Skip to main content
SpringerLink
Log in

Interfacial bonding between graphene oxide and calcium silicate hydrate gel of ultra-high performance concrete

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

Abstract

The incorporation of graphene oxide (GO) into ultra-high performance concrete (UHPC) can solve the problems of brittle fracture and low tensile strength of UHPC to some extent. By means of molecular dynamics simulation, this paper provided an insight into the interfacial bonding between GO and calcium silicate hydrate (C-S-H) gel, the dominant component of bonding phase in cement-based materials, in the chemical environment of UHPC in terms of C-S-H/GO interfacial structure, energies, and mechanical properties and gave the comparison with the case of ordinary Portland cement (OPC) materials. The results show that, as compared with the case of OPC, the C-S-H produced in UHPC has more calcium and hydroxyls distributed in the interlayer, leading to larger interlayer spacing with more water molecules absorbed. Water and hydroxyls occupy the sites of interfacial chemical bonds and weakens the C-S-H/GO interfacial Ca–O ionic bonds and H-bond network, but serve as bridges connecting C-S-H gel and GO sheet. More interlayer calcium for the UHPC case leads to larger interfacial interaction energies, which results in the higher tensile strength of the C-S-H/GO interface of UHPC sample. During tensile process, water molecules in the interface deforms with the structure and forms H-bond network serving to C-S-H/GO adhesion, which improves ductility of the structure. Furthermore, the configuration during elongation that the edge of GO sheet is tightly attached to C-S-H indicates the strong strength of Ca–Ocoo− bonds.

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. Wang D, Shi C, Wu Z, Xiao J, Huang Z, Fang Z (2015) A review on ultra high performance concrete: part II. Hydration, microstructure and properties. Constr Build Mater 96:368–377

    Google Scholar 

  2. Lee NK, Koh K, Kim MO, Ryu G (2018) Uncovering the role of micro silica in hydration of ultra-high performance concrete (UHPC). Cem Concr Res 104:68–79

    Google Scholar 

  3. Yi N-H, Kim J-HJ, Han T-S, Cho Y-G, Lee JH (2012) Blast-resistant characteristics of ultra-high strength concrete and reactive powder concrete. Constr Build Mater 28:694–707

    Google Scholar 

  4. Wicklein B, Kocjan A, Salazar-Alvarez G, Carosio F, Camino G, Antonietti M, Bergström L (2015) Thermally insulating and fire-retardant lightweight anisotropic foams based on nanocellulose and graphene oxide. Nat Nanotechnol 10:277

    Google Scholar 

  5. Lee C, Wei X, Kysar JW, Hone J (2008) Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science 321:385–388

    Google Scholar 

  6. Bunch JS, Van Der Zande AM, Verbridge SS, Frank IW, Tanenbaum DM, Parpia JM, Craighead HG, McEuen PL (2007) Electromechanical resonators from graphene sheets. Science 315:490–493

    Google Scholar 

  7. Dreyer DR, Park S, Bielawski CW, Ruoff RS (2010) The chemistry of graphene oxide. Chem Soc Rev 39:228–240

    Google Scholar 

  8. Lu L, Ouyang D (2017) Properties of cement mortar and ultra-high strength concrete incorporating graphene oxide nanosheets. Nanomaterials 7:187

    Google Scholar 

  9. Zhou C, Li F, Hu J, Ren M, Wei J, Yu Q (2017) Enhanced mechanical properties of cement paste by hybrid graphene oxide/carbon nanotubes. Constr Build Mater 134:336–345

    Google Scholar 

  10. Lv S, Ma Y, Qiu C, Sun T, Liu J, Zhou Q (2013) Effect of graphene oxide nanosheets of microstructure and mechanical properties of cement composites. Constr Build Mater 49:121–127

    Google Scholar 

  11. Gong K, Pan Z, Korayem AH, Qiu L, Li D, Collins F, Wang CM, Duan WH (2014) Reinforcing effects of graphene oxide on Portland cement paste. J Mater Civ Eng 27:A4014010

    Google Scholar 

  12. Shang Y, Zhang D, Yang C, Liu Y, Liu Y (2015) Effect of graphene oxide on the rheological properties of cement pastes. Constr Build Mater 96:20–28

