超滤污水深度处理特性及膜污染机理研究
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摘要
本研究采用截留分子量分别为100,000Da和20,000Da的国产中空纤维超滤膜对西安市北石桥污水净化中心的二沉池出水进行了深度处理实验。实验采用超滤自动控制系统实现了对操作条件的自动控制和实验数据的自动采集，提高了实验精度。实验分析了超滤对污水的处理效果及消毒效果。并比较了同种膜材质，不同截留分子量的超滤膜对污水中几种重要指标的去除效果，以及在运行过程中膜通量的变化情况。实验还通过周期反冲洗以及无反冲洗时不同压力下、不同回收率下的膜阻力变化情况分析了运行条件对膜污染的影响。
从滤后水质看出超滤膜对浊度、细菌总数及大肠杆菌的去除效果良好。原水浊度在1.82～3.56NTU范围内，出水浊度均小于0.5NTU。细菌总数和大肠杆菌的去除率均大于99％。超滤膜对污水中有机物有一定的去除，但去除率不高。不同截留分子量的膜对COD_(Cr)、TOC、UV_(254,)、色度的去除率稍有差异，20,000Da膜的去除率略高于100,000Da膜。截留分子量对超滤过程中膜通量的变化有很大影响，膜过滤初期20,000Da膜通量衰减严重。膜长期运行时，100,000Da膜通量衰减幅度较大。
直接超滤实验结果表明，反冲洗能够在一定程度上缓解膜污染。适当的回收率和进膜压力都可以有效减小膜污染。通过对膜污染数学模型的分析，明确了在过滤初期，膜孔窄化是造成渗透通量下降的主要机理；而过滤后期，滤饼层的形成是造成渗透通量下降的主要机理，因此运用阶段模型可更好的模拟膜污染过程。
Hollow fiber UF membrane with 1 105 and 2 104Da were used to treat the secondary effluent from Xi'an Bei Shi Qiao Sewage Purification center. The study investigated the characteristics of UF for the removal of turbidity, organic substances and bacteria. When MWCO of UF membrane is different, the removal efficiency of UF membrane for waste is different and the permeate flux decline with operation time is also different. At the same time the study investigated the effect of backwashing, feed-water recovery and pressure on membrane resistance.
In order to realize automatic control of the UF system and date acquisition and improve the accuracy of experiment result, the UF automatic system was used to meet the need of continuous experiment.
The results show that UF can almost remove the turbidity completely. The permeate turbidity is lower than 0.5NTU when raw water turbidity isl.82~3.56 NTU. UF also performs physical disinfection well. It can achieve 99% removal efficiency of bacteria and E.coli. UF can remove organic substances in wastewater, but the removal efficiency is not high. Compared with UF membrane with 1 105Da, UF membrane with 2 104Da can remove organic substances in wastewater more effectively, but the difference is not obvious. In the initial period of a filtration circle, the permeate flux decline of UF membrane with 2x 104Da is larger, but the permeate flux decline is smaller afterwards.
The results show that membrane fouling can be prevented more or less by backwashing. Lower feed-water recovery and higher pressure can keep higher flux. By the analysis of membrane fouling mathematic model, a conclusion can be drown that in the initial period of a filtration circle , permeate flux decline is resulted mainly by membrane pore blocking ;while in the final period, mainly by cake formation. Based on this, a two-stage mathematic model for the description mechanism of membrane fouling was proposed.
从滤后水质看出超滤膜对浊度、细菌总数及大肠杆菌的去除效果良好。原水浊度在1.82～3.56NTU范围内，出水浊度均小于0.5NTU。细菌总数和大肠杆菌的去除率均大于99％。超滤膜对污水中有机物有一定的去除，但去除率不高。不同截留分子量的膜对COD_(Cr)、TOC、UV_(254,)、色度的去除率稍有差异，20,000Da膜的去除率略高于100,000Da膜。截留分子量对超滤过程中膜通量的变化有很大影响，膜过滤初期20,000Da膜通量衰减严重。膜长期运行时，100,000Da膜通量衰减幅度较大。
直接超滤实验结果表明，反冲洗能够在一定程度上缓解膜污染。适当的回收率和进膜压力都可以有效减小膜污染。通过对膜污染数学模型的分析，明确了在过滤初期，膜孔窄化是造成渗透通量下降的主要机理；而过滤后期，滤饼层的形成是造成渗透通量下降的主要机理，因此运用阶段模型可更好的模拟膜污染过程。
Hollow fiber UF membrane with 1 105 and 2 104Da were used to treat the secondary effluent from Xi'an Bei Shi Qiao Sewage Purification center. The study investigated the characteristics of UF for the removal of turbidity, organic substances and bacteria. When MWCO of UF membrane is different, the removal efficiency of UF membrane for waste is different and the permeate flux decline with operation time is also different. At the same time the study investigated the effect of backwashing, feed-water recovery and pressure on membrane resistance.
