中孔洞二氧化矽奈米顆粒(MSNs)作為顯影劑的研究日益發展，而具中空形貌MSNs相較非空心MSNs有更高的藥物裝載量和降解速率。本論文以全氟癸烷官能基全表面修飾於中空MSNs，MMT-2，形成之F-MMT-2與文獻中的超疏水性非空心MSNs在慣性穴蝕效應劑量(ICD)上有相似的效果。為增加疏水顆粒於水中的分散性以及降解性，本研究進一步以3-(Trihydroxysilyl)propyl methylphosphonate, monosodium salt solution (THMP)或Carboxyethylsilanetriol, disodium salt (CES)嫁接於F-MMT-2外表面，同時藉由調控修飾程度，探討表面性質對ICD以及顆粒在水溶液中穩定性的影響，研究結果顯示所有顆粒皆於純水中穩定分散至少一天，而在離子濃度較高的磷酸鹽緩衝生理鹽水中，顆粒穩定性因表面電位下降以及二氧化矽溶解而隨時間下降。相較於全表面修飾全氟癸烷之顆粒，THMP或CES之修飾雖未改善疏水顆粒在磷酸鹽緩衝生理鹽水中的穩定性，但顆粒降解性明顯提高。
同時，本研究藉由於MMT-2外表面成長放射狀中孔洞二氧化矽層以改變表面粗糙度，並觀察其對ICD之影響。於顆粒全表面修飾全氟癸烷後之ICD結果顯示未經二次成長之F-MMT-2具有最高之ICD，而具有小於10 nm的孔洞之表面粗糙度變化對ICD之影響可忽略。

Recently, mesoporous silica nanoparticles (MSNs) as contrast agents have attracted significant attention due to their capacity for sustained cavitation duration under ultrasound irradiation. In this thesis, a type of hollow MSNs, designated as MMT-2, with ~110 nm diameter and Ia3d mesopore symmetry is modified with differrent functional groups for evaluating the effect of particle surface property on ultrasound bio-application efficacy. Functionalization of the outer surface with hydrophilic (phosphonate or carboxylic acid) group, followed by functionalization of hydrophobic (perfluorodecy group on the inner surface generate particles. Compared to the non-hollow and just perfluorodecy group functionalized counterpart MCM-48 reported by our group previously, the dual-functionalized MMT-2 particles had similar inertial cavitation dose (ICD) but degradated faster in phosphate buffered saline (PBS, pH = 7.4). Meanwhile, surface roughness of MMT-2 was modified by growing radial mesopore on the outer surface via an oil−water biphase stratification reaction system. The silica growth on MMT-2 did increase surface roughness, as indicated by increase of contact angle, yet the influence on ICD value was subtle.

摘要 I
Abstract II
目錄 III
圖目錄 VI
表目錄 IX
第一章 緒論 1
1-1 超音波效應與顯影劑 1
1-1-1 超音波效應...... 1
1-1-2 超音波顯影劑的發展 5
1-1-3 中孔洞二氧化矽奈米顆粒與超音波顯影劑 7
1-2 疏水材料 9
1-2-1 接觸角...... 10
1-2-2 介面奈米氣泡與慣性穴蝕效應 12
1-2-3 材料的疏水性 13
1-2-4 疏水材料在溶液中的分散性 15
1-3 中孔洞二氧化矽奈米顆粒 17
1-3-1 中空中孔洞二氧化矽奈米顆粒MMT-2簡介 17
1-3-2 中孔洞二氧化矽奈米顆粒與表面修飾 19
1-3-3 中空放射狀中孔洞二氧化矽奈米複合球 22
1-4 研究動機 26
第二章 實驗部分 27
2-1 實驗藥品 27
2-2 中孔洞二氧化矽的製備 29
2-2-1 MMT-2和MCM-48的合成 29
2-2-2 中空放射狀中孔洞二氧化矽奈米複合球的合成 29
2-3 嫁接官能基於中孔洞二氧化矽 30
2-3-1 全表面嫁接PFDTS 30
2-3-2 全表面嫁接THMP 31
2-3-3 全表面嫁接CES 31
2-3-4 選擇性表面嫁接THMP和PFDTS 31
2-3-5 選擇性表面嫁接CES和PFDTS 32
2-4 材料鑑定與分析方法 35
2-4-1 X光粉末繞射法 (Powder X-Ray Diffraction, PXRD) 35
2-4-2 29Si固態核磁共振光譜術(Solid State 29Si MAS NMR,29Si MAS NMR) 36
2-4-3 氮氣物理吸脫附法 (Nitrogen Physisorption) 37
2-4-4 掃描式電子顯微鏡 (Scanning Electron Microscopy, SEM) 41
2-4-5 穿透式電子顯微鏡 (Transmission Electron Microscopy, TEM) 41
2-4-6 接觸角測試儀(Contact Angle Meter) 42
2-5 慣性穴蝕效應偵測與分析 42
2-5-1 樣品配置 .....................................................................................................................42
2-5-2 慣性穴蝕效應偵測架構與操作方式 43
2-5-3 數值分析 .....................................................................................................................45
2-6 MMT-2的分散性及穩定性測試 46
2-6-1 動態光散射粒徑分析儀 (Dynamic Light Scattering ,DLS)與介面電位量測儀(Zeta Potential Analyzer) 46
2-6-2 在DI water中分散性測試 48
2-6-3 在DI water或PBS中穩定性測試 48
第三章 結果與討論 50
3-1 中孔洞二氧化矽的分析與鑑定 50
3-1-1 MMT-2及MCM-48 50
3-1-2 全表面修飾與選擇性修飾 52
3-2 MMT-2分散性和慣性穴蝕效應之研究 60
3-2-1 MCM-48與MMT-2於慣性穴蝕效應之比較 60
3-2-2 表面修飾程度對分散性之影響 62
3-2-3 表面修飾程度對慣性穴蝕效應之影響 64
3-3 MMT-2於DI water及PBS中穩定性之研究 67
3-3-1 MMT-2於DI water中的穩定性 67
3-3-2 MMT-2於PBS中的穩定性 76
3-4 中空放射狀中孔洞二氧化矽奈米複合球 92
3-4-1 中空放射狀中孔洞二氧化矽奈米複合球之鑑定 92
3-4-2 全表面修飾 96
3-4-3 粗糙度對慣性穴蝕效應之影響 99
第四章 結論 100
參考文獻 101

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