臺灣博碩士論文加值系統

本研究應用電泳沉積技術（Electrophoretic Deposition, EPD），製備單純TiO2光觸媒與系列摻雜不同比例(0.5 %、1.0 %、1.5 %)石墨烯(GR)之TiO2複合光觸媒薄膜，藉以進行水溶液中磺胺嘧啶(Sulfadiazine, SDZ)光催化分解研究。首先，進行觸媒製備參數對薄膜光觸媒活性之測試實驗，分別探討不同煅燒溫度(250至450 oC)及EPD鍍膜電壓(15至35V)，藉以確認活性較佳之薄膜光觸媒製備參數。其後，再繼續針對較佳活性的光觸媒試片，測試它們在不同環境條件下(光源及pH值)，對磺胺嘧啶有機物的分解速率之影響。此外，本研究除了進行污染物的分解實驗外，同時也藉由多種光觸媒表面特性的分析(如X光繞射分析儀、掃描式電子顯微鏡)，確認觸媒本質特性與光觸媒活性的關係。
研究結果顯示：本研究所製備的光觸媒，對於SDZ的光催化分解反應，符合近一階反應動力關係；在250至450℃的煅燒溫度範圍內，以煅燒溫度450℃的光觸媒試片，具有最快的反應速率，其中，以TG0.5試片具有最高活性(SDZ分解速率k= 0.348 hr-1)，較TiO2試片之反應速率高出13.7 %；另外，EPD製備電壓對於光催化分解速率影響的研究中，TiO2試片的光催化活性會隨著EPD製備電壓上升而增加，以製備電壓35 V時，具有最高活性；而TG系列光觸媒中，則會在某個EPD製備電壓下，具有最快反應速率，其分別依序為：TG0.5(25 V)、TG1.0(20 V)、TG1.5(20 V)。根據上述結果，可以發現在煅燒溫度為450℃具有最高活性，而不同系列光觸媒也具有最佳EPD製備電壓，可彙整出具有較高活性之光觸媒試片，試片編號依序為：450TiO2-35V、450TG0.5-25V、450TG1.0-20V、450TG1.5-20V。
最後，針對較佳活性的光觸媒試片進行不同光源與pH值，對光催化分解反應影響的研究。根據實驗結果發現，各系列觸媒均在pH= 3環境條件下，SDZ分解效率最快，且觸媒吸附污染物比例也最多；另外，由於TiO2光觸媒本身對於可見光吸收能力極差，實驗結果發現摻雜石墨烯的光觸媒試片，不僅可以增加原本TiO2光觸媒的活性之外，同時也可增加觸媒對可見光源的吸收，使得相關污染物在可見光光源下，進行光催化分解反應。最後，本研究所製備的光觸媒中，以摻雜0.5 %石墨烯之光觸媒，在UV光及LED光下具有最高活性。

This study investigated liquid-phase photocatalysis of sulfadiazine(SDZ) by both titanium dioxide (TiO2) and graphene doped TiO2 (GR/TiO2) thin-film. The thin-film photocatalysts were prepared with an electrophoretic deposition (EPD) technique by immobilizing P-25 TiO2, with various amount of GR, onto pure titanium (Ti) metal plates. This study explored the effects of preparation recipes on the photocatalytic activities of prepared samples, which were determined by the degradation rate of SDZ assisted by the prepared samples irradiated with a near-UV light. Several preparation parameters including applied DC biases (15~35 V), and terminal calcination temperatures (250~450℃) for the samples were evaluated. The study also used SEM and XRD to identify surface morphology, and crystal phase of prepared samples. Selected photocatalysts with better activities were further used for conducting SDZ photocatalytic degradation tests in variation pH levels and light sources.
The results showed the photocatalysis of SDZ following pseudo first-order reaction kinetics. A better photocatalytic activities of prepared samples were achieved when the they were prepared with calcined in a 450℃ oven. Among them, TG0.5 photocatalyst has the highest activity (k = 0.348 hr-1), which is 13.7 % higher than that of TiO2 photocatalyst. In addition, the effect of EPD of DC biases on the degradation rate of SDZ, the photocatalytic activity of TiO2 increases with the increase of EPD of DC biases, with the highest activity at 35 V. The TG series of photocatalyst, it will be in a EPD of DC biases, with the fastest response rate, which are: TG0.5 (25 V), TG1.0 (20 V), TG1.5 (20 V). Based on the above results, it can be found that the calcination temperature is 450 ℃ with the highest activity, and different series of photocatalyst also has the best EPD of DC biases, can be assembled with a high activity of the photocatalyst, in order: 450TiO2-35V, 450TG0.5-25V, 450TG1.0-20V, 450TG1.5-20V.
Finally, the effects of different light sources and pH values on degradation rate of SDZ were investigated. According to the experimental results, it was found that the degradation rate was the fastest and the proportion of pollutants adsorbed by the catalyst at pH= 3. In addition, the TiO2 photocatalyst itself is very poor for the visible light absorption capacity. The experimental results show that the photocatalyst doping of graphene can not only increase the activity of the original TiO2 photocatalyst, but also increase the absorption of the visible light source. Finally, the photocatalyst prepared in this study has the highest activity in UV light and LED light with photocatalyst doped with 0.5% graphene.

