INVESTIGATION OF nZVI AND TiO2 NANOPARTICLES EFFECT ON THE MEMBRANE FOULING RATE IN ANAEROBIC MEMBRANE BIOREACTOR

Abstract

In recent years, membrane bioreactor technology (MBRs) has been increasingly used for wastewater treatment. However, the MBR system faces membrane fouling problems, which lead to higher operating costs, membrane replacement expenses, and reduced competitiveness. Therefore, understanding membrane fouling is essential not only for solving these issues but also as a key factor in advancing membrane technology. In this study, the effects of nano zero-valent iron (nZVI) and titanium dioxide (TiO2) nanoparticles on the membrane fouling rate in a laboratory-scale submerged anaerobic membrane bioreactor (AnMBR) treating landfill leachate (LFL) were investigated under controlled conditions (50-300 mg/L nZVI and TiO2). Additionally, both nZVI and TiO2 nanoparticles were compared regarding their impact on membrane fouling. The optimal membrane performance was observed at 100 mg/L TiO2 and 100 mg/L nZVI, with membrane fouling rates of 36 mbar/day and 34 mbar/day, respectively. The addition of TiO2 and nZVI significantly reduced membrane fouling (by 40% with TiO2 and 70% with nZVI) in the AnMBR. When comparing nZVI and TiO2 regarding membrane fouling rate, nZVI demonstrated the best performance. Based on the results, applying NPs in MBR systems significantly improves performance and reduces membrane fouling.

Keywords

• Nanoparticles
• Membrane bioreactor
• Landfill leachate
• nZVI
• TiO2

ANAEROBİK MEMBRAN BİYOREAKTÖRÜNDE nZVI VE TiO2 NANOPARTİKÜLLERİNİN MEMBRAN KİRLENME ORANI ÜZERİNDEKİ ETKİSİNİN ARAŞTIRILMASI

Abstract

Son yıllarda, membran biyoreaktör teknolojisi (MBR'ler) atıksu arıtımında giderek daha fazla kullanılmaktadır. Ancak MBR sistemi, daha yüksek işletme maliyetlerine, membran değiştirme masraflarına ve azalan rekabet gücüne yol açan membran kirlenme sorunlarıyla karşı karşıyadır. Bu nedenle, membran kirlenmesini anlamak yalnızca bu sorunları çözmek için değil, aynı zamanda membran teknolojisinin ilerlemesinde de önemli bir faktör olarak önemlidir. Bu çalışmada, nano sıfır değerlikli demir (nZVI) ve titanyum dioksit (TiO2) nanopartiküllerinin, LFL arıtan laboratuvar ölçekli bir batık anaerobik membran biyoreaktörde (AnMBR) membran kirlenme oranı üzerindeki etkileri kontrollü koşullar altında (50-300 mg/L nZVI ve TiO2) incelenmiştir. Ayrıca hem nZVI hem de TiO2 nanopartikülleri membran kirlenmesi üzerindeki etkileri açısından karşılaştırılmıştır. Optimum membran performansı, sırasıyla 36 mbar/gün ve 34 mbar/gün membran kirlenme oranlarıyla 100 mg/L TiO2 ve 100 mg/L nZVI'da gözlenmiştir. TiO2 ve nZVI ilavesi, AnMBR'de membran kirlenmesini önemli ölçüde azaltmıştır (TiO2 ile %40, nZVI ile %70). Membran kirlenme oranı açısından nZVI ve TiO2 karşılaştırıldığında, nZVI en iyi performansı göstermiştir. Sonuçlara dayanarak, MBR sistemlerine NP uygulanması performansı önemli ölçüde artırmakta ve membran kirlenmesini azaltmaktadır.

