CN112209714A - Preparation technology of one-step-formed sintered aluminum-based garnet type luminescent ceramic - Google Patents
Preparation technology of one-step-formed sintered aluminum-based garnet type luminescent ceramic Download PDFInfo
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- 239000000919 ceramic Substances 0.000 title claims abstract description 32
- 239000002223 garnet Substances 0.000 title claims abstract description 16
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 title claims abstract description 14
- 229910052782 aluminium Inorganic materials 0.000 title claims abstract description 14
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 238000005516 engineering process Methods 0.000 title claims abstract description 10
- 238000005245 sintering Methods 0.000 claims abstract description 34
- 238000000137 annealing Methods 0.000 claims abstract description 27
- 239000000843 powder Substances 0.000 claims abstract description 24
- 238000007731 hot pressing Methods 0.000 claims abstract description 14
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 12
- 238000001816 cooling Methods 0.000 claims abstract description 9
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 8
- 239000010439 graphite Substances 0.000 claims abstract description 8
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 6
- 238000000498 ball milling Methods 0.000 claims abstract description 6
- 229910052593 corundum Inorganic materials 0.000 claims abstract description 6
- 229910001845 yogo sapphire Inorganic materials 0.000 claims abstract description 6
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 claims abstract description 5
- 238000002156 mixing Methods 0.000 claims abstract description 5
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 4
- 238000005303 weighing Methods 0.000 claims abstract 2
- 238000000034 method Methods 0.000 claims description 9
- 238000004321 preservation Methods 0.000 claims description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- 229910052681 coesite Inorganic materials 0.000 claims description 2
- 229910052906 cristobalite Inorganic materials 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 229910052682 stishovite Inorganic materials 0.000 claims description 2
- 229910052905 tridymite Inorganic materials 0.000 claims description 2
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 claims 1
- 230000001276 controlling effect Effects 0.000 abstract description 4
- 238000004020 luminiscence type Methods 0.000 abstract description 2
- 230000001105 regulatory effect Effects 0.000 abstract description 2
- 238000000465 moulding Methods 0.000 description 5
- 239000013078 crystal Substances 0.000 description 3
- 230000007613 environmental effect Effects 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 238000001228 spectrum Methods 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 238000004134 energy conservation Methods 0.000 description 2
- 230000003287 optical effect Effects 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 238000002834 transmittance Methods 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 238000000975 co-precipitation Methods 0.000 description 1
- 238000000280 densification Methods 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 239000003292 glue Substances 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000008204 material by function Substances 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 238000007569 slipcasting Methods 0.000 description 1
- 238000003746 solid phase reaction Methods 0.000 description 1
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Abstract
The invention discloses a preparation technology of one-step forming sintering aluminum-based garnet type luminescent ceramic, which comprises the following specific steps: respectively weighing Y according to the proportion2O3、Al2O3、CeO2Adding MgO as sintering aid into the powder; ball-milling the powder, adding the powder into a graphite mould after fully mixing, compacting and putting the graphite mould into a vacuum hot-pressing furnace; regulating and controlling the pressurizing pressure, sintering temperature and time of the hot pressing furnace, and setting gradient cooling; twice annealing, once annealing in air, carbon reduction and twice annealing to obtain aluminum-based garnet yellow luminescence with good compactnessA ceramic.
Description
Technical Field
The invention relates to a preparation technology of one-step molding sintering aluminum-based garnet type luminescent ceramic, which can realize one-step molding sintering of aluminum-based garnet type luminescent ceramic by raw materials and belongs to the technical field of photoelectric functional materials.
Background
Under the background of increasingly tense energy sources and prominent environmental problems, all countries in the world develop green energy technology with enhanced energy conservation and high efficiency, and the solid-state lighting light source has the advantages of energy conservation, environmental protection, high potential lighting effect, long service life, small volume and the like, is a green light source with the greatest development potential, and has become a consensus of all countries in the world for vigorously developing the solid-state lighting industry. It is known that the phenomenon of 'efficiency dip' of a high-power LED, which is unrelated to heat dissipation, is that the light extraction efficiency is rapidly attenuated with the increase of the driving power density, and no reasonable solution has been found so far. The Laser Diode (LD) produced in the same era as the LED has not only many advantages of the LED, such as fast response speed, low power consumption, long service life, environmental protection, etc., but also no "efficiency dip" phenomenon in the range of lighting requirements, and high conversion efficiency even when working under high current density, thus ensuring the high efficiency of the lighting source and having more application potential in the field of high-power lighting. The LD has no light decay phenomenon, has obvious advantages compared with the LED, and is possible to replace the LED to become a new solid-state light source in the future. Although laser lighting has many advantages, the related technology is not mature, and the current AB glue coated fluorescent powder is difficult to meet the requirement of high-power laser lighting.
