CN102531564A - Red-yellow light composite transparent ceramics packaged by white light LED (light-emitting diode) and preparation method thereof - Google Patents
Red-yellow light composite transparent ceramics packaged by white light LED (light-emitting diode) and preparation method thereof Download PDFInfo
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- CN102531564A CN102531564A CN2012100503209A CN201210050320A CN102531564A CN 102531564 A CN102531564 A CN 102531564A CN 2012100503209 A CN2012100503209 A CN 2012100503209A CN 201210050320 A CN201210050320 A CN 201210050320A CN 102531564 A CN102531564 A CN 102531564A
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Abstract
The invention relates to a red-yellow light composite transparent ceramics packaged by a white light LED (light-emitting diode) and a preparation method thereof. The composite transparent ceramics is formed by an upper-layer transparent ceramics and a lower-layer transparent ceramics, wherein the upper-layer transparent ceramics has the chemical composition of (CeyY1-y)3Al5O12, and the y is larger than or equal to 0.0003 and less than or equal to 0.06; and the lower-layer transparent ceramics has the chemical composition of (EuxY1-x)3Al5O12 or (EuxY1-x)2O3, and the x is larger than or equal to 0.0003 and less than or equal to 0.1. The composite transparent ceramics is stimulated by adopting a blue light LED chip; red light generated by the lower-layer transparent ceramics, yellow light generated by the upper-layer transparent ceramics and the residual blue light are mixed to form high-quality white light, which has the characteristics of high color rendering index and adjustable color temperature. The composite transparent ceramics has the advantages of high lighting cancellation temperature, stable spectrum performance, adaptability in packaging the high-power LED, and the like.
Description
Technical field
The present invention relates to the fluorescence transparent ceramic material, particularly a kind of red/gold-tinted composite transparent pottery that is used for white light emitting diode (abbreviating LED as) encapsulation and preparation method thereof, this composite transparent pottery is by upper strata (Ce
yY
1-y)
3Al
5O
12(0.0003≤y≤0.06) crystalline ceramics, (the Eu of lower floor
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3(0.0003≤x≤0.1) crystalline ceramics constitutes.
Background technology
One of gordian technique that the LED encapsulation technology prepares as LED obtains to show great attention to, and its technical level is directly connected to the work-ing life of LED product and temperature, the time stability of light source light parameter.The most general white light LEDs encapsulation scheme is that InGaN/GaN base blue chip adds the yttrium aluminum garnet Ce that mixes cerium at present
3+: Y
3Al
5O
12(Ce:YAG) fluorescent material, InGaN/GaN chip send blue-light excited Ce:YAG fluorescent material and produce gold-tinted, and remaining blue light and yellow light mix form white light.
Adopt the fluorescent material encapsulation need fluorescent material be dispersed in epoxy resin or the layer of silica gel and form phosphor gel; The heat dispersion of these organic polymer packaged materials is relatively poor; Make LED in use the encapsulated layer temperature raise rapidly; Thereby cause fluorescence efficiency to descend, and packaged material self also is prone to wear out, flavescence, causes the output of device light to descend.Particularly in the occasion of great power LED, this packaged type directly influences the work-ing life of device and the stability of optical parameter.In addition, lack the ruddiness composition in the fluorescence spectrum of Ce:YAG, make the colour temperature of mixing the back white light higher, light is not soft, and colour rendering index is lower.Can make Ce through codoped Gd, Tb etc.
3+The luminous peak position of ionic produces red shift, but moving range is very limited, and colour temperature is improved DeGrain.If adopt codoped Pr
3+Can directly replenish red light-emitting Deng then, but Ce
3+With Pr
3+Interionic energy shifts will cause Ce
3+Luminous efficiency obviously descends, and the way of luminescence quenching temperature significantly reduces.
