Toward Cartilage-Mimicking Biomaterials: Biotribological, Biochemical and Structural Evaluation of pHEMA and PVA-Based Hydrogels
Status PubMed-not-MEDLINE Jazyk angličtina Země Spojené státy americké Médium electronic-ecollection
Typ dokumentu časopisecké články
PubMed
41487215
PubMed Central
PMC12756760
DOI
10.1021/acsomega.5c10283
Knihovny.cz E-zdroje
- Publikační typ
- časopisecké články MeSH
This study compares the biotribological and structural behavior of PVA and pHEMA hydrogels under conditions simulating the cartilage environment to understand the lubrication mechanisms. PVA samples exhibited very low apparent friction coefficients and high-water uptake due to their hydrophilic, hydroxyl-rich network. In contrast, pHEMA hydrogels showed higher friction but substantially enhanced wear resistance, particularly under extended sliding against rough counterfaces. While PVA offers excellent lubrication performance, its wear stability remains limited. On the other hand, the low wear observed in pHEMAdespite its higher frictionsuggests strong structural resilience, making it a promising platform for further tailoring toward cartilage-mimicking applications. The results highlight the importance of balancing interfacial lubrication and mechanical durability when designing hydrogel-based cartilage replacements.
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Kim J.-R., Cho Y. S., Park J.-H., Kim T.-H.. Poly(HEMA-co-MMA) hydrogel scaffold for tissue engineering with controllable morphology and mechanical properties through self-assembly. Polymers. 2024;16:3014. doi: 10.3390/polym16213014. PubMed DOI PMC
Yang F., Zhao J., Koshut W. J., Watt J., Riboh J. C., Gall K., Wiley B. J.. A synthetic hydrogel composite with the mechanical behavior and durability of cartilage. Adv. Funct. Mater. 2020;30:2003451. doi: 10.1002/adfm.202003451. DOI
Lin W., Klein J.. Recent progress in cartilage lubrication. Adv. Mater. 2021;33:2005513. doi: 10.1002/adma.202005513. PubMed DOI
Suzuki A., Sasaki S., Murakami T.. Development of PVA hydrogels with superior lubricity for artificial cartilage. Rheol. Biol. Soft Matter. 2017:339–374. doi: 10.1007/978-4-431-56080-7_13. DOI
Yu P., Li Y., Sun H., Ke X., Xing J., Zhao Y., Xu X., Qin M., Xie J., Li J.. Cartilage-Inspired Hydrogel with Mechanical Adaptability, Controllable Lubrication, and Inflammation Regulation Abilities. ACS Appl. Mater. Interfaces. 2022;14:27360–27370. doi: 10.1021/acsami.2c04609. PubMed DOI
Chen W., Deng H., Dong Y., Wu X., Xia Z., Zhou Y., Yang L., Huang Z., Xu W., Xu P., Xu H.. Double-Network Bilayer Hydrogel Loaded with Puerarin and Curcumin for Osteochondral Repair. ACS Omega. 2025;10:42282–42299. doi: 10.1021/acsomega.5c01794. PubMed DOI PMC
Feng H., Wang S., Chen K., Zhang X., Feng C., Li X., Yang W., Zhang D., Ge S.. Strong Bonding of Robust Lubricating Hydrogels to Porous Substrates for Joint Replacement. ACS Appl. Mater. Interfaces. 2024;16:64074–64086. doi: 10.1021/acsami.4c16046. PubMed DOI
Awasthi S., Gaur J. K., Pandey S. K., Bobji M. S., Srivastava C.. High-Strength, Strongly Bonded Nanocomposite Hydrogels for Cartilage Repair. ACS Appl. Mater. Interfaces. 2021;13:24505–24523. doi: 10.1021/acsami.1c05394. PubMed DOI
