本研究基於對環境中有機錫污染情形監控的需要，主要針對生物體中有機錫分析方法進行探討，開發準確、簡單及省時的生物體有機錫分析流程，提供作為環境中有機錫污染監測工具；為了確認本研究所開發之生物體有機錫分析步驟對不同環境特性樣品的適用性，因此研究中另規劃於鹿耳門溪河段及四草漁港內、外分別設置測站進行環境基質及生物體丁基錫累積情形的研究，分別於夏季(2003年7月)及冬季(2004年2月)進行水樣、懸浮顆粒、長牡蠣(Crassostrea gigas)、綠貽貝(Perna viridis)、蚵岩螺(Thais clavigera)及紅棕岩螺(Thais rufotincta)的採樣，以進行有機錫含量之分析，調查時亦於現場進行一般水質的檢測；另外，亦採集沉積物樣品進行丁基錫含量之分析，用以呈現鹿耳門溪河口環境整體之有機錫污染分佈情形。
研究中所開發之生物體有機錫分析方法可用於魚肉中丁基錫及苯基錫的分析，其流程是將樣品鹼性水解後同步進行乙基化與萃取的步驟，然後以氣相層析配合火燄光度偵測器進行分析，並針對方法中影響分析回收率的關鍵參數進行探討以及條件最佳化。其中於鹼性水解步驟為了確保樣品可充分水解及避免有機錫發生分解，建議樣品應以3 % (w/v)的氫氧化鉀溶液於60 ℃下進行水解1小時，而乙基化與萃取步驟中的pH值應介於6~7之間，然後加入1 % (w/v)的四乙基硼化鈉溶液反應1小時，其中為避免過多水解之魚肉組織與有機錫陽離子結合產生基質效應，建議分析之魚肉樣品量與乙基化反應之體積比例不要超過0.2 g (乾重)/100 mL；整體而言，本分析方法既簡單又省時，且可應用於一般生物體的有機錫分析。
環境基質中丁基錫的含量反映出四草漁港內TBT污染明顯高於鹿耳門溪河段，然而透過生物體丁基錫的分析則還能反映出四草漁港及鹿耳門溪河段間過渡的TBT污染情形，顯然相對於環境基質生物體所能反映出的環境TBT污染差異更為詳細，然而鹿耳門溪水體中MBT的污染情形則無法反映於生物體中MBT的累積上。
長牡蠣及綠貽貝體內三丁基錫的累積皆呈現高於蚵螺(蚵岩螺與紅棕岩螺)的情形，其中在三丁基錫污染程度較低的環境中長牡蠣體內三丁基錫的累積又呈現高於綠貽貝的情形，然而隨著環境中三丁基錫污染程度變高，長牡蠣體內三丁基錫的累積情形則變成低於綠貽貝；於三丁基錫污染程度較高的環境中，長牡蠣及蚵螺體內所累積的三丁基錫代謝物比例呈現出較高的情況，而其對三丁基錫的生物累積係數則呈現明顯較低的情形，然而此情形於綠貽貝則不明顯；此外，相對於生長在鹿耳門溪河段中之生物(長牡蠣、綠貽貝及蚵螺)，生長於四草漁港出口處的生物對TBT的BAF又明顯較高。
夏季時長牡蠣及綠貽貝體內所累積的三丁基錫代謝物比例呈現高於冬季的情形，而其體內三丁基錫含量則於冬季時呈現高於夏季的情形；所有生物於夏季時對環境中三丁基錫的生物累積係數則皆呈現明顯高於冬季的情形，顯示夏季時生物體對環境中的三丁基錫有較高的累積能力。
蚵螺體內三丁基錫的累積情形明顯低於長牡蠣或綠貽貝，其體內累積之丁基錫以三丁基錫的代謝物為主，而與長牡蠣或綠貽貝主要以三丁基錫為主的情形不同，這是因為蚵螺對三丁基錫的代謝效能較高所致。

