CN109133940A - A kind of yellow fluorescence complex phase ceramic and the preparation method and application thereof - Google Patents
A kind of yellow fluorescence complex phase ceramic and the preparation method and application thereof Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title claims abstract description 79
- 238000002360 preparation method Methods 0.000 title claims abstract description 23
- 238000000498 ball milling Methods 0.000 claims abstract description 29
- 238000000034 method Methods 0.000 claims abstract description 20
- 235000015895 biscuits Nutrition 0.000 claims abstract description 16
- 230000008569 process Effects 0.000 claims abstract description 13
- 238000003825 pressing Methods 0.000 claims abstract description 8
- 239000002994 raw material Substances 0.000 claims abstract description 8
- 238000007873 sieving Methods 0.000 claims abstract description 6
- 239000000126 substance Substances 0.000 claims abstract description 6
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 18
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 claims description 18
- 238000005245 sintering Methods 0.000 claims description 14
- 229910052757 nitrogen Inorganic materials 0.000 claims description 9
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 6
- 229910052710 silicon Inorganic materials 0.000 claims description 6
- 239000010703 silicon Substances 0.000 claims description 6
- 229910006415 θ-Al2O3 Inorganic materials 0.000 claims description 6
- 238000010792 warming Methods 0.000 claims description 5
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 4
- 239000001257 hydrogen Substances 0.000 claims description 4
- 229910052739 hydrogen Inorganic materials 0.000 claims description 4
- 238000011084 recovery Methods 0.000 claims 1
- 238000002156 mixing Methods 0.000 abstract description 12
- 229910019655 synthetic inorganic crystalline material Inorganic materials 0.000 description 40
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 13
- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 13
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 13
- 229910052593 corundum Inorganic materials 0.000 description 13
- 229910001845 yogo sapphire Inorganic materials 0.000 description 13
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 8
- 239000002002 slurry Substances 0.000 description 8
- 238000001035 drying Methods 0.000 description 7
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 description 6
- 239000007789 gas Substances 0.000 description 6
- 239000011812 mixed powder Substances 0.000 description 6
- 229960000935 dehydrated alcohol Drugs 0.000 description 5
- 239000000463 material Substances 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 4
- 239000012752 auxiliary agent Substances 0.000 description 3
- 229910010293 ceramic material Inorganic materials 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 230000003247 decreasing effect Effects 0.000 description 2
- 230000005284 excitation Effects 0.000 description 2
- 239000002223 garnet Substances 0.000 description 2
- 230000001795 light effect Effects 0.000 description 2
- 239000000377 silicon dioxide Substances 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 239000004411 aluminium Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 1
- 239000000292 calcium oxide Substances 0.000 description 1
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 125000004494 ethyl ester group Chemical group 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 230000002706 hydrostatic effect Effects 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000000395 magnesium oxide Substances 0.000 description 1
- 238000003701 mechanical milling Methods 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 230000008439 repair process Effects 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 229910019901 yttrium aluminum garnet Inorganic materials 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/58—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides
- C04B35/581—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides based on aluminium nitride
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/44—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on aluminates
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- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
- C04B35/62605—Treating the starting powders individually or as mixtures
- C04B35/6261—Milling
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- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
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- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
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Abstract
The present invention relates to a kind of yellow fluorescence complex phase ceramics and the preparation method and application thereof, belong to ceramic field.The raw material of the yellow fluorescence complex phase ceramic includes Ce3+: YAG and AlN, Ce3+: the chemical formula of YAG is [Y(1‑x)Cex]3Al5O12, x=0.05-3%.The yellow fluorescence complex phase ceramic thermal conductivity with higher, thermal stability and luminous intensity, heat fade are lower.Preparation method includes: mixing Ce3+: biscuit is made in YAG and AlN, ball milling, sieving, isostatic cool pressing, is sintered.The preparation method is simple, and time-consuming short, process is easily-controllable.It prepares resulting yellow fluorescence complex phase ceramic and can be used for preparing high power and show or illuminating device.
Description
Technical field
The invention belongs to ceramic field, in particular to a kind of yellow fluorescence complex phase ceramic and preparation method thereof with answer
With.
