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標題: 高分子薄膜與多層複合薄膜氣體分離特性之研究
Preparation and characterization of polymer & multi-layer composite membranes for gas separation
作者: 翁子翔
Weng, Tzu-Hsiang
關鍵字: Blend membrane;混合薄膜;Permeability;Selectivity;Crosslinking;d-spacing;滲透率;選擇率;交聯;層間距離
出版社: 環境工程學系所
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玻璃轉化溫度及層間距離對應出高分子鏈移動性與氣體滲透之相關性是本研究重點,經混合後之PPSU/PBNPI高分子薄膜高分子鏈與鏈之間互相作用,產生之層間距離大小取決於混合薄膜中PPSU之濃度比例,67/33 wt% PPSU/PBNPI因層間距離大,明顯提高氣體滲透率,此外混合後薄膜轉為較無結晶型結構,高分子鏈容易移動且有相分離現象產生均是導致提升氣體滲透率之要素。此外,以交聯劑改質混合薄膜經交聯作用後高分子鏈共價作用導致高分子鏈緊密鏈移動性降低層間距離縮小提升了薄膜結晶度,因此使得交聯後PPSU/PBNPI混合薄膜能提升氣體選擇率。
在有機-無機複合薄膜中,由XRD結果證實,無機材料的添加將影響了高分子鏈的移動及層間距離,就添加奈米碳管而言,複合薄膜玻璃轉化溫度下降,證實其高分子鏈的移動性隨添加量的增加而提升。此外,就具支撐層之高分子複合薄膜而言,薄膜厚度以及表面及底層粗糙係數亦會對氣體滲透及選擇率產生影響,PPO/CMS/Al2O3多層複合薄膜之H2/CH4及H2/N2選擇率分別高達31.8及37.1,該值較純PPO高分子高,主要原因為PPO塗佈於經由CMS修飾過的CMS/Al2O3支撐層上能夠使PPO薄膜表面更為平滑,薄膜結構粗糙係數由表面往底層增加可有效提升氣體滲透率及選擇率。除了改變了薄膜表面結構外,高分子鏈亦因添加了SBA-15轉變為較堅硬分子鏈降低了移動性,使得玻璃轉化溫度增加提升了氣體選擇率,特別是在添加10 wt% SBA-15時, H2/CH4、H2/N2及CO2/CH4選擇率分別提升為50.9、38.9及25.6。

The mobility, crystallization, and d-spacing of polymer membranes are the key parameters for controlling gas permeation behavior through the blend and composite membranes. Among them, the polymer chain mobility is dominant. The polymer chain mobility property is related to the polymer structure itself and to the interaction of composite materials. Therefore, the aim of this study is to show the relationship between the polymer chain mobility interaction and gas separation properties of the different composite membranes. The composite membranes include the following: (1) blend membrane, (2) cross-linking membrane, (3) organic-inorganic composite membrane, and (4) supported multi-layer composite membrane. The morphological studies, roughness coefficient, crystalline structure, glass transition temperature (Tg), and functional group of all the composite membranes were obtained using scanning electron microscopy (SEM), atomic force microscopy (AFM), differential scanning calorimetry (DSC), and Fourier transform infrared spectroscopy (FTIR) to identify the relationship between the characterizations and gas separations of the composite membranes. In this study, highly permeable and highly selective composite membranes were fabricated for later use in the field of gas separation.
This study reports the glass transport temperature and the polymer chain d-spacing corresponding to polymer chain mobility and gas permeation. The results indicate that for PPSU/PBNPI blend polymer membranes, the variation of the d-spacing depends on the PPSU content of the PPSU/PBNPI blend membrane. When the PPSU content increased to 67 wt%, the polymer d-spacing increased, resulting in improving gas permeability. Furthermore, the increased gas permeation was attributed to the crystalline structure transformation to amorphous structure, easy polymer chain mobility, and phase separation phenomenon, which resulted in the blend membranes. For the crosslinking membranes, the reduction of polymer chain mobility and d-spacing was attributed to the polymer chain covalent bond caused by the crosslinking agent in the blend membranes, which resulted in the increased gas selectivity of the crosslinking blend membranes.
Based on the X-ray diffraction (XRD) result, adding the inorganic particle into the polymer matrix affected the polymer chain mobility and d-spacing of the organic-inorganic composite membranes. For example, when the carbon nanotubes were added, the chain mobility and d-spacing of the organic-inorganic hybrid membranes increased with the increasing carbon nanotube content. Furthermore, supporting the polymer membranes with CSM/Al2O3 materials, the membrane thickness and roughness coefficients of the top and bottom surfaces of PPO changed, also affecting the gas permeability and selectivity of PPO/CMS/Al2O3 composite membranes. The H2/CH4 and H2/N2 selectivity of the PPO/CMS/Al2O3 composite membranes increased remarkably, reaching 31.8 and 37.1, respectively, which are higher than the values of homogeneous PPO. This result was confirmed by preparing a composite membrane by first coating a CMS layer onto the Al2O3 support. The top surface of the PPO selective layer became very smooth and tended to reduce the defects between the selective layer and the CMS layer, yielding composite membranes with better separation performance. Furthermore, the increments of the glass transition temperature of the composite membranes with SBA-15 confirmed that SBA-15 causes the polymer chains to become rigid and the reduction of polymer chain mobility. This phenomenon enhanced the H2/CH4, H2/CH4, and H2/N2 gas selectivities, reaching to 50.9, 38.9, and 25.6, respectively, especially when the SBA-15 loading increased to 10 wt%.
The blend of different polymer precursors, crosslinking, and added nano inorganic material affects the polymer chain mobility of polymer membranes. Meanwhile, the roughness coefficient of the membranes also affects the gas separation performance of polymeric membranes. Thus, this thesis aims to understand the relationship between polymer chain mobility interaction and gas separation properties of the different kinds of membranes, helping to clarify the gas separation mechanism of polymeric membranes.
其他識別: U0005-1708201015322400
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