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A tree-growing graphic model for asymmetrical phantom networks in polymeric gels undergoing dynamic mechanochemical coupling

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Abstract

Network structures of various polymers have significant effects on their mechanical properties; therefore, numerous studies have investigated the constitutive relationship between symmetrical network structures and their rubber elasticity in polymers. However, few studies have focused on asymmetrical network structures in polymers that undergo bond exchange reactions, self-assembly, or mechanochemical coupling—all of which are induced by transition probabilities of chemical bonding processes. In this study, an extended constraint junction and phantom network model is formulated using the tree-growing theory to establish a constitutive relationship between asymmetrical network structures and their rubber elasticity in polymers. A free-energy equation is further developed to explore working principles of configurational transitions on the dynamic rubber elasticity of symmetrical and asymmetrical network structures. The constitutive relationship between dynamic rubber elasticity and symmetrical and asymmetrical network structures has also been proposed for the gels undergoing mechanochemical and hydromechanical coupling. Finally, the effectiveness of this newly proposed tree-growing model has been verified by comparing with the classical affine network model, finite element analysis, and the experimental results of gels reported in literature.

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References

  1. Sun J Y, Zhao X, Illeperuma W R K, et al. Highly stretchable and tough hydrogels. Nature, 2012, 489: 133–136

    Article  Google Scholar 

  2. Zhang Y H, Cui C Y, Sun Y G, et al. A hyperbranched polymer-based water-resistant adhesive: Durable underwater adhesion and primer for anchoring anti-fouling hydrogel coating. Sci China Tech Sci, 2022, 65: 201–213

    Article  Google Scholar 

  3. Wei Z Z, Dong X, Zhang Y Q. A mechanically robust egg white hydrogel scaffold with excellent biocompatibility by three-step green processing. Sci China Tech Sci, 2022, 65: 1599–1612

    Article  Google Scholar 

  4. Na H, Kang Y W, Park C S, et al. Hydrogel-based strong and fast actuators by electroosmotic turgor pressure. Science, 2022, 376: 301–307

    Article  Google Scholar 

  5. Liu Z, Toh W, Ng T Y. Advances in mechanics of soft materials: A review of large deformation behavior of hydrogels. Int J Appl Mech, 2015, 7: 1530001

    Article  Google Scholar 

  6. Hua M, Wu S, Ma Y, et al. Strong tough hydrogels via the synergy of freeze-casting and salting out. Nature, 2021, 590: 594–599

    Article  Google Scholar 

  7. Arno M C, Inam M, Weems A C, et al. Exploiting the role of nanoparticle shape in enhancing hydrogel adhesive and mechanical properties. Nat Commun, 2020, 11: 1420

    Article  Google Scholar 

  8. Chen G Y, Guo Y, Hsiao S B, et al. Tough, conductive hydrogels with double-network based on hydrophilic polymer assistant well-dispersed carbon nanotube for innovative force sensor. Sci China Tech Sci, 2022, 65: 1160–1168

    Article  Google Scholar 

  9. Hua Y, Xia H, Jia L, et al. Ultrafast, tough, and adhesive hydrogel based on hybrid photocrosslinking for articular cartilage repair in water-filled arthroscopy. Sci Adv, 2021, 7: eabg0628

    Article  Google Scholar 

  10. Wang G, Zhang Q, Wang Q, et al. Bio-based hydrogel transducer for measuring human motion with stable adhesion and ultrahigh toughness. ACS Appl Mater Interfaces, 2021, 13: 24173–24182

    Article  Google Scholar 

  11. Gong J P, Katsuyama Y, Kurokawa T, et al. Double-network hydrogels with extremely high mechanical strength. Adv Mater, 2003, 15: 1155–1158

    Article  Google Scholar 

  12. Zhang X, Wang K, Hu J, et al. Role of a high calcium ion content in extending the properties of alginate dual-crosslinked hydrogels. J Mater Chem A, 2020, 8: 25390–25401

    Article  Google Scholar 

  13. Newham G, Evans S D, Ong Z Y. Mechanically tuneable physical nanocomposite hydrogels from polyelectrolyte complex templated silica nanoparticles for anionic therapeutic delivery. J Colloid Interface Sci, 2022, 617: 224–235

    Article  Google Scholar 

  14. Sun P, Zhang H, Xu D, et al. Super tough bilayer actuators based on multi-responsive hydrogels crosslinked by functional triblock copolymer micelle macro-crosslinkers. J Mater Chem B, 2019, 7: 2619–2625

    Article  Google Scholar 

  15. Gu S, Cheng G, Yang T, et al. Mechanical and rheological behavior of hybrid cross-linked polyacrylamide/cationic micelle hydrogels. Macromol Mater Eng, 2017, 302: 1700402

    Article  Google Scholar 

  16. Sarrigiannidis S O, Rey J M, Dobre O, et al. A tough act to follow: Collagen hydrogel modifications to improve mechanical and growth factor loading capabilities. Mater Today Bio, 2021, 10: 100098

