物理缔合增韧水凝胶及其黏弹行为研究进展

徐思瑞; 杜淼; 郑强; 吴子良

doi:10.14028/j.cnki.1003-3726.2025.24.334

您当前的位置：

首页 >

文章列表页 >

物理缔合增韧水凝胶及其黏弹行为研究进展

综述 | 更新时间：2025-01-23

- 物理缔合增韧水凝胶及其黏弹行为研究进展
- Recent Progress in the Design of Tough Hydrogels with Physical Associations and Their Viscoelastic Behaviors
- 高分子通报 2025年38卷第2期页码：354-369
- 作者机构：
  
  浙江大学高分子科学与工程学系，杭州 310058
- 作者简介：
  
  *吴子良，E-mail: wuziliang@zju.edu.cn
- 基金信息：
- DOI：10.14028/j.cnki.1003-3726.2025.24.334
  中图分类号：
- 收稿日期：2024-11-03，
  
  录用日期：2024-12-06，
  
  网络出版日期：2025-01-08，
  
  纸质出版日期：2025-02-20
- 稿件说明：
移动端阅览
徐思瑞，杜淼，郑强，吴子良. 物理缔合增韧水凝胶及其黏弹行为研究进展. 高分子通报, 2025, 38(2), 355–370

Xu, S. R.; Du, M.; Zheng, Q.; Wu, Z. L. Recent progress in the design of tough hydrogels with physical associations and their viscoelastic behaviors. Polym. Bull. (in Chinese), 2025, 38(2), 355–370
徐思瑞，杜淼，郑强，吴子良. 物理缔合增韧水凝胶及其黏弹行为研究进展. 高分子通报, 2025, 38(2), 355–370 DOI： 10.14028/j.cnki.1003-3726.2025.24.334.

Xu, S. R.; Du, M.; Zheng, Q.; Wu, Z. L. Recent progress in the design of tough hydrogels with physical associations and their viscoelastic behaviors. Polym. Bull. (in Chinese), 2025, 38(2), 355–370 DOI： 10.14028/j.cnki.1003-3726.2025.24.334.

摘要

水凝胶作为一类含有大量水的三维网络聚合物，具有与生物软组织类似的结构特征，在医学、工程等领域具有广泛应用。近年来，通过引入离子键、氢键等物理缔合作用，研究者们成功制备了多种具有优异力学性能的水凝胶，其宏观性能与物理键及其缔合体的松弛关系密切相关；力学测试与流变学相结合已成为研究其增韧机制及结构-性能关系的有效手段。本文以物理键动态特征及其对水凝胶力学、黏弹行为的影响为纽带，梳理该领域的研究进展。首先，介绍了几种理想高分子网络中物理键的松弛行为，讨论了Sticky-reptation模型在描述含物理缔合作用水凝胶黏弹行为中的应用；其次，探讨了物理键如何影响高强韧水凝胶的宏观性能，并运用物理网络模型建立微观结构与宏观性能之间的联系；此外，进一步讨论了物理键之外的其他因素对水凝胶的动态力学及黏弹行为的影响，以及通过物理键调控水凝胶宏观性能的途径；最后，对水凝胶领域发展所面临的挑战与机遇进行了展望。

Abstract

Hydrogels

as a class of three-dimensional polymer network containing large amount of water

exhibit characteristics similar to soft biotissues

affording them with broad applications in biomedical and engineering fields. In recent years

scientists have developed various tough hydrogels with excellent mechanical properties by incorporating physical associations such as ionic bonds

hydrogen bonds

etc. The macroscopic properties of these hydrogels are closely related to the dynamics of physical bonds and their associations. The combination of mechanical test and rheological analysis has become a powerful approach to investigate the toughening mechanism and to reveal the structure-property relationship of hydrogels. This review focuses on the dynamic feature of physical bonds and their influences on mechanical and viscoelastic behaviors of the hydrogels

by summarizing recent advances in this field. First

we introduce the relaxation behavior of physical bonds in ideal polymer networks and discuss the application of sticky-reptation model in describing the viscoelastic behavior of hydrogels with physical associations. Next

we explore how physical bonds affect the macroscopic properties of tough hydrogels

and employ physical network models to correlate their microstructures and macroscopic performances. Additionally

we consider other factors that impact the mechanical and viscoelastic behaviors of hydrogels

as well as strategies for modulating their properties of gels with physical bonds. Finally

we provide an outlook on the challenges and opportunities facing the development of hydrogels in this field.

关键词

Keywords

references

Aghajanzadeh, M. S. ; Imani, R. ; Nazarpak, M. H. ; McI-nnes, S . Augmented physical, mechanical, and cellular responsiveness of gelatin-aldehyde modified xanthan hydrogel through incorporation of silicon nanoparticles for bone tissue engineering . Int. J. Biol. Macromol. , 2024 , 259 ( Pt 2 ), 129231 .

