| 研究生: |
王甜 Wang, Tien |
|---|---|
| 論文名稱: |
近海、野生及養殖魚種有機錫污染調查及一般民眾食入暴露風險評估 The investigation of contamination levels of organotins in the fish and exposure assessment of general population by uptake fish in Taiwan |
| 指導教授: |
李俊璋
Lee, Ching-Chang |
| 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: | 2003 |
| 畢業學年度: | 91 |
| 語文別: | 中文 |
| 論文頁數: | 232 |
| 中文關鍵詞: | 養殖 、非致癌風險評估 、野生 、丁基錫 、苯基錫 、近海 |
| 外文關鍵詞: | cultured fish, hazard index, butyltins, phenyltin, offshore, benthic deep-sea |
| 相關次數: | 點閱:95 下載:4 |
| 分享至: |
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常用於船舶底部及漁具作為抗生物附著塗料或浸泡劑之有機錫化合物主要包括丁基錫(Butyltins, BTs)與苯基錫(Phenyltins, PhTs)。有機錫化合物為已知之內分泌干擾物質(endocrine disruptor chemicals),可能透過水生生物食物鏈進入人體進而影響人體健康。本研究針對台灣民眾經常食用之近海野生及養殖魚種進行有機錫污染含量調查,並完成一般民眾食入暴露風險評估。
本研究以台灣北(碧砂)、中(梧棲)、南(興達)及東部(成功)漁港為對象,分別於夏季及冬季在當地魚市場購買民眾經常食用之浮游、底棲及養殖魚類進行BTs及PhTs分析。所採集魚體先取下肌肉組織經冷凍乾燥後均質,取約2g均質後之肌肉組織樣本先後以1% tropolone-acetone、1% tropolone-benzene、飽和正己烷-乙晴溶液, 10%苯-正己烷進行萃取後除水濃縮,再經烷基化反應後,以GC/MS定量分析。六種有機錫物種包括TBT、DBT、MBT、MPhT、DPhT及TPhT之準確度、精密度(CV值)、基質樣本添加回收率分別為83-92%、2-8%、68-93%。由於有機錫對人體不具致癌性,其對人體之主要危害為免疫毒性,故以危害指標(Hazard index, HI)進行非致癌風險評估。
本研究於台灣地區北、中、南及東部等四大不同採樣點中所採集之浮游、底棲及養殖魚種體內所測得之丁基錫(BTs)與苯基錫類(PhTs)含量分析顯示,所測得之ΣBTs值以浮游魚種之測值(550.4±417.2 μg/kg乾重)遠高於底棲(349.3±207.6 μg/kg 乾重)及養殖魚種(191.2±52.2 μg/kg 乾重); ΣPhTs含量,則以底棲性魚種ΣPhTs含量(875.3±238.1 μg/kg乾重)高於浮游(782.1±358.0 μg/kg乾重)及養殖魚種(549.5±223.9 μg/kg 乾重)。就BTs而言,以興達港所採集的魚種測值含量為最高為622.6±326.2 μg/kg 乾重,其他依序為梧棲港(428.7±466.2 μg/kg 乾重)、成功港(350.7±90.0 μg/kg 乾重)及碧砂港(241.7±89.0 μg/kg 乾重);PhT之含量分析則以梧棲港(843.7±437.0 μg/kg 乾重)>興達港(800.6±204.3 μg/kg 乾重)>碧砂港(768.3±231.9 μg/kg 乾重)及成功港(645.6±259.5 μg/kg 乾重),顯示台灣地區魚類均受到BTs及PhTs排放之TPhT影響。此外,所有魚體內之BTs與PhT含量分布亦受到季節性因子影響,TBT以冬季測值高(386.7±372.3 μg/kg乾重)於夏季(108.6±49.4 μg/kg 乾重);TPhT則以夏季(445.7±210.3 μg/kg 乾重)測值含量高冬季(277.1±149.9 μg/kg乾重),且經統計分析結果顯示具統計意義(p value <0.05);而降解指數之BDI及PhDI運算分析結果與有機錫呈現季節性變化趨勢相同,BTs則以夏季之BDI>1與冬季PhDI>1,TBT於夏季已明顯地降解成毒性較低之二丁基錫與單丁基錫,此外,由浮游、底棲及養殖魚種肌肉組織中所測得之TBT及TPhT含量,求得全年平均暴露濃度後代入美國環保署所公告建立之暴露劑量及危害指標公式運算後,求得TBT與TPhT兩物種之暴露劑量於30年至70年間則界於0.2-0.3μg/kg/day,危害指標(HI)均小於1(0.3-0.9),顯示一般民眾終其一生食入該些魚獲產品並不會對人體產生不良健康效應。
Tritbutyltin and triphenyltin (TBT and TPhT) are used as antifouling paints owing to their strong biocidal activity toward the aquatic organisms such as mollusks. Many studies have showed TBT and TPhT are endocrine disruptors which at very low concentration (1 ng/L in water) will cause “imposex”, the imposition of the male characteristics in females of some gastropods. Organotin compounds can also enter the food chain through bioaccumulation of marine organisms destined for human consumption, such as oyster, farmed salmon, mussels, calms. This study was conducted to determine the concentration of butyltins(BTs)and phenyltins(PhTs)in benthic, offshore and cultured fish in Taiwan in order to understand current contamination levels. Finally, the analytical data and fish uptake data were used to estimate the non-carcinogenic effects expressed as hazard index (HI) for general human population.
