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<p>This study employed a multi-scale approach to investigate the impact of aging on the physicochemical composition and interfacial adhesion behavior within asphalt-aggregate systems. Combining laboratory experiments with molecular dynamics (MD) simulations, it systematically characterized the evolution of virgin asphalt, short-term and long-term aged asphalt. The experimental techniques included saturate, aromatic, resin, and asphaltene (SARA) fractionation, gel permeation chromatography (GPC), elemental analysis, and atomic force microscopy (AFM). The results show oxidative aging promotes asphalt hardening through increased oxygen content and growth in large molecular-size fractions. Aggregates (albite, calcite) exhibit enhanced interfacial adhesion owing to intensified electrostatic interactions, with the adhesion work sequence being albite &gt; calcite &gt; quartz. These alkaline aggregates impose a greater inhibition effect on molecular diffusion. While short-term aging increased adhesion work (69.89% increase with albite) through enhanced molecular polarity and pull-off tensile strength (POTS) by 2.44–3.81%. Long-term aging caused POTS reductions of 3.74–8.55%, the further increase in simulated adhesion work unravels the underlying discrepancy between the molecular-scale adhesion energy and macroscopic mechanical behavior. Z-axis concentration profiles confirmed aging-induced accumulation of polar molecules towards aggregate surfaces, with higher aggregation density on albite than quartz, providing a molecular-scale explanation for reinforced interfaces from a mobility perspective. This study bridges molecular-scale mechanisms with macroscopic performance, providing insights for optimizing asphalt-aggregate interfaces in pavement durability.</p>

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Multi-scale characterization of aging-induced evolution in physicochemical properties and adhesion behavior at asphalt-aggregate interfaces

  • 期刊论文

  • 发表日期：

    2026年1月8日

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  • Guoqing Sun,
  • Peixin Shi,
  • Jiupeng Zhang,
  • Qiang Tang,
  • Yucheng Huang,
  • Yan Li

摘要

This study employed a multi-scale approach to investigate the impact of aging on the physicochemical composition and interfacial adhesion behavior within asphalt-aggregate systems. Combining laboratory experiments with molecular dynamics (MD) simulations, it systematically characterized the evolution of virgin asphalt, short-term and long-term aged asphalt. The experimental techniques included saturate, aromatic, resin, and asphaltene (SARA) fractionation, gel permeation chromatography (GPC), elemental analysis, and atomic force microscopy (AFM). The results show oxidative aging promotes asphalt hardening through increased oxygen content and growth in large molecular-size fractions. Aggregates (albite, calcite) exhibit enhanced interfacial adhesion owing to intensified electrostatic interactions, with the adhesion work sequence being albite > calcite > quartz. These alkaline aggregates impose a greater inhibition effect on molecular diffusion. While short-term aging increased adhesion work (69.89% increase with albite) through enhanced molecular polarity and pull-off tensile strength (POTS) by 2.44–3.81%. Long-term aging caused POTS reductions of 3.74–8.55%, the further increase in simulated adhesion work unravels the underlying discrepancy between the molecular-scale adhesion energy and macroscopic mechanical behavior. Z-axis concentration profiles confirmed aging-induced accumulation of polar molecules towards aggregate surfaces, with higher aggregation density on albite than quartz, providing a molecular-scale explanation for reinforced interfaces from a mobility perspective. This study bridges molecular-scale mechanisms with macroscopic performance, providing insights for optimizing asphalt-aggregate interfaces in pavement durability.