METHOD FOR PREPARING A B-SiAION PHOSPHOR

Abstract

There is provided a method for preparing a β-SiAlON phosphor capable of be controlled to show characteristics such as high brightness and desired particle size distribution. The method for preparing a β-SiAlON phosphor represented by Formula: Si (6-x) Al x O y N (8-y) :Ln z (wherein, Ln is a rare earth element, and the following requirements are satisfied: 0<x≦4.2, 0<y≦4.2, and 0<z≦1.0) includes: mixing starting materials to prepare a raw material mixture; and heating the raw material mixture in a nitrogen-containing atmospheric gas, wherein the starting materials includes a host raw material including a silicon raw material including metallic silicon, and at least one aluminum raw material selected from the group consisting of metallic aluminum and aluminum compound, and at least activator raw material selected from the rare earth elements for activating the host raw material.

1 - 8 . (canceled) 
     
     
         9 . A method for preparing a β-SiAlON phosphor, the method comprising:
 weighing starting material in order to prepare the β-SiAlON phosphor represented by Formula: Si (6-x) Al x O y N (8-y) :Ln z  (wherein, Ln is a rare earth element, and the following requirements are satisfied: 0<x≦4.2, 0<y≦4.2, and 0<z≦1.0), 
 mixing the starting materials to prepare a raw material mixture; and 
 firing the raw material mixture in a nitrogen-containing atmospheric gas, 
 wherein the starting materials comprises: 
 a silicon raw material including metallic silicon, an aluminum raw material including at least one of metallic aluminum and aluminum compound, and 
 at least one activator raw material selected from the rare earth elements for activating the host raw material. 
 
     
     
         10 . The method of  claim 9 , wherein the rare earth element includes Eu or Ce. 
     
     
         11 . The method of  claim 9 , wherein the silicon raw material includes at least one of silicon nitride and silicon oxide. 
     
     
         12 . The method of  claim 9 , wherein the aluminum compound includes at least one selected from the group consisting of aluminum nitride, aluminum oxide and aluminum hydroxide. 
     
     
         13 . The method of  claim 9 , wherein the β-SiAlON phosphor has a peak wavelength of 500 to 570 nm. 
     
     
         14 . The method of  claim 9 , wherein the nitrogen-containing atmospheric gas has an N 2  concentration of 90% or more. 
     
     
         15 . The method of  claim 9 , wherein the nitrogen-containing atmospheric gas has a gas pressure of 0.1 to 20 Mpa. 
     
     
         16 . The method of  claim 9 , wherein the operation of firing the raw material mixture is performed at a temperature of 1850 to 2150° C. 
     
     
         17 . The method of  claim 9 , wherein the metallic silicon is in the form of powder and an has an average particle-diameter of 300 μm or less. 
     
     
         18 . The method of  claim 9 , wherein the aluminum raw material includes an aluminum compound. 
     
     
         19 . A method of preparing a β-SiAlON phosphor, the method comprising:
 weighing a silicon raw material, an aluminum raw material and an activator raw material in order to prepare a β-SiAlON phosphor represented by the following formula: Si (6-x) Al x O y N (8-y) :Ln z  (wherein, Ln is a rare earth element, and the following requirements are satisfied: 0<x≦4.2, 0<y≦4.2, and 0<z≦1.0), 
 preparing a raw material mixture by mixing the weighed silicon raw material, the aluminum raw material and the activator raw material; and 
 firing the raw material mixture in a nitrogen-containing atmospheric gas, 
 wherein the preparing of the aluminum raw material includes controlling a mixing ratio of metallic aluminum and an aluminum compound in order to control particle characteristics of the β-SiAlON phosphor. 
 
     
     
         20 . The method of  claim 19 , wherein the rare earth element includes Eu or Ce. 
     
     
         21 . The method of  claim 19 , wherein the silicon raw material includes a silicon compound, and the silicon compound is at least one of silicon nitride and silicon oxide. 
     
     
         22 . The method of  claim 21 , wherein the silicon raw material further includes metallic silicon. 
     
