Multidimension‐Controllable Synthesis of MOF‐Derived Co@N‐Doped Carbon Composite with Magnetic‐Dielectric Synergy toward Strong Microwave Absorption

Abstract Metal–organic framework (MOF) is highly desirable as a functional material owing to its low density, tunable pore size, and diversity of coordination formation, but limited by the poor dielectric properties. Herein, by controlling the solvent and mole ratio of cobalt/linker, multidimension‐controllable MOF‐derived nitrogen‐doped carbon materials exhibit tunable morphology from sheet‐, flower‐, cube‐, dodecahedron‐ to octahedron‐like. Tunable electromagnetic parameters of Co@N‐doped carbon composites (Co@NC) can be obtained and the initial MOF precursor determines the distribution of carbon framework and magnetic cobalt nanoparticles. Carbonized Co@NC composites possess the following advantages: i) controllable dimension and morphology to balance the electromagnetic properties with evenly charged density distribution; ii) magnetic‐carbon composites offer plenty of interfacial polarization and strong magnetic coupling network; iii) a MOF‐derived dielectric carbon skeleton provides electronic transportation paths and enhances conductive dissipation. Surface‐mediated magnetic coupling reflects the stray magnetic flux field, which is corroborated by the off‐axis electron holography and micro‐magnetic simulation. Optimized octadecahedral Co@NC sample exhibits the best microwave absorption (MA) of −53.0 dB at the thickness of 1.8 mm and broad effective frequency from 11.4 to 17.6 GHz (Ku‐band). These results pave the way to fabricate high‐performance MA materials with balanced electromagnetic distribution and controlled morphology.