Keywords

• Nanopartiküller
• Membran Biyoreaktör
• Çöp sızıntı suları
• nZVI
• TiO2

References

1. Abdelrasoul, A., Doan, H., Lohi, A., 2013. Fouling in membrane filtration and remediation methods. Mass Transfer - Advances in Sustainable Energy and Environment Oriented Numerical Modeling, 195.
2. Alimoradi, H., Greish, K., Barzegar-Fallah, A., Alshaibani, L., Pittalà, V., 2018. Nitric oxide-releasing nanoparticles improve doxorubicin anticancer activity. International Journal of Nanomedicine, 7771-7787.
3. Amouamouha, M., Gholikandi, G.B., 2018. Assessment of anaerobic nanocomposite membrane bioreactor efficiency intensified by biogas backwash. Chemical Engineering and Processing - Process Intensification, 131, 51-58.
4. Anjum, M., Al-Makishah, N.H., Barakat, M.A., 2017. Wastewater sludge stabilization using anaerobic digestion: A review. Renewable and Sustainable Energy Reviews, 70, 1055-1064.
5. APHA, 1998. Standard Methods for the Examination of Water and Wastewater. 20th ed. American Public Health Association, Washington, DC, USA.
6. Bae, T.H., Tak, T.M., 2005. Effect of TiO2 nanoparticles on fouling mitigation of ultrafiltration membranes for activated sludge filtration. Journal of Membrane Science, 249(1-2), 1-8.
7. Bagheri, M., Mirbagheri, S.A., 2018. Critical review of fouling mitigation strategies in membrane bioreactors treating water and wastewater. Bioresource Technology, 258, 318-334.
8. Bagheri, S., Julkapli, N.M., 2016. Modified iron oxide nanomaterials: functionalization and application. Journal of Magnetism and Magnetic Materials, 416, 117-133.

