The Oxidation-Microfiltration Removal of Fe(II) from Water｜國立臺灣科技大學博碩士論文系統

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研究生：	李彩虹 Lanny - Setyadhi
論文名稱：	The Oxidation-Microfiltration Removal of Fe(II) from Water The Oxidation-Microfiltration Removal of Fe(II) from Water
指導教授：	劉志成 Jhy-Chern, Liu
口試委員:	Suryadi Ismadji Suryadi Ismadji 李奇旺 Chi-Wang, Li 顧洋 Young, Ku
學位類別：	碩士 Master
系所名稱：	工程學院 - 化學工程系 Department of Chemical Engineering
論文出版年：	2008
畢業學年度：	96
語文別：	英文
論文頁數：	118
外文關鍵詞：	manganese, iron, humic acid
相關次數：	點閱：163 下載：1
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The presence of iron in groundwater can cause some health and aesthetic problems. Generally, the iron concentration in groundwater is below 10 mg/L. However, the higher iron concentration is not unusual phenomena to be found in groundwater. The maximum contaminant level (MCL) for iron in drinking water is 0.2 or 0.3 mg/L, depending on national policy. Among all treatment technologies, iron oxidation and microfiltration has been recognized as a cost effective technology in groundwater treatment.
In this study, high iron concentration (75 mg/L) was used. Iron removal was investigated by oxidation followed by microfiltration process. This study had three objectives: The first was to find the optimum pH for iron removal. Secondly, the effects of various operating conditions in filtration system, including membrane type, filtration pressure, and crossflow velocity, were investigated. Mixed cellulose ester membrane and polyvinylidene fluoride (PVDF) membrane represents hydrophilic and hydrophobic membrane, respectively. Filtration pressure used was 5, 8, and 10 psi. Crossflow velocity used was 0.48, 0.90, and 1.33 m/s. The suspension was maintained at 25oC in order to eliminate the effect of temperature. Lastly, the effects of manganese and organic matter (humic acid) on iron removal efficiency and permeate flux were also being studied. These experiments used fixed operating conditions (pH 8, hydrophobic PVDF membrane, 8 psi, and 1.33 m/s).
It was observed that the iron removal efficiency mainly depended on oxidation process conditions, although filtration process had additional effect on iron removal efficiency. Oxidation process at pH 8 followed by microfiltration membrane process produced permeate containing iron concentration below 0.3 mg/L. X-ray diffraction (XRD) and infrared analysis showed that iron oxides produced from oxidation process at pH 8 were lepidocrocite (-FeOOH) co-existing with magnetite (Fe3O4). Under laminar and turbulent flow condition, permeate flux would increase with filtration pressure. However, under laminar flow condition, there is certain anomaly beyond certain filtration pressure. Increasing crossflow velocity would increase the permeate flux. Cake resistance was the dominant resistances causing flux decline for all filtration conditions. Cake resistance increased with filtration pressure and decreased with the increase of crossflow velocity. The change of cake resistance value with filtration pressure and crossflow velocity could be explained by average specific cake resistance and cake mass per unit filtration area analysis. High value of average specific cake resistance means the lower cake porosity. High filtration pressure reduced the cake porosity and added more amounts of iron oxides on membrane surface. High crossflow velocity reduced the cake formation and increased the pressure drop across the filter cake. Permeate flux obtained using hydrophobic membrane was higher than that using hydrophilic membrane. The presence of manganese and organic matter decreased the iron removal efficiency and permeate flux. Permeate flux would increase with initial manganese concentration and decrease with increasing initial organic matter concentration. Cake resistance was the dominant resistances causing flux decline.

TABLE OF CONTENT

ABSTRACT	iv
ACKNOWLEDGEMENTS	vi
TABLE OF CONTENT	vii
LIST OF FIGURES	ix
LIST OF TABLES	xiii
LIST OF SYMBOLS	xiv
CHAPTER 1	INTRODUCTION	1
1.1	Background	1
1.2	Objectives	2
CHAPTER 2	LITERATURE REVIEW	3
2.1	Iron and manganese: effects, regulations, and removal methods	3
2.2	Kinetics of iron oxidation by aeration	4
2.3	Oxidation of iron in the presence of manganese	8
2.4	Oxidation of iron in the presence of natural organic matter (NOM)	9
2.5	Membrane filtration process	11
2.5.1	Crossflow microfiltration	12
2.5.2	Permeate flux and membrane fouling	13
CHAPTER 3	EXPERIMENTAL	15
3.1	Materials	15
3.2	Equipments	15
3.3	Procedures	17
3.3.1	The preparation of standard solution for:	17
3.3.2	Oxidation of water sample	17
3.3.3	Filtration of water sample	17
3.3.4	Oxidation of binary water sample	18
3.3.5	Filtration of binary water sample	18
3.3.6	Water sample analysis	19
3.3.7	Data Analysis	20
CHAPTER 4	RESULTS and DISCUSSION	21
4. 1	Optimum pH of iron oxidation reaction	21
4. 2	The effects of filtration pressure and crossflow velocity using hydrophilic membrane	43
4. 3	The effects of filtration pressure and crossflow velocity using hydrophobic membrane	60
4.4	The effects of manganese (Mn) on iron removal efficiency	76
4.5	The effects of organic matter on iron removal efficiency	92
CHAPTER 5	CONCLUSION AND SUGGESTION	108
5.1	Conclusions	108
5.2	Suggestions	108
REFERENCES	109
VITA	118



