硅酸盐学报

尖晶石/岩盐型（Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2）Co_xO_y高熵陶瓷的制备与吸波性能

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王中义 ¹ , 任玉美 ¹ , 杨帅 ¹ , 席通 ¹ , 郭晓琴 ¹ , 赵彪 ² , 张锐 ¹^,³

硅酸盐学报 | 研究论文 2025,53(3): 647-657

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硅酸盐学报 |研究论文 2025 , 53 (3) : 647 -657

尖晶石/岩盐型（Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2）Co_xO_y高熵陶瓷的制备与吸波性能

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王中义¹, 任玉美¹, 杨帅¹, 席通¹, 郭晓琴¹, 赵彪², 张锐¹^,³

作者信息

^1．郑州航空工业管理学院材料学院，郑州 450046

^2．复旦大学微电子学院，上海 200433

^3．河南省科学院，郑州 450046

通讯作者:

任玉美（1987—），女，博士，副教授。

赵彪（1988—），男，博士，副教授。

作者简介:

王中义（1999—），男，硕士研究生。

Preparation and Microwave Absorption Properties of Spinel/Rock Salt (Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2)Co_xO_y High-Entropy Ceramics

Zhongyi WANG¹, Yumei REN¹, Shuai YANG¹, Tong XI¹, Xiaoqin GUO¹, Biao ZHAO², Rui ZHANG¹^,³

Affiliations

^1.School of Material, Zhengzhou University of Aeronautics, Zhengzhou 450046, China

^2.School of Microelectronics, Fudan University, Shanghai 200433, China

^3.Henan Academy of Sciences, Zhengzhou 450046 China

Corresponding Author:

REN Yumei (1987-), female, Ph.D., Associate Professor; E-mail: ymren@zua.edu.cn;

ZHAO Biao (1988-), male, Ph.D., Associate Professor. zhao_biao@fudan.edu.cn

WANG Zhongyi (1999-), male, Master candidate. E-mail: wzyjun414@163.com

出版时间: 2025-03-20 doi: 10.14062/j.issn.0454-5648.20240607

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摘要

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高熵氧化物陶瓷因其独特的性质被认为是潜在的高性能吸波材料。采用简单的固相反应烧结法成功合成出尖晶石/岩盐型复相结构的（Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2）Co_xO_y高熵陶瓷。全面分析了其晶体结构、微观结构、元素含量及价态，并测定其电磁波吸收性能，探究了该高熵复相陶瓷的吸波性能随烧结温度的变化规律。结果表明，烧结温度为900 ℃时所得样品具有最多的氧空位以及最大的介电常数，在匹配厚度为3.0 mm，频率为9.37 GHz时，可获得-36.14 dB的最小反射损耗，有效吸收带宽为2.86 GHz，表现出最佳的电磁波吸收性能。

关键词

高熵氧化物陶瓷 / 尖晶石结构 / 岩盐结构 / 介电损耗 / 电磁波吸收性能

Abstract

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Introduction

With the rapid development of wireless communication technology, electromagnetic waves are regarded as a main medium for energy and information transmission. Absorbing materials, as a focus of scientific research in recent years, play a key role in effectively reducing electromagnetic radiation pollution in the environment, thereby reducing the negative effect of electromagnetic waves. The design of absorbing materials follows the principles of "thin, light, wide, and strong" to meet practical applications. At present, there are various types of absorbing materials, mainly including magnetic metals, polymer based composite materials, ferrites, and carbon-based materials. However, all the materials have their limitations. For instance, magnetic materials have a superior performance, but they have a poor oxidation resistance, which are prone to eddy current losses, thus affecting the absorption efficiency. The preparation cost of polymer-based composite materials is high, and their application fields are limited. Ferrite materials have an insufficient temperature stability and a high surface density. In addition, carbon-based materials suffer from poor impedance matching and narrow absorption frequency bands. These inherent limitations hinder a widespread applicability of absorbing materials in diverse application scenarios. Therefore, developing novel absorbing materials with superior oxidation resistance and high-temperature stability has an important practical significance.

