CN103361059A - Ammonia homogeneous precipitation method for preparing Ce-doped yttrium aluminum garnet phosphor - Google Patents
Ammonia homogeneous precipitation method for preparing Ce-doped yttrium aluminum garnet phosphor Download PDFInfo
- Publication number
- CN103361059A CN103361059A CN2013103187532A CN201310318753A CN103361059A CN 103361059 A CN103361059 A CN 103361059A CN 2013103187532 A CN2013103187532 A CN 2013103187532A CN 201310318753 A CN201310318753 A CN 201310318753A CN 103361059 A CN103361059 A CN 103361059A
- Authority
- CN
- China
- Prior art keywords
- aluminum garnet
- yttrium aluminum
- doped yttrium
- cerium
- ammonia
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Pending
Links
Images
Abstract
The invention discloses an ammonia homogeneous precipitation method for preparing a Ce-doped yttrium aluminum garnet phosphor. The chemical formula of the Ce-doped yttrium aluminum garnet is CexY3-xAl5O12, wherein 0<x<0.8. The preparation method comprises processes of preparation of a solution, mixing, precipitating, washing, drying and calcining. The prepared Ce-doped yttrium aluminum garnet polycrystalline powder is ultrafine in granularity, uniform in dispersion, narrow in particle size distribution, and uniform in chemical ingredient. The preparation method is simple, and industrialization is easy to realize.
Description
Technical field
The invention belongs to the fluorescent material preparing technical field, be specifically related to a kind of ammonia homogeneous precipitation method for preparing the cerium-doped yttrium aluminum garnet fluorescent powder.
Background technology
Photodiode (Light emitting diode, LED) many advantages have been compared as lighting source with the traditional lighting light source,, less energy consumption little such as volume, response is fast, the life-span is long, pollution-free etc., therefore be called the 4th generation lighting source, be widely used in mobile communication, landscape light in city, auto lamp, traffic lights, LCD backlight, indoor and outdoor general lighting etc.Yttrium aluminum garnet (yttrium aluminum garnet, Y
3Al
5O
12, YAG) belonging to isometric system, lattice parameter is 1.2nm.The radius of Y ionic radius and trivalent rare earth Ce ion is close, usually in YAG, mix Ce as active ions with preparation YAG:Ce fluorescent material.Pure YAG is transparent at visible region and near-infrared region, and with the blue-light excited YAG:Ce fluorescent material that blue-light LED chip sends, making its emission wavelength is the gold-tinted of 550～580 nm, and this gold-tinted can become white light with remaining blue light.
At present, the main flow white light LEDs adopts YAG:Ce fluorescent material to cooperate the mode of blue-ray LED, and the production of YAG:Ce fluorescent material now realized industrialization, and the industrial preparative method of fluorescent material still is high temperature solid-state method.The deficiency of high temperature solid-state method is to make fluorescent material, and size distribution is generally wider, powder secondary poor performance; The emission wavelength of fluorescent material is shorter, and the ruddiness composition is not enough, and the compound white light colour temperature that goes out is more high.Had a strong impact on the performance after LED encapsulates.
In addition, sol-gel method, combustion method, hydrothermal synthesis method, spray method etc. also have the research report.Though these methods have solved subproblem, also there are some drawbacks, such as spray method apparatus expensive, complexity, easily obtain the particle of hollow morphology, cause twinkler brightness and stability to reduce; And hydro-thermal reaction is carried out under high temperature, high pressure, so reaction is very high to equipment requirements, and the technique more complicated, not easy to operate; Combustion method is easily brought impurity such as carbon etc. into.
Summary of the invention
The object of the present invention is to provide a kind of ammonia homogeneous precipitation method for preparing the cerium-doped yttrium aluminum garnet fluorescent powder, the cerium-doped yttrium aluminum garnet polycrystal powder granularity that makes is ultra-fine, be uniformly dispersed, narrow particle size distribution, chemical composition homogeneous.The preparation method is simple, is easy to realize industrialization.
