Atomically dispersed metals on N-doped carbon supports (M–NxCs) have great potential applications in various fields. However, a precise understanding of the definitive relationship between the configuration of metal single atoms and the dielectric loss properties of M–NxCs at the atomic-level is still lacking. Herein, we report a general approach to synthesize a series of three-dimensional (3D) honeycomb-like M–NxC (M = Mn, Fe, Co, Cu, or Ni) containing metal single atoms. Experimental results indicate that 3D M–NxCs exhibit a greatly enhanced dielectric loss compared with that of the NC matrix. Theoretical calculations demonstrate that the density of states of the d orbitals near the Fermi level is significantly increased and additional electrical dipoles are induced due to the destruction of the symmetry of the local microstructure, which enhances conductive loss and dipolar polarization loss of 3D M–NxCs, respectively. Consequently, these 3D M–NxCs exhibit excellent electromagnetic wave absorption properties, outperforming the most commonly reported absorbers. This study systematically explains the mechanism of dielectric loss at the atomic level for the first time and is of significance to the rational design of high-efficiency electromagnetic wave absorbing materials containing metal single atoms.
Nanocarbons with single-metal atoms (M-SAs) have displayed considerable potential in various fields of application due to high free energy of M-SAs and strong metal-support interaction. However, the uniform dispersion of M-SAs within the whole carbon matrix still remains a great challenge. Herein, Ni-SAs are uniformly dispersed within hierarchically porous carbon nanoflowers (Ni-SA/HPCF) via a spatial confinement of Ni ions within the periodic pores in metal-organic frameworks (MOFs) with a subsequent carbonization process. The Ni-SA/HPCF with abundant mesopores and an ultrahigh surface area (1137.2 m 2 g −1 ) exhibits unexpected electromagnetic wave (EMW) absorption property with a minimal reflection loss of -53.2 dB and an effective absorption bandwidth of 5.0 GHz, while the filler ratio in the matrix is merely 10 wt.%. Density functional theory calculations and experimental results reveal that the uniformly dispersed Ni-SAs break local symmetry of the electronic structure and increase electrical conductivity of host carbon matrix, thereby enhancing the EMW absorption properties. In addition, the unique 3D hierarchical porous morphology boosts the impedance matching property, which synergistically improves the EMW absorption performance of the Ni-SA/HPCF. This study provides an efficient approach to uniformly disperse M-SAs within hierarchically porous nanocarbons for EMW absorption and other potential applications.
Herein, we use reduced graphene oxide as a substrate and NiFe as
a catalyst to fabricate three-dimensional (3D) nitrogen-doped carbon
nanotube (NCNT)/reduced graphene oxide heteronanostructures (3D NiFe/N-GCTs).
The 3D NiFe/N-GCTs are composed of two-dimensional (2D) reduced graphene
oxide-supported one-dimensional (1D) NiFe nanoparticle-encapsulated
NCNT arrays. The NCNTs exhibit bamboo-like shapes with the length
and diameter of 3–10 μm and 15–45 nm, respectively.
Besides integration of advantages of 1D and 2D nanomaterials, the
3D NiFe/N-GCT heteronanostructure possesses interconnected network
structures, sufficient interfaces, numerous defects, hundreds of void
spaces enclosed by bamboo joints and the walls of the NCNT in an individual
carbon nanotube, and large surface areas, which can improve their
dielectric losses toward electromagnetic wave. Thus, the 3D NiFe/N-GCTs
show satisfied property toward electromagnetic wave absorption. Typically,
the optimized 3D NiFe/N-GCT displays excellent minimal reflection
loss (−40.3 dB) and outstanding efficient absorption bandwidth
(4.5 GHz), outperforming most of the reported absorbers. Remarkably,
the synthesis of 3D NiFe/N-GCTs only involves vacuum freeze-drying
and subsequent thermal treatment process at a high temperature, and
thus, the large-scale production of 3D NiFe/N-GCTs can be achieved
in each batch, affording the possibility of the practical applications
of the 3D NiFe/N-GCTs.
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