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研究生：	李寶萌 Lee, Pao-Meng
論文名稱：	多功能雙邊不對稱球體之共自組裝行為及其螢光共振能量轉移感測機制之研究 Co-assembly of Multi-functionalized Janus Particles & the FRET-based Sensing Mechanism
指導教授：	郭昌恕 Kuo, Chang-Shu
學位類別：	碩士 Master
系所名稱：	工學院 - 材料科學及工程學系 Department of Materials Science and Engineering
論文出版年：	2019
畢業學年度：	107
語文別：	英文
論文頁數：	111
中文關鍵詞：	雙邊不對稱球體、多功能、中孔洞、專一性共同自組裝、螢光共振能量轉移、吸收度、螢光
外文關鍵詞：	Janus particles, Multi-functionality, Mesoporous silica, Specific co-assembly, FRET, Absorbance, Fluorescence
相關次數：	點閱：149 下載：0
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由本實驗室所製備的兩種半球體螢光染料官能化之中孔洞雙邊不對稱球體，分別作為施體與受體來進行共同自組裝行為之研究。分別以具有磁性與否之粒徑480奈米的中孔洞二氧化矽球體作為主體材料，經由蝕刻形成的中孔洞二氧化矽球體使之增加表面官能基密度。經由氨基官能化改質三分之一半球表面形成雙邊不對稱球體，並在相同的三分之一表面分別接上名為Atlantic Blue或Di-4-ANEPPS的螢光染料。另外，使用聚苯乙烯奈米微珠作為共同自組裝行為的另一項材料，其平均粒徑為100奈米且帶有羧酸化表面官能基。Atlantic Blue與Di-4-ANEPPS官能化的雙邊不對稱球體分別作為螢光共振能量轉移配對中的施體和受體。
　　由480奈米帶有正電荷之雙邊不對稱球體與100奈米帶有負電荷聚苯乙烯微珠在水溶液中透過靜電荷相互作用進行共同自組裝行為，且用磁鐵對於形成共同自組裝之聚合體進行再分離步驟。而螢光共振能量轉移的現象，來自於球體之共同自組裝行為使施體與受體之雙邊不對稱球體靠近產生的結果。這些球體的共同自組裝行為藉由動態光散射粒徑分析儀來觀測，透過紫外光-可見光分光光譜儀與螢光光譜來定量及分析自組裝聚合體之組成。藉由365奈米之入射光去激發施體雙面不對稱球體，可以觀察到位於630奈米波段之受體雙面不對稱球體因能量轉移所產生的放射波長，以此證實螢光共振能量轉移的發生。在這些獨特的共同自組裝行為的過程中，研究與討論對於不同比例之雙邊不對稱球體與聚苯乙烯奈米微珠之間的定量分析和螢光共振能量轉移效率。

For the FRET sensing platform, two kinds of mesoporous Janus particles hemispherically-functionalized with fluorescence dyes were fabricated as donor and acceptor in a unique co-assembly system. Mesoporous silica particles with diameter of 480 nm were used as the core materials. The mesoporous silica particles with magnet nanoparticles in pores were used as the magnetic core materials, which the magnetic manipulation in the co-assembly system. Janus particles were first functionalized with amino-silane on 1/3 hemispheric surfaces, followed by the fluorescent donor and acceptor dye attachments to the same 1/3 hemisphere. Polystyrene beads with diameter of 100 nm and carboxylic surface-functionalities were utilized as the co-assembly counterpart. Both Janus particles served as the donor/acceptor pair for the FRET (Forster Resonance Energy Transfer).
Co-assembly process was carried out in an aqueous solution by using the positively-charged 480nm Janus particles and the negatively-charged 100nm polystyrene beads via the electrostatic interaction. FRET occurred in the co-assembled cluster, where the donor Janus particles and the acceptor Janus particles were brought very close. Co-assembly structure of these particles were monitored by the dynamic light scattering (DLS). The formation of assembled clusters was quantified and analyzed the UV-vis and PL spectra. FRET was confirmed by excitation at 365nm to donor Janus particles, which can observe the energy transfer to the acceptor Janus particles at 630nm emission. Particles quantification and FRET of these unique co-assembly process with different PS/JPs ratio was investigated.

