CN110982526A - Double perovskite type red light fluorescent powder and preparation method and application thereof - Google Patents
Double perovskite type red light fluorescent powder and preparation method and application thereof Download PDFInfo
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- 239000000843 powder Substances 0.000 title claims abstract description 24
- 238000002360 preparation method Methods 0.000 title abstract description 11
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000000126 substance Substances 0.000 claims abstract description 12
- 239000000463 material Substances 0.000 claims abstract description 8
- 238000005245 sintering Methods 0.000 claims description 23
- 150000001875 compounds Chemical class 0.000 claims description 20
- 238000000034 method Methods 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 10
- 239000000347 magnesium hydroxide Substances 0.000 claims description 5
- 229910001862 magnesium hydroxide Inorganic materials 0.000 claims description 5
- RSEIMSPAXMNYFJ-UHFFFAOYSA-N europium(III) oxide Inorganic materials O=[Eu]O[Eu]=O RSEIMSPAXMNYFJ-UHFFFAOYSA-N 0.000 claims description 4
- PBCFLUZVCVVTBY-UHFFFAOYSA-N tantalum pentoxide Inorganic materials O=[Ta](=O)O[Ta](=O)=O PBCFLUZVCVVTBY-UHFFFAOYSA-N 0.000 claims description 3
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 claims description 2
- KTUFCUMIWABKDW-UHFFFAOYSA-N oxo(oxolanthaniooxy)lanthanum Chemical compound O=[La]O[La]=O KTUFCUMIWABKDW-UHFFFAOYSA-N 0.000 claims description 2
- LEDMRZGFZIAGGB-UHFFFAOYSA-L strontium carbonate Chemical compound [Sr+2].[O-]C([O-])=O LEDMRZGFZIAGGB-UHFFFAOYSA-L 0.000 claims description 2
- 229910000018 strontium carbonate Inorganic materials 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 abstract description 6
- 238000009877 rendering Methods 0.000 abstract description 4
- 238000010532 solid phase synthesis reaction Methods 0.000 abstract description 3
- 238000002795 fluorescence method Methods 0.000 abstract description 2
- 229910002410 SrLa Inorganic materials 0.000 abstract 1
- 238000000227 grinding Methods 0.000 description 6
- -1 rare earth ion Chemical class 0.000 description 6
- 229910052761 rare earth metal Inorganic materials 0.000 description 6
- 239000000047 product Substances 0.000 description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 3
- 238000000295 emission spectrum Methods 0.000 description 3
- 239000001095 magnesium carbonate Substances 0.000 description 3
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 3
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- 239000004570 mortar (masonry) Substances 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 230000005284 excitation Effects 0.000 description 2
- 238000000695 excitation spectrum Methods 0.000 description 2
- 238000004020 luminiscence type Methods 0.000 description 2
- 230000002194 synthesizing effect Effects 0.000 description 2
- 238000004458 analytical method Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 230000002596 correlated effect Effects 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000005090 crystal field Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000002019 doping agent Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 238000011031 large-scale manufacturing process Methods 0.000 description 1
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- 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
- C09K11/7701—Chalogenides
- C09K11/7703—Chalogenides with alkaline earth metals
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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
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/7729—Chalcogenides
- C09K11/7731—Chalcogenides with alkaline earth metals
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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
- C09K11/7783—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals one of which being europium
- C09K11/7784—Chalcogenides
- C09K11/7786—Chalcogenides with alkaline earth metals
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- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Luminescent Compositions (AREA)
Abstract
本发明特别涉及一种双钙钛矿型红光荧光粉及其制备方法与应用。本发明的双钙钛矿型红光荧光粉，化学式为SrLa(1‑x)MgTaO6:xEu3+，其中0≤x≤1.0。本发明的荧光法通过高温固相法，利用Eu3+掺杂在双钙钛矿结构主体SrLaMgTaO6而合成。本发明的荧光粉具有良好的显色指数，稳定性高、发光效率高、发光纯度高、强度高，在发光材料的应用中具有广阔的应用前景。本发明的荧光粉的制备方法简单易行、生产条件要求低、生产效率高、重复性好。
The invention particularly relates to a double perovskite type red light phosphor and a preparation method and application thereof. The double perovskite type red fluorescent powder of the present invention has a chemical formula of SrLa (1-x) MgTaO 6 :xEu 3+ , wherein 0≤x≤1.0. The fluorescence method of the present invention is synthesized by a high-temperature solid-phase method, using Eu 3+ doping in the double perovskite structure host SrLaMgTaO 6 . The fluorescent powder of the invention has good color rendering index, high stability, high luminous efficiency, high luminous purity and high intensity, and has broad application prospects in the application of luminescent materials. The preparation method of the phosphor of the invention is simple and feasible, has low requirements on production conditions, high production efficiency and good repeatability.
