CN114181702B - Preparation method of cerium-doped yttrium aluminum garnet fluorescent powder - Google Patents
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- 239000000843 powder Substances 0.000 title claims abstract description 22
- 229910019990 cerium-doped yttrium aluminum garnet Inorganic materials 0.000 title claims abstract description 18
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 239000002243 precursor Substances 0.000 claims abstract description 40
- 238000010304 firing Methods 0.000 claims abstract description 20
- 238000000034 method Methods 0.000 claims abstract description 13
- 238000001035 drying Methods 0.000 claims abstract description 11
- 239000004094 surface-active agent Substances 0.000 claims abstract description 11
- 238000000498 ball milling Methods 0.000 claims abstract description 8
- 238000005406 washing Methods 0.000 claims abstract description 8
- 239000000243 solution Substances 0.000 claims description 32
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 19
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 19
- 239000004202 carbamide Substances 0.000 claims description 19
- 239000012266 salt solution Substances 0.000 claims description 15
- 238000004448 titration Methods 0.000 claims description 13
- 239000002270 dispersing agent Substances 0.000 claims description 12
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 12
- 239000002244 precipitate Substances 0.000 claims description 11
- 239000008367 deionised water Substances 0.000 claims description 10
- 229910021641 deionized water Inorganic materials 0.000 claims description 10
- 235000019441 ethanol Nutrition 0.000 claims description 10
- 238000001914 filtration Methods 0.000 claims description 10
- 239000000047 product Substances 0.000 claims description 9
- 230000032683 aging Effects 0.000 claims description 8
- IDGUHHHQCWSQLU-UHFFFAOYSA-N ethanol;hydrate Chemical compound O.CCO IDGUHHHQCWSQLU-UHFFFAOYSA-N 0.000 claims description 7
- 239000012046 mixed solvent Substances 0.000 claims description 7
- 150000000703 Cerium Chemical class 0.000 claims description 6
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical class [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 claims description 6
- JNDMLEXHDPKVFC-UHFFFAOYSA-N aluminum;oxygen(2-);yttrium(3+) Chemical compound [O-2].[O-2].[O-2].[Al+3].[Y+3] JNDMLEXHDPKVFC-UHFFFAOYSA-N 0.000 claims description 6
- 150000002500 ions Chemical class 0.000 claims description 6
- 150000003746 yttrium Chemical class 0.000 claims description 6
- 229910019901 yttrium aluminum garnet Inorganic materials 0.000 claims description 6
- 229910052845 zircon Inorganic materials 0.000 claims description 6
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 claims description 6
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 claims description 5
- 239000011259 mixed solution Substances 0.000 claims description 5
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 5
- 239000012716 precipitator Substances 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- 150000004677 hydrates Chemical class 0.000 claims description 4
- 238000000643 oven drying Methods 0.000 claims description 4
- 229950008882 polysorbate Drugs 0.000 claims description 4
- 229920000136 polysorbate Polymers 0.000 claims description 4
- 238000001132 ultrasonic dispersion Methods 0.000 claims description 3
- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical group [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 claims description 2
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 2
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 2
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 2
- 238000000926 separation method Methods 0.000 claims description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims 2
- 230000002776 aggregation Effects 0.000 abstract description 9
- 238000005054 agglomeration Methods 0.000 abstract description 8
- 238000001556 precipitation Methods 0.000 abstract description 4
- AOBXGGAGUYYNQH-UHFFFAOYSA-N ammonium sulfate urea Chemical compound [NH4+].[NH4+].NC(N)=O.[O-]S([O-])(=O)=O AOBXGGAGUYYNQH-UHFFFAOYSA-N 0.000 abstract 1
- 239000002245 particle Substances 0.000 description 25
- 229910019655 synthetic inorganic crystalline material Inorganic materials 0.000 description 13
- 230000000052 comparative effect Effects 0.000 description 7
- ATRRKUHOCOJYRX-UHFFFAOYSA-N Ammonium bicarbonate Chemical compound [NH4+].OC([O-])=O ATRRKUHOCOJYRX-UHFFFAOYSA-N 0.000 description 6
- 229910000013 Ammonium bicarbonate Inorganic materials 0.000 description 6
- 235000012538 ammonium bicarbonate Nutrition 0.000 description 6
- 239000001099 ammonium carbonate Substances 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 238000005507 spraying Methods 0.000 description 4