Kaviani, S. ; Talebi, A. ; Labbaf, S. ; Karimzadeh, F . Conductive GelMA/alginate/polypyrrole/graphene hydro-gel as a potential scaffold for cardiac tissue engineering; Physiochemical, mechanical, and biological evaluations . Int. J. Biol. Macromol. , 2024 , 259 ( Pt 2 ), 129276 .

Serafin, A. ; Culebras, M. ; Collins, M. N . Synthesis and evaluation of alginate, gelatin, and hyaluronic acid hybrid hydrogels for tissue engineering applications . Int. J. Biol. Macromol. , 2023 , 233 , 123438 .

Alipournazari, P. ; Pourmadadi, M. ; Abdouss, M. ; Rahdar, A. ; Pandey, S . Enhanced delivery of doxorubicin for breast cancer treatment using pH-sensitive starch/PVA/g-C(3)N(4) hydrogel . Int. J. Biol. Macromol , 2024 , 265 ( Pt 1 ), 130901 .

Thang, N. H. ; Chien, T. B. ; Cuong, D. X . Polymer-based hydrogels applied in drug delivery: an overview . Gels , 2023 , 9 ( 7 ), 523 .

Zhang, H. ; Wu, S. L. ; Chen, W. K. ; Hu, Y. ; Geng, Z. ; Su, J. C . Bone/cartilage targeted hydrogel: strategies and applications . Bioact. Mater. , 2023 , 23 , 156 − 169 .

Hu, L. X. ; Chee, P. L. ; Sugiarto, S. ; Yu, Y. ; Shi, C. Q. ; Yan, R. ; Yao, Z. Q. ; Shi, X. W. ; Zhi, J. C. ; Kai, D. ; Yu, H. D. ; Huang, W . Hydrogel-based flexible electronics . Adv. Mater. , 2023 , 35 ( 14 ), 2205326 .

Zhang, C. W. ; Zou, W. F. ; Yu, H. C. ; Hao, X. P. ; Li, G. R. ; Li, T. F. ; Yang, W. ; Wu, Z. L. ; Zheng, Q . Manta ray inspired soft robot fish with tough hydrogels as struct-ural elements . ACS Appl. Mater. Interfaces , 2022 , 14 ( 46 ), 52430 − 52439 .

Ullah, R. ; Shah, L. A. ; Khan, M. T . Cellulose nano-crystals boosted hydrophobically associated self-healable conductive hydrogels for the application of strain sen-sors and electronic devices . Int. J. Biol. Macromol. , 2024 , 260 ( Pt 2 ), 129376 .

Hao, X. P. ; Li, C. Y. ; Zhang, C. W. ; Du, M. ; Ying, Z. M. ; Zheng, Q. ; Wu, Z. L . Self-shaping soft electronics based on patterned hydrogel with stencil-printed liquid metal . Adv. Funct. Mater. , 2021 , 31 ( 47 ), 2105481 .

Zhao, B. ; Bai, Z. Y. ; Lv, H. L. ; Yan, Z. K. ; Du, Y. Q. ; Guo, X. Q. ; Zhang, J. C. ; Wu, L. M. ; Deng, J. S. ; Zhang, D. W. ; Che, R. C . Self-healing liquid metal magnetic hydro-gels for smart feedback sensors and high-performance electromagnetic shielding . Nanomicro Lett. , 2023 , 15 ( 1 ), 79 .

Hao, X. P. ; Xu, Z. ; Li, C. Y. ; Hong, W. ; Zheng, Q. ; Wu, Z. L . Kirigami-design-enabled hydrogel multimorphs with application as a multistate switch . Adv. Mater. , 2020 , 32 ( 22 ), 2000781 .

Yu, C. T. ; Cui, K. P. ; Guo, H. L. ; Ye, Y. N. ; Li, X. Y. ; Gong, J. P . Structure frustration enables thermal history-dependent responsive behavior in self-healing hydrogels . Macromolecules , 2021 , 54 ( 21 ), 9927 − 9936 .

Luo, F. ; Sun, T. L. ; Nakajima, T. ; Kurokawa, T. ; Li, X. F. ; Guo, H. L. ; Huang, Y. W. ; Zhang, H. J. ; Gong, J. P . Tough polyion-complex hydrogels from soft to stiff controlled by monomer structure . Polymer , 2017 , 116 , 487 − 497 .