    Google Scholar 

  13. Huang W, Kazemi-Kamyab H, Sun W, Scrivener K (2017) Effect of cement substitution by limestone on the hydration and microstructural development of ultra-high performance concrete (UHPC). Cem. Concr. Compos. 77:86–101

    Google Scholar 

  14. Schachinger I, Hilbig H, Stengel T, Fehling E (2008) Effect of curing temperature at an early age on the long-term strength development of UHPC. In: 2nd international symposium on ultra high performance concrete, vol 10, pp 205–213

  15. Reda M, Shrive N, Gillott J (1999) Microstructural investigation of innovative UHPC. Cem Concr Res 29:323–329

    Google Scholar 

  16. Pan Z, He L, Qiu L, Korayem AH, Li G, Zhu JW, Collins F, Li D, Duan WH, Wang MC (2015) Mechanical properties and microstructure of a graphene oxide–cement composite. Cem Concr Compos 58:140–147

    Google Scholar 

  17. Wang Q, Wang J, Lu C-X, Liu B-W, Zhang K, Li C-Z (2015) Influence of graphene oxide additions on the microstructure and mechanical strength of cement. New Carbon Mater 30:349–356

    Google Scholar 

  18. Li X, Liu YM, Li WG, Li CY, Sanjayan JG, Duan WH, Li Z (2017) Effects of graphene oxide agglomerates on workability, hydration, microstructure and compressive strength of cement paste. Constr Build Mater 145:402–410

    Google Scholar 

  19. Lv S, Ting S, Liu J, Zhou Q (2014) Use of graphene oxide nanosheets to regulate the microstructure of hardened cement paste to increase its strength and toughness. CrystEngComm 16:8508–8516

    Google Scholar 

  20. Li W, Li X, Chen SJ, Liu YM, Duan WH, Shah SP (2017) Effects of graphene oxide on early-age hydration and electrical resistivity of Portland cement paste. Constr Build Mater 136:506–514

    Google Scholar 

  21. Lin C, Wei W, Hu YH (2016) Catalytic behavior of graphene oxide for cement hydration process. J Phys Chem Solids 89:128–133

    Google Scholar 

  22. Hou D, Yang T, Tang J, Li S (2018) Reactive force-field molecular dynamics study on graphene oxide reinforced cement composite: functional group de-protonation, interfacial bonding and strengthening mechanism. Phys Chem Chem Phys 20:8773–8789

    Google Scholar 

  23. Hou D, Lu Z, Li X, Ma H, Li Z (2017) Reactive molecular dynamics and experimental study of graphene–cement composites: structure, dynamics and reinforcement mechanisms. Carbon 115:188–208

    Google Scholar 

  24. Sanchez F, Zhang L (2008) Molecular dynamics modeling of the interface between surface functionalized graphitic structures and calcium-silicate-hydrate: interaction energies, structure, and dynamics. J Colloid Interface Sci 323:349–358

    Google Scholar 

  25. Pellenq RJ-M, Kushima A, Shahsavari R, Van Vliet KJ, Buehler MJ, Yip S, Ulm F-J (2009) A realistic molecular model of cement hydrates. Proc Natl Acad Sci 106:16102–16107

    Google Scholar 

  26. Allen AJ, Thomas JJ, Jennings HM (2007) Composition and density of nanoscale calcium-silicate-hydrate in cement. Nat Mater 6:311

    Google Scholar 

  27. Sorelli L, Constantinides G, Ulm F-J, Toutlemonde F (2008) The nano-mechanical signature of ultra high performance concrete by statistical nanoindentation techniques. Cem Concr Res 38:1447–1456

    Google Scholar 

  28. Allington R, Attwood D, Hamerton I, Hay J, Howlin B (1998) A model of the surface of oxidatively treated carbon fibre based on calculations of adsorption interactions with small molecules. Compos A Appl Sci Manuf 29:1283–1290

    Google Scholar 

  29. Montes-Morán M, Van Hattum F, Nunes J, Martinez-Alonso A, Tascón J, Bernardo C (2005) A study of the effect of plasma treatment on the interfacial properties of carbon fibre–thermoplastic composites. Carbon 8:1795–1799