    Article  Google Scholar 

  17. Slawinski M, Kaeek M, Rajmiel Y, et al. Acetic acid enables precise tailoring of the mechanical behavior of protein-based hydrogels. Nano Lett, 2022, 22: 6942–6950

    Article  Google Scholar 

  18. Chen K, Lin Q, Wang L, et al. An all-in-one tannic acid-containing hydrogel adhesive with high toughness, notch insensitivity, self-healability, tailorable topography, and strong, instant, and on-demand underwater adhesion. ACS Appl Mater Interfaces, 2021, 13: 9748–9761

    Article  Google Scholar 

  19. Shibaev A V, Kuklin A I, Torocheshnikov V N, et al. Double dynamic hydrogels formed by wormlike surfactant micelles and cross-linked polymer. J Colloid Interface Sci, 2022, 611: 46–60

    Article  Google Scholar 

  20. Li S, Zhou H, Li Y, et al. Mussel-inspired self-adhesive hydrogels by conducting free radical polymerization in both aqueous phase and micelle phase and their applications in flexible sensors. J Colloid Interface Sci, 2022, 607: 431–439

    Article  Google Scholar 

  21. Yang Y. Graph theory of viscoelastic and configurational properties of Gaussian chains. Macromol Theor Simul, 1998, 7: 521–549

    Article  Google Scholar 

  22. Yang Y, Qiu F, Zhang H, et al. The rouse dynamic properties of dendritic chains: A graph theoretical method. Macromolecules, 2017, 50: 4007–4021

    Article  Google Scholar 

  23. Xiang Y, Zhong D, Wang P, et al. A general constitutive model of soft elastomers. J Mech Phys Solids, 2018, 117: 110–122

    Article  MathSciNet  Google Scholar 

  24. Bergström J S, Boyce M C. Deformation of elastomeric networks: Relation between molecular level deformation and classical statistical mechanics models of rubber elasticity. Macromolecules, 2001, 34: 614–626

    Article  Google Scholar 

  25. Flory P J. Theory of elasticity of polymer networks. The effect of local constraints on junctions. J Chem Phys, 1977, 66: 5720–5729

    Article  Google Scholar 

  26. Kloczkowski A, Mark J E, Erman B. A diffused-constraint theory for the elasticity of amorphous polymer networks. 1. Fundamentals and stress-strain isotherms in elongation. Macromolecules, 1995, 28: 5089–5096

    Article  Google Scholar 

  27. Erman B, Monnerie L. Theory of elasticity of amorphous networks: Effect of constraints along chains. Macromolecules, 1989, 22: 3342–3348

    Article  Google Scholar 

  28. Cantwell G T, St-Onge G, Young J G. Inference, model selection, and the combinatorics of growing trees. Phys Rev Lett, 2021, 126: 038301

    Article  MathSciNet  Google Scholar 

  29. Rubinstein M, Colby R H. Polymer Physics. New York: Oxford University Press, 2003

    Book  Google Scholar 

  30. Cohen M H, Grest G S. Liquid-glass transition, a free-volume approach. Phys Rev B, 1979, 20: 1077–1098

    Article  Google Scholar 

  31. Dobrynin A V, Carrillo J M Y. Universality in nonlinear elasticity of biological and polymeric networks and gels. Macromolecules, 2011, 44: 140–146

    Article  Google Scholar 

  32. Treloar L R G. The Physics of Rubber Elasticity. New York: Oxford University, 1975

    Google Scholar 

  33. Fried J R. Polymer Science and Technology. New York: Pearson Education Press, 2014

    Google Scholar 

  34. Xiao L, Zhu J, Londono J D, et al. Mechano-responsive hydrogels crosslinked by block copolymer micelles. Soft Matter, 2012, 8: 10233–10237

    Article  Google Scholar 

  35. Huang H, Zhang X, Dong Z, et al. Nanocomposite conductive tough hydrogel based on metal coordination reinforced covalent Pluronic F-127 micelle network for human motion sensing. J Colloid Interface Sci, 2022, 625: 817–830

    Article  Google Scholar 

  36. Xu C, Lee W, Dai G, et al. Highly elastic biodegradable single-network hydrogel for cell printing. ACS Appl Mater Interfaces, 2018, 10: 9969–9979

    Article  Google Scholar 

  37. Shen B, Peng W, Su B, et al. Elastic-electric coefficient-sensitive hydrogel sensors toward sweat detection. Anal Chem, 2022, 94: 1910–1917

    Article  Google Scholar 

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Correspondence to HaiBao Lu or Yong-Qing Fu.

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This work was supported by the National Natural Science Foundation of China (Grant No. 12172107).

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Shi, W., Zhou, J., Lu, H. et al. A tree-growing graphic model for asymmetrical phantom networks in polymeric gels undergoing dynamic mechanochemical coupling. Sci. China Technol. Sci. 67, 558–567 (2024). https://doi.org/10.1007/s11431-023-2430-3

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  • DOI: https://doi.org/10.1007/s11431-023-2430-3

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