Elsevier

Materials Letters

Volume 62, Issues 4–5, 29 February 2008, Pages 619-622
Materials Letters

The red phosphor NaEu(MoO4)2 prepared by the combustion method

https://doi.org/10.1016/j.matlet.2007.06.021Get rights and content

Abstract

The red phosphor NaEu(MoO4)2 was prepared by the combustion method, and its morphology and structure were measured by the X-ray diffraction (XRD) and scanning electronic microscopy (SEM). Its photo-luminescent properties were investigated and compared with that prepared by the high temperature solid state reaction method. The sample prepared by the combustion method with the firing temperature at 800 °C is of uniform particles size (about 500 nm), and it shows the intense red light emission under 395 nm excitation with the appropriate CIE chromaticity coordinates (x = 0.66, y = 0.34), therefore it may find application on near UV InGaN chip-based white light-emitting diodes.

Introduction

More and more interests are focused on the white-light-emitting diodes (W-LEDs), which have many advantages, such as high efficiency, long lifetime, low power consumption and environmental-friendly characteristics [1]. At present, the most common method to obtain the white light is to combine a yellow-emitting phosphor with blue LED chip, however, there are some problems for such “blue + yellow” white LEDs, such as lower color-rendering index, lower luminous efficiency [2], [3]. In order to improve the luminous efficiency, a new approach using near UV (around 400 nm) InGaN-based LED chip coated with blue/green/red tricolor phosphors was introduced [2]. The current red-emitting phosphor for near UV InGaN-based white LEDs is Y2O2S:Eu3+, which shows some problems: lower efficiency compared with that of blue and green phosphors, shorter working lifetime under UV irradiation, and instability due to releasing of sulfide gas [3], [4], hence it is urgent to find new red phosphors with high efficiency.

The double molybdates AB(MoO4)2 (A = Li+, Na+, K+, Rb+, Cs+; B = trivalent rare earth ions), which share the scheelite-like (CaWO4) iso-structure, show excellent thermal and hydrolytic stability, then they were considered to be efficient luminescent hosts [5], [6], [7], [8]. In this scheelite structure, Mo(VI) is coordinated by four oxygen atoms in a tetrahedral site and the alkali metal ion/rare earth ion site is eight coordinated [9]. In our previous work [10], the photo-luminescent properties of NaLa1  x(MoO4)2:xEu3+ were systematically investigated, and the results suggested that the phosphor NaEu(MoO4)2 showed the intense red emission with the good CIE (Commission Internationale de l’Eclairage, International Commission on Illumination) chromaticity coordinates under 400 nm excitation.

The phosphors particles prepared by the conventional solid-state reaction were of bigger size with irregular morphology, which were not suitable for the application. Therefore, the wet-chemical methods seem to be an attractive alternative to the classical approach [11]. The combustion process [12], [13], [14] to prepare the phosphor is very facile, and only takes a few minutes, which has been extensively applied to the preparation of various nano-scale inorganic phosphors. So in present paper, the phosphor NaEu(MoO4)2 was prepared by the combustion method, and its photo-luminescence properties were investigated.

Section snippets

Preparation of NaEu(MoO4)2 by the combustion method

The starting materials include 99.99 % purity Eu2O3, analytical reagent grade HNO3, (NH4)6Mo7O24·4H2O, NaHCO3, EDTA and urea. Firstly, 2 mmol (NH4)6Mo7O24·4H2O was dissolved in aqueous solution. Secondly, Eu2O3 (1.2317 g) were dissolved with nitric acid aqueous solution, and EDTA (2.5000 g), NaHCO3 (0.5880 g) were added in the aqueous solution, adjusting the pH to ∼ 5 with NH3·H2O/citric acid. Then the (NH4)6Mo7O24·4H2O aqueous solution was added in the Eu3+-containing solution. The transparent

Results and discussion

The XRD patterns of NaEu(MoO4)2 prepared by the combustion method fired at 600 °C (a), 700 °C (b), 800 °C (c), and prepared by the solid state reaction at 800 °C (d) are shown in Fig. 1. The single crystalline phase of scheelite structure has been formed at 600 °C, and these XRD patterns of the samples are consistent with that given in JCPDS card 25-0828 [Na0.5Gd0.5MoO4], the result shows that these phosphors are of single phase with the scheelite structure.

The SEM micrographs of NaEu(MoO4)2

Conclusions

The phosphor NaEu(MoO4)2 was prepared the combustion method, and its structure, the morphology and the luminescent properties were compared with that of NaEu(MoO4)2 prepared by the solid state reaction. The emission intensity of the phosphor prepared by the combustion method fired at 800 °C is about 1.6 times stronger than that prepared by the solid state reaction fired at 800 °C.

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (20571088), and by a research grant from the Guangdong province government (ZB2003A07).

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