CN114181702A - Preparation method of cerium-doped yttrium aluminum garnet fluorescent powder - Google Patents
Preparation method of cerium-doped yttrium aluminum garnet fluorescent powder Download PDFInfo
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- 239000000843 powder Substances 0.000 title claims abstract description 24
- 229910019990 cerium-doped yttrium aluminum garnet Inorganic materials 0.000 title claims abstract description 16
- 238000002360 preparation method Methods 0.000 title abstract description 6
- 239000002243 precursor Substances 0.000 claims abstract description 39
- 238000000034 method Methods 0.000 claims abstract description 23
- 238000010304 firing Methods 0.000 claims abstract description 14
- 238000005406 washing Methods 0.000 claims abstract description 13
- 239000004094 surface-active agent Substances 0.000 claims abstract description 10
- 238000001035 drying Methods 0.000 claims abstract description 9
- 238000000498 ball milling Methods 0.000 claims abstract description 8
- 239000000243 solution Substances 0.000 claims description 29
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 25
- 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 21
- 229910019901 yttrium aluminum garnet Inorganic materials 0.000 claims description 21
- 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 18
- 239000002244 precipitate Substances 0.000 claims description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 14
- 238000004448 titration Methods 0.000 claims description 13
- 235000019441 ethanol Nutrition 0.000 claims description 12
- 239000012716 precipitator 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
- 238000001914 filtration Methods 0.000 claims description 10
- 239000000047 product Substances 0.000 claims description 10
- 239000002270 dispersing agent Substances 0.000 claims description 9
- 230000032683 aging Effects 0.000 claims description 8
- 239000012046 mixed solvent Substances 0.000 claims description 7
- 229910052845 zircon Inorganic materials 0.000 claims description 7
- GFQYVLUOOAAOGM-UHFFFAOYSA-N zirconium(iv) silicate Chemical compound [Zr+4].[O-][Si]([O-])([O-])[O-] GFQYVLUOOAAOGM-UHFFFAOYSA-N 0.000 claims description 7
- 150000000703 Cerium Chemical class 0.000 claims description 6
- 238000006243 chemical reaction Methods 0.000 claims description 6
- 238000005303 weighing Methods 0.000 claims description 6
- 150000003746 yttrium Chemical class 0.000 claims description 6
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 5
- VSCWAEJMTAWNJL-UHFFFAOYSA-K aluminium trichloride Chemical group Cl[Al](Cl)Cl VSCWAEJMTAWNJL-UHFFFAOYSA-K 0.000 claims description 5
- IDGUHHHQCWSQLU-UHFFFAOYSA-N ethanol;hydrate Chemical compound O.CCO IDGUHHHQCWSQLU-UHFFFAOYSA-N 0.000 claims description 5
- 239000011259 mixed solution Substances 0.000 claims description 5
- 238000000643 oven drying Methods 0.000 claims description 5
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 5
- 238000005507 spraying Methods 0.000 claims description 5
- 238000003756 stirring Methods 0.000 claims description 5
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical class [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 claims description 4
- 229910000329 aluminium sulfate Inorganic materials 0.000 claims description 4
- 229950008882 polysorbate Drugs 0.000 claims description 4
- 229920000136 polysorbate Polymers 0.000 claims description 4
- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical group [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 claims description 2
- 229910009523 YCl3 Inorganic materials 0.000 claims description 2
- JLDSOYXADOWAKB-UHFFFAOYSA-N aluminium nitrate Inorganic materials [Al+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O JLDSOYXADOWAKB-UHFFFAOYSA-N 0.000 claims description 2
- 159000000013 aluminium salts Chemical class 0.000 claims description 2
- DIZPMCHEQGEION-UHFFFAOYSA-H aluminium sulfate (anhydrous) Chemical compound [Al+3].[Al+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O DIZPMCHEQGEION-UHFFFAOYSA-H 0.000 claims description 2
- 150000004677 hydrates Chemical class 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
- 238000002604 ultrasonography Methods 0.000 claims description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims 2
- 230000001376 precipitating effect Effects 0.000 claims 1
- 238000005054 agglomeration Methods 0.000 abstract description 9
- 238000001556 precipitation Methods 0.000 abstract description 4
- 238000004020 luminiscence type Methods 0.000 abstract description 2
- 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 27
- 230000002776 aggregation Effects 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 8
- 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
- 150000002500 ions Chemical class 0.000 description 4
- 239000002202 Polyethylene glycol Substances 0.000 description 3
- 238000001027 hydrothermal synthesis Methods 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 229920001223 polyethylene glycol Polymers 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- 238000000975 co-precipitation Methods 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 238000009776 industrial production Methods 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 239000000126 substance Substances 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
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 230000007547 defect Effects 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
- 230000000813 microbial effect Effects 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000011241 protective layer Substances 0.000 description 1
- 238000004062 sedimentation Methods 0.000 description 1
- 235000019333 sodium laurylsulphate Nutrition 0.000 description 1
- 238000004729 solvothermal method Methods 0.000 description 1
- 230000009466 transformation Effects 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 method for preparing cerium-doped yttrium aluminum garnet fluorescent powder, which comprises the following steps: preparation of YAG Ce by urea-ammonium sulfate homogeneous precipitation method3+Separating and washing the precursor, treating the precursor by a surfactant, drying, firing, ball milling and drying to obtain the cerium-doped yttrium aluminum garnet fluorescent powder. The invention obtains (Y) which has high-efficiency luminescence, is spherical and highly dispersed without agglomeration1‑XCeX）3Al5O12And (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
(Y1-xCex)3Al5O12 is used as an important luminescent 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 the special fluorescent property.
