سنتز سبز نانوذرات اکسید روی با استفاده از عصاره بره‌موم و استفاده از آن در تهیه فیلم زیست‌تخریب‌پذیر فعال بر پایه ایزوله پروتئین آب پنیر

نوع مقاله : مقاله پژوهشی

نویسندگان

بهنوش ایمانی ¹

هادی الماسی ¹

میرخلیل پیروزی فرد ¹

هیمن نوربخش ²

¹ گروه علوم و صنایع غذایی، دانشکده کشاورزی، دانشگاه ارومیه، ارومیه، ایران

² گروه علوم و مهندسی صنایع غذایی، دانشکده کشاورزی، دانشگاه کردستان، سنندج، ایران

https://doi.org/10.22067/ifstrj.2025.95130.1470

چکیده

این مطالعه با هدف سنتز سبز نانوذرات اکسید روی با استفاده از عصاره برموم و امواج فراصوت و کاربرد آن‌ها در فیلم ایزوله پروتئین آب پنیر انجام شد. نتایج مربوط به FTIR نانوذرات کاهش شدت یا حذف برخی باندهای موجود در عصاره بره‌موم را نشان داد که بیانگر شرکت این گروه‌های عاملی در فرآیند احیای یون‌های روی و پوشش‌دهی سطحی نانوذرات بود. مورفولوژی نانوذرات نیز نشان داد نمونه‌هایی که با فراصوت سنتز شده بودند مورفولوژی همگن­تری نسبت به حالت بدون فراصوت داشتند. نانوذره اکسید روی سنتز شده در غلظت 0.25 مولار نیترات روی با فراصوت به‌دلیل تراکم مناسب، شکل منظم و توزیع یکنواخت ذرات، به‌عنوان نمونه برتر انتخاب شد. این نمونه همراه با نانوذره اکسید روی سنتز شده با غلظت 0.25 مولار نیترات روی اما بدون استفاده از فراصوت به‌منظور مقایسه عملکرد آن‌ها در غلظت‌های 3، 5 و 7 درصد به فیلم ایزوله پروتئین آب پنیر اضافه و ویژگی‌های آن‌ها در مقایسه با فیلم شاهد ایزوله پروتئین آب پنیر مورد مطالعه قرارگرفت. نتایج مربوط به فیلم‌ها نشان داد که با افزایش درصد نانوذرات، درصد حلالیت و میزان نفوذپذیری به بخار آب کاهش و خاصیت آنتی‌اکسیدانی، مقاومت به کشش، ازدیاد طول و مدول یانگ به‌طور معنی‌داری افزایش یافت (0.05 >p). این افزایش در نمونه‌های حاوی نانوذرات اکسید روی سنتز شده با فراصوت بیشتر از نمونه‌های بدون فراصوت بود (0.05 >p). یافته‌های بررسی خاصیت ضدمیکروبی نیز حاکی از آن بود که باکتری گرم مثبت استافیلوکوکوس اورئوس حساسیت بیشتری به نانوذرات اکسید روی سنتز شده با عصاره بره‌موم نسبت به باکتری گرم منفی اشریشیا کلی داشت. به‌طور کلی نتایج این پژوهش نشان داد که استفاده از نانوذرات اکسید روی سنتز شده با عصاره بره‌موم با استفاده از فراصوت باعث بهبود خصوصیات فیزیکوشیمیایی و میکروبی فیلم ایزوله پروتئین آب پنیر می‌گردد و می‌توان از فیلم حاصل برای بسته‌بندی محصولات غذایی حساس به فساد میکروبی استفاده کرد.

