A novel natural rubber/multi-walled carbon nanotubes (NR/MWCNTs) nanocomposite is developed by combining self-assembly technique. Natural rubber composites containing carboxylated multiwalled carbon nanotubes dispersed with sodium dodecyl sulfate generated in situ by the sol-gel process are investigated. The functionalization of CNTs was carried out by diazonium salt methodology in acid medium. The sol-gel processing is conducted in order to obtain a good dispersion of the inorganic particles. In each case, the different content of functionalized carbon nanotubes was mixed with natural rubber latex. Results from FESEM, FTIR and Raman analyses indicated that homogeneous dispersion of CNT throughout NR matrix with strong interfacial adhesion between oxidized CNT and the matrix are responsible for the considerable enhancement on the properties of the composite. The NR/MWCNTs have great potential to manufacture products with high mechanical performances.

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