The antibacterial hydrogels can be widely used in the biomedical area owing to their excellent properties. The main limitation of antibacterial hydrogels is their poor mechanical strength. In this study, the novel hydrogels were fabricated with a mixture of silk fibroin (SF), chitosan (CH), agarose (AG), and silver nanoparticles (SNPs) via facile reaction condition without inorganic substances. The mechanical property of these fabricated hydrogels can be modulated by the concentration of SF or AG. The rheological studies demonstrated enhanced elasticity of CH-doped hydrogels. Because of the presence of CH and Ag in hydrogels, the antimicrobial property against gram-positive and gram-negative bacteria was exhibited. Cytocompatibility test proved the very low toxic nature of the hydrogels. In addition, these composite hydrogels have a smaller porosity, higher swelling ratio, and good compatibility, indicating their great potential for biomedical application.
This is a preview of subscription content, access via your institution.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
Tax calculation will be finalised during checkout.
R. Xu, G. Luo, H. Xia, W. He, J. Zhao, B. Liu, J. Tan, J. Zhou, D. Liu, Y. Wang, Z. Yao, R. Zhan, S. Yang, and J. Wu: Novel bilayer wound dressing composed of silicone rubber with particular micropores enhanced wound re-epithelialization and contraction. Biomaterials 40, 1–11 (2015).
C. Gong, Q. Wu, Y. Wang, D. Zhang, F. Luo, X. Zhao, Y. Wei, and Z. Qian: A biodegradable hydrogel system containing curcumin encapsulated in micelles for cutaneous wound healing. Biomaterials 34, 6377–6387 (2013).
X. Zhao, H. Wu, B. Guo, R. Dong, Y. Qiu, and P.X. Ma: Antibacterial anti-oxidant electroactive injectable hydrogel as self-healing wound dressing with hemostasis and adhesiveness for cutaneous wound healing. Biomaterials 122, 34–47 (2017).
A.R. Unnithan, G. Gnanasekaran, Y. Sathishkumar, Y.S. Lee, and C.S. Kim: Electrospun antibacterial polyurethane-cellulose acetate-zein composite mats for wound dressing. Carbohydr. Polym. 102, 884–892 (2014).
S. MacNeil: Progress and opportunities for tissue-engineered skin. Nature 445, 874–880 (2007).
S. Duchi, C. Onofrillo, C.D. O’Connell, R. Blanchard, C. Augustine, A.F. Quigley, R.M.I. Kapsa, P. Pivonka, G. Wallace, C. Di Bella, and P.F.M. Choong: Handheld co-axial bioprinting: Application to in situ surgical cartilage repair. Sci. Rep. 7, 5837 (2017).
J.L. Drury and D.J. Mooney: Hydrogels for tissue engineering: Scaffold design variables and applications. Biomaterials 24, 4337–4351 (2003).
G.P. Raeber, M.P. Lutolf, and J.A. Hubbell: Molecularly engineered PEG hydrogels: A novel model system for proteolytically mediated cell migration. Biophys. J. 89, 1374–1388 (2005).
B.K. Mann, A.S. Gobin, A.T. Tsai, R.H. Schmedlen, and J.L. West: Smooth muscle cell growth in photopolymerized hydrogels with cell adhesive and proteolytically degradable domains: Synthetic ECM analogs for tissue engineering. Biomaterials 22, 3045–3051 (2001).
T. Ngoc Quyen, Y.K. Joung, E. Lih, and K.D. Park: In situ forming and rutin-releasing chitosan hydrogels as injectable dressings for dermal wound healing. Biomacromolecules 12, 2872–2880 (2011).
B. Balakrishnan, M. Mohanty, A.C. Fernandez, P.V. Mohanan, and A. Jayakrishnan: Evaluation of the effect of incorporation of dibutyryl cyclic adenosine monophosphate in an in situ-forming hydrogel wound dressing based on oxidized alginate and gelatin. Biomaterials 27, 1355–1361 (2006).
J.Z. Yang, Y.S. Zhang, K. Yue, and A. Khademhosseini: Cell-laden hydrogels for osteochondral and cartilage tissue engineering. Acta Biomater. 57, 1–25 (2017).