The fluorescence transparent ceramic material has thermal conductivity and the thermostability more much higher than silica gel, can realize high work-ing life and device stability; And the pottery have higher hardness and fracture toughness property, can conveniently be applied on different environments for use, the especially car light.At present, well-known mechanisms such as Philip Luminleds company, Osram company and Kyoto Univ Japan all are being engaged in the research of this respect in the world.Wherein, Philip Luminleds has developed the great power LED product-Lumiramic LUXEONa LED that uses ceramic fluorescent material; Its technological core be exactly ceramic fluorescent plate (Lumiramic) combination film flip-chip (Thin Film Flip Chip, TFFC).This technology can change the colour temperature of white light LEDs and be reduced to originally 1/4, has improved the uneven phenomenon of colour temperature between each LED greatly, and it is stable also to have improved brightness and spectrographic.
Summary of the invention
The object of the present invention is to provide a kind of red/gold-tinted composite transparent pottery that is used for the white light LEDs encapsulation and preparation method thereof; Composite transparent pottery of the present invention; Adopt blue-ray LED to excite this composite transparent pottery; The ruddiness that lower floor's crystalline ceramics produces passes through the gold-tinted of pottery generation with the upper strata and the blue light that sees through becomes high-quality white light, has the colour rendering index height, the characteristics that colour temperature is gentle; And composite transparent pottery of the present invention has way of luminescence quenching temperature height, advantages such as physical and chemical performance is stable, good mechanical property.
Technical solution of the present invention is following:
A kind of red/gold-tinted composite transparent pottery that is used for the white light LEDs encapsulation, its characteristics are that this pottery constitutes by two-layer crystalline ceramics is bonding up and down: the chemical constitution of upper strata crystalline ceramics is (Ce
yY
1-y)
3Al
5O
12, wherein the span of y is respectively: 0.0003≤y≤0.06; The chemical constitution of lower floor's crystalline ceramics is (Eu
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3, wherein the span of x is: 0.0003≤x≤0.1.
Described composite transparent pottery can adopt upper and lower two-layer moulding preparation method respectively, or the once shaped preparation method, prepares.The wherein upper and lower two-layer preparation method of moulding respectively may further comprise the steps:
The chemical constitution of 1. selected composite transparent pottery and parameter x, y adopt yttrium oxide (Y
2O
3), aluminum oxide (Al
2O
3), europium sesquioxide (Eu
2O
3), cerium oxide (CeO
2) be raw material, by upper strata crystalline ceramics (Ce
yY
1-y)
3Al
5O
12Chemical constitution and the crystalline ceramics (Eu of lower floor
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3Chemical constitution disposes upper strata transparent ceramic powder raw material and lower floor's transparent ceramic powder raw material respectively;
2. use wet ball grinding to prepare ceramic powder as medium more respectively with absolute ethyl alcohol or deionized water, two kinds of powders respectively through dry, sieve, compressing tablet, again it is imposed the above isostatic cool pressing of 150MPa and becomes upper strata ceramic body and lower floor's ceramic body;
3. described upper strata ceramic body and lower floor's ceramic body are put into vacuum sintering furnace or hot-pressed sintering furnace sintering, obtain upper strata crystalline ceramics and lower floor's crystalline ceramics;
4. with described upper strata crystalline ceramics and lower floor's crystalline ceramics surface finish, the bonding composite transparent pottery that constitutes by upper strata crystalline ceramics and lower floor's crystalline ceramics of obtaining in its side, junction again.
The once shaped preparation method may further comprise the steps:
The chemical constitution of 1. selected composite transparent pottery and parameter x, y adopt yttrium oxide (Y
2O
3), aluminum oxide (Al
2O
3), europium sesquioxide (Eu
2O
3), cerium oxide (CeO
2) be raw material, by upper strata crystalline ceramics (Ce
yY
1-y)
3Al
5O
12Chemical constitution and the crystalline ceramics (Eu of lower floor
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3Chemical constitution disposes upper strata transparent ceramic powder raw material and lower floor's transparent ceramic powder raw material respectively;
2. use wet ball grinding to prepare ceramic powder as medium more respectively with absolute ethyl alcohol or deionized water, two kinds of powders respectively through dry, sieve, powder is pressed into contains a compound idiosome of two-layer heterogeneity up and down, it is (Ce at the middle and upper levels
yY
1-y)
3Al
5O
12Chemical constitution, lower floor is (Eu
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3Chemical constitution imposes the above isostatic cool pressing of 150MPa to it again;
3. described composite ceramics base substrate is put into vacuum sintering furnace or hot-pressed sintering furnace sintering, obtain composite ceramics;
4. with described composite transparent ceramic surface polishing.
