journal article·2021-12Open access

A universal method to easily design tough and stretchable hydrogels

Chisa Norioka, Yuino Inamoto, Chika Hajime, Akifumi Kawamura, Takashi Miyata

NPG Asia Materials· Volume 13· Issue 1

Abstract

Abstract Hydrogels are flexible materials that have high potential for use in various applications due to their unique properties. However, their applications are greatly restricted by the low mechanical performance caused by high water content and inhomogeneous networks. This paper reports a universal strategy for easily preparing hydrogels that are tough and stretchable without any special structures or complicated processes. Our strategy involves tuning the polymerization conditions to form networks with many polymer chain entanglements to achieve energy dissipation. Tough and stretchable hydrogels can be prepared by free radical polymerization with a high monomer concentration and low cross-linker content to optimize the balance between physical and chemical cross-links by entanglements and covalent bonds, respectively. The strategy of using polymer chain entanglements for energy dissipation allows us to overcome the limitation of low mechanical performance, which leads to the wide practical use of hydrogels.
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Research context

OpenAlex topics: Hydrogels: synthesis, properties, applications · Advanced Sensor and Energy Harvesting Materials · Advanced Materials and Mechanics

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (36)

Show source-provided references
1. Hoffman, A. S. Hydrogels for biomedical applications. Adv. Drug Deliv. Rev. 54, 3–12 (2002).10.1016/S0169-409X(01)00239-3 ↗
2. Peppas, N. A., Hilt, J. Z., Khademhosseini, A. & Langer, R. Hydrogels in biology and medicine: from molecular principles to bionanotechnology. Adv. Mater. 18, 1345–1360 (2006).10.1002/adma.200501612 ↗
3. Li, J. & Mooney, D. J. Designing hydrogels for controlled drug delivery. Nat. Rev. Mater. 1, 1–17 (2016).
4. Zhang, Y. S. & Khademhosseini, A. Advances in engineering hydrogels. Science 356, eaaf3627 (10pp) (2017).10.1126/science.aaf3627 ↗
5. Buwalda, S. J., Vermonden, T. & Hennink, W. E. Hydrogels for therapeutic delivery: current developments and future directions. Biomacromolecules 18, 316–330 (2017).10.1021/acs.biomac.6b01604 ↗
6. Lake, G. J. & Thomas, A. G. The strength of highly elastic materials. Proc. R. Soc. A 300, 108–119 (1967).
7. Lake, G. J. Fatigue and fracture of elastomers. Rubber Chem. Technol. 68, 435–460 (1995).10.5254/1.3538750 ↗
8. Simha, N. K., Carlson, C. S. & Lewis, J. L. Evaluation of fracture toughness of cartilage by micropenetration. J. Mater. Sci. Mater. Med. 14, 631–639 (2003).
9. Okumura, Y. & Ito, K. The polyrotaxane gel: a topological gel by figure-of-eight cross-links. Adv. Mater. 13, 485–487 (2001).10.1002/1521-4095(200104)13:7<485::AID-ADMA485>3.0.CO;2-T ↗
10. Noda, Y., Hayashi, Y. & Ito, K. From topological gels to slide-ring materials. J. Appl. Polym. Sci. 131, 40509 (2014). (9pp).10.1002/app.40509 ↗
11. Haraguchi, K. & Takehisa, T. Nanocomposite hydrogels: a unique organic-inorganic network structure with extraordinary mechanical, optical, and swelling/de-swelling properties. Adv. Mater. 14, 1120–1124 (2002).10.1002/1521-4095(20020816)14:16<1120::AID-ADMA1120>3.0.CO;2-9 ↗
12. Gong, J. P., Katsuyama, Y., Kurokawa, T. & Osada, Y. Double-network hydrogels with extremely high mechanical strength. Adv. Mater. 15, 1155–1158 (2003).10.1002/adma.200304907 ↗
13. Gong, J. P. Why are double network hydrogels so tough? Soft Matter 6, 2583–2590 (2010).10.1039/b924290b ↗
14. Nakajima, T. Generalization of the sacrificial bond principle for gel and elastomer toughening. Polym. J. 49, 447–485 (2017).10.1038/pj.2017.12 ↗
15. Sun, J.-Y. et al. Highly stretchable and tough hydrogels. Nature 489, 133–136 (2012).10.1038/nature11409 ↗
