ABSTRACT
High-efficiency electromagnetic (EM) wave (EMW)-absorbing materials have attracted extensive scientific and technical interest. Although identifying the dominant EM loss mechanism in dielectric-loss materials is indispensable, it is challenging due to a complex synergism between dipole/interfacial polarization and conduction loss. Modulation of defects and microstructures can be a possible approach to determine the dominant EM loss mechanism and realize high-efficiency absorption. Herein, 2D reduced graphene oxide (rGO) flakes are integrated into a 3D hollow bowl-like structure, which increases defect sites (i.e., oxygen vacancy and lattice defect) and reduces the stacked thickness of rGO. Despite their lower stacked thicknesses, the hollow rGO bowls with more defects exhibit lower conductivities but higher permittivities. Accompanied by the transformation from 2D flakes to 3D hollow bowls, the dominant EM loss mechanism of rGO transforms from conduction loss to defect-induced polarization. Furthermore, the defect engineering and structural design endow rGO with well-matched impedance and strong EMW-absorbing capacity. A minimum reflection loss of -41.6 dB (1.3 mm) and an effective absorption bandwidth of 4.8 GHz (1.5 mm) is achieved at a filler loading of 5 wt%. This study will provide meaningful insights into the development of materials with superior EMW-absorbing performances via defect engineering and structural design.
ABSTRACT
Although transition metal carbides/carbonitrides (MXenes) exhibit immense potential for electromagnetic wave (EMW) absorption, their absorbing ability is hindered by facile stacking and high permittivity. Layer stacking and geometric structures are expected to significantly affect the conductivity and permittivity of MXenes. However, it is still a formidable task to simultaneously regulate layer stacking and microstructure of MXenes to realize high-performance EMW absorption. Herein, a simple and viable strategy using electrostatic adsorption is developed to integrate 2D Ti3 C2 Tx MXene nanosheets into 3D hollow bowl-like structures with tunable layer stacking thickness. Density functional theory calculations indicate an increase in the density of states of the d orbital from the Ti atom near the Fermi level and the generation of additional electrical dipoles in the MXene nanosheets constituting the bowl walls upon reducing the layer stacking thickness. The hollow MXene bowls exhibit a minimum reflection loss (RLmin ) of -53.8 dB at 1.8 mm. The specific absorbing performance, defined as RLmin (dB)/thickness (mm)/filler loading (wt%), exceeds 598 dB mm-1 , far surpassing that of the most current MXene and bowl-like materials reported in the literature. This work can guide future exploration on designing high-performance MXenes with "lightweight" and "thinness" characteristics for superior EMW absorption.
