本論文探討輻射、溶劑與應力對高分子材料結構的影響，主要為探討高分子材料在受到輻射、溶劑與應力時，如何使材料結構產生變化，進而降低自由能，包含產生結晶，使分子鏈重新排列，消耗所獲得的熱能，產生表面結構進而抵銷表層與基材間材料性質的差異，改變分子鏈間距以容納溶劑的進入，以及在無法承受所被施加的應力時，形成表面裂縫，釋放其應力，內容包括以下四部分：
第一部分研究(第二章)未照射與照射紫外光的聚甲基丙烯酸羥乙酯(PHEMA)在去離子水內的質傳行為，其中使用Harmon模型對實驗結果進行模擬，實驗結果顯示去離子水在未照射與照射紫外光PHEMA的質傳行為是非常態的擴散(Anomalous diffusion)，同時包含Case I的擴散與Case II質傳，其中Case I擴散主要受由濃度梯度影響，而Case II質傳則是受高分子鏈是否容易應力鬆弛影響，而隨著劑量上升PHEMA Case I活化能與Case II活化能皆會上升，並使用DSC與FTIR觀察PHEMA在照射紫外光前後，玻璃轉換溫度與官能基的變化，實驗結果顯示，當照射紫外光會使PHEMA玻璃轉換溫度下降，且C=O與C-O鍵結強度下降，代表PHEMA產生斷鍵，第二部分探討不同紫外光照射劑量的PHEMA在吸收去離子水後，其表面在解吸(Desorption)後形成皺波的機制，由於照射紫外光後，會在表面形成表層薄膜(Skin layer)，其薄膜受紫外光影響而產生斷鍵，降低表層的楊氏係數，而在解吸過程中，表層薄膜解吸速度較快，而基材則會較慢，因此會在界面處形成張應力，並在表面形成皺波結構，其皺波的特徵波長(Characteristic wavelength, λc)會使用美國國家衛生研究院(National Insitute Health in USA, NIH)的開放軟體Image J，對皺波結構的OM圖進行傅立葉轉換，求出波數與波長，實驗結果顯示，初次浸泡時間越長、照射紫外光劑量越大或浸泡的去離子水溫度越高，皆會使皺波的特徵波長越大，另外，重複浸泡會使高分子膨潤而使分子鏈應力鬆弛，使得皺波特徵波長變大。
第二部分研究(第三章)聚二甲基矽氧烷/金複合材料在預拉伸應變(Prestrain)回復後，其表面漣漪結構(Ripple structure)與其缺陷漣漪差排(Ripple dislocations)在受到不同角度之壓縮應變時，其漣漪差排的運動行為，其結果顯示，漣漪結構會出現與金屬差排滑移類似的行為，漣漪差排會離開初始位置並連結到鄰近的漣漪結構上，並改變經過之漣漪結構的方向，使其較為垂直壓縮應變，其滑移距離與時間之關係會使用牛頓運動定律進行模擬。當壓縮應變與預拉伸應變夾角越大與增加壓縮應變時，會對漣漪差排造成較大的剪應力，因此其滑移距離增長與滑移速度增快，而溫度上升會使高分子黏度下降，使漣漪差排滑移變得容易，此外，由DMA進行鍍金後的PDMS的應力鬆弛與潛變實驗，並使用Standard solid linear model進行模擬後，亦發現當溫度上升時，會使鍍金後PDMS的楊氏係數與黏度下降，與使用牛頓運動定律模擬漣漪差排滑移的結果相似。而增加預拉伸應變時，會使儲存較大的殘留應力在漣漪結構上，漣漪波長會變短，因此會使漣漪差排所需的臨界剪應力上升。
第三部分(第四章)則研究聚丁二酸二乙酯(Polyehtylene succinate, PESu)經過γ-ray照射後的結晶動力學，以Avrami equation分析DSC結晶放熱峰與時間之關係，將其轉換成相對結晶度與時間的關係圖，並使用Avrami plot求出速率常數(Rate constant)、Avrami指數與半結晶期，發現各個γ-ray劑量PESu的速率常數會在35 oC達到最大值，但當γ-ray照射劑量上升時，結晶常數下降，由於結晶的活化能並無法藉由速率常數或半結晶期直接獲得，因此會使用Lauritzen Hoffman theory分析PESu的結晶動力學，發現在30 oC~70 oC的等溫結晶溫度中會有Rigime II 往Rigime III的轉換出現，即由成核速率與結晶成長速率相當的狀態轉換成以成核速率主導的狀況，且其轉換溫度會隨著劑量增加而降低，結晶活化能也會隨劑量增加而上升。另外，在真空中照射γ-ray的對位聚苯乙烯(Syndiotactic Polystyrene, sPS)，其相對結晶度隨結晶時間的變化，則是藉由DSC獲得其不同結晶時間的β’與β相的結晶後，搭配Avrami方程式進行轉換，並使用Avrami plot求出結晶常數與Avrami指數，發現隨著照射γ-ray劑量越大，其結晶常數越小且半結晶期越長，為了獲得真空照射γ-ray sPS的結晶活化能，此部分使用修正後的Lauritzen Hoffman模型分析sPS內 β與β’結晶相所需克服的能障與其熱力學驅動力，結果顯示當照射劑量越大，β與β’結晶相的活化能與所需的熱力學驅動力也會上升。
第四部份(第五章)則探討二乙基己醇(2-Ethyl hexonal)對吸收甲醇的PMMA的解吸產生裂縫的機制及其官能基的變化，由FTIR的結果可以看到PMMA內源自甲醇的C-O、C-H與O-H鍵結所對應的訊號強度皆隨著浸泡聚二乙基醇而下降，且隨著浸泡甲醇溫度上升，裂縫數量下降，浸泡甲醇的時間增長亦會使表面裂縫數目下降，相反的浸泡二乙基醇越久，則會使表面裂縫增加。

