Stiffening and Toughening of Asphalt Mastic Induced by Bitumen–Mineral Selective Molecular Adsorption and Nanostructural Reconstruction

Asphalt mastic is the most important binder in asphalt mixtures and its rheology is inevitably influenced by the mineral aggregates. Due to the little consideration that has been paid to aggregates’ effects, the rheological properties of mastic films have not been accurately characterized for the present method. Therefore, this study aimed to investigate the rheological characteristics of mastic affected by mineral aggregates and reveal its fundamental mechanism of interfacial interaction. The results suggest that the aggregates increased the stiffness and toughness of mastic within the linear and nonlinear viscoelastic regions. The mastic on limestone had a higher linear viscoelastic modulus than that on basalt below 35 °C, and its ratio reached up to 1.18. However, the modulus of the mastic on basalt surpassed that on limestone by over 50 °C, and the maximum ratio reached 2.17. The mastic in contact with the limestone had a higher failure strain and failure modulus than that in contact with the basalt, the ratios of which reached 1.60 and 1.32, respectively. The macrorheological characteristics are closely related to the nanostructures and intermolecular interactions of bitumen–mineral systems. The coexistence of a stable bitumen nanostructure and an adsorbed layer on the calcite substrate provided a strong bonding energy and high resistance to external shear deformation, leading to the high stiffness and toughness of the limestone. Abundant metal ions from augite and albite diffused into the bitumen layer and destroyed its nanostructure, decreasing the stability of the mastic–basalt interface system. The non-bond energy of bitumen-calcite was 14.15% higher than that of bitumen-albite, and the ratio of shear stress of the bitumen-calcite to the bitumen-albite reached up to 6.8. Therefore, the calcite in limestone reinforced the bitumen, and the augite and albite in basalt destroyed the bitumen colloidal structure. This provides a fundamental understanding of the rheological characterization of mastic on mineral aggregates.