Colloid and Polymer Science

, Volume 294, Issue 3, pp 537–543 | Cite as

Self-healing properties of poly(ethylene-co-vinyl acetate)

  • Ryuya Osato
  • Takumi Sako
  • Jiraporn Seemork
  • Sunatda Arayachukiat
  • Shogo Nobukawa
  • Masayuki Yamaguchi
Original Contribution


Poly(ethylene-co-vinyl acetate) with 42 wt% of vinyl acetate shows autonomic self-healing at room temperature without macroscopic flow. Intermolecular diffusion of amorphous chains through the jointed boundary, which occurs because of the large amount of amorphous chains with low glass transition temperature, is responsible for the healing phenomenon. Furthermore, the healing efficiency is found to be enhanced when the separated pieces are recombined immediately after cutting. This result indicates that the cut surface has marked molecular mobility owing to the destruction of crystallites during the cutting process, which is supported by differential scanning calorimetry (DSC) measurements. The marked molecular mobility at the surface is, however, observed only for a short period after cutting, because further crystallization after cutting restricts the molecular motion.


Ethylene-co-vinyl acetate copolymer Self-healing Rheology Crystallinity 



This work was promoted by COI program “Construction of next-generation infrastructure system using innovative materials”—realization of safe and secure society that can coexist with the Earth for centuries—supported by the Japan Science and Technology Agency (JST). Further, a part of this study was supported by Grand-in-Aid for Scientific Research No. 25410221.

Compliance with ethical standards

Conflict of interest

The authors declare that they have no competing interests.

Supplementary material

396_2015_3817_Fig9_ESM.gif (90 kb)
Supplementary information 1

Schematic illustration of the sample preparation procedures for the DSC surface crystallinity evaluation measurements: (a) a large piece measuring 3 × 3 × 1.1 mm3 was cut out from the compressed sheet and kept at 25 °C for 64 h prior to the measurement, (b) 30 small pieces each with dimensions of 0.7 × 0.7 × 0.7 mm3 were cut from the compressed sheet and used immediately after cutting, and (c) the small pieces were kept at 25 °C for 64 h prior to the measurement. (GIF 90 kb)

396_2015_3817_MOESM1_ESM.tif (82 kb)
High resolution image (TIF 82 kb)
396_2015_3817_Fig10_ESM.gif (89 kb)
Supplementary information 2

Schematic illustration of molecular chains after cutting (GIF 89 kb)

396_2015_3817_MOESM2_ESM.tif (96 kb)
High resolution image (TIF 95 kb)


