Carbon nanofiller/polymer nanocomposites: Diffusion, mechanical and electrical properties

Since the discovery two decades ago, fullerene family has drawn remarkable attention because of their unique electrical, thermal, optical, mechanical and flammable properties. They have been widely used to improve polymer properties. These nanofillers produce huge interfacial areas between the polymer and the fillers. Despite the intensive research on fullerene nanocomposites, understanding of the importance of the filler-polymer interface is still limited and further investigation of the structure-property relationships is needed. This dissertation probed influence of nanoparticles on polymer tracer diffusion and molecular weight dependence of composite mechanical properties, and developed a coated particle process to obtain composites with high electrical conductivity.;Deuterated polystyrene (dPS) diffusion in nanoparticle/polystyrene (PS) nanocomposites was measured by an elastic recoil detection method. We used single wall carbon nanotubes (SWCNTs), multiwall carbon nanotubes (MWCNTs) and C60 as nanofillers and found that the nanofillers have a significant influence on polymer tracer diffusion. When the tracer molecules ( Rg) are larger than the fillers ( RCNT), the tracer diffusion coefficient exhibits a minimum as a function of filler concentration. In contrast, the tracer diffusion in nanocomposites is constant when the tracer chains are smaller than the fillers. A trap model simulation was developed to understand the minimum diffusion coefficient.;The load transfer mechanism from polymer matrix to fillers were studied by tensile testing and Raman spectroscopy in SWCNT/poly(methyl methacrylate) (PMMA) nanocomposite fibers. Without strong filler-polymer interactions, effective load transfer is limited to small strains, and Raman peak shift and stress-strain curve of composite fibers are reversible, suggesting an elastic deformation. Beyond this strain region, the load transfer is nonlinear because of a slippage at the polymer-filler interface. The stress on nanotubes reaches a maximum and then decreases with further increase in the strain.;A coated particle process (CPP) method was developed to prepare nanocomposites with a cellular filler structure. The fillers are SWCNTs and PMMA is used as polymer matrix. Compared with the coagulated nanocomposites with well dispersed SWCNTs, the CPP-made nanocomposites have a higher electrical conductivity (2 orders higher), a smaller percolation threshold (50%).