Currently,
the microwave absorption materials with high absorbing
efficiency are in urgent need to reduce electromagnetic pollution.
Herein, the ZnFe2O4@SiO2 core–shell
microspheres were synthesized and combined with reduced graphene oxide
(RGO) to form the ingenious hierarchical composites (ZnFe2O4@SiO2@RGO), which were used as wave absorbing
functional nanofillers of semicrystalline polyvinylidene fluoride
(PVDF) matrix. The microstructure and crystallization behavior of
ZnFe2O4@SiO2@RGO/PVDF composite membranes
were systematically analyzed. The addition of ZnFe2O4@SiO2@RGO nanofillers facilitated the formation
of β-phase crystal of PVDF, and the transition from β-phase
to α-phase of PVDF occurred when the processing temperature
increased. The effects of the crystallization behavior of the PVDF
matrix on the microwave absorption performance were investigated in
detail. The wave absorbing properties of the resulting composites
can be effectively regulated by changing the processing temperature,
sample thickness, and nanofiller content. The heterogeneous interfaces
(ZnFe2O4–SiO2, SiO2–RGO, and RGO–PVDF) also contributed to the wave absorption
performance. The optimal reflection loss (RL) of ZnFe2O4@SiO2@RGO/PVDF composite membranes with a thickness
of only 1.6 mm can reach −49.8 dB with 10 wt % nanofiller content
when the processing temperature is 60 °C. The strong wave absorption
function of the composite system can be attributed to the synergy
of good impedance matching, interfacial polarization, dipole polarization,
eddy current loss, and ferromagnetic resonance loss under the optimal
process conditions.