An application of CoFe2O4/alginate magnetic beads: drug delivery system of 5-fluorouracil

Öz

Magnetic hyperthermia therapy is expected to play an important role in the treatment of more and more cancers. The synergistic effects of using together hyperthermia and cancer drugs have been shown by literature studies to be more effective than either hyperthermia treatment alone or chemotherapy alone. In addition, magnetic materials that can be used as a contrast agent enable magnetic resonance imaging of the tumor, which is also useful in seeing the treatment progress. This study, which was designed for this purpose, occurred in three parts: In the first part, magnetic CoFe2O4/alginate composite beads were prepared and characterized with thermogravimetric analysis (TGA) and scanning electron microscope (SEM). In the second part, the swelling behaviour of magnetic composite beads was investigated at pH 1.2, pH 7.4 and pH 6.8. It was seen that at pH 7.4 and pH 6.8, that is, near neutral pH, CFA swelled by 81.54% and 82.69%, respectively. In the third part, 5-Fluorouracil was encapsulated at the different ratios in CoFe2O4/alginate composite beads, and release experiments were performed at pH 1.2, pH 7.4 and pH 6.8. 5-FU release was calculated with Korsmeyer-Peppas, Higuchi, first-order, and zero-order models. It was seen that the drug release systems prepared were suitable for all kinetic models. Magnetic CoFe2O4/alginate composite bead, which is the drug carrier, was determined to be suitable for controlled release for 5-Fluorouracil.

Anahtar Kelimeler

• Drug release
• Cancer drug
• Polymer
• Magnetic particles
• Hyperthermia

References

1. Amini-Fazl, M.S., Mohammadi, R., & Kheiri, K. (2019). 5 Fluorouracil loaded chitosan/polyacrylic acid/Fe3O4 magnetic nanocomposite hydrogel as a potential anticancer drug delivery system. International Journal of Biological Macromolecules, 132, 506 513. https://doi.org/10.1016/j.ijbiomac.2019.04.005
2. Amiri, M., Akbari, A., Ahmadi, M., & Pardakhti, A.M. (2018). Synthesis and in vitro evaluation of a novel magnetic drug delivery system; proecological method for the preparation of CoFe2O4 nanostructures. Journal of Molecular Liquids, 249, 1151 1160. https://doi.org/ 10.1016/j.molliq.2017.11.133
3. Amiri, M., Salavati-Niasari, M., Pardakhty, A., Ahmadi, M., & Akbari, A. (2017). Caffeine: A novel green precursor for synthesis of magnetic CoFe2O4 nanoparticles and pH-sensitive magnetic alginate beads for drug delivery, Materials Science and Engineering: C, 76, 1085-1093. https://doi.org/10.1016/j.msec.2017.03.208
4. Anirudhan, T.S., & Christa, J. (2018). pH and magnetic field sensitive folic acid conjugated protein–polyelectrolyte complex for the controlled and targeted delivery of 5-fluorouracil. Journal of Industrial and Engineering Chemistry, 57, 199 207. https://doi.org/10.1016/j.jiec.2017.08.024
5. Arami, H., Khandhar, A., Liggitt, D., & Krishnan, K.M. (2015). In Vivo Delivery, Pharmacokinetics, biodistribution and toxicity of Iron Oxide nanoparticles. Chemical Society Reviews, 44, 8576−8607. https://doi.org/10.1039/C5CS00541H
6. Chang, C., & Zhang, L. (2011). Cellulose-based hydrogels: present status and application prospects. Carbohydrate Polymers,84, 40 53. https://doi.org/10.1016/j.carbpol.2010.12.023
7. Chen, F.H., Zhang, L.M., Chen, Q.T., Zhang, Y., & Zhang, Z.J. (2010). Synthesis of a novel magnetic drug delivery system composed of doxorubicin-conjugated Fe3O4 nanoparticle cores and a PEG-functionalized porous silica shell. Chemical Communications, 46(45), 8633-8635. https://doi.org/10.1039/C0CC02577A
8. Chen, X., Fan, M., Tan, H., Ren, B., Yuan, G., Jia, Y., & Hu, X. (2019). Magnetic and self-healing chitosan-alginate hydrogel encapsulated gelatin microspheres via covalent cross-linking for drug delivery. Materials Science and Engineering: C, 101, 619 629. https://doi.org/10.1016/j.msec.2019.04.012

