硅酸盐学报

A₂B₂O₇（A = Ln³⁺，B = Zr⁴⁺，Hf⁴⁺ Ti⁴⁺ Ce⁴⁺）型透明陶瓷研究进展

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赖扬群 ¹ , 陶世旭 ¹ , 麻朝阳 ¹ , 曹永革 ¹^,²

硅酸盐学报 | 综合评述 2024,52(3): 1157-1170

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硅酸盐学报 |综合评述 2024 , 52 (3) : 1157 -1170

A₂B₂O₇（A = Ln³⁺，B = Zr⁴⁺，Hf⁴⁺ Ti⁴⁺ Ce⁴⁺）型透明陶瓷研究进展

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赖扬群¹, 陶世旭¹, 麻朝阳¹, 曹永革¹^,²

作者信息

^1．松山湖材料实验室，广东东莞 523808

^2．中国科学院物理研究所，北京 100190

通讯作者:

麻朝阳（1985—），男，博士，副研究员。

作者简介:

赖扬群（1995—），男，硕士，助理工程师。

Research Progress on A₂B₂O₇(A = Ln³⁺, B = Zr⁴⁺, Hf⁴⁺ Ti⁴⁺ Ce⁴⁺) Transparent Ceramics

Yangqun LAI¹, Shixu TAO¹, Chaoyang MA¹, yongge CAO¹^,²

Affiliations

^1.Songshan Lake Materials Laboratory, Dongguan 523808, Guangdong, China

^2.Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Corresponding Author:

MA Chaoyang (1985-), male, PhD, Associate Professor. E-mail: machaoyang@sslab.org.cn

LAI Yangqun (1995-), male, Master, Assistant Engineer. E-mail: laiyangqun@sslab.org.cn

出版时间: 2024-03-20 doi: 10.14062/j.issn.0454-5648.20230635

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摘要

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A₂B₂O₇型化合物具有高熔点、高密度和高折射率等特点，在照明材料、航空材料、医疗成像、磁光材料等领域具有潜在应用价值。随着陶瓷制备工艺的进步，透明陶瓷的光学、力学和热学等性能不断提升使A₂B₂O₇型透明陶瓷受到越来越多研究者的关注，本文介绍了一些A₂B₂O₇型透明陶瓷的制备工艺、性能参数和其潜在的应用价值。

关键词

透明陶瓷 / 烧绿石 / 萤石

Abstract

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Conventional transparent materials can be primarily divided into four categories, i.e., glasses, polymers, single crystals, and transparent ceramics. Growing large single crystals with high melting points is difficult, and glass and polymers have poor mechanical and chemical stability. These shortcomings limit their applications. Transparent ceramics are favored because of their high refractive index, high hardness, high strength, high thermal conductivity, and high chemical stability. In 2005, La₂Hf₂O₇ was fabricated into transparent ceramics with a high density and a high atomic number, having a great potential in the detection field of scintillators. Since then, A₂B₂O₇ transparent ceramics has attracted much attention. The structure of A₂B₂O₇ ceramics is mainly determined by the radius ratio of A-site and B-site ions (r_A/r_B), and includes three structures (i.e., fluorite structure (r_A/r_B<1.46), pyrochlore structure (1.46<r_A/r_B<1.78) and monoclinic structure (r_A/r_B>1.78)). While, only the fluorite- and pyrochlore-structure A₂B₂O₇ ceramics could be transparent monolith when sintered at proper temperature and pressure.

A₂B₂O₇ ceramics with fluorite and pyrochlore two-phase coexisting structures have the advantage of smaller grains, compared with conventional A₂B₂O₇ transparent ceramics with single-phase structures. The mechanical properties of two-phase coexisting structures ceramics can be improved due to the smaller grains. LaLuZr₂O₇ transparent ceramics with two phases of fluorite and pyrochlore were fabricated in 2014. Two phases are uniformly distributed in the ceramic and the average grain size of the ceramic is only 2-3μm. The in-line transmittance of LaLuZr₂O₇ transparent ceramic is 73.4% at 1 100 nm due to the close refractive index between the two phases of fluorite and pyrochlore, and the scattering of light across the interface between the two phases is negligible. In 2019, (La_0.2Nd_0.2Sm_0.2Gd_0.2Yb_0.2)₂Zr₂O₇ was fabricated into transparent ceramics with a fluorite and pyrochlore two-phase coexisting structure. Compared with conventional transparent ceramics, high-entropy transparent ceramics may have better mechanical properties, corrosion resistance, and high-temperature resistance. The enhanced atomic disorder due to multi-element doping in high-entropy ceramics makes it a promising material for high-temperature windows with a lower thermal conductivity. However, there are some challenges in the preparation of two-phase coexistence transparent A₂B₂O₇ ceramics. In some previous reports on A₂B₂O₇ transparent ceramics with two-phase coexistence, the transmittance of the ceramics was severely reduced when there was a large difference in the grain sizes of the fluorite and pyrochlore phases. It is necessary to ensure that the grain growth rates of the pyrochlore and fluorite phases are similar during sintering.

