Recovery of polyphenols from orange peel extract involving 3D printed PLA ultrafiltration membrane
DOI:
https://doi.org/10.15407/hftp17.02.200Keywords:
orange peel extract, polyphenols, 3D printing membrane, polylactic acid, ultrafiltrationAbstract
Such biologically active compounds as polyphenols are widely used in pharmaceutical, food and cosmetic industry, since they possess high antimicrobial and antioxidant activity. These substances are recovered from plant extracts. For their concentrating, baromembrane separation is desirable, since it provides no degradation of target products. In this work, ultrafiltration membrane produced from polylactic acid (PLA) using 3D printing (fused deposition modelling technique) was applied to the recovery of polyphenols from orange peel extract. Main advantage of 3D printing is a possibility to manufacture membranes of any shape and size, which are needed for customers. The particles with a size of several hundred nanometers and larger have been preliminarily removed from the extract to accelerate filtration. The effect of polyphenol concentration and pressure on the filtration process has been studied. As found, the rejection of polyphenols from the extract, which contains no large particles, reaches » 90 %, it is independent on pressure within the interval of 0.5–2.0 bar. The flux increases with pressure and reaches 1.7-3.2 L m–2h–1 for the most concentrated solution. In the case of pristine extract, rejection decreases with pressure. Different behavior of membrane towards extracts is explained from the point of view of concentration polarization, which results in a formation of dynamic layers, where large or small particles dominate. The transport properties of the membrane are restored after regeneration with ethanol.
References
1. Someda S.K., Takahashi Y. Applications of three-dimensional printing technology in oculoplastic and orbital surgery: updates and trends. Expert Rev. Ophthalmol. 2023. 18(5): 275. https://doi.org/10.1080/17469899.2023.2267757
2. Zhu Y., Qin J., Shi G., Sun C., Ingram M., Qian S. A focus review on 3D printing of wearable energy storage devices. Carbon Energy. 2022. 4(1): 1242. https://doi.org/10.1002/cey2.199
3. Jivrakh K.B., Kuppireddy S., Dum?e L.F., Polychronopoulou K., Abu Al-Rub R.K., Alamoodi N. A critical review on 3D-printed adsorbents, membranes, and catalysts for carbon dioxide capture, separation, and conversion. J. Clean. Prod. 2024. 472(1): 143522. https://doi.org/10.1016/j.jclepro.2024.143522
4. Wu T., Karimi-Maleh H., Li Y., Zhang Z., Zhang D., Wen Y., Fu L., Zhong N., Dragoi E.N., Aminabhavi T.M. 3D printed monolithic nanocomposites as adsorbents to remove Congo Red and mercury (II) from wastewater. Chem. Eng. J. 2024. 501: 157710. https://doi.org/10.1016/j.cej.2024.157710
5. Dzyazko Yu., Molina L.C.A., Ribeiro A.C., Wernke G., Bergamasco R. Obtaining a low cost adsorbent from a biodegradable polymer for the removal of low molecular organic compounds from solutions of technological origin. Ukr. Chem. J. 2024. 90(7): 3. https://doi.org/10.33609/2708-129X.90.7.2024.3-24
6. Chen T., Xu P., Qiu M., Chen X., Zhong Z., Fan Y. Construction of anti-fouling ceramic tubular membranes with corrugated inner surfaces using DLP 3D printing. J. Membr. Sci. 2024. 706: 122941. https://doi.org/10.1016/j.memsci.2024.122941