کلیدواژه‌ها

سنتز سبز نانوذرات

عصاره بره‌موم

فیلم زیست‌تخریب‌پذیر

نانوذرات اکسید روی

موضوعات

• فناوری مواد غذایی

---

عنوان مقاله English

Green synthesis of ZnO nanoparticles by using propolis extract and its application in preparation of biodegradable active film based on whey protein isolate

نویسندگان English

Behnoush Imani ¹

Hadi Almasi ¹

Mir Khalil Pirouzifard ¹

Himan Nourbakhsh ²

¹ Department of Food Science and Technology, Faculty of Agriculture, Urmia University, Urmia, Iran

² Department of Food Science and Engineering, Faculty of Agriculture, University of Kurdistan, Sanandaj, Iran

چکیده English

Introduction
Whey protein isolate has been considered in food packaging due to its edibility, biodegradability, ability to produce transparent, colorless and odorless films and coatings, cheapness and high relative abundance, as well as high barrier to oxygen and aromatic compounds at low relative humidity. However, the poor mechanical properties of these films, such as low tensile strength, inherent stiffness and poor water vapor barrier, have limited their application. Therefore, to overcome this limitation, in this study, the use of zinc oxide nanoparticles produced by green synthesis method from propolis alcoholic extract in the production of biodegradable films based on whey protein isolate was investigated. The effect of ultrasound treatment on the green synthesis process and the characteristics of the manufactured nanoparticles were also studied.
Materials and Methods
The production of zinc oxide nanoparticles by green synthesis method was as follows: first, zinc nitrate was prepared with different concentrations of 0.075, 0.15 and 0.25 M. The alcoholic extract of propolis was slowly and dropwise added to the prepared zinc nitrate solution. The reaction was carried out on a heater stirrer at 60 °C for 5 h. The pH of the solution was adjusted to 10 during the reaction using sodium hydroxide so that after the end of mixing, a brick-colored precipitate of zinc oxide nanoparticles was observed at the bottom of the container. The precipitates were centrifuged for 10 min at 4000 rpm. After this stage, the accumulated zinc oxide precipitates were washed with distilled water to separate impurities and finally placed in an electric furnace at 350 °C for 2 h. After this time, zinc oxide nanoparticles can be obtained in a light gray to white color. In the ultrasonic method, the brick-colored solution obtained before centrifugation was subjected to ultrasonic waves in an ultrasonic bath for 15 min, and then the same procedure was followed. To prepare the alcoholic extract of propolis, 15 g of propolis was mixed with 20 mL of 99% ethanol and placed in a shaker at 180 rpm for 24 h at room temperature. The resulting solution was filtered with Whatman paper No. 1. Finally, the solvent was recovered in a rotary evaporator at 45 °C. The superior nanoparticles were then obtained to be incorporated in the films of whey protein isolate at different concentrations of 3, 5 and 7 % and the physicochemical, antioxidant and antimicrobial properties were studied.
Results and Discussion
The results of FTIR analysis of nanoparticles showed a decrease in the intensity or elimination of some bands presented in propolis extract, which indicated the participation of these functional groups in the process of zinc ion reduction and surface coating of nanoparticles. The morphology of nanoparticles also showed that the samples treated by ultrasound had a more homogeneous morphology than those without ultrasound. So, zinc oxide nanoparticles synthesized at a concentration of 0.25 M zinc nitrate with ultrasound were selected as the superior sample due to their appropriate density, regular shape and uniform distribution of particles. These particles were then added to whey protein isolate film at concentrations of 3, 5 and 7% to compare their performance and their properties in comparison with the control whey protein isolate film. The results showed that with increasing the percentage of nanoparticles, the solubility and water vapor permeability decreased and the antioxidant property, tensile strength, elongation and Young's modulus increased significantly (p < 0.05). This increase was greater in samples containing zinc oxide nanoparticles treated with ultrasound than in samples without ultrasound (p < 0.05). The findings of the antimicrobial property also indicated that the gram-positive bacterium Staphylococcus aureus was more sensitive to zinc oxide nanoparticles treated with propolis extract than the gram-negative bacterium Escherichia coli.
Conclusion
In general, the findings of this study showed that the use of zinc oxide nanoparticles synthesized with propolis extract using ultrasound improves the physicochemical and microbial properties of the whey protein isolate.
Founding Source
This research did not receive any specific grant from funding agencies in the public, commercial, or not-for-profit sectors.