Transparent ceramic scintillators of La₂Hf₂O₇:Ti⁴⁺ were fabricated in 2005. The transmittance of La₂Hf₂O₇:Ti⁴⁺ transparent ceramics at 600-800 nm is close to 60%. La₂Hf₂O₇:Ti⁴⁺ transparent ceramics gain a high X-ray stopping power due to its high density and high atomic number. The integrated emission intensity of La₂Hf₂O₇:Ti⁴⁺ transparent ceramics is 1.5 times greater than that of Bi₄Ge₃O₁₂ single crystals for the same size and the same excitation conditions. In 2019, Tb₂Hf₂O₇ was fabricated into transparent ceramics. Tb₂Hf₂O₇ transparent ceramic ceramics perform well in the Faraday magneto-optical effect tests, having higher measured Verdet constants than commercial Tb₃Ga₅O₁₂ single crystals and a potential application as an excellent magneto-optical material. It is indicated that the magneto-optical properties of magneto-optical materials are related to the concentration of Tb³⁺ in the materials, and the higher the Tb³⁺ concentration is, the better the magneto-optical properties will be. Tb₂Hf₂O₇ transparent ceramics can be doped with higher concentrations of Tb³⁺ due to the structural advantages of A₂B₂O₇, thus having better magneto-optical properties rather than garnet-structured Tb₃Ga₅O₁₂ single crystal.

Summary and prospects

This review represented the preparation methods, performances, and potential applications of A₂B₂O₇ transparent ceramic. A₂B₂O₇ transparent ceramics have the characteristics of a high melting point, a high density, and a high refractive index, which are potentially valuable in the fields of optical material. However, the optical loss and optical homogeneity of A₂B₂O₇ transparent ceramics are difficult to guarantee, a further study of optical quality improvement for A₂B₂O₇ transparent ceramics is still needed. At present, the preparation process of A₂B₂O₇ transparent ceramics is still immature, there are many residual pores in the sintered A₂B₂O₇ transparent ceramics, affecting the optical quality of the A₂B₂O₇ transparent ceramics. It is necessary to optimize the raw powder preparation process and add sintering additives to reduce the pores in the sintered A₂B₂O₇ transparent ceramics.

Although A₂B₂O₇ transparent ceramics have great application prospects in solid-state lasers, the low thermal conductivity of A₂B₂O₇ transparent ceramics makes heat dissipation a challenge. If A₂B₂O₇ transparent ceramics can be used in solid-state lasers, a superior heat dissipation system needs to be designed. In summary, A₂B₂O₇ transparent ceramics is a promising transparent material, but there are still many problems to be solved before the application.

Key words

transparent ceramics / pyrochlore / fluorite

引用本文

赖扬群, 陶世旭, 麻朝阳, 曹永革. A₂B₂O₇（A = Ln³⁺，B = Zr⁴⁺，Hf⁴⁺ Ti⁴⁺ Ce⁴⁺）型透明陶瓷研究进展. 硅酸盐学报, 2024 , 52 (3) : 1157 -1170 . DOI: 10.14062/j.issn.0454-5648.20230635

Yangqun LAI, Shixu TAO, Chaoyang MA, yongge CAO. Research Progress on A₂B₂O₇(A = Ln³⁺, B = Zr⁴⁺, Hf⁴⁺ Ti⁴⁺ Ce⁴⁺) Transparent Ceramics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (3) : 1157 -1170 . DOI: 10.14062/j.issn.0454-5648.20230635

基金

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广东省珠江人才引进计划创新创业团队(2019ZT08C321)

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2024年第52卷第3期

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doi: 10.14062/j.issn.0454-5648.20230635

接收时间：2023-08-25
首发时间：2026-10-22
出版时间：2024-03-20

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收稿日期：2023-08-25
修回日期：2023-12-05

基金

广东省珠江人才引进计划创新创业团队(2019ZT08C321)

作者信息

^1．松山湖材料实验室，广东东莞 523808

^2．中国科学院物理研究所，北京 100190

通讯作者:

麻朝阳（1985—），男，博士，副研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230635

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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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