Effects of Reactive Compatibilizers on the Morphology and Properties of Natural Rubber/SiO2 Composites

  • Lee, Min Young (Department of Polymer Engineering, Chonnam National University) ;
  • Park, Jin Young (Department of Polymer Engineering, Chonnam National University) ;
  • Song, Ki Chan (Engineering Research Institute, Chonnam National University) ;
  • Kim, Su Kyung (Department of Polymer Engineering, Chonnam National University)
  • Received : 2016.02.12
  • Accepted : 2016.03.28
  • Published : 2016.06.30


Maleimidopropyltriethoxysilane grafted natural rubber (MISNR) was prepared by reaction of maleic anhydride grafted natural rubber and 3-aminopropyl triethoxysilane. MISNR was used as the compatibilizer of natural rubber/silica composites. The composites were prepared by two-step mixing procedures. The final mixtures were cured with optimum cure condition, which was established by a rheometer. Effects of the amounts of compatibilizer in the composites on the cure characteristics, morphology, thermal stability, and physical and mechanical behaviors were investigated. The composites having MISNR had shown cure characteristics and physical and mechanical properties superior to those without MISNR. Silica particles in the former appeared to be more uniform and reduced in size compared with the latter. The effects of the types of silica were also evaluated.


  1. M. P. Wagner, "Reinforcing Silicas and Silicates", Rubber Chem. Technol., 49, 703 (1976).
  2. J. H. Bachmann, J. W. Sellers, M. P. Wagner, and R. F. Wolf, "Fine Particle Reinforcing Silicas and Silicates in Elastomers", Rubber Chem. Technol., 32, 1286 (1959).
  3. T. A. Okel and W. H. Waddell, "Silica Properties/Rubber Performance Correlation. Carbon Black-Filled Rubber Compounds", Rubber Chem. Technol., 67, 217 (1994).
  4. W. H. Waddell and L. R. Evans, "Use of Nonblack Fillers in Tire Compounds", Rubber Chem. Technol., 69, 377 (1996).
  5. C. J. Brinker and G. W. Scherer, "Sol-Gel Science", p. 745, Academic Press, 1990.
  6. M. Kluppel, R. H. Schuster, and G. Heinrich, "Structure and Properties of Reinforcing Fractal Filler Networks in Elastomers", Rubber Chem. Technol., 70(2), 243 (1997).
  7. Wolff, "Chemical Aspects of Rubber Reinforcement by Fillers", Rubber Chem. Technol., 69(3), 325 (1996).
  8. M. Zaborski, L. Slusarski, and A. Vidal, "Surface Modification of Silica and Its Activity in Ethylene-Propylene Rubber", Int. Polym. Sci., 20(11), 99 (1993).
  9. J. S. Dick, "Rubber Technology", 2nd ed., p. 325, Hanser, 2010.
  10. J. E. Mark, B. Erman, and F. R. Eirich, "Science and Technology of Rubber", 2nd ed., p. 432, Academic Press, 1994.
  11. J. O. Park, "Organic-Inorganic Polymer Hybrids by Sol-Gel Process", Polym. Sci. Technol., 8(3), 261 (1997).
  12. S. Sakka, "Sol-Gel Science and Technology", Vol. 3, p. 27, Kluwer Academic Publishers, Norwell, 2004.
  13. A. Ansarifar, H.P. Lim, and R. Nijhawan, "Assessment of the Effect of a Bifunctional Organosilane on the Bound Rubber and Properties of Some Natural Rubber Compounds", Int. J. Adhes. Adhes., 24(1), 9 (2004).
  14. Y. Ikeda, A. S. Hashim, and Kohjiya, "Development in Organic-Inorganic Hybrid Elastomers Prepared by the Sol-Gel and Related Processes", Bull. Inst. Chem. Res. Kyoto Univ., 72(5-6), 406 (1995).
  15. Y. Ikeda and S. Kohjiya, "In Situ Formed Silica Particles in Rubber Vulcanizate by the Sol-Gel Method", Polymer, 38(17), 4417 (1997).
  16. Y. Ikeda and Y. Kameda, "Preparation of "Green" Composites by the Sol-Gel Process: In Situ Silica Filled Natural Rubber", J. Sol-Gel Sci. Technol., 31, 137 (2004).
  17. K. Murakami, S. Iio, Y. Ikeda, H. Ito, M. Tosaka, and S. Kohjiya, "Effect of Silane-Coupling Agent on Natural Rubber Filled with Silica Generated In Situ", J. Mater. Sci., 38(7), 1447 (2003).
  18. S. Kohjiya and Y. Ikeda, "In Situ Formation of Particulate Silica in Natural Rubber Matrix by the Sol-Gel Reaction", J. Sol-Gel Sci. Technol., 26(1), 495 (2003).
  19. Y. Ikeda, S. Poompradub, Y. Morita, and S. Kohjiya, "Preparation of High Performance Nanocomposite Elastomer: Effect of Reaction Conditions on In Situ Silica Genertion of High Content in Natural Rubber", J. Sol-Gel Sci. Technol., 45, 299 (2008).
  20. V. Tangpasuthadol, A. Intasiri, D. Nuntivanich, N. Niyompanich, and S. Kiatkamjornwong, "Silica-Reinforced Natural Rubber Prepared by the Sol-Gel Process of Ethoxysilanes in Rubber Latex", J. Appl. Polym. Sci., 109, 424 (2008).
  21. B. Chaichua, P. Prasassarakich, and S. Poompradub, "In Situ Silica Reinforcement of Natural Rubber by Sol-Gel Process via Rubber Solution", J. Sol-Gel Sci. Technol., 52, 219 (2009).
  22. E. Miloskovska, E. Nies, D. H. Bogerds, M. Duin, and G. With, "Influence of Reaction Parameters on the Structure of In Situ Rubber/Silica Compounds Synthesized via Sol-Gel Reaction", J. Polym. Sci. Polym. Phys., 52, 967 (2014).
  23. S. Poompradub, M. Thirakulrati, and P. Prasassarakich, "In Situ Generated Silica in Natural Rubber Latex via Sol-Gel Technique and Properties of the Silica Rubber Composites", Mater. Chem. Phys., 144, 122 (2014).
  24. J. A. Brydson, "Rubber Materials and Their Compounds", p. 16, Elsevier, New York, 1995.
  25. S. S. Park, B. H. Park, K. C. Song and S. K. Kim, "Effects of Mixing Mode on the Fracture Properties of Silica and Carbon Black Filled NR Vulcanizates", Polymer (Korea), 24(2), 220 (2000).
  26. S. K. Kim and S. C. Kim, "Polyurethane-Polystyrene Interpenetrating Polymer Networks Synthesized in the Presence of a Common Solvent", Polym. Bull., 23, 141 (1990).
  27. B. J. Bauer, D. W. Liu, C. L. Jackson, and J. D. Barnes, "Epoxy/$SiO_2$ Interpenetrating Polymer Networks", Polym. Adv. Technol., 7, 333 (1995).
  28. S. Wolff, "Chemical Aspects of Rubber Reinforcement by Fillers", Rubber Chem. Technol., 69, 325 (1996).
  29. S. Wolff, M. J. Wang, and E. H. Tan, "Filler-Elastomer Interactions. Part VII. Study on Bound Rubber", Rubber Chem. Technol., 66, 163 (1993).
  30. S. S. Park, "Influence of Silica and Ingredients on Properties of Natural Rubber Compounds", Ph. D. Thesis, Chonnam National University, p.19, 2000.