Bacterial cellulose/polyacrylic acid (BC/PAA) pH-responsive hydrogels were prepared by free-radical polymerization ( in situ ) using BC as the raw material and AA as the monomer. The hydrogels were loaded with curcumin (Cur) to prepare pH-responsive intelligent medical dressings. The preparation process of the hydrogels was optimized by a single factor and response surface experiment using their swelling degree as an index. The structures of BC/PAA pH-responsive hydrogels were characterized by scanning electron microscope (SEM), Fourier Transform Infrared spectrometer (FTIR), X-ray diffraction (XRD), and tensile tester, and the swelling properties, mechanical properties, bacteriostatic properties, and drug release behavior were investigated. The results showed that the BC/PAA pH-responsive hydrogel has a three-dimensional network structure with the swelling rate up to 1600 g/g, compressive strength of up to 8 KPa, and good mechanical properties, and the drug release behavior was in line with the logistic dynamics model, and it has good inhibitory effects on common pathogens of wound infection: E. coli , S. aureus , and P. aeruginosa.
KeywordsBacterial CellulosePolyacrylic Acid<i>In Situ</i>PolymerizationpH-Responsive HydrogelBC/PAA-Cur Intelligent Medical Dressing
Yeo, D.C., Chew, S.W.T. and Xu, C.J. (2019) Polymeric Biomaterials for Management of Pathological Scarring. ACS Applied Polymer Materials, 1, 612-624. https://doi.org/10.1021/acsapm.8b00203
Shi, M., Zhang, H., Song, T., Liu, X.F., Gao, Y.F. and Zhou, G.H. (2019) Sustainable Dual Release of Antibiotic and Growth Factor from pH-Responsive Uniform Alginate Composite Microparticles to Enhance Wound Healing. ACS Applied Materials & Interfaces, 11, 22730-22744. https://doi.org/10.1021/acsami.9b04750
Jiang, M.Y., Ju, X.J., Lu, F., Liu, Z., Wang, W., Xie, R., Chen, Q., et al. (2014) A Novel Smart Microsphere with K+-Induced Shrinking and Aggregating Property Based on Responsive Host-Guest System. ACS Applied Materials & Interfaces, 6, 19405-19415. https://doi.org/10.1021/am505506v
Zhong, Y., Xiao, H., Seidi, F. and Jin, Y.C. (2020) Natural Polymer-Based Antimicrobial Hydrogels without Synthetic Antibiotics as Wound Dressings. Biomacromolecules, 21, 2983-3006. https://doi.org/10.1021/acs.biomac.0c00760
Xu, C., Akakuru, O.U., Ma, X.H., Zheng, J.P., Zheng, J.J. and Wu, A. (2020) Nanoparticle-Based Wound Dressing: Recent Progress in the Detection and Therapy of Bacterial Infections. Bioconjugate Chemistry, 31, 1708-1723. https://doi.org/10.1021/acs.bioconjchem.0c00297
Memic, A., Abudula, T., Mohammed, H.S., Navare, J.K. and Colombani, T. (2019) Latest Progress in Electrospun Nanofibers for Wound Healing Applications. ACS Applied Bio Materials, 2, 952-969. https://doi.org/10.1021/acsabm.8b00637
Wu, H., Li, F.Y., Shao, W., Gao, J.Q. and Ling, D.S. (2019) Promoting Angiogenesis in Oxidative Diabetic Wound Microenvironment Using a Nanozyme-Reinforced Self-Protecting Hydrogel. ACS Center Science, 5, 477-485. https://doi.org/10.1021/acscentsci.8b00850
Xie, J.B. and Hsieh, Y.-L. (2003) Thermosensitive Poly(N-Isopropylacrylamide) Hydrogels Bonded on Cellulose Supports. Journal of Applied Polymer Science, 89, 999-1006. https://doi.org/10.1002/app.12206
Shao, W., Liu, H., Liu, X.F., Wang, S.X. and Zhang, R. (2015) Anti-Bacterial Performances and Biocompatibility of Bacterial Cellulose/Graphene Oxide Composites. RSC Advances, 5, 4795-4803. https://doi.org/10.1039/C4RA13057J
