CN101586030A - Wavelength conversion substance and application thereof - Google Patents

Wavelength conversion substance and application thereof Download PDF

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CN101586030A
CN101586030A CN 200810100503 CN200810100503A CN101586030A CN 101586030 A CN101586030 A CN 101586030A CN 200810100503 CN200810100503 CN 200810100503 CN 200810100503 A CN200810100503 A CN 200810100503A CN 101586030 A CN101586030 A CN 101586030A
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light
fluorescent powder
wavelength
metal halogen
wavelength conversion
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CN 200810100503
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CN101586030B (en
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汤友圣
刘如熹
胡淑芬
王健源
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Epistar Corp
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Epistar Corp
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Abstract

The invention discloses a wavelength conversion substance which comprises fluorescent powder of metal halogen aluminate compound and has the general formula of Mw-pAlyOzXq:Rp, wherein the w, the y, the z and the q are all more than 0, the p is more than 0.005 and less than 0.5, the q=2w+3y-2z, the m is at least one element selected from the group including Be, Mg, Ca, Sr, Ba and Zn, X is at least one element selected from the group including F, Cl, Br and I, and the R is one or more transition elements and comprises one lanthanide element; and the wavelength of the light emitted by the fluorescent powder of the metal halogen aluminate compound is 550-650nm covering green light wavelength range and the red light wavelength range, thus the white light obtained by mixing the light with blue light has better color rendering properties. In addition, the invention further discloses a photoelectric element applying the fluorescent powder of the metal halogen aluminate compound.

