A developed SBS vitrimer for asphalt modification: Synergistic self-healing and aging resistance via dynamic covalent crosslinking
Source abstract
Abstract
This study develops a styrene-butadiene-styrene (SBS) vitrimer via disulfide bond-mediated dynamic covalent crosslinking to address the inherent aging susceptibility and non-healing properties of conventional SBS in asphalt modification. Epoxidized SBS (eSBS) was synthesized and crosslinked with 4,4′-dithiodibutyric acid (DTBA) to construct covalent adaptable networks. Fourier-transform infrared spectroscopy (FTIR) confirmed successful vitrimer formation through ester bond formation (1734 cm −1 peak). Optical microscopy revealed rapid self-healing behavior in the optimized SBS vitrimer (SV3, 0.3 ‰ DTBA of the butadiene structural units in SBS), with surface notches fully closing within 50 min at 90 °C, whereas unmodified SBS exhibited no healing under identical conditions. Thermogravimetric analysis demonstrated comparable thermal stability between SV3 and pristine SBS, with maximum degradation temperatures (T max ) near 463 °C. Mechanically, SV3 achieved a 25 % increase in tensile strength while retaining 63 % elongation relative to SBS, along with 100 % creep recovery at 80–100 °C, contrasting with irreversible deformation in unmodified SBS. Aging resistance was evaluated via Rolling Thin Film Oven (RTFO) and Pressure Aging Vessel (PAV) tests. The SV3-modified binder (SV3mB) outperformed conventional SBS-modified binder (SBSmB), showing 54–58 % higher elastic recovery ( R -value) and 19–20 % lower non-recoverable creep compliance ( J nr ) post-RTFO aging. After PAV aging, SV3mB exhibited 46–105 % higher R -values and 62–70 % lower J nr values. A healing index ( H ), derived from viscoelastic continuum damage (VECD) theory, quantified self-healing efficiency, revealing SV3mB’s superior damage mitigation under high strain (25 %–30 %) and extended fatigue life ( N f ) due to dynamic bond exchange. These results demonstrate that SBS vitrimers enhance asphalt binder durability, aging resistance, and autonomous repair capabilities, offering transformative potential for pavement materials in extreme environmental conditions.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Asphalt Pavement Performance Evaluation · Polymer composites and self-healing · Polymer Nanocomposites and Properties
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (60)
Show source-provided references
1. Preparation and properties of self-healing SBS modified bitumen with dynamic acylhydrazone bonds10.1016/j.eurpolymj.2024.112932 ↗
2. Investigation of influence factors on low temperature properties of SBS modified asphalt10.1016/j.conbuildmat.2017.06.118 ↗
3. Effect of acylhydrazone self-healing agents with different structures on the properties of SBS modified asphalt waterproofing membrane10.1016/j.conbuildmat.2024.136238 ↗
4. Optimizing rural pavements with SBS-modified asphalt binders and petroleum resin10.3390/buildings14010116 ↗
5. Review of the state-of-the-art techniques for enhancing the toughness of thermosetting epoxy asphalt10.1016/j.conbuildmat.2024.137660 ↗
6. The modification mechanism, evaluation method, and construction technology of direct-to-plant SBS modifiers in asphalt mixture: a review10.3390/polym15132768 ↗
7. Influence of residual SB di-block in SBS on the thermo–oxidative aging behaviors of SBS and SBS modified asphalt10.1617/s11527-022-01882-3 ↗
8. Aging mechanism and rejuvenating possibility of SBS copolymers in asphalt binders10.3390/polym12010092 ↗
9. Multiscale study on fatigue healing performance and molecular healing behavior of self-healing SBS modified bitumen10.1016/j.molliq.2024.125976 ↗
10. Long-term mechanical deterioration trends and mechanisms of SBS-modified asphalt mixtures10.3390/coatings14111363 ↗
11. Efficacy of cellulose fiber as bacteria carrier for self-healing concrete and 3d polymer microstructure
12. Preparation and characterization of vanillin-based self-healing polyurethane-modified asphalts based on acylhydrazone chemistry10.1016/j.eurpolymj.2024.113010 ↗
13. Dynamic chemistry based self-healing of asphalt modified by diselenide-crosslinked polyurethane elastomer10.1016/j.conbuildmat.2021.123480 ↗
14. Preparation and performance of self-healing SBS modified bitumen based on dynamic disulfide bonds10.1016/j.conbuildmat.2023.132394 ↗
15. Investigation of microstructure, rheological property and self-healing performance of SBS modified bitumen with dynamic disulfide bonds prepared by one-step method10.1016/j.conbuildmat.2024.135158 ↗
16. Elastic vitrimers: Beyond thermoplastic and thermoset elastomers10.1016/j.matt.2022.04.007 ↗
17. Vitrimers: directing chemical reactivity to control material properties10.1039/D0SC01069C ↗
18. Vitrimers: associative dynamic covalent adaptive networks in thermoset polymers10.1016/j.cej.2019.123820 ↗
19. Revolutionizing elastomer technology: advances in reversible crosslinking, reprocessing, and self-healing applications
20. Shape-memory and self-healing polymers based on dynamic covalent bonds and dynamic noncovalent interactions: synthesis, mechanism, and application10.1021/acsabm.1c00606 ↗
21. Castor oil-based polyurethane Vitrimer modified asphalts regulated by dual dynamic reversible reactions and crosslinking density: preparation, basic assessment and self-healing behavior
22. Preparation and properties of lignin-based vitrimer system containing dynamic covalent bonds for reusable and recyclable epoxy asphalt10.1016/j.indcrop.2023.116498 ↗