- 239000002202 Polyethylene glycol Substances 0.000 description 3
- 238000001027 hydrothermal synthesis Methods 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 239000000203 mixture Substances 0.000 description 3
- 229920001223 polyethylene glycol Polymers 0.000 description 3
- 238000000975 co-precipitation Methods 0.000 description 2
- 238000009776 industrial production Methods 0.000 description 2
- 238000004729 solvothermal method Methods 0.000 description 2
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 1
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 235000011114 ammonium hydroxide Nutrition 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000008204 material by function Substances 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 244000005700 microbiome Species 0.000 description 1
- 239000011241 protective layer Substances 0.000 description 1
- 238000004062 sedimentation Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7766—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
- C09K11/7774—Aluminates
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
- Y02B20/00—Energy efficient lighting technologies, e.g. halogen lamps or gas discharge lamps
Abstract
The invention relates to a preparation method of cerium-doped yttrium aluminum garnet fluorescent powderThe preparation method comprises the following steps: YAG-Ce prepared by urea-ammonium sulfate homogeneous precipitation method 3+ And (3) separating and washing the precursor, drying, firing, ball-milling and drying after the treatment of the surfactant to obtain the cerium-doped yttrium aluminum garnet fluorescent powder. The invention obtains the light-emitting (Y) which is high-efficiency, spherical, highly dispersed and free from agglomeration 1‑X Ce X ） 3 Al 5 O 12 And (3) powder.
Description
Technical Field
The invention belongs to the technical field of functional materials, and particularly relates to a preparation method of cerium-doped yttrium aluminum garnet fluorescent powder.
Background
The (Y1-xCex) 3Al5O12 is taken as an important luminous matrix material of the current LED, and can be combined with a blue LED to obtain a white LED, and the powder has a huge market prospect due to special fluorescent property.
The preparation method of the cerium-doped yttrium aluminum garnet fluorescent powder described in the prior art has the following defects:
(1) Ammonium bicarbonate is used as a precipitator, a non-uniform precipitation system is not easy to control, and the precipitated particles have uneven particle size and larger particle size;
(2) The system is used in a closed hydrothermal reaction kettle, and the precursor is dispersed in alcohol to carry out solvothermal reaction, so that a great potential safety hazard exists under the conditions of high temperature and high pressure;
(3) The ammonia water direct precipitation method is relatively simple to operate, but anions in the original solution are not easy to wash out, and the obtained particles have wider particle size distribution;
(4) The performance is not well controlled, and the method is not suitable for process production.
Chinese patent 201710903703.9 discloses a preparation method of cerium-doped yttrium aluminum garnet spherical fluorescent powder, which uses ammonium bicarbonate as precipitant to prepare YAG Ce by coprecipitation 3+ Or YAG precursor, and then performing solvothermal reaction in a reaction kettle by using ethylenediamine or ethylenediamine-alcohol solution as a solvent, wherein ammonium bicarbonate is used as a precipitant to form a non-uniform precipitation system, the non-uniform and larger particle size of the precipitated particles is difficult to control, and the precursor is dispersed in alcohol in a closed hydrothermal reaction kettle in the system, so that the potential safety hazard is large under the conditions of high temperature and high pressure.
A preparation method of cerium-doped yttrium aluminum garnet fluorescent powder is disclosed in Chinese patent 20110070153. X, and YAG is prepared from Ce by a microorganism-coprecipitation method 3+ The method involves microorganism operation, the condition is not easy to control compared with a chemical method, the method is not economical and is not easy to realize industrial production, and the obtained fluorescent split has agglomeration phenomenon.
According to the method for preparing the nano-scale spherical yttrium aluminum garnet powder disclosed in Chinese patent 200710118421.4, the precursor is subjected to subsequent high-temperature roasting treatment to enable YAG powder with small size to be rapidly aggregated and agglomerated, so that the particle size is increased, and the dispersibility is poor.
