臺灣博碩士論文加值系統

奈米過濾(Nanofiltration, NF)薄膜程序因其選擇性而在近幾年代受到極大關注。本研究探討兩種NF薄膜 (NF270、NSK98) 在固定4 bars透膜壓差下的通量及鹽類去除率。其中實驗條件設為不同價數的硫酸鹽類溶液、進流液掃流速度以及溶液濃度。最後，利用薄膜質傳理論 (Film theory) 以及阻力串聯模式 (Resistance-in-series) 分析及量化兩個薄膜所受到的濃度極化 (Concentration Polarization) 現象。
研究結果顯示NF270薄膜的純水通量高於NSK98薄膜，表示其具有較佳的透水性。兩個薄膜的透水性分別為14.99 L/m²-hr-bar及10.40 L/m²-hr-bar。兩種薄膜對鹽類溶液中的鈉、鎂及鋁離子去除率分別為87%、99.1%及99.7%。NSK98薄膜的去除率也稍微高過NF270。薄膜的去除機制辨認為位阻排斥、Donnan排斥及雙電排斥。
增加掃流速度因促進剪切力而可減緩濃度極化的效應，導致通量及去除率上升。反之，增加進流液濃度會增加薄膜兩邊的滲透壓差，導致更多溶質累積在膜表上而降低通量及去除率。
溶質在過濾程序中的物質傳輸受濃度極化影響，其中在低流速及高濃度的條件下，極化效應較顯著。增加掃流速度可增加質傳係數，因此降低濃度極化層的厚度。
雖然積垢在本研究中視為可略，兩個薄膜所受到的濃度極化效應可能不同。NF270薄膜因通量較高，導致較多溶質被截留在膜表上，較難反擴散回巨相溶液中而形成較薄但較稠密的極化層，因此濃度極化係數較高。NSK98薄膜因通量較小，而去除率較佳，導致溶質較容易反擴散回巨相溶液，形成較厚但較稀疏的極化層，因此濃度極化對過濾產生的阻力較大。

Nanofiltration (NF) membrane processes have gained much attention over the past decades due to their selective rejection properties. The performance in relation to permeate flux and sulfate salt rejection under 4 bars constant transmembrane pressure of two commercial NF membranes (NF270 and NSK98) was examined in this study by varying the feed salt cation, cross-flow velocity and salt solution concentration. The concentration polarization effect encountered by the membranes was analyzed using the film theory and resistance-in-series model.
Results showed that the permeability of the NF270 membrane was significantly higher than that of NSK98, which were 14.99 L/m²-hr-bar and 10.40 L/m²-hr-bar respectively. However, both membranes displayed high rejection of cations, in which sodium, magnesium and aluminum ion rejection rates were over 87%, 99.1% and 99.7%. Furthermore, NSK98 had a slightly higher rejection than NF270. The main rejection mechanisms of salt solutions were identified as steric hindrance, Donnan exclusion and dielectric exclusion.
Increasing the cross-flow velocity resulted in higher permeate flux and salt rejections, which was due to enhanced shear rates, reducing the extent of concentration polarization. On the other hand, increasing the feed concentration lowered permeate flux and rejections, due to higher osmotic pressure difference on both sides of the membrane and accumulation of solutes on the membrane surface.
The mass transfer of solutes during filtration was governed by concentration polarization, which was more prominent at lower cross-flow velocities and higher feed concentrations. The value of the mass transfer coefficient increased with increasing cross-flow velocities, reducing the thickness of the polarization layer.
While fouling was negligible in all experiments conducted in this study, concentration polarization experienced by both membranes was speculated to be different. The higher flux of NF270 led to more solute accumulation on the membrane surface, which resulted in a higher concentration polarization modulus. The higher rejection of NSK98, coupled with its lower flux, enhanced solute back-diffusion, which resulted in a thicker, more resistant but less dense concentration polarization layer.