Described two kinds prepare process in vacuum sintering furnace during sintering, and the sintered heat insulating temperature is 1650～1780 ℃, and the sintered heat insulating time is 1～24 hour.
Said two kinds prepare process in hot-pressed sintering furnace during sintering, and applied pressure is 10～40MPa, and the sintered heat insulating temperature is 1400～1700 ℃, and the sintered heat insulating time is 1～10 hour.
Technique effect of the present invention:
1, to adopt the upper strata be that cerium-doped yttrium aluminum garnet (Ce:YAG) crystalline ceramics, lower floor are yttrium aluminum garnet or yttrium oxide transparent ceramic (Eu:YAG or the Eu:Y that mixes europium in the present invention
2O
3) be combined to form the composite transparent stupalith.At the wavelength that led chip sends is blue-light excited time about 465 nanometers, but the upper layer of material emission peak is the wide spectrum gold-tinted of 531 nanometers, and lower floor can launch near the ruddiness 610 nanometers.The compound competent white-light spectrum of red composition that obtains of this kind realizes high color rendering index (CRI) and adjustable colour temperature.
If 2 lower floors adopt the yttrium aluminum garnet base transparent ceramic (Eu:YAG) mix europium, because two-layer use same matrix material up and down can be avoided because of the different scatter losses that caused of materials at two layers specific refractory power.
If 3 lower floors adopt the yttria-base transparent ceramics (Eu:Y that mixes europium
2O
3), yttria-base transparent ceramics has the thermal conductivity higher than yttrium aluminum garnet base transparent ceramic, adopts the lower floor of yttria-base transparent ceramics as composite structure, is close to led chip, the heat that produces in the time of can more effectively sharing chip operation.In addition, yttria-base transparent ceramics can be through changing preparation technology's easy adjustment transmitance, and lower transmitance means stronger scattering of light, can make that like suitable reduction transmitance the spatial distribution of light is more even, helps the demand of floodlighting.Adjusting through the yttria-base transparent ceramics transmitance can obtain different ray space distributions, thereby adapts to the demand of different illumination Design.Subsurface material adopts yttrium aluminum garnet base transparent ceramic or each tool advantage of yttria-base transparent ceramics, can select wherein a kind of according to practical application request.
4, the composite transparent stupalith among the present invention; Can effectively solve run in the development of current white light LEDs because the scattering loss that organic packaged material and fluorescent material refractive index difference cause; The luminous efficiency of fluorescent material descends along with the rising of LED temperature, and the wear out painted light decay that causes, spectrum stability of organic packaged material is not ideal enough, and problem such as Ce:YAG fluorescent material ruddiness composition deficiency; Improve blue-ray LED excite down the colour temperature of mixing the gained white light (＜5300K) and colour rendering index (Ra＞90); Simultaneously this composite transparent stupalith way of luminescence quenching temperature high (＞400K), physical and chemical performance is stable, good mechanical property.
Description of drawings
Fig. 1 is the structural representation of composite structure fluorescence ceramics of the present invention
Fig. 2 is the Eu:Y of lower floor of the present invention
2O
3The luminescent spectrum of fluorescence ceramics under blue-light excited
Embodiment
Below in conjunction with embodiment the present invention is described further, but should limit protection scope of the present invention with this.
It is as shown in Figure 1 that the present invention is used for the structure of red/gold-tinted composite transparent pottery of white light LEDs encapsulation, and lower floor is (Eu among the figure
xY
1-x)
3Al
5O
12Or Eu:Y
2O
3Ruddiness crystalline ceramics, upper strata are Ce:YAG gold-tinted crystalline ceramics.