LIST OF FIGURES

Figure 2.1	Concentrations of hydrolysis products of Fe(III) in equilibrium at zero ionic strength and 25oC	6
Figure 2.2	Mole fraction of hydrolysis products of Fe(III) in equilibrium at zero ionic strength and 25oC	6
Figure 2.3	Hypothetical of humic acid molecular structure 	9
Figure 2.4	Iron behavior in presence of organic matter and oxygen 	10
Figure 3.1	Plate and sheet type module of crossflow microfiltration	16
Figure 3.2	Membrane filtration equipment	18
Figure 4.1	Iron concentration after oxidation process at different pH	22
Figure 4.2	The effects of oxidation condition on flux using hydrophilic membrane at 5 psi	25
Figure 4.3	The effects of oxidation condition on flux using hydrophilic membrane at 8 psi	26
Figure 4.4	The effects of oxidation condition on flux using hydrophobic membrane at 5 psi	30
Figure 4.5 	The effects of oxidation condition on flux using hydrophobic membrane at 8 psi	31
Figure 4.6	X-ray diffraction of iron oxides	37
Figure 4.7 	Fourier transform infra red spectrum of iron oxides formed at pH 8	38
Figure 4.8 	Zeta potential of iron oxides	39
Figure 4.9(a) 	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of original hydrophilic membrane	40
Figure 4.9(b) 	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of original hydrophobic membrane	40
Figure 4.9(c) 	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled hydrophilic membrane by iron oxides	40
Figure 4.9(d) 	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled hydrophobic membrane by iron oxides	41
Figure 4.9(e) 	Field emission scanning electron microscopy (FESEM) of iron oxides on hydrophilic membrane surface	41
Figure 4.9(f) 	Field emission scanning electron microscopy (FESEM) of iron oxides on hydrophobic membrane surface	41
Figure 4.9(g) 	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of iron oxides	42
Figure 4.10 	Flux under different filtration pressures in laminar region using hydrophilic membrane	43
Figure 4.11 	Total resistance under different filtration pressures in laminar region using hydrophilic membrane	44
Figure 4.12 	Flux under different filtration pressures in turbulent region using hydrophilic membrane	45
Figure 4.13 	Total resistance under different filtration pressures in turbulent region using hydrophilic membrane	46
Figure 4.14 	Resistance under different filtration pressures in laminar region using hydrophilic membrane	50
Figure 4.15 	Resistance under different filtration pressures in turbulent region using hydrophilic membrane	51
Figure 4.16 	Specific cake resistance and cake mass under different filtration pressures using hydrophilic membrane	52
Figure 4.17 	Flux under different crossflow velocities using hydrophilic membrane	54
Figure 4.18 	Total resistance under different crossflow velocities using hydrophilic membrane	55
Figure 4.19 	Resistance under different crossflow velocities using hydrophilic membrane	56
Figure 4.20 	Specific cake resistance and cake mass under different crossflow velocities using hydrophilic membrane at 8 psi	57
Figure 4.21 	Flux under different filtration pressures in laminar region using hydrophobic membrane	61
Figure 4.22 	Total resistance under different filtration pressures in laminar region using hydrophobic membrane	62
Figure 4.23 	Flux under different filtration pressures in turbulent region using hydrophobic membrane	63
Figure 4.24 	Total resistance under different filtration pressures in turbulent region using hydrophobic membrane	64
Figure 4.25 	Resistance under different filtration pressures in laminar region using hydrophobic membrane	66
Figure 4.26 	Resistance under different filtration pressures in turbulent region using hydrophobic membrane	67
Figure 4.27 	Specific cake resistance and cake mass under different filtration pressures using hydrophobic membrane	68
Figure 4.28 	Flux under different crossflow velocities using hydrophobic membrane	70
Figure 4.29 	Total resistance under different crossflow velocities using hydrophobic membrane	71
Figure 4.30 	Resistance under different crossflow velocities using hydrophobic membrane	72
Figure 4.31 	Specific cake resistance and cake mass under different crossflow velocities using hydrophobic membrane at 8 psi	73
Figure 4.32 	Iron removal under initial manganese concentrations after oxidation process	77
Figure 4.33 	Manganese removal under initial manganese concentrations after oxidation process	78
Figure 4.34 	Iron removal under initial manganese concentrations after filtration process	79
Figure 4.35 	Manganese removal under initial manganese concentrations after filtration process	80
Figure 4.36 	Flux under various initial manganese concentrations	83
Figure 4.37 	Particle size distributions in the presence of manganese after oxidation process	85
Figure 4.38 	Resistance under various initial manganese concentration	86
Figure 4.39 	Specific cake resistance and cake mass under various initial manganese concentrations	87
Figure 4.40(a)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when initial manganese concentration was 2 mg/L	88
Figure 4.40(b)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when initial manganese concentration was 37 mg/L	88
Figure 4.40(c)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of original hydrophobic membrane	88
Figure 4.40(d)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when manganese concentration was 37 mg/L	89
Figure 4.40(e)	Field emission scanning electron microscopy (FESEM) of original hydrophobic membrane (CROSS SECTIONAL VIEW)	89
Figure 4.40(f)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when initial manganese concentration was 2 mg/L (CROSS SECTIONAL VIEW)	89
Figure 4.40(g)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when initial manganese concentration was 37 mg/L (CROSS SECTIONAL VIEW)	90
Figure 4.40(h)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of precipitates when initial manganese concentration was 37 mg/L	90
Figure 4.41	Iron removal under various initial concentration of dissolved organic matter	94
Figure 4.42 	Organic matter removal under various initial concentration of dissolved organic matter	95
Figure 4.43 	Iron removal under various initial concentration of dissolved organic matter after filtration process	96
Figure 4.44 	Organic matter removal under various initial concentration of dissolved organic matter after filtration process	97
Figure 4.45	Flux under various concentrations of organic matter	98
Figure 4.46 	Particle size distributions in the presence of dissolved organic matter after oxidation process	100
Figure 4.47 	Resistance under various initial concentrations of organic matter	102
Figure 4.48 	Specific cake resistance and cake mass under various initial concentrations of NOM	103
Figure 4.49 	Fourier transform infra red (FTIR) spectrum of precipitated obtained after oxidation process: CFe = 75 mg/L; pH = 8; t = 15 min; DOC = 0 mg/L (A); DOC = 30 mg/L (B); DOC = 12 mg/L (C); DOC = 4 mg/L (D); humic acid (E)	104
Figure 4.50(a)	Field emission scanning electron microscopy (FESEM) of original hydrophobic membrane	105
Figure 4.50(b)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when initial dissolved organic matter concentration was 30 mg/L	105
Figure 4.50(c)	Field emission scanning electron microscopy (FESEM) of original hydrophobic membrane (CROSS SECTIONAL VIEW)	105
Figure 4.50(d)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of fouled membrane when initial dissolved organic matter concentration was 30 mg/L (CROSS SECTIONAL VIEW)	106
Figure 4.50(e)	Field emission scanning electron microscopy (FESEM) and energy dispersive x-ray spectrometer (EDX) of precipitates when initial dissolved organic matter concentration was 30 mg/L	106