Background technique
The semiconductor lighting and display technology realized using light emitting diode, minimum, the environmental-friendly, longevity with power consumption
Many advantages, such as life is long and flexible in application is just increasingly obtaining the application popularization that various countries pay attention to and obtain social life various aspects.Example
Yellow light such as is generated using blue light LD or LED excitation fluorescence ceramics, yellow light is mainly Ce at present3+Yttrium-aluminium-garnet Y3Al5O12(letter
Claim YAG) ceramic material.The material of this garnet structure can launch the yellow light of 550nm under blue light excitation.However Ce3+:
YAG fluorescence ceramics in use, heat fade is significant, seriously constrain the practical application of YAG ceramic material in high power.
Summary of the invention
One of the objects of the present invention is to provide a kind of yellow fluorescence complex phase ceramic, the yellow fluorescence complex phase ceramic have compared with
High thermal conductivity, thermal stability and luminous intensity, heat fade are lower.
The second object of the present invention is to provide a kind of preparation method of above-mentioned yellow fluorescence complex phase ceramic, the preparation method
Simply, time-consuming short, process is easily-controllable.
The third object of the present invention is to provide a kind of application of above-mentioned yellow fluorescence complex phase ceramic, such as can be used
It is shown or illuminating device in preparing high power.
The present invention solves its technical problem and adopts the following technical solutions to realize.
The invention proposes a kind of yellow fluorescence complex phase ceramic, raw material includes Ce3+: YAG and AlN, Ce3+: the change of YAG
Formula is [Y(1-x)Cex]3Al5O12, x=0.05-3%.
The invention also provides a kind of preparation methods of above-mentioned yellow fluorescence complex phase ceramic, comprising the following steps:
Mix Ce3+: biscuit is made in YAG and AlN, ball milling, sieving, isostatic cool pressing, is sintered.
The invention also provides a kind of applications of above-mentioned yellow fluorescence complex phase ceramic, such as can be used for preparing high power
Display or illuminating device.
The beneficial effect packet of the yellow fluorescence complex phase ceramic that present pre-ferred embodiments provide and the preparation method and application thereof
It includes:
The yellow fluorescence complex phase ceramic that present pre-ferred embodiments provide is by by Ce3+: YAG and AlN cooperates, and keeps yellow glimmering
Phase ceramics thermal conductivity, thermal stability and luminous intensity with higher are recovered, heat fade is lower.Preparation method is simple, time-consuming
Short, process is easily-controllable.Resulting yellow fluorescence complex phase ceramic can be used for preparing high power and show or illuminating device, expand YAG ceramics
The scope of application of material, especially applicability under the conditions of high-power.
Specific embodiment
Yellow fluorescence complex phase ceramic provided in an embodiment of the present invention and the preparation method and application thereof is carried out specifically below
It is bright.
Yellow fluorescence complex phase ceramic provided by the present application, raw material include Ce3+: YAG and AlN.Wherein, Ce3+: the change of YAG
Formula is [Y(1-x)Cex]3Al5O12, x=0.05-3%.
In some embodiments, Ce3+: YAG can be prepared through following methods: by CeO2、Al2O3And Y2O3By chemistry
Formula is [Y(1-x)Cex]3Al5O12, x=0.05-3% mixing obtains oxide mixed powder, by oxide mixed powder and ball milling Jie
The common ball milling 4-12h of matter, dry, then sieving is sintered jointly with auxiliary agent.
It is preferably carried out in mode some, CeO2、Al2O3And Y2O3Purity be all larger than 99.99%.It is worth explanation
It is, in other embodiments, CeO2、Al2O3And Y2O3Purity may be lower than 99.99%.CeO2、Al2O3And Y2O3Preferably
Sub-micrometer scale.
In the application, ball milling can carry out ball milling in planetary ball mill, and Ball-milling Time for example can be 4-12h.Ball
Grinding media may include dehydrated alcohol, be convenient for rapid draing.
After ball milling, dry resulting slurry, such as be placed in dry in the drying box that temperature is 90-100 DEG C.Then it is sieved
Powder is made in (such as 200 mesh), and 9-11h is sintered under conditions of 1400-1500 DEG C, obtains Ce3+:YAG。
Optionally, auxiliary agent may include ethyl orthosilicate in the application.In sintering system, the quality of ethyl orthosilicate
Score effectively enough can prevent oxide from mixing for 0.6-1%, preferably 0.7-0.9% under this mass fraction range
Crystal transfer occurs during the sintering process for powder, and making mixed system, structure is finer and close during the sintering process.Specifically, positive silicic acid
The mass fraction of ethyl ester for example can be 0.6%, 0.7%, 0.8%, 0.9% or 1%, or 0.65%, 0.75%,
0.85% or 0.95%.It is worth noting that auxiliary agent may also include silica, calcium oxide or magnesia.
