Ozonation as an efficient pretreatment method to alleviate reverse osmosis membrane fouling caused by complexes of humic acid and calcium ion

Highlights

Humic acids (HA) didn’t cause obvious reverse osmosis (RO) membrane fouling in 45 h.

Osmotic pressure (NaCl) affected slightly the RO membrane fouling behavior of HA.

Ca²⁺ promoted aggregation of HA molecules and thus aggravated RO membrane fouling.

Ozonation eliminated the effect of Ca²⁺ on the RO membrane fouling behavior of HA.

The change of the structure of HA was related to its membrane fouling behavior.

Abstract

Humic acid has been considered as one of the most significant sources in feed water causing organic fouling of reverse osmosis (RO) membranes, but the relationship between the fouling behavior of humic acid and the change of its molecular structure has not been well developed yet. In this study, the RO membrane fouling behavior of humic acid was studied systematically with ozonation as a pretreatment method to control RO membrane fouling. Furthermore, the effect of ozone on the structure of humic acid was also explored to reveal the mechanisms. Humic acid alone (10–90 mg/L, in deionized water) was found not to cause obvious RO membrane fouling in 45-h operation. However, the presence of Ca²⁺ aggravated significantly the RO membrane fouling caused by humic acid, with significant flux reduction and denser fouling layer on RO membrane, as it was observed by scanning electron microscope (SEM) and atomic force microscope (AFM). However, after the pretreatment by ozone, the influence of Ca²⁺ was almost eliminated. Further analysis revealed that the addition of Ca²⁺ increased the particle size of humic acid solution significantly, while ozonation reduced the SUVA₂₅₄, particle size and molecular weight of the complexes of humic acid and Ca²⁺ (HA-Ca²⁺ complexes). According to these results and literature, the bridge effect of Ca²⁺ aggregating humic acid molecules and the cleavage effect of ozone breaking HA-Ca²⁺ complexes were summarized. The change of the structure of humic acid under the effect of Ca²⁺ and ozone is closely related to the change of its membrane fouling behavior.

Graphical abstract

Keywords

Reverse osmosis / Membrane fouling / Humic acid / Ca²⁺ / Ozone

References

[1] Ang W S, Tiraferri A, Chen K L, Elimelech M (2011). Fouling and cleaning of RO membranes fouled by mixtures of organic foulants simulating wastewater effluent. Journal of Membrane Science, 376(1–2): 196–206

[2] Brown S L, Leonard K M, Messimer S L (2008). Evaluation of ozone pretreatment on flux parameters of reverse osmosis for surface water treatment. Ozone Science and Engineering, 30(2): 152–164

[3] Elimelech M, Wui Seng A (2007). Protein (BSA) fouling of reverse osmosis membranes: Implications for wastewater reclamation. Journal of Membrane Science, 296(1–2): 83–92

[4] Fritzmann C, Löwenberg J, Wintgens T, Melin T (2007). State-of-the-art of reverse osmosis desalination. Desalination, 216(1–3): 1–76

[5] Hong S, Elimelech M (1997). Chemical and physical aspects of natural organic matter (NOM) fouling of nanofiltration membranes. Journal of Membrane Science, 132(2): 159–181

[6] Jiang S, Li Y, Ladewig B P (2017). A review of reverse osmosis membrane fouling and control strategies. Science of the Total Environment, 595: 567–583

[7] Kalinichev A G, Iskrenova-Tchoukova E, Ahn W Y, Clark M M, Kirkpatrick R J (2011). Effects of Ca²⁺ on supramolecular aggregation of natural organic matter in aqueous solutions: A comparison of molecular modeling approaches. Geoderma, 169: 27–32

[8] Lee S, Ang W S, Elimelech M (2006). Fouling of reverse osmosis membranes by hydrophilic organic matter: implications for water reuse. Desalination, 187(1–3): 313–321

[9] Li H, Lin Y, Yu P, Luo Y, Hou L (2011). FTIR study of fatty acid fouling of reverse osmosis membranes: Effects of pH, ionic strength, calcium, magnesium and temperature. Separation and Purification Technology, 77(1): 171–178

[10] Lin J, Tang C Y, Huang C, Tang Y P, Ye W, Li J, Shen J, Van Den Broeck R, Van Impe J, Volodin A, Van Haesendonck C, Sotto A, Luis P, Van Der Bruggen B (2016). A comprehensive physico-chemical characterization of superhydrophilic loose nanofiltration membranes. Journal of Membrane Science, 501: 1–14

[11] Lin J, Tang C Y, Ye W, Sun S P, Hamdan S H, Volodin A, Haesendonck C V, Sotto A, Luis P, Van Der Bruggen B (2015). Unraveling flux behavior of superhydrophilic loose nanofiltration membranes during textile wastewater treatment. Journal of Membrane Science, 493: 690–702

[12] Manka J, Rebhun M, Mandelbaum A, Bortinger A (1974). Characterization of organics in secondary effluents. Environmental Science & Technology, 8(12): 1017–1020

[13] Matilainen A, Vepsäläinen M, Sillanpää M (2010). Natural organic matter removal by coagulation during drinking water treatment: A review. Advances in Colloid and Interface Science, 159(2): 189–197

[14] Mo H, Tay K G, Ng H Y (2008). Fouling of reverse osmosis membrane by protein (BSA): Effects of pH, calcium, magnesium, ionic strength and temperature. Journal of Membrane Science, 315(1–2): 28–35

[15] Nguyen V, Karunakaran E, Collins G, Biggs C A (2016). Physicochemical analysis of initial adhesion and biofilm formation of Methanosarcina barkeri on polymer support material. Colloids and Surfaces. B, Biointerfaces, 143: 518–525

