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Impact of Aging on the Microstructure of Asphalt Binder Modified with Antioxidant Additives and Copolymers

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Abstract

The effect of long-term aging on asphalt binders mixed with antioxidant additives and copolymers demonstrated potential for retarding oxidative aging at the nanoscale based on atomic force microscopy (AFM) characterization. Two antioxidants (Redicote and Solprene) were effective in retarding the aging of asphalt binders (PG 64-22 and PG 76-22) from a previous study. This new complementary study further evaluates the change in micromechanical properties and microstructural phases of antioxidant-modified binders subjected to aging in the pressure aging vessel (PAV) to simulate the harsh aging conditions. The results were compared to those of asphalt binders extracted from field cores of two test sections in Qatar. Microstructural analysis based on the change in the percent area of the different phases from adhesion maps indicated that long-term aging caused a significant quantitative change in various surface phases of test binders. The dispersive phase area (measured from adhesion maps) increased due to aging with an associated increase in the number of so-called bee structures. This was accompanied by an increase in micromechanical adhesion and stiffness of the asphalt surface zone. An increased number of bee structures surrounded by higher stiffness regions acted as nuclei for crack initiation, eventually leading to fatigue cracking under repetitive loading. Aging also increased the surface roughness parameters of the asphalt binders and caused an overall sharpness on the asphalt surface. However, both antioxidants and copolymers retarded the increase in relative stiffness in laboratory-aged binders compared to field-aged binders.

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The authors confirm that the derived data supporting the findings of this study are available within the article. Raw data supporting the findings of this study are available from the corresponding author upon reasonable request.

References

  1. Davies, R.M., Sorenson, J. (2000). Pavement preservation: Preserving our investment in highways. Public Roads (FHWA), 63 (4). (Source: https://highways.dot.gov/public-roads/januaryfebruary-2000/pavement-preservation-preserving-our-investment-highways).

  2. Asphalt Pavement: Your Path to the National Mall, National Asphalt Pavement Association. (Source: https://www.asphaltpavement.org/news-resources/for-press/asphalt-pavement-your-path-to-the-national-mall).

  3. Petersen, J. C. (1986). Quantitative functional group analysis of asphalts using differential infrared spectrometry and selective chemical reactions--theory and application. Transportation Research Record, (1096). (Source: https://trid.trb.org/view/284300).

  4. Glover, C. J., Martin, E., Chowdhury, A., Han, R., Prapaitrakul, N., Jin, X., Lawrence, J. (2009). Evaluation of binder aging and its influence in aging of hot mix asphalt concrete: Literature review and experimental design, Research Report No. FHWA/TX-08/0-6009-1, Texas Transportation Institute, College Station, Texas.(Source: https://static.tti.tamu.edu/tti.tamu.edu/documents/0-6009-2.pdf).

  5. Apeagyei, A. K. (2011). Laboratory evaluation of antioxidants for asphalt binders. Construction and Building Materials, 25, 47–53.

    Article  Google Scholar 

  6. Masson, J. F., Collins, P., & Polomark, G. (2005). Steric hardening and the ordering of asphaltenes in bitumen. Energy and Fuels, 19, 120–122.

    Article  Google Scholar 

  7. Swiertz, D. (2010). Asphalt Aging Characteristics, Rheological Implications and Laboratory Techniques. University of Wisconsin, Madison, WI, USA.

  8. Ouyang, C., Wang, S., Zhang, Y., & Zhang, Y. (2006). Improving the aging resistance of styrene-butadiene-styrene tri-block copolymer modified asphalt by addition of antioxidants. Polymer Degradation and Stability, 91, 795–804.

    Article  Google Scholar 

  9. Cortizo, M. S., Larsen, D. O., Bianchetto, H., & Alessandrini, J. L. (2004). Effect of the thermal degradation of SBS copolymers during the ageing of modified asphalts. Polymer Degradation and Stability, 86, 275–282.