23. Preparation and characterization of polyurethane-modified asphalt containing dynamic covalent bonds10.1016/j.conbuildmat.2023.133303 ↗
24. Green synthesis of polyurethane with reversible oxime-urethane bond to enhance the self-healing properties of asphalt binder at room temperature10.1016/j.conbuildmat.2023.134766 ↗
25. Preparation and characterization of a novel self-healing polyurethane-modified asphalt based on dynamic disulfide bond10.1061/JMCEE7.MTENG-16893 ↗
26. Research on self-healing behavior of asphalt modified by polyurea elastomer containing dynamic disulfide/diselenide bond10.1016/j.eurpolymj.2023.111990 ↗
27. Dual dynamic bonds approach for polyurethane recycling and self-healing of emulsified asphalt10.1016/j.scitotenv.2023.163915 ↗
28. Advancing carbon nanomaterials-engineered self-sensing cement composites for structural health monitoring: a state-of-the-art review
29. Fire-retarding asphalt pavement for urban road tunnels: a state-of-the-art review and beyond
30. Endeavour to balance mechanical properties and self-healing of nature rubber by increasing covalent crosslinks via a controlled vulcanization10.1016/j.eurpolymj.2021.110823 ↗
31. Understanding the effects of cross-linking density on the self-healing performance of epoxidized natural rubber and natural rubber10.1021/acsomega.2c00971 ↗
32. Fast self-healing at room temperature in Diels–Alder elastomers10.3390/polym15173527 ↗
33. Polymers with dynamic bonds: adaptive functional materials for a sustainable future10.1021/acs.jpcb.1c03511 ↗
34. Dynamic bonds: adaptable timescales for responsive materials10.1002/ange.202206938 ↗
35. Recent advances in self-healing polymer-modified asphalt utilizing dynamic covalent bonds10.1007/s10965-024-04244-5 ↗
36. Characterization of fatigue damage in high-modulus asphalt mixtures at different aging degrees10.1016/j.conbuildmat.2025.140961 ↗
37. Simulation of the time needed for long-term asphalt ageing in the rolling thin film oven relative to that of the pressure ageing vessel10.3390/ma16227081 ↗
38. Long-term effectiveness of waste soybean oil (WSO) to rejuvenate aged asphalt binder
39. Approach for accurately characterizing nonlinear viscoelastic and nonrecoverable properties of asphalt binders based on MSCR test10.1016/j.conbuildmat.2023.133098 ↗
40. Laboratory evaluation of the relationship of asphalt binder and asphalt mastic via a modified MSCR test10.3390/coatings13020304 ↗
41. Linking asphalt binder fatigue to asphalt mixture fatigue performance using viscoelastic continuum damage modeling10.1007/s11043-016-9304-1 ↗
42. Application of the Viscoelastic continuum damage theory to study the fatigue performance of asphalt mixtures—a literature review10.3390/su14094973 ↗
43. Correspondence principles and a generalized J integral for large deformation and fracture analysis of viscoelastic media10.1007/BF01140837 ↗
44. Fatigue performance analysis of fine aggregate matrix using a newly designed experimental strategy and viscoelastic continuum damage theory10.1617/s11527-024-02338-6 ↗
45. A proposed approach for accurate fatigue quantification of the base asphalt binders coupling nonlinear viscoelastic effects in S-VECD theoretical framework10.1016/j.conbuildmat.2023.131850 ↗
46. Estimating asphalt binder fatigue at multiple temperatures using a simplified pseudo-strain energy analysis approach in the LAS test10.1016/j.conbuildmat.2020.120911 ↗
47. Viscoelastic continuum damage (VECD) models for cracking problems in asphalt mixtures10.1080/10298436.2017.1279492 ↗
48. Rapid determination of styrene-butadiene-styrene (SBS) content in modified asphalt based on Fourier transform infrared (FTIR) spectrometer and linear regression analysis10.1016/j.measurement.2019.107204 ↗
49. Dual dynamic network system constructed by waterborne polyurethane for improved and recoverable performances10.1016/j.cej.2022.136204 ↗
50. Bio-based vitrimer-like polyurethane based on dynamic imine bond with high-strength, reprocessability, rapid-degradability and antibacterial ability10.1016/j.polymer.2021.124208 ↗
51. Dynamic polymeric materials via hydrogen-bond Cross-linking: effect of multiple network topologies10.1016/j.progpolymsci.2024.101890 ↗
52. Fast upcycling of poly (ethylene terephthalate) into catalyst-free vitrimers10.1021/acssuschemeng.2c06829 ↗
53. Upgrade SBS into vitrimers with excellent mechanical and physical properties10.1016/j.eurpolymj.2022.111600 ↗
54. Dynamic and reconfigurable materials from reversible network interactions10.1038/s41578-021-00412-x ↗
55. Effect of sterics and degree of cross-linking on the mechanical properties of dynamic poly (alkylurea–urethane) networks10.1021/acs.macromol.7b01016 ↗
56. Dynamic covalent polymer networks: a molecular platform for designing functions beyond chemical recycling and self-healing10.1021/acs.chemrev.0c00938 ↗
57. Y. Wang, X. Yan, T. Ai, C. Wang, K. Li, K. Fang, Curing Behavior Analysis and Performance Characterization of Recyclable Epoxy Vitrimer Asphalt with Dual Dynamic Covalent Crosslinking Network, Available at SSRN 4796964.
58. Challenges and opportunities of self-healing polymers and devices for extreme and hostile environments10.1002/adma.202008052 ↗
59. Evaluation on the fatigue and self-healing properties of aged and rejuvenated SBS-modified asphalt10.1016/j.conbuildmat.2023.134773 ↗
60. Enhancing accuracy of predictive fatigue life model in rejuvenated RAP binders through LAS test and complex modulus test at multiple temperatures10.1016/j.jclepro.2024.141654 ↗