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研究生:張恆瑞
研究生(外文):Heng-JuiChang
論文名稱:樹脂製造業勞工血液中多溴二苯醚暴露及代謝速率研究
論文名稱(外文):Exposure assessment and metabolic rate of Polybrominated diphenyl ethers(PBDEs) in serum for workers in synthetic resin industry
指導教授:李俊璋李俊璋引用關係
指導教授(外文):Ching-Chang Lee
學位類別:碩士
校院名稱:國立成功大學
系所名稱:環境醫學研究所
學門:醫藥衛生學門
學類:公共衛生學類
論文種類:學術論文
論文出版年:2010
畢業學年度:98
語文別:中文
論文頁數:119
中文關鍵詞:樹脂製造業勞工血液中多溴二苯醚代謝半衰期甲狀腺荷爾蒙
外文關鍵詞:synthetic resin industryworkersserum PBDEshalf-lifethyroid related hormones
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多溴二苯醚(polybrominated diphenyl ethers, PBDEs)是含溴耐燃劑,常用於樹脂、橡膠、電子、建築材?及紡織等產品。環保署自2003?起?管十溴二苯醚為毒性化學物質,2005?起?管五溴及八溴二苯醚。彙整環保署毒性化學物質管?系統之申報資?後發現,國內業者申報PBDEs使用?至2008?仍以樹脂業為最大宗,且依據2007?「樹脂製造及應用產業?工多溴二苯醚??評估研究」結果顯示,樹脂製造業?工於製造過程中??PBDEs情形嚴重,甚至干擾甲?腺素分?,該研究顯示PBDEs與T3/T4比?呈現正相關,也證實T4濃?可能隨著PBDEs濃?上升而下?。然因過去尚未有文獻曾證實高溴?多溴二苯醚確實會對人體具有甲?腺毒性,因此尚需深入研究以證實PBDEs可能產生的危害。但該廠仍依據研究建議於2009年4月14日停止使用PBDEs。
本研究於該廠停止使用PBDEs後,持續監測勞工血液中PBDEs及甲狀腺荷爾蒙濃度,藉此長期追蹤資料,以瞭解勞工血液中PBDEs濃度之降解變化情形,進而探討PBDEs於人體內代謝而由高溴數降解為低溴數之可能性。並藉觀察勞工體內代謝後同源物分布比例的改變,探討該化合物代謝後對人類健康效應的影響程度。本研究依據前期研究之暴露情節嚴重程度篩選20名該廠勞工(其中兩名勞工因個人因素無法配合故退出計畫,實際18名勞工完成全程研究)進行為期6個月之半衰期研究,研究項目包括每月採血進行PBDEs分析及問卷調查,進行四次血液生化及荷爾蒙檢測。研究結果顯示,18名受檢勞工血液中PBDEs以BDE-209、BDE-207、BDE-197、BDE-206、BDE-196等8-10溴之高溴數二苯醚濃度含量較高且為主要同源物。進一步探討高溴數二苯醚在勞工血液中的代謝速率與半衰期,發現其中9名勞工經過6個月後,血液中BDE-209濃度有下降的趨勢,而其餘9名則有持續上升的現象,以一階代謝速率公式估算勞工血液中BDE-209之半衰期並依工作性質區分,分別為行政人員(含司機)約26.0-117.5天,加工課勞工約90-128.3天,製造課勞工約1155.0-3465.0天。此外,由相關性分析結果發現,9名可計算BDE-209半衰期的勞工第一次採樣血液中BDE-209與BDE-207、BDE-206具統計上顯著正相關。經過6個月後,9名勞工血液中的BDE-209與BDE-207、BDE-206、BDE-197及BDE-196皆有統計上的顯著正相關,顯示隨著停止暴露PBDEs的時間愈長,勞工血液中10溴二苯醚降解代謝為較低溴數之二苯醚的現象愈明顯。
由四次荷爾蒙檢測結果顯示,經過6個月後,T4及FT4濃度分布仍有顯著下降的現象(p=0.017、p <0.001),而T3及E2之濃度分布則有顯著上升(p<0.001、p <0.001);若將18名員工以工作部門區分,?發現行政部門員工及加工課操作勞工在甲狀腺荷爾蒙各項指標皆未有統計上的顯著差異,但製造課勞工則發現TSH、T4及FT4濃度有顯著下降。此外,比較9名可計算BDE-209半衰期的作業勞工之四次荷爾蒙檢驗結果發現,各項甲狀腺指標濃度變化的趨勢雖未達統計上的顯著意義,但T4與FT4濃度經過6個月後有顯著下降(p=0.012),而T3及T3/T4濃度則呈顯著上升(p=0.008、p=0.004)。然此結果與96?度發現的影響結論一致。這也說明該廠勞工停止使用10溴二苯醚,其體內的甲狀腺荷爾蒙仍持續受到影響。
本研究結果顯示該工廠雖然已停止使用10溴二苯醚,但部份勞工血液中BDE-209的濃度仍有上升的跡象,說明受檢勞工還有持續暴露的可能性存在,推測可能係該工廠停止PBDE使用後,並未進行整體環境及機台進行清理措施,導致負責製造之勞工仍有暴露的可能性。另外,建議該樹脂製造業勞工應定期作身體健康檢查,特別是甲狀腺相關之荷爾蒙,以確認勞工體內的甲狀腺荷爾蒙干擾是否回復,確保勞工健康。

