Pre-treated waste cooking oil (WCO) and organic montmorillonite (OMMT) were employed for the recycling of aged asphalt, which resulted in the improvement of the design of WCO asphalt rejuvenators and the enhancement of high-temperature performance of WCO-recycled asphalt. The effect of the rejuvenator and the properties of recycled asphalt were evaluated by viscosity, dynamic shear rheometer (DSR), bending beam rheometer (BBR) and scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), and gel permeation chromatography (GPC) tests. The results indicated that aged asphalt could be obviously softened and restored to the level of original asphalt by adding 6% WCO. However, the high-temperature properties of recycled asphalt would be declined by adding too large a dose of WCO rejuvenator. The high-temperature performance of recycled asphalt was significantly improved by the WCO-OMMT complex rejuvenator, and the viscosity and rutting factor of recycled asphalt were increased. Light components of aged asphalt could be supplemented by WCO of the complex rejuvenator. The volatilization of small molecules could be slowed down by the peel structure formed by OMMT and small molecules of the asphalt, which resulted in the proportion of small molecular substances (SMS) being increased by 4% and improvement of the colloidal structure of aged asphalt. The high-temperature and low-temperature performance of recycled asphalt can be improved concurrently by the combination of 6% WCO and 1% OMMT, and this was evidenced by the fact that the high-temperature and low-temperature PG were all upgraded by one level.

Owing to the pronounced compositional heterogeneity of waste cooking oil (WCO), WCO-rejuvenated asphalt often exhibits unstable performance. To improve the compositional controllability of WCO-based rejuvenators, WCO was fractionated according to molecular weight differences into three characteristic fractions: light, medium, and heavy components. Nine rejuvenator formulations with different component ratios were prepared to investigate the synergistic mechanism among WCO fractions with different molecular weights and to propose an optimal blending range. Thermal stability tests, dynamic shear rheometer (DSR) tests, multiple stress creep recovery (MSCR) tests, and bending beam rheometer (BBR) tests were conducted to evaluate the performance of the rejuvenators and rejuvenated asphalts. Gas chromatography (GC) and gel permeation chromatography (GPC) were further used to analyze the chemical composition and molecular-weight distribution. The results show that increasing the proportions of light and medium WCO components improves the low-temperature performance of rejuvenated asphalt; however, when the combined content of light and medium components exceeds 40%, the high-temperature performance is adversely affected. The heavy component improves the rutting factor, creep recovery capacity, and thermal oxidative aging resistance of rejuvenated asphalt, and the coefficient of determination between the long-term aging CAI and heavy-component content reaches 0.959. Thermal stability tests show that the mass loss rate of the nine rejuvenators after 1.5 h of heating ranges from 2.8% to 4.3%, with greater mass loss for formulations containing higher light-component contents. GPC results show that the Mn and Mw of R-4 (492 g/mol and 641 g/mol) are higher than those of R-8 (463 g/mol and 600 g/mol), indicating that a higher macromolecular fraction contributes to improved thermal stability. Considering high-temperature, low-temperature, and aging performance together, rejuvenated asphalt achieves the closest overall performance to the base binder when the heavy component is controlled at 50–60% and the medium component is approximately 30%.