Enhanced Dielectric Loss Induced by Asymmetrically Coordinated Iron Single‐Atoms with Curved Configurations on Turing‐Like Surfaces for Electromagnetic Wave Absorption

Abstract Curved support can significantly change the electronic structure of a metal single‐atom (M‐SA) and thereby fine tune its intrinsic physicochemical properties. However, constructing asymmetrically coordinated M‐SAs on highly curved supports remains challenging. Here, an efficient strategy driven by the different thermal decomposition rates of two polymers is proposed to create Turing surface with highly curved stripes on hollow carbon spheres (HCSs) for anchoring asymmetrically coordinated Fe‐N 3 S 1 moieties. Experimental and theoretical calculation results reveal that asymmetric Fe‐N 3 S 1 atoms and the strain of Fe─N bonds induced by the highly curved Turing surface efficiently break the symmetric distribution of the charge around the Fe atoms and significantly enhance the dielectric loss of the HCSs, thereby synergistically improving the electromagnetic wave absorption property. Remarkably, the film constructed with Fe‐N 3 S 1 ‐anchored HCSs and natural rubber exhibits a wide effective absorption bandwidth of 7.68 GHz at a filling ratio of 6%. Moreover, the film also possesses excellent hydrophobicity, frost‐resistant ability, adhesiveness, flexibility, stretchability, and heat‐dispersion ability, which expand its practical applications into various environments. This work provides insights into the synergistic effects of asymmetrically coordinated configurations and curved supports of M‐SAs on their dielectric properties and offers a new method for the preparation of multifunctional films.