In the application, the preparation method of yellow fluorescence complex phase ceramic for example be may comprise steps of: mixing Ce3+: YAG with
Biscuit is made in AlN, ball milling, sieving, isostatic cool pressing, is sintered.
In some embodiments, it is used to prepare the Ce of yellow fluorescence complex phase ceramic3+: the mass ratio of YAG and AlN such as may be used
Think (2:8)-(8:2).Preferably, Ce3+: the mass ratio of YAG and AlN is (3:7)-(7:3).It is highly preferred that Ce3+: YAG with
The mass ratio of AlN is (3.5:6.5)-(4:6).
Specifically, Ce3+: the mass ratio of YAG and AlN can for 2:8,2.5:7.5,3:7,3.5:6.5,4:6,4.5:5.5,
5:5,5.5:4.5,6:4,6.5:3.5,7:3,7.5:2.5 or 8:2.It is worth noting that Ce in yellow fluorescence complex phase ceramic3+:
YAG content is too low, will be greatly reduced transfer efficiency, Ce3+: YAG too high levels, and can make thermal conductivity that cannot be promoted.
AlN in the application can be commercially available common AlN, preferably with θ-Al2O3For silicon source, using citric acid as nitrogen source
The AlN synthesized through carbothermic method.Uniform as AlN structure made from raw material using above two substance, partial size is tiny, can be more other
The AlN that raw material is prepared is more conducive to and Ce3+: the yellow fluorescence of high heat conductance, high thermal stability and high luminous intensity is made in YAG
Complex phase ceramic.
In the preparation process of yellow fluorescence complex phase ceramic, mechanical milling process can refer to preparation Ce3+: the ball milling mistake during YAG
Journey.Ball-milling medium also may include dehydrated alcohol, to prevent Y2O3Aquation is convenient for rapid draing.Ball milling can be in planetary type ball-milling
It is carried out in machine, Ball-milling Time for example may be 4-12h.
The dry resulting ball milling slurry of ball milling, sieving, in the isostatic cool pressing condition of room temperature (10-30 DEG C) and 180-220MPa
Under biscuit is made.The size of biscuit is set according to size needed for producing, and in one embodiment, the size of biscuit can be
Diameter of phi: 20mm, thickness d: 2mm.
Biscuit is sintered, yellow fluorescence complex phase ceramic is obtained.It is sintered in gas atmosphere and carries out, gas includes hydrogen and nitrogen
At least one of, to reduce the content of oxygen, oxygen atom is avoided to enter in the lattice of sinter phase, improves the cause of sinter phase
Close property.The flowing velocity of gas can be 55-65mL/min.It is preferably carried out in mode some, being sintered in flowing velocity is
The N of 60mL/min2It is carried out in atmosphere.
In the application, sintering includes temperature rise period, constant temperature stage and the temperature-fall period being carried out continuously, the temperature in constant temperature stage
For 1600-1800 DEG C (preferably 1650-1700 DEG C), constant temperature time 9-11h, the temperature rise period be in 2.5-3.5h from 10-
30 DEG C are warming up to 1600-1800 DEG C, temperature-fall period be in 4.5-5.5h from 1600-1800 DEG C of cooling room temperature.Thermostat temperature is low
It will cause that complex phase ceramic is bad at phase performance and remaining pore is excessive in 1600 DEG C, will cause sample higher than 1800 DEG C and burn,
At glassy state, light efficiency is reduced.Cooling step can eliminate the internal stress that may be introduced in sintering process.
Through above-mentioned sintering process, it can be avoided new phase constituent during nitride and oxide material cofiring and occur, it is real
Existing YAG phase and AlN phase coexist.Also, by using with θ-Al2O3It can for silicon source, the AlN synthesized by nitrogen source of citric acid
Make AlN and itself and Ce3+: the compound of YAG compactness extent with higher in above-mentioned sintering process, to significantly be promoted
The thermal conductivity of material reduces heat fade, improves luminous intensity.
Present invention also provides a kind of purposes of above-mentioned yellow fluorescence complex phase ceramic, such as can be used for preparing high power
Display or illuminating device expand the scope of application of YAG ceramic material, especially applicability under the conditions of high-power.
