Compound of phosphor and the manufacturing method thereof

Abstract

Provided is a metal oxonitridosilicate phosphor of a general formula M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a:Eu.sub.z,Mn.sub.b, wherein M is one or more alkaline earth metals; 0; 0; 0<z≦; and 0<b≦.

Claims

1. A metal oxonitridosilicate phosphor of a general formula M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a:Eu.sub.z,Mn.sub.b, wherein M is one or more alkaline earth metals; 0≦x≦7; 0≦a≦1; 0<z≦0.3; and 0<b≦0.3, and wherein the metal oxonitridosilicate phosphor is configured to emit a light with a CIEx between 0.2753 and 0.2917 and a CIEy between 0.5103 and 0.5203.

2. The metal oxonitridosilicate phosphor according to claim 1, wherein M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a in the general formula is a host lattice, Eu is a first active center and Mn is a second active center.

3. The metal oxonitridosilicate phosphor according to claim 1, emitting a fluorescence with a wavelength ranging from 480 nm to 700 nm when excited by a light source with a wavelength ranging from 300 nm to 460 nm.

4. The metal oxonitridosilicate phosphor according to claim 3, wherein the light source with the wavelength ranging from 300 nm to 460 nm is from a light-emitting diode or plasma.

5. The metal oxonitridosilicate phosphor according to claim 3, emitting a green fluorescence when excited by the light source with the wavelength ranging from 300 nm to 460 nm.

6. A manufacturing method of the metal oxonitridosilicate phosphor according to claim 1, comprising the steps of: mixing a first reactant comprising a material selected from the group consisting of strontium oxide and strontium nitride, a second reactant comprising Al, a third reactant comprising Si, a fourth reactant comprising Eu, and a fifth reactant comprising Mn to form a mixture; and forming the mixture into a metal oxonitridosilicate phosphor with a general formula M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a:Eu.sub.z,Mn.sub.b by solid-state reaction at a pressure ranging from 0.5 MPa to 1.5 MPa, wherein 0≦x≦7; 0≦a≦1; 0<z≦0.3; and 0<b≦0.3, and the phosphor emits a fluorescence with a wavelength ranging from 480 nm to 700 nm when excited by a light source with a wavelength ranging from 300 nm to 460 nm.

7. The manufacturing method of a metal oxonitridosilicate phosphor according to claim 6, wherein M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a in the general formula is a host lattice, Eu is a first active center and Mn is a second active center.

8. The manufacturing method of a metal oxonitridosilicate phosphor according to claim 6, wherein the second reactant comprising Al, the third reactant comprising Si, the fourth reactant comprising Eu, and the fifth reactant comprising Mn respectively comprise a material selected from the group consisting of oxides and nitrides.

9. The manufacturing method of a metal oxonitridosilicate phosphor according to claim 6, wherein forming the mixture into a metal oxonitridosilicate phosphor by solid-state reaction at high pressure comprises forming the mixture into a metal oxonitridosilicate phosphor under nitrogen atmosphere, at a temperature ranging from 1700° C. to 2300° C. for 3 to 8 hours.

10. The manufacturing method of a metal oxonitridosilicate phosphor according to claim 6, further comprising grinding the mixture after forming the mixture into the metal oxonitridosilicate phosphor by solid-state reaction.

11. The metal oxonitridosilicate phosphor according to claim 1, wherein z>b.

Description

BRIEF DESCRIPTION OF THE DRAWINGS

(1) FIG. 1 is an XRD pattern of the phosphor (a) in accordance with the first embodiment, the phosphors (b) to (f) in accordance with the second embodiment of the application and a standard compound having a formula Sr.sub.5Al.sub.5Si.sub.21N.sub.35O.sub.2;

(2) FIG. 2 is an excitation spectrum of the phosphor (a) in accordance with the first embodiment and the phosphors (b) to (f) in accordance with the second embodiment of the application;

(3) FIG. 3 is an emission spectrum of the phosphor (a) in accordance with the first embodiment and the phosphors (b) to (f) of the second embodiment of the application under an excitation wavelength ranging from 300 nm to 460 nm; and

(4) FIG. 4 is a CIE chromaticity diagram of the phosphor (a) in accordance with the first embodiment and the phosphors (b) to (f) in accordance with the second embodiment of the application under a 460 nm excitation.

