Single-step electrospraying fabrication of composite nanofiltration membranes for efficient bentazone herbicide removal from water

Mohammadpour, Rezvane; Beigmoradi, Razieh; Samimi, Abdolreza; Mohebbi-Kalhori, Davod

doi:10.22104/jpst.2026.8363.1295

Single-step electrospraying fabrication of composite nanofiltration membranes for efficient bentazone herbicide removal from water

Document Type : Research Article

Authors

Rezvane Mohammadpour ¹

Razieh Beigmoradi ²

Abdolreza Samimi ¹

Davod Mohebbi-Kalhori ¹

¹ Department of Chemical Engineering, University of Sistan and Baluchestan, Zahedan, Iran.

² Department of Chemical Engineering, Faculty of Engineering, Ardakan University, P. O. Box 184, Ardakan, Iran

10.22104/jpst.2026.8363.1295

Abstract

A composite nanofiltration membrane was successfully fabricated via a single-step electrospraying process for the efficient removal of bentazone from contaminated water. Key electrospraying parameters—polymer concentration, solution flow rate, and applied electric field strength—were systematically optimized using the Taguchi design of experiments, which identified polymer concentration as the most influential factor governing membrane performance. The optimum fabrication conditions were determined to be a 5 wt% polymer concentration, a 2.2 mL.h^-1 flow rate, and a 0.66 kV.cm^-1 electric field strength. The fabricated membranes were characterized using scanning electron microscopy, nitrogen adsorption–desorption, water contact angle, and surface profilometry. Membrane performance was evaluated using a 200 mg.L^-1 bentazone feed solution in a vacuum-assisted dead-end filtration system operated at a transmembrane pressure of 10 psi. Under these optimal conditions, the membrane exhibited a pure water flux of 34.7 L.m^-2.h^-1. During bentazone filtration, the flux decreased to 19.75 L.m^-2.h^-1, while achieving an excellent bentazone rejection of 96.2 ± 1.44 %. These findings confirm that optimizing electrospraying parameters, particularly polymer concentration, is critical for developing high-performance composite nanofiltration membranes. Overall, the proposed single-step electrospraying method offers a simple, highly controllable, and practical alternative to conventional approaches for fabricating composite nanofiltration membranes.

Graphical Abstract

Single-step electrospraying fabrication of composite nanofiltration membranes for efficient bentazone herbicide removal from water

Highlights

Single-step electrospraying is used to fabricate TFC polyamide membranes.
Layer - by - layer electrospray deposition controls the membrane structure.
The membrane achieved > 9 % bentazone rejection with satisfactory flux.
The solvent-free process offers a green alternative to interfacial polymerization.

Keywords

Electrospray deposition

Polyethersulfone support

Composite nanofiltration

Polyamide membrane

Bentazone rejection

Subjects

Water and Wastewater

[1] Kim, S., Jun, B. -M., Jung, B., Park, C. M., Jang, M., Nam, S. -N., & Yoon, Y. (2025). Removal of Contaminants of Emerging Concern by Membranes in Water and Wastewater: An Updated Review. Environmental Engineering Research, 30(1), 240103. https://doi.org/10.4491/eer.2024.103

[2] Panagopoulos, A., & Michailidis, P. (2025). Membrane Technologies for Sustainable Wastewater Treatment: Advances, Challenges, and Applications in Zero Liquid Discharge (ZLD) and Minimal Liquid Discharge (MLD) Systems. Membranes, 15(2), 64. https://doi.org/10.3390/membranes15020064

[3] Ali, J., Alhseinat, E., Jaoude, M. A., Nashef, I. M. A., Adeyemi, I. A., Aminabhavi, T. M., & Arafat, H. A. (2022). A Mixed Matrix Polyimide Ultrafiltration Membrane for Efficient Removal of Mentazon from Water. Chemical Engineering Journal, 433, 134596. https://doi.org/10.1016/j.cej.2022.134596

[4] Nematzadeh, M., Samimi, A., Shokrollahzadeh, S., & Mohebbi-Kalhori, D. (2019). Bentazon Removal from Aqueous Solution by Reverse Osmosis; Optimization of Effective Parameters Using Response Surface Methodology. Advances in Environmental Technology, 5(4), 193-201.https://doi.org/10.22104/aet.2020.4228.1209

[5] Utzeri, G., Guirado-Moreno, J. C., Cova, T. F. G. G., Pais, A. A. A. C., Batista De Carvalho, L. A. E., Ibeas, S., García, J. M., Valente, A. J. M., & Vallejos, S. (2024). Reusable and Effective Polyacrylic Membranes for Mecoprop and Bentazon Extractions. npj Clean Water, 7(1), 39. https://doi.org/10.1038/s41545-024-00328-3

[6] Herschy, R. W. (2012). Water Quality for Drinking, WHO Guidelines. In L. Bengtsson, R. W. Herschy, & R. W. Fairbridge (Eds.), Encyclopedia of Lakes and Reservoirs (pp. 876-883). Springer, Dordrecht. https://doi.org/10.1007/978-1-4020-4410-6_184

