Multiscale study on fatigue healing performance and molecular healing behavior of self-healing SBS modified bitumen

Self-healing polymer modified bitumen based on dynamic chemical bonds is a potential approach to improve the durability of bitumen pavement and save fossil energy. Herein, a novel self-healing SBS modified bitumen on the basis of dynamic disulfide bonds and hydrogen bonds was prepared. Firstly, an aliphatic disulfide (A-ALD) with disulfide bonds and hydrogen bonds was synthesized. Then A-ALD/SBS modified bitumen (A-ALD/SMB) was prepared by blending A-ALD and SBS modified bitumen. The chemical structure and microstructure of A-ALD/SMB were evaluated. In addition, the self-healing performance of A-ALD/SMB at the macroscopic scale and the self-healing behavior at the molecular scale were investigated by a combination of fatigue healing test and molecular dynamics (MD) simulation. The chemical structure analysis showed the formation of disulfide bonds and hydrogen bonds in A-ALD, and A-ALD was successfully attached to the C C bonds in SBS. Fluorescent images revealed that a better network structure appeared in A-ALD/SMB and formed a two-phase continuous morphology. The optimal dosage of A-ALD in SBS modified bitumen was 0.6 %. The fatigue healing test results indicated that A-ALD markedly enhanced the self-healing ability of SBS modified bitumen, and prolonging resting time and raising healing temperature can increase the self-healing performance of A-ALD/SMB. When the damage degree, healing temperature, and resting time were 30 %, 30 °C, and 60 min, respectively, the healing rate of A-ALD/SMB was 98.5 %, which was 30.2 % higher than SMB. The MD simulation results showed that the A-ALD enhanced the molecular diffusion capacity of SBS modified bitumen, and crack healing time of A-ALD/SMB was earlier than that of SMB under the same conditions. When the healing temperature was 40 °C, the time for the A-ALD/SMB and SMB molecular chain segments to start contacting and healing was 27 ps and 49 ps, respectively, which was improved by 44.9 % for A-ALD/SMB compared to SMB. Furthermore, the self-healing behavior of A-ALD/SMB at the molecular scale was consistent with the self-healing performance at the macroscopic scale under different healing temperatures and damage degrees. This study provided a theoretical basis for exploring the self-healing mechanism of SBS modified bitumen.