In this thesis, thermal and mechanical properties of polymers and carbon nanotubes-polymer composites, which were modified and studied under high pressure, are presented. The results concern the thermal conductivity κ and heat capacity per unit volume ρc_p of pure polymers: polyisoprene (PI), polybutadiene (PB), and nylon-6, and their multi-wall and single-wall carbon nanotube (MWCNT and SWCNT) composites both before (untreated) and after high pressure treatments. As shown here, a suitable high pressure high temperature (HP&HT) treatment induces either cross-links in the polymers (PI and PB), i.e. transforms these into elastomers, or increases the crystallinity (nylon-6).

The experiments were done, in situ, in the temperature range 100-520 K for pressures up to 1.5 GPa, and the results show that cross-linking under high pressure can be monitored in data for κ and ρc_p. Moreover, κ for a well cross-linked (ebonite-like) polymer near ambient conditions can be up to 50% higher than the untreated states, whereas ρc_p becomes similar as the glassy state of the untreated polymer. The glass transition of the cross-linked states becomes broader and shifts to higher temperatures with increasing degree of cross-linking. In the case of nylon-6, the HP&HT treatment causes microstructural changes, viz. increased crystallinity and crystals with a preferred orientation and increased size, which enhances κ and improves the thermal stability.

The thermal property studies of the CNT polymer composite show that k of the composites increases significantly, e.g. 120% for 5wt% SWCNTs in PI, which is attributed to the very high k of CNTs. Moreover, MWCNTs also improve k, but not as much as SWCNTs. This is accounted for by their lower aspect ratio (length/diameter), whereas their lower k is less important. Adding CNTs normally raise the glass transition temperatures of the polymers. More specifically, SWCNTs in PB raise the glass transition temperature slightly more than MWCNTs and, in particular, under the most densified conditions and for a high molecular weight PB, which may be due to more favorable conditions for coating/wrapping of the CNTs.

The mechanical studies of the HP&HT treated polymers and composites show that CNTs strongly enhances the tensile strength and Young’s modulus, e.g. 5 wt% SWCNT in PI synthesized at 1 GPa and 513 K showed 2 times higher tensile strength and 2.3 times higher Young’s modulus than that of similarly treated pure PI. The results indicate that the treatment improves the poor interfacial contact between the CNTs and polymer, which is one of the obstacles for achieving stronger CNT composites