    Google Scholar 

  30. Dhakate S, Bahl O (2003) Effect of carbon fiber surface functional groups on the mechanical properties of carbon–carbon composites with HTT. Carbon 41:1193–1203

    Google Scholar 

  31. Cygan RT, Liang J, Kalinichev AG (2004) Molecular models of hydroxide, oxyhydroxide, and clay phases and the development of a general force field. J Phys Chem B 108:1255–1266

    Google Scholar 

  32. Hou D, Li Z (2014) Molecular dynamics study of water and ions transport in nano-pore of layered structure: a case study of tobermorite. Microporous Mesoporous Mater 195:9–20

    Google Scholar 

  33. Shinoda W, Devane R, Klein ML (2008) Coarse-grained molecular modeling of non-ionic surfactant self-assembly. Soft Matter 4:2454–2462

    Google Scholar 

  34. Wang Y, Noid WG, Liu P, Voth GA (2009) Effective force coarse-graining. Phys Chem Chem Phys 11:2002–2015

    Google Scholar 

  35. Vinod S, Tiwary CS, Samanta A, Ozden S, Narayanan TN, Vajtai R, Agarwal V, Singh AK, John G, Ajayan PM (2017) Graphene oxide epoxy (GO-xy): GO as epoxy adhesive by interfacial reaction of functionalities. Adv Mater Interfaces 5:1700657

    Google Scholar 

  36. Kabbani MA, Kochat V, Bhowmick S, Soto M, Som A, Krishnadas KR, Woellner CF, Jaques YM, Barrera EV, Asif S (2018) Consolidation of functionalized graphene at ambient temperature via mechano-chemistry. Carbon 134:491–499

    Google Scholar 

  37. Bonnaud PA, Labbez C, Miura R, Suzuki A, Miyamoto N, Hatakeyama N, Miyamoto A, Van Vliet KJ (2016) Interaction grand potential between calcium-silicate-hydrate nanoparticles at the molecular level. Nanoscale 8:4160–4172

    Google Scholar 

  38. Hou D, Yu J, Wang P (2019) Molecular dynamics modeling of the structure, dynamics, energetics and mechanical properties of cement–polymer nanocomposite. Compos B Eng 162:433–444

    Google Scholar 

  39. Dauber-Osguthorpe P, Roberts VA, Osguthorpe DJ, Wolff J, Genest M, Hagler AT (2010) Structure and energetics of ligand binding to proteins: escherichia coli dihydrofolate reductase-trimethoprim, a drug-receptor system. Proteins 4:31–47

    Google Scholar 

  40. Hoover WG (1985) Canonical dynamics: equilibrium phase-space distributions. Phys Rev A 31:1695

    Google Scholar 

  41. Hoover WG (1986) Constant-pressure equations of motion. Phys Rev A 34:2499

    Google Scholar 

  42. Esteves LP (2011) On the hydration of water-entrained cement–silica systems: combined SEM, XRD and thermal analysis in cement pastes. Thermochim Acta 518:27–35

    Google Scholar 

  43. Hesse C, Goetz-Neunhoeffer F, Neubauer J, Braeu M, Gaeberlein P (2009) Quantitative in situ X-ray diffraction analysis of early hydration of Portland cement at defined temperatures. Powder Diffr 24:112–115

    Google Scholar 

  44. Liu Z, Zhang Y, Liu L, Jiang Q (2013) An analytical model for determining the relative electrical resistivity of cement paste and C-S-H gel. Constr Build Mater 48:647–655

    Google Scholar 

  45. Dikin DA, Stankovich S, Zimney EJ, Piner RD, Dommett GHB, Evmenenko G, Nguyen ST, Ruoff RS (2007) Preparation and characterization of graphene oxide paper. Nature 448:457–460

    Google Scholar 

  46. Matsuyama H, Young JF (1999) Synthesis of calcium silicate hydrate/polymer complexes: part I. Anionic and nonionic polymers. J Mater Res 14:3379–3388