    Article  Google Scholar 

  10. E. Kassem, M. S. Khan, S. Katukuri, O. Sirin, A. Muftah & F. Bayomy (2019). Retarding aging of asphalt binders using antioxidant additives and copolymers. International Journal of Pavement Engineering, 20 (10), 1154–1169. (Source: https://doi.org/10.1080/10298436.2017.1394098).

  11. Lesueur, D. (2009). The colloidal structure of bitumen: Consequences on the rheology and on the mechanisms of bitumen modification. Advances in Colloid and Interface Science, 145 (1–2), 42-82. (Source: https://doi.org/10.1016/j.cis.2008.08.011).

  12. Corbett, L. W. (1969). Composition of asphalt based on generic fractionation, using solvent deasphaltening, elution-adsorption chromatography, and densimetric characterization. Analytical Chemistry, 41, 576–579.

    Article  Google Scholar 

  13. Dealy, J. M. (1979). Rheological properties of oil sand bitumens. The Canadian Journal of Chemical Engineering, 57, 677–683.

    Article  Google Scholar 

  14. Robertson, R. E., Branthaver, J. F., Plancher, H., Duvall, J. J., Ensley, E. K., Harnsberger, P. M., & Peterson, J. C. (1991). Chemical properties of asphalts and their relationships to pavement performance. Asphalt Paving Technology: Association of Asphalt Paving Technologists-Proceedings of the Technical Sessions, 60, 413–436.

    Google Scholar 

  15. Michalica, P., Kazatchkov, I. B., Stastna, J., & Zanzotto, L. (2008). Relationship between chemical and rheological properties of two asphalts of different origins. Fuel, 87, 3247–3253.

    Article  Google Scholar 

  16. Loeber, L., Sutton, O., Morel, J., Valleton, J. M., & Muller, G. (1996). New direct observations of asphalts and asphalt binders by scanning electron microscopy and atomic force microscopy. Journal of Microscopy, 182, 32–39.

    Article  Google Scholar 

  17. Pauli, A. T., Branthaver, J. F., Robertson, R. E., Grimes, W., & Eggleston, C. M. (2001). Atomic force microscopy investigation of SHRP asphalts. American Chemical Society, Division of Petroleum Chemistry, 46, 104–110.

    Google Scholar 

  18. Pauli, A. T., Grimes, R. W., Beemer, A. G., Turner, T. F., & Branthaver, J. F. (2011). Morphology of asphalts, asphalt fractions and model wax-doped asphalts studied by atomic force microscopy. International Journal of Pavement Engineering, 12, 291–309.

    Article  Google Scholar 

  19. Jäger, A., Lackner, R., Eisenmenger-Sittner, C., & Blab, R. (2004). Identification of microstructural components of bitumen by means of atomic force microscopy (AFM). Proceedings in Applied Mathematics and Mechanics, 4, 400–401.

    Article  Google Scholar 

  20. Masson, J. F., Leblond, V., & Margeson, J. (2006). Bitumen morphologies by phase-detection atomic force microscopy. Journal of Microscopy, 221, 17–29.

    Article  MathSciNet  Google Scholar 

  21. Allen, R. G., Little, D. N., & Bhasin, A. (2012). Structural characterization of micromechanical properties in asphalt using atomic force microscopy. Journal of Materials in Civil Engineering, 24, 1317–1327.

    Article  Google Scholar 

  22. Jahangir, R., Little, D., & Bhasin, A. (2015). Evolution of asphalt binder microstructure due to tensile loading determined using AFM and image analysis techniques. International Journal of Pavement Engineering, 16, 337–349.

    Article  Google Scholar 

  23. Khan, M. S., Kassem, E., McDonald, A., Sirin, O., Aston, D. E. (2022). Comparative characterization of field and laboratory-aged binder modified with antioxidant additives and copolymers using fourier transform infrared spectroscopy and gel permeation chromatography. Journal of Transportation Engineering, Part B: Pavements, 148(2). https://ascelibrary.org/doi/abs/10.1061/JPEODX.0000376.

  24. Sirin, O., Paul, D. K., Ohiduzzaman, M., & Kassem, E. (2017). Effect of ageing on asphalt binders in the State of Qatar: A case study. Road Materials and Pavement Design, 18, 165–184.