Jalageri M. B., Kumar G. C. M.. Graphene oxide reinforced polyvinyl alcohol/Chitosan composite hydrogel for cartilage regeneration. Polym. Bull. 2024;81:10915–10932. doi: 10.1007/s00289-024-05228-7. DOI
Hashemi-Afzal F., Fallahi H., Bagheri F., Collins M. N., Eslaminejad M. B., Seitz H.. Advancements in hydrogel design for articular cartilage regeneration: A comprehensive review. Bioact. Mater. 2025;43:1–31. doi: 10.1016/j.bioactmat.2024.09.005. PubMed DOI PMC
Li A., Huang J., Chen J., Wu L., Zeng H., Deng Z., Liu P., Lin J.. Evolving functional hydrogel strategies for cartilage engineering: from fundamentals to functional regeneration. Burns Trauma. 2025;13:tkaf041. doi: 10.1093/burnst/tkaf041. PubMed DOI PMC
Rudge R. E. D., Scholten E., Dijksman J. A.. Natural and induced surface roughness determine frictional regimes in hydrogel pairs. Tribiol. Int. 2020;141:105903. doi: 10.1016/j.triboint.2019.105903. DOI
Zhao J., Tong H., Kirillova A., Koshut W. J., Malek A., Brigham N. C., Becker M. L., Gall K., Wiley B. J.. A Synthetic Hydrogel Composite with a Strength and Wear Resistance Greater than Cartilage. Adv. Funct. Mater. 2022;32:2205662. doi: 10.1002/adfm.202205662. DOI
Kim S., Hwang Y., Kashif M., Jeong D., Kim G.. Evaluation of bone regeneration on polyhydroxyethyl-polymethyl methacrylate membrane in a rabbit calvarial defect model. In Vivo. 2016;30:587–591. PubMed
Wang Y., Chu X., Sun Y., Teng P., Xia T., Chen Y.. A convenient approach by using poly-(scpHEMA-co-NIPAM/scp)/Cu2+ solution sol–gel transition for wound protection and healing. J. Biomed. Mater. Res., Part B. 2021;109:50–59. doi: 10.1002/jbm.b.34679. PubMed DOI
Ghanbarinia Firozjah R., Sadeghi A., Khoee S.. Ultrasonic de-cross-linking of the pH- and magneto-responsive PHEMA/PMMA microgel to Janus nanoparticles: A new synthesis based on “grafting from”/“grafting to” polymerization. ACS Omega. 2020;5:27119–27132. doi: 10.1021/acsomega.0c02710. PubMed DOI PMC
Krajňák T., Černá E., Šuráňová M., Šamořil T., Zicha D., Vojtová L., Čechal J.. Replica-mold nanopatterned PHEMA hydrogel surfaces for ophthalmic applications. Sci. Rep. 2022;12:14497. doi: 10.1038/s41598-022-18564-3. PubMed DOI PMC
Musgrave C. S. A., Fang F.. Contact lens materials: A materials science perspective. Materials. 2019;12:261. doi: 10.3390/ma12020261. PubMed DOI PMC
Zare M., Bigham A., Zare M., Luo H., Ghomi E. R., Ramakrishna S.. PHEMA: An overview for biomedical applications. Int. J. Mol. Sci. 2021;22:6376. doi: 10.3390/ijms22126376. PubMed DOI PMC
Kadlecova Z., Chamradova I., Tuslova K., Rebenda D., Cipek P., Gregora J., Stredanska A., Sawae Y., Mencik P., Vrbka M., Vojtova L.. Biomimetic pHEMA Hydrogels as an Alternative Cartilage-like Model Material for Biotribological Evaluations. Acs Omega. 2025;10:44147–44161. doi: 10.1021/acsomega.5c05569. PubMed DOI PMC
Hua Z., Hu M., Chen Y., Huang X., Gao L.. Investigation of the friction properties of a new artificial imitation cartilage material: PHEMA/glycerol gel. Materials. 2023;16:4023. doi: 10.3390/ma16114023. PubMed DOI PMC
Yarimitsu S., Sasaki S., Murakami T., Suzuki A.. Evaluation of lubrication properties of hydrogel artificial cartilage materials for joint prosthesis. Biosurf. Biotribol. 2016;2:40–47. doi: 10.1016/j.bsbt.2016.02.005. DOI
