CN116813327A - Preparation method of composite fluorescent ceramic - Google Patents
Preparation method of composite fluorescent ceramic Download PDFInfo
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- CN116813327A CN116813327A CN202310684424.3A CN202310684424A CN116813327A CN 116813327 A CN116813327 A CN 116813327A CN 202310684424 A CN202310684424 A CN 202310684424A CN 116813327 A CN116813327 A CN 116813327A
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- 239000000919 ceramic Substances 0.000 title claims abstract description 152
- 239000002131 composite material Substances 0.000 title claims abstract description 43
- 238000002360 preparation method Methods 0.000 title claims abstract description 18
- 238000005245 sintering Methods 0.000 claims abstract description 46
- 235000015895 biscuits Nutrition 0.000 claims abstract description 34
- 238000005266 casting Methods 0.000 claims abstract description 15
- 238000010345 tape casting Methods 0.000 claims abstract description 9
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 claims description 27
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 20
- 238000000498 ball milling Methods 0.000 claims description 20
- 238000000034 method Methods 0.000 claims description 16
- 239000000843 powder Substances 0.000 claims description 15
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 14
- 238000005520 cutting process Methods 0.000 claims description 12
- 238000002156 mixing Methods 0.000 claims description 11
- 239000002994 raw material Substances 0.000 claims description 10
- 238000007873 sieving Methods 0.000 claims description 10
- 239000002002 slurry Substances 0.000 claims description 10
- 238000002834 transmittance Methods 0.000 claims description 10
- 238000001035 drying Methods 0.000 claims description 9
- 238000005498 polishing Methods 0.000 claims description 7
- 230000008569 process Effects 0.000 claims description 7
- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 6
- 238000003475 lamination Methods 0.000 claims description 6
- 239000011812 mixed powder Substances 0.000 claims description 5
- 238000000465 moulding Methods 0.000 claims description 5
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 claims description 5
- 238000010030 laminating Methods 0.000 claims description 4
- 238000004519 manufacturing process Methods 0.000 claims description 2
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 2
- 238000004321 preservation Methods 0.000 claims description 2
- 238000012216 screening Methods 0.000 claims description 2
- 150000002576 ketones Chemical class 0.000 claims 1
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 claims 1
- 238000005303 weighing Methods 0.000 claims 1
- 230000017525 heat dissipation Effects 0.000 abstract description 6
- 238000005286 illumination Methods 0.000 abstract description 6
- 238000004020 luminiscence type Methods 0.000 abstract description 6
- 239000000758 substrate Substances 0.000 abstract description 5
- 239000000203 mixture Substances 0.000 abstract description 4
- 238000007493 shaping process Methods 0.000 abstract description 3
- 239000002344 surface layer Substances 0.000 description 6
- 230000000694 effects Effects 0.000 description 5
- 238000010791 quenching Methods 0.000 description 5
- 230000000171 quenching effect Effects 0.000 description 5
- 238000000748 compression moulding Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 230000004907 flux Effects 0.000 description 3
- 239000000463 material Substances 0.000 description 2
- 238000004806 packaging method and process Methods 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 229910052594 sapphire Inorganic materials 0.000 description 2
- 239000010980 sapphire Substances 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000012190 activator Substances 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 238000010344 co-firing Methods 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000005056 compaction Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
- 239000000741 silica gel Substances 0.000 description 1
- 229910002027 silica gel Inorganic materials 0.000 description 1
- 229910000679 solder Inorganic materials 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
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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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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
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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
- C04B35/50—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on rare-earth compounds
- C04B35/505—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on rare-earth compounds based on yttrium oxide
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- C—CHEMISTRY; METALLURGY
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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
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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
- C04B35/64—Burning or sintering processes
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F21—LIGHTING
- F21V—FUNCTIONAL FEATURES OR DETAILS OF LIGHTING DEVICES OR SYSTEMS THEREOF; STRUCTURAL COMBINATIONS OF LIGHTING DEVICES WITH OTHER ARTICLES, NOT OTHERWISE PROVIDED FOR
