本研究以溶膠-凝膠法製備二氧化鈦光觸媒(TiO2)，並與採用廢玻璃及二次鋁渣合成之再生沸石載體進行複合。探討此複合材料於紫外光照射下對五氟丙酸光降解反應之影響，其原理為結合多孔吸附材料沸石載體上，載體能有效抑制TiO2晶粒尺寸增長，載體充當吸附劑以富集污染物，導致電子空穴對分離和轉移加快光催化處理能力。降解後之濃度以離子層析儀(IC)分析，並以氟離子濃度觀察其降解礦化情形。
研究數據顯示(最佳條件)在UV紫外光、劑量效應控制為0.5g與鹼性條件下，TiO2與Zeolite/TiO2複合材料光催化五氟丙酸反應8小時後分別處理效率為44.8% 與54.5 %。Zeolite/TiO2總處理效率高於光觸媒9.70%。在透過實驗計算法與統計變異數分析，歸納各因子的效應關係與最佳參數的範圍。藉由變異數分析的主因子效應顯示，研究顯示之劑量濃度與pH值為影響本次實驗最重要之兩項因子，在鹼性環境有較佳處理效率，推測主要原因是產生高反應性之．OH氫氧自由基對五氟丙酸進行降解反應曲面法結果透過最佳預測參數，所得到之最佳預測效益為60.2%之去除效率。本研究選用廢玻璃及鋁渣合成沸石，其多孔性結構可作為光觸媒附著的載體，而實驗結果證實沸石載體之添加確實可提升降解之效果。

In this study, a sol-gel method was used to prepare titanium dioxide photocatalyst (TiO2) and composite it with a regenerated zeolite carrier synthesized from waste glass and secondary aluminum slag. To investigate the effect of this composite material on the photodegradation reaction of perfluoropropionic acid under ultraviolet light irradiation. The principle is to combine the porous adsorbent material zeolite support. The support can effectively inhibit the growth of TiO2 grain size, and the support acts as an adsorbent to enrich pollutants , Resulting in the separation and transfer of electron-hole pairs to speed up the photocatalytic processing capability. The concentration after degradation was analyzed by ion chromatography (IC), and the degradation and mineralization of the fluoride ion concentration was observed.
The research data shows that (optimum conditions) under UV ultraviolet light, dose effect control of 0.5g and alkaline conditions, TiO2 and Zeolite / TiO2 composite materials photocatalyzed pentafluoropropionic acid after 8 hours of reaction efficiency of 44.8% and 54.5 %, The total processing efficiency of Zeolite / TiO2 is 9.70% higher than that of photocatalyst. This study speculates that Zeolite / TiO2 is higher than TiO2. It is presumed that TiO2 nanoparticles are combined with porous adsorbent zeolite carrier. The carrier can effectively inhibit the growth of TiO2 grain size. The carrier acts as an adsorbent to enrich the pollutants, leading to the separation of The transfer accelerates the photocatalytic processing capacity. In this study, the microwave hydrothermal synthesis method is used, which can effectively reduce the synthesis time, reduce the temperature and save energy efficiency, and use secondary aluminum slag and waste glass recycled zeolite to achieve the effect of waste reduction and recycling and the vision of recycling economy.

