硅酸盐学报

用于高功率交流白光发光二极管的半透明GdAGG：Ce-SiO₂玻璃陶瓷的制备、结构和发光性能

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徐祖盛 ¹ , 张瑞 ¹^,² , 覃贤壮 ¹

硅酸盐学报 | 研究论文 2024,52(10): 3291-3300

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硅酸盐学报 |研究论文 2024 , 52 (10) : 3291 -3300

用于高功率交流白光发光二极管的半透明GdAGG：Ce-SiO₂玻璃陶瓷的制备、结构和发光性能

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徐祖盛¹, 张瑞¹^,², 覃贤壮¹

作者信息

^1．桂林理工大学材料科学与工程学院，广西桂林 541004

^2．有色金属及材料加工新技术教育部重点实验室，广西光电材料与器件重点实验室，广西桂林 541004

通讯作者:

张瑞（1986—），男，博士，教授。

作者简介:

徐祖盛（1998—），男，硕士研究生。

Structure and Luminescence Properties of Translucent GdAGG:Ce-SiO₂ Glass Ceramics for High-Power Alternating Current-White Light Emitting Diodes

Zusheng XU¹, Rui ZHANG¹^,², Xianzhuang QIN¹

Affiliations

^1.College of Materials Science and Engineering, Guilin University of Technology, Guilin 541004, Guangxi, China

^2.Key Laboratory of New Processing Technology for Non-ferrous Metals and Materials, Ministry of Education; Guangxi Key Laboratory of Optical and Electronic Materials and Devices, Guilin 541004, Guangxi, China

Corresponding Author:

ZHANG Rui (1986-), male, Ph.D., Professor. E-mail: rzhang@glut.edu.cn

XU Zusheng (1998-), male, Master candidate. E-mail: 2465284805@qq.com

出版时间: 2024-10-20 doi: 10.14062/j.issn.0454-5648.20240143

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摘要

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透明玻璃陶瓷荧光转换材料是高功率固态照明技术领域的研究热点。以非晶SiO₂纳米粉体和Gd_2.94Al₂Ga₃O₁₂：0.06Ce³⁺（GdAGG：Ce）荧光粉为原料，采用低温共烧工艺制备了半透明GdAGG：Ce-SiO₂玻璃陶瓷。结果表明：GdAGG：Ce荧光粉颗粒未受到明显破坏，均匀分散于SiO₂玻璃基体中；玻璃陶瓷保留了GdAGG：Ce荧光粉的发光性能，在450 nm激发下呈现峰值位于536 nm的宽发射带，量子效率约为63%，且荧光热猝灭效应不显著；停止激发后，玻璃陶瓷呈现明亮的黄绿色余辉，余辉强度衰减到初始强度80%时的寿命约为27 ms；将玻璃陶瓷与450 nm蓝光芯片或激光器耦合，所得白光发光二极管器件在150 mA直流电驱动下的光效为81.7 lm/W、色温为5 805 K、显色指数为70.8，在交流电驱动下的闪烁指数降低为68.9%，所得白光激光器件的光效为132.6 lm/W、色温为6 528 K、显色指数为70.6；因此，GdAGG：Ce-SiO₂玻璃陶瓷是一种优良的交流白光发光二极管用荧光转换材料。

关键词

玻璃陶瓷 / 低温共烧法 / 发光性能 / 交流白光发光二极管

Abstract

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Introduction

White light emitting diodes directly driven by alternating current (AC-LEDs) become increasingly popular in lighting. However, the harmful flicker occurs because the blue LED chips only work over the threshold voltage. Transparent afterglow phosphor-glass composites are thus proposed as excellent color converters to eliminate the flicker. In this paper, Gd_2.94Al₂Ga₃O₁₂:0.06Ce³⁺-SiO₂ (GdAGG:Ce-SiO₂) glass ceramics were prepared via cold isostatic pressing molding and pressureless sintering at a low temperature. The transparency, structures, microscopic morphologies and luminescence properties were investiagted. Besides, the samples were assembled on the commercial blue LED chips or blue laser diodes (LDs) to explore the potential application.

Methods

For the preparation of GdAGG:Ce phosphor, stoichiometric Gd₂O₃, Al₂O₃, Ga₂O₃ and CeF₃ (99.9%) were weighed and placed in a mortar. After fully ground for 30 min, the obtained powder was transferred into a 20 mL corundum boat and placed in a tube furnace. The gas flow of 95%N₂/5%H₂ (in volume ratio) was introduced, and the temperature was hold at 1 450 ℃ for 4 h. After cooling to room temperature, the powder was ground in a mortar.

For the preparation of GdAGG:Ce-SiO₂ glass ceramics, 0.9 g GdAGG:Ce phosphor and 9.1 g amorphous SiO₂ nanoparticles were weighed and fully ground in a mortar for 30 min. The obtained powder was sieved with a 200 mesh standard sieve. Then, 0.8 g sieved powder was poured into a stainless-steel mold with an inner diameter of 20 mm, and pressed at 40 MPa for 30 s. The obtained blocks were placed in a cold isostatic press and kept at 250 MPa for 5 min. The green compacts were sintered in a muffle furnace in air at 600-800 ℃ for 5 h. After cooling down to room temperature, the samples were double-side polished.

