Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe<sup>3+</sup> Coordination Interactions

Zhao-Yang Yuan; Zhen-Xing Cao; Rui Wu; Hui Li; Qiong-Jun Xu; Hai-Tao Wu; Jing Zheng; Jin-Rong Wu

doi:10.1007/s10118-022-2818-x

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Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe³⁺ Coordination Interactions

RESEARCH ARTICLE | Updated：2023-01-06

- Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe³⁺ Coordination Interactions
- Chinese Journal of Polymer Science Vol. 41, Issue 2, Pages: 250-257(2023)
- 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/s10118-022-2818-x
  CLC：
- Received：11 May 2022，
  
  Revised：2022-5-22，
  
  Accepted：10 June 2022，
  
  Online First：31 August 2022，
  
  Published：01 February 2023
- Accepted：
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Yuan, Z. Y.; Cao, Z. X.; Wu, R.; Li, H.; Xu, Q. J.; Wu, H. T.; Zheng, J.; Wu, J. R. Ultra-robust metallosupramolecular hydrogels with unprecedented self-recoverability using asymmetrically distributed carboxyl-Fe³⁺ coordination interactions. Chinese J. Polym. Sci. 2023, 41, 250–257 DOI: 10.1007/s10118-022-2818-x.

Zhao-Yang Yuan, Zhen-Xing Cao, Rui Wu, et al. Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe³⁺ Coordination Interactions[J]. Chinese Journal of Polymer Science, 2023, 41(2): 250-257. DOI: 10.1007/s10118-022-2818-x.
Yuan, Z. Y.; Cao, Z. X.; Wu, R.; Li, H.; Xu, Q. J.; Wu, H. T.; Zheng, J.; Wu, J. R. Ultra-robust metallosupramolecular hydrogels with unprecedented self-recoverability using asymmetrically distributed carboxyl-Fe³⁺ coordination interactions. Chinese J. Polym. Sci. 2023, 41, 250–257 DOI: 10.1007/s10118-022-2818-x. DOI：

Zhao-Yang Yuan, Zhen-Xing Cao, Rui Wu, et al. Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe³⁺ Coordination Interactions[J]. Chinese Journal of Polymer Science, 2023, 41(2): 250-257. DOI: 10.1007/s10118-022-2818-x. DOI：

摘要

Mechanically robust metallosupramolecular hydrogels with unprecedented self-recoverability are crosslinked via asymmetrically distributed coordination interactions and minimal chemical crosslinkers. The hydrogels possess excellent mechanical properties and stretch rate- and temperature-dependent mechanical behavior as well as unprecedented self-recovery performance ever recorded for metallosupramolecular hydrogels.

Abstract

Recently

numerous mechanically robust synthetic hydrogels have been created. However

unlike natural loading-bearing materials such as cartilages and muscles

most hydrogels have inherently contradictory requirements

obstructing the design of hydrogels with characteristics of robustness and rapid self-recoverability. Herein

we present a facile strategy for constructing mechanically robust and rapidly self-recoverable hydrogels. The linear poly(acrylamide-

-itaconic acid) chains crosslink

via

coordination bonds and minimal chemical crosslinkers to form the hydrogel network. Such design endows the coordination interactions to be asymmetrically distributed. Under deformation

the coordination interactions exhibit a reversible dissociation-and-reorganization property

demonstrating a new mechanism for energy dissipation and stress redistribution. Thus

the hydrogels possess tensile strength up to 12.5 MPa and toughness up to 28.2 MJ/m

. Moreover

the inherent dynamic nature of the coordination bonds imparts these hydrogels with stretch rate- and temperature-dependent mechanical behavior as well as excellent self-recovery performance. The method employed in this study is universal and is applicable to other polymers with load-bearing yet rapid recovery conditions. This study will facilitate diverse applications of most metallosupramolecular hydrogels.

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references

Gjorevski, N.; Nikolaev, M.; Brown, T. E.; Mitrofanova, O.; Brandenberg, N.; DelRio, F. W.; Yavitt, F. M.; Liberali, P.; Anseth, K. S.; Lutolf, M. P . Tissue geometry drives deterministic organoid patterning . Science , 2022 . 375 eaaw9021 DOI: 10.1126/science.aaw9021 http://doi.org/10.1126/science.aaw9021 .

Miao, S.; Castro, N.; Nowicki, M.; Xia, L.; Cui, H.; Zhou, X.; Zhu, W.; Lee, S. jun; Sarkar, K.; Vozzi, G.; Tabata, Y.; Fisher, J.; Zhang, L. G . 4D printing of polymeric materials for tissue and organ regeneration . Mater. Today , 2017 . 20 577 - 591 . DOI: 10.1016/j.mattod.2017.06.005 http://doi.org/10.1016/j.mattod.2017.06.005 .

