UV radiation can change the internal molecular composition, macroscopic rheological properties, and microscopic chemical composition of asphalt. To study the effect of ultraviolet aging on asphalt and its structure–activity relationship, its rheological properties were measured by dynamic shear rheology and multiple stress recovery creep tests, its chemical compositions were measured by component composition, elemental composition, and infrared spectrum tests, and its molecular weight, distribution, and molecular structure were determined by gel permeation chromatography and nuclear magnetic resonance tests. Then, the molecular weight and molecular structure, rheological properties, and microchemical aging behavior of asphalt after UV aging were characterized by correlation analysis, and the structure–activity relationship was analyzed. The results show that the deformation resistance and elastic recovery ability of asphalt after UV aging are enhanced, and the flow performance is decreased. The ultraviolet radiation caused the aromatic hydrocarbons containing naphthenes and long alkyl chains in the asphalt to break and connect with asphaltenes with a ring structure. The asphaltene content in each bitumen sample exceeded 46%, and that in KL reached 55%, indicating that the bitumen changed into a gel structure. UV aging causes the aggregation of asphalt molecules, and the aggregation of molecules narrows the molecular distribution boundary and moves in the direction of macromolecules, resulting in the reduction of the dispersion coefficient by 2–10%. Hydrogen atoms will undergo condensation and substitution reactions due to long-chain breaking, cyclization, or aromatization under UV action, and the breaking of C=C bonds in carbon atoms will increase the stable aromatic ring, strengthen the stiffness of the molecular backbone, and make it difficult for the backbone to spin. Through correlation analysis, it was found that the molecular composition index could characterize the aging behavior index of asphalt, and that the aromatic structure was the most critical molecular change. Further, it was found that the sulfoxide group and carbonyl group could be used as evaluation criteria for the UV aging of asphalt because the correlation between them was above 0.7. This study provides an essential index reference for evaluating the performance change of asphalt under ultraviolet aging to save testing time. Moreover, the molecular structure characterization revealed the changes in internal molecular composition that were behind the observed aging properties, providing a theoretical basis for research on asphalt anti-aging technology. [ABSTRACT FROM AUTHOR]

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