ABSTRACT The depolymerisation mechanism of various regenerants, when applied to the aged asphalt aggregate structure, was investigated to provide insights for the design and development of regenerants. This study focused on the molecular aggregation of the regenerant-aged asphalt system using molecular dynamics simulation technology. Simulation showcased that the uneven charge distribution in asphaltene molecules and the absence of charge in the central region are prerequisites for the electrostatic attraction of asphaltene molecules, which significantly affects their aggregation, and asphaltene molecules in heavy-aged asphalt are prone to forming stable aggregation structures. Among the four components of aged asphalt, asphaltene molecules exhibited the most significant self-aggregation, followed by saturates, while resin and aromatic molecules showed relatively weaker self-aggregation. Low temperatures encouraged aggregation, whereas high temperatures discouraged it, and ageing elevated the molecular self-aggregation, intensifying with the progression of asphalt ageing. Regenerants improved the depolymerisation of asphaltene aggregates, and fatty acid glycerides presented the most effective depolymerisation, followed by aromatic hydrocarbons and alkanes, while glycerol’s performance was the least effective. To choose regenerant composition materials, those with low electrical potential energy, weak polarity, low polar functional group content or non-polarity should be selected to ensure superior depolymerisation, permeation fusion, and regeneration effects.
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