Disclosure of Invention
The invention aims to provide a preparation method of cerium-doped yttrium aluminum garnet fluorescent powder, which can obtain the light-emitting (Y) with high efficiency, spherical shape, high dispersion and no agglomeration 1-X Ce X ） 3 Al 5 O 12 And (3) powder.
Description of the terminology: YAG, ce is (Y1-xCex) 3Al5O12, and is named as cerium-doped yttrium aluminum garnet.
The invention solves the problems by adopting the following technical scheme: the preparation method of the cerium-doped yttrium aluminum garnet fluorescent powder comprises the following steps:
(1) Preparing a precursor reaction solution
S1 according to the formula (Y) 1-X Ce X ） 3 Al 5 O 12 Weighing yttrium salt, cerium salt and aluminum salt according to a metering ratio of 0 < x < 0.1, dissolving the yttrium salt, cerium salt and aluminum salt in deionized water, and preparing a mixed mother salt solution with ion molar concentration of 0.05-0.8 mol/L;
s2, the (NH) 4 ) 2 SO 4 Dissolving in ethanol-water mixed solvent, and preparing (NH) 4 ) 2 SO 4 A dispersant solution having a molar concentration of 0.0005 to 0.001 mol/L;
s3, dissolving urea in the dispersant solution prepared in the step S2 to prepare a precipitant solution with the molar concentration of urea of 0.02-1 mol/L;
(2) Titration and aging
In terms of molar amount of urea with Y 3+ 、Ce 3+ And Al 3+ Measuring the precipitant solution and the mixed mother salt solution prepared in the step (1) according to the total molar ratio of 10-20:1, gradually titrating the mixed mother salt solution into the precipitant solution at the normal pressure and the temperature of 80-95 ℃, continuously stirring during titration, and aging for 16-24 hours after titration is finished;
（3）YAG:Ce 3+ precursor separation and washing
Vacuum filtering, washing and vacuum filtering the aged mixed solution to obtain white precipitate YAG: ce 3+ The precursor, the obtained white precipitate is washed by deionized water and absolute ethyl alcohol in sequence;
（4）YAG:Ce 3+ drying of precursors
Washed YAG-Ce 3+ The precursor is treated by a surfactant, and is dried at 100 ℃ after ultrasonic dispersion to obtain the dried YAG-Ce 3+ A precursor;
(5) Firing of precursors
Firing the precursor obtained in the step (4) for 3-6 hours to obtain a firing product, wherein the firing temperature is 900-1000 ℃;
(6) Ball milling and drying
Spraying alcohol on the obtained burnt product, and ball-milling with zirconDrying to obtain target (Y) 1-X Ce X ） 3 Al 5 O 12 And (3) powder.
Preferably, the zircon diameter in step (6) is less than or equal to 2mm.
Preferably, the yttrium salt is Y (NO 3 ) 3 、Y(CH 3 COO) 3 Or YCl 3 Or their hydrates, the aluminum salts being AlCl 3 、Al 2 (SO 4 ) 3 、Al(NO 3 ) 3 Or NH4Al (SO 4) 2 or their hydrates, the cerium salt being Ce (NO) 3 ) 3 Or a hydrate thereof.
Preferably, the surfactant is sodium dodecyl sulfate, polyvinyl alcohol, polyethylene glycol or polyvinylpyrrolidone.
Preferably, the surfactant is combined with YAG: ce 3+ The molar ratio of the precursors is 0.01-0.2:1.
Preferably, in the ethanol-water mixed solvent in the step (1), the volume ratio of ethanol to water is 0.2:1-0.5:1.
Compared with the prior art, the invention has the advantages that:
(1) With the rise of temperature, urea is dissolved to be an equilibrium uniform system, and is hydrolyzed to generate precipitator NH at a certain temperature 4 OH，NH 4 The structure crystal ion OH < - > which is slowly and uniformly electrolyzed from OH is uniformly distributed in the solution, the precipitate can be uniformly generated, and the dispersity of the reaction process is easy to control.
