Phase and Valence State Engineering of MOFs-Derived Iron Oxide@Carbon Polyhedrons for Advanced Microwave Absorption

MOFs-derived magnetic carbon-based composites are considered to be valuable materials for the design of high-performance microwave absorbents. Regulating phase structures and introducing mixed-valence states within the composites is a promising strategy to enhance their charge transfer properties, resulting in improved microwave absorption performance. In this study, iron oxide components show a temperature-dependent phase evolution process (α-Fe₂O₃→Fe₃O₄→Fe₃O₄/FeO), during which the valence states of iron ions are regulated. The tunable phases modulate the magnetic Fe₃O₄ component, resulting in enhanced magnetic loss. The changed valence states affect the polarization relaxation by adjusting the electronic structure and tune the electron scattering by introducing defects, leading to enhanced dielectric loss. The microwave absorption properties of iron oxide@carbon composites display phase- and valence state-dependent characteristics. Especially, Fe₃O₄@C composites exhibit superior microwave absorption properties, ascribed to the improved magnetic/dielectric losses induced by good impedance matching and strong microwave attenuation capacity. The minimum reflection loss of Fe₃O₄@C composites reaches -73.14 dB at 10.35 GHz with an effective absorption bandwidth of 4.9 GHz (7.69-12.59 GHz) when the absorber thickness is 2.31 mm. This work provides new insights into the adjustment of electromagnetic parameters and microwave absorption properties by regulating the phase and valence state.