Graphite nanoplatelets (GNPs)—the segregated ultra-high molecular weight polyethylene (UHMWPE)-based composites with hybrid filler—decorated with Fe3O4 were developed. Using X-ray diffraction and scanning electron microscopy, it was shown that the decorated component has the shape of separate granules, or their clusters were distributed evenly over the GNPs surface. The individual Fe3O4 nanoparticles are predominantly rounded, with diameters of approximately 20–60 nm. The use of GNPs/Fe3O4 as a filler leads to significant decreases in the percolation limit ϕc, 0.97 vol% vs. 0.56 vol% for GNPs/UHMWPE- and (GNPs/Fe3O4)/UHMWPE segregated composite material (SCM), respectively. Modification of the GNP surface with Fe3O4 leads to an essential improvement in the electromagnetic interference shielding due to enhanced microwave absorption in the 26–37 GHz frequency range in its turn by abundant surface functional groups and lattice defects of GNPs/Fe3O4 nanoparticles.
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