Xi Y., Sharma P. K., Kaper H. J., Choi C.-H.. Tribological properties of micropored poly(2-hydroxyethyl methacrylate) hydrogels in a biomimetic aqueous environment. ACS Appl. Mater. Interfaces. 2021;13:41473–41484. doi: 10.1021/acsami.1c13718. PubMed DOI
Murakami T., Yarimitsu S., Nakashima K., Sawae Y., Sakai N.. Influence of synovia constituents on tribological behaviors of articular cartilage. Friction. 2013;1:150–162. doi: 10.1007/s40544-013-0010-6. DOI
Bostan L., Trunfio-Sfarghiu A.-M., Verestiuc L., Popa M. I., Munteanu F., Rieu J.-P., Berthier Y.. Mechanical and tribological properties of poly(hydroxyethyl methacrylate) hydrogels as articular cartilage substitutes. Tribiol. Int. 2012;46:215–224. doi: 10.1016/j.triboint.2011.06.035. DOI
Němeček, D. ; Nečas, D. ; Shinmori, H. ; Yarimitsu, S. ; Marian, M. ; Vrbka, M. . et al. A glance into the boundary lubrication mechanism of PVA hydrogel after the reduction of interstitial fluid pressurization Friction 2025. 10.26599/FRICT.2025.9441106. DOI
Karadag E., Saraydin D., Sahiner N., Güven O.. Radiation induced acrylamide/citric acid hydrogels and their swelling behaviors. J. Macromol. Sci., Part A. 2001;38:1105–1121. doi: 10.1081/MA-100107132. DOI
Manaila E., Craciun G., Ighigeanu D., Cimpeanu C., Barna C., Fugaru V.. Hydrogels synthesized by electron beam irradiation for heavy metal adsorption. Materials. 2017;10:540. doi: 10.3390/ma10050540. PubMed DOI PMC
Mehta, S. Characterizing Hydrogels using Dynamic Mechanical Analysis Methods Application Note EF034;TA Instruments.
Furmann D., Nečas D., Rebenda D., Čípek P., Vrbka M., Křupka I., Hartl M.. The Effect of Synovial Fluid Composition, Speed and Load on Frictional Behaviour of Articular Cartilage. Materials. 2020;13:1334. doi: 10.3390/ma13061334. PubMed DOI PMC
Rebenda D., Vrbka M., Čípek P., Toropitsyn E., Nečas D., Pravda M., Hartl M.. On the Dependence of Rheology of Hyaluronic Acid Solutions and Frictional Behavior of Articular Cartilage. Materials. 2020;13:2659. doi: 10.3390/ma13112659. PubMed DOI PMC
Ranuša M., Ondra M., Rebenda D., Vrbka M., Gallo J., Křupka I.. Effects of Viscosupplementation on Tribological Behaviour of Articular Cartilage. Lubricants. 2022;10:361. doi: 10.3390/lubricants10120361. DOI
Shi Y., Xiong D., Li J., Li L., Liu Q., Dini D.. Tribological Rehydration and Its Role on Frictional Behavior of PVA/GO Hydrogels for Cartilage Replacement Under Migrating and Stationary Contact Conditions. Tribol. Lett. 2020;69:7. doi: 10.1007/s11249-020-01371-0. DOI
Chen Q., Zhang X., Chen K., Feng C., Wang D., Qi J., Li X., Zhao X., Chai Z., Zhang D.. Bilayer Hydrogels with Low Friction and High Load-Bearing Capacity by Mimicking the Oriented Hierarchical Structure of Cartilage. ACS Appl. Mater. Interfaces. 2022;14:52347–52358. doi: 10.1021/acsami.2c13641. PubMed DOI
Sardinha V. M., Lima L. L., Belangero W. D., Zavaglia C. A., Bavaresco V. P., Gomes J. R.. Tribological characterization of polyvinyl alcohol hydrogel as substitute of articular cartilage. Wear. 2013;301:218–225. doi: 10.1016/j.wear.2012.11.054. DOI
Mostakhdemin M., Nand A., Ramezani M.. Articular and Artificial Cartilage, Characteristics, Properties and Testing ApproachesA Review. Polymers. 2021;13:2000. doi: 10.3390/polym13122000. PubMed DOI PMC
Kanca Y., Milner P., Dini D., Amis A. A.. Tribological properties of PVA/PVP blend hydrogels against articular cartilage. J. Mech. Behav. Biomed. Mater. 2018;78:36–45. doi: 10.1016/j.jmbbm.2017.10.027. PubMed DOI