Feature and performance of the invention are described in further detail with reference to embodiments.
Embodiment 1
By CeO2、Al2O3And Y2O3It is [Y by chemical formula(1-x)Cex]3Al5O12, it is mixed to obtain oxide x=0.05% mixing
Close powder.Wherein, CeO2、Al2O3And Y2O3Purity be all larger than 99.99% and CeO2、Al2O3And Y2O3It is sub-micrometer scale.
By oxide mixed powder and dehydrated alcohol, ethyl orthosilicate the ball milling 10h in planetary ball mill jointly, by ball milling
Resulting slurry is dry in 100 DEG C of drying box, crosses 200 meshes, is sintered 10h under conditions of 1450 DEG C, obtains Ce3+:YAG。
In sintering system, the mass fraction of ethyl orthosilicate is 0.8%.
With 4:6 mixing Ce in parts by weight3+: YAG and AlN, then with dehydrated alcohol in planetary ball mill ball milling 10h,
The resulting slurry of ball milling is dry in 100 DEG C of drying box, 200 meshes are crossed, in room temperature and the isostatic cool pressing item of 200MPa
It is made that diameter of phi is 20mm, thickness d is 2mm biscuit under part.By above-mentioned biscuit in N2Flowing velocity be 60mL/min condition
Under be warming up to 1650 DEG C from 30 DEG C in 3h, maintain temperature 10h, 30 DEG C be then cooled in 5h, obtain yellow fluorescence complex phase
Ceramics.
Wherein, AlN is with θ-Al2O3For silicon source, the AlN synthesized by nitrogen source of citric acid through carbothermic method.
Embodiment 2
The present embodiment the difference from embodiment 1 is that: Ce3+: the proportion of YAG and AlN is 3.5:6.5.
Embodiment 3
The present embodiment the difference from embodiment 1 is that: Ce3+: the proportion of YAG and AlN is 3:7.
Embodiment 4
By CeO2、Al2O3And Y2O3It is [Y by chemical formula(1-x)Cex]3Al5O12, x=3% mixing, obtain oxide mixed powder
Body.Wherein, CeO2、Al2O3And Y2O3Purity be all larger than 99.99% and CeO2、Al2O3And Y2O3It is sub-micrometer scale.
By oxide mixed powder and dehydrated alcohol, ethyl orthosilicate the ball milling 4h in planetary ball mill jointly, by ball milling
Resulting slurry is dry in 90 DEG C of drying box, crosses 200 meshes, is sintered 11h under conditions of 1400 DEG C, obtains Ce3+:YAG.It burns
In knot body system, the mass fraction of ethyl orthosilicate is 0.6%.
With 3.5:6.5 mixing Ce in parts by weight3+: YAG and AlN, then with dehydrated alcohol jointly in planetary ball mill
Ball milling 4h, the resulting slurry of ball milling is dry in 90 DEG C of drying box, 200 meshes are crossed, in the cold etc. of room temperature and 180MPa
It is made that diameter of phi is 20mm, thickness d is 2mm biscuit under hydrostatic pressure condition.By above-mentioned biscuit in N2Flowing velocity be 55mL/min
Under conditions of be warming up to 1600 DEG C from 20 DEG C in 2.5h, maintain temperature 9h, 20 DEG C be then cooled in 4.5h, obtains yellow
Fluorescence complex phase ceramic.
Wherein, AlN is with θ-Al2O3For silicon source, the AlN synthesized by nitrogen source of citric acid through carbothermic method.
Embodiment 5
By CeO2、Al2O3And Y2O3It is [Y by chemical formula(1-x)Cex]3Al5O12, x=0.5% mixing, obtain oxide mixing
Powder.Wherein, CeO2、Al2O3And Y2O3Purity be all larger than 99.99% and CeO2、Al2O3And Y2O3It is sub-micrometer scale.
By oxide mixed powder and dehydrated alcohol, ethyl orthosilicate the ball milling 12h in planetary ball mill jointly, by ball milling
Resulting slurry is dry in 95 DEG C of drying box, crosses 200 meshes, is sintered 9h under conditions of 1500 DEG C, obtains Ce3+:YAG.It burns
In knot body system, the mass fraction of ethyl orthosilicate is 1%.
