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研究生:林宜
研究生(外文):Yi Lin
論文名稱:臺灣嘉南平原溪口鄉地下水層砷之礦物學特徵及釋出機制
論文名稱(外文):Mineralogy and Mobilization Mechanisms of Arsenic in Groundwater in Xikou township, Chianan Plain, Taiwan
指導教授:王尚禮
指導教授(外文):Shan-Li Wang
口試委員:陳尊賢李達源簡錦樹鄒裕民
口試委員(外文):ZUENG-SANG CHENDAR-YUAN LEEJiin-Shuh JeanYu-Min Tzou
口試日期:2015-07-23
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:農業化學研究所
學門:農業科學學門
學類:農業化學類
論文種類:學術論文
論文出版年:2015
畢業學年度:103
語文別:中文
論文頁數:110
中文關鍵詞:嘉南平原地下水水化學岩芯地質化學X光吸收近緣結構
外文關鍵詞:ArsenicChianan plainGroundwater chemistryX-ray absorption spectroscopySequential extraction
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臺灣嘉南平原地區地下水中含高濃度砷,但對於通氣帶 (vadose zone) 中砷之釋出機制仍不夠瞭解,因此本研究自嘉南平原選擇高砷地區,進行80公尺的岩芯鑽探,採集不同深度的岩芯和地下水,分析砷礦物學特徵組成和地下水溶液化學,以探討通氣帶中砷的釋出機制。所採集之地下水樣進行pH、Eh、砷物種,以及化學組成分析。岩芯則以連續萃取法和As K-edge X光吸收近緣結構 (XANES) 分析其砷礦物組成。在不同深度之地下水層中,砷的濃度範圍為8-355 μg L-1。以HPLC-ICP-MS分析地下水的砷物種,結果顯示無機態As(III) 為優勢物種,有機砷含量則低於偵測極限。地下水層分別於20-30公尺與50-70公尺處的砷濃度最高,而此兩個水層亦分別含有最高的硫酸鹽與鐵濃度,推論此兩個深度有不同的砷釋出機制。於As K-edge之XANES圖譜中發現,除了接近表層之岩芯 (深度6.2公尺) 以As(V) 為主之外,其他深度皆以As(III) 與As(V) 混合之形式存在;進一步以LCF分析發現,砷黃鐵礦 (Arsenopyrite, FeAsS) 主要分布於深度15-35公尺之岩芯。連續萃取法之結果顯示,在深度15-35公尺之岩芯中,砷主要為硫化物與有機型態。由於此層之地下水中亦富含硫酸鹽,推測此深度岩芯之砷釋出機制為含砷硫化物的氧化溶解。而深度約50公尺之岩芯的砷型態以無定形與結晶性良好鐵鋁氧化物結合相為主,對照此層地下水富含Fe2+,推測此層砷的釋出機制為鐵氧化物的還原溶解。基於上述結果並結合溶液化學之熱力學計算,進一步確認於深度20-30公尺與50-70公尺處的砷釋出機制分別為含砷之硫化物氧化溶解,以及含砷之鐵氧化物的還原溶解。

Chianan plain in southwestern Taiwan has long been well known for the prevalence of black-foot disease since 1920s, but the mobilization mechanism of As in the vadose zone in this area has not been well understood. To elucidate the mechanisms of As release in the vadose zone in Chianan plain, drilling of a borehole was conducted at a selected site and the groundwater and core samples were collected at different depths up to 80 m. The groundwater samples were analyzed for pH, Eh, As speciation, and elemental composition. The As-containing minerals in the core samples were determined using As K-edge X-ray absorption spectroscopy (XAS) in conjunction with sequential extraction. The As concentrations in the groundwater samples of different depths ranged from 9 to 370 ppb. As(III) was predominant in all the samples, while the concentration of organic As was negligible. The concentration of As was relatively high in the groundwater samples collected at the depths of 20-30 and 50-60 m, accompanying with the high concentrations of sulfate (41.1-51.1 mg L-1) and Fe (8.3-10.4 mg L-1), respectively. The As K-edge XANES spectra revealed that arsenopyrite (FeAsS) was predominantly present in the core at the depth of 15-35 m. The results of sequential extraction showed that the As in cores at the depths of 15-35 and 50-70 m were associated with sulfides and Fe hydroxides, respectively. Based on these results, it was therefore proposed that the predominant mechanisms of As release to groundwater at the depths of 20-30 and 50-60 m were the oxidative dissolution of As-containing sulfide minerals and the reductive dissolution of As-containing Fe minerals, respectively.

目錄
摘要 i
Abstract iii
第一章 前言 1
第二章 文獻回顧 4
2-1 砷 4
2-1.1 砷的來源 4
2-1.2 砷之物種與化學形態 5
2-1.3 砷之毒性 8
2-1.4 砷於固相-液相間之交互作用 9
2-2 地下水層之氧化還原反應 10
2-3 含高砷地下水之區域分布 11
2-3.1 全球地區 11
2-3.2 臺灣地區 12
2-4 地質環境中砷之釋出機制 13
2-5 研究地區之水文地質背景與地下水層劃分 16
2-6 嘉南平原含砷地下水之地質化學研究 22
第三章 材料與方法 23
3-1 岩芯 23
3-1.1 採樣與前處理 23
3-1.2 分析方法 24
3-1.2.1 總砷含量測定 24
3-1.2.2 砷物種含量測定 25
3-1.2.3 連續萃取法 (Sequential Extraction Procedure, SEP) 28
3-1.2.4 X光繞射分析 (X-ray Diffraction, XRD) 33
3-1.2.5 X光吸收光譜 (X-ray absorption spectroscopy, XAS) 34
3-1.2.6 SEM-EDS 37
3-1.2.7 統計分析 38
3-2 岩芯孔隙溶液 39
3-2.1 採樣與前處理 39
3-2.2 分析方法 39
3-2.2.1 砷物種含量 39
3-3監測井井水 40
3-3.1 採樣與前處理 40
3-3.2 分析方法 43
3-3.2.1 酸鹼度 (pH) 與氧化還原電位 (Eh) 43
3-3.2.2 總砷與砷物種含量 44
3-3.2.3 鐵比色法 (Colorimetric determination of iron) 45
3-3.2.4 硫化物含量 46
3-3.2.5 陰離子濃度 (Cl-, NO3-, PO43-, SO42-) 48
3-3.2.6 熱力學計算 49
第四章 結果與討論 50
4-1 季節性變動與地下水層分帶 50
4-2 地下水層中固-液相間砷物種變化與移動 52
4-3 地下水層之水化學特徵 54
4-4 岩芯之砷型態劃分 59
4-5 岩芯之礦物學與地質化學特徵 69
4-5.1 X光繞射分析 69
4-5.2 X光吸收光譜分析 71
4-5.3 SEM-EDS分析 79
4-6 熱力學計算 82
4-7 含砷地下水之曝氣試驗 86
第五章 結論 90
第六章 參考文獻 92
附 錄 107



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