Abstract
Due to the good biocompatibility, polyvinyl alcohol (PVA) hydrogels have attracted the attention of many biomaterial researchers. However, the low strength and poor toughness of pure PVA hydrogel prepared by freeze–thaw method limit the application. In this study, silica was used to enhance the performances of PVA hydrogel. Different from previous PVA/SiO2 hydrogels, urea was used to regulate the formation and distribution of silica in PVA, which greatly improved the mechanical properties of hydrogels. The tensile stress and toughness of the obtained PVA(Urea)/SiO2 hydrogels reached 8.10 MPa and 44.45 MJ/m3, which were 39 times and 212 times as that of pure PVA hydrogel, respectively. In PVA(Urea)/SiO2 hydrogels, SiO2 had both strengthening and toughening effects on hydrogels, which is very different from the ordinary composite hydrogels. In addition, PVA(Urea)/SiO2 hydrogels showed unique self-reinforcing characteristics with increasing the number of tensile recoveries in cyclic stretching and recovery tests. Thus, PVA(Urea)/SiO2 hydrogel with high strength and toughness, constructed by a simple strategy, is a potential candidate in cartilage repair.
Similar content being viewed by others
Data availability
The data in the manuscript can be obtained from the corresponding author.
References
Xia B, Chen G (2022) Research progress of natural tissue-derived hydrogels for tissue repair and reconstruction. Int J Biol Macromol 214:480–491
Shi W, Wang Z, Song H et al (2022) High-sensitivity and extreme environment-resistant sensors based on PEDOT: PSS@ PVA hydrogel fibers for physiological monitoring. ACS Appl Mater Interfaces 14(30):35114–35125
Koshut WJ, Kwon N, Zhao J, Amendola A, Wiley BJ, Gall K (2022) Flaw sensitivity and tensile fatigue of a high-strength hydrogel. Int J Fatigue 163:107071
Duan SD, Liu ZX, Wu SW, Hua MT, He XM (2022) Tuning structural and mechanical anisotropy of PVA hydrogels. Mech Mater 172:104411
Wang X, Wang X, Pi M, Ran R (2022) High-strength, highly conductive and woven organic hydrogel fibers for flexible electronics. Chem Eng J 428:131172
Hao M, Wang Y, Li L et al (2022) Tough engineering hydrogels based on swelling–freeze–thaw method for artificial cartilage. ACS Appl Mater Interfaces 14(22):25093–25103
Wang K, Cheng W, Ding Z et al (2021) Injectable silk/hydroxyapatite nanocomposite hydrogels with vascularization capacity for bone regeneration. J Mater Sci Technol 63:172–181
Vashist A, Kaushik A, Vashist A et al (2018) Advances in carbon nanotubes–hydrogel hybrids in nanomedicine for therapeutics. Adv Healthc Mater 7(9):1701213
Du H, Liu W, Zhang M, Si C, Zhang X, Li B (2019) Cellulose nanocrystals and cellulose nanofibrils based hydrogels for biomedical applications. Carbohydr Polym 209:130–144
Alam A, Zhang Y, Kuan H-C, Lee S-H, Ma J (2018) Polymer composite hydrogels containing carbon nanomaterials—morphology and mechanical and functional performance. Prog Polym Sci 77:1–18
Takeno H, Aoki Y, Kimura K (2021) Effects of silica and clay nanoparticles on the mechanical properties of poly (vinyl alcohol) nanocomposite hydrogels. Colloids Surf A Physicochem Eng Asp 630:127592
Yang M, Shi J, Xia Y (2018) Effect of SiO2, PVA and glycerol concentrations on chemical and mechanical properties of alginate-based films. Int J Biol Macromol 107:2686–2694
Zhang C, Liang K, Zhou D et al (2018) High-performance photopolymerized poly (vinyl alcohol)/silica nanocomposite hydrogels with enhanced cell adhesion. ACS Appl Mater Interfaces 10(33):27692–27700
Rose S, Marcellan A, Narita T, Boué F, Cousin F, Hourdet D (2015) Structure investigation of nanohybrid PDMA/silica hydrogels at rest and under uniaxial deformation. Soft Matter 11(29):5905–5917
Alam MA, Takafuji M, Ihara H (2013) Thermosensitive hybrid hydrogels with silica nanoparticle-cross-linked polymer networks. J Colloid Interface Sci 405:109–117
