Skip to main content
Log in

An autonomous self-healing hydrogel with high polydopamine content for improved tensile strength

  • Polymers & biopolymers
  • Published:
Journal of Materials Science Aims and scope Submit manuscript

Abstract

Biocompatible polydopamine–polyacrylamide (PDA–PAM) hydrogel has good self-healing performance. However, there is a trade-off between the self-healing ability and the mechanical strength. Excellent self-healing often results in the poor mechanical strength, which limits the application in load-bearing field. Here, we successfully prepare PDA–PAM hydrogels with improved strength and good self-healing properties simultaneously. By adjusting the pH and ammonium persulfate (APS) content of the hydrogel solution to promote dopamine (DA) polymerization, PDA–PAM hydrogel with a high content of polydopamine (PDA) is developed, which demonstrates excellent self-healing properties and mechanical strength. In particular, the PDA–PAM hydrogel with high PDA content (DA/AM = 5%) has a tensile strength of 16 kPa and the tensile strength spontaneously recovers 96% in 2 h after the tensile fracture. The obtained hydrogel also displays good biocompatibility.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Figure 1
Figure 2
Figure 3
Figure 4
Figure 5
Figure 6
Figure 7

Similar content being viewed by others

References

  1. Jing X, Mi HY, Lin YJ, Enriquez E, Peng XF, Turng LS (2018) Highly stretchable and biocompatible strain sensors based on mussel-inspired super-adhesive self-healing hydrogels for human motion monitoring. ACS Appl Mater Interfaces 10(24):20897–20909

    CAS  Google Scholar 

  2. Han YY, Wu XD, Zhang XX, Lu CH (2017) Self-healing, highly sensitive electronic sensors enabled by metal–ligand coordination and hierarchical structure design. ACS Appl Mater Interfaces 9(23):20106–20114

    CAS  Google Scholar 

  3. Highley CB, Rodell CB, Burdick JA (2015) Direct 3D printing of shear-thinning hydrogels into self-healing hydrogels. Adv Mater 27(34):5075–5079

    CAS  Google Scholar 

  4. Huebsch N, Kearney CJ, Zhao XH, Kim J, Cezar CA, Suo Z, Mooney DJ (2014) Ultrasound-triggered disruption and self-healing of reversibly cross-linked hydrogels for drug delivery and enhanced chemotherapy. Proc Natl Acad Sci USA 111(27):9762–9767

    CAS  Google Scholar 

  5. Liu SQ, Zheng RM, Chen S, Wu YH, Liu HZ, Wang PP, Deng ZF, Liu L (2018) A compliant, self-adhesive and self-healing wearable hydrogel as epidermal strain sensor. J Mater Chem C 6(15):4183–4190

    CAS  Google Scholar 

  6. Liu SJ, Li L (2017) Ultrastretchable and Self-healing double-network hydrogel for 3d printing and strain sensor. ACS Appl Mater Interfaces 9(31):26429–26437

    CAS  Google Scholar 

  7. Krogsgaard M, Hansen MR, Birkedal H (2014) Metals & polymers in the mix: fine-tuning the mechanical properties & color of self-healing mussel-inspired hydrogels. J Mater Chem B 2(47):8292–8297

    CAS  Google Scholar 

  8. Hohlbein N, Shaaban A, Schmidt AM (2015) Remote-controlled activation of self-healing behavior in magneto-responsive ionomeric composites. Polymer 69:301–309

    CAS  Google Scholar 

  9. Yang L, Wang ZH, Fei GX, Xia HS (2017) Polydopamine particles reinforced poly(vinyl alcohol) hydrogel with NIR light triggered shape memory and self-healing capability. Macromol Rapid Commun 38(23):1700421

    Google Scholar 

  10. Ryplida B, Lee KD, In I, Park SY (2019) Light-induced swelling-responsive conductive, adhesive, and stretchable wireless film hydrogel as electronic artificial skin. Adv Funct Mater 29(32):1903209

    Google Scholar 

  11. Kang MM, Liu SL, Oderinde O, Yao F, Fu GD, Zhang ZH (2018) Template method for dual network self-healing hydrogel with conductive property. Mater Des 148:96–103

    CAS  Google Scholar 

  12. Wang WD, Narain R, Zeng HB (2018) Rational design of self-healing tough hydrogels: a mini review. Front Chem 6:497

    CAS  Google Scholar 

  13. Han LL, Liu MF, Yan B, Li YS, Lan J, Shi LY, Ra R (2020) Polydopamine/polystyrene nanocomposite double-layer strain sensor hydrogel with mechanical, self-healing, adhesive and conductive properties. Mater Sci Eng C 109:110567

    CAS  Google Scholar 

  14. Holten-Andersen N, Harrington MJ, Birkedal H, Lee BP, Messersmith PB, Lee KYC, Waite JH (2011) pH-induced metal-ligand cross-links inspired by mussel yield self-healing polymer networks with near-covalent elastic moduli. Proc Natl Acad Sci USA 108(7):2651–2655