- F21V9/00—Elements for modifying spectral properties, polarisation or intensity of the light emitted, e.g. filters
- F21V9/30—Elements containing photoluminescent material distinct from or spaced from the light source
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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
- C04B2235/3229—Cerium oxides or oxide-forming salts thereof
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- C04B2235/6581—Total pressure below 1 atmosphere, e.g. vacuum
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- C04B2235/65—Aspects relating to heat treatments of ceramic bodies such as green ceramics or pre-sintered ceramics, e.g. burning, sintering or melting processes
- C04B2235/66—Specific sintering techniques, e.g. centrifugal sintering
- C04B2235/668—Pressureless sintering
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- C04B2235/9646—Optical properties
Abstract
The invention discloses a preparation method of composite fluorescent ceramics, and relates to the technical field of laser illumination. The composite fluorescent ceramic consists of a Ce YAG fluorescent ceramic and a YAG transparent ceramic plate up and down; the preparation method comprises the following steps: firstly, preparing YAG transparent ceramic plates; secondly, preparing a Ce-YAG tape casting biscuit; and finally, combining the Ce-YAG casting biscuit with the YAG transparent ceramic plate up and down, and putting the mixture into a vacuum sintering furnace for sintering. The invention adopts a cofiring scheme to sinter the Ce-YAG tape casting biscuit on the YAG transparent ceramic sheet, is tightly adhered with the heat dissipation substrate, has excellent heat dissipation performance and stable luminescence; meanwhile, the fluorescent ceramic has the size of millimeter level, smaller luminous area, higher brightness and lower light shaping difficulty.
Description
Technical Field
The invention relates to the technical field of laser illumination, in particular to a preparation method of composite fluorescent ceramics.
Background
Laser Diode (LD) is the next generation illumination technology following white LED illumination technology. With the gradual development of laser illumination to high brightness, the rapidly increased thermal load, thermal shock and continuously compressed space bring more serious challenges to the reliability, light efficiency and luminescence stability of fluorescent ceramics. Researchers at home and abroad have conducted extensive researches on the cause of thermal effects. The university of Korea Chengjun proposes the application of fluorescent ceramics to high-power laser-driven automotive headlights for the first time, and as a result, it was found that different light saturation thresholds are mainly caused by the concentration of the activator, and the highest power density is 19.1W/mm 2 The method comprises the steps of carrying out a first treatment on the surface of the Thermal quenching is considered by the university of Norway to be an important factor in the reduction of luminous flux; studies by Eulerian Germany show that as temperature increases, quantum efficiency decreases, which can lead to thermal "runaway", ultimately leading to thermal saturation. The university of Jiangsu analyzed that the main reasons for lower luminous efficiency than LEDs when applied to laser lighting applications were luminescence thermal quenching and concentration quenching, and first confirmed that the thermal quenching ratio was 4 times the concentration quenching ratio. The high-temperature thermal attenuation under the high-energy laser radiation is mainly characterized by thermal-induced quantum efficiency reduction, chromaticity drift, luminescence saturation and the like, and becomes a key technical bottleneck for influencing the wide application of fluorescent ceramics.
The main technical proposal for relieving the heat effect is to introduce a scattering function two-phase (Al 2 O 3 Material) to increase the thermal conductivity of the fluorescent ceramic. However, current research work is almost always focused on large-size complex-phase fluorescent ceramicsGreatly reduces the luminous brightness (lm/mm) 2 )。
In addition, the packaging form of the complex phase ceramic material also has the following fatal problems:
1. the connection mode of the complex phase ceramic and the sapphire substrate. The aluminum oxide substrate after coating is difficult to be adhered to the complex phase ceramic in the current technical scheme, and the heat dissipation capacity of the complex phase ceramic is greatly attenuated by mechanical fixing or silica gel adhesion.
2. And the complex phase ceramic and the sapphire are co-fired. The cofiring mode needs to search sintering temperature; the co-firing technology of single crystals and ceramics has great difficulty, extremely high requirements on the precision of equipment and is not beneficial to industrialized production.
3. The complex phase ceramic is fixed on the red copper substrate through solder. The packaging mode is reflective, is only suitable for the field of laser projection, and can cause obvious blue spots in a laser lighting system to influence the lighting effect.
