The poor mechanical properties of self-healing hydrogels limited their applications in the fields of biomedicine and industry. Here, a series of self-healing polymeric ionic liquid (PIL) hydrogels with high mechanical strength and electrical conductivity were prepared through hydrophobic association. Hydrophilic monomer vinyl ionic liquids (VILs) based on choline and amino acids, acrylamide (AAm) and hydrophobic monomers stearyl methacrylate (C18) were copolymerized in a micellar solution of sodium dodecyl sulfate (SDS); meanwhile, bacterial cellulose was introduced to enhance the mechanical strength of hydrogels. The resultant hydrogels exhibited excellent mechanical strength (5.8 MPa), extensive elongation at break (4250%) and outstanding self-healing efficiency (85%) without any external intervention. Even after healing, the tensile strength of most hydrogels could reach 2.5–3.9 MPa. At the same time, the incorporation of ILs endowed hydrogels with good electrical conductivity (a maximum of 1.258 S/m). These excellent properties predicted the potential application of the obtained PIL hydrogels in the fields of biomedicine and industry.
This is a preview of subscription content, access via your institution.
Buy single article
Instant access to the full article PDF.
Tax calculation will be finalised during checkout.
Subscribe to journal
Immediate online access to all issues from 2019. Subscription will auto renew annually.
Tax calculation will be finalised during checkout.
Fantner GE, Oroudjev E, Schitter G, Golde LS, Thurner P, Finch MM, Turner P, Gutsmann T, Morse DE, Hansma H, Hansma PK (2006) Sacrificial bonds and hidden length: unraveling molecular mesostructures in tough materials. Biophys J 90:1411–1418
Araya-Hermosilla R, Lima GMR, Raffa P, Fortunato G, Pucci A, Moreno-Villoslada I, Broekhuis AA, Picchioni F (2016) Intrinsic self-healing thermoset through covalent and hydrogen bonding interactions. Eur Polym J 81:186–197
Hao X, Liu H, Xie Y, Fang C, Yang H (2013) Thermal-responsive self-healing hydrogel based on hydrophobically modified chitosan and vesicle. Colloid Polym Sci 291:1749–1758
Xu Y, Wu Q, Sun Y, Bai H, Shi G (2010) Three-dimensional self-assembly of graphene oxide and DNA into multifunctional hydrogels. ACS Nano 4:7358–7362
Appel EA, Biedermann F, Rauwald U, Jones ST, Zayed JM, Scherman OA (2010) Supramolecular cross-Linked networks via host-guest complexation with cucurbituril. J Am Chem Soc 132:14251–14260
Haraguchi K, Uyama K, Tanimoto H (2011) Self-healing in nanocomposite hydrogels. Rapid Commun 32:1253–1258
Froimowicz P, Klinger D, Landfester K (2011) Photoreactive nanoparticles as nanometric building blocks for the generation of self-healing hydrogel thin films. Chem Eur J 17:12465–12475
Shao CY, Chang HL, Wang M, Xu F, Yang J (2017) 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 9:28305–28318
Sun JY, Zhao X, Illeperuma WRK, Chaudhuri O, Oh KH, Money DJ, Vlassak JJ, Suo Z (2012) Highly stretchable and tough hydrogels. Nature 489:133–136
Tuncaboylu DC, Sari M, Oppermann W, Okay O (2011) Tough and self-healing hydrogels formed via hydrophobic interactions. Macromolecules 44:4997–5005
Tuncaboylu DC, Argun A, Sahin M, Sari M, Okay O (2012) Structure optimization of self-healing hydrogels formed via hydrophobic interactions. Polymer 53:5513–5522
Tuncaboylu DC, Sahin M, Argun A, Oppermann W, Okay O (2012) Dynamics and large strain behavior of self-healing hydrogels with and without surfactants. Macromolecules 45:1991–2000
Gulyuz U, Okay O (2013) Self-healing polyacrylic acid hydrogels. Soft Matter 43:10287–10293
Akay G, Hassan-Raeisi A, Tuncaboylu DC, Orakdogen N, Abdurrahmanoglu S, Oppermann W, Okay O (2013) Self-healing hydrogels formed in catanionic surfactant solutions. Soft Matter 7:2254–2261
