硅酸盐学报

不同掺杂量Eu_xLu_1.4_-_xGd_0.6O₃透明陶瓷的制备与性能

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陈宇洋 ¹^,² , 毕愿 ¹^,³ , 朱丹阳 ¹^,² , 贺宁桐 ¹^,⁴ , 胡辰 ¹ , 王雁斌 ¹^,⁴ , 张芳 ³ , 李江 ¹^,²

硅酸盐学报 | 研究论文 2024,52(3): 828-835

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硅酸盐学报 |研究论文 2024 , 52 (3) : 828 -835

不同掺杂量Eu_xLu_1.4_-_xGd_0.6O₃透明陶瓷的制备与性能

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陈宇洋¹^,², 毕愿¹^,³, 朱丹阳¹^,², 贺宁桐¹^,⁴, 胡辰¹, 王雁斌¹^,⁴, 张芳³, 李江¹^,²

作者信息

^1．中国科学院上海硅酸盐研究所透明陶瓷研究中心，上海 201899

^2．中国科学院大学，北京 100049

^3．武汉工程大学材料科学与工程学院，武汉 430205

^4．江苏大学材料科学与工程学院，江苏镇江 212013

通讯作者:

李江（1977—），男，博士，研究员。

作者简介:

陈宇洋（1999—），男，博士研究生。

Preparation and Performance of Eu_xLu_1.4_-_xGd_0.6O₃ Transparent Ceramics

Yuyang CHEN¹^,², Yuan BI¹^,³, Danyang ZHU¹^,², Nington HE¹^,⁴, Chen HU¹, Yanbin WANG¹^,⁴, Fang ZHANG³, Jiang LI¹^,²

Affiliations

^1.Transparent Ceramic Research Center of Chinese Academy of Sciences Shanghai Silicate Institute, Shanghai 201899, China

^2.Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

^3.School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430205, China

^4.School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China

Corresponding Author:

LI Jiang (1977-), male, Ph.D., Professor. E-mail: lijiang@mail.sic.ac.cn

CHEN Yuyang (1999-), male, Doctorial candidate. E-mail: chenyuyang21@mails.ucas.ac.cn

出版时间: 2024-03-20 doi: 10.14062/j.issn.0454-5648.20230629

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摘要

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为了满足高能射线成像对闪烁陶瓷的应用要求，并探究Eu³⁺掺杂量对陶瓷微观结构和光学性能的影响，采用液相共沉淀法合成了不同Eu³⁺掺杂量的Eu_xLu_1.4-_xGd_0.6O₃（x=0、0.02、0.06、0.10、0.14、0.18）粉体并通过真空预烧结合热等静压烧结，制备出Eu_xLu_1.4-_xGd_0.6O₃透明陶瓷。随着Eu³⁺掺杂量的增加，陶瓷直线透过率先升高后降低，在x=0.10时达到最高（71.4%@611 nm）。Eu_xLu_1.4-_xGd_0.6O₃陶瓷的光致激发光谱和光致发光光谱证明了Eu³⁺掺杂量的增加能够提升陶瓷的吸收峰和发射峰强度。陶瓷在X射线激发下的发光强度随着Eu³⁺掺杂量的升高呈现先升高后降低的趋势，在Eu³⁺掺杂量（摩尔分数）为3%时达到最高。Eu_xLu_1.4-_xGd_0.6O₃陶瓷在可见光和X射线激发下都呈现强烈的红光发射，与硅光电二极管光谱响应有着良好的耦合性。

关键词

透明陶瓷 / 闪烁陶瓷 / 发光性能

Abstract

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Introduction

In non-destructive testing of large devices, industrial computed tomography (CT) with high-energy radiation sources requires scintillators with a high performance of light yield, short decay time, high effective atomic number, and strong radiation resistance to achieve high-resolution imaging. Eu³⁺ doped Gd₂O₃-Lu₂O₃ solid solution ceramics have a high density and an effective atomic number, having high X-ray stopping power and radiation resistance. The ceramics have a high light yield that is beneficial to improving imaging quality. Moreover, Eu³⁺ emits a light in the red region, which matches well with the spectral sensitivity of silicon photodiodes. Eu_xLu_1.4—_xGd_0.6O₃ transparent ceramics are one of scintillators with great application prospects in the field of X-ray imaging. A recentl study managed to prepare commercial products of Eu_xLu_1.4—_xGd_0.6O₃ transparent ceramics with a high transparency and a high light output. However, such a research is still at the initial stage, and the optical quality of ceramics needs to be improved to meet practical application needs. There is also a lack of research on component design. Especially, the effect of Eu³⁺ concentration on the structure and spectral properties of Eu_xLu_1.4-_xGd_0.6O₃ ceramics is still unclear. In this paper, Eu_xLu_1.4-_xGd_0.6O₃ (x=0, 0.02, 0.06, 0.10, 0.14, 0.18) ceramics with different Eu³⁺ concentrations were prepared via coprecipitation and subsequent vacuum sintering/hot isostatic pressing (HIP), and their microstructure and optical properties were analyzed.

Methods

In the synthesis of nano-powder, the obtained precursor was calcined in air at 1 100 ℃ for 4 h to obtain Eu_xLu_1.4-_xGd_0.6O₃ (x=0, 0.02, 0.06, 0.10, 0.14, 0.18) powders. The synthesized powders were molded in a 18 mm mold at 40 MPa, and then the ceramic green bodies were obtained by cold isostatic pressing at 250 MPa, pre-sintered in vacuum at 1 600 ℃ for 2 h and then sintered in argon atmosphere under 176 MPa at 1 750 ℃ for 2 h. The fabricated Eu_xLu_1.4-_xGd_0.6O₃ ceramics were annealed in air at 1 100 ℃ for 20 h to remove oxygen vacancies introduced by sintering in a reducing atmosphere.

