Investigation of Al-hydroxide Precipitate Fouling on the Nanofiltration Membrane System with Coagulation Pretreatment: Effect of Inorganic Compound, Organic Compound, and Their Combination

Choi, Yang-Hun;Kweon, Ji-Hyang

  • Received : 2011.03.30
  • Accepted : 2011.07.25
  • Published : 2011.09.30


Nanofiltration (NF) experiments were conducted to investigate fouling of Al-hydroxide precipitate and the influence of organic compound, inorganic compound, and their combination, i.e., multiple foulants. $CaCl_2$ and $MgSO_4$ were employed as surrogates of inorganic compounds while humic acid was used as surrogate of organic compound. The flux attained from NF experiments was fitted with the mathematical fouling model to evaluate the potential fouling mechanisms. Al-hydroxide fouling with a cake formation mechanism had little effect on the NF membrane fouling regardless of the Al concentration. The NF fouling by Al-hydroxide precipitate was deteriorated in presence of inorganic matter. The effect of Mg was more critical in increasing the fouling than Ca. This is because the Mg ions enhanced the resistances of the cake layer accumulated by the Al-hydroxide precipitate on the membrane surfaces. However, the fouling with Mg was dramatically mitigated by adding humic acid. It is interesting to observe that the removal of the conductivity was enhanced to 61.2% in presence of Mg and humic acid from 30.9% with Al-hydroxide alone. The influence of dissolved matter (i.e., colloids) was more negative than particulate matter on the NF fouling for Al-hydroxide precipitate in presence of inorganic and organic matter.