    Article  Google Scholar 

  25. Sirin, O., Paul, D. K., Khan, M. S., Kassem, E., Darabi, M. K. (2019). Effect of aging on viscoelastic properties of asphalt mixtures. Journal of Transportation Engineering, Part B: Pavements, 145(4). https://ascelibrary.org/doi/abs/10.1061/JPEODX.0000137.

  26. Redicote AP asphalt additive—asphalt applications, Akzo Nobel (2019). Retrieved from https://e-asphalt.com/wp-content/uploads/2019/04/ap.pdf.

  27. Solprene SSBR (1205)—Safety data sheet, Dynasol Elastomers (2018). Retrieved from https://dynasolgroup.com/documents/37150/107414/Solprene+1205-SDS-Eng.pdf.

  28. Oxford Instruments and WITec (2023). Alpha300A - Atomic Force Microscopes, Nanoscale Surface Characterization. https://raman.oxinst.com/assets/uploads/raman/materials/WITec-AFM-Brochure.pdf.

  29. Oxford Instruments and WITec (2023). Scanning Probe Microscopy. https://raman.oxinst.com/techniques/scanning-probe-microscopy.

  30. Allen, R. G., Little, D. N., Bhasin, A. (2012). Structural characterization of micromechanical properties in asphalt using atomic force microscopy. Journal of Materials in Civil Engineering, 24(10), 104. https://ascelibrary.org/doi/10.1061/%28ASCE%29MT.1943-5533.0000510.

    Article  Google Scholar 

  31. Schindelin, J., Rueden, C. T., Hiner, M. C., & Eliceiri, K. W. (2015). The ImageJ ecosystem: An open platform for biomedical image analysis. Molecular Reproduction and Development, 82, 518–529.

    Article  Google Scholar 

  32. Redicote AP asphalt additive—technical information, Akzo Nobel (2019). Retrieved from https://e-asphalt.com/wp-content/uploads/2019/04/aptr.pdf.

  33. Technical Bulletin—Redicote AP, Nouryon (2023). Retrieved from https://www.nouryon.com/globalassets/inriver/resources/technical-bulletin-asphalt-redicote-ap-global-en.pdf.

  34. Guo, M., Huang, Y., Wang, L., Yu, J., & Hou, Y. (2018). Using atomic force microscopy and molecular dynamics simulation to investigate the asphalt micro properties. International Journal of Pavement Research and Technology, 11(4), 321–326. https://doi.org/10.1016/j.ijprt.2017.09.017.

    Article  Google Scholar 

  35. Blunt, L., Jiang, X. (2003). Advanced Techniques for Assessment Surface Topography, Development of a Basis for 3D Surface Texture Standards “SURFSTAND”. Kogan Page Science. https://www.sciencedirect.com/book/9781903996119/advanced-techniques-for-assessment-surface-topography.

  36. Schmidt, U., Hild, S., Ibach, W., & Hollricher, O. (2005). Characterization of thin polymer films on the nanometer scale with confocal Raman AFM. Macromolecular symposia, 230, 133–143.

    Article  Google Scholar 

  37. Allen, R. G. (2013). Microstructural characterization of the chemomechanical behavior of asphalt in terms of aging and fatigue performance properties. Texas A&M University. https://www.proquest.com/docview/1427878632?pq-origsite=gscholar&fromopenview=true.

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Acknowledgements

The authors express their gratitude to the Qatar Foundation for the financial support of this work.

Funding

This paper was made possible by the NPRP grant (NPRP 6-773-2-320) from the Qatar National Research Fund (a member of Qatar Foundation). The AFM was purchased from an NSF major equipment grant # 0619310.

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Correspondence to Emad Kassem.

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Khan, M.S., Kassem, E., Aston, D.E. et al. Impact of Aging on the Microstructure of Asphalt Binder Modified with Antioxidant Additives and Copolymers. Int. J. Pavement Res. Technol. (2023). https://doi.org/10.1007/s42947-023-00347-2

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  • DOI: https://doi.org/10.1007/s42947-023-00347-2

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