In order to realize automatic control of the UF system and date acquisition and improve the accuracy of experiment result, the UF automatic system was used to meet the need of continuous experiment.
The results show that UF can almost remove the turbidity completely. The permeate turbidity is lower than 0.5NTU when raw water turbidity isl.82~3.56 NTU. UF also performs physical disinfection well. It can achieve 99% removal efficiency of bacteria and E.coli. UF can remove organic substances in wastewater, but the removal efficiency is not high. Compared with UF membrane with 1 105Da, UF membrane with 2 104Da can remove organic substances in wastewater more effectively, but the difference is not obvious. In the initial period of a filtration circle, the permeate flux decline of UF membrane with 2x 104Da is larger, but the permeate flux decline is smaller afterwards.
The results show that membrane fouling can be prevented more or less by backwashing. Lower feed-water recovery and higher pressure can keep higher flux. By the analysis of membrane fouling mathematic model, a conclusion can be drown that in the initial period of a filtration circle , permeate flux decline is resulted mainly by membrane pore blocking ;while in the final period, mainly by cake formation. Based on this, a two-stage mathematic model for the description mechanism of membrane fouling was proposed.
引文
[1] 国家环保总局，中国环境状况公报，1999
[2] 杨鲁豫，王琳，王宝贞，我国水资源污染治理的技术策略，给水排水Vol．27．No．1，2001
[3] 刘茉娥等，膜分离技术，化学工业出版社，1998
[4] 王占生，刘文君编，微污染水源饮用水处理，中国建筑工业出版社，1999
[5] 许振良，膜法水处理技术，化学工业出版社，2000
[6] 时均，袁权等编，膜技术手册，化学工业出版社，2001
[7] J. F Hayes, et al. Studies on whey processing by Ultra filtration. Ⅱ. Improving permeation rates by preventing fouling. J. Dairy Technol.29-132, 1974, 8
[8] 董秉直，膜技术应用于净水处理的研究和现状，给水排水，Vol．25 No．1 1999
[9] R. J. Wakeman, G Akay. Membrane-solute and liquid-particle interaction effects in filtration. Filter.&Separ. 34(4):511-519, 1997
[10] M. Hlavacek, F Bouchet Constant flow rate blocking laws and an example of their application to dead-end micro filtration of protein solutions. J.Membr.Sci.82: 285-295, 1993
[11] C H Xing,E Tardieu,Y Qian,et al. Ultrafiltration membrane bioreactor for urban wastewater reclamation, Journal of membrane science, 177(2000)73-82
[12] G Green, G Belfort. Fouling of ultrafiltration membranes: lateral migration and the particle trajectory modle. Desalination, 35:129-147, 1980
[13] J G Jacangelo, UF with pretreatment for removing DBP precursors. our. AWWA.Vol.87(3): 100-112,1995.
[14] L Y Wang, L F Song, Flux decline in crossflow microfiltration and ultrafiltration: experimental verification of fouling dynamics. J. Membrane Science, 160(1999):41-50
[15] 王志等，膜过程中防治膜污染强化渗透通量技术进屐(Ⅰ)操作策略，膜科学与技术19(1)：1-5，1999
[16] 邵刚，膜法水处理技术与工程实例，化学工业出版社，2002．
[17] 李琳(译)，膜技术基本原理(第二版)，清华大学出版社，1999
[18] J. Granger, D.Leclere, J A Dodds. Filtration of dilute suspensions of latexes. Filtr& Separ.22 (1985)58-60
[19] 彭安等，水体腐植酸及其络合物，环境科学学报，Vol 1(2)：126-129，1981．
[20] 李志华，硕士论文，2002
[21] Y Lee, M Clark. Modeling of flux decline during cross-flow microfiltration of colloidal
suspensions. J. Membrane Science, 149:181-202, 1998.