The effects of irradiation/solvent/stress on structures of polymeric materials is studied. Here, we discuss how the structures of polymeric materials change after the materials are immersed in solvent or applied stress. The materials might crystallized、produce surface structure、change the interval of polymer chains or occur surface cracks to reduce the free energy.
In the chapter 2, the mass transport of non-irradiated and UV-irradiated PHEMA in distill water is studied. The Harmon model is applied to simulate the experimental results of mass transport. The result show that the mass transport of non-irradiated and UV irradiated PHEMA in DI water is anomalous diffusion which include Case I transport and Case II transport at the same time. The Case I transport is dominated by concentration gradient of solvent, the Case II transport is dominated by stress relaxation of polymer chains. The diffusion coefficient and the velocity for the Case I and Case II transport follow the Arrhenius equation. The activation energies of Case I and Case II transport increase with increasing UV doses. Moreover, the DSC and FTIR is applied to analyze the glass transition temperature and function group for non-irradiated and UV-irradiated PHEMA. The results show that the glass transition temperature and the bonding intensities of C=O and C-O decrease with increasing UV doses, it means that the PHEMA produce chain scission after UV-irradiated. In the second part of chapter 2, the effect of UV irradiation on solvent induced surface wrinkle of PHEMA is investigated. The surface wrinkle of PHEMA is induced by desorption of DI water when DI water escape from the PHEMA sample. Because the DI water in UV-irradiated layer desorbed first, It caused much bigger deformation than non-irradiated section of PHEMA and induce the interfacial tensile stress between the UV-irradiated layer and non-irradiated section of PHEMA. Here, we use the Image J (NIH) to analyze the characteristic wavelength of surface wrinkle. The Image J can transform the OM images of surface wrinkle into reciprocal space by Fourier transform, so that we can find the wavenumber of surface wrinkle and calculate the wavelength by modify Bragg’s equation. The result show that the characteristic wavelength increases, as the increase of UV doses, temperature of DI water and the first immersion time in DI water increase. In addition, the characteristic wavelength increases as increasing total immersion time in DI water due to the stress relaxation caused by swelling.