Taylor S. D., Tsiridis E., Ingham E., Jin Z., Fisher J., Williams S.. Comparison of human and animal femoral head chondral properties and geometries. Proc. Inst. Mech. Eng., Part H. 2012;226:55–62. doi: 10.1177/0954411911428717. PubMed DOI
Brand R. A., Iglič A., Kralj-iglič V.. Contact Stresses in the Human Hip: Implications for Disease and Treatment. Hip Int. 2001;11:117–126. doi: 10.1177/112070000101100301. DOI
Brand R. A.. Joint contact stress: a reasonable surrogate for biological processes? Iowa Orthop. J. 2005;25:82–94. PubMed PMC
Akanda S. R., Kupratis M. E., Bhattacharjee A., Benson J., Burris D. L., Price C.. Elevated Contact Stresses Compromise Activity-Mediated Cartilage Rehydration but not Lubrication. Ann. Biomed. Eng. 2025;53:1672–1688. doi: 10.1007/s10439-025-03708-z. PubMed DOI PMC
Duque-Ossa L. C., Ruiz-Pulido G., Medina D. I.. Triborheological study under physiological conditions of PVA hydrogel/HA lubricant as synthetic system for soft tissue replacement. Polymers. 2021;13:746. doi: 10.3390/polym13050746. PubMed DOI PMC
Plugariu I.-A., Bercea M., Gradinaru L. M., Rusu D., Lupu A.. Poly(vinyl alcohol)/pullulan composite hydrogels as a potential platform for wound dressing applications. Gels. 2023;9:580. doi: 10.3390/gels9070580. PubMed DOI PMC
Hassan C. M., Peppas N. A.. Cellular PVA hydrogels produced by freeze/thawing. J. Appl. Polym. Sci. 2000;76:2075–2079. doi: 10.1002/(SICI)1097-4628(20000628)76:14<2075::AID-APP11>3.0.CO;2-V. DOI
Otsuka, E. ; Suzuki, E. A. In Swelling Properties of Physically Cross-Linked PVA Gels Prepared by a Cast-Drying Method, Gels: Structures, Properties, and Functions. Progress in Colloid and Polymer Science; Springer, 2009; pp 121–126.
Oliveira A. S., Colaço R., Serro A. P.. Hydrogels based on poly(vinyl alcohol) for cartilage substitution. Ann. Med. 2021;53:2069–2089. doi: 10.1080/07853890.2021.1896896. DOI
Bajpai A. K., Saini R.. Preparation and characterization of biocompatible spongy cryogels of poly(vinyl alcohol)–gelatin and study of water sorption behaviour. Polym. Int. 2005;54:1233–1242. doi: 10.1002/pi.1813. DOI
Aversa R., Petrescu R. V., Petrescu F. I. T., Perrotta V., Apicella D., Apicella A.. Biomechanically tunable nano-silica/P-HEMA structural hydrogels for bone scaffolding. Bioengineering. 2021;8:45. doi: 10.3390/bioengineering8040045. PubMed DOI PMC
Mabilleau G., Baslé M. F., Chappard D.. Evaluation of surface roughness of hydrogels by fractal texture analysis during swelling. Langmuir. 2006;22:4843–4845. doi: 10.1021/la060368v. PubMed DOI
Zhong Y., Lin Q., Yu H., Shao L., Cui X., Pang Q.. et al. Construction methods and biomedical applications of PVA-based hydrogels. Front. Chem. 2024;12:1398712. doi: 10.3389/fchem.2024.1376799. PubMed DOI PMC
Charron P. N., Braddish T. A., Floreani R.. PVA-gelatin hydrogels formed using combined theta-gel and cryo-gel fabrication techniques. J. Mech. Behav. Biomed. Mater. 2019;92:90–96. doi: 10.1016/j.jmbbm.2019.01.002. PubMed DOI PMC
Zhang P., Xu Z., Wu Z., Xu P., Yang C.. Strengthening poly(2-hydroxyethyl methacrylate) hydrogels using biochars and hydrophobic aggregations. Int. J. Smart Nano Mater. 2022;13:561–574. doi: 10.1080/19475411.2022.2107115. DOI