Description

Wavelength conversion substance and application thereof
Technical field
The invention provides a kind of Wavelength conversion substance, particularly is the fluorescent powder of metal halogen aluminate compound about material, and the application of this metal halogen aluminate compound fluorescent powder.
Background technology
Utilizing photodiode (Light Emitting Diode) to produce and white light like the sunlight form and aspect, significantly to replace white-light illuminating such as traditional fluorescent lamp, is the positive target of research and development of lighting source sciemtifec and technical sphere in this century.The technology of present known Single chip white light LED is mainly the blue-light LED chip that utilizes emission wavelength 440nm to 460nm and excites gold-tinted fluorescent material, by blue light and mixing of gold-tinted producing white light; Preparation is simple, low cost and other advantages though have in the aforesaid method, yet its colorimetric purity of the white light that is produced and color developing and sunlight still have a segment distance.
The also ultraviolet light-emitting diodes of development utilization emission wavelength 360nm to 400nm (UV-LED) chip excites red (R), green (G) and blue (B) three kinds of different photochromic fluorescent material in recent years, forms white light and mix; Above-mentioned method has luminous efficiency height, color developing height, and the many advantages of the fluorescent material that can arrange in pairs or groups, yet, need to mix the fluorescent agent that several match well in process of production, just can control the white light source quality, degree of difficulty is higher on making.
Therefore, the present invention is for solving above-mentioned puzzlement, the luminous element that a kind of gold-tinted fluorescent powder of metal halogen aluminate compound is provided and uses this kind metal halogen aluminate compound fluorescent powder.
Summary of the invention
The purpose of this invention is to provide a kind of Wavelength conversion substance, its material is the fluorescent powder of metal halogen aluminate compound, and its general expression is:
M w-pAl yO zX q:R p
Wherein w, y, z, q＞0; 0.005＜p＜0.5; And satisfy q=2w+3y-2z; In addition, M is a single or two or more element in the group that Be, Mg, Ca, Sr, Ba, Zn formed; X is selected from single or two or more element in the group that F, Cl, Br, I form; R is selected from transition element for one or more materials, and comprises a kind of material that is selected from lanthanon at least.
Another object of the present invention is to provide metal halogen aluminate compound fluorescent powder, because metal halogen aluminate compound fluorescent powder radiating light is that wavelength is the gold-tinted of 550nm to 660nm, and the halfwidth (Full Width at half maximun) with about 120nm makes the white light that obtains after itself and the blue light have preferable color developing.
Another purpose of the present invention is to provide the sealed cell of applied metal halogen aluminate compound fluorescent powder, comprises the wavelength conversion layer that a luminous lamination and is made up of metal halogen aluminate fluorescent powder body at least.
A further object of the present invention is to provide the sealed cell of applied metal halogen aluminate compound fluorescent powder, at least comprise that a printed circuit board (PCB), a light-emitting diode chip for backlight unit are positioned on the above-mentioned printed circuit board (PCB), on a transparent enclosure glue material covering luminousing diode chip and the part printed circuit board (PCB), wherein have Wavelength conversion substance in the transparent enclosure glue material, and comprise metal halogen aluminate compound fluorescent powder in the Wavelength conversion substance at least in wherein.
Beneath by the appended graphic explanation in detail of specific embodiment cooperation, when the effect that is easier to understand purpose of the present invention, technology contents, characteristics and is reached.
The accompanying drawing summary
Fig. 1 is the embodiment of the invention (Sr 3-xEu x) (Al 2O 5) Cl 2The X-ray diffractogram of (x=0.05,0.1,0.15,0.2) sample.
Fig. 2 is the embodiment of the invention (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2Fluorescent material (Y with another jaundice light commercialization 3A 5O 12: Ce 3+) UV-light-excited by visible light source collection of illustrative plates.
