臺灣博碩士論文加值系統

汞為人體有害重金屬，而人體汞曝露的主要來源係經由魚類的攝取，故而，了解市售水產品和其加工製品的汞含量，再以此資料基礎進一步分析探討汞攝入之風險，遂為近年頗受重視之課題。因此，本研究嘗試建立適當之魚肉汞含量測定方法，並分析調查市售水產品的汞含量，並據以推估攝取魚類之汞風險，以為後續標準訂定和消費者攝食之參考。結果顯示，以微波消化儀及冷蒸氣汞螢光光譜儀進行檢測。微波消化條件以800W，200℃，每次八管分解瓶，添加2 mL過氧化氫於硝酸中輔助消化，並加熱排除干擾物，再進入汞分析儀測定，測定時添加7%還原劑，可得最適之汞含量分析結果。實驗以油魚和鱰魚進行基質添加試驗，分別添加5 ppb 及 10 ppb汞，其回收率分別為94.1±1.9%及 92.2±4.3%，進一步以標準參考物質DORM-4及BCR-463驗證能力、回收率，測定值分別是0.397±0.017 ppm及2.83±0.07 ppm，均符合驗證範圍，顯示此方法測定汞有良好的準確度。而方法偵測極限與定量極限則分別為0.0039 ppb及0.013 ppb。
以建立之汞含量分析方法，檢測市售23種水產品，共計211件樣品。結果發現，全部樣品均符合國內規定之限量範圍，其中迴游性大型魚類，鯊魚、油魚、旗魚等平均含汞量分別為0.647 ppm、0.619 ppm和0.556 ppm，均大於0.5 ppm，屬最高汞魚類。而鮪魚及鱰魚的汞含量較低，分別為0.204 ppm 及0.126 ppm。其餘中小型魚類及淡水養殖水產品汞含量分別為0.084 ppm、0.014 ppm ，均屬中、低汞魚類。加工製品方面分魚鬆、魚罐及魚卵類，汞含量分佈分別為0.05~5.45 ppm、0.028~0.079 ppm、0.002~0.008 ppm，以魚鬆的檢測值最高，魚鬆又區分為未標示魚鬆、旗魚鬆、鮪魚鬆及鮭魚鬆，除了鮭魚鬆外，其餘各種魚鬆平均總汞值均超過0.5 ppm。惟實驗抽選樣本檢測甲基汞與總汞比例，以評估風險假設之合理性，鯊魚、油魚魚肉甲基汞總汞比例均超過95%，可就總汞值代替甲基汞，惟旗魚鬆甲基汞約只佔總汞值之20%。經評估國人每週特定魚類容許攝取量，比較JECFA的PTWI 1.6 μg/Kg/weekly建議值。6-12歲之兒童，鯊魚、旗魚、油魚每週攝食不超過85.8~92.2 g，而13歲以上的國人，每週攝取不超過140~170 g 左右，則不會超過JECFA建議的甲基汞PTWI建議值。未標示魚種之魚鬆則每週僅約可攝食120 g 左右，13歲以上者，則可每週攝食600多克旗魚鬆或200克左右未標示魚種之魚鬆。
推估國人每日攝入魚肉汞之風險值，顯示6-12歲之兒童專吃鯊魚、旗魚、油魚等，依每日魚肉攝取量計算風險百分比為382~445%，約高於安全風險值4倍之多。攝取不明魚種之魚鬆，風險值仍高達安全風險值的3倍。最後，就國人魚類攝取統計資料推估合適攝取的最大魚類汞含量， 0.3 ppm以下汞含量較適於13歲以上青少年及成人，而6-12兒童及老人則宜再減半，比較本研究檢測結果，僅水鯊、旗魚、油魚及未標示魚鬆等超過推估值，可能較具汞風險危害，需留意攝食量。