9. Dai, Y., Li, P., Zhang, J., Wang, A., & Wei, Q. (2008). Swelling Characteristics and Drug Delivery Properties of Nifedipine-Loaded pH Sensitive Alginate–Chitosan Hydrogel Beads. Journal of Biomedical Materials Research Part B: Applied Biomaterials, 86, 493 500. https://doi.org/10.1002/jbm.b.31046
10. Dhiman, P., Mehta, T., Kumar, A., Sharma, G., Naushad, M., Ahamad, T., & Mola, G.T. (2020). Mg0. 5NixZn0. 5-xFe2O4 spinel as a sustainable magnetic nano-photocatalyst with dopant driven band shifting and reduced recombination for visible and solar degradation of Reactive Blue 19. Advanced Powder Technology, 31(12), 4585 4597. https://doi.org/10.1016/j.apt.2020.10.010
11. Doğaç, Y.İ., & Teke, M. (2021). Urease immobilized core–shell magnetic Fe [NiFe]O4/alginate and Fe3O4/alginate composite beads with improved enzymatic stability properties: removal of artificial blood serum urea. Journal of the Iranian Chemical Society, 18(10), 2637 2648, https://doi.org/10.1007/s13738-021-02219-7
12. Doğaç, Y.İ., Çınar, M., & Teke, M. (2015). Improving of catalase stability properties by encapsulation in alginate/Fe3O4 magnetic composite beads for enzymatic removal of H2O2. Preparative Biochemistry & Biotechnology, 45(2), 144 157. https://doi.org/ 10.1080/10826068.2014.907178
13. Fan, W., Yung, B., Huang, P., & Chen X. (2017). Nanotechnology for multimodal synergistic cancer therapy, Chemical Reviews, 117, 13566 13638. https://doi.org/10.1021/acs.chemrev. 7b00258
14. Fomina, M., & Gadd, G.M. (2014). Biosorption: Current perspectives on concept, definition and application. Bioresource Technology, 160, 3 14. https://doi.org/10.1016/j.biortech.2013.12.102
15. Gaharwar, A.K., Peppas, N.A. & Khademhosseini, A. (2014). Nanocomposite hydrogels for biomedical applications. Biotechnology and Bioengineering, 111, 441 453. https://doi.org/ 10.1002/bit.25160
16. Ganguly, S., & Margel, S. (2021). Design of Magnetic Hydrogels for Hyperthermia and Drug Delivery. Polymers, 13(23), 4259. https://doi.org/10.3390/polym13234259
17. Gong, L, Yan, L., Zhou, R., Xie, J., Wu, W., & Gu, Z. (2017). Two-dimensional transition metal dichalcogenide nanomaterials for combination cancer therapy, Journal of Materials Chemistry B, 5, 1873-1895. https://doi.org/10.1039/C7TB00195A
18. Hariharan, M.S., Sivaraj, R., Ponsubha, S., Jagadeesh, R., & Enoch, I.V.M.V. (2019). 5-Fluorouracil-loaded β-cyclodextrin-carrying polymeric poly (methylmethacrylate)-coated samarium ferrite nanoparticles and their anticancer activity. Journal of Materials Science, 54(6), 4942-4951. https://doi.org/10.1007/s10853-018-3161-z
19. Higuchi T. (1963). Mechanism of sustained‐action medication. Theoretical analysis of rate of release of solid drugs dispersed in solid matrices. Journal of Pharmaceutical Sciences, 52(12), 1145-49. https://doi.org/10.1002/jps.2600521210
20. Hu, X., Wang, Y., Zhang, L., Xu, M., Zhang, J., & Dong, W. (2018). Design of a pH-sensitive magnetic composite hydrogel based on salecan graft copolymer and Fe3O4@ SiO2 nanoparticles as drug carrier. International Journal of Biological Macromolecules, 107, 1811 1820. https://doi.org/10.1016/j.ijbiomac.2017.10.043
21. Huang, Y., He, S., Cao, W., Cai, K., & Liang, X.J. (2012). Biomedical nanomaterials for imaging guided cancer therapy, Nanoscale, 4(20), 6135 49. https://doi.org/10.1039/C2NR31715J
22. Ito, A., Matsuoka, F., Honda, H., & Kobayashi, T. (2003). Heat shock protein 70 gene therapy combined with hyperthermia using magnetic nanoparticles. Cancer Gene Therapy, 10(12), 918-25. https://doi.org/10.1038/sj.cgt.7700648
23. Jahanban-Esfahlan, R., Derakhshankhah, H., Haghshenas, B., Massoumi, B., Abbasian, M., & Jaymand, M. (2020). A bio-inspired magnetic natural hydrogel containing gelatin and alginate as a drug delivery system for cancer chemotherapy. International Journal of Biological Macromolecules, 156, 438-445. https://doi.org/10.1016/j.ijbiomac.2020.04.074