Luo, F. ; Sun, T. L. ; Nakajima, T. ; King, D. R. ; Kurokawa, T. ; Zhao, Y. ; Ihsan, A. B. ; Li, X. F. ; Guo, H. L. ; Gong, J. P . Strong and tough polyion-complex hydrogels from oppositely charged polyelectrolytes: a comparative study with polyampholyte hydrogels . Macromolecules , 2016 , 49 ( 7 ), 2750 − 2760 .

Zhu, C. N. ; Zheng, S. Y. ; Qiu, H. N. ; Du, C. ; Du, M. ; Wu, Z. L. ; Zheng, Q . Plastic-like supramolecular hydrogels with polyelectrolyte/surfactant complexes as physical cross-links . Macromolecules , 2021 , 54 ( 17 ), 8052 − 8066 .

Sun, T. L. ; Luo, F. ; Kurokawa, T. ; Karobi, S. N. ; Nakajima, T. ; Gong, J. P . Molecular structure of self-healing polyampholyte hydrogels analyzed from tensile behaviors . Soft Matter , 2015 , 11 ( 48 ), 9355 − 9366 .

Dai, X. Y. ; Zhang, Y. Y. ; Gao, L. N. ; Bai, T. ; Wang, W. ; Cui, Y. L. ; Liu, W. G . A mechanically strong, highly stable, thermoplastic, and self-healable supramolecular polymer hydrogel . Adv. Mater. , 2015 , 27 ( 23 ), 3566 − 3571 .

Han, Z. L. ; Wang, P. ; Lu, Y. C. ; Jia, Z. ; Qu, S. X. ; Yang, W . A versatile hydrogel network-repairing strategy achieved by the covalent-like hydrogen bond interaction . Sci. Adv. , 2022 , 8 ( 8 ), eabl5066 .

Ouyang, Y. ; Zhao, Y. ; Zheng, X. ; Zhang, Y. ; Zhao, J. ; Wang, S. ; Gu, Y . Rapidly degrading and mussel-inspired multifunctional carboxymethyl chitosan/montmorillonite hydrogel for wound hemostasis . Int. J. Biol. Macromol. , 2023 , 242 ( Pt 3 ), 124960 .

Zhao, D. W. ; Feng, M. ; Zhang, L. ; He, B. ; Chen, X. Y. ; Sun, J . Facile synthesis of self-healing and layered sodium alginate/polyacrylamide hydrogel promoted by dynamic hydrogen bond . Carbohydr. Polym. , 2021 , 256 , 117580 .

Hou, L. X. ; Ju, H. Q. ; Hao, X. P. ; Zhang, H. K. ; Zhang, L. ; He, Z. Y. ; Wang, J. J. ; Zheng, Q. ; Wu, Z. L . Intrinsic anti-freezing and unique phosphorescence of glassy hydrogels with ultrahigh stiffness and toughness at low temperatures . Adv. Mater. , 2023 , 35 ( 21 ), 2300244 .

Dai, C. F. ; Zhang, X. N. ; Du, C. ; Frank, A. ; Schmidt, H. W. ; Zheng, Q. ; Wu, Z. L . Photoregulated gradient struc-ture and programmable mechanical performances of tough hydrogels with a hydrogen-bond network . ACS Appl. Mater. Interfaces , 2020 , 12 ( 47 ), 53376 − 53384 .

Zheng, S. Y. ; Ding, H. Y. ; Qian, J. ; Yin, J. ; Wu, Z. L. ; Song, Y. H. ; Zheng, Q . Metal-coordination complexes mediated physical hydrogels with high toughness, stick-slip tearing behavior, and good processability . Macromolecules , 2016 , 49 ( 24 ), 9637 − 9646 .

Li, X. F. ; Wang, H. ; Li, D. P. ; Long, S. J. ; Zhang, G. W. ; Wu, Z. L . Dual ionically cross-linked double-network hydrogels with high strength, toughness, swelling resis-tance, and improved 3D printing processability . ACS Appl. Mater. Interfaces , 2018 , 10 ( 37 ), 31198 − 31207 .

Grindy, S. C. ; Learsch, R. ; Mozhdehi, D. ; Cheng, J. ; Barrett, D. G. ; Guan, Z. B. ; Messersmith, P. B. ; Holten-Andersen, N . Control of hierarchical polymer mechanics with bioinspired metal-coordination dynamics . Nat. Mater. , 2015 , 14 ( 12 ), 1210 − 1216 .

Ju, H. Q. ; Zhu, Q. L. ; Zuo, M. ; Liang, S. M. ; Du, M. ; Zheng, Q. ; Wu, Z. L . Toughening hydrogels by forming robust hydrazide-transition metal coordination compl-exes . Chem. Eur. J. , 2023 , 29 ( 38 ), e202300969 .

