硅酸盐学报

高熵ReVO₄陶瓷与微波介电性能

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陈德钦 ¹ , 莫尘 ¹ , 农莲汀 ¹ , 崔洪波 ¹ , 王政锋 ² , 刘来君 ¹ , 李纯纯 ¹^,²

硅酸盐学报 | 研究论文 2024,52(9): 2907-2914

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硅酸盐学报 |研究论文 2024 , 52 (9) : 2907 -2914

高熵ReVO₄陶瓷与微波介电性能

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陈德钦¹, 莫尘¹, 农莲汀¹, 崔洪波¹, 王政锋², 刘来君¹, 李纯纯¹^,²

作者信息

^1．桂林理工大学材料科学与工程学院，广西大学，有色金属氧化物电子功能材料与器件重点实验室，广西桂林 541004

^2．桂林理工大学材料科学与工程学院，广西嵌入式技术与智能系统重点实验室，广西桂林 541004

通讯作者:

李纯纯（1987—），男，博士，副研究员。

作者简介:

陈德钦（1999—），男，硕士研究生。

High-Entropy Ceramics ReVO₄ and Microwave Dielectric Properties

Deqin CHEN¹, Chen MO¹, Lianting NONG¹, Hongbo CUI¹, Zhengfeng WANG², Laijun LIU¹, Chunchun LI¹^,²

Affiliations

^1.Guangxi University Key Laboratory of Non-ferrous Metal Oxide Electronic Functional Materials and Devices, College of Material Science and Engineering, Guilin University of Technology, Guilin 541004, Guangxi, China

^2.Guangxi Key Laboratory of Embedded Technology and Intelligent System, Guilin University of Technology, Guilin 541004, China

Corresponding Author:

LI Chunchun (1987-), male, Ph.D., Associate Professor. E-mail: lichunchun2003@126.com

CHEN Deqin (1999-), male, Master candidate. E-mail: deqin_c@163.com

出版时间: 2024-09-20 doi: 10.14062/j.issn.0454-5648.20240163

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摘要

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采用固相反应法制备了3种高熵ReVO₄陶瓷，对其物相结构、微观形貌和振动特征采用X射线衍射、扫描电子显微镜和Raman光谱进行表征，并对微波介电性能进行了分析。结果表明：所有陶瓷样品均表现出空间群为I4₁/amd的四方锆石结构，致密的微观结构使其展现出良好的微波介电性能。采用Clausius-Mossotti公式解释了介电常数的变化，介电常数与离子极化率呈正相关；品质因数与填充因子具有相似的变化趋势；键价理论被用于反映晶格畸变的程度，并与谐振频率温度系数具有强关联性。

关键词

高熵陶瓷 / 微波频率 / 介电性能 / 锆石结构 / 钒酸盐

Abstract

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Introduction

Microwave dielectric ceramics are widely used in microwave frequency (i.e., 300 MHz-300 GHz) circuits as communication electronic components such as resonators, filters, and antennas. The dielectric permittivity (ε_r), quality factor (Q×f) and the temperature coefficient of resonant frequency (τ_f) are the main performance index to measure the quality of microwave dielectric ceramics. However, there is a constraint relationship between the performance parameters. In general, the giant ε_r may cause a large dielectric loss and a low Q×f, and the volatility of ε_r originates an enormous τ_f value. Therefore, materials with superior intrinsic microwave dielectric properties are rare. The existing methods of controlling microwave dielectric properties mainly include ion substitution, composite control, laminated control and non-stoichiometric ratio control. These methods often require sacrificing one parameter to satisfy other parameters. High-entropy strategy is a novel regulation method used in inorganic materials. High-entropy ceramics refer to a ceramic system with a configuration entropy (S_c) of 1.5R. The high-entropy effect, sluggish diffusion effect, lattice distortion effect and synergy in components (i.e., cocktail effect) are four special effects of high-entropy ceramics. The high-entropy strategy shows a great potential in dielectric ceramics due to these unique effects. In this paper, high-entropy strategy was used to design rare-earth vanadate ceramics. The impact of high-entropy structure on the microwave dielectric properties was investigated.