9. Banu, J.R., Uan, D.K., Kaliappan, S., Yeom, I.T., 2011. Effect of sludge pretreatment on the performance of anaerobic/anoxic/oxic membrane bioreactor treating domestic wastewater. International Journal of Environmental Science & Technology, 8, 281-290.
10. Baolong, Z., Baishun, C., Keyu, S., Shangjin, H., Xiaodong, L., Zongjie, D., Kelian, Y., 2003. Preparation and characterization of nanocrystal grain TiO2 porous microsphere. Applied Catalysis B: Environmental, 40, 253-258.
11. Battistelli, A.A., Belli, T.J., Costa, R.E., Justino, N.M., Silveira, D.D., Lobo-Recio, M.A., Lapolli, F.R., 2019. Application of low-density electric current to performance improvement of membrane bioreactor treating raw municipal wastewater. International Journal of Environmental Science and Technology, 16, 3949-3960.
12. Chang, I.S., Le Clech, P., Jefferson, B., Judd, S., 2002. Membrane fouling in membrane bioreactors for wastewater treatment. Journal of Environmental Engineering, 128(11), 1018-1029.
13. De Souza Vandenberghe, L.P., Valladares-Diestra, K.K., Bittencourt, G.A., de Mello, A.F.M., Vásquez, Z.S., de Oliveira, P.Z., Soccol, C.R., 2022. Added-value biomolecules’ production from cocoa pod husks: A review. Bioresource Technology, 344, 126252.
14. DuBois, M., Gilles, K.A., Hamilton, J.K., Rebers, P.A., Smith, F., 1956. Colorimetric method for determination of sugars and related substances. Analytical Chemistry, 28(3), 350-356.
15. Feng, Y., Panwar, N., Tng, D.J.H., Tjin, S.C., Wang, K., Yong, K.T., 2016. The application of mesoporous silica nanoparticle family in cancer theranostics. Coordination Chemistry Reviews, 319, 86-109.
16. Gharibian, S., Hazrati, H., 2022. Towards practical integration of MBR with electrochemical AOP: Improved biodegradability of real pharmaceutical wastewater and fouling mitigation. Water Research, 218, 118478.
17. Gkotsis, P.K., Banti, D.C., Peleka, E.N., Zouboulis, A.I., Samaras, P.E., 2014. Fouling issues in membrane bioreactors (MBRs) for wastewater treatment: Major mechanisms, prevention and control strategies. Processes, 2(4), 795-866.
18. Göçer, S., Kozak, M., Akgül, V., Duyar, A., Zaimoğlu, Z., Cırık, K., 2019. Synthesis of nanoscale zero-valent iron (nZVI). International Symposium on Advanced Engineering Technologies (ISADET), 02-04 May 2019, Kahramanmaraş, Türkiye, pp. 828-833.
19. Göçer, S., Zaimoğlu, Z., Cırık, K., 2020. Synthesis of titanium dioxide (TiO2). Kahramanmaraş Sütçü İmam Üniversitesi Mühendislik Bilimleri Dergisi, 23(4), 219-226.
20. Göçer, S., Zaimoğlu, B.Z., Cırık, K., 2024. Effects of suspended titanium dioxide (TiO2) nanoparticles on cake layer formation in submerged anaerobic membrane bioreactor (AnMBR) for landfill leachate treatment (LFL). Process Biochemistry, 146, 525-538.
21. Göçer, S., Zaimoğlu, Z., Cırık, K., 2025. Effects of nano zero-valent iron nanoparticles on membrane fouling mitigation in a submerged anaerobic membrane bioreactor for landfill leachate treatment. Environmental Technology, 1-15.
22. Guo, W., Ngo, H.H., Li, J., 2012. A mini-review on membrane fouling. Bioresource Technology, 122, 27-34.
23. Guo, Y., Clark, S.J., Robertson, J., 2012. Electronic and magnetic properties of Ti2O3, Cr2O3, and Fe2O3 calculated by the screened exchange hybrid density functional. Journal of Physics: Condensed Matter, 24(32), 325504.
24. Gündoğdu, M., Jarma, Y.A., Kabay, N., Pek, T.Ö., Yüksel, M., 2019. Integration of MBR with NF/RO processes for industrial wastewater reclamation and water reuse: Effect of membrane type on product water quality. Journal of Water Process Engineering, 29, 100574.
25. Hawari, A.H., Larbi, B., Alkhatib, A., Yasir, A.T., Du, F., Baune, M., Thöming, J., 2019. Impact of aeration rate and dielectrophoretic force on fouling suppression in submerged membrane bioreactors. Chemical Engineering and Processing - Process Intensification, 142, 107565.
26. Hu, Y., Wang, X., Zhang, Y., Li, Y., Yang, F., 2020. Effect of iron-based additives on membrane fouling and microbial community in anaerobic membrane bioreactors. Water Research, 172, 115515.
27. Jiang, T., Kennedy, M.D., van der Meer, W.G., Vanrolleghem, P.A., Schippers, J.C., 2003. The role of blocking and cake filtration in MBR fouling. Desalination, 157(1-3), 335-343.
28. Kim, J., Van der Bruggen, B., 2010. The use of nanoparticles in polymeric and ceramic membrane structures: Review of manufacturing procedures and performance improvement for water treatment. Environmental Pollution, 158(7), 2335-2349.
29. Kjeldsen, P., Barlaz, M.A., Rooker, A.P., Baun, A., Ledin, A., Christensen, T.H., 2002. Present and long-term composition of MSW landfill leachate: A review. Critical Reviews in Environmental Science and Technology, 32(4), 297-336. DOI: 10.1080/10643380290813462
30. Le-Clech, P., Chen, V., Fane, T.A.G., 2006. Fouling in membrane bioreactors used for wastewater treatment. Journal of Membrane Science, 284(1-2), 17-53.
31. Lefevre, E., Bossa, N., Wiesner, M.R., Gunsch, C.K., 2016. A review of the environmental implications of in situ remediation by nanoscale zero valent iron (nZVI): Behavior, transport and impacts on microbial communities. Science of the Total Environment, 565, 889-901.