Li, L. ; Yan, B. ; Yang, J. Q. ; Chen, L. Y. ; Zeng, H. B . Novel mussel-inspired injectable self-healing hydrogel with anti-biofouling property . Adv. Mater. , 2015 , 27 ( 7 ), 1294 − 1299 .

Veiseh, O. ; Doloff, J. C. ; Ma, M. L. ; Vegas, A. J. ; Tam, H. H. ; Bader, A. R. ; Li, J. ; Langan, E. ; Wyckoff, J. ; Loo, W. S. ; Jhunjhunwala, S. ; Chiu, A. ; Siebert, S. ; Tang, K. ; Hollister-Lock, J. ; Aresta-Dasilva, S. ; Bochenek, M. ; Mendoza-Elias, J. ; Wang, Y. ; Qi, M. ; Lavin, D. M. ; Chen, M. ; Dholakia, N. ; Thakrar, R. ; Lacík, I. ; Weir, G. C. ; Oberholzer, J. ; Greiner, D. L. ; Langer, R. ; Anderson, D. G . Size- and shape-dependent foreign body immune response to materials implanted in rodents and non-human Primates . Nat. Mater. , 2015 , 14 ( 6 ), 643 − 651 .

Qamar, S. ; Wang, G. Z. ; Randle, S. J. ; Ruggeri, F. S. ; Varela, J. A. ; Lin, J. Q. ; Phillips, E. C. ; Miyashita, A. ; Williams, D. ; Ströhl, F. ; Meadows, W. ; Ferry, R. ; Dardov, V. J. ; Tartaglia, G. G. ; Farrer, L. A. ; Kaminski Schierle, G. S. ; Kaminski, C. F. ; Holt, C. E. ; Fraser, P. E. ; Schmitt-Ulms, G. ; Klenerman, D. ; Knowles, T. ; Vendruscolo, M. ; St George-Hyslop, P . FUS phase separation is modulated by a molecular chaperone and methylation of arginine cation- π interactions . Cell , 2018 , 173 ( 3 ), 720 − 734.e15 .

Smith, A. M. ; Williams, R. J. ; Tang, C. ; Coppo, P. ; Collins, R. F. ; Turner, M. L. ; Saiani, A. ; Ulijn, R. V . Fmoc-di phenylalanine self assembles to a hydrogel via a novel architecture based on π-π interlocked β-sheets . Adv. Mater. , 2008 , 20 ( 1 ), 37 − 41 .

Zhuang, W. R. ; Wang, Y. ; Cui, P. F. ; Xing, L. ; Lee, J. ; Kim, D. ; Jiang, H. L. ; Oh, Y. K . Applications of π - π stacking interactions in the design of drug-delivery systems . J. Control. Release , 2019 , 294 , 311 − 326 .

Qiu, H. N. ; Hao, X. P. ; Hou, L. X. ; Cui, K. P. ; Du, M. ; Zheng, Q. ; Wu, Z. L . Formation and destruction of polyelectrolyte/surfactant complexes for the toughening of hydrogels . Macromolecules , 2023 , 56 ( 21 ), 8887 − 8898 .

Zhang, X. N. ; Wang, Y. J. ; Sun, S. T. ; Hou, L. ; Wu, P. Y. ; Wu, Z. L. ; Zheng, Q . A tough and stiff hydrogel with tunable water content and mechanical properties based on the synergistic effect of hydrogen bonding and hydrophobic interaction . Macromolecules , 2018 , 51 ( 20 ), 8136 − 8146 .

张雅涵 , 崔春燕 , 谢飞 , 刘文广 . 水凝胶医用防污涂层研究进展 . 中国科学: 技术科学 , 2021 , 51 ( 11 ), 1348 − 1361 .

Zhang, Y. S. ; Khademhosseini, A . Advances in engine-ering hydrogels . Science , 2017 , 356 ( 6337 ), eaaf3627 .

Taylor, D. L. ; in het Panhuis, M . Self-healing hydrogels . Adv. Mater. , 2016 , 28 ( 41 ), 9060 − 9093 .

Chen, Y. N. ; Peng, L. F. ; Liu, T. Q. ; Wang, Y. X. ; Shi, S. J. ; Wang, H. L . Poly(vinyl alcohol)–tannic acid hydrogels with excellent mechanical properties and shape memory behaviors . ACS Appl. Mater. Interfaces , 2016 , 8 ( 40 ), 27199 − 27206 .

Liu, C. ; Morimoto, N. ; Jiang, L. ; Kawahara, S. ; Norito-mi, T. ; Yokoyama, H. ; Mayumi, K. ; Ito, K . Tough hydro-gels with rapid self-reinforcement . Science , 2021 , 372 ( 6546 ), 1078 − 1081 .