The preparation method of cerium-doped yttrium aluminum garnet fluorescent powder recorded 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 non-uniform and larger particle size;
(2) a closed hydrothermal reaction kettle is used in the system, the precursor is dispersed in alcohol for solvothermal reaction, and great potential safety hazard exists under the conditions of high temperature and high pressure;
(3) the ammonia direct precipitation method is relatively simple to operate, but anions in the original solution are not easy to wash out, and the particle size distribution of the obtained particles is wide;
(4) the performance is not easy to control, and the method is not suitable for process production.
Chinese patent 201710903703.9 discloses a method for preparing cerium-doped yttrium aluminum garnet spherical fluorescent powder, which is prepared by coprecipitation of YAG and Ce by using ammonium bicarbonate as a precipitator3+Or YAG precursor, and then using ethylenediamine or ethylenediamine-alcohol solution as a solvent in a reaction kettle to carry out solvent thermal reaction, wherein ammonium bicarbonate as a precipitator is a non-uniform precipitation system which is not easy to control, the precipitated particles have non-uniform and larger particle size, and a closed hydrothermal reaction kettle is used in the system, the precursor is dispersed in alcohol, so that great potential safety hazard exists under the conditions of high temperature and high pressure.
Chinese patent 201110070153.X discloses a preparation method of cerium-doped yttrium aluminum garnet fluorescent powder, which is characterized in that YAG and Ce are mixed by a microorganism-coprecipitation method3+The method relates to microbial operation, conditions are not easy to control compared with a chemical method, the method is not economical and easy for industrial production, and the obtained fluorescent split bodies have an agglomeration phenomenon.
In the method for preparing nano-scale spherical yttrium aluminum garnet powder disclosed in chinese patent 200710118421.4, the precursor is subjected to subsequent high-temperature roasting treatment to rapidly aggregate and agglomerate the YAG powder of the original small size, so that the particle size is increased and the dispersibility is deteriorated.
Disclosure of Invention
The invention aims to provide a method for preparing cerium-doped yttrium aluminum garnet fluorescent powder, which can obtain spherical highly-dispersed agglomeration-free (Y) fluorescent powder with high-efficiency luminescence1-XCeX）3Al5O12And (3) powder.
Description of terms: YAG Ce is a abbreviation for (Y1-xCex)3Al5O12, named cerium-doped yttrium aluminum garnet.