摘要 i
Abstract iii
致謝 v
目錄 vi
表目錄 viii
圖目錄 x
第一章 前言 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 磺醯胺類藥物(sulfonamides) 5
2.1.1 磺醯胺類藥物簡介 5
2.1.2 磺醯胺類藥物流佈現況及危害性 6
2.1.3 磺醯胺類藥物之處理技術 10
2.2 光催化反應程序原理 11
2.2.1 半導體材料性質 11
2.2.2 光催化反應程序 14
2.2.3 異相光催化反應動力模式 16
2.2.4 影響光催化反應速率之可能因子 19
2.3 二氧化鈦光觸媒 22
2.3.1 二氧化鈦之結構與特性 22
2.3.2 二氧化鈦光催化反應機制 24
2.3.3 二氧化鈦光觸媒之製備技術 25
2.3.3.1 電泳沉積(Electrophoretic deposition, EPD) 26
2.4 摻雜改質之二氧化鈦光觸媒 31
2.4.1 石墨烯之結構與特性 32
2.4.2 複合石墨烯之光觸媒於污染物去除應用 33
第三章 研究方法與材料 34
3.1 實驗內容與規畫 34
3.1.1 研究概要 34
3.1.2 研究流程 34
3.2 實驗材料與設備 36
3.2.1 實驗材料 36
3.2.2 實驗儀器與設備 36
3.3 實驗方法與分析 37
3.3.1 光觸媒薄膜之製備 37
3.3.2 異相光催化反應系統 40
3.3.4 磺胺嘧啶藥品濃度檢測 43
3.4 光觸媒表面特性分析儀器 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 47
4.1光觸媒薄膜特性分析 47
4.1.1光觸媒薄膜之表面形貌分析(SEM) 47
(1)純鈦金屬板表面形貌 48
(2)單純二氧化鈦光觸媒表面形貌 49
(3)摻雜石墨烯二氧化鈦光觸媒表面形貌 52
4.1.2光觸媒表面化學組成成分分析(EDX) 56
4.1.3光觸媒晶相特徵分析(XRD) 59
4.2電泳沉積製備參數對觸媒活性影響 63
4.2.1電泳沉積-電壓影響 63
4.2.2煅燒溫度之影響 66
4.3磺胺嘧啶光催化分解實驗 69
4.3.1觸媒煅燒溫度的影響 69
4.3.2電泳沉積-沉積電壓的影響 82
4.3.3水溶液pH值之影響 85
4.3.3.1 pH值對SDZ光催化分解速率之影響 85
4.3.3.2 pH值對光觸媒暗吸附SDZ之影響 90
4.3.4光源之影響 93
4.3.5石墨烯摻雜比例之影響 97
4.4光催化反應機制探討 101
第五章 結論與建議 103
5.1結論 103
5.2建議事項 104
參考文獻 104
附錄A. 磺醯胺類化合物光催化分解反應濃度隨時間變化一覽表 A-1

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