LIST OF TABLES

Table 2.1	Hydrolysis and solubility constants for Fe(III) at zero ionic strength and 25oC	5
Table 4.1 	Iron concentrations under various pH and oxidation time	22
Table 4.2 	Experimental results from different oxidation condition using hydrophilic membrane	27
Table 4.3 	Experimental results from different oxidation conditions using hydrophobic membrane	32
Table 4.4 	Various resistances in different pH, membrane types, and filtration pressure	33
Table 4.5 	Infrared bands of lepidocrocite	34
Table 4.6 	X-ray powder diffraction data for iron oxides	36
Table 4.7 	Experimental results under different filtration conditions using hydrophilic membrane	48
Table 4.8 	Experimental results under different crossflow velocities using hydrophilic membrane at 8 psi	58
Table 4.9. 	Resistances under different filtration pressures and crossflow velocities using hydrophilic membrane	59
Table 4.10 	Experimental results under different filtration pressures using hydrophobic membrane	65
Table 4.11 	Experimental results under different crossflow velocities using hydrophobic membrane at 8 psi	74
Table 4.12 	Resistances under different filtration pressures and crossflow velocities using hydrophobic membrane	75
Table 4.13 	Experimental results under various initial manganese concentration	84
Table 4.14 	Experimental results under various initial dissolved organic matter concentration	99

                                

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