WO2018145288A1 - Luminescent material composition and light emitting device - Google Patents

Luminescent material composition and light emitting device Download PDF

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Publication number
WO2018145288A1
WO2018145288A1 PCT/CN2017/073175 CN2017073175W WO2018145288A1 WO 2018145288 A1 WO2018145288 A1 WO 2018145288A1 CN 2017073175 W CN2017073175 W CN 2017073175W WO 2018145288 A1 WO2018145288 A1 WO 2018145288A1
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luminescent material
substituted
light
formula
mgal
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PCT/CN2017/073175
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French (fr)
Chinese (zh)
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刘元红
刘荣辉
邵冷冷
马小乐
高慰
陈磊
周小芳
张霞
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有研稀土新材料股份有限公司
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Priority to PCT/CN2017/073175 priority Critical patent/WO2018145288A1/en
Publication of WO2018145288A1 publication Critical patent/WO2018145288A1/en

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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
    • 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
    • C09K11/62—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing gallium, indium or thallium
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof

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  • the present invention relates to the field of optical materials, and in particular to a luminescent material composition and a light-emitting device.
  • liquid crystal display (LCD) technology has been rapidly developed, and it has been widely used in mobile phones, notebook computers, and high-definition televisions. Since the liquid crystal material itself does not emit light, the backlight becomes an indispensable key component of the liquid crystal display device.
  • the backlights of LCDs mainly include cold cathode lamps (CCFLs) and white light diodes (LEDs).
  • CCFLs cold cathode lamps
  • LEDs white light diodes
  • the white LED has many advantages such as good color reproduction, low power consumption and long life, so its market share in the field of liquid crystal display backlights is growing rapidly.
  • the "LED chip + phosphor” method is still the mainstream way of white LED production due to high technology maturity and relatively low cost.
  • white light is mainly produced by "blue LED chip + phosphor".
  • the commonly used schemes are three kinds of Y 3 Al 5 O 12 :Ce(YAG:Ce) scheme, ⁇ -SiAlON:Eu green phosphor (Low-end backlight uses silicate green powder) and nitride red phosphor combination scheme, ⁇ -SiAlON: Eu green phosphor and K 2 SiF 6 : Mn 4+ red phosphor.
  • the spectral peaks are relatively wide and the color purity is not good, and the display color gamut display range of the display is about 70% NTSC.
  • the second technical solution shows that the gamut range can only be increased to 80% NTSC.
  • the display color gamut range can only be increased to above 85% NTSC.
  • a main object of the present invention is to provide a luminescent material composition and a light-emitting device to solve the problem of low display gamut range of LED devices in the prior art.
  • a luminescent material composition comprising: a blue luminescent material selected from the group consisting of any one or more of the following formulas: Formula Ia 2-x LuHf 2 Al 3 O 12 :xCe, General Formula IICa 3-y Zr 2 SiGa 2 O 12 :yCe, Formula IIIBa 1-r MgAl 10 O 17 :rEu and Formula IVSr 5-m (PO 4 ) 3 Cl:mEu, wherein 0.002 ⁇ x ⁇ 0.2, 0.002 ⁇ y ⁇ 0.2, 0.002 ⁇ r ⁇ 0.2, 0.002 ⁇ m ⁇ 0.5, Ca in the formula I may be one of Ba, Sr, Mg or a plurality of substitutions, the Al element may be substituted by one or more of B, Ga, Si; Ca in the general formula II may be substituted by one or more of Ba, Sr, Mg, and the Al element may be B, Ga, One or more substitutions in Si, Si may be substituted by
  • the blue light-emitting material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu
  • the green light-emitting material is La 3-v Si 6 N 11 : Any one of vTb and Ba 1-st MgAl 10 O 17 : sEu, tMn.
  • the green light-emitting material is any one of Si 6-z Al z O z N 8-z :kEu and Ba 1-st MgAl 10 O 17 :sEu, tMn.
  • a light emitting device includes an LED chip and a light conversion portion, and the light conversion portion absorbs primary light emitted from the LED chip and converts it into a higher wavelength secondary light, and the light conversion portion
  • the luminescent material is contained, and the luminescent material is a luminescent material of any of the above.
  • the LED chip emits a peak wavelength range of 355 to 375 nm
  • the blue light-emitting material of the luminescent material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu.
  • the green luminescent material is any one of La 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 :sEu, tMn.
  • the red luminescent material in the luminescent material is a mixture of any one or more of 3.5MgO ⁇ 0.5MgF 2 ⁇ j(Ge 1-n Mn n )O 2 ⁇ iM 3 N 4 , wherein 0.05 ⁇ i ⁇ 0.067.
  • the LED chip emits a peak wavelength in the range of 360 to 370 nm, preferably 362 to 367 nm.
  • the LED chip emits a peak wavelength range of 380 to 420 nm
  • the green light-emitting material in the luminescent material is Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn Any one.
  • the red luminescent material in the luminescent material is a mixture of any one or more of 3.5MgO ⁇ 0.5MgF 2 ⁇ j(Ge 1-n Mn n )O 2 ⁇ iM 3 N 4 , wherein 0.05 ⁇ i ⁇ 0.067.
  • the LED chip emits a peak wavelength in the range of 390 to 410 nm, preferably 400 to 407 nm.
  • the luminescent material composition comprises a blue luminescent material having a stable structure, a green luminescent material having a relatively high radiant energy, and a red luminescent material having a longer wavelength, which can be expanded when applied to a white light LED light source.
  • the spectral range of the white light emitted by the wide white LED further broadens the display color gamut range when the white LED is used for the backlight of the display device, and improves the display effect of the liquid crystal display device.
  • FIG. 1 is a schematic cross-sectional structural view of a light-emitting device provided by the present invention
  • Figure 3 is a luminescence spectrum of the green luminescent material Ba 0.85 MgAl 10 O 17 : 0.05Eu, 0.1 Mn provided by the present invention
  • the inventors of the present invention analyzed the factors influencing the display color gamut of the LED device one by one, and found that the conventional green phosphor has lower luminescence energy, and the fluoride series red powder has a shorter emission peak, which leads to the display gamut range of the LED device. Lower, for this reason, the present application has performed various performance tests on the prior art green light-emitting materials and red light-emitting materials, and proposed a new combination of light-emitting materials and a light-emitting device using the same.
  • a luminescent material composition including a blue luminescent material, a green luminescent material, and a red luminescent material, and the blue luminescent material is represented by any one or more of the following formulas.
  • Si 6-z Al z O z N 8-z :kEu has the same crystal structure as Si 5 AlON 7 ; red luminescent material, the red luminescent material is of the formula VIII3.5MgO ⁇ 0.5MgF 2 ⁇ j (Ge 1 a mixture of any one or more of -n Mn n )O 2 ⁇ iM 3 N 4 wherein F may be substituted by one or more of Cl, Br, I, and Ge may be Ti and/or Substituting Si, Mg may be substituted by one or more of Ca, Sr, Ba, M element is selected from Si and/or Ti, 0.77 ⁇ j ⁇ 0.9 0, 0 ⁇ i ⁇ 0.067, 0.015 ⁇ n ⁇ 0.03.
  • the luminescent material composition includes a blue luminescent material having a stable structure, a green luminescent material having a relatively high radiant energy, and a red luminescent material having a longer wavelength, which can broaden the white light emitted by the white LED when applied to the white LED light source.
  • the spectral range further broadens the display color gamut range when the white LED is used for the backlight of the display device, and improves the display effect of the liquid crystal display device.
  • the blue light-emitting material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu
  • the green light-emitting material is La. 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 : sEu, tMn.
  • the luminescent material composition formed by the above blue luminescent material, green luminescent material and red luminescent material emits a wider spectrum of white light under the excitation of an LED chip emitting a peak wavelength range of 355 to 375 nm, and displays the LED display device. The expansion effect of the color gamut is more obvious.
  • the green luminescent material is any one of Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn .
  • the luminescent material composition formed by the above blue luminescent material, green luminescent material and red luminescent material emits a wider spectrum of white light under the excitation of an LED chip emitting a peak wavelength range of 380 to 420 nm, and displays the LED display device. The expansion effect of the color gamut is more obvious.
