Modulating d‐Band Center via Atomic Doping in Core–Shell Topological Architectures for Efficient Electromagnetic Wave Absorption

ABSTRACT Precisely regulating heterostructure electronic states and interfacial properties is critical for high‐performance electromagnetic wave absorption. This study first proposes a synergistic strategy combining d‐band center modulation and 3D hierarchical hetero‐interface engineering to synthesize transition metal‐substituted flower‐like core–shell structured composites. Using metal glycerate spheres as precursors, transition metal (Zn) is introduced to induce lattice substitution. Electronegativity differences drive charge rearrangement and induce a significant negative d‐band center shift, achieving precise electronic state regulation. Subsequently, combining controlled annealing with an in‐situ hydrothermal strategy realizes the vertical growth of MoNi‐LDH nanosheets on the oxide surface. The strong electronic coupling at these hetero‐interfaces further promotes the negative d‐band center shift. Through synergistic optimization of electronic and hierarchical core–shell structures, the composite achieves a minimum reflection loss of ‐42.18 dB at an ultrathin 2.1 mm matching thickness. Furthermore, an effective absorption bandwidth of 6.32 GHz is achieved at 2.5 mm thickness. Finally, using an electromagnetic energy conversion model and multiphysics simulations, the contribution mechanisms of electronic structure regulation and interfacial polarization to electromagnetic energy dissipation and radar stealth are deeply analyzed, providing precise theoretical guidance for designing novel absorbing materials.