Synthesis of hierarchical core-shell NiFe2O4@MnO2 composite microspheres decorated graphene nanosheet for enhanced microwave absorption performance
Introduction
With the rapid development of radar detection techniques, electromagnetic (EM) wave absorption materials with strong EM wave absorption and wide-absorbing frequency, have drawn much attention from scientists in the civil and military fields [1], [2], [3]. EM wave absorption materials can convert the EM wave into thermal energy for consumption [4]. According to EM wave absorption principle, the radar absorbers can be divided into dielectric materials, such as graphene [5], [6], [7], conducting polymers [8], [9], [10], and carbon nanotubes [11], [12], and magnetic materials such as Fe3O4 [13], [14], [15], NiFe2O4 [16] and CoFe2O4 [17]. As an outstanding carbon material, graphene is used in various kinds of fields owing to its unique chemical and physical properties [18], [19]. Due to its low density, high permittivity and ease of functionalization, it has been investigated thoroughly as an EM wave absorption material. However, the impedance mismatching of materials with high electrical conductivity may hinder the EM waves from entering into the materials and result in weak absorption and strong reflection [20], which is not beneficial for the attenuation of EM energy. Generally, several types of magnetic materials have been introduced into graphene to decrease the complex permittivity [21]. For instance, Zong et al. synthesized a reduced graphene oxide-CoFe2O4 composite and it can reach −44.1 dB at 15.6 GHz, which is ascribed to proper impedance matching and electromagnetic wave attenuation [22]. A minimal reflection loss of −30 dB could be achieved by coupling hollow Fe3O4-Fe with graphene composite, at the thickness range of 2–5 nm [23]. Urchinlike Ni/reduced graphene oxide composite displayed the maximum reflection loss of −32.1 dB with an optimal thickness of 2 mm, due to the multi-interfaces, polarization relaxation and synergistic effect [24].
Furthermore, composite microspheres with magnetic core and dielectric shell possess a favorable impedance matching and synergistic effect between permeability and permittivity because of the special core-shell structure [25]. Also, porous composites with hierarchical structure have attracted increasing attention, because the special structure not only enhances the multiple scattering and absorption of EM wave but also decreases the weight of materials. More importantly, the presence of defects from pores and cracks can act as polarized centers and enhance the charge polarizations, bringing about the improvement of EM wave absorption performance [26].
These previous researches inspired this study on developing improved EM absorbers. In this work, a three-dimensional porous composite with NiFe2O4 core and MnO2 shell decorated graphene was synthesized via hydrothermal method. As-prepared NiFe2O4@MnO2 composite possesses higher specific surface area and properer impedance matching compared with NiFe2O4 particles. Furthermore, NiFe2O4@MnO2@graphene composite possesses the largest permittivity and can convert EM wave into thermal energy, which is helpful for EM wave absorption performances. Investigations of EM wave absorption properties demonstrate that NiFe2O4@MnO2@graphene composite displays the strongest reflection loss of −47.4 dB at 7.4 GHz with the thickness of 3 mm. The enhanced EM wave absorption mechanism of the NiFe2O4@MnO2@graphene composite was also studied in detail.
Section snippets
Synthesis of NiFe2O4@MnO2@graphene composite
NiFe2O4 particles were prepared by a similar procedure as a previous literature [27]. Subsequently, the NiFe2O4@MnO2@graphene composite was synthesized by one-pot hydrothermal method. Briefly, graphene oxide was dissolved in KMnO4 aqueous solution (1 mg/mL) and the as-obtained NiFe2O4 particles (0.3 g) were dispersed in the 0.11 mol/L KMnO4 (80 mL) solution. The above solution was placed in an ultrasonic bath for 30 min to disperse NiFe2O4 particles well. Then, HCl (5 mL) was added drop-wise to the
Results and discussion
The crystal structure of NiFe2O4@MnO2@graphene composite was analyzed by XRD and the results are shown in Fig. 1. The diffraction peaks located at 12.1° and 24.6° can be ascribed to (0 0 1) and (0 0 2) planes of MnO2 phase (JCPDS No. 80-1098) [25]. Moreover, the peaks at 30.2°, 35.9°, 43.3°, 57.6° and 62.9° correspond to the (2 2 0), (3 1 1), (4 0 0), (5 1 1) and (4 4 0) planes of cubic spinel NiFe2O4 (JCPDS No. 10-0325) and no other impurity peaks can be detected [27]. The morphologies and
Conclusion
In summary, a hierarchical 3D NiFe2O4@MnO2@graphene composite was synthesized successfully via a facile method. The NiFe2O4 particles were firstly obtained, and then MnO2 nanosheet arrays grew around the NiFe2O4 particles and distributed on the surface of graphene by one-pot hydrothermal method. The introduction of MnO2 and graphene results in a high attenuation constant and proper impedance matching of the sample. The maximum reflection loss of NiFe2O4@MnO2@graphene composite is −47.4 dB at 7.4
Acknowledgements
The authors acknowledge the financial support from the National Natural Science Foundation of China (Grant No 51303147 and No 51502233), President's Fund of Xi’an Technological University (project No. XAGDXJJ16002) and Natural Science Foundation of Shaanxi Provincial Department of Education (16JK1367).
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