WO2012032818A1 - Ｅｕ固溶β型サイアロンの製造方法 - Google Patents

Ｅｕ固溶β型サイアロンの製造方法 Download PDF

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Publication number
WO2012032818A1
WO2012032818A1 PCT/JP2011/063122 JP2011063122W WO2012032818A1 WO 2012032818 A1 WO2012032818 A1 WO 2012032818A1 JP 2011063122 W JP2011063122 W JP 2011063122W WO 2012032818 A1 WO2012032818 A1 WO 2012032818A1
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WO
WIPO (PCT)
Prior art keywords
sialon
container
mpa
raw material
firing
Prior art date
Application number
PCT/JP2011/063122
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English (en)
French (fr)
Japanese (ja)
Inventor
史博 中原
市川　恒希
隆二 徳永
山田　鈴弥
Original Assignee
電気化学工業株式会社
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Application filed by 電気化学工業株式会社 filed Critical 電気化学工業株式会社
Publication of WO2012032818A1 publication Critical patent/WO2012032818A1/ja

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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
    • H05B33/00—Electroluminescent light sources
    • H05B33/10—Apparatus or processes specially adapted to the manufacture of electroluminescent light sources
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
    • C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
    • C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
    • C09K11/77348—Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05B—ELECTRIC HEATING; ELECTRIC LIGHT SOURCES NOT OTHERWISE PROVIDED FOR; CIRCUIT ARRANGEMENTS FOR ELECTRIC LIGHT SOURCES, IN GENERAL
    • H05B33/00—Electroluminescent light sources
    • H05B33/12—Light sources with substantially two-dimensional radiating surfaces
    • H05B33/14—Light sources with substantially two-dimensional radiating surfaces characterised by the chemical or physical composition or the arrangement of the electroluminescent material, or by the simultaneous addition of the electroluminescent material in or onto the light source

Definitions

  • the present invention relates to a method for producing ⁇ -sialon in which Eu (europium) is dissolved.
  • the characteristics of the baked phosphor greatly change depending on the shape of the container used at the time of firing and the amount of raw material powder to be filled, and a high emission intensity cannot be obtained. It was difficult to produce Eu solid-solution ⁇ -sialon with less reproducibility with good reproducibility.
  • An object of the present invention is to provide a method for producing Eu solid-solution ⁇ -sialon having high luminous efficiency with little variation in quality and good reproducibility.
  • the present invention relates to one or both of aluminum oxide and silicon oxide filled in a boron nitride container having an air permeability of 0.1 cm 3 / cm 2 ⁇ s ⁇ MPa or less, silicon nitride, aluminum nitride, and a europium compound. It is a manufacturing method of Eu solid solution beta-sialon characterized by including the baking process which bakes the raw material which consists of these in nitrogen atmosphere.
  • Eu solid-solution ⁇ -sialon produced by the method of the present invention has a small decrease in luminance even at high temperatures, and a light emitting device using the Eu solute ⁇ -sialon has a small decrease in luminance and chromaticity deviation and is excellent in heat resistance. Good quality and stability.
  • a light emitting device that emits a desired color can be configured by using together with a phosphor having other light emission characteristics together with Eu solid solution ⁇ -type sialon.
  • a blue LED is used as an excitation source
  • white light emission with a wide color temperature is possible when the phosphor of this embodiment is combined with a yellow phosphor having an emission peak in a region of 575 nm or more and 590 nm or less.
  • the present invention relates to one or both of aluminum oxide and silicon oxide filled in a boron nitride container having an air permeability of 0.1 cm 3 / cm 2 ⁇ s ⁇ MPa or less, silicon nitride, aluminum nitride, and a europium compound.
  • This is a method for producing Eu solid solution ⁇ -sialon, comprising a firing step of firing a raw material made of
  • a boron nitride container is used as a container for filling the raw material.
  • a container made of boron nitride (hereinafter referred to as a BN container) is used because the container made of boron nitride plate crystals has air permeability, and the component of the raw material powder is mainly used as a gas phase of SiO during firing. This is because it can volatilize out of the vessel through the pores of boron nitride.
  • the BN container is small, the effect of suppressing the volatilization amount of SiO tends to be small, and if the BN container is large, the SiO volatilization amount in the container tends to be non-uniform. Therefore, it is preferable to use a cylindrical container having an inner diameter of 5 cm to 15 cm and a height of 5 cm to 15 cm so that the powder physical properties and light emission characteristics of Eu solid solution ⁇ -sialon do not become uneven.
  • the fired product After firing, the fired product is cooled and pulverized to obtain a powder having a uniform particle size.
  • the decrease in the weight of the raw material and the decrease in the amount of oxygen due to the firing are suppressed. This makes it possible to produce Eu solid-solution ⁇ -sialon with high emission intensity with reproducibility.
  • the obtained powder is reheated in a vacuum or a gas atmosphere other than nitrogen gas (hereinafter referred to as a reheating step), and further subjected to an acid treatment. Also good.
  • the reheating step it is effective to perform reheating in a gas atmosphere containing as little as possible nitrogen and oxygen as elements constituting the low crystalline portion.
  • a gas containing as little oxygen as possible there is a rare gas selected from helium, neon, argon, krypton, xenon, and radon, and preferably argon.
  • the acid treatment heat step is a treatment step for removing the destabilized low crystalline portion by dipping in a strongly acidic liquid.
  • the acid include hydrofluoric acid and nitric acid alone or as a mixture.
  • what was already used for 50 times or more of baking was used for the BN container of Example 1.
  • the fired product was a loosely agglomerated lump.
  • Eu solid solution ⁇ -sialon phosphor powder was obtained through a sieve having an opening of 45 ⁇ m.
  • the amount of oxygen in the phosphor powder was 1.15% by mass, and the amount of decrease in the amount of oxygen with respect to the raw material mixed powder was 31.5%.
  • the phosphor powder of Eu solid solution ⁇ -sialon obtained in Example 2 is again filled in a BN container, heated to 1000 ° C., argon gas is introduced at 1000 ° C. to make the gas pressure atmospheric pressure, and every minute The temperature was raised to 1500 ° C. at 10 ° C. and held at 1500 ° C. for 6 hours for reheating treatment. Then, it cooled to 1200 degreeC at 10 degreeC / min, and cooled below 1200 degreeC by the furnace cooling to room temperature vicinity. The obtained powder turned dark green, but did not solidify and remained powdery.
  • Comparative Example 1 The raw material powder is fired under the same conditions as in Example 2 except that a BN container (air permeation time is 88 seconds) with an air permeability of 0.18 cm 3 / cm 2 ⁇ s ⁇ MPa, and the mesh is opened after pulverization. Eu solid solution ⁇ -sialon phosphor powder was obtained through a 45 ⁇ m sieve. The obtained phosphor powder was evaluated in the same manner as in Example 1. The decrease in the weight of the raw material before and after firing was 1.83%, the decrease in oxygen content was 41.7%, and the emission intensity was 100%. The BN container used in Comparative Example 1 is the second use.
  • All of the phosphors of Examples 1 to 3 had a raw material weight reduction of 1.5% or less and an oxygen reduction amount of 40% or less, and had higher emission intensity than Comparative Examples 1 to 3. Further, as shown in FIG. 1, the higher the raw material weight reduction value, the lower the emission intensity of the phosphor.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Luminescent Compositions (AREA)
PCT/JP2011/063122 2010-09-09 2011-06-08 Ｅｕ固溶β型サイアロンの製造方法 WO2012032818A1 (ja)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2010202511A JP2012057070A (ja) 2010-09-09 2010-09-09 Ｅｕ固溶β型サイアロンの製造方法
JP2010-202511 2010-09-09

