Abstract
In this study ciprofloxacin-loaded carboxymethyl cellulose (CMC)/ polyvinyl alcohol (PVA) cryogel systems were prepared by using low molecular weight PVA. The high degree of segmental mobility of PVA molecules makes them more prone to form CMC/PVA cryogels via hydrogen bondings with CMC. Physically crosslinked gels were characterised by using Fourier-transform infrared spectroscopy (FTIR). Swelling results have shown that low molecular weight PVA had a fast-swelling rate and this can explain the fast release of ciprofloxacin within 30 min from CMC/PVA cryogels during release studies. Release of ciprofloxacin from the CMC/PVA cryogel system was the best fit to first-order release model with R2 = 0.9980. It was found that the release exponent is lower than 0.45 and it is a good indication of quasi-Fickian diffusion, which means that ciprofloxacin can be released without swelling of the cryogel. Ciprofloxacin was found to have even better antimicrobial activity against E. coli than positive control as having a higher inhibition zone. In addition, CMC/PVA cryogels can be used for water treatment application to remove Methylene Blue (MB) dye from water and this was supported by adsorption kinetics and isotherm studies.
Similar content being viewed by others
REFERENCES
Bakhshpour, M., Idil, N., Perçin, I., and Denizli, A., Biomedical applications of polymeric cryogels, Appl. Sci., 2019, vol. 9, no. 3, p. 553. https://doi.org/10.3390/app9030553
Welzel, P.B., Friedrichs, J., Grimmer, M., Vogler, S., Fruedenberg, U., and Werner C., Cryogel micromechanics unraveled by atomic force microscopy-based nanoindentation, Adv. Healthcare Mater., 2014, vol. 3, pp.1849–1853. https://doi.org/10.1002/adhm.201400102
Okay, O., and Lozinsky, V.I., Synthesis and structure−property relationships of cryogels. Polym. cryogels, 2014, vol. 263, pp. 103–157. https://doi.org/10.1007/978-3-319-05846-7_3
Adibfar, A., Hosseini, S., and Baghaban Eslaminejad, M., Smart polymeric systems: A biomedical viewpoint, Adv. Exp. Med. Biol., 2020, vol. 10, pp. 133–148. https://doi.org/10.1007/5584_2020_563
Chen, X., Sui, W., Ren, D., Ding, Y., Zhu, X. and Chen, Z., Synthesis of hydrophobic polymeric cryogels with supermacroporous structure, Macromol. Mater. Eng., 2016, vol. 301, pp. 659–664. https://doi.org/10.1002/mame.201500454
Oun, A.A., Rhim, and J.W., Preparation and characterization of sodium carboxymethyl cellulose/cotton linter cellulose nanofibril composite films, Carbohydr. Polym., 2015, vol. 127, pp. 101–109. https://doi.org/10.1016/j.carbpol.2015.03.073
Khiari, R., Salon, M.C.B., Mhenni, M.F., Mauret, E. and Belgacem, M.N., Synthesis and characterization of cellulose carbonate using greenchemistry: Surface modification of Avicel, Carbohydr. Polym., 2017, vol. 163, pp. 254–260. https://doi.org/10.1016/j.carbpol.2017.01.037
Baker, M.I., Walsh, S.P., Schwartz, Z., and Boyan, B.D., A review of polyvinyl alcohol and its uses in cartilage and orthopedic applications, J. Biomed. Mater. Res., Part B, 2012, vol. 100, pp. 1451–1457. https://doi.org/10.1002/jbm.b.32694
Hassan, C.M., and Peppas, N.A., Structure and applications of poly (vinyl alcohol) hydrogels produced by conventional crosslinking or by freezing/thawing methods, in Biopolymers: PVA Hydrogels, Anionic Polymerisation Nanocomposites, Advances in Polymer Science, vol. 153, Berlin: Springer, 2000, pp. 37–65. https://doi.org/10.1007/3-540-46414-X_2
Chalkley, L.J., and Koornhof, H.J., Antimicrobial activity of ciprofloxacin against Pseudomonas aeruginosa, Escherichia coli, and Staphylococcus aureus determined by the killing curve method: Antibiotic comparisons and synergistic interactions, Antimicrob. Agents Chemother., 1985, vol. 28, pp. 331–342. https://doi.org/10.1128/aac.28.2.331
Mabrouk, M., Mostafa, A.A., Oudadesse, H., Mahmoud, A.A. and El-Gohary, M.I., Effect of ciprofloxacin incorporation in PVA and PVA bioactive glass composite scaffolds, Ceram. Int., 2014, vol. 40, pp. 4833–4845. https://doi.org/10.1016/j.ceramint.2013.09.033
Ustürk, S., Altundag, E.M., and Yilmaz, E., Pullulan/polyHEMA cryogels: Synthesis, physicochemical properties, and cell viability, J. Appl. Polym. Sci., 2022, vol. 139, p. 51822. https://doi.org/10.1002/app.51822