For achieving the above object, the present invention adopts following technical scheme:
A kind ofly prepare the cerium-doped yttrium aluminum garnet fluorescent powder (chemical formula is Ce
xY
3-xAl
5O
12, 0＜x＜0.8 wherein) the ammonia homogeneous precipitation method comprise preparation, mixing, precipitation, washing, drying and the calcination process of solution:
(1) metal cation salt adopts deionized water to dissolve as solvent, and the addition of solvent is 5 ~ 30 times of metal cation salt quality;
(2) Ce (NO
3)
3, Y (NO
3)
3And Al (NO
3)
3The temperature of mixing solutions be controlled at 20-50 ℃, stir constantly that lower ammonia flow is controlled at 5-60mL/min to wherein passing into ammonia, the pH value of solution was 8.0-9.0 after precipitin reaction was finished, and is still aging, gets the precipitation suspension liquid;
(3) will precipitate the suspension liquid decompress filter, after filter cake fully washs with deionized water and dehydrated alcohol respectively, the precursor that places 40-60 ℃ baking oven vacuum-drying 20-30h to obtain loosening;
(4) precursor 900-1100 ℃ calcine be uniformly dispersed, the cerium-doped yttrium aluminum garnet polycrystal powder that spherical, individual particle is of a size of 40 ~ 80nm.
The present invention utilizes ammonia to be dissolved in the aqueous solution hydrolysis reaction occurs and slowly and equably discharges OH
-Ion, thus realize with the metal ion generation coprecipitation reaction in the solution.Lead to ammonia in the solution of metal ion, ammonia contacts with solution, and following balanced reaction will occur:
NH
3+H
2O NH
3·H
2O
NH
3·H
2O NH
4 ++OH
-
Above two balanced reactions can guarantee slowly and equably to discharge in the whole solution OH
-Ion is avoided OH
-Density unevenness is spared phenomenon, degree of supersaturation is controlled in the suitable scope, slowly separate out equably thereby make to be deposited in the whole solution, can prepare relatively easily granularity ultra-fine, be uniformly dispersed, the YAG:Ce fluorescent powder of narrow particle size distribution, chemical composition homogeneous.It is a kind of comparatively desirable method of multivariant oxide for preparing.
Remarkable advantage of the present invention is: the cerium-doped yttrium aluminum garnet polycrystal powder granularity that makes is ultra-fine, be uniformly dispersed, narrow particle size distribution, chemical composition homogeneous.The preparation method is simple, is easy to realize industrialization.
Description of drawings
Fig. 1 is scanning electronic microscope (SEM) photo of the cerium doped yttrium aluminum garnet fluorescent powder of embodiment 1 preparation.
Fig. 2 is X-ray diffraction (XRD) collection of illustrative plates of the cerium doped yttrium aluminum garnet fluorescent powder of embodiment 1 preparation.
Embodiment
Following example is unrestricted the present invention in order further to illustrate technological process feature of the present invention.
EXAMPLE l
During x=0.09, according to chemical formula Ce
0.09Y
2.91Al
5O
12, take by weighing respectively 0.200g six water cerous nitrates, 5.706g six water Yttrium trinitrates and 9.600g nine water aluminum nitrates.The raw material that weighs up is dissolved in the 80ml deionized water, and fully stirring makes it to mix.Under the room temperature, pass into ammonia while stir in above-mentioned metallic ion mixed liquor, ammonia flow is controlled at 30ml/min.When the pH of solution value becomes 8.8, stop to pass into ammonia, gained is precipitated the still aging 30min of suspension liquid, then carry out decompress filter, after filter cake fully washs with deionized water and dehydrated alcohol respectively, the presoma that places 60 ℃ baking oven vacuum-drying 24h to obtain loosening.After precursor ground in agate mortar repeatedly, the quartz crucible of packing into placed retort furnace namely to get flaxen cerium-doped yttrium aluminum garnet nano powder 2 hours 2 ~ 3 times in the lower 1000 ℃ of calcinings of normal pressure.