Al-hydroxide precipitate;Coagulation;Fouling;Nanofiltration


  1. Lee S, Lee CH. Effect of operating conditions on $CaSO_4$ scale formation mechanism in nanofiltration for water softening. Water Res. 2000;34:3854-3866.
  2. Tay JH, Liu J, Delai Sun D. Effect of solution physico-chemistry on the charge property of nanofiltration membranes. Water Res. 2002;36:585-598.
  3. Kilduff JE, Mattaraj S, Belfort G. Flux decline during nanofiltration of naturally-occurring dissolved organic matter: effects of osmotic pressure, membrane permeability, and cake formation. J. Membr. Sci. 2004;239:39-53.
  4. Koyuncu I, Topacik D, Wiesner MR. Factors influencing flux decline during nanofiltration of solutions containing dyes and salts. Water Res. 2004;38:432-440.
  5. Bodzek M, Koter S, Wesolowska K. Application of membrane techniques in a water softening process. Desalination 2002;145:321-327.
  6. Lin CJ, Shirazi S, Rao P, Agarwal S. Effects of operational parameters on cake formation of $CaSO_4$ in nanofiltration. Water Res. 2006;40:806-816.
  7. Nanda D, Tung KL, Hsiung CC, et al. Effect of solution chemistry on water softening using charged nanofiltration membranes. Desalination 2008;234:344-353.
  8. Hilal N, Al-Zoubi H, Darwish NA, Mohammad AW, Abu Arabi M. A comprehensive review of nanofiltration membranes: treatment, pretreatment, modelling, and atomic force microscopy. Desalination 2004;170:281-308.
  9. Wittmann E, Thorsen T. Water treatment. In: Schaefer AI, Fane AG, Waite TD, eds. Nanofiltration: principles and applications. Oxford: Elsevier Advanced Technology; 2007. Ch. 10. p. 273-284.
  10. Vickers JC, Thompson MA, Kelkar UG. The use of membrane filtration in conjunction with coagulation processes for improved NOM removal. Desalination 1995;102:57-61.
  11. Carroll T, King S, Gray SR, Bolto BA, Booker NA. The fouling of microfiltration membranes by NOM after coagulation treatment. Water Res. 2000;34:2861-2868.
  12. Berube PR, Mavinic DS, Hall ER, Kenway SE, Roett K. Evaluation of adsorption and coagulation as membrane pretreatment steps for the removal of organic material and disinfection-by-product precursors. J. Environ. Eng. Sci. 2002;1:465-476.
  13. Pikkarainen AT, Judd SJ, Jokela J, Gillberg L. Pre-coagulation for microfiltration of an upland surface water. Water Res. 2004;38:455-465.
  14. Kim HC, Hong JH, Lee S. Fouling of microfiltration membranes by natural organic matter after coagulation treatment: a comparison of different initial mixing conditions. J. Membr. Sci. 2006;283:266-272.
  15. Waite TD. Chemical speciation effect in nanofiltration separation. In: Schaefer AI, Fane AG, Waite TD, eds. Nanofiltration: principles and applications. Oxford: Elsevier Advanced Technology; 2007. Ch. 7. p. 166-167.
  16. Park PK, Lee CH, Choi SJ, Choo KH, Kim SH, Yoon CH. Effect of the removal of DOMs on the performance of a coagulation-UF membrane system for drinking water production. Desalination 2002;145:237-245.
  17. Oh JI, Lee S. Influence of streaming potential on flux decline of microfiltration with in-line rapid pre-coagulation process for drinking water production. J. Membr. Sci. 2005;254:39-47.
  18. Cho MH, Lee CH, Lee S. Effect of flocculation conditions on membrane permeability in coagulation-microfiltration. Desalination 2006;191:386-396.
  19. Jefferson B, Jarvis P, Sharp E, Wilson S, Parsons SA. Flocs through the looking glass. Water Sci. Technol. 2004;50:47-54.
  20. Lee JD, Lee SH, Jo MH, Park PK, Lee CH, Kwak JW. Effect of coagulation conditions on membrane filtration characteristics in coagulation--microfiltration process for water treatment. Environ. Sci. Technol. 2000;34:3780-3788.
  21. Listiarini K, Sun DD, Leckie JO. Organic fouling of nanofiltration membranes: evaluating the effects of humic acid, calcium, alum coagulant and their combinations on the specific cake resistance. J. Membr. Sci. 2009;332:56-62.
  22. Kim HA, Choi JH, Takizawa S. Comparison of initial filtration resistance by pretreatment processes in the nanofiltration for drinking water treatment. Sep. Purif. Technol. 2007;56:354-362.
  23. Park N, Lee S, Yoon SR, Kim YH, Cho J. Foulants analyses for NF membranes with different feed waters: coagulation/sedimentation and sand filtration treated waters. Desalination 2007;202:231-238.
  24. Ohno K, Matsui Y, Itoh M, et al. NF membrane fouling by aluminum and iron coagulant residuals after coagulation-MF pretreatment. Desalination 2010;254:17-22.
  25. Pernitsky DJ, Edzwald JK. Solubility of polyaluminium coagulants. J. Water Supply Res. Technol. Aqua 2003;52:395-406.
  26. Schaep J, Vandecasteele C. Evaluating the charge of nanofiltration membranes. J. Membr. Sci. 2001;188:129-136.
  27. Her N, Amy G, Jarusutthirak C. Seasonal variations of nanofiltration (NF) foulants: identification and control. Desalination 2000;132:143-160.
  28. Tanninen J, Manttari M, Nystrom M. Effect of salt mixture concentration on fractionation with NF membranes. J. Membr. Sci. 2006;283:57-64.
  29. Bargeman G, Vollenbroek JM, Straatsma J, Schroen CGPH, Boom RM. Nanofiltration of multi-component feeds. Interactions between neutral and charged components and their effect on retention. J. Membr. Sci. 2005;247:11-20.
  30. Balannec B, Vourch M, Rabiller-Baudry M, Chaufer B. Comparative study of different nanofiltration and reverse osmosis membranes for dairy effluent treatment by dead-end filtration. Sep. Purif. Technol. 2005;42:195-200.
  31. Field RW, Wu D, Howell JA, Gupta BB. Critical flux concept for microfiltration fouling. J. Membr. Sci. 1995;100:259-272.
  32. Jarusutthirak C, Mattaraj S, Jiraratananon R. Influence of inorganic scalants and natural organic matter on nanofiltration membrane fouling. J. Membr. Sci. 2007;287:138-145.
  33. Zelazny LW, Jardine PM. Surface reactions of aqueous aluminum species. In: Sposito G, ed. The environmental chemistry of aluminum. Boca Raton, FL: CRC Press; 1989. p. 149-155.
  34. Manttari M, Pihlajamaki A, Nystrom M. Effect of pH on hydrophilicity and charge and their effect on the filtration efficiency of NF membranes at different pH. J. Membr. Sci. 2006;280:311-320.
  35. Bouranene S, Fievet P, Szymczyk A, El-Hadi Samar M, Vidonne A. Influence of operating conditions on the rejection of cobalt and lead ions in aqueous solutions by a nanofiltration polyamide membrane. J. Membr. Sci. 2008;325:150-157.
  36. Gabelich CJ, Ishida KP, Gerringer FW, Evangelista R, Kalyan M, Suffet IHM. Control of residual aluminum from conventional treatment to improve reverse osmosis performance. Desalination 2006;190:147-160.
  37. Schrader GA, Zwijnenburg A, Wessling M. The effect of WWTP effluent zeta-potential on direct nanofiltration performance. J. Membr. Sci. 2005;266:80-93.
  38. Choi YH, Kim HS, Kweon JH. Role of hydrophobic natural organic matter flocs on the fouling in coagulation-membrane processes. Sep. Purif. Technol. 2008;62:529-534.
  39. Li Q, Elimelech M. Organic fouling and chemical cleaning of nanofiltration membranes: measurements and mechanisms. Environ. Sci. Technol. 2004;38:4683-4693.
  40. Li Q, Elimelech M. Synergistic effects in combined fouling of a loose nanofiltration membrane by colloidal materials and natural organic matter. J. Membr. Sci. 2006;278:72-82.
  41. Bertsh PM. Aqueous polynuclear aluminum species. In: Sposito G, ed. The environmental chemistry of aluminum. Boca Raton, FL: CRC Press; 1989. p. 107-109.


Supported by : National Research Foundation of Korea (NRF)