Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation

Yu-Hong Zhang; Jian-Fei Ma; Hao-Bo Wei; Jie Wang; Feng Wang

doi:10.1007/s10118-026-3700-z

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Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation

Special Topic: Chirality in Polymers | Updated：2026-08-31

- Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation
- Chinese Journal of Polymer Science Vol. 44, Issue 9, Pages: 2862-2871(2026)
- Affiliations：
  
  a.Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei 230026, China
  b.School of Chemistry and Pharmaceutical Engineering, Jilin University of Chemical Technology, Jilin 132022, China
- Author bio：
  
  drfwang@ustc.edu.cn
- Funds：
- DOI：10.1007/s10118-026-3700-z
  CLC：
- Received：10 April 2026，
  
  Accepted：04 May 2026，
  
  Online First：06 July 2026，
  
  Published：05 September 2026
- Accepted：
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Zhang, Y. H.; Ma, J. F.; Wei, H. B.; Wang, J.; Wang, F. Squaramide-directed cooperative one-dimensional assembly in telechelic polydimethylsiloxane for hierarchical network formation. Chinese J. Polym. Sci. 2026, 44, 2862–2871

Yu-Hong Zhang, Jian-Fei Ma, Hao-Bo Wei, et al. Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation[J]. Chinese Journal of Polymer Science, 2026, 44(9): 2862-2871.
Zhang, Y. H.; Ma, J. F.; Wei, H. B.; Wang, J.; Wang, F. Squaramide-directed cooperative one-dimensional assembly in telechelic polydimethylsiloxane for hierarchical network formation. Chinese J. Polym. Sci. 2026, 44, 2862–2871 DOI： 10.1007/s10118-026-3700-z.

Yu-Hong Zhang, Jian-Fei Ma, Hao-Bo Wei, et al. Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation[J]. Chinese Journal of Polymer Science, 2026, 44(9): 2862-2871. DOI： 10.1007/s10118-026-3700-z.

摘要

A squaramide-directed cooperative assembly strategy was developed to construct hierarchical polymer networks by integrating 1D supramolecular nanofibers into covalent architectures. This approach effectively reconciles the trade-off between covalent robustness and supramolecular reversibility

leading to a significantly enhanced thermal stability and mechanical performance.

Abstract

Polymer crosslinked networks often face a fundamental trade-off between the mechanical robustness of covalent systems and the dynamic reversibility of supramolecular assemblies. Inspired by the hierarchical organization of biological extracellular matrix

where fibrous structures are reinforced by covalent crosslinking

we report a squaramide-directed cooperative assembly strategy that integrates one-dimensional (1D) supramolecular nanofiber formation with covalent macromolecular architecture to construct hierarchical polymer networks. Telechelic macromolecules were designed by tethering orthogonally arranged squaramide–amide hydrogen-bonding motifs to polydimethylsiloxane (PDMS) spacers. In the model system

these motifs undergo cooperative nucleation-elongation assembly into long-range nanofibers

while comparison with a urea analogue reveals enhanced intermolecular binding and assembly stability arising from the squaramide motif. Covalent integration of the assembling units transforms discrete nanofibers into microphase-separated networks with increased thermal stability and storage modulus. This work establishes a molecular design principle linking cooperative self-assembly with hierarchical polymer network formation and macroscopic mechanical performance.

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references

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