  • a light-emitting device in another exemplary embodiment of the present application, includes an LED chip 2 and a light conversion portion 3, and the light conversion portion 3 absorbs the primary light emitted by the LED chip 2, And converted into secondary light of a higher wavelength, the light conversion part contains a light-emitting material, and the light-emitting material is any one of the above-mentioned light-emitting materials.
  • the luminescent material composition includes a blue luminescent material having a stable structure, a green luminescent material having a relatively high luminescent energy, and a red luminescent material having a longer wavelength, which can broaden the spectral range of the emitted white light when applied to the illuminating device. Further, when the white LED is used for the backlight of the display device, the color gamut range is displayed, and the display effect of the liquid crystal display device is improved.
  • the LED chip 2 emits a peak wavelength range of 355-375 nm
  • the blue luminescent material in the luminescent material is Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 Any one of 3 Cl:mEu
  • the green luminescent material is any one of La 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 :sEu, tMn.
  • the luminescent material composition formed by the blue luminescent material, the green luminescent material and the red luminescent material emits a wider spectrum of white light, and the effect of expanding the display gamut of the LED display device is more obvious.
  • the red luminescent material in the luminescent material is any of 3.5MgO ⁇ 0.5MgF 2 ⁇ j(Ge 1-n Mn n )O 2 ⁇ iM 3 N 4 .
  • the LED chip 2 emits a peak wavelength range of 360 to 370 nm, more preferably 362 to 367 nm.
  • the LED chip 2 emits a peak wavelength range of 380 to 420 nm
  • the green light-emitting material of the luminescent material is Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn.
  • the luminescent material composition formed by the blue luminescent material, the green luminescent material and the red luminescent material emits a wider spectrum of white light, and the effect of expanding the display gamut of the LED display device is more obvious.
  • the red luminescent material in the luminescent material is any of 3.5MgO ⁇ 0.5MgF 2 ⁇ j(Ge 1-n Mn n )O 2 ⁇ iM 3 N 4 .
  • the present application includes a luminescent material composition of a blue luminescent material, a green luminescent material, and a red luminescent material, which can broaden the spectral range of white light emitted by the white LED when applied to a white LED light source, thereby widening
  • the white LED is used for a backlight of a display device, the color gamut range is displayed, and the display effect of the liquid crystal display device is improved.
  • the amount of each of the above-mentioned luminescent materials has no essential influence on the realization of the above effects.
  • the weight ratio of the blue luminescent material, the green luminescent material and the red luminescent material is (1 to 3): (2 to 6): (2 to 4).
  • the LED chip 2 emits a peak wavelength in the range of 390 to 410 nm, more preferably 400 to 407 nm.
  • the light-emitting device of the present application is not particularly limited as long as it has the above characteristics.
  • the sealant silica gel, epoxy resin, silicone resin, urea resin or the like can be used, but it is not limited thereto.
  • the light conversion unit may contain an additive such as SiO 2 , TiO 2 , ZrO 2 or Al 2 O 3 in addition to the phosphor and the sealant.
  • the blue light-emitting material, the green light-emitting material, and the red light-emitting material used in the light-emitting device of the present invention may be produced by a known appropriate method or may be directly obtained.
  • the LED chip 2 is a peak wavelength chip at 450 nm
  • the green light-emitting material in the light conversion portion 3 is Si 5.70 Al 0.30 O 0.30 N 7.70 : 0.05Eu 2+
  • the red luminescent material is K 2 SiF 6 : 0.01 Mn 4+ .
  • the green light-emitting material and the red light-emitting material were mixed and dispersed in a silica gel at a weight ratio of 25:75 to prepare a light conversion portion.
  • the light conversion portion is further assembled into an LED light emitting device.
  • the LED chip 2 is a peak wavelength chip at 365 nm
  • the blue light-emitting material in the light conversion portion 3 is Ba 0.85 MgAl 10 O 17 :0.15Eu
  • the green light-emitting material is Lu 2.94 Al 5 Si 12 :0.06Ce, red light-emitting material.
  • Ca 0.99 AlSiN 3 : 0.01 Eu was used.
  • the blue light-emitting material, the green light-emitting material and the red light-emitting material were mixed and dispersed in a silica gel at a weight ratio of 25:40:35 (the weight ratio of the silica gel to the phosphor was 88:12) to prepare a light conversion portion.
  • the light conversion portion is further assembled into an LED light emitting device.
  • the white LED light-emitting device of the present invention was prepared in the manner as shown in FIG.
  • the LED chip 2 is a peak wavelength chip at 365 nm
  • the blue light in the light conversion portion 3 is Ba 0.85 MgAl 10 O 17 : 0.15Eu
  • the green light emitting material is La 2.84 Si 6 N 11 : 0.16 Tb, red light emitting material.
  • 3.5 MgO ⁇ 0.5 MgF 2 ⁇ 0.85 (Ge 0.9821 Mn 0.0179 )O 2 ⁇ 0.15/3Si 3 N 4 was used .
  • the blue light-emitting material, the green light-emitting material and the red light-emitting material were mixed and dispersed in a silica gel at a weight ratio of 30:40:30 (the weight ratio of the silica gel to the phosphor was 90:10) to prepare a light conversion portion.
  • the light conversion portion is further assembled into an LED light emitting device.
  • the white LED light-emitting device of the present invention was prepared in the manner as shown in FIG.
  • the LED chip 2 is a peak wavelength chip at 405 nm
  • the blue light-emitting material in the light conversion portion 3 is Sr 4.8 (PO 4 ) 3 Cl: 0.2Eu
  • the green light-emitting material is Ba 0.5 MgAl 10 O 17 : 0.07Eu, 0.43.
  • Mn red luminescent material is 3.5MgO ⁇ 0.5MgF 2 ⁇ 0.8(Ge 0.981 Mn 0.019 )O 2 ⁇ 0.2/3Si 3 N 4 .
  • the blue light-emitting material, the green light-emitting material and the red light-emitting material are mixed and dispersed in an epoxy resin at a weight ratio of 25:45:30 (the weight ratio of the epoxy resin to the phosphor is 92:8) to prepare a light conversion portion. .
  • the light conversion portion is further assembled into an LED light emitting device.
  • the preparation process of the embodiment 3-12 is basically the same as that of the embodiment 2, and different LED chips and luminescent materials are used, as shown in Table 1.
  • the light effect and color coordinates were detected by HAAS-2000 high-precision fast spectrum analyzer.
  • the color gamut was calculated by color coordinate and color gamut calculation formula.
  • the test results are shown in Table 2.
  • the display color gamut of the illuminating device is remarkably improved while maintaining high luminous efficiency.
  • the luminescent material composition is combined with the LED chip having an appropriate emission peak wavelength, the display color gamut can be further broadened, and the light effect can be improved.
  • the luminescent material composition includes a blue luminescent material having a stable structure, a green luminescent material having a relatively high radiant energy, and a red luminescent material having a longer wavelength, which can broaden the white light emitted by the white LED when applied to the white LED light source.
  • the spectral range further broadens the display color gamut range when the white LED is used for the backlight of the display device, and improves the display effect of the liquid crystal display device.

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Abstract

A luminescent material composition and a light emitting device. The luminescent material composition comprises a blue luminescent material, a green luminescent material, and a red luminescent material; the blue luminescent material is selected from any one or more of the following general formulae: Ca2-xLuHf2Al3O12:xCe, Ca3-yZr SiGa2O12:yCe, Ba1-rMgAl10O17:rEu, and Sr5 - m(PO4)3Cl:mEu; the green luminescent material is selected from any one or more of the following general formulae: Si6-zAl zOzN8-z:kEu, Ba 1-s-tMgAl10O17:sEu,tMn, and La3-vSi6N11:vTb; and the red luminescent material is formed of any one or more of 3.5Mg•O0.5MgF2•j(Ge1-nMnn)O2•iM3N4. The composition broadens display color gamut.

Description

发光材料组合物以及发光装置Luminescent material composition and illuminating device 技术领域Technical field
本发明涉及光学材料领域，具体而言，涉及一种发光材料组合物以及发光装置。The present invention relates to the field of optical materials, and in particular to a luminescent material composition and a light-emitting device.