Cong, H. P. ; Chen, J. F. ; Yu, S. H . Graphene-based macroscopic assemblies and architectures: an emerging material system . Chem. Soc. Rev. , 2014 , 43 ( 21 ), 7295 − 7325 .

Hu, J. Y. ; Jiao, D. J. ; Hao, X. P. ; Kong, X. R. ; Zhang, X. N. ; Du, M. ; Zheng, Q. ; Wu, Z. L . A facile strategy to fabricate tough and adhesive elastomers by in situ formation of coordination complexes as physical crosslinks . Adv. Funct. Mater. , 2023 , 33 ( 51 ), 2307402 .

倪楚君 , 谢涛 . 可时空编程的超分子形状记忆高分子 . 高分子学报 , 2022 , 53 ( 10 ), 1161 − 1172 .

Cui, C. Y. ; Fan, C. C. ; Wu, Y. H. ; Xiao, M. ; Wu, T. L. ; Zhang, D. F. ; Chen, X. Y. ; Liu, B. ; Xu, Z. Y. ; Qu, B. ; Liu, W. G . Water-triggered hyperbranched polymer univ-ersal adhesives: from strong underwater adhesion to rapid sealing hemostasis . Adv. Mater. , 2019 , 31 ( 49 ), 1905761 .

Liu, S. J. ; Li, L . Ultrastretchable and self-healing double-network hydrogel for 3D printing and strain sensor . ACS Appl. Mater. Interfaces , 2017 , 9 ( 31 ), 26429 − 26437 .

Wang, Z. W. ; Cong, Y. ; Fu, J . Stretchable and tough conductive hydrogels for flexible pressure and strain sensors . J. Mater. Chem. B , 2020 , 8 ( 16 ), 3437 − 3459 .

Wirthl, D. ; Pichler, R. ; Drack, M. ; Kettlguber, G. ; Moser, R. ; Gerstmayr, R. ; Hartmann, F. ; Bradt, E. ; Kaltseis, R. ; Siket, C. M. ; Schausberger, S. E. ; Hild, S. ; Bauer, S. ; Kal-tenbrunner, M . Instant tough bonding of hydrogels for soft machines and electronics . Sci. Adv. , 2017 , 3 ( 6 ), e1700053 .

刘玉霞 , 陈列 , 赵紫光 , 房若辰 , 刘明杰 . 仿生多尺度功能水凝胶的设计与制备：从二维界面到三维网络 . 高分子学报 , 2018 , 49 ( 9 ), 1155 − 1174 .

Zhang, Z. J. ; Chen, Q. ; Colby, R. H . Dynamics of assoc-iative polymers . Soft Matter , 2018 , 14 ( 16 ), 2961 − 2977 .

Van Ruymbeke, E . Preface: special issue on associating polymers . J. Rheol. , 2017 , 61 ( 6 ), 1099 − 1102 .

Zhang, L. H. ; Brostowitz, N. R. ; Cavicchi, K. A. ; Weiss, R. A . Perspective: ionomer research and applications . Macromol. React. Eng. , 2014 , 8 ( 2 ), 81 − 99 .

Wang, Z. F. ; Li, H. F. ; Tang, Z. J. ; Liu, Z. X. ; Ruan, Z. H. ; Ma, L. T. ; Yang, Q. ; Wang, D. H. ; Zhi, C. Y . Hydrogel electrolytes for flexible aqueous energy storage devices . Adv. Funct. Mater. , 2018 , 28 ( 48 ), 1804560 .

胡佳妤 , 杜聪 , 张歆宁 , 郑强 , 吴子良 . 玻璃态水凝胶: 从凝胶材料的新状态到高性能 . 高分子学报 , 2023 , 54 ( 12 ), 1795 − 1816 .

Yang, J. W. ; Bai, R. B. ; Chen, B. H. ; Suo, Z. G . Hydro-gel adhesion: a supramolecular synergy of chemistry, topology, and mechanics . Adv. Funct. Mater. , 2020 , 30 ( 2 ), 1901693 .

Sun, J. Y. ; Zhao, X. H. ; Illeperuma, W. R. K. ; Chaudhuri, O. ; Oh, K. H. ; Mooney, D. J. ; Vlassak, J. J. ; Suo, Z. G . Highly stretchable and tough hydrogels . Nature , 2012 , 489 ( 7414 ), 133 − 136 .

Du, C. ; Zhang, X. N. ; Sun, T. L. ; Du, M. ; Zheng, Q. ; Wu, Z. L . Hydrogen-bond association-mediated dynamics and viscoelastic properties of tough supramolecular hydrogels . Macromolecules , 2021 , 54 ( 9 ), 4313 − 4325 .

