WO2012144686A1 - Diode électroluminescente blanche ayant un luminophore monophasique - Google Patents

Diode électroluminescente blanche ayant un luminophore monophasique Download PDF

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Publication number
WO2012144686A1
WO2012144686A1 PCT/KR2011/003675 KR2011003675W WO2012144686A1 WO 2012144686 A1 WO2012144686 A1 WO 2012144686A1 KR 2011003675 W KR2011003675 W KR 2011003675W WO 2012144686 A1 WO2012144686 A1 WO 2012144686A1
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WIPO (PCT)
Prior art keywords
phosphor
white light
emitting diode
light emitting
wavelength
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Ceased
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PCT/KR2011/003675
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English (en)
Korean (ko)
Inventor
조성매
성재석
손석진
이태범
나움소쉬친
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10H—INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS
    • H10H20/00—Individual inorganic light-emitting semiconductor devices having potential barriers, e.g. light-emitting diodes [LED]
    • H10H20/80—Constructional details
    • H10H20/85—Packages
    • H10H20/851—Wavelength conversion means
    • H10H20/8511—Wavelength conversion means characterised by their material, e.g. binder
    • H10H20/8512—Wavelength conversion materials
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10H—INORGANIC LIGHT-EMITTING SEMICONDUCTOR DEVICES HAVING POTENTIAL BARRIERS
    • H10H20/00—Individual inorganic light-emitting semiconductor devices having potential barriers, e.g. light-emitting diodes [LED]
    • H10H20/80—Constructional details
    • H10H20/85—Packages
    • H10H20/851—Wavelength conversion means
    • 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 materials, e.g. electroluminescent or chemiluminescent
    • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
    • C09K11/77—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals
    • C09K11/7766—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
    • C09K11/7774—Aluminates
    • 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 materials, e.g. electroluminescent or chemiluminescent
    • C09K11/08—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials
    • C09K11/77—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals
    • C09K11/7766—Luminescent materials, e.g. electroluminescent or chemiluminescent containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
    • C09K11/7776—Vanadates; Chromates; Molybdates; Tungstates
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
    • Y02B20/00—Energy efficient lighting technologies, e.g. halogen lamps or gas discharge lamps

Definitions

  • the present invention relates to a white light emitting diode including a single phase phosphor.
  • a single phase phosphor capable of emitting warm white using a single phase phosphor based on gadolinium (Gd), a rare earth metal ion of garnet type, is provided. It relates to a white light emitting diode comprising.
  • a white LED using a light emitting device has attracted attention as a white light source for illumination or a white light source of a backlight unit.
  • a YAG: Ce (yttrium aluminum garnet) phosphor is mainly used.
  • the white LED using the YAG: Ce phosphor has the following characteristics.
  • the excitation wavelength variable depends on the concentration of YAG: Ce, and has the advantage of high efficiency of the raw material for phosphor synthesis.
  • the YAG: Ce phosphor has a disadvantage in that the practicality of the Y 3 Al 5 O 12 structure, that is, the color invariance is poor.
  • particle size which is a standard of known phosphors, can be synthesized only at very high temperature, and has a disadvantage of forming a very narrow spectral band with a fluorescent excitation wavelength of 445 to 465 nm.
  • the phosphor using TAG is a very expensive starting material (tebium oxide ( ⁇ b 4 O 7 )), there is a disadvantage that the unit price of the product increases. In addition, there is a problem that the brightness is about 20% lower than that of the phosphor based on the conventional YAG: Ce.
  • the present invention is to solve the above-mentioned problems, to provide a white light emitting diode comprising a single-phase phosphor that emits warm white light, and has a high light efficiency.
  • the present invention is to provide a white light emitting diode comprising a single-phase phosphor which can obtain a light emission wavelength of 1cd luminous intensity in the axial direction.
  • the present invention is to provide a white light emitting diode comprising a single-phase phosphor having a color rendering index of Ra ⁇ 75 or more and a relatively low raw material cost.
