<p>This work presents a multi-scale investigation into the thermal aging mechanism of styrene–butadiene–styrene (SBS) modified bitumen. By employing extended Rolling Thin Film Oven Test (RTFOT) aging and integrating techniques including gel permeation chromatography, Fourier transform infrared spectroscopy, dynamic shear rheometry, and fluorescence microscopy, a critical transition in the SBS degradation mechanism was identified at approximately 160 min of thermal aging. Before this threshold, SBS undergoes cross-linking between polymer chains, while beyond it, dominant chain scission prevails, as conclusively evidenced by the reversal in the polydispersity index trend and a marked decrease in the Z-average molecular weight. Chemo-mechanical correlations were established, decoupling the competing effects of bitumen matrix oxidation and SBS degradation: penetration loss was correlated with carbonyl formation (increase in <i>I</i><sub>C=O</sub>) and the consumption of polybutadiene bonds (decrease in <i>I</i><sub>–CH=CH–</sub>), while ductility failure was primarily correlated with sulfoxide growth (increase in <i>I</i><sub>S=O</sub>) and large molecular structuring (increase in large molecular size (LMS)). Rheologically, the increase in overall stiffness (rise in modulus coefficient “<i>a</i>”) was mainly correlated with SBS chain scission (decrease in <i>I</i><sub>–CH=CH–</sub>) and bitumen oxidation (increase in <i>I</i><sub>C=O</sub>), whereas the shift in viscoelastic balance (decrease in viscoelastic index “<i>n</i>”) was more sensitive to the oxidized bitumen matrix (LMS, <i>I</i><sub>S=O</sub>). Overall, this work provides valuable guidance not only for optimizing construction control to prevent excessive SBS degradation, but also for designing advanced modifiers and rejuvenators that target the critical thermal aging transition.</p>

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Multi-scale characterization of styrene–butadiene–styrene modified bitumen during thermal aging

  • Shizhan Xu,
  • Zhigang Zhao,
  • Yating Zhao,
  • Chenguang Wan,
  • Xiaofeng Wang

摘要

This work presents a multi-scale investigation into the thermal aging mechanism of styrene–butadiene–styrene (SBS) modified bitumen. By employing extended Rolling Thin Film Oven Test (RTFOT) aging and integrating techniques including gel permeation chromatography, Fourier transform infrared spectroscopy, dynamic shear rheometry, and fluorescence microscopy, a critical transition in the SBS degradation mechanism was identified at approximately 160 min of thermal aging. Before this threshold, SBS undergoes cross-linking between polymer chains, while beyond it, dominant chain scission prevails, as conclusively evidenced by the reversal in the polydispersity index trend and a marked decrease in the Z-average molecular weight. Chemo-mechanical correlations were established, decoupling the competing effects of bitumen matrix oxidation and SBS degradation: penetration loss was correlated with carbonyl formation (increase in IC=O) and the consumption of polybutadiene bonds (decrease in I–CH=CH–), while ductility failure was primarily correlated with sulfoxide growth (increase in IS=O) and large molecular structuring (increase in large molecular size (LMS)). Rheologically, the increase in overall stiffness (rise in modulus coefficient “a”) was mainly correlated with SBS chain scission (decrease in I–CH=CH–) and bitumen oxidation (increase in IC=O), whereas the shift in viscoelastic balance (decrease in viscoelastic index “n”) was more sensitive to the oxidized bitumen matrix (LMS, IS=O). Overall, this work provides valuable guidance not only for optimizing construction control to prevent excessive SBS degradation, but also for designing advanced modifiers and rejuvenators that target the critical thermal aging transition.