This thesis is concerned with the development of high performance ultrahigh molecular polyethylene (UHMWPE) fibers reinforced using multiwalled carbon nanotubes (MWCNTs). A novel process has been developed, whereby, MWCNT/UHMWPE nanocomposite fibers with Young's modulus up to 137 GPa and tensile strength of ~4.2 GPa has been produced. This fiber possesses the best specific mechanical properties amongst all current commercial high performance fibers. Systematic investigations were carried out to elucidate the mechanisms of reinforcement....[ Read more ]

This thesis is concerned with the development of high performance ultrahigh molecular polyethylene (UHMWPE) fibers reinforced using multiwalled carbon nanotubes (MWCNTs). A novel process has been developed, whereby, MWCNT/UHMWPE nanocomposite fibers with Young's modulus up to 137 GPa and tensile strength of ~4.2 GPa has been produced. This fiber possesses the best specific mechanical properties amongst all current commercial high performance fibers. Systematic investigations were carried out to elucidate the mechanisms of reinforcement.

Firstly, systematical experimental studies were carried out to investigate the CNT reinforcing effect on nanocomposite fibers prepared with different PE molecular orientations. The overall effect can be classified into three regions. At low molecular orientation levels, the CNTs act to toughen and strengthen the nanocomposites. At the intermediate molecular orientations, the CNTs have negligible effects on the mechanical properties of the nanocomposites. At very high molecular orientations, the CNTs act to mainly stiffen and strengthen the nanocomposite.

Secondly, systematic investigations were carried out to investigate the structure evolution as well as the load transfer between the embedded CNTs and that of the matrix PE. Thermal and morphological studies demonstrate that CNTs act as effective nucleation sites for PE crystal growth. The load transfer mechanisms in both the low and high molecular orientation fibers are similar. Major differences were related to CNT alignment effects. The highly oriented fibers show CNT alignment effect in the initial elastic regime, whereas the CNTs in the fibers of low molecular orientations show no appreciable alignment in the elastic regime.

Finally, based on the experimental observations, a mechanistic model has been proposed to elucidate the reinforcement mechanisms. This model proposes that there exists an absorption layer surrounding CNTs. The thickness of this layer decreases as fiber molecular orientation increases. The chain mobility of the molecules inside this absorption layer is higher than those in the bulk. Consequently, at low molecular orientation levels, significant toughening effects are attributed to the molecular orientational development within this layer. This oriented structure acts as a load transfer interface which eventually leads to the alignment of CNTs inside the composite and hence the producing the strengthening effects. At very high molecular orientation levels, this absorption layer mainly acts as a highly deformable cushion to relieve local stress concentrations and transfers the load from the matrix to the CNTs. Efforts were also made to simulate the interfacial shear stresses using molecular dynamics simulations.