Coupling between the 2D "Ligand" and 2D "Host" and Their Assembled Hierarchical Heterostructures for Electromagnetic Wave Absorption

Constructing the strong interaction between the matrix and the active centers dominates the design of highperformance 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 CoCx species. As a result, strong reactions emerged between the CoAl-LDH matrix and the active CoFe-CoCx@NC centers. Based on the experimental results, the CoAl/CoFe-CoCx@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-CoCx "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.