To elucidate the impact mechanism of the interfacial characteristics of Calcium Silicate Hydrate gel (CSH)–Montmorillonite (MMT) at the nanoscale on the strength of cement-stabilized montmorillonite soil, this paper begins by examining the interfacial energy. Through Molecular Dynamics (MD) simulation methods, the energy at the MMT and CSH binding interface is quantitatively calculated, and the correlation between the interfacial energy and macroscopic strength is determined in conjunction with grey relational analysis. Finally, based on the characterization results from X-ray diffraction (XRD), the accuracy and sources of deviation in the MD simulation results are discussed. The study shows the CSH-MMT interfacial energy is composed of van der Waals forces, hydrogen bond energy, and electrostatic interactions, which are influenced by the migration of cations; there is a good consistency between the CSH-MMT interfacial energy and the unconfined compressive strength (UCS) of cement-stabilized soil (cemented soil), with the interfacial energy decreasing as the number of water molecules increases and first decreasing then increasing as the number of MMT layers grows; by adjusting the mix proportions, the magnitude of the CSH-MMT interfacial energy can be altered, thereby optimizing the strength of the cemented soil.

This study developed three composite slurries for coating recycled aggregate by incorporating polyacrylate emulsion, fly ash, and gypsum into a cement-based mixture. The filling and pozzolanic effects of fly ash help to improve microcracks in the recycled aggregates. The polyacrylate emulsion forms a strong bonding layer between the cement matrix and the aggregates, enhancing the interfacial bond strength. Based on relevant studies, the following mix designs were developed: Slurry 1 consists of pure cement paste; Slurry 2 contains 15% fly ash and 3% gypsum added to the cement paste; Slurry 3 adds 22% polyacrylate emulsion to the slurry. The study first compared the effects of the three composite slurries on the crushing value and water absorption of recycled aggregates, and then analyzed their impact on the mechanical properties, permeability, and drying shrinkage of concrete. Finally, the mechanisms behind the enhancement were investigated using the Vickers Hardness Test (HV), Mercury Intrusion Porosimetry (MIP), and scanning electron microscopy–energy-dispersive spectroscopy (SEM-EDS). The results showed that the polyacrylate emulsion composite slurry had the most significant improvement effect. For recycled aggregate AL, the crushing value decreased from 28.8% to 22.5% and the saturated surface–dry water absorption decreased from 15.1% to 13.8% after cement slurry modification. After coating with the composite slurry, the crushing value further dropped to 18.2% and the water absorption to 9.5%. Two aspects of the performance of recycled aggregates are enhanced with the polymer composite slurry: first, fly ash provides nucleation sites for CH, reducing the tendency for directional CH alignment. Second, the long chains of PAE (polyacrylic ester) encapsulate cementitious particles, effectively filling surface defects on the recycled aggregates, improving the bonding strength at the new-to-old interface, and significantly enhancing the performance of both recycled aggregates and recycled concrete.