[16] Ochando-Pulido J M, Martinez-Ferez A (2017). Fouling modelling on a reverse osmosis membrane in the purification of pretreated olive mill wastewater by adapted crossflow blocking mechanisms. Journal of Membrane Science, 544: 108–118

[17] Pandey S R, Jegatheesan V, Baskaran K, Shu L (2012). Fouling in reverse osmosis (RO) membrane in water recovery from secondary effluent: A review. Reviews in Environmental Science and Biotechnology, 11(2): 125–145

[18] Rodríguez F J, Marcos L A, Núñez L A, García M (2012). Effects of ozonation on molecular weight distribution of humic substances and coagulation processes—A case study: The uzquiza reservoir water. Ozone Science and Engineering, 34(5): 342–353

[19] She Q, Wong Y K W, Zhao S, Tang C Y (2013). Organic fouling in pressure retarded osmosis: Experiments, mechanisms and implications. Journal of Membrane Science, 428: 181–189

[20] Sun Y X, Hu H Y, Shi C Z, Yang Z, Tang F (2016). Changes in the components and biotoxicity of dissolved organic matter in a municipal wastewater reclamation reverse osmosis system. Environmental Technology, 37(17): 2149–2156

[21] Tang C Y, Kwon Y N, Leckie J O (2007). Fouling of reverse osmosis and nanofiltration membranes by humic acid— Effects of solution composition and hydrodynamic conditions. Journal of Membrane Science, 290(1–2): 86–94

[22] Tang C Y Y, Chong T H, Fane A G (2011). Colloidal interactions and fouling of NF and RO membranes: A review. Advances in Colloid and Interface Science, 164(1–2): 126–143

[23] Tang F, Hu H Y, Sun L J, Wu Q Y, Jiang Y M, Guan Y T, Huang J J (2014). Fouling of reverse osmosis membrane for municipal wastewater reclamation: Autopsy results from a full-scale plant. Desalination, 349: 73–79

[24] Tipping E (2002). Cation Binding by Humic Substances. New York: Cambridge University Press

[25] Van Geluwe S, Braeken L, Van der Bruggen B (2011). Ozone oxidation for the alleviation of membrane fouling by natural organic matter: A review. Water Research, 45(12): 3551–3570

[26] Wang H Y, Guan Y T, Mizuno T, Tsuno H (2010). RO filtration of biologically treated textile and dyeing effluents using ozonation as a pre-treatment. Water Science and Technology, 62(4): 751–758

[27] Wang J, Wang L, Miao R, Lv Y, Wang X, Meng X, Yang R, Zhang X (2016). Enhanced gypsum scaling by organic fouling layer on nanofiltration membrane: Characteristics and mechanisms. Water Research, 91: 203–213

[28] Wang L F, He D Q, Chen W, Yu H Q (2015). Probing the roles of Ca²⁺ and Mg²⁺ in humic acids-induced ultrafiltration membrane fouling using an integrated approach. Water Research, 81: 325–332

[29] Wenk J, Aeschbacher M, Salhi E, Canonica S, von Gunten U, Sander M (2013). Chemical oxidation of dissolved organic matter by chlorine dioxide, chlorine, and ozone: Effects on its optical and antioxidant properties. Environmental Science & Technology, 47(19): 11147–11156

[30] Wu J, Huang X (2009). Effect of mixed liquor properties on fouling propensity in membrane bioreactors. Journal of Membrane Science, 342(1–2): 88–96

[31] Yang Q, Liu Y, Li Y (2010a). Humic Acid fouling mitigation by antiscalant in reverse osmosis system. Environmental Science & Technology, 44(13): 5153–5158

[32] Yang Q F, Liu Y Q, Li Y J (2010b). Control of protein (BSA) fouling in RO system by antiscalants. Journal of Membrane Science, 364(1–2): 372–379

[33] Yavich A A, Masten S J (2001). Modeling the kinetics of the reaction of ozone with natural organic mmol/Latter in Huron River water. Ozone Science and Engineering, 23(2): 105–119

[34] Ye W, Bernstein N J, Lin J, Jordens J, Zhao S, Tang C Y, Van Der Bruggen B (2018). Theoretical and experimental study of organic fouling of loose nanofiltration membrane. Journal of the Taiwan Institute of Chemical Engineers, 93: 509–518

[35] Yu W, Liu T, Crawshaw J, Liu T, Graham N (2018). Ultrafiltration and nanofiltration membrane fouling by natural organic matter: Mechanisms and mitigation by pre-ozonation and pH. Water Research, 139: 353–362

[36] Zhang J N, Lin T, Chen W (2017). Micro-flocculation/sedimentation and ozonation for controlling ultrafiltration membrane fouling in recycling of activated carbon filter backwash water. Chemical Engineering Journal, 325: 160–168

[37] Zhang M, Lin H, Shen L, Liao B Q, Wu X, Li R (2016). Effect of calcium ions on fouling properties of alginate solution and its mechanisms. Journal of Membrane Science, 525: 320– 329 doi: 10.1016/j.memsci.2016.12.006

[38] Zhu H, Wen X, Huang X (2010). Membrane organic fouling and the effect of pre-ozonation in microfiltration of secondary effluent organic matter. Journal of Membrane Science, 352(1–2): 213–221

Acknowledgements

This study was funded by the National Key Research and Development Program of China (Grant No. 2016YFE0118800) and Key Program of the National Natural Science Foundation of China (No. 51738005). The Collaborative Innovation Center for Regional Environmental Quality also supported this research.

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