    Google Scholar 

  47. Matsuyama H, Young JF (1999) Synthesis of calcium silicate hydrate/polymer complexes: part II. Cationic polymers and complex formation with different polymers. J Mater Res 14:3389–3396

    Google Scholar 

  48. Pelisser F, Gleize PJP, Mikowski A (2014) Structure and micro-nanomechanical characterization of synthetic calcium-silicate-hydrate with poly(vinyl alcohol). Cem Concr Compos 48:1–8

    Google Scholar 

  49. Yamaguchi T, Hayashi S, Ohtaki H (1989) X-ray diffraction study of calcium(II) chloride hydrate melts: CaCl2.cntdot.RH2O (R = 4.0, 5.6, 6.0, and 8.6). Inorg Chem 28:2434–2439

    Google Scholar 

  50. Zhang R, Gao B, Ma Q, Zhang J, Cui H, Liu L (2016) Directly grafting graphene oxide onto carbon fiber and the effect on the mechanical properties of carbon fiber composites. Mater Des 93:364–369

    Google Scholar 

  51. Song Y, Chen Y, Liu W, Li W, Wang Y, Zhao D, Liu X (2016) Microscopic mechanical properties of titanium composites containing multi-layer graphene nanofillers. Mater Des 109:256–263

    Google Scholar 

  52. Lu Z, Hou D, Hanif A, Hao W, Li Z, Sun G (2018) Comparative evaluation on the dispersion and stability of graphene oxide in water and cement pore solution by incorporating silica fume. Cem Concr Compos 94:33–42

    Google Scholar 

  53. Lu Z, Hanif A, Ning C, Shao H, Yin R, Li Z (2017) Steric stabilization of graphene oxide in alkaline cementitious solutions: mechanical enhancement of cement composite. Mater Des 127:154–161

    Google Scholar 

  54. Farrokhpay S, Morris GE, Fornasiero D, Self P (2004) Effects of chemical functional groups on the polymer adsorption behavior onto titania pigment particles. J Colloid Interface Sci 274:33–40

    Google Scholar 

  55. Zhang X, Wang J-C, Lacki KM, Liapis AI (2004) Molecular dynamics simulation studies of the transport and adsorption of a charged macromolecule onto a charged adsorbent solid surface immersed in an electrolytic solution. J Colloid Interface Sci 277:483–498

    Google Scholar 

  56. Ter Horst J, Sang KWF, de Vreugd C, Geertman R, Witkamp G, van Rosmalen G (1999) Adsorption behaviour of polyelectrolytes on calcium fluoride: part II: molecular modeling of the adsorption behaviour. Colloids Surf A 154:273–284

    Google Scholar 

  57. Pellenq R-M, Caillol J, Delville A (1997) Electrostatic attraction between two charged surfaces: a (N, V, T) Monte Carlo simulation. J Phys Chem B 101:8584–8594

    Google Scholar 

  58. Hou D, Lu C, Zhao T, Zhang P, Ding Q (2015) Structural, dynamic and mechanical evolution of water confined in the nanopores of disordered calcium silicate sheets. Microfluid Nanofluid 19:1309–1323

    Google Scholar 

Download references

Acknowledgements

The research is financially supported from the National Key Research and Development Program of China (2018YFC0705400), China Postdoctoral Science Foundation (2018M642630), Guangdong Provincial Key Laboratory of Durability for Marine Civil Engineering, Shenzhen Durability Center for Civil Engineering, Shenzhen University (GDDCE 18-4), Shandong Provincial Natural Science Foundation of China (ZR2019MEM041).

Author information

Authors and Affiliations

  1. School of Materials Science and Engineering, Southeast University, Nanjing, 211189, China

    Hongyan Wan & Yu Zhang

Authors
  1. Hongyan Wan
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yu Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Yu Zhang.

Ethics declarations

Conflict of interest

The authors declare no conflict of interest.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Wan, H., Zhang, Y. Interfacial bonding between graphene oxide and calcium silicate hydrate gel of ultra-high performance concrete. Mater Struct 53, 34 (2020). https://doi.org/10.1617/s11527-020-01467-y

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1617/s11527-020-01467-y

Keywords

Search

Navigation