Jayaramudu T., Ko H.-U., Kim H. C., Kim J. W., Muthoka R. M., Kim J.. Electroactive hydrogels made with polyvinyl alcohol/cellulose nanocrystals. Materials. 2018;11:1615. doi: 10.3390/ma11091615. PubMed DOI PMC
Temple D. K., Cederlund A. A., Lawless B. M., Aspden R. M., Espino D. M.. Viscoelastic properties of human and bovine articular cartilage: a comparison of frequency-dependent trends. BMC Musculoskeletal Disord. 2016;17:419. doi: 10.1186/s12891-016-1279-1. PubMed DOI PMC
Makarova E. B., Korch M. A., Fadeyev F. A., Bliznets D. G., Bugayova A. V., Shklyar T. F., Safronov A. P., Nokhrin K. A., Blyakhman F. A.. Testing of the pHEMA hydrogel as an implantation material for replacement of osteochondral defects in animals. Russ. J. Transplantol. Artif. Organs. 2022;24:71–82. doi: 10.15825/1995-1191-2022-2-71-82. DOI
Spoljaric S., Salminen A., Luong N. D., Seppälä J.. Stable, self-healing hydrogels from nanofibrillated cellulose, poly(vinyl alcohol) and borax via reversible crosslinking. Eur. Polym. J. 2014;56:105–117. doi: 10.1016/j.eurpolymj.2014.03.009. DOI
Wang M., Bai J., Shao K., Tang W., Zhao X., Lin D., Huang S., Chen C., Ding Z., Ye J.. Poly(vinyl alcohol) Hydrogels: The Old and New Functional Materials. Int. J. Polym. Sci. 2021;2021:2225426. doi: 10.1155/2021/2225426. DOI
Murakami T., Sakai N., Yarimitsu S., Nakashima K., Yamaguchi T., Sawae Y., Suzuki A.. Evaluation of influence of changes in permeability with aging on friction and biphasic behaviors of artificial hydrogel cartilage. Biotribology. 2021;26:100178. doi: 10.1016/j.biotri.2021.100178. DOI
Yarimitsu, S. ; Sawae, Y. In Development of PVA Hydrogels for Artificial Cartilage with Superior Lubricity; Proceedings of JSME International Conference on Materials and Processing, 2022.
Sakai N., Hashimoto C., Yarimitsu S., Sawae Y., Komori M., Murakami T.. A functional effect of the superficial mechanical properties of articular cartilage as a load bearing system in a sliding condition. Biosurf. Biotribol. 2016;2:26–39. doi: 10.1016/j.bsbt.2016.02.004. DOI
Simič R., Mandal J., Zhang K., Spencer N. D.. Oxygen inhibition of free-radical polymerization is the dominant mechanism behind the “mold effect” on hydrogels. Soft Matter. 2021;17:6394–6403. doi: 10.1039/D1SM00395J. PubMed DOI PMC
Simič R., Spencer N. D.. Controlling the friction of gels by regulating interfacial oxygen during polymerization. Tribol. Lett. 2021;69:86. doi: 10.1007/s11249-021-01459-1. PubMed DOI PMC
Hu D., Yan Y., Wei W., Bai C., Lu Y., Wang Y.. et al. Mechanically robust lubricating hydrogels contrived by harnessing low-entropy nanocrystalline polymer network. Adv. Funct. Mater. 2025;35:2409023. doi: 10.1002/adfm.202508450. DOI
Asy-Syifa N., Kusjuriansah, Waresindo W. X., Edikresnha D., Suciati T., Khairurrijal K.. The study of the swelling degree of the PVA hydrogel with varying concentrations of PVA. J. Phys.: Conf. Ser. 2022;2243:012053. doi: 10.1088/1742-6596/2243/1/012053. DOI
Ou K., Dong X., Qin C., Ji X., He J.. Properties and toughening mechanisms of PVA/PAM double-network hydrogels prepared by freeze-thawing and anneal-swelling. Mater. Sci. Eng.: C. 2017;77:1017–1026. doi: 10.1016/j.msec.2017.03.287. PubMed DOI
Krzeminski J., Molisak-tolwinska H.. Molisak-Tolwinska, The structure of water-swollen poly(vinyl alcohol) and the swelling mechanism. J. Macromol. Sci.Chem. 1991;28:413–429.
