臺灣博碩士論文加值系統

鑒於氣候變遷對環境威脅與日俱增，以「2050淨零碳排」目標創造具競爭力又永續循環的綠色經濟已是全球趨勢，因此碳捕獲、碳儲存、碳利用等技術備受矚目。而在碳捕獲技術中，高分子薄膜因具備低成本、低耗能、低污染等優點，已廣泛應用於二氧化碳分離程序。 促進CO2傳輸型氣體分離膜多使用富含胺基之薄膜，乃鑒於胺基上氮原子含有未配對電子，可與CO2產生作用，增加CO2對薄膜之溶解度，促進傳輸效果。本研究著眼於使用富含胺基之高分子Pebax，摻入胺基改質之TiO2顆粒，製備成混合基質薄膜，既強化薄膜機械強度，又增加薄膜中胺基數量以促進CO2傳輸，且可拉大與薄膜親和力弱的氣體N2間之分離選擇率。此外，高分子鑄膜液採用綠色溶劑70%乙醇水溶液，且使用後高分子容易回收，為環境友善程序。本研究探討200 nm TiO2顆粒表面接枝不同數量胺基(1-3)之矽烷分子以及摻混wt%對氣體分離效果的影響，可得摻混0.5 wt% TiO2-AAAPTMS (3-[2-(2-aminoethylamino)ethylamino]propyl-trimethoxysilane)時獲致最佳CO2滲透率及CO2 /N2分離選擇率。為更提升氣體分離效能，本研究採用PEG 200為添加劑，因其EO單元對極性CO2具強親和力，且可增加Pebax基材的無定型區域，提高薄膜內自由體積。本研究所製備之以0.2 μm PTFE/PP為支撐層、膜厚10 μm的Pebax-80% PEG 200/0.5% TiO2-AAAPTMS混合基質薄膜可達到15.5 GPU之CO2通量、170 barrer之CO2滲透率、68之CO2 /N2分離選擇率，與純Pebax薄膜相比，效能有顯著提升，且已超越2008年Robeson’s upper bound。考慮薄膜碳捕獲技術於工業實際應用，本研究亦測試混合氣體之分離效率，純Pebax薄膜及混合基質薄膜均可獲致高達89%以上之CO2的純化效果，且高溫下可獲得較大之氣體通量。

The escalating threat of climate change accentuates the global imperative to pursue the "Net-Zero Emissions by 2050" target and instigate a competitive, sustainable, and circular green economy. Among the myriad Carbon capture and storage (CCS) technologies, polymer membranes stand out as particularly noteworthy due to their inherent advantages, including low cost, low energy consumption, simplified operation, and minimal environmental impact, leading to their extensive application in carbon dioxide separation processes. The technological highlights of this work involve the utilization of amino group based polymer (Pebax 1657), incorporating amine functionalized titanium dioxide particles to fabricate Pebax/TiO2-NH2 mixed matrix membranes (MMMs), subsequently applied in CO2/N2 separation processes. Since the unpaired electrons on nitrogen atom facilitate interaction with CO2, amplifying CO2 solubility. Therefore, the incorporation of amino-functionalized titanium dioxide particles not only enhances the mechanical strength of membranes but also augments the density of amino groups within, facilitating the reaction between carbon dioxide and amino-functionalized carrier－solution-diffusion mechanism. This not only facilitates CO2 transport but also increases the separation selectivity between CO2 and other gases. Furthermore, the solvent utilize in this work is 70% ethanol aqueous solution, which is easily to recyclable, making it an environmentally friendly fabrication process. Meanwhile, this work investigates the influence of grafting silanol compounds with varying quantities of amine groups (1-3) on TiO2 particles and the incorporation of loading wt% on gas separation performance. It is revealed that the addition of 0.5wt% TiO2-AAAPTMS yields the optimal CO2 permeability and CO2/N2 selectivity. To further enhance gas permeability and separation performance, polyethylene glycol (PEG 200) is selected as an additive. PEG 200, with its high chain mobility, increases the amount of amorphous EO segments and thus the free volume of the membrane. The 10 μm MMMs with 0.5 wt% TiO2-AAAPTMS and 80% PEG, consisting of a 0.2 μm PTFE/PP support layer showed the best separation performance exhibiting distinct increases of 130% permeability and 40% selectivity (CO2 170 barrer, CO2/N2 = 68) compared to primitive Pebax membrane, and surpassed 2008 Robeson’s upper bound. Considering the practical application of membrane carbon capture technology in industry, this study conducted mixed gas experiments using different ratios of CO2 and N2. Both pure Pebax membranes and mixed matrix membranes achieved purification of over 89% CO2. Additionally, higher gas fluxes were obtained at elevated temperatures.

摘要 i
Abstract ii
目錄 iv
圖目錄 vii
表目錄 ix
第一章 緒論 1
第二章 文獻回顧 4
2.1 薄膜分離技術簡介 4
2.2 高分子薄膜製備方法 6
2.3 氣體分離程序 8
2.3.1 薄膜於氣體分離之機制 8
2.3.2 薄膜於氣體分離之應用 10
2.4混合基質薄膜 13
2.5 填料 18
2.5.1 無機填料 18
2.5.2 胺基改質填料 19
2.6 以Pebax為基材之混合基質薄膜 22
第三章 研究方法 24
3.1 材料 24
3.2 儀器 25
3.3含氨基TiO2顆粒之製備 26
3.3.1 TiO2-APTMS顆粒製備 26
3.3.2 TiO2-AAPTMS和TiO2-AAPTMS顆粒製備 26
3.4 TiO2顆粒之特性分析 27
3.4.1 FTIR分析 27
3.4.2 TGA分析 27
3.4.3 XRD分析 28
3.4.4 XPS分析 28
3.5 高分子薄膜之製備 29
3.5.1 純高分子薄膜之製備 29
3.5.2 Pebax/TiO2-APTMS混合基質薄膜之製備 29
3.6 混合基質薄膜之特性分析 30
3.6.1 SEM、EDS分析 30
3.6.2 FTIR分析 30
3.6.3 TGA分析 30
3.6.4 XPS分析 31
3.6.5 GC分析 31
3.7 氣體滲透分離實驗 31
第四章 結果與討論 35
4.1 TiO2顆粒之特性分析結果 35
4.2 Pebax/TiO2混合基材薄膜之特性分析 39
4.3 Pebax純膜與Pebax/TiO2-NH2混合基質薄膜氣體分離結果 44
4.4 Pebax/TiO2-NH2 on PTFE/PP氣體分離結果 52
4.5進料壓力對Pebax純膜及Pebax/0.5% TiO2-AAAPTMS on PTFE/PP混合基質薄膜影響 54
4.6 溫度對Pebax純膜及Pebax/0.5% TiO2-AAAPTMS on PTFE/PP混合基質薄膜影響 56
4.7 Pebax/PEG 200混合基質薄膜氣體分離結果 58
4.8 Pebax-PEG200/TiO2-AAAPTMS混合基質薄膜氣體分離結果 60
4.9混合氣體分離結果 63
第五章 結論 66
參考文獻 67

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