Solid-state reaction induced defects in multi-walled carbon nanotubes for improving microwave absorption properties

doi:10.1016/j.jmst.2021.08.051

Abstract

Abstract:

Dielectric polarization performance induced by defect engineering approach has been proved to be an effective way for improving the microwave absorption property of carbon-based materials. Assisting by the solid-state reaction, the structural integrity of multi-walled carbon nanotubes (MWCNTs) would be broken along with the volume expansion and etching process of cobalt oxides. Therefore, the defects could be obtained and result in the enhancement of microwave absorption property. Ascribing to the broken wall structures, the defect-distances (L_D) and concentrations (n_D) have been optimized to be 9.80 nm and 3.37 × 10¹¹ cm^-2. The minimum reflection loss (RL) had reached -54.6 dB at 4.5 GHz with a thickness of 4.13 mm and the corresponding effective absorption bandwidth (EAB_{<-10 dB}) was analyzed to be 14.6 GHz. Such enhancement is correlated to the dielectric polarization and the permeability-to-permittivity transformation raised from the defect structures and concentrations. The present work demonstrates an effective strategy for tailoring the microwave absorption property of MWCNTs by engineering defect concentrations, and could be further extended to other carbon-based absorbents.

Key words: MWCNTs, Defect engineering, Microwave absorption, Solid-state reaction, Impedance matching

Tong Gao, Zhengyu Zhang, Yixing Li, Yujuan Song, Huawei Rong, Xuefeng Zhang. Solid-state reaction induced defects in multi-walled carbon nanotubes for improving microwave absorption properties[J]. J. Mater. Sci. Technol., 2022, 108: 37-45.

Figures/Tables 10

Fig. 1. Schematic illustration of the synthesis process of DE-MWCNTs, exhibiting the transformation process of solid-state reaction.

Fig. 2. Phase component characterizations (XRD) of different MWCNTs: (a) CoO on MWCNTs after reduction reaction, (b) Co3O4 on MWCNTs after oxidation reaction, (c) DE-MWCNTs after removing Co3O4 by H2SO4.

Fig. 3. Microstructure characterizations (TEM) of different MWCNTs: (a-d) CoO on MWCNTs after reduction reaction, (e-h) Co3O4 on MWCNTs after oxidation reaction, (i-l) DE-MWCNTs after removing Co3O4 by H2SO4.

Fig. 4. High-resolution TEM images of DE-MWCNTs, which is employed to illustrate the nanoscale structural defects creating via the solid-state reactions.

Fig. 5. Raman spectra of MWCNTs with different raw material weight ratio (1:1, 1:5, and 1:10). (a)-(c) CoO-MWCNTs, (d)-(f) Co3O4-MWCNTs, (g)-(i) DE-MWCNTs.

Fig. 6. Electromagnetic parameters of original-MWCNTs, CoO-MWCNTs, Co3O4-MWCNTs, and DE-MWCNTs: (a) real part of the relatively complex permittivity, (b) imaginary part of the relatively complex permittivity, (c) dielectric loss factor plots, (d) real part of the relatively complex permeability, (e) imaginary part of the relatively complex permeability, (f) magnetic loss factor plots.

Fig. 7. Plots of ε′ vs B0 (B0=ε′′/f) of four samples: (a) original- MWCNTs, (b) CoO-MWCNTs, (c) Co3O4-MWCNTs, (d) DE-MWCNTs, (e) k values of four samples.

Fig. 8. Three-dimensional reflection loss mapping, corresponding contour plots, and microwave absorbing performances of original-MWCNTs, CoO-MWCNTs, Co3O4-MWCNTs, and DE-MWCNTs: (a-d) 3D plots of microwave absorption (RL), (e-h) microwave absorption (RL) versus frequency, (i-j) effective bandwidth and minimum RL at different thicknesses.

Table 1. Comparison of electromagnetic wave absorption performances.

Sample	Electromagnetic wave absorption properties RL (min)	EAB	f (min)
DE-MWCNTs	-54.6	14.6	4.5
Fe₂O₃/Fe₃O₄/ MWCNTs	-44.1	3.3	10.4
ZnO@MWCNTs@NiFe₂O₄	-45.5	5.4	12.4
MWCNTs/AlN	-47.34	3.28	9.12
CoFe₂O₄/C/PANI	-51.81	8.88	12.4
C@Fe₂O₃@MWCNTs	-49.9	15	10
RGO/MWCNTs/CeO₂	-59.3	3.2	4.6
Ni@C-ZIF	-86.8	7.4	13.2
NiSe/C	-59.7	4.67	7.89

Fig. 9. Electrical conductivity and impedance matching calculations of original-MWCNTs, CoO-MWCNTs, Co3O4-MWCNTs, and DE-MWCNTs: (a) I-V curve and R-V curve, (b) attenuation constant α, (c)-(f) impedance matching degree Δ dependence of frequency.

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