To enhance the adhesion between tuff and asphalt, this study investigates the efficacy of alkalinization treatment technology using a molecular self-assembly layer derived from the silane-coupling agent γ-aminopropyltriethoxysilane (APTES). APTES hydrolysis solutions at varying concentrations were prepared to assess their impact on the adhesive strength of the aggregate–asphalt interface and water damage resistance. Using surface energy theory, the interface adhesion work of tuff was analyzed, while SEM and EDS were employed to examine changes in surface morphology and composition after treatment. The results demonstrate that an APTES:water:ethanol mass ratio of 5:45:50, along with a curing temperature of 200 °C, significantly improves the bonding strength between tuff and asphalt. The silanol groups on APTES react with hydroxyl groups on the tuff surface to form siloxane bonds (Si-O-Si), anchoring APTES to the tuff. This study elucidates the self-assembly mechanisms of APTES on tuff aggregates and demonstrates the consequent enhancement of interfacial adhesion, providing valuable insights for the application of tuff as tunnel spoil in road engineering.
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