The technical scheme adopted by the invention for solving the problems is as follows: a method for preparing cerium-doped yttrium aluminum garnet fluorescent powder comprises the following steps:
(1) preparing precursor reaction solution
S1 according to formula (Y)1-XCeX）3Al5O12Weighing yttrium salt, cerium salt and aluminum salt at a metering ratio of x being more than 0 and less than or equal to 0.1, dissolving the yttrium salt, the cerium salt and the aluminum salt in deionized water, and preparing a mixed mother salt solution with the ionic molar concentration of 0.05-0.8 mol/L;
s2 (NH)4)2SO4Dissolving in mixed solvent of ethanol and water to prepare (NH)4)2SO4A dispersant solution with a molar concentration of 0.0005-0.001 mol/L;
s3, dissolving urea in the dispersant solution prepared in S2 to prepare a precipitator solution with the molar concentration of the urea of 0.02-1 mol/L;
(2) titration and aging
According to the molar amount of urea and Y3+、Ce3+And Al3+Weighing the precipitant solution and the mixed mother salt solution prepared in the step (1) at a total molar ratio of 10-20: 1, gradually titrating the mixed mother salt solution into the precipitant solution at a temperature of 80-95 ℃ under normal pressure, continuously stirring during titration, and aging for 16-24 hours after titration is finished;
（3）YAG:Ce3+precursor separation and washing
Vacuum filtering the aged precipitate mixed solution, washing, and vacuum filtering to obtain white precipitate YAG: Ce3+Precursor, washing the obtained white precipitate with deionized water and absolute ethyl alcohol successively;
（4）YAG:Ce3+drying treatment of precursor
Washed YAG Ce3+The precursor is treated by a surfactant, is dried at the temperature of 100 ℃ after being dispersed by ultrasound, and then dried YAG (yttrium aluminum garnet): Ce is obtained3+A precursor;
(5) ignition of precursor
Firing the precursor obtained in the step (4) for 3-6 h to obtain a firing product, wherein the firing temperature is 900-1000 ℃;
(6) ball milling and drying
Spraying alcohol on the obtained ignition product, ball-milling with zircon, and oven-drying to obtain target (Y)1-XCeX）3Al5O12And (3) powder.
Preferably, the diameter of zircon in the step (6) is less than or equal to 2 mm.
Preferably, the yttrium salt is Y (NO)3)3、Y(CH3COO)3Or YCl3Or their hydrates, and the aluminium salt is AlCl3、Al2(SO4)3、Al(NO3)3Or NH4Al (SO4)2 or a hydrate thereof, and the cerium salt is Ce (NO)3)3Or a hydrate thereof.
Preferably, the surfactant is sodium lauryl sulfate, polyvinyl alcohol, polyethylene glycol or polyvinylpyrrolidone.
Preferably, the surfactant is mixed with YAG to Ce3+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) along with the rise of temperature, the urea is dissolved to form a balanced and uniform system, and is hydrolyzed at a certain temperature to generate a precipitator NH4OH，NH4The crystal-forming ions OH-electrolyzed slowly and uniformly are uniformly distributed in the solution, precipitates can be generated uniformly, and the dispersity of the reaction process is easy to control.
(2) During the titration aging reaction, (NH) is added into the system4)2SO4The 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) before drying and firing, the precursor is treated with surfactant, which volatilizes to avoid chemical bond between particles, so as to form spherical and non-agglomerated YAG, Ce3+Nano/micron powder;
(4) the precursor is prevented from being dispersed in alcohol in a closed hydrothermal reaction kettle, so that the method is safer and is easy for industrial production;
(5) the polysorbate is added into the precipitator, so that the surface tension of particles can be reduced, and a protective layer can be formed on the surface of colloidal particles after the precursor adsorbs the polysorbate to play a role in steric hindrance, so that agglomeration is prevented.
Detailed Description
The present invention will be described in further detail with reference to examples.
Example 1:
according to the formula Y2.94Ce0.06Al5O120.00735mol of Y (NO)3)30.00015mol of Ce (NO)3)3And 0.0125mol AlCl3Dissolving the mixed mother salt solution in 100ml of deionized water to prepare a mixed mother salt solution with the ion molar concentration of 0.2 mol/L; 0.0005mol of (NH)4)2SO4Dissolving in 500ml of ethanol-water mixed solvent with volume ratio of 0.2:1 to prepare (NH)4)2SO4Dissolving 0.025mol of urea in the prepared dispersant solution to prepare a precipitator solution with the molar concentration of the urea of 0.5 mol/L;
according to the molar amount of urea and Y3+、Ce3+And Al3+The total molar ratio is 10:1Gradually titrating the mixed mother salt solution into the precipitant solution under normal pressure and 85 ℃ in the prepared precipitant solution and the mixed mother salt solution, continuously stirring during titration, and aging for 20 hours after titration is finished; vacuum filtering the aged precipitate mixed solution, washing, and vacuum filtering to obtain white precipitate YAG: Ce3+Precursor, washing the obtained white precipitate with deionized water and absolute ethyl alcohol successively;
washed YAG Ce3+The surface of the precursor was mixed with polyvinyl alcohol, ultrasonically dispersed, and dried at 100 ℃ to obtain 0.21g of dried YAG: Ce3+A precursor; firing the dried precursor at 900 ℃ for 6h to obtain a firing product; spraying alcohol on the obtained ignition product, ball-milling with zircon, and oven drying to obtain spherical (Y) with particle diameter of 800nm and high luminous efficiency1-XCeX）3Al5O12And (3) powder.