Description
Technical Field
The invention particularly relates to double perovskite type red light fluorescent powder and a preparation method and application thereof.
Background
The phosphor-converted white Light Emitting Diode (LED) has remarkable advantages, such as low power consumption, high electro-optic conversion efficiency, high brightness, good stability, fast response, and environmental friendliness, and is a new light source for the next generation of lighting industry and display systems. Currently, blue InGaN-based LED chips and yellow phosphor Y are combined3Al5O12：Ce3+In combination, the method for emitting white light remains one of the simplest and most efficient methods in commercial applications. However, the current technical bottleneck is that white light emitted due to lack of red component shows poor Color Rendering Index (CRI)<80) And higher Correlated Color Temperature (CCT)>4500K) This has led to limitations in the application of this method of emitting white light in certain fields. Therefore, there is an urgent need to develop a red phosphor with high efficiency and excellent chemical stability to create an environment-friendly lighting environment meeting the requirements of warm white light emitting diodes.
The double perovskite structure compound is an important functional material, and the crystal structure of the compound is stable and has special physical and chemical properties. Many studies have shown that ordered double perovskite structure hosts AA 'BB' O with various dopant ions6(A, A ═ Ba, Sr, Ca; B ═ Ca, Mg; B ═ W, Mo, Ta) have different color emissions. Among them, since the A 'site becomes the best position for the optically active ion due to lack of inversion symmetry and high crystal field strength, it is desirable that the A' site is occupied by the doped rare earth ion. However, in most double perovskite structures, the degree of matching of the B site is high due to the property limitation of the material, and therefore, the B site is occupied by the doped rare earth ions, and the luminescence performance is not good. Furthermore, B' O6The energy absorbed by the radicals is in a double perovskite structureAlong B' O6The energy transfer of the backbone is strongly quenched, resulting in almost no energy transfer into the rare earth ions of the luminescent center. Therefore, if all the rare earth ions occupy the a' site and all the incident photons are absorbed by the charge transfer states of the rare earth ions, the luminous efficiency of the rare earth ions in the double perovskite structure can be greatly improved.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide double perovskite type red light fluorescent powder and a preparation method and application thereof. The fluorescence method of the invention uses Eu through a high-temperature solid phase method3+Doping double perovskite structure body SrLaMgTaO6And synthesizing. The fluorescent powder has the advantages of good color rendering index, high stability, high luminous efficiency, high luminous purity and high intensity, and has wide application prospect in the application of luminescent materials. The preparation method of the fluorescent powder is simple and easy to implement, low in production condition requirement, high in production efficiency and good in repeatability.
The invention adopts the following technical scheme.
A double perovskite type red light fluorescent powder has a chemical formula of SrLa(1-x)MgTaO6:xEu3+Wherein x is more than or equal to 0 and less than or equal to 1.0.
Preferably, x is 0.01, 0.05, 0.1, 0.3, 0.5, 0.7, 0.9, 1.0.