Hezarkhani, M., Ustürk, S., Özbilenler, C., and Yilmaz, E., Pullulan/poly(N-vinylimidazole) cryogel: An efficient adsorbent for methyl orange, J. Appl. Polym. Sci., 2021, vol. 138, p. 50958. https://doi.org/10.1002/app.50958
Özbilenler, C., Altundağ, E.M. and Gazi, M., Synthesis of quercetin-encapsulated alginate beads with their antioxidant and release kinetic studies, J. Macromol. Sci., Part A, 2020, vol. 58, no. 1, pp. 22–31. https://doi.org/10.1080/10601325.2020.1817756
Mustafa, F.S., Güran, and M., Gazi, M., Effective removal of dyes from aqueous solutions using a novel antibacterial polymeric adsorbent, J. Polym. Res., 2020, vol. 27, p. 247. https://doi.org/10.1007/s10965-020-02227-w
Alokour, M., and Yilmaz, E., A polymer hybrid film based on poly(vinyl cinnamate) and poly(2-hydroxy ethyl methacrylate) for controlled flurbiprofen release, J. Polym. Res., 2021, vol. 28, p. 137. https://doi.org/10.1007/s10965-021-02493-2
Ozudogru, Y., and Tekne, E., Adsorption of Methylene Blue from aqueous solution using spent coffee/chitosan composite, J. Water Chem. Technol., 2023, vol. 45, pp. 234–245. https://doi.org/10.3103/S1063455X23030086
Benosman, A., Slimane, S.K., and Roger, P., Adsorption of anionic dye by cross-linked chitosan–polyaniline composites, J. Water Chem. Technol., 2021, vol. 43, pp. 14–21. https://doi.org/10.3103/S1063455X21010057
Ghosh, S., Qi, R., Carter, K.A., Zhang, G., Pfeifer, B.A. and Lovell, J.F., Loading and releasing ciprofloxacin in photoactivatable liposomes, Biochem. Eng. J., 2019, vol. 141, pp. 43–48. https://doi.org/10.1016/j.bej.2018.10.008
Albesa, I., Becerra, M.C., Battán, P.C., and Páez, P.L., Oxidative stress involved in the antibacterial action of different antibiotics, Biochem. Biophys. Res. Commun., 2004, vol. 317, pp. 605–609. https://doi.org/10.1016/j.bbrc.2004.03.085
Masadeh, M.M., Alzoubi, K.H., Khabour, O.F., and Al-Azzam, S.I., Ciprofloxacin-induced antibacterial activity is attenuated by phosphodiesterase inhibitors, Curr. Ther. Res., 2015, vol. 77, pp. 14–17. https://doi.org/10.1016/j.curtheres.2014.11.001
Valdes, L., Perez, I., De Ménorval, L.C., Altshuler, E., Fossum, J.O. and Rivera, A., A simple way for targeted delivery of an antibiotic: In vitro evaluation of a nanoclay-based composite, PLoS One, 2017, vol. 12, p. e0187879. https://doi.org/10.1371/journal.pone.0187879
Agarwal, R., Alam, M.S., and Gupta, B., Polyvinyl alcohol–polyethylene oxide–carboxymethyl cellulose membranes for drug delivery, J. Appl. Polym. Sci., 2013, vol. 129, pp. 3728–3736. https://doi.org/10.1002/app.39144
Parhi, R., Cross-linked hydrogel for pharmaceutical applications: A review, Adv. Pharm. Bull., 2017, vol. 7, pp. 515–530. https://doi.org/10.15171/apb.2017.064
Che Nan, N.F., Zainuddin, N., and Ahmad, M., Preparation and swelling study of CMC hydrogel as potential superabsorbent, Pertanika J. Sci. Technol., 2019, vol. 27, no. 1, pp. 489–498.
El Salmawi, K.M., Application of polyvinyl alcohol (PVA)/carboxymethyl cellulose (CMC) hydrogel produced by conventional crosslinking or by freezing and thawing, J. Macromol. Sci., Part A, 2007, vol. 44, pp. 619–624. https://doi.org/10.1080/10601320701285045
Hooper, D.C., and Jacoby, G.A., Topoisomerase inhibitors: Fluoroquinolone mechanisms of action and resistance, Cold Spring Harb. Perspect. Med., 2016, vol. 6, no. 9, p. a025320. https://doi.org/10.1101/cshperspect.a025320
Funding
This work was supported by the Eastern Mediterranean University. No additional grants to carry out or direct this particular research were obtained.
Author information
Authors and Affiliations
Corresponding authors
Ethics declarations
The authors of this work declare that they have no conflicts of interest.
Additional information
Publisher’s Note.
Allerton Press remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
İlkkan Abakan, Özbilenler, C., Ustürk, S. et al. Preparation of Carboxymethyl Cellulose/Polyvinyl Alcohol Cryogels for the Removal of Methylene Blue Dye from Aqueous Media. J. Water Chem. Technol. 46, 157–168 (2024). https://doi.org/10.3103/S1063455X24020024
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.3103/S1063455X24020024