To take swift action towards tackling the global pollution crisis of discarded lithium-ion batteries (LIBs) while reinforcing road structures, this investigation was undertaken. The influence of various proportions of spent graphite (e.g., 5, 10, and 15 wt.% SG), harvested from end-of-life LIBs, on the performance of base AP-5 asphalt cement was studied. Multiple laboratory techniques have been employed to characterize the internal physiochemical interaction between the additive and the binder. These techniques include: elemental analysis (EA), thin-layer chromatography-flame ionization detection (TLC-FID), Fourier transform-infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM), empirical test methods (e.g., penetration, softening point, viscosity, and ductility), dynamic shear rheometer (DSR), and multiple stress-creep recovery (MSCR). Prior to aging, SARA analysis demonstrated that the incremental SG addition into the AP-5 bitumen reduced the contents of saturates, aromatics, and resins, and increased the proportion of asphaltenes. After aging, the saturated and aromatic hydrocarbons kept decreasing; however, the resins increased and the asphaltenes declined. Accordingly, this has brought a progressive shift tendency in the stable–colloidal system for all binders from sol-state towards sol-gel-state. FT-IR scan revealed that the SG has no apparent chemical interaction with the binder, and is endowed solely with filling effects. XRD diagnosis highlighted that the steady SG incorporation into the binder amplified its crystallinity; thereby boosting the thermomechanical properties of mastics. SEM imaging unveiled that the lower-dose of SG exhibited higher compatibility within the bitumen matrix; nevertheless, the intermediate/higher-doses made the binder body relatively rougher. DSR/MSCR/conventional tests indicated that when the asphalt is blended with the graphitic powder under unaged/aged conditions, it becomes stiffer, more viscous, and less cohesive; thereby rendering it more resistant to deformation but not to cracking. In summary, it is promisingly proven that the SG could be successfully used as an asphalt additive and could be beneficial for improving paving performance and mitigating the pollution caused by dead LIBs as well.
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