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研究生: 曾于珊
Yu-Shan Tseng
論文名稱: 利用相分離機制以磷灰石奈米粒子備製新型多孔複合材料
Novel fabrication of porous network structure by hydroxyapatite particles from phase separation mechanism
指導教授: 洪伯達
Po-Da Hong
口試委員: 洪伯達
Po-Da Hong
戴子安
Chi-An Dai
白孟宜
Meng-Yi Bai
學位類別: 碩士
Master
系所名稱: 工程學院 - 材料科學與工程系
Department of Materials Science and Engineering
論文出版年: 2022
畢業學年度: 110
語文別: 英文
論文頁數: 57
中文關鍵詞: 微/奈米複合材料界面堵塞乳液凝膠滲流堵塞轉變相分離氫氧基磷灰石氨丙基三乙氧基矽烷表面改質
外文關鍵詞: Hydroxyapatite, APTS, Modification, Surface science, Bijel, Percolation, Jamming transition, Phase separation
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本研究嘗試由水/2,6-二甲基吡啶相分離系統組成之雙連續界面堵塞乳液凝膠( Bicontinuous Interfacially Jammed Emulsion Gels, Bijel ),結合化學改性的羥基磷灰石(HAp)奈米粒子網目製造一新型雙連續滲流軟材料。首先為了拓展奈米粒子的功能性,特別用氨丙基三乙氧基矽烷(APTS)修飾表面以得疏水HAp-APTS。這種化學修飾可做為染料連接劑,也能進一步被其他生物活性分子功能化。在控制溫度的情况下,觀察到隨相分離後界面出現,粒子聚集、形成網目能有效減緩兩相成長粗化。接著為了進一步了解粒子網目形成時「相分離動力學」與「相疇幾何」的複雜互動,紀錄該Bijel系統在不同粒子參數(粒徑和濃度)下隨時間的相疇尺寸演變。最後藉由聚乙二醇二丙烯酸酯(PEGDA)的選擇性光固化,強化由HAp-APTS 網目形成的微米尺度Bijel 模板。即能在維持結構型態的前提下,為後續不同應用領域精準設計高比表面積且相疇尺寸可控制的多孔結構。


In this research, we have tried to fabricate the Bicontinuous Interfacially Jammed Emulsion Gels (Bijel) by adding the modified hydroxyapatite particles, which could be applied to be the candidate for the principal component of human bones to polymer mixtures. Firstly, hydroxyapatite (HAp) particles were synthesized by a simple one-step method followed by rapid surface modification with aminopropyltriethoxysilane (APTS). This chemical modification would enhance the degree of functionalization, and it can be precisely controlled and reproduced via the APTS concentration and the treatment time. Furthermore, functionalized hydroxyapatite (HAp-APTS) nanoparticles with amino groups on the surface could also act as the dye linker to further apply bioactive molecules. Under controlled temperature, it was observed that the network formed by the aggregation of particles with the emergence of the interface after phase separation effectively slowed down the coarsening of the two-phase growth. Then, to further understand the complex interaction between "phase separation kinetics" and "phase geometry" during the formation of particle network, the evolution of the characteristic length scale of the Bijel system was recorded over time for different particle parameters (particle size and concentration). Finally, the micron-scale Bijel formed by the HAp-APTS network is enhanced by selective photopolymerization of polyethylene glycol diacrylate (PEGDA). This enables the precise design of porous structures with high specific surface area and a tunable phase dimension for subsequent applications while maintaining the structural form.

Abstract II Acknowledgment III Contents IV Chart Catalogues VI Principal Notation IX Chapter 1. Introduction 10 1.1. Composites 10 1.2. Emulsions 10 1.3. Particles and Wettability 11 1.4. A special emulsion: the Bijel 14 1.5. Bijel Fabrication: Spinodal Decomposition 15 1.6. Post-Processing and Applications 17 1.7. The Purpose of This Thesis 21 Chapter 2. Materials and Experiments 22 2.1. Samples Preparation 22 2.1.1. Materials 22 2.1.2. HAp Nanoparticles Modification 23 2.1.3. Fabrication of Bijel 23 2.1.4. Photo-polymerization in Bijel 24 2.2. Methods 25 2.2.1. Dynamic Light Scattering (DLS) 25 2.2.2. UV-VIS Spectrophotometer 25 2.2.3. Phase Contrast Microscope (PCM) 25 2.2.4. Contact Angle Analyzer 25 2.2.5. Scanning Electron Microscope (SEM) 25 2.2.6. Dark Field Microscopy 26 2.3. Surface Free Energy and Wettability of Nanoparticles 27 2.3.1. Contact Angle Measurement 27 2.3.2. Surface Free Energy Calculation 27 2.4. Microscopic image analysis 29 2.4.1. Image Processing 29 2.4.2. Image Interface Outline 30 Chapter 3. Results and Discussion 31 3.1. Hap-APTS nanoparticles Surface Modification 31 3.1.1. Presence of Coating 31 3.1.2. HAp Nanoparticles Surface Property 32 3.2. HAp-APTS nanoparticles characterization 37 3.3. Formation of Bijel 41 3.3.1. Demixing Behavior in the Presence of HAp-APTS 41 3.3.2. Parameters of Bijel’s design 44 3.3.3. Time-traced Morphology of the Bijel 46 3.4. Bijel’s application – Porous scaffold 48 Chapter 4. Conclusion 49 References 50

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