24. Kayal, S., & Ramanujan, R.V. (2010). Doxorubicin loaded PVA coated iron oxide nanoparticles for targeted drug delivery. Materials Science and Engineering: C, 30(3), 484 90. https://doi.org/10.1016/j.msec.2010.01.006
25. Kitazawa, S., Johno, I., Minouchi, T., & Okada, J. (1977). Interpretation of dissolution rate data from in vitro testing of compressed tablets. Journal of Pharmacy and Pharmacology, 29(1), 453-459. https://doi.org/10.1111/j.2042-7158.1977.tb11368.x
26. Korsmeyer, R.W., & Peppas, N.A. (1983). Controlled release delivery systems. TJ Roseman and SZ Mansdorf, M. Dekker, New York, 77-90.
27. Köseoğlu, Y. (2013). Structural, magnetic, electrical and dielectric properties of MnxNi1− xFe2O4 spinel nanoferrites prepared by PEG assisted hydrothermal method. Ceramics International, 39(4), 4221-4230. https://doi.org/10.1016/j.ceramint.2012.11.004
28. Kumar C.S.S.R., & Mohammad F., (2011). Magnetic nanomaterials for hyperthermia-based therapy and controlled drug delivery. Advanced Drug Delivery Reviews, 63(9), 789-808. https://doi.org/10.1016/j.addr.2011.03.008
29. Lal, G., Punia, K., Dolia, S.N., Alvi, P.A., Choudhary, B.L., & Kumar, S. (2020). Structural, cation distribution, optical and magnetic properties of quaternary Co0. 4+ xZn0. 6-xFe2O4 (x= 0.0, 0.1 and 0.2) and Li doped quinary Co0. 4+ xZn0. 5-xLi0. 1Fe2O4 (x= 0.0, 0.05 and 0.1) nanoferrites. Journal of Alloys and Compounds, 828, 154388. https://doi.org/10.1016/j.jallcom.2020.154388
30. Lartigue, L., Alloyeau, D., Kolosnjaj-Tabi, J., Javed, Y., Guardia, P., Riedinger, A., Pechoux, C., Pellegrino, T., Wilhelm, C., Gazeau, F. (2013). Biodegradation of Iron Oxide nanocubes: High resolution in situ monitoring. ACS Nano, 7, 3939−3952. https://doi.org/10.1021/nn305719y
31. Laurent, S., Dutz, S., Häfeli U.O., & Mahmoudi, M. (2011) Magnetic fluid hyperthermia: focuson superparamagnetic iron oxide nanoparticles. Advances in Colloid and Interface science, 166, 8-23. https://doi.org/10.1016/j.cis.2011.04.003
32. Luo, L., Shu, R., & Wu, A., (2017). Nanomaterial-based cancer immunotherapy. Journal of Materials Chemistry B, 5, 5517-5531. https://doi.org/10.1016/j.cis.2011.04.003
33. Osterrieth, J.W., & Fairen‐Jimenez, D. (2021). Metal–organic framework composites for theragnostics and drug delivery applications. Biotechnology Journal, 16(2), 2000005. https://doi.org/10.1002/biot.202000005
34. Pooresmaeil, M., Javanbakht, S., Nia, S.B., & Namazi, H., (2020). Carboxymethyl cellulose/mesoporous magnetic graphene oxide as a safe and sustained ibuprofen delivery bio-system: Synthesis, characterization, and study of drug release kinetic. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 594, 124662. https://doi.org/10.1016/j.colsurfa.2020.124662
35. Prasad, N.K., Rathinasamy, K., Panda, D., & Bahadur, D., (2007). Mechanism of cell death induced by magnetic hyperthermia with nanoparticles of γ-MnxFe2–xO3 synthesizedby a single step process. Journal of Materials Chemistry, 48, 5042 5051. https://doi.org/10.1039/B708156A
36. Ramakrishna, K.S., Srinivas, C., Meena, S.S., Tirupanyam, B.V., Bhatt, P., Yusuf, S.M., & Sastry, D.L. (2017). Investigation of cation distribution and magnetocrystalline anisotropy of NixCu0. 1Zn0. 9− xFe2O4 nanoferrites: role of constant mole percent of Cu2+ dopant in place of Zn2+. Ceramics International, 43(11), 7984 7991. https://doi.org/10.1016/j.ceramint.2017.03.078
37. Reddy, M.P., Mohamed, A.M.A., Zhou, X.B., Du, S., & Huang, Q., (2015). A facile hydrothermal synthesis, characterization and magnetic properties of mesoporous CoFe2O4 nanospheres. Journal of Magnetism and Magnetic Materials, 388, 40-4. https://doi.org/ 10.1016/j.jmmm.2015.04.009
38. Ribeiro, M., Boudoukhani, M., Belmonte-Reche, E., Genicio, N., Sillankorva, S., Gallo, J., & Bañobre-López, M. (2021). Xanthan-Fe3O4 Nanoparticle Composite Hydrogels for Non-Invasive Magnetic Resonance Imaging and Magnetically Assisted Drug Delivery. ACS Applied Nano Materials, 4(8), 7712-7729. https://doi.org/10.1021/acsanm.1c00932