中文摘要…………………………………………………………………………………….I
Abstract……………………………………………………………………………………III
致謝………………………………………………………………………………………..IV
Table of Contents	V
List of Tables	IX
List of Illustrations	X
Chapter1  Introduction	1
1	Janus Particles and Asymmetric micro- and nano-Materials	1
1.1	Janus-like Materials	2
1.2	Fabrication of Janus Particles	4
One-dimensional Electrospun Fibers as Particle Embedding Substrates	14
1.3	Application	16
2	Mesoporous Materials	19
2.1	Silicate Mesoporous Materials	20
2.2	Mechanism of Formation Mesoporous Materials	21
2.3	Applications	23
3	Particle Self-assembly	26
3.1	Introduction to self-assembly	26
3.2	Applications of Self-Assembly	27
4	Förster resonant energy transfer (FRET)	30
4.1	Mechanism	30
4.2	Applications	31
Chapter 2  Motivation	33
Chapter 3  Experimental	34
1  Chemicals	34
2  Instruments	36
3	Fabrication of Magnetic &Fluorescence Mesoporous Janus Particles	37
3.1  Preclean of 480nm silica particles	37
3.2  Fabrication of Mesoporous Silica Particles	37
3.3  Fabrication of Magnetic Silica Particles	37
3.4  TEOS sol-gel Process	38
3.5  Electrospinning of PMMA/P4VP Blend Fibers Mat	39
3.6  Adsorption of 480nm Silica Particles and Magnetic Silica Particles on Fibers	40
3.7  Thermal Embedding Process	40
3.8  1st APS Surface Modified Process	40
3.9  Dye Grafting Process	41
3.10  Adsorption of Di-4-ANEPPS mesoporous Silica Particles	43
3.11  2nd APS Surface Modified Process	44
3.12  The Process of TEOS Protection Layer	44
3.13  The Process of Wax Protection Layer	45
3.14  Polymer Fibers Dissolving Process	45
3.15  Dewaxing Process	45
3.16  Alkaline Cleaning Process	46
4	Analytical Instruments	48
4.1  Dynamic Light Scattering (DLS)	48
4.2  Zeta Potential Measurement	48
4.3  Optical Microscope (OM)	50
4.4  Scanning Electron Microscope (SEM)	50
4.5  UV-visible Spectrometer	50
4.6  Photoluminescence Spectroscopy (PL)	51
4.7  Photoluminescence Optical System	52
Chapter 4 	Result and Discussion	53
1 	Synthesis of Mesoporous Silica Particles	53
1.1  Surface-Protected Etching Process	53
1.2  Influence of Reaction Time on Etching Process	54
2  Fabrication and Characterization of Multi-functionalized Mesoporous Janus Particles	57
2.1  Fabrication of Magnetic Particles	57
2.2  Sol-gel of TEOS layer on silica particles	61
2.3  Protection Layer of TEOS via CVD Process	62
2.4  Dye-functionalization and Optical Properties of Janus Particles	66
2.5 	Quantification on Dye-functionalized Janus Particles	68
3 The Co-assembly Behavior of Janus Particles and 100nm Polystyrene	75
3.1 Electrostatic Interaction	75
3.2  Amount of Amino-group on Dye-functionalized Janus Particles	80
3.3  Assembly for Two Dye-functionalized Janus Particles	82
3.5 Quantification for Dye-functionalized Janus Particles via Absorbance Measurement during Assembly Process	86
4  FRET Effect of Specific Co-assembly of Janus Particles	93
4.1  Specific Interaction Co-assembly and FRET Effect of Janus Particles	93
4.2  Lifetime Measurement of Assembled Janus Particles	101
Chapter 5  Conclusions	103
Chapter 6  Reference	104
                                    

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