W. Li, X. Li, W. Li, T. Wang, X. Li, S. Pan, and H. Deng: Nanofibrous mats layer-by-layer assembled via electrospun cellulose acetate and electrosprayed chitosan for cell culture. Eur. Polym. J. 48, 1846–1853 (2012).
S. Mohammed, G. Chouhan, O. Anuforom, M. Cooke, A. Walsh, P. Morgan-Warren, M. Jenkins, and F. de Cogan: Thermosensitive hydrogel as an in situ gelling antimicrobial ocular dressing. Mater. Sci. Eng., C 78, 203–209 (2017).
V. Normand, D.L. Lootens, E. Amici, K.P. Plucknett, and P. Aymard: New insight into agarose gel mechanical properties. Biomacromolecules 1, 730–738 (2000).
Y. Yuan, L. Wang, R.J. Mu, J.N. Gong, Y.Y. Wang, Y.Z. Li, J.Q. Ma, J. Pang, and C.H. Wu: Effects of konjac glucomannan on the structure, properties, and drug release characteristics of agarose hydrogels. Carbohydr. Polym. 190, 196–203 (2018).
H.M. Pauly, L.W. Place, T.L.H. Donahue, and M.J. Kipper: Mechanical properties and cell compatibility of agarose hydrogels containing proteoglycan mimetic graft copolymers. Biomacromolecules 18, 2220–2229 (2017).
N.R. Raia, B.P. Partlow, M. McGill, E.P. Kimmerling, C.E. Ghezzi, and D.L. Kaplan: Enzymatically crosslinked silk-hyaluronic acid hydrogels. Biomaterials 131, 58–67 (2017).
L. Tozzi, P.A. Laurent, C.A. Di Buduo, X. Mu, A. Massaro, R. Bretherton, W. Stoppel, D.L. Kaplan, and A. Balduini: Multi-channel silk sponge mimicking bone marrow vascular niche for platelet production. Biomaterials 178, 122–133 (2018).
P. Dubey, S. Kumar, V.K. Aswal, S. Ravindranathan, P.R. Rajamohanan, A. Prabhune, and A. Nisal: Silk fibroin-sophorolipid gelation: Deciphering the underlying mechanism. Biomacromolecules 17, 3318–3327 (2016).
R. Gharibi, H. Yeganeh, A. Rezapour-Lactoee, and Z.M. Hassan: Stimulation of wound healing by electroactive, antibacterial, and antioxidant polyurethane/siloxane dressing membranes: In vitro and in vivo evaluations. ACS Appl. Mater. Interfaces 7, 24296–24311 (2015).
W-Y. Chen, H-Y. Chang, J-K. Lu, Y-C. Huang, S.G. Harroun, Y-T. Tseng, Y-J. Li, C-C. Huang, and H-T. Chang: Self-assembly of antimicrobial peptides on gold nanodots: Against multidrug-resistant bacteria and wound-healing application. Adv. Funct. Mater. 25, 7189–7199 (2015).
M. Dash, F. Chiellini, R.M. Ottenbrite, and E. Chiellini: Chitosan-A versatile semi-synthetic polymer in biomedical applications. Prog. Polym. Sci. 36, 981–1014 (2011).
H. Ueno, T. Mori, and T. Fujinaga: Topical formulations and wound healing applications of chitosan. Adv. Drug Delivery Rev. 52, 105–115 (2001).
R.R. Klossner, H.A. Queen, A.J. Coughlin, and W.E. Krause: Correlation of chitosan’s rheological properties and its ability to electrospin. Biomacromolecules 9, 2947–2953 (2008).
J. Chedly, S. Soares, A. Montembault, Y. von Boxberg, M. Veron-Ravaille, C. Mouffle, M.N. Benassy, J. Taxi, L. David, and F. Nothias: Physical chitosan microhydrogels as scaffolds for spinal cord injury restoration and axon regeneration. Biomaterials 138, 91–107 (2017).
H. Pirvanescu, M. Balasoiu, M.E. Ciurea, A.T. Balasoiu, and R. Manescu: Wound infections with multi-drug resistant bacteria. Chirurgia 109, 73–79 (2014).
