臺灣博碩士論文加值系統

隨著環保意識的提高，海上洩漏油污、工業含油廢水與餐廳含油廢水的處理在成為迫切解決的議題。然傳統的含油廢水處理方法常有許多詬病之處。因此如何快速、簡單與有效率的處理含油廢水成為研究學者們重要課題。其中特殊潤濕性材料具有體積小、高效率、簡單等優點常被認為是油廢水處理的救星。
本研究以四級銨鹽高分子製備新型的抗菌油水分離膜處理含油廢水。研究分為四個部分作為探討：(1)合成的四級銨高分子之物理性質；(2)油水分離膜的性能；(3)乳液分離膜的性能；(4)破乳特性。
第一部份中，探討[2-(Methacryloyloxy)ethyl] trimethylammonium chloride solution (MATEAC)與[3-(Methacryloylamino) propyl)] trimethylammonium chloride solution (MAPTAC)兩種四級銨鹽單體及交聯劑的添加量對合成高分子之轉化率、耐水解度與溶脹比的影響。實驗結果顯示合成的四級銨鹽高分子轉化率皆大於99%，沒有未反應的單體殘留；MAPTAC高分子具有優異的耐水解特性，可做為油水分離膜材的合適選擇；MAPTAC高分子的溶脹比會隨著交聯劑的添加量增加而下降。
第二部份中，將四級銨鹽單體聚合在不鏽鋼網狀基材上，製成油水分離膜。製備的油水分離膜顯示出超親水與水下超疏油的潤濕特性，且能以大於 99％油水分離效率和4308 L·h-1·m-2 高滲透通量分離油水混合物並具有良好的抗菌性能。此外在酸、鹼、鹽水與高溫的條件下，油水分離效率仍可超過99％及高達120次重複使性，顯示製備的油水分離膜具有實務應用的潛力。
第三部份使用美耐皿海綿和聚乙烯醇海綿作為油水分離膜的基材製得油水分離海綿，製備的海綿具有水下超疏油性，對氯仿、庚烷、煤油、甲苯和植物油的油/水乳狀液的分離效率均達到99％以上。此外製備的海綿對大腸桿菌和金黃色葡萄球菌的抗菌效率超過99％。
第四部份探討製備的海綿之自發破乳特性。由於所製得的海綿中的MAPTAC高分子具有高的十二烷基硫酸鈉(SDS)吸附能力，因此製備的海綿可以自發的破壞SDS 乳液的平衡，被破壞平衡的乳液也會自發聚集形成大而不穩定的乳液，最後從乳液中自發分離而形成觀察到油層。上述的現象，本研究提出了一張自動破乳的機制圖來解釋。
綜上所述，本論文的研究成果有望在今後處理含油廢水和乳化含油廢水中發揮重要作用。

With increasing environmental awareness, the treatment of oil spills, industrial oily wastewater and restaurant oily wastewater had become an urgent problem. However, traditional methods often had many criticisms. So special wettability materials with advantages of small size, high efficiency, and simplicity to treat oily wastewater had played an important role. They are often considered as the savior of oily wastewater treatment.
In this study, a novel antibacterial oil water separation membranes were prepared by using a quaternary ammonium polymer to treated oily wastewater. The study was divided into four parts for discussion: (1) the physical properties of the synthesized quaternary ammonium polymer; (2) the performance of oil water separation membranes; (3) the performance of emulsion separation membranes; (4) demulsification characteristics.
In the first part, the effects of the addition of two quaternary ammonium salt monomers [2-(Methacryloyloxy) ethyl] trimethylammonium chloride solution (MATEAC) and [3-(Methacryloylamino) propyl)] trimethyl ammonium chloride solution (MAPTAC), and cross-linking agents, on the conversion rate, hydrolysis resistance and swelling ratio of synthetic polymers are discussed. The experimental results showed that the conversion of the synthesized quaternary ammonium polymer was above 99%, and no monomers remain for the reaction. MAPTAC polymer has excellent hydrolysis resistance and can be a suitable choice for oil-water separation membranes. The swelling ratio of MAPTAC polymer decreased with increasing cross-linking agent.
In the second part, a quaternary ammonium salt monomer was polymerized on a stainless steel mesh substrate to make an oil-water separation membrane. The prepared oil-water separation membrane exhibited superhydrophilic and underwater superoleophobic properties, and could separate oil water mixtures with oil-water separation efficiency of above 99% and flux of 4308 L·h-1·m-2, and possessed good antibacterial properties. Under the conditions of acid, alkali, saline and high temperature, the oilwater separation efficiency could also exceed 99% and the repeatability of the efficiency was 120 times, which showed that the prepared oil-water separation membrane had the potential for practical application.
In the third part, the quaternary ammonium salt monomer was polymerized on a melamine sponge and a polyvinyl alcohol substrate to make an oil water separation sponge. The prepared sponges exhibited the property of underwater superoleophobicity and its separation efficiencies for separating oil water emulsions of chloroform, heptane, kerosene, toluene, and vegetable oil were above 99%. Besides, the sponge’s antibacterial efficiency was above 99% for Escherichia coli and Staphylococcus aureus.
The fourth part discussed the spontaneous demulsification characteristics of the prepared sponge. Since the MAPTAC polymer in the prepared sponge had a high adsorption capacity of sodium lauryl sulfate (SDS), the prepared sponge could spontaneously break the balance of the SDS emulsion, and the emulsion would also spontaneously aggregate to form a large unstable emulsion. Finally, large unstable emulsion also spontaneous separated formed an observed oil layer. In this study, the above phenomenon was explained by a mechanism diagram of automatic demulsification.
In summary, the achievement of this paper were expected to play an important role in the treatment of general oily wastewater and emulsified oily wastewater in the future.

