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Synthesis of bioadhesive PHEA hydrogels without crosslinkers through in situ polymerization and sustained mechanical mixing

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Abstract

This study presents a novel methodology for the fabrication of bioadhesives composed of poly(2-hydroxyethyl acrylate) (PHEA), which demonstrate superior mechanical properties. Hydrogels based on PHEA were effectively synthesized through a strategy that obviates the need for crosslinkers, utilizing in situ polymerization of high-concentration 2-hydroxyethyl acrylate (HEA) monomers under persistent agitation. Optimal operational conditions, such as polymerization duration and HEA monomer concentration, were screened through rheological evaluations. In addition, the introduction of glycerol to the PHEA hydrogels yielded improvements in water-retention capacity, thus resolving limitations frequently observed in conventional aqueous-based hydrogels. Tests assessing adhesive properties indicated that the PHEA hydrogels, synthesized without crosslinkers, exhibited exceptional adhesion capabilities that exceeded those of commercially available tissue sealants. This economically viable and readily scalable fabrication technique provides a compelling pathway for the creation of robust, biocompatible bioadhesives well-suited for biomedical utilization.

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The data supporting the findings of this study are available from the corresponding author upon reasonable request.

References

  1. Spotnitz WD, Burks S (2008) Hemostats, sealants, and adhesives: components of the surgical toolbox. Transfusion 48:1502–1516. https://doi.org/10.1111/j.1537-2995.2008.01703.x

    Article  PubMed  Google Scholar 

  2. Mehdizadeh M, Weng H, Gyawali D, Tang L, Yang J (2012) Injectable citrate-based mussel-inspired tissue bioadhesives with high wet strength for sutureless wound closure. Biomaterials 33:7972–7983. https://doi.org/10.1016/j.biomaterials.2012.07.055

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  3. Mehdizadeh M, Yang J (2013) Design strategies and applications of tissue bioadhesives. Macromol Biosci 13:271–288. https://doi.org/10.1002/mabi.201200332

    Article  CAS  PubMed  Google Scholar 

  4. Padula C, Colombo G, Nicoli S, Catellani PL, Massimo G, Santi P (2003) Bioadhesive film for the transdermal delivery of lidocaine: in vitro and in vivo behavior. J Control Release 88:277–285. https://doi.org/10.1016/S0168-3659(03)00015-4

    Article  CAS  PubMed  Google Scholar 

  5. Singer AJ, Quinn JV, Hollander JE (2008) The cyanoacrylate topical skin adhesives. Am J Emerg Med 26:490–496. https://doi.org/10.1016/j.ajem.2007.05.015

    Article  PubMed  Google Scholar 

  6. Lee KY, Mooney DJ (2012) Alginate: properties and biomedical applications. Prog Polym Sci 37:106–126. https://doi.org/10.1016/j.progpolymsci.2011.06.003

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  7. Burdick JA, Prestwich GD (2011) Hyaluronic acid hydrogels for biomedical applications. Adv Mater 23:H41–H56. https://doi.org/10.1002/adma.201003963

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  8. Wendels S, Avérous L (2021) Biobased polyurethanes for biomedical applications. Bioact Mater 6:1083–1106. https://doi.org/10.1016/j.bioactmat.2020.10.002

    Article  CAS  PubMed  Google Scholar 

  9. Pei X, Wang J, Cong Y, Fu J (2021) Recent progress in polymer hydrogel bioadhesives. J Polym Sci 59:1312–1337. https://doi.org/10.1002/pol.20210249

    Article  CAS  Google Scholar 

  10. Peppas NA, Hilt JZ, Khademhosseini A, Langer R (2006) Hydrogels in biology and medicine: from molecular principles to bionanotechnology. Adv Mater 18:1345–1360. https://doi.org/10.1002/adma.200501612

    Article  CAS  Google Scholar 

  11. MonleónPradas M, Gómez Ribelles JL, Serrano Aroca A, Gallego Ferrer G, Suay Antón J, Pissis P (2001) Porous poly(2-hydroxyethyl acrylate) hydrogels. Polymer 42:4667–4674. https://doi.org/10.1016/S0032-3861(00)00742-4

    Article  Google Scholar 

  12. Andreopoulos AG (1989) Properties of poly(2-hydroxyethyl acrylate) networks. Biomaterials 10:101–104. https://doi.org/10.1016/0142-9612(89)90040-9

    Article  CAS  PubMed  Google Scholar 

  13. Wu S, Wang TW, Du Y et al (2022) Tough, anti-freezing and conductive ionic hydrogels. NPG Asia Mater 14:65. https://doi.org/10.1038/s41427-022-00410-7

    Article  CAS  Google Scholar 

  14. Park SH, Shin HS, Park SN (2018) A novel pH-responsive hydrogel based on carboxymethyl cellulose/2-hydroxyethyl acrylate for transdermal delivery of naringenin. Carbohydr Polym 200:341–352. https://doi.org/10.1016/j.carbpol.2018.08.011

    Article  CAS  PubMed  Google Scholar 

  15. Kim JH, Sim SJ, Lee DH et al (2004) Preparation and properties of phea/chitosan composite hydrogel. Polym J 36:943–948. https://doi.org/10.1295/polymj.36.943