背景技术Background technique
近年来，液晶显示(LCD)技术得到迅速发展，其在手机、笔记本电脑、高清电视领域均得到了广泛应用。由于液晶材料本身不发光，因此背光源就成为液晶显示器件不可缺少的关键元件。目前，LCD的背光源主要有冷阴极灯(CCFL)和白光二极管(LED)两种方式。而白光LED具有色彩还原性好、功耗低、长寿命等众多优势，因此其在液晶显示背光源领域的市场份额迅速增长。In recent years, liquid crystal display (LCD) technology has been rapidly developed, and it has been widely used in mobile phones, notebook computers, and high-definition televisions. Since the liquid crystal material itself does not emit light, the backlight becomes an indispensable key component of the liquid crystal display device. At present, the backlights of LCDs mainly include cold cathode lamps (CCFLs) and white light diodes (LEDs). The white LED has many advantages such as good color reproduction, low power consumption and long life, so its market share in the field of liquid crystal display backlights is growing rapidly.
目前“LED芯片+荧光粉”的方式因技术成熟度高、成本相对较低，仍是白光LED产生的主流方式。对于液晶显示LED背光而言，主要采用“蓝光LED芯片+荧光粉”产生白光，普遍使用的方案有三种Y3Al5O12:Ce(YAG:Ce)方案、β-SiAlON:Eu绿色荧光粉(低端背光源采用硅酸盐绿粉)和氮化物红色荧光粉组合方案、β-SiAlON:Eu绿色荧光粉和K2SiF6:Mn4+红色荧光粉。第一种方案光谱波峰比较宽，色纯度不佳，其所制作的显示器色域显示范围约70％NTSC。第二种技术方案显示色域范围仅可提高到80％NTSC。第三种技术方案，由于氟化物红粉色纯度较高，显示色域范围仅可提高到85％NTSC以上。At present, the "LED chip + phosphor" method is still the mainstream way of white LED production due to high technology maturity and relatively low cost. For liquid crystal display LED backlights, white light is mainly produced by "blue LED chip + phosphor". The commonly used schemes are three kinds of Y 3 Al 5 O 12 :Ce(YAG:Ce) scheme, β-SiAlON:Eu green phosphor (Low-end backlight uses silicate green powder) and nitride red phosphor combination scheme, β-SiAlON: Eu green phosphor and K 2 SiF 6 : Mn 4+ red phosphor. In the first scheme, the spectral peaks are relatively wide and the color purity is not good, and the display color gamut display range of the display is about 70% NTSC. The second technical solution shows that the gamut range can only be increased to 80% NTSC. In the third technical solution, since the purity of the fluoride red and pink is high, the display color gamut range can only be increased to above 85% NTSC.
然而，现有技术所制备的LED器件的显示色域范围仍较低。However, the display color gamut range of the LED devices prepared in the prior art is still low.
发明内容Summary of the invention
本发明的主要目的在于提供一种发光材料组合物以及发光装置，以解决现有技术中的LED器件的显示色域范围较低的问题。A main object of the present invention is to provide a luminescent material composition and a light-emitting device to solve the problem of low display gamut range of LED devices in the prior art.
为了实现上述目的，根据本发明的一个方面，提供了一种发光材料组合物，包括：蓝色发光材料，蓝色发光材料选自以下通式表示的任一种或多种形成的混合物：通式ⅠCa2-xLuHf2Al3O12:xCe、通式ⅡCa3-yZr2SiGa2O12:yCe、通式ⅢBa1-rMgAl10O17:rEu和通式ⅣSr5-m(PO4)3Cl:mEu，其中，0.002≤x≤0.2，0.002≤y≤0.2，0.002≤r≤0.2，0.002≤m≤0.5，通式Ⅰ中的Ca可被Ba、Sr、Mg中的一个或多个取代，Al元素可被B、Ga、Si中的一个或多个取代；通式Ⅱ中的Ca可被Ba、Sr、Mg中的一个或多个取代，Al元素可被B、Ga、Si中的一个或多个取代，Si可被Al取代，Ce可被Eu、Dy、Tb中的一个或多个部分取代；通式Ⅲ中的Ba可被Ca和/或Sr取代，Eu可被Ce和/或Mn部分取代；通式Ⅳ中的Sr可被Ba、Ca、Mg中的一种或多种取代，Eu可被Ce和/或Mn部分取代；绿色发光材料，绿色发光材料选自以下通式表示的任一种或多种形成的混合物：通式ⅤSi6-zAlzOzN8-z:kEu、通式ⅥBa1-s-tMgAl10O17:sEu,tMn和通式ⅦLa3-vSi6N11:vTb中任意一种，其中，0.1≤z≤0.6，0.0001≤k≤0.1，0.001≤s≤0.2，0.01 ≤t≤0.6，0＜v≤0.5，通式Ⅴ中的Eu可被Ce和/或Mn部分取代；通式Ⅵ中的Ba可被Ca和/或Sr取代，Eu可被Ce部分取代；通式Ⅶ中的La可被Y、Lu、Gd中的一种或多种取代，Si可被C、Ge、Ti中的一种或多种取代，N可被O部分取代，Tb可被Ce和/或Eu取代，且Si6-zAlzOzN8-z:kEu具有与Si5AlON7相同的晶体结构；红色发光材料，红色发光材料为通式Ⅷ3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，F可被Cl、Br、I中的一种或多种取代，Ge可被Ti和/或Si取代，Mg可被Ca、Sr、Ba中的一种或多种取代，M元素选自Si和/或Ti，0.77≤j<0.90，0≤i≤0.067，0.015≤n≤0.03。In order to achieve the above object, according to an aspect of the invention, there is provided a luminescent material composition comprising: a blue luminescent material selected from the group consisting of any one or more of the following formulas: Formula Ia 2-x LuHf 2 Al 3 O 12 :xCe, General Formula IICa 3-y Zr 2 SiGa 2 O 12 :yCe, Formula IIIBa 1-r MgAl 10 O 17 :rEu and Formula IVSr 5-m (PO 4 ) 3 Cl:mEu, wherein 0.002≤x≤0.2, 0.002≤y≤0.2, 0.002≤r≤0.2, 0.002≤m≤0.5, Ca in the formula I may be one of Ba, Sr, Mg or a plurality of substitutions, the Al element may be substituted by one or more of B, Ga, Si; Ca in the general formula II may be substituted by one or more of Ba, Sr, Mg, and the Al element may be B, Ga, One or more substitutions in Si, Si may be substituted by Al, Ce may be substituted by one or more moieties of Eu, Dy, Tb; Ba in Formula III may be substituted by Ca and/or Sr, and Eu may be Ce and / or Mn partial substitution; Sr in Formula IV may be substituted by one or more of Ba, Ca, Mg, Eu may be partially substituted by Ce and / or Mn; green luminescent material, green luminescent material is selected from The following formula represents Any one or more of a mixture formed: Formula ⅤSi 6-z Al z O z N 8-z: kEu, Formula ⅥBa 1-st MgAl 10 O 17 : sEu, tMn general formula ⅦLa 3-v Si 6 Any one of N 11 :vTb, wherein 0.1≤z≤0.6, 0.0001≤k≤0.1, 0.001≤s≤0.2, 0.01 ≤t≤0.6, 0<v≤0.5, Eu in the general formula V may be Ce And/or Mn partial substitution; Ba in formula VI may be substituted by Ca and/or Sr, Eu may be substituted by Ce moiety; La in formula VII may be substituted by one or more of Y, Lu, Gd , Si may be substituted by one or more of C, Ge, Ti, N may be substituted by O moiety, Tb may be substituted by Ce and/or Eu, and Si 6-z Al z O z N 8-z : kEu Has the same crystal structure as Si 5 AlON 7 ; red luminescent material, red luminescent material is any one of general formula VIII3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 Or a plurality of formed mixtures, wherein F may be substituted by one or more of Cl, Br, I, Ge may be substituted by Ti and/or Si, and Mg may be one or more of Ca, Sr, Ba Substituting, the M element is selected from the group consisting of Si and/or Ti, 0.77 ≤ j < 0.90, 0 ≤ i ≤ 0.067, and 0.015 ≤ n ≤ 0.03.