(2) In the titration aging reaction process, (NH) is added into the system 4 ) 2 SO 4 The bonding effect of OH < - > on the surface of the precursor can be reduced, colloidal particles are dispersed to prevent agglomeration, and the colloidal particles and urea act together to control the morphology and size of the particles;
(3) The precursor is treated by a surfactant before drying and firing, and the surfactant volatilizes under the drying and firing to avoid chemical bonds between particles, thereby forming spherical and non-agglomerated YAG: ce 3+ Nano/micron-sized powder;
(4) The precursor is prevented from being dispersed in alcohol of the closed hydrothermal reaction kettle, so that the method is safer and easy for industrial production;
(5) The addition of polysorbate to the precipitant reduces the surface tension of the particles, and the precursor can form a protective layer on the surface of the colloidal particles to play a role in steric hindrance after adsorbing the polysorbate, thereby preventing agglomeration.
Detailed Description
The present invention is described in further detail below with reference to examples.
Example 1:
according to chemical formula Y 2.94 Ce 0.06 Al 5 O 12 0.00735mol of Y (NO) 3 ) 3 0.00015mol of Ce (NO) 3 ) 3 And 0.0125molAlCl 3 Dissolving the mixture in 100ml of deionized water to prepare a mixed mother salt solution with the ion molar concentration of 0.2 mol/L; 0.0005mol (NH) 4 ) 2 SO 4 Dissolving in 500ml ethanol-water mixed solvent with volume ratio of 0.2:1, and preparing (NH) 4 ) 2 SO 4 A dispersant solution with a molar concentration of 0.001mol/L, and 0.025mol of urea is dissolved in the prepared dispersant solution to prepare a precipitator solution with a molar concentration of 0.5mol/L of urea;
in terms of molar amount of urea with Y 3+ 、Ce 3+ And Al 3+ Measuring the prepared precipitant solution and mixed mother salt solution at the total molar ratio of 10:1, gradually titrating the mixed mother salt solution into the precipitant solution at normal pressure and 85 ℃, continuously stirring during titration, and aging for 20 hours after the titration is finished; vacuum filtering, washing and vacuum filtering the aged mixed solution to obtain white precipitate YAG: ce 3+ The precursor, the obtained white precipitate is washed by deionized water and absolute ethyl alcohol in sequence;
washed YAG-Ce 3+ Mixing the precursor surface with polyvinyl alcohol, dispersing with ultrasonic wave, drying at 100deg.C to obtain 0.21g dried YAG: ce 3+ A precursor; firing the dried precursor at 900 ℃ for 6 hours to obtain a firing product; spraying alcohol on the obtained burnt product, ball milling with zircon, and oven drying to obtain high-efficiency luminous, spherical, highly dispersed, non-agglomerated and granuleWith a diameter of 800nm (Y 1-X Ce X ） 3 Al 5 O 12 And (3) powder.
Example 2:
according to chemical formula Y 2.95 Ce 0.05 Al 5 O 12 0.00295mol of Y (NO) 3 ) 3 0.00005mol of Ce (NO) 3 ) 3 And 0.005mol Al (NO) 3 ) 3 Dissolving the mixture in 100ml of deionized water to prepare a mixed mother salt solution with the ion molar concentration of 0.08 mol/L; 0.0004mol (NH) 4 ) 2 SO 4 Dissolving in 500ml ethanol-water mixed solvent with volume ratio of 0.2:1, and preparing (NH) 4 ) 2 SO 4 Dispersing agent solution with the molar concentration of 0.0008mol/L, dissolving 0.02mol of urea in the prepared dispersing agent solution, and preparing precipitant solution with the molar concentration of urea of 0.4 mol/L;
in terms of molar amount of urea with Y 3+ 、Ce 3+ And Al 3+ Measuring the prepared precipitant solution and mixed mother salt solution at the total molar ratio of 15:1, gradually titrating the mixed mother salt solution into the precipitant solution at normal pressure and 85 ℃, continuously stirring during titration, and aging for 20 hours after the titration is finished; vacuum filtering, washing and vacuum filtering the aged mixed solution to obtain white precipitate YAG: ce 3+ The precursor, the obtained white precipitate is washed by deionized water and absolute ethyl alcohol in sequence;
washed YAG-Ce 3+ Mixing the surface of the precursor with polyvinyl alcohol, performing ultrasonic dispersion, and drying at 100 ℃ to obtain 0.19g of dried YAG:Ce3+ precursor; firing the dried precursor at 900 ℃ for 6 hours to obtain a firing product; spraying alcohol on the obtained burnt product, ball milling with zircon, and oven drying to obtain high-efficiency luminous (Y) with spherical, highly dispersed, non-agglomerated and particle size of 600nm 1-X Ce X ） 3 Al 5 O 12 And (3) powder.