Therefore, a technical scheme capable of reducing the size of the laser-illuminated fluorescent ceramic and realizing stable operation of the fluorescent material is highly demanded.
Disclosure of Invention
In view of the above, the invention discloses a preparation method of composite fluorescent ceramics, which adopts a cofiring scheme to prepare the composite fluorescent ceramics, and has the advantages of small area of a light-emitting unit, high brightness and low light shaping difficulty; the adhesion between the YAG tape casting biscuit and the transparent ceramic is stronger, the heat dissipation effect is better, the operating temperature is low, and the luminous efficiency is high.
According to the preparation method of the composite fluorescent ceramic provided by the invention, the composite fluorescent ceramic consists of Ce, YAG fluorescent ceramic and YAG transparent ceramic plates; the preparation method comprises the following steps:
step one: and preparing the YAG transparent ceramic plate.
S1-1, proportioning: alumina and yttrium oxide are respectively weighed according to the stoichiometric ratio of each element in YAG.
S1-2, ball milling: mixing the raw material powder by adopting alumina balls.
S1-3, sieving: and drying and sieving the mixed powder.
S1-4, tabletting: and (5) compacting and forming the sieved powder by adopting a dry press.
S1-5, vacuum sintering: and (5) putting the pressed biscuit into a vacuum sintering furnace, and sintering the biscuit.
S1-6, polishing and cutting: polishing and cutting the upper and lower surfaces of the ceramic.
Step two: preparing Ce-YAG casting biscuit.
S2-1, proportioning: y is respectively weighed according to the stoichiometric ratio of each element in Ce-YAG 2 O 3 、Al 2 O 3 、Ce 2 O, methyl ethyl ketone and 95% ethanol are added.
S2-2, ball milling: mixing the raw material powder by adopting alumina balls.
S2-3, defoaming: and removing bubbles in the ceramic slurry by adopting a vacuum bubble removing mode.
S2-4, molding: pouring the slurry after bubble removal into a trough of a casting machine.
S2-5, lamination and cutting: and (5) laminating the biscuit.
Step three: and preparing the composite fluorescent ceramic device.
S3-1, sintering: and combining the Ce-YAG casting biscuit with the YAG transparent ceramic plate up and down, and placing the combined Ce-YAG casting biscuit and the YAG transparent ceramic plate into a vacuum sintering furnace for sintering to obtain the fluorescent ceramic device based on the combination of the Ce-YAG fluorescent ceramic and the YAG transparent ceramic plate.
Preferably, in S1-2, the ball milling time is 24-48 hours; the ball milling rotating speed is 140-150 r/min.
Preferably, in S1-3, the drying temperature is 40-65 ℃ and the drying time is 15-20 hours; the number of the screening meshes is 100-200 meshes.
Preferably, in S1-4, the tabletting pressure is 4-20 Mpa, and the pressure is maintained for 2-10 min.
Preferably, in S1-5, the sintering temperature is 1750-1780 ℃, and the temperature is kept for 12-24 hours.
Preferably, in S2-1, the mass ratio of methyl ethyl ketone to 95% ethanol is 1.5:1.0-2.0:1.0.
Preferably, in S3-1, the sintering temperature is 1650-1750 ℃, the heat preservation time is 10-12 h, and a weight with the mass of 2.0-3.0 kg is placed above the composite fluorescent ceramic in the sintering process.
Preferably, in the Ce-YAG fluorescent ceramic, the doping concentration of Ce is 0.05-0.2at%; the thickness is 0.5-1.0 mm, and the side length is 1.0-2.0 mm; the YAG transparent ceramic plate has a diameter of 16.0-20.0 mm and a thickness of 0.5-1.0 mm.
Preferably, the YAG transparent ceramic plate has a linear transmittance of 79.0-81.0% at 800nm, and the linear transmittance of the fluorescent ceramic device compounded by the YAG fluorescent ceramic and the YAG transparent ceramic plate based on Ce is 5.0-20.0%.