Example 2:
according to the formula Y2.95Ce0.05Al5O120.00295mol of Y (NO)3)30.00005mol of Ce (NO)3)3And 0.005molAl (NO)3)3Dissolving the mixed mother salt solution in 100ml of deionized water to prepare a mixed mother salt solution with the ion molar concentration of 0.08 mol/L; 0.0004mol of (NH)4)2SO4Dissolving in 500ml of ethanol-water mixed solvent with volume ratio of 0.2:1 to prepare (NH)4)2SO4Dissolving 0.02mol of urea in a dispersant solution with the molar concentration of 0.0008mol/L to prepare a precipitator solution with the molar concentration of 0.4mol/L of urea;
according to the molar amount of urea and Y3+、Ce3+And Al3+Weighing the prepared precipitant solution and the mixed mother salt solution according to the total mol ratio of 15:1, gradually titrating the mixed mother salt solution into the precipitant solution at the normal pressure and 85 ℃, continuously stirring during titration, and aging for 20 hours after titration; vacuum filtering the aged precipitate mixed solution, washing, and vacuum filtering to obtain white precipitate YAG: Ce3+Precursor, washing the obtained white precipitate with deionized water and absolute ethyl alcohol successively;
washed YAG Ce3+Mixing the precursor with polyvinyl alcohol, ultrasonically dispersing, and drying at 100 deg.C to obtain 0.19g dried YAG: Ce3 +; firing the dried precursor at 900 ℃ for 6h to obtain a firing product; spraying alcohol on the obtained ignition product, ball-milling with zircon, and oven drying to obtain spherical (Y) with high luminous efficiency, high dispersion, no agglomeration and particle diameter of 600nm1-XCeX）3Al5O12And (3) powder.
Example 3:
according to the formula Y2.95Ce0.05Al5O12Stoichiometric ratio of (2) 0.0018mol of Y (NO)3)30.000032mol of Ce (NO)3)3And 0.0032molAl (NO)3)3Dissolving the mixed mother salt solution in 100ml of deionized water to prepare a mixed mother salt solution with the ion molar concentration of 0.05 mol/L; 0.0005mol of (NH)4)2SO4Dissolving in 500ml of ethanol-water mixed solvent with volume ratio of 0.2:1 to prepare (NH)4)2SO4Dissolving 0.025mol of urea in the prepared dispersant solution to prepare a precipitator solution with the molar concentration of the urea of 0.05 mol/L;
according to the molar amount of urea and Y3+、Ce3+And Al3+Weighing the prepared precipitant solution and the mixed mother salt solution at a total mol 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 titration; vacuum filtering the aged precipitate mixed solution, washing, and vacuum filtering to obtain white precipitate YAG: Ce3+Precursor, washing the obtained white precipitate with deionized water and absolute ethyl alcohol successively;
washed YAG Ce3+The surface of the precursor was mixed with polyvinyl alcohol, ultrasonically dispersed, and dried at 100 ℃ to obtain 0.22g of dried YAG: Ce3+A precursor; drying the precursorBurning the mixture for 4 hours at 950 ℃ to obtain a burning product; spraying alcohol on the obtained ignition product, ball-milling with zircon, and oven drying to obtain spherical (Y) with high luminous efficiency, high dispersion, no agglomeration and particle diameter of 500nm1-XCeX）3Al5O12And (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 hydrogencarbonate.
Comparative example 2:
the procedure was substantially the same as in example 3, except that (NH) was not added to the precipitant4)2SO4A dispersant.
Comparative example 3:
the procedure of example 3 was followed except that polyethylene glycol was added to the precipitant.
Comparative example 4:
the production process was substantially the same as that of example 3, except that no surfactant treatment was performed upon firing.
