Urinary carboxylic acid metabolites as possible novel biomarkers of exposures to alkylated polycyclic aromatic hydrocarbons
Urinary carboxylic acid metabolites as possible novel biomarkers of exposures to alkylated polycyclic aromatic hydrocarbons
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尿羧酸代谢物可能作为烷基化多环芳烃暴露的新型生物标志物
DOI：
10.1016/j.envint.2020.106325
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发表时间：
2021
影响因子：
11.8
通讯作者：
Zhu Yifang
中科院分区：
文献类型：
--
作者：
Lin Yan;Gao Xueyao;Qiu Xinghua;Liu Jinming;Tseng Chi-Hong;Zhang Junfeng Jim;Araujo Jesus A.;Zhu Yifang
先前的研究发现，烷基化多环芳烃（烷基-PAH）在石油来源（例如原油及其精炼产品）中比不完全燃烧的热解来源更丰富。虽然未取代的多环芳烃的尿羟基化代谢物已被广泛用作多环芳烃暴露的生物标志物，但关于烷基多环芳烃代谢物的出现的信息很少。在这项研究中，我们在 2014 年至 2017 年夏天在北京度过 10 周之前、期间和之后重复收集的 45 名洛杉矶居民的 314 份尿液样本中检测到了烷基萘 (2-NAPCA) 和烷基菲 (2-PHECA) 的羧酸代谢物。我们发现，从洛杉矶到北京的旅行导致 2-NAPCA 和 2-PHECA 浓度分别增加 348%（95% CI：243 至 485%）和 209%（95% CI：149 至 282%），在参与者返回洛杉矶后恢复到基线水平。北京的 2-PHECA 与羟基菲之间的浓度比（中位数：0.40，IQR：0.27-0.53）显着（p < 0.05）低于洛杉矶（中位数：0.51，IQR：0.32-0.77），洛杉矶拥有超过 5,000 口活跃的油气井。从 2014 年到 2017 年，洛杉矶 2-PHECA 与羟基菲的浓度比每年增加 28.7（95%CI：12.3 至 47.6）%，北京增加 18.6（95%CI：7.9 至 30.3）%/年，这可能是两个城市努力减少热原排放（例如汽车尾气）的结果。这些结果提供了间接证据，支持使用 2-PHECA 与羟基菲的比率作为反映石成源和热成源相对暴露贡献的指数。虽然我们的研究表明尿液中的多环芳烃可能是烷基多环芳烃暴露的新型生物标志物，但未来的外部暴露特征研究有必要进一步验证这些生物标志物。
Previous studies have found that alkylated polycyclic aromatic hydrocarbons (alkyl-PAHs) were more abundant in petrogenic sources (e.g., crude oil and its refined products) than pyrogenic sources of incomplete combustion. While urinary hydroxylated metabolites of unsubstituted PAHs have been widely used as biomarkers of PAHs exposures, little information is available as to the occurrence of alkyl-PAH metabolites. In this study, we have detected carboxylic acid metabolites of alkyl-naphthalene (2-NAPCA) and alkyl-phenanthrene (2-PHECA) in 314 urine samples repeatedly collected from 45 Los Angeles residents before, during, and after they spent ten weeks in Beijing in summers of 2014–2017. We found that traveling from Los Angeles to Beijing led to 348% (95% CI: 243 to 485%) and 209% (95% CI: 149 to 282%) increases in 2-NAPCA and 2-PHECA concentrations, respectively, which returned to baseline levels after participants came back to Los Angeles. The concentration ratio between 2-PHECA and hydroxy-phenanthrenes was significantly (p < 0.05) lower in Beijing (median: 0.40, IQR: 0.27–0.53) than in Los Angeles (median: 0.51, IQR: 0.32–0.77), where more than 5,000 active gas and oil wells were located. From 2014 to 2017, the concentration ratio of 2-PHECA to hydroxy-phenanthrenes increased by 28.7 (95%CI: 12.3 to 47.6) %/yr in Los Angeles and 18.6 (95%CI: 7.9 to 30.3) %/yr in Beijing, likely resulted from both cities’ efforts to reduce pyrogenic emissions (e.g. vehicle exhaust). These results provided indirect evidence supporting the use of 2-PHECA to hydroxy-phenanthrene ratio as an index to reflect the relative exposure contributions from petrogenic and pyrogenic sources. While our study suggested that urinary PAHCAs may be novel biomarkers of exposure to alkyl-PAHs, future studies with external exposure characterization are warranted to further validate these biomarkers.