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Co-substitution Strategy to Improve the Luminescence Property of NaLaCaTeO6:Eu3+ Phosphor and Its Application in White Light Emitting Diode
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Bing ZHAO1, Jingjing RU1, Feiyun GUO2, Shiying GUO1
Journal of the Chinese Ceramic Society | 2025, 53(2) : 257 - 266
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Journal of the Chinese Ceramic Society | 2025, 53(2): 257-266
• Research Article •
Co-substitution Strategy to Improve the Luminescence Property of NaLaCaTeO6:Eu3+ Phosphor and Its Application in White Light Emitting Diode
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Bing ZHAO1, Jingjing RU1, Feiyun GUO2, Shiying GUO1
Affiliations
  • 1.Fujian Province University Key Laboratory of Green Energy and Environment Catalysis, Ningde Normal University, Ningde 352100, Fujian, China
  • 2.College of Chemistry, Fuzhou University, Fuzhou 350108, China
  • ZHAO Bing (1982-), male, Master, Associate Professor. E-mail:

About Author:

ZHAO Bing (1982-), male, Master, Associate Professor. E-mail:

Published: 2025-02-20 doi: 10.14062/j.issn.0454-5648.20240386
Outline
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Introduction

As a high-quality light source, the performance of phosphor-converted white light emitting diodes (pc-WLEDs) is closely related to the performance of the selected luminescent materials. The traditional method of combining blue LED chips and yellow phosphors to generate white light has problems of low color rendering index and high color temperature. To address the pressing requirements of lighting and display technologies, the development of novel red phosphors with high efficiency and excellent thermal stability is urgent. Perovskite tellurites have attracted extensive attention due to their elemental diversity and structural tunability. Based on the double perovskite Ca3TeO6, a series of NaLaCaTeO6:xEu3+ phosphors that can be effectively excited by near-ultraviolet light have been designed and synthesized by elemental design. Through a co-substitution strategy of [Na+-La3+] substitution of [Ca2+-Ca2+] ion pair, the problem of low Eu3+ doping concentration in Ca3TeO6:Eu3+ is effectively improved by regulating the matrix structure. Meanwhile, the luminous intensity and thermal stability of the sample were also significantly improved.

Methods

Series of NLCT:xEu3+ (0.05 ≤ x ≤ 1.0) samples were successfully synthesized by a high-temperature solid-state reaction. The stoichiometric amounts of raw materials, including Na2CO3 (105.99 g/mol, 99.9%), CaCO3 (100.09 g/mol, 99.9%), TeO2 (159.6 g/mol, 99.99%), La2O3 (325.84 g/mol, 99.99%) and Eu2O3 (351.93 g/mol, 99.99%) purchased from Shanghai Aladdin Biochemical Technology Co., Ltd., were weighed and grounded into homogeneous powder for 30 min. Afterward, the obtained powder was put into crucibles and heated at 1473 K for 12 h in a muffle furnace. Eventually, the target substances were obtained after cooling down and grinding again. A red LED device was assembled using the NLCT:0.6Eu3+ phosphor with a 395 nm chip. The WLED device was fabricated by connecting tricolor phosphors including BaMgAl10O17:Eu2+ (BAM:Eu2+, blue), (Ba, Sr)2SiO4:Eu2+ (BSS:Eu2+, green), along with the prepared NLCT:0.6Eu3+ (red) with a 395 nm chip.

Results and discussion

The results of XRD patterns showed that [Na+-La3+] substituted the [Ca2+-Ca2+] ion pair, which did not affect the structure of the sample. The diffraction peaks of the samples with x = 0.1-0.6 did not show obvious impurity peaks, indicating that the synthesized samples were pure phases. Eu3+ ions tended to occupy the site of La in the matrix rather than Te. DRS results also confirmed that Eu3+ ions were successfully introduced into the NLCT matrix. The dominant absorption peak at 395 nm matches well with InGaN-based LED, and the emission intensity reaches the maximum at x = 0.6. The primary mechanism among Eu3+ ions in NLCT:xEu3+ samples was proved to the dipole-dipole interaction.

