臺灣博碩士論文加值系統

汞是一種常見的重金屬污染物，其中以經由微生物代謝轉換所形成的代謝物質甲基汞所具毒性最為強烈，為一般無機汞之毒性的10~100倍。本研究之目的為建立一套簡易、實用、快速之魚貝類中甲基汞含量測定方法，利用液相層析儀串聯感應耦合電漿質譜儀(LC-ICP-MS)進行汞物種包括甲基汞 (Me-Hg)、丙基汞 (Pr-Hg)及二價汞 (Hg2+)之分離定量，並探討層析管柱、移動相pH值、ICP-MS之電漿功率強度與霧化(載體)氣體流速以及樣品萃取液條件之最適化。其次，建立此LC-ICP-MS檢測魚肉樣品之確效性評估，再以所建立方法針對台灣南部地區販售之魚類進行可食肉中汞物種含量分析。
研究結果顯示，在樣品前處理方面，pH為4.0之50 mM半胱胺酸及50 mM過氯酸鈉混合萃取液，具有最佳萃取樣品中汞物種之效果。其次，以 pH 為4.0之50 mM 半胱胺酸及50 mM 過氯酸鈉混合溶液為移動相，並使用離子交換樹脂分析管柱 IonPacTM CS5A (4×250 mm, 9.0 μm)，電漿功率為1550W 以及0.96 L/min 的霧化氣體流速等是LC-ICP-MS 分析的最適條件。另外，於檢體中分別添加 Me-Hg、Pr-Hg及Hg2+標準品0.04、0.1及0.2 mg/kg等三種濃度，以此 LC-ICP-MS 檢測方法分析，得知其準確度 (回收率)介於86.13至101.37%之間、重複性 (CV%)介於1.45至3.69%之間及中間精密度 (CV%)介於1.85至5.01%之間，皆符合食品化學檢驗方法之確效規範，各項汞物種之定量極限值 LOQ 皆為0.02 mg/kg。另外，以所建立之方法針對南部地區販售之生魚片進行分析，發現所有採集的鮪魚、旗魚肉以及鮭魚、海鱺魚肉樣品之甲基汞含量，皆低於食品衛生標準之規定 (分別為2 mg/kg以及0.5 mg/kg以下)。

Mercury is a common heavy metal pollutant. Among them, methylmercury, a metabolite formed by microbial metabolic conversion, is the most toxic, 10 to 100 times more toxic than general inorganic mercury. The purpose of this study was to establish a simple, practical, and fast method for the determination of methylmercury in fish and shellfish. This liquid chromatography coupled to inductively coupled plasma mass spectrometry (LC-ICP-MS) was used to determine mercury species including the separation and quantification of methylmercury (Me-Hg), propylmercury (Pr-Hg) and divalent mercury (Hg2+). The chromatographic column, mobile phase pH, ICP-MS plasma power in-tensity and aerosol gas flow rate, and sample extraction solution condi-tions are optimized. Moreover, the LC-ICP-MS was established to de-termine the validity of the fish samples, and the mercury species in the edible meat were analyzed by the established method for the fish sold in southern Taiwan.
The results showed that the mixed solution of 50 mM L-cysteine and 50 mM sodium perchlorate (pH=4.0) used as the mobile phase, and IonPacTM CS5A (4×250 mm, 9.0 μm) column with ion exchange resin for LC method are the optimum conditon. In ICP-MS condition, the plasma power set at 1550 W and the carrier flow rate of 0.96 L/min are the op-timum conditions for analysis. In addition, 0.04, 0.1 and 0.2 mg/kg concentrations of Me-Hg, Pr-Hg and Hg2+ standards were spiked to fish samples, and the average recovery (accuracy), repeatability (CV%) and intermediate precision (CV%) obtained by LC-ICP-MS ranged from 86.13 to 101.37%, 1.45 to 3.69% and 1.85 to 5.01%, respectively, all in accordance with the validation of food chemical testing methods. Moreover, the analysis of the fish sold in southern Taiwan by the es-tablished method showed that the methylmercury contents in tuna and marlin fish meats, and salmon and cobia fish meats all were lesser than the methylmercury limit of food hygienic standard (2 mg/kg and 0.5 mg/kg, respectively).

中文摘要 I
英文摘要 III
誌謝 V
目錄 VI
表目錄 VIII
圖目錄 X
壹、緒論 1
貳、文獻探討 3
一、汞 3
二、甲基汞 6
三、我國水產動物中汞之現行規範及標準 7
四、各國對於魚貝類中汞含量之規範 9
五、汞物種分析方法探討 9
六、食品中甲基汞分析探討 12
七、感應耦合電漿質譜儀 13
參、材料與方法 19
一、魚體檢體 19
二、儀器裝置 19
三、藥品 22
四、器具及材料 22
五、萃取溶液配製 23
六、檢液調製 24
七、鑑別試驗及含量測定 24
八、檢測方法之最適化條件 25
九、檢驗方法之確效評估 26
十、魚類樣品的萃取與分析 32
肆、結果與討論 33
一、LC-ICP-MS 分析條件最適化 33
二、樣品前處理條件 36
三、檢驗方法之確效評估 38
四、水產品汞含量分析 44
伍、結論 66
陸、參考文獻 68

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