硅酸盐学报

Sc₂O₃对CsPbBr₃量子点玻璃析晶行为的影响

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李菊清 ¹ , 雷炳富 ¹ , 刘应亮 ¹ , 张学杰 ¹ , 王静 ²

硅酸盐学报 | 研究论文 2024,52(12): 3663-3672

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硅酸盐学报 |研究论文 2024 , 52 (12) : 3663 -3672

Sc₂O₃对CsPbBr₃量子点玻璃析晶行为的影响

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李菊清¹, 雷炳富¹, 刘应亮¹, 张学杰¹, 王静²

作者信息

^1．华南农业大学材料与能源学院，广州 510642

^2．中山大学化学学院，广州 510275

通讯作者:

张学杰（1987—），男，博士，副教授。

王静（1976—），男，博士，教授。

作者简介:

李菊清（1997—），女，硕士研究生。

Influence of Sc₂O₃ on Crystallization Behavior of CsPbBr₃ Quantum Dot Glass

Juqing LI¹, Bingfu LEI¹, Yingliang LIU¹, Xuejie ZHANG¹, Jing WANG²

Affiliations

^1.College of Materials and Energy, South China Agricultural University, Guangzhou 510642, China

^2.School of Chemistry, Sun Yat-sen University, Guangzhou 510275, China

Corresponding Author:

ZHANG Xuejie (1987-), male, Ph.D., Associate Professor; E-mail: zhangxuejie@scau.edu.cn;

WANG Jing (1976-), male, Ph.D., Professor. ceswj@mail.sysu.edu.cn

LI Juqing (1997-), female, Master candidate. E-mail: 202310191487@mail.scut.edu.cn

出版时间: 2024-12-20 doi: 10.14062/j.issn.0454-5648.20240265

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摘要

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玻璃网络结构对玻璃中CsPbBr₃量子点的析晶行为及发光性质具有重要影响作用。通过高温熔融及后续热处理制备了一系列CsPbBr₃量子点玻璃，系统研究了Sc₂O₃引入量对CsPbBr₃量子点玻璃析晶行为及发光性能的影响。结果表明：Sc₂O₃作为一种玻璃网络中间体，添加至玻璃组分中可以有效增强玻璃网络结构，且随着引入量的增多，CsPbBr₃量子点析出尺寸逐渐减小。经优化，最佳CsPbBr₃量子点玻璃样品在460 nm激发下内、外量子效率高达62.98%及37.92%，该样品在455 nm蓝光发光二极管芯片上（20 V，20 mA）持续点亮7 d后依旧可以保持其原始发光强度的64.51%。上述优异的发光性能为其在宽色域背光显示领域中的应用奠定了基础。

关键词

三溴化铅铯量子点 / 玻璃网络 / 组分调控 / 发光性能

Abstract

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Introduction

CsPbBr₃ perovskite quantum dots are considered as excellent green light materials in the field of wide color gamut displays due to their excellent luminescence characteristics, such as high photoluminescence quantum yield (PLQY) and narrow full width at half maximum (FWHM). However, CsPbBr₃ quantum dots irreversibly deteriorate when exposed to oxygen, water, light and heat due to their low formation energy and strong ionic properties, which restricts their application. The preparation of CsPbBr₃ quantum dots via in-situ crystallization in glass is considered as one of the effective strategies to improve their stability. In this study, borosilicate glass was used as a matrix to investigate the effect of Sc₂O₃ introduction on the glass network structure and the regulatory effect on the crystallization behavior and luminescence performance of CsPbBr₃. In addition, the photostability and thermostability of the samples were analyzed. CsPbBr₃ quantum dot glass powder with the high quantum efficiency and narrow FWHM could be used to prepare white LED with a high luminous efficiency and a wide color gamut.

Methods

A series of CsPbBr₃ quantum dot glasses were prepared by a conventional melt quenching-heat treatment method. The specific molar composition ratio of the glass was 42B₂O₃-20SiO₂-4Li₂O-8ZnO-3MgO-3Cs₂O-6PbBr₂-6NaBr-xSc₂O₃ (mole fraction, x = 0, 0.1, 0.3, 0.5, and 0.7). According to the composition of each glass stoichiometric ratio, the raw materials were weighed, and fully ground in a mortar for 30 min. The mixed powder was then transferred to a corundum crucible and placed in a high-temperature muffle furnace at 1200 ℃ for 15 min. Subsequently, the melt was poured into a preheated graphite mold and annealed for 3 h to relieve thermal stress. After cooling to room temperature, a transparent precursor glass (referred to as PG) was obtained. CsPbBr₃ quantum dot glass was obtained via heat treatment of precursor glass samples at different temperatures (i.e., 460, 470, 480, 490 ℃, and 500 ℃) for 10 h. Finally, the prepared CsPbBr₃ quantum dot glass was cut, polished or ground into a powder for further characterization and use.

