我們提出了一套氣相電場分離方法，來鑑定奈米氧化石墨烯(Graphene oxide)、孔性金屬-有機配位聚合物(Metal-organic frameworks)和陶瓷奈米材料(Ceramic nanoparticle)膠體懸浮液。在我們的研究中，電噴灑式氣相奈米粒徑分析儀(electrospray-differential mobility analysis，ES-DMA)除了能用來取得膠體奈米材料的數量濃度與物理尺寸的資訊外，其亦能用於分析粒子的解體(de-aggregation)與解聚(dis-assembly)現象之可逆過程、及配體-奈米粒子間交互作用對其膠體穩定性的影響。同時，TEM與SEM亦被我們用於觀察這些非球型奈米粒子的影像資訊，並對ES-DMA的結果予以佐證。結果顯示解聚、解體與聚集(aggregation)現象的發生與奈米材料的表面電位(zeta potential)和等電點(isoelectric point)、所使用配體的酸解離常數(pKa)和環境的酸鹼值有強烈的關聯性。透過調整這些影響因素，我們就能控制其粒徑大小與分佈區間。因此，這個方法能成功地對這些非球型奈米粒子進行定量分析，並期許它能提供液相配方化學合成和氣溶膠科學的研究一個前進未來的方向與動力。

We report a state-of-the-art gas-phase electrophoresis method for the characterization of nanosheet graphene oxide, metal-organic frameworks (MOF), and ceramic nanoparticle aggregates in the form of nanomaterial suspension. In this study, electrospray-differential mobility analysis (ES-DMA) is used to quantify number concentration and dimensional properties, analyze the reversibly dis-assembly and de-aggregation processes and ligand-nanoparticle interactions to colloidal stability of nanomaterial. Transmission electron microscopy and scanning electron microscopy are employed orthogonally to provide complementary data and imagery of nanomaterial. Results show that the equivalent mobility sizes, size distributions, and number concentrations of these functional nanomaterials are able to be successfully measured by ES-DMA. Aggregation, de-aggregation, and dis-assembly processes of nanomaterial colloids are strongly correlated to the zeta potential and isoelectric point of nanomaterials, dissociation constant of the functional ligands, and the pH in the environment, providing an effective route to control the primary size as well as the size homogeneity. This prototype study demonstrates a proof of concept of using ES-DMA to quantitatively characterize nonspherical functional nanomaterials. The results provide beneficial guidelines for the aqueous formulation chemistry of nanomaterial-based platforms (e.g., metalation in MOF) and the subsequent electrospray-assisted device integration.

誌謝 I
摘要 III
Abstract IV
目錄 V
圖目錄 VII
表目錄 IX
第 1 章 緒論 1
1-1 分散式非球型奈米材料之簡介 1
1-2 非球型奈米材料之簡介 2
1-2.1 氧化石墨烯(Graphene Oxide，GO) 2
1-2.2 孔性金屬-有機配位聚合物(Metal-organic framework，MOF) 3
1-2.3 奈米陶瓷材料-二氧化矽(SiO2)、二氧化鈦(TiO2)與二氧化鈰(CeO2)與配體(ligands) 4
1-3 非球型奈米材料在當今所遇到之困難與挑戰 5
1-3.1 奈米級氧化石墨烯（N-GOs）之物理性質與其應用性之關聯 5
1-3.2 孔性金屬-有機配位聚合物(MOF)之鑑定方法與穩定性之影響 7
1-3.3 奈米陶瓷材料與配體之交互作用與其對環境健康安全之影響 9
1-4 研究方法與目的 10
第 2 章 實驗方法 12
2-1 實驗藥品 12
2-2 樣品準備方式 13
2-2.1 N-GOs膠體溶液樣品製備方式 13
2-2.2 MOF-525膠體溶液樣品製備方式 14
2-2.3 TiO2、SiO2和CeO2膠體樣品與配體參雜樣品之製備方式 15
2-3 實驗儀器 16
2-4 實驗儀器原理及方法 17
2-4.1 電噴灑式氣相奈米粒子流動分析儀 17
2-4.2 穿透式電子顯微鏡(TEM)與掃描式電子顯微鏡(SEM) 20
第 3 章 結果與討論 22
3-1 N-GOs在ES-DMA系統下之表現 22
3-1.1 N-GOs的流動粒徑分布圖 22
3-1.2 數量濃度、過濾對N-GOs的穩定性影響 24
3-1.3 N-GOs的平面長度 27
3-1.4 資料分析的優勢和限制 31
3-1.5 N-GOs研究之總結 32
3-2 MOF-525之粒子與晶體結構於酸鹼環境下之變化與探討 33
3-2.1 MOF-525之氣動粒徑分佈 33
3-2.2 MOF-525膠體溶液在不同酸鹼環境下所受到之影響 35
3-2.3 MOF-525晶體結構變化之機制與可逆性探討 38
3-2.4 MOF-525研究之總結 42
3-3 SiO2-NP、TiO2-NP和CeO2-NP與配體間之相互作用與影響 43
3-3.1 未擔載配體之奈米粒子(unconjugated nanoparticle)的各項性質探討 43
3-3.2 配體與奈米粒子於表面之相互作用與影響 47
3-3.3 配體-奈米粒子之交互作用與穩定性探討 50
3-3.4 配體-奈米粒子之結果統整與分析 60
3-3.5 Ligands與TiO2-NPs、SiO2-NPs和CeO2-NPs研究之總結 65
第 4 章 結論 66
第 5 章 未來展望 67
第 6 章 參考文獻 68

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