Embodiment 2
During x=0.12, according to chemical formula Ce
0.12Y
2.88Al
5O
12, take by weighing respectively the 0.200g cerous nitrate, 4.236g Yttrium trinitrate and 7.200g aluminum nitrate.The raw material that weighs up is dissolved in the 80ml deionized water, and fully stirring makes it to mix.Place water bath with thermostatic control, keeping bath temperature is 40 ℃, passes into ammonia while stir in above-mentioned metallic ion mixed liquor, and ammonia flow is controlled at 20ml/min.When the pH of solution value becomes 8.9, stop to pass into ammonia, gained is precipitated the still aging 30min of suspension liquid, then carry out decompress filter, after filter cake fully washs with deionized water and dehydrated alcohol respectively, the presoma that places 60 ℃ baking oven vacuum-drying 24h to obtain loosening.After precursor ground in agate mortar repeatedly, the quartz crucible of packing into placed retort furnace namely to get yellowish cerium-doped yttrium aluminum garnet nano powder 2 hours 2 ~ 3 times in the lower 1000 ℃ of calcinings of normal pressure.
Embodiment 3
During x=0.18, according to chemical formula Ce
0.18Y
2.82Al
5O
12, take by weighing respectively the 0.200g cerous nitrate, 2.765g Yttrium trinitrate and 4.800g aluminum nitrate.The raw material that weighs up is dissolved in the 70ml deionized water, and fully stirring makes it to mix.Under the room temperature, pass into ammonia while stir in above-mentioned metallic ion mixed liquor, ammonia flow is controlled at 30ml/min.When the pH of solution value becomes 8.8, stop to pass into ammonia, gained is precipitated the still aging 30min of suspension liquid, then carry out decompress filter, after filter cake fully washs with deionized water and dehydrated alcohol respectively, the presoma that places 60 ℃ baking oven vacuum-drying 24h to obtain loosening.After precursor ground in agate mortar repeatedly, the quartz crucible of packing into placed retort furnace namely to get flaxen cerium-doped yttrium aluminum garnet nano powder 2 hours 2 ~ 3 times in the lower 1000 ℃ of calcinings of normal pressure.
Embodiment 4
During x=0.42, according to chemical formula Ce
0.42Y
2.58Al
5O
12, take by weighing respectively the 0.200g cerous nitrate, 1.084g Yttrium trinitrate and 2.057g aluminum nitrate.The raw material that weighs up is dissolved in the 60ml deionized water, and fully stirring makes it to mix.Under the room temperature, pass into ammonia while stir in above-mentioned metallic ion mixed liquor, ammonia flow is controlled at 50ml/min.When the pH of solution value becomes 8.8, stop to pass into ammonia, gained is precipitated the still aging 30min of suspension liquid, then carry out decompress filter, after filter cake fully washs with deionized water and dehydrated alcohol respectively, the presoma that places 60 ℃ baking oven vacuum-drying 24h to obtain loosening.After precursor ground in agate mortar repeatedly, the quartz crucible of packing into placed retort furnace namely to get flaxen cerium-doped yttrium aluminum garnet nano powder 2 hours 2 ~ 3 times in the lower 1000 ℃ of calcinings of normal pressure.
Adopt HITACHI S-4300 type scanning electronic microscope (SEM) observation post to get individual particle granularity and the pattern of cerium doped yttrium aluminum garnet fluorescent powder.Adopt Switzerland's Bruker D8 advance Rigaku D/Max-rA X-ray diffractometer (XRD) that the gained powder is carried out material phase analysis.
The above only is preferred embodiment of the present invention, and all equalizations of doing according to the present patent application claim change and modify, and all should belong to covering scope of the present invention.
