Effect of Pb2+ on the Luminescent Performance of Borosilicate Glass Coated CsPbBr3 Perovskite Quantum Dots

doi:10.15541/jim230501

Abstract

Abstract:

Perovskite CsPbBr₃ quantum dots (PQDs) encapsulated within borosilicate glass can markedly improve their stability, expanding their applicability in sectors under lighting and display of light emitting diode (LED). However, this encapsulation has unintended consequence of reducing both the photoluminescence (PL) intensity and PL quantum yields (PLQY). This research aims to enhance the PL intensity of CsPbBr₃ perovskite quantum dots glass (PQDs@glass) by exploring the effects of thermal induction temperature and Pb²⁺ content on its structural properties. The results demonstrate that the optimal thermal induction temperature for maximizing PL intensity is 460 ℃, with a Pb²⁺ concentration of 6 mol. The study revealed that the increase in Pb²⁺ concentration led to the densification of the glass network structure and altered the diffusion behavior of glass components. This alteration affected the crystallization process of PQDs, which ultimately resulted in variations in the luminous intensity of PQDs@glass. This study achieved a highly desirable PLQY of 95.6% for PQDs@glass and successfully carried out size-controllable preparation of PQDs within a borosilicate glass matrix. Remarkably, the obtained results show that over 86% of the obtained PQDs particles fall within a narrow size range of 6-14 nm with average diameter of 10 nm, leading to a well-defined size distribution. Notably, these PQDs exhibit exceptional stability, as evidenced by their ability to retain an extraordinary 98.9% of the initial emission intensity following ten consecutive thermal cycles spanning from room temperature to 200 ℃. Finally, to verify its applicability in LED lighting and display, the obtained PQDs@glass powder was blended with polydimethylsiloxane (PDMS), yielding exemplary LED devices which exhibit an exceptional color gamut range surpassing 110% of the standard RGB (sRGB) color space. In conclusion, this study lays the groundwork for the scalable synthesis of PQDs@glass and paves the way for its utilization in the realm of LED device technology.

Key words: CsPbBr₃, Pb²⁺, LED, quantum dot, borosilicate glass

CLC Number:

TQ174

YUE Zihao, YANG Xiaotu, ZHANG Zhengliang, DENG Ruixiang, ZHANG Tao, SONG Lixin. Effect of Pb²⁺ on the Luminescent Performance of Borosilicate Glass Coated CsPbBr₃ Perovskite Quantum Dots[J]. Journal of Inorganic Materials, 2024, 39(4): 449-456.

Figures/Tables 8

Fig. 1 Schematic of preparation of quantum dots glass- ceramics AC: After crystallization; BC: Before crystallization

Fig. 2 Crystal structures and optical properties of PQDs@glass at different temperatures for 2 h (a) XRD patterns; (b) PL spectra; (c) PLQY and PL intensity; (d) Fluorescence lifetime curves Colorful images are available on website

Fig. 3 TEM characterization and size distribution analyses of PQDs@glass (a, b) TEM images before (a) and after (b) heat-treatment; (c) High-resolution TEM image; (d, e) TEM image and EDS mappings; (f) Schematic diagram of the relationship between size and band gap of CsPbBr3 QDs; (g-k) TEM images and size statistics

Table 1 Component regulation of Pb2+ ions (all data in molar ratios)

Code	SiO₂	H₃BO₃	ZnO	CaF₂	Cs₂CO₃	PbBr₂	NaBr	PbO
Pb-1	85	170	55	5	16	4	17	0.5
Pb-2	85	170	55	5	16	5	15	0.5
Pb-3	85	170	55	5	16	6	13	0.5
Pb-4	85	170	55	5	16	7	11	0.5

Fig. 4 (a) Photographs, (b) XRD patterns and (c) PL spectra of CsPbBr3 QDs@glass with different Pb2+ concentrations