This composite structural ceramic fluorescent material excites down at InGaN/GaN base blue-ray LED, (the Eu of lower floor
xY
1-x)
3Al
5O
12Or Eu:Y
2O
3Eu in the material
3+By the blue-light excited ruddiness that sends, Ce in the Ce:YAG material of upper strata
3+Seen through the blue-light excited jaundice light of lower floor.Red, yellow light intensity can be through the thickness of two-layer crystalline ceramics and Ce wherein
3+, Eu
3+Ionic concn is regulated.Because red, yellow, blue intensity can independent regulation, this composite structure can obtain the white light of fine colour temperature and colour rendering index.
Fig. 2 is the crystalline ceramics (Eu:Y of lower floor of the present invention
2O
3) spectrogram under 465 nano blue lights excite, europium ion can be excited by 465 nano blue lights very effectively and send the ruddiness that peak value is 613 nanometers.This ruddiness composition is joined in the yellow spectrum of Ce:YAG, can improve the colour rendering index of device effectively, and regulate the colour temperature that to regulate light source easily through red, yellow, blue relative intensity.As adopt Eu:YAG as lower floor's transparent ceramic material, can obtain similar spectrum.
The preparation method of composite transparent pottery of the present invention is:
Adopt yttrium oxide (Y
2O
3), aluminum oxide (Al
2O
3), europium sesquioxide (Eu
2O
3), cerium oxide (CeO
2) be raw material, by (Ce
yY
1-y)
3Al
5O
12, (Eu
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3(wherein, 0.0003≤x≤0.1,0.0001≤y≤0.06) forms and to configure two kinds of powder raw materials respectively, use wet ball grinding to prepare ceramic powder with absolute ethyl alcohol or deionized water as medium more respectively, two kinds of powders respectively through dry, sieve, compressing tablet; The back imposes the above isostatic cool pressing of 150MPa to it and becomes base substrate; After put into vacuum or hot-pressed sintering furnace sintering some hrs at a certain temperature, obtain (Eu
xY
1-x)
2O
3, (Ce
yY
1-y)
3Al
5O
12Crystalline ceramics, resulting two kinds of transparent fluorescence ceramics material surface polishings are bonding in its side, junction again, obtain composite transparent pottery as shown in Figure 1.
Embodiment 1
Adopt yttrium oxide (Y
2O
3), aluminum oxide (Al
2O
3), europium sesquioxide (Eu
2O
3), cerium oxide (CeO
2) be raw material, by (Eu
0.0003Y
0.9997)
2O
3, (Ce
0.0003Y
0.9997)
3Al
5O
12Chemical constitution configures two kinds of each 50g of powder respectively, uses wet ball grinding to prepare ceramic powder with absolute ethyl alcohol as medium more respectively, two kinds of powders respectively through dry, sieve upper and lower two-layer single shaft compression molding or a single shaft compression molding respectively; Again it is imposed the 200MPa isostatic cool pressing and become base substrate, put into vacuum sintering furnace, obtain required crystalline ceramics 1650 ℃ of following sintering 24 hours.
If adopt moulding respectively, with resulting two kinds of transparent ceramic material surface finish, bonding in its side, junction again must (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3The composite transparent pottery.
If adopt once shaped,, obtain (Ce with resulting crystalline ceramics twin polishing
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3The composite transparent pottery.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 2
The sintered heat insulating temperature is 1680 ℃, and the sintered heat insulating time is 20 hours, and other condition can get (Ce equally with embodiment 1
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3The composite transparent pottery.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 3
The sintered heat insulating temperature is 1780 ℃, and the sintered heat insulating time is 0.5 hour, and other conditions can get (Ce equally with embodiment 1
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3Crystalline ceramics composite structure fluorescent material.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 4
By (Eu
0.01Y
0.99)
2O
3, (Ce
0.01Y
0.99)
3Al
5O
12Chemical constitution disposes each 50g of powder raw material respectively, and the sintered heat insulating temperature is 1700 ℃, and the sintered heat insulating time is 16 hours, and other condition can get (Ce with embodiment 1
0.01Y
0.99)
3Al
5O
12/ (Eu
0.01Y
0.99)
2O
3The composite transparent pottery.
