Effect of styrene-butadiene-styrene copolymer on the aging resistance of asphalt: An atomistic understanding from reactive molecular dynamics simulations

doi:10.1007/s11709-021-0761-5

Front. Struct. Civ. Eng.

2021, Vol. 15

Issue (5) : 1261-1276 https://doi.org/10.1007/s11709-021-0761-5

RESEARCH ARTICLE

Effect of styrene-butadiene-styrene copolymer on the aging resistance of asphalt: An atomistic understanding from reactive molecular dynamics simulations

Dongliang Hu^1,², Xingyu Gu^1,³(

), Bingyan Cui⁴

¹. School of Transportation, Southeast University, Nanjing 211189, China
². National Demonstration Center for Experimental Road and Traffic Engineering Education, Southeast University, Nanjing 211189, China
³. College of Engineering, Tibet University, Lhasa 850000, China
⁴. Department of Civil and Environmental Engineering, School of Engineering, Rutgers, The State University of New Jersey, New Brunswick, NJ 08854, USA

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Abstract

To reveal the potential influence of styrene-butadiene-styrene (SBS) polymer modification on the anti-aging performance of asphalt, and its mechanism, we explored the aging characteristics of base asphalt and SBS-modified asphalt by reaction force field (ReaxFF) and classical molecular dynamics simulations. The results illustrate that the SBS asphalt is more susceptible to oxidative aging than the base asphalt under oxygen-deficient conditions due to the presence of unsaturated C=C bonds in the SBS polymer. In the case of sufficient oxygen, the SBS polymer inhibits the oxidation of asphalt by restraining the diffusion of asphalt molecules. Compared with the base asphalt, the SBS asphalt exhibits a higher degree of oxidation at the early stage of pavement service and a lower degree of oxidation in the long run. In addition, SBS polymer degrades into small blocks during aging, thus counteracting the hardening of aged asphalt and partially restoring its low-temperature cracking resistance.

Keywords SBS asphalt oxidative aging asphalt hardening ReaxFF molecular dynamics

Corresponding Author(s): Xingyu Gu

Just Accepted Date: 23 September 2021 Online First Date: 29 October 2021 Issue Date: 29 November 2021

Cite this article:

Dongliang Hu,Xingyu Gu,Bingyan Cui. Effect of styrene-butadiene-styrene copolymer on the aging resistance of asphalt: An atomistic understanding from reactive molecular dynamics simulations[J]. Front. Struct. Civ. Eng., 2021, 15(5): 1261-1276.

URL:

https://academic.hep.com.cn/fsce/EN/10.1007/s11709-021-0761-5
https://academic.hep.com.cn/fsce/EN/Y2021/V15/I5/1261

Fig.1 Representative molecules of asphalt compositions for the simulated SHRP AAA-1 asphalt.

Tab.1 Detailed information for molecule IDs in Fig. 1 and their number in the simulated AAA-1 asphalt

Fig.2 SBS copolymers with different degree of polymerization: (a) SBS_2-12-2 chain; (b) SBS_6-37-6.

Fig.3 Calculated shear viscosity of base asphalt and SBS modified asphalt.

Fig.4 The reaction system of SBS asphalt for the ReaxFF MD simulation (115.04 ? × 115.04 ? × 115.04 ?). The orange atoms are carbon atoms, the red molecules are oxygen molecules, and the green chain is the SBS polymer.

Fig.5 Oxygen content of oxidized asphalt in the ReaxFF MD simulations (equivalent O₂ level = 1). The oxygen content of actual aged asphalt is generally less than 10%.

Fig.6 Diffusivities of asphalt binders: (a) dtermination of diffusivity from the MSD plotting; (b) diffusivities of asphalt binders under different conditions.

Fig.7 Model of SBS modified asphalt for unreactive simulations (39.03 ? × 39.03 ? × 39.03 ?). The atom coloring is the same as in Fig. 4.

Fig.8 Oxidation characteristics with respect to simulation time of SBS modified and unmodified asphalts at different oxygen levels: (a) number of C?O bonds generated during the simulation; (b) number of H?O bonds generated during the simulation; (c) number of S?O bonds generated during the simulation; (d) total number of C/H/S?O bonds; (e) oxygen contents of the simulated oxidized asphalt binders; (f) number of oxygen molecules consumed during the simulation. reaction force field (ReaxFF).

Fig.9 ATR-FTIR spectra of SBS modified and unmodified asphalts before and after aging.

Fig.10 Velocities of atoms in continuous 100 ps in the equilibrated system: (a) in the simulation systems for base asphalt; (b) in the simulation systems for SBS asphalt.

Fig.11 pressures of simulation systems under different oxygen levels.

Fig.12 The concentration of reactant atoms (the total number of atoms in unit volume) of systems under different oxygen levels.

Fig.13 Oxidative aging mechanisms of asphalt and SBS polymer: (a) oxidation mechanism of asphaltene; (b) oxidation and cleavage mechanisms of SBS polymer.

Fig.14 Representative molecules of oxidized compositions for the simulated aged asphalt.

Fig.15 Determination of oxidative aging features of SBS polymer: (a) SBS polymer degrades to smaller blocks during the oxidative aging; (b) representative moleculues of oxidized SBS polymer.

Tab.2 Thermodynamic parameters of virgin and aged asphalts from simulations and experimental measurements

Fig.16 Thermodynamic parameters related to asphalt: (a) shear viscosity; (b) bulk modulus; (c) cohesion energy density and solubility parameter.

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