Si3N4掺杂氮化对Sr3SiO5:Eu2+荧光粉发光性能的影响

doi:10.15541/jim20160327

无机材料学报 ›› 2017, Vol. 32 ›› Issue (3): 252-256.DOI: 10.15541/jim20160327

Si₃N₄掺杂氮化对Sr₃SiO₅:Eu²⁺荧光粉发光性能的影响

张双双, 田文郁, 张建新, 宋开新, 秦会斌

(杭州电子科技大学新型电子器件与应用研究所, 杭州 310018)

收稿日期:2016-05-19 修回日期:2016-09-12 出版日期:2017-03-20 网络出版日期:2017-02-24
作者简介:张双双(1989－), 女, 硕士研究生. E-mail: 774032628@qq.com
基金资助:
浙江省公益性技术应用研究计划资助项目(2016C31110) Zhejiang Public Welfare Technology Application Research Project (2016C31110)

Luminescence Properties of Si₃N₄ Doped Nitride Sr₃SiO₅: Eu²⁺ Phosphor

ZHANG Shuang-Shuang, TIAN Wen-Yu, ZHANG Jian-Xin, SONG Kai-Xin, QIN Hui-Bin

(Institute of Electron Device &Application, Hangzhou Dianzi University,Hangzhou 310018, China)

Received:2016-05-19 Revised:2016-09-12 Published:2017-03-20 Online:2017-02-24
About author:ZHANG Shuang-Shuang. E-mail: 774032628@qq.com

摘要/Abstract

摘要：

采用高温固相法制备Si₃N₄掺杂氮化Sr_2.99SiO_5-6xN_4x:0.01Eu²⁺荧光粉。采用XRD、EDS和SEM测试结果表明: N^3-进入Sr₃SiO₅基质晶格中取代部分O^2-离子, 形成了单一相Sr_2.99SiO_5-6_xN₄_x:0.01Eu²⁺固溶体。PL&PLE荧光光谱测试结果显示, Sr_2.99SiO_5-6_xN₄_x:0.01Eu²⁺荧光粉在344nm紫外光的激发下发射出红橙光, 属于Eu²⁺离子典型的 4f⁶5d¹→4f⁷电子跃迁。随着N浓度的增加, Sr_2.99SiO_5-6_xN₄_x:0.01Eu²⁺荧光粉发射光谱和激发光谱的强度明显增强。热稳定性测试结果表明, Si₃N₄掺杂氮化能够显著提高Sr₃SiO₅:Eu²⁺荧光粉的热稳定性。通过Arrhennius模型拟合结果表明横向穿越过程(crossover)引起的Sr₃SiO₅:Eu²⁺荧光粉氮化前后的温度猝灭。

关键词: Sr3SiO5:Eu2+, 荧光粉, Si3N4

Abstract:

Si₃N₄ doped Sr_2.99SiO_5-6_xN₄_x:0.01Eu²⁺ phosphorssampless were prepared by high temperature solid-state reaction method. Testing results of XRD, EDS and CHNS of the phosphor samples demonstrated that the nitrogen atoms could be incorporated into the host lattice of Sr₃SiO₅ through partial occupation of the oxygen atoms sites to form Sr_2.99SiO_5-6_xN₄_x:0.01Eu²⁺solid solution. Under the excitation of 344 nm ultraviolet, the Sr_2.99SiO_5-6_xN₄_x: 0.01Eu²⁺ phosphor samples emit orange lights peaked at 580 nm, which originates from 4f⁶5d¹→4f⁷ transitions of Eu²⁺ ions. With the increase of N³⁺-ions concentration, the intensities of emission and excitation spectra of Sr_2.99SiO_5-6_xN₄_x: 0.01Eu²⁺ phosphor samples are obviously enhanced. The thermal stability testing results of the phosphor samples show that the incorporation of N^3-ions significantly improve the thermal stability better than that of undoped samples. The curves analyzed and fitted by the Arrhennius formula model indicate that the quenching temperature is caused by crossover process.

Key words: Sr3SiO5, phosphors, Si3N4

中图分类号:

O482

张双双, 田文郁, 张建新, 宋开新, 秦会斌. Si₃N₄掺杂氮化对Sr₃SiO₅:Eu²⁺荧光粉发光性能的影响[J]. 无机材料学报, 2017, 32(3): 252-256.

ZHANG Shuang-Shuang, TIAN Wen-Yu, ZHANG Jian-Xin, SONG Kai-Xin, QIN Hui-Bin. Luminescence Properties of Si₃N₄ Doped Nitride Sr₃SiO₅: Eu²⁺ Phosphor[J]. Journal of Inorganic Materials, 2017, 32(3): 252-256.