Claims (5)
1. ammonia homogeneous precipitation method for preparing the cerium-doped yttrium aluminum garnet fluorescent powder, it is characterized in that: the chemical formula of described cerium-doped yttrium aluminum garnet is Ce
xY
3-xAl
5O
12, 0＜x＜0.8 wherein;
The preparation method comprises preparation, mixing, precipitation, washing, drying and the calcination process of solution:
(1) metal cation salt adopts deionized water to dissolve as solvent, and the addition of solvent is 5 ~ 30 times of metal cation salt quality;
(2) Ce (NO
3)
3, Y (NO
3)
3And Al (NO
3)
3The temperature of mixing solutions be controlled at 20-50 ℃, stir constantly that lower ammonia flow is controlled at 5-60mL/min to wherein passing into ammonia, the pH value of solution was 8.0-9.0 after precipitin reaction was finished, and is still aging, gets the precipitation suspension liquid;
(3) will precipitate the suspension liquid decompress filter, after filter cake fully washs with deionized water and dehydrated alcohol respectively, the precursor that places 40-60 ℃ baking oven vacuum-drying 20-30h to obtain loosening;
(4) calcine to get cerium-doped yttrium aluminum garnet polycrystal powder for precursor 900-1100 ℃.
2. the ammonia homogeneous precipitation method of preparation cerium-doped yttrium aluminum garnet fluorescent powder according to claim 1 is characterized in that: metal ion Ce
3+ ,Y
3+With Al
3+Introduce with the form of nitrate, or with the corresponding metal of nitric acid dissolve or metal oxide, or adopt the combination of corresponding muriate and nitrate, the proportioning of nitrate is pressed chemical formula Ce
xY
3-xAl
5O
12, wherein calculate 0＜x＜0.8.
3. the ammonia homogeneous precipitation method of preparation cerium-doped yttrium aluminum garnet fluorescent powder according to claim 1 is characterized in that: the cerium-doped yttrium aluminum garnet polycrystal powder granularity of preparation is uniformly dispersed, spherical, individual particle is of a size of 40 ~ 80nm.
4. the ammonia homogeneous precipitation method of preparation cerium-doped yttrium aluminum garnet fluorescent powder according to claim 1 is characterized in that: what 900 ℃ of calcination processing obtained is the cerium-doped yttrium aluminum garnet polycrystal powder of pure phase.
5. the application of the cerium-doped yttrium aluminum garnet fluorescent powder that makes of the method for claim 1, it is characterized in that: cerium-doped yttrium aluminum garnet polycrystal powder is used for making white light LEDs.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2013103187532A CN103361059A (en) | 2013-07-26 | 2013-07-26 | Ammonia homogeneous precipitation method for preparing Ce-doped yttrium aluminum garnet phosphor |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2013103187532A CN103361059A (en) | 2013-07-26 | 2013-07-26 | Ammonia homogeneous precipitation method for preparing Ce-doped yttrium aluminum garnet phosphor |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN103361059A true CN103361059A (en) | 2013-10-23 |
Family
ID=49363340
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN2013103187532A Pending CN103361059A (en) | 2013-07-26 | 2013-07-26 | Ammonia homogeneous precipitation method for preparing Ce-doped yttrium aluminum garnet phosphor |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN103361059A (en) |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20050012446A1 (en) * | 2003-05-28 | 2005-01-20 | Frank Jermann | Conversion led |
| CN101602944A (en) * | 2009-07-09 | 2009-12-16 | 宁波大学 | A kind of production method of rare earth ion doped yttrium aluminum garnet nano phosphor powder |
| CN102391871A (en) * | 2011-10-25 | 2012-03-28 | 湘潭大学 | Preparation method of nano yttrium aluminum garnet fluorescent powder |
-
2013
- 2013-07-26 CN CN2013103187532A patent/CN103361059A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20050012446A1 (en) * | 2003-05-28 | 2005-01-20 | Frank Jermann | Conversion led |
