应用化学 ›› 2021, Vol. 38 ›› Issue (11): 1469-1478.DOI: 10.19894/j.issn.1000-0518.210119

• 研究论文 • 上一篇    下一篇

单一基质白光荧光粉Na3Sc2(PO4)3∶Tm3+,Dy3+的合成及发光性质

王森1,2,4, 庞然1, 李达1*, 李成宇1,2*, 张洪杰1,3   

  1. 1中国科学院长春应用化学研究所,稀土资源利用国家重点实验室,长春 130022;
    2中国科学技术大学,合肥 230026;
    3广东粤港澳大湾区国家纳米科技创新研究院,广州 510535;
    4中科稀土(长春)有限责任公司,长春 130000
  • 收稿日期:2021-03-16 接受日期:2021-06-09 出版日期:2021-11-01 发布日期:2022-01-01
  • 通讯作者: *E-mail:lida2185@ciac.ac.cn; cyli@ciac.ac.cn
  • 基金资助:
    国家重点研究开发项目(No.2019YFA0709101)、自然科学基金青年科学基金(No.51902305)和广东省重点领域研发项目(No.2020B0101010001)资助

Synthesis and Luminescence Properties of a Single-Phase White-Emitting and Tunable Color Phosphor Na3Sc2(PO4)3∶Tm3+,Dy3+

WANG Sen1,2,4, PANG Ran1, LI Da1*, LI Cheng-Yu1,2*, ZHANG Hong-Jie1,3   

  1. 1State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences, Changchun 130022, China;
    2University of Science and Technology of China, Hefei 230026, China;
    3The GBA National Institute for Nanotechnology Innovation, Guangzhou, 510535, China;
    4Zhongke Rare Earth (Changchun) Co., Ltd, Changchun 130000, China
  • Received:2021-03-16 Accepted:2021-06-09 Published:2021-11-01 Online:2022-01-01
  • Supported by:
    National Key R&D Program of China (No.2019YFA0709101), the National Natural Science Foundation of China (No.51902305) and the Project in Key Areas of Guangdong Province (No.2020B0101010001)

摘要: 采用高温固相法成功制备了Na3Sc2-x-y(PO4)3xTm3+,yDy3+荧光粉,利用X射线衍射仪、扫描电子显微镜和荧光光谱仪对荧光粉进行了物相、形貌和发光性能进行了表征。 在Na3Sc2(PO4)3∶0.06Tm3+,yDy3+荧光粉中,物质的量分数6%的Tm3+和6%的Dy3+在360 nm激发下呈现出白光发射,其发射光谱在460~685 nm范围内存在Tm3+位于457 nm的特征发射峰,对应于Tm3+3H61D2跃迁,以及Dy3+位于483、577和672 nm处的3个特征发射峰,分别对应于Dy3+4F9/26H15/24F9/26H13/24F9/26H11/2的跃迁。 观测到Na3Sc2(PO4)3∶Tm3+荧光粉的发射光谱与Na3Sc2(PO4)3∶Dy3+的激发光谱有较好的重叠,且Tm3+的荧光寿命随Dy3+浓度的增加逐渐降低,因此在Na3Sc2(PO4)3∶Tm3+,Dy3+荧光粉中存在Tm3+向Dy3+的能量传递。 利用Dexter和Reisfeld近似分析了能量转移机制,发现从Tm3+到Dy3+的能量传递临界距离为1.6 nm,能量传递过程是通过偶极-偶极相互作用进行的。 Na3Sc2(PO4)3∶0.06Tm3+,0.06Dy3+荧光粉具有较好的耐受热猝灭性能,在423、473和523 K时的发射强度分别为298 K时发射强度的97.6%、89.2%和78.6%。 随着Dy3+浓度的增加,Na3Sc2(PO4)3∶0.06Tm3+,yDy3+荧光粉的发光颜色由蓝色转变为白色,再由白色变黄色。 Na3Sc2(PO4)3∶Tm3+,Dy3+荧光粉作为一种可调色或单相白光荧光粉在发光二极管上具有潜在的应用前景。

关键词: 白光荧光粉, 耐热稳定性, 发光二极管

Abstract: A series of NSPO∶0.06Tm3+, yDy3+(y=0~0.10) phosphors were synthesized by the high-temperature solid-state method, and their phase, morphology and luminescent properties of the phosphors were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and fluorescence spectrometer. Under the excitation of 360 nm, the photoluminescence (PL) spectrum of Na3Sc2(PO4)3∶Tm3+,Dy3+ shows the Tm3+ characteristic emission peak at 457 nm and three characteristic emission peaks of Dy3+ at 483, 577, and 672 nm, respectively. There is an energy transfer from Tm3+ to Dy3+ ion in Na3Sc2(PO4)3∶Tm3+,Dy3+ phosphor due to the good overlap between the emission spectrum of Na3Sc2(PO4)3∶Tm3+ and the excitation spectrum of Na3Sc2(PO4)3∶Dy3+, which is further confirmed by the fluorescence lifetime decrease of Tm3+ ion with the increase of Dy3+ concentration. The process of energy transfer is via dipole-dipole interaction which is confirmed by applying Dexter and Reisfeld's theory. By increasing the Dy3+ concentration, the color coordinates of the Na3Sc2(PO4)3∶0.06Tm3+,yDy3+ phosphors could be adjusted from blue to white, and then to yellow. The Na3Sc2(PO4)3∶0.06Tm3+,0.06Dy3+ phosphor shows fairly good resistance to thermal quenching with a high preservation of the emission intensities of 97.6%, 89.2% and 78.6% at 423, 473 and 523 K, respectively. These results suggest that the Na3Sc2(PO4)3∶Tm3+,Dy3+ phosphors have potential applications as the color-tunable or a single-phase white emitting phosphor in white light-emitting diodes (LEDs).

Key words: White phosphor, Thermal quenching, Light-emitting diodes

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