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研究生(外文):Kuo-Kai Chao
論文名稱(外文):Removal of Target PPCPs in Aqueous Solution using NF Membranes
口試委員(外文):Chin-Pao Huang
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。

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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