     
         23 . The method of  claim 19 , wherein the controlling of the mixing ratio of the metallic aluminum and the aluminum compound is performed to control the mixing ratio so that the metallic aluminum and the aluminum compound exist at a uniform ratio within the aluminum raw material. 
     
     
         24 . The method of  claim 23 , wherein the metallic aluminum is in the form of powder having an average particle-diameter of 300 μm or less. 
     
     
         25 . The method of  claim 19 , wherein the aluminum raw material includes an aluminum compound. 
     
     
         26 . The method of  claim 25 , wherein the aluminum compound is at least one selected from the group consisting of aluminum nitride, aluminum oxide and aluminum hydroxide. 
     
     
         27 . The method of  claim 19 , wherein the β-SiAlON phosphor has a peak wavelength of 500 to 570 nm. 
     
     
         28 . A white light emitting diode (LED) device, having a β-SiAlON phosphor used therein and manufactured by the method of  claim 9 . 
     
     
         29 . A lighting device, having the white LED device of  claim 28 . 
     
     
         30 . A display device, having the white LED device of  claim 28 . 
     
     
         31 . A white LED device as a β-SiAlON phosphor, having a blue LED chip, a red phosphor, and a green phosphor manufactured by the method of  claim 9 . 
     
     
         32 . A lighting device, having the white LED device of  claim 31 . 
     
     
         33 . A display device, having the white LED device of  claim 31 . 
     
     
         34 . A lighting device, having a β-SiAlON phosphor manufactured by the method of  claim 9  and used therein. 
     
     
         35 . A display device, having a β-SiAlON phosphor manufactured by the method of  claim 9  and used therein. 
     
     
         36 . A white LED device comprising:
 a blue LED chip; and   a silicon resin provided on the blue LED chip, and including a green phosphor as a β-SiAlON phosphor represented by the following formula: Si(6−x)AlxOyN(8−y):Lnz (wherein, Ln is a rare earth element, and the following requirements are satisfied: 0<x≦4.2, 0<y≦4.2, and 0<z≦1.0), and a red phosphor as a nitride-based phosphor represented by CaAlSiN 3 :Eu, the green phosphor having an excitation wavelength band at a portion of band in ultraviolet rays and visual rays and an emission peak within the range of 500 to 570 nm.   
     
     
         37 . The white LED device of  claim 36 , wherein Ln is at least one element selected from the group consisting of Eu, Ce, Sm, Yb, Dy, Pr and Tb. 
     
     
         38 . The white LED device of  claim 36 , wherein Ln is Eu, and the β-SiAlON phosphor and the nitride-based phosphor respectively further include a rare earth element Re different from Eu, where Re is at least one selected from Y, La, Ce, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, F, Cl, Br and I, and each thereof is contained in the range of 1 ppm to 50000 ppm in the respective phosphor. 
     
     
         39 . The white LED device of  claim 36 , wherein a color rendering index (CRI) of white light emitted from the white LED device is 70 or more. 
     
     
         40 . The white LED device of  claim 36 , wherein a dominant wavelength of the blue LED chip is in the range of 430 to 455 nm. 
     
     
         41 . The white LED device of  claim 40 , wherein an emission wavelength peak of the red phosphor is 610 to 660 nm, and an emission wavelength peak of the green phosphor is 500 to 550 nm. 
     
     
         42 . The white LED device of  claim 40 , wherein the blue LED chip has a full width of half maximum of 10 to 30 nm, the green phosphor has a full width of half maximum of 30 to 100 nm, and the red phosphor has a full width of half maximum of 50 to 150 nm. 
     
     
         43 . The white LED device of  claim 40 , further comprising a yellow or orange yellow phosphor disposed in the periphery of the blue LED chip, an emission wavelength peak of the yellow or orange yellow phosphor being in the range of 550 to 600 nm. 
     
     
         44 . The white LED device of  claim 43 , wherein the yellow or orange yellow phosphor has a full width of half maximum of 20 to 100 nm. 
     
