Tensile and microstructural properties of multiwall carbon nanotube (MWCNT)/polyisoprene (PI) composites have been investigated after cross-linking achieved purely by simultaneous high-pressure high-temperature treatment. The method enables gradual increase of the cross-link density without interference of vulcanization chemicals, and the results suggest a link between an interfacial PI layer wrapped/coated on the MWCNTs and reinforcement in carbon nanotube (CNT)/PI composites. The interfacial layer, which is augmented by high-pressure treatment, was detected indirectly in swelling experiments and also reflected in results of atomic force microscopy. The results imply more efficient load transfer and mechanical reinforcement by CNTs with improved interfacial layer and that changes in the layer can be probed by swelling measurements.
■ INTRODUCTIONThe filler/polymer composite materials of today have a long history of development. 1,2 Various fillers such as carbon black, carbon fibers, silica, and clays, etc., 3 have been tested and proven favorable for mechanical and thermal reinforcement of polymers. But the recent discovery of new nanostructured materials and their extraordinary properties have raised expectations of major further improvements. 4 In particular, carbon nanotubes (CNTs) 5,6 and graphene 7 have mechanical and structural properties which are superior to those of the most commonly used fillers. 8 For example, assuming that CNTs in the perimeter of a bundle carried all the load, Yu et al. 9 obtained a tensile strength (σ UTS ) and a Young's modulus (E) of ∼22 and ∼1050 GPa, respectively, for a single-wall carbon nanotube (SWCNT) in a 19 nm bundle. Moreover, a 13 nm in diameter multiwall carbon nanotube (MWCNT) shows σ UTS of 28 GPa and E in the range from ∼270 to 950 GPa, 10 or an E average of 1.8 TPa, as reported by Treacy et al. 11 In general, theoretical calculations for SWCNTs and MWCNT indicate even higher strength and typically show σ UTS and E values of order of ∼1 TPa. 8,12 Besides the excellent mechanical properties, the unique structure with high aspect ratio (∼10 3 ) and low density make CNTs particularly interesting for the purpose of fabricating lightweight composites with high strength and stiffness. 1,13 In order to obtain CNT-based polymer composites with much improved mechanical performance, it is essential that the microstructure provides an efficient load transfer between the polymer matrix and the CNTs. 14 Covalent functionalization of CNTs is one method that opens the possibility of strong bonding between the otherwise essentially inert CNTs and a polymer matrix. The capability of this method is shown by Moniruzzaman et al.'s 15 results of more than 2 times higher σ UTS for fibers made of nylon-6, 10, and 1 wt % alkyl acid chloride group functionalized SWCNTs (SWCNT-(CH 2 ) n -COCl) than fibers of nylon-6, 10, and 1 wt % nonfunctionalized SWCNTs, which implies increased reinforcement due to covalent bonds between the nylon matrix and the functionalized CNTs. Another method to ob...