Preferably, the prepared composite fluorescent ceramic device has the luminous efficiency of 150-180 lm/W and the brightness of 405-1350 lm/mm 2 。
Compared with the prior art, the preparation method of the composite fluorescent ceramic has the advantages that:
(1) The invention adopts a cofiring scheme to sinter the Ce-YAG tape casting biscuit on the YAG transparent ceramic sheet, and the Ce-YAG tape casting biscuit is tightly adhered to a heat dissipation substrate, and has excellent heat dissipation performance and stable luminescence. In addition, the sintering temperature is controlled to form the pore-Ce-YAG fluorescent ceramic, which accords with the laser propagation characteristic and has more uniform luminescence.
(2) The fluorescent ceramic has the size of millimeter level, compared with the prior large-size fluorescent ceramic deviceThe LED lamp has smaller luminous area, higher brightness and lower light shaping difficulty. Meanwhile, the millimeter-level size is very good to match with the laser spot, and the light mixing and illumination effects are more excellent.
(3) According to the invention, weight compaction is adopted in the ceramic sintering process, so that the combination degree of the Ce-YAG casting biscuit and the YAG transparent ceramic plate is improved.
Drawings
For a clearer description of embodiments of the invention or of the prior art, the drawings which are used in the description of the embodiments or of the prior art will be briefly described, it being evident that the drawings in the description below are only some embodiments of the invention, and that other drawings can be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a schematic diagram of a composite fluorescent ceramic.
FIG. 2 is a flow chart of a method for preparing composite fluorescent ceramics according to the present invention.
In the figure: YAG fluorescent ceramics; 2-YAG transparent ceramic plate.
Detailed Description
The following is a brief description of embodiments of the present invention with reference to the accompanying drawings. It is apparent that the described embodiments are only some embodiments of the present invention, but not all embodiments, and that all other embodiments obtained by a person having ordinary skill in the art without making creative efforts based on the embodiments in the present invention are within the protection scope of the present invention.
Fig. 1-2 illustrate a preferred embodiment of the present invention, which is described in detail.
Example 1
The invention discloses a preparation method of composite fluorescent ceramics, which is shown in figure 1, wherein the prepared composite fluorescent ceramics comprises a Ce-YAG fluorescent ceramics 1 and a YAG transparent ceramic plate 2, wherein the upper surface layer is the Ce-YAG fluorescent ceramics 1, and the lower surface layer is the YAG transparent ceramic plate 2. The linear transmittance of the YAG transparent ceramic plate 2at 800nm is 79.0%, and the linear transmittance of the fluorescent ceramic device compounded by the YAG fluorescent ceramic 1 and the YAG transparent ceramic plate 2at 800nm is 5.0% based on Ce.
As shown in fig. 2, the preparation method comprises the following steps:
step one: a YAG transparent ceramic plate 2 was prepared.
S1-1, proportioning: alumina and yttrium oxide are respectively weighed according to the stoichiometric ratio of each element in YAG.
S1-2, ball milling: mixing the raw material powder by adopting an alumina ball, wherein the ball milling time is 24 hours, and the ball milling rotating speed is 140r/min.
S1-3, sieving: drying the mixed powder at 40 ℃ for 15 hours; sieving with 100 mesh sieve.
S1-4, tabletting: and (3) carrying out compression molding on the sieved powder by adopting a dry press, wherein the tabletting pressure is 4.0Mpa, and the pressure is maintained for 2.0min.
S1-5, vacuum sintering: and (3) putting the pressed biscuit into a vacuum sintering furnace, sintering the biscuit at 1750 ℃ and preserving heat for 12 hours.
S1-6, polishing and cutting: the upper and lower surfaces of the ceramic were polished and cut to a final diameter of 16.0mm and a thickness of 0.5mm.
Step two: preparing Ce-YAG casting biscuit.
S2-1, proportioning: y is respectively weighed according to the stoichiometric ratio of each element in Ce-YAG 2 O 3 、Al 2 O 3 、Ce 2 O, wherein the doping concentration of Ce is 0.2at.%. Methyl ethyl ketone and 95% ethanol are added, and the mass ratio of the methyl ethyl ketone to the 95% ethanol is 1.5:1.0.
S2-2, ball milling: mixing the raw material powder by adopting alumina balls.
S2-3, defoaming: and removing bubbles in the ceramic slurry by adopting a vacuum bubble removing mode.
