在本研究中設計及合成各種不同新穎性功能性自組合膽固醇液晶材料，包括(1)含膽固醇基團的側鏈型液晶高分子；(2)具有光致變性的特殊液向型膽固醇液晶材料；(3)轉印膽固醇液晶分子排列的非對掌性高分子網狀結構及(4)含有高螺旋扭轉能力對掌性鏈段的主鏈型液晶高分子。探討對掌效應、溶劑效應、溫度致變性或光致變性分別對於不同膽固醇液晶材料的選擇性光反射之影響，並研究其顏色可調變的特性。此外，利用簡便的方式以功能性高分子如膽固醇液晶高分子或兩性雙團聯式共聚高分子來製備不同形式的銀奈米材料，包括高分子-奈米銀複合材料、包埋奈米銀顆粒的高分子纖維及銀奈米線，並探討其性質。對於實驗中所合成的單體及高分子材料利用紅外光光譜儀(FT-IR)、核磁共振光譜儀(1H NMR)及元素分析(EA)來鑑定其分子化學結構。而各功能性材料的熱性質與光學特性則利用差式掃描熱分析儀(DSC)、熱重分析儀(TGA)、紫外光-可見光光譜儀(UV-Vis)、X光繞射儀(XRD)及偏光顯微鏡(POM)來分析。銀奈米材料的型態則藉由掃描式電子顯微鏡(SEM)及穿透式電子顯微鏡(TEM)觀察。

本論文共包含五個部份。第一部份中，合成新穎性含膽固醇基團的單體並以不同比例與液晶單體共聚合；對於單體混合系統與共聚合系統，當膽固醇單體含量分別為10~25及15~75 mol%時，具有可見光的選擇性光反射，且隨著溫度增加而藍位移；而利用在不同溫度下對高分子反射薄膜作急速冷卻可得到穩定的色彩薄膜。第二部份中，首度發現特殊的液向型膽固醇液晶系統於所合成的光致變性cinnamoyl液晶單體在適當溶劑中，對於溶劑或蒸氣的感測應用上可顯示不同的光學特性；此外，對於所表現的可調變之選擇性光反射，升高溫度會造成可逆的波長藍位移；而UV光照射則會導致分子異構化引發不可逆的藍位移。第三部份中，我們構想出利用非對掌性及非液晶的高分子網狀結構誘導膽固醇液晶的方式，並顯示出選擇性光反射的光學特性；利用導入不同折射率的向列型液晶於此網狀結構中可達到多彩反射的效果。第四部份中，利用縮合劑p-TsCl/Py/DMF進行含有高HTP的對掌性鏈段及液晶元結構的聚縮合反應，合成新穎性主鏈型膽固醇聚酯，並利用in situ熱還原反應製備含有5~10 nm奈米銀顆粒於膽固醇液晶高分子中的奈米複合材料；各材料皆表現出高的熱穩定性及寬廣的膽固醇液晶相範圍；而奈米銀顆粒的存在會使得膽固醇液晶聚酯的選擇性光反射發生紅位移並提高對溫度效應的影響；此新穎性液晶高分子-奈米銀複合材料可能在異方性導電性或光學特性具有高度應用性。第五部份中，利用ATRP及水解程序所合成的兩性雙團聯式共聚高分子PMMA-b-PMAA形成逆微胞來合成奈米銀顆粒，並配合氧化鋁模板進一步製備包埋奈米銀顆粒的高分子纖維及銀奈米線，可應用在奈米電子元件上的連接裝置。

The novel functional materials based on self-assembled cholesteric liquid crystals in various types, including (1) side-chain cholesteric liquid crystalline polymers containing cholesteryl pendant groups; (2) photochromic cholesteric liquid crystalline monomers with unconventional lyotropic properties; (3) cholesteric liquid crystalline-imprinted architectures on achiral non-liquid crystalline polymer networks; and (4) main-chain cholesteric liquid crystalline polyesters containing high HTP isosorbide segments, were designed and synthesized. The chiral effect, solvent effect, thermochromic effect, and photochromic effect on the selectively reflective colors of various cholesteric liquid crystalline materials were explored, and the color-tunable properties of these functional materials were investigated. In addition, the characterizations of the nanomaterials in the forms of polymer-silver nanocomposites, silver nanoparticle-embedded nanofibers and silver nanowires which were fabricated using convenient methods in functional polymers such as cholesteric liquid crystalline polyester and amphiphilic diblock copolymer were studied. The chemical structures of the synthesized monomers and polymers were identified using FT-IR, 1H NMR, and elemental analyses. The characterizations of thermal and optical properties of these functional materials were analyzed using DSC, TGA, UV-Vis, XRD, and POM. The morphologies of nanomaterials were observed from SEM and TEM analysis.

This thesis consists of five parts: In Part I, a new cholesteryl-containing liquid crystalline monomer was synthesized and copolymerized with an achiral liquid crystalline monomer in various molar ratios. The selective reflection in the region of visible light could be observed at cholesteric liquid crystal phase for monomer mixtures and copolymers containing about 10-25 mol% and 15-75 mol% cholesteryl units, respectively. As the temperature increased, the variation of reflection wavelength for both systems revealed blue-shifts. Stable colorful reflective patterns or color recordings can be obtained through quenching the copolymers from various temperatures. In Part II, the unique lyotropic properties of cholesteric liquid crystals were first discovered for the synthesized monomers containing a functional photochromic cinnamoyl group, which were mixed with proper solvents in the suitable ratio. It is believed that the novel materials have great potential in application for the sensor of solvent or solvent vapors. In addition, the tunable colorful selective reflection properties of lyotropic cholesteric liquid crystals exhibit a reversible blue shift with increasing the temperature, and an irreversible blue shift upon around 20 min of UV exposure. In Part III, we conceived a new methodology for preparing achiral non-liquid crystalline polymer networks with the performance to induce cholesteric liquid crystals with selective light reflection from flash nematic liquid crystals in the absence of chiral dopants. In addition, the tunable colorful patterns can be achieved by refilling the nematic liquid crystals with various refractive indices into the polymer networks. In Part IV, new main-chain cholesteric liquid crystalline polyesters containing high HTP isosorbide segments were synthesized by direct polycondensation using p-TsCl/Py/DMF as a condensing agent. The cholesteric liquid crystalline polyester composites containing 5~10 nm of silver nanoparticles was prepared by in situ thermal reduction of silver complex. The cholesteric liquid crystalline polyesters and nanocomposite exhibited high thermal stability and wide temperature range of cholesteric liquid crystal phase. The presence of 1 wt% silver nanoparticles in cholesteric liquid crystalline polyesters caused a red shift of selective light reflection band and presented more temperature dependence on reflected light. It is believed that the novel materials of cholesteric liquid crystalline polyester-silver nanocomposites might have great potential to possess the increased electrical conductivity and the unique anisotropic electric and optical properties. In Part V, an amphiphilic diblock copolymer (PMMA-b-PMAA) which was synthesized using ATRP and a hydrolysis process was used as a surfactant to prepare reverse micelles for the fabrication of silver nanoparticles. PMMA-silver nanocomposite fibers were then fabricated through photopolymerization of mixtures of MMA and silver nanoparticles in an anodic aluminum oxide template. After sintering of silver nanoparticle-embedded PMMA fibers at 500°C, the fabrication of silver nanowires can be achieved. These 1D nanostructures of silver metals might display highly potential functions as anisotropic interconnections in fabricating nanoscale electronic devices.

Ch2

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