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
- Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe³⁺ Coordination Interactions
- 高分子科学（英文版） 2023年41卷第2期页码：250-257
- 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：
  
  This work was financially supported by National Natural Science Foundation of China (No. 51873110).;Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-022-2818-x.
- DOI：10.1007/s10118-022-2818-x
  中图分类号：
- 收稿：2022-05-11，
  
  修回：2022-5-22，
  
  录用：2022-6-10，
  
  网络首发：2022-08-31，
  
  纸质出版：2023-02-01
- 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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Ultra-robust Metallosupramolecular Hydrogels with Unprecedented Self-recoverability Using Asymmetrically Distributed Carboxyl-Fe3+ Coordination Interactions

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

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