Sajjad, W., He, F., Ullah, M.W., Ikre, M., Shah, S.M., Khan, T., et al. (2020) Fabrication of Bacterial Cellulose-Curcumin Nanocomposite as a Novel Dressing for Partial Thickness Skin Burn. Frontiers in Bioengineering and Biotechnology, 8, Article 553037. https://doi.org/10.3389/fbioe.2020.553037
Lee, S.E. and Park, Y.S. (2017) The Role of Bacterial Cellulose in Artificial Blood Vessels. Molecular & Cellular Toxicology, 13, 257-261. https://doi.org/10.1007/s13273-017-0028-3
Zheng, L., Li, S.S., Luo, J. and Wang, X.Y. (2020) Latest Advances on Bacterial Cellulose-Based Antibacterial Materials as Wound Dressings. Frontiers in Bioengineering and Biotechnology, 8, Article 593768. https://doi.org/10.3389/fbioe.2020.593768
Jalababu, R., Satya, S., Veni, S. and Reddy, K.V.N.S. (2019) Development, Characterization, Swelling, and Network Parameters of Amino Acid Grafted Guar Gum Based pH Responsive Polymeric Hydrogels. International Journal of Polymer Analysis and Characterization, 24, 304-312. https://doi.org/10.1080/1023666X.2019.1594058
Mao, L., Wang, L., Zhang, Y.M., Ullah, W.M., Zhao, W.W. and Li, Y. (2021) In Situ Synthesized Selenium Nanoparticles-Decorated Bacterial Cellulose/Gelatin Hydrogel with Enhanced Antibacterial, Antioxidant, and Anti-Inflammatory Capabilities for Facilitating Skin Wound Healing. Advanced Healthcare Materials, 10, e2100402. https://doi.org/10.1002/adhm.202100402
Zhang, Z.Y., Sun, Y., Zheng, Y.D., He, W., Yang, Y.Y., Xie, J.Y., et al. (2020) A Biocompatible Bacterial Cellulose/Tannic Acid Composite with Antibacterial and Anti-Biofilm Activities for Biomedical Applications. Materials Science Engineering: C, 106, Article ID: 110249. https://doi.org/10.1016/j.msec.2019.110249
Ahmad, N., Amin, M.C., Mahali, S.M., Ismail, I. and Chuang, G.T.V. (2014) Biocompatible and Mucoadhesive Bacterial Cellulose-g-Poly(Acrylic Acid) Hydrogels for Oral Protein Delivery. Molecular Pharmaceutics, 11, 4130-4143. https://doi.org/10.1021/mp5003015
Zhang, H., Tang, N., Yu, X., Guo, Z.K., Liu, Z. and Sun, X.M. (2022) Natural Glycyrrhizic Acid-Tailored Hydrogel with In-Situ Gradient Reduction of AgNPs Layer as High-Performance, Multi-Functional, Sustainable Flexible Sensors. Chemical Engineering Journal, 430, Article ID: 132779. https://doi.org/10.1016/j.cej.2021.132779
Napavichayanun, S., Ampawong, S., Harnsilpong, T., Angspatt, A., Aramwit, P. (2018) Inflammatory Reaction, Clinical Efficacy, and Safety of Bacterial Cellulose Wound Dressing Containing Silk Sericin and Polyhexamethylene Biguanide for Wound Treatment. Archives of Dermatological Research, 310, 795-805. https://doi.org/10.1007/s00403-018-1871-3
Rueda, J.C., Suarez, C., Komber, H., Zschoche, S. and Voit, B. (2020) Synthesis and Characterization of pH- and Thermo-Responsive Hydrogels Based on Poly(2-Cyclopropyl-2-Oxazoline) Macromonomer, Sodium Acrylate, and Acrylamide. Polymer Bulletin, 77, 5553-5565. https://doi.org/10.1007/s00289-019-03034-0
Warune, T., Jate, P. and Sayant, S. (2019) Novel Biodegradable Hydrogel Based on Natural Polymers: Synthesis, Characterization Swelling/Reswelling and Biodegradability. European Polymer Journal, 112, 678-687. https://doi.org/10.1016/j.eurpolymj.2018.10.033