Gulyuz U, Okay O (2015) Self-healing poly(N-isopropylacrylamide) hydrogels. Eur Polym J 72:12–22
Gulyuz U, Okay O (2014) Self-healing poly(acrylic acid) hydrogels with shape memory behavior of high mechanical strength. Macromolecules 47:6889–6899
Zhao JS, Zhang C, Zou D, Liu XK, Cai LX, Li XY, Shi MX (2019) A structured design for highly stretchable electronic skin. Adv Mater Technol 10:1900492
Wei Y, Zeng Q, Hu Q (2018) Self-cleaned electrochemical protein imprinting biosensor basing on a thermo-responsive memory hydrogel. Biosens Bioelectron 99:136–141
Shi Y, Wang M, Ma C, Wang Y, Li X, Yu G (2015) A conductive self-healing hybrid gel enabled by metal ligand supramolecule and nanostructured conductive polymer. Nano Lett 15:6276–6281
Lim C, Shin Y, Jung J (2019) Stretchable conductive nanocomposite based on alginate hydrogel and silver nanowires for wearable electronics. APL Mater 3:031502
Dev A, Mohanbhai SJ, Kushwaha AC (2020) Kappa-carrageenan-C- phycocyanin based smart injectable hydrogels for accelerated wound recovery and real-time monitoring. Acta Biomater 109:121–131
Yang WX, Shao BW, Liu TY, Zhang YY, Huang R, Chen F, Fu Q (2018) Robust and mechanically and electrically self-healing hydrogel for efficient. ACS Appl Mater Inter 10:8245–8257
Wang Y, Maurel G, Couty M, Detcheverry F, Merabia S (2019) Implicit medium model for fractal aggregate polymer nanocomposites: linear viscoelastic properties. Macromolecules 5:2021–2032
Gunduz G, Kiziltas EE, Kiziltas A, Gencer A, Aydemir D, Asik N (2019) Production of bacterial cellulose fibers in the presence of effective microorganism. J Nat Fibers 16:567–575
Chen P, Cho SY, Jin HJ (2010) Modification and applications of bacterial celluloses in polymer science. Macromol Res 18:309–320
Ul-Islam M, Khan S, Ullah MW, Park JK (2015) Bacterial cellulose composites: synthetic strategies and multiple applications in bio-medical and electro-conductive fields. Biotechnol J 12:1847–1861
Meziane R, Bonnet JP, Courty M, Djellab K, Armand M (2011) Single-ion polymer electrolytes based on adelocalized polyanion for lithium batteries. Electrichim Acta 57:14–19
Sugimura R, Qiao K, Tomida D, Yokoyama C (2007) Immobilization of acidic ionic liquids by copolymerization with styrene and their catalytic use for acetal formation. Catal Commun 5:770–772
Nakajima H, Ohno H (2005) Preparation of thermally stable polymer electrolytes from imidazolium-type ionic liquid derivatives. Polymer 46:11499–11504
Tang HD, Tang JB, Ding SJ (2005) Atom transfer radical polymerization of styrenic ionic liquid monomers and carbon dioxide absorption of the polymerized ionic liquids. J Polym Sci Pol Chem 43:1432–1443
Ohno H, Fukumoto K (2007) Amino acid ionic liquids. Accounts Chem Res 11:1122–1129
Qian WJ, Texter J, Yan F (2017) Frontiers in poly(ionic liquid)s: syntheses and applications. Chem Soc Rev 46:1124–1159
Chen H, Elabd YA (2009) Polymerized ionic liquids: solution properties and electrospinning. Macromolecules 42:3368–3373
Bandomir J, Schulz A, Taguchi S, Schmitt L, Ohno H, Sternberg K, Schmitz KP, Kragl U (2014) Synthesis and characterization of polymerized ionic liquids: mechanical and thermal properties of a novel type of hydrogels. Macromol Chem Phys 215:716–724
Men Y, Schlaad H, Voelkel A, Yuan J (2014) Thermoresponsive polymerized gemini dicationic ionic liquid. Polym Chem 5:3719–3724
Li SL, Gao Y, Jiang HC, Duan LJ, Gao GH (2018) Tough, sticky and remoldable hydrophobic association hydrogel regulated by polysaccharide and sodium dodecyl sulfate as emulsifiers. Carbohyd Polym 201:591–598
Zhang Q, Wu M, Hu X (2020) A novel double-network, self-healing hydrogel based on hydrogen bonding and hydrophobic effect. Macromol Chem Phys 3:1900320