For the preparation of lighting devices, Gd₃Al₂Ga₃O₁₂:Ce-SiO₂ glass ceramics of different thicknesses were encapsulated on the surface of 1 W commercial 450 nm LED lamp to assemble white LED devices. Besides, 1.0 mm thick Gd₃Al₂Ga₃O₁₂:Ce-SiO₂ glass ceramic was excited by a power-adjustable 450 nm laser to simulate a reflective white LD device.

Results and discussion

The translucent GdAGG:Ce-SiO₂ glass ceramics are yellowish green, and the color becomes lighter with increasing sintering temperature. The transmittance of glass ceramics (1.0 mm thickness) in the visible region is approximately 60% due to the mismatch of refractive index between GdAGG:Ce phosphor and SiO₂. The X-ray diffraction patterns show that the glass ceramics exhibit both bulge peak of glass phase and diffraction peaks of Gd₃Al₂Ga₃O₁₂ (JCPDS 46-0448). The scanning electron microscopy images and laser scanning confocal microscopy images indicate that GdAGG:Ce phosphor powders with the sizes of 1-10 μm are uniformly dispersed in SiO₂ glass matrix. The transmission electron microscopy image indicates that the interfacial reaction is well suppressed at a low sintering temperature.

Under 450 nm excitation, the glass ceramics show typical Ce³⁺: 5d₁→4f broadband emissions peaked at 536 nm, whose luminescence characteristics are similar to those of GdAGG:Ce phosphor. The luminescent intensity firstly increases and then decreases, reaching the maximum value at 700 ℃. After removing the excitation source, the glass ceramics show a bright yellowish green afterglow. The longest afterglow appears from GdAGG:Ce-SiO₂ glass ceramic obtained at 700 ℃. Besides, the lifetime when the afterglow intensity decays to 80% of initial one is 27 ms, which meets a requirement of AC-LED devices (no less than 0.4 ms).

The internal quantum efficiency of glass ceramics is 63%, which meets the practical application standard of white LED devices (no less than 60%). The emission intensity at 150 ℃ maintains 85.3% of that at room temperature, indicating that the glass ceramics have an excellent thermal stability.

In coupling the glass ceramic with a 450 nm blue chip, the resulting white LED device exhibits a luminous efficiency (LE) of 81.7 lm/W, a correlated color temperature (CCT) of 5 805 K and a color rendering index (CRI) of 70.8 when driven by 150 mA direct current (DC). Besides, the flicker index decreases to 68.9% when driven via alternating current (AC). Coupled with a 450 nm blue laser, the white LD device shows the LE of 132.6 lm/W, the CCT of 6 528 K and the CRI of 70.6.

Conclusions

Translucent GdAGG:Ce-SiO₂ glass-ceramics were prepared via cold isostatic pressing and low temperature sintering (i.e., 700 ℃/5 h). The self-made GdAGG:Ce afterglow phosphor was uniformly embedded in SiO₂ glass matrix. The glass ceramic retained the luminescent properties of GdAGG:Ce phosphor due to little interfacial reaction. The glass ceramic exhibited a broad emission band peaked at 536 nm, whose quantum efficiency was 63% after excited at 450 nm. The emission intensity at 150 ℃ was 85.3% of that at room temperature. Besides, the glass ceramic exhibited a bright yellowish green afterglow, and the lifetime was 27 ms when the intensity decayed to 80% of initial one. The glass ceramic based white LED device had the LE of 81.7 lm/W, the CCT of 5 805 K, and the CRI of 70.8 when driven by 150 mA DC, and the flicker index reduced to 68.9% when driven by AC. The white LD device showed the LE of 132.6 lm/W, the CCT of 6 528 K and the CRI of 70.6. The results indicated that GdAGG:Ce-SiO₂ glass-ceramic could have a great application potential for AC-LEDs.

Key words

glass ceramics / low-temperature co-firing method / luminous performance / alternating current-white light emitting diodes

引用本文

徐祖盛, 张瑞, 覃贤壮. 用于高功率交流白光发光二极管的半透明GdAGG：Ce-SiO₂玻璃陶瓷的制备、结构和发光性能. 硅酸盐学报, 2024 , 52 (10) : 3291 -3300 . DOI: 10.14062/j.issn.0454-5648.20240143

Zusheng XU, Rui ZHANG, Xianzhuang QIN. Structure and Luminescence Properties of Translucent GdAGG:Ce-SiO₂ Glass Ceramics for High-Power Alternating Current-White Light Emitting Diodes[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (10) : 3291 -3300 . DOI: 10.14062/j.issn.0454-5648.20240143

基金

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国家自然科学基金(52062008)

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2024年第52卷第10期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240143

接收时间：2024-02-26
首发时间：2026-10-22
出版时间：2024-10-20

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收稿日期：2024-02-26
修回日期：2024-03-27

基金

国家自然科学基金(52062008)

作者信息

^1．桂林理工大学材料科学与工程学院，广西桂林 541004

^2．有色金属及材料加工新技术教育部重点实验室，广西光电材料与器件重点实验室，广西桂林 541004

通讯作者:

张瑞（1986—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240143

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2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 total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
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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