Eu3+掺杂Y2O3单分散红色荧光球形颗粒的尺寸可控合成与荧光性能

doi:10.15541/jim20160207

无机材料学报 ›› 2016, Vol. 31 ›› Issue (10): 1087-1093.DOI: 10.15541/jim20160207

Eu³⁺掺杂Y₂O₃单分散红色荧光球形颗粒的尺寸可控合成与荧光性能

曲姣^{1, 2}, 朱琦², 李继光², 孙旭东²

(1. 沈阳工学院机械与运载学院, 抚顺 113122; 2. 东北大学材料科学与工程学院, 材料各向异性与织构教育部重点实验室, 沈阳 110819)

收稿日期:2016-03-30 修回日期:2016-05-24 出版日期:2016-10-20 网络出版日期:2016-09-23
作者简介:曲姣(1987–), 女, 讲师. E-mail: qujiaomail@163.com
基金资助:
国家自然科学基金(51172038, 51302032);中央高校基本科研业务费资助项目(N140204002)

Eu³⁺Activated Y₂O₃ Red Phosphor Monospheres: Size-controlled Processing and Luminescence Property

QU Jiao^{1, 2}, ZHU Qi², Li Ji-Guang², SUN Xu-Dong¹

(1. College of Mechanical and Vehicle Engineering, Shenyang Institute of Technology, Fushun 113122, China; 2. Key Laboratory for Anisotropy and Texture of Materials (Ministry of Education), School of Materials Science and Engineering, Northeastern University, Shenyang 110819, China)

Received:2016-03-30 Revised:2016-05-24 Published:2016-10-20 Online:2016-09-23
About author:QU Jiao. E-mail: qujiaomail@163.com
Supported by:
National Natural Science Foundation of China (51172038, 51302032);Fundamental Research Funds for the Central Universi ties (N140204002)

摘要/Abstract

摘要：

结合籽晶法和添加矿化剂硝酸铵, 通过均相沉淀合成和后续煅烧实现了(Y, Eu)₂O₃单分散球形颗粒(直径范围110~550 nm)的可控合成。通过XRD、FE-SEM、TEM和PLE/PL分析等手段对产物进行了系统表征。发现采用籽晶法和添加矿化剂硝酸铵可以促进球形颗粒长大。碱式碳酸盐前驱体经600℃煅烧分解为立方晶(Y, Eu)₂O₃, 且经1000℃煅烧后(Y, Eu)₂O₃依然继承球形形貌特征。所得多晶(Y, Eu)₂O₃球形荧光颗粒在242 nm激发下于615 nm处呈现最强红色荧光发射(Eu³⁺的⁵D₀→⁷F₂跃迁)。荧光粉的荧光性能呈现明显的尺寸依存性。增大球形颗粒尺寸减小了荧光寿命(1.15~1.57 ms)和荧光不对称因子[I(⁵D₀→⁷F₂)/I(⁵D₀→⁷F₁)], 但增强了荧光发射强度。

关键词: 单分散球, 尺寸可控合成, 荧光性能, 氧化钇

Abstract:

Monodispersed (Y, Eu)₂O₃ spheres (110-550 nm in diameter) were calcined from precursors synthesized via homogeneous precipitation. Systematic characterizations of the products were carried out by XRD, FE-SEM, TEM, and PLE/PL analyses. Large spherical particles were resulted via seeded growth and NH₄NO₃ addition. Calcining the basic carbonate precursor at 600℃ yielded cubic (Y, Eu)₂O₃. The spherical shape and excellent dispersion of the precursor particles were largely retained to the oxides after annealing up to 1000℃. The polycrystalline (Y, Eu)₂O₃spheres exhibited typical red emission at 615 nm (the ⁵D₀→⁷F₂ transition of Eu³⁺) under UV excitation at 242 nm. The phosphors showed a substantially size-dependent luminescent behavior. Shorter fluorescence lifetime (1.15-1.57 ms), decreased asymmetry factor (I(⁵D₀→⁷F₂)/I(⁵D₀→⁷F₁)) of luminescence, and enhanced luminescent intensity were observed along with increasing particle size.

Key words: monospheres, size-controlled processing, luminescent property, yttria

中图分类号:

TB34

曲姣, 朱琦, 李继光, 孙旭东. Eu³⁺掺杂Y₂O₃单分散红色荧光球形颗粒的尺寸可控合成与荧光性能[J]. 无机材料学报, 2016, 31(10): 1087-1093.

QU Jiao, ZHU Qi, Li Ji-Guang, SUN Xu-Dong. Eu³⁺Activated Y₂O₃ Red Phosphor Monospheres: Size-controlled Processing and Luminescence Property[J]. Journal of Inorganic Materials, 2016, 31(10): 1087-1093.

图/表 9

表1 前驱体均相沉淀的合成条件

Table 1 UBHP conditions for precursor synthesis

Sample ID	Ln³⁺ (Ln=Y, Eu) conentration /(mol·L^-1)	Urea concentration /(mol·L^-1)	NH₄NO₃ concentration /(mol·L^-1)	Urea/Ln³⁺ molar ration, R
S1	0.015	0.3	0	20
S2	0.015	0.5	0	33.3
S3	0.015	0.3 (adding in three times: 0.1, 0.1, 0.1)	0	20
S4	0.015	0.5 (adding in three times: 0.15, 0.15, 0.20)	0	33.3
S5	0.015	0.5	0.015	33.3
S6	0.015	0.5	0.045	33.3

图1 前驱体S1~S6(a~f)的FE-SEM照片

Fig. 1 FE-SEM images of precursors S1-S6 (a-f)

图2 前驱体S6经不同温度煅烧所得产物的XRD图谱

Fig. 2 XRD patterns of the products calcined from precursor S6 at different temperatures

图3 前驱体S6经不同温度煅烧所得产物的晶粒尺寸

Fig. 3 Crystallite size of the products calcinated from precursor S6 at different temperatures

图4 前驱体S6经(a)800℃、(b)1000℃和(c)1300℃煅烧所得产物的FE-SEM形貌; (d, f)前驱体S1和(e)前驱体S4经1000℃煅烧所得产物的FE-SEM和TEM形貌

Fig. 4 FE-SEM images of the products calcinated from precursor S6 at (a) 800℃, (b) 1000℃, (c) 1300℃; (d-e) are FE-SEM and TEM micrographs of the products calcinated from precursors S1 and S4, at 1000℃ for 4 h respectively

图5 不同前驱体经1000℃煅烧4 h所得产物的XRD图谱

Fig. 5 XRD patterns of the (Y0.95Eu0.05)2O3 oxides calcined from different precursors at 1000℃ for 4 h

图6 前驱体S6经不同温度煅烧所得产物的(a)PLE和(b)PL光谱图

Fig. 6 (a) PLE and (b) PL spectra of the (Y0.95Eu0.05)2O3 oxides calcined from precursor S6 at various temperatures

图7 不同尺寸(Y0.95Eu0.05)2O3颗粒的荧光发射光谱

Fig. 7 PL spectra of the (Y0.95Eu0.05)2O3 oxides with various particle sizes

图8 三种典型前驱体经1000℃煅烧所得产物在615 nm处的荧光衰变曲线

Fig. 8 Fluorescence decay curves for 615 nm emission of three typical samples calcined from different precursors at 1000℃

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Eu³⁺掺杂Y₂O₃单分散红色荧光球形颗粒的尺寸可控合成与荧光性能

Eu³⁺Activated Y₂O₃ Red Phosphor Monospheres: Size-controlled Processing and Luminescence Property

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