Table of Contents
摘要 I
Abstract III
Acknowledgments V
Table of Contents VI
List of Figures XI
List of Tables IX
Chapter 1 Introduction 1
1.1 Research background 1
1.2 Research objectives 3
Chapter 2 Literature Review 6
2.1 Membrane processes 6
2.1.1 Pressure-driven membrane filtration 6
2.1.2 Nanofiltration (NF) membrane 8
2.2 Separation mechanisms in nanofiltration 10
2.2.1 Steric Effects 11
2.2.2 Non-steric Effects 13
2.2.3 Factors affecting separation mechanisms in NF 18
2.3 Fouling in nanofiltration 20
2.3.1 Factors affecting fouling in NF 21
2.3.2 Effect of fouling on rejection 23
2.3.3 Assessment of fouling 24
2.3.4 Fouling control strategies 25
2.4 Concentration polarization (CP) 26
2.4.1 Description of CP 26
2.4.2 Concentration polarization control strategies 28
2.5 Modeling mass transport in NF 29
2.5.1 Film theory 30
2.5.2 Spiegler-Kedem model 37
2.5.3 Extended Nernst-Planck equation 40
2.5.4 Resistance-in-series model 43
Chapter 3 Materials and Methods 45
3.1 Chemicals and NF Membranes 45
3.1.1 Chemicals and reagents 45
3.1.2 Membrane properties 46
3.2 Experimental Setup 46
3.3 Experimental Protocol 50
3.3.1 Membrane pretreatment 50
3.3.2 Filtration experiments with salt solutions 51
3.4 Analytical Methods 55
3.4.1 Ion analysis 55
3.4.2 Membrane morphology 55
3.4.3 Contact angle measurements 55
3.5 Calculations 56
3.5.1 Film theory and mass transfer coefficient 56
3.5.2 Resistance-in-series model 59
Chapter 4 Results and Discussion 60
4.1 Membrane characterization 60
4.1.1 Morphology 60
4.1.2 Contact angle 63
4.2 Effect of salt solutions on membrane performance 64
4.2.1 Effect on permeate flux 64
4.2.2 Effect on rejection 67
4.3 Effect of cross-flow velocity on membrane performance 74
4.3.1 Effect on permeate flux 74
4.3.2 Effect on solute rejection 79
4.4 Effect of feed concentration on membrane performance 87
4.4.1 Effect on permeate flux 87
4.4.2 Effect on solute rejection 89
4.5 Effect of concentration polarization on membrane performance 93
4.5.1 Calculation of solute real rejection 93
4.5.2 Evaluation of membrane resistance to filtration 99
Chapter 5 Conclusions and Recommendations 106
5.1 Conclusions 106
5.2 Recommendations 108
References 109
Appendix 128

List of Tables
Table 2.1 Characteristics of different filtration methods 7
Table 2.2 Mass transport models in NF with inclusion of CP 30
Table 2.3 Sherwood number correlations 35

Table 3.1 Characteristics of feed salt solutions 45
Table 3.2 Properties of NF membranes 48

Table 4.1 Stabilized flux and flux reduction ratio of salt solutions 66
Table 4.2 Ionic and hydrated radii of ions 68
Table 4.3 Stabilized observed conductivity rejections and permeate conductivities of salt solutions 69
Table 4.4 Stabilized observed cation rejections and permeate conductivities of salt solutions 70
Table 4.5 Limiting molar ionic conductivities and mobilities of ions 73
Table 4.6 Stabilized flux and flux reduction ratio of Na2SO4 solution 75
Table 4.7 Stabilized flux and flux reduction ratio of MgSO4 solution 76
Table 4.8 Stabilized flux and flux reduction ratio of Al2(SO4)3 solution 77
Table 4.9 Stabilized observed conductivity rejections and permeate conductivities of Na2SO4 solution at three cross-flow velocities 80
Table 4.10 Stabilized observed conductivity rejections and permeate conductivities of MgSO4 solution at three cross-flow velocities 81
Table 4.11 Stabilized observed conductivity rejections and permeate conductivities of Al2(SO4)3 solution at three cross-flow velocities 82
Table 4.12 Stabilized observed sodium ion rejections and permeate concentrations at three cross-flow velocities 83
Table 4.13 Stabilized observed magnesium ion rejections and permeate concentrations at three cross-flow velocities 84
Table 4.14 Stabilized observed aluminum ion rejections and permeate concentrations at three cross-flow velocities 85
Table 4.15 Stabilized flux and flux reduction ratio of MgSO4 solution at three feed concentrations 88
Table 4.16 Stabilized observed conductivity rejections and permeate conductivities of MgSO4 solution at three feed concentrations 91
Table 4.17 Stabilized observed magnesium ion rejections and permeate concentrations at three feed concentrations 92
Table 4.18 Derivations of the mass transfer coefficients and boundary layer thickness of ions 94
Table 4.19 Summary of real and observed cation rejections and CP transport parameters for NF270 membrane 97
Table 4.20 Summary of real and observed cation rejections and CP transport parameters for NSK98 membrane 98
Table 4.21 Resistances to salt filtration 101
Table 4.22 Resistances to Na2SO4 filtration with variation of CFV 102
Table 4.23 Rresistances to MgSO4 filtration with variation of CFV 103
Table 4.24 Resistances to Al2(SO4)3 filtration with variation of CFV 104
Table 4.25 Resistances to MgSO4 filtration with variation of concentration 105
 
