單粒子感應耦合電漿質譜儀( Single Particle ICP-MS，SP-ICP-MS )是一種檢測及量化奈米粒子的新興技術，能夠提供元素組成、粒徑分布、數目濃度等資訊。
第一部分研究將以單粒子感應耦合電漿質譜儀對民生用品中的銀奈米粒子釋放量及化學試劑中的銀奈米粒子含量進行分析。研究中使用氣動式霧化器 (Pneumatic Nebulizer，PN )、超音波霧化器(Ultrasonic nebulizer，USN )、薄膜去溶劑系統( Membrane desolvation introduction system，ARIDUS)，探討不同進樣系統於銀奈米粒子的分析特性。實驗中探討進樣系統參數、取樣時間、傳輸效率後，使用最適化條件進行分析結果顯示使用USN因具有去溶劑的功能以及較高的霧化效率有較佳偵測極限結果，此方法對銀奈米粒子粒徑偵測極限為18 nm;數目濃度偵測極限為36 particles mL-1。實驗中使用陽離子交換樹酯(Chelex-100)管柱線上結合SP-ICP-MS進行分析以去除大量銀離子干擾，且在高濃度的共存陽離子 (Na+、K+、Ca2+、Mg2+) 環境下Chelex-100仍然有良好的去除銀離子效果。最後使用USN-SP-ICP-MS對於市售口罩、食品保鮮袋、濾水器中的銀奈米粒子釋放量進行探討以及分析化學試劑中的銀奈米粒子含量及型態，並且搭配穿透式電子顯微鏡進行實驗結果驗證。
第二部分使用超音波霧化器連接SP-ICP-MS分析化學試劑中氧化鐵奈米粒子，搭配使用動態反應室(Dynamic reaction cell，DRC)，選擇氨氣為反應氣體以減輕分子離子40Ar16O+干擾，實驗中探討進樣系統參數、奈米粒子濃度、傳輸效率。使用最適化條件進行分析後顯示方法的粒徑偵測極限為16 nm；數目濃度偵測極限為36 particles mL-1。實驗中使用陽離子交換樹酯(Chelex-100)管柱線上結合SP-ICP-MS進行分析以去除大量鐵離子干擾，且在高濃度的共存陽離子 (Na+、K+、Ca2+、Mg2+) 環境下Chelex-100仍然有良好的去除鐵離子效果。最後將此方法運用於分析化學試劑中的氧化鐵奈米粒子含量及型態，並且搭配穿透式電子顯微鏡進行實驗結果驗證。

Single particle ICP-MS (SP-ICP-MS) is promising technique for nanoparticle characterization in its ability to provide information on elemental composition, nanoparticle size, size distribution and number concentration.
The first research, determination of silver nanoparticles (AgNPs) in daily commodities and chemical solvents based on single particle detection by ICP-MS was studied. In the experiment, the analytical performance of three sample introduction systems, a pneumatic nebulizer (PN), a ultrasonic nebulizer (USN) and a membrane desolvation introduction system (ARIDUS), was compared for the characterization of AgNPs and the system parameters, nanoparticle concentration and transport efficiency, were investigated. Using optimal conditions, the results showed that USN had better performance due to its ability to remove solvents and enhance nebulization efficiency. Size detection limit was 18 nm and number concentration detection limit was 36 particles mL-1. Using online coupling of cation exchange column (Chelex-100) with SP-ICP-MS successfully removed interfering silver ions and in condition of high concentration cations (Na+、K+、Ca2+、Mg2+), the remove efficiency of silver ions was still well. This method was applied to masks, food storage bags, water filters and chemical solvents. Finally, size measurements performed by SP-ICP-MS were validated by transmission electron microscopy measurements.
The second research, determination of iron oxide nanoparticles (Fe3O4 NPs)in chemical solvents by USN-SP-ICP-MS was studied. The interfering 40Ar16O+ ions were reduced by using NH3 as reaction cell gas. In the experiment,the USN system parameters, nanoparticle concentration and transport efficiency were investigated. Using optimal conditions, the results showed that size detection limit was 16 nm and number concentration detection limit was 36 particles mL-1. Using online coupling of cation exchange column (Chelex-100) with SP-ICP-MS successfully removed interfering iron ions even if the solution was in condition of high concentration cations. Eventually, this method was applied to chemical solvents and size measurements performed by SP-ICP-MS were validated by transmission electron microscopy measurements.

論文審定書 i
謝誌 ii
摘要 iii
Abstract iv
目錄 vii
圖目錄 ix
表目錄 xii
第一章 單粒子感應耦合電漿質譜儀於民生用品與化學試劑中銀奈米粒子之分析
壹、前言 1
一、研究背景 1
二、單粒子感應耦合電漿質譜儀簡介 4
貳、實驗部分 7
一、儀器裝置及操作條件 7
二、試藥及溶液的配製 9
參、實驗過程 13
一、進樣系統操作條件之最適化 13
二、取樣時間之最適化 13
三、銀奈米粒子濃度與傳輸效率之探討 13
四、銀奈米粒子粒徑分析 14
五、銀奈米粒子數目濃度分析 14
六、銀奈米粒子標準品之分析驗證 15
七、陽離子交換樹脂之探討 15
八、樣品製備與分析 16
肆、結果與討論 18
一、進樣系統操作條件之最適化 18
二、取樣時間之最適化 29
三、銀奈米粒子濃度與傳輸效率之探討 29
四、銀奈米粒子粒徑分析 30
五、銀奈米粒子數目濃度分析 41
六、超音波霧化器優點 44
七、銀奈米粒子標準品之分析驗證 46
八、陽離子交換樹脂之探討 48
九、真實樣品之分析應用 53
伍、結論 69
陸、參考文獻 70
第二章 單粒子感應耦合電漿質譜儀於化學試劑中氧化鐵奈米粒子之分析
壹、前言 76
一、研究背景 76
二、動態反應室簡介 78
貳、實驗部分 80
一、儀器裝置及操作條件 80
二、試藥及溶液的配製 83
參、實驗過程 84
一、DRC系統之最適化 84
二、超音波霧化器操作條件之最適化 85
三、動態反應室對單粒子分析之影響 85
四、氧化鐵奈米粒子濃度與傳輸效率之探討 85
五、氧化鐵奈米粒子粒徑分析 85
六、氧化鐵奈米粒子數目濃度分析 86
七、陽離子交換樹脂之探討 87
八、樣品製備與分析 87
肆、結果與討論 89
一、DRC系統之最適化 89
二、超音波霧化器操作條件之最適化 93
三、動態反應室對單粒子分析之影響 97
四、氧化鐵奈米粒子濃度與傳輸效率之探討 100
五、氧化鐵奈米粒子粒徑分析 100
六、氧化鐵奈米粒子數目濃度分析 101
七、陽離子交換樹脂之探討 106
八、真實樣品之分析應用 109
伍、結論 120
陸、參考文獻 121

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