Zhu, J.; Yang, S.; Qi, Y.; Gong, Z.; Zhang, H.; Liang, K.; Shen, P.; Huang, Y.; Zhang, Z.; Ye, W.; Yue, L.; Fan, S.; Shen, S.; Mikos, A . G.; Wang, X.; Fang, X. Stem cell-homing hydrogel-based miR-29b-5p delivery promotes cartilage regeneration by suppressing senescence in an osteoarthritis rat model . Sci. Adv. , 2022 . 8 eabk0011 DOI: 10.1126/sciadv.abk0011 http://doi.org/10.1126/sciadv.abk0011 .

Liang, Q.; Xia, X.; Sun, X.; Yu, D.; Huang, X.; Han, G.; Mugo, S . M.; Chen, W.; Zhang, Q. Highly stretchable hydrogels as wearable and implantable sensors for recording physiological and brain neural signals . Adv. Sci. , 2022 . 2201059 .

Zhang, C.; Wang, M.; Jiang, C.; Zhu, P.; Sun, B.; Gao, Q.; Gao, C.; Liu, R . Highly adhesive and self-healing γ -PGA/PEDOT:PSS conductive hydrogels enabled by multiple hydrogen bonding for wearable electronics . Nano Energy , 2022 . 95 106991 DOI: 10.1016/j.nanoen.2022.106991 http://doi.org/10.1016/j.nanoen.2022.106991 .

Zhuo, S.; Song, C.; Rong, Q.; Zhao, T.; Liu, M . Shape and stiffness memory ionogels with programmable pressure-resistance response . Nat. Commun. , 2022 . 13 1743 DOI: 10.1038/s41467-022-29424-z http://doi.org/10.1038/s41467-022-29424-z .

Li, J.; Jiang, Z.; Wang, Y.; Zheng, J.; Huang, G . Stability, seepage and displacement characteristics of heterogeneous branched-preformed particle gels for enhanced oil recovery . RSC Adv. , 2018 . 8 4881 - 4889 . DOI: 10.1039/C7RA13152F http://doi.org/10.1039/C7RA13152F .

Yin, H.; Yin, X.; Cao, R.; Zeng, P.; Wang, J.; Wu, D.; Luo, X.; Zhu, Y.; Zheng, Z.; Feng, Y . In situ crosslinked weak gels with ultralong and tunable gelation times for improving oil recovery . Chem. Eng. J. , 2021 . 432 134350 .

Kim, J.; Zhang, G.; Shi, M.; Suo, Z . Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links . Science , 2021 . 374 212 - 216 . DOI: 10.1126/science.abg6320 http://doi.org/10.1126/science.abg6320 .

Cao, Z.; Wang, Y.; Wang, H.; Ma, C.; Li, H.; Zheng, J.; Wu, J.; Huang, G . Tough, ultrastretchable and tear-resistant hydrogels enabled by linear macro-cross-linker . Polym. Chem. , 2019 . 10 3503 - 3513 . DOI: 10.1039/C9PY00600A http://doi.org/10.1039/C9PY00600A .

Hua, M.; Wu, S.; Ma, Y.; Zhao, Y.; Chen, Z.; Frenkel, I.; Strzalka, J.; Zhou, H.; Zhu, X.; He, X . Strong tough hydrogels via the synergy of freeze-casting and salting out . Nature , 2021 . 590 594 - 599 . DOI: 10.1038/s41586-021-03212-z http://doi.org/10.1038/s41586-021-03212-z .

Liu, X.; Wu, J.; Qiao, K.; Liu, G.; Wang, Z.; Lu, T.; Suo, Z.; Hu, J . Topoarchitected polymer networks expand the space of material properties . Nat. Commun. , 2022 . 13 1622 DOI: 10.1038/s41467-022-29245-0 http://doi.org/10.1038/s41467-022-29245-0 .

Gong, J . P.; Katsuyama, Y.; Kurokawa, T.; Osada, Y. Double-network hydrogels with extremely high mechanical strength . Adv. Mater. , 2003 . 15 1155 - 1158 . DOI: 10.1002/adma.200304907 http://doi.org/10.1002/adma.200304907 .

Gong, J. P . Why are double network hydrogels so tough . Soft Matter , 2010 . 6 2583 - 2590 . DOI: 10.1039/b924290b http://doi.org/10.1039/b924290b .

Liu, C.; Morimoto, N.; Jiang, L.; Kawahara, S.; Noritomi, T.; Yokoyama, H.; Mayumi, K.; Ito, K . Tough hydrogels with rapid self-reinforcement . Science , 2021 . 372 1078 - 1081 . DOI: 10.1126/science.aaz6694 http://doi.org/10.1126/science.aaz6694 .

Liu, R.; Wang, H.; Lu, W.; Cui, L.; Wang, S.; Wang, Y.; Chen, Q.; Guan, Y.; Zhang, Y . Highly tough, stretchable and resilient hydrogels strengthened with molecular springs and their application as a wearable, flexible sensor . Chem. Eng. J. , 2021 . 415 128839 DOI: 10.1016/j.cej.2021.128839 http://doi.org/10.1016/j.cej.2021.128839 .

