减压膜蒸馏过程中的钙镁污染研究
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摘要
膜蒸馏是一种新型的膜分离技术。由于其低温低压操作、脱盐率高、适用范围广等优点,在脱盐领域具有广泛的应用前景,因而广受关注。在目前制约其应用的多种因素中膜污染现象是研究的重点之一。
本论文以膜蒸馏过程中的钙镁污染为重点研究对象,系统考察了减压膜蒸馏过程中的温度极化和浓度极化现象及其对膜污染的影响。研究发现,减压膜蒸馏过程中的极化现象受到流量、温度、真空度等因素的影响。流量是影响极化现象的主要因素,适当的提高流量可以在很大程度上减弱减压膜蒸馏(VMD)过程中的极化现象;另一个重要的影响因素是通量,一般来说通量越大极化现象越严重,所以温度、真空度等操作参数均会对极化现象产生影响。
论文重点对膜蒸馏过程中容易形成膜污染的钙、镁离子的污染机理分别进行了探讨,实验结果表明:碳酸钙和硫酸钙的污染主要是在料液中形成的难溶物在膜丝表面附着,形成堵塞污染;硫酸钙晶体在膜表面的吸附力较差,其污染过程有一定的不稳定性,而多方面的实验表明硫酸钙易对膜产生较为严重的污染;碳酸镁的污染则主要是在膜丝微孔处及其周围形成较小的晶须状结晶,造成膜污染。实验还考察了海水中NaCl的存在对钙镁离子结垢倾向的影响。结果显示,NaCl的存在能够增加钙镁难溶物的溶解度,从而减弱钙镁难溶物对膜蒸馏过程的污染。
最后,实验研究了被污染膜的清洗和恢复。结果显示,对于钙镁碳酸盐造成的膜污染,使用传统的反冲洗和稀盐酸酸洗可以使被污染膜得到很好的恢复;对于硫酸钙引起的膜污染,反冲洗和稀盐酸酸洗效果不明显,采用柠檬酸清洗效果更好。
综上所述,实验对减压膜蒸馏(VMD)过程中普遍存在的钙镁污染的机理进行了研究,并建立模型,为减压膜蒸馏(VMD)过程中膜污染的系统研究奠定了基础。
Membrane distillation is a novel membrane separation technology for desalination. With the advantages of low operating pressure, high salt rejection and widely application, membrane distillation is a promising technology in desalination, drawing great attentions by many researchers. Of all the factors of restricting its application, membrane fouling is one of the key factors.
In this thesis, the key object is calcium and magnesium fouling in the process of membrane distillation. The experiment research force on the temperature polarization and concentration polarization and their effects on membrane fouling systematically. Founding that the polarization in vacuum membrane distillation process was influenced by feed flow rate, feed temperature and the vacuum. The feed flow rate is the main factor which affected the polarization. Increasing the feed flow rate could weaken the polarization phenomenon significantly in vacuum membrane distillation (VMD) process. Another important influencing factor is the pure water flux. Generally speaking, the bigger the flux is, the more serious the polarization is. Therefore, the operating parameters such as temperature and vacuum would influence the polarization too.
The fouling mechanism of calcium and magnesium ions which were easy to contaminate the film had been discussed respectively in this thesis. The results showed that the contamination caused by calcium carbonate and calcium sulfate was mainly formed by the attachment of the insoluble substance on the fibers. The adsorptivity of calcium sulfate crystals on the membrane was poor and its contamination was unstable. Many experiment results showed that calcium sulfate produced serious contamination to the membrane. The contamination of magnesium carbonate was caused by the formation of small whisker-like crystals around the membrane pores. The effect of NaCl on the scaling of calcium and magnesium ions had been investigated. The results showed that NaCl would increase the solubility of the calcium and magnesium ions and it would weaken their contamination to the membrane distillation process.
Finally, the washing and recovery of membrane had been studied. The results showed that for membrane fouling caused by calcium and magnesium carbonate, the membrane can be well resumed by the use of traditional anti-flush and dilute hydrochloric acid. For membrane fouling caused by calcium sulfate, the effect of anti-flush and dilute hydrochloric acid wash washing not obvious. Citric acid washing will be better.
In summary, the mechanism of calcium and magnesium fouling in the process of vacuum membrane distillation had been investigated and the model had been established. These work laid elementary foundation for the systematic research on the membrane fouling in the VMD desalination process.
本论文以膜蒸馏过程中的钙镁污染为重点研究对象,系统考察了减压膜蒸馏过程中的温度极化和浓度极化现象及其对膜污染的影响。研究发现,减压膜蒸馏过程中的极化现象受到流量、温度、真空度等因素的影响。流量是影响极化现象的主要因素,适当的提高流量可以在很大程度上减弱减压膜蒸馏(VMD)过程中的极化现象;另一个重要的影响因素是通量,一般来说通量越大极化现象越严重,所以温度、真空度等操作参数均会对极化现象产生影响。
论文重点对膜蒸馏过程中容易形成膜污染的钙、镁离子的污染机理分别进行了探讨,实验结果表明:碳酸钙和硫酸钙的污染主要是在料液中形成的难溶物在膜丝表面附着,形成堵塞污染;硫酸钙晶体在膜表面的吸附力较差,其污染过程有一定的不稳定性,而多方面的实验表明硫酸钙易对膜产生较为严重的污染;碳酸镁的污染则主要是在膜丝微孔处及其周围形成较小的晶须状结晶,造成膜污染。实验还考察了海水中NaCl的存在对钙镁离子结垢倾向的影响。结果显示,NaCl的存在能够增加钙镁难溶物的溶解度,从而减弱钙镁难溶物对膜蒸馏过程的污染。
最后,实验研究了被污染膜的清洗和恢复。结果显示,对于钙镁碳酸盐造成的膜污染,使用传统的反冲洗和稀盐酸酸洗可以使被污染膜得到很好的恢复;对于硫酸钙引起的膜污染,反冲洗和稀盐酸酸洗效果不明显,采用柠檬酸清洗效果更好。
综上所述,实验对减压膜蒸馏(VMD)过程中普遍存在的钙镁污染的机理进行了研究,并建立模型,为减压膜蒸馏(VMD)过程中膜污染的系统研究奠定了基础。
Membrane distillation is a novel membrane separation technology for desalination. With the advantages of low operating pressure, high salt rejection and widely application, membrane distillation is a promising technology in desalination, drawing great attentions by many researchers. Of all the factors of restricting its application, membrane fouling is one of the key factors.