Example 3:
according to chemical formula Y 2.95 Ce 0.05 Al 5 O 12 0.0018mol of stoichiometric proportion of (A) to (B)Y(NO 3 ) 3 0.000032mol of Ce (NO) 3 ) 3 And 0.0032mol Al (NO) 3 ) 3 Dissolving the mixture in 100ml of deionized water to prepare a mixed mother salt solution with the ion molar concentration of 0.05 mol/L; 0.0005mol (NH) 4 ) 2 SO 4 Dissolving in 500ml ethanol-water mixed solvent with volume ratio of 0.2:1, and preparing (NH) 4 ) 2 SO 4 A dispersant solution with a molar concentration of 0.001mol/L, and 0.025mol of urea is dissolved in the prepared dispersant solution to prepare a precipitator solution with a molar concentration of 0.05mol/L of urea;
in terms of molar amount of urea with Y 3+ 、Ce 3+ And Al 3+ Measuring the prepared precipitant solution and mixed mother salt solution at the total molar ratio of 20:1, gradually titrating the mixed mother salt solution into the precipitant solution at normal pressure and 85 ℃, continuously stirring during titration, and aging for 20 hours after the titration is finished; vacuum filtering, washing and vacuum filtering the aged mixed solution to obtain white precipitate YAG: ce 3+ The precursor, the obtained white precipitate is washed by deionized water and absolute ethyl alcohol in sequence;
washed YAG-Ce 3+ Mixing the precursor surface with polyvinyl alcohol, dispersing with ultrasonic wave, drying at 100deg.C to obtain 0.22g dried YAG: ce 3+ A precursor; firing the dried precursor for 4 hours at 950 ℃ to obtain a firing product; spraying alcohol on the obtained burnt product, ball milling with zircon, and oven drying to obtain high-efficiency luminous (Y) with spherical, highly dispersed, non-agglomerated and particle size of 500nm 1-X Ce X ） 3 Al 5 O 12 And (3) powder.
Comparative example 1:
the production process was substantially the same as in example 1, except that the precipitant was 1.5mol/L ammonium bicarbonate.
Comparative example 2:
the production process is essentially the same as in example 3, except that No (NH) 4 ) 2 SO 4 A dispersing agent.
Comparative example 3:
the production process was substantially the same as in example 3, except that polyethylene glycol was added to the precipitant.
Comparative example 4:
the production process was substantially the same as in example 3, except that the surfactant treatment was not performed at the time of firing.
As can be seen from the above table, according to the comparison of examples 1 to 3, the molar amount of urea is as follows with Y 3+ 、Ce 3+ And Al 3+ The larger the ratio of the total molar quantity of the three components is, the smaller the formed particle size is; as can be seen from examples and comparative example 1, the precipitant is ammonium bicarbonate with non-uniform and large particle size, and urea with uniform and small particle size; as is clear from the comparison of example 3 with comparative examples 1 and 2, no (NH) was added to the precipitant 4 ) 2 SO 4 Dispersing agent or adding (NH) into ammonium bicarbonate precipitant 4 ) 2 SO 4 Hard agglomeration of particles cannot be avoided; as is clear from examples 3 and 4, the absence of surfactant treatment during firing resulted in aggregation and agglomeration of particles, increased particle size and rough particle surface; as is clear from examples 3 and comparative examples 2 and 3, the addition of polyethylene glycol to the precipitant reduced agglomeration during sedimentation but also changed the particle shape, making the particles olive-shaped, and was not practical.
