Skip to main content
SpringerLink
Log in

Atomic level simulations of the interaction of asphaltene with quartz surfaces: role of chemical modifications and aqueous environment

  • Original Article
  • Published:
Materials and Structures Aims and scope Submit manuscript

Abstract

Understanding the properties of bitumen and its interaction with mineral aggregates is crucial for future strategies to improve roads and highways. Knowledge of basic molecular and electronic structures of bitumen, one out of the two main components of asphalt, poses a major step towards achieving such a goal. In the present work we employ atomistic simulation techniques to study the interaction of asphaltenes, a major constituent of bitumen, with quartz surfaces. As an effective means to tune adhesion or cohesion properties of asphaltenes and mineral surfaces, we propose chemical modification of the pristine asphaltene structure. By the choice of substituent and site of substitution we find that adhesion between the asphaltene molecule and the quartz surface can easily be improved at the same time as the cohesive interaction between the asphaltene units is reduced, while other substituents may lead to the opposite effect. We also provide insight at the molecular level into how water molecules affect interactions between asphaltenes and quartz. Our approach emphasizes a future role for advanced atomistic modeling to understand the properties of bitumen and suggest further improvements.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

References

  1. Wiehe A, Liang KS (1996) Asphaltenes, resin, and other petroleum macromolecules. Fluid Phase Equilib 117:201–210

    Article  Google Scholar 

  2. Barth EJ (1962) Asphalt, science and technology. Gordon and Breach, New York

    Google Scholar 

  3. Rostler FS, Whiteoak D (2003) The shell bitumen handbook, 5th edn. Shell UK Oil Products Limited, London

    Google Scholar 

  4. Corbett LW (1969) Composition of asphalt based on generic fractionation using solvent deasphalting, elution-adsorption chromatography, and densimetric characterization. Anal Chem 41:576

    Article  Google Scholar 

  5. Sheu EY, Mullins OC (1995) Asphaltenes: fundamentals and applications. Plenum Press, New York

    Book  Google Scholar 

  6. Yen TF, Chilingarian GV (1994) Asphaltenes and asphalts. Elsevier, Amsterdam

    Google Scholar 

  7. Eberhardsteiner L, Fu J, Hofko B, Handle F, Hospodka M, Blab R, Grothe H (2015) Influence of asphaltene content on mechanical bitumen behavior: experimental investigation and micromechanical modeling. Mater Struct. doi:10.1617/s11527-014-0383-7

    Google Scholar 

  8. Greenfield ML (2011) Molecular modeling and simulation of asphaltenes and bituminous materials. Int J Pavement Eng 12(4):325–341

    Article  Google Scholar 

  9. Zhang L, Greenfield ML (2007) Analyzing properties of model asphalts using molecular simulation. Energy Fuels 21:1712–1716

    Article  Google Scholar 

  10. Zhang L, Greenfield ML (2007) Molecular orientation in model asphalts using molecular simulation. Energy Fuels 21:1102–1111

    Article  Google Scholar 

  11. Zhang L, Greenfield ML (2007) Relaxation time, diffusion, and viscosity analysis of model asphalt systems using molecular simulation. J Chem Phys 127:194502

    Article  Google Scholar 

  12. Li DD, Greenfield ML (2014) Viscosity, relaxation time, and dynamics within a model asphalt of larger molecules. J Chem Phys 140:034507

    Article  Google Scholar 

  13. Zhang L, Greenfield ML (2010) Rotational relaxation times of individual compounds within simulations of molecular asphalt models. J Chem Phys 132:184502

    Article  Google Scholar 

  14. Zhang L, Greenfield ML (2008) Effect of polymer modification in properties and microstructures of model asphalt systems. Energy Fuels 22:3363–3375

    Article  Google Scholar 

  15. Li DD, Greenfield ML (2014) Chemical compositions of improved model asphalt systems for molecular simulations. Fuel 115:347–356

    Article  Google Scholar 

  16. Li DD, Greenfield ML (2011) High internal energies of proposed asphaltene structures. Energy Fuels 25:3698–3705

    Article  Google Scholar 

  17. Tarefder RA, Arisa I (2011) Molecular dynamic simulations for determining change in thermodynamic properties of asphaltene and resin because of aging. Energy Fuels 25:2211–2222

