以RO/NF薄膜處理電廠模擬廢液之研究｜國立清華大學博碩士論文庫

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研究生：	顧雨軒 Ku, Yu-Hsuan
論文名稱：	以RO/NF薄膜處理電廠模擬廢液之研究 The study of RO/NF membrane processes for simulated liquid radioactive waste treatment
指導教授：	王竹方 Wang, Chu-Fang
口試委員:	蔣本基張怡怡王竹方林俊德倪辰華
學位類別：	碩士 Master
系所名稱：	原子科學院 - 生醫工程與環境科學系 Department of Biomedical Engineering and Environmental Sciences
論文出版年：	2012
畢業學年度：	100
語文別：	英文
論文頁數：	111
中文關鍵詞：	低放射性廢液、逆滲透、奈濾、雷射剝蝕感應耦合電漿質譜儀
外文關鍵詞：	LLRW, reverse osmosis, nanofiltration, Hermia model
相關次數：	點閱：2 下載：0
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薄膜過濾已被廣泛地運用在電廠低放射性廢液處理當中，其中奈濾膜及逆滲透膜可用來濾除廢液中之膠體粒子及溶解性鹽類。本研究探討市售幾種奈濾膜及逆滲透膜在不同pH條件下對電廠廢液中常見金屬物種之阻擋率變化情形，其中過渡金屬阻擋率隨pH值上升而增加，但因為濾餅層堆積所加強的濃度極化效應，反而導致鹼金屬與鹼土金屬元素隨pH值上升阻擋率下降。其他操作參數如壓力、進流濃度也在研究中一併被探討。為了解薄膜阻塞的機制，本研究嘗試應用雷射剝蝕感應耦合電漿質譜儀(LA-ICP-MS)搭配α-step表面輪廓儀，針對已堵塞之薄膜進行分析，取得不同元素在表面及深度累積分布的資訊。此分析結果與Hermia阻塞模式計算結果頗為一致，極具潛力成為新的探討阻塞機制之分析工具。此外，超音波造影可以微米尺度觀察薄膜表面及堵塞物之型態，可作為觀察薄膜阻塞及後續清洗評估的簡易快速方法。

Membrane filtration has been applied to the treatment of liquid low-level radioactive wastes (LLRW) worldwide. In this study, removal of dissolved salts and transition metal species from simulated nuclear wastewater was investigated with NF270 and several RO membranes at different pH conditions. Rejection rates of various species are highly dependent on the solution pH. Generally, rejection rates of transition metals increased with elevated pH levels while the opposite trend occurred in those of alkali and alkaline earth metal species due to cake-enhanced concentration polarization. Other operating parameters such as pressure and feed concentration were also discussed. To investigate membrane fouling mechanism, laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) combined with α-step profilometer was first applied in fouled membrane analysis. The results of foulants spatial distribution and depth profile are quite consistent with the two-phase fouling mechanisms based on Hermia model. Besides, ultrasonic imaging system was used to observe the morphology of membrane surface in micro-scale. It provides a quick and convenient way to evaluate the severity of membrane fouling.

摘要    I
Abstract    II
Contents    III
Table index    VI
Figure index    VII
Chapter 1 Introduction    1
1.1  General overview    1
1.2  Aims of this study    3
Chapter 2 Literature Review    6
2.1  Membrane basics    6
2.1.1  Classification of membranes    6
2.1.2  Membrane materials    8
2.1.3  Transport mechanisms of membrane filtration     11
2.2  Membrane filtration for liquid radioactive waste (LRW) process    14
2.3  Membrane fouling    18
2.3.1  Scale formation    18
2.3.2  Hermia model for membrane fouling    20
2.4  Conventional analytical methods for fouled membranes    24
2.5  Introduction of LA-ICP-MS    29
2.5.1  Developments and applications of LA-ICP-MS    29
2.5.2  Mapping technique of LA-ICP-MS     32
2.5.3  Depth profile of LA-ICP-MS    34
Chapter 3 Experimental    36
3.1  Reagents and materials     36
3.2  Apparatus    39
3.2.1  Three-channels high pressure plate-and-frame membrane filtration system    39
3.2.2  LA-ICP-MS    41
3.2.3  α-step profilometer    45
3.2.4  Ultrasound imaging system    47
3.3  Details of experimental methods     49
3.3.1  Filtration methods    49
3.3.2  RO/NF scaling tests    50
3.3.3  Preparation of LA-ICP-MS standard for quantitation    52
3.3.4  Mapping technique of LA-ICP-MS    53
3.3.5  Depth profile of fouled membranes    54
Chapter 4 Results and discussion    56
4.1  Performance of membranes    56
4.1.1  Permeate flux    56
4.1.2  Conductivity rejection at different operating pressure    59
4.1.3  Metal rejection at different pH    62
4.1.4  Cs and Co rejections    73
4.2  Studies of membrane fouling    75
4.2.1  Fouling mechanism identified by Hermia model    75
4.2.2  Scalants distribution on the membrane surface    79
4.3  Identification of Hermia model by LA-ICP-MS/α-step profilometer analysis    88
4.3.1  The foulants distribution based on Hermia model    88
4.3.2  Depth profile of the fouled membranes    90
4.4  Ultrasonic imaging of the fouled membranes    95
Chapter 5 Conclusions and future work    100
5.1  Conclusions    100
5.2  Future work    101
Reference    102 