DETAILED DESCRIPTION OF PREFERRED EMBODIMENTS

(5) Exemplary embodiments of the present application will be described in detail with reference to the accompanying drawings hereafter. The following embodiments are given by way of illustration to help those skilled in the art fully understand the spirit of the present application. Hence, it should be noted that the present application is not limited to the embodiments herein and can be realized by various forms. Further, the drawings are not precise scale and components may be exaggerated in view of width, height, length, etc. Herein, the similar or identical reference numerals will denote the similar or identical components throughout the drawings.

(6) The embodiments of the present application provide a phosphor having a general formula M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a:Eu.sub.z,Mn.sub.b, wherein M is one or more alkaline earth metals; 0≦x≦7; 0≦a≦1; 0<z≦0.3; and 0<b≦0.3. M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a of the phosphor is a host lattice, Eu is a first active center, and Mn is a second active center.

First Embodiment

(7) The present embodiment is a comparative embodiment of the metal oxonitridosilicate phosphor (a), wherein M is Sr, x=2, a=0, z=0.1, b=0, namely, the phosphor is Sr.sub.4.9Al.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1. The phosphor is prepared by solid-state reaction at high pressure, and the method is shown as follows.

(8) First, a stoichiometric first reactant comprising Sr, such as Sr.sub.3N.sub.2; a stoichiometric second reactant comprising Al, such as AlN; a stoichiometric third reactant comprising Si, such as Si.sub.3N.sub.4 or SiO.sub.2; and a stoichiometric fourth reactant comprising Eu, such as EuN are provided to form a mixture having a formula Sr.sub.4.9Al.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1.

(9) Second, a pestle is used to grind and mix the mixture uniformly, and subsequently the uniform mixture is put into a boron nitride crucible, and then the boron nitride crucible is put into a high-temperature sintering furnace to carry out a sintering step under a temperature ranging from 1700° C. to 2300° C. for 3 to 8 hours, so as to form the metal oxonitridosilicate phosphor. More specifically, the mixture is heated to the temperature ranging from 1700° C. to 2300° C. at a heating rate of 35° C./minute under nitrogen atmosphere at a pressure ranging from 0.5 to 1.5 Mpa, and then the mixture is kept for 3 to 8 hours, and subsequently the mixture was cooled down to room temperature at a cooling rate of 15° C./minute. After the sintering step, a pestle is used again to grind the metal oxonitridosilicate phosphor into powders having uniform particle sizes after the metal oxonitridosilicate phosphor is taken out from the high-temperature sintering furnace.

(10) The reactants can be oxides or nitrides comprising corresponding element respectively.

Second Embodiment

(11) In the present embodiment, five metal oxonitridosilicate phosphors (b) to (f) having the general formula M.sub.5−z−a−bAl.sub.3+xSi.sub.23−xN.sub.37−x−2aO.sub.x+2a:Eu.sub.z,Mn.sub.b are prepared, wherein M of each phosphor is Sr, x of each phosphor is 2, a of each phosphor is 0, z of each phosphor is 0.1, namely the five phosphors having a formula Sr.sub.4.9−bAl.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1,Mn.sub.b, and wherein b is 0.02, 0.04, 0.06, 0.08, 0.1 respectively. Each of the phosphor is prepared by solid-state reaction at high pressure, and the method is shown as follows.

(12) First, a stoichiometric first reactant comprising Sr, such as Sr.sub.3N.sub.2; a stoichiometric second reactant comprising Al, such as AlN; a stoichiometric third reactant comprising Si, such as Si.sub.3N.sub.4 or SiO.sub.2; a stoichiometric fourth reactant comprising Eu, such as EuN; and a stoichiometric fifth reactant comprising Mn, such as MnO.sub.2 are provided to form a mixture having a formula Sr.sub.4.9−bAl.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1,Mn.sub.b.

(13) Second, a pestle is used to grind and mix the mixture uniformly, and subsequently the uniform mixture is put into a boron nitride crucible, and then the boron nitride crucible is put into a high-temperature sintering furnace to carry out a sintering step under a temperature ranging from 1700° C. to 2300° C. for 3 to 8 hours. More specifically, the mixture is heated to the temperature ranging from 1700° C. to 2300° C. at a heating rate of 35° C./minute under nitrogen atmosphere at a pressure ranging from 0.5 to 1.5 Mpa, and then the mixture is kept for 3 to 8 hours, and subsequently the mixture was cooled down to room temperature at a cooling rate of 15° C./minute. After the sintering step, a pestle is used again to grind the sintered mixture into powders having uniform particle sizes after the sintered mixture is taken out from the high-temperature sintering furnace.