Same preparation technology may be implemented in (Ce
0.01Y
0.99)
3Al
5O
12/ (Eu
0.01Y
0.99)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 5
By (Eu
0.1Y
0.9)
2O
3, (Ce
0.06Y
0.94)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the sintered heat insulating temperature is 1650 ℃, and the sintered heat insulating time is 20 hours, and other condition can get (Ce with embodiment 1
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
2O
3The composite transparent pottery.
Same preparation technology may be implemented in (Ce
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 6
By (Eu
0.1Y
0.9)
2O
3, (Ce
0.06Y
0.94)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the sintered heat insulating temperature is 1780 ℃, and the sintered heat insulating time is 0.5 hour, and other condition can get (Ce with embodiment 1
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
2O
3The composite transparent pottery.
Same preparation technology may be implemented in (Ce
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 7
By (Eu
0.1Y
0.9)
2O
3, (Ce
0.06Y
0.94)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the sintered heat insulating temperature is 1720 ℃, and the sintered heat insulating time is 6 hours, and other condition can get (Ce with embodiment 1
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
2O
3The composite transparent pottery.
Same preparation technology may be implemented in (Ce
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 8
With (Eu
0.0003Y
0.9997)
2O
3, (Ce
0.0003Y
0.9997)
3Al
5O
12Ceramic body is put into hot-pressed sintering furnace separately at 10MPa, and 1400 ℃ of following sintering 10 hours are smooth, bonding in its side, junction again with resulting two kinds of transparent fluorescence ceramics material surfaces polishings, can get (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3Transparent composite ceramic material.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 9
With (Eu
0.0003Y
0.9997)
2O
3, (Ce
0.0003Y
0.9997)
3Al
5O
12Ceramic body is put into hot-pressed sintering furnace separately at 40MPa, 1700 ℃ of following sintering 0.5 hour, and other condition can get (Ce equally with embodiment 8
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3Transparent composite ceramic material.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 10
With (Eu
0.0003Y
0.9997)
2O
3, (Ce
0.0003Y
0.9997)
3Al
5O
12Ceramic body is put into hot-pressed sintering furnace separately at 20MPa, 1600 ℃ of following sintering 6 hours, and other condition can get (Ce equally with embodiment 8
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
2O
3Transparent composite ceramic material.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.0003Y
0.9997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 11
With (Eu
0.1Y
0.9)
2O
3, (Ce
0.06Y
0.94)
3Al
5O
12Ceramic body is put into hot-pressed sintering furnace separately at 10MPa, 1400 ℃ of following sintering 9 hours, and other condition can get (Ce equally with embodiment 8
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
2O
3Transparent composite ceramic material.
Same preparation technology may be implemented in (Ce
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 12
With (Eu
0.1Y
0.9)
2O
3, (Ce
0.06Y
0.94)
3Al
5O
12Ceramic body is put into hot-pressed sintering furnace separately at 40MPa, 1700 ℃ of following sintering 1 hour, and other condition can get (Ce equally with embodiment 8
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
2O
3Transparent composite ceramic material.
Same preparation technology may be implemented in (Ce
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 13
With (Eu
0.1Y
0.9)
2O
3, (Ce
0.06Y
0.94)
3Al
5O
12Ceramic body is put into hot-pressed sintering furnace separately at 40MPa, 1500 ℃ of following sintering 4 hours, and other condition can get (Ce equally with embodiment 8
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
2O
3Transparent composite ceramic material.
