Designing High-Performance Rejuvenators: A Theoretical Approach to Asphaltene Dimer Aggregation and Disaggregation
Publication: Journal of Materials in Civil Engineering
Volume 36, Issue 6
Abstract
The aging process of asphalt materials encompasses varying levels of oxidation reactions within its components. This process increases the polarity of the molecules, prompting aggregation among asphaltenes. Thus, a thorough examination of asphaltene molecule aggregation and disaggregation patterns holds vital implications for the performance restoration of aged asphalt. According to the density functional theory (DFT), the interaction form between oxidized asphaltene dimers was inferred by electrostatic potential (ESP) and confirmed through the charge density difference. This study identified asphaltene dimers optimal configurations via energy minimization principles and determined the factors influencing aggregation based on interaction energy. On the basis of the molecular structure design theory, the basic structures of three different rejuvenators—chain alkanes, aromatic hydrocarbons, and cycloalkanes—were constructed. Functional groups such as hydroxyl, carboxyl, ether, ester, and amide were incorporated to explore the disaggregation patterns of oxidized asphaltene dimers induced by varying rejuvenator structures. Our results revealed that asphaltene molecules form dimers through the stacking interaction of aromatic rings and the electrostatic interaction between positive-negative ESP regions. Dimer disaggregation predominantly follows two rejuvenation mechanisms: T-shaped and parallel. Parallel rejuvenation is the primary mechanism for chain alkanes, aromatic hydrocarbons, cycloalkanes ether, and ester groups. Here, methyl decyl ether exhibited the most potent disaggregation effect, reducing interaction energy between asphaltene dimers by 61.7%. The conclusions could offer a theoretical foundation for understanding asphaltene molecule aggregation and disaggregation and suggest strategies for high-performance rejuvenator design.
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Data Availability Statement
Some or all data, models, or code that support the findings of this study are available from the corresponding author upon reasonable request.
Acknowledgments
The work described in this paper is supported by the Postgraduate Research and Practice Innovation Program of Jiangsu Province (422003297) and the National Natural Science Foundation of China (52278451).
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Journal of Materials in Civil Engineering
Volume 36 • Issue 6 • June 2024
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© 2024 American Society of Civil Engineers.
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Received: Jun 30, 2023
Accepted: Nov 20, 2023
Published online: Mar 26, 2024
Published in print: Jun 1, 2024
Discussion open until: Aug 26, 2024
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