Cristiane, S., Francisco, H.A.R., Antonio, G.B.P., André, R.F., Adley, F.R. and Edvani, C.M. (2012) Superabsorbent Hydrogel Composite Made of Cellulose Nanofibrils and Chitosan-Graft-Poly(Acrylic Acid). Carbohydrate Polymers, 87, 2038-2045. https://doi.org/10.1016/j.carbpol.2011.10.017
Sajjad, W., He, F., Ullah, M.W., Ikram, M., Shah, S.S., Khan, R., et al. (2020) Fabrication of Bacterial Cellulose-Curcumin Nanocomposite as a Novel Dressing for Partial Thickness Skin Burn. Frontiers in Bioengineering and Bioengineering, 8, Article 553037. https://doi.org/10.3389/fbioe.2020.553037
Chen, X.Y., Low, H.R., Loi, X.Y., Merel, L. and Iqbal, M.A.M.C. (2019) Fabrication and Evaluation of Bacterial Nanocellulose/Poly(Acrylic Acid)/Graphene Oxide Composite Hydrogel: Characterizations and Biocompatibility Studies for Wound Dressing. Journal of Biomedical Materials Research Part B: Applied Biomaterials, 107, 2140-2151. https://doi.org/10.1002/jbm.b.34309
Amin, M.C.I.M., Ahmad, N., Halib, N. and Ahmad, I. (2012) Synthesis and Characterization of Thermo and pH-Responsive Bacterial Cellulose/Acrylic Acid Hydrogels for Drug Delivery. Carbohydrate Polymers, 88, 465-473. https://doi.org/10.1016/j.carbpol.2011.12.022
Ozay, O. (2014) Synthesis and Swelling Behavior of Novel pH Responsive Hydrogels for Environmental Applications. Polymer-Plastics Technology and Engineering, 53, 130-140. https://doi.org/10.1080/03602559.2013.843697
Zhang, X., Meng, Y., Shen, W., Dou, J.C., Liu, R., et al. (2021) pH-Responsive Injectable Polysaccharide Hydrogels with Self-Healing, Enhanced Mechanical Properties Based on POSS. Reactive and Functional Polymers, 158, Article ID: 104773. https://doi.org/10.1016/j.reactfunctpolym.2020.104773
Shang, J.J. and Theato, P. (2018) Smart Composite Hydrogel with pH-, Ionic Strength- and Temperature-Induced Actuation. Soft Matter, 14, 8401-8407. https://doi.org/10.1039/C8SM01728J
Sun, L., Wang, Y., Jiang, T.Y., Zheng, X., Zhang, H.J., Sun, J. and Sun, C.S. (2013) A Novel Chitosan Functionalized Spherical Nanosilica Matrix as a Sustained Drug Delivery System for the Poorly Water-Soluble Drug Carvedilol. ACS Applied Materials & Interfaces, 5, 103-113. https://doi.org/10.1021/am302246s
Korsmeyer, R.W., Gumy, R., Doelker, E., Buri, P. and Peppas, N.A. (1983) Mechanisms of Solute Release from Porous Hydrophilic Polymers. International Journal of Pharmaceutics, 15, 25-35. https://doi.org/10.1016/0378-5173(83)90064-9
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, 1145-1149. https://doi.org/10.1002/jps.2600521210
Berry, M.R. and Likar, M.D. (2007) Statistical Assessment of Dissolution and Drug Release Profile Similarity Using a Model-Dependent Approach. Journal of Pharmaceutical and Biomedical Analysis, 45, 194-200. https://doi.org/10.1016/j.jpba.2007.05.021
Van Boekel, M.A.J.S. (2002) On the Use of the Weibull Model to Describe Thermal Inactivation of Microbial Vegetative Cells. International Journal of Food Microbiology, 74, 139-159. https://doi.org/10.1016/S0168-1605(01)00742-5
Wang, H., Hao, L., Wang, P., Chen, M., Jiang, S.W. and Jiang, S.T. (2016) Release Kinetics and Antibacterial Activity of Curcumin Loaded Zein Fibers. Food Hydrocolloids, 63, 437-446. https://doi.org/10.1016/j.foodhyd.2016.09.028
Yun, D.G. and Lee, D.G. (2016) Antibacterial Activity of Curcumin via Apoptosis-Like Response in Escherichia coli. Applied Microbiology and Biotechnology, 100, 5505-5514. https://doi.org/10.1007/s00253-016-7415-x