Mercury is one kind of heavy metals that do harms to human body, and the mercury exposure is mainly caused by fishes that take in mercury. Therefore, to learn the mercury content in aquatic products and processed products that are sold in markets and then further analyze the risks of mercury intake has become an important topic in recent years. This paper attempts to develop a suitable measurement method of mercury content contained in fish, and then analyzes the mercury content in commercial aquatic products to estimate the risks of mercury by taking in fish, which will be served as references for the standard establishment and suggested intake for consumers. The results show that the microwave digestion oven and cold vapor atomic fluorescence spectroscopy can be used for mercury detection. For the conditions of microwave digestion, it shall add 2 mL hydrogen peroxide into nitric acid with eight decomposition bottles under the condition of 800W and 200℃, which is heated to exclude interference chemicals, then reduced with 7% stannous chloride to convert Hg(II) to volatile Hg(0) in mercury analyzer, by which the appropriate analysis results of mercury contents. In the experiment, it takes oilfish and mahi to conduct the matrix spike experiments, with 5 ppb and 10 ppb mercury added into the samples and the respective recovery rate of 94.1±1.9% and 92.2±4.3%, and it further utilizes the standard reference material DORM-4 and BCR-463 to testify the capacity and recovery rate, showing that the proposed method can produce the fine accuracy rating. Moreover, the limit of detection and limit of quantification of the proposed method are 0.0039 ppb and 0.013 ppb.
With the proposed mercury content analysis method, it detects 23 kinds of aquatic products sold in the market, with 211 samples to be detected in total mercury. The results show that all samples meet the limitation scope stipulated in relevant domestic regulations, among which the average mercury content in large pelagic marine fishes meat, shark, oilfish and swordfish are 0.647 ppm、0.619 ppm and 0.556 ppm respectively, which are higher than 0.5 ppm, belonging to the fishes of highest mercury; however, tuna and mahi have a lower content of mercury, which are 0.204 ppm and 0.126 ppm respectively. In which, the medium- and small-size marine fishes and freshwater aquacultures aquatic product are respectively 0.084 ppm and 0.014 ppm, belonging to the fishes of moderate and least mercury content. In terms of processed fish products, it can be divided into fish floss, canned fish and fish roe, and the corresponding mercury contents are 0.05~5.45 ppm, 0.028~0.079 ppm, and 0.002~0.008 ppm, in which the content in fish floss is the highest. Moreover, fish floss can also be categorized as unlabeled fish floss, swordfish floss, tuna floss and salmon floss, all of which have an average mercury content of more than 0.5 ppm except the salmon floss. In addition, the selected samples are also taken to measure the proportion of methyl mercury in total mercury to estimate the rationality of the risk assessment. According to the experiment, the ratio of methyl mercury to total mercury in shark meat and oil fish meat exceed 95%, so the total mercury value can be used to represent the methyl mercury value, but the ratio of methyl mercury to total mercury in swordfish floss only account for 20%. After estimating the acceptable weekly intake of specified fish and comparing with the recommended PTWI value of 1.6 μg/kg/weekly by JECFA, it suggests that children of 6 to 12 years old shall take in the shark meat, swordfish and oilfish meat less than 85.8-92.2 g, and people above 13 years old less than 140-170 g. As for the fish floss of unlabeled fish specie, the weekly intake shall be no more than 120g for children, and people above 13 years old can take 600 g swordfish floss or 200 g unlabeled fish floss a week.
From the estimated risk value of daily fish mercury intake, the risk percentage for children of 6-12 years old only taking in shark meat, swordfish meat and oilfish meat is 382~445% calculated based on their daily fish intake, which is 4 times higher than the JECFA PTDI value. The risk value of taking in fish floss of unknown species is still 3 times higher than the JECFA PTDI value. In the end, it estimated the maximum acceptable fish mercury intake, finding that mercury content of fish lower than 0.3 ppm is suitable for teenagers and adults above 13 years old, which shall be halved for children of 6-12 years old and elder people. Through comparing the measured value in the paper, the values in blue shark, swordfish, oilfish and unlabeled fish floss exceed the suggested value, which is of high risk of mercury hazard and needed to pay attention to the intake amount.

