Tough Semi-interpenetrating Polyvinylpyrrolidone/Polyacrylamide Hydrogels Enabled by Bioinspired Hydrogen-bonding Induced Phase Separation

Qiong-Jun Xu; Zhao-Yang Yuan; Chang-Cheng Wang; Hao Liang; Yu Shi; Hai-Tao Wu; Hu Xu; Jing Zheng; Jin-Rong Wu

doi:10.1007/s10118-024-3066-z

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Tough Semi-interpenetrating Polyvinylpyrrolidone/Polyacrylamide Hydrogels Enabled by Bioinspired Hydrogen-bonding Induced Phase Separation

RESEARCH ARTICLE | Updated：2024-04-12

- Tough Semi-interpenetrating Polyvinylpyrrolidone/Polyacrylamide Hydrogels Enabled by Bioinspired Hydrogen-bonding Induced Phase Separation
- Chinese Journal of Polymer Science Vol. 42, Issue 5, Pages: 591-603(2024)
- Affiliations：
  
  State Key Laboratory of Polymer Materials Engineering, College of Polymer Science and Engineering, Sichuan University, Chengdu 610065, China
- Author bio：
  
  zhengjing@scu.edu.cn (J.Z.)
  wujinrong@scu.edu.cn (J.R.W.)
- Funds：
- DOI：10.1007/s10118-024-3066-z
  CLC：
- Published：1 May 2024，
  
  Published Online：7 December 2023，
  
  Received：12 October 2023，
  
  Revised：7 November 2023，
  
  Accepted：8 November 2023
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Xu, Q. J.; Yuan, Z. Y.; Wang, C. C.; Liang, H.; Shi, Y.; Wu, H. T.; Xu, H.; Zheng, J.; Wu, J. R. Tough semi-interpenetrating polyvinylpyrrolidone/polyacrylamide hydrogels enabled by bioinspired hydrogen-bonding induced phase separation. Chinese J. Polym. Sci. 2024, 42, 591–603

Qiong-Jun Xu, Zhao-Yang Yuan, Chang-Cheng Wang, et al. Tough Semi-interpenetrating Polyvinylpyrrolidone/Polyacrylamide Hydrogels Enabled by Bioinspired Hydrogen-bonding Induced Phase Separation. [J]. Chinese Journal of Polymer Science 42(5):591-603(2024)
Xu, Q. J.; Yuan, Z. Y.; Wang, C. C.; Liang, H.; Shi, Y.; Wu, H. T.; Xu, H.; Zheng, J.; Wu, J. R. Tough semi-interpenetrating polyvinylpyrrolidone/polyacrylamide hydrogels enabled by bioinspired hydrogen-bonding induced phase separation. Chinese J. Polym. Sci. 2024, 42, 591–603 DOI： 10.1007/s10118-024-3066-z.

Qiong-Jun Xu, Zhao-Yang Yuan, Chang-Cheng Wang, et al. Tough Semi-interpenetrating Polyvinylpyrrolidone/Polyacrylamide Hydrogels Enabled by Bioinspired Hydrogen-bonding Induced Phase Separation. [J]. Chinese Journal of Polymer Science 42(5):591-603(2024) DOI： 10.1007/s10118-024-3066-z.

摘要

Hydrogen bonding-induced phase separation strategy to construct poly(vinylpyrrolidone)/poly(acrylamide) semi-IPN hydrogels. SAXS and CLSM to study the phase separation. The unique phase-separated structure endowed the semi-IPN hydrogels with excellent mechanical properties and impact damping performance.