Fig. 5 Structural characterization of PQDs@glass at different Pb2+ concentrations (a, b) FT-IR and XPS spectra, and (c) the ratio of bridging to non-bridging oxygen bonds; Colorful figures are available on website

Fig. 6 Stability experiments of PQDs@glass (a, b) Variations in PL intensity and FWHM of water resistance (a) and UV stability (b), and (c) experimental results of thermal cycling stability

Fig. 7 (a) LED device fabricated with CsPbBr3 QDs@glass, and (b) CIE coordinates of CsPbBr3 QDs@glass LED devices at different Pb2+ concentrations

References 29

[1]	SU W, TENG Q, YUAN F. All-thermally evaporated perovskite LEDs toward high-resolution active-matrix displays. Matter, 2023, 6(8): 2539. DOI URL
[2]	KIM D, PARK S, CHOI B C, et al. The tetravalent manganese activated SrLaMgTaO₆ phosphor for w-LED applications. Materials Research Bulletin, 2018, 97: 115. DOI URL
[3]	CHRISTENSEN A, GRAHAM S. Thermal effects in packaging high power light emitting diode arrays. Applied Thermal Engineering, 2009, 29(2/3): 364. DOI URL
[4]	WEN Z, XIE F, CHOY W C H. Stability of electroluminescent perovskite quantum dots light-emitting diode. Nano Select, 2021, 3(3): 505. DOI URL
[5]	WANG S, BI C, YUAN J, et al. Original core-shell structure of cubic CsPbBr₃@Amorphous CsPbBr_x perovskite quantum dots with a high blue photoluminescence quantum yield of over 80%. ACS Energy Letters, 2017, 3(1): 245. DOI URL
[6]	RAIN G, YAZDANI N, BOEHME S C, et al. Ultra-narrow room-temperature emission from single CsPbBr₃ perovskite quantum dots. Nature Communications, 2022, 13(1): 2587. DOI
[7]	ZHOU X, CHANG Q, XIANG G, et al. A and B sites dual substitution by Na⁺ and Cu²⁺ co-doping in CsPbBr₃ quantum dots to achieve bright and stable blue light emitting diodes. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 2023, 300: 122773. DOI URL
[8]	WU W, ZHAO C, HU M, et al. CsPbBr₃ perovskite quantum dots grown within Fe-doped zeolite X with improved stability for sensitive NH₃ detection. Nanoscale, 2023, 15(12): 5705. DOI URL
[9]	LIN C Q, LIU M L, YANG Z, et al. Mn²⁺ doped CsPbBr₃ perovskite quantum dots with high quantum yield and stability for flexible array displays. Journal of Solid State Chemistry, 2023, 327: 124295. DOI URL
[10]	LIU S, SHAO G, DING L, et al. Sn-doped CsPbBr₃ QDs glasses with excellent stability and optical properties for WLED. Chemical Engineering Journal, 2019, 361: 937. DOI URL
[11]	HUANG D, BO J, ZHENG R, et al. Luminescence and stability enhancement of CsPbBr₃ perovskite quantum dots through surface sacrificial coating. Advanced Optical Materials, 2021, 9(16): 2100474. DOI URL
[12]	ZOU L, LI X, YANG M, et al. ZnPc/CsPbBr₃ QDs collaborative interface modification to improve the performance of CsPbBr₃ perovskite solar cells. Solar Energy Materials and Solar Cells, 2023, 251: 112157. DOI URL
[13]	XU Y, YU L, PENG K, et al. Ultra-stable perovskite quantum dot composites encapsulated with mesoporous SiO₂ and PbBr(OH) for white light-emitting diodes. Luminescence, 2023, 38(5): 536. DOI URL
[14]	REN J, LI T, ZHOU X, et al. Encapsulating all-inorganic perovskite quantum dots into mesoporous metal organic frameworks with significantly enhanced stability for optoelectronic applications. Chemical Engineering Journal, 2019, 358: 30. DOI URL
