臺灣博碩士論文加值系統

本研究以溶膠凝膠法(sol-gel)製備不同的二氧化鈦光觸媒，以鑲嵌Fe與S的方式進行改質二氧化鈦光觸媒，包括FeT-S、FeT-SL、ST-S，在可見光下進行MB染料的降解實驗；並探討其最佳的改質條件(鑲嵌量與鍛燒溫度)與最佳的操作條件(pH值與MB初始濃度)。
本實驗使用BET、SEM/EDX、XRD與UV-vis等儀器鑑定光觸媒之物化特性。實驗結果顯示，以本實驗的改質方法確實能成功將金屬Fe與非金屬S鑲嵌於TiO2上，比表面積大約為38.7~79.4 m2/g；XRD分析結果顯示其多為銳鈦礦晶相；UV-vis分析顯示改質過後的光觸媒其可見光吸收能力增強，並有明顯的紅位移現象。若觀察MB染料濃度的降解情形，與以擬一階反應速率方程式來描述實驗結果，可以發現改質過後的二氧化鈦光觸媒，在可見光下可具有較佳的光降解效果；最佳的改質觸媒為ST-S在鑲嵌劑量為硫脲0.15 mole和鍛燒溫度為500℃；最佳的操作條件為pH=11、初始濃度=10ppm。綜合實驗結果，本研究在反應60分鐘後MB的降解率最高可達88%。

The objectives of this work are to prepare Fe-doped and S-doped TiO2 photocatalysts using the sol-gel method, and to investigate the photo-degradation of methylene blue (MB) in aqueous solutions under visible light irradiation. The preparation conditions, including the type and amount of dopants and calcinations temperature were studied the characteristics of the resulting photocatalysts were analyzed. Additionally, the optimum experimental conditions (including pH value and initial dye concentration) were evaluated.
The physical-chemical characteristics of the prepared photocatalysts were analyzed by BET, SEM, EDX, XRD, and UV-Vis. Results showed that the specific surface area of the photocatalysts is about 38.7~79.4 m2/g. XRD patterns indicated that the major crystalline type of the prepared TiO2 is anatase. UV-Vis diffuse reflectance spectra showed that absorption of Fe-doped and S-doped TiO2 in the visible light region was strengthened and the phenomena of red-shift was apparent. As for the photocatalytic degradation of MB, the pseudo-first-order rate equation can be used to fit the concentration vs. time data. It also revealed that the prepared photocatalysts had greater reaction rates and could react with MB more effectively under visible light irradiation. The S-doped TiO2, using 0.15 mole thiourea as the dopant, and at the calcination temperature of 500℃ would exhibit the highest catalytic activity with respect to MB in this study. The optimum experimental conditions are found to be pH 3, and at the initial MB concentration of 10ppm. The removal efficiency of MB reached 88% after 60 minutes of visible light irradiation.

目錄

封面內頁
簽名頁
授權書 iii
中文摘要 iv
英文摘要 v
誌謝 vi
目錄 vii
圖目錄 x
表目錄 xiii

第一章 前言 01
1.1 研究緣起 01
1.2 研究目的 02
1.3 研究內容 02
第二章 文獻回顧 03
2.1 光催化反應的原理與應用 03
2.1.1 光催化反應原理 03
2.1.2 光觸媒的材料簡介 04
2.1.3 光催化反應的應用 05
2.2 二氧化鈦光觸媒降解有機污染物的機制 07
2.2.1 二氧化鈦的基本特性 07
2.2.2 有機污染物的光降解機制 07
2.2.3 光催化反應動力模式 09
2.3 二氧化鈦光觸媒的製備與改質 11
2.3.1 二氧化鈦製備方法 11
2.3.2 二氧化鈦光觸媒的改質 13
2.3.3 光觸媒鍛燒溫度 18
2.3.4 鑲嵌量 19
2.4 影響光催化反應效能之因子 21
2.4.1 光觸媒添加量 21
2.4.2 反應物初始濃度 22
2.4.3 pH值 23
第三章 實驗材料與研究方法 24
3.1 實驗設備與材料 24
3.1.1 實驗裝置與儀器 24
3.1.2 實驗藥品與耗材 26
3.2 研究流程 27
3.3 二氧化鈦光觸媒的製備 29
3.4 光觸媒的特性鑑定與分析 31
3.4.1 比表面積分析－BET 31
3.4.2 表面形貌及表面元素分析－SEM/EDX 31
3.4.3 晶相分析－XRD 32
3.4.4 觸媒吸收光譜分析－紫外光-可見光光譜儀 32
3.5 實驗設計與步驟 33
3.6 實驗分析方法 34
3.6.1 光能強度測定分析 34
3.6.3 亞甲基藍濃度的分析 35
第四章 結果與討論 37
4.1 改質二氧化鈦光觸媒之特性分析 37
4.1.1 改質光觸媒比表面積分析-BET 37
4.1.2 改質光觸媒之表面形貌與元素鑑定-SEM/EDX 38
4.1.3 改質光觸媒晶相鑑定-XRD 46
4.1.4 改質光觸媒吸收光譜分析 49
4.2 二氧化鈦之改質條件對光催化效果的影響 51
4.2.1 觸媒之鑲嵌劑量對MB的光催化效果 51
4.2.2 觸媒之鍛燒溫度對MB的光催化效果 54
4.3 反應條件對改質光觸媒的MB之降解效果 59
4.3.1 背景實驗與改質光觸媒對MB溶液的降解效果比較 60
4.3.2 pH值對染料的去除效果影響 61
4.3.3 MB初始濃度對去除效果的影響 63
第五章 結論與建議 68
5.1 結論 68
5.2 建議 69
參考文獻 70

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