臺灣博碩士論文加值系統

本研究應用浸漬-沈澱法(Immersion precipitation method)製備TiO2-PVDF複合薄膜光觸媒將光觸媒固定化，此薄膜光觸媒結合PVDF良好的物理特性(高可塑性、低機械阻抗、高可撓性等特性)，以及摻雜奈米碳管與氧化石墨烯改良觸媒活性等特性，研發兼顧優良物理特性與催化活性之複合薄膜光觸媒，並探討相關的反應機制。研究中以苯(Benzene)為目標污染物，經系列光催化分解實驗，探討不同種類光觸媒與環境參數(如：反應溫度、濕度、光源)，對於苯蒸氣分解速率的影響。
研究結果顯示：苯蒸氣之光催化分解反應，遵循一階反應動力關係；苯在本研究中，於近紫外光照射下具有較明顯分解效果，但在可見光下的反應不明顯，僅有少量吸附效果；未摻雜奈米碳材料的光觸媒(TP)，在35 ~ 75 ℃環境溫度範圍，以35 ℃環境中分解速率較快，此時一階分解反應速率常數為0.328 hr-1；另外，在0 ~ 30 g/m3濕度環境條件下，則以在乾燥環境中苯的分解速率較快，顯示過多的水氣，會與反應物競爭吸附活化位置，使得反應速率降低；在摻雜奈米碳管光觸媒(TP-C)的研究中，於所測試的摻雜範圍，奈米碳摻雜的比例愈高，苯的光催化分解速率愈快，並可減少因溫度提高，導致苯分解速率趨緩的現象，可在稍微高溫下，仍維持光觸媒對於苯的催化分解效果。測試結果發現以摻雜奈米碳管比率為1%時，在35 ℃下，苯蒸氣有最快的一階分解速率(k= 0.354 hr-1)；此外，添加適量濕度(10 g/m3)，可使光觸媒與水反應產生更多的自由基，有助於較高反應溫度下維持苯分解速率；最後，相較於原始純的光觸媒(TP)，本研究所製備之摻雜氧化石墨烯的光觸媒(TP-G)，在所測試之摻雜比例範圍(< 2%)，並未見具有提高苯蒸氣分解反應速率的小果，其可能是其與二氧化鈦光觸媒間的化學鍵結尚不足所致，值得後續再進行更多的觸媒研發。

Powder-form photocatalysts are widely tested in various studies for developing advanced oxidation processes for organic pollutants removal. However, they are difficult to be used in real application, since that powder-form photocatalysts are difficult to stay in the photocatalytic reactors for a long time. It is necessary to develop immobilized form photocatalysts for practical application purposes. Thin-film form photocatalysts should be one of the best choices.
Accordingly, this study developed and prpared TiO2-PVDF composite thin-films as photocatalysts for controlling typical a volatile organic pollutant, benzene (C6H6), from contaminated gaseous streams. The thin-film photocatalysts were prepared with an immersion precipitation method by mixing P-25 TiO2 and PVDF powders with some suitable solvents. Other than good photocatalytic oxidation capabilities, the prepared TiO2-PVDF thin films have several superior physical properties including high plasticity, low mechanical resistance, and high flexibility. In addition, easy to modify their activities by co-doping with other nano-carbon containing substances, such as, carbon nanotubes and graphene oxide, is another advantage, which has been demonstrated in this study. For confirming the prepared sample with good photocatalytic activities, some typical affecting factors for photocatalytic oxidation, such as, reaction temperature (35~75 oC), humidity, and types of light sources, were tested as well.
Some important results have been achieved in this study. The photocatalytic decomposition of benzene vapor basically followed the first-order reaction kinetics. Fast photocatalysis of benzene was observed under the illumination of near-UV light, but slow degradation rate of benzene was detected while using visible blue light as an only light source. For simple TiO2-PVDF thin-film as the photocatalyst, benzene peaked its decomposition rate at a reaction temperature 35oC in dry environment (k= 0.328 hr-1). Less degradation rate for benzene was also detected in higher temperature environment. The occurrence of water vapor would retard the photocatalysis of benzene due to adsorption competition among water and benzene vapor for the activated sites on photocatalysts.
On the other hand, after being doped with suitable amount of carbon-nanotube (CNT), the photocatalytic activities of TiO2-PVDF thin films were enhanced. Higher benzene degradation rates were demonstrated in the study. It is expected that the recombination rate of electron-hole pairs of photocatalysts was retarded due to CNT co-doping. It was found that the TiO2-PVDF thin film co-doped with 1% CNT achieved the highest benzene degradation rate (k= 0.354 hr-1, in dry condition). It was also observed that higher degradation rate of benzene was achieved in the presence of 10 g/cm3 water vapor, which might be due to more hydroxyl radicals formed while some humidity presenting if water vapor was not too much. One benefit for adding some CNT to the TiO2-PVDF thin films was to keep them with good photocatalytic activities in high temperature and humid conditions.
Finally, the photocatalytic activities of prepared TiO2-PVDF thin films were not enhanced much while co-doping with graphene oxide below 2%. It might be that the bonding between TiO2 and graphene oxide was not good enough by the current using preparation recipies or the amount of doped graphene oxide was not suitable. More investigation required is suggested.