Hu, J.; Hiwatashi, K.; Kurokawa, T.; Liang, S. M.; Wu, Z. L.; Gong, J. P . Microgel-reinforced hydrogel films with high mechanical strength and their visible mesoscale fracture structure . Macromolecules , 2011 . 44 7775 - 7781 . DOI: 10.1021/ma2016248 http://doi.org/10.1021/ma2016248 .

Xia, L. W.; Xie, R.; Ju, X. J.; Wang, W.; Chen, Q.; Chu, L. Y . Nano-structured smart hydrogels with rapid response and high elasticity . Nat. Commun. , 2013 . 4 1 - 11 . .

Nan, W.; Wang, W.; Gao, H.; Liu, W . Fabrication of a shape memory hydrogel based on imidazole-zinc ion coordination for potential cell-encapsulating tubular scaffold application . Soft Matter , 2013 . 9 132 - 137 . DOI: 10.1039/C2SM26918J http://doi.org/10.1039/C2SM26918J .

Sun, T. L.; Kurokawa, T.; Kuroda, S.; Ihsan, A. Bin; 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 . 12 932 - 937 . DOI: 10.1038/nmat3713 http://doi.org/10.1038/nmat3713 .

Lin, P.; Ma, S.; Wang, X.; Zhou, F . Molecularly engineered dual-crosslinked hydrogel with ultrahigh mechanical strength, toughness, and good self-recovery . Adv. Mater. , 2015 . 27 2054 - 2059 . DOI: 10.1002/adma.201405022 http://doi.org/10.1002/adma.201405022 .

Hu, Y.; Du, Z.; Deng, X.; Wang, T.; Yang, Z.; Zhou, W.; Wang, C . Dual physically cross-linked hydrogels with high stretchability, toughness, and good self-recoverability . Macromolecules , 2016 . 49 5660 - 5668 . DOI: 10.1021/acs.macromol.6b00584 http://doi.org/10.1021/acs.macromol.6b00584 .

Zheng, S. Y.; Ding, H.; Qian, J.; Yin, J.; Wu, Z . L.; Song, Y.; Zheng, Q. Metal-coordination complexes mediated physical hydrogels with high toughness, stick-slip tearing behavior, and good processability . Macromolecules , 2016 . 49 9637 - 9646 . DOI: 10.1021/acs.macromol.6b02150 http://doi.org/10.1021/acs.macromol.6b02150 .

Cao, J.; Li, J.; Chen, Y.; Zhang, L.; Zhou, J . Dual physical crosslinking strategy to construct moldable hydrogels with ultrahigh strength and toughness . Adv. Funct. Mater. , 2018 . 28 1800739 DOI: 10.1002/adfm.201800739 http://doi.org/10.1002/adfm.201800739 .

Ma, C.; Wang, Y.; Jiang, Z.; Cao, Z.; Yu, H.; Huang, G.; Wu, Q.; Ling, F.; Zhuang, Z.; Wang, H.; Zheng, J.; Wu, J . Wide-range linear viscoelastic hydrogels with high mechanical properties and their applications in quantifiable stress-strain sensors . Chem. Eng. J. , 2020 . 399 125697 DOI: 10.1016/j.cej.2020.125697 http://doi.org/10.1016/j.cej.2020.125697 .

Yu, H. C.; Zheng, S. Y.; Fang, L.; Ying, Z.; Du, M.; Wang, J.; Ren, K. F.; Wu, Z. L.; Zheng, Q . Reversibly transforming a highly swollen polyelectrolyte hydrogel to an extremely tough one and its application as a tubular grasper . Adv. Mater. , 2020 . 32 2005171 DOI: 10.1002/adma.202005171 http://doi.org/10.1002/adma.202005171 .

Jiao, C.; Zhang, J.; Liu, T.; Peng, X.; Wang, H . Mechanically strong, tough, and shape deformable poly(acrylamide- co -vinylimidazole) hydrogels based on Cu 2+ complexation . ACS Appl. Mater. Interfaces , 2020 . 12 44205 - 44214 . DOI: 10.1021/acsami.0c13654 http://doi.org/10.1021/acsami.0c13654 .

Yu, H. C.; Hao, X. P.; Zhang, C. W.; Zheng, S. Y.; Du, M.; Liang, S.; Wu, Z. L.; Zheng, Q . Engineering tough metallosupramolecular hydrogel films with kirigami structures for compliant soft electronics . Small , 2021 . 17 2103836 DOI: 10.1002/smll.202103836 http://doi.org/10.1002/smll.202103836 .

Sun, J. Y.; Zhao, X.; Illeperuma, W. R. K.; Chaudhuri, O.; Oh, K. H.; Mooney, D. J.; Vlassak, J. J.; Suo, Z . Highly stretchable and tough hydrogels . Nature , 2012 . 489 133 - 136 . DOI: 10.1038/nature11409 http://doi.org/10.1038/nature11409 .

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 - 28318 . DOI: 10.1021/acsami.7b09614 http://doi.org/10.1021/acsami.7b09614 .

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Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe3+ Coordination Interactions

DOI：10.1007/s10118-022-2818-x

摘要

Abstract

关键词

Keywords

references

Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe³⁺ Coordination Interactions