Same preparation technology may be implemented in (Ce
0.06Y
0.94)
3Al
5O
12/ (Eu
0.1Y
0.9)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 14
By (Eu
0.001Y
0.999)
2O
3, (Ce
0.0003Y
0.9997)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1720 ℃, and soaking time is 12 hours, and other condition can get (Ce with embodiment 1
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.001Y
0.999)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.001Y
0.999)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 15
By (Eu
0.003Y
0.997)
2O
3, (Ce
0.001Y
0.999)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1700 ℃, and soaking time is 16 hours, and other condition can get (Ce with embodiment 1
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.003Y
0.997)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.003Y
0.997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 16
By (Eu
0.001Y
0.999)
2O
3, (Ce
0.003Y
0.999)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1700 ℃, and soaking time is 16 hours, and other condition can get (Ce with embodiment 1
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.001Y
0.999)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.0003Y
0.9997)
3Al
5O
12/ (Eu
0.001Y
0.999)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 17
By (Eu
0.003Y
0.997)
2O
3, (Ce
0.005Y
0.995)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1750 ℃, and soaking time is 5 hours, and other condition can get (Ce with embodiment 1
0.005Y
0.995)
3Al
5O
12/ (Eu
0.003Y
0.997)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.005Y
0.995)
3Al
5O
12/ (Eu
0.003Y
0.997)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 18
By (Eu
0.01Y
0.99)
2O
3, (Ce
0.005Y
0.995)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1680 ℃, and soaking time is 20 hours, and other condition can get (Ce with embodiment 1
0.005Y
0.995)
3Al
5O
12/ (Eu
0.01Y
0.99)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.005Y
0.995)
3Al
5O
12/ (Eu
0.01Y
0.99)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 19
By (Eu
0.03Y
0.97)
2O
3, (Ce
0.01Y
0.99)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1780 ℃, and soaking time is 0.5 hour, and other condition can get (Ce with embodiment 1
0.01Y
0.99)
3Al
5O
12/ (Eu
0.03Y
0.97)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.01Y
0.99)
3Al
5O
12/ (Eu
0.03Y
0.97)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 20
By (Eu
0.01Y
0.99)
2O
3, (Ce
0.03Y
0.97)
3Al
5O
12Chemical constitution disposes each 50g of powder respectively, and the vacuum sintering holding temperature is 1780 ℃, and soaking time is 0.5 hour, and other condition can get (Ce with embodiment 1
0.03Y
0.97)
3Al
5O
12/ (Eu
0.01Y
0.99)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.01Y
0.99)
3Al
5O
12/ (Eu
0.03Y
0.97)
3Al
5O
12The composite transparent pottery of chemical constitution.
Embodiment 21
Adopt yttrium oxide (Y
2O
3), aluminum oxide (Al
2O
3), europium sesquioxide (Eu
2O
3), cerium oxide (CeO
2) be raw material, by (Eu
0.006Y
0.9993)
2O
3, (Ce
0.001Y
0.999)
3Al
5O
12Form and to configure two kinds of each 50g of powder respectively, use wet ball grinding to prepare ceramic powder respectively as medium more respectively with deionized water, two kinds of powders respectively through dry, sieve upper and lower two-layer compression molding or a compression molding respectively; Again it is imposed the 200MPa isostatic cool pressing and become base substrate, put into vacuum sintering furnace 1680 ℃ of following sintering 20 hours.
If adopt upper and lower two-layer compression molding respectively, with resulting two kinds of transparent fluorescence ceramics material surface polishings, the bonding (Ce that gets again in its side, junction
0.001Y
0.999)
3Al
5O
12/ (Eu
0.006Y
0.9994)
2O
3The transparent fluorescence ceramics of composite structure.
If adopt a compression molding,, obtain (Ce with resulting crystalline ceramics twin polishing
0.001Y
0.999)
3Al
5O
12/ (Eu
0.006Y
0.9994)
2O
3The transparent fluorescence ceramics of composite structure.
Same preparation technology may be implemented in (Ce
0.001Y
0.999)
3Al
5O
12/ (Eu
0.006Y
0.9994)
3Al
5O
12The composite transparent pottery of chemical constitution.
