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
- Squaramide-directed Cooperative One-dimensional Assembly in Telechelic Polydimethylsiloxane for Hierarchical Network Formation
- Chinese Journal of Polymer Science 2026年44卷第9期页码：2862-2871
- 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：
  
  This study was financially supported by the National Natural Science Foundation of China (Nos. 22371272 and 92356302) and the International Partnership Program of the Chinese Academy of Sciences (No. 123GJHZ2022064MI). We are grateful for the technical support provided by the High Performance Computing Center of the University of Science and Technology of China for the DFT and TD-DFT computations.;The authors declare no interest conflict.Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-026-3700-z.The data supporting the findings of this study are available from the corresponding author upon reasonable request.
- DOI：10.1007/s10118-026-3700-z
  中图分类号：
- 收稿：2026-04-10，
  
  录用：2026-05-04，
  
  网络首发：2026-07-06，
  
  纸质出版：2026-09-05
- 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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