Abstract

Semi-interpenetrating (semi-IPN) hydrogels formed by the continuous interpenetration of cross-linked polymer network and linear non-crosslinked polymer with multifunctionality are widely used in biomedical and other fields. However

the negative impact of linear polymer on the homogeneity of the cross-linked network often leads to a decrease in the mechanical properties of semi-IPN hydrogels and severely limits their applications. Herein

a bioinspired hydrogen-bonding induced phase separation strategy is presented to construct the tough semi-IPN polyvinylpyrrolidone/polyacrylamide hydrogels (named PVP

/PAM hydrogels)

including the linear polymer polyvinylpyrrolidone (PVP) and cross-linked polyacrylamide (PAM) network. The resultant PVP

/PAM hydrogels exhibit unique phase separation induced by the hydrogen bonding between PVP and PAM and affected by the amount of substance of PVP. Meanwhile

the phase separation of PVP

/PAM hydrogels results in excellent mechanical properties with a strain of 2590%

tensile strength of 0.28 MPa and toughness of 2.17 MJ/m

. More importantly

the hydrogen bonding between PVP and PAM firstly disrupts to dissipate energy under external forces

so the PVP

/PAM hydrogels exhibit good self-recovery properties and outperform chemically cross-linked PAM hydrogels in impact resistance and damping applications. It is believed that the PVP

/PAM hydrogels with hydrogen-bonding induced phase separation possess more potential application prospects.

关键词

Keywords

ToughSemi-interpenetrating networksPolyvinylpyrrolidone/polyacrylamideHydrogelsPhase separation

references

Cui, X.; Liu, Z.; Zhang, B.; Tang, X.; Fan, F.; Fu, Y.; Zhang, J.; Wang, T.; Meng, F. J. Sponge-like, semi-interpenetrating self-sensory hydrogel for smart photothermal-responsive soft actuator with biomimetic self-diagnostic intelligence.Chem. Eng. J.2023, 467, 143515..

Yang, M.; Chen, P.; Qu, X.; Zhang, F.; Ning, S.; Ma, L.; Yang, K.; Su, Y.; Zang, J.; Jiang, W.; Yu, T.; Dong, X.; Luo, Z. Robust neural interfaces with photopatternable, bioadhesive, and highly conductive hydrogels for stable chronic neuromodulation.ACS Nano2023, 17, 885−895..

Samanta, H. S.; Ray, S. K. Synthesis, characterization, swelling and drug release behavior of semi-interpenetrating network hydrogels of sodium alginate and polyacrylamide.Carbohyd. Polym.2014, 99, 666−678..

Hebeish, A.; Farag, S.; Sharaf, S.; Shaheen, T. I. Thermal responsive hydrogels based on semi interpenetrating network of poly(NIPAm) and cellulose nanowhiskers.Carbohyd. Polym.2014, 102, 159−166..

Dai, Z.; Yang, X.; Wu, F.; Wang, L.; Xiang, K.; Li, P.; Lv, Q.; Tang, J.; Dohlman, A.; Dai, L.; Shen, X.; You, L. Living fabrication of functional semi-interpenetrating polymeric materials.Nat. Commun.2021, 12, 3422..

Jiang, X.; Li, S.; Shao, L. Pushing CO2-philic membrane performance to the limit by designing semi-interpenetrating networks (SIPN) for sustainable CO2separations.Energ. Environ. Sci.2017, 10, 1339−1344..

Wang, M.; Nie, C.; Liu, J.; Wu, S. Organic-inorganic semi-interpenetrating networks with orthogonal light- and magnetic-responsiveness for smart photonic gels.Nat. Commun.2023, 14, 1000..

Wahid, F.; Hu, X. H.; Chu, L. Q.; Jia, S. R.; Xie, Y. Y.; Zhong, C. Development of bacterial cellulose/chitosan based semi-interpenetrating hydrogels with improved mechanical and antibacterial properties.Int. J. Biol. Macromol.2019, 122, 380−387..

Zhu, B.; Ma, D.; Wang, J.; Zhang, S. Structure and properties of semi-interpenetrating network hydrogel based on starch.Carbohyd. Polym.2015, 133, 448−455..

Sampath, U. G. T. M.; Ching, Y. C.; Chuah, C. H.; Singh, R.; Lin, P. C. Preparation and characterization of nanocellulose reinforced semi-interpenetrating polymer network of chitosan hydrogel.Cellulose2017, 24, 2215−2228..

Chan, B. K.; Wippich, C. C.; Wu, C. J.; Sivasankar, P. M.; Schmidt, G. Robust and semi-interpenetrating hydrogels from poly(ethylene glycol) and collagen for elastomeric tissue scaffolds.Macromol. Biosci.2012, 12, 1490−1501..