[7] Grillo-Avila, D., Antón-Pardo, M., Armengol, J., Puche, E., Carballeira, R., Moratalla-López, J., Palacios-Abella, J. F., López, I., Minaglia, M. C. C., Amador, P., Rochera, C., Picazo, A., Mesquita-Joanes, F., Camacho, A., & Rico, A. (2025). Effects of the Herbicide Bentazone on the Structure of Plankton and Benthic Communities Representative of Mediterranean Coastal Wetlands: A Mesocosm Experiment. Hydrobiologia, 852(10), 2709-2728. https://doi.org/10.1007/s10750-024-05779-w

[8] Oros, A. (2025). Bioaccumulation and trophic transfer of heavy metals in marine fish: Ecological and ecosystem-level impacts. Journal of Xenobiotics, 15(2), 59. https://doi.org/10.3390/jox15020059

[9] Matisāne, L., Akūlova, L., Kolossa-Gehring, M., & Vanadziņš, I. (2026). Public Views on Pesticide Exposure and Human Biomonitoring in Latvia: Evidence from Focus Groups and Media Analysis. Toxics, 14(6), 466. https://doi.org/10.3390/toxics14060466

[10] Gavrilaș, S., Gerőcs, T., Chereji, B.-D., & Munteanu, F. -D. (2026). Trends in Advanced Wastewater Treatment Technologies: From Membrane Bioreactors to Advanced Oxidation Processes. Water, 18(3), 350. https://doi.org/10.3390/w18030350

[11] Hübner, U., Spahr, S., Lutze, H., Wieland, A., Rüting, S., Gernjak, W., & Wenk, J. (2024). Advanced Oxidation Processes for Water and Wastewater Treatment–Guidance for Systematic Future Research. Heliyon, 10(9), e30402. https://doi.org/10.1016/j.heliyon.2024.e30402

[12] Moreira, A., & da Silva, M. V. (2025). Exposure to Pesticides, Risk Assessment and Analysis of Occupational Health and Safety in Agriculture Context: A Systematic Review. In J. S. Baptista, R. B. Melo, P. Carneiro, J. C. Branco, N. Costa, J. Duarte, J. C. Guedes, & G. Perestrelo (Eds.), Occupational and Environmental Safety and Health VI. Studies in Systems, Decision and Control, Vol. 230. (pp. 119-135). Springer, Cham. https://doi.org/10.1007/978-3-031-82166-0_11

[13] Nure J. F., & Nkambule, T. T. I. (2023). The Recent Advances in Adsorption and Membrane Separation and Their Hybrid Technologies for Micropollutants Removal from Wastewater. Journal of Industrial and Engineering Chemistry, 126, 92-114. https://doi.org/10.1016/j.jiec.2023.06.034

[14] Priyadarshini, M., Das, I., Ghangrekar, M. M., & Blaney, L. (2022). Advanced Oxidation Processes: Performance, Advantages, and Scale-Up of Emerging Technologies. Journal of Environmental Management, 316, 115295. https://doi.org/10.1016/j.jenvman.2022.115295

[15] Tufail, A., Price, W. E., & Hai, F. I. (2020). A Critical Review on Advanced Oxidation Processes for the Removal of Trace Organic Contaminants: A Voyage from Individual to Integrated Processes. Chemosphere, 260, 127460. https://doi.org/10.1016/j.chemosphere.2020.127460

[16] Moreira, J. B., Santos, T. D., Zaparoli, M., de Almeida, A. C. A., Costa, J. A. V., & de Morais, M. G. (2022). An Overview of Nanofiltration and Nanoadsorption Technologies to Emerging Pollutants Treatment. Applied Sciences, 12(16), 8352. https://doi.org/10.3390/app12168352

[17] Farah, I. F. (2025). Pesticides in surface and groundwater: occurrence, environmental and human health risk, and removal efficiency by membrane technologies. [Master’s thesis, Federal University of Minas Gerais]. https://hdl.handle.net/1843/83804

[18] Zhou, B., Luo, J., Jin, M., Xue, N., He, R., Li, W., & He, T. (2025). Micropollutants Removal from Aquaculture Water Using Layer-by-Layer Self-Assembled Nanofiltration Membranes. Water research, 271, 122933. https://doi.org/10.1016/j.watres.2024.122933

[19] Namla, D., Oves, M., Alshaeri, M. A., Al-Maaqar, S. M., Issa, H. N. Y., & Mangse, G. (2025). Nanofiltration as an Advanced Wastewater Treatment Technique: A Comprehensive Review. Discover Applied Sciences, 7,(4), 355. https://doi.org/10.1007/s42452-025-06576-3

[20] Maroufi, N., & Hajilary, N. (2023). Nanofiltration Membranes Types and Application in Water Treatment: A Review. Sustainable Water Resources Management, 9(5), 142. https://doi.org/10.1007/s40899-023-00899-y

[21] Yin, H., Wang, D., Shi, M., & Xu, X. (2025). Wastewater Treatment and Resource Recovery by Loose Nanofiltration Membrane: A Critical Review. Environmental Engineering Research, 31(1), 250122. https://doi.org/10.4491/eer.2025.122