D. Liang, Z. Lu, H. Yang, J. Gao, and R. Chen: Novel asymmetric wettable AgNPs/chitosan wound dressing: In vitro and in vivo evaluation. ACS Appl. Mater. Interfaces 8, 3958–3968 (2016).
Z. Lu, J. Gao, Q. He, J. Wu, D. Liang, H. Yang, and R. Chen: Enhanced antibacterial and wound healing activities of microporous chitosan-Ag/ZnO composite dressing. Carbohydr. Polym. 156, 460–469 (2017).
T. Jayaramudu, K. Varaprasad, G.M. Raghavendra, E.R. Sadiku, K. Mohana Raju, and J. Amalraj: Green synthesis of tea Ag nanocomposite hydrogels via mint leaf extraction for effective antibacterial activity. J. Biomater. Sci., Polym. Ed. 28, 1588–1602 (2017).
M. Ahamed, M.S. AlSalhi, and M.K.J. Siddiqui: Silver nanoparticle applications and human health. Clin. Chim. Acta 411, 1841–1848 (2010).
P. Matricardi, C. Di Meo, T. Coviello, W.E. Hennink, and F. Alhaique: Interpenetrating polymer networks polysaccharide hydrogels for drug delivery and tissue engineering. Adv. Drug Delivery Rev. 65, 1172–1187 (2013).
Z.H. Ayub, M. Arai, and K. Hirabayashi: Mechanism of the gelation of fibroin solution. Biosci., Biotechnol., Biochem. 57, 1910–1912 (1993).
T. Asakura, A. Kuzuhara, R. Tabeta, and H. Saito: Conformation characterization of bombyx mori silk fibroin in the solid state by high-frequency 13c cross polarization–magic angle spinning NMR, X-ray diffraction, and infrared spectroscopy. Macromolecules 18, 1841–1845 (1985).
J. Magoshi, Y. Magoshi, M.A. Becker, and S. Nakamura: Biospinning by bombyx mori silkworm. Abstr. Pap. 212, 53–CELL (1996).
T. Hanawa, A. Watanabe, T. Tsuchiya, R. Ikoma, M. Hidaka, and M. Sugihara: New oral dosage form for elderly patients—preparation and characterization of silk fibroin gel. Chem. Pharm. Bull. 43, 284–288 (1995).
Y. Zhou, Q. Dong, H. Yang, X. Liu, X. Yin, Y. Tao, Z. Bai, and W. Xu: Photocrosslinked maleilated chitosan/methacrylated poly(vinyl alcohol) bicomponent nanofibrous scaffolds for use as potential wound dressings. Carbohydr. Polym. 168, 220–226 (2017).
Y.P. Singh, N. Bhardwaj, and B.B. Mandal: Potential of agarose/silk fibroin blended hydrogel for in vitro cartilage tissue engineering. ACS Appl. Mater. Interfaces 8, 21236–21249 (2016).
M.V. Priya, R.A. Kumar, A. Sivashanmugam, S.V. Nair, and R. Jayakumar: Injectable amorphous chitin-agarose composite hydrogels for biomedical applications. J. Funct. Biomater. 6, 849–862 (2015).
K.J. Le Goff, C. Gaillard, W. Helbert, C. Garnier, and T. Aubry: Rheological study of reinforcement of agarose hydrogels by cellulose nanowhiskers. Carbohydr. Polym. 116, 117–123 (2015).
L.Y. Zheng and J.A.F. Zhu: Study on antimicrobial activity of chitosan with different molecular weights. Carbohydr. Polym. 54, 527–530 (2003).
M. Rai, A. Yadav, and A. Gade: Silver nanoparticles as a new generation of antimicrobials. Biotechnol. Adv. 27, 76–83 (2009).
The research was supported by the Hi-Tech Research and Development 863 Program of China Grant (No. 2013AA102507), Funds of China Agriculture Research System (No. CARS-18-ZJ0102), and Chongqing Research Program of Basic Research and Frontier Technology (No. cstc2017jcyjAX0087).
About this article
Cite this article
Chen, SH., Li, Z., Liu, ZL. et al. Antimicrobial hydrogels with controllable mechanical properties for biomedical application. Journal of Materials Research 34, 1911–1921 (2019). https://doi.org/10.1557/jmr.2019.77