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Peer-reviewedCC BY 4.0Polymers

Self-Healing Behavior of Medium-Temperature Thermoresponsive Polyurethane-Modified Asphalt: Multiscale Structure–Property Relationships

  • Kenan Li1,2
  • Dengke Yang1
  • Lang Liu2
  • Mengbo Zhu2
  • Zhizhen Liu2
  • Tao Ai3
  1. 1School of Civil and Architectural Engineering, Xi’an University of Science and Technology, Xi ‘an 710054, China
  2. 2College of Energy and Mining Engineering, Xi’an University of Science and Technology, Xi ‘an 710054, China
  3. 3School of Materials Science and Engineering, Chang ‘an University, Xi ‘an 710064, China
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Abstract

Asphalt surface layers are prone to deterioration under long-term vehicle loads and environmental factors, making active healing binders essential for pavement durability. This study designed a polyurethane-modified asphalt (PUA) with dynamic disulfide bonds that can be thermally activated at medium temperatures (40–60 °C). Rheological tests, adhesion tests, and molecular simulations revealed the relationship between chemical composition, molecular structure, and healing performance from molecular to macroscopic scales. Results showed that asphalt cohesion and asphalt–aggregate bond strength were key intrinsic factors. Compared with the disulfide-free PUA, the DSDDP-containing formulations exhibited higher fatigue-healing indices and modest improvements in adhesion-healing indices under the tested conditions. For PUA with a DSDDP molar fraction of 10% in composite chain extender, the fitted healing curve predicted that the complex-modulus-based healing index (HI1) would reach 0.9 after approximately 680 s at 50 °C. At construction temperatures (>135 °C), dynamic exchange reduced network density and improved workability. Molecular dynamics simulations demonstrated that diffusion and movement accelerated with increasing initial spacing and rising temperature. S-S bonds reduced intermolecular forces via topological rearrangement, accelerating migration toward cracks and forming a denser structure after healing. This thermoresponsive PUA mitigates crack formation and expansion, enabling sustainable pavement applications.

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Cite

BibTeXRIS
BibTeX
@article{li2026selfhealing,
  title = {{Self-Healing Behavior of Medium-Temperature Thermoresponsive Polyurethane-Modified Asphalt: Multiscale Structure–Property Relationships}},
  author = {Kenan Li and Dengke Yang and Lang Liu and Mengbo Zhu and Zhizhen Liu and Tao Ai},
  journal = {Polymers},
  year = {2026},
  month = nov,
  doi = {10.3390/polym18212711},
  url = {https://www.mdpi.com/2073-4360/18/21/2711},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Self-Healing Behavior of Medium-Temperature Thermoresponsive Polyurethane-Modified Asphalt: Multiscale Structure–Property Relationships
AU  - Kenan Li
AU  - Dengke Yang
AU  - Lang Liu
AU  - Mengbo Zhu
AU  - Zhizhen Liu
AU  - Tao Ai
PY  - 2026
DA  - 2026/11/01
JO  - Polymers
DO  - 10.3390/polym18212711
UR  - https://www.mdpi.com/2073-4360/18/21/2711
AB  - Asphalt surface layers are prone to deterioration under long-term vehicle loads and environmental factors, making active healing binders essential for pavement durability. This study designed a polyurethane-modified asphalt (PUA) with dynamic disulfide bonds that can be thermally activated at medium temperatures (40–60 °C). Rheological tests, adhesion tests, and molecular simulations revealed the relationship between chemical composition, molecular structure, and healing performance from molecular to macroscopic scales. Results showed that asphalt cohesion and asphalt–aggregate bond strength were key intrinsic factors. Compared with the disulfide-free PUA, the DSDDP-containing formulations exhibited higher fatigue-healing indices and modest improvements in adhesion-healing indices under the tested conditions. For PUA with a DSDDP molar fraction of 10% in composite chain extender, the fitted healing curve predicted that the complex-modulus-based healing index (HI1) would reach 0.9 after approximately 680 s at 50 °C. At construction temperatures (>135 °C), dynamic exchange reduced network density and improved workability. Molecular dynamics simulations demonstrated that diffusion and movement accelerated with increasing initial spacing and rising temperature. S-S bonds reduced intermolecular forces via topological rearrangement, accelerating migration toward cracks and forming a denser structure after healing. This thermoresponsive PUA mitigates crack formation and expansion, enabling sustainable pavement applications.
SN  - 2073-4360
ER  -