进一步地，上述蓝色发光材料为Ba1-rMgAl10O17:rEu和Sr5-m(PO4)3Cl:mEu中任意一种，绿色发光材料为La3-vSi6N11:vTb和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。Further, the blue light-emitting material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu, and the green light-emitting material is La 3-v Si 6 N 11 : Any one of vTb and Ba 1-st MgAl 10 O 17 : sEu, tMn.
进一步地，上述通式Ⅷ中0.05≤i≤0.067。Further, in the above formula VIII, 0.05 ≤ i ≤ 0.067.
进一步地，上述绿色发光材料为Si6-zAlzOzN8-z:kEu和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。Further, the green light-emitting material is any one of Si 6-z Al z O z N 8-z :kEu and Ba 1-st MgAl 10 O 17 :sEu, tMn.
进一步地，上述通式Ⅷ中0.05≤i≤0.067。Further, in the above formula VIII, 0.05 ≤ i ≤ 0.067.
根据本发明的另一方面，提供了一种发光装置，该发光装置包括LED芯片和光转化部，光转化部吸收LED芯片发出的一次光，并转换为更高波长的二次光，光转化部含有发光材料，发光材料为上述任一种的发光材料。According to another aspect of the present invention, a light emitting device includes an LED chip and a light conversion portion, and the light conversion portion absorbs primary light emitted from the LED chip and converts it into a higher wavelength secondary light, and the light conversion portion The luminescent material is contained, and the luminescent material is a luminescent material of any of the above.
进一步地，上述LED芯片发射峰值波长范围355～375nm，发光材料中蓝色发光材料为Ba1-rMgAl10O17:rEu和Sr5-m(PO4)3Cl:mEu中任意一种，绿色发光材料为La3-vSi6N11:vTb和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。Further, the LED chip emits a peak wavelength range of 355 to 375 nm, and the blue light-emitting material of the luminescent material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu. The green luminescent material is any one of La 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 :sEu, tMn.
进一步地，上述发光材料中红色发光材料为3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，0.05≤i≤0.067。Further, the red luminescent material in the luminescent material is a mixture of any one or more of 3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 , wherein 0.05≤ i ≤ 0.067.
进一步地，上述LED芯片发射峰值波长范围360～370nm，优选为362～367nm。Further, the LED chip emits a peak wavelength in the range of 360 to 370 nm, preferably 362 to 367 nm.
进一步地，上述LED芯片发射峰值波长范围380～420nm，发光材料中绿色发光材料为Si6-zAlzOzN8-z:kEu和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。Further, the LED chip emits a peak wavelength range of 380 to 420 nm, and the green light-emitting material in the luminescent material is Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn Any one.
进一步地，上述发光材料中红色发光材料为3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，0.05≤i≤0.067。Further, the red luminescent material in the luminescent material is a mixture of any one or more of 3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 , wherein 0.05≤ i ≤ 0.067.
进一步地，上述LED芯片发射峰值波长范围390～410nm，优选为400～407nm。Further, the LED chip emits a peak wavelength in the range of 390 to 410 nm, preferably 400 to 407 nm.
应用本发明的技术方案，该发光材料组合物包括具有稳定结构的蓝色发光材料、发光能量较高的绿色发光材料和较长波长的红色发光材料，在应用至白光LED光源中时，能够扩宽白光LED所发出白光的光谱范围，进而扩宽将该白光LED用于显示装置的背光源时显示色域范围，并提高了液晶显示装置的显示效果。 According to the technical solution of the present invention, the luminescent material composition comprises a blue luminescent material having a stable structure, a green luminescent material having a relatively high radiant energy, and a red luminescent material having a longer wavelength, which can be expanded when applied to a white light LED light source. The spectral range of the white light emitted by the wide white LED further broadens the display color gamut range when the white LED is used for the backlight of the display device, and improves the display effect of the liquid crystal display device.
附图说明DRAWINGS
构成本申请的一部分的说明书附图用来提供对本发明的进一步理解，本发明的示意性实施例及其说明用于解释本发明，并不构成对本发明的不当限定。在附图中：The accompanying drawings, which are incorporated in the claims of the claims In the drawing:
图1本发明提供的发光装置的横截面结构示意图；1 is a schematic cross-sectional structural view of a light-emitting device provided by the present invention;
图2用于本发明提供的蓝色发光材料Sr4.8(PO4)3Cl:0.2Eu的发光光谱图；2 is a luminescence spectrum of the blue light-emitting material Sr 4.8 (PO 4 ) 3 Cl:0.2Eu provided by the present invention;
图3用于本发明提供的绿色发光材料Ba0.85MgAl10O17:0.05Eu,0.1Mn的发光光谱图；以及Figure 3 is a luminescence spectrum of the green luminescent material Ba 0.85 MgAl 10 O 17 : 0.05Eu, 0.1 Mn provided by the present invention;
图4用于本发明提供的红色发光材料3.5MgO·0.5MgF2·0.85(Ge0.9821Mn0.0179)O2·0.15/3Si3N4的发光光谱图。 4 is a luminescence spectrum of a red luminescent material 3.5MgO· 0.5MgF 2 ·0.85(Ge 0.9821 Mn 0.0179 )O 2 ·0.15/3Si 3 N 4 provided by the present invention.
其中，上述附图包括以下附图标记：Wherein, the above figures include the following reference numerals:
2、LED芯片；3、光转化部。2, LED chip; 3, light conversion department.
具体实施方式detailed description
需要说明的是，在不冲突的情况下，本申请中的实施例及实施例中的特征可以相互组合。下面将参考附图并结合实施例来详细说明本发明。It should be noted that the embodiments in the present application and the features in the embodiments may be combined with each other without conflict. The invention will be described in detail below with reference to the drawings in conjunction with the embodiments.
本申请发明人对导致LED器件的显示色域的影响因素进行了逐一分析之后，发现常规的绿色荧光粉发光能量较低，氟化物系列红粉发射峰较短，会导致LED器件的显示色域范围较低，针对这一原因，本申请对现有技术的绿色发光材料和红色发光材料进行了各项性能测试，并提出来一种新的发光材料的组合形式以及应用其的发光装置。The inventors of the present invention analyzed the factors influencing the display color gamut of the LED device one by one, and found that the conventional green phosphor has lower luminescence energy, and the fluoride series red powder has a shorter emission peak, which leads to the display gamut range of the LED device. Lower, for this reason, the present application has performed various performance tests on the prior art green light-emitting materials and red light-emitting materials, and proposed a new combination of light-emitting materials and a light-emitting device using the same.
