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

Your Location：

Home >

Browse articles >

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：
- Received：12 October 2023，
  
  Revised：2023-11-7，
  
  Accepted：08 November 2023，
  
  Online First：07 December 2023，
  
  Published：01 May 2024
- Accepted：
Scan QR Code
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, 2024, 42(5): 591-603.
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, 2024, 42(5): 591-603. 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

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 Nano 2023 , 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 CO 2 -philic membrane performance to the limit by designing semi-interpenetrating networks (SIPN) for sustainable CO 2 separations. 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. Cellulose 2017 , 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. C 2023 , 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. Macromolecules 2017 , 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. Interfaces 2023 , 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. Macromolecules 2013 , 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. Polymer 2019 , 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. Small 2020 , 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 via ferric ion-induced of hierarchical structure. Adv. Funct. Mater. 2023 , 33 , 2210224..

Views

866

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

A Transparent Acoustic Damping Hydrogel with Dual-scale Bicontinuous Microphase Separation

Enhanced Mechanical Properties and Prolonged Recovery Onset Period of Timed Shape Memory Hydrogels via Hydrophobic Interaction

Multifunctional Property Enhancement of 2-Acrylamido-2-methyl-1-propanesulfonic Acid/Acrylic Acid Hydrogels with Dual-ionic Liquid Functionalized Carbon Nanotubes

Optically Active Helical Poly(phenyl isocyanide)s Bearing Achiral Benzanilide Pendants: from Controlled Synthesis to Enantioseparation Application

Circularly Polarized Luminescence Based on Helical Polymers: Structure-Property Relationships and Regulation Mechanisms

Related Author

Chen-Chen Lou

Bao-Hu Wu

Sheng-Tong Sun

Pei-Yi Wu

Xiao-Ting Jia

Yi-Ting Sun

Chu-Jun Ni

Qian Zhao

Related Institution

State Key Laboratory of Advanced Fiber Materials, College of Chemistry and Chemical Engineering & Center for Advanced Low-dimension Materials, Donghua University

Jülich Centre for Neutron Science (JCNS) at Heinz Maier-Leibnitz Zentrum (MLZ) Forschungszentrum Jülich, Garching

State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University

Eye Center, Affiliated Second Hospital, School of Medicine, Zhejiang University

School of Chemical Engineering, Changchun University of Technology

⁰