7. Kirkeb?k B.S., Artemeva M., Navas J.L., Danielak A.H., Pedersen D.B., Ali A., Quist-Jensen C.A. Tunable physicochemical properties of 3D printed membranes via copolymerization and micropatterning. J. Membr. Sci. 2025. 735: 124483. https://doi.org/10.1016/j.memsci.2025.124483
8. Thiam B.G., El Magri A., Vanaei H.R., Vaudreuil S. 3D Printed and Conventional Membranes - A Review. Polymers. 2022. 14(5): 1023. https://doi.org/10.3390/polym14051023
9. Han L., Chen C., Shen L., Lin H., Li B., Huang Z., Xu Y., Li R., Hong H. Novel membranes with extremely high permeability fabricated by 3D printing and nickel coating for oil/water separation. J. Mater. Chem. A. 2022. 10(22): 12055. https://doi.org/10.1039/D2TA01971J
10. Zhang Q., Pardo M., Rudich Y., Kaplan-Ashiri I., Wong J.P.S., Davis A.Y., Black M.S., Weber R.J. Chemical composition and toxicity of particles emitted from a consumer-level 3D printer using various materials. Environ. Sci. Technol. 2019. 53(20): 12054. https://doi.org/10.1021/acs.est.9b04168
11. Qian X., Anvari A., Hoek E.M.V., McCutcheon J.R. Advancements in conventional and 3D printed feed spacers in membrane modules. Desalination. 2023. 556: 116518. https://doi.org/10.1016/j.desal.2023.116518
12. Barman S.R., Gavit P., Chowdhury S., Chatterjee K., Nain A. 3D-Printed Materials for Wastewater Treatment. JACS Au. 2023. 3: 2930. https://doi.org/10.1021/jacsau.3c00409
13. Thiam B.G., El Magri A., Vanaei H.R., Vaudreuil S. 3D Printed and Conventional Membranes - A Review. Polymers. 2022. 14(5): 1023. https://doi.org/10.3390/polym14051023
14. Aghaei A., Dadashi Firouzjaei M., Karami P., Aghapour Aktij S., Elliott M., Mansourpanah Y., Rahimpour A., Soares J.B.P., Sadrzadeh M. The implications of 3D?printed membranes for water and wastewater treatment and resource recovery. Can. J. Chem. Eng. 2022. 100(9): 2309. https://doi.org/10.1002/cjce.24488
15. Soo A., Ali S.M., Shon H.K. 3D printing for membrane desalination: Challenges and future prospects. Desalination. 2021. 520: 115366. https://doi.org/10.1016/j.desal.2021.115366
16. Chowdhury M.R., Steffes J., Huey B.D., McCutcheon J.R. 3D printed polyamide membranes for desalination. Science. 2018. 361(6403): 682. https://doi.org/10.1126/science.aar2122
17. Li X., Shan H., Zhang W., Li B. 3D printed robust superhydrophilic and underwater superoleophobic composite membrane for high efficient oil/water separation. Sep. Purif. Technol. 2019. 237: 116324. https://doi.org/10.1016/j.seppur.2019.116324
18. Zhang J., Li Y., He B., Zhang T., Yang W., Yu W., Hu L., Jiang G. 3D-printed flexible thermoplastic polyurethane membrane for ultrafast oil/water separation. Chem. Eng. J. 2025. 503: 158500. https://doi.org/10.1016/j.cej.2024.158500
19. Al-Shimmery A., Mazinani S., Ji J., Chew Y.M.J., Mattia D. 3D printed composite membranes with enhanced anti-fouling behaviour. J. Membr. Sci. 2019. 574: 76. https://doi.org/10.1016/j.memsci.2018.12.058
20. Issac M.N., Kandasubramanian B. Review of manufacturing three-dimensional-printed membranes for water treatment. Environ. Sci. Pollut. Res. 2020. 27: 36091. https://doi.org/10.1007/s11356-020-09452-2
21. He J., Yang J., McCutcheon J.R., Li Y. Molecular insights into the structure-property relationships of 3D printed polyamide reverse-osmosis membrane for desalination. J. Membr. Sci. 2022. 658: 120731. https://doi.org/10.1016/j.memsci.2022.120731
