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利用液相色谱-高分辨质谱法对佛兰芒青少年尿液中新兴关注污染物进行全面可疑物筛查。

Comprehensive suspect screening for the identification of contaminants of emerging concern in urine of Flemish adolescents by liquid chromatography high-resolution mass spectrometry.

机构信息

Toxicological Centre, University of Antwerp, Antwerp, Belgium.

Toxicological Centre, University of Antwerp, Antwerp, Belgium.

出版信息

Environ Res. 2022 Nov;214(Pt 3):114105. doi: 10.1016/j.envres.2022.114105. Epub 2022 Aug 15.

DOI:10.1016/j.envres.2022.114105
PMID:35981609
Abstract

The increasing human exposure to contaminants of emerging concern (CECs) cannot be fully assessed by targeted biomonitoring methods alone as these are limited to a subset of known analytes. On the contrary, suspect screening approaches based on liquid chromatography coupled to high-resolution mass spectrometry (LC-HRMS) allow the simultaneous detection of a high number of CECs and/or their (predicted) metabolites leading to a more comprehensive assessment of possible human exposure to these compounds. Within this study, 83 urine samples of Flemish adolescents (47 males, 36 females) collected in the frame of the 4th cycle of the Flemish Environment and Health Study (FLEHS IV) were selected with the aim of including a high and a low exposure group based on the overall exposure of 45 known contaminants. Samples were analyzed using a previously developed method involving a suspect screening approach to annotate CECs and their metabolites. The applied suspect list contained a total of >12,500 CECs and their known and predicted metabolites resulting from metabolization reactions, such as hydroxylation, glucuronidation and methylation. In total, 63 compounds were annotated at a confidence level of 3 or better, with most of the detected compounds not included in current biomonitoring programs. 5 out of the 63 compounds could be assigned with confidence level 2. Five compounds could unequivocally be identified (confidence level 1) through the comparison with reference standards. Personal care products were the main detected compound class (42% of detected compounds). Additionally, a detailed literature search indicated potential toxic effects for several of the detected CECs. Lastly, in the urine samples, a significantly higher number (p < 0.05) of compounds was detected in the high exposure group as opposed to the low exposure group. This difference could only be observed between high and low exposure load samples of female participants (p < 0.01).

摘要

由于目标生物监测方法仅限于已知分析物的一部分,因此,仅通过这些方法无法充分评估人类接触新兴关注污染物(CECs)的情况。相反,基于液相色谱与高分辨率质谱(LC-HRMS)的可疑筛选方法可以同时检测大量的 CECs 和/或它们的(预测)代谢物,从而更全面地评估这些化合物对人类可能产生的暴露情况。在本研究中,从 Flemish 环境与健康研究(FLEHS IV)第四轮中收集的 83 份 Flemish 青少年尿液样本(47 名男性,36 名女性)被选中,目的是根据 45 种已知污染物的总体暴露情况,纳入高暴露组和低暴露组。这些样本使用一种先前开发的方法进行分析,该方法采用可疑筛选方法来注释 CEC 及其代谢物。应用的可疑清单包含了超过 12500 种 CEC 及其已知和预测代谢物,这些代谢物是由羟化、葡萄糖醛酸化和甲基化等代谢反应产生的。在置信水平为 3 或更高的情况下,共注释了 63 种化合物,其中大部分检测到的化合物未包含在当前的生物监测计划中。在置信水平为 2 的情况下,有 5 种化合物可以被分配。有 5 种化合物可以通过与参比标准进行比较,被明确鉴定(置信水平 1)。个人护理产品是主要检测到的化合物类别(42%的检测化合物)。此外,详细的文献检索表明,检测到的一些 CECs 可能具有潜在的毒性作用。最后,在尿液样本中,高暴露组中检测到的化合物数量明显高于低暴露组(p<0.05)。这种差异仅在高暴露组和低暴露组的女性参与者之间观察到(p<0.01)。

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