摘要 I
Abstract III
致謝 V
目錄 VI
圖目錄 VIII
表目錄 XII
第一章 緒論 1
1-1研究緣起 1
1-2研究目的 4
第二章 文獻回顧 5
2-1苯環類揮發性有機物之污染現況與控制技術 5
2-1-1污染特性與環境衝擊 5
2-1-2苯蒸氣污染流佈現況 7
2-1-3苯控制技術相關文獻 7
2-1-4揮發性有機污染物控制技術 9
2-2半導體氧化物特性與光催化分解反應 10
2-2-1半導體氧化物特性 10
2-2-2半導體氧化物光催化分解反應程序 12
2-2-3影響半導體氧化物之光催化反應速率可能因子 14
2-2-4苯蒸氣之光催化分解研究 18
2-3光催化反應機制 19
2-3-1異相光催化反應原理 19
2-3-2異相光催化反應動力模式 19
2-4光觸媒製備技術 21
2-4-1薄膜光觸媒之製備技術 21
2-4-2聚偏氟乙烯薄膜製備技術 23
2-4-3奈米碳管特性與應用 24
2-4-4石墨烯特性與應用 25
2-4-5摻雜奈米碳材料之複合薄膜光觸媒製備技術與應用 27
第三章 研究材料與方法 32
3-1研究架構與規劃 32
3-1-1研究概要 32
3-2-2研究流程 33
3-2實驗材料與儀器 34
3-2-1實驗材料 34
3-2-2實驗儀器與設備 35
3-3實驗方法與分析 36
3-3-1薄膜光觸媒製備 36
3-3-2異相光催化反應系統 37
3-3-3苯環狀揮發性有機物分析 43
3-4複合材料表面特性分析 44
3-4-1掃描式電子顯微鏡 (Scanning Electron Microscope, SEM) 44
3-4-2 X光繞射分析儀 (X-ray Diffractometer, XRD) 46
第四章 結果與討論 49
4-1薄膜光觸媒特性分析 49
4-1-1薄膜光觸媒形貌分析(SEM) 50
4-1-2薄膜光觸媒表面化學成份分析(EDX) 56
4-1-3薄膜光觸媒晶相特徵分析(XRD) 61
4-2苯蒸氣應用於複合薄膜光觸媒光催化分解反應 64
4-2-1苯蒸氣分解反應速率關係 64
4-2-2光源對苯蒸氣分解反應之影響 65
4-2-3溫度對苯蒸氣分解速率影響 73
4-2-4濕度對苯蒸氣分解反應速率的影響 76
4-3奈米碳材之複合薄膜光觸媒對苯光催化分解反應 83
4-3-1摻雜奈米碳管比例對苯蒸氣分解速率影響 83
4-3-2摻雜氧化石墨烯比例對苯蒸氣分解反應速率的影響 90
4-3-3溫度、濕度及奈米碳材料比例對苯蒸氣分解反應速率複合影響 97
4-4苯去除效能比較 103
4-5薄膜及奈米碳材料對苯蒸氣之光催化分解反應機制 105
4-5-1薄膜對苯蒸氣之光催化分解反應機制 105
4-5-2摻雜奈米碳材料之光催化分解反應機制 106
第五章 結論與建議 108
5-1結論 108
5-2建議 109
參考文獻 110
附錄 A.各操作參數下之實驗值 125

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