Eu～（2+）激活碱土金属铝硅酸盐发光材料的研究
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摘要
本论文针对目前各发光材料的发光颜色单一、亮度不高、稳定性差等特点，旨在开发出一种全新型的发光材料。通过高温固相法合成了一系列Eu~(2+)激活的碱土金属铝硅酸盐发光材料MeAl_2Si_2O_8：Eu~(2+)，Dy~(3+)(Me=Mg，Ca，Sr，Ba)。X射线衍射分析表明，此类发光材料基质的主要物相组成为物理与化学性能稳定的长石结构硅酸盐。结合荧光光谱、差热-热重、红外光谱及扫描电镜等现代分析测试手段，研究了Mg~(2+)取代长石结构中部分阳离子，及掺杂Dy~(3+)、Nd~(3+)、Mn~(2+)等与Eu~(2+)形成共激活对晶体结构和发光性能的影响。
研究发现，Eu~(2+)激活的长石基发光材料均有很好的发光性能，发光颜色白色发光，发光亮度高。通过Eu~(2+)和Mn~(2+)之间的能量传递，可得到较纯的白色发光，且呈现出较长的余辉寿命。
Eu~(2+)激活的碱土金属铝硅酸盐作为发光材料基质具有物理和化学性质稳定性好，发光强度大等特点，在陶瓷发光釉料、大功率LED照明等领域必将开辟一片出诱人的新天地。
The object of this paper is to develop a kind of new phosphor in order to overcome the shortcoming of present luminescent materials such as single luminescence color, low luminosity, low stability, etc. A series of Eu -actived alkaline-earth metals aluminasilicate phosphors, which is MeAl_2Si_2O_8: Eu~(2+), Dy~(3+) (Me=Mg, Ca, Sr, Ba), have been synthesized through high temperature solid-phase method. X-ray diffraction analysis indicate that the main constitutes of the hot phase of this kind of materials are feldspar whose physical and chemical performance are fairly stable. By means of modern analysis and testing tools such as flurescence spectrum, TG-DTA, FTIR and SEM, the influence of some aspects to the crystal constitution and luminescence performance of materials have been investigated, such as the substitution of parts of cation of feldspar for Mg~(2+) and adulterating cations, for example, Dy~(3+) Nd~(3+) Mn~(2+) ions, to active luminescence ions in materials together with Eu~(2+) ion. It was found that all of Eu~(2+)-actived feldspar radix-phase luminescence materials have good luminescence performance which can emit white and high brightness light, and pure white light can be gained through energy transfer between Eu~(2+) and Mn~(2+)ions and its afterglow is fairly long.
Eu~(2+)-actived alkaline-earth metals aluminasilicate phosphors have many good characteristic such as stable physical and chemical property and high luminescence strength. And it shows great possibility for application in fields such as luminescent ceramic glaze and high-power LED illumination.
研究发现，Eu~(2+)激活的长石基发光材料均有很好的发光性能，发光颜色白色发光，发光亮度高。通过Eu~(2+)和Mn~(2+)之间的能量传递，可得到较纯的白色发光，且呈现出较长的余辉寿命。
Eu~(2+)激活的碱土金属铝硅酸盐作为发光材料基质具有物理和化学性质稳定性好，发光强度大等特点，在陶瓷发光釉料、大功率LED照明等领域必将开辟一片出诱人的新天地。
The object of this paper is to develop a kind of new phosphor in order to overcome the shortcoming of present luminescent materials such as single luminescence color, low luminosity, low stability, etc. A series of Eu -actived alkaline-earth metals aluminasilicate phosphors, which is MeAl_2Si_2O_8: Eu~(2+), Dy~(3+) (Me=Mg, Ca, Sr, Ba), have been synthesized through high temperature solid-phase method. X-ray diffraction analysis indicate that the main constitutes of the hot phase of this kind of materials are feldspar whose physical and chemical performance are fairly stable. By means of modern analysis and testing tools such as flurescence spectrum, TG-DTA, FTIR and SEM, the influence of some aspects to the crystal constitution and luminescence performance of materials have been investigated, such as the substitution of parts of cation of feldspar for Mg~(2+) and adulterating cations, for example, Dy~(3+) Nd~(3+) Mn~(2+) ions, to active luminescence ions in materials together with Eu~(2+) ion. It was found that all of Eu~(2+)-actived feldspar radix-phase luminescence materials have good luminescence performance which can emit white and high brightness light, and pure white light can be gained through energy transfer between Eu~(2+) and Mn~(2+)ions and its afterglow is fairly long.
Eu~(2+)-actived alkaline-earth metals aluminasilicate phosphors have many good characteristic such as stable physical and chemical property and high luminescence strength. And it shows great possibility for application in fields such as luminescent ceramic glaze and high-power LED illumination.
