Interfacial Bonding Induced d‐p‐π Orbital Coupling to Drive Electron Migration for High‐Efficiency Microwave Absorption

ABSTRACT Heterointerface and heteroatom doping are effective strategies for enhancing microwave absorption (MA) through regulating electronic structure. Here, a series of N‐doped V 2 O 3 /C composites were synthesized, and a strategy was proposed to enhance MA performance by interfacial coupling between orbitals and π bonds. Specifically, heteroatoms N partially substituted O and C atoms to form N─V and C─N (Pyrrole N) bonds, and their relative proportions adjusted the d‐p‐π orbital coupling strength at the heterointerface among d orbital of V, p orbital of pyrrole N, and delocalized π bond of pyrrole. It efficiently regulated the electron migration efficiency from the p orbital and delocalized π‐bond to the d orbital of V, which not only formed a conjugated conductive network but also generated a large number of dipoles. Benefiting from enhanced conduction and polarization loss due to interface bonding, as well as dipole polarization induced by oxygen vacancy, the 2NVOC achieved the minimum reflection loss of −55.4 dB and effective absorbed bandwidth of 5.49 GHz at loading mass of 10 wt.%. In addition, the derived carbon also imparted the absorbers with outstanding corrosion resistance. This work provides a new idea for the design of absorbers at the atomic scale.