The preparation method of the double perovskite type red light fluorescent powder comprises the following steps:
(1) according to the chemical formula SrLa(1-x)MgTaO6:xEu3+In stoichiometric amount, Sr will be contained2+Compound of (1), La-containing3+Compound of (2), containing Mg2+Compound of (1), containing Ta5+Compound of (1), containing Eu3+The compound (2) is mixed evenly to obtain a mixture;
(2) and sintering the mixture to obtain the double perovskite type red light fluorescent powder.
Preferably, the Sr content2+The compound of (A) is SrCO3。
Preferably, the La-containing3+The compound of (A) is La2O3。
Preferably, said Mg is contained2+The compound of (MgCO)3)4Mg(OH)2·5H2O。
Preferably, the Ta-containing5+The compound of (A) is Ta2O5。
Preferably, the Eu-containing3+Is Eu2O3。
Preferably, the sintering is carried out in air, and comprises a first sintering and a second sintering; the first sintering is carried out at 650 ℃ for 2 hours; the second sintering was carried out at 1400 ℃ for 12 hours.
In the first sintering, the low-temperature pre-sintering ensures that the crystallinity of the sample is higher in the next sintering, so that the luminescence property of the product is more stable. Synthesizing the final product through secondary sintering.
Further preferably, the product of the first sintering is ground.
The double perovskite type red fluorescent powder is applied to luminescent materials.
The invention has the beneficial effects that:
(1) the invention synthesizes the red fluorescent powder with high efficiency and excellent chemical stability by a high-temperature solid phase method;
(2) compared with the existing luminescent material, the fluorescent powder has the advantages of good color rendering index, high stability, high luminous efficiency, high luminous purity and high intensity, and has wide application prospect in the application of the luminescent material;
(3) the preparation method is simple and feasible, has low requirement on production conditions, high production efficiency and good repeatability, and is suitable for large-scale production.
Drawings
FIG. 1 is an X-ray diffraction pattern of the double perovskite type red phosphor prepared in example 1;
FIG. 2 is an excitation and emission spectrum of the double perovskite red phosphor prepared in example 2;
FIG. 3 is an emission spectrum of the double perovskite red phosphor prepared in example 3.
Detailed Description
The present invention will be described in detail below with reference to specific embodiments.
Example 1
A double perovskite type red light fluorescent powder has a chemical formula of SrLaMgTaO6。
The preparation method of the double perovskite type red light fluorescent powder comprises the following steps:
(1) according to the formula SrLaMgTaO6In a stoichiometric amount of 0.28g SrCO3、0.31g La2O3、0.185g(MgCO3)4Mg(OH)2·5H2O、0.42g Ta2O5Grinding and uniformly mixing in an agate mortar to obtain a mixture;
(2) and (3) performing primary sintering on the mixture at 650 ℃ for 2 hours in a muffle furnace and in an air atmosphere, grinding the primary sintered product, and performing secondary sintering at 1400 ℃ for 12 hours to obtain the double perovskite type red fluorescent powder.
The X-ray diffraction pattern analysis of the double perovskite red phosphor prepared in example 1 was carried out, and the obtained results are shown in fig. 1.
Example 2
A double perovskite type red light fluorescent powder has a chemical formula of SrLa0.5MgTaO6:0.5Eu3+。
The preparation method of the double perovskite type red fluorescent powder comprises the following steps:
(1) according to the chemical formula SrLa0.5MgTaO6:0.5Eu3+In a stoichiometric amount of 0.28g SrCO3、0.155g La2O3、0.185g(MgCO3)4Mg(OH)2·5H2O、0.42g Ta2O5、0.167g Eu2O3Grinding and uniformly mixing in an agate mortar to obtain a mixture;
(2) and (3) performing primary sintering on the mixture at 650 ℃ for 2 hours in a muffle furnace and in an air atmosphere, grinding the primary sintered product, and performing secondary sintering at 1400 ℃ for 12 hours to obtain the double perovskite type red fluorescent powder.