[22] Committee Report: Membrane processes. AWWA Membrane Technology Research Committee
[23] 王锦，超滤水处理特性和膜污染研究，博士论文，2001．
[24] 王晓琳，膜的污染和劣化及其防治对策，工业水处理，21(9)，1-5 2001
[25] 刘茉娥，超滤膜污染机理的研究及控制，水处理技术，15(3)：163
[26] G F Crozes, Impact of u ltrafiltration o perating conditions o n m embrane i rreversible f ouling. Journal of Membrane Science 1241(1997) 63-76
[27] P.Ramesh Babu, Membrane characteristics as determinant in fouling of UF membrane, Separation and Purification Technology 24(2001)23-34
[28] 何义亮等，膜生物反应器生物降解与膜分离共作用特性研究，环境污染与防治，1998；20(6)：56-60．
[29] R.Bian,K, Yamamoto, The effect of shear rate on controlling the concentration polarization and membrane fouling. Desalination 131(2000)225-236
[30] 邵刚，膜法水处理技术(第二版)，冶金工业出版社，2000
[31] 刘忠洲，续曙光，微滤、超滤过程中的膜污染与清洗，水处理技术 23(4) 1997．8
[32] 罗敏，纳滤膜污染的分析与机理研究，水处理技术24 (6) 1998．12
[33] 张国俊，刘忠州，膜过程中超滤膜污染机制的研究及其防治技术进展，膜科学与技术，Vol．21 No．4，2001
[34] I G Wenten, Mechanisms and control fouling in cross-flow microfiltation. Filt. Sep.3 (1995)252-253
[35] 刘忠洲，膜的污染及其防治对策，工业水处理，Vol．21 No．9，2001
[36] Sheikho leslami R. Fouling mitigation in membrane process. Desalination,1999,123(1):45～53
[37] 王锦，王晓昌，膜的污染及其控制，给水排水，Vol．26 No．9，2000．
[38] S V Graham et al, Improving reverse osmosis performance through periodic cleaning, Desalination 1989,74(1-3):13-124
[39] J. Lindau, Adsorptive fouling of modified and unmodified commercial polymeric ultrafiltration membranes. Journal of Membrane Science 160(1999)65-76
[40] 张颖，顾平，膜技术应用于饮用水处理的进展，中国给水排水，Vol．17 No．5 2001
[41] 王宝贞，膜生物反应器中膜的堵塞与清洗的机理研究，给水排水，Vol．26 No．9 2000
[42] APHA,AWWA,WPCF编，水和废水标准检验法，第15版，中国建筑工业出版社1985
[43] T.Stephenson, K Briendle. Membrane Bioreactors-Dual Processing in One Unit Operation. World Marketing Series, Business Briefing,1999. 164—169
[44] Zenon, Municipal Intemational. Advanced Membrane Systems for Municipal Wastewater
Treatment. ISO9002-87, Cept. #002946,CANADA,1996
[45] J L Bersillon, C Anselme, J Mallevialle, et al. Ultrafiltration applied to drinking water treatment: case of a small system. Water Nagoya-ASPAC, Nagoya, 1989, 209-219
[46] J M Laine, J P Hagstrom, M Clark, et al. Effects of ultrafiltration membrane composition. Jour. AWWA. 81(11):61-67, 1989
[47] AWWARF, Lyonnaise des Eaux, water Research commission of South Africa, Water Treatment Memhrane Processes, Me Graw Hill, New York, 1996
[48] 何义亮等，厌氧超滤膜反应器截留分子量研究，中国给水排水，Vol．15 No．9 1999．
[49] 顾平等，应用膜生物反应其处理生活污水的研究，中国给水排水，14(5)：1998
[50] N Mugnier, J A howell, M Ruf. Optimisation of a back-flush sequence for zeolite microfiltration. J. Member. Sci. 175(2000):149-161
[51] 董秉直，曹达文，范谨初等，UF过滤天然原水阻力特性的研究，水处理技术，Vol．27No．2，2001
[52] 王磊，运行条件对超滤膜污染的影响，中国给水排水 vol．17，No．10，2001
[53] Huimin Ma, Christopher N, Membrane fouling reduction by back-pulsing and surface modification, Journal of Membrane Science 173(2000)191-200
[54] K.Khatib, Physic-Chemical study of fouling mechanisms of ultrafiltration membrane on Biwa Lake (Japan), Journal of Membrane Science 130(1997)53-62
[55] Raja Ghosh, Study of membrane fouling by BSA using pulsed injection technique, Journal of Membranes Science 195(2002)115-123
[56] Ilias shamsuddin, Govind Rekesh, Simulation of flux decline due to percolate fouling in ultra filtratrtion [J]. Part SCI Technol, 1989, 7(3); 187-199
[57] Yiantsios S.G, Karabelas A J. The effect of colloid stability on membrane fouling [J].Desalination, 1998 118(1-3)143-152
[58] H C Flemming et al, Biofouling on membranes-a microbiological approach Desalination, 70(1988),95-119.