在本申请一种典型的实施方式中，提供了一种发光材料组合物，包括蓝色发光材料、绿色发光材料和红色发光材料，蓝色发光材料自以下通式表示的任一种或多种形成的混合物：通式ⅠCa2-xLuHf2Al3O12:xCe、通式ⅡCa3-yZr2SiGa2O12:yCe、通式ⅢBa1-rMgAl10O17:rEu和通式ⅣSr5-m(PO4)3Cl:mEu，其中，0.002≤x≤0.2，0.002≤y≤0.2，0.002≤r≤0.2，0.002≤m≤0.5，通式Ⅰ中的Ca可被Ba、Sr、Mg中的一个或多个取代，Al元素可被B、Ga、Si中的一个或多个取代；通式Ⅱ中的Ca可被Ba、Sr、Mg中的一个或多个取代，Al元素可被B、Ga、Si中的一个或多个取代，Si可被Al取代，Ce可被Eu、Dy、Tb中的一个或多个部分取代；所述通式Ⅲ中的Ba可被Ca和/或Sr取代，Eu可被Ce和/或Mn部分取代；所述通式Ⅳ中的Sr可被Ba、Ca、Mg中的一种或多种取代，Eu可被Ce和/或Mn部分取代；绿色发光材料，所述绿色发光材料选自以下通式表示的任一种或多种形成的混合物：通式ⅤSi6-zAlzOzN8-z:kEu、通式ⅥBa1-s-tMgAl10O17:sEu,tMn和通式ⅦLa3-vSi6N11:vTb中任意一种，其中，0.1≤z≤0.6，0.0001≤k≤0.1，0.001≤s≤0.2，0.01≤t≤0.6，0＜v≤0.5，所述通式Ⅴ中的Eu可被Ce和/或Mn部分取代；所述通式Ⅵ中的Ba可被Ca和/或Sr取代，Eu可被Ce部分取代；所述通式Ⅶ中的La可被Y、Lu、Gd中的一种或多种取代，Si可被C、Ge、Ti中的一种或多种取代，N可被O部分取代，Tb可被Ce和/或Eu取代，且Si6-zAlzOzN8-z:kEu具有与Si5AlON7相同的晶体结构； 红色发光材料，所述红色发光材料为通式Ⅷ3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，F可被Cl、Br、I中的一种或多种取代，Ge可被Ti和/或Si取代，Mg可被Ca、Sr、Ba中的一种或多种取代，M元素选自Si和/或Ti，0.77≤j<0.90，0≤i≤0.067，0.015≤n≤0.03。In an exemplary embodiment of the present application, a luminescent material composition is provided, including a blue luminescent material, a green luminescent material, and a red luminescent material, and the blue luminescent material is represented by any one or more of the following formulas. A mixture formed: general formula ICa 2-x LuHf 2 Al 3 O 12 :xCe, general formula IICa 3-y Zr 2 SiGa 2 O 12 :yCe, general formula IIIBa 1-r MgAl 10 O 17 :rEu and general formula IVSr 5-m (PO 4 ) 3 Cl:mEu, wherein 0.002≤x≤0.2, 0.002≤y≤0.2, 0.002≤r≤0.2, 0.002≤m≤0.5, Ca in the formula I can be Ba, Sr, One or more substitutions in Mg, Al may be substituted by one or more of B, Ga, Si; Ca in Formula II may be substituted by one or more of Ba, Sr, Mg, and Al may be Substituted by one or more of B, Ga, Si, Si may be substituted by Al, and Ce may be substituted by one or more moieties of Eu, Dy, Tb; Ba in the general formula III may be Ca and / Or Sr substituted, Eu may be partially substituted by Ce and / or Mn; Sr in the general formula IV may be substituted by one or more of Ba, Ca, Mg, Eu may be partially substituted by Ce and / or Mn; Green luminescent material, the green Forming a mixture of any one or more luminescent material is selected from the following general formula: Formula ⅤSi 6-z Al z O z N 8-z: kEu, Formula ⅥBa 1-st MgAl 10 O 17 : sEu, tMn And any one of the formula VIILa 3-v Si 6 N 11 :vTb, wherein 0.1≤z≤0.6, 0.0001≤k≤0.1, 0.001≤s≤0.2, 0.01≤t≤0.6, 0<v≤0.5, The Eu in the general formula V may be partially substituted by Ce and/or Mn; the Ba in the general formula VI may be substituted by Ca and/or Sr, and the Eu may be substituted by a Ce moiety; It may be substituted by one or more of Y, Lu, Gd, Si may be substituted by one or more of C, Ge, Ti, N may be substituted by O moiety, and Tb may be substituted by Ce and/or Eu. And Si 6-z Al z O z N 8-z :kEu has the same crystal structure as Si 5 AlON 7 ; red luminescent material, the red luminescent material is of the formula VIII3.5MgO·0.5MgF 2 ·j (Ge 1 a mixture of any one or more of -n Mn n )O 2 ·iM 3 N 4 wherein F may be substituted by one or more of Cl, Br, I, and Ge may be Ti and/or Substituting Si, Mg may be substituted by one or more of Ca, Sr, Ba, M element is selected from Si and/or Ti, 0.77≤j<0.9 0, 0 ≤ i ≤ 0.067, 0.015 ≤ n ≤ 0.03.
上述发光材料组合物包括具有稳定结构的蓝色发光材料、发光能量较高的绿色发光材料和较长波长的红色发光材料，在应用至白光LED光源中时，能够扩宽白光LED所发出白光的光谱范围，进而扩宽将该白光LED用于显示装置的背光源时显示色域范围，并提高了液晶显示装置的显示效果。The luminescent material composition includes a blue luminescent material having a stable structure, a green luminescent material having a relatively high radiant energy, and a red luminescent material having a longer wavelength, which can broaden the white light emitted by the white LED when applied to the white LED light source. The spectral range further broadens the display color gamut range when the white LED is used for the backlight of the display device, and improves the display effect of the liquid crystal display device.
在本申请一种优选的实施例中，上述蓝色发光材料为Ba1-rMgAl10O17:rEu和Sr5-m(PO4)3Cl:mEu中任意一种，绿色发光材料为La3-vSi6N11:vTb和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。由上述蓝色发光材料、绿色发光材料和红色发光材料形成的发光材料组合物，在发射峰值波长范围355～375nm的LED芯片的激发下，发出的白光光谱范围更广，对LED显示器件的显示色域的拓展效果较为明显。In a preferred embodiment of the present application, the blue light-emitting material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu, and the green light-emitting material is La. 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 : sEu, tMn. The luminescent material composition formed by the above blue luminescent material, green luminescent material and red luminescent material emits a wider spectrum of white light under the excitation of an LED chip emitting a peak wavelength range of 355 to 375 nm, and displays the LED display device. The expansion effect of the color gamut is more obvious.
为了进一步利用红色发光材料的波长的变化拓宽显示色域，优选上述3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中0.05≤i≤0.067。In order to further broaden the display color gamut by utilizing the change in the wavelength of the red luminescent material, it is preferable that 0.05 ≤ i ≤ 0.067 in the above 3.5 MgO·0.5 MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 .
在本申请另一种优选的实施例中，优选上述绿色发光材料为Si6-zAlzOzN8-z:kEu和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。由上述蓝色发光材料、绿色发光材料和红色发光材料形成的发光材料组合物，在发射峰值波长范围380～420nm的LED芯片的激发下，发出的白光光谱范围更广，对LED显示器件的显示色域的拓展效果较为明显。In another preferred embodiment of the present application, preferably, the green luminescent material is any one of Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn . The luminescent material composition formed by the above blue luminescent material, green luminescent material and red luminescent material emits a wider spectrum of white light under the excitation of an LED chip emitting a peak wavelength range of 380 to 420 nm, and displays the LED display device. The expansion effect of the color gamut is more obvious.
为了进一步利用红色发光材料的波长的变化拓宽显示色域，优选上述3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中0.05≤i≤0.067。In order to further broaden the display color gamut by utilizing the change in the wavelength of the red luminescent material, it is preferable that 0.05 ≤ i ≤ 0.067 in the above 3.5 MgO·0.5 MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 .
在本申请另一种典型的实施方式中，提供了一种发光装置，如图1所示，该发光装置包括LED芯片2和光转化部3，光转化部3吸收LED芯片2发出的一次光，并转换为更高波长的二次光，光转化部含有发光材料，发光材料为上述任一种发光材料。In another exemplary embodiment of the present application, a light-emitting device is provided. As shown in FIG. 1 , the light-emitting device includes an LED chip 2 and a light conversion portion 3, and the light conversion portion 3 absorbs the primary light emitted by the LED chip 2, And converted into secondary light of a higher wavelength, the light conversion part contains a light-emitting material, and the light-emitting material is any one of the above-mentioned light-emitting materials.
上述发光材料组合物包括具有稳定结构的蓝色发光材料、发光能量较高的绿色发光材料和较长波长的红色发光材料，在应用至发光装置中时，能够扩宽所发出白光的光谱范围，进而扩宽将该白光LED用于显示装置的背光源时显示色域范围，并提高了液晶显示装置的显示效果。The luminescent material composition includes a blue luminescent material having a stable structure, a green luminescent material having a relatively high luminescent energy, and a red luminescent material having a longer wavelength, which can broaden the spectral range of the emitted white light when applied to the illuminating device. Further, when the white LED is used for the backlight of the display device, the color gamut range is displayed, and the display effect of the liquid crystal display device is improved.