Zitouni M. A., Kara Slimane B.. Preparation and characterization of hydrogels based on chitosan/polyvinyl alcohol blends. Adv. Mater. Res. 2015;1105:203–207.
Nakano T., Nakaoki T.. Coagulation size of freezable water in poly(vinyl alcohol) hydrogels formed by different freeze/thaw cycle periods. Polym. J. 2011;43:875–880. doi: 10.1038/pj.2011.92. DOI
Chhatri A., Bajpai J., Bajpai A. K., Sandhu S. S., Jain N., Biswas J.. Cryogenic fabrication of savlon loaded macroporous blends of alginate and polyvinyl alcohol (PVA): swelling, deswelling and antibacterial behaviors. Carbohydr. Polym. 2011;83:876–882. doi: 10.1016/j.carbpol.2010.08.077. DOI
O Muratoglu, S. ; Spiegelberg, J. ; Ruberti, N. . Abt, PVA hydrogel. United States Patent and Trademark Office. US Patent US20060079597A1, 2006.
Guan Y., Bian J., Peng F., Zhang X.-M., Sun R.-C.. High strength of hemicelluloses-based hydrogels by freeze/thaw technique. Carbohydr. Polym. 2014;101:272–280. doi: 10.1016/j.carbpol.2013.08.085. PubMed DOI
Chaturvedi A., Bajpai A. K., Bajpai J.. Preparation and characterization of poly(vinyl alcohol) cryogel-silver nanocomposites and evaluation of blood compatibility, cytotoxicity, and antimicrobial behaviors. Polym. Compos. 2015;36:1983–1997. doi: 10.1002/pc.23108. DOI
Górska A., Baran E., Knapik-Kowalczuk J., Szafraniec-Szczęsny J., Paluch M., Kulinowski P., Mendyk A.. Physically cross-linked PVA hydrogels as potential wound dressings: How freezing conditions and formulation composition define cryogel structure and performance. Pharmaceutics. 2024;16:1388. doi: 10.3390/pharmaceutics16111388. PubMed DOI PMC
Link J. M., Salinas E. Y., Hu J. C., Athanasiou K. A.. The tribology of cartilage: Mechanisms, experimental techniques, and relevance to translational tissue engineering. Clin. Biomech. 2020;79:104880. doi: 10.1016/j.clinbiomech.2019.10.016. PubMed DOI PMC
Caligaris M., Ateshian G. A.. Effects of sustained interstitial fluid pressurization under migrating contact area, and boundary lubrication by synovial fluid, on cartilage friction. Osteoarthritis Cartilage. 2008;16:1220–1227. doi: 10.1016/j.joca.2008.02.020. PubMed DOI PMC
Ateshian G. A.. The role of interstitial fluid pressurization in articular cartilage lubrication. J. Biomech. 2009;42:1163–1176. doi: 10.1016/j.jbiomech.2009.04.040. PubMed DOI PMC
Burris D. L., Ramsey L., Graham B. T., Price C., Moore A. C.. How Sliding and Hydrodynamics Contribute to Articular Cartilage Fluid and Lubrication Recovery. Tribol. Lett. 2019;67:46. doi: 10.1007/s11249-019-1158-7. DOI
Accardi M. A., Dini D., Cann P. M.. Experimental and numerical investigation of the behaviour of articular cartilage under shear loadingInterstitial fluid pressurisation and lubrication mechanisms. Tribiol. Int. 2011;44:565–578. doi: 10.1016/j.triboint.2010.09.009. DOI