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研究生： 黃瑋軒
Huang, Wei-Xuan
論文名稱： 還原氧化石墨烯碳複合薄膜於正滲透系統之應用
Reduced Graphene Oxide Carbon-based Thin-film Composite Membrane for the Application in Forward Osmosis
指導教授： 戴念華
Tai, Nyan-Hwa
李紫原
Lee, Chi-Young
口試委員: 林冠佑
Lin, Guan-you
洪仁陽
Horng, Ren-Yang
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年： 2020
畢業學年度： 108
語文別： 中文
論文頁數： 90
中文關鍵詞： 複合薄膜 、正滲透 、還原氧化石墨烯
外文關鍵詞： thin-film composite membrane, forward osmisis, reduced graphene oxide
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    • 本研究目的為開發一具有高通量及低逆溶質擴散之碳複合薄膜，並應用於正滲透(Forward Osmosis, FO)分離系統中。實驗分為兩個階段：第一階段首要探討以市售混和纖維素酯(Mixed Cellulose Ester, MCE)作為基材膜，還原氧化石墨烯(Reduced Graphene Oxide, rGO)作為阻鹽層之可行性，並分析rGO厚度對FO效能之影響，找出最佳厚度參數。此外也進一步使用聚多巴胺(Polydopamine)對rGO表面進行親水改質，試圖提升水通量。於此基礎下，第二階段將使用不織布取代MCE作為基材膜，並以塗佈的方式形成奈米碳管(Carbon Nanotube, CNT)層，再以浸鍍的方式被覆一層聚乙烯亞胺(Polyetherimide, PEI)，最後結合rGO及PDA完成碳複合膜之製備，研究將討論基材膜的改變對薄膜效能的影響。結果顯示，由於不織布表面較MCE粗糙許多，需要較厚的rGO才能覆蓋完整，此外PEI的帶電特性，能增加CNT和rGO之貼覆性，提升FO效能，以進流液為去離子水，提取液為1M氯化鈉水溶液的FO測試條件下，具有水通量25.74 LMH及逆溶質擴散5.94 gMH的優良成果，顯示本研究之碳複合薄膜於FO系統應用深具潛力。

    The work aims to develop a carbon-based thin-film composite (TFC) membrane with great performance in forward osmosis (FO) application. This study has two subjects; the first subject is focusing on the study of feasibility of salt ion rejection of the reduced graphene oxide (rGO) film using mixed cellulose ester (MCE) filter paper as the supporting layer. This study find that the rGO thickness plays a significant role of rGO on the water flux and salt rejection. In addition, the rGO membrane coated with polydopamine (PDA) possesses superhydrophilic property which significantly enhances the FO performance. On this basic, nonwoven fabric is adopted as the substrate on the second subject of this study. Using the results obtained from the first subject and casting the carbon nanotubes (CNTs) on the nonwoven fabric through casting followed and dip-coating of polyetherimide (PEI) onto the CNT surface, we successfully prepared the carbon-based TFC membrane. Results show that PEI with positive charges can enhance the adhesion between CNT and rGO, as a result, improving the FO performance. The water flux of 25.74 LMH with reverse salt flux of 5.94 gMH are achieved, implying this carbon-based membrane possesses great potential in FO application.

    摘要 I Abstract II 目錄 III 圖目錄 VII 第一章 緒論 1 1.1 前言 1 1.2 研究動機 1 第二章 文獻回顧 3 2.1 薄膜技術簡介 3 2.1.1 薄膜分離程序 3 2.1.2 薄膜型態 5 2.2 複合薄膜簡介與製備方式 7 2.2.1 多孔支撐層之製備 7 2.2.2 緻密選擇層之製備 9 2.3 正向滲透之簡介 10 2.3.1 正向滲透薄膜之發展 10 2.3.2 正向滲透分離原理與應用 11 2.3.3 正向滲透之關鍵與瓶頸 12 2.4 石墨烯之簡介 15 2.4.1 石墨烯及其衍生物於水處理薄膜之應用 17 2.5 本實驗室水處理組探討回顧 19 第三章 實驗方法與分析 29 3.1 實驗步驟與流程 29 3.1.1 基材膜製備 29 3.1.2 活性阻鹽層-還原氧化石墨烯之製備 30 3.1.2.1 氧化石墨烯的製備 30 3.1.2.2 氧化石墨烯之抽濾 31 3.1.2.3 氧化石墨烯薄膜之還原 31 3.1.3 聚多巴胺之製備與聚合 32 3.2 分析方式與設備 33 3.2.1場發射掃描式電子顯微鏡 33 3.2.2 拉曼光譜儀 33 3.2.3 傅立葉轉換紅外光譜儀 34 3.2.5 X射線繞射分析儀 34 3.2.6 水接觸角測量儀 35 3.2.7 Zeta電位分析儀 36 3.2.8 正向滲透效能測試 36 3.2.8.1 裝置與測試條件 36 3.2.8.2 FO效能數據分析 37 第四章 結果與討論 46 4.1 還原氧化石墨烯阻鹽層之可行性探討 46 4.1.1 SEM形貌分析 46 4.1.2 XRD層間距分析 47 4.1.3 拉曼光譜分析 47 4.1.4 XPS 元素分析 48 4.1.5傅立葉轉換紅外光譜分析 49 4.1.6 FO效能分析 49 4.2 還原氧化石墨烯的厚度與聚多巴胺對複合膜效能影響之探討 50 4.2.1 rGO厚度對FO效能影響之探討 50 4.2.1.1 SEM 形貌分析 50 4.2.1.2 FO效能分析 50 4.2.2 被覆PDA對FO效能影響之探討 51 4.2.2.1 SEM表面形貌分析 51 4.2.2.2 XRD分析 52 4.2.2.3 XPS 元素分析 52 4.2.2.4傅立葉轉換紅外光譜分析 52 4.2.2.5水接觸角分析 53 4.2.2.6 FO效能分析 53 4.3 還原氧化石墨烯-聚多巴胺應用於不織布-奈米碳管支撐層之探討 54 4.3.1抽濾參數再調整 54 4.3.1.1 SEM形貌討論 54 4.3.1.2 FO 效能分析 55 4.3.2 導入PEI於不織布系統中 55 4.3.2.1 SEM形貌討論 55 4.3.2.2 Zeta電位分析 57 4.3.2.3 傅立葉轉換紅外光譜分析 57 4.3.2.4 水接觸角分析 57 4.3.2.5 FO效能分析 58 4.4 碳複合薄膜之正滲透效能分析 59 4.4.1 A、B、S值 59 4.4.2 提取液濃度對薄膜效能之影響 60 4.4.3 有機溶液濃縮測試 62 第五章 結論 84

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