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姓名	謝姿渝(Tzu-Yu Hsieh)  查詢紙本館藏	畢業系所	化學工程與材料工程學系
論文名稱	聚合物-奈米粒子複合材料在玻璃轉移溫度下的結構與動力學相關性之實驗與模擬研究 (Combined Experimental and Computational Study of Structure-Dynamics Correlations for Polymer-Nanoparticle Composites Across The Glass Transition Temperatures)
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摘要(中)	聚合物-無機奈米顆粒複合材料通常表現出優於其原本單一成分的材料 性能，所以獲得廣泛的應用。然而，許多科學和技術問題仍未得到解決， 特別是複合材料的動態行為及其與微觀結構的相關性。在這項研究中，我 們目的在透過實驗和模擬解決動力學和結構相關性發展的問題。 實驗上，將在兩種分子量的聚(2-乙烯基吡啶) (P2VP)聚合物基質中的 乙醯丙酮鈀(Pd(acac)2)還原成鈀(Pd)，形成奈米顆粒複合材料。利用熱微差 掃描分析儀、流變學以及小角度和廣角 X 光散射儀，分析了在溫度高過玻 璃轉移溫度下，Pd 濃度和 P2VP 分子量會如何影響複合材料的動力學和結 構-動力學相關性。在模擬上，我們使用分子動力學模擬在各種條件下的結 構和分子運動，從中可以得到聚合物鏈的迴轉半徑(Rg)、玻璃轉化溫度 (Tg)和均方位移(MSD)。 綜合模擬和實驗的結果，我們希望深入了解複合材料的結構和動力學 如何相互關聯，以及這些微觀尺度的相關性如何決定宏觀尺度的材料特 性。本研究確定由還原反應製備出 Pd NPs，並使用 SAXS 分析樣品形態， 符合預期的模型及分散性。後續使用 DSC 分析熱性質，隨著分子量與 Pd(acac)2濃度的提高，Tg 也會有增加的趨勢。最後使用流變儀分析不同濃 度下的運動行為。在模擬中加入吸引的作用力均會有和實驗相符的趨勢出 現，而沒有吸引力的系統則與實驗不符，所以我們發現在聚合物和奈米粒 子間有吸引力的存在，使這些樣品顯現出這樣的熱性質與動態性質。
摘要(英)	Polymer-inorganic nanoparticle composites exhibit materials properties superior to their constituents and thereby enable a wide range of applications. However, many scientific and technical issues remain unaddressed, especially the dynamic behaviors of the composites and their correlation with the microscopic structures, which are practically important due to their influences on materials processing and production. In this research, we aim to address the issues evolving around the dynamics and structure-dynamics correlations via experiments and simulations. Experimentally, by in-situ reduction of metal salts (Palladium (II) acetylacetonate) dispersed in a polymer matrix, we are able to prepare nanocomposites of palladium (Pd) nanoparticles embedded in the polymer, poly(2-vinyl pyridine) (P2VP), featured with different Pd loadings and polymer molecular weights (MWs). By exploiting differential scanning calorimetry, rheology, and small- and wide-angle X-ray scattering, we explore how variations in Pd loadings and P2VP MWs (below and above the entanglement MW) affect the dynamics and structure-dynamics correlations of the composites at temperatures across the glass transition temperature. Computationally, molecular-dynamics simulations are employed to examine the structures and molecular motions of the composite systems under a variety of conditions, from which the radius of gyration of the polymer chains, glass transition temperature and the mean-square displacement of the polymer chains are calculated. Integrating the results from the simulations and experiments, we expect to develop insights on how the structures and dynamics of the composites correlate iii with each other and how these correlations in the microscopic scale dictate materials properties in the macroscopic scale. In this study, it was determined that Pd NPs were prepared by the reduction reaction, and the sample morphology was analyzed by SAXS, which was in line with the expected model and dispersion. And in the simulation, adding the attraction interaction in the systems would have a dispersion that was consistent with the experiment. Then using DSC to analyze thermal properties shows that with increasing the molecular weight and Pd(acac)2 concentration, Tg will also increase. Last, using a rheometer to analyze the motion behavior, with increasing the concentrations of the Pd(acac)2, the motion become slow. Finally, adding an attractive interaction in the simulation will have a consistent trend with the experiment, and these properties are due to the attractive interaction between polymers and nanoparticles in the samples
關鍵字(中)	★ 奈米顆粒複合材料	關鍵字(英)
論文目次	摘要 i Abstract ii 誌謝 iv 目錄 v 圖目錄 viii 表目錄 xiii 第一章 緒論 1 1.1 簡介 1 1.2 研究目的及動機 2 第二章 文獻回顧 3 2.1 複合材料 3 2.2 奈米複合材料 4 2.3 金屬奈米複合材料之發展和重要性 4 2.4 金屬奈米複合材料的應用 5 2.4.1 催化劑 6 2.5 奈米複合材料的製備技術 6 2.5.1 Ex situ技術 7 2.5.2 In situ技術 7 2.6 聚合物無機奈米粒子複合材料的性質 8 2.7 P2VP與Pd之簡介 11 2.8 分子動力學模擬的目標與發展 16 2.9 LAMMPS (Large-scale Atomic/Molecular Massively Parallel Simulator) 17 2.9.1 LAMMPS 簡介 17 2.9.2 使用 LAMMPS 進行 MD 模擬的方法 18 2.9.3 LAMMPS的應用 20 第三章 實驗與模擬方法 23 3.1 樣品製備 23 3.2 分析用儀器原理介紹 24 3.2.1 小角度與廣角Ｘ光散射儀 24 3.2.2 熱微差掃描分析儀 27 3.2.3 真空壓合機與流變儀 29 3.3 模型架構與參數設定 34 3.3.1 聚合物系統 34 3.3.2 聚合物加奈米粒子系統 43 第四章 結果與討論 53 4.1 分散與結構 (Dispersion and structure) 53 4.1.1 SAXS分析 53 4.1.2 模擬分析 59 4.2 熱性質(Thermal properties) 63 4.2.1 DSC分析 63 4.2.2 模擬分析 65 4.2.3 綜合模擬與實驗討論熱性質 70 4.3 流變性質 72 4.3.1 流變儀分析 72 4.3.2 模擬分析 75 4.3.3 綜合模擬與實驗討論動態性質 81 第五章 結論 82 參考文獻 83
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指導教授	陳儀帆(Yi-Fan Chen)	審核日期	2022-9-19
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