  1. 1.
    Wool RP (1994) Polymer interfaces: structure and strength. Hanser Gardener, CincinnatiGoogle Scholar
  2. 2.
    Wool RP (2008) Self-healing materials: a review. Soft Matter 4:400–418CrossRefGoogle Scholar
  3. 3.
    Wu DY, Meure S, Solomon D (2008) Self-healing polymeric materials; a review of recent developments. Prog Polym Sci 33:479–522CrossRefGoogle Scholar
  4. 4.
    Blaszik BJ, Kramer SLB, Olugebefola SC, Moore JS, Sottos NR, White SR (2010) Self-healing polymers and composites. Annu Rev Mater Res 40:179–211CrossRefGoogle Scholar
  5. 5.
    Murphy B, Wudl F (2010) The world of smart healable materials. Prog Polym Sci 35:223–251CrossRefGoogle Scholar
  6. 6.
    Zhang MQ, Rong MZ (2010) Self-healing polymers and polymer composites. Wiley, New YorkGoogle Scholar
  7. 7.
    Yamaguchi M, Maeda R, Kobayashi R, Wada T, Ono S, Nobukawa S (2012) Autonomic healing and welding by interdiffusion of dangling chains in weak gel. Polym Int 61:9–16CrossRefGoogle Scholar
  8. 8.
    Binder WH (2013) Self-healing polymers, from principles to applications. Wiley-VCH, WeinheimCrossRefGoogle Scholar
  9. 9.
    Yamaguchi M, Ono S, Terano M (2007) Self-repairing property of polymer network with dangling chains. Mater Lett 61:1396–1399CrossRefGoogle Scholar
  10. 10.
    Yamaguchi M, Ono S, Okamoto K (2009) Interdiffusion of dangling chains in weak gel and its application to self-repairing material. Mater Sci Eng B 162:189–194CrossRefGoogle Scholar
  11. 11.
    Summers JW (1981) The nature of poly(vinyl chloride) crystallinity—the microdomain structure. J Vinyl Technol 3:107–110CrossRefGoogle Scholar
  12. 12.
    Yamaguchi M (2001) Flow instability in capillary extrusion of plasticized poly(vinyl chloride). J Appl Polym Sci 82:1277–1283CrossRefGoogle Scholar
  13. 13.
    Nobukawa S, Shimada H, Aoki Y, Miyagawa A, Doan VA, Yoshimura H, Tachikawa Y, Yamaguchi M (2014) Extraordinary wavelength dispersion of birefringence in cellulose triacetate film with anisotropic nanopores. Polymer 55:3247–3253CrossRefGoogle Scholar
  14. 14.
    Yamaguchi M, Wakabayashi T (2006) Rheological properties and processability of chemically modified poly(ethylene terephthalate-co-ethylene isophthalate). Adv Polym Technol 25:236–241CrossRefGoogle Scholar
  15. 15.
    Yamaguchi M, Wakabayashi T, Kanoh T (2008) Effect of mixing conditions on rheological and optical properties for chemically modified poly(ethylene terephthalate-co-ethylene isophthalate). J Appl Polym Sci 107:2665–2670CrossRefGoogle Scholar
  16. 16.
    Rujirek W, Hachiya Y, Endo T, Nobukawa S, Yamaguchi M (2015) Anomalous transfer phenomenon of carbon nanotube in the blend of poly(ethylene terephthalate) and polycarbonate. Compos Part B 78:409–414CrossRefGoogle Scholar
  17. 17.
    Yamane H, Sakai K, Takano M, Takahashi M (2004) Poly(D-lactic acid) as a rheological modifier of poly(L-lactic acid): shear and biaxial extensional flow behavior. J Rheol 48:599–609CrossRefGoogle Scholar
  18. 18.
    Jimenez A, Peltzer M, Ruseckaite R (2014) Poly(lactic acid) science and technology: processing, properties, additives, and applications. Royal Society of Chemistry, OxfordshireGoogle Scholar
  19. 19.
    Salyer IO, Kenyon AS (1971) Structure and property relationships of ethylene-vinyl acetate copolymers. J Polym Sci Part A-1(9):3083–3103CrossRefGoogle Scholar
  20. 20.
    Shankernarayanan MJ, Sun DC, Kojima M, Magill JH (1987) Rolletrusion: doubly-orientation processing and morphology—property relationships for commercial plastics. Int Polym Proc 1:66–76CrossRefGoogle Scholar
  21. 21.
    Arsac A, Carrot C, Guillet J (1999) Rheological characterization of ethylene vinyl acetate copolymer. J Appl Polym Sci 74:2625–2630CrossRefGoogle Scholar
  22. 22.
    Dlubek G, Lpke T, Stejny J, Alam MA, Arnold M (2000) Local free volume in ethylene-vinyl acetate copolymers: a positron lifetime study. Macromolecules 33:990–996CrossRefGoogle Scholar
  23. 23.
    Peacock AJ (2000) Handbook of polyethylene. Marcel Dekker, New YorkGoogle Scholar
  24. 24.
    Takahashi S, Okada H, Nobukawa S, Yamaguchi M (2012) Optical properties of polymer blends composed of poly(methyl methacrylate) and ethylene-vinyl acetate copolymer. Eur Polym J 48:974–980CrossRefGoogle Scholar
  25. 25.
    Yamaguchi M, Arakawa K (2007) Control of structure and mechanical properties for binary blends of poly(3-hydroxybutyrate) and cellulose-derivative. J Appl Polym Sci 103:3447–3452CrossRefGoogle Scholar
  26. 26.
    Huang T, Miura M, Nobukawa S, Yamaguchi M (2014) Crystallization behavior and dynamic mechanical properties of poly(L-lactic acid) with poly(ethylene glycol) terminated by benzoate. J Polym Environ 22:183–189CrossRefGoogle Scholar
  27. 27.
    Zhu L (1999) In: Brandrup J, Immergut EH, Grulke EA (eds) Polymer handbook, V/9-19, 4th edn. Wiley Interscience, New YorkGoogle Scholar
  28. 28.
    Ferry JD (1980) Viscoelastic properties of polymers, 3rd edn. Wiley, New YorkGoogle Scholar
  29. 29.
    Wunderlich B (1980) Macromolecular physics, vol. 3, crystal melting. Academic, New YorkGoogle Scholar
  30. 30.
    Rodriguez-Cabello JC, Alonso M, Merino JC, Pasor JM (1996) Scanning electron microscopy and differential scanning calorimetry study of the transition front in uniaxially stretched isotactic polypropylene. J Appl Polym Sci 60:1709–1717CrossRefGoogle Scholar

Copyright information

© Springer-Verlag Berlin Heidelberg 2015

Authors and Affiliations

  • Ryuya Osato
    • 1
  • Takumi Sako
    • 1
  • Jiraporn Seemork
    • 1
    • 2
  • Sunatda Arayachukiat
    • 1
    • 2
  • Shogo Nobukawa
    • 1
  • Masayuki Yamaguchi
    • 1
  1. 1.School of Materials ScienceJapan Advanced Institute of Science and TechnologyNomiJapan
  2. 2.Program in Petrochemistry, Faculty of ScienceChulalongkorn UniversityPathumwanThailand

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