本研究以2008年1月OR1 855 冬季航次及7月OR1 870夏季航次所採集到的樣本，採用氫化-填充冷指-原子螢光法(HG-PCF-AFS)進行溶解態可氫化砷物種(AsV、AsIII、MA和DMA)的分析。870夏季航次樣品依其溫鹽性質，分別歸類於長江沖淡水(C)、低氧水(L)、台灣暖流水(T)、黃海混合水(Y)與黃海冷水(YC)五種水團；855冬季航次樣品則分別歸類於長江沿岸水(CCC)、陸棚混合水(SMW)和黑潮水(K)三種水團。本研究除了探討砷物種消長的季節性變化，並比較不同水團中dAsIII、dAsV、dMA和dDMA之組成比例的差異，其目標為以砷物種消長作為環境壓力的指標。
870夏季航次樣品C水團中PO4的濃度影響dDMA的產生，PO4濃度較低時出現較高濃度的dDMA，符合較低磷濃度之環境下浮植攝取AsV後經由AsV→ AsIII → MA→ DMA，將DMA排出體外的機制。水團中的dAsIII推測主要來自於細菌降解機制，水溫越高dAsIII濃度越高。T水團中水溫較高的測站，總溶解砷中dDMA和dAsIII佔了30%的比例，dDMA和dAsIII的成因與C水團類似。低光照的L水團缺少浮植的活動，dDMA的濃度亦低，主要砷物種為細菌降解的最終產物dAsV。YC水團與L水團類似，dAsIII和dDMA的濃度均低，主要砷物種為dAsV。Y水團之dAsIII和dDMA濃度較C水團和T水團低，但比L水團和YC水團高。
855冬季航次受陸源輸出影響導致CCC水團與SMW水團含有較高濃度的dAsV和dAsIII，而黑潮的稀釋導致K水團中dAsV和dAsIII的濃度降低。855航次溫鹽密度的差異小於870航次，垂直分佈無顯著的層化現象。由於冬季東海水體垂直混合較夏季強烈，導致各砷物種之水平分佈或是垂直分佈，均未呈現特別顯著的分佈趨勢。

Arsenic speciation variation over the shelf of the East China Sea (ECS) was investigated at Cruise OR1-855 (from January 1 to 11, 2008) and Cruise OR1-870 (July 3 to 13, 2008) using hydride generation-packed cold ginger-atomic fluorescence spectrometer (HG-PCF-AFS). The samples of OR1-870 were classified into five water mass types: Changjiang Diluted Water (C), Low Oxygen Water (L), Taiwan Current Warm Water (T), Yellow Sea Mixed Water (Y) and Yellow Sea Cold Water (YC). The samples of the OR1-855 were classified into three water mass types: Changjiang Coastal Current (CCC), Shelf Mixing Water (SMW) and Kuroshio Water (K). In addition to evaluate the arsenic speciation variation between the two seasons, this study also assesses the dissimilarity of arsenic species constitution among different water mass. Adopting arsenic species constitution as the indicator for the environment stress is the objective.
In the OR1 870, phosphate in the C water mass has an effect on production of dDMA where the higher dDMA associates with the lower phosphate. It agree with biotransformation pathway by phytoplankton in phosphate deplete environment: AsV→AsIII →MA→DMA. The bacterial degradation was proposed to be the reason of high dAsIII concentrations in C water mass because the temperature of the water mass is also high. Similar to the C water mass, about 30% of total dissolved arsenic were in the forms of either dDMA or dAsIII for certain samples in T water mass that present the higher temperature. The dDMA in L water mass was very low because of lacking light radiance as well as the phytoplankton. The mainly arsenic species in L water is dAsV which is the final degradation product of the arsenic species. Similar to the L water, either dAsIII or dDMA were low in YC water mass was concentration, and the dominant arsenic species was dAsV. The concentration of dAsIII and dDMA in the Y water mass was lower than that in the C and T water mass, but higher than that in the L and YC water mass.
In the OR1-855, the terrestrial export led to the higher concentration of dAsV and dAsIII in the CCC and SMW water mass. In contrast, the K water mass appeared the lower concentrations of dAsV and dAsIII because of Kuroshio dilution. The density (σt) variation in OR1-855 was much narrower than the variation in OR1-870, thus, the water column readily mixed in winter. Neither horizontal distribution nor vertical distribution appeared particular trend for any arsenic species.

謝誌............................................ I
中文摘要........................................ II
ABSTRACT....................................... IV
目錄........................................... VI
圖目錄.......................................... VIII
表目錄...........................................X
縮寫及中英文對照表............................... XI
第一章、前言..................................... 1
1.1 海洋砷物種的消長........................... 1
1.2 砷物種在浮植中的代謝機制.................... 2
1.3 研究目的與動機............................. 3
第二章、材料與方法............................... 4
2.1 氫化冷指原子螢光砷物種分析系統.............. 4
2.2 試藥及材料................................ 5
2.3 檢量線溶液製備.............................6
2.4 採樣及保存................................ 8
2.5 樣品分析.................................. 9
2.6 樣品溫鹽性質及分類.........................11
第三章、結果與討論...............................13
3.1 OR1 870夏季航次研究結果...................13
3.1.1 OR1 870夏季砷物種測線剖面分佈...........14
3.1.2 OR1 870夏季砷物種與水團之關係...........16
3.2 OR1 855冬季航次研究結果...................19
3.2.1 OR1 855冬季砷物種測線剖面分佈...........20
3.2.2 OR1 855冬季砷物種與水團之關係...........20
第四章、結論.....................................22
參考文獻........................................ 24

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