In addition to the above embodiments, the present invention also includes other embodiments, and all technical solutions that are formed by equivalent transformation or equivalent substitution should fall within the protection scope of the claims of the present invention.
Claims (4)
1. The preparation method of the cerium-doped yttrium aluminum garnet fluorescent powder is characterized by comprising the following steps of:
(1) Preparing a precursor reaction solution
S1 according to the formula (Y) 1-X Ce X ） 3 Al 5 O 12 、0＜xWeighing yttrium salt, cerium salt and aluminum salt according to a metering ratio of less than or equal to 0.1, dissolving the yttrium salt, cerium salt and aluminum salt in deionized water, and preparing a mixed mother salt solution with the ion molar concentration of 0.05-0.8 mol/L;
s2, the (NH) 4 ) 2 SO 4 Dissolving in ethanol-water mixed solvent, and preparing (NH) 4 ) 2 SO 4 Dispersing agent solution with the molar concentration of 0.0005-0.001 mol/L, wherein the volume ratio of ethanol to water in the ethanol-water mixed solvent is 0.2:1-0.5:1;
s3, dissolving urea in the dispersant solution prepared in the step S2, and preparing a precipitator solution with the urea molar concentration of 0.02-1 mol/L;
(2) Titration and aging
In terms of molar amount of urea with Y 3+ 、Ce 3+ And Al 3+ Measuring the precipitant solution and the mixed mother salt solution prepared in the step (1) according to the total molar ratio of 10-20:1, gradually titrating the mixed mother salt solution into the precipitant solution at the normal pressure and the temperature of 80-95 ℃, continuously stirring during titration, and aging for 16-24 hours after titration is finished;
（3）YAG:Ce 3+ precursor separation and washing
Vacuum filtering, washing and vacuum filtering the aged mixed solution to obtain white precipitate YAG: ce 3+ The precursor, the obtained white precipitate is washed by deionized water and absolute ethyl alcohol in sequence;
(4) Drying treatment of YAG (yttrium aluminum garnet) Ce < 3+ > precursor
Washed YAG-Ce 3+ The precursor is treated by a surfactant, and is dried at 100 ℃ after ultrasonic dispersion to obtain the dried YAG-Ce 3+ A precursor; the surfactant is mixed with YAG, ce 3+ The mol ratio of the precursors is 0.01-0.2:1; the surfactant is sodium dodecyl sulfate, polyvinyl alcohol or polyvinylpyrrolidone;
(5) Firing of precursors
Firing the precursor obtained in the step (4) for 3-6 hours to obtain a firing product, wherein the firing temperature is 900-1000 ℃;
(6) Ball milling and drying
The obtained firing productSpraying alcohol, ball milling with zircon, and oven drying to obtain target (Y) 1-X Ce X ） 3 Al 5 O 12 And (3) powder.
2. The method for preparing cerium-doped yttrium aluminum garnet fluorescent powder according to claim 1, wherein the diameter of zircon in the step (6) is less than or equal to 2mm.
3. The method for preparing cerium-doped yttrium aluminum garnet phosphor according to claim 1, wherein the yttrium salt is Y (NO 3 ) 3 、Y(CH 3 COO) 3 Or YCl 3 Or their hydrates, the aluminum salts being AlCl 3 、Al 2 (SO 4 ) 3 、Al(NO 3)3 Or NH 4 Al(SO 4 ) 2 Or their hydrates, the cerium salt being Ce (NO 3 ) 3 Or a hydrate thereof.
4. The method of preparing cerium-doped yttrium aluminum garnet phosphor according to claim 1, wherein the precipitant solution in step (1) further comprises polysorbate, polysorbate and YAG: ce 3+ The molar ratio of the precursors is 0.01-0.2:1.
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| CN1907860A (en) * | 2006-08-16 | 2007-02-07 | 四川大学 | Alcohol-water compounded solvents coprecipitation method of preparing yttrium aluminium garnet nano-powder |
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