[59] Meireles matine, Aimar perre. Effects of protein fouling on the apparent pore size distribution of sieving membranes. J Membrane Sci, 1991 56(1):13～28
[60] 张原，超滤膜污染的机理和控制，净水技术，Vol．20 No．4 2001 11～15
[61] N Tambo, K Kamei, Treat ability evaluation of general organic matter-matrix conception and its application for a regional water and waste water system. Water Research. 12:931-950, 1978
[2] 杨鲁豫，王琳，王宝贞，我国水资源污染治理的技术策略，给水排水Vol．27．No．1，2001
[3] 刘茉娥等，膜分离技术，化学工业出版社，1998
[4] 王占生，刘文君编，微污染水源饮用水处理，中国建筑工业出版社，1999
[5] 许振良，膜法水处理技术，化学工业出版社，2000
[6] 时均，袁权等编，膜技术手册，化学工业出版社，2001
[7] J. F Hayes, et al. Studies on whey processing by Ultra filtration. Ⅱ. Improving permeation rates by preventing fouling. J. Dairy Technol.29-132, 1974, 8
[8] 董秉直，膜技术应用于净水处理的研究和现状，给水排水，Vol．25 No．1 1999
[9] R. J. Wakeman, G Akay. Membrane-solute and liquid-particle interaction effects in filtration. Filter.&Separ. 34(4):511-519, 1997
[10] M. Hlavacek, F Bouchet Constant flow rate blocking laws and an example of their application to dead-end micro filtration of protein solutions. J.Membr.Sci.82: 285-295, 1993
[11] C H Xing,E Tardieu,Y Qian,et al. Ultrafiltration membrane bioreactor for urban wastewater reclamation, Journal of membrane science, 177(2000)73-82
[12] G Green, G Belfort. Fouling of ultrafiltration membranes: lateral migration and the particle trajectory modle. Desalination, 35:129-147, 1980
[13] J G Jacangelo, UF with pretreatment for removing DBP precursors. our. AWWA.Vol.87(3): 100-112,1995.
[14] L Y Wang, L F Song, Flux decline in crossflow microfiltration and ultrafiltration: experimental verification of fouling dynamics. J. Membrane Science, 160(1999):41-50
[15] 王志等，膜过程中防治膜污染强化渗透通量技术进屐(Ⅰ)操作策略，膜科学与技术19(1)：1-5，1999
[16] 邵刚，膜法水处理技术与工程实例，化学工业出版社，2002．
[17] 李琳(译)，膜技术基本原理(第二版)，清华大学出版社，1999
[18] J. Granger, D.Leclere, J A Dodds. Filtration of dilute suspensions of latexes. Filtr& Separ.22 (1985)58-60
[19] 彭安等，水体腐植酸及其络合物，环境科学学报，Vol 1(2)：126-129，1981．
[20] 李志华，硕士论文，2002
[21] Y Lee, M Clark. Modeling of flux decline during cross-flow microfiltration of colloidal
suspensions. J. Membrane Science, 149:181-202, 1998.