Polybrominated diphenyl ethers (PBDEs) are blended with polymers which are used in electrical and electronic equipment, plastic products, building materials, and textiles. In Taiwan, Environmental Protection Administration had announced Deca-BDE, Penta-BDE, Octa-BDE as toxic chemicals in 2003 and 2005, respectively. According to registered data, the highest amount of Deca-BDE was used in synthetic resin industry during 2003 to 2008 in Taiwan. Previous studies reported that serum PBDEs of resin industry workers were negatively associated with thyroid hormones T4. In addition, the significantly positive correlation between serum PBDEs and T3/T4 was found. Therefore, this plant declared that they had phased out the PBDEs in their products from April, 2009.
The aims of this longitudinal study are (1) to determine the association between serums PBDEs and thyroid hormone disruption after cease of PBDEs use; (2) to evaluate the metabolic rates and half-lifes of serum PBDEs congeners in workers; (3) to examine the variations of thyroid hormones after cease of PBDEs use.
18 selected workers in a flame retardative resin manufacturing plant were recruited as study subjects. 108 serum samples of workers were collected once a month for six months. The results shows that high brominated diphenyl ethers such as BDE-196, BDE-197, BDE-207, BDE-209 were the dominant congeners for all serum samples. However, we found serum deca-BDE of nine workers showed decreased trend, and the serum deca-BDE of other workers were not decreased significantly. Therefore, we used measured serum PBDEs data of nine workers to calculate metabolic rate and half-life. Apparent half-life for BDE-209 among official workers、process workers and manufacture workers were 26.0-117.5、90-128.3 and 1155-3465 days, respectively. The present study showed that serum BDE-209 levels of nine workers were positively associated with serum levels of BDE-207 and BDE-206. After six months, serum BDE-209 levels of these nine workers were also positively associated with serum levels of BDE-207, BDE-206, BDE-197, BDE-196. Significantly negative association were found between the levels of T4, FT4 with serum PBDEs respectively; otherwise, significantly positive association were found between the levels of T3 with serum PBDEs. We also found the ratio of T3/T4 was significant increased during six months (p<0.001). All results showed that the effects on related thyroid hormones still existed for those PBDEs exposed workers.
This research indicated serum BDE-209 levels were continued elevated in manufactured workers, even thought this resin manufacturing plant had cease to use deca-BDE as flame retardant. Further environment and manufactured machines should be cleaned up to reduce the PBDEs exposure potential of workers. We also suggested that occupational PBDEs exposed workers should regularly examine their thyroid related hormones level.

口試合格證明
摘要i
Abstract iii
致謝v
目錄vii
表目錄x
圖目錄xii
第一章 緒論1
1-1研究緣起1
1-2研究目的3
第二章 文獻回顧4
2-1耐燃劑簡介與應用4
2-2多溴二苯醚基本特性5
2-3多溴二苯醚之排放來源及途徑6
2-3-1室內環境空氣中PBDEs流布6
2-3-2室外環境空氣中PBDEs流布7
2-3-3作業環境空氣中PBDEs濃度分布8
2-4多溴二苯醚之毒性9
2-4-1甲狀腺干擾9
2-4-2神經毒性11
2-4-3其它毒性相關研究12
2-5多溴二苯醚之吸收、代謝與排出12
2-6一般民眾PBDES暴露研究14
2-7PBDES職業暴露相關研究15
2-8各國對多溴二苯醚管制之相關法令18
第三章 材料與方法20
3-1研究架構20
3-2研究對象選取20
3-2-1工廠現況及相關資料說明20
3-2-2樹脂製造業勞工之樣本挑選原則20
3-2-3採樣對象選取及說明21
3-3資料與樣本收集的方法21
3-3-1問卷設計與資料調查方法21
3-3-2時間-活動模式調查22
3-3-3職業病檢查之內容及執行方法22
3-3-4血液採集與生化檢查等生物指標之量測及分析23
3-3-5健康效應指標檢測及分析23
3-4作業勞工血液中多溴二苯醚之量測24
3-4-1樣本前處理方法24
3-4-2樣本測脂方法26
3-4-3樣本分析方法26
3-4-4數據品保品管26
3-5統計分析30
3-6樹脂製造業操作勞工之體內危害物代謝速率評估30
第四章 結果與討論31
4-1受檢員工基本資料31
4-1-1勞工基本資料分布31
4-1-2勞工生活習慣、健康情形及飲食習慣資料分布31
4-2受檢勞工血液生化、荷爾蒙檢查結果32
4-2-1受檢勞工血液生化檢查結果32
4-2-2受檢勞工荷爾蒙檢查結果32
4-3受檢勞工血液中多溴二苯醚分析結果32
4-3-1受檢勞工血液中多溴二苯醚濃度分布32
4-3-2受測勞工血液中多溴二苯醚同源物分布34
4-3-3受測勞工血液中多溴二苯醚代謝速率評估35
4-3-4受測勞工血液荷爾蒙檢查結果36
第五章 結論與建議39
5-1結論39
5-2建議40
參考文獻42
附件一 樹脂製造及應用產業勞工健康調查問卷105
附件二 人體試驗委員會審查通過證明文件116
附件三 臨床試驗同意書117
自述119
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工業材料雜誌,249期,中華民國九十六年。
行政院勞工安全衛生研究所,資源回收業勞工空氣中多溴二苯醚暴露調查研究,中華民國九十六年1月。
行政院環保署環境檢驗所,多溴二苯醚檢測方法—氣相層析/高解析質譜法,NIEA M802.00B,中華民國九十六年5月
行政院環保署毒物管理系統http://flora2.epa.gov.tw/epa/
林翊嘉,廢棄家電及電腦處理業勞工多溴聯苯醚暴露評估研究,國立成功大學/環境醫學研究所/碩士論文,中華民國九十五年七月。
劉家瑋,樹脂製造及應用產業勞工多溴二苯醚暴露評估研究,國立成功大學/環境醫學研究所/碩士論文,中華民國九十七年六月。

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