Excitation and emission spectrograms of the phosphor prepared in example 2 were analyzed, and the results are shown in fig. 2 (the left part of the graph is an excitation spectrum, and the right part is an emission spectrum), respectively.
Example 3
A double perovskite type red light fluorescent powder has a chemical formula of SrMgTaO6:1.0Eu3+。
(1) According to the formula SrMgTaO6:1.0Eu3+In a stoichiometric amount of 0.28g SrCO3、0.185g(MgCO3)4Mg(OH)2·5H2O、0.42g Ta2O5、0.334g Eu2O3Grinding and uniformly mixing in an agate mortar to obtain a mixture;
(2) and (3) performing primary sintering on the mixture at 650 ℃ for 2 hours in a muffle furnace and in an air atmosphere, grinding the primary sintered product, and performing secondary sintering at 1400 ℃ for 12 hours to obtain the double perovskite type red fluorescent powder.
The emission spectrograms of the double perovskite red phosphors prepared in example 3 were analyzed, and the obtained results are shown in fig. 3, respectively.
Claims (9)
1. The double perovskite type red light fluorescent powder is characterized in that the chemical formula is SrLa(1-x)MgTaO6:xEu3+Wherein x is more than or equal to 0 and less than or equal to 1.0.
2. The method for preparing a double perovskite red phosphor according to claim 1, comprising the steps of:
(1) according to the chemical formula SrLa(1-x)MgTaO6:xEu3+In stoichiometric amount, Sr will be contained2+Compound of (1), La-containing3+Compound of (2), containing Mg2+Compound of (1), containing Ta5+Compound of (1), containing Eu3+The compound (2) is mixed evenly to obtain a mixture;
(2) and sintering the mixture to obtain the double perovskite type red light fluorescent powder.
3. The method for preparing a double perovskite red phosphor according to claim 2, wherein said Sr is contained2+The compound of (A) is SrCO3。
4. The method for preparing a double perovskite red phosphor according to claim 2, wherein the La is contained3+The compound of (A) is La2O3。
5. The method for preparing a double perovskite red phosphor according to claim 2, wherein the Mg is contained2+The compound of (MgCO)3)4Mg(OH)2·5H2O。
6. The method for preparing a double perovskite red phosphor according to claim 2, wherein the Ta-containing phosphor5+The compound of (A) is Ta2O5。
7. The method for preparing a double perovskite red phosphor according to claim 2, wherein the Eu-containing component3+Is Eu2O3。
8. The method for preparing a double perovskite red phosphor according to claim 2, wherein the sintering is performed in air, and comprises a first sintering and a second sintering; the first sintering is carried out at 650 ℃ for 2 hours; the second sintering was carried out at 1400 ℃ for 12 hours.
9. Use of the double perovskite red phosphor of claim 1 in luminescent materials.
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| Application Number | Priority Date | Filing Date | Title |
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| CN201911318790.7A CN110982526A (en) | 2019-12-19 | 2019-12-19 | Double perovskite type red light fluorescent powder and preparation method and application thereof |
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| CN201911318790.7A CN110982526A (en) | 2019-12-19 | 2019-12-19 | Double perovskite type red light fluorescent powder and preparation method and application thereof |
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- 2019-12-19 CN CN201911318790.7A patent/CN110982526A/en active Pending
Non-Patent Citations (2)
| Title |
|---|
| YUE GUO ET AL.: "A red-emitting perovskite-type SrLa(1-x)MgTaO6:xEu3+ for white LED application", 《JOURNAL OF LUMINESCENCE》 * |
| YUE GUO ET AL.: "Color-tunable luminescence and energy transfer behaviors of Dy3+/Eu3+ co-doped SrLaMgTaO6 phosphors for solid state lighting applications", 《MATERIALS RESEARCH BULLETIN》 * |
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