CsPbBr3@MIL-53 Nanocomposite Phosphors: Synthesis, Properties and Applications in White LEDs

doi:10.15541/jim20240141

Abstract

Abstract:

The all-inorganic CsPbX₃ (X=Cl, Br, I) perovskite nanocrystals have been widely applied in optoelectronic devices due to their excellent optoelectronic properties. However, their poor stability remains one of the main factors restricting their commercial development. This research focuses on improving the stability and solid-state luminescence performance of CsPbBr₃ nanocrystals. The porous MIL-53 (Al) metal-organic frameworks (MOFs) with outstanding hydrophobic properties was chosen as the encapsulation matrix. CsPbBr₃ nanocrystals were grown in situ within the MIL-53 (Al) channels by using a thermal injection process to successfully synthesize CsPbBr₃@MIL-53 nanocomposite phosphors with outstanding solid-state luminescence performance and high stability. MIL-53 chelates with CsPbBr₃ nanocrystals through benzene rings and organic ligands, firmly anchoring nanocrystals in the pores. This not only protects the CsPbBr₃ nanocrystals from external environmental influences but also effectively prevents aggregation between nanocrystals, thereby avoiding quenching of solid-state fluorescence. Additionally, the COO^- functional groups in MIL-53 bind with the unpaired Pb²⁺ on the surface of CsPbBr₃ nanocrystals, passivating the surface defects and suppressing non-radiative carrier recombination. Furthermore, the contained benzene rings and organic long chains endow the nanocomposite phosphors with excellent hydrophobic properties. The synergistic effect of these factors significantly enhances the optical performance and water stability of CsPbBr₃@MIL-53 nanocomposite phosphors. As a result, photoluminescence quantum yield (PLQY) of CsPbBr₃@MIL-53 nanocomposite phosphors reaches 75.4%, which is 2.3 times of that of solid-state CsPbBr₃ nanocrystal powders (33.2%). Even after being completely immersed in water for 10 h, its fluorescence intensity can still maintain 75.6% of the initial value. Finally, the green-emitting CsPbBr₃@MIL-53 nanocomposite phosphors were applied to white LED devices, achieving a wide-color-gamut coverage area of 126% NTSC and 85% Rec. 2020, which demonstrates its application prospects in wide-color-gamut display devices.

Key words: all-inorganic perovskite, metal-organic framework, CsPbBr₃@MIL-53, stability, white LEDs

CLC Number:

TQ174

QU Mujing, ZHANG Shulan, ZHU Mengmeng, DING Haojie, DUAN Jiaxin, DAI Henglong, ZHOU Guohong, LI Huili. CsPbBr₃@MIL-53 Nanocomposite Phosphors: Synthesis, Properties and Applications in White LEDs[J]. Journal of Inorganic Materials, 2024, 39(9): 1035-1043.

Figures/Tables 9

Fig. 1 Synthesis schematic of mesoporous MIL-53 (Al)[25]

Fig. 2 Schematic diagram of synthesis for CsPbBr3@MIL-53 nanocomposite phosphors

Fig. 3 (a, c, d, e) TEM and (b, f) HRTEM images of CsPbBr3 NCs, MIL-53 MOFs and CsPbBr3@MIL-53 nanocomposite phosphors (a, b) CsPbBr3 NCs; (c) MIL-53 MOFs; (d-f) CsPbBr3@MIL-53 nanocomposite phosphors with the inserted histogram in the figure (e) showing the statistical results of the particle size distribution of CsPbBr3 NCs in the composite phosphors

Fig. 4 XRD patterns of MIL-53 and CsPbBr3@MIL-53 nanocomposite phosphors before and after water treatment

Fig. 5 BET specific surface area testing of MIL-53 and CsPbBr3@MIL-53 (a) N2 adsorption-desorption isotherms; (b) Pore size distribution; Colorful figures are available on website

Fig. 6 XPS spectra of MIL-53, CsPbBr3 and CsPbBr3@MIL-53 (a) Total spectra; (b) Pb4f high-resolution spectra; (c) O1s high-resolution spectra

Fig. 7 Optical properties of CsPbBr3@MIL-53 nanocomposite phosphors (a) Emission spectra of CsPbBr3@MIL-53 with different weights of MIL-53; (b) Time-resolved photoluminescence (TRPL) curves and PLQYs of the optimized sample as well as CsPbBr3 NCs; Colorful figures are available on website

Fig. 8 Thermal- and water-stability of CsPbBr3@MIL-53 nanocomposite phosphors and CsPbBr3 NCs (a, b) Temperature-dependent PL spectra (λex=365 nm); (c) Normalized temperature-dependent PL spectra; (d, e) PL spectra of samples immersed in water for different periods; (f) Normalized time-dependent PL spectra

Fig. 9 Properties of white LED device fabricated by using green CsPbBr3@MIL-53 nanocomposite phosphors (a) EL spectrum of white LED driven by 2.6 V and 35.0 mA with inset photo showing the lighted white LED device; (b) Color gamut coverage of the white LED in comparison with NTSC and Rec. 2020 standard

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CsPbBr₃@MIL-53 Nanocomposite Phosphors: Synthesis, Properties and Applications in White LEDs

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