Entropy-driven phase regulation of high-entropy transition metal oxide and its enhanced high-temperature microwave absorption by in-situ dual phases

doi:10.1016/j.jmst.2021.11.032

Abstract

Abstract:

High-temperature microwave absorbers are significant for military equipment which experiences severe aerodynamic heat. In this work, high-entropy oxide (HEO) (FexCoNiCrMn)mOn with excellent high-temperature microwave absorption is studied. Driven by the effect of entropy, the composition of the oxide can be transformed from spinel-type phase (FexCoNiCrMn)3O4 to corundum-type phase (FexCoNiCrMn)2O3 with the increasing content of iron. Only spinel-type or corundum-type structure composes the oxide when x ≤ 3 or x ≥ 5. But in-situ dual phases can coexist when x equals 4 during phase transition. Interestingly, obliged to abundant heterogeneous interfaces and crystal defects in the dual-phase HEO, magnetic property, dielectric polarization, and microwave loss ability are all well enhanced. The Smith chart analysis demonstrates the impedance matching condition is well improved due to the enhanced loss ability. These findings pave a new way for the adjustment of electromagnetic properties of HEO by entropy-driven phase regulation. Meanwhile, the dual-phase absorber can achieve better than 90% absorption in 9.6-12.4 GHz at 800 °C with a thickness of 2.6 mm, a low thermal diffusivity of 0.0038 cm2/s at 900 °C, and excellent high-temperature stability, which indicates it's promising as a high-temperature microwave absorber.

Key words: High entropy oxide, In-situ dual phases, High temperature, Microwave absorption

Guohao Dai, Ruixiang Deng, Xiao You, Tao Zhang, Yun Yu, Lixin Song. Entropy-driven phase regulation of high-entropy transition metal oxide and its enhanced high-temperature microwave absorption by in-situ dual phases[J]. J. Mater. Sci. Technol., 2022, 116: 11-21.

Figures/Tables 11

Fig. 1. Preparation procedures of entropy-stabilized (FexCoNiCrMn)mOn.

Fig. 2. XRD patterns of the (a) HEO-1 at different sintering temperatures. (b) HEO-x (x = 1, 2, 3, 4, 5 and 6) sintered at 1050 °C. (c) HEO-1, HEO-4, and HEO-6 after 1000 °C post-annealing.

Fig. 3. SEM images of the (a-c) HEO-1, HEO-4, and HEO-6 without post-annealing, (d-f) HEO-1, HEO-4, and HEO-6 annealed at 700 °C for 12 h, (g-i) HEO-1, HEO-4, and HEO-6 after annealed at 1000 °C for 12 h. (j-p) Distribution of the Fe, Co, Ni, Cr, Mn, and O elements in HEO-4 characterized by EDS.

Fig. 4. (a) TEM image, (b) HRTEM image, and (c) selected-area electron diffraction (SAED) pattern of the composite HEO-4. (d) The corresponding Fast Fourier Transform (FFT) morphology of the (b) HRTEM image.

Fig. 5. The configuration entropy Sconf changing with component.

Fig. 6. The high-resolution XPS spectra of (a-c) O 1s and (d-f) Fe 2p for HEO-1, HEO-4, and HEO-6.

Fig. 7. (a-c) 3D plots of reflection loss for HEO-1, HEO-4, and HEO-6 at different thicknesses. (d) The reflection loss of HEO-1, HEO-4, and HEO-6 when thickness equals 10 mm.

Fig. 8. (a) The reflection loss of composite HEO-4 after annealing at 700 °C and 1000 °C for 10 h in the air. (b, c) Microwave absorption of the HEO-4 by in-situ measurement at 800 °C. (d) Measured thermal diffusivity of the high-entropy oxides.

Table 1. Comparison of microwave absorption with other similar absorbers.

Material	Temperature	Absorption bandwidth	Refs.
FeCoNiAlCr_0.9 alloy	Room temperature	9.3-13.58 GHz	[26]
HERSC-3	Room temperature	13.5-18 GHz	[35]
HE REB₆/HE REBO₃	Room temperature	13.6-17.5 GHz	[46]
CNTs/ZnO	in-situ 400 °C	9.2-12.4 GHz	[61]
SiBCN	in-situ 600 °C	8.9-12.4 GHz	[36]
SiC/Si₃N₄	in-situ 800 °C	9.78-11.69 GHz	[5]
HEO-4	in-situ 800 °C	9.6-12.4 GHz	This work

Fig. 9. Frequency dependence of the (a) complex permittivity and (b) complex permeability. Hysteresis loops of HEO-1, HEO-4, and HEO-6 at 300 K (c) under the applied magnetic fields up to 10,000 Oe and (d) under the applied magnetic fields up to 1000 Oe.

Fig. 10. The input impedance of (a) HEO-1, (b) HEO-4, and (c) HEO-6 showed by the Smith chart (frequency range is 2-18 GHz and thickness is 10 mm). (d) Attenuation constant of the three composites. (e) Evaluation process and microwave absorbing mechanisms of the dual-phase coexistence HEO.

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