کلیدواژه‌ها English

Biodegradable Film

Green Synthesis of Nanoparticles

Nanoparticles

Propolis Extract

Zinc Oxide

Authors retain the copyright. This is an open access article distributed under Creative Commons Attribution 4.0 International License (CC BY 4.0)

مراجع

1. Adame, D., & Beall, G.W. (2009). Direct measurement of the constrained polymer region in polyamide/clay nanocomposites and the implications for gas diffusion. Applied Clay Science, 42(3-4), 545-552. https://doi.org/10.1016/j.clay.2008.03.005
2. Ahmed, S., Ahmad, M., Swami, B.L., & Ikram, S. (2016).Green synthesis of silver nanoparticles using Azadirachta indica aqueous leaf extract. Journal of Radiation Research and Applied Sciences, 9(1), 1-7. https://doi.org/10.1016/j.jrras.2015.06.006
3. Almasi, H., Azizi, S., & Amjadi, S. (2020). Development and characterization of pectin films activated by nanoemulsion and Pickering emulsion stabilized marjoram (Origanum majorana ) essential oil. Food Hydrocolloids, 99, 105338. https://doi.org/10.1016/j.foodhyd.2019.105338
4. Bandeira, M., Giovanela, M., Roesch-Ely, M., Devine, D.M., & da Silva Crespo, J. (2020). Green synthesis of zinc oxide nanoparticles: A review of the synthesis methodology and mechanism of formation. Sustainable Chemistry and Pharmacy, 15, 100223. https://doi.org/10.1016/j.scp.2020.100223
5. Dash, K.K., Ali, N.A., Das, D., & Mohanta, D. (2019). Thorough evaluation of sweet potato starch and lemon-waste pectin based-edible films with nano-titania inclusions for food packaging applications. International Journal of Biological Macromolecules, 139, 449-458. https://doi.org/10.1016/j.ijbiomac. 2019.07.193
6. Dwi Ajeng, P.D., Plashintania, D.R., Putri, R.M., Wibowo, I., Ramli, Y., & Herdianto, S. (2023). Synthesis of zinc oxide nanoparticles using methanol propolis extract (Pro-ZnO NPs) as antidiabetic and antioxidant. PLoS ONE, 18(7), e0289125. https://doi.org/10.1371/journal. pone.0289125
7. Emamifar, A., Kadivar, M., Shahedi, M., & Soleimanian-Zad, S. (2011). Effect of nanocomposite packaging containing Ag and ZnO on inactivation of Lactobacillus plantarum in orange juice. Food Control, 22(3-4), 408-413. https://doi.org/10.1016/j.foodcont.2010.09.011
8. Fernandes, F.F., Dias, A.L.T., Ramos, C.L., Ikegaki, M., Siqueira, A.M.D., & Franco, M.C. (2007). The" in vitro" antifungal activity evaluation of propolis G12 ethanol extract on Cryptococcus neoformans. Revista do Instituto de Medicina Tropical de São Paulo, 49, 93-95. https://doi.org/10.1590/S0036-46652007000200005
9. Ghadetaj, A., Almasi, H., & Mehryar, L. (2018). Development and characterization of whey protein isolate active films containing nanoemulsions of Grammosciadium ptrocarpum essential oil. Food Packaging and Shelf Life, 16, 31-40. https://doi.org/10.1016/j.fpsl.2018.01.012
10. Ghafoori Ahangar, Z., Pourashouri, P., Ojagh, S.M., & Shabanpour, B. (2018). The assessment of of bilayer agar-sodium caseinat film properties containing ZnO nanoparticles. Journal of Utilization and Cultivation of Aquatics, 7(2), 41-51. (In Persian with English abstract)
