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dc.description.abstract汞的高毒性和累積性對人體與土壤環境會造成很大的威脅,土壤汞的檢測與監控是相當重要的課題。本論文研究主要探討不同烷銨插層鍍金修飾電極對汞離子的偵測,並以汞離子添加到土壤抽出液中找出最佳試驗參數與最佳烷銨插層鍍金修飾電極,期望能發展出可快速檢測土壤中汞離子的電化學方法。試驗結果顯示,烷銨插層多鐵蒙特石鍍金修飾電極搭配微分脈衝伏安法對200 ~ 1000 ppb Hg2+ 有較好的偵測效果,且其不易受鉛存在所影響。此外,利用相同的電極搭配方波伏安法對20 ~ 250 ppb Hg2+ 有較佳的偵測效果,其方波最佳參數為階梯電位:8 mV、頻率:20 Hz;預濃縮最佳電位為–0.8 V、6分鐘。十四碳烷銨插層多鐵蒙特石鍍金修飾電極對秀水系土壤抽出液中的汞離子有較佳的電化學分析結果,其偵測範圍為20 ~ 100 ppb (R2 = 0.9726)。以中興湖水和地下水中利用100 ppb Hg2+ 的標準添加可獲得回收率分別為80.16 ~ 104.51 % 和89.11 ~ 109.78 %。以此電極偵測秀水系土壤抽出液中100和1000 ppb汞離子可得到良好的穩定性與再現性。以台灣農業耕地土壤為真實樣品,利用十四碳烷銨插層多鐵蒙特石鍍金修飾電極與汞分析儀作分析比較,其有R2 = 0.4500的相關性,由於汞分析儀是測定土壤總汞量,故與電化學分析方法測定間有所差別,土壤汞離子與總汞量之間的比值範圍為14.33 ~ 273.14 %。以土壤總汞量和汞離子量之間所做的相對差異百分比得知,其之間的差異易受土壤鉻和鋅含量的影響,此也顯示土壤鉻、鋅含量增加會影響到電化學對土壤汞離子的分析。zh_TW
dc.description.abstractHigh toxicity and accumulation of mercury has caused a great threat to human body and soil environment, and it is important task to determine and monitor soil mercury. The objective of this study was to find better determination of mercury ions using gold plated alkylammonium- intercalated clay modified electrode (Au_AICME), and hope to develop electrochemical methods for rapid detection of mercury ions in the soils. The results indicated that Au_AICME of ferruginous smectite (SWa-1) had good determination for 200 ~ 1000 ppb Hg2+ coupling with electroanalysis of differential-pulse voltammetry, and that for 20 ~ 250 ppb Hg2+ coupling with square-wave voltammetry. Eletroanalysis of Au_AICME (SWa-1) coupling with differential-pulse voltammetry was not affected by presence of Pb(II).The optimum parameters of square-wave voltammetry were 8 mV for step potential, 20 Hz for frequency,–0.8 V for deposition potential and 6 minutes for deposition time. Au_AICME of 14C_SWa-1 had excellent analysis for 20 ~ 100 ppb Hg2+ (R2 = 0.9726) in the extracted solution of Shiushui soil. Good recoveries of 100 ppb Hg2+ added in Chung Hsing lake and underground water were respectively 80.16 ~ 104.51 % and 89.11 ~ 109.78 %. Au_AICME of 14C_SWa-1 had good stability and repeatability for 100 and 1000 ppb Hg2+. The relationship between electroanalysis of Au_14C_SWa-1 electrode and mercury analyzer was R2 = 0.4500 for real samples of Taiwan agricultural soils. Analysis of mercury analyzer was different with Au_AICME due to total mercury for mercury analyzer and mercury ions for electroanalysis, so the ratio between mercury ions and total mercury was 14.33 to 273.14 % in agricultural soils. Relative difference percent of mercury ions and total mercury in soils indicated the difference of two analytic methods that was affected by the contents of chromium and zinc, and that also showed much amounts of soil chromium and zinc would affect the electroanalysis of mercury ions in agricultural soils.en_US
dc.description.tableofcontents致 謝 I 摘 要 II Abstract III 目 次 V 圖 次 VII 表 次 IX 第一章 前言 1 第二章 前人研究 3 一、黏土礦物及烷銨插層黏土礦物 3 二、汞的介紹 13 (一) 汞的來源 13 (二) 汞的應用與毒害 14 (三) 汞的分析方法 15 三、電化學分析 17 (一) 化學修飾電極簡介及應用 17 (二) 黏粒修飾電極簡介及應用 21 (三) 電化學分析技術簡介 24 1. 方波伏安法 (Square Wave Voltammetry) 24 2. 微分脈衝伏安法 (Differential Pulse Voltammetry) 26 第三章 材料與方法 27 一、藥品 27 二、儀器 27 三、藥品配製方法 28 四、烷銨插層黏土礦物之製備 30 五、烷銨插層黏粒鍍金修飾電極之製備 30 六、土壤樣品之前處理 31 (一) 台灣典型土壤之土壤抽出液 31 (二) 湖水和地下水樣品 31 (三) 台灣農耕地土壤樣品 31 第四章 結果與討論 34 一、不同黏粒修飾電極對汞離子之偵測 34 (一) 高濃度範圍汞離子之偵測 34 1. 偵測參數探討 34 2. 不同陽極剝除伏安法之比較 35 3. 不同修飾方式對汞離子偵測結果 37 4. 烷銨黏粒之電子顯微鏡影像 40 5. 不同烷銨插層鍍金修飾電極偵測汞離子結果 42 6. 鉛對汞離子偵測之干擾性 47 (二) 低濃度範圍汞離子之偵測 49 1. 不同陽極剝除伏安法之比較 49 2. 方波伏安法參數和預濃縮電位之探討 52 (1) 十二碳烷銨插層SWa-1鍍金修飾電極 52 (2) 十四碳烷銨插層SWa-1鍍金修飾電極 55 (3) 十六碳烷銨插層SWa-1鍍金修飾電極 55 二、烷銨插層多鐵蒙特石鍍金修飾電極對汞離子之偵測 60 (一) 於三種土系之土壤抽出液找出最佳電極 60 1. 大里系土壤 (Tali) 60 2. 吳厝系土壤 (Wutso) 62 3. 秀水系土壤 (Shiushui) 63 (二) 添加Hg(II) 於湖水和地下水 67 (三) 添加Hg(II) 於秀水系土壤抽出液 67 三、烷銨插層多鐵蒙特石鍍金修飾電極對土壤汞之偵測 73 (一) 偵測台灣耕地土壤樣品並和汞分析儀作比較 73 (二) 不同配位基對烷銨插層黏粒鍍金修飾電極測定汞離子之影響 84 1. EDTA 84 2. 草酸 (Oxalic acid) 84 3. 檸檬酸 (Citric acid) 85 4. 水楊酸 (Salicylic acid) 86 5. 腐植酸 (Humic acid) 86 結 論 92 參考文獻 93 附 錄 115zh_TW
dc.subjectalkylammonium-intercalated clayen_US
dc.titleElectroanalytic Reactions of Mercury Ions Using Clay-modified Electrodesen_US
dc.typeThesis and Dissertationzh_TW
item.openairetypeThesis and Dissertation-
item.fulltextno fulltext-
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