Citation: Yi Sun, Yong-Yuan Ren, Qi Li, Rong-Wei Shi, Yin Hu, Jiang-Na Guo, Zhe Sun, Feng Yan. Conductive, Stretchable, and Self-healing Ionic Gel Based on Dynamic Covalent Bonds and Electrostatic Interaction[J]. Chinese Journal of Polymer Science, ;2019, 37(11): 1053-1059. doi: 10.1007/s10118-019-2325-x shu

Conductive, Stretchable, and Self-healing Ionic Gel Based on Dynamic Covalent Bonds and Electrostatic Interaction

  • Corresponding author: Feng Yan, fyan@suda.edu.cn
  • † These authors contributed equally to this work
  • Received Date: 28 May 2019
    Revised Date: 25 June 2019
    Accepted Date: 26 June 2019
    Available Online: 12 September 2019

  • Integrating multiple functions into one gel that can be widely applied to electronic devices as well as chemical and biomedical engineering remains a big challenge. Here, a multifunctional ionic liquid/dynamic covalent bonds (ionic/DCB) type gel was designed and synthesized via one-pot polymerization. With the assistance of electrostatic interaction provided by the imidazolium cations of IL and the reversible DCB of boronic ester, as-prepared ionic/DCB gel showed good stretchable properties and high ionic conductivity at ambient conditions. In addition, the electrostatic interaction between imidazolium cations and sulfonate anions and the reversible DCB led to enhanced chain mobility and thereby excellent self-healing properties. Particularly, sulfonate anions in ionic/DCB gel could alleviate the migration of electronegative polysulfide and promote the transportation of electropositive lithium ion in lithium-sulfur battery system. Therefore, this work provides a new insight to promote the current research on self-healing gels, hopefully expanding their applications in electronic devices.
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    1. [1]

      Cordier, P.; Tournilhac, F.; Soulie-Ziakovic, C.; Leibler, L. Self-healing and thermoreversible rubber from supramolecular assembly. Nature 2008, 451, 977.  doi: 10.1038/nature06669

    2. [2]

      By, E.; Ghosh, S. K. Self-healing materials. Adv. Mater. 2010, 22, 5424.  doi: 10.1002/adma.201003036

    3. [3]

      Brown, E. N.; White, S. R.; Sottos, N. R. Microcapsule induced toughening in a self-healing polymer composite. J. Mater. Sci. 2004, 39, 1703.  doi: 10.1023/B:JMSC.0000016173.73733.dc

    4. [4]

      Yang, L.; Lu, L.; Zhang, C. Highly stretchable and self-healing hydrogels based on poly(acrylic acid) and functional POSS. Chinese J. Polym. Sci. 2016, 34, 185.  doi: 10.1007/s10118-016-1744-1

    5. [5]

      Wathier, M.; Grinstaff, M. W. Synthesis and creep-recovery behavior of a neat viscoelastic polymeric network formed through electrostatic interactions. Macromolecules 2010, 43, 9529.  doi: 10.1021/ma101506p

    6. [6]

      Zhang, Y.; Liang, L.; Chen, Y.; Chen, X. M.; Liu, Y. Construction and efficient dye adsorption of supramolecular hydrogels by cyclodextrin of pseudorotaxane and clay. Soft Matter 2018, 15, 73.  doi: 10.1039/c8sm02203h

    7. [7]

      Rahman, M. A.; Penco, M.; Peroni, I.; Ramorino, G.; Grande, A. M.; Di Landro, L. Self-repairing systems based on ionomers and epoxidized natural rubber blends. ACS Appl. Mater. Interfaces 2011, 3, 4865.  doi: 10.1021/am201417h

    8. [8]

      Luan, Y.; Zhang, X.; Jiang, S.; Chen, J.; Lyu, Y. Self-healing supramolecular polymer composites by hydrogen bonding interactions between hyperbranched polymer and graphene oxide. Chinese J. Polym. Sci. 2018, 36, 584.  doi: 10.1007/s10118-018-2025-y

    9. [9]

      Liu, C.; Zhang, A.; Ye, L.; Feng, Z. Self-healing biodegradable poly(urea-urethane) elastomers based on hydrogen bonding interactions. Chinese J. Polym. Sci. 2013, 31, 251.  doi: 10.1007/s10118-013-1211-1

    10. [10]

      Zhang, Q.; Zhu, X.; Li, C.-H.; Cai, Y.; Jia, X.; Bao, Z. Disassociation and reformation under strain in polymer with dynamic metal-ligand coordination cross-linking. Macromolecules 2019, 52, 660.  doi: 10.1021/acs.macromol.8b02414

    11. [11]

      Burnworth, M.; Tang, L.; Kumpfer, J. R.; Duncan, A. J.; Beyer, F. L.; Fiore, G. L.; Rowan, S. J.; Weder, C. Optically healable supramolecular polymers. Nature 2011, 472, 334.  doi: 10.1038/nature09963

    12. [12]

