Different
amounts of graphene-wrapped magnesium oxide (G@MgO) powders
are uniformly dispersed in poly(vinyl alcohol) (PVA) solution in different
experiments to obtain solutions which are coagulated to obtain solid
materials, which are then hot pressed at 413 K and 3 t of pressure
to finally obtain 1 mm thick freestanding G@MgO/PVA composite sheets
in which the constituents, namely, graphene and MgO (in the form of
G@MgO), are the nanofillers in PVA matrix. During synthesis of G@MgO
powder, MgO nanoparticles are in situ wrapped by the graphene nanosheets
as revealed by electron microscopy. Uniformity of G@MgO dispersion
in PVA was confirmed by secondary electron micrographs and the consistency
in X-ray diffraction and Raman scattering data collected from different
locations of the samples. Temperature (303–393 K) dependent
complex permittivity of G@MgO/PVA composite sheets (including those
prepared by casting) in low frequency (20 Hz to 2 MHz) and high frequency
(i.e., X-band, 8.2–12.4 GHz) ranges are measured. In both frequency
ranges, G@MgO/PVA composite sheets prepared by coagulation exhibited
dielectric properties superior to those of PVA and G@MgO/PVA composite
sheets prepared by casting. A strong interfacial polarization is observed
in coagulated and as-cast G@MgO/PVA composite sheets. It is noticed
from the calculated activation energies that conduction is the dominating
mechanism for energy transfer in both composite sheets’ cases,
while it is predominating in coagulated composite sheets due to the
better network formation of the fillers in the coagulated samples
than in the cast composite samples. The electromagnetic interference
shielding effectiveness (EMI SE) values in the X-band frequency range
(i.e., 8.2–12.4 GHz) of the G@MgO/PVA composite sheets prepared
by coagulation are more than those prepared by casting for a particular
weight fraction of G@MgO. At 393 K, for a particular G@MgO/PVA composite
sheet prepared by coagulation, an excellent EMI SE of ∼27.5
dB is measured. It is also experimentally elucidated that the absorption
is the dominating mechanism for EMI SE in the prepared composite sheets.