臺灣博碩士論文加值系統

本文選用結構富含羥基的微晶纖維素作為薄膜材料，為提升膜材對於
二氧化碳分離效能，於纖維素化學結構中摻混對二氧化碳有強親和力的胺
基，以期促進二氧化碳傳輸，達精準且有效之分離。為此，本文藉由高溫
反應將三種不同鹼度之含胺化合物分別接枝聚合在微晶纖維素上，並透過
旋轉塗佈技術製備出氮摻雜微晶纖維素高分子薄膜，並探討塗覆層數影響
之厚度與孔洞及氮摻雜微晶纖維素對衍生膜材氣體分離效能之影響。
結合場發射掃描式電子顯微鏡(FE-SEM)觀察結果、氮摻雜前後之纖維
素粉體重量的量測、X射線光電子能譜之化學鍵結擬合分析，確認含胺化
合物非但成功地接枝於材料上，亦對粉體形貌無負面影響; 由氣體分離試
驗結果可知，不同級別胺接枝之氮摻雜微晶纖維素膜確實比純微晶纖維素
膜更為理想，其中以鹼度最高之接枝二級胺之微晶纖維素膜的氣體分離性
能為最佳，其二氧化碳滲透率由1.26 GPU增長到了1.79 GPU，二氧化碳/
氮氣氣體對之選擇率也從26上升到57，此結果表明在膜結構中添加胺基
是有利於二氧化碳分離的。

Present work adopted microcrystalline cellulose (MCC) possessing abundant
hydroxyl groups as the precursor for gas separation membrane. In order to enhance the CO₂ separation performance, amine groups were incorporated into the chemical structure of MCC to facilitate CO₂ transport and thus achieve precise and efficient separation, which is because of the strong affinity for CO₂. As such, three kinds alkalinity of amine-containing compounds were grafted onto MCC through high-temperature reaction, and then nitrogen-doped MCC polymeric membranes were obtained through spin-coating technique. Moreover, the effects of coating layer thickness and porosity, as well as the influence of nitrogen-doped microcrystalline cellulose on the gas separation performance of the derived membrane materials, were also investigated. Based on observations from field emission scanning electron microscopy (FE-SEM), weight measurements of MCC powder with/without nitrogen doping, and chemical bond fitting analysis from X-ray photo electron spectroscopy, it can be found that the amine-containing compounds were successfully grafted onto the MCC material and the morphology of the nitrogen-doped precursor was akin to pristine ones. Single-gas permeation test also showed that separation performance
of nitrogen-doped MCC membranes grafted with different levels of amines were outstanding than that of pristine membrane. Among them, the microcrystalline cellulose membrane grafted with secondary amine, which has the highest basicity, exhibited the best gas separation performance. The CO₂ permeance increased from 1.26 GPU to 1.79 GPU, and the CO₂/N₂ selectivity also increased from 26 to 57. These results indicate that the presence of amine groups within the membrane structure is beneficial for CO₂ separation.

摘要 i
Abstract ii
目錄 iv
圖目錄 vii
表目錄 ix
第一章 前言 1
1.1 研究背景 1
1.2 研究動機 4
1.3 研究目的 7
1.4 研究架構 8
第二章 文獻回顧 9
2.1 氣體分離薄膜技術 9
2.1.1 膜材料 10
2.1.2 氣體分離之傳輸機制 13
2.1.3 氣體傳輸方程式 17
2.1.4 影響膜材氣體分離性能之關鍵因子 21
2.1.5 應用領域 23
2.2 高分子膜介紹 25
2.2.1 膜形態 25
2.2.2 成膜方式 26
2.2.3 膜製備方法 29
2.2.4 影響高分子膜氣體分離性能之關鍵因子 31
2.2.5 化學結構改質 35
2.3 微晶纖維素 38
2.3.1 溶劑選擇 39
2.3.2 纖維素之氣體分離性能 39
2.3.3 微晶纖維素改質 40
2.4 文獻總結 42
第三章 材料與方法 44
3.1 材料與儀器 44
3.2 微晶纖維素接枝含胺化合物之步驟 46
3.3 微晶纖維素平板膜製備之步驟 47
3.4 特性分析 48
3.5 單一氣體滲透測試 49
第四章 結果與討論 51
4.1 氮摻雜微晶纖維素之粉體特性分析 51
4.1.1 氮摻雜前後微晶纖維素之表面形貌比較 51
4.1.2 氮摻雜前後微晶纖維素之熱穩定性比較 54
4.1.3 氮摻雜前後微晶纖維素之元素分析 55
4.2 氮摻雜微晶纖維素膜之氣體分離性能 58
4.2.1 純微晶纖維素膜不同層數之單一氣體分離性能比較 59
4.2.2 不同級別胺接枝之氮摻雜微晶纖維素之單一氣體分離性能比較 61
4.2.3 不同級別胺接枝之氮摻雜微晶纖維素與相關纖維素膜之氣體分離性能比較 63
第五章 結論與建議 65
5.1 結論 65
5.2 建議 66
參考資料 67

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