Fig. 3 is the embodiment of the invention (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2With the photoemissive spectrogram of YAG:Ce sample.
Fig. 4 A is the structural representation of sealed cell embodiment of the present invention.
Fig. 4 B is another structural representation of sealed cell embodiment of the present invention.
Fig. 5 A is the another structural representation of sealed cell embodiment of the present invention.
Fig. 5 B is the structural representation again of sealed cell embodiment of the present invention.
Fig. 6 is the structural representation of backlight module embodiment of the present invention.
Fig. 7 is the structural representation of means of illumination embodiment of the present invention.
Fig. 8 is the embodiment of the invention (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2CIE1931 tristimulus coordinates figure with YAG:Ce.
The main element nomenclature
400 sealed cells, 40 substrates
42 luminous lamination 44 electrodes
46 wavelength conversion layers, 460 metal halogen aluminate fluorescent powder bodies
462 UV-light or near ultraviolet excitation blue light fluorescent powder body
500 sealed cells, 50 printed circuit board (PCB)s
52 circuit patterns, 54 light-emitting diode chip for backlight unit
56 metal wires, 58 transparent enclosure glue materials
580 metal halogen aluminate fluorescent powder bodies
582 UV-light or near ultraviolet excitation blue light fluorescent powder body
Embodiment
The present invention discloses Wavelength conversion substance and application thereof.In order to make narration of the present invention more detailed and complete, can and cooperate Fig. 1 to Fig. 8 with reference to following description.
The present invention discloses a kind of Wavelength conversion substance, and this Wavelength conversion substance is a metal halogen aluminate compound, and its chemical formula is M W-pAl yO zX q: R pWherein w, y, z, q＞0; 0.005＜p＜0.5; And satisfy q=2w+3y-2z; In addition, M is a single or two or more element in the group that Be, Mg, Ca, Sr, Ba, Zn formed; X is selected from single or two or more element in the group that F, Cl, Br, I form; R is selected from transition element for one or more materials, and comprises a kind of material that is selected from lanthanon at least.
The preparation method of metal halogen aluminate fluorescent powder body of the present invention below will be described, and with (Sr 3-xEu x) (Al 2O 5) Cl 2Be example, illustrate that disclosed metal halogen aluminate fluorescent powder system makes method.
Disclosed alkaline earth halogen aluminate can utilize solid state reaction, chemical synthesis, Citrate trianion gel method, and mode such as spray pyrolysis method is synthetic obtains, and present embodiment is to be example with the solid state reaction, illustrate to synthesize (Sr 3-xEu x) (Al 2O 5) Cl 2Method.At first, get first reactant, second reactant that contains aluminium (Al) that contain strontium (Sr) respectively, contain the 3rd reactant of chlorine (Cl) according to stoichiometric ratio, and the 4th reactant that contains europium (Eu); Then first reactant, second reactant, the 3rd reactant and the 4th reactant are ground and thorough mixing with mortar, uniform mixture is placed alumina crucible, and the reducing atmosphere of again alumina crucible being inserted in 1000 to 1300 ℃ of tube furnaces heated 2 to 6 hours down; In the present embodiment, be to feed hydrogen (H 2), nitrogen (N 2) the mixing reducing gas, wherein the ratio that feeds of hydrogen-oxygen and nitrogen is about 5%: 95%; Be heated to 1300 ℃ with 5 ℃/minute temperature rise rate again and reduce (reduction) reaction, and lasting constant temperature 3 hours; Continue it, be cooled to room temperature with 5 ℃/minute rate of temperature fall again; Behind the reduction sintering, ground, make it become evengranular powder, promptly obtained metal hydracid aluminium salt compounds fluorescent material (Sr with mortar 3-xEu x) (Al 2O 5) Cl 2
First reactant that wherein contains strontium (Sr) can be selected from Strontium carbonate powder (SrCO 3), strontium nitrate (Sr (NO 3) 2) or strontium oxide (SrO), also can directly make through oxide treatment with Preparation of Metallic Strontium; Second reactant that contains aluminium (Al) can be aluminium sesquioxide (Al 2O 3); The 3rd reactant that contains chlorine (Cl) can be water strontium chloride (SrCl 26H 2O) or anhydrous strontium chloride (SrCl 2); And the 4th reactant that contains europium (Eu) can be selected from europiumsesquioxide (Eu 2O 3), moisture europium nitrate (Eu (NO 3) 3.5H 2O), anhydrous nitric acid europium (Eu (NO 3) 3) or europium carbonate (EuCO 3), perhaps prepare through oxide treatment with the metal europium.