List of Figures
Figure 1.1 Research framework 5

Figure 2.1 The filtration spectrum 7
Figure 2.2 Schematic of membrane filtration process 8
Figure 2.3 Filtration modes 8
Figure 2.4 Schematic layers of a TFC membrane 10
Figure 2.5 Schematic diagram of membrane modules 10
Figure 2.6 Separation mechanisms in NF 11
Figure 2.7 Molecular sieving and solution-diffusion mechanism 12
Figure 2.8 Transport of solutes with hydration shells through a membrane 13
Figure 2.9 Donnan effect in a solution 16
Figure 2.10 Dielectric exclusion effect 17
Figure 2.11 Factors affecting fouling in NF 21
Figure 2.12 Membrane fouling mechanisms in the Hermia model 25
Figure 2.13 Concentration polarization (CP) and Cake-enhanced CP 26
Figure 2.14 Turbulent flow patterns around spacer nettings 28
Figure 2.15 Mass transfer of solutes in the CP layer 31
Figure 2.16 Resistances of NF membrane during filtration 44

Figure 3.1 Schematic representation of bench-scale NF setup 49
Figure 3.2 Picture of bench-scale NF setup 49
Figure 3.3 Picture of the cross-flow membrane filtration cell 50
Figure 3.4 Flow diagram of membrane pretreatment protocol 53
Figure 3.5 Flow diagram of experimental protocol for various CFVs and feed concentrations and salt solutions 54

Figure 4.1 Cross-sections of NF270 and NSK98 62
Figure 4.2 Membrane pores of NF270 and NSK98 62
Figure 4.3 Surface morphologies of NF270 and NSK98 62
Figure 4.4 EDS spectra of virgin NF270 and NSK98 63
Figure 4.5 Comparison of permeate flux of salt solutions to pure water flux 66
Figure 4.6 Observed conductivity rejections of salt solutions 69
Figure 4.7 Observed cation rejections of salt solutions 70
Figure 4.8 Effect of cross-flow velocity (CFV) on flux of Na2SO4 solution 75
Figure 4.9 Effect of CFV on flux of MgSO4 solution 76
Figure 4.10 Effect of CFV on flux of Al2(SO4)3 solution 77
Figure 4.11 Effect of CFV on observed conductivity rejection of Na2SO4 80
Figure 4.12 Effect of CFV on observed conductivity rejection of MgSO4 81
Figure 4.13 Effect of CFV on observed conductivity rejection of Al2(SO4)3 82
Figure 4.14 Effect of CFV on observed sodium ion rejection 83
Figure 4.15 Effect of CFV on observed magnesium ion rejection 84
Figure 4.16 Effect of CFVon observed aluminum ion rejection 85
Figure 4.17 Effect of feed concentration on flux of MgSO4 solution 88
Figure 4.18 Effect of feed concentration on observed conductivity rejection of MgSO4 solution 91
Figure 4.19 Effect of feed concentration on observed magnesium ion rejection 92
Figure 4.20 Effect of salt on filtration resistance of both membranes 101
Figure 4.21 Effect of CFV on resistance during filtration of Na2SO4 102
Figure 4.22 Effect of CFV on resistance during filtration of MgSO4 103
Figure 4.23 Effect of CFV on resistance during filtration of Al2(SO4)3 104
Figure 4.24 Effect of concentration on resistance during filtration of MgSO4 105

Figure A1 Static contact angle images of (a) NF270; (b) NSK98 128

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