白光发光二极管用几种典型氮（氧）化物荧光材料的制备及其发光性能的研究
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摘要
作为一类新型的白光发光二极管用荧光转换材料,氮(氧)化物因其丰富的发光颜色、较高的荧光转换效率、稳定的化学-物理性质以及较小的热猝灭性能,近年来备受关注。但是,相对于氧化物荧光材料来说,氮(氧)化物的研究还处于起步阶段。本论文针对目前氮(氧)化物荧光材料的研究中存在的主要问题,从三个方面展开研究：
1.通过Al、Ga对典型硅基氮氧化物CaSi2O2N2:Eu2+晶体非金属层[Si2O2N2]2-中Si的部分替代对样品的光谱性能进行了调节与改善,探索了其中的光谱峰位移动以及发光强度提高的机理,结果表明：样品的光谱调控可以通过这种阴离子基团杂化的方式实现；此外,通过改变激活剂配位多面体的大小、对称性,减小激活剂离子进入基质晶格后的失配度,减弱其周围的晶格应变力,可以增加其在基质晶格中的稳定性,从而提高激活剂离子融入基质晶格中的几率,使荧光材料的发射强度增强。
2.选用空气中稳定、简单易得的α-Si3N4、SrCO3、SiO2和Eu203为原料,在1400-1500℃、NH3-N2保护下制备合成了一种性能突出的新型红色硅基氮氧化物荧光材料Sr2SiNzO4-1.5z:Eu2+(0.7 3.通过对氮化硼基氮(氧)化物的制备和研究,提出了一种可用于较低温度、常压下制备氮(氧)化物荧光材料的方法。(1)在700-900℃,空气气氛,常压下,获得无稀土掺杂的BCNO:Al氮氧化物荧光材料。该材料在紫外和蓝光区均有较强的吸收,可被LED紫外或蓝光芯片有效激发：通过原料配比、制备条件的调控,BCNO:Al氮氧化物发光颜色从蓝光到橙红光可调,量子效率最高可达74.7%。(2)通过制备方法的探索和改进,采用了较为简便的两步合成方案,在较低温度、常压、无模板剂和催化剂的条件下,成功合成了大量具有六边形形貌、径向尺寸300-500nm、厚度～30nm的h-BN纳米片。该方案拓展了可用于在低温、常压下制备细小颗粒、均匀分布的氮化物发光材料的合成方法。
(Oxy)nitride phosphors, as a new class of luminescent materials for use in white LED, have received significant attention in recent years, due to their abundant emission colors, high conversion efficiency, high physical-chemical stability, as well as their low thermal quenching. However, compared with oxide phosphors, the study of (oxy)nitrides is at an early stage. In this paper, focus on the problems of the existing research on the nitride/oxynitride phosphors, the researches have been carried out in three aspects:
1. Luminescence spectra have been tuned and improved by simultaneous equivalent substitution of Al or Ga for Si in the anion [Si2O2N2]2-layer of typical oxynitride CaSi2O2N2:Eu2+. And the mechanism of the spectra shift and the luminescence intensity increasing have been explored. It indicated that the anion substitution is the other choice to tune the emission color, shift their excitation and emission bands. In addition, the photoluminescence intensity or the intensity of the emission maximum could be strengthen by reducing the lattice mismatch between the activator ions and the replaced host crystal ions and increase the critical dopant concentration of Eu+.
2. A novel remarkable red oxonitridosilicate phosphor Sr2SiNzO4-1.5z:Eu2+(0.7 3. A viable method for the production of (oxy)nitride phosphors with fine and well-dispersed powders at relatively low temperatures under ambient atmospheric pressure have been developed during the synthesis and investigation of the BN-based (oxy)nitride phosphors.(1) The oxynitride phosphors, which is composed of BCNO: Al without rare earth ions, have been synthesized at low sintering temperature (700-900℃) under atmospheric pressure. The result indicates that these BCNO:Al phosphors can emit under excitation not only by UV but also blue light; the color emission can be easily tuned from the blue to the orange regions of the photoluminescence spectrum by manipulating both the composition ratios of the raw materials as well as the reaction conditions; and with high quantum efficiency, i.e.,74.7%.(2) Large quantities of h-BN nanoplates with hexagonal morphologies have been successfully prepared by a facile template-and catalyst-free two-step method, which was carried out at comparatively low-temperature and under normal pressure conditions. The synthesized nanoplates have diameters of300-500nm and the thickness is about30nm. This two-step facile route developed the methods for growing nanosize nitride phosphors with uniform size distribution at relatively low temperatures under ambient atmospheric pressure.
1.通过Al、Ga对典型硅基氮氧化物CaSi2O2N2:Eu2+晶体非金属层[Si2O2N2]2-中Si的部分替代对样品的光谱性能进行了调节与改善,探索了其中的光谱峰位移动以及发光强度提高的机理,结果表明：样品的光谱调控可以通过这种阴离子基团杂化的方式实现；此外,通过改变激活剂配位多面体的大小、对称性,减小激活剂离子进入基质晶格后的失配度,减弱其周围的晶格应变力,可以增加其在基质晶格中的稳定性,从而提高激活剂离子融入基质晶格中的几率,使荧光材料的发射强度增强。
2.选用空气中稳定、简单易得的α-Si3N4、SrCO3、SiO2和Eu203为原料,在1400-1500℃、NH3-N2保护下制备合成了一种性能突出的新型红色硅基氮氧化物荧光材料Sr2SiNzO4-1.5z:Eu2+(0.7
(Oxy)nitride phosphors, as a new class of luminescent materials for use in white LED, have received significant attention in recent years, due to their abundant emission colors, high conversion efficiency, high physical-chemical stability, as well as their low thermal quenching. However, compared with oxide phosphors, the study of (oxy)nitrides is at an early stage. In this paper, focus on the problems of the existing research on the nitride/oxynitride phosphors, the researches have been carried out in three aspects:
1. Luminescence spectra have been tuned and improved by simultaneous equivalent substitution of Al or Ga for Si in the anion [Si2O2N2]2-layer of typical oxynitride CaSi2O2N2:Eu2+. And the mechanism of the spectra shift and the luminescence intensity increasing have been explored. It indicated that the anion substitution is the other choice to tune the emission color, shift their excitation and emission bands. In addition, the photoluminescence intensity or the intensity of the emission maximum could be strengthen by reducing the lattice mismatch between the activator ions and the replaced host crystal ions and increase the critical dopant concentration of Eu+.
2. A novel remarkable red oxonitridosilicate phosphor Sr2SiNzO4-1.5z:Eu2+(0.7
引文
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