臺灣博碩士論文加值系統

目前在高級氧化處理(AOPs)中，主要是以自由基氧化來去除污染物，而其中自由基主要來自於氧化劑，本研究中的氧化劑為過一硫酸氫鉀(PMS)，其產生的硫酸根自由基(SO4-•)有著比氫氧根自由基(OH•)更強的氧化還原電位，但是PMS產生硫酸根自由基速度過慢，通常需要過渡金屬作為催化劑，而為了減少金屬催化劑的成本及對環境的影響，所以非金屬催化劑為未來趨勢，本研究中以一步製備的硫摻雜碳氮化物（CNS）作為非金屬和易於製備的催化劑來激活PMS以降解目標污染物羅丹明B (RhB)及酚甲烷(BPA)。
CNS分別以FE-SEM、TEM、BET、XRD、XPS等儀器詳細分析材料特性，由於所製備的CNS顯示出比未摻雜硫的碳氮化物（CN）更高的表面積和催化活性，且在可見光照射下，CNS激活PMS降解污染物的程度也遠高於CN激活的PMS，所以我們推測CNS中硫和氮共摻雜的協同作用可能使CNS表現出更高的催化能力和光催化性。
於降解污染物RhB及BPA的測試實驗中，以溫度、pH值、共存離子模擬目標污染物可能出現的環境，在CNS催化PMS在高溫、中性條件下更有利於降解污染物，而在污染水體中含有濃縮NaCl當共存離子下，CNS催化PMS降解污染物的效果則不受影響。透過自由基清除劑的測試證明實驗中主要作用的自由基為硫酸根自由基，最後在CNS回收實驗中以同一批CNS來催化PMS的降解污染物效果幾乎不受影響，由這些特徵表明CNS是一種方便製備、有效的非金屬光催化劑，且適用於催化PMS降解RhB及BPA。

Advanced Oxidation Processes (AOPs) mainly removes contaminants by free radical oxidation which is produced from oxidants. In this study, Potassium peroxymonosulfate (PMS) was used as the oxidant to produce sulfate radicals (SO4-•) which had stronger redox potential than hydroxyl radical (OH•). However, it shows slow response for PMS producing sulfate radicals. A transition metal catalyst to enhance activate degradation speed is needed. In order to reduce the cost and environmental impact of the metal catalyst, non-metallic catalysts will be seen as a future trend. In this work, one-step preperation for sulfur-doped carbon nitride (CNS) was used as a non-metallic and easily prepared catalyst to activate PMS to degrade target contaminants Rhodamine B (RhB) and Bisphenol A (BPA).
CNS was analyzed by FE-SEM, TEM, BET, XRD, XPS and other instruments.
Since the prepared CNS exhibits a higher surface area and catalytic activity than the undoped sulfur-based carbonitride (CN). Contaminants degradation by CNS activated PMS exhibits a much higher efficiency than CN activated PMS. Therefore we speculate that the synergistic effect of sulfur and nitrogen co-doping in CNS may lead CNS exhibit higher catalytic and photocatalytic properties.
From RhB and BPA degradation test, temperature, pH, co-existing ion simulation of the target contaminants may occur in the environment. It is more conducive for CNS catalyzed PMS to degrade contaminants in high temperature and neutral conditions. When high concentrated NaCl as co-existing ions was added into contaminated water, the effect of CNS catalyzed PMS degradation was not affected. The free radical scavenger test proved that sulfate radicals are the main free radicals in this experiment. Finally, five times CNS recyclability recveals almost the same result to CNS catalyzed PMS degradation batch experiment. These characteristics indicate that CNS is a convenient preparation and effective nonmetallic photocatalyst and is suitable for catalyzing PMS degradation of RhB and BPA.

摘要 i
abstract ii
目錄 iii
圖目錄 v
表目錄 vi
第一章緒論 1
1-1.研究動機 1
1-2.研究目的 2
第二章文獻回顧 3
2-1.降解水中污染物 3
2-1-1.染整廢水 3
2-1-2.Rhodamine B 5
2-1-3.新興污染物 9
2-1-4.Bisphenol A 10
2-2.高級氧化程序(AOPs) 13
2-2-1.高級氧化程序介紹 13
2-2-2.硫酸根自由基氧化 15
2-2-3.過一硫酸氫鉀光催化 16
2-3.製作觸媒 17
2-3-1.非金屬碳氮化物異相光催化劑 17
2-3-2.CNS可見光催化過一硫酸氫鉀 19
第三章實驗材料與方法 20
3-1.實驗設計 20
3-2.實驗藥品及儀器 22
3-3.材料製作與鑑定 24
3-3-1.CNS合成方法 24
3-3-2.CNS材料鑑定 24
3-3-2-1.場發射掃描式電子顯微鏡(FE-SEM) 24
3-3-2-2.穿透式電子顯微鏡(TEM) 25
3-3-2-3.比表面積及孔徑分析儀(BET) 25
3-3-2-4.X射線繞射分析儀(XRD) 26
3-3-2-5.X射線光電子能譜儀(XPS) 26
3-3-2-6.界達電位分析(Zeta potential) 26
3-3-2-7.紫外可見慢反射光譜(DRS) 27
3-4.實驗方法 28
3-4-1.CNS催化實驗 29
3-4-1-1.吸附排除實驗 29
3-4-1-2.單純氧化實驗 29
3-4-1-3.光催化實驗 29
3-4-1-4.光催化比較實驗 30
3-4-2.最佳參數實驗 30
3-4-2-1.催化劑加藥量變化 30
3-4-2-2.氧化劑加藥量變化 30
3-4-2-3.溫度變化 30
3-4-2-4.pH值變化 31
3-4-2-5.離子強度變化 31
3-4-2-6.抑制劑測試 31
3-4-2-7.催化劑穩定性回收測試 31
第四章結果與討論 32
4-1.材料鑑定 32
4-1-1.表面結構及內部晶格構造(FE-SEM、TEM、BET、XRD) 32
4-1-2.材料與表面之特性和結構(XPS、Zeta potential、DRS) 35
4-2.CNS光催化PMS降解染整目標污染物RhB 39
4-2-1.CNS催化實驗 39
4-2-2.催化劑加藥量變化 41
4-2-3.氧化劑加藥量變化 42
4-2-4.溫度變化 43
4-2-5.pH值變化 44
4-2-6.離子強度變化 45
4-2-7.抑制劑測試 46
4-2-8.催化劑穩定性回收測試 47
4-3.CNS光催化PMS降解新興目標污染物BPA 48
4-3-1.CNS催化實驗 48
4-3-2.催化劑加藥量變化 49
4-3-3.氧化劑加藥量變化 50
4-3-4.溫度變化 51
4-3-5.pH值變化 52
4-3-6.離子強度變化 53
4-3-7.抑制劑測試 54
4-3-8.催化劑穩定性回收測試 55
第五章結論與建議 56
5-1.結論 56
5-2.建議 57
參考文獻 58

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