在本申请另一种优选的实施例中，上述LED芯片2发射峰值波长范围355～375nm，发光材料中蓝色发光材料为Ba1-rMgAl10O17:rEu和Sr5-m(PO4)3Cl:mEu中任意一种，绿色发光材料为La3-vSi6N11:vTb和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。在上述LED芯片的激发下，上述蓝色发光材料、绿色发光材料和红色发光材料形成的发光材料组合物发出的白光光谱范围更广，对LED显示器件的显示色域的拓展效果较为明显。 In another preferred embodiment of the present application, the LED chip 2 emits a peak wavelength range of 355-375 nm, and the blue luminescent material in the luminescent material is Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 Any one of 3 Cl:mEu, the green luminescent material is any one of La 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 :sEu, tMn. Under the excitation of the LED chip, the luminescent material composition formed by the blue luminescent material, the green luminescent material and the red luminescent material emits a wider spectrum of white light, and the effect of expanding the display gamut of the LED display device is more obvious.
为了进一步利用红色发光材料的波长的变化拓宽显示色域，优选上述发光材料中红色发光材料为3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，0.05≤i≤0.067。为了提高蓝光激发能量，以拓展显示色域，进一步优选上述LED芯片2发射峰值波长范围360～370nm，更优选为362～367nm。In order to further broaden the display color gamut by utilizing the change in the wavelength of the red luminescent material, it is preferable that the red luminescent material in the luminescent material is any of 3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 . One or more formed mixtures, wherein 0.05 ≤ i ≤ 0.067. In order to increase the blue light excitation energy to expand the display color gamut, it is further preferred that the LED chip 2 emits a peak wavelength range of 360 to 370 nm, more preferably 362 to 367 nm.
在本申请又一种优选的实施例中，上述LED芯片2发射峰值波长范围380～420nm，发光材料中绿色发光材料为Si6-zAlzOzN8-z:kEu和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。在上述LED芯片的激发下，上述蓝色发光材料、绿色发光材料和红色发光材料形成的发光材料组合物发出的白光光谱范围更广，对LED显示器件的显示色域的拓展效果较为明显。In still another preferred embodiment of the present application, the LED chip 2 emits a peak wavelength range of 380 to 420 nm, and the green light-emitting material of the luminescent material is Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn. Under the excitation of the LED chip, the luminescent material composition formed by the blue luminescent material, the green luminescent material and the red luminescent material emits a wider spectrum of white light, and the effect of expanding the display gamut of the LED display device is more obvious.
为了进一步利用红色发光材料的波长的变化拓宽显示色域，优选上述发光材料中红色发光材料为3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，0.05≤i≤0.067。In order to further broaden the display color gamut by utilizing the change in the wavelength of the red luminescent material, it is preferable that the red luminescent material in the luminescent material is any of 3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 . One or more formed mixtures, wherein 0.05 ≤ i ≤ 0.067.
如前所述，本申请包含蓝色发光材料、绿色发光材料和红色发光材料的发光材料组合物，在应用至白光LED光源中时，能够扩宽白光LED所发出白光的光谱范围，进而扩宽将该白光LED用于显示装置的背光源时显示色域范围，并提高了液晶显示装置的显示效果。上述各发光材料的用量对于上述效果的实现没有本质影响，为了调整所发出白光的光强、色温等至常规优选范围内，优选上述蓝色发光材料、绿色发光材料与红色发光材料重量比范围为(1～3):(2～6):(2～4)。As described above, the present application includes a luminescent material composition of a blue luminescent material, a green luminescent material, and a red luminescent material, which can broaden the spectral range of white light emitted by the white LED when applied to a white LED light source, thereby widening When the white LED is used for a backlight of a display device, the color gamut range is displayed, and the display effect of the liquid crystal display device is improved. The amount of each of the above-mentioned luminescent materials has no essential influence on the realization of the above effects. In order to adjust the light intensity, color temperature and the like of the emitted white light to a conventional preferred range, it is preferable that the weight ratio of the blue luminescent material, the green luminescent material and the red luminescent material is (1 to 3): (2 to 6): (2 to 4).
为了提高蓝光激发能量，以拓展显示色域，进一步优选上述LED芯片2发射峰值波长范围390～410nm，更优选为400～407nm。In order to increase the blue light excitation energy to expand the display color gamut, it is further preferred that the LED chip 2 emits a peak wavelength in the range of 390 to 410 nm, more preferably 400 to 407 nm.
本申请的发光装置只要具有上述特征，对其他构成没有特别限定。作为密封剂，可以使用硅胶、环氧树脂、硅酮树脂、尿素树脂等，但并不限定于此。另外，在光转化部除上述荧光粉及密封剂以外，亦可包含适当的SiO2、TiO2、ZrO2、Al2O3等添加剂。The light-emitting device of the present application is not particularly limited as long as it has the above characteristics. As the sealant, silica gel, epoxy resin, silicone resin, urea resin or the like can be used, but it is not limited thereto. Further, the light conversion unit may contain an additive such as SiO 2 , TiO 2 , ZrO 2 or Al 2 O 3 in addition to the phosphor and the sealant.
需要说明的是，用于本发明的发光装置的上述蓝色发光材料、绿色发光材料、红色发光材料，即可用公知的适当的方法制造，也可以直接购得。Incidentally, the blue light-emitting material, the green light-emitting material, and the red light-emitting material used in the light-emitting device of the present invention may be produced by a known appropriate method or may be directly obtained.
以下将结合实施例和对比例，进一步说明本申请的有益效果。Advantageous effects of the present application will be further described below in conjunction with the examples and comparative examples.
比较例1Comparative example 1
按照如图1所示的方式制备LED发光装置。其中，LED芯片2为450nm处峰值波长芯片，光转化部3中的绿色发光材料采用Si5.70Al0.30O0.30N7.70:0.05Eu2+，红色发光材料采用K2SiF6:0.01Mn4+。将上述绿色发光材料与红色发光材料按照重量比为25:75混合分散在硅胶中，制备出光转化部。光转化部进一步地组装成LED发光装置。An LED light-emitting device was prepared in the manner as shown in FIG. The LED chip 2 is a peak wavelength chip at 450 nm, the green light-emitting material in the light conversion portion 3 is Si 5.70 Al 0.30 O 0.30 N 7.70 : 0.05Eu 2+ , and the red luminescent material is K 2 SiF 6 : 0.01 Mn 4+ . The green light-emitting material and the red light-emitting material were mixed and dispersed in a silica gel at a weight ratio of 25:75 to prepare a light conversion portion. The light conversion portion is further assembled into an LED light emitting device.
比较例2Comparative example 2
按照如图1所示的方式制备LED发光装置。其中，LED芯片2为365nm处峰值波长芯片，光转化部3中的蓝色发光材料采用Ba0.85MgAl10O17:0.15Eu，绿色发光材料采用 Lu2.94Al5Si12:0.06Ce，红色发光材料采用Ca0.99AlSiN3:0.01Eu。将上述蓝色发光材料、绿色发光材料与红色发光材料按照重量比为25:40:35混合分散在硅胶中(硅胶与荧光粉的重量比为88:12)，制备出光转化部。光转化部进一步地组装成LED发光装置。An LED light-emitting device was prepared in the manner as shown in FIG. The LED chip 2 is a peak wavelength chip at 365 nm, the blue light-emitting material in the light conversion portion 3 is Ba 0.85 MgAl 10 O 17 :0.15Eu, and the green light-emitting material is Lu 2.94 Al 5 Si 12 :0.06Ce, red light-emitting material. Ca 0.99 AlSiN 3 : 0.01 Eu was used. The blue light-emitting material, the green light-emitting material and the red light-emitting material were mixed and dispersed in a silica gel at a weight ratio of 25:40:35 (the weight ratio of the silica gel to the phosphor was 88:12) to prepare a light conversion portion. The light conversion portion is further assembled into an LED light emitting device.
