臺灣博碩士論文加值系統

當今半導體產業的製品充斥於日常生活中，卻缺乏針對其原料中的鎵、銦與鉈等新興污染元素於土壤中系統性之研究與相關地質化學知識。此外，鎵、銦與鉈於不同母質所化育形成的土壤中之濃度變異極大，因此對於環境以及人體的健康風險難以評估。本研究藉由調查37個來自6種不同母質（第四紀沖積物、砂頁岩、黏板岩、安山岩、玄武岩與蛇紋岩）之土壤剖面，進行金屬全量分析、單一試劑萃取以及序列萃取，以探討鎵、銦與鉈於各類型土壤中的分佈、潛在移動性、地質化學分化以及與土壤性質的關係。結果顯示，由ICP-MS所測定以王水所消化之鎵、銦與鉈在所有樣本的全量濃度範圍分別為2.22 – 24.5 mg kg-1、2.63 – 678 μg kg-1、3.17 μg kg-1 – 1.00 mg kg-1，平均值分別為12.2 mg kg-1、20.6 μg kg-1、103 μg kg-1，其中鎵、銦與鉈在第四紀沖積物母質之農田土壤中濃度高於其他樣本。此外，地質累積指數 (geoaccumulation index, Igeo)與富集因子 (enrichment factor, EF)顯示，樣本中所含有的鎵、銦與鉈受到人為污染的可能性低。利用1N KCl、0.1N HCl以及0.05M EDTA的單一萃取結果顯示，鎵、銦與鉈潛在生物有效性的含量低，但在第四紀沖積物母質樣本中，鎵、銦與鉈的萃取量高於其他母質樣本，BCR序列萃取的結果也指出不同母質樣本中，大部份的鎵被固定於礦物晶格中，因此具有潛在移動性的比例偏低。EDTA可萃取之鎵與鉈，可由土壤鎵與鉈全量濃度、pH值以及黏粒含量之多變因迴歸式計算而出。

Nowadays, the products of semi-conductor are full of our daily life. However, few studies and geochemical knowledge focus on emerging contaminant elements such as gallium, indium and thallium which are ones of raw marerials of these products. Besides, the concentrations of Ga, In and Tl in soils derived from different parent materials vary greatly, so the potential risk to the environment and human health is difficult to assess. This study investigated 37 soil profiles from six different parent materials including the Quaternary sediemnt, sandstone and shale, slate, andesite, basalt and serpentine, to explore the distribution, fractionation, potential mobility and bioavalibility of these metals. The total Ga, In and Tl contents meseaured by ICP-MS followed with the auqa regia digestion ranged in 2.22 – 24.5 mg kg-1, 2.63 – 678 μg kg-1 and 3.17 μg kg-1 – 1.00 mg kg-1 with the average of 12.2 mg kg-1, 20.6 μg kg-1, 103 μg kg-1, respectively. Furthermore, the total Ga, In and Tl contents are higher in the soils from the Quaternary sediments related to those from the other soil types. The geo-accumulation index (Igeo) and enrichment factor (EF) indicated that Ga, In and Tl in all cases were low in contamination levels. Low potential bioavalibility of these metals was found according to th eingle extractions of Ga, In, and Tl by using KCl, HCl and EDTA, however, the samples from the Quaternary sediment contained higher extractable levels. Additionally, the Commission of the European Communities Bureau of Reference (BCR) selective sequential extraction method indicated Ga was primarily fixed in the mineral lattices and exhibited low potential mobility. The EDTA-extractable Ga and Tl, representing the potential bioavalibility can be estimated by using multivariate regression equations considering the soil pH, clay and total content of Ga and Tl.