論文審定書 .....................................................................................................................i
摘要................................................................................................................................ii
ABSTRACT.................................................................................................................. iii
目錄...............................................................................................................................iv
圖目錄...........................................................................................................................ix
表目錄..........................................................................................................................xii
第一章 前言.................................................................................................................... 1
1-1 研究緣起........................................................................................................... 1
1-2 研究目的........................................................................................................... 2
第二章 文獻回顧 ............................................................................................................ 3
2-1有機氟化物基本特性與用途 ............................................................................ 3
2-1-1 全氟化合物 ............................................................................................ 4
2-1-2 全氟羧酸環境宿命 ................................................................................ 4
2-1-3 全氟羧酸人體健康之影響 ..................................................................... 5
2-1-4 全氟羧酸濃度規範 ................................................................................ 6
2-1-5 有機氟化物的處理技術現況 ................................................................. 8
2-2光催化反應(photocatalytic reactions) ................................................................ 9
2-2-1 光催化光解模式與能帶位置 ............................................................... 10
2-3光觸媒（Photocatalyst） ................................................................................ 11
2-3-1 二氧化鈦(TiO₂) .................................................................................... 13
2-3-2二氧化鈦晶相物理性質 ....................................................................... 14
2-3-3二氧化鈦結構 ...................................................................................... 15
2-3-4二氧化鈦晶相相變 .............................................................................. 16
2-3-5 二氧化鈦光觸媒能隙 .......................................................................... 18
2-4二氧化鈦合成技術 ......................................................................................... 20
2-4-1化學氣相沉積法（Chemical vapour deposition , CVD） .................... 21
2-4-2真空濺鍍法（Vacumn sputtering） ..................................................... 22
2-4-3 陽極氧化法 (anodic oxidation)............................................................ 22
2-4-4溶膠-凝膠法(Sol-Gel) .......................................................................... 23
2-5 廢棄物資源化再利用 ..................................................................................... 25
2-5-1廢玻璃 .................................................................................................. 25
2-5-2廢鋁渣 .................................................................................................. 26
2-5-3廢棄物再生沸石 .................................................................................. 27
2-5-4沸石基本特性 ...................................................................................... 29
2-6光觸媒結合沸石多孔性載體材料 .................................................................. 30
2-7固定二氧化鈦載體技術 .................................................................................. 32
2-7-1含浸法(impregnation) ........................................................................... 32
2-7-2共沉澱法 (Co-precipitation Method) .................................................... 33
第三章 研究方法與流程 .............................................................................................. 34
3-1研究流程 ......................................................................................................... 34
3-2實驗規劃與材料製備方法 .............................................................................. 36
3-2-1 前置作業與實驗規劃 .......................................................................... 36
3-2-2 控制因子與操作因子 .......................................................................... 38
3-2-3 實驗設計法 .......................................................................................... 40
3-3 實驗使用之檢測方法及儀器設備 .................................................................. 42
3-3-1 實驗耗材與藥品 .................................................................................. 42
3-3-2 實驗儀器與設備 .................................................................................. 43
3-4品保及品管 (QA&QC) ................................................................................... 50
第四章 結果與討論 ...................................................................................................... 51
4-1 感應耦合電漿質譜儀 (ICP-OES)微量金屬元素分析 .................................... 51
4-2 材料基本性質分析 ......................................................................................... 53
4-2-1光觸媒晶相分析 .................................................................................. 53
4-2-2沸石結構鑑定 ...................................................................................... 55
4-3環境掃描式顯微鏡分析二次鋁渣 .................................................................. 57
4-3-1環境掃描式顯微鏡分析合成沸石載體 ................................................ 58
4-3-2環境掃描式顯微鏡分析合成光觸媒.................................................... 60
4-3-3環境掃描式顯微鏡分析光觸媒結合沸石載體 .................................... 62
4-3-4能量分散式光譜儀分析沸石載體材料 ................................................ 64
4-3-5能量分散式光譜儀分析光觸媒結合沸石載體複合材料 ..................... 65
4-4表面積分析儀分析光觸媒與沸石 .................................................................. 67
4-5光催化降解脫氟五氟丙酸之研究 .................................................................. 68
4-5-1背景實驗-直接光解 ............................................................................. 69
4-5-3 pH對於光催化降解脫氟五氟丙酸之影響 .......................................... 70
4-5-4 溫度對於光催化降解脫氟五氟丙酸之影響 ........................................ 71
4-5-5 劑量對於光催化降解脫氟五氟丙酸之影響 ........................................ 72
4-5-6複合材料混合比對於光催化降解脫氟五氟丙酸之影響 ..................... 73
4-6複合材料光催化降解脫氟之反應條件因次分析 ........................................... 74
4-6-1複合材料搭配紫外光對五氟丙酸脫氟之最佳應用 ............................ 76
4-6-2主因子效應之各因子水準分析 ........................................................... 76
4-6-3主因子效應之各因子水準分析 ........................................................... 78
4-6-4主因子效應之常態性與殘差分析 ....................................................... 79
4-7 複合材料於紫外光環境降解脫氟之反應條件反應曲面............................... 80
4-7-1 二次反應曲面之變異數分析 ............................................................... 82
4-7-2 二次反應曲面之常態性與殘差分析 .................................................. 83
4-7-3 二次反應曲面各因子之最佳預測效益水準分析 ............................... 84
4-8 二次反應曲面最佳參數預測效益水準分析 .................................................. 90
4-9 紫外光降解環境五氟丙酸之去除率 ............................................................. 91
4-10 成本效益分析 ............................................................................................... 93
第五章 結論與建議 ...................................................................................................... 96
5-1 結論 ................................................................................................................ 96
5-2 建議 ................................................................................................................ 97
參考文獻 ...................................................................................................................... 98

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