Narrow barred Spanish mackerel(Scomberomorus commerson), red porgy (Pagrus major), dentex tumifron(Yellowback sea-bream)and milkfish (Chanos chanos)were collected from fishery markets of the northern, southern, eastern and central Taiwan. The organotins in fish were analyzed following the method developed by Iwata et al. with slight modification. The muscle of fish was dried by lyophilization and extract with 0.1% trpolone-acetone, 0.1% trpolone- benzene and hexane saturated acetonitrile. The extract was hexylated with hexylmagnesium bromide as Grignard reagent. The derivative was transferred to 10% benzene-hexane and then passed through Florisil column with 10% benzene-hexane for clean up. A GC/MS was used for organotins determination. The accuracy and precision(CV value)of the method were ranged from 83 to 92% and 2 to 8%, respectively. The extraction efficiency of spiked standard in sample were ranged from 68 to 93 %. Due to the immunotoxicological effect of organotin compounds on human, the analyzed data and uptake data of fish was used to estimate the noncarcinogenic risk of general population with hazard index.
The amount of organotin compounds such as butyltin ﹝ΣBTs:TBT, DBT, MBT﹞and phenyltins﹝ΣPhTs:TPhT, DPhT, MPhT﹞in fish from the northern(Bi-Sa), central(Wu-chi), eastern (Cheng-Kang) and southern(Shin-Da) Taiwan fishery markets varied with season and location. High values of ΣBTs(mainly TBT, 409.4±316.7 μg/kg, dry weight)at Shin-Da and low values of ΣPhTs(mainly TPhT, 293.7±115.4 μg/kg, dry weight)were found during winter (January 2002)at Cheng Kang, while high amount of ΣPhTs(mainly TPhT, 396.3±124.9 μg/kg, dry weight) at Bi-Sa and low ΣBTs(mainly TBT, 125.3±66.3 μg/kg, dry weight)were found during summer(August 2002). The data shows that the concentrations of BTs in fish at summer were lower than at winter due to the higher degradtion of butyltins was happened by microorganism and UV light in summer. At the lower trophic levels, phenyltin concentrations were higher in benthic species(Pagrus major, yellowback sea-bream), while butyltin concentrations were higher in inshore species(Scombermorous , Caesio caerulaurea), this is may indicates that TBT is passed on primarily via the water, while TPhT is passed on to a larger extend via the sediment. To compare the offshore species and maricultured species revealed the higher contents of OTCs(ΣBTs+ΣPhTs)in muscle of fish(offshore species, 1332.5 μg/kg, dry weight)and lower values in cultured fish(740.7 μg/kg, dry weight)might indicated that the organotion pollution problem in Taiwan is more serious in offshore coast compared with mariculture sites, where the fish live. Given these results, on the basis of calculated tolerable daily intake levels of tributyltin and triphenyltin are lower than the tolerable limits(0.1-0.2 μg/kg bw/day) and the hazard index(HI)are lower than 1. We concluded that the levels of organotin compounds in the marine products in fishery market of Taiwan were not sufficiently high to have any immunological toxic effect on human health.
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