摘要 I
Abstract II
目錄 IV
表目錄 VI
圖目錄 VII
第一章　前言 1
第二章　文獻回顧 3
2.1 新興污染元素的種類與特性 3
2.1.1 新興污染元素的定義 3
2.1.2 鎵、銦、鉈 4
2.1.3 錫、銻 7
2.2 土壤中的新興污染元素 9
2.2.1 土壤中的背景值 9
2.2.2 污染源 17
2.2.3 新興污染元素的型態 20
2.2.4 新興污染元素在植物中的濃度 25
2.3 新興污染元素之污染評估 27
第三章　材料與方法 28
3.1 研究區域 28
3.2 土壤樣品之收集與製備 33
3.3 土壤理化性質分析 33
3.3.1 水分含量 34
3.3.2 金屬全量含量分析 34
3.3.3 交換性鋁、鎵、銦、鉈分析 34
3.3.4 單一化學試劑萃取法 – 0.05 M EDTA 35
3.3.5 單一化學試劑萃取法 – 0.1 N HCl 35
3.3.6 序列萃取 36
3.4 污染指標 37
3.4.1 富集因子 37
3.4.2 地質累積指數 37
3.5 品質保證與品質控制 37
3.6 統計分析 38
第四章　結果與討論 39
4.1 供試農田土壤之基本理化性質 39
4.2新興污染元素於不同母質與化育層土壤中之全量濃度 43
4.2.1 化育層 43
4.2.2 第四紀沖積物 46
4.2.3 砂頁岩沖積物 49
4.2.4 黏板岩沖積物 52
4.2.5 農田土壤母質間比較 55
4.2.6 安山岩、玄武岩、蛇紋岩土壤 58
4.3 新興污染元素富集因子與地質累積指數 63
4.4 新興污染元素單一萃取法之濃度 67
4.4.1 1N KCl 67
4.4.2 0.1N HCl 70
4.4.3 0.05M EDTA 72
4.5 新興污染元素序列萃取濃度 76
4.6 新興污染元素與土壤性質間之關係 79
4.6.1 相關係數 79
4.6.2 主成份分析 81
4.7 新興污染元素潛在有效性評估 84
第五章　結論 85
第六章　參考文獻 86
第七章　附錄 98
表目錄
表 1、鎵於不同地區土壤中含量 10
表 2、銦於不同地區土壤中含量 12
表 3、鉈於不同地區土壤中含量 14
表 4、錫於不同地區土壤中含量 16
表 5、銻於不同地區土壤中含量 16
表 6、工業區或礦區附近土壤鎵、銦與鉈含量 19
表 7、不同植物體中鎵、銦與鉈的濃度 26
表 8、供試土壤剖面之代號與所在行政區 29
表 9、供試土壤剖面之地理與分類資訊 30
表 10、各研究提供之基本理化性質 33
表 11、所有樣本中A層與B層基本理化性質之敘述統計 40
表 12、第四紀沖積物中A層與B層基本理化性質之敘述統計 40
表 13、砂頁岩土壤中A層與B層基本理化性質之敘述統計 41
表 14、黏板岩土壤中A層與B層基本理化性質之敘述統計 41
表 15、所有樣本中C層基本理化性質之敘述統計 42
表 16、不同母質中EDTA可萃取之鎵、銦與鉈含量範圍 73
表 17、土壤理化性質與不同處理獲得之新興污染元素濃度之皮爾森相關係數 80
表 18、土壤理化性質與不同處理獲得之新興污染元素濃度之前四主成分負荷量 82
附錄表A 1、供試土壤基本理化性質 98
附錄表A 2、供試土壤中鎵、銦、鉈、錫和銻全量 106
附錄表A 3、供試土壤不同萃取劑可萃取之鎵、銦與鉈含量 114
附錄表A 4、鎵於不同母質剖面中序列萃取測值、比例與回收率 120
圖目錄
圖 1、鎵在不同pH-Eh下物種變化圖 21
圖 2、銦在不同pH-Eh下物種變化圖 22
圖 3、鉈在不同pH-Eh下物種變化圖 24
圖 4、不同化育層中不同金屬近似全量盒狀圖 45
圖 5、第四紀沖積物中A與B化育層中不同金屬近似全量盒狀圖 48
圖 6、砂頁岩土壤A層與B層中不同金屬近似全量盒狀圖 51
圖 7、黏板岩土壤A層與B層中不同金屬近似全量盒狀圖 54
圖 8、不同母質中各金屬近似全量之盒狀圖 57
圖 9、安山岩中不同金屬近似全量盒狀圖 60
圖 10、安山岩剖面中不同金屬近似全量之深度分布圖 60
圖 11、玄武岩剖面中金屬全量的深度分布圖 61
圖 12、蛇紋岩剖面中金屬全量的深度分布圖 62
圖 13、不同母質中不同金屬之富集因子盒狀圖 64
圖 14、不同母質中不同金屬地質累積因子之盒狀圖 66
圖 15、不同母質中KCl可萃取鉈結果 69
圖 16、鉈全量與KCl可萃取量之散佈圖與迴歸直線 69
圖 17、不同母質中HCl可萃取鉈鎵含量盒狀圖 71
圖 18、不同母質中HCl可萃取鎵百分比盒狀圖 71
圖 19、不同母質中EDTA萃取結果盒狀圖 74
圖 20、鉈全量與EDTA可萃取量之散佈圖與迴歸直線 75
圖 21、鎵於不同母質剖面中序列萃取各項態之結果 78
圖 22、土壤理化性質與不同處理獲得之新興污染元素含量之主成分分析結果 83

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