| 研究生: |
揭佳蕙 Chieh, Chia-Hui |
|---|---|
| 論文名稱: |
成人及兒童於室內外環境中有機磷耐燃劑之暴露評估與生物偵測研究 Study on biomonitoring and exposure assessment of organophosphate flame retardants in indoor and outdoor environment for adults and children |
| 指導教授: |
李俊璋
Lee, Ching-Chang |
| 共同指導: |
張偉翔
Chang, Wei-Hsiang |
| 學位類別: |
碩士 Master |
| 系所名稱: |
醫學院 - 環境醫學研究所 Department of Environmental and Occupational Health |
| 論文出版年: | 2021 |
| 畢業學年度: | 109 |
| 語文別: | 中文 |
| 論文頁數: | 267 |
| 中文關鍵詞: | 有機磷耐燃劑 、多重環境暴露-生物偵測模式 、皮膚擦拭 、暴露評估 、尿液代謝物 |
| 外文關鍵詞: | Organophosphate flame retardant, Multiple exposure-biomonitoring model (MEBM), Skin wipe, Exposure assessment, Urinary metabolites |
| 相關次數: | 點閱:191 下載:0 |
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歐盟於2011年正式公告禁用溴化耐燃劑於電子電器設備,世界各國亦紛紛提出禁用及管制策略,有機磷耐燃劑(Organophosphate flame retardant, OPFRs)隨即被使用作為溴化耐燃劑的主要替代品之一。OPFRs具有穩定性、阻燃及增塑等多項特性,由於OPFRs在使用時係為物理性添加,而非化學鍵合方式添加至各種室內建材及消費性產品中,因此民眾在使用消費性產品、居家用品及工業產品使用時,OPFRs可能經揮發、磨損和轉移釋放到環境當中,導致人體暴露而產生不良健康影響。各國研究亦指出於室內外環境介質(如室內外空氣、灰塵、底泥等)、食物及飲水中皆可量測到高低不等之OPFRs濃度;而人體暴露研究亦發現可經由吸入、灰塵食入及皮膚接觸等途徑暴露OPFRs,且可於人體尿液及血液中檢測出OPFRs之代謝物。近年來,動物毒理學研究指出OPFRs具有弱雌激素及抗雄性素作用,暴露後可能會導致生殖、甲狀腺、神經及腎臟等毒性。此外,生物蓄積研究亦發現OPFRs具生物累積特性。國內至今尚未針對國人,尤其敏感性族群(兒童),調查環境中OPFRs多重暴露途徑與人體生物偵測之相關性。因此,本研究建置多重暴露-生物偵測模式以探討成人及兒童於室內外環境中空氣吸入、灰塵食入、皮膚接觸等多重途徑之暴露特徵,進而探討其與體內OPFRs內在暴露劑量之相關性。
本研究於臺南地區招募60間家戶之主要照顧者及3-12歲孩童,使用過去已完成家戶中室內外空氣及灰塵樣本之採樣分析資料,並採集成人及兒童之皮膚擦拭樣本及早晨第一泡尿液樣本,分別以氣相層析質譜儀分析皮膚擦拭樣本中11種OPFRs濃度,並以液相層析串聯質譜儀分析尿液樣本中5種OPFRs代謝物濃度,整合所有資料解析臺南地區家戶室內外環境介質及皮膚擦拭樣本中OPFRs濃度分布,以及成人與兒童其尿液中OPFRs代謝物濃度分布特性;利用實測值估算成人及兒童經由多重暴露途徑暴露OPFRs之暴露劑量及其內在吸收劑量,並探討兩者之相關性;另以標準化問卷探討影響因子對OPFRs暴露濃度與劑量之影響。最後綜合所有量測結果,利用多重環境暴露-生物偵測模式探討成人及兒童於室內外環境中多重暴露途徑對其體內吸收劑量之貢獻程度,並確認成人及兒童暴露OPFRs之健康風險是否為可接受風險,進而研析一般民眾(尤其兒童)降低OPFRs暴露之參考建議。
本研究結果顯示,家戶於主要活動空間、次要活動空間及室外活動空間之空氣中OPFRs濃度皆以TCIPP濃度最高,其次為TEP、TiBP及TBOEP;家戶灰塵中OPFRs濃度於主要活動空間及次要活動空間中皆以TBOEP濃度最高,其次為TCIPP、TDCIPP及TPHP;成人及兒童皮膚擦拭樣本中OPFRs皆以TBOEP濃度最高,其次為TCIPP及TDCIPP;成人及兒童尿液樣本中5種OPFRs代謝物皆以DPHP濃度最高,其次為BCIPP。以斯皮爾曼等級相關係數分析,顯示室外空氣樣本與兒童皮膚擦拭樣本中TBP、TCEP及TDCIPP呈顯著正相關;兒童皮膚擦拭樣本與室內空氣樣本中TBP及TCP呈顯著正相關,與室內空氣樣本中TCIPP呈顯著負相關;兒童皮膚擦拭樣本與灰塵樣本中TPHP呈顯著正相關;成人及兒童皮膚擦拭樣本中11種OPFRs皆呈顯著正相關;成人及兒童尿液樣本中5種OPFRs代謝物皆呈顯著正相關;成人尿液樣本中BDCIPP與兒童尿液樣本中BCIPP呈顯著正相關;成人尿液樣本中BCIPP與兒童尿液樣本中DBP呈顯著負相關。進一步估算家戶成人、成年男性、成年女性、兒童、男性兒童及女性兒童經由室內空氣吸入、室外空氣吸入、灰塵食入及皮膚接觸途徑之平均暴露劑量,其中以皮膚接觸途徑之劑量最高(7.50×10-4至1.05×100 µg/kg bw/day),以灰塵食入途徑之劑量最低(1.11×10-5至8.45×10-3 µg/kg bw/day)。綜合上述四個暴露途徑,在平均暴露情況下,家戶成人、成年男性、成年女性、兒童、男性兒童及女性兒童經由吸入、灰塵食入及皮膚接觸途徑暴露OPFRs之平均暴露劑量,其中以成年女性之劑量最高(4.78×10-3至1.06×100 µg/kg bw/day),以成年男性之劑量最低(1.80×10-3至5.12×10-1 µg/kg bw/day)。此外,分別估算家戶成人、成年男性、成年女性、兒童、男性兒童及女性兒童經由尿液中OPFRs代謝物濃度推估之體內吸收劑量,其中以成年女性之平均暴露劑量最高(0.658-8.92 µg/kg bw/day),以男性兒童之平均暴露劑量最低(0.872-3.44 µg/kg bw/day)。