Ahmadi, M. ; Jangizehi, A. ; van Ruymbeke, E. ; Seiffert, S . Deconvolution of the effects of binary associations and collective assemblies on the rheological properties of entangled side-chain supramolecular polymer networks . Macromolecules , 2019 , 52 ( 14 ), 5255 − 5267 .

Chen, Q. ; Zhang, Z. J. ; Colby, R. H . Viscoelasticity of entangled random polystyrene ionomers . J. Rheol. , 2016 , 60 ( 6 ), 1031 − 1040 .

Takata, T. ; Aoki, D . Topology-transformable polymers: linear-branched polymer structural transformation via the mechanical linking of polymer chains . Polym. J. , 2018 , 50 ( 1 ), 127 − 147 .

Lewis, C. L. ; Stewart, K. ; Anthamatten, M . The influ-ence of hydrogen bonding side-groups on viscoelas-tic behavior of linear and network polymers . Macromolecules , 2014 , 47 ( 2 ), 729 − 740 .

Ianniruberto, G. ; Brasiello, A. ; Marrucci, G . Modeling unentangled polystyrene melts in fast elongational flows . Macromolecules , 2019 , 52 ( 12 ), 4610 − 4616 .

De Gennes, P. G. Dynamics of entangled polymer solu-tions. I . Rouse model . Macromolecules , 1976 , 9 ( 4 ), 587 − 593 .

Rubinstein, M. ; Colby, R. H . Polymer Physics . New York : Oxford University Press , 2003 .

Kremer, K. ; Grest, G. S . Dynamics of entangled linear polymer melts: a molecular-dynamics simulation . 1990 , 92 ( 8 ), 5057 − 5086 .

Ahmadi, M. ; Hawke, L. G. D. ; Goldansaz, H. ; van Ruymbeke, E . Dynamics of entangled linear supramo-lecular chains with sticky side groups: influence of hinde-red fluctuations . Macromolecules , 2015 , 48 ( 19 ), 7300 − 7310 .

Tang, S. C. ; Wang, M. Z. ; Olsen, B. D . Anomalous self-diffusion and sticky rouse dynamics in associative protein hydrogels . J. Am. Chem. Soc. , 2015 , 137 ( 11 ), 3946 − 3957 .

Tanaka, F. ; Edwards, S. F . Viscoelastic properties of physically crosslinked networks. 1. Transient network theory . Macromolecules , 1992 , 25 ( 5 ), 1516 − 1523 .

Biswas, C. S. ; Wu, Y. H. ; Wang, Q. ; Du, L. ; Mitra, K. ; Ray, B. ; Yan, Z. C. ; Du, B. ; Stadler, F. J . Effect of tacti-city and molecular weight on the rheological properties of poly( N -isopropylacrylamide) gels in benzyl alcohol . J. Rheol. , 2017 , 61 ( 6 ), 1345 − 1357 .

Shivokhin, M. E. ; Narita, T. ; Talini, L. ; Habicht, A. ; Seiffert, S. ; Indei, T. ; Schieber, J. D . Interplay of entanglement and association effects on the dynamics of semidilute solutions of multisticker polymer chains . J. Rheol. , 2017 , 61 ( 6 ), 1231 − 1241 .

Shabbir, A. ; Huang, Q. ; Baeza, G. P. ; Vlassopoulos, D. ; Chen, Q. ; Colby, R. H. ; Alvarez, N. J. ; Hassager, O . Nonlinear shear and uniaxial extensional rheology of polyether-ester-sulfonate copolymer ionomer melts . J. Rheol. , 2017 , 61 ( 6 ), 1279 − 1289 .

Leibler, L. ; Rubinstein, M. ; Colby, R. H . Dynamics of reversible networks . Macromolecules , 1991 , 24 ( 16 ), 4701 − 4707 .

Chen, Q. ; Tudryn, G. J. ; Colby, R. H . Ionomer dynamics and the sticky Rouse model . J. Rheol. , 2013 , 57 ( 5 ), 1441 − 1462 .

Wang, Y. H. ; He, J. ; Aktas, S. ; Sukhishvili, S. A. ; Kalyon, D. M . Rheological behavior and self-healing of hydrogen-bonded complexes of a triblock Pluronic ® copolymer with a weak polyacid . J. Rheol. , 2017 , 61 ( 6 ), 1103 − 1119 .

Sun, T. L. ; Kurokawa, T. ; Kuroda, S. ; Ihsan, A. B. ; Akasaki, T. ; Sato, K. ; Haque, M. A. ; Nakajima, T. ; Gong, J. P . Physical hydrogels composed of polyampholytes demonstrate high toughness and viscoelasticity . Nat. Mater. , 2013 , 12 ( 10 ), 932 − 937 .