16. Ducrot, E., Chen, Y., Bulters, M., Sijbesma, R. P. & Creton, C. Toughening elastomers with sacrificial bonds and watching them break. Science 344, 186–189 (2014).10.1126/science.1248494 ↗
17. Imran, A. B. et al. Extremely stretchable thermosensitive hydrogels by introducing slide-ring polyrotaxane cross-linkers and ionic groups into the polymer network. Nat. Commun. 5, 5124 (2014). (8pp).10.1038/ncomms6124 ↗
18. Sun, G., Li, Z., Liang, R., Weng, L.-T. & Zhang, L. Super stretchable hydrogel achieved by non-aggregated spherulites with diameters <5 nm. Nat. Commun. 7, 12095 (2016). (8pp).10.1038/ncomms12095 ↗
19. Filippidi, E. et al. Toughening elastomers using mussel-inspired iron-catechol complexes. Science 358, 502–505 (2017).10.1126/science.aao0350 ↗
20. Gotoh, H. et al. Optically transparent, high-toughness elastomer using a polyrotaxane cross-linker as a molecular pulley. Sci. Adv. 4, eaat7629 (2018).10.1126/sciadv.aat7629 ↗
21. Ke, H. et al. Shear-induced assembly of a transient yet highly stretchable hydrogel based on pseudopolyrotaxanes. Nat. Chem. 11, 470–477 (2019).10.1038/s41557-019-0235-8 ↗
22. Matsuda, T., Kawakami, R., Namba, R., Nakajima, T. & Gong, J. P. Mechanoresponsive self-growing hydrogels inspired by muscle training. Science 363, 504–508 (2019).10.1126/science.aau9533 ↗
23. Sinawang, G., Osaki, M., Takashima, Y., Yamaguchi, H. & Harada, A. Biofunctional hydrogels based on host-guest interactions. Polym. J. 52, 839–859 (2020).10.1038/s41428-020-0352-7 ↗
24. Nakahata, M., Takashima, Y. & Harada, A. Highly flexible, tough, and self-Healing supramolecular polymeric materials using host–guest interaction. Macromol. Rapid Commun. 37, 86–92 (2016).10.1002/marc.201500473 ↗
25. Miyata, T. Preparation of smart soft materials using molecular complexes. Polym. J. 42, 277–289 (2010).10.1038/pj.2010.12 ↗
26. Miyata, T., Asami, N. & Uragami, T. A reversibly antigen-responsive hydrogel. Nature 399, 766–769 (1999).10.1038/21619 ↗
27. Miyata, T., Jige, M., Nakaminami, T. & Uragami, T. Tumor marker-responsive behavior of gels prepared by biomolecular imprinting. PNAS 103, 1190–1193 (2006).10.1073/pnas.0506786103 ↗
28. Matsumoto, K., Sakikawa, N. & Miyata, T. Thermo-responsive gels that absorb moisture and ooze water. Nat. Commun. 9, 2315 (2018).10.1038/s41467-018-04810-8 ↗
29. Kavanagh, G. M. & Ross-Murphy, S. B. Rheological characterisation of polymer gels. Prog. Polym. Sci. 23, 533–562 (1998).10.1016/S0079-6700(97)00047-6 ↗
30. Norioka, C., Kawamura, A. & Miyata, T. Mechanical and responsive properties of temperature-responsive gels prepared via atom transfer radical polymerization. Polym. Chem. 8, 6050–6057 (2017).10.1039/C7PY01323J ↗
31. Sakai, T. et al. Design and fabrication of a high-strength hydrogel with ideally homogeneous network structure from tetrahedron-like macromonomers. Macromolecules 41, 5379–5384 (2008).10.1021/ma800476x ↗
32. Rivlin, R. S. & Thomas, A. G. Rupture of rubber. I. Characteristic energy for tearing. J. Poly. Sci. 10, 291–318 (1953).10.1002/pol.1953.120100303 ↗
33. Tanaka, Y. et al. Determination of fracture energy of high strength double network hydrogels. J. Phys. Chem. B 109, 11559–11562 (2005).10.1021/jp0500790 ↗
34. Liu, C. et al. Unusual fracture behavior of slide-ring gels with movable cross-links. ACS Macro Lett. 6, 1409–1413 (2017).10.1021/acsmacrolett.7b00729 ↗
35. Xue, W., Huglin, M. B. & Jones, T. G. J. Swelling and network parameters of crosslinked thermoreversible hydrogels of poly(N-ethylacrylamide). Eur. Polym. J. 41, 239–248 (2005).10.1016/j.eurpolymj.2004.10.005 ↗
36. Iwasaki, Y. & Ishihara, K. Cell membrane-inspired phospholipid polymers for developing medical devices with excellent biointerfaces. Sci. Technol. Adv. Mater. 13, 064101 (2012). (14pp).10.1088/1468-6996/13/6/064101 ↗