Role of Fluxes in the Synthesis and Luminescence Properties of Ba3Si6O12N2:Eu2+ Oxynitride Phosphors by Microwave Sintering

doi:10.15541/jim20150597

Abstract

Abstract:

Eu²⁺ activated Ba₃Si₆O₁₂N₂ oxynitride green phosphors were synthesized by microwave sintering method with the aid of fluxes, namely BaCl₂, H₃BO₃, KF, and NH₄F. We employed a combination of X-ray diffraction, photoluminescence spectra and scanning electron microscopy measurements, in conjunction with detailed quantum efficiency (QE), life time and thermal quenching studies of luminescence properties to understand the origins of the improved luminescence properties. The results showed that the photoluminescence intensity of the phosphors was increased obviously by using varied fluxes and the intensity rise was recorded in order of fluxes as following: H₃BO₃ > KF > BaCl₂ > no flux > NH₄F. The maximum emission intensity of the Ba₃Si₆O₁₂N₂:Eu²⁺ phosphor was achieved at containing 1.0wt% H₃BO₃, due to the high crystallinity, narrow particle-size distribution and smooth surface, which showed low thermal quenching, shorter life time and increased external quantum efficiency, compared with that of the sample with other fluxes or without flux.

Key words: oxynitride phosphor, flux, microwave sintering, quantum efficiency

CLC Number:

TQ174

HAN Bin, WANG Yi-Fei, LIU Qian, HUANG Qing. Role of Fluxes in the Synthesis and Luminescence Properties of Ba₃Si₆O₁₂N₂:Eu²⁺ Oxynitride Phosphors by Microwave Sintering[J]. Journal of Inorganic Materials, 2016, 31(6): 652-660.

Figures/Tables 9

Fig. 1 Photoluminescence intensity (a) of the Ba3Si6O12N2:Eu2+ phosphor sintered without flux and with 1wt% flux as a function of the calcination temperature (λex=428 nm) and XRD patterns (b) of the Ba3Si6O12N2:Eu2+ phosphor sintered at various temperatures without flux and with 1wt% flux

Fig. 2 XRD patterns of the Ba3Si6O12N2:Eu2+ phosphor adding various amounts flux. (a) BaCl2 (1200℃); (b) H3BO3 (1250℃); (c) KF (1200℃); (d) NH4F (1150℃)

Fig. 3 Effects of flux adding amounts on the emission intensity (a) of the Ba3Si6O12N2:Eu2+ phosphor and excitation and emission spectra (b) of the Ba3Si6O12N2:Eu2+ phosphors. λex=428 nm; λem=527 nm

Fig. 4 Particle size distribution of the Ba3Si6O12N2:Eu2+ phosphor with various kinds of flux. (a) None (1250℃); (b) BaCl2 (1200℃, 2wt%); (c) H3BO3 (1250℃,1wt%); (d) KF (1200℃, 0.5wt%); (e) NH4F (1150℃, 1wt%)

Fig. 5 SEM images of the Ba3Si6O12N2:Eu2+ phosphor with various kinds of flux. (a) None (1250℃); (b) BaCl2 (1200℃, 2wt%); (c) H3BO3 (1250℃, 1wt%); (d) KF (1200℃, 0.5wt%); (e) NH4F (1150℃, 1wt%)

Fig. 6 External quantum efficiencies of the Ba3Si6O12N2:Eu2+ phosphor with various kinds of fluxes

Fig. 7 Fluorescence decay curve of 527 nm emission for samples prepared with various kinds of fluxes

Fig. 8 PL emission spectra (a) as a function of the calcination temperature of the Ba3Si6O12N2:Eu2+ phosphor prepared with 1wt% H3BO3 and plots of -ln [(I0/IT) -1] vs 1/kT for the Ba3Si6O12N2:Eu2+ sample (b) prepared with 1wt% H3BO3. The inset indicating the emission intensity at varying temperatures of the sample (λex=455 nm)

Fig. 9 CIE chromaticity coordinate of the Ba3Si6O12N2:Eu2+ phosphor from 25℃ to 300℃ calculated by using the emission spectra under 455 nm excitation. The inset shows the colorless powder of the Ba3Si6O12N2:Eu2+ phosphors which are filled into the logo of CAS and letters CNITECH. The logo and letters display green color under 365 nm UV light

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Role of Fluxes in the Synthesis and Luminescence Properties of Ba₃Si₆O₁₂N₂:Eu²⁺ Oxynitride Phosphors by Microwave Sintering

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