     
         45 . The white LED device of  claim 43 , wherein the yellow phosphor is a silicate-based phosphor, and the orange yellow phosphor is α-SiAlON:Eu,Re phosphor, where Re is at least one selected from Y, La, Ce, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, F, Cl, Br and I, and Re has the range of 1 ppm to 50000 ppm. 
     
     
         46 . The white LED device of  claim 36 , wherein the green phosphor further includes at least one selected from the group consisting of an M 2 SiO 4 :Eu,Re silicate-based phosphor, an MA 2 D 2 :Eu,Re sulfide-based phosphor, and an M′A′2O4:Ce,Re′ oxide-based phosphor, where M′ is at least one selected from Ba, Sr, Ca, and Mg, and D is at least one selected from S, Se and Te, and A′ is at least one selected from Sc, Y, Gd, La, Lu, Al and In, and Re is at least one selected from Y, La, Ce, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, F, Cl, Br and I; and the content of Re is within the range of 1 ppm to 50000 ppm. 
     
     
         47 . The white LED device of  claim 36 , wherein the red phosphor further includes at least one selected from an M′AlSiN x :Eu,Re(1≦x≦5) nitride-based phosphor and an M′D:Eu,Re sulfide based phosphor; where M′ is at least one selected from Ba, Sr and Mg, D is at least one selected from S, Se and Te, A′ is at least one selected from Sc, Y, Gd, La, Lu, Al and In, and Re is at least one selected from Y, La, Ce, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, F, Cl, Br and I, and the content of Re is in the range of 1 ppm to 50000 ppm. 
     
     
         48 . A liquid crystal display (LCD) backlight unit, comprising the white LED device of  claim 36 . 
     
     
         49 . A lighting device, comprising the white LED device of  claim 36 . 
     
     
         50 . A display device, comprising the white LED device of  claim 36 . 
     
     
         51 . A white LED device comprising:
 a blue LED chip; and   a green phosphor and a red phosphor disposed in the periphery of the blue LED chip,   wherein the green phosphor is at least one selected from the group consisting of an M 2 SiO 4 :Eu,Re silicate-based phosphor, an MA 2 D 4 :Eu,Re sulfide-based phosphor, a β-SiAlON:Eu,Re phosphor and an M′A′ 2 O 4 :Ce,Re′ oxide-based phosphor, and the red phosphor is at least one selected from an M′AlSiN x :Eu,Re(1≦x≦5) nitride-based phosphor and an M′D:Eu,Re sulfide-based phosphor,   M being at least two elements selected from Ba, Sr, Ca and Mg, A being at least one selected from Ga, Al and In, D being at least one selected from S, Se and Te, M′ at least one selected from Ba, Sr, Ca and Mg, A′ at least one selected from Sc, Y, Gd, La, Lu, Al and In, Re at least one selected from Y, La, Ce, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, F, Cl, Br and I, and Re′ at least one selected from Nd, Pm, Sm, Tb, Dy, Ho, Er, Tm, Yb, F, Cl, Br and I, and   Re and Re′ being respectively within the range of 1 ppm to 50000 ppm.   
     
     
         52 . The white LED device of  claim 51 , further comprising a yellow or orange yellow phosphor disposed in the periphery of the blue LED chip, the yellow phosphor being a silicate-based phosphor, and the orange yellow phosphor being an α-SiAlON:Eu,Re phosphor. 
     
     
         53 . The white LED device of  claim 51 , wherein a dominant wavelength of the blue LED chip is in the range of 430 to 455 nm. 
     
     
         54 . The white LED device of  claim 53 , wherein an emission wavelength peak of the red phosphor is 610 to 660 nm, and an emission wavelength peak of the green phosphor is 500 to 550 nm. 
     
     
         55 . The white LED device of  claim 53 , wherein the blue LED chip has a full width of half maximum of 10 to 30 nm, the green phosphor has a full width of half maximum of 30 to 100 nm, and the red phosphor has a full width of half maximum of 50 to 150 nm. 
     
     
         56 . The white LED device of  claim 51 , further comprising a package main body having a groove part on which the blue LED chip is mounted. 
     