Wan J, Tang F, Wang Y, Lu QP, Liu SQ, Li LD (2020) Self-healing and highly stretchable gelatin hydrogel for self-powered strain sensor. ACS Appl Mater Interfaces 1:1558–1566
Wen J, Zhang X, Pan M (2020) A robust, tough and multifunctional polyurethane/tannic acid hydrogel fabricated by physical-chemical dual crosslinking. Polymers 1:239
Wei D, Yang J, Zhu L, Chen F, Tang Z, Qin G, Chen Q (2018) Semicrystalline hydrophobically associated hydrogels with integrated high performances. ACS Appl Mater Interfaces 10:2946–2956
Zhang B, Gao Z, Gao G, Zhao W, Li J, Ren X (2018) Highly mechanical and fatigue-resistant double network hydrogels by dual physically hydrophobic association and ionic crosslinking. Macromol Mater Eng 303:1800072
Xia S, Jia F, Gao GH (2019) A flexible, adhesive and self-healable hydrogel -based wearable strain sensor for human motion and physiological signal monitoring. J Mater Chem B 7(30):4638–4648
Ye L, Lv Q, Sun XY, Liang YZ, Fang PW, Yuan XY, Li M, Zhang XZ, Shang XF, Liang HY (2020) Fully physically cross-linked double network hydrogels with strong mechanical properties, good recovery and self-healing properties. Soft Matter 16(7):1840–1849
Pan JZ, Jin Y, Lai SQ, Shi LJ, Fan WH, Shen YC (2019) An antibacterial hydrogel with desirable mechanical, self-healing and recyclable properties based on triple-physical crosslinking. Chem Eng J 370:1228–1238
Ying Y, Urban MW (2018) Self-Healing of polymers via supramolecular chemistry. Adv Mater Interfaces 5(17):1800384
Chen H, Hao BB, Ge PH, Chen SJ (2020) Highly stretchable, self-healing, and 3D printing prefabricatable hydrophobic association hydrogels with the assistance of electrostatic interaction. Polym Chem 11(29):4741–4748
Liang XX, Ding HY, Wang Q, Sun GX (2019) Tough physical hydrogels reinforced by hydrophobic association with remarkable mechanical property, rapid stimuli-responsiveness and fast self-recovery capability. Eur Polym J 120:109278
Sohrabi M, Yekta BE, Rezaie HR, Naimi-Jamal MR (2020) Rheology, injectability, and bioactivity of bioactive glass containing chitosan/gelatin nano pastes. Polym Sci 41:e49240
Chen YY, Lu KY, Song YH, Han JQ, Yue YY, Biswas SK, Wu QL, Xiao HN (2019) A skin-inspired stretchable, self-healing and electro-conductive hydrogel with a synergistic triple network for wearable strain sensors applied in human-motion detection. Nanomaterials 12:1737
Dai XY, Zhang YY, Gao LN, Bai T, Wang W, Cui YL, Liu WG (2015) A mechanically strong, highly stable, thermoplastic, and self-healable supramolecular polymer hydrogel. Adv Mater 23:3566–3571
Vilela C, Sousa N, Pinto RJB, Silvestre AJD, Figueiredo FML, Freire CSR (2017) Exploiting poly(ionic liquids) and nanocellulose for the development of bio-based anion-exchange membranes. Biomass Bioenerg 100:116–125
Zhang HT, Wu XJ, Qin ZH, Sun X, Zhang H, Yu QY, Yao MM, He SS, Dong XR, Yao FL, Li JJ (2020) Dual physically cross-linked carboxymethyl cellulose-based hydrogel with high stretchability and toughness as sensitive strain sensors. Cellulose 27:9975–9989
This work was supported by the National Natural Science Foundation of China (No. 22075207), Natural Science Foundation of Tianjin (No. 18JCYBJC87200) and the Training Program of Innovation and Entrepreneurship for Undergraduates (No. 201910058052).
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Handling Editor: Maude Jimenez.
Below is the link to the electronic supplementary material.
About this article
Cite this article
He, X., Sun, X., Meng, H. et al. Self-healing polymeric ionic liquid hydrogels with high mechanical strength and ionic conductivity. J Mater Sci 56, 10231–10248 (2021). https://doi.org/10.1007/s10853-021-05930-1