Tuning Dielectric-Magnetic Synergy in (Fe/TiC)@C Nanocomposites via Phase Composition Control for Broadband Microwave...

The development of cost-effective and resource-rich materials is crucial for the practical application of microwave absorbers. This study demonstrates the successful fabrication of core-shell Fe and TiC nanoparticles encapsulated within carbon shells using the arc discharge method. The samples are designated as Fe3Ti1 and Fe1Ti3, where the numbers indicate the Fe-to-Ti mass ratio in the precursor (e.g., Fe1Ti3 = 1:3 by mass). In the arc discharge synthesis mechanism, the mass ratio of Fe to Ti in the raw material was adjusted from 3:1 to 1:3 to optimize the Fe/TiC/C interfaces under a CH₄ forming gas atmosphere. TEM analysis reveals spherical and polyhedral nanoparticles with diameters of 30-50 nm and a uniform carbon shell thickness of 3-4 nm. Raman spectroscopy shows that the Fe1Ti3 sample has a higher defect density (I_D/I_G = 1.13) compared to Fe3Ti1 (0.87), indicating a more disordered carbon structure. Magnetic measurements yield saturation magnetization values of 87 emu/g for Fe3Ti1 and 50 emu/g for Fe1Ti3, with coercivities of 190.72 Oe and 203.65 Oe, respectively. When composited with paraffin at 50 wt% loading, the Fe1Ti3 sample exhibits superior microwave absorption performance, achieving a minimum reflection loss (RL) of -25.22 dB at 8.23 GHz and an effective absorption bandwidth (RL ≤ -10 dB) of 4 GHz (6.5-10.5 GHz) at a thickness of 2.5 mm. This enhanced performance is attributed to the synergistic effect of multiple loss mechanisms, including conduction loss within the three-dimensional core-shell architecture, interfacial polarization at the heterojunctions between the core and the carbon shell, and magnetic loss induced by ferromagnetic behavior associated with defects in both the shell and carbon atomic layers. The magnetic loss in the (Fe/TiC)@C nanocomposites primarily arises from the natural resonance (at ~6.5 GHz) and exchange resonance (at ~12 GHz) of the Fe cores. The dielectric loss is primarily attributed to dipole, interfacial, and space charge polarization from TiC and the carbon shell, as well as multiple scattering effects between nanoparticles. Furthermore, far-field radar cross-section simulations substantiate that the Fe/TiC@C nanocomposite demonstrates excellent radar wave attenuation capability. Further, first principles simulations reveal that introducing Fe at the C/TiC interface induces strong charge redistribution and orbital hybridization, transforming a localized dielectric interface into a highly conductive and electronically coupled C/Fe/TiC system. This interfacial modulation enhances both dielectric loss (via charge transport and polarization) and magnetic loss (via Fe-induced magnetic interactions), thereby enabling optimized dielectric-magnetic synergy for broadband microwave absorption in (Fe/TiC)@C nanocomposites.