[22] Chowdhury, M. R., Steffes, J., Huey, B. D., & McCutcheon, J. R. (2018). 3D Printed Polyamide Membranes for Desalination. Science (New York, N.Y.), 361(6403), 682-686. https://doi.org/10.1126/science.aar2122

[23] Kingsley, B. J., Pawliczak, E. E., Hurley, T. R., & Chiarot, P. R. (2021). Electrospray Printing of Polyimide Films Using Passive Material Focusing. ACS Applied Polymer Materials, 3(12), 6274-6284. https://10.1021/acsapm.1c01073

[24] Al-Ghafri, B., Kyaw, H. H., Al-Abri, M., & Lau, W. -J. (2022). Performance Study of novel PES membrane using electrospray deposition method for organic contaminants separation. Chemical Engineering Research and Design, 186, 73-81. https://doi.org/10.1016/j.cherd.2022.07.028

[25] Green-Warren, R. A., Fassler, A. L., Juhl, A., McAllister, N. M., Huth, A., Arkhipov, M., Grzenda, M. J., Pejman, S. R., Durstock, M. F., & Singer, J. P. (2024). Self-Limiting Electrospray Deposition (SLED) of Porous Polyimide Coatings as Effective Lithium-Ion Battery Separator Membranes. RSC Applied Polymers, 2(6), 1074-1081. https://doi.org/10.1039/d4lp00192c

[26] Kovacevich D. A., Lei, L., Han, D., Kuznetsova, C., Kooi, S. E., Lee, H., & Singer, J. P. (2020). Self-Limiting Electrospray Deposition for the Surface Modification of Additively-Manufactured Parts. ACS Applied Materials & Interfaces,12(18), 20901-20911. https://doi.org/10.1021/acsami.9b23544

[27] Vatanpour, V., Kose-Mutlu, B., & Koyuncu, I. (2022). Electrospraying technique in fabrication of separation membranes: A review. Desalination, 533, 115765. https://doi.org/10.1016/j.desal.2022.115765

[28] Lei, L., Kovacevich, D. A., Nitzsche, M. P., Ryu, J., Al-Marzoki, K., Rodriguez, G., Klein, L. C., Jitianu, A., & Singer, J. P. (2018). Obtaining Thickness-Limited Electrospray Deposition for 3D Coating. ACS Applied Materials & Interfaces, 10(13), 11175-11188. https://doi.org/10.1021/acsami.7b19812

[29] Beigmoradi, R., Samimi, A., & Mohebbi-Kalhori, D. (2018). Fabrication of Polymeric Nanofibrous Mats with Controllable Structure and Enhanced Wetting Behavior Using One-Step Electrospinning. Polymer, 143, 271-280. https://doi.org/10.1016/j.polymer.2018.04.025

[30] Moghadam, H., Samimi, M., Samimi, A., & Khorram, M. (2008). Electro-Spray of High Viscous Liquids for Producing Mono-Sized Spherical Alginate Beads. Particuology, 6(4), 271-275. https://doi.org/10.1016/j.partic.2008.04.005

[31] Tabeei, A., Samimi, A., Khorram, M., & Moghadam, H. (2012). Study Pulsating Electrospray of Non-Newtonian and Thixotropic Sodium Alginate Solution. Journal of Electrostatics, 70(1), 77-82. https://doi.org/10.1016/j.elstat.2011.10.006

[32] Montgomery, D. C. (2017). Design and Analysis of Experiments (9^thed.). John Wiley & Sons.

[33] Roy, R. K. (2010). A Primer on the Taguchi Method (2^nd ed.). Society of Manufacturing Engineers.

[34] Thommes, M., Kaneko, K., Neimark, A., Olivier, J., Rodriguez-Reinoso, F., Rouquerol, J. & Sing, K. (2015). Physisorption of Gases, with Special Reference to the Evaluation of Surface Area and Pore Size Distribution (IUPAC Technical Report). Pure and Applied Chemistry, 87(9-10), 1051-1069. https://doi.org/10.1515/pac-2014-1117

[35] Braga, C. S., Bessegato, G. G., Maestre, K., Espinoza-Quiñones, F. R., Alves, H. J., da Silva, L. C., Eising, R., & Bariccatti, R. A. (2023). Photocatalytic Degradation of Bentazon Pesticide by a Fe₂O₃-TiO₂ Composite Catalyst Irradiated by UVA, UVB, and Natural Light. Journal of the Brazilian Chemical Society, 34(9), 1284-1292. https://doi.org/10.21577/0103-5053.20230039

[36] Jin, J., Sun, X., Yu, G., Wang, H. & Zhang, S. (2025). Characterization of Bentazone in Potable Water by Combined UV-Visible Spectroscopy [Paper presentation]. 2025 IEEE 7^th International Conference on Artificial Intelligence, Computer Science, and Information Processing (AICSIP), Hangzhou, China. https://doi.org/10.1109/aicsip65423.2025.11427287