Luo X, Akram M, Yuan Y, Nie J, Zhu X (2019) Silicon dioxide/poly (vinyl alcohol) composite hydrogels with high mechanical properties and low swellability. J Appl Polym Sci 136(1):46895
Krumrine P, Boyce S (1985) Profile modification and water control with silica gel-based systems. In: Paper presented at: society of petroleum engineers
Hatzignatiou DG, Giske NH (2018) Sodium silicate gelants for water management in naturally fractured hydrocarbon carbonate formations. Chem Eng Res Des 132:40–56
Lynn K (1965) Kinetics of base-catalyzed hydrolysis of urea. J Phys Chem 69(2):687–689
Ma T (2019) Study on silicic acid gel system initiated by CO2. Appl Chem 48(08):1817–1819
Chen Y, Hong Y, Zheng F, Li J, Wu Y, Li L (2009) Preparation of silicate stalagmite from sodium silicate. J Alloys Compd 478(1):411–414
Politi MJ, Chaimovich H, Liu C, Triboni ER, Briotto Filho D, Cuccovia IM (2017) Effect of urea on ion pair formation. The hydrophilic effect of urea. Colloids Surf A Physicochem Eng Asp 520:173–177
Dias LG, Florenzano FH, Reed WF et al (2002) Effect of urea on biomimetic systems: neither water 3-D structure rupture nor direct mechanism, simply a more “polar water.” Langmuir 18(2):319–324
Jiang X, Xu W, Tang Y, Zhang X, Dai H (2010) Study on properties of urea/ethanolamine compound plasticized polyvinyl alcohol. Acta Polym Sin 09:1143–1147
Xu L, Gao S, Guo Q, Wang C, Qiao Y, Qiu D (2020) A solvent-exchange strategy to regulate noncovalent interactions for strong and antiswelling hydrogels. Adv Mater 32(52):2004579
Hou Y, Chen C, Liu K, Tu Y, Zhang L, Li YJRA (2015) Preparation of PVA hydrogel with high-transparence and investigations of its transparent mechanism. RSC Adv 5(31):24023–24030
Yusong P, Jie D, Yan C, Qianqian S (2016) Study on mechanical and optical properties of poly (vinyl alcohol) hydrogel used as soft contact lens. Mater Technol 31(5):266–273
Park H, Englezos P (1998) Osmotic coefficient data for Na2SiO3 and Na2SiO3–NaOH by an isopiestic method and modeling using Pitzer’s model. Fluid Phase Equilib 153(1):87–104
Vo PT, Nguyen HT, Trinh HT et al (2021) The nitrogen slow-release fertilizer based on urea incorporating chitosan and poly (vinyl alcohol) blend. Environ Technol Innov 22:101528
Yan J, Tian H, Zhang Y, Xiang A (2015) Effect of urea and formamide plasticizers on starch/PVA bioblend sheets. J Appl Polym Sci 132(33):42311
Liu C, Morimoto N, Jiang L et al (2021) Tough hydrogels with rapid self-reinforcement. Science 372(6546):1078–1081
Zhang Y, Hu Q, Yang S, Wang T, Sun W, Tong Z (2021) Unique self-reinforcing and rapid self-healing polyampholyte hydrogels with a ph-induced shape memory effect. Macromolecules 54(11):5218–5228
Gan S, Bai S, Chen C et al (2021) Hydroxypropyl cellulose enhanced ionic conductive double-network hydrogels. Int J Biol Macromol 181:418–425
Bai J, Wang H (2020) Determination of melamine and urea in milk powder by infrared spectroscopy. Food Ferment Ind 46(08):267–272
Dubey R, Rajesh Y, More M (2015) Synthesis and characterization of SiO2 nanoparticles via sol-gel method for industrial applications. Mater Today Proc 2(45):3575–3579
Acknowledgements
Inapplicable.
Author information
Authors and Affiliations
Contributions
XT, SB and CL were involved in experimental design, carrying out measurements and manuscript composition. JR and JZ took part in conceptualization, supervision, project administration, validation, funding acquisition, writing—review and editing. PL and YR were involved in conceptualization and editing.
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Ethical approval
Inapplicable.
Additional information
Handling Editor: Annela M. Seddon.
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Tan, X., Liang, C., Bai, S. et al. PVA/silica hybrid hydrogel with ultra-high strength and toughness. J Mater Sci 59, 6916–6928 (2024). https://doi.org/10.1007/s10853-023-09061-7
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10853-023-09061-7