Background and aim

Metofluthrin, profluthrin, tefluthrin, and transfluthrin are pyrethroid (PYR) insecticides increasingly used to control mosquitoes, flies, and moths in households and public places (hygiene-PYRs). Currently, there is limited data available concerning exposure to these novel hygiene-PYRs. The goal of this study was to monitor exposure to these hygiene-PYRs by analysing their urinary metabolites and to investigate the temporal and seasonal trends in the concentrations of these metabolites.

Methods

First morning urine samples were obtained from 50 Japanese children (four-six years old) in October of 2006, 2011, and 2015 (total = 150 children) in order to investigate temporal trends. Additionally, first-morning urine samples were collected from 44 three-year-old children in August–September of 2012 (summer) and in February of 2013 (winter) to investigate seasonal differences. The urinary concentrations of 2,3,5,6-tetrafluorobenzyl alcohol (FB-Al; a specific metabolite of transfluthrin), 4-methyl-2,3,5,6-tetrafluorobenzyl alcohol (CH₃-FB-Al; a common metabolite of tefluthrin and profluthrin), 4-methoxymethyl-2,3,5,6-tetrafluorobenzyl alcohol (CH₃OCH₂-FB-Al; a specific metabolite of metofluthrin), and 2,3,5,6-tetrafluoro-1,4-benzenedimethanol (HOCH₂-FB-Al; a common metabolite of metofluthrin, tefluthrin, and profluthrin) were measured using GC-MS/MS.

Results

For the investigated years, rapid increases in the detection rates of the hygiene-PYR metabolites were observed. In 2015, FB-Al was identified in 64% of the samples, CH₃-FB-Al in 46%, CH₃OCH₂-FB-Al in 50%, and HOCH₂-FB-Al in 83%. Significant increasing trends were found for the concentrations of all hygiene-PYR metabolites from 2006 to 2015 (Jonckheere-Terpstra test, p < 0.001). The concentrations of FB-Al and CH₃OCH₂-FB-Al were higher in summer than in winter (Mann Whitney-U test, p < 0.05).

Conclusions

These findings suggest that, in Japanese children, exposure to hygiene-PYRs has increased over the past decade, and that children are exposed to higher levels of hygiene-PYRs in summer than in winter.

中文翻译：

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日本儿童新颖的，习惯使用的拟除虫菊酯的十年时间趋势（2006-2015年）和尿中代谢物浓度的季节性差异。

背景和目标

Metofluthrin，profluthrin，tefluthrin和transfluthrin是拟除虫菊酯（PYR）杀虫剂，越来越多地用于控制家庭和公共场所的蚊子，苍蝇和蛾子（卫生PYR）。当前，关于这些新型卫生PYR暴露的可用数据有限。这项研究的目的是通过分析其尿中代谢物来监测这些卫生-PYRs的暴露情况，并调查这些代谢物浓度的时间和季节趋势。

方法

为了调查时间趋势，分别于2006年，2011年和2015年10月从50名日本儿童（四岁，六岁）获得了第一天早上的尿液样本（总计= 150名儿童）。此外，在2012年8月至9月（夏季）和2013年2月（冬季）从44名三岁儿童中收集了第一时间的尿液样本，以调查季节性差异。尿液中的2,3,5,6-四氟苄醇（FB-Al;特氟菊酯的特定代谢产物），4-甲基-2,3,5,6-四氟苄醇（CH ₃ -FB-Al;常见氟替林和普罗氟汀的代谢产物），4-甲氧基甲基-2,3,5,6-四氟苄醇（CH ₃ OCH ₂ -FB-Al;甲氟蝶呤的特定代谢产物）和2,3,5,6-四氟-1 ，4-苯二甲醇（HOCH₂ -FB-Al；使用GC-MS / MS测定了甲胃氟灵，替氟菊酯和普鲁氟灵的常见代谢产物）。

结果

在过去的几年中，人们观察到了卫生PYR代谢物的检出率迅速提高。2015年，在64％的样品中鉴定出FB-Al，在46％的样品中鉴定出CH ₃ -FB-Al，在50％的样品中鉴定出CH ₃ OCH ₂ -FB-Al，在83％的样品中鉴定出HOCH ₂ -FB-Al。从2006年到2015年，所有卫生PYR代谢产物的浓度都有显着增加的趋势（Jonckheere-Terpstra检验，p  <0.001）。夏季，FB-Al和CH ₃ OCH ₂ -FB-Al的浓度高于冬季（Mann Whitney- U检验，p  <0.05）。

结论

这些发现表明，在过去的十年中，日本儿童中暴露于卫生PYR的比例有所增加，并且与冬季相比，夏季儿童暴露于较高水平的卫生PYR。