Methods

High-entropy ceramics of ReVO₄ were synthesized by a solid-phase method with high-purity rare earth oxides (Re₂O₃ with a purity of > 99.9%) and V₂O₅. The ceramics with different chemical formulas (La_0.2Ce_0.2Nd_0.2Sm_0.2Eu_0.2)VO₄, (La_0.2Ce_0.2Nd_0.2Sm_0.2 Gd_0.2)VO₄, and (La_0.2Ce_0.2Nd_0.2Sm_0.2Y_0.2)VO₄, were denoted as Eu-5RVO, Gd-5RVO, and Y-5RVO, respectively. The raw materials were weighed according to a stoichiometric ratio and mixed in a ball mill at a rotational speed of 300 r/min for 6 h. The slurry after milling was dried in an oven at 120 ℃ for 24 h. After grinding, the powders were pre-fired in a Muffle furnace at 800 ℃ for 6 h. Then the prepared powders were further ground for 6 h, dried, and added with a polyvinyl alcohol solution (PVA, 5%) as a binder. The granulated powders were sieved by a 80/120 mesh screen and then pressed into cylindrical bulks with a thickness of 5.5-6.5 mm and diameter of 10 mm at 10 MPa. The samples were heated at 550 ℃ for 6 h to eliminate the binder and sintered at 1 400-1 500 ℃ for 6 h with an increment of 20 ℃ to obtain the dense ceramics.

The crystal structure of the ceramics was analyzed by X-ray diffraction (XRD, PANalytical Co., the Netherlands). The apparent density was determined by Archimedes' drainage method. The microstructure was evaluated by a model S-4800 scanning electron microscope (SEM, Hitachi High-Technologies Co., Japan). The dielectric properties at different microwave frequencies (i.e., 1-20 GHz) were measured by a model Keysight E5071C vector network analyzer (Keysight Technologies Co., USA) in TE₀₁₁ mode based on the Hakki-Coleman method. The temperature coefficient of resonant frequency (τ_f) was calculated via recording the frequency drifting at 25-85 ℃ (i.e., f₂₅ and f₈₅).

Results and discussion

The high-entropy ceramics Eu-5RVO, Gd-5RVO, and Y-5RVO exhibit a tetragonal zircon structure with a space group I4₁/amd. The SEM images of the fractured cross-section of high-entropy ceramics ReVO₄ show uniform grains and clear grain boundaries, along with the spatial distribution of elements based on EDS analysis. The ceramics all exhibit a dense microstructure, as well as a promising microwave dielectric performance. The dielectric permittivity is analyzed via the Clausius-Mossotti formula, which is positively correlated to ion polarization. The quality factor is primarily determined by the packing fraction. The bond valence theory is used to reflect the degree of lattice distortion, having a strong relationship with the temperature coefficient of resonance frequency. The results show that the high-entropy strategy can effectively regulate the microwave dielectric properties.

Conclusions

A series of high-entropy ceramics of ReVO₄ were prepared by a solid-state reaction method. All the ceramics were a tetragonal zircon structure with a space group I4₁/amd. The phase structure, microscopic morphology, and vibration characteristics of high-entropy ceramics ReVO₄ were analyzed, and the microwave dielectric properties were analyzed by the Clausius-Mossotti formula, packing fraction, and bond valence theory. The results showed that ceramic Y-5RVO exhibited an optimal microwave dielectric properties (i.e., ε_r of 10.69, Q×f of 11 704 GHz, and τ_f of -21.70×10^-6/℃). It was indicated that the high-entropy ceramics of ReVO₄ could be used as competitive microwave dielectric materials.

Key words

high-entropy ceramic / microwave frequency / dielectric properties / zircon structure / vanadate

引用本文

陈德钦, 莫尘, 农莲汀, 崔洪波, 王政锋, 刘来君, 李纯纯. 高熵ReVO₄陶瓷与微波介电性能. 硅酸盐学报, 2024 , 52 (9) : 2907 -2914 . DOI: 10.14062/j.issn.0454-5648.20240163

Deqin CHEN, Chen MO, Lianting NONG, Hongbo CUI, Zhengfeng WANG, Laijun LIU, Chunchun LI. High-Entropy Ceramics ReVO₄ and Microwave Dielectric Properties[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (9) : 2907 -2914 . DOI: 10.14062/j.issn.0454-5648.20240163

基金

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国家自然科学基金(62061011)

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2024年第52卷第9期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240163

接收时间：2024-02-28
首发时间：2026-10-22
出版时间：2024-09-20

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收稿日期：2024-02-28
修回日期：2024-04-08

基金

国家自然科学基金(62061011)

作者信息

^1．桂林理工大学材料科学与工程学院，广西大学，有色金属氧化物电子功能材料与器件重点实验室，广西桂林 541004

^2．桂林理工大学材料科学与工程学院，广西嵌入式技术与智能系统重点实验室，广西桂林 541004

通讯作者:

李纯纯（1987—），男，博士，副研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240163

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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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