The microstructure of the sample was characterized by a model SU9000 field emission scanning electron microscope (Hitachi Co., Japan). The XRD pattern was detected by a model D8/DISCOVER DAVINCIX X-ray diffractometer (Brooke Co., Germany). The photoluminescence spectra (PL) and photoluminescence excited spectra (PLE) of ceramics were tested by a model FLS-980 fluorescence spectrometer (Edinburgh Instruments Ltd., UK). The performance of scintillating ceramics was characterized by an X-ray excitation emission spectrometer. The emission signals of the test samples were analyzed by a model QE65000 spectrometer (Ocean Optics Co., USA) excited by an X-ray tube operating at a voltage of 70 kV and a current of 1.5 mA. The transmittance curve was tested by a model Cary-5000 ultraviolet visible near-infrared spectrophotometer (Varian Co., USA).

Results and discussion

The Eu_xLu_1.4-_xGd_0.6O₃ (x=0, 0.02, 0.06, 0.10, 0.14, 0.18) powders are all cubic crystalline, and the diffraction peak position shifts towards a lower angle as Eu³⁺ doping concentration increases because the ion radius of Eu³⁺(i.e., 0.950 Å) or Gd³⁺(i.e., 0.938 Å) is larger than that of Lu³⁺(i.e., 0.848 Å). According to Scherrer's formula, the average grain size of the powders gradually decreases from 63.7 nm to 55.0 nm as the concentration of Eu³⁺ increases. The Eu_xLu_1.4-_xGd_0.6O₃ ceramics have uniform grain sizes, no obvious pores occur, and there is no second phase. The grain size measured by a linear intercept method decreases from 1.0 μm to 0.9 μm as the Eu³⁺ doping concentration increases. This is because the lattice distortion caused by Eu³⁺ doping suppresses the growth of ceramic grains in sintering. Compared to the prepared ceramics, the grain sizes of the ceramics after HIP increase. The average grain size of the ceramics after HIP decreases from 76.5 μm to 30.1 μm as the Eu³⁺ doping concentration increases from 0 to 9%.

The in-line transmittance of ceramics firstly increases and then decreases with the increase of Eu³⁺ concentration. When x=0.1, the in-line transmittance of ceramics reaches a maximum of 71.4% at 611 nm. When the concentration of Eu³⁺ is high, the lattice distortion inside the ceramic intensifies, leading to a decrease in the in-line transmittance. In the XEL patterns of Eu_xLu_1.4-_xGd_0.6O₃ ceramics, the emission spectrum is composed of Eu³⁺ characteristic emission peaks. The main emission peak is located at 611 nm, which is an intense red light emitted from the ⁵D₀→⁷F₂ transition. When the Eu³⁺ concentration is low, the emission intensity of the ceramic gradually increases with the increase of the number of emission centers. When the concentration of Eu³⁺ exceeds 3%, the distance between the emission centers decreases. Also, the energy transfer between Eu³⁺ increases and the transition probability between Eu³⁺ and defects increases due to the high energy of the excitation source, resulting in a decrease in scintillation luminescence intensity. The ceramic exhibits an intense red light emission matching well with silicon photodiodes.

Conclusions

The maximum in-line transmittance of the ceramic could be obtained at the Eu³⁺ doping concentration of 5%, reaching 71.4% at 611 nm. The photoluminescence and photoluminescence excited spectra of Eu_xLu_1.4-_xGd_0.6O₃ ceramics demonstrated that increasing the concentration of Eu³⁺ could enhance the absorption and emission peak intensities of the ceramics. At the concentration of Eu³⁺ of 3%, the ceramic exhibited the most intense red light emission under X-ray excitation with the main emission peak located at 611 nm, corresponding to the ⁵D₀→F₂ transition of Eu³⁺. High transmittance and high red light emission intensity were of great significance for achieving a high-resolution X-ray imaging.

Key words

transparent ceramics / scintillation ceramics / luminescence performance

引用本文

陈宇洋, 毕愿, 朱丹阳, 贺宁桐, 胡辰, 王雁斌, 张芳, 李江. 不同掺杂量Eu_xLu_1.4_-_xGd_0.6O₃透明陶瓷的制备与性能. 硅酸盐学报, 2024 , 52 (3) : 828 -835 . DOI: 10.14062/j.issn.0454-5648.20230629

Yuyang CHEN, Yuan BI, Danyang ZHU, Nington HE, Chen HU, Yanbin WANG, Fang ZHANG, Jiang LI. Preparation and Performance of Eu_xLu_1.4_-_xGd_0.6O₃ Transparent Ceramics[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (3) : 828 -835 . DOI: 10.14062/j.issn.0454-5648.20230629

基金

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中国科学院国际伙伴计划(121631KYSB20200039)
上海市“一带一路”国际合作项目(20520750200)

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2024年第52卷第3期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230629

接收时间：2023-08-23
首发时间：2026-10-22
出版时间：2024-03-20

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收稿日期：2023-08-23
修回日期：2023-09-12

基金

中国科学院国际伙伴计划(121631KYSB20200039)

上海市“一带一路”国际合作项目(20520750200)

作者信息

^1．中国科学院上海硅酸盐研究所透明陶瓷研究中心，上海 201899

^2．中国科学院大学，北京 100049

^3．武汉工程大学材料科学与工程学院，武汉 430205

^4．江苏大学材料科学与工程学院，江苏镇江 212013

通讯作者:

李江（1977—），男，博士，研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230629

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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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