Construction of hierarchical defect networks comprising heterointerfaces, vacancies, and heteroatoms for superior microwave attenuation

A phosphorus-doped hierarchical Co₃S₄/NiS₂ encapsulated within nitrogen-doped graphitic carbon is synthesized via a tailored multi-step thermal treatment of NiCo-Prussian blue analogues. The integrated structure combines magnetic components, porous features, and a multilevel defect network (including Co₃S₄/NiS₂ heterointerfaces, sulfur vacancies, and heteroatoms), significantly optimizing impedance matching and electromagnetic (EM) loss capabilities. As a result, the resultant composite achieves a remarkable minimum reflection loss of −72.8 dB at 2.4 mm. To elucidate the intrinsic correlation between the microstructure and macroscopic performance, a multi-scale computational framework integrating first-principles calculations, micromagnetic theory, and finite element analysis is established. This framework systematically reveals how heterointerface engineering, vacancies, and heteroatom doping govern the dielectric polarization, magnetic domain configurations, and overall EM attenuation. This work bridges the gap between microstructure and macroscopic properties via cross-scale theoretical analysis, offering critical guidelines for the rational design of microwave absorption materials (MAMs).