In this thesis, the key object is calcium and magnesium fouling in the process of membrane distillation. The experiment research force on the temperature polarization and concentration polarization and their effects on membrane fouling systematically. Founding that the polarization in vacuum membrane distillation process was influenced by feed flow rate, feed temperature and the vacuum. The feed flow rate is the main factor which affected the polarization. Increasing the feed flow rate could weaken the polarization phenomenon significantly in vacuum membrane distillation (VMD) process. Another important influencing factor is the pure water flux. Generally speaking, the bigger the flux is, the more serious the polarization is. Therefore, the operating parameters such as temperature and vacuum would influence the polarization too.
The fouling mechanism of calcium and magnesium ions which were easy to contaminate the film had been discussed respectively in this thesis. The results showed that the contamination caused by calcium carbonate and calcium sulfate was mainly formed by the attachment of the insoluble substance on the fibers. The adsorptivity of calcium sulfate crystals on the membrane was poor and its contamination was unstable. Many experiment results showed that calcium sulfate produced serious contamination to the membrane. The contamination of magnesium carbonate was caused by the formation of small whisker-like crystals around the membrane pores. The effect of NaCl on the scaling of calcium and magnesium ions had been investigated. The results showed that NaCl would increase the solubility of the calcium and magnesium ions and it would weaken their contamination to the membrane distillation process.
Finally, the washing and recovery of membrane had been studied. The results showed that for membrane fouling caused by calcium and magnesium carbonate, the membrane can be well resumed by the use of traditional anti-flush and dilute hydrochloric acid. For membrane fouling caused by calcium sulfate, the effect of anti-flush and dilute hydrochloric acid wash washing not obvious. Citric acid washing will be better.
In summary, the mechanism of calcium and magnesium fouling in the process of vacuum membrane distillation had been investigated and the model had been established. These work laid elementary foundation for the systematic research on the membrane fouling in the VMD desalination process.
引文
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[4] Mulder M. Basic Principles of Membrane Technology [M]. Netherlands: Kluwer Academic publish 1996: 1
[5]王学松,膜分离技术及其应用,北京,科学出版社,1994
[6]许振良,膜法水处理技术,北京,化学工业出版社,2001
[7]缪晖,膜分离技术的发展及应用,天然气与石油,2004,22(3):46~47.
[8]高从墙,俞三传,张建飞等,纳滤膜科学与技术[J],1999,19(2):1~5
[9]许振良,污水处理膜分离技术的研究进展[J],净水技术,2000,19(1):3~7
[10] Victory Guy. Treatment of effluent from the process for electrodeposition of paint[P] , GB1 (07) , 458, 1967
[11]冯书博,膜分离技术的发展及在工业中应用,广西轻工业,2008,6,30~31.
[12] Lawson K W, Lloyd D R. Membrane distillation, Journal of Membrane Science, 1997, 124: 1~25
[13]吴庸烈,膜蒸馏技术及其应用进展,膜科学与技术,2003,23(4):67~92
[14]马润宇,膜蒸馏技术的回顾与展望,第四届全国膜和膜过程学术报告会论文集,增补[C].南京:南京工业大学,2002,33~39
[15] Ding Zhongwei, Liu Liying, Mohamed S E1-Bourawi. Analysis of a solar-powered membrane distillation system [J]. Desalination, 2005, 172(1): 27~40
[16] Khayet M, Velázquez A, Mengual J I. Direct contact membrane distillation of humic acid solutions [J]. J Membr Sci, 2004, 240(1/2): 123~128
[17] Mohamed Khayet,Paz Godino,Juan I Mengual. Nature of flow on sweeping gas membrane distillation[J]. J Membr Sci, 2000, 170 (2): 243~255.
[18]高振,徐世昌,马友光等,真空膜蒸馏技术应用研究现状及进展,海湖盐与化工,2003,32(6):21~29
[19]孔瑛,吴庸烈,杨金荣等,膜蒸馏用聚偏氟乙烯微孔膜的结构控制Ⅲ——制膜条件的选择和膜蒸馏性能[J],水处理技术,992,18(3):167~172
[20]吴庸烈,孔瑛,林晓等,亲水膜的表面改性及膜蒸馏中的应用[J],功能高分子学报,1991,4(3),199~206
[21] Martinez D L, Florido D F J. Study of evaporation efficiency in membrane distillation[J],Desalination, 1999, 126(1~3): 193~197
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