39. Salmanian, G., Hassanzadeh-Tabrizi, S.A., & Koupaei, N. (2021). Magnetic chitosan nanocomposites for simultaneous hyperthermia and drug delivery applications: A review. International Journal of Biological Macromolecules, 184,618 635. https://doi.org/10.1016/j.ijbiomac.2021.06.108
40. Soumia, A., Adel, M., Amina, S., Bouhadjar, B., Amal, D., Farouk, Z., Abdelkader, B., & Mohamed, S., (2020). Fe3O4-alginate nanocomposite hydrogel beads material: One-pot preparation, release kinetics and antibacterial activity. International Journal of Biological Macromolecules, 145, 466-75. https://doi.org/10.1016/j.ijbiomac.2019.12.211
41. Supramaniam, J., Adnan, R., Kaus, N.H.M., & Bushra, R. (2018). Magnetic nanocellulose alginate hydrogel beads as potential drug delivery system. International Journal of Biological Macromolecules,118, 640-48. https://doi.org/10.1016/j.ijbiomac.2018.06.043
42. Varelas, C.G., Dixon, D.G., & Steiner, C. (1995). Zero-order release fromstudies. II. Dissolution of particles under conditions of rapid agitation.biphasic polymer hydrogels. Journal of Controlled Release, 34, 185–192. https://doi.org/10.1016/0168-3659(94)00085-9
43. Wan Ngah, W.S., Teong, L.C., & Hanafiah, M.A K.M. (2011). Adsorption of dyes and heavy metal ions by chitosan composites: A review. Carbohydrate Polymers, 83(4), 1446–1456. https://doi.org/10.1016/j.carbpol.2010.11.004
44. Wang, B., Gao, B., Zimmerman, A., & Lee, X. (2018). Impregnation of multiwall carbon nanotubes in alginate beads dramatically enhances their adsorptive ability to aqueous methylene blue. Chemical Engineering Research and Design, 133, 235 242. https://doi.org/10.1016/j.cherd.2018.03.026
45. Wang, B., Wan, Y., Zheng, Y., Lee, X., Liu, T., Yu, Z., & Gao, B. (2019). Alginate-based composites for environmental applications: a critical review. Critical Reviews in Environmental Science and Technology, 49(4), 318 356. https://doi.org/10.1080/10643389.2018.1547621
46. Wang, D.S., Li, J.G., Li, H.P., & Tang, F.Q. (2009). Preparation and drug releasing property of magnetic chitosan-5-fluorouracil nano-particles. Transactions of Nonferrous Metals Society of China, 19(5), 1232-1236. https://doi.org/10.1016/S1003-6326(08)60434-3
47. Wang, G., Zhao, D., Li, N., Wang, X., & Ma, Y. (2018). Drug-loaded poly (ε-caprolactone)/Fe3O4 composite microspheres for magnetic resonance imaging and controlled drug delivery. Journal of Magnetism and Magnetic Materials, 456, 316 23. https://doi.org/10.1016/j.jmmm.2018.02.053
48. Wang, Q., Liu, S., Yang, F., Gan, L., Yang, X., & Yang, Y. (2017). Magnetic alginate microspheres detected by MRI fabricated using microfluidic technique and release behavior of encapsulated dual drugs. International Journal of Nanomedicine, 12, 4335. https://doi.org/10.2147/IJN.S131249
49. Yadollahi, M., Namazi, H., & Barkhordari, S. (2014). Preparation and properties of carboxymethyl cellulose/layered double hydroxide bionanocomposite films. Carbohydrate Polymers, 108, 83-90. https://doi.org/10.1016/j.carbpol.2014.03.024
50. Yagub, M.T., Sen, T.K., Afroze, S., & Ang, H.M. (2014). Dye and its removal from aqueous solution by adsorption: A review. Advances in Colloid and Interface Science, 209, 172–184. https://doi.org/10.1016/j.cis.2014.04.002
51. Yusefi, M., Lee-Kiun, M.S., Shameli, K., Teow, S.Y., Ali, R.R., Siew, K.K., & Kuča K. (2021). 5-fluorouracil loaded magnetic cellulose bionanocomposites for potential colorectal cancer treatment. Carbohydrate Polymers, 273, 118523. https://doi.org/10.1016/j.carbpol.2021.118523
52. Zhalechin, M., Dehaghi, S. M., Najafi, M., & Moghimi, A. (2021). Magnetic polymeric core-shell as a carrier for gradual release in-vitro test drug delivery. Heliyon, 7(5), e06652. https://doi.org/10.1016/j.heliyon.2021.e06652
53. Zhao, K., Gong, P., Huang, J., Huang, Y., Wang, D., Peng, J., & Liu, Z. (2021). Fluorescence turn-off magnetic COF composite as a novel nanocarrier for drug loading and targeted delivery. Microporous and Mesoporous Materials, 311, 110713. https://doi.org/10.1016/j.micromeso.2020.110713