11. Ghanbarzadeh, B., Pezeshki Najafabadi, A., & Almasi, H. (2011). Antimicrobial edible films for food packaging. (In Persian with English abstract)
12. Ghramh, H.A., Khan, K.A., Ibrahim, E.H., & Ansari, M.J. (2019). Biogenic synthesis of silver nanoparticles using propolis extract, their characterization, and biological activities. Science of Advanced Materials, 11(6), 876-883. https://doi.org/10.1166/sam.2019.3571
13. Jafari, H., Pirouzifard, M., Khaledabad, M.A., & Almasi, H. (2016). Effect of chitin nanofiber on the morphological and physical properties of chitosan/silver nanoparticle bionanocomposite films. International Journal of Biological Macromolecules, 92, 461-466. https://doi.org/10.1016/j.ijbiomac.2016.07.051
14. Kanmani, P., & Rhim, J.-W. (2014). Properties and characterization of bionanocomposite films prepared with various biopolymers and ZnO nanoparticles. Carbohydrate Polymers, 106, 190-199. https://doi.org/10.1016/j.carbpol.2014.02.007
15. Li, H., Li, F., Wang, L., Sheng, J., Xin, Z., Zhao, L., Hu, Q. (2009). Effect of nano-packing on preservation quality of Chinese jujube (Ziziphus jujuba var. inermis (Bunge) Rehd). Food Chemistry, 114(2), 547-552. https://doi.org/10.1016/j.foodchem.2008.09.085
16. Li, X., Zhang, F., Ma, C., Deng, Y., Wang, Z., Elingarami, S., & He, N. (2012). Controllable synthesis of ZnO with various morphologies by hydrothermal method. Journal of Nanoscience and Nanotechnology, 12(3), 2028-2036. https://doi.org/10.1166/jnn.2012.5177
17. Manjamadha, V., & Muthukumar, K. (2016). Ultrasound assisted green synthesis of silver nanoparticles using weed plant. Bioprocess and Biosystems Engineering, 39(3), 401-411. https://doi.org/10.1007/s00449-015-1523-3
18. Marvizadeh, M.M., Mohammadi Nafchi, A., & Jokar, M. (2014). Improved physicochemical properties of tapioca starch/bovine gelatin biodegradable films with zinc oxide nanorod. Journal of Chemical Health Risks, 4(4), 25-31. (In Persian with English abstract). https://doi.org/10.1016/j.ijbiomac.2017.02.067
19. Mocanu, A., Isopencu, G., Busuioc, C., Popa, -M., Dietrich, P., & Socaciu-Siebert, L. (2019). Bacterial cellulose films with ZnO nanoparticles and propolis extracts: Synergistic antimicrobial effect. Scientific Reports, 9(1), 17687. https://doi.org/10.1038/s41598-019-54118-w
20. Munoz, V.A., Ferrari, G.V., Sancho, M.I., & Montaña, M.P. (2016). Spectroscopic and thermodynamic study of chrysin and quercetin complexes with Cu (II). Journal of Chemical & Engineering Data, 61(2), 987-995. https://doi.org/10.1021/acs.jced.5b00837
21. Nabavi, M., Esmaiili, M., & Ghaitaranpour, A. (2025). Lallemantia royleana seed mucilage-based active edible films: The effects of zinc oxide nanoparticles and zoulang plant’s essential oil. Journal of Food Science & Technology (2008-8787), 21(160). (In Persian with English abstract). https://doi.org/10.22034/FSCT.22.160.110
22. Nafchi, A.M., Mahmud, S., & Robal, M. (2012). Antimicrobial, rheological, and physicochemical properties of sago starch films filled with nanorod-rich zinc oxide. Journal of Food Engineering, 113(4), 511-519. https://doi.org/10.1016/j.jfoodeng.2012.07.017