[15]	LV W, LI L, XU M, et al. Improving the stability of metal halide perovskite quantum dots by encapsulation. Advanced Materials, 2019, 31(28): 1900682. DOI URL
[16]	LI S, NIE L, MA S, et al. Environmentally friendly CsPbBr₃ QDs multicomponent glass with super-stability for optoelectronic devices and up-converted lasing. Journal of the European Ceramic Society, 2020, 40(8): 3270. DOI URL
[17]	YANG B, MEI S, ZHU Y, et al. Precipitation promotion of highly emissive and stable CsPbX₃ (Cl, Br, I) perovskite quantum dots in borosilicate glass with alkaline earth modification. Ceramics International, 2023, 49(4): 6720. DOI URL
[18]	TONG Y, WANG Q, LIU X, et al. The promotion of TiO₂ induction for finely tunable self-crystallized CsPbX₃(X = Cl, Br and I) nanocrystal glasses for LED backlighting display. Chemical Engineering Journal, 2022, 429: 132391. DOI URL
[19]	SHAO G, LIU S, DING L, et al. K_xCs_1-_xPbBr₃ NCs glasses possessing super optical properties and stability for white light emitting diodes. Chemical Engineering Journal, 2019, 375: 122031. DOI URL
[20]	LIU S, HE M, DI X, et al. Precipitation and tunable emission of cesium lead halide perovskites (CsPbX₃, X = Br, I) QDs in borosilicate glass. Ceramics International, 2018, 44(4): 4496. DOI URL
[21]	LIU J, SHEN L, CHEN Y, et al. Highly luminescent and ultrastable cesium lead halide perovskite nanocrystal glass for plant-growth lighting engineering. Journal of Materials Chemistry C, 2019, 7(43): 13606. DOI URL
[22]	STOCH P, STOCH A. Structure and properties of Cs containing borosilicate glasses studied by molecular dynamics simulations. Journal of Non-Crystalline Solids, 2015, 411: 106. DOI URL
[23]	LIU Q, FENG L, SUN Y, et al. Effects of phosphate glass on Cs⁺ immobilization in geopolymer glass-ceramics. Ceramics International, 2023, 49(4): 6545. DOI URL
[24]	YANG B, MEI S, HE H, et al. Lead oxide enables lead volatilization pollution inhibition and phase purity modulation in perovskite quantum dots embedded borosilicate glass. Journal of the European Ceramic Society, 2022, 42(1): 258. DOI URL
[25]	KAUR N, KHANNA A, G NZ LEZ-BARRIUSO M, et al. Effects of Al³⁺, W⁶⁺, Nb⁵⁺ and Pb²⁺ on the structure and properties of borotellurite glasses. Journal of Non-Crystalline Solids, 2015, 429: 153. DOI URL
[26]	OTHMAN H, TOPPER B, ELKHOLY H, et al. Structural, spectroscopic, and radiation shielding properties of Pb²⁺‐doped borate and phosphate glasses. International Journal of Applied Glass Science, 2023, 14(3): 408. DOI URL
[27]	LI P, TIAN Y, HUANG F, et al. Highly efficient photostimulated luminescence of Pb²⁺ doped SrAl₂O₄:Eu²⁺, Dy³⁺ borate glass for long-term stable optical information storage. Journal of the European Ceramic Society, 2022, 42(12): 5065. DOI URL
[28]	EL-EGILI K, DOWEIDAR H, MOUSTAFA Y M, et al. Structure and some physical properties of PbO-P₂O₅ glasses. Physica B: Condensed Matter, 2003, 339(4): 237. DOI URL
[29]	CHENG Y, XIAO H, GUO W, et al. Structure and crystallization kinetics of PbO-B₂O₃ glasses. Ceramics International, 2007, 33(7): 1341. DOI URL

Effect of Pb²⁺ on the Luminescent Performance of Borosilicate Glass Coated CsPbBr₃ Perovskite Quantum Dots

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