32. Li, K., Li, S., Sun, C., Huang, T., Li, G., Liang, H., 2020. Membrane fouling in an integrated adsorption-UF system: Effects of NOM and adsorbent properties. Environmental Science: Water Research & Technology, 6(1), 78-86.
33. Liu, X., Zhang, S., Zhang, X., Guo, H., Cao, X., Lou, Z., Wang, C., 2022. A novel lignin hydrogel supported nZVI for efficient removal of Cr(VI). Chemosphere, 301, 134781.
34. Lowry, O.H., Rosebrough, N.J., Farr, A.L., Randall, R.J., 1951. Protein measurement with the Folin phenol reagent. Journal of Biological Chemistry, 193(1), 265-275.
35. Maaz, M., Karim, A., Kumar, G., Kim, S.H., Bhatnagar, A., 2019. Iron-based additives for anaerobic digestion: A review on enhancement of biogas production and process stability. Bioresource Technology, 282, 496-512.
36. Mei, X., Wang, Z., Zheng, X., Huang, F., Ma, J., Tang, J., Wu, Z., 2014. Soluble microbial products in membrane bioreactors in the presence of ZnO nanoparticles. Journal of Membrane Science, 451, 169-176.
37. Meng, F., Chae, S.R., Drews, A., Kraume, M., Shin, H.S., Yang, F., 2009. Recent advances in membrane bioreactors (MBRs): Membrane fouling and membrane material. Water Research, 43(6), 1489-1512.
38. Nabi, M., Zhang, J., Zhang, X., Li, Y., 2023. Recent advances in anaerobic membrane bioreactors for wastewater treatment: Fouling control and performance enhancement. Water Research, 231, 119599.
39. Patil, S.S., Shedbalkar, U.U., Truskewycz, A., Chopade, B.A., Ball, A.S., 2016. Nanoparticles for environmental clean-up: A review of potential risks and emerging solutions. Environmental Technology & Innovation, 5, 10-21.
40. Rahman, T.U., Roy, H., Islam, M.R., Tahmid, M., Fariha, A., Mazumder, A., Islam, M.S., 2023. The advancement in membrane bioreactor (MBR) technology toward sustainable industrial wastewater management. Membranes, 13(2), 181.
41. Renou, S., Givaudan, J.G., Poulain, S., Dirassouyan, F., Moulin, P., 2008. Landfill leachate treatment: Review and opportunity. Journal of Hazardous Materials, 150(3), 468-493.
42. Sacca, M.L., Fajardo, C., Nande, M., Martín, M., 2013. Effects of nano zero-valent iron on Klebsiella oxytoca and stress response. Microbial Ecology, 66(4), 806-812.
43. Sevcu, A., El-Temsah, Y.S., Joner, E.J., Cernik, M., 2012. Oxidative stress induced in microorganisms by zero-valent iron nanoparticles. Microbes and Environments, 27(2), 215-215.
44. Sichinga, M.C., Frazee, J., Tong, A.Z., 2016. Efficiency and kinetics in treatment of wastewater from garages and residential oil spills using membrane bioreactor technology. International Journal of Environmental Science and Technology, 13, 135-146.
45. Teng, J., Wu, M., Chen, J., Lin, H., He, Y., 2020. Different fouling propensities of loosely and tightly bound extracellular polymeric substances (EPSs) and the related fouling mechanisms in a membrane bioreactor. Chemosphere, 255, 126953.
46. Tian, Y., Li, Z., Ding, Y., Lu, Y., Yang, F., 2013. Filtration characteristics of soluble microbial products (SMPs) in membrane bioreactor. Journal of Membrane Science, 441, 205-213.
47. Ugarte, P., Ramo, A., Quílez, J., del Carmen Bordes, M., Mestre, S., Sánchez, E., Menéndez, M., 2022. Low-cost ceramic membrane bioreactor: Effect of backwashing, relaxation and aeration on fouling. Protozoa and bacteria removal. Chemosphere, 306, 135587.
48. Wang, Z., Ma, J., Tang, C.Y., Kimura, K., Wang, Q., Han, X., 2014. Membrane cleaning in membrane bioreactors: A review. Journal of Membrane Science, 468, 276-307.
49. Wang, Z., Wu, Z., 2009. A review of membrane fouling in MBRs: Characteristics and role of sludge cake formed on membrane surfaces. Separation Science and Technology, 44(15), 3571-3596.
50. Wu, M., Chen, Y., Lin, H., Zhao, L., Shen, L., Li, R., He, Y., 2020. Membrane fouling caused by biological foams in a submerged membrane bioreactor: Mechanism insights. Water Research, 181, 115932.
51. Xi, W., Geissen, S.U., 2001. Separation of titanium dioxide from photocatalytically treated water by cross-flow microfiltration. Water Research, 35(1), 256-1262.
52. Xiang, Q., Meng, G., Zhang, Y., Xu, J., Xu, P., Pan, Q., Yu, W., 2010. Ag nanoparticle embedded-ZnO nanorods synthesized via a photochemical method and its gas-sensing properties. Sensors and Actuators B: Chemical, 143(2), 635-640.
53. Yuniarto, A., Noor, Z.Z., Ujang, Z., Olsson, G., Aris, A., Hadibarata, T., 2013. Bio-fouling reducers for improving the performance of an aerobic submerged membrane bioreactor treating palm oil mill effluent. Desalination, 316, 146-153.
54. Zhang, J., Wang, Z., Wu, Z., Zhou, Z., 2018. Membrane fouling mechanisms in membrane bioreactors for wastewater treatment: A review. Journal of Environmental Sciences, 64, 9-20.
55. Zhang, Y., Hu, Y., Wang, X., Yang, F., 2020. Enhanced membrane fouling in anaerobic membrane bioreactors induced by excessive iron release. Journal of Membrane Science, 610, 118261.
56. Zhou, L., Zhuang, W., Wang, X., Yu, K., Yang, S., Xia, S., 2017. Potential effects of loading nano zero valent iron discharged on membrane fouling in an anoxic/oxic membrane bioreactor. Water Research, 111, 140-146.
57. Zhu, H., Wen, X., Huang, X., 2012. Characterization of membrane fouling in a microfiltration ceramic membrane system treating secondary effluent. Desalination, 284, 324-331.