High performance natural rubber composites with a hierarchical reinforcement structure of carbon nanotube modified natural fibers

•Natural rubber (NR) composites reinforced with CNT-modified short jute fibers.•MWCNTs deposited to the surface of jute fibers via non-covalent interactions.•Hierarchical reinforcement structure with improved wettability towards the NR.•Increased interfacial adhesion strength via mechanical interlocking.•Natural-based elastomer composites with high mechanical performance.

A simple and facile method for depositing multiwall carbon nanotubes (MWCNTs) onto the surface of naturally occurring short jute fibers (JFs) is reported. Hierarchical multi-scale structures were formed with CNT-networks uniformly distributed and fully covering the JFs (JF–CNT), as depicted by the scanning electron microscopy (SEM) micrographs. The impact of these hybrid fillers on the mechanical properties of a natural rubber (NR) matrix was systematically investigated. Pristine JFs were cut initially to an average length of 2.0 mm and exposed to an alkali treatment (a-JFs) to remove impurities existing in the raw jute. MWCNTs were treated under mild acidic conditions to generate carboxylic acid moieties. Afterward, MWCNTs were dispersed in an aqueous media and short a-JFs were allowed to react with them. Raman spectroscopy confirmed the chemical interaction between CNTs and JFs. The JF–CNT exposed quite hydrophobic behavior as revealed by the water contact angle measurements, improving the wettability of the non-polar NR. Consequently, the composite interfacial adhesion strength was significantly enhanced while a micro-scale “mechanical interlocking” mechanism was observed from the interphase-section transmission electron microscopy (TEM) images. SEM analysis of the composite fracture surfaces demonstrated the interfacial strength of NR/a-JF and NR/JF–CNT composites, at different fiber loadings. It can be presumed that the CNT-coating effectively compatibillized the composite structure acting as a macromolecular coupling agent. A detailed analysis of stress-strain and dynamic mechanical spectra confirmed the high mechanical performance of the hierarchical composites, consisting mainly of materials arising from natural resources.

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