環境用藥係指使用於環境衛生、污染防治用藥等，依其所使用之濃度及使用方式分為環境用藥原體、一般環境用藥與特殊環境用藥。由於環境用藥施用地點包括公共場所如社區、公園、學校與居家室內場所，與民眾活動範圍十分接近，造成民眾暴露機會增加，其施作安全與環境殘留成為公共衛生重要議題。研究目的包括(1)建立環境用藥於環境介質水體、植物體與個人空氣暴露前處理方法與超高效液相層析串聯式質譜儀(UHPLC-MS/MS)分析方法；(2)探討環境用藥於水體與植物體殘留量；(3)執行環境用藥噴藥工人健康風險評估。
為釐清噴藥前後水體與植物體中環境用藥殘留量與評估噴藥工人健康風險，本研究於2019年6-9月間配合內湖、北投、新莊、台南與高雄等五個地區登革熱防疫工作，採集噴藥前一天、噴藥中、噴藥後三小時、後一天與後一週的水體與植物體樣本分析。水體前處理使用HLB (hydrophilic-lipophilic balance)固相萃取膜進行萃取與淨化；植物體前處理則使用高葉綠素農藥快速萃取套組 (fast pesticide extraction-chlorophyll, FaPEx-CHL)，以乙腈溶液含1%醋酸進行萃取；個人空氣樣本則以ACN做為脫附劑，超音波震盪30分鐘；尿液檢體檢測環境用藥原型物及氧化壓力生物指標。並依據個人空氣樣本數據進一步使用蒙地卡羅進行不確定性分析，計算呼吸暴露量 (ADDRE)、安全限值 (margin of safety, MOS)與危害指數 (hazard index, HI)，以執行噴藥工人健康風險評估。
分別採集水體、植物體、個人空氣樣本與尿液樣本26、32、13與17件。結果顯示，水體多於噴藥後一週檢出7種環境用藥有效成份包含益達胺、安丹、協力精、陶斯松、治滅寧、第滅寧與依酚寧，但檢出與噴灑藥劑無關，可能與公園周遭有其他目的施藥有關。植物體多於噴藥時與噴藥後一天檢出7種環境用藥有效成份包含亞特松、協力精、賽洛寧、賽滅寧、亞滅寧、治滅寧與第滅寧，除治滅寧可能與當地居民使用居家環境用藥或農藥因而檢出，其餘6種檢出環境用藥皆與施用藥劑有關。
個人空氣樣本檢出8種環境用藥有效成份包含亞特松、協力精、陶斯松、賽滅寧、賽酚寧、百滅寧、治滅寧與第滅寧，檢出環境用藥皆與施用藥劑有關。北投噴藥工人尿中第滅寧原型物濃度2811.52 μg /g creatinine，其尿中8-OHdG濃度為70.42 μg /g creatinine，工人噴藥過程是否造成氧化壓力增加，未來仍需更多樣本數支持。
使用蒙地卡羅進行不確定性分析以評估噴藥工人健康風險，結果顯示MOS值皆大於100且HI小於1，表示噴藥過程僅考慮呼吸暴露途徑未達顯著風險，但仍建議噴藥工人施藥時應穿戴個人防護具，對於一般民眾應避免接近噴藥點以降低環境用藥對人體健康危害。

Environmental agents means the following types of chemical agents or microbial preparations used for environmental sanitation, and which are distinguished as technical grade environmental agents, general use environmental agents, and restricted use environmental agents. The application safety and environmental residues of environmental agents has become an important public health issue because of the vicinityto the public places such as community, parks, schools and indoor places. The objectives of this study was to (1) establish pretreatment methods for environmental agents in water, plant and personal air sample and analytical method in ultra high performance liquid chromatography tandem mass spectrometer (UHPLC-MS/MS)；(2) explore the environmental residues in water and plant, and (3) perform health risk assessment for spray workers.