22. Aghaei A., Dadashi Firouzjaei M., Karami P., Aghapour Aktij S., Elliott M., Mansourpanah Y., Rahimpour A., Soares J.B.P., Sadrzadeh M. The implications of 3D printed membranes for water and wastewater treatment and resource recovery. Can. J. Chem. Eng. 2022. 100(9): 2309. https://doi.org/10.1002/cjce.24488
23. Pereira P.P., Gon?alves I.P., Molina L.C.A., Delcolle R., Dzyazko Y.S., Paraiso C.M., Batista Neto G.L., Di?rio A., Vieira A.M.S., Bergamasco R. Membrane for pressure-driven separation prepared with a method of 3D printing: performance in concentrating orange peel extract. Membranes. 2025. 15(4): 105. https://doi.org/10.3390/membranes15040105
24. Tian M., De Coninck H., Zhu J., Zhang Y. Exploring the potential usage of 3D printed membranes combined with PVDF coating in direct contact membrane distillation. Desalination. 2021. 513: 115134. https://doi.org/10.1016/j.desal.2021.115134
25. Navarro-Tovar R., Zoumpouli G.A., Gorgojo P., Martin P., Chew Y.M.J., Mattia D., P?rez-Page M. Mitigation of organic fouling in membrane distillation via 3D printed wavy composite membranes. Desalination. 2025. 614: 119201. https://doi.org/10.1016/j.desal.2025.119201
26. Gutierrez D.B., Caldona E.B., Yang Z., Suo X., Cheng X., Dai S., Espiritu R.D., Advincula R.C. 3D-printed PDMS-based membranes for CO? separation applications. MRS Commun. 2022. 12(6): 1174. https://doi.org/10.1557/s43579-022-00287-1
27. Alkandari S.H., Ghosh S., Kandasubramanian B. Recycling and 3D-printing biodegradable membranes for gas separation. ACS Appl. Energy Mater. 2024. 7(4): 2232. https://doi.org/10.1021/acsaenm.4c00060
28. Yu X., Yang H., Lv X., Zhang X., Jegatheesan V., Zhou X., Zhang Y. Characterization and performance evaluation of digital light processing 3D printed functional anion exchange membranes in electrodialysis. Processes. 2024. 12(6): 1043. https://doi.org/10.3390/pr12061043
29. Venu M., Galinha C.F., Crespo J.G., Pawlowski S. Development of cation-exchange membranes using solvent-free 3D printing: Towards tailored surface topographies. Sep. Purif. Technol. 2025. 378: 134567. https://doi.org/10.1016/j.seppur.2025.134567
30. Z?rybnick? L. The effect of 3D printing parameters on electrochemical properties of heterogeneous cation exchange membranes. Rapid Prototyp. J. 2021. 27(3): 563. https://doi.org/10.1108/RPJ-08-2020-0207
31. Santos J.A., Silva R.M., Oliveira M.R., Costa A.C., Souza A.P., Lima E.C., Silva M.A., Lima J.S., Silva A.F. 3D printing of polymer matrix composites: A review and future perspectives. Mater. Today Proc. 2022. 52: 1224.
32. Kristiawan R.B., Imaduddin F., Ariawan D., Ubaidillah, Arifin Z. A review on the fused deposition modeling (FDM) 3D printing: filament processing, materials, and printing parameters. Open Eng. 2021. 11(1): 639. https://doi.org/10.1515/eng-2021-0063
33. Kudelko K., Rozhdestvenskaya L., Ogenko V., Chmilenko V. Formation and characterisation of porous anodized aluminum oxide, synthesized electrochemically in the presence of graphene oxide. Appl. Nanosci. 2022. 12(6): 1967. https://doi.org/10.1007/s13204-022-02457-y
34. Kudelko K.O., Dziazko O.H., Rozhdestvenskaya L.M., Kharkova L.B., Ogenko V.M. Formation of nanopores in anodic oxidized aluminium under the influence of carbon nanoparticles. Nanosistemi, Nanomateriali, Nanotehnologii. 2024. 22(1): 53. https://doi.org/10.15407/nnn.22.01.053
35. Wang X., Li Y., Zhang L., Xu L., Wei J., Zhang Z. 3D printing of polymer matrix composites: A review and future perspectives. Mater. Today Proc. 2018. 5(1): 1960.