23. Ojagh, S.M., Adeli, A., Abdollahi, M., Kazemi, M., & Habibi, M. (2017). Effect of ZnO nanoparticles on the physico-mechanical properties of agar/kappa carrageenan bilayer film. Innovative Food Technologies, 5(1), 13-23. (In Persian with English abstract). https://doi.org/10.1016/j.lwt.2016.03.011
24. Osman, M.S., Al-qubati, M., Saeed, M., Abdulqawi, N., Algradee, M.A., Alwan, A., & Sultan, A.M. (2023). Effective inhibition of waterborne and fungal pathogens using ZnO nanoparticles prepared from an aqueous extract of propolis: Optimum biosynthesis, characterization, and antimicrobial activity. Applied Nanoscience, 13(6), 4515-4526. https://doi.org/10.1007/s13204-022-02726-w
25. PP, V. (2020). In vitro biocompatibility and antimicrobial activities of zinc oxide nanoparticles (ZnO NPs) prepared by chemical and green synthetic route—a comparative study. BioNanoScience, 10(1), 112-121. https://doi.org/10.1007/s12668-019-00698-w
26. Rafiee, B., Ghani, S., Sadeghi, D., & Ahsani, M. (2018). Green synthesis of zinc oxide nanoparticles using eucalyptus mellidora leaf extract and evaluation of its antimicrobial effects. Journal of Babol University of Medical Sciences, 20(10), 28-35. (In Persian with English abstract)
27. Rajakumar, G., Thiruvengadam, M., Mydhili, G., Gomathi, T., & Chung, I.-M. (2018). Green approach for synthesis of zinc oxide nanoparticles from Andrographis paniculata leaf extract and evaluation of their antioxidant, anti-diabetic, and anti-inflammatory activities. Bioprocess and Biosystems Engineering, 41, 21-30. https://doi.org/10.1007/s00449-017-1840-9
28. Rešček, A., Kratofil Krehula, L., Katančić, Z., & Hrnjak-Murgić, Z. (2015). Active bilayer PE/PCL films for food packaging modified with zinc oxide and casein. Croatica Chemica Acta, 88(4), 461-473. https://doi.org/10.5562/cca2768
29. Rezaei, M., Pirsa, S., & Chavoshizadeh, S. (2020). Photocatalytic/antimicrobial active film based on wheat gluten/ZnO nanoparticles. Journal of Inorganic and Organometallic Polymers and Materials, 30(7), 2654-2665. https://doi.org/10.1007/s10904-019-01407-6
30. Sabet, B.J.P., Mahdavi-Ourtakand, M., & Baghbani-Arani, F. (2022). Green synthesis of zinc oxide nanoparticles by Zataria multiflora extract and evaluation of its antimicrobial, cytotoxic and apoptotic effects on HT-29 cell line. (In Persian with English abstract). https://doi.org/10.1007/s42247-022-00413-8
31. Saha, S.K., Chowdhury, P., Saini, P., & Babu, S.P.S. (2014). Ultrasound assisted green synthesis of poly (vinyl alcohol) capped silver nanoparticles for the study of its antifilarial efficacy. Applied Surface Science, 288, 625-632. https://doi.org/10.1016/j.apsusc.2013.10.085
32. Salama, S.A., Essam, D., Tagyan, A.I., Farghali, A.A., Khalil, E.M., Abdelaleim, Y.F., Eweis, A.A. (2024). Novel composite of nano zinc oxide and nano propolis as antibiotic for antibiotic-resistant bacteria: a promising approach. Scientific Reports, 14(1), 20894. https://doi.org/10.1038/s41598-024-70490-8
33. Sanaeimehr, Z., Javadi, I., & Namvar, F. (2018). Antiangiogenic and antiapoptotic effects of green-synthesized zinc oxide nanoparticles using Sargassum muticum algae extraction. Cancer Nanotechnology, 9(1), 3. https://doi.org/10.1186/s12645-018-0037-5