Methods

High-entropy multiphase oxide ceramics was prepared by a solid-state reaction method. In the preparation process, FeO, CoO, NiO, CuO, ZnO and Co₂O₃ as raw materials in a molar ratio of 1∶1∶1∶1∶1∶5 were ground with anhydrous ethanol in a mill at 200 r/min for 8 h, and then dried at 80 ℃ to obtain a mixed powder. Subsequently, 8 g of the mixed powder was pressed into a round billet with a diameter of 30 mm at 10 MPa. The obtained round billet was then heated and reacted in a model BR-12N muffle furnace at different temperatures (i.e., 800, 900, 1000 ℃ and 1100 ℃) for 6 h to obtain the samples of (Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2)Co_xO_y high-entropy ceramics (HEO), which were named samples HEO-800, HEO-900, HEO-1000, and HEO-1100, respectively.

Results and discussion

The results show that the obtained samples HEO-800, HEO-900, HEO-1000, and HEO-1100 all exhibit spinel and rock salt phases, as well as pore structures and irregular blocks. The degree of crystallization gradually increases with increasing temperature, which can be attributed to the accelerated diffusion of atoms at the interface and the gradual increase in grain size due to the presence of oxygen vacancies. The XPS analysis indicates that the high-entropy multiphase oxide ceramics sintered at different temperatures all have oxygen vacancies, and the maximum oxygen vacancies occur at 900 ℃. The conductivity test shows that the sample HEO-900 has the maximum conductivity. The electromagnetic wave absorption test results reveal that the RL_min values of the samples HEO-800, HEO-900, HEO-1000, and HEO-1100 are -9.85, -36.14, -13.73 dB, and -4.61 dB, respectively. The sample HEO-900 obtained via sintering at 900 ℃ has the optimum absorbing property. Except for the sample HEO-900, the reflection loss of other samples is not high mainly due to the weak dielectric loss caused by low oxygen vacancy, while the magnetic loss is opposite to the dielectric loss. The magnetic loss and dielectric loss synergistically promote the improvement of absorption performance of the material. In addition, the impedance matching area also firstly increases and then decreases as the temperature increases. The impedance area of the sample HEO-900 is relatively large, indicating that there are more electromagnetic waves incident on the interior of the material and the absorption efficiency increases.

Conclusions

The results indicated that oxygen vacancies were easily generated in (Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2)Co_xO_y high-entropy ceramics due to the multivalent state and multiple transformations of element Co, which was conducive to electron transfer. The presence of multiphase structure and oxygen vacancies increased the dielectric loss of the material and the interface polarization and defect polarization of the system, thus significantly improving the absorption capacity of electromagnetic waves. This study found that the sample HEO-900 sintered at 900 ℃ had the optimum absorption performance (i.e., the RL_min value of -36.14 dB and an optimal bandwidth of 2.86 GHz at a matching thickness of 3.0 mm and a frequency of 9.37 GHz).

Key words

high-entropy oxide ceramics / spinel structure / rock salt structure / dielectric loss / electromagnetic wave absorption performance

引用本文

王中义, 任玉美, 杨帅, 席通, 郭晓琴, 赵彪, 张锐. 尖晶石/岩盐型（Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2）Co_xO_y高熵陶瓷的制备与吸波性能. 硅酸盐学报, 2025 , 53 (3) : 647 -657 . DOI: 10.14062/j.issn.0454-5648.20240607

Zhongyi WANG, Yumei REN, Shuai YANG, Tong XI, Xiaoqin GUO, Biao ZHAO, Rui ZHANG. Preparation and Microwave Absorption Properties of Spinel/Rock Salt (Fe_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2)Co_xO_y High-Entropy Ceramics[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (3) : 647 -657 . DOI: 10.14062/j.issn.0454-5648.20240607

基金

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国家自然科学基金项目(U21A2064)
河南省自然科学基金重点项目(242300421188)
河南省航空材料与技术重点实验室开放基金(ZHKF-240104/05)
河南省高等学校重点科研项目(24A150045)

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2025年第53卷第3期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240607

接收时间：2024-09-20
首发时间：2026-10-22
出版时间：2025-03-20

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出版历史

收稿日期：2024-09-20
修回日期：2024-10-08

基金

国家自然科学基金项目(U21A2064)

河南省自然科学基金重点项目(242300421188)

河南省航空材料与技术重点实验室开放基金(ZHKF-240104/05)

河南省高等学校重点科研项目(24A150045)

作者信息

^1．郑州航空工业管理学院材料学院，郑州 450046

^2．复旦大学微电子学院，上海 200433

^3．河南省科学院，郑州 450046

通讯作者:

任玉美（1987—），女，博士，副教授。

赵彪（1988—），男，博士，副教授。

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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