The goal of this study is to establish an accurate, simple and fast method for analysis of organotin in bio-tissues and for routine analysis of organotin in pollution control. This study also conducted the field survey investigating the accumulation status of butyltin (BT) in organisms and environments for validation of analytical method and applicability in different environmental samples. Stations had been set up from the Sih-Cao fishing port to the upstream of Luermen Stream Estuary. General water quality factors were measured in situ, and water samples, suspended particles, Pacific oysters (Crassostrea gigas), green mussels (Perna viridis), and rockshells (Thais clavigera and Thais rufotincta) were collected in summer (July 2003) and winter (February 2004) seasons and the concentrations of butyltins were measured. Surface sediment samples were also collected from each sampling station and the concentrations of butyltins were measured to present pollution status of butyltins in Luermen Stream Estuary.
To determine butyl- and phenyl-tins in fish muscle, a method including base digestion pretreatment, followed by an ethylation-extraction procedure together with gas chromatography-flame photometric detection (GC-FPD) analysis is outlined. Parameters that affect analyte recovery were investigated and optimized. A solution of 3 % (w/v) potassium hydroxide and 1 h digestion time at 60 ℃ were chosen in the base digestion step to ensure complete solubilization of fish muscle and the decomposition of organotins was found to be negligivle. We found that the ratio of fish muscle/reaction solution volume should not exceed 0.2 g (dry weight) per 100 mL in order to avoid the matrix effect caused by the binding of hydrolyzed fish tissue with organotin ions. Ethylation of organotins were conducted at pH 6~7 with a 1 % (w/v) sodium tetraethylborate (NaBEt4) solution for 1 h. This simple and timesaving procedure could be applied to the routine analysis of organotins in other bio-tissues.
The BT content of environments and organisms reflected that the tributyltin (TBT) pollution levels were higher in Sih-Cao fishing port than in Luermen Stream. The BT content of organisms reflected more detail TBT pollution status between Sih-Cao fishing port and Luermen Stream. However, the MBT pollution status in Luermen Stream was not reflected in MBT accumulation status of organisms.
The ability of TBT accumulation in oysters and mussels was higher than in rockshells. Moreover, oysters had higher TBT accumulation ability than mussels at lower TBT pollution level, but following the increase of TBT pollution level, the ability of TBT accumulation in oysters had shifted to be lower than in mussels. The results also showed that in the higher TBT pollution level, the ratios of MBT and DBT over the total butyltins had changed to higher status and the bioaccumulation factors (BAF) had changed to smaller values in oysters and rockshells. In mussels, this phenomenon was not significant. However, the organisms (oyster, mussel and rockshells) revealed smaller BAF of TBT in Luermen Stream than in the Sih-Cao fishing port entrance.
For oysters and mussels, the TBT contents and the composition ratios of TBT in total butyltins were both higher in winter season. All organisms (oysters, mussels and rockshells) had higher ability to accumulate TBT according to the larger BAF observed in summer season.
The ability of TBT accumulation in rockshells was lower than in oysters or mussels. Moreover, the BT accumulation status was mainly composed of MBT and DBT (the metabolites of TBT ) in rockshells and TBT in oysters and mussels. That was attributed to higher metabolic rate of TBT in rockshells.

第一章 前 言…………………………………………………………1

第一節 有機錫化合物的用途及環境中的來源……………………… 1
第二節 有機錫化合物之毒性………………………………………… 5
第三節 溶液系統中有機錫化合物之物種分佈……………………… 7
第四節 有機錫化合物與懸浮顆粒(沉積物)之吸附現象…………… 9
第五節 有機錫化合物於環境中的分解現象…………………………12
第六節 有機錫化合物的生物累積現象………………………………15
第七節 有機錫化合物使用對環境之影響……………………………23
第八節 有機錫化合物的使用管制……………………………………27

第二章 生物體有機錫分析方法之探討…………………………… 39

第一節 引言……………………………………………………………39
第二節 研究規劃與材料方法…………………………………………42
2.1 藥品及儀器……………………………………………………… 42
2.2 鹼性水解試驗…………………………………………………… 45
2.3 有機錫分析步驟………………………………………………… 45
第三節 結果與討論……………………………………………………47
3.1 鹼性水解條件…………………………………………………… 47
3.2 乙基化條件……………………………………………………… 48
3.3 基質效應………………………………………………………… 51
3.4 分析步驟有效性確認…………………………………………… 52

第三章 環境中有機錫累積情形之探討…………………………… 63

第一節 研究規劃………………………………………………………63
1.1 採樣規劃………………………………………………………… 63
1.2 樣品處理及分析………………………………………………… 65
1.3 藥品及儀器設備………………………………………………… 70
第二節 結果……………………………………………………………72
2.1 一般水質項目…………………………………………………… 72
2.2 水體中溶解態丁基錫含量……………………………………… 73
2.3 沉積物部分……………………………………………………… 75
2.4 懸浮顆粒………………………………………………………… 77
第三節 討論……………………………………………………………84

第四章 生物體中有機錫累積情形之探討…………………………111

第一節 研究規劃…………………………………………………… 111
1.1 採樣規劃…………………………………………………………111
1.2 樣品處理及分析…………………………………………………111
1.3 藥品及儀器設備…………………………………………………113
第二節 結果………………………………………………………… 114
2.1 長牡蠣……………………………………………………………114
2.2 綠貽貝……………………………………………………………119
2.3 蚵岩螺……………………………………………………………123
2.4 紅棕岩螺…………………………………………………………127
2.5 不同生物體內丁基錫累積情形之比較…………………………131
第三節 討論………………………………………………………… 133

結 語………………………………………………………………… 167

英文參考資料…………………………………………………………169
中文參考資料…………………………………………………………188

附錄一 原始數值
附錄二 本研究已發表之生物體有機錫含量分析方法

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