Akkaoui, K. ; Yang, M. ; Digby, Z. A. ; Schlenoff, J. B . Ultraviscosity in entangled polyelectrolyte complexes and coacervates . Macromolecules , 2020 , 53 ( 11 ), 4234 − 4246 .

Ahmadi, M. ; Seiffert, S . Dynamic model metallo-supramolecular dual-network hydrogels with independently tunable network crosslinks . J. Polym. Sci. , 2020 , 58 ( 2 ), 330 − 342 .

Holten-Andersen, N. ; Jaishankar, A. ; Harrington, M. J. ; Fullenkamp, D. E. ; DiMarco, G. ; He, L. H. ; McKinley, G. H. ; Messersmith, P. B. ; Lee, K. Y. C . Metal-coordination: using one of nature's tricks to control soft material mechanics . J. Mater. Chem. B , 2014 , 2 ( 17 ), 2467 − 2472 .

Li, X. Y. ; Gong, J. P . Role of dynamic bonds on fatigue threshold of tough hydrogels . Proc. Natl. Acad. Sci. USA , 2022 , 119 ( 20 ), e2200678119 .

Ali, S. ; Prabhu, V. M . Relaxation behavior by time-salt and time-temperature superpositions of polyelectrolyte complexes from coacervate to precipitate . Gels , 2018 , 4 ( 1 ), 11 .

Spruijt, E. ; Sprakel, J. ; Lemmers, M. ; Stuart, M. A. C. ; van der Gucht, J . Relaxation dynamics at different time scales in electrostatic complexes: time-salt superposition . Phys. Rev. Lett. , 2010 , 105 ( 20 ), 208301 .

Hu, X. B. ; Zhou, J. ; Daniel, W. F. M. ; Vatankhah-Varnoosfaderani, M. ; Dobrynin, A. V. ; Sheiko, S. S . Dynamics of dual networks: strain rate and temperature effects in hydrogels with reversible H-bonds . Macromolecules , 2017 , 50 ( 2 ), 652 − 659 .

Wang, C. ; Deitrick, K. ; Seo, J. ; Cheng, Z. W. ; Zacharia, N. S. ; Weiss, R. A. ; Vogt, B. D . Manipulating the mecha-nical response of hydrophobically cross-linked hydro-gels with ionic associations . Macromolecules , 2019 , 52 ( 16 ), 6055 − 6067 .

Karobi, S. N. ; Sun, T. L. ; Kurokawa, T. ; Luo, F. ; Naka-jima, T. ; Nonoyama, T. ; Gong, J. P . Creep behavior and delayed fracture of tough polyampholyte hydrogels by tensile test . Macromolecules , 2016 , 49 ( 15 ), 5630 − 5636 .

Henderson, K. J. ; Shull, K. R . Effects of solvent composition on the assembly and relaxation of triblock copolymer-based polyelectrolyte gels . Macromolecules , 2012 , 45 ( 3 ), 1631 − 1635 .

Niu, H. ; Wang, F. ; Weiss, R. A . Hydrophobic/hydrophilic triblock copolymers: synthesis and properties of physically cross-linked hydrogels . Macromolecules , 2015 , 48 ( 3 ), 645 − 654 .

杜宇 , 杨凯 , 俞炜 , 周持兴 . 触变/非触变水凝胶的傅里叶变换流变学研究 . 高分子学报 , 2012 , 43 ( 12 ), 1376 − 1382 .

Grindy, S. C. ; Lenz, M. ; Holten-Andersen, N . Engi-neering elasticity and relaxation time in metal-coordinate cross-linked hydrogels . Macromolecules , 2016 , 49 ( 21 ), 8306 − 8312 .

Cui, K. P. ; Ye, Y. N. ; Yu, C. T. ; Li, X. Y. ; Kurokawa, T. ; Gong, J. P . Stress relaxation and underlying structure evolution in tough and self-healing hydrogels . ACS Macro Lett. , 2020 , 9 ( 11 ), 1582 − 1589 .

Holten-Andersen, N. ; Harrington, M. J. ; Birkedal, H. ; Lee, B. P. ; Messersmith, P. B. ; Lee, K. Y. C. ; Waite, J. H . pH-induced metal-ligand cross-links inspired by mussel yield self-healing polymer networks with near-covalent elastic moduli . Proc. Natl. Acad. Sci. USA , 2011 , 108 ( 7 ), 2651 − 2655 .

Wang, Y. J. ; Zhang, X. N. ; Song, Y. H. ; Zhao, Y. P. ; Chen, L. ; Su, F. M. ; Li, L. B. ; Wu, Z. L. ; Zheng, Q . Ultrastiff and tough supramolecular hydrogels with a dense and robust hydrogen bond network . Chem. Mater. , 2019 , 31 ( 4 ), 1430 − 1440 .