In the chapter 3, the slip of ripple dislocations on PDMS/Au bilayer structure surface is studied. A 5 nm gold layer is sputtered on a pre-strained PDMS, then the ripple structure and its defects like ripple dislocations and cracks appear on the Au/PDMS surface after the pre-strain of PDMS is released. Here, we applied compression strain with different direction from the pre-strain to observe the slip of ripple dislocations. The ripple dislocation connect to nearby ripple structure and change the alignment of ripple structure when it passes through. The Newton’s law is applied to simulate the moving ripple dislocations. When the angle between compression strain and pre-strain direction increases, it causes much bigger shear stress on ripple dislocations, and the velocity of ripple dislocations increases. When the temperature increases, the viscosity of PDMS decreases and makes the slip of ripple dislocation easier. In addition, the creep and stress relaxation test of Au/PDMS are measured by DMA. We use standard solid linear model to derive the creep and stress relaxation model. The viscosity and young’s modulus with different temperature can be determined from the simulation parameters of creep and stress relaxation model. The results show that the viscosity and Young’s modulus increase with increasing temperature, which is similar to the result of the moving ripple dislocations from Newton law. The ripple wavelength decreases when the pre-strain is increased, which might store more residual stress on ripple structure and increase the critical shear stress for ripple dislocations.
In the chapter 4, the isothermal crystallization kinetic of gamma-irradiated polymer is studied. This chapter can be individed into 2 sections. In the first section, we study the isothermal crystallization kinetic of gamma-irradiated PESu. The PESu samples are irradiated in air with γ-ray at various doses from 0 to 600 kGy, and isothermal crystallized at different temperatures and times. The Avrami equation is applied to calculate the relative crystallization at different times and γ-ray doses from the crystallization exothermic peak of DSC thermograms. After that the rate constant, Avrami exponent and half-life crystallization can be determined by Avrami plot. The results show that the rate constant has maximum at 35 oC, but decreases with increasing γ-ray doses. Because the activation energy of isothermal crystallization cannot be determined by rate constant, the Lauritzen Hoffman theory is applied to analyze the isothermal crystallization kinetic of irradiated and non-irradiated PESu. We find that there are regime transition from regime II to regime III between 30 oC to 70 oC, which means that the rate control has a transition from compatible between nucleation and grow rate to dominate nucleation rate. In addition, the activation energy of isothermal crystallization on PESu and the transition temperature from regime II to regime III increases as increasing γ-ray dose. In the second section, the isothermal crystallization kinetics of γ-ray irradiated sPS is studied by DSC. The sPS sample is irradiated in vacuum with γ-ray at various doses from 0 to 800 kGy, and melt-crystallized at different times and temperatures. We apply the Avrami equation to transform the multiple endothermic melting peaks from DSC at different times to the relative crystallization of β and β’ form at different times. After that the Avrami exponent and rate constant can be determined from the slope and intercept of Avrami plot, respectively. The result shows that the rate constant decrease and the half-life crystallization increase with increasing γ-ray dose. Here, the modified Lauritzen Hoffman model is applied to calculate the activation energy and thermodynamic driving force of crystallization. The results show that the activation energy and thermodynamic driving force increase with increasing γ-ray dose.
In the chapter 5, the solvent induced cracks on PMMA surface is studied. After the PMMA absorbs in methanol at different temperatures and times, the PMMA is immersed in the 2EA to desorb methanol, and it causes the cracks on PMMA surface. The FTIR is applied to observe the function groups change of PMMA during the absorption/desorption process. The results show that the C-O、C-H and O-H bonding, which relate to methanol, decrease after immersing in 2EA. The number of cracks decrease with increasing temperature and immersion time of methanol. In contrast, the number of cracks increases with increasing immersion time in 2EA.

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