Insight into the salt damage mechanism to the asphalt-aggregate interface in recycled asphalt mixtures at different salt environments using molecular dynamics and DFT simulations

Abstract

In coastal areas, the complex salt environment poses new challenges to the interfacial stability and service durability of hot recycled asphalt pavements. To investigate the influence mechanism of salt environment on the adhesion properties of asphalt-aggregate interface, this study employed molecular dynamics (MD) simulation and density functional theory (DFT) to analyze the interfacial interaction energy, molecular diffusion behavior, component distribution, and molecular electrostatic property at asphalt-aggregate interface. The results show that as the content of aged asphalt increased, the interaction between asphalt and anions (Cl⁻ and SO₄²⁻) is weaker than that with cations (Na⁺, Mg²⁺ and Ca²⁺). H₂O causes the aromatics, saturates and resins to move away from the interface. Cl⁻ causes the saturates to further move away from the interface, while Na⁺ and Mg²⁺ bring the aromatics closer to the interface. Due to the greater polarity of SO₄²⁻, it moves the resins closer to the interface. With increasing aged asphalt content, the number of hydrogen bonds between asphalt and SiO₂ increases from none to some, thus enhancing the interfacial adhesion. However, this adhesion becomes more susceptible to salts. The aging effect redistributes the charge of asphalt molecules, concentrating negative potentials on the carbonyl and sulfoxide functional groups located on the outside of molecules. This increases the polarity of the asphalt molecules, making them more susceptible to salt ion attack. These findings contribute to the understanding of the adhesion properties of recycled asphalt mixtures in extreme salt environments.