Xing, L.; Song, Y.; Zou, X.; Tan, H.; Yan, J.; Wang, J. A mussel-inspired semi-interpenetrating structure hydrogel with superior stretchability, self-adhesive properties, and pH sensitivity for smart wearable electronics.J. Mater. Chem. C2023, 11, 13376−13386..

Olad, A.; Pourkhiyabi, M.; Gharekhani, H.; Doustdar, F. Semi-IPN superabsorbent nanocomposite based on sodium alginate and montmorillonite: Reaction parameters and swelling characteristics.Carbohyd. Polym.2018, 190, 295−306..

Rokhade, A. P.; Patil, S. A.; Aminabhavi, T. M. Synthesis and characterization of semi-interpenetrating polymer network microspheres of acrylamide grafted dextran and chitosan for controlled release of acyclovir.Carbohyd. Polym.2007, 67, 605−613..

Zhu, T.; Cheng, Y.; Cao, C.; Mao, J.; Li, L.; Huang, J.; Gao, S.; Dong, X.; Chen, Z.; Lai, Y. A semi-interpenetrating network ionic hydrogel for strain sensing with high sensitivity, large strain range, and stable cycle performance.Chem. Eng. J.2020, 385, 123912..

Zhang, G.; Chen, Y.; Deng, Y.; Ngai, T.; Wang, C. Dynamic supramolecular hydrogels: regulating hydrogel properties through self-complementary quadruple hydrogen bonds and thermo-switch.ACS Macro Lett.2017, 6, 641−646..

Yang, Y.; Wang, X.; Yang, F.; Wang, L.; Wu, D. Highly elastic and ultratough hybrid ionic–covalent hydrogels with tunable structures and mechanics.Adv. Mater.2018, 30, 1707071..

Peppas, N. A.; Hilt, J. Z.; Khademhosseini, A.; Langer, R. Hydrogels in biology and medicine: from molecular principles to bionanotechnology.Adv. Mater.2006, 18, 1345−1360..

Mihajlovic, M.; Staropoli, M.; Appavou, M.-S.; Wyss, H. M.; Pyckhout-Hintzen, W.; Sijbesma, R. P. Tough Supramolecular hydrogel based on strong hydrophobic interactions in a multiblock segmented copolymer.Macromolecules2017, 50, 3333−3346..

Wang, H.; Heilshorn, S. C. Adaptable hydrogel networks with reversible linkages for tissue engineering.Adv. Mater.2015, 27, 3717−3736..

Huo, P.; Ding, H.; Tang, Z.; Liang, X.; Xu, J.; Wang, M.; Liang, R.; Sun, G. Conductive silk fibroin hydrogel with semi-interpenetrating network with high toughness and fast self-recovery for strain sensors.Int. J. Biol. Macromol.2022, 212, 1−10..

Wang, A.; Wang, Y.; Zhang, B.; Wan, K.; Zhu, J.; Xu, J.; Zhang, C.; Liu, T. Hydrogen-bonded network enables semi-interpenetrating ionic conductive hydrogels with high stretchability and excellent fatigue resistance for capacitive/resistive bimodal sensors.Chem. Eng. J.2021, 411..

Dai, X.; Zhang, Y.; Gao, L.; Bai, T.; Wang, W.; Cui, Y.; Liu, W. A mechanically strong, highly stable, thermoplastic, and self-healable supramolecular polymer hydrogel.Adv. Mater.2015, 27, 3566−3571..

Yao, M.; Wei, Z.; Li, J.; Guo, Z.; Yan, Z.; Sun, X.; Yu, Q.; Wu, X.; Yu, C.; Yao, F.; Feng, S.; Zhang, H.; Li, J. Microgel reinforced zwitterionic hydrogel coating for blood-contacting biomedical devices.Nat. Commun.2022, 13, 5339..

Zhang, L.; Yan, H.; Zhou, J.; Zhao, Z.; Huang, J.; Chen, L.; Ru, Y.; Liu, M. High-performance organohydrogel artificial muscle with compartmentalized anisotropic actuation under microdomain confinement.Adv. Mater.2023, 35, 2202193..