S2-4, molding: pouring the slurry after bubble removal into a trough of a casting machine.
S2-5, lamination and cutting: laminating the biscuit with the final thickness of 0.5mm; the side length is 1.0mm.
Step three: and preparing the composite fluorescent ceramic device.
S3-1, sintering: and (3) combining the Ce-YAG tape casting biscuit with the YAG transparent ceramic plate 2 up and down, and placing the mixture into a vacuum sintering furnace for sintering at a sintering temperature of 1650 ℃ for 10 hours. And placing a weight with the mass of 2.0kg above the composite fluorescent ceramic in the sintering process to finally obtain the fluorescent ceramic device based on the composite of the Ce-YAG fluorescent ceramic and the YAG transparent ceramic plate.
The complex-phase fluorescent ceramic device is excited by laser, and when the blue light output power of the laser is 9W, the complex-phase fluorescent ceramic device stably emits light: the operating temperature of the light-emitting unit is 120 ℃; the luminous efficiency is 150lm/W; the light flux is up to 1350lm; lumen density of 1350lm/mm 2 。
Example 2
The invention discloses a preparation method of composite fluorescent ceramics, which is shown in figure 1 and consists of a Ce-YAG fluorescent ceramic 1 and a YAG transparent ceramic plate 2, wherein the upper surface layer is the Ce-YAG fluorescent ceramic 1, and the lower surface layer is the YAG transparent ceramic plate 2. The linear transmittance of the YAG transparent ceramic plate 2at 800nm is 81.0%, and the linear transmittance of the fluorescent ceramic device based on the combination of the Ce, YAG fluorescent ceramic 1 and the YAG transparent ceramic plate 2at 800nm is 20.0%.
As shown in fig. 2, the preparation method comprises the following steps:
step one: a YAG transparent ceramic plate 2 was prepared.
S1-1, proportioning: alumina and yttrium oxide are respectively weighed according to the stoichiometric ratio of each element in YAG.
S1-2, ball milling: mixing the raw material powder by adopting alumina balls, wherein the ball milling time is 48 hours, and the ball milling rotating speed is 150r/min.
S1-3, sieving: drying the mixed powder for 20 hours at 65 ℃; sieving with 200 mesh sieve.
S1-4, tabletting: and (3) carrying out compression molding on the sieved powder by adopting a dry press, wherein the tabletting pressure is 20Mpa, and the pressure is maintained for 10min.
S1-5, vacuum sintering: and (3) putting the pressed biscuit into a vacuum sintering furnace, sintering the biscuit at 1780 ℃ and preserving the heat for 24 hours.
S1-6, polishing and cutting: the upper and lower surfaces of the ceramic were polished and cut to a final diameter of 20.0mm and a thickness of 1.0mm.
Step two: preparing Ce-YAG casting biscuit.
S2-1, proportioning: y is respectively weighed according to the stoichiometric ratio of each element in Ce-YAG 2 O 3 、Al 2 O 3 、Ce 2 O, where CeThe doping concentration was 0.05at.%. Methyl ethyl ketone and 95% ethanol are added, and the mass ratio of the methyl ethyl ketone to the 95% ethanol is 2.0:1.0.
S2-2, ball milling: mixing the raw material powder by adopting alumina balls.
S2-3, defoaming: and removing bubbles in the ceramic slurry by adopting a vacuum bubble removing mode.
S2-4, molding: pouring the slurry after bubble removal into a trough of a casting machine.
S2-5, lamination and cutting: the biscuit is subjected to lamination treatment, and the final thickness is 1.0mm and the side length is 2.0mm.
Step three: and preparing the composite fluorescent ceramic device.
S3-1, sintering: and (3) combining the Ce-YAG tape casting biscuit with the YAG transparent ceramic plate 2 up and down, and placing the mixture into a vacuum sintering furnace for sintering at 1750 ℃ for 12 hours. And placing a weight with the mass of 3.0kg above the composite fluorescent ceramic in the sintering process to finally obtain the fluorescent ceramic device based on the composite of the Ce-YAG fluorescent ceramic and the YAG transparent ceramic sheet.