  • the present invention provides a white light emitting diode comprising a single phase phosphor, comprising a phosphor which is a single phase compound based on rare earth metal ion gadolinium (Gd) of garnet type activated by cerium; Ions contained in the phosphor is implemented by a material belonging to the 1.3.7 group of the periodic table, it is achieved by a white light emitting diode comprising a single-phase phosphor, characterized by the following formula.
  • Gd rare earth metal ion gadolinium
  • the rare earth metal ion concentration is 70% ⁇ Gd ⁇ 90%, 1% ⁇ Y ⁇ 2%, 1% ⁇ Lu ⁇ 2%, 0.01% ⁇ Tb ⁇ 2%, 0.1% ⁇ Ce ⁇ 6.5
  • Tb, Ce, Pr, Sm based on the Gd, Y, Lu metal among the rare earth metal corresponding to%, 0.001% ⁇ Sm ⁇ 0.01%, 0.001% ⁇ Pr ⁇ 0.2% do.
  • oxygen ions of O 2 may be substituted with F ⁇ 1 or N ⁇ 3 to increase the intensity of the radiation wavelength.
  • the phosphor adds at least one of Ce + 3 , Pr + 3 , and Sm + 3 as activation ions, and the added activation ions may form different radiation wavelengths.
  • the basic fluorescent material of the phosphor is Y + Lu + Tb / Gd, and the group 5 elements Nb and Ta may be added to the basic fluorescent material to increase the half width at half maximum of the spectrum.
  • Phosphor particles distributed in the transparent polymer may reradiate light by binding to a polymer dispersed in a 6% to 18% mass concentration, and the side and the radiation substrate of the transparent polymer have the same thickness. It is preferable.
  • the color rendering index may increase to 81 or more.
  • the X coordinate and the Y coordinate may be adjacent to each other.
  • the present invention can emit warm white light having a high color rendering index through a single-phase phosphor based on gadolinium, which is a garnet rare earth metal ion, and does not need to mix various colors and has a uniform chemical composition.
  • gadolinium which is a garnet rare earth metal ion
  • a white light emitting diode comprising a phosphor is provided.
  • the present invention provides a white light emitting diode including a single-phase phosphor that can emit a uniform warm white light using a single-phase phosphor, a relatively low manufacturing cost.
  • the present invention provides a white light emitting diode including a single-phase phosphor having an economic effect compared to the conventional light emitting lamp because the light speed and light efficiency is increased when the supply current to the hetero transition increases.
  • FIG. 1 is a view showing the structure of a white light emitting diode including a single-phase phosphor according to an embodiment of the present invention
  • FIG. 2 shows the emission of a phosphor having a structure of (Gd, Y, Lu, Tb, Ce, Pr, Sm) 3 (Al 1.99 K 0.005 N 0.005 ) [AlO 0.96 F 0.02 N 0.02 ] 3 according to an embodiment of the present invention. Shows the spectrum,
  • FIG. 3 is a diagram illustrating an XRD analysis graph of phosphors according to an embodiment of the present invention.
  • a white light emitting diode is a nitride semiconductor in which sapphire (Al 2 O 3 ) is formed on a surface thereof, and includes an LED device 1, heterotransition lines 2 and 3, and sapphire.
  • substrate 4 and the transparent polymer 5 are included.
  • the LED device 1 is implemented with an InGaN-based light emitting diode, and two lines 2 and 3 for hetero transition from the LED device 1 are generated.
  • the sapphire substrate 4 is provided on the upper side of the transparent polymer 5 in the shape of a cone packaged with an aluminum polymer, and the transparent polymer 5 is distributed or coated with a phosphor. Description of the phosphor will be described later.
  • the white light emitting diode according to the present invention is operated by the form of the fluorescent substance coated transparent polymer 5 and the phosphor, and is fixed to the radiation surface of the hetero transition.
  • Application of the hetero phase is named by the fluorescent substance distributed in the transparent polymer 5 and the transparent polymer 5, and particle
  • the hetero transition of the LED element 1 is radiated not only on the surface of the sapphire substrate 4 but also on the hetero transition side.
  • particles of phosphor are applied to all four sides of the LED element 1 and to the surface substrate of the hetero transition.