实施例1Example 1
按照如图1所示的方式制备本发明的白光LED发光装置。其中，LED芯片2为365nm处峰值波长芯片，光转化部3中的蓝色发光下来采用Ba0.85MgAl10O17:0.15Eu，绿色发光材料采用La2.84Si6N11:0.16Tb，红色发光材料采用3.5MgO·0.5MgF2·0.85(Ge0.9821Mn0.0179)O2·0.15/3Si3N4。将上述蓝色发光材料、绿色发光材料与红色发光材料按照重量比为30:40:30混合分散在硅胶中(硅胶与荧光粉的重量比为90:10)，制备出光转化部。光转化部进一步地组装成LED发光装置。The white LED light-emitting device of the present invention was prepared in the manner as shown in FIG. Wherein, the LED chip 2 is a peak wavelength chip at 365 nm, the blue light in the light conversion portion 3 is Ba 0.85 MgAl 10 O 17 : 0.15Eu, and the green light emitting material is La 2.84 Si 6 N 11 : 0.16 Tb, red light emitting material. 3.5 MgO · 0.5 MgF 2 ·0.85 (Ge 0.9821 Mn 0.0179 )O 2 ·0.15/3Si 3 N 4 was used . The blue light-emitting material, the green light-emitting material and the red light-emitting material were mixed and dispersed in a silica gel at a weight ratio of 30:40:30 (the weight ratio of the silica gel to the phosphor was 90:10) to prepare a light conversion portion. The light conversion portion is further assembled into an LED light emitting device.
实施例2Example 2
按照如图1所示的方式制备本发明的白光LED发光装置。其中，LED芯片2为405nm处峰值波长芯片，光转化部3中的蓝色发光材料采用Sr4.8(PO4)3Cl:0.2Eu，绿色发光材料采用Ba0.5MgAl10O17:0.07Eu,0.43Mn，红色发光材料采用3.5MgO·0.5MgF2·0.8(Ge0.981Mn0.019)O2·0.2/3Si3N4。将上述蓝色发光材料、绿色发光材料与红色发光材料按照重量比为25:45:30混合分散在环氧树脂中(环氧树脂与荧光粉的重量比为92:8)，制备出光转化部。光转化部进一步地组装成LED发光装置。The white LED light-emitting device of the present invention was prepared in the manner as shown in FIG. The LED chip 2 is a peak wavelength chip at 405 nm, the blue light-emitting material in the light conversion portion 3 is Sr 4.8 (PO 4 ) 3 Cl: 0.2Eu, and the green light-emitting material is Ba 0.5 MgAl 10 O 17 : 0.07Eu, 0.43. Mn, red luminescent material is 3.5MgO·0.5MgF 2 ·0.8(Ge 0.981 Mn 0.019 )O 2 ·0.2/3Si 3 N 4 . The blue light-emitting material, the green light-emitting material and the red light-emitting material are mixed and dispersed in an epoxy resin at a weight ratio of 25:45:30 (the weight ratio of the epoxy resin to the phosphor is 92:8) to prepare a light conversion portion. . The light conversion portion is further assembled into an LED light emitting device.
实施例3-12制备工艺基本与实施例2相同，采用不同的LED芯片及发光材料，具体见表1。The preparation process of the embodiment 3-12 is basically the same as that of the embodiment 2, and different LED chips and luminescent materials are used, as shown in Table 1.
表1Table 1
Figure PCTCN2017073175-appb-000001
Figure PCTCN2017073175-appb-000001
Figure PCTCN2017073175-appb-000002
Figure PCTCN2017073175-appb-000002
采用HAAS-2000高精度快速光谱分析仪检测得到光效和色坐标，利用色坐标和色域计算公式计算得到显示色域，检测结果见表2。The light effect and color coordinates were detected by HAAS-2000 high-precision fast spectrum analyzer. The color gamut was calculated by color coordinate and color gamut calculation formula. The test results are shown in Table 2.
表2Table 2
  显示色域(％NTSC)Display color gamut (%NTSC) 光效(lm/W)Light efficiency (lm/W)
比较例1Comparative example 1 9090 9595
比较例2Comparative example 2 9191 9090
实施例1Example 1 9898 9898
实施例2Example 2 9595 9696
实施例3Example 3 9696 9595
实施例4Example 4 9595 9797
实施例5Example 5 9696 9696
实施例6Example 6 9494 9898
实施例7Example 7 9797 9494
实施例8Example 8 9494 9797
实施例9Example 9 9393 9898
实施例10Example 10 9494 9696
实施例11Example 11 9393 9696
实施例12Example 12 9393 9898
根据表2中的数据可以看出，光转换部采用本申请的发光材料形成的混合物时，发光装置的显示色域明显提高，且同时保持高光效。另外，根据实施例1和2的对比可以发现，当发光材料组合物和具有适当发射峰值波长的LED芯片配合时，能够进一步拓宽显示色域，提高光效。As can be seen from the data in Table 2, when the light converting portion is a mixture formed of the luminescent material of the present application, the display color gamut of the illuminating device is remarkably improved while maintaining high luminous efficiency. In addition, according to the comparison of Examples 1 and 2, it can be found that when the luminescent material composition is combined with the LED chip having an appropriate emission peak wavelength, the display color gamut can be further broadened, and the light effect can be improved.
从以上的描述中，可以看出，本发明上述的实施例实现了如下技术效果：From the above description, it can be seen that the above-described embodiments of the present invention achieve the following technical effects:
上述发光材料组合物包括具有稳定结构的蓝色发光材料、发光能量较高的绿色发光材料和较长波长的红色发光材料，在应用至白光LED光源中时，能够扩宽白光LED所发出白光的光谱范围，进而扩宽将该白光LED用于显示装置的背光源时显示色域范围，并提高了液晶显示装置的显示效果。 The luminescent material composition includes a blue luminescent material having a stable structure, a green luminescent material having a relatively high radiant energy, and a red luminescent material having a longer wavelength, which can broaden the white light emitted by the white LED when applied to the white LED light source. The spectral range further broadens the display color gamut range when the white LED is used for the backlight of the display device, and improves the display effect of the liquid crystal display device.
以上所述仅为本发明的优选实施例而已，并不用于限制本发明，对于本领域的技术人员来说，本发明可以有各种更改和变化。凡在本发明的精神和原则之内，所作的任何修改、等同替换、改进等，均应包含在本发明的保护范围之内。 The above description is only the preferred embodiment of the present invention, and is not intended to limit the present invention, and various modifications and changes can be made to the present invention. Any modifications, equivalent substitutions, improvements, etc. made within the spirit and scope of the present invention are intended to be included within the scope of the present invention.

