Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement <italic style="font-style: italic">via</italic> Synergistic Disulfide-Zr<sup>4</sup><sup>+</sup> Coordination Bonds

Hao-Kai Yuan; Qian-Qian Hou; Peng Wang; Yao Xu; Lin Zhang; Ying Li; Jie Zhang; Lu Wang; Bing Geng; Chuan-Yong Zong

doi:10.1007/s10118-026-3620-y

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Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds

RESEARCH ARTICLE | Updated：2026-07-01

- Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds
- Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds
- Chinese Journal of Polymer Science 2026年44卷第7期页码：2199-2211
- Affiliations：
  
  a.School of Chemistry and Chemical Engineering, Shandong Provincial Key Laboratory of Extreme Environment-tolerant Specialty Chemicals, University of Jinan, Jinan 250022, China
  b.Shandong Institute of Non-Metallic Materials, Jinan 250031, China
  c.National Key Laboratory of Aerospace Chemical Power, Hubei Institute of Aerospace Chemotechnology, Xiangyang 441003, China
  d.School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
- Author bio：
  
  chm_wangl@ujn.edu.cn (L.W.)
  chm_gengb@ujn.edu.cn (B.G.)
  chm_zongcy@ujn.edu.cn (C.Y.Z.)
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China (No. 52503154) and Shandong Provincial Natural Science Foundation (Nos. ZR2022MB034 and ZR2025QC512).;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/s10118-026-3620-y.The data supporting the findings of this study are available from the corresponding author upon reasonable request.
- DOI：10.1007/s10118-026-3620-y
  中图分类号：
- 收稿：2025-12-24，
  
  录用：2026-02-09，
  
  网络首发：2026-04-30，
  
  纸质出版：2026-07-05
- Accepted：
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Yuan, H. K.; Hou, Q. Q.; Wang, P.; Xu, Y.; Zhang, L.; Li, Y.; Zhang, J.; Wang, L.; Geng, B.; Zong, C. Y. Molecular engineering of fluorine-containing polyurethane adhesives: toughness and self-healing enhancement via synergistic disulfide-Zr⁴⁺ coordination bonds. Chinese J. Polym. Sci. 2026, 44, 2199–2211 DOI: 10.1007/s10118-026-3620-y.

Hao-Kai Yuan, Qian-Qian Hou, Peng Wang, et al. Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds[J]. Chinese Journal of Polymer Science, 2026, 44(7): 2199-2211. DOI: 10.1007/s10118-026-3620-y.
Yuan, H. K.; Hou, Q. Q.; Wang, P.; Xu, Y.; Zhang, L.; Li, Y.; Zhang, J.; Wang, L.; Geng, B.; Zong, C. Y. Molecular engineering of fluorine-containing polyurethane adhesives: toughness and self-healing enhancement via synergistic disulfide-Zr⁴⁺ coordination bonds. Chinese J. Polym. Sci. 2026, 44, 2199–2211 DOI: 10.1007/s10118-026-3620-y. DOI：

Hao-Kai Yuan, Qian-Qian Hou, Peng Wang, et al. Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds[J]. Chinese Journal of Polymer Science, 2026, 44(7): 2199-2211. DOI: 10.1007/s10118-026-3620-y. DOI：

摘要

This work reports a self-healable

high-toughness fluorinated polyurethane adhesive

via

synergistic disulfide and Zr

coordination. Zr

coordination boosts tensile strength by 18-fold and imparts excellent recyclability for sustainable adhesive applications.

Abstract

High-performance adhesives integrating high mechanical toughness

excellent environmental durability

and self-healing capability exhibit broad application potential. Herein

leveraging the excellent stress dissipation capability of multiple dynamic bonds

a self-healing fluorine-containing polyurethane (PU) adhesive with signifi

cantly enhanced toughness was designed by incorporating dynamic aromatic disulfide bonds and metal-coordination interactions. The incorporation of disulfide bonds endows the PU adhesive (named as SN-PU) with efficient low-temperature self-healing performance

while the fluorine-containing side chains confer enhanced resistance to harsh environments. The SN-PU adhesive exhibited a tensile strength of 1.39 MPa

an elongation at break of 1300%

and a self-healing efficiency of 99.3% at 50 °C for 4 h

along with excellent recyclability

via

solvent-assisted casting molding. More importantly

further introduction of interchain Zr

coordination bonds into the SN-PU adhesive (named as Zr-PU) yields a maximum tensile strength of 24.92 MPa

approximately an 18-fold enhancement compared to the SN-PU adhesive. Meanwhile

the lap shear strengths of the SN-PU adhesive on various substrates

including steel plates

aluminum plates

epoxy-based composite plates

and polyamide

were significantly enhanced from 3.45

2.65

3.72

and 1.26 MPa to 5.60

5.66

4.03

and 3.51 MPa

respectively

for the Zr-PU system. This strategy of tailoring molecular chain structures and intermolecular interactions to enhance the strength

toughness

and reusability of adhesives offers a facile approach for the development of high-performance adhesive materials.

关键词

Keywords

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Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr4+ Coordination Bonds

DOI：10.1007/s10118-026-3620-y

摘要

Abstract

关键词

Keywords

references

Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds

Molecular Engineering of Fluorine-containing Polyurethane Adhesives: Toughness and Self-healing Enhancement via Synergistic Disulfide-Zr⁴⁺ Coordination Bonds