Sr2Si5N8:Eu2+荧光粉的制备及其发光性能研究

doi:10.15541/jim20140057

无机材料学报 ›› 2014, Vol. 29 ›› Issue (12): 1281-1286.DOI: 10.15541/jim20140057

Sr₂Si₅N₈:Eu²⁺荧光粉的制备及其发光性能研究

彭霞^{1, 2}, 李淑星^{1, 2}, 刘学建¹, 黄政仁¹, 李会利³

(1. 中国科学院上海硅酸盐研究所, 高性能陶瓷和超微结构国家重点实验室, 上海200050; 2. 中国科学院大学, 北京 100049; 3. 华东师范大学物理系, 上海 200062)

收稿日期:2014-02-10 修回日期:2014-03-23 出版日期:2014-12-20 网络出版日期:2014-11-20
作者简介:彭霞(1988–), 女, 硕士研究生. E-mail: pengxia@student.sic.cn
基金资助:
国家自然科学基金 (51172263);上海市自然科学基金(13ZR1412500)

Syntheses and Photoluminescence Properties of Sr₂Si₅N₈:Eu²⁺Phosphors

PENG Xia^1,2, LI Shu-Xing^1,2, LIU Xue-Jian¹, HUANG Zheng-Ren¹, LI Hui-Li³

(1. The State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China; 2. University of Chinese Academy of Sciences, Beijing 100049, China; 3. Department of Physics, East China Normal University, Shanghai 200062, China)

Received:2014-02-10 Revised:2014-03-23 Published:2014-12-20 Online:2014-11-20
About author:PENG Xia. E-mail: pengxia@student.sic.cn
Supported by:
National Natural Science Foundation of C hina (51172263);Shanghai Municipal Natural Science Foundation (13ZR1412500)

摘要/Abstract

摘要：

以Sr₂CO₃、Si₃N₄和Eu₂O₃为原料, 以C为主要还原剂, 采用碳热还原氮化工艺合成Sr₂Si₅N₈:Eu²⁺荧光粉, 着重研究了C、Sr₂CO₃添加量及Eu²⁺浓度对产物物相及发光性能的影响。研究结果表明: 当C与Si₃N₄的摩尔比 n_c/=9/5时,合成出Sr₂Si₅N₈:Eu²⁺单相荧光粉, 添加适当过量的Sr₂CO₃可提高合成产物的N含量, 且荧光粉的发光强度与其N含量呈现正相关关系。在450 nm蓝光激发下, 受Eu²⁺的4f⁶5d¹→ 4f⁷跃迁作用, Sr₂Si₅N₈:Eu²⁺荧光粉在550~700 nm波段范围产生非对称宽带发射。随着Eu²⁺掺杂浓度由1.5mol%增加到20mol%, 荧光粉的发光强度先增强后减弱, 达到2mol%时发生浓度淬灭现象; 发射主峰由608 nm逐步红移至641 nm; CIE色坐标从(0.606, 0.393)位移至(0.656, 0.343), 是一种可用于白光LED的优质红色荧光粉。

关键词: 碱土金属氮硅化物, 荧光粉, 碳热还原氮化法, 发光性能

Abstract:

Sr₂Si₅N₈:Eu²⁺ phosphors were prepared by carbothermal reduction and nitridation method using Sr₂CO₃, Si₃N₄ and Eu₂O₃ as raw materials, and C as main reduction agent. The influence of C, Sr₂CO₃and Eu²⁺ contents on phase composition and photoluminescence properties of as-prepared phosphors were investigated. The experimental results indicate that single-phase Sr₂Si₅N₈:Eu²⁺is produced with molar ratio n_c/n_Si3N4=9/5. Excessive Sr₂CO₃ addition contributes to the N contents of the as-prepared phosphors, which enhances emission intensity. There is an asymmetric wide emission peaks between 550 nm and 700 nm due to the electron transfer of Eu²⁺ from 4f⁶5d¹to 4f⁷ excited by 450 nm. Increasing Eu²⁺ concentration from 1.5mol% to 20mol%, the luminescence intensity hits the maximum value at Eu²⁺ concentration of 2mol% followed by continuous decline. Meanwhile the emission peak position is red-shifted from 608 nm to 641 nm, and the CIE chromaticity coordinates varies from (0.606, 0.393) to (0.656, 0.343), which indicates that Sr₂Si₅N₈:Eu²⁺ is a promising phosphor for white LEDs.

Key words: alkaline-earth-silicon-nitrides, phosphor, carbothermal reduction and nitridation method, luminescence

中图分类号:

Q614

彭霞, 李淑星, 刘学建, 黄政仁, 李会利. Sr₂Si₅N₈:Eu²⁺荧光粉的制备及其发光性能研究[J]. 无机材料学报, 2014, 29(12): 1281-1286.

PENG Xia,LI Shu-Xing, LIU Xue-Jian, HUANG Zheng-Ren, LI Hui-Li. Syntheses and Photoluminescence Properties of Sr₂Si₅N₈:Eu²⁺Phosphors[J]. Journal of Inorganic Materials, 2014, 29(12): 1281-1286.

图/表 11

图1 不同C含量配方的合成产物的XRD图谱

Fig. 1 XRD patterns of samples with different molar ratios of nc/

图2 不同C含量配方的合成产物的激发和发射谱(λem= 609 nm, λex=450 nm)

Fig. 2 Excitation and emission spectra of samples with different molar ratios of nc/(λem=609 nm, λex=450 nm)

图3 Sr2CO3不同程度过量的合成产物的XRD图谱

Fig. 3 XRD patterns of samples produced with different excessive Sr2CO3 additions as a function of temperature

表1 添加不同程度过量Sr2CO3配方的合成产物的元素分析

Table 1 Elements analyses of samples produced with different excessive Sr2CO3 additions

Sr₂CO₃ excessive/ mol%	0	5	10	15	20
O/wt%	0.58	0.89	1.13	1.80	2.08
N/wt%	22.88	23.06	23.30	21.28	19.58

图4 Sr2CO3不同程度过量的合成产物的发射光谱(λex=450 nm)

Fig. 4 Emission spectra of samples produced with different excessive Sr2CO3 additions (λex=450 nm)

图5 不同Eu2+掺杂浓度的合成产物的XRD图谱

Fig. 5 XRD patterns of samples doped with different concentrations of Eu2+

图6 不同浓度Eu2+掺杂样品的发射谱图

Fig. 6 Emission spectra of samples doped with different concentrations of Eu2+

图7 Sr2Si5N8:2mol%Eu2+样品发射光谱的高斯拟合曲线

Fig. 7 Gaussian deconvoluted emission curves of Sr2Si5N8: 2mol%Eu2+

图8 不同浓度Eu2+掺杂样品的色坐标图

Fig. 8 CIE chromaticity coordinates of samples doped with different concentrations of Eu2+

图9 通过碳热还原法和高温固相法合成荧光粉的XRD图谱

Fig. 9 XRD patterns of samples synthesized by CTRN and SSR method

图10 通过碳热还原法和高温固相法合成荧光粉的发射光谱比较

Fig. 10 Emission spectra of samples synthesized by CTRN and SSR methods

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Sr₂Si₅N₈:Eu²⁺荧光粉的制备及其发光性能研究

Syntheses and Photoluminescence Properties of Sr₂Si₅N₈:Eu²⁺Phosphors

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