Luminescent ceramics not only have the excellent performance of traditional ceramics, but also have better optical performance, thereby being widely researched. The garnet structure has an isotropic cubic crystal structure and has excellent mechanical, thermal and mechanical properties, so that the garnet structure is idealA luminescent ceramic material matrix. In 2000, Zych et al used a hot pressing method at 1700 ℃ C. and 3.4X 107The first Ce is successfully prepared by hot pressing for 10h under Pa pressure3+Ion-doped YAG fluorescent ceramic. In 2005, Yanagida et al reported that Ce was doped by vacuum sintering3+YAG transparent ceramics with mole fractions of 0.005%, 0.05% and 0.5%, respectively. Ce is synthesized from YAG by using hydroxide coprecipitation method in 2009 by S.Nishiura et al3+Powder, ball milling and slip casting the powder, and then placing the powder in a container2Keeping the temperature at 800 ℃ for 100h under the atmosphere to remove organic impurities. Finally, the sample is calcined for 20 hours at 1780 ℃ in vacuum to obtain YAG Ce with the transmittance reaching 70-87% at 800nm3+A transparent ceramic. 2016, Song dynasty and the like adopt a solid-phase reaction method combined with a vacuum sintering technology to prepare different Ce3+Doping concentration of YAG to Ce3+The result of the transparent ceramic shows that the prepared transparent ceramic sample has excellent optical quality and can replace YAG to Ce3+A novel fluorescent material of fluorescent powder. At present, no relevant technology for preparing the garnet-based luminescent ceramic by one-step molding and sintering is available.
Disclosure of Invention
The invention aims to develop a preparation technology for one-step molding sintering of aluminum-based garnet luminescent ceramic, and realize one-step molding sintering preparation of the aluminum-based garnet luminescent ceramic from raw materials. The technique uses Al2O3、Y2O3、CeO2The powder is used as a raw material, a sintering aid is added, the powder is placed into a mold after being ball-milled and mixed uniformly, the generation of ceramic grains and the formation of crystal boundaries are promoted by adjusting the sintering temperature, the heat preservation time, the pressurization size and the like of a vacuum hot-pressing furnace, the densification of the ceramic is realized, and meanwhile, the transmittance of the ceramic can be regulated and controlled. By setting the annealing temperature and the annealing times, the oxygen vacancy is reduced, and the Ce is reduced4+And ions are added to improve the luminous intensity of the LD device.
The general formula of the one-time forming sintering aluminum-based garnet type luminescent ceramic is Y2.94Al5O12:0.06Ce3+The sintering aid is used for assisting the generation, and the types of the sintering aid are MgO and SiO2、B2O3TEOS, etc., sintering aidThe content of the agent is as follows: 0.5 wt% -4.0 wt%, and the reaction temperature is as follows: 1625-1750 ℃, and the reaction time is as follows: 3-6 h, the annealing temperature is 1250-1550 ℃, and the return time is as follows: : 3-10 h.
Drawings
Figure 1 is an XRD pattern of samples at different sintering temperatures.
FIG. 2 is an SEM image of the ceramic at a sintering temperature of 1725 ℃.
Figure 3 is an XRD pattern of samples at different annealing temperatures.
FIG. 4 is a graph of luminescence spectra of samples prepared with different annealing times.
FIG. 5 is a CIE spectrum of samples prepared at different sintering temperatures.
Detailed Description
The specific process of the sample in the invention is described in detail as follows:
1. first according to Y2.94Al5O12:0.06Ce3+Chemical formula, adopting a precise electronic balance to respectively weigh Y according to the proportion2O3、Al2O3、CeO2Adding MgO and SiO into the powder2、B2O3TEOS powder is used as a sintering aid;
2. ball-milling the powder, adding the powder into a graphite mould after fully mixing, compacting and putting the graphite mould into a vacuum hot-pressing furnace;
3. adjusting and controlling the sintering temperature and time of the hot pressing furnace, raising the temperature from room temperature to 1625-1750 ℃ in a gradient manner, and preserving the temperature for 3-5 h; and finally, gradient cooling is set.
4. And annealing the taken sample for 1-2 times, annealing in primary air at 1250-1550 ℃, and keeping the temperature for 10 hours, wherein the secondary annealing is a double-crucible carbon reducing atmosphere, and the temperature is raised to 1250 ℃, and the temperature is kept for 4 hours.