    Article  Google Scholar 

  18. Hansen JS, Lemarchand CA, Nielsen E, Dyre JC, Schrøder T (2013) Four-component united-atom model of bitumen. J Chem Phys 138:094508

    Article  Google Scholar 

  19. Lemarchand CA, Schrøder TB, Dyre JC, Hansen JS (2013) Cooee bitumen: chemical aging. J Chem Phys 139:124506

    Article  Google Scholar 

  20. Lemarchand CA, Schrøder TB, Dyre JC, Hansen JS (2014) Cooee bitumen. II. Stability of linear asphaltene nanoaggregates. J Chem Phys 141:144308

    Article  Google Scholar 

  21. CP2K version 2.3. the CP2K developers group 2012; http://www.cp2k.org/

  22. VandeVondele J, Hutter J (2003) An efficient orbital transformation method for electronic structure calculations. J Chem Phys 118:4365

    Article  Google Scholar 

  23. VandeVondele J, Krack M, Mohamed F, Parrinello M, Chassaing T, Hutter J (2005) Quickstep: fast and accurate density functional calculations using a mixed Gaussian and plane waves approach. Comp Phys Commun 167:103

    Article  Google Scholar 

  24. Krack M (2005) Pseudopotentials for H to Kr optimized for gradient-corrected exchange-correlation functionals. Theo Chem Acc 114:145–152

    Article  Google Scholar 

  25. VandeVondele J, Hutter J (2007) Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases. J Chem Phys 127:114105

    Article  Google Scholar 

  26. Frisch MJ et al (2009) Gaussian 09, revision A.02. Gaussian, Inc, Wallingford

    Google Scholar 

  27. Case DA, Darden TA, Cheatham TE, Simmerling CL, Wang J, Duke RE, Luo R, Walker RC, Zhang W, Merz KM, Roberts B, Hayik S, Roitberg A, Seabra G, Swails J, Götz AW, Kolossváry I, Wong KF, Paesani F, Vanicek J, Wolf RM, Liu J, Wu X, Brozell SR, Steinbrecher T, Gohlke H, Cai Q, Ye X, Wang J, Hsieh MJ, Cui G, Roe DR, Mathews DH, Seetin MG, Salomon-Ferrer R, Sagui C, Babin V, Luchko T, Gusarov S, Kovalenko A, Kollman PA. AMBER 12 2012; University of California, San Francisco

  28. Wang J, Wolf R, Caldwell J, Kollman P, Case DA (2004) Development and testing of a general AMBER force field. J Comput Chem 34:1157–1174

    Article  Google Scholar 

  29. Sieffert N, Wipff G (2008) Ordering of imidazolium-based ionic liquids at the α-quartz (001) surface: a molecular dynamics study. J Phys Chem C 112:19590–19603

    Article  Google Scholar 

  30. Joule J, Mills K (2010) Heterocyclic chemistry, 5th edn. Wiley, New York

    Google Scholar 

Download references

Acknowledgements

We acknowledge Dr. Yaoquan Tu for helpful advice and discussions. This work was supported by a grant from the Swedish Infrastructure Committee (SNIC) for the project “Multiphysics Modeling of Molecular Materials”, SNIC2013-26-31.

Author information

Authors and Affiliations

  1. Division of Theoretical Chemistry and Biology, School of Biotechnology, KTH Royal Institute of Technology, 10691, Stockholm, Sweden

    Naresh K. Jena, N. Arul Murugan & Hans Ågren

  2. Sustainable Buildings, Swedish Cement and Concrete Research Institute, 100 44, Stockholm, Sweden

    Åsa Laurell Lyne & Björn Birgisson

  3. CEOB (Civil Engineering Office Building), Texas A&M University, 3136 TAMU, College Station, TX, 77843-3136, USA

    Björn Birgisson

Authors
  1. Naresh K. Jena
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Åsa Laurell Lyne
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. N. Arul Murugan
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Hans Ågren
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Björn Birgisson
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Åsa Laurell Lyne.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Jena, N.K., Lyne, Å.L., Arul Murugan, N. et al. Atomic level simulations of the interaction of asphaltene with quartz surfaces: role of chemical modifications and aqueous environment. Mater Struct 50, 99 (2017). https://doi.org/10.1617/s11527-016-0880-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1617/s11527-016-0880-y

Keywords

Search

Navigation