| CN101602944A (en) * | 2009-07-09 | 2009-12-16 | 宁波大学 | A kind of production method of rare earth ion doped yttrium aluminum garnet nano phosphor powder |
| CN102391871A (en) * | 2011-10-25 | 2012-03-28 | 湘潭大学 | Preparation method of nano yttrium aluminum garnet fluorescent powder |
Non-Patent Citations (2)
| Title |
|---|
| YUEXIAO PAN等: "Comparative investigation on synthesis and photoluminescence of YAG:Ce phosphor", 《MATERIALS SCIENCE AND ENGINEERING B》 * |
| 孙海鹰: "氨水、尿素、碳酸氢铵共沉淀法制备YAG 超细粉体", 《长春理工大学学报（自然科学版）》 * |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| Li et al. | Multiform La 2 O 3: Yb 3+/Er 3+/Tm 3+ submicro-/microcrystals derived by hydrothermal process: Morphology control and tunable upconversion luminescence properties | |
| Wang et al. | 3D-hierachical spherical LuVO4: Tm3+, Dy3+, Eu3+ microcrystal: synthesis, energy transfer, and tunable color | |
| CN111057399B (en) | Preparation method of rare earth doped clay mineral-based bismuth yellow hybrid pigment with adjustable fluorescence and color | |
| CN104353400A (en) | Preparation method of high-purity high-solid content transparent aluminum sol | |
| Hu et al. | Preparation of LaPO4: Ce, Tb phosphor with different morphologies and their fluorescence properties | |
| CN107163942A (en) | Small particle cerium dropped yttrium aluminum garnet fluorescent material and method and application prepared by a kind of coprecipitation | |
| CN102181291B (en) | Method for preparing cerium doped yttrium aluminum garnet fluorescent powder | |
| CN1718669A (en) | Method of preparing cerium activated yttrium aluminium garnet ultrafine fluorescent powder using coprecipitation | |
| CN112029502B (en) | Lanthanum silicate luminescent powder material with apatite structure, and preparation method and application thereof | |
| CN101831292A (en) | Strontium aluminate luminous material and controllable synthesis method thereof | |
| Raju et al. | Development of dumbbell-shaped La2Si2O7: Eu3+ nanocrystalline phosphors for solid-state lighting applications | |
| CN100478417C (en) | Sol-gel method for fast synthesizing luminescent material | |
| CN116199270B (en) | Treatment process for reducing wastewater in cobalt oxide production process | |
| CN100422288C (en) | Process for preparing yttrium aluminum garnet | |
| Zhou et al. | Effect of surfactants on morphology and luminescent properties of Ca3 (VO4) 2: Bi, Eu3+ red phosphors | |
| CN104845615B (en) | A kind of rare-earth doped beta phase Sr2SiO4Nano-powder and preparation method thereof | |
| CN113321233B (en) | Method for preparing hexagonal system lanthanum hydroxycarbonate by adopting precipitation firing method | |
| CN102618279B (en) | Preparation method of shape-controllable aluminate luminous materials | |
| CN102337122B (en) | Silicate green fluorescent powder and preparation method thereof | |
| CN113800574B (en) | Nickel-manganese-iron-aluminum-lithium positive electrode material and preparation method thereof | |
| CN103361059A (en) | Ammonia homogeneous precipitation method for preparing Ce-doped yttrium aluminum garnet phosphor | |
| CN103849386B (en) | A kind of colloidal sol auto-combustion method prepares the method for aluminate blue fluorescent powder | |
| CN109810705B (en) | Europium-doped barium magnesium niobate red fluorescent powder and preparation method thereof | |
| CN102618263B (en) | Preparation method for silicate luminescent material | |
| CN104861974A (en) | Fluorescent compound using pyrochlore structure metatitanic acid lanthanum as substrate and preparation method and application |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| C06 | Publication | ||
| PB01 | Publication | ||
| C10 | Entry into substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| C12 | Rejection of a patent application after its publication | ||
| RJ01 | Rejection of invention patent application after publication |
Application publication date: 20131023 |