With 3:7 mixing Ce in parts by weight3+: YAG and AlN, then with the dehydrated alcohol ball milling in planetary ball mill jointly
12h, the resulting slurry of ball milling is dry in 95 DEG C of drying box, 200 meshes are crossed, in the isostatic cool pressing of room temperature and 220MPa
Under the conditions of be made that diameter of phi is 20mm, thickness d is 2mm biscuit.By above-mentioned biscuit in N2Flowing velocity be 65mL/min item
1800 DEG C are warming up to from 10 DEG C in 3.5h under part, temperature 11h is maintained, 10 DEG C is then cooled in 5.5h, it is glimmering to obtain yellow
Recover phase ceramics.
Wherein, AlN is with θ-Al2O3For silicon source, the AlN synthesized by nitrogen source of citric acid through carbothermic method.
Embodiment 6
The present embodiment the difference from embodiment 1 is that: Ce3+: ethyl orthosilicate is in sintering system in YAG preparation process
Mass fraction is 0.7wt%.
Embodiment 7
The present embodiment the difference from embodiment 1 is that: Ce3+: it is sintered and helps in YAG and yellow fluorescence complex phase ceramic preparation process
Agent is silica.
Embodiment 8
The present embodiment the difference from embodiment 1 is that: Ce in yellow fluorescence complex phase ceramic3+: the mass ratio of YAG and AlN is
7:3。
Embodiment 9
The present embodiment the difference from embodiment 1 is that: Ce in yellow fluorescence complex phase ceramic3+: the mass ratio of YAG and AlN is
2:8。
Embodiment 10
The present embodiment the difference from embodiment 1 is that: Ce in yellow fluorescence complex phase ceramic3+: the mass ratio of YAG and AlN is
8:2。
Embodiment 11
The present embodiment the difference from embodiment 1 is that: AlN be the commercially available Direct-Nitridation as aluminium powder obtained by product.
Embodiment 12
The present embodiment the difference from embodiment 1 is that: the sintering process of biscuit, the gas of flowing are hydrogen.
Embodiment 13
The present embodiment the difference from embodiment 1 is that: the sintering process of biscuit, the gas of flowing are that flow-rate ratio is 2:1's
The mixed gas of nitrogen and hydrogen.
Embodiment 14
The present embodiment provides a kind of applications of yellow fluorescence complex phase ceramic, are used for preparing illuminating device, wherein yellow
Fluorescence complex phase ceramic can refer to the yellow fluorescence complex phase ceramic of embodiment 1-13 any embodiment offer.
Test example 1
Embodiment above-described embodiment 1-13 is repeated, enough yellow fluorescence complex phase ceramics are obtained.To use convention transparent
The ceramics for not mixing AlN of ceramic process preparation are control group, and the yellow fluorescence complex phase ceramic that the application is prepared is as examination
Test group, test group and control group is each takes 5 samples according to " GB/T 22588-2008 flicker method measures thermal diffusion coefficient at random
Or thermal coefficient " thermal conductivity test is carried out, it is measured according to spectroanalysis instrument integrating sphere light efficiency, the results are shown in Table 1.
1 test result of table
As can be seen from Table 1, the thermal conductivity of test group ceramics and light efficiency illustrate this Shen obviously higher than control group ceramics
Please provided by mixed with AlN yellow fluorescence complex phase ceramic can it is more in the prior art ceramics have higher thermal conductivity and light
Effect.
In addition, the ceramics that provide of test group under conditions of 300 DEG C using 100h after thermal stability without being decreased obviously, compare
Group provide ceramics under conditions of 300 DEG C using 100h after thermal stability be decreased obviously, illustrate it is provided herein mixed with
The yellow fluorescence complex phase ceramic of AlN can be more in the prior art ceramic with high thermal stability.
Test example 2
By taking embodiment 1 as an example, be arranged contrast groups 1-6, wherein contrast groups 1-5 the difference from embodiment 1 is that: yellow fluorescence
The Ce of complex phase ceramic3+: the mass ratio of YAG and AlN is followed successively by 3.5:6.5,3:7,2:8 (embodiment 9), 1:9 and 10:0, comparison
Group 6 is embodiment 11.
It is surveyed by yellow fluorescence complex phase ceramic of the test method in test example 1 to embodiment 1 and contrast groups 1-6
Examination, every group of result are the average value of 5 samples randomly selected in the group, and the results are shown in Table 2.