36. Dzyaz'ko Y.S., Belyakov V.N., Stefanyak N.V., Vasilyuk S.L. Anion-Exchange Properties of Composite Ceramic Membranes Containing Hydrated Zirconium Dioxide. Russ. J. Appl. Chem. 2006. 79(5): 769. https://doi.org/10.1134/S1070427206050132
37. Dzyazko Y., Rozhdestvenska L., Kudelko K., Ogenko V., Kolomiiets Y. Membranes modified with advanced carbon nanomaterials. Springer Proc. Phys. 2021. 263: 151. https://doi.org/10.1007/978-3-030-74741-1_10
38. Dzyazko Yu.S., Volfkovich Yu.M., Chaban M.O. Composites containing inorganic ion exchangers and graphene oxide: hydrophilic-hydrophobic and sorption properties (review). Springer Proc. Phys. 2020. 246: 93. https://doi.org/10.1007/978-3-030-51905-6_8
39. Goncharuk V., Dubrovin I., Dubrovina L., Kucheruk D., Naboka O., Ogenko V. Synthesis of Carbon-Silica Nanomaterials by Carbonization of Cellulose Acetate and Polyisocyanate Copolymer. Phys. Chem. Solid State. 2016. 17(2): 241. https://doi.org/10.15330/pcss.17.2.241-246
40. Dzyazko Y.S., Rozhdestvenskaya L.M., Vasilyuk S.L., Belyakov V.N. Electro-deionization of Cr(VI)-Containing Solution. Part I. Chem. Eng. Commun. 2008. 196(1): 3. https://doi.org/10.1080/00986440802303681
41. Dar W., Cord-Ruwisch R., Charles W. Ethanol and lactic acid production from sugar and starch wastes by anaerobic acidification. Eng. Life Sci. 2018. 18(9): 635. https://doi.org/10.1002/elsc.201700178
42. Manso T., Lores M., de Miguel T. Antimicrobial activity of polyphenols and natural polyphenolic extracts on clinical isolates. Antibiotics. 2022. 11(1): 46. https://doi.org/10.3390/antibiotics11010046
43. Mandal M.K., Domb A.J. Antimicrobial activities of natural bioactive polyphenols. Pharmaceutics. 2024. 16(6): 718. https://doi.org/10.3390/pharmaceutics16060718
44. Liu Y., Benohoud M., Galani Yamdeu J.H., Gong Y.Y., Orfila C. Green extraction of polyphenols from citrus peel by-products and their antifungal activity against Aspergillus flavus. Food Chem.: X. 2021. 12: 100144. https://doi.org/10.1016/j.fochx.2021.100144
45. Haida Z., Ab Ghani S., Juju Nakasha J., Hakiman M. Determination of experimental domain factors of polyphenols, phenolic acids and flavonoids of lemon (Citrus limon) peel using two-level factorial design. Saudi J. Biol. Sci. 2022. 29(1): 574. https://doi.org/10.1016/j.sjbs.2021.09.022
46. Sharma A., Bhardwaj P., Arya S.K. Naringin: a potential natural product in the field of biomedical applications. Carbohydr. Polym. Technol. Appl. 2021. 2: 100068. https://doi.org/10.1016/j.carpta.2021.100068
47. Yao L., Liu W., Bashir M., Nisar M.F., Wan C. Eriocitrin: a review of pharmacological effects. Biomed. Pharmacother. 2022. 154: 113563. https://doi.org/10.1016/j.biopha.2022.113563
48. Mba O.I., Kwofie E.M., Ngadi M. Kinetic modelling of polyphenol degradation during common beans soaking and cooking. Heliyon. 2019. 5(5): e01613. https://doi.org/10.1016/j.heliyon.2019.e01613
49. Dzah C.S., Duan Y., Zhang H., Serwah Boateng N.A., Ma H. Latest developments in polyphenol recovery and purification from plant by-products: A review. Trends Food Sci. Technol. 2020. 99: 375. https://doi.org/10.1016/j.tifs.2020.03.003
50. Mulder M. Basic principles of membrane technology. (Dordrecht: Kluwer Academic Publishers, 1996). https://doi.org/10.1007/978-94-009-1766-8
51. Para?so C.M., Madrona G.S., Pizzo J.S., Santos L.C., Oliveira A.C., Silva M.A.A., Silva M.A.A., Oliveira R.A. Intensified ultrafiltration process for fouling mitigation during concentration of bioactive compounds from hibiscus (Hibiscus sabdariffa L.) extract: innovation by using ultrasound and 3D turbulence promoters. Chem. Eng. Process. Process Intensif. 2023. 180: 109612. https://doi.org/10.1016/j.cep.2023.109612
