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研究生:趙國凱
研究生(外文):Kuo-Kai Chao
論文名稱:以奈米薄膜處理含標的藥物及個人保健用品水溶液之研究
論文名稱(外文):Removal of Target PPCPs in Aqueous Solution using NF Membranes
指導教授:蔣本基蔣本基引用關係
口試委員:黃金寶顧洋曾迪華張怡怡
口試委員(外文):Chin-Pao Huang
口試日期:2012-07-22
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:環境工程學研究所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2013
畢業學年度:101
語文別:英文
論文頁數:120
中文關鍵詞:奈米薄膜過濾藥物及個人保健用品吸附能力腐植酸褐藻酸鈉
外文關鍵詞:nanofiltrationpharmaceutical and personal care productsadsorption capacityhumic acidsodium alginate
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在本研究中,系統性地研究了所選出的四個在水環境中常見的藥物及個人保健用品 (acetaminophen, carbamazepine, sulfamethoxazole, 和naproxen),經過奈米薄膜NF270掃流式過濾後的去除率。水中酸鹼值對於目標汙染物的去除率的影響,在酸鹼值4到10的範圍內試驗。除此之外,腐植酸和褐藻酸鈉被選為模型有機積垢物,用以研究薄膜積垢對於目標汙染物去除率的影響。並且,鈣和有機積垢物的交互作用,在本研究中也一併納入考量。
研究結果顯示,經腐植酸或褐藻酸積垢的奈米薄膜NF270,皆比清淨的薄膜,具有較高的疏水性。除此之外,清淨膜面的界達電位,在酸性的水中酸鹼值範圍內,有著劇烈的變化。且離子強度是影響膜面界達電位的重要因子。
對於在中性水中酸鹼值範圍內帶負電的化合物,也就是sulfamethoxazole和naproxen而言,當水中酸鹼值接近其酸解離常數時,水中酸鹼值對去除率的影響顯得相當重要。而有機積垢物和鈣的影響,會造成中性化合物去除率的改變,特別是疏水中性的化合物,carbamazepine。
清淨奈米薄膜NF270吸附所選的藥物及個人保健用品,其結果分為三類。第一類是在水中酸鹼值為10時,四種目標藥物都呈現有限的吸附能力,皆低於0.06微克/平方公分;第二類為水中酸鹼值範圍為5到9時,疏水中性的carbamazepine為主要吸附到清淨膜面的藥物。且在水中酸鹼值為7時,有最大的吸附能力0.22微克/平方公分;第三類是水中酸鹼值為4時,主要吸附到清淨膜面的藥物為naproxen,具有0.57微克/平方公分的吸附能力。這結果可歸因於在水中酸鹼值為4時,中性的naproxen成為主要的物種,而不再是解離帶負電的naproxen,且較其他藥物具有更高的疏水性,其正辛醇/水分配係數為3.18。


In this study, the rejection of four selected compounds (acetaminophen, carbamazepine, sulfamethoxazole, and naproxen) by cross-flow nanofiltration using membrane NF270 was systematically investigated. These compounds, pharmaceutical and personal care products, are ubiquitous in the aquatic environment. The effect of pH on rejection of target compounds was also conducted in the range between 4 and 10. Furthermore, the effect of organic fouling on rejection of selected compounds was studied using humic acid and sodium alginate as model organic foulants. Besides, the interaction between organic foulants (humic acid and sodium alginate) and calcium was also considered in this research.
The results show that NF270 membrane fouled by humic acid and by alginate became more hydrophobic than clean membrane, regardless of which organic foulant was present. Furthermore, zeta potential of clean NF270 membrane surface dramatically changed around the acidic pH range. Moreover, ion strength is a key factor in affecting zeta potential of membrane surface.
For negatively charged compounds, namely sulfamethoxazole and naproxen, at neutral pH range, pH played an important role in rejection, especially when pH was near the pKa of the target compounds. The organic foulants and calcium could affect the rejection of organic compounds, especially the hydrophobic and neutral carbamazepine.
Results of the adsorption of selected PPCPs on clean NF270 membrane as a function of pH was can be divided into three groups according to the pattern of figure. In group Ⅰ, all four compounds have limited adsorption capacity at pH 10, and the adsorbed mass was less than 0.06 μg/cm2 for each compound. In group Ⅱ, hydrophobic and neutral compound, CBZ, was the major compound adsorbed among all four selected compounds at pH range between 5 and 9. In addition, the mass of CBZ adsorbed on clean NF270 membrane was maximum at pH 7, where the adsorbed mass of CBZ was 0.22 μg/cm2. In group Ⅲ, naproxen became the major compound adsorbed with an adsorption density of 0.57 μg/cm2 at pH 4. This result could be attributed to the neutral NAP species being a dominant species at pH 4, and its relative high hydrophobicity with 3.18 of Log Kow compared to other compounds.


誌謝 i
Abstract ii
摘要 iv
Contents v
List of figures viii
List of tables xii
Chapter 1 Introduction 1
1-1 Background 1
1-2 Objectives 3
Chapter 2 Literature Review 4
2-1 Occurrence of pharmaceutical and personal care products 4
2-1-1 Carbamazepine 4
2-1-2 Acetaminophen 5
2-1-3 Sulfamathoxazole 6
2-1-4 Naproxen 7
2-1-5 Occurrence of selected PPCPs in nature water and engineered process 7
2-2 Removal and rejection mechanisms of PPCPs by nanofiltration 12
2-2-1 Size exclusion 12
2-2-2 Electrostatic repulsion 13
2-2-3 Adsorption 14
2-3 Influences of water solution chemistry and solute/membrane properties on PPCPs rejection during nanofiltration 18
2-3-1 Presence of calcium ion 21
2-3-2 Organic foulants 22
2-3-3 Natural organic matters 24
2-4 Nanofiltration predicting model 25
Chapter 3 Materials and Methods 30
3-1 Research planning 30
3-1-1 Research flowchart 30
3-1-2 Experimental design 31
3-2 Characteristics of NF membrane 32
3-3 Target compounds 33
3-4 Experimental methods 35
3-4-1 Cross-flow filtration protocol 35
3-4-2 Adsorption tests 36
3-5 Analytical technique 38
3-5-1 Atomic absorption spectrophotometer (AAS) 38
3-5-2 Total organic carbon (TOC) 38
3-5-3 HPLC/UV 39
3-5-4 Scanning electron microscope/Energy dispersive spectrometer (SEM/EDS) 41
3-5-5 Contact angle measurement 42
3-5-6 Zeta potential measurement 43
3-6 Chemical reagents 44
Chapter 4 Results and Discussion 45
4-1 Characterization of membranes 45
4-1-1 SEM image 45
4-1-2 Contact angle 51
4-1-3 Zeta potential of membranes 57
4-2 Influences of membrane fouling on rejections 62
4-2-1 Effect of pH 62
4-2-2 Effect of humic acid/calcium fouling 63
4-2-3 Effect of alginate/calcium fouling 69
4-3 Determination of adsorption capacity 74
4-3-1 Multi-components adsorption on clean NF270 membrane under various pH values 74
4-3-2 Adsorption capacity on fouled NF270 membranes 85
Chapter 5 Conclusions and Recommendations 98
5-1 Conclusions 98
5-2 Recommendations 100
References 101
Appendix 110


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