Fig. 1 is the embodiment of the invention (Sr 3-xEu x) (Al 2O 5) Cl 2The X-ray diffractogram of (x=0.05,0.1,0.15,0.2) sample, the sample and the standard alkaline earth halogen aluminate compound (Sr that make of the present invention as shown in Figure 1 3(Al 2O 6) Cl 2, ICSD No.:68365) and the comparison of X light powder diffraction collection of illustrative plates, disclosed as can be known metal halogen aluminate class compound fluor is the structure of rhombic system (orthorhombic).
Fig. 2 is the embodiment of the invention (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2Fluorescent material (Y with another jaundice light commercialization 3A 5O 12: Ce 3+, hereinafter to be referred as YAG:Ce) UV-light-excited by visible light source collection of illustrative plates; Please refer to Fig. 2, disclosed (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2Fluorescent powder is fit to UV-light and excites, and above-mentioned excitaton source wavelength can all can be excited to the near-ultraviolet light wave band from UV-light between 200 to 400nm, and particularly 360nm to 410nm excites the preferable characteristic that is excited between the wave band.
Fig. 3 is embodiments of the invention (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2With the photoemissive spectrogram of YAG:Ce sample, wherein excitaton source is the UV-light of wavelength 370nm.Please refer to Fig. 3, (Sr 2.85Eu 0.15) (Al 2O 5) Cl 2The maximum radiation of fluorescent powder wavelength is 586nm, for emission light is the fluorescent material of gold-tinted; Its maximum radiation wavelength of the fluorescent material (YAG:Ce) of another jaundice light is 544nm.Since the wavelength of transmitted light of the metal halogen aluminate compound fluorescent powder that the present invention discloses compared to the YAG:Ce fluorescent powder near red spectral band, so gold-tinted and the blue light of utilizing metal halogen aluminate compound fluorescent powder to be launched, can be mixed into the lower warm white of colour temperature, rather than utilize YAG:Ce fluorescent material to mix the higher cold white light of colour temperature.Moreover, also can find that by Fig. 3 YAG:Ce fluorescent material halfwidth is about 100nm, and the fluorescent material that this disclosed, (Sr 3-xEu x) (Al 2O 5) Cl 2, can reach 120nm, therefore use this fluorescent material can use YAG:Ce blended white light to have better color developing.
Fig. 8 is the tristimulus coordinates figure of International Commission on Illumination in 1931 (Commission International de l ' Eclairage is called for short CIE) of disclosed metal halogen aluminate compound fluorescent powder; Please refer to Fig. 8 about the disclosed further optical property of metal halogen aluminate compound fluorescent powder, a point is the position of Fig. 3 YAG:Ce sample tristimulus coordinates among the figure, and its coordinate figure is (0.4792,0.4861); To select be Fig. 3 metal halogen aluminate class compound fluorescent powder (Sr to b among the figure 2.85Eu 0.15) (Al 2O 5) Cl 2The position of tristimulus coordinates, its coordinate figure are (0.4087,0.5668); And triangle symbol place representative is theoretical white light position, and its coordinate figure is (0.31,0.32).Position on the CIE coordinate diagram, compared to the predominant wavelength of YAG:Ce fluorescent powder, the predominant wavelength of the fluorescent material that makes in the embodiment of the invention (dominant wavelength) is 578nm, near ruddiness.
The disclosed metal halogen aluminate compound fluorescent powder that consists of more is widely used on all kinds of sealed cells, such as solid state illumination devices such as photodiode, luminescence of plasma elements.Fig. 4 A and Fig. 4 B are the embodiment that disclosed metal halogen aluminate compound fluorescent powder is applied to sealed cell.Shown in Fig. 4 A, sealed cell 400 comprises substrate 40; Luminous lamination 42 is positioned on the substrate 40; At least one electrode 44 is positioned on the luminous lamination; And wavelength conversion layer 46 is covered on the luminous lamination 42; Emitting light into of wherein luminous lamination 420 comprises UV-light or the near-ultraviolet light of wavelength between 200nm to 420nm less, and comprise disclosed metal halogen aluminate compound fluorescent powder 460 in the wavelength conversion layer 46 at