The complex-phase fluorescent ceramic device is excited by laser, and when the blue light output power of the laser is 9W, the complex-phase fluorescent ceramic device stably emits light: the operating temperature of the light-emitting unit is 100 ℃; the luminous efficiency is 180lm/W; the light flux is as high as 1620lm; lumen density of 405lm/mm 2 。
Comparative example
The invention discloses a preparation method of composite fluorescent ceramics, which is shown in figure 1 and consists of a Ce-YAG fluorescent ceramic 1 and a YAG transparent ceramic plate 2, wherein the upper surface layer is the Ce-YAG fluorescent ceramic 1, and the lower surface layer is the YAG transparent ceramic plate 2. The linear transmittance of the YAG transparent ceramic plate 2at 800nm is 81.0%, and the linear transmittance of the fluorescent ceramic device based on the combination of the Ce, YAG fluorescent ceramic 1 and the YAG transparent ceramic plate 2at 800nm is 12.0%.
As shown in fig. 2, the preparation method comprises the following steps:
step one: a YAG transparent ceramic plate 2 was prepared.
S1-1, proportioning: alumina and yttrium oxide are respectively weighed according to the stoichiometric ratio of each element in YAG.
S1-2, ball milling: mixing the raw material powder by adopting alumina balls, wherein the ball milling time is 48 hours, and the ball milling rotating speed is 150r/min.
S1-3, sieving: drying the mixed powder at 60 ℃ for 16 hours; sieving with 200 mesh sieve.
S1-4, tabletting: and (3) carrying out compression molding on the sieved powder by adopting a dry press, wherein the tabletting pressure is 20Mpa, and the pressure is maintained for 10min.
S1-5, vacuum sintering: and (3) putting the pressed biscuit into a vacuum sintering furnace, sintering the biscuit at 1780 ℃ and preserving the heat for 24 hours.
S1-6, polishing and cutting: the upper and lower surfaces of the ceramic were polished and cut to a final diameter of 20.0mm and a thickness of 1.0mm.
Step two: preparing Ce-YAG casting biscuit.
S2-1, proportioning: y is respectively weighed according to the stoichiometric ratio of each element in Ce-YAG 2 O 3 、Al 2 O 3 、Ce 2 O, wherein the doping concentration of Ce is 0.10at.%. Methyl ethyl ketone and 95% ethanol are added, and the mass ratio of the methyl ethyl ketone to the 95% ethanol is 2.0:1.0.
S2-2, ball milling: mixing the raw material powder by adopting alumina balls.
S2-3, defoaming: and removing bubbles in the ceramic slurry by adopting a vacuum bubble removing mode.
S2-4, molding: pouring the slurry after bubble removal into a trough of a casting machine.
S2-5, lamination and cutting: and (5) laminating the biscuit. The final thickness was 1.0mm; the side length is 2.0mm.
Step three: and preparing the composite fluorescent ceramic device.
S3-1, sintering: and (3) combining the Ce-YAG tape casting biscuit with the YAG transparent ceramic plate 2 up and down, and placing the mixture into a vacuum sintering furnace for sintering at 1750 ℃ for 12 hours. And (3) no heavy object is placed above the composite fluorescent ceramic in the sintering process, and finally the fluorescent ceramic device based on the composite of the Ce-YAG fluorescent ceramic and the YAG transparent ceramic sheet is obtained.
When the blue light output power of the laser is 9W, the temperature of the luminescence center of the complex phase fluorescent ceramic device is rapidly increased, and as no heavy object is placed above the complex fluorescent ceramic in the sintering process, after the complex phase fluorescent ceramic device is cooled, ce is that the YAG fluorescent ceramic 1 falls off from the surface of the YAG transparent ceramic plate 2, and the device fails.
The previous description of the disclosed embodiments is provided to enable any person skilled in the art to make or use the present invention. Various modifications to these embodiments will be readily apparent to those skilled in the art, and the generic principles defined herein may be applied to other embodiments without departing from the spirit or scope of the invention. Thus, the present invention is not intended to be limited to the embodiments shown herein but is to be accorded the widest scope consistent with the principles and novel features disclosed herein.