(14) The reactants can be oxides or nitrides comprising corresponding element respectively.

(15) The crystal phase purity and crystal structure of the phosphors of the embodiments are determined by an X-ray diffractometer. FIG. 1 is an XRD pattern of the phosphor (a) in accordance with the first embodiment having a formula Sr.sub.4.9Al.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1, the phosphors (b) to (f) in accordance with the second embodiment having a formula Sr.sub.4.9−bAl.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1,Mn.sub.b, and standard compound having a formula Sr.sub.5Al.sub.5Si.sub.21N.sub.35O.sub.2, wherein b of the phosphor (b) to (f) is 0.02, 0.04, 0.06, 0.08, 0.1 respectively. As shown in FIG. 1, phosphors (a) to (f) respectively have pure crystal phases instead of impurity crystal phases.

(16) Referring to FIG. 2, which is an excitation spectrum of the phosphor (a) in accordance with the first embodiment having a formula Sr.sub.4.9Al.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1, the phosphors (b) to (f) in accordance with the second embodiment having a formula Sr.sub.4.9−bAl.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1,Mn.sub.b, wherein b of the phosphor (b) to (f) is 0.02, 0.04, 0.06, 0.08, 0.1 respectively. As shown in FIG. 2, the phosphors are suitable for being excited with ultraviolet (UV) light or blue light, which is an excitation source having a wavelength ranging from 300 nm to 460 nm from a light-emitting diode or plasma. Accordingly, the metal oxonitridosilicate phosphor of the application is suitable for being exited with a wide excitation wavelength.

(17) Referring to FIG. 3, which is an emission spectrum of the phosphor (a) in accordance with the first embodiment having a formula Sr.sub.4.9Al.sub.15Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1, the phosphors (b) to (f) in accordance with the second embodiment having a formula Sr.sub.4.9−bAl.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1,Mn.sub.b, wherein b of the phosphors (b) to (f) is 0.02, 0.04, 0.06, 0.08, 0.1 respectively. As shown in FIG. 3, under an excitation source having a wavelength ranging from 300 nm to 460 nm, the strongest emission intensity is in a wavelength ranging from 480 nm to 700 nm. As a result, the phosphors of the application emitting green light. Besides, when Mn as a second active center is added, each emission intensity of phosphors (b) to (f) is stronger than the emission intensity of the phosphor (a), which only has Eu as a first active center. Furthermore, the emission intensity is stronger as the amount of Mn increases.

(18) Table 1 shows chromaticity coordinates of the phosphor (a) in accordance with the first embodiment having a formula Sr.sub.4.9Al.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1, the phosphors (b) to (f) in accordance with the second embodiment having a formula Sr.sub.4.9−bAl.sub.5Si.sub.21N.sub.35O.sub.2:Eu.sub.0.1, Mn.sub.b, wherein b of the phosphor (b) to (f) is 0.02, 0.04, 0.06, 0.08, 0.1 respectively. The chromaticity coordinates are obtained by converting the data by the equation standardized by Commission internationale de l'éclairage (CIE), wherein the data are obtained from the emission spectrum. Furthermore, FIG. 4 shows a CIE chromaticity diagram of the phosphors (a) to (f). As shown in FIG. 4, the light emitted by the phosphors of the embodiments of the present application lies in the green region of CIE color coordinate and is with high color purity.

(19) TABLE-US-00001 TABLE 1 The chromaticity coordinates of the phosphor (a) to (f) Chromaticity Coordinates CIEx CIEy a 0.3385 0.5085 b 0.2854 0.5201 c 0.2886 0.5149 d 0.2753 0.5203 e 0.2917 0.5103 f 0.2863 0.5180

(20) The foregoing description of preferred and other embodiments in the present disclosure is not intended to limit or restrict the scope or applicability of the inventive concepts conceived by the Applicant. In exchange for disclosing the inventive concepts contained herein, the Applicant desires all patent rights afforded by the appended claims. Therefore, it is intended that the appended claims include all modifications and alterations to the full extent that they come within the scope of the following claims or the equivalents thereof.