Volume 23 Issue 2
Apr.  2023
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Article Navigation >  Journal of Traffic and Transportation Engineering  > 2023  >  23(2): 141-152
HU Dong-liang, GU Xing-yu, SUN Li-jun, BO Wu, WU Cheng-bin. Quantum chemistry-based thermal and UV aging mechanism of asphalt[J]. Journal of Traffic and Transportation Engineering, 2023, 23(2): 141-152. doi: 10.19818/j.cnki.1671-1637.2023.02.010
Citation: HU Dong-liang, GU Xing-yu, SUN Li-jun, BO Wu, WU Cheng-bin. Quantum chemistry-based thermal and UV aging mechanism of asphalt[J]. Journal of Traffic and Transportation Engineering, 2023, 23(2): 141-152. doi: 10.19818/j.cnki.1671-1637.2023.02.010
shu

Quantum chemistry-based thermal and UV aging mechanism of asphalt

doi: 10.19818/j.cnki.1671-1637.2023.02.010
  • 1.

    School of Transportation, Southeast University, Nanjing 211189, Jiangsu, China

  • 2.

    School of Highway, Chang'an University, Xi'an 710064, Shaanxi, China

  • 3.

    School of Engineering, Tibet University, Lasa 850000, Tibet, China

  • 4.

    Tibet Tianlu Co., Ltd., Lasa 850000, Tibet, China

Funds:

National Natural Science Foundation of China 52278442

National Natural Science Foundation of China 51878162

Science and Technology Project of Tibet Autonomous Region XZ2019TL-G-01

Special Fund Project for Transportation Development of Jiangsu Province 2020Y19-1

More Information
  • Author Bio:

    HU Dong-liang(1991-), male, doctoral student, dongliangwho@163.com

    GU Xing-yu(1976-), male, professor, PhD, guxingyu1976@163.com

  • Received Date: 2022-11-03
    Available Online: 2023-05-09
  • Publish Date: 2023-04-25
    Abstract
  • In order to reveal the underlying mechanisms of thermal and ultraviolet (UV) aging of asphalt at the atomic level, the aging reaction paths and corresponding potential energy parameters of asphaltenes under various temperature and UV radiation conditions were analyzed based on ab initio molecular dynamics and density functional theory. The change rules of chemical functional groups on the surfaces of virgin, thermal-aged, and UV-aged asphalt specimens were analyzed based on Fourier transform infrared spectroscopy tests, and their aging degrees were compared. Research results indicate that the involved subreactions of asphaltene aging include the cycloalkane aromatization and the formation of oxygen-containing groups triggered by O2 or radicals induced hydrogen abstraction, as well as direct homolytic cleavage on the side chains. The aging mechanism of asphaltenes can be summarized as follows: asphaltenes lose hydrogen atoms constantly and transform into highly reactive and unstable structures under the attack of O2 molecules or radicals, and thus their energy reduces through subsequent reactions such as molecular isomerization or adsorption of oxygen atoms. As a result, the continuous progress of asphaltene aging behavior is triggered. The increase in temperature not only accelerates the rate of aging reactions, but also triggers more types of aging reactions. The aromatization reaction has the lowest energy barrier and thus can occur at lower temperatures, followed by the formation of oxygen-containing groups, and the homolytic cleavage reaction on the side chains has the highest energy barrier and can only occur at higher temperatures. Under UV radiation, the asphaltene molecule transitions to the excited state, and its reaction energy barrier is significantly lower than that under the ground state. Therefore, it can significantly accelerate the aging reaction. Fourier transform infrared spectroscopy tests show that the aging degree of UV aging asphalt specimens is much higher than that of thermal-aged asphalt specimens, which verifies the theoretical calculation results.

     

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