Rutile TiO₂ Nanoparticles Encapsulated in a Zeolitic Imidazolate Framework-Derived Hierarchical Carbon Framework with Engineered Dielectricity as an Excellent Microwave Absorber

Aiming to solve the poor response of titanium dioxide (TiO 2 ) in the microwave frequency, versatile series of N-doped carbon (NC) components are employed to improve the conductivity and polarization strength of TiO 2 -based composites. The bimetallic zeolitic imidazolate framework-derived TiO 2 @NC complex (TNC-3) exhibits hierarchical microstructures and large-scale hetero-interfaces, whereas the pyrolysis composite of metal–polydopamine-coated TiO 2 (TNC-4) possesses the vesicle-like NC shell and bulk TiO 2 core. Thus, the optimal reflection loss and efficient absorption bandwidth of TNC-3 realize −44.0 dB at 3.0 mm and 5.4 GHz at only 2.0 mm of coating thickness, respectively. Nevertheless, the corresponding attenuation ability of TNC-4 is separately −24.3 dB and 4.8 GHz with a thickness of 5.0 and 2.0 mm, respectively. Importantly, the conduction and polarization loss can be enhanced by the large-scale interfacial contacts between nanoscale rutile nanoparticles and hierarchical graphitized carbon. Meanwhile, the superior performance of TNC-3 stems from the large proportion of pyridinic N and pyrrolic N, which provides asymmetric lone pairs to strengthen the dipole rotation. These results are of great value in constructing semiconductor-based complexes by carbon-coating engineering as functional materials.