  • the application method for wavelength conversion is divided into two parts. That is, the circumference
  • the thickness of the side of the transparent polymer (5) layer in which the conversion of the wavelength of light occurs and the thickness of the radiating substrate should be the same.
  • the thickness of the transparent polymer (5) was adjusted to 80 ⁇ 200 ⁇ m, the optimum thickness was 120 ⁇ 160 ⁇ m. At this time, color change does not occur in all layers, and uniform warm-white light is emitted.
  • M molecular weight of the silicone-organic polymer
  • the ratio of the phosphor particles and the transparent polymer 5 is also important. If the concentration of the phosphor is lower than 4 ⁇ 5%, the dark blue radiation wavelength is emitted without causing the phosphor particles to emit light. If the particle concentration is 8-9%, the radiation of the original cold light is emitted, and if the concentration is slightly increased, natural and warm colors are emitted.
  • the concentration of the phosphor particles was selected as an optimal concentration range of 12 to 16% to increase the luminance and uniformity of the radiation wavelength.
  • the phosphor according to the present invention is based on gadolinium (Gd), a rare earth metal ion of garnet type activated with cerium (Ce), and the phosphor element is a substance belonging to groups 1, 3 and 7 of the periodic table and is represented by the following chemical formula. Can be.
  • ⁇ Ln Gd, Y, Lu, ⁇ b, Ce, Pr, Sm, and constants A, x, and y are molar ratios, 0.25 ⁇ A ⁇ 3.5, 0.001 ⁇ X ⁇ 0.1, 0.001 ⁇ y ⁇ 0.05.
  • Gd is gadolinium
  • Y is yttrium
  • Lu is lutetium
  • ⁇ b is terbium
  • Ce cerium
  • Pr is praseodymium
  • Sm is samarium.
  • This long wavelength has two maximum peaks, and the distance between the two peaks is about ⁇ > 25 nm.
  • the rare earth metal ions that may be included in the phosphor of the above structure may be used having a concentration range as follows.
  • the radiation wavelength emitted from the phosphor changes.
  • the concentration of Gd when the concentration of Gd is less than 70%, the position of the short wavelength is shifted, yellow light is emitted, and when 90% is exceeded, the light is reduced.
  • the concentration of Y is less than 1%, the light is reduced to emit dark colors, and if it exceeds 2%, yellow light is emitted.
  • the concentration of Lu is less than 1%, the light decreases, and if it exceeds 2%, the excitation spectrum of the short wavelength is changed.
  • the concentration of Tb is less than 0.01%, the light decreases, and if it exceeds 2%, the light decreases.
  • the concentration of Ce is less than 0.1%, the duration of the phosphor increases, and if it exceeds 6.5%, the luminous intensity is lowered.
  • the concentration of Sm When the concentration of Sm is less than 0.001%, the brightness decreases, and when it exceeds 0.01%, the brightness of the light decreases. If the concentration of Pr is less than 0.001%, the brightness decreases. If the concentration of Pr exceeds 0.2%, the emission color of the phosphor becomes worse.
  • the phosphor when the phosphor is used in the concentration outside the concentration range of the metal ion is used to reduce the light, or to emit a color other than white, it is preferable to implement using a metal having the concentration range. .
  • the reason why the sum of the upper limit of the rare earth metal ion exceeds 100% in the composition of the phosphor obtained by using the metal ion is that the initial raw material is volatilized in the process of reducing (nitrogen + hydrogen) at high temperature (about 1000 degrees Celsius) and is lost. (loss) occurs.
  • the mixed weight percent exceeds 100%, but this is to compensate for the loss due to volatilization during the chemical reaction, and the composition of the final phosphor is The sum of the above conditions has a composition ratio of not more than 100%.
  • each rare earth metal ion has the following characteristics.
  • Gd +3 ions together with Ce +3 and Pr +3 form an orange emission wavelength in the radiation phosphor, Y ions shift the radiation wavelength peak in the short wavelength region, and Lu ions shift the radiation wavelength in the short wavelength, To increase the brightness.
  • Each particle is in the form of the same compound, creating an immiscible radiation wavelength from fluorