In this work, the synergistic effect of graphene nanosheets (GNs), as well as multiwalled carbon nanotubes (MWCNTs), as reinforcing agents of polydimethylsiloxane (PDMS) was investigated, in order to explore the possibilities of designing composite materials, tailored for use in the field of coatings, which might be, in fact, a very interesting application. It was shown that the addition of GNs and MWCNTs in PDMS matrices significantly improves the thermal stability of the obtained nanocomposites, especially those reinforced exclusively with GNs. The tensile tests indicated that strength increased for all the examined composites. It was also observed that the Young’s moduli had an increasing trend, with the exception of the composites containing only GNs, while those reinforced solely with MWCNTs exhibited the best performance. The O2 permeability measurements revealed that the highest reduction in the permeability was observed in GN-MWCNT/PDMS composite membranes, in comparison to those reinforced only with graphene or carbon nanotubes. Dielectric relaxation spectroscopy showed that all the examined composites, and especially those of MWCNTs, possess electrical conductivity, apart from the samples reinforced exclusively with graphene. The electromagnetic shielding effectiveness was also improved at higher filler loadings, which is more evident in composites reinforced with MWCNTs. It was concluded that the improved properties of the above studied hybrid composites make them suitable for protective coating applications.
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