Liang, X.; Chen, G.; Lei, I. M.; Zhang, P.; Wang, Z.; Chen, X.; Lu, M.; Zhang, J.; Wang, Z.; Sun, T.; Lan, Y.; Liu, J. Impact-resistant hydrogels by harnessing 2D hierarchical structures.Adv. Mater.2022, 35, 2207587..

Mastrangelo, R.; Chelazzi, D.; Poggi, G.; Fratini, E.; Pensabene Buemi, L.; Petruzzellis, M. L.; Baglioni, P. Twin-chain polymer hydrogels based on poly(vinyl alcohol) as new advanced tool for the cleaning of modern and contemporary art.Proc. Natl. Acad. Sci. U. S. A.2020, 117, 7011−7020..

Chen, G.; Xu, S.; Zhou, Q.; Zhang, Y.; Song, Y.; Mi, J.; Liu, Y.; Hou, K.; Pan, J. Temperature-gated light-guiding hydrogel fiber for thermoregulation during optogenetic neuromodulation.Adv. Fiber Mater.2023, 5, 968−978..

Flory, P. J. Statistical mechanics of swelling of network structures.J. Chem. Phys.1950, 18, 108−111..

Yuan, Z.; Cao, Z.; Ma, C.; Wu, R.; Wu, H.; Xu, Q.; Zheng, J.; Wu, J. Ultra-robust, repairable and smart physical hydrogels enabled by nano-domain reconfiguration of network topology.Chem. Eng. J.2022, 450, 138085..

Vichai, V.; Kirtikara, K. Sulforhodamine B colorimetric assay for cytotoxicity screening.Nat. Protoc.2006, 1, 1112−1116..

Xu, H.; Ma, C. S.; Yu, C. Y.; Tong, F.; Qu, D. H. Reversible inversion of circularly polarized luminescence in a coassembly supramolecular structure with achiral sulforhodamine B Dyes.ACS Appl. Mater. Interfaces2023, 15, 25201−25211..

Song, G.; Zhang, L.; He, C.; Fang, D. C.; Whitten, P. G.; Wang, H. Facile fabrication of tough hydrogels physically cross-linked by strong cooperative hydrogen bonding.Macromolecules2013, 46, 7423−7435..

Wang, Y. J.; Zhang, X. N.; Song, Y.; Zhao, Y.; Chen, L.; Su, F.; Li, L.; Wu, Z. L.; Zheng, Q. Ultrastiff and tough supramolecular hydrogels with a dense and robust hydrogen bond network.Chem. Mater.2019, 31, 1430−1440..

Wang, Y.; Wu, J.; Cao, Z.; Ma, C.; Tong, Q.; Li, J.; Liu, H.; Zheng, J.; Huang, G. Mechanically robust, notch-insensitive, fatigue resistant and self-recoverable hydrogels with homogeneous and viscoelastic network constructed by a novel multifunctional cross-linker.Polymer2019, 179, 121661..

Mou, L.; Qi, J.; Tang, L.; Dong, R.; Xia, Y.; Gao, Y.; Jiang, X. Highly stretchable and biocompatible liquid metal-elastomer conductors for self-healing electronics.Small2020, 16, e2005336..

Chen, Q.; Zhu, L.; Zhao, C.; Wang, Q.; Zheng, J. A robust, one-pot synthesis of highly mechanical and recoverable double network hydrogels using thermoreversible sol-gel polysaccharide.Adv. Mater.2013, 25, 4171−4176..

Erdodi, G.; Kennedy, J. P. Amphiphilic conetworks: definition, synthesis, applications.Prog. Polym. Sci.2006, 31, 1−18..

Wang, Y.; Xie, Y.; Xie, X.; Wu, D.; Wu, H.; Luo,X.; Wu, Q.; Zhao, L.; Wu, J. Compliant and robust tissue-like hydrogels viaferric ion-induced of hierarchical structure.Adv. Funct. Mater.2023, 33, 2210224..

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