引文
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2 杨吉．矿物及宝石的发光机理和应用．西安工程学院学报[J]．24(3)：44～46
3 张希艳．稀土长余辉发光材料及其应用[M]．长春：吉林科学技术出版社， 2005：19～22
4 石春山，叶泽人．Eu~(2+)在固体中的发光．发光与显示，1982，(4)：1～3
5 《固体发光》编写组．固体发光．吉林：吉林物理所，1976：370～383
6 石春山．关于Eu~(2+)的f→f跃迁．发光与显示．1981，(1)：39～46
7 T.Katsumata, T.Nabae, K. Sasajima, et al. Growth and characteristics of long persistent SrAl_2O_4 - and CaAl_2O_4 - based phosphor crystals by a floating zone techmique. J. of Crystal Growth. 1998, 183 (3) : 361～365
8 W. Lehmann. Activators and co-activators in calcium sulfide phosphors. J. Lumin.[J]. 用1972, 5 (2) : 87～107
9 杨志平，郭智．Y_2O_2S：Eu~(3+)，Mg~(2+)，Ti~(4+)红色材料的制备和长余辉性能发光学报[J]．2004，25(2)：183～187
10 李治霞，张玉奇．CaTiO_3：pr~(3+)红色磷光体余辉性能的改进．重庆大学学报[J]．2004，27(7)：53～55
11 刘正伟，刘应亮．CaWO_4中Eu~(2+)的长余辉发光．无机化学学报[J]．2004，20(12)：1432～1436
12 Jing Wang, Qiang Su ,Shubin Wang. A novel red long phosphorescent(LLP) material β -Zn_3(PO_4)_2: Mn~(2+), Sm~(3+) Material Research Bullitin, 40(2005): 590～598
13 林元华，张中太等．掺杂稀土CaAl_2O_4基发光材料的制备及发光机制．材料工程，2001，8：29～35
14 施朝淑，戚泽明．长余辉(寿命)材料研究的最新进展．无机材料学报[J]．2004，19(5)： 961～969
15 Palilla FC, Albere AK,Tomkus, MR, Fluorescence properties of SrAl_2O_4: Eu~(2+) sputtered films with long phosphorescence, Elextrchem Soc, 1968, 115(6): 642～645
16 宋庆梅，黄锦斐，吴茂钧．铝酸锶铕的合成与发光的研究．发光学报[J]．1991，12(2)：144～149
17 川松尺隆嗣等．日本第248回荧光体同学会讲演预稿，1993，1：1
18 肖志国．蓄光型发光材料及其制品．北京：化学工业出版社，2002：191～209
19 李成宇，苏锵，邱建荣．稀土元素掺杂长余辉发光材料研究的最新进展[J]．发光学报，2003，24(1)：19～27
20 罗昔贤等．新型硅酸盐长余辉发光材料．发光学报[J]，2003，24(2)：165～170
21 肖志国．长余辉夜光材料[P]．中国专利：CN11573 12A，1997-08-20[16]
22 Barry. L.Equilibria and Eu~(2+) luminescence of subsolidus phase bounded by Ba_3MgSi_2O_8, Sr_3MgSi_2O_8, Ca_3MgSi_2O_8 [J]. Electrochem.Soc., 1968, 15(7): 733～738
23 L. Jiang, C. Chang, D.Mao, et al. Luminescent properties of CaMgSi_2O_6 -based phosphors co-doped with different rare earth ions[J]. Journal of Alloys and Compounds. 377 (2004):11～215
24 Yuanhua Lin, et al. Luminescent properties of a new long afterglow Eu~(2+) and Dy~(3+) activated Ca_3MgSi_2O_8 phosphor[J]. Journal of the European Ceramic Society. 21 (2001): 683～685
25 Qin Fei, et al. Luminescent properties of Sr_2MgSi_2O_7 and CazMgSi_2O_7 long lasting phosphor activated by Eu~(2+), Dy~(3+)[J]. Journal of Alloys and Compounds 390(2005): 133～137
26 乔彬，张中太，唐子龙．Eu~(2+)，Mn~(2+)共激活碱土镁硅酸盐基红色荧光粉的发光性能[J]．中国稀土学报，2003，21(2)： 192～195
27 Xiao-Jun Wang, Dongdong Jia. Mn~(2+) actived green, yellow, and red long persistent phosphors[J]. Journal of Luminescence 2003(102-103): 34～37
28 Yingliang Liu, Bingfu Lei, Chunshan Shi. Luminescent Properties of a White Afterglow Phosphor CdSiO_3: Dy~(3+)[J]. Chem. Mater. 2005, 17:2108～2113
29 Chengyu Li, Qiang Su, Shunbin Wang. Multi-color long-lasting phosphorescence in Mn~(2+)-doped ZnO-B_2O_3-SiO_2 glass-ceramics. Materials research Bulletin 37 (2002) : 1443～1449
30 夏志国，孙家跃，杜海燕．Sr4_(4-r)MgrSi_3O_8Cl_4：Eu~(2+)荧光粉的发光特性和晶格环境研究[J]．Journal of Rare Earths，2004，22(3)：370～373
31 孙家跃，夏志国，杜海燕．用碱土氯硅酸盐基稀土光致发光材料的研究[J]．国外建材科技，2004，25(4)：11～13
32 Sho Abe, Kazuyoshi Uematsu, Kenji Toda et al. Luminescent properties of red long persistence phosphors, BaMg_2Si_2O_7: Eu~(2+), Mn~(2+)[J]. Journal of Alloys and Compounds, 2005, 3:1～4
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