢物在一般人群HBM中的普遍适用性,并显示出暴露量明显增加。在防晒霜使用增加的人群中,如(夏季)度假者、儿童和户外工作者,预计会有更高的(共同)暴露量。

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