Claims (10)
1. A preparation method of composite fluorescent ceramics is characterized in that the composite fluorescent ceramics consist of a Ce-YAG fluorescent ceramics (1) and a YAG transparent ceramic plate (2) up and down; the preparation method comprises the following steps:
step one: preparing a YAG transparent ceramic sheet (2);
s1-1, proportioning: respectively weighing aluminum oxide and yttrium oxide according to the stoichiometric ratio of each element in YAG;
s1-2, ball milling: mixing raw material powder by adopting alumina balls;
s1-3, sieving: drying and sieving the mixed powder;
s1-4, tabletting: adopting a dry press to press and shape the sieved powder;
s1-5, vacuum sintering: placing the pressed biscuit into a vacuum sintering furnace, and sintering the biscuit;
s1-6, polishing and cutting: polishing and cutting the upper and lower surfaces of the ceramic;
step two: preparing a Ce-YAG tape casting biscuit;
s2-1, proportioning: y is respectively weighed according to the stoichiometric ratio of each element in Ce-YAG 2 O 3 、Al 2 O 3 、Ce 2 O, add methyl ethylA ketone base, 95% ethanol;
s2-2, ball milling: mixing raw material powder by adopting alumina balls;
s2-3, defoaming: removing bubbles in the ceramic slurry by adopting a vacuum bubble removing mode;
s2-4, molding: pouring the slurry after bubble removal into a trough of a casting machine;
s2-5, lamination and cutting: laminating the biscuit;
step three: preparing a composite fluorescent ceramic device;
s3-1, sintering: and (3) combining the Ce-YAG casting biscuit with the YAG transparent ceramic plate (2) up and down, and putting the combined Ce-YAG casting biscuit and the YAG transparent ceramic plate (2) into a vacuum sintering furnace for sintering to obtain the fluorescent ceramic device based on the combination of the Ce-YAG fluorescent ceramic (1) and the YAG transparent ceramic plate (2).
2. The method for preparing the composite fluorescent ceramic according to claim 1, wherein in S1-2, the ball milling time is 24-48 hours; the ball milling rotating speed is 140-150 r/min.
3. The method for preparing the composite fluorescent ceramic according to claim 1, wherein in S1-3, the drying temperature is 40-65 ℃ and the drying time is 15-20 h; the number of the screening meshes is 100-200 meshes.
4. The method for preparing the composite fluorescent ceramic according to claim 1, wherein in S1-4, the tabletting pressure is 4-20 Mpa, and the pressure is maintained for 2-10 min.
5. The method for preparing the composite fluorescent ceramic according to claim 1, wherein in S1-5, the sintering temperature is 1750-1780 ℃, and the temperature is kept for 12-24 hours.
6. The preparation method of the composite fluorescent ceramic according to claim 1, wherein in S2-1, the mass ratio of methyl ethyl ketone to 95% ethanol is 1.5:1.0-2.0:1.0.
7. The method for preparing the composite fluorescent ceramic according to claim 1, wherein in the step S3-1, the sintering temperature is 1650-1750 ℃, the heat preservation time is 10-12 h, and a weight with the mass of 2.0-3.0 kg is placed above the composite fluorescent ceramic in the sintering process.
8. The method for preparing the composite fluorescent ceramic according to any one of claims 1 to 7, wherein the doping concentration of Ce in the YAG fluorescent ceramic (1) is 0.05 to 0.2at%; the thickness is 0.5-1.0 mm, and the side length is 1.0-2.0 mm; the diameter of the YAG transparent ceramic plate (2) is 16.0-20.0 mm, and the thickness is 0.5-1.0 mm.
9. The method for producing a composite fluorescent ceramic according to any one of claims 1 to 7, wherein the linear transmittance of the YAG transparent ceramic plate (2) at 800nm is 79.0 to 81.0%, and the linear transmittance of a fluorescent ceramic device based on Ce, wherein the composite of the YAG fluorescent ceramic (1) and the YAG transparent ceramic plate (2) at 800nm is 5.0 to 20.0%.
10. The method for preparing composite fluorescent ceramic according to any one of claims 1 to 7, wherein the prepared composite fluorescent ceramic device has a luminous efficiency of 150 to 180lm/W and a brightness of 405 to 1350lm/mm 2 。
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