The luminous intensity of the prepared NLCT:0.6Eu3+ red phosphor is about 1.98 and 3.97 times than that of CT:0.2Eu3+ and Y2O3:Eu3+, confirming the feasibility of the co-substitution strategy. The internal quantum yield and color purity of NLCT:0.6Eu3+ are 67.6% and 99.87%, respectively. The CIE color coordinates of this sample (0.658 1, 0.341 0) are closer to the ideal red point (0.670, 0.330) than that of the purchased commercial red phosphor Y2O3:Eu3+. Compared with CT:0.2Eu3+ (about 77.5%), the thermal stability of NLCT:0.6Eu3+ is significantly improved. When the temperature rises to 420 K, the emission intensity at 616 nm remains 91.7% of that at 300 K. Furthermore, the sample exhibits excellent color stability by the CIE coordinates shifting only slightly from (0.658 2, 0.340 8) to (0.646 6, 0.351 9) with increasing temperature. The CCT and Ra of the prepared WLED device are 6215 K and 80.6, respectively, and the CIE coordinates (0.317 6, 0.334 0) are located in the white light region.

Conclusions

A series of innovative NaLaCaTeO6:xEu3+ phosphors were synthesized using a high temperature solid-state reaction method. Under 395 nm excitation, the NaLaCaTeO6:Eu3+ samples exhibit a strong red emission at 616 nm (5D0→7F2) of Eu3+ ions. Through a co-substitution strategy where [Na+-La3+] replaced the [Ca2+-Ca2+] ion pair, the optimized doping concentration of the NaLaCaTeO6:xEu3+ is elevated to 60% (molar fractior), leading to exceptional color purity and high internal quantum efficiency reaching 99.87% and 67.60%, respectively. Furthermore, compared to the Ca3TeO6:0.2Eu3+ sample pre-substitution, the luminous intensity and thermal stability of NaLaCaTeO6:0.6Eu3+ phosphor witness a notable increase. Even at 420 K, the emission intensity remains at 91.7% compared to 300 K. The resultant WLED displays a color rendering index Ra of 80.6 and CIE chromaticity coordinates of (0.317 6, 0.334 0), underscoring the broad application potential of NaLaCaTeO6:0.6Eu3+ in solid-state lighting.

co-substitution  /  luminescence  /  phosphors  /  thermal stability
赵兵, 茹晶晶, 郭飞云, 郭诗莹. 共取代策略增强NaLaCaTeO6:Eu3+的发光性能及在白光发光二极管中的应用. 硅酸盐学报, 2025 , 53 (2) : 257 -266 . DOI: 10.14062/j.issn.0454-5648.20240386
Bing ZHAO, Jingjing RU, Feiyun GUO, Shiying GUO. Co-substitution Strategy to Improve the Luminescence Property of NaLaCaTeO6:Eu3+ Phosphor and Its Application in White Light Emitting Diode[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (2) : 257 -266 . DOI: 10.14062/j.issn.0454-5648.20240386
Year 2025 volume 53 Issue 2
21
7
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Article Info
doi: 10.14062/j.issn.0454-5648.20240386
  • Receive Date:2024-06-03
  • Online Date:2026-10-22
  • Published:2025-02-20
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History
  • Received:2024-06-03
  • Revised:2024-06-28
Funding
Affiliations
    1.Fujian Province University Key Laboratory of Green Energy and Environment Catalysis, Ningde Normal University, Ningde 352100, Fujian, China
    2.College of Chemistry, Fuzhou University, Fuzhou 350108, China

Corresponding:

RU Jingjing (1983-), female, Ph.D., Senior Experimentalist. E-mail:
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表12种不同金属材料的力学参数
科
Family
属数
Number of
genus
种数
Number of
species
占总种数比例
Percentage of
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属
Genus
种数
Number of
species
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Percentage of total
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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