发光学报, 2019, 40 (12): 1494, 网络出版: 2020-01-09  

基于相图原理定量预测(Mg1-x-yBaxSry)1.95SiO4∶0.05Eu系列荧光粉的结构和发光性能

Quantitative Prediction of Structure and Luminescent Properties of (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu via Phase Diagram Approach
作者单位
1 南昌大学 材料科学与工程学院, 江西 南昌 330001
2 南昌大学 江西省轻质高强结构材料重点实验室, 江西 南昌 330001
摘要
为了研究随着三元碱土离子配比变化其正硅酸盐物相组成、发光性能的变化规律, 优选高效荧光粉,同时探讨单相区和混合相区发光性能的变化内在机制, 建立组分-结构-发光性能关联, 本文采用高温固相法制备(Mg1-x-yBaxSry)1.95SiO4∶0.05Eu系列荧光粉, 共计44个样, 分析其二元、三元物相组成和光谱, 得出其物相组成和紫外激发发光CIE值。实验表明, (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu体系中物相组成随着组元含量存在渐变性; 富Ba端形成了Ba2SiO4相单相区(Sr最大量含量为35%、Mg为30%), 单相区随着Sr2+、Mg2+固溶, 晶格常数减小, 结晶度提高。(Mg1-x-yBaxSry)1.95SiO4∶0.05Eu荧光粉在紫外激发下其颜色和亮度随着组元含量也呈现渐变性, Ba2SiO4相单相区荧光粉均为绿色荧光粉且随着Sr2+、Mg2+固溶荧光亮度逐渐增大(精细光谱表明单相区内Mg2+、Sr2+离子有促进Eu2+离子进入高发光效率的格位的效果); Mg2SiO4-Sr2SiO4二元系列为红色荧光粉; 单相区外的样品点随着Ba2+的减少, 荧光粉紫外激发荧光颜色逐渐由绿变红(混合物相中Eu离子配位空间逐渐减小, Eu离子逐渐以Eu3+离子形式存在)。 (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu系列荧光粉的相组成、结构及发光性能随组元呈现渐变性关系, 借鉴相图建立方法, 可建立三元色像图(由样品发射光谱得出的CIE色像点, 基于散点分布建立色像图); 利用三元色像图可系统性优选高效荧光粉(优选出最佳绿色和红色荧光粉样品点为: (Mg0.3Ba0.65Sr0.05)1.95SiO4∶0.05Eu和(Mg0.65Sr0.35)1.95SiO4∶0.05Eu)。
Abstract
In order to study the variation of anosilicate phase composition and luminescence properties with the ternary alkaline ion ratio, high-efficiency phosphors are preferred. The internal mechanism of luminescence properties in single-phase and mixed-phase regions is also discussed and component-structure-luminescence properties are established. (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu phosphors were synthesized by high temperature solid-state reaction, a total of 44 samples. By the analysis of binary and ternary powders’ phase constitutions and the luminescent spectra, the phases and the ultraviolet excitation luminescence CIE values were obtained. The experimental results showed that the phases of (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu is gradually changed with compositions, Ba2SiO4-phase region is formed on the Ba-rich corner(the maximum amount of Sr is 35%, and Mg is 30%). The lattices of Ba2SiO4-phase powder decrease and the crystallines increase as the Sr2+ and Mg2+ content increasing. (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu phosphors also have a gradually changing in photoluminescent color and intensity under the ultraviolet excitation. Ba2SiO4-phase powders are green phosphors and the intensity increases with Sr2+ or Mg2+ substitution. High resolution emission spectra indicate that Sr2+ or Mg2+ substitution promotes Eu2+ in taking place of Ba2+(I)(the relative higher luminescent efficiency site).The binary series of Mg2SiO4-Sr2SiO4 matrix powders activated by Eu ion are red phosphors. The other mixture-phase phosphors would gradually change from green to red as decreasing of Ba content (Eu ion trends to be +3 for coordination space gradually decreaseses). For (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu series, relationship both the structure and luminescent properties changes with composition. Profiting from the essence of the phase diagram, a ternary color image could be created, and used to screen the candidates. It should be an efficient and systematic approach to make the phosphor discovering(optimized green and red phosphor sample points are: ((Mg0.3Ba0.65Sr0.05)1.95SiO4∶0.05Eu and (Mg0.65Sr0.35)1.95SiO4∶0.05Eu).

汪雨, 罗岚, 郭锐, 孙传耀, 高明远. 基于相图原理定量预测(Mg1-x-yBaxSry)1.95SiO4∶0.05Eu系列荧光粉的结构和发光性能[J]. 发光学报, 2019, 40(12): 1494. WANG Yu, LUO Lan, GUO Rui, SUN Chuan-yao, GAO Ming-yuan. Quantitative Prediction of Structure and Luminescent Properties of (Mg1-x-yBaxSry)1.95SiO4∶0.05Eu via Phase Diagram Approach[J]. Chinese Journal of Luminescence, 2019, 40(12): 1494.

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