least, by the fluorescent powder 460 of the metal halogen aluminate compound in the wavelength conversion layer 46, the UV-light or the near-ultraviolet light that luminous lamination 420 can be sent are converted to the gold-tinted that wavelength is 550nm to 650nm.In addition, sealed cell 400 also can be shown in Fig. 4 B, the fluorescent powder 462 that in wavelength conversion layer 46, adds UV-light or near ultraviolet excitation blue light, make UV-light that luminous lamination sends or near-ultraviolet light can be respectively absorb and be converted to gold-tinted and blue light by the fluorescent powder 462 of metal halogen aluminate compound gold-tinted fluorescent powder 460 and UV-light or near ultraviolet excitation blue light, and then mix the acquisition white light, wherein the material of the fluorescent powder of ultraviolet excitation generation blue light can be selected from Si 3MgSi 2O 8: Eu, BaMgAl 10O 17: Eu, (SrBaCa) 5(PO 4) 3Cl:Eu and Sr 4Al 14O 25: the groups that material constituted such as Eu.
Fig. 5 A and Fig. 5 B are another embodiment that disclosed metal halogen aluminate compound fluorescent powder is applied to sealed cell.Shown in Fig. 5 A, sealed cell 500 comprises printed circuit board (PCB) 50, wherein has at least one circuit pattern 52 on this printed circuit board (PCB) 50; Light-emitting diode chip for backlight unit 54 is positioned on the substrate 50, and wherein emitting light into of this light-emitting diode chip for backlight unit 54 comprises UV-light or the near-ultraviolet light of wavelength between 200nm to 420nm less; At least one metal wire 56 is used so that light-emitting diode chip for backlight unit 54 produces electric connection with circuit pattern 52; And transparent enclosure glue material 58, be positioned on the printed circuit board (PCB) 50, covering luminousing diode chip 54, partial circuit pattern 52 and metal wire 56 wherein comprise disclosed metal halogen aluminate compound fluorescent powder 580 at least and intersperse among wherein in the transparent enclosure glue material 58; In present embodiment, the emission light of light-emitting diode chip for backlight unit 54 will excite the metal halogen aluminate compound fluorescent powder 580 in the transparent enclosure glue material 58, and be converted into the gold-tinted of wavelength between 550nm to 650nm.In addition, sealed cell 500 more can be shown in Fig. 5 B, the fluorescent powder 582 that more can comprise UV-light or near ultraviolet excitation blue light in the transparent enclosure glue material 58, make UV-light that light-emitting diode chip for backlight unit 54 sent or near-ultraviolet light be absorbed by the fluorescent powder 582 of metal halogen aluminate compound fluorescent powder 580 and UV-light or near ultraviolet excitation blue light respectively and be converted to gold-tinted and blue light, and then mix the acquisition white light, wherein the material of the fluorescent powder of ultraviolet excitation generation blue light can be selected from Si 3MgSi 2O 8: Eu, BaMgAl 10O 17: Eu, (SrBaCa) 5(PO 4) 3Cl:Eu and Sr 4Al 14O 25: the groups that material constituted such as Eu.。
Fig. 6 display backlight modular device.Wherein back light module device 600 comprises: the light supply apparatus 62 that is made of the sealed cell 60 of above-mentioned any embodiment; Optical devices 64 place going out on the light path of light supply apparatus 62, are responsible for light is done suitable processing back bright dipping; And power system 66, provide above-mentioned light supply apparatus 62 required power supply.
Fig. 7 display illumination device.Above-mentioned means of illumination can be car light, street lamp, torch light, street lamp, pilot lamp or the like.Wherein means of illumination 700 comprises: light supply apparatus 70 is made of the sealed cell 72 of above-mentioned any embodiment; Power system 74 provides light supply apparatus 70 required power supply; And controlling elements 76 is with the power supply of control power system 74 input light supply apparatuses 70.
Above-described embodiment only is for technological thought of the present invention and characteristics are described, its purpose makes the personage who has the knack of this skill can understand content of the present invention and is implementing according to this, when can not with qualification claim of the present invention, promptly the equalization of doing according to disclosed spirit generally changes or modifies, and must be encompassed in the claim of the present invention.