Claims (12)

  1. 一种发光材料组合物，其特征在于，包括：A luminescent material composition, comprising:
    蓝色发光材料，所述蓝色发光材料选自以下通式表示的任一种或多种形成的混合物：通式ⅠCa2-xLuHf2Al3O12:xCe、通式ⅡCa3-yZr2SiGa2O12:yCe、通式ⅢBa1-rMgAl10O17:rEu和通式ⅣSr5-m(PO4)3Cl:mEu，其中，0.002≤x≤0.2，0.002≤y≤0.2，0.002≤r≤0.2，0.002≤m≤0.5，所述通式Ⅰ中的Ca可被Ba、Sr、Mg中的一个或多个取代，Al元素可被B、Ga、Si中的一个或多个取代；所述通式Ⅱ中的Ca可被Ba、Sr、Mg中的一个或多个取代，Al元素可被B、Ga、Si中的一个或多个取代，Si可被Al取代，Ce可被Eu、Dy、Tb中的一个或多个部分取代；所述通式Ⅲ中的Ba可被Ca和/或Sr取代，Eu可被Ce和/或Mn部分取代；所述通式Ⅳ中的Sr可被Ba、Ca、Mg中的一种或多种取代，Eu可被Ce和/或Mn部分取代；a blue luminescent material selected from the group consisting of any one or more of the following formulas: Formula ICa 2-x LuHf 2 Al 3 O 12 :xCe, Formula IICa 3-y Zr 2 SiGa 2 O 12 :yCe, the general formula IIIBa 1-r MgAl 10 O 17 :rEu and the general formula IVSr 5-m (PO 4 ) 3 Cl:mEu, wherein 0.002≤x≤0.2, 0.002≤y≤0.2, 0.002≤r≤0.2, 0.002≤m≤0.5, Ca in the general formula I may be substituted by one or more of Ba, Sr, Mg, and the Al element may be one or more of B, Ga, Si Substituting; Ca in the general formula II may be substituted by one or more of Ba, Sr, Mg, Al may be substituted by one or more of B, Ga, Si, Si may be substituted by Al, Ce may Substituted by one or more moieties of Eu, Dy, Tb; Ba in the general formula III may be substituted by Ca and/or Sr, and Eu may be partially substituted by Ce and/or Mn; Sr may be substituted by one or more of Ba, Ca, Mg, and Eu may be partially substituted by Ce and/or Mn;
    绿色发光材料，所述绿色发光材料选自以下通式表示的任一种或多种形成的混合物：通式ⅤSi6-zAlzOzN8-z:kEu、通式ⅥBa1-s-tMgAl10O17:sEu,tMn和通式ⅦLa3-vSi6N11:vTb中任意一种，其中，0.1≤z≤0.6，0.0001≤k≤0.1，0.001≤s≤0.2，0.01≤t≤0.6，0＜v≤0.5，所述通式Ⅴ中的Eu可被Ce和/或Mn部分取代；所述通式Ⅵ中的Ba可被Ca和/或Sr取代，Eu可被Ce部分取代；所述通式Ⅶ中的La可被Y、Lu、Gd中的一种或多种取代，Si可被C、Ge、Ti中的一种或多种取代，N可被O部分取代，Tb可被Ce和/或Eu取代，且Si6-zAlzOzN8-z:kEu具有与Si5AlON7相同的晶体结构；a green luminescent material selected from the group consisting of any one or more of the following formulas: a formula VSi 6-z Al z O z N 8-z : kEu, a formula VIBa 1-st MgAl 10 O 17 : sEu, tMn and any one of the formula VIILa 3-v Si 6 N 11 :vTb, wherein 0.1≤z≤0.6, 0.0001≤k≤0.1, 0.001≤s≤0.2, 0.01≤t≤0.6 , 0 < v ≤ 0.5, Eu in the general formula V may be partially substituted by Ce and / or Mn; Ba in the general formula VI may be substituted by Ca and / or Sr, Eu may be partially substituted by Ce; La in the general formula VII may be substituted by one or more of Y, Lu, Gd, Si may be substituted by one or more of C, Ge, Ti, N may be substituted by O moiety, and Tb may be Ce and/or Eu substituted, and Si 6-z Al z O z N 8-z :kEu has the same crystal structure as Si 5 AlON 7 ;
    红色发光材料，所述红色发光材料为通式Ⅷ3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，F可被Cl、Br、I中的一种或多种取代，Ge可被Ti和/或Si取代，Mg可被Ca、Sr、Ba中的一种或多种取代，M元素选自Si和/或Ti，0.77≤j<0.90，0≤i≤0.067，0.015≤n≤0.03。a red luminescent material, the red luminescent material being a mixture of any one or more of the formula VIII3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 , wherein F may be substituted by one or more of Cl, Br, I, Ge may be substituted by Ti and/or Si, Mg may be substituted by one or more of Ca, Sr, Ba, and M element is selected from Si and / or Ti, 0.77 ≤ j < 0.90, 0 ≤ i ≤ 0.067, 0.015 ≤ n ≤ 0.03.
  2. 根据权利要求1所述的发光材料组合物，其特征在于，所述蓝色发光材料为Ba1-rMgAl10O17:rEu和Sr5-m(PO4)3Cl:mEu中任意一种，所述绿色发光材料为La3-vSi6N11:vTb和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。The luminescent material composition according to claim 1, wherein the blue luminescent material is any one of Ba 1-r MgAl 10 O 17 :rEu and Sr 5-m (PO 4 ) 3 Cl:mEu The green luminescent material is any one of La 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 :sEu, tMn.
  3. 根据权利要求1或2所述的发光材料组合物，其特征在于，所述通式Ⅷ中0.05≤i≤0.067。The luminescent material composition according to claim 1 or 2, wherein 0.05 ≤ i ≤ 0.067 in the formula VIII.
  4. 根据权利要求1所述的发光材料组合物，其特征在于，所述绿色发光材料为Si6-zAlzOzN8-z:kEu和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。The luminescent material composition according to claim 1, wherein the green luminescent material is Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn Any of them.
  5. 根据权利要求1或4所述的发光材料组合物，其特征在于，所述通式Ⅷ中0.05≤i≤0.067。The luminescent material composition according to claim 1 or 4, wherein 0.05 ≤ i ≤ 0.067 in the formula VIII.
  6. 一种发光装置，其特征在于，所述发光装置包括LED芯片(2)和光转化部(3)，所述光转化部(3)吸收所述LED芯片(2)发出的一次光，并转换为更高波长的二次光，所述光转化部含有发光材料，所述发光材料为权利要求1至5中任一项所述的发光材料。 A light-emitting device, characterized in that the light-emitting device comprises an LED chip (2) and a light conversion portion (3), and the light conversion portion (3) absorbs the primary light emitted by the LED chip (2) and converts it into The higher wavelength secondary light, the light conversion portion containing a light-emitting material, the light-emitting material being the light-emitting material according to any one of claims 1 to 5.
  7. 根据权利要求6所述的发光装置，其特征在于，所述LED芯片(2)发射峰值波长范围355～375nm，所述发光材料中蓝色发光材料为Ba1-rMgAl10O17:rEu和Sr5-m(PO4)3Cl:mEu中任意一种，绿色发光材料为La3-vSi6N11:vTb和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。The illuminating device according to claim 6, wherein the LED chip (2) emits a peak wavelength range of 355 to 375 nm, and the blue luminescent material of the luminescent material is Ba 1-r MgAl 10 O 17 :rEu and Any one of Sr 5-m (PO 4 ) 3 Cl:mEu, the green light-emitting material is any one of La 3-v Si 6 N 11 :vTb and Ba 1-st MgAl 10 O 17 :sEu, tMn.
  8. 根据权利要求6或7所述的发光装置，其特征在于，所述发光材料中红色发光材料为3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，0.05≤i≤0.067。The illuminating device according to claim 6 or 7, wherein the red luminescent material in the luminescent material is 3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 Any one or more of the resulting mixtures, wherein 0.05 ≤ i ≤ 0.067.
  9. 根据权利要求8所述的发光装置，其特征在于，所述LED芯片(2)发射峰值波长范围360～370nm，优选为362～367nm。Light-emitting device according to claim 8, characterized in that the LED chip (2) emits a peak wavelength in the range of 360 to 370 nm, preferably 362 to 367 nm.
  10. 根据权利要求6所述的发光装置，其特征在于，所述LED芯片(2)发射峰值波长范围380～420nm，所述发光材料中绿色发光材料为Si6-zAlzOzN8-z:kEu和Ba1-s-tMgAl10O17:sEu,tMn中的任意一种。The illuminating device according to claim 6, wherein the LED chip (2) emits a peak wavelength range of 380 to 420 nm, and the green luminescent material of the luminescent material is Si 6-z Al z O z N 8-z : kEu and Ba 1-st MgAl 10 O 17 : sEu, tMn.
  11. 根据权利要求6或10所述的发光装置，其特征在于，所述发光材料中红色发光材料为3.5MgO·0.5MgF2·j(Ge1-nMnn)O2·iM3N4中的任意一种或多种形成的混合物，其中，0.05≤i≤0.067。The illuminating device according to claim 6 or 10, wherein the red luminescent material in the luminescent material is 3.5MgO·0.5MgF 2 ·j(Ge 1-n Mn n )O 2 ·iM 3 N 4 Any one or more of the resulting mixtures, wherein 0.05 ≤ i ≤ 0.067.
  12. 根据权利要求11所述的发光装置，其特征在于，所述LED芯片(2)发射峰值波长范围390～410nm，优选为400～407nm。 Light-emitting device according to claim 11, characterized in that the LED chip (2) emits a peak wavelength in the range from 390 to 410 nm, preferably from 400 to 407 nm.
PCT/CN2017/073175 2017-02-09 2017-02-09 Luminescent material composition and light emitting device WO2018145288A1 (en)

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