Super Tough, Highly Ionically Conductive, Self-healing Elastomers with Dynamic Metal Coordination Crosslinks for Flexible Sensors

Ming-Jun Tang; Jian-Hui Yan; Yu-Jun Liu; Yi Wei; Yu-Xi Li; Xu-Ming Xie

doi:10.1007/s10118-025-3377-8

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Super Tough, Highly Ionically Conductive, Self-healing Elastomers with Dynamic Metal Coordination Crosslinks for Flexible Sensors

RESEARCH ARTICLE | Updated：2025-08-25

- Super Tough, Highly Ionically Conductive, Self-healing Elastomers with Dynamic Metal Coordination Crosslinks for Flexible Sensors
- Super Tough, Highly Ionically Conductive, Self-healing Elastomers with Dynamic Metal Coordination Crosslinks for Flexible Sensors
- 高分子科学（英文） 2025年43卷第9期页码：1565-1575
- Affiliations：
  
  Key Laboratory of Advanced Materials (MOE), Department of Chemical Engineering, Tsinghua University, Beijing 100084, China
- Author bio：
  
  xxm-dce@mail.tsinghua.edu.cn
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (Nos. 52273023, 51973103, and 21774069).;Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-025-3377-8.
- DOI：10.1007/s10118-025-3377-8
  中图分类号：
- 收稿日期：2025-04-10，
  
  修回日期：2025-05-05，
  
  录用日期：2025-05-06，
  
  网络出版日期：2025-07-08，
  
  纸质出版日期：2025-09-05
- Accepted：
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Tang, M. J.; Yan, J. H.; Liu, Y. J.; Wei, Y.; Li, Y. X.; Xie, X. M. Super tough, highly ionically conductive, self-healing elastomers with dynamic metal coordination crosslinks for flexible sensors. Chinese J. Polym. Sci. 2025, 43, 1565–1575

Ming-Jun Tang, Jian-Hui Yan, Yu-Jun Liu, et al. Super Tough, Highly Ionically Conductive, Self-healing Elastomers with Dynamic Metal Coordination Crosslinks for Flexible Sensors[J]. Chinese journal of polymer science, 2025, 43(9): 1565-1575.
Tang, M. J.; Yan, J. H.; Liu, Y. J.; Wei, Y.; Li, Y. X.; Xie, X. M. Super tough, highly ionically conductive, self-healing elastomers with dynamic metal coordination crosslinks for flexible sensors. Chinese J. Polym. Sci. 2025, 43, 1565–1575 DOI： 10.1007/s10118-025-3377-8.

Ming-Jun Tang, Jian-Hui Yan, Yu-Jun Liu, et al. Super Tough, Highly Ionically Conductive, Self-healing Elastomers with Dynamic Metal Coordination Crosslinks for Flexible Sensors[J]. Chinese journal of polymer science, 2025, 43(9): 1565-1575. DOI： 10.1007/s10118-025-3377-8.

摘要

A transparent

self-healing elastomer with superior mechanical properties and high ionic conductivity was fabricated

via

physically blending of polyethylene glycol (PEG) free chains and structurally similar polyacrylate elastomers

enabled by imidazole-Zn

coordination crosslinking.

Abstract

Integrated conductive elastomers with excellent mechanical performance

stable high conductivity

self-healing capabilities

and high transparency are critical for advancing wearable devices. Nevertheless

achieving an optimal balance among these properties remains a significant challenge. Herein

through in situ free-radical copolymerization of 2-[2-(2-methoxyethoxy)ethoxy

]

ethyl acrylate (TEEA) and vinylimidazole (VI) in the presence of polyethylene glycol (PEG;

=400)

tough P(TEEA-

-VI)/PEG elastomers with multiple functionalities were prepared

in which P(TEEA-

-VI) was dynamically cross-linked by imidazole-Zn

metal coordination crosslinks

and physically blended with PEG as polymer electrolyte to form a homogeneous mixt

ure. Notably

has a negligible impact on the polymerization process

allowing for the in situ formation of numerous imidazole-Zn

metal coordination crosslinks

which can effectively dissipate energy upon stretching to largely reinforce the elastomers. The obtained P(TEEA-

-VI)/PEG elastomers exhibited a high toughness of 10.0 MJ·m

–3

with a high tensile strength of 3.3 MPa and a large elongation at break of 645%

along with outstanding self-healing capabilities due to the dynamic coordination crosslinks. Moreover

because of the miscibility of PEG with PTEEA copolymer matrix

and Li

can form weak coordination interactions with the ethoxy (EO) units in PEG and PTEEA

acting as a bridge to integrate PEG into the elastomer network. The resulted P(TEEA-

-VI)/PEG elastomers showed high transparency (92%) and stable high conductivity of 1.09×10

–4

S·cm

–1

. In summary

the obtained elastomers exhibited a well-balanced combination of high toughness

high ionic conductivity

excellent self-healing capabilities

and high transparency

making them promising for applications in flexible strain sensors.

关键词

Keywords

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