    CAS  Google Scholar 

  15. Zhou HW, Li SL, Liu HB, Zheng BH, Jin XL, Ma AJ, Chen WX (2020) High-performance flexible sensors of self-healing, reversibly adhesive, and stretchable hydrogels for monitoring large and subtle strains. Macromol Mater Eng 305(2):1900621

    CAS  Google Scholar 

  16. Wang W, Narain R, Zeng H (2018) Rational design of self-healing tough hydrogels: a mini review. Front Chem 6:497

    CAS  Google Scholar 

  17. Han L, Yan LW, Wang KF, Fang LM, Zhang HP, Tang YH, Ding YH, Weng LT, Xu JL, Weng J, Liu YJ, Ren FZ, Lu X (2017) Tough, self-healable and tissue-adhesive hydrogel with tunable multifunctionality. NPG Asia Mater 9(4):e372–e372

    CAS  Google Scholar 

  18. Chan BK, Wippich CC, Wu CJ, Sivasankar PM, Robust GS (2012) Semi-interpenetrating hydrogels from poly (ethylene glycol) and collagen for elastomeric tissue scaffolds. Macromol Biosci 12(11):1490–1501

    CAS  Google Scholar 

  19. Kang HG, Kim SY, Lee YM (2006) Novel porous gelatin scaffolds by overrun/particle leaching process for tissue engineering applications. J Biomed Mater Res Part B 79(2):388–397

    Google Scholar 

  20. Han LL, He Y, An R, Wang XD, Zhang YL, Shi LY, Ran R (2019) Mussel-inspired, robust and self-healing nanocomposite hydrogels: effective reusable absorbents for removal both anionic and cationic dyes. Coll Surf A 569:18–27

    CAS  Google Scholar 

  21. Xu J, Wang G, Wu Y, Ren X, Gao G (2019) Ultrastretchable wearable strain and pressure sensors based on adhesive, tough, and self-healing hydrogels for human motion monitoring. ACS Appl Mater Interfaces 11(28):25613–32562

    CAS  Google Scholar 

  22. Han L, Lu X, Wang MH, Gan DL, Deng WL, Wang KF, Fang LM, Liu KZ, Chan CW, Tang YH, Weng LT, Yuan HP (2017) A mussel-inspired conductive, self-adhesive, and self-healable tough hydrogel as cell stimulators and implantable bioelectronics. Small 13(2):1601916

    Google Scholar 

  23. Zhang HJ, Xia HS, Zhao Y (2012) Poly (vinyl alcohol) hydrogel can autonomously self-heal. ACS Macro Lett 1(11):1233–1236

    CAS  Google Scholar 

  24. Talebian S, Mehrali M, Taebnia N, Pennisi CP, Kadumudi FB, Foroughi J, Hasany M, Nikkhah M, Akbari M, Orive G, Pirouz AD (2019) Self-healing hydrogels: The next paradigm shift in tissue engineering? Adv Sci 6(16):1801664

    Google Scholar 

  25. Gao Y, Du HY, Xie ZJ, Li MM, Zhu JJ, Xu JW, Zhang LB, Tao J, Zhu JT (2019) Self-adhesive photothermal hydrogel films for solar-light assisted wound healing. J Mater Chem B 7(23):3644–3651

    CAS  Google Scholar 

  26. Suneetha M, Rao KM, Han SS (2019) Mussel-inspired cell/tissue-adhesive, hemostatic hydrogels for tissue engineering applications. ACS Omega 4(7):12647–12656

    CAS  Google Scholar 

  27. Zhao Z, Li L, Geleta GS, Ma L, Wang Z (2017) Polyacrylamide-phytic acid-polydopamine conducting porous hydrogel for efficient removal of water-soluble dyes. Sci Rep 7(1):1–10

    Google Scholar 

  28. Xia Y, Xia YM, Wu YP, Yu T, Xue SS, Guo ML, Li JL, Li ZY (2019) Multifunctional glycerol–water hydrogel for biomimetic human skin with resistance memory function. ACS Appl Mater Interfaces 11(23):21117–21125

    CAS  Google Scholar 

  29. Feng ZB, Zuo HL, Hu J, Gao WS, Yu B, Ning NY, Tian M, Zhang LQ (2020) Mussel-inspired highly stretchable, tough nanocomposite hydrogel with self-healable and near-infrared actuated performance. Ind Eng Chem Res 59(1):166–174

    CAS  Google Scholar 

  30. Fang YZ, Yang S, Wu GY (2002) Free radicals, antioxidants, and nutrition. Nutrition 18:872–879

    CAS  Google Scholar 

  31. Herlinger E, Jameson RF, Linert W (1995) Spontaneous autoxidation of dopamine. J Chem Soc Perkin Trans 2:259–263

    Google Scholar 

  32. Wei Q, Zhang F, Li J, Li B, Zhao C (2010) Oxidant-induced dopamine polymerization for multifunctional coatings. Polym Chem 1(9):1430–1433