As can be seen from the above table, it can be seen from the comparison of examples 1 to 3 that the molar amount of urea and Y are varied3+、Ce3+And Al3+The larger the ratio of the total molar weight of the three is, the smaller the formed particle size is; as can be seen from the examples and comparative example 1, the precipitant is ammonium bicarbonate precipitated particles with uneven and larger particle size, and urea decomposed and precipitated particles with even and small particle size; as is clear from the comparison of example 3 with comparative examples 1 and 2, No (NH) is added to the precipitant4)2SO4Dispersing agent or adding (NH) into ammonium bicarbonate precipitator4)2SO4Hard agglomeration of particles cannot be avoided; as can be seen from example 3 and comparative example 4, the aggregation and agglomeration phenomenon of the particles can be generated without surfactant treatment during firing, the particle size is increased, and the particle surface is rough; as can be seen from example 3 and comparative examples 2 and 3, the precipitant was addedAlthough the polyethylene glycol can reduce agglomeration phenomenon during sedimentation, the shape of the particles is also changed, so that the particles are olive-shaped, and the practicability is not high.
In addition to the above embodiments, the present invention also includes other embodiments, and any technical solutions formed by equivalent transformation or equivalent replacement should fall within the scope of the claims of the present invention.
Claims (7)
1. A method for preparing cerium-doped yttrium aluminum garnet fluorescent powder is characterized by comprising the following steps:
(1) preparing precursor reaction solution
S1 according to formula (Y)1-XCeX）3Al5O12Weighing yttrium salt, cerium salt and aluminum salt at a metering ratio of x being more than 0 and less than or equal to 0.1, dissolving the yttrium salt, the cerium salt and the aluminum salt in deionized water, and preparing a mixed mother salt solution with the ionic molar concentration of 0.05-0.8 mol/L;
s2 (NH)4)2SO4Dissolving in mixed solvent of ethanol and water to prepare (NH)4)2SO4A dispersant solution with a molar concentration of 0.0005-0.001 mol/L;
s3, dissolving urea in the dispersant solution prepared in S2 to prepare a precipitator solution with the molar concentration of the urea of 0.02-1 mol/L;
(2) titration and aging
According to the molar amount of urea and Y3+、Ce3+And Al3+Weighing the precipitant solution and the mixed mother salt solution prepared in the step (1) at a total molar ratio of 10-20: 1, gradually titrating the mixed mother salt solution into the precipitant solution at a temperature of 80-95 ℃ under normal pressure, continuously stirring during titration, and aging for 16-24 hours after titration is finished;
（3）YAG:Ce3+precursor separation and washing
Vacuum filtering the aged precipitate mixed solution, washing, and vacuum filtering to obtain white precipitate YAG: Ce3+Precursor, washing the obtained white precipitate with deionized water and absolute ethyl alcohol successively;
(4) drying treatment of YAG Ce3+ precursor
Washed YAG Ce3+The precursor is treated by a surfactant, is dried at the temperature of 100 ℃ after being dispersed by ultrasound, and then dried YAG (yttrium aluminum garnet): Ce is obtained3+A precursor;
(5) ignition of precursor
Firing the precursor obtained in the step (4) for 3-6 h to obtain a firing product, wherein the firing temperature is 900-1000 ℃;
(6) ball milling and drying
Spraying alcohol on the obtained ignition product, ball-milling with zircon, and oven-drying to obtain target (Y)1-XCeX）3Al5O12And (3) powder.
2. The method of claim 1, wherein the surfactant and the YAG Ce are mixed to form the Ce-doped YAG phosphor3+The molar ratio of the precursors is 0.01-0.2: 1.
3. The method of claim 2, wherein the surfactant is sodium dodecyl sulfate, polyvinyl alcohol, or polyvinyl pyrrolidone.
4. The method as claimed in claim 1, wherein the zircon diameter in step (6) is not more than 2 mm.
5. The method as claimed in claim 1, wherein the yttrium salt is Y (NO)3)3、Y(CH3COO)3Or YCl3Or their hydrates, and the aluminium salt is AlCl3、Al2(SO4)3、Al(NO3)3Or NH4Al (SO4)2 or a hydrate thereof, and the cerium salt is Ce (NO)3)3Or a hydrate thereof.
6. The method for preparing cerium-doped yttrium aluminum garnet phosphor powder according to claim 1, wherein the volume ratio of ethanol to water in the ethanol-water mixed solvent in the step (1) is 0.2: 1-0.5: 1.
7. The method as claimed in claim 1, wherein the precipitating solution in step (1) further comprises polysorbate, and the polysorbate and YAG Ce are added3+The molar ratio of the precursors is 0.01-0.2: 1.
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