Guo, J. Y. ; Long, R. ; Mayumi, K. ; Hui, C. Y . Mechanics of a dual cross-link gel with dynamic bonds: steady state kinetics and large deformation effects . Macromolecules , 2016 , 49 ( 9 ), 3497 − 3507 .

Long, R. ; Mayumi, K. ; Creton, C. ; Narita, T. ; Hui, C. Y . Rheology of a dual crosslink self-healing gel: theory and measurement using parallel-plate torsional rheom-etry . J. Rheol. , 2015 , 59 ( 3 ), 643 − 665 .

Long, R. ; Mayumi, K. ; Creton, C. ; Narita, T. ; Hui, C. Y . Time dependent behavior of a dual cross-link self-healing gel: theory and experiments . Macromolecules , 2014 , 47 ( 20 ), 7243 − 7250 .

Narita, T. ; Mayumi, K. ; Ducouret, G. ; Hébraud, P . Viscoelastic properties of poly(vinyl alcohol) hydrogels having permanent and transient cross-links studied by microrheology, classical rheometry, and dynamic light scattering . Macromolecules , 2013 , 46 ( 10 ), 4174 − 4183 .

Ahmadi, M. ; Nicolella, P. ; Seiffert, S . Network perco-lation in transient polymer networks with temporal hierarchy of energy dissipation . Macromolecules , 2022 , 55 ( 22 ), 9960 − 9971 .

Ahmadi, M. ; Seiffert, S . Coordination geometry prefe-rence regulates the structure and dynamics of metallo-supramolecular polymer networks . Macromolecules , 2021 , 54 ( 3 ), 1388 − 1400 .

Zhang, X. N. ; Du, C. ; Wang, Y. J. ; Hou, L. X. ; Du, M. ; Zheng, Q. ; Wu, Z. L . Influence of the α -methyl group on elastic-to-glassy transition of supramolecular hydrogels with hydrogen-bond associations . Macromolecules , 2022 , 55 ( 17 ), 7512 − 7525 .

Huang, Z. H. ; Chen, X. Y. ; O’Neill, S. J. K. ; Wu, G. L. ; Whitaker, D. J. ; Li, J. X. ; McCune, J. A. ; Scherman, O. A . Highly compressible glass-like supramolecular polymer networks . Nat. Mater. , 2022 , 21 ( 1 ), 103 − 109 .

Huang, Z. H. ; Chen, X. Y. ; Wu, G. L. ; Metrangolo, P. ; Whitaker, D. ; McCune, J. A. ; Scherman, O. A . Host-enhanced phenyl-perfluorophenyl polar- π interactions . J. Am. Chem. Soc. , 2020 , 142 ( 16 ), 7356 − 7361 .

Gong, J. P. ; Katsuyama, Y. ; Kurokawa, T. ; Osada, Y . Double-network hydrogels with extremely high mech-anical strength . Adv. Mater. , 2003 , 15 ( 14 ), 1155 − 1158 .

Luo, F. ; Sun, T. L. ; Nakajima, T. ; Kurokawa, T. ; Zhao, Y. ; Sato, K. ; Ihsan, A. B. ; Li, X. F. ; Guo, H. L. ; Gong, J. P . Oppositely charged polyelectrolytes form tough, self-healing, and rebuildable hydrogels . Adv. Mater. , 2015 , 27 ( 17 ), 2722 − 2727 .

Yang, C. H. ; Suo, Z. G . Hydrogel ionotronics . Nat. Rev. Mater. , 2018 , 3 ( 6 ), 125 − 142 .

Wang, Y. J. ; Li, C. Y. ; Wang, Z. J. ; Zhao, Y. P. ; Chen, L. ; Wu, Z. L. ; Zheng, Q . Hydrogen bond-reinforced double-network hydrogels with ultrahigh elastic modulus and shape memory property . J. Polym. Sci. Part B Polym. Phys. , 2018 , 56 ( 19 ), 1281 − 1286 .

Zhang, X. N. ; Du, C. ; Du, M. ; Zheng, Q. ; Wu, Z. L . Kinetic insights into glassy hydrogels with hydrogen bond complexes as the cross-links . Mater. Today Phys. , 2020 , 15 , 100230 .

侯磊 , 武培怡 . 二维相关红外光谱分析技术在高分子表征中的应用 . 高分子学报 , 2022 , 53 ( 5 ), 522 − 538 .

浏览量

255

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

两个典型橡胶树品种制备烟片胶的结构与性能研究

超高分子量聚乙烯纤维的工业化制备和构效关系综述

熔融沉积成型3D打印聚醚醚酮工艺优化研究进展

热、力及其复合外场原位辅助熔融沉积成型技术研究进展

刺激响应性水凝胶在肿瘤治疗中的研究进展