摘要 I
Abstract III
致謝 VI
總目錄 VII
表目錄 XI
圖目錄 XII
第一章 緒論 1
1-1 前言 1
1-2 研究動機、目的與架構 2
第二章 相關知識與文獻回顧 5
2-1 含油廢水的來源及處理方法 5
2-1-1 含油廢水的來源及危害 5
2-1-2 現行的含油廢水分離技術 6
2-2 膜分離技術 10
2-2-1 膜分離技術及應用 10
2-2-2 膜污染及影響因素 12
2-3 表面潤濕理論 14
2-3-1 楊氏(Young)方程式 14
2-3-2 溫佐(Wenzel)方程式 16
2-3-3 卡西-巴斯特(Cassie and Baxter)方程式 18
2-4 油水分離膜 20
2-4-1 阻水型油水分離膜 21
2-4-2 阻水型乳液分離膜 41
2-4-3 阻油型油水分離膜 45
2-4-4 阻油型乳液分離膜 52
2-5 多功能之油水分離膜 60
2-5-1 具抗菌功能之油水分離膜 60
2-5-2 具破乳功能之油水分離膜 68
第三章 實驗方法、設備及藥品 72
3-1 實驗藥品及材料 72
3-2 實驗器材 74
3-3 分析儀器 75
3-4 實驗方法 80
3-4-1 高分子溶液的配置與合成 80
3-4-2油水分離膜的製備 81
3-5 測試方法 82
3-5-1 轉化率測定(拜耳試驗) 82
3-5-2 油水分離效率測試 83
3-5-3 乳液分離效率測試 85
3-5-4 耐水解性測試 86
3-5-5 高分子溶脹比測試 87
3-5-6 抗菌測試 88
3-5-7 界面活性劑的吸附測試 89
3-5-8 破乳試驗 90
第四章 結果與討論 91
4-1 四級銨高分子之物理性質 91
4-1-1 四級銨高分子之合成與鑑定 91
4-1-2 四級銨高分子之耐水解特性 93
4-1-3 交聯劑添加量對溶脹比之影響 95
4-1-4 小節 96
4-2 油水分離網之特性 97
4-2-1 油水分離膜之表面潤濕特性 97
4-2-2不鏽鋼網孔徑對油水分離之影響 97
4-2-3 交聯劑添加量對油水分離效率與通量之影響 99
4-2-4 油水分離膜之耐候與耐用性 101
4-2-5 油水分離膜之表面型態與抗菌特性 104
4-2-6 小結 107
4-3 乳液分離海綿之特性 108
4-3-1 乳液分離海綿之表面型態 108
4-3-2 乳液分離海綿之油水分離性能與表面潤濕性 111
4-3-3 乳液分離海綿之抗菌機制與抗菌特性 114
4-3-4 小節 116
4-4 破乳性質 116
4-4-1 乳液分離海綿之巨觀破乳觀察 116
4-4-2 乳液分離海綿對SDS之的吸附特性 118
4-4-3 乳液分離海綿之破乳機制 120
第五章 結 論 122
5-1 結論與建議 122
5-2 建議 126
第六章 參考文獻 127
附錄A. 水中陰離子界面活性劑（甲烯藍活性物質）檢測方法－甲烯藍比色法 162
附錄B. 著作目錄 167

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