     
         57 . The white LED device of  claim 52 , further comprising a resin package part packaging the blue LED chip, wherein the green phosphor, the red phosphor and the yellow or orange yellow phosphor are dispersed within the resin packaging part. 
     
     
         58 . The white LED device of  claim 52 , wherein the green phosphor, the red phosphor and the yellow or orange yellow phosphor are respectively constituted by different phosphor layers, the respective phosphor layers having a stacked structure. 
     
     
         59 . The white LED device of  claim 52 , wherein the green phosphor, the red phosphor and the yellow or orange yellow phosphor are mixed with a transparent resin to respectively constitute different phosphor-containing resin layers, and the respective phosphor-containing resin layers have a stacked structure. 
     
     
         60 . The white LED device of  claim 51 , wherein a color rendering index (CRI) of white light emitted from the white LED device is 70 or more. 
     
     
         61 . A white LED module, comprising:
 a circuit board and at least one white LED device mounted on the circuit board,   where the white LED device includes:   a blue LED chip; and   a green phosphor and a red phosphor disposed in the periphery of the blue LED chip,   wherein the green phosphor is at least one selected from the group consisting of an M 2 SiO 4 :Eu,Re silicate-based phosphor, an MA 2 D 4 :Eu,Re sulfide-based phosphor, a β-SiAlON:Eu,Re phosphor and an M′A′ 2 O 4 :Ce,Re′ oxide-based phosphor, and the red phosphor is at least one selected from an M′AlSiN x :Eu,Re(1≦x≦5) nitride-based phosphor and an M′D:Eu,Re sulfide-based phosphor,   M being at least two elements selected from Ba, Sr, Ca and Mg, A being at least one selected from Ga, Al and In, D being at least one selected from S, Se and Te, M′ at least one selected from Ba, Sr, Ca and Mg, A′ at least one selected from Sc, Y, Gd, La, Lu, Al and In, Re at least one selected from Y, La, Ce, Nd, Pm, Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, F, Cl, Br and I, and Re′ at least one selected from Nd, Pm, Sm, Tb, Dy, Ho, Er, Tm, Yb, F, Cl, Br and I, and   Re and Re′ being respectively in the range of 1 ppm to 50000 ppm.   
     
     
         62 . The white LED module of  claim 61 , further comprising a yellow or orange yellow phosphor disposed in the periphery of the blue LED chip, the yellow phosphor being a silicate-based phosphor, and the orange yellow phosphor being an α-SiAlON:Eu,Re phosphor. 
     
     
         63 . The white LED module of  claim 61 , wherein a dominant wavelength of the blue LED chip is in the range of 430 to 455 nm. 
     
     
         64 . The white LED module of  claim 63 , wherein an emission wavelength peak of the red phosphor is 610 to 660 nm, and an emission wavelength peak of the green phosphor is 500 to 550 nm. 
     
     
         65 . The white LED module of  claim 63 , wherein the blue LED chip has a full width of half maximum of 10 to 30 nm, the green phosphor has a full width of half maximum of 30 to 100 nm, and the red phosphor has a full width of half maximum of 50 to 150 nm. 
     
     
         66 . The white LED module of  claim 61 , further comprising a package main body having a groove part on which the blue LED chip is mounted. 
     
     
         67 . The white LED module of  claim 62 , further comprising a resin package part packaging the blue LED chip, wherein the green phosphor, the red phosphor and the yellow or orange yellow phosphor are dispersed within the resin packaging part. 
     
     
         68 . The white LED device of  claim 62 , wherein the green phosphor, the red phosphor and the yellow or orange yellow phosphor are respectively constituted by different phosphor layers, and the respective phosphor layers have a stacked structure. 
     
     
         69 . The white LED module of  claim 62 , wherein the green phosphor, the red phosphor and the yellow or orange yellow phosphor are mixed with a transparent resin to respectively constitute different phosphor-containing resin layers, and the respective phosphor-containing resin layers have a stacked structure. 
     
     
         70 . The white LED module of  claim 61 , wherein a color rendering index (CRI) of white light emitted from the white LED device is 70 or more.