Effect of Sintering Temperature on Luminescence Properties of Color Conversion Glasses in Borosilicate Glasses

doi:10.15541/jim20160374

Abstract

Abstract:

The color conversion glass is a promising material for light emitting diodes encapsulation due to its high thermal conductivity and good thermal stability. In present study, color conversion glasses were prepared by sintering a mixture of borosilicate glass frits and a YAG phosphor at temperature from 600℃ to 900℃. The effects of sintering temperature on luminescence properties were examined. Characteristics of color conversion glasses, with respect to luminescence intensity, CIE (Commission International de I’Eclairage) chromaticity and CCT (Correlated Color Temperature) were analyzed based on luminescence excitation and emission spectra. These characteristics are dependent on sintering temperature of the color conversion glasses. The CIE coordinates shift with increase of sintering temperature. The glass, sintered at 700℃, shows the best luminescence properties. But for the glasses sintered above 850℃, their luminescence properties may be destroyed. Test results of X-ray diffraction (XRD), differential scanning calorimetry (DSC) and X-ray photoelectron spectroscopy (XPS) reveal that degradation of luminescence properties with increase of sintering temperature is ascribed to the lattice disturbance of YAG and oxidation of Ce³⁺, which is caused by reactions between glass matrix and YAG phosphors. The present study may promote the application of color conversion glasses in light emitting diodes encapsulation.

Key words: Ce: YAG color conversion glass, luminescence intensity, CIE coordinates shift, sintering temperature

CLC Number:

TB383

LI Yang, HU Li-Li, YANG Bo-Bo, SHI Ming-Ming, ZOU Jun. Effect of Sintering Temperature on Luminescence Properties of Color Conversion Glasses in Borosilicate Glasses[J]. Journal of Inorganic Materials, 2017, 32(3): 257-262.

Figures/Tables 8

Fig. 1 PLE and PL spectra of their phosphors and their color conversion glasses sintered at different temperatures(a) PLE of the phosphors; (b) PL of the phosphors; (c) PLE of the color conversion glasses; (d) PL of the color conversion glasses

Fig. 2 CIE of Ce: YAG phosphors (a) and color conversion glasses (b) sintered at different temperatures

Fig. 3 Variable value of color temperature between color conversion glasses and Ce: YAG phosphors sintered at different temperatures

Fig. 4 XRD patterns of Ce: YAG phosphors (a) and color conversion glasses (b) sintered at different temperatures

Fig. 5 XPS spectrum of C1s for the equipment calibration

Fig. 6 XPS spectra and fitting curves of Ce3d in color conversion glasses sintered at 700℃ (a) and 850℃ (b)

Table 1 Relative percentage of Ce3+ in the color conversion glasses sintered at 700℃ and 850℃

	Sintering temperature/℃	Peak/eV	FWHM/eV	Area /(a.u)	Sum/(a.u.)	Relative percentage/%
Ce⁴⁺3d_5/2	700	885.391	5.71	83433.797	204219.715	42.04
Ce⁴⁺3d_3/2	700	899.953	5.36	120785.918	204219.715	42.04
Ce³⁺3d_5/2	700	890.518	4.75	98702.643	281556.319	57.96
Ce³⁺3d_3/2	700	904.473	5.75	182853.676	281556.319	57.96
Ce⁴⁺3d_5/2	850	887.956	4.83	52640.837	195529.716	82.33
Ce⁴⁺3d_3/2	850	901.529	8.00	142888.879	195529.716	82.33
Ce³⁺3d_5/2	850	891.148	3.51	24062.383	41966.744	17.67
Ce³⁺3d_3/2	850	906.428	3.62	17904.361	41966.744	17.67

Fig. 7 DSC curves of Ce: YAG phosphor, glass matrix and the color conversion glass

References 16

[1]	MAO Z Y, ZHU Y C, GAN L, et al.Novel white-light-emitting SiAlON-crystal/glass composite phosphor prepared by facile strategy for white light-emitting-diode.Materials Letters, 2012, 80(8): 63-65.
[2]	NAKAMURA S.III-V nitride-based light-emitting diodes.Diamond and Related Materials, 1996, 5(3): 496-500.
[3]	CRAWFORD M H.LEDs for solid-state lighting: performance challenges and recent advances. IEEE Journal of Selected Topics in Quantum Electronics, 2009, 15(4): 1028-1040.
[4]	HUANG K C, HUANGY R, TING S Y, et al.Facile fabrication of spherical silicone encapsulant with Pt nanoparticles for applications as white light-emitting diode. Materials Letters, 2014, 134(7): 244-247.
[5]	TSAI CC, WANG J, CHEN M H, et al.Investigation of Ce: YAG doping effect on thermal aging for high-power phosphor-converted white-light-emitting diodes.IEEE Transactions on Device and Materials Reliability, 2009, 9(3): 367-370.
[6]	CHEN D Q, XIANG W D, LIANG X J, et al.Advances in transparent glass-ceramic phosphors for white light-emitting diodes—a review.Journal of the European Ceramic Society, 2014, 35(3): 859-869.
[7]	ZHANG R, LIN H, YU Y L, et al.A new-generation color converter for high-power white LED: transparent Ce3+: YAG phosphor-in-glass.Laser & Photonics R, 2014, 8(1): 158-164.
[8]	BORRELLI N F, LAMBERSON L A, MORENAR M,et al. Phosphor containing glass frit materials for LED lighting applications. US, C03C3/066, US8822032. 2014.09.02.
[9]	CHEN H, LIN H, XU J, et al.Chromaticity-tunable phosphor-in-glass for long-lifetime high-power warm w-LEDs.Journal of Materials Chemistry C, 2015, 3(31): 8080-8089.
[10]	SEGAWA H, HIROSAKI N, OHKI S, et al.Exploration of zinc phosphate glasses dispersed with Eu-doped SiAlON for white LED applications.Optical Materials, 2013, 35(12): 2677-2684.
[11]	ZHANG Y, LIU S, XU H J, et al.Preparation and performance of Ce: YAG phosphor-in-glass.Journal of Inorganic Materials, 2015, 30(6): 588-592.
[12]	REN L J, LEI X H, DU X Q, et al.Effect of Eu2O3 concentration on luminescent properties of Ce/Tb/Eu co-doped calcium borosilicate glass for white LED.Journal of Luminescence, 2013, 142(8): 150-154.
[13]	2015/863/EU(ROHS 2.0), the Restriction of the use of certain hazardous substances in electrical and electronic equipment.
[14]	张中太, 张俊英. 无机光致发光材料及应用, 2版. 北京: 化学工业出版社, 2011: 93.
[15]	WANG L M, ZHUANG L Q, HUANG Y X, et al.Application of XPS in semi-quantitative estimation of Ce3+ in YAG: Ce3+ phosphor.Journal of East China University of Science and Technology (Natural Science Edition), 2015, 41(4): 484-488.
[16]	陈珍霞. LED用低熔点发光玻璃的研究. 武汉: 武汉理工大学硕士学位论文, 2010.