Due to the concerns of sustainability, environment, and economy that are associated with non-renewable petroleum-based additives, there has been a growing interest in bio-additives derived from renewable feedstocks. This study aims to reveal the modification mechanism of three bio-additives derived from rapeseed on the base asphalt. The exploration of modification mechanism helped to explain the distinct rheological properties of bio-modified asphalt binders presented in a previous study. The effect of three bio-additives on the surface morphology, micro-mechanical properties, adhesivity, and chemical structure of base asphalt binders were investigated via Atomic Force Microscopy (AFM) and Fourier Transform Infrared spectrometer (FTIR) tests. The Electrostatic potential distribution and the orbital energy was analyzed via density functional theory (DFT) calculation to explore the inherit polarity of both the three bio-additives and asphalt components. Furthermore, molecular dynamic (MD) methods were used to evaluate the compatibility mechanism and aggregation tendency of asphalt components and bio-additives. The results showed that the electrostatic potential and the orbital energy of three bio-additives predominantly centered around the polar group. Specifically, AERO exhibited highest electrostatic potential distribution and lowest energy gap, indicating its heightened polarity. Moreover, the solution parameter difference value of bio-modified asphalt fell within 0.2 (J/m3)0.5, indicating great compatibility between asphalt and bio-additives, especially for ERO. Additionally, three bio-additives mitigated the aggregation of asphaltene within the asphalt due to their electrostatic interaction, especially notable in the cases of ERO and AERO. Furthermore, a cross-link network was formed within AERO-modified asphalt binders owing to its heightened polarity, fostering hydrogen bonding interactions internally and promoting the aggregation of saturate and resin factions around it. Consequently, this led to enhanced modulus and elasticity in the AERO-modified asphalt binders. Rapeseed derivatives as asphalt additives would be a sustainable and durable material for pavement construction and maintenance. It provides a theoretical basis for advancing the practical application of renewable vegetable oils in road engineering, which has exceptional economic and social benefits.
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