图/表 8

图1 Sr2.99SiO5-6xN4x:0.01Eu2+荧光粉的XRD图谱

Fig. 1 XRD patterns of Sr2.99SiO5-6xN4x:0.01Eu2+ phosphors

图2 Sr2.99SiO5-6xN4x:0.01Eu2+(x= 0 , 0.1, 0.2和0.3)样品的SEM照片

Fig. 2 SEM images of Sr2.99SiO5-6xN4x:0.01Eu2+(x= 0 , 0.1, 0.2 and 0.3)

图3 Sr2.99SiO5-6xN4x:0.01Eu2+荧光粉样品的EDS图谱

Fig. 3 The EDS of Sr2.99SiO5-6xN4x:0.01Eu2+ (a) x=0; (b) x=0.1

图4 Sr3SiO5:xEu2+荧光粉的发射光谱图

Fig. 4 Emission spectra of Sr3SiO5:xEu2+ phosphors

图5 Sr2.99SiO5-6xN4x:0.01Eu2+(x = 0, 0.05, 0,1, 0,2, 0.3)荧光粉的激发(a)和发射(b)光谱图

Fig. 5 Excitation (a) and emission (b) spectra of Sr2.99SiO5-6xN4x:0.01 Eu2+ (x = 0, 0.05, 0,1, 0,2, 0.3)

图6 Sr2.99SiO5-6xN4x:0.01Eu2+荧光粉的热稳定性

Fig. 6 Thermostability pattern of Sr2.99SiO5-6xN4x:0.01Eu2+ phosphors as function of x

图7 热猝灭位形坐标图

Fig. 7 Coordinate figure of thermal quenching

图8 Sr2.99SiO5-6xN4x:0.01Eu2+荧光粉的热稳定性Arrhennius公式非线性拟合图

Fig. 8 Thermostability fitting curve of Sr2.99SiO5-6xN4x: 0.01Eu2+ phosphors by using Arrhennius equation

参考文献 11

[1]	洪广言. 稀土发光材料—基础与应用. 科学出版社, 2011: 224-225.
[2]	NAKAMURA S, MUKAI T, SENOH M.Candela class high brightness InGaN/AlGaN double heterostructure blue light emitting diodes.Applied Physics Letters, 1994, 64(13): 1687-1689.
[3]	EUN-HEE KANG, SUNG-WOO CHOI, SU EUN CHUNG, et al.Photoluminescence characteristics of Sr3SiO5:Eu2+ yellow phosphors synthesized by solid-state method and pechini process.Journal of the Electrochemical Society, 2011, 158(11): J330-J333.
[4]	LAKSHMINARASIMHAN N, VARADARAJU U V.White-light generation in Sr2SiO4: Eu2+, Ce3+ under near-UV excitation a novel phosphor for solid-state lighting.Journal of the Electrochemical Society, 2005, 152(9): H152-H156.
[5]	SONG KAIXIN, ZHANG FANGFANG, CHEN DAQIN, et al.Enhancement of photoluminescence properties and modification of crystal structures of Si3N4 doping Li2Sr0.995SiO4:0.005Eu2+ phosphors.Materials Research Bulletin, 2015, 70: 309-314.
[6]	CHEN LEI, LIN CHUN-CHE, LIN CHIAO-WEN, et al.Light converting inorganicphosphors for white light-emitting diodes.Materials, 2010, 3(3): 2172-2195.
[7]	PHILIPPE F, SMET KOEN, VAN DEN EECKHOUT, et al.Temperature and wavelength dependent trap filling in M2Si5N8:Eu (M = Ca, Sr, Ba) persistent phosphors.Journal of Luminescence, 2012, 132: 682-689.
[8]	SEIBALD M, ROSENTHAL T, OECKLER O, et al.Unexpected luminescence properties of Sr0.25Ba0.75Si2O2N2:Eu2+-a narrow blue emitting oxonitridosilicate with cation ordering. Chemistry-A European Journal, 2012, 18(42): 13446-13452.
[9]	LI Y Q, FANG Y, HIROSAKI N, et al.Crystal and electronic structures, photoluminescence properties of Eu2+-doped novel oxynitride Ba4Si6O16-3x/2Nx.Materials, 2010, 3(3): 1692-1708.
[10]	WANG MEIYUAN, ZHANG XIA, HAO ZHENDONG, et al.Enhanced phosphorescence in N contained Ba2SiO4:Eu2+for X-ray and cathode ray tubes.Optical Materials, 2010, 32(9): 1042-1045.
[11]	TIAN Y, CHEN B J, HUA R, et al.Self-assembled 3D flowersh aped NaY(WO4)2:Eu3+microarchitectures: microwaveassisted hydrothermal synthesis, growth mechanism and luminescent properties.Cryst. Eng. Comm., 2012, 14(5): 1760-1769.

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Si₃N₄掺杂氮化对Sr₃SiO₅:Eu²⁺荧光粉发光性能的影响

Luminescence Properties of Si₃N₄ Doped Nitride Sr₃SiO₅: Eu²⁺ Phosphor

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