With (the Eu of lower floor
0.006Y
0.9994)
2O
3Or (Eu
0.006Y
0.9993)
3Al
5O
12The crystalline ceramics sanding and polishing is to 0.2mm, upper strata (Ce
0.001Y
0.999)
3Al
5O
12The crystalline ceramics sanding and polishing is to 0.45mm, and is blue-light excited down at 465nm, can obtain colour temperature gentleness, high-quality white light that colour rendering index is high.
Claims (4)
1. red/gold-tinted composite transparent pottery that is used for white light LEDs encapsulation, it is characterized in that being made up of two-layer crystalline ceramics up and down: the chemical constitution of upper strata crystalline ceramics is (Ce
yY
1-y)
3Al
5O
12, wherein the span of y is: 0.0003≤y≤0.06; The chemical constitution of lower floor's crystalline ceramics is (Eu
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3, wherein the span of x is: 0.0003≤x≤0.1.
2. the preparation method of the described composite transparent pottery of claim 1 it is characterized in that adopting upper and lower two-layer moulding preparation method respectively, or the once shaped preparation method prepares.
3. the preparation method of composite transparent pottery according to claim 2 is characterized in that the described upper and lower two-layer preparation method of moulding respectively comprises the following steps:
The chemical constitution of 1. selected composite transparent pottery and parameter x, y, adopting yttrium oxide, aluminum oxide, europium sesquioxide, cerium oxide is raw material, by upper strata crystalline ceramics (Ce
yY
1-y)
3Al
5O
12Chemical constitution and the crystalline ceramics (Eu of lower floor
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3Chemical constitution disposes upper strata transparent ceramic powder raw material and lower floor's transparent ceramic powder raw material respectively;
2. use wet ball grinding to prepare ceramic powder as medium more respectively with absolute ethyl alcohol or deionized water, two kinds of powders respectively through dry, sieve, the single shaft compressing tablet, again it is imposed the above isostatic cool pressing of 150MPa and becomes upper strata ceramic body and lower floor's ceramic body;
3. described upper strata ceramic body and lower floor's ceramic body are put into vacuum sintering furnace respectively 1650～1780 ℃ of insulations 0.5～24 hour; Or put into hot-pressed sintering furnace under 10～40MPa pressure; 1400～1700 ℃ of insulations 0.5～10 hour, obtain upper strata crystalline ceramics and lower floor's crystalline ceramics;
4. with described upper strata crystalline ceramics and lower floor's crystalline ceramics surface finish, again with the bonding composite transparent pottery that constitutes by upper strata crystalline ceramics and lower floor's crystalline ceramics of obtaining in the side of the junction of described upper strata crystalline ceramics and lower floor's crystalline ceramics.
4. the preparation method of composite transparent pottery according to claim 2 is characterized in that described once shaped preparation method comprises the following steps:
The chemical constitution of 1. selected composite transparent pottery and parameter x, y, adopting yttrium oxide, aluminum oxide, europium sesquioxide, cerium oxide is raw material, by upper strata crystalline ceramics (Ce
yY
1-y)
3Al
5O
12Chemical constitution and the crystalline ceramics (Eu of lower floor
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3Chemical constitution disposes upper strata transparent ceramic powder raw material and lower floor's transparent ceramic powder raw material respectively;
2. use wet ball grinding to prepare ceramic powder as medium more respectively with absolute ethyl alcohol or deionized water, two kinds of powders respectively through dry, sieve, the powder single shaft is pressed into contains the compound idiosome of two-layer heterogeneity up and down, it is (Ce at the middle and upper levels
yY
1-y)
3Al
5O
12Chemical constitution, lower floor is (Eu
xY
1-x)
3Al
5O
12Or (Eu
xY
1-x)
2O
3Chemical constitution imposes the above isostatic cool pressing of 150MPa to it again;
3. described composite ceramics base substrate is put into vacuum sintering furnace 1650～1780 ℃ of insulations 0.5～24 hour, or put into hot-pressed sintering furnace under 10～40MPa pressure,, obtain composite ceramics 1400～1700 ℃ of insulations 0.5～10 hour;
4. with described composite transparent ceramic surface polishing.
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Application publication date: 20120704 |