Example one:
1. according to Y2.94Al5O12:0.06Ce3+Chemical formula, adopting a precise electronic balance to respectively weigh Y according to the proportion2O3、Al2O3、CeO2Adding MgO powder as sintering aid into the powder;
2. ball-milling the powder for 30min, fully mixing, adding into a graphite mold, compacting, and putting into a vacuum hot-pressing furnace;
3. and adjusting and controlling the sintering temperature and time of the hot pressing furnace, carrying out gradient temperature rise from room temperature to 1625-1750 ℃, carrying out heat preservation for 3h, finally, carrying out gradient temperature reduction, cooling to 1200 ℃ at the speed of 5 ℃/min, and carrying out furnace cooling.
4. And annealing the taken out sample for 1 time, annealing in air at 1250-1550 ℃, preserving heat for 10 hours, and cooling along with the furnace to obtain the sample.
XRD diffraction patterns of samples prepared at different sintering temperatures are shown in figure 1, and garnet type luminescent ceramics are synthesized.
FIG. 2 is an SEM image of the microstructure of the ceramic at a sintering temperature of 1725 ℃. The ceramic has uniform granularity, clear crystal boundary and good compactness.
XRD of samples prepared under the conditions that the sintering temperature is 1725 ℃ and the annealing temperatures are different is shown in figure 3, the samples are garnet type luminescent ceramics, and the diffraction peaks of phases are sharp, the intensity is high, and the crystallinity is good.
Example two:
1. according to Y2.94Al5O12:0.06Ce3+Chemical formula, adopting a precise electronic balance to respectively weigh Y according to the proportion2O3、Al2O3、CeO4Adding MgO powder as sintering aid into the powder;
2. ball-milling the powder for 30min, fully mixing, adding into a graphite mold, compacting, and putting into a vacuum hot-pressing furnace;
3. and adjusting and controlling the sintering temperature and time of the hot pressing furnace, carrying out gradient temperature rise from room temperature to 1625-1750 ℃, carrying out heat preservation for 3h, finally, carrying out gradient temperature reduction, cooling to 1200 ℃ at the speed of 5 ℃/min, and carrying out furnace cooling.
4. And annealing the taken sample for 2 times, annealing in primary air at 1450 ℃ for 10h, and performing secondary annealing in a double-crucible carbon reduction atmosphere, heating to 1250 ℃, and performing heat preservation for 4 h. Annealing in air, and cooling along with the furnace to obtain a sample.
FIG. 4 is a graph showing the spectrum of a ceramic at 1725 deg.C after annealing for different times, from which it can be seen that the emission intensity of the sample after the second annealing is greater than that of the sample after the first annealing.
FIG. 5 is a CIE coordinate diagram of samples prepared after annealing at different sintering temperatures. The figures show that the samples all emit yellow light.
Claims (5)
1. A preparation technology of one-step forming sintering aluminum-based garnet type luminescent ceramic is characterized in that: comprises the following steps:
A. respectively weighing Y according to the proportion2O3、Al2O3、CeO2Adding sintering aid into the powder;
B. ball-milling the powder, adding the powder into a graphite mould after fully mixing, compacting and putting the graphite mould into a vacuum hot-pressing furnace;
C. adjusting and controlling the sintering temperature and time of the hot pressing furnace, and setting gradient temperature rise and temperature reduction;
D. and annealing twice, annealing once in the air, and annealing twice in a reducing atmosphere to obtain the garnet yellow luminescent ceramic with good compactness.
2. The preparation technique of the one-shot-formed sintered aluminum-based garnet-type luminescent ceramic according to claim 1, characterized in that: the sintering aid in A is MgO and SiO2、B2O3And TEOS powder.
3. The preparation technique of the one-shot-formed sintered aluminum-based garnet-type luminescent ceramic according to claim 1, characterized in that: the ultimate vacuum degree of the vacuum hot pressing furnace in the B is less than or equal to 8 multiplied by 10-4Pa。
4. The preparation technique of the one-shot-formed sintered aluminum-based garnet-type luminescent ceramic according to claim 1, characterized in that: and the sintering condition in the step C is that the temperature is increased to 1000 ℃ at the speed of 10 ℃/min, the temperature is increased to 1625-1750 ℃ at the speed of 6 ℃/min, the temperature is kept for 3-5 h, the temperature is reduced to 1200 ℃ at the speed of 5 ℃/min, and then the furnace cooling is carried out.
5. The preparation technique of the one-shot-formed sintered aluminum-based garnet-type luminescent ceramic according to claim 1, characterized in that: and D, performing primary annealing at 1250-1550 ℃ for 10h, and performing secondary annealing in a double-crucible carbon reduction atmosphere, heating to 1250 ℃, and performing heat preservation for 4 h.
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