    Article  CAS  Google Scholar 

  16. Sánchez-Correa F, Vidaurre-Agut C, Serrano-Aroca Á, Campillo-Fernández AJ (2018) Poly(2-hydroxyethyl acrylate) hydrogels reinforced with graphene oxide: remarkable improvement of water diffusion and mechanical properties. J Appl Polym Sci 135:46158. https://doi.org/10.1002/app.46158

    Article  CAS  Google Scholar 

  17. Huang X, Li J, Luo J, Gao Q, Mao A, Li J (2021) Research progress on double-network hydrogels. Mater Today Commun 29:102757. https://doi.org/10.1016/j.mtcomm.2021.102757

    Article  CAS  Google Scholar 

  18. Tang L, Zhang D, Gong L et al (2019) Double-network physical cross-linking strategy to promote bulk mechanical and surface adhesive properties of hydrogels. Macromolecules 52:9512–9525. https://doi.org/10.1021/acs.macromol.9b01686

    Article  CAS  Google Scholar 

  19. Tanii H, Miki N, Hayashi M, Hashimoto K (1988) Cytotoxicity of acrylamide and related compounds to mouse neuroblastoma and rat schwannoma cells. Arch Toxicol 61:298–305. https://doi.org/10.1007/BF00364853

    Article  CAS  PubMed  Google Scholar 

  20. Bielecka-Kowalska A, Czarny P, Wigner P et al (2018) Ethylene glycol dimethacrylate and diethylene glycol dimethacrylate exhibits cytotoxic and genotoxic effect on human gingival fibroblasts via induction of reactive oxygen species. Toxicol Vitr 47:8–17. https://doi.org/10.1016/j.tiv.2017.10.028

    Article  CAS  Google Scholar 

  21. Seo Y, Kim BS, Balance WC, Aw N, Sutton B, Kong H (2020) Transparent and flexible electronics assembled with metallic nanowire-layered nondrying glycerogel. ACS Appl Mater Interfaces 12:13040–13050. https://doi.org/10.1021/acsami.9b21697

    Article  CAS  PubMed  Google Scholar 

  22. Zeng L, Gao G (2023) Stretchable organohydrogel with adhesion, self-healing, and environment-tolerance for wearable strain sensors. ACS Appl Mater Interfaces 15:28993–29003. https://doi.org/10.1021/acsami.3c05208

    Article  CAS  PubMed  Google Scholar 

  23. Gao Y, Zhou J, Xu F et al (2023) Highly stretchable, self-healable and self-adhesive double-network eutectogel based on gellan gum and polymerizable deep eutectic solvent for strain sensing. ChemistrySelect 8:e202204463. https://doi.org/10.1002/slct.202204463

    Article  CAS  Google Scholar 

  24. Zhang R, Liu C, Wei C et al (2023) Charge-transfer polymeric hydrogels with self-healing, injectable, thermosensitive, adhesive, and antibacterial properties for diabetic wound healing. Adv Mater Technol 8:2201527. https://doi.org/10.1002/admt.202201527

    Article  CAS  Google Scholar 

  25. Zhu J, Zhou H, Gerhard EM et al (2023) Smart bioadhesives for wound healing and closure. Bioact Mater 19:360–375. https://doi.org/10.1016/j.bioactmat.2022.04.020

    Article  PubMed  Google Scholar 

Download references

Acknowledgements

This work was supported by funding from the National Research Foundation of Korea (NRF) grants funded by the Korean Government (MSIT) (2021R1F1A1056201, 2021R1C1C1013157, 2021M3C1C3097647). This research was also supported by a grant from the Korea Health Technology R&D Project through the Korea Health Industry Development Institute (KHIDI), funded by the Ministry of Health & Welfare (No. HP23C0040) and the Korea Institute of Ceramic Engineering and Technology (KICET, 1415187241).

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Author notes

  1. Seo Yoon Kim, Ji-Won Kang and Eun Hui Jeong have contributed equally to this work.

Authors and Affiliations

  1. Bio-convergence R&D Division, Korea Institute of Ceramic Engineering and Technology (KICET), Chungbuk, 28160, Republic of Korea

    Seo Yoon Kim, Ji-Won Kang & Byoung Soo Kim

  2. Department of Materials Science and Engineering, Yonsei University, Seoul, 03722, Republic of Korea

    Seo Yoon Kim & Jang-Ung Park

  3. Department of Chemical and Biological Engineering, Korea University, Seoul, 02841, Republic of Korea

    Ji-Won Kang & Jinhan Cho

  4. Department of Chemical and Biological Engineering, Sookmyung Women’s University, Seoul, 04310, Republic of Korea

    Eun Hui Jeong & Jun Dong Park

  5. Research Institute of YOUNGWOO Co., Ltd, Gyeonggi-Do, 15880, Republic of Korea

    Taeho Kim & Ha Lim Jung

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Correspondence to Jun Dong Park or Byoung Soo Kim.

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Kim, S.Y., Kang, JW., Jeong, E.H. et al. Synthesis of bioadhesive PHEA hydrogels without crosslinkers through in situ polymerization and sustained mechanical mixing. Korea-Aust. Rheol. J. 36, 71–78 (2024). https://doi.org/10.1007/s13367-023-00084-9

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  • DOI: https://doi.org/10.1007/s13367-023-00084-9

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