We collected samples of water and plant during the environmental agent application for dengue prevention in five areas including Neihu, Beitou, Tainan, Xinzhuang and Kaohsiung. In order to study environmental residues in environmental media, 5 sampling times were selected including before-, during-, 3 hours after-, 1 day after- and 1 week after- the spraying. The pretreatment methods were hydrophilic-lipophilic balance (HLB), fast pesticide extraction-chlorophyll (FaPEx-CHL) and sonication for water, plant, and personal air samples. We analyzed the parent compound of environmental agents and biomarkers of oxidative stress in urine. Moreover, we conducted health risk assessment to calculate average daily dose (ADDRE), margin of safety (MOS), and hazard index (HI) using the Monte Carlo simulation method.
We collected samples of water (n=26), plant (n=32), personal air sample (n=13), and urine (n=17). A total of 7 environmental agents ingredients were detected in water samples including imidacloprid, propoxur, piperonyl butoxide, chlorpyrifos, tetramethrin, deltamethrin, and etofenprox. However, all of the effective ingredients were not related to spraying proess. A total of 7 environmental agents ingredients were detected in plant samples including pirimiphos-methyl, piperonyl butoxide, λ- cyhalothrin, cypermethrin, α-cypermethrin, tetramethrin and deltamethrin. All of the effective ingredients were related to spraying proess, except for tetramethrin.
A total of 8 environmental agents ingredients were detected in personal air samples including pirimiphos-methyl, piperonyl butoxide, chlorpyrifos, cypermethrin, cyphenothrin, permethrin, tetramethrin, and deltamethrin. All of the effective ingredients were related to spraying proess. For workers in Beitou, the urinary level of deltamethrin was 2811.52 μg/g creatinine and 8-OHdG level was 70.42 μg/g creatinine. Further study with a larger sample size is needed to explore the association between spray process and oxidative stress.
The results of health risk assessment showed that MOS was higher than 100 and HI less than 1 indicating no potential risk for workers. We recommended that workers should wear personal protective equipment during spraying and for general population should leave away from spraying exposure.
We collected samples of water and plant during the environmental agent application for dengue prevention in five areas including Neihu, Beitou, Tainan, Xinzhuang and Kaohsiung. In order to study environmental residues in environmental media, 5 sampling times were selected including before-, during-, 3 hours after-, 1 day after- and 1 week after- the spraying. The pretreatment methods were hydrophilic-lipophilic balance (HLB), fast pesticide extraction-chlorophyll (FaPEx-CHL) and sonication for water, plant, and personal air samples. We analyzed the parent compound of environmental agents and biomarkers of oxidative stress in urine. Moreover, we conducted health risk assessment to calculate average daily dose (ADDRE), margin of safety (MOS), and hazard index (HI) using the Monte Carlo simulation method.
We collected samples of water (n=26), plant (n=32), personal air sample (n=13), and urine (n=17). A total of 7 environmental agents ingredients were detected in water samples including imidacloprid, propoxur, piperonyl butoxide, chlorpyrifos, tetramethrin, deltamethrin, and etofenprox. However, all of the effective ingredients were not related to spraying proess. A total of 7 environmental agents ingredients were detected in plant samples including pirimiphos-methyl, piperonyl butoxide, λ- cyhalothrin, cypermethrin, α-cypermethrin, tetramethrin and deltamethrin. All of the effective ingredients were related to spraying proess, except for tetramethrin.
A total of 8 environmental agents ingredients were detected in personal air samples including pirimiphos-methyl, piperonyl butoxide, chlorpyrifos, cypermethrin, cyphenothrin, permethrin, tetramethrin, and deltamethrin. All of the effective ingredients were related to spraying proess. For workers in Beitou, the urinary level of deltamethrin was 2811.52 μg/g creatinine and 8-OHdG level was 70.42 μg/g creatinine. Further study with a larger sample size is needed to explore the association between spray process and oxidative stress.
The results of health risk assessment showed that MOS was higher than 100 and HI less than 1 indicating no potential risk for workers. We recommended that workers should wear personal protective equipment during spraying and for general population should leave away from spraying exposure.