Claims (18)

1. Wavelength conversion substance, it consists of the fluorescent powder of metal halogen aluminate compound.
2. Wavelength conversion substance as claimed in claim 1, this metal halogen aluminate fluorescent powder body chemical general formula is M W-pAl yO zX q: R pWherein w, y, z, q＞0,0.005＜p＜0.5, and satisfy q=2w+3y-2z, and being at least a element, M is selected from the group that Be, Mg, Ca, Sr, Ba and Zn constitute, X is that at least a element is selected from the group that F, Cl, Br and I constitute, and R is selected from the material of transition element for one or more, and comprises a kind of material that is selected from lanthanon at least.
3. Wavelength conversion substance as claimed in claim 1, wherein the excitaton source of this metal halogen aluminate fluorescent powder body is UV-light or the near-ultraviolet light of wavelength between 300nm to 450nm.
4. Wavelength conversion substance as claimed in claim 1, wherein the emission of this metal halogen aluminate fluorescent powder body only wavelength between the gold-tinted of 550nm to 650nm.
5. sealed cell comprises at least:
Luminous lamination;
Wavelength conversion layer is positioned on this luminous lamination; And
At least one electrode is positioned on this luminous lamination, and wherein the material of this wavelength conversion layer comprises metal halogen aluminate fluorescent powder body.
6. sealed cell as claimed in claim 5, wherein this luminous lamination comprises at least:
First conductive-type semiconductor layer;
Luminescent layer is positioned on this first conductive-type semiconductor layer; And
Second conductive-type semiconductor layer is positioned on this luminescent layer.
7. sealed cell as claimed in claim 5, wherein the light that this luminescent layer sent is that wavelength is between UV-light between 300nm to 450nm or near-ultraviolet light.
8. sealed cell as claimed in claim 5, the chemical general formula of this metal halogen aluminate fluorescent powder body is M W-pAl yO zX q: R pWherein w, y, z, q＞0,0.005＜p＜0.5, and satisfy q=2w+3y-2z, and being at least a element, M is selected from the group that Be, Mg, Ca, Sr, Ba and Zn constitute, X is that at least a element is selected from the group that F, Cl, Br and I constitute, and R is selected from the material of transition element for one or more, and comprises a kind of material that is selected from lanthanon at least.
9. sealed cell as claimed in claim 8, wherein the excitaton source of this metal halogen aluminate fluorescent powder body is UV-light or the near-ultraviolet light of wavelength between 300nm to 450nm, and launches only wavelength between the gold-tinted of 550nm to 650nm.
10. sealed cell as claimed in claim 5, wherein this wavelength conversion layer more comprises the fluorescent powder of UV-light or near ultraviolet excitation blue light.
11. sealed cell as claimed in claim 10, wherein the fluorescent powder material of this UV-light or near ultraviolet excitation generation blue light is to be selected from Si 3MgSi 2O 8: Eu, BaMgAl 10O 17: Eu, (SrBaCa) 5(PO 4) 3Cl:Eu and Sr 4Al 14O 25: the groups that material constituted such as Eu.
12. a sealed cell comprises at least:
Printed circuit board (PCB) comprises substrate and the circuit pattern that is positioned on this substrate;
Light-emitting diode chip for backlight unit is positioned on the printed circuit board (PCB);
Transparent enclosure glue material is positioned on this printed circuit board (PCB), and covers this light-emitting diode chip for backlight unit; And
A plurality of Wavelength conversion substances intersperse among in this transparent enclosure glue material, and wherein this Wavelength conversion substance comprises metal halogen aluminate fluorescent powder body at least.
13. sealed cell as claimed in claim 12 more comprises at least one metal wire, in order to electrically connect this circuit pattern and this light-emitting diode chip for backlight unit.
14. luminous element as claimed in claim 12, wherein the light that this light-emitting diode chip for backlight unit sent is that wavelength is between UV-light between 300nm to 450nm or near-ultraviolet light.
15. luminous element as claimed in claim 12, wherein the chemical general formula of this metal halogen aluminate fluorescent powder body is M W-pAl yO zX q: R pWherein w, y, z, q＞0,0.005＜p＜0.5, and satisfy q=2w+3y-2z, and being at least a element, M is selected from the group that Be, Mg, Ca, Sr, Ba and Zn constitute, X is that at least a element is selected from the group that F, Cl, Br and I constitute, and R is selected from the material of transition element for one or more, and comprises a kind of material that is selected from lanthanon at least.
16. sealed cell as claimed in claim 15, wherein the excitaton source of this metal halogen aluminate fluorescent powder body is UV-light or the near-ultraviolet light of wavelength between 300nm to 450nm, and launches only wavelength between the gold-tinted of 550nm to 650nm.
17. sealed cell as claimed in claim 16, wherein this Wavelength conversion substance more can comprise the fluorescent powder of UV-light or near ultraviolet excitation blue light.
18. sealed cell as claimed in claim 17, wherein the fluorescent powder of this UV-light or near ultraviolet excitation generation blue light is to be selected from Si 3MgSi 2O 8: Eu, BaMgAl 10O 17: Eu, (SrBaCa) 5(PO 4) 3Cl:Eu and Sr 4Al 14O 25: the groups that material constituted such as Eu.
CN 200810100503 2008-05-20 2008-05-20 Wavelength conversion substance and application thereof Active CN101586030B (en)

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CN102458019A (en) * 2010-10-26 2012-05-16 财团法人工业技术研究院 Photochromic modulation method, light emitting diode light source module and packaging structure thereof
CN105322096A (en) * 2014-07-30 2016-02-10 财团法人工业技术研究院 Organic light emitting element

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JP3704057B2 (en) * 2000-07-07 2005-10-05 ザ ウエステイム コーポレイション Phosphor thin film and method for manufacturing the same, and EL panel
CN100568554C (en) * 2006-08-16 2009-12-09 晶元光电股份有限公司 Light-emitting diode assembly and luminescence chip
CN101140967B (en) * 2006-09-08 2010-05-19 晶元光电股份有限公司 High efficient phosphor conversion light emitter and its making process

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Publication number Priority date Publication date Assignee Title
CN102458019A (en) * 2010-10-26 2012-05-16 财团法人工业技术研究院 Photochromic modulation method, light emitting diode light source module and packaging structure thereof
CN102458019B (en) * 2010-10-26 2014-01-22 财团法人工业技术研究院 Light color modulation method and light emitting diode light source module
CN105322096A (en) * 2014-07-30 2016-02-10 财团法人工业技术研究院 Organic light emitting element

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