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WO2012032818A1 true WO2012032818A1 (ja) 2012-03-15

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JP (1) JP2012057070A (zh)
TW (1) TWI454556B (zh)
WO (1) WO2012032818A1 (zh)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP6024849B1 (ja) * 2015-06-05 2016-11-16 日亜化学工業株式会社 βサイアロン蛍光体の製造方法
WO2022209178A1 (ja) * 2021-03-31 2022-10-06 デンカ株式会社 ユウロピウム賦活β型サイアロン蛍光体、及び発光装置

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP7335112B2 (ja) * 2019-08-21 2023-08-29 デンカ株式会社 酸窒化物蛍光体の製造方法

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2007129713A1 (ja) * 2006-05-10 2007-11-15 Denki Kagaku Kogyo Kabushiki Kaisha サイアロン蛍光体及びその製造方法並びにそれを用いた照明器具及び発光素子
WO2007142289A1 (ja) * 2006-06-09 2007-12-13 Denki Kagaku Kogyo Kabushiki Kaisha 蛍光体及びその製造方法並びにそれを用いた照明器具
WO2008041452A1 (fr) * 2006-09-29 2008-04-10 Dowa Electronics Materials Co., Ltd. Procédé de fabrication du nitrure ou oxonitrure
WO2008062781A1 (fr) * 2006-11-20 2008-05-29 Denki Kagaku Kogyo Kabushiki Kaisha Substance fluorescente et son procédé de fabrication, et dispositif électroluminescent

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2004210921A (ja) * 2002-12-27 2004-07-29 Nichia Chem Ind Ltd オキシ窒化物蛍光体及びその製造方法並びにそれを用いた発光装置
JP5125039B2 (ja) * 2006-09-12 2013-01-23 日亜化学工業株式会社 希土類酸窒化物系蛍光体及びこれを用いた発光装置
JP5832713B2 (ja) * 2008-04-14 2015-12-16 日亜化学工業株式会社 蛍光体及びこれを用いた発光装置並びに蛍光体の製造方法

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2007129713A1 (ja) * 2006-05-10 2007-11-15 Denki Kagaku Kogyo Kabushiki Kaisha サイアロン蛍光体及びその製造方法並びにそれを用いた照明器具及び発光素子
WO2007142289A1 (ja) * 2006-06-09 2007-12-13 Denki Kagaku Kogyo Kabushiki Kaisha 蛍光体及びその製造方法並びにそれを用いた照明器具
WO2008041452A1 (fr) * 2006-09-29 2008-04-10 Dowa Electronics Materials Co., Ltd. Procédé de fabrication du nitrure ou oxonitrure
WO2008062781A1 (fr) * 2006-11-20 2008-05-29 Denki Kagaku Kogyo Kabushiki Kaisha Substance fluorescente et son procédé de fabrication, et dispositif électroluminescent

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP6024849B1 (ja) * 2015-06-05 2016-11-16 日亜化学工業株式会社 βサイアロン蛍光体の製造方法
JP2017002278A (ja) * 2015-06-05 2017-01-05 日亜化学工業株式会社 βサイアロン蛍光体の製造方法
WO2022209178A1 (ja) * 2021-03-31 2022-10-06 デンカ株式会社 ユウロピウム賦活β型サイアロン蛍光体、及び発光装置

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JP2012057070A (ja) 2012-03-22
TWI454556B (zh) 2014-10-01

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