摘要 I
Abstract III
第一章 緒論 1
1.1 前言 1
1.2 環境用藥使用量及其用途資料蒐集 2
1.3 本研究使用環境用藥基本特性簡介 6
1.4 研究目標 10
第二章 文獻回顧 12
2.1 水體環境用藥前處理方法開發 12
2.2 植物體中環境殘留量濃度回顧 15
2.3 國內外空氣中環境用藥前處理與濃度研究 17
2.4 國外農藥暴露與尿液原型物研究 20
2.5 氧化壓力生物指標 22
第三章 材料與方法 28
3.1 材料 28
3.2 藥品 29
3.3 標準溶液配置 31
3.4 分析儀器 33
3.5 建立環境用藥於超高效液相層析串聯式質譜儀分析方法 33
3.6 品保/品管與樣本定量 35
3.7 水體、植物體與個人空氣樣本前處理方法開發 36
3.8 採樣規劃與實地採樣 38
3.9 尿液中肌酸酐與環境用藥原型物分析 42
3.10 尿液中氧化壓力分析 43
3.11 噴藥工人健康風險評估 45
第四章 結果與討論 48
4.1 建立UHPLC-MS/MS上機分析方法 48
4.2 環境用藥於水體中方法表現 52
4.3 環境用藥於植物體方法表現 59
4.4 建立個人空氣暴露前處理方法 66
4.5 分析方法確效總結 75
4.6 環境用藥水體實地採樣結果 76
4.6.1 噴灑藥劑 76
4.6.2 實地採樣樣本總數 77
4.6.3 噴藥工人基本特性 78
4.7 環境用藥環境殘留量採樣結果 80
4.7.1 環境用藥水體實地採樣結果 80
4.7.2 環境用藥植物體實地採樣結果 87
4.7.3 環境用藥噴藥工人個人空氣暴露結果 90
4.7.4 尿液中環境用藥原型物分析 92
4.7.5 噴藥工人尿中氧化壓力濃度結果 94
4.8 執行環境用藥噴藥工人健康風險評估 100
第五章 結論與建議 104
參考文獻 106
附 錄 116
附錄一 環境用藥之化學結構式 117
附錄二 環境用藥於標準品 100 μg/L UHPLC-MS/MS 層析圖譜 121
附錄三 環境用藥於XAD-2、水體與植物體 1 μg/L UHPLC-MS/MS 層析圖譜 125

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安全資料表
百滅寧：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P026_2016_v1.pdf.
亞滅寧：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P089_2016_v1.pdf.
賽洛寧：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P373_2016_v1.pdf.
陶斯松：http://ghs.baphiq.gov.tw/images/upload/msds/GHS_SDS_P007_2013v2.pdf
撲滅松：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P101_2016_v1.pdf.
亞特松：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P355_2016_v1.pdf.
馬拉松：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P018_2016_v1.pdf.
安丹：http://ghs.baphiq.gov.tw/images/upload/msds/GHS_SDS_P106_2013v2.pdf.
協力精：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P365_2016_v1.pdf.
第滅寧: http://www.chia-tai.com.tw/MSDS/76.pdf.
賽滅寧：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P401_2016_v1.pdf.
亞培松：http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P152_2016_v1.pdf.
芬化利: http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P016_2016_v1.pdf.
畢芬寧: http://ghs.baphiq.gov.tw/images/upload/msds/SDS_P041_2016_v1.pdf.
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衛生福利部食品及藥物管理署: https://www.fda.gov.tw/TC/index.aspx.
美國國家衛生研究院: https://www.nih.gov/
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行政院農業委員會動植物防疫檢疫局: https://pesticide.baphiq.gov.tw/web/briefDetailView.aspx?sn=15.
環境用藥簡介及管理: https://www.tcsb.gov.tw/fp-107-360-14bbe-1.html.
環保署毒物及化學物質局: https://www.tcsb.gov.tw/mp-1.html.
美國國家衛生研究院: https://www.nih.gov/