另外針對成人及兒童體內吸收劑量與各途徑暴露劑量之相關性進行探討,兒童經由尿液中BDCIPP代謝物濃度推估之體內吸收劑量與經室內外空氣吸入及皮膚接觸途徑暴露TDCIPP之每日暴露劑量呈顯著正相關;兒童經由尿液中DBP代謝物濃度推估之體內吸收劑量與經皮膚接觸途徑暴露TBP之每日暴露劑量呈顯著正相關。而成人體內吸收劑量與其對應之各途徑暴露劑量均無呈現顯著相關,可能原因為成人及兒童暴露程度不同所導致。此外,成人及兒童經由多重暴露途徑之暴露劑量對於內在暴露劑量的相對貢獻,結果顯示均以皮膚接觸途徑為主要貢獻,佔成人及兒童內在暴露劑量之93.2%及84.0%之貢獻百分比,且經由WQS迴歸分析探討成人及兒童經由多重暴露途徑暴露OPFRs之外在暴露劑量對其內在暴露劑量之貢獻權重影響結果,亦以皮膚接觸途徑之貢獻比例為最大(44.6%及37.5%),顯示皮膚接觸途徑為成人及兒童對於OPFRs暴露的主要途徑。最後藉由多重環境暴露-生物偵測模式探討多重暴露途徑對尿液中OPFRs代謝物濃度影響及貢獻,大多數成人及兒童之體內吸收劑量來自於本研究探討之暴露途徑的貢獻。至於非致癌風險評估中,本研究成人及兒童於各暴露途徑中11種OPFRs之危害指數(Hazard index, HI)均小於1,預期將不會造成顯著健康危害,表示暴露低於會產生不良反應的閾值,為可接受風險;關於致癌風險評估,成人及兒童經由吸入、灰塵食入及皮膚接觸途徑中暴露TBP、TCEP及TEHP之Risk均小於10-6,表示沒有致癌風險。
綜合上述結果,家戶成人及兒童OPFRs暴露評估中顯示均以皮膚接觸為主要暴露途徑,且經由生物偵測評估結果得知成人及兒童體內OPFRs之內在暴露情形,進而瞭解皮膚接觸途徑為體內吸收劑量之主要貢獻來源。此外,亦藉由多重環境暴露-生物偵測模式得知本研究探討之多重暴露途徑對尿液中OPFRs代謝物濃度影響及貢獻,以尿液代謝物的生物監測數據和多重暴露途徑之每日暴露劑量的相對累積頻率圖得知大多數成人及兒童之體內吸收劑量來自於本研究探討之室內空氣吸入、室外空氣吸入、灰塵食入及皮膚接觸途徑的貢獻。
The objectives of present study are to explore the profile and distribution of organophosphate flame retardant (OPFRs) in the indoor and outdoor environment from Taiwanese resident houses, and to explore the exposure characteristics of OPFRs through multiple pathways (inhalation, ingestion and dermal absorption) for adults and children. TBOEP was the most abundant OPFRs followed by TCIPP in house dust and skin wipe from adults and children. TCIPP was responsible for almost all OPFRs content in indoor and outdoor air from households. The urinary concentrations of adults and children ranged from 0.176 to 0.475 μg/L and 0.192 to 0.683 μg/L, respectively. The estimated average daily exposure dose of Σ11OPFRs for adults and children via inhalation of indoor air, inhalation of outdoor air, ingestion of house dust and dermal absorption were assessed. The results showed that the OPFRs dose from dermal absorption was the highest, and the ingestion of house dust was the lowest. The daily intakes dose of DBP back estimated from urinary metabolite concentrations of children was significantly positively associated with the daily exposure dose of TBP via dermal absorption. The established multiple exposure-biomonitoring model (MEBM) showed that most of the internal dose in adults and children was contributed from multiple exposure pathways via dermal absorption, inhalation of indoor air, inhalation of outdoor air, and ingestion of house dust. The non- carcinogenic and carcinogenic risk assessment showed that the exposure risk is acceptable and cause no significant damage.
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