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Metal–organic frameworks (MOFs) have diverse structures and compositions, inspiring the boundless enthusiasm and creativity of researchers in the field of electromagnetism. The synthesis of MOF-derived nanomaterials for electromagnetic wave (EMW) absorption with ultrathin matching thickness (below 1.6 mm) is highly desired and challenging. Here, we demonstrate a general synthesis strategy for metal (Co, Ni, Fe)-based MOFs, which transformed into metal/metal-oxide nanoparticles (NPs) of being coated by nitrogen (N)-doped graphitized carbon. The obtained carbon-coated NPs show excellent EMW absorption properties. Specifically, Co-based MOFs are pyrolyzed into rhombic dodecahedrons with numerous ultrasmall Co NPs coated by N-doped carbon (Co-NC core–shell NPs). The synthesized Co-NC core–shell NPs possess a unique porous structure, abundant defects, and doped N heteroatoms, resulting in good magnetic loss (eddy current loss), dielectric loss (multiple reflections, interfacial polarization, conduction loss), and impedance matching. Therefore, the Co-NC core–shell NPs exhibit an excellent EMW absorption property with a very strong reflection loss of −56.5 dB at a matching thickness of only 1.58 mm. The effective absorption bandwidth (EAB) is 4.4 GHz. In addition, the EAB between 1 and 5 mm in thickness is up to 13.2 GHz, which already includes all C bands and X bands, even the absolute S bands and Ku bands. This work provides an avenue to design high-performance EMW absorption devices based on MOF-derived nanomaterials.

Constructing the strong interaction between the matrix and the active centers dominates the design of high-performance electromagnetic wave (EMW) absorption materials. However, the interaction-relevant absorption mechanism is still unclear, and the design of ultrahigh reflection loss (R L < −80 dB) absorbers remains a great challenge. Herein, CoFe-based Prussian blue (PB) nanocubes are coprecipitated on the surface of ultrathin CoAl-LDH nanoplates with the assistance of unsaturated coordination sites. During the subsequent pyrolysis process, CoAl-LDH serves as a “ligand” providing a Co source and reacts with Fe or C in the CoFe-PB “host” to form stable CoFe alloys or CoC x species. As a result, strong reactions emerged between the CoAl-LDH matrix and the active CoFe-CoC x @NC centers. Based on the experimental results, the CoAl/CoFe-CoC x @NC hierarchical heterostructure delivers good dielectric losses (dipolar polarization, interface polarization, and conductive loss), magnetic losses (eddy current loss, natural resonance, and exchange resonance), and impedance matching, resulting in a remarkable EMW absorption performance with a reflection loss (R L) value of −82.1 dB at a matching thickness of 3.8 mm. Theoretical results (commercial CST) identify that the strong interaction between the 2D CoAl-LDH “ligand” and 2D CoFe-CoC x “host” promotes a robust heterointerface among the nanoparticles, nanosheets, and nanoplates, which extremely contribute to the dielectric loss. Meanwhile, the coupling effect of nanosheets and nanoplates greatly contributes to the matching performance. This work provides an aggressive strategy for the effect of ligands and hosts on high-performance EMW absorption.

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