52. Conidi C., Drioli E., Cassano A. Membrane-based agro-food production processes for polyphenol separation, purification and concentration. Curr. Opin. Food Sci. 2018. 23: 7. https://doi.org/10.1016/j.cofs.2017.10.009
53. Castro-Mu?oz R., Y??ez-Fern?ndez J., F?la V. Phenolic compounds recovered from agro-food by-products using membrane technologies: an overview. Food Chem. 2016. 213: 753. https://doi.org/10.1016/j.foodchem.2016.07.030
54. Chen X.-M., Tait A.R., Kitts D.D. Flavonoid composition of orange peel and its association with antioxidant and anti-inflammatory activities. Food Chem. 2017. 218: 15. https://doi.org/10.1016/j.foodchem.2016.09.016
55. Omoba O.S., Obafaye R.O., Salawu S.O., Boligon A.A., Athayde M.L. HPLC-DAD phenolic characterization and antioxidant activities of ripe and unripe sweet orange peels. Antioxidants. 2015. 4(3): 498. https://doi.org/10.3390/antiox4030498
56. Gao H., Zhong S., Dangayach R., Chen Y. Understanding and designing a high-performance ultrafiltration membrane using machine learning. Environ. Sci. Technol. 2023. 57(46): 17831. https://doi.org/10.1021/acs.est.2c05404
57. Dzyazko Y.S., Rozhdestvenska L.M., Kudelko K.O., Ponomaryova L.M., Shteinberg L.Ya., Yatsenko T.V. Polymer-inorganic membranes for removal of pesticides from water using pressure-driven technique. Himia, Fizika ta Tehnologia Poverhni. 2024. 15(4): 534. https://doi.org/10.15407/hftp15.04.534
58. Bilad M.R., Junaeda S.R., Khery Y., Nufida B.A., Shamsuddin N., Usman A., Violet V. Compaction of a polymeric membrane in ultra-low-pressure water filtration. Polymers. 2022. 14(16): 3254. https://doi.org/10.3390/polym14163254
59. Molina L.C.A., Magalh?es-Ghiotto G.A.V., Nichi L., Dzyazko Y.S., Bergamasco R. Membranes modified with rigid polymer for processing solutions of vegetable proteins. Acta Period. Technol. 2023. 54: 313. https://doi.org/10.2298/APT2354313M
60. Bildyukevich A.V., Plisko T.V., Shustikov A.A., Dzyazko Yu.S., Rozhdestvenska L.M., Pratsenko S.A. Effect of the solvent nature on the structure and performance of poly(amide-imide) ultrafiltration membranes. J. Mater. Sci. 2020. 55(18): 9638. https://doi.org/10.1007/s10853-020-04714-3
61. Ho C.-C., Zydney A.L. A combined pore blockage and cake filtration model for protein fouling during microfiltration. J. Colloid Interface Sci. 2000. 232: 389. https://doi.org/10.1006/jcis.2000.7231
62. Dzyazko Yu., Rozhdestveskaya L., Zmievskii Yu., Zakharov V., Myronchuk V. Composite inorganic anion exchange membrane for electrodialytic desalination of milky whey. Mater. Today: Proc. 2019. 6(2): 250. https://doi.org/10.1016/j.matpr.2018.10.102
63. Myronchuk V., Zmievskii Y., Dzyazko Y., Rozhdestveska L., Zakharov V., Bildyukevich A. Electrodialytic whey demineralization involving polymer-inorganic membranes, anion exchange resin and graphene-containing composite. Acta Periodica Technologica. 2019. 50: 163. https://doi.org/10.2298/APT1950163M
64. Rozhdesvenska L., Kudelko K., Palchik A., Vygovska L., Ushkalov V., Chaban M., Ponomarova L. Macroporous filtration PTFE membranes modified with polymer-based nanocomposite containing zirconium hydrophosphate and silver nanoparticles. In: Proc. 14th IEEE International Conference on Nanomaterials: Applications & Properties (Sept. 8-13, 2024, Riga, Latvia) P. 1. https://doi.org/10.1109/NAP62956.2024.10739731
65. Pini Pereira P., Pacola Gon?alves I., Arnaut Braz L.V., Molina L.C.A., Dzyazko Yu.S., Ribeiro A.C., Bergamasco R. Removal of anionic dyes from lightly colored solutions with 3d printed ultrafiltration PLA membrane. Water Air and Soil Pollution. 2026. 237: 30. https://doi.org/10.1007/s11270-025-08731-3
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Copyright (c) 2026 П. Піні Перейра, I. Пакола Гонсалвес, Л.В. Арнаут Браз, Ю.С. Дзязько, К. Moзeр Парайсо, A. Maркелотти Салседо Виейра, Р. Бергамаско

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