2 test result of table
As can be seen from Table 2, the thermal conductivity of the ceramics of contrast groups 5 and light efficiency are minimum, and illustrating can be bright containing AlN in raw material
The aobvious thermal conductivity for improving ceramics.
The thermal conductivity of the ceramics of embodiment 1 and contrast groups 1 is lower than contrast groups 2-3, but light efficiency is higher than contrast groups 2-3,
In terms of comprehensive in conjunction with thermal conductivity and light efficiency, Ce in embodiment 1 and contrast groups 13+: matching for YAG and AlN compares contrast groups 2-3 more
Conducive to making yellow fluorescence complex phase ceramic while there is preferable thermal conductivity and light efficiency.
Contrast groups 4 ceramics thermal conductivity be higher than embodiment 1 and contrast groups 1-3, but light efficiency significantly lower than embodiment 1 with
And contrast groups 1-3, illustrate that the mass percent of AlN in raw material is unfavorable for yellow fluorescence complex phase ceramic higher than 80% and has preferable light
Effect.
The thermal conductivity and light efficiency of the ceramics of contrast groups 6 are obviously lower compared with the thermal conductivity and light efficiency of 1 ceramics of embodiment, say
AlN is more conducive to make yellow fluorescence complex phase ceramic while having preferable thermal conductivity and light efficiency in bright embodiment 1.
In conclusion yellow fluorescence complex phase ceramic provided by the present application is by by Ce3+: YAG and AlN cooperates, and keeps yellow glimmering
Phase ceramics thermal conductivity, thermal stability and luminous intensity with higher are recovered, heat fade is lower.Preparation method is simple, time-consuming
Short, process is easily-controllable.Resulting yellow fluorescence complex phase ceramic can be used for preparing high power and show or illuminating device, expand YAG ceramics
The scope of application of material, especially applicability under the conditions of high-power.
The foregoing is only a preferred embodiment of the present invention, is not intended to restrict the invention, for the skill of this field
For art personnel, the invention may be variously modified and varied.All within the spirits and principles of the present invention, made any to repair
Change, equivalent replacement, improvement etc., should all be included in the protection scope of the present invention.
Claims (10)
1. a kind of yellow fluorescence complex phase ceramic, which is characterized in that the raw material of the yellow fluorescence complex phase ceramic includes Ce3+: YAG and
AlN, the Ce3+: the chemical formula of YAG is [Y(1-x)Cex]3Al5O12, x=0.05-3%.
2. yellow fluorescence complex phase ceramic according to claim 1, which is characterized in that the Ce3+: the matter of YAG and the AlN
Amount is than being (2:8)-(8:2).
3. yellow fluorescence complex phase ceramic according to claim 2, which is characterized in that the Ce3+: the matter of YAG and the AlN
Amount is than being (3:7)-(7:3).
4. yellow fluorescence complex phase ceramic according to claim 3, which is characterized in that the Ce3+: the matter of YAG and the AlN
Amount is than being (3.5:6.5)-(4:6).
5. yellow fluorescence complex phase ceramic according to claim 1-4, which is characterized in that the AlN is with θ-Al2O3
It is prepared for silicon source, by nitrogen source of citric acid.
6. the preparation method of yellow fluorescence complex phase ceramic as described in any one in claim 1-5, which is characterized in that including following
Step:
Mix the Ce3+: biscuit is made in the YAG and AlN, ball milling, sieving, isostatic cool pressing, is sintered.
7. preparation method according to claim 6, which is characterized in that isostatic cool pressing is in 10-30 DEG C and 180-220MPa
Under conditions of carry out.
8. preparation method according to claim 6, which is characterized in that sintering process is that nitrogen or hydrogen atmosphere are sintered.
9. preparation method according to claim 6, which is characterized in that sintering includes the temperature rise period being carried out continuously, constant temperature
Stage and temperature-fall period, constant temperature stage are that 1600-1800 DEG C of sintering temperature is maintained 9-11h, and the temperature rise period is in 2.5-
It is warming up to 1600-1800 DEG C in 3.5h from 10-30 DEG C, temperature-fall period is in being cooled to 10- from 1600-1800 DEG C in 4.5-5.5h
30℃。
10. the application of yellow fluorescence complex phase ceramic as described in any one in claim 1-5, which is characterized in that the yellow is glimmering
Recovery phase ceramics are used to prepare high power and show or illuminating device.
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