目錄

摘要-----------------------------------------------------------------------------------------I
Abstract------------------------------------------------------------------------------------III
目錄-----------------------------------------------------------------------------------------VI
表目錄---------------------------------------------------------------------------------------IX
圖目錄---------------------------------------------------------------------------------------X
壹、前言-------------------------------------------------------------------------------------1
貳、文獻回顧----------------------------------------------------------------------------------4
一、汞的特性與用途-------------------------------------------------------------------------4
二、汞之散佈------------------------------------------------------------------------------5
三、汞之危害------------------------------------------------------------------------------6
(一)野生動物----------------------------------------------------------------------------6
(二)魚類-------------------------------------------------------------------------------7
(三)人類-------------------------------------------------------------------------------7
四、人體汞中毒症狀與治療--------------------------------------------------------------------8
五、汞含量分析方法------------------------------------------------------------- ------------9
(一)固態樣本消化前處理方法----------------------------------------------------------------9
(二)汞分析儀----------------------------------------------------------------------------10
六、每日魚類攝取量------------------------------------------------------------- ------------12
七、人體汞攝取容許值和魚類汞含量標準----------------------------------------------------------15
八、魚類汞污染分類標準----------------------------------------------------------------------19
九、近年我國市售水產品汞污染調查--------------------------------------------------------------19
十、風險評估方法---------------------------------------------------------------------------21
(一)美國採用的風險評估方式----------------------------------------------------------------21
(二)聯合國採用的風險評估方式--------------------------------------------------------------22
參、實驗架構----------------------------------------------------------------------------------25
一、分析條件之建立------------------------------------------------------------- ------------25
(一)微波消化部份------------------------------------------------------------------------25
(二)汞分析儀部份------------------------------------------------------------------------26
二、汞含量分析及風險評估--------------------------------------------------------------------27
肆、材料與方法--------------------------------------------------------------------------------28
一、實驗材料------------------------------------------------------------------------------28
二、藥品及器材----------------------------------------------------------------------------29
(一)藥品-------------------------------------------------------------------------------29
(二)器材-------------------------------------------------------------------------------31
三、方法---------------------------------------------------------------------------------31
(一)微波消化條件------------------------------------------------------------------------31
(二)消化液後續去干擾物處理----------------------------------------------------------------31
(三)汞含量分析--------------------------------------------------------------------------32
1.檢量線建立------------------------------------------------------------------------32
2.原子螢光分析儀-------------------------------------------------------- ------------33
(四)精密度評估--------------------------------------------------------------------------34
1.同日、異日精密度-------------------------------------------------------------------34
2.品質查核樣本----------------------------------------------------------------------34
(五)準確度評估--------------------------------------------------------------------------34
1.添加回收率試驗-------------------------------------------------------- ------------35
2.標準參考物質----------------------------------------------------------------------35
(六)最低偵測極限(LOD)與定量極限(LOQ)測定---------------------------------------------------35
(七)甲基汞檢測方法-----------------------------------------------------------------------36
(八)風險評估方式-------------------------------------------------------------------------36
1.推估國人每週特定魚類之容許攝取量------------------------------------------------------36
2.推估吃魚攝入汞之風險百分比-------------------------------------- ---------------------36
3.每日容許攝取魚肉汞濃度之推估----------------------------------------------------------37
肆、結果與討論----------------------------------------------------------------------------------38
一、魚肉汞含量分析條件之探討------------------------------------------------------------------38
(一)微波消化處理的影響因素------------------------------------------------------------------38
1.微波消化溫度------------------------------------------------------------------------38
2.微波消化管數量-------------------------------------------------------- --------------38
3.添加過氧化氫------------------------------------------------------------------------39
4.微波消化液加熱去除干擾物效應-----------------------------------------------------------40
(二)汞分析儀的影響因素----------------------------------------------------------------------40
1.稀釋液對標準曲線及樣品之影響-----------------------------------------------------------40
2.分析過程中還原劑濃度的影響-------------------------------------- -----------------------41
二、分析方法的確效------------------------------------------------------------- ---------------42
(一)精密度--------------------------------------------------------------------------------42
(二)準確度--------------------------------------------------------------------------------42
1.回收率------------------------------------------------------------------------------42
2.魚肉標準參考物質(SRM)之比較結果--------------------------------------------------------42
(三)最低檢測極限(LOD)和定量極限(LOQ)---------------------------------------------------------43
三、市售水產品的汞含量-------------------------------------------------------------------------43
(一) 迴游性大型魚類-------------------------------------------------------------------------43
(二)中小型魚類------------------------------------------------------------------------------46
(三)淡水養殖水產品---------------------------------------------------------------------------48
(四) )市售魚類加工製品-----------------------------------------------------------------------48
四、市售水產品汞含量之風險評估------------------------------------------- ------------------------52
(一)魚類之汞與甲基汞-------------------------------------------------------------------------52
(二)國人每週特定魚類容許攝取量-----------------------------------------------------------------53
(三)國人每日攝入魚肉汞之風險百分比--------------------------------------------------------------54
(四)國人每日可攝入魚肉含汞濃度之推估------------------------------------------------------------55
伍、結論------------------------------------------------------------------------------------------57
陸、參考文獻---------------------------------------------------------------------------------------58
柒、表--------------------------------------------------------------------------------------------82
捌、圖--------------------------------------------------------------------------------------------97

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