Table index
Table 2.1  Features and limitation of different treatment options    15
Table 2.2  Examples of membrane technology for nuclear waste processing    16
Table 2.3  Radioactive liquid wastes at Oconee Nuclear Station    17
Table 2.4  Recent applications of LA-ICP-MS    30
Table 2.5  Comparison of LA-ICP-MS and other analytical techniques    31
Table 3.1  Properties of the membranes employed in this study    38
Table 3.2  Operation conditions for laser ablation    43
Table 3.3  The scan parameters of Dektak 150 α-step profilometer system in this study    46
Table 3.4  The elements of feed solution analyzed by ICP-MS    51
Table 3.5  The information of calibration curves for LA-ICP-MS quantitation    53
Table 4.1  Water permeability and linearity correlation of tested membranes    58
Table 4.2  Mass balance of the elements analyzed in the fouling test    87
Table 4.3  Signal intensity of each crater    91
 

Figure index
Figure 1.1  Flowchart of the experimental scheme    5
Figure 2.1  Semi-permeable membrane pore size ranges, with categories of impurities for which they are effective    7
Figure 2.2  Schematic representation of the concentration polarization    12
Figure 2.3  Scale formation mechanism on membranes    19
Figure 2.4  Hermia model solutions    22
Figure 2.5  Schematic representation of the principle of UTDR measurement in a membrane module. (a) cross-sectional view of the separation cell (b) time-domain response    25
Figure 2.6  AFM images of AFC99 membrane. (a) Scanned by tip (b) Scanned by silica colloid probe (diameter 4.2 μm)    27
Figure 3.1  A photograph of membrane filtration system    39
Figure 3.2  The schematic diagram of membrane filtration system (Dead-end). 1. feed tank ; 2. pump ; 3. by-pass ; 4. valve ; 5. pressure gauge ; 6. membrane cell ; 7. membrane ; 8. permeate    40
Figure 3.3  A photograph of Newwave UP 213 laser system    41
Figure 3.4  The schematic diagram of the LA system    42
Figure 3.5  A photograph of Agilent 7500a ICP-MS    43
Figure 3.6  The schematic diagram of ICP-MS    44
Figure 3.7  A photograph of α-step profilometer (Dektak 150, Veeco) system    45
Figure 3.8  The block diagram of Dektak 150 profilometer system    46
Figure 3.9  Schematic diagram of a homemade ultrasound imaging system    47
Figure 3.10  Illustrations of C-mode scanning    48
Figure 3.11  Photographs of fouled membranes (a)AD (at pH 4) ; (b)AD (at pH 9) ; (c)NF270 (at pH 4)    51
Figure 3.12  The multi-element mixed standard solutions on the membrane    52
Figure 3.13  The track of laser spot in line scan mode    54
Figure 3.14  (a) Craters on the membrane surface ablated by laser system for 1, 5, 10, 20, 40, 60 seconds ; (b) Cross-section of the ablation craters measured by Dektak 150    55
Figure 4.1  Effect of pressure on permeate flux    56
Figure 4.2  Effect of pressure on conductivity rejection    59
Figure 4.3  Speciation of IA、IIA dissolved salts in the feed solution at different pH obtained by (a) Na, Cs ; (b) Mg, Ca    63
Figure 4.4  Rejection for IA,IIA species at different pH(a)Na(b)Mg(c)Ca(d)Cs    64
Figure 4.5  Rejection for transition metals at different pH (a) Mn ; (b) Co ; (c) Cu ; (d) Zn    65
Figure 4.6  Saturation index of the transition metal species (a) Mn ; (b) Co ; (c) Cu ; (d) Zn    66
Figure 4.7  Speciation of transition metals in the feed solution at different pH. (a) Mn (b) Co (c) Cu (d) Zn    68
Figure 4.8  Rejection for trivalent metals and Ag at different pH (a) Cr (b) Fe (c) Sb (d) Ag    69
Figure 4.9  Saturation index of (a)Cr(b)Fe(c)Sb(d)Ag species at different pH    70
Figure 4.10  Speciation of (a) Cr (b) Fe (c) Sb (d) Ag in the feed solution at different pH    71
Figure 4.11  Effects of the concentration and pH on the rejection rates (a)Cs(b)Co    73
Figure 4.12  Change of normalized flux as a function of operation time and fouling mode optimized curves at (a) pH 4 (b) pH 9    76
Figure 4.13  Flux vs. time: fouling model optimization assuming more than one phase at pH 4    78
Figure 4.14  The distribution of alkali metals and alkaline earth metal on the fouled membranes (a) Na (b) Cs (c) Mg on AD; (d) Na (e) Cs (f) Mg on NF270    79
Figure 4.15  Saturation index of alkali metal and alkaline earth metal species    81
Figure 4.16  The distribution of transition metals on the fouled membranes (a) Mn (b) Co (c) Cu (d) Zn on AD; (e) Mn (f) Co (g) Cu (h) Zn on NF270    82
Figure 4.17  The distribution of transition metals on the fouling membranes (a) Cr (b)Fe (c)Sb (d)Ag on AD; (e)Cr (f)Fe (g)Sb (h)Ag on NF270    84
Figure 4.18  Cumulative normalized signal intensity of each element in the depth of the fouled AD membranes (a) fouled at pH 4 (b) fouled at pH 9    92
Figure 4.19  The distribution of foulants in vertical direction (a) fouled at pH 4 (b) fouled at pH 9    94
Figure 4.20  Ultrasonic images of membrane surface (a) AD-virgin (b) NF270 -virgin (c) AD-fouled (d) NF270-fouled    95
Figure 4.21  The morphology of membranes detected by ultrasound imaging system (a) AD-virgin (b) AD-fouled    97
Figure 4.22  The morphology of membranes detected by ultrasound imaging system (a) NF270-virgin (b) NF270-fouled    98
Figure 4.23  SEM image for NF270 fouled membrane in Ref. [75]    99
Figure 4.24  Ultrasonic imaging of PES membrane morphology (a)cross section (b)layers upon the nonwoven support (c)thin film layer(Ref.[68])    99

                                

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