34. Shah, M., Fawcett, D., Sharma, S., Tripathy, S.K., & Poinern, G.E.J. (2015). Green synthesis of metallic nanoparticles via biological entities. Materials, 8(11), 7278-7308. https://doi.org/10.3390/ma8115377
35. Shahab-Navaei, F., & Asoodeh, A. (2023). Synthesis of optimized propolis solid lipid nanoparticles with desirable antimicrobial, antioxidant, and anti-cancer properties. Scientific Reports, 13(1), 18290. https://doi.org/10.1038/s41598-023-45768-y
36. Shankar, S.S., Rai, A., Ahmad, A., & Sastry, M. (2004). Rapid synthesis of Au, Ag, and bimetallic Au core–Ag shell nanoparticles using Neem (Azadirachta indica) leaf broth. Journal of Colloid and Interface Science, 275(2), 496-502. https://doi.org/10.1016/j.jcis.2004.03.003
37. Sharma, N., Jandaik, S., & Kumar, S. (2016). Synergistic activity of doped zinc oxide nanoparticles with antibiotics: ciprofloxacin, ampicillin, fluconazole and amphotericin B against pathogenic microorganisms. Anais da Academia Brasileira de Ciências, 88(3 Suppl), 1689-1698. https://doi.org/10.1590/0001-3765201620150713
38. Sherafatkhah Azari, S., Alizadeh, A., Asefi, N., & Hamishehkar, H. (2021). Investigation the effect of ZnO and β-glucan on chemical and microbial characteristic of gelatin based biodegradable film over storage of chicken fillet. Journal of Food Science and Technology (Iran), 18(114), 169-180. (In Persian with English abstract). https://org/10.52547/fsct.18.114.169
39. Soleimani-Gorgani, A., & Alborz, R. (2020). Green synthesis of nanoparticles for using as antibacterial materials. Journal of Biosafety, 13(1), 23-44. (In Persian). DOR: 20.1001.1.27170632.1399.13.1.3.3
40. Sulaiman, A.Z., Ajit, A., Yunus, R.M., & Chisti, Y. (2011). Ultrasound-assisted fermentation enhances bioethanol productivity. Biochemical Engineering Journal, 54(3), 141-150. https://doi.org/10.1016/j.bej. 2011.01.006
41. Taherian, S.M.R., Hosseini, S.A., Jafari, A., & Etminan, A. (2019). The green synthesis and characterization of Zinc Oxide nanoparticles from the leaf extracts of Satureja hortensis. Herbal Medicines Journal, 3(4), 147-153. https://doi.org/10.4194/1303-2712-v20_6_06
42. Tunç, S., & Duman, O. (2010). Preparation and characterization of biodegradable methyl cellulose/montmorillonite nanocomposite films. Applied Clay Science, 48(3), 414-424. https://doi.org/10.1016/j.clay.2010.01.016
43. Yu, J., Yang, J., Liu, B., & Ma, X. (2009). Preparation and characterization of glycerol plasticized-pea starch/ZnO–carboxymethylcellulose sodium nanocomposites. Bioresource Technology, 100(11), 2832-2841. https://doi.org/10.1016/j.biortech.2008.12.045
44. Zhang, L., Jiang, Y., Ding, Y., Daskalakis, N., Jeuken, L., Povey, M., York, D.W. (2010). Mechanistic investigation into antibacterial behaviour of suspensions of ZnO nanoparticles against coli. Journal of Nanoparticle Research, 12(5), 1625-1636. https://doi.org/10.1007/s11051-009-9711-1
45. Zhang, L., Jiang, Y., Ding, Y., Povey, M., & York, D. (2007). Investigation into the antibacterial behaviour of suspensions of ZnO nanoparticles (ZnO nanofluids). Journal of Nanoparticle Research, 9, 479-489. https://doi.org/10.1007/s11051-006-9150-1