    CAS  Google Scholar 

  33. Thakur A, Ranote S, Kumar D, Bhardwaj KK, Gupta R, Chauhan GS (2018) Synthesis of a pegylated dopamine ester with enhanced antibacterial and antifungal activity. ACS Omega 3(7):7925–7933

    CAS  Google Scholar 

  34. Muller M, Kessler B (2011) Deposition from dopamine solutions at Ge substrates: an in situ ATR-FTIR study. Langmuir 27(20):12499–12505

    CAS  Google Scholar 

  35. Han LL, He Y, An R, Wang X, Zhang Y, Shi L, Ran R (2019) Mussel-inspired, robust and self-healing nanocomposite hydrogels: effective reusable absorbents for removal both anionic and cationic dyes. Coll Surf A 569:18–27

    CAS  Google Scholar 

  36. Shao CY, Wang M, Meng L, Chang HL, Wang B, Xu F, Yang J, Wan PB (2018) Mussel-inspired cellulose nanocomposite tough hydrogels with synergistic self-healing, adhesive, and strain-sensitive properties. Chem Mater 30(9):3110–3121

    CAS  Google Scholar 

  37. Kim UJ, Park J, Kim HJ, Wada M, Kapla DL (2005) Three-dimensional aqueous-derived biomaterial scaffolds from silk fibroin. Biomaterials 26(15):2775–2785

    CAS  Google Scholar 

  38. Ikeda T, Ikeda K, Yamamoto K, Ishizaki H, Yoshizawa Y, Yanagiguchi K, Yamada S, Hayashi Y (2014) Fabrication and characteristics of chitosan sponge as a tissue engineering scaffold. BioMed Res Int 2014:1–8

    Google Scholar 

  39. Wang ZW, Zhou HW, Lai JL, Yan B, Liu HB, Jin XL, Ma AJ, Zhang G, Zhao WF, Chen WX (2018) Extremely stretchable and electrically conductive hydrogels with dually synergistic networks for wearable strain sensors. J Mater Chem C 6(34):9200–9207

    Google Scholar 

  40. Anseth KS, Bowman CN, Brannonpeppas L (1996) Mechanical properties of hydrogels and their experimental determination. Biomaterials 17:1647–1657

    CAS  Google Scholar 

  41. Bai HY, Li ZK, Zhang SW, Wang W, Dong WF (2018) Interpenetrating polymer networks in polyvinyl alcohol/cellulose nanocrystals hydrogels to develop absorbent materials. Carbohydr Polym 200:468–476

    CAS  Google Scholar 

  42. Han L, Zhang YN, Lu X, Wang KF, Wang ZM, Zhang HP (2016) Polydopamine nanoparticles modulating stimuli-responsive pnipam hydrogels with cell/tissue adhesiveness. ACS Appl Mater Interfaces 8(42):29088–29100

    CAS  Google Scholar 

  43. Anjum S, Gurave PM, Badiger MV, Torris ATA, Tiwari N, Gupta B (2017) Design and development of trivalent aluminum ions induced self-healing polyacrylic acid novel hydrogels. Polymer 126:196–205

    CAS  Google Scholar 

  44. Chen MS, Gong GS, Zhou L, Zhang FA (2017) Facile fabrication of a magnetic self-healing poly (vinyl alcohol) composite hydrogel. RSC Adv 7(35):21476–21483

    CAS  Google Scholar 

  45. Jia YG, Jin JH, Liu S, Ren L, Luo JT, Zhu XX (2012) Self-healing hydrogels of low molecular weight poly (vinyl alcohol) assembled by host−guest recognition. J Appl Polym Sci 125(4):2890–2895

    Google Scholar 

  46. Baron RI, Culica ME, Biliuta G, Bercea M, Gherman S, Zavastin D, Ochiuz L, Avadanei M, Coseri S (2019) Physical hydrogels of oxidized polysaccharides and poly (vinyl alcohol) for wound dressing applications. Materials 12(9):1569

    CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by National Key R&D Program of China (2018YFA0704104, 2018YFA0704103), NSFC (U1908233, 51775541, 11772086), NSFC of Liaoning Province (2019-KF-02-01).

Author information

Authors and Affiliations

Authors

Contributions

JXH: Conceptualization, Methodology, Validation, Investigation, Writing-original draft. HL: Cytotoxicity Test. XGY: Formal Analysis. SWD: Writing-original draft. WZ: Conceptualization, Funding Acquisition, Supervision, Project Administration. CWW: Conceptualization, Funding Acquisition, Supervision. All authors have given approval to the final version of the manuscript.

Corresponding authors

Correspondence to Wei Zhang or Chengwei Wu.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

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.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Huang, J., Zhang, W., Li, H. et al. An autonomous self-healing hydrogel with high polydopamine content for improved tensile strength. J Mater Sci 55, 17255–17265 (2020). https://doi.org/10.1007/s10853-020-05252-8

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10853-020-05252-8

Navigation