Results and discussion

The results show that the average particle size of CsPbBr₃ quantum dots gradually decreases from 13.22 nm to 3.42 nm as the amount of Sc₂O₃ introduced increases. This indicates that the introduction of Sc₂O₃ can alter the glass network structure under identical external conditions, which in turn affects the particle size of the quantum dots. Note that the peak intensity of the [PbBr₆]^4- firstly increases and then decreases with increasing the amount of Sc₂O₃ introduced. The peak intensity of [BO₃]/[SiO₄] gradually decreases. This is primarily attributed to the Sc₂O₃ additive, which reduces the [BO₃] content within the network structure, strengthens the glass network, and affects the crystallization behavior of the quantum dots.

The obtained samples exhibit a typical narrow-band luminescence. Under the same amount of Sc₂O₃ introduced, PL spectra of CsPbBr₃ quantum dot glass samples heat-treated at different temperatures show that the luminescence intensity firstly increases and then decreases with the increase of the temperature, and a phenomenon is attributed to fluorescence quenching. The long lifetime is reduced by 20 ns, but the proportion of long-lived emission gradually is increased as the amount of Sc₂O₃ introduction is increased. This is due to the improvement of the surface quality of the quantum dot, indicating that carrier quenching can be effectively minimized. Also, the the internal and external photoluminescence quantum yields of the optimal CsPbBr₃ quantum dot glass samples are 62.98% and 37.92% at 460 nm excitation. Moreover, they can maintain 64.51% of the original luminescence intensity after continuous illumination upon a 455 nm blue LED chip (20 V, 20 mA) for a week, laying a foundation for developing high-brightness LED devices. After three cycles of heating and cooling (at 298-473 K), the luminescence intensity of the optimal sample can gradually return to the initial value, and the peak emission wavelength and FWHM also show obvious temperature dependence and excellent recovery ability, indicating that the CsPbBr₃ quantum dot glass has a good luminescence thermal stability.

Conclusions

CsPbBr₃ perovskite quantum dots with different amounts of Sc₂O₃ were precipitated in a borosilicate glass matrix by a conventional melt quenching-heat treatment method. Under the same heat treatment conditions, the structure of the glass network improved and became dense, as well as the average size of the quantum dots decreased from 13.22 nm to 3.42 nm with the increase of the amount of Sc₂O₃ introduced. After optimization, the internal and external photoluminescence quantum yields of the optimal CsPbBr₃ quantum dot glass samples were 62.98% and 37.92% at 460 nm excitation. The denser network structure effectively isolated the quantum dots from air, water, and oxygen erosion, significantly reducing phase separation and degradation caused by external environmental factors, thus having a good thermal cycle recovery. For the white LED prepared with the superior luminescent properties of the CsPbBr₃ quantum dot glass powder, the color coordinates were located at (0.3135, 0.3077), the correlated color temperature was 6647 K, and the color gamut reached 130.95% of the NTSC standard and 97.90% of the Rec. 2020 standard, indicating a potential application in the backlight display field.

Key words

cesium lead tribromide perovskite quantum dots / glass network structure / composition control / luminescence properties

引用本文

李菊清, 雷炳富, 刘应亮, 张学杰, 王静. Sc₂O₃对CsPbBr₃量子点玻璃析晶行为的影响. 硅酸盐学报, 2024 , 52 (12) : 3663 -3672 . DOI: 10.14062/j.issn.0454-5648.20240265

Juqing LI, Bingfu LEI, Yingliang LIU, Xuejie ZHANG, Jing WANG. Influence of Sc₂O₃ on Crystallization Behavior of CsPbBr₃ Quantum Dot Glass[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (12) : 3663 -3672 . DOI: 10.14062/j.issn.0454-5648.20240265

基金

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国家自然科学基金(52372147; 51802101)

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2024年第52卷第12期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240265

接收时间：2024-04-07
首发时间：2026-10-22
出版时间：2024-12-20

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收稿日期：2024-04-07
修回日期：2024-04-19

基金

国家自然科学基金(52372147; 51802101)

作者信息

^1．华南农业大学材料与能源学院，广州 510642

^2．中山大学化学学院，广州 510275

通讯作者:

张学杰（1987—），男，博士，副教授。

王静（1976—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240265

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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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