In Situ Exsolution-Prepared Solid-Solution-Type Sulfides with Intracrystal Polarization for Efficient and Selective...

The excellent dielectric properties and tunable structural design of metal sulfides have attracted considerable interest in realizing electromagnetic wave (EMW) absorption. However, compared with traditional monometallic and bimetallic sulfides that are extensively studied, the unique physical characteristics of solid-solution-type sulfides in response to EMW have not been revealed yet. Herein, a unique method for preparing high-purity solid-solution-type sulfides is proposed based on solid-phase in situ exsolution of different metal ions from hybrid precursors. Utilizing CoAl-LDH/MIL-88A composite as a precursor, Fe_0.8Co_0.2S single-phase nanoparticles are uniformly in situ formed on an amorphous substrate (denoted as CoAl), forming CoAl/Fe_0.8Co_0.2S heterostructure. Combing with density functional theory (DFT) calculations and wave absorption simulations, it is revealed that Fe_0.8Co_0.2S solid solution has stronger intracrystal polarization and electronic conductivity than traditional monometallic and bimetallic sulfides, which lead to higher dielectric properties in EM field. Therefore, CoAl/Fe_0.8Co_0.2S heterostructure exhibits significantly enhanced EMW absorption ability in the low-frequency region (2-6 GHz) and can achieve frequency screening by selectively absorbing EMW of specific frequency. This work not only provides a unique method for preparing high-purity solid-solution-type sulfides but also fundamentally reveals the physical essence of their excellent EMW absorption performance.