[22] Committee Report: Membrane processes. AWWA Membrane Technology Research Committee
[23] 王锦，超滤水处理特性和膜污染研究，博士论文，2001．
[24] 王晓琳，膜的污染和劣化及其防治对策，工业水处理，21(9)，1-5 2001
[25] 刘茉娥，超滤膜污染机理的研究及控制，水处理技术，15(3)：163
[26] G F Crozes, Impact of u ltrafiltration o perating conditions o n m embrane i rreversible f ouling. Journal of Membrane Science 1241(1997) 63-76
[27] P.Ramesh Babu, Membrane characteristics as determinant in fouling of UF membrane, Separation and Purification Technology 24(2001)23-34
[28] 何义亮等，膜生物反应器生物降解与膜分离共作用特性研究，环境污染与防治，1998；20(6)：56-60．
[29] R.Bian,K, Yamamoto, The effect of shear rate on controlling the concentration polarization and membrane fouling. Desalination 131(2000)225-236
[30] 邵刚，膜法水处理技术(第二版)，冶金工业出版社，2000
[31] 刘忠洲，续曙光，微滤、超滤过程中的膜污染与清洗，水处理技术 23(4) 1997．8
[32] 罗敏，纳滤膜污染的分析与机理研究，水处理技术24 (6) 1998．12
[33] 张国俊，刘忠州，膜过程中超滤膜污染机制的研究及其防治技术进展，膜科学与技术，Vol．21 No．4，2001
[34] I G Wenten, Mechanisms and control fouling in cross-flow microfiltation. Filt. Sep.3 (1995)252-253
[35] 刘忠洲，膜的污染及其防治对策，工业水处理，Vol．21 No．9，2001
[36] Sheikho leslami R. Fouling mitigation in membrane process. Desalination,1999,123(1):45～53
[37] 王锦，王晓昌，膜的污染及其控制，给水排水，Vol．26 No．9，2000．
[38] S V Graham et al, Improving reverse osmosis performance through periodic cleaning, Desalination 1989,74(1-3):13-124
[39] J. Lindau, Adsorptive fouling of modified and unmodified commercial polymeric ultrafiltration membranes. Journal of Membrane Science 160(1999)65-76
[40] 张颖，顾平，膜技术应用于饮用水处理的进展，中国给水排水，Vol．17 No．5 2001
[41] 王宝贞，膜生物反应器中膜的堵塞与清洗的机理研究，给水排水，Vol．26 No．9 2000
[42] APHA,AWWA,WPCF编，水和废水标准检验法，第15版，中国建筑工业出版社1985
[43] T.Stephenson, K Briendle. Membrane Bioreactors-Dual Processing in One Unit Operation. World Marketing Series, Business Briefing,1999. 164—169
[44] Zenon, Municipal Intemational. Advanced Membrane Systems for Municipal Wastewater
Treatment. ISO9002-87, Cept. #002946,CANADA,1996
[45] J L Bersillon, C Anselme, J Mallevialle, et al. Ultrafiltration applied to drinking water treatment: case of a small system. Water Nagoya-ASPAC, Nagoya, 1989, 209-219
[46] J M Laine, J P Hagstrom, M Clark, et al. Effects of ultrafiltration membrane composition. Jour. AWWA. 81(11):61-67, 1989
[47] AWWARF, Lyonnaise des Eaux, water Research commission of South Africa, Water Treatment Memhrane Processes, Me Graw Hill, New York, 1996
[48] 何义亮等，厌氧超滤膜反应器截留分子量研究，中国给水排水，Vol．15 No．9 1999．
[49] 顾平等，应用膜生物反应其处理生活污水的研究，中国给水排水，14(5)：1998
[50] N Mugnier, J A howell, M Ruf. Optimisation of a back-flush sequence for zeolite microfiltration. J. Member. Sci. 175(2000):149-161
[51] 董秉直，曹达文，范谨初等，UF过滤天然原水阻力特性的研究，水处理技术，Vol．27No．2，2001
[52] 王磊，运行条件对超滤膜污染的影响，中国给水排水 vol．17，No．10，2001
[53] Huimin Ma, Christopher N, Membrane fouling reduction by back-pulsing and surface modification, Journal of Membrane Science 173(2000)191-200
[54] K.Khatib, Physic-Chemical study of fouling mechanisms of ultrafiltration membrane on Biwa Lake (Japan), Journal of Membrane Science 130(1997)53-62
[55] Raja Ghosh, Study of membrane fouling by BSA using pulsed injection technique, Journal of Membranes Science 195(2002)115-123
[56] Ilias shamsuddin, Govind Rekesh, Simulation of flux decline due to percolate fouling in ultra filtratrtion [J]. Part SCI Technol, 1989, 7(3); 187-199
[57] Yiantsios S.G, Karabelas A J. The effect of colloid stability on membrane fouling [J].Desalination, 1998 118(1-3)143-152
[58] H C Flemming et al, Biofouling on membranes-a microbiological approach Desalination, 70(1988),95-119.
[59] Meireles matine, Aimar perre. Effects of protein fouling on the apparent pore size distribution of sieving membranes. J Membrane Sci, 1991 56(1):13～28
[60] 张原，超滤膜污染的机理和控制，净水技术，Vol．20 No．4 2001 11～15
[61] N Tambo, K Kamei, Treat ability evaluation of general organic matter-matrix conception and its application for a regional water and waste water system. Water Research. 12:931-950, 1978
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