      Yang, Q.; Wang, P.; Zhao, C.; Wang, W.; Yang, J.; Liu, Q. Light-switchable self-healing hydrogel based on host-guest macro-crosslinking. Macromol. Rapid Commun. 2017, 38, 1600741.  doi: 10.1002/marc.v38.6

    13. [13]

      Nakahata, M.; Takashima, Y.; Harada, A. Highly flexible, tough, and self-healing supramolecular polymeric materials using host-guest interaction. Macromol. Rapid Commun. 2016, 37, 86.  doi: 10.1002/marc.v37.1

    14. [14]

      Guan, Y.; Zhang, Y. Boronic acid-containing hydrogels: synthesis and their applications. Chem. Soc. Rev. 2013, 42, 8106.  doi: 10.1039/c3cs60152h

    15. [15]

      Cromwell, O. R.; Chung, J.; Guan, Z. Malleable and self-healing covalent polymer networks through tunable dynamic boronic ester bonds. J. Am. Chem. Soc. 2015, 137, 6492.  doi: 10.1021/jacs.5b03551

    16. [16]

      Yang, W. J.; Tao, X.; Zhao, T.; Weng, L.; Kang, E. T.; Wang, L. Antifouling and antibacterial hydrogel coatings with self-healing properties based on a dynamic disulfide exchange reaction. Polym. Chem. 2015, 6, 7027.  doi: 10.1039/C5PY00936G

    17. [17]

      Oku, T.; Furusho, Y.; Takata, T. A concept for recyclable cross-linked polymers: topologically networked polyrotaxane capable of undergoing reversible assembly and disassembly. Angew. Chem. Int. Ed. 2004, 43, 966.  doi: 10.1002/(ISSN)1521-3773

    18. [18]

      Wang, L.; Deng, F.; Wang, W.; Li, A.; Lu, C.; Chen, H.; Wu, G.; Nan, K.; Li, L. Construction of injectable self-healinng macroporous hydrogels via a template-free method for tissue engineering and drug delivery. ACS Appl. Mater. Interfaces 2018, 10, 36721.  doi: 10.1021/acsami.8b13077

    19. [19]

      Kang, J.; Son, D.; Wang, G. N.; Liu, Y.; Lopez, J.; Kim, Y.; Oh, J. Y.; Katsumata, T.; Mun, J.; Lee, Y.; Jin, L.; Tok, J. B.; Bao, Z. Tough and water-insensitive self-healing elastomer for robust electronic skin. Adv. Mater. 2018, 30, 1706846.  doi: 10.1002/adma.v30.13

    20. [20]

      Guo, Y.; Zheng, K.; Wan, P. A flexible stretchable hydrogel electrolyte for healable all-in-one configured supercapacitors. Small 2018, 14, 1704497.  doi: 10.1002/smll.201704497

    21. [21]

      Zuo, X.; Ma, X.; Wu, J.; Deng, X.; Xiao, X.; Liu, J.; Nan, J. Self-supporting ethyl cellulose/poly(vinylidene fluoride) blended gel polymer electrolyte for 5 V high-voltage lithium-ion batteries. Electrochim. Acta 2018, 271, 582.  doi: 10.1016/j.electacta.2018.03.195

    22. [22]

      He, Y.; Liao, S.; Jia, H.; Cao, Y.; Wang, Z.; Wang, Y. A self-healing electronic sensor based on thermal-sensitive fluids. Adv. Mater. 2015, 27, 4622.  doi: 10.1002/adma.v27.31

    23. [23]

      Shao, C.; Chang, H.; Wang, M.; Xu, F.; Yang, J. High-strength, tough, and self-healing nanocomposite physical hydrogels based on the synergistic effects of dynamic hydrogen bond and dual coordination bonds. ACS Appl. Mater. Interfaces 2017, 9, 28305.  doi: 10.1021/acsami.7b09614

    24. [24]

      Pu, W.; Jiang, F.; Chen, P.; Wei, B. A POSS based hydrogel with mechanical robustness, cohesiveness and a rapid self-healing ability by electrostatic interaction. Soft Matter 2017, 13, 5645.  doi: 10.1039/C7SM01492A

    25. [25]

      Chen, W. P.; Hao, D. Z.; Hao, W. J.; Guo, X. L.; Jiang, L. Hydrogel with ultrafast self-healing property both in air and underwater. ACS Appl. Mater. Interfaces 2018, 10, 1258.  doi: 10.1021/acsami.7b17118

    26. [26]

      Xu, D.; Guo, J.; Yan, F. Porous ionic polymers: design, synthesis, and applications. Prog. Polym. Sci. 2018, 79, 121.  doi: 10.1016/j.progpolymsci.2017.11.005

    27. [27]

      Zhao, Q.; Zhang, P.; Antonietti, M.; Yuan, J. Poly(ionic liquid) complex with spontaneous micro-/mesoporosity: template-free synthesis and application as catalyst support. J. Am. Chem. Soc. 2012, 134, 11852.  doi: 10.1021/ja303552p

    28. [28]

      Qian, W.; Texter, J.; Yan, F. Frontiers in poly(ionic liquid)s: syntheses and applications. Chem. Soc. Rev. 2017, 46, 1124.  doi: 10.1039/C6CS00620E

    29. [29]

      Ren, Y.; Zhang, J.; Chen, F.; Yan, F. Porous poly(ionic liquid) membranes as efficient and recyclable absorbents for heavy metal ions. Macromol. Rapid Commun. 2017, 38, 1700151.  doi: 10.1002/marc.v38.14

    30. [30]

      Guo, P.; Su, A.; Wei, Y.; Liu, X.; Li, Y.; Guo, F.; Li, J.; Hu, Z.; Sun, J. Healable, highly conductive, flexible, and nonflammable supramolecular ionogel electrolytes for lithium-ion batteries. ACS Appl. Mater. Interfaces 2019, 11, 19413.  doi: 10.1021/acsami.9b02182

    31. [31]

      Guo, P.; Zhang, H.; Liu, X.; Sun, J. Counteranion-mediated intrinsic healing of poly(ionic liquid) copolymers. ACS Appl. Mater. Interfaces 2018, 10, 2105.  doi: 10.1021/acsami.7b16880

    32. [32]

      Suckow, M.; Mordvinkin, A.; Roy, M.; Singha, N. K.; Heinrich, G.; Voit, B.; Saalwächter, K.; Böhme, F. Tuning the properties and self-healing behavior of ionically modified poly(isobutylene-co-isoprene) rubber. Macromolecules 2017, 51, 468.  doi: 10.1021/acs.macromol.7b02287

    33. [33]

      Cui, J.; Nie, F. M.; Yang, J. X.; Pan, L.; Ma, Z.; Li, Y. S. Novel imidazolium-based poly(ionic liquid)s with different counterions for self-healing. J. Mater. Chem. A 2017, 5, 25220.  doi: 10.1039/C7TA06793C

    34. [34]

      Xia, Y.; Liang, Y. F.; Xie, D.; Wang, X. L.; Zhang, S. Z.; Xia, X. H.; Gu, C. D.; Tu, J. P. A poly(vinylidene fluoride-hexafluoropropylene) based three-dimensional network gel polymer electrolyte for solid-state lithium-sulfur batteries. Chem. Eng. J. 2019, 358, 1047.  doi: 10.1016/j.cej.2018.10.092

    35. [35]

      Han, D.-D.; Liu, S.; Liu, Y.-T.; Zhang, Z.; Li, G. R.; Gao, X. P. Lithiophilic gel polymer electrolyte to stabilizze the lithium anode for a quasi-solid-state lithium-sulfur battery. J. Mater. Chem. A 2018, 6, 18627.  doi: 10.1039/C8TA07685E

    36. [36]

      Deng, Z.; Guo, Y.; Zhao, X.; Ma, P. X.; Guo, B. Multifunctional stimuli-responsive hydrogels with self-healing, high conductivity, and rapid recovery through host-guest interactions. Chem. Mater. 2018, 30, 1729.  doi: 10.1021/acs.chemmater.8b00008

    37. [37]

      Shevchenko, V. V.; Stryutsky, A. V.; Klymenko, N. S.; Gumenna, M. A.; Fomenko, A. A.; Bliznyuk, V. N.; Trachevsky, V. V.; Davydenko, V. V.; Tsukruk, V. V. Protic and aprotic anionic oligomeric ionic liquids. Polymer 2014, 55, 3349.  doi: 10.1016/j.polymer.2014.04.020

    38. [38]

      Guo, R.; Su, Q.; Zhang, J.; Dong, A.; Lin, C.; Zhang, J. Facile access to multi-sensitive and self-healing hydrogels with reversible and dynamic boronic ester and disulfide linkages. Biomacromolecules 2017, 18, 1356.  doi: 10.1021/acs.biomac.7b00089

    39. [39]

      Khan, A.; Jain, R. K.; Banerjee, P.; Ghosh, B.; Inamuddin; Asiri, A. M. Development, characterization and electromechanical actuation behavior of ionic polymer metal composite actuator based on sulfonated poly(1, 4-phenylene ether-ether-sulfone)/carbon nanotubes. Sci. Rep. 2018, 8, 9909.  doi: 10.1038/s41598-018-28399-6

    40. [40]

      Cash, J. J.; Kubo, T.; Bapat, A. P.; Sumerlin, B. S. Room-temperature self-healing polymers based on dynamic-covalent boronic esters. Macromolecules 2015, 48, 2098.  doi: 10.1021/acs.macromol.5b00210

    41. [41]

      Bapat, A. P.; Roy, D.; Ray, J. G.; Savin, D. A.; Sumerlin, B. S. Dynamic-covalent macromolecular stars with boronic ester linkages. J. Am. Chem. Soc. 2011, 133, 19832.  doi: 10.1021/ja207005z

    42. [42]

      Cao, Y.; Morrissey, T. G.; Acome, E.; Allec, S. I.; Wong, B. M.; Keplinger, C.; Wang, C. A transparent, self-healing, highly stretchable ionic conductor. Adv. Mater. 2017, 29, 1605099.  doi: 10.1002/adma.201605099

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