Blending of two or more immiscible polymers is an attractive route to generate new materials. However, during processing in the liquid state, the flow-induced microstructure changes continuously due to a complex interplay between break-up and coalescence, typically resulting in a coarse morphology with poor properties. Hence, the need to generate and stabilize a fine morphology is obvious and block copolymers are typically used as compatibilizers. The use of nanoparticles has been suggested to be an alternative to ‘compatibilize’ immiscible polymer pairs. In the present work, the role of interfacially located nanoparticles on the coalescence in immiscible blends is investigated systematically to clarify their role as compared to that of block copolymers. A (70/30 vol%) polydimethylsiloxane (PDMS)/polyisobutylene (PIB) blend with a droplet/matrix microstructure is chosen as a model system. Contact angle measurements and theoretical models are used to select the surface chemistry of the nanoparticles to ensure their localization at the polymer/polymer interface, which is experimentally verified by scanning microscopy under cryogenic conditions. Using a rheological method it is shown that coalescence of the dispersed phase is slowed down or even totally suppressed when nanoparticles are present at the interface. This effect becomes stronger when the particle concentration is increased or the (aggregate) size is reduced. Additionally, anisotropic nanoparticles tend to stabilize blends more efficiently than their spherical counterparts. A combination of optical microscopy and interfacial rheometry using planar interfaces has been used to demonstrate that the nanoparticles mainly affect the surface rheological properties, whereas traditional compatibilizers also strongly affect the interfacial tension. As a result, nanoparticles with a suitable surface chemistry can be used to tune the flow-induced microstructure of immiscible polymer blends by optimizing their concentration, size and shape.
The effect of the reduction method to prepare reduced graphene oxide (rGO) on the melt linear viscoelastic properties, electrical conductivity, polymer matrix crystalline behavior and dielectric properties of PEO-rGO nanocomposites was investigated. Reduction was performed chemically with either sodium borohydride (NaBH4) or hydrazine monohydrate (N2H4·H2O) or both reduction agents consecutively as well as thermally at 1000 °C. The different reduction methods resulted in exfoliated rGO sheets with different types and amounts of remaining functional groups, as indicated by FT-IR, Raman, TGA and XRD characterization. Moreover, their electrical conductivity ranged between 10−4 and 10−1 S/cm, with the consecutive use of both chemical reduction agents being far superior. PEO nanocomposites with filler loadings of 0.5 wt %, 1 wt % and 2 wt % were prepared by solvent mixing. The rGO fillers affected the melt linear viscoelastic and crystalline behavior of the PEO matrix and resulted in nanocomposites with a substantially increased electrical conductivity. Despite the wide variability in filler conductivity, the effects on the polymer nanocomposite properties were less distinctive. A correlation was obtained between the reduction of the mobility of the polymer chains (evaluated by the glass transition temperature) and the dielectric strength of the interfacial polarisation originating from the effective entrapment of GO/rGO filler charges at the interface with the less conductive PEO. Thus, favorable interactions of the polar PEO with the filler led to reduced mobility of the PEO chains and thereby a more effective entrapment of the filler charges at the PEO interface.