(Mg1-x-yBaxSry)1.95SiO4∶0.05Eu荧光粉的光谱研究及紫外激发色像图建立

doi:10.3964/j.issn.1000-0593(2020)01-0098-09

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Abstract A novel (Mg_1-x-yBa_xSr_y)_1.95SiO₄∶0.05Eu phosphor was prepared by high-temperature solid state reaction method, including 3 binary alkaline earth ion ratio series and 3 representative ternary alkaline earth ion ratio series (Ba is constant and the Mg/Sr ratio is continuously changed, the Mg/Sr ratio is constant and the Ba content is continuously changed.). As for the 6 series, the spectral properties (excitation and emission spectra), ultraviolet (254 and 365 nm) luminescence recordings and CIE values corresponding to the color images were studied in detail. Like the way to establish a ternary phase diagram, a ternary colour image is derived from these binary and representative ternary data. It can be used to study and screen a new phosphor series in a more efficient way. The prepared phosphor series include: Mg₂SiO₄-Sr₂SiO₄, Ba₂SiO₄-Sr₂SiO₄, Mg₂SiO₄-Ba₂SiO₄, Ba atomic ratio of 0.2 (Mg/Sr atomic ratio continuously changed), Ba atomic ratio of 0.6 (Mg/Sr atomic ratio continuously changes), the atomic ratio of Mg/Sr is 1/4 (the series of continuous changes in Ba atomic content). Its corresponding spectral performance, luminescence recording, and CIE chromatic analysis at 254 nm excitation indicate that: Eu ions exist trivalent and divalent in (Mg_1-x-yBa_xSr_y)₂SiO₄; for the binary series (as the matrix as (Mg_1-xBa_x)₂SiO₄ or (Ba_1-ySr_y)₂SiO₄), with the increase of Ba atomic ratio, the phosphor gradually turns red (corresponding to Eu³⁺ ions ⁵D₀→⁷F₁ and ⁵D₀→⁷F₂ electron transition narrow band emission) to green (corresponding to Eu²⁺ ion 4f^n-15d→4fⁿ electronic transition emission broadband emission), and the former series change faster; the binary series as (Mg_1-ySr_y)₂SiO₄ were red phosphors, and the red luminescence increases with the increase of Sr content. For the ternary series (Ba_x(Mg_0.2Sr_0.8)_1-x)₂SiO₄ (Mg/Sr=1/4), as Ba ion amount increases, the phosphor gradually changes from red to green, and the rate of change is determined by the ratio of Mg/Sr equal to 0 (ie Ba₂SiO₄-Sr₂SiO₄ series) and the ratio of Mg/Sr is equal to ∝ (ie Ba₂SiO₄-Mg₂SiO₄ series); the ternary series (Ba_0.2Sr_yMg_0.8-y)_1.95SiO₄ are also red phosphors, and (Ba_0.6Sr_yMg_0.4-y)₂SiO₄ gradually turn blue and green with the atomic ratio of Mg/Sr increasing. The evolution of fluorescence emission at 365 nm excitation is generally consistent with that at 254 nm excitation, but the emission of green light in the same sample at 365 nm is stronger than that at 254 nm and the emission in the red band is weaker than that at 254 nm. Therefore, the contents of Ba in (Mg_1-xBa_x)₂SiO₄, (Ba_1-ySr_y)₂SiO₄, (Ba_x(Mg_0.2Sr_0.8)_1-x)₂ from red to green are 40at%, 60at%, 60at%, respectively (60at%, 80at%, 70at% at 254nm excitation), and Mg/Sr ratio from red to green in (Ba_0.6Sr_yMg_0.4-y)₂SiO₄ is 1/4 (2/3 at 254 nm excitation). Based on this, ternary CIE colour image of Eu-doped Ba₂SiO₄-Mg₂SiO₄-Sr₂SiO₄ is established. It can be seen from the spectral image that the (Mg_1-x-yBa_xSr_y)_1.95SiO₄∶0.05Eu phosphor emits light under UV excitation, that is, the matrix component emits green near the Ba₂SiO₄ corner and emits red near the Mg₂SiO₄ or Sr₂SiO₄ corner. The larger the Mg/Sr ratio is, the faster the phosphor turns from red to green as the Ba atom increases. The green light emission of the same sample is stronger than the 254 nm excitation at 365 nm excitation and the red emission is weaker than the 254nm excitation. (Mg_1-x-yBa_xSr_y)_1.95SiO₄∶0.05Eu phosphor is Ba>80at%, and Mg>90at% (or Sr>80at%) phosphor can be used as high-efficiency green and red fluorescence, respectively; when the composition is (Mg_0.8Sr_0.2)_1.95SiO₄∶0.05Eu, (Ba_0.8Mg_0.16Sr_0.04)_1.95SiO₄∶0.05Eu is the best red and green phosphor for UV excitation.

Key words：Alkaline earth silicate; Phosphor; Solid state reaction method; Eu-doped; Ultraviolet excitation

Received: 2018-12-03 Accepted: 2019-04-15

ZTFLH:

TB332

Corresponding Authors: LUO Lan E-mail: luolan1190@163.com；luolan1190@sina.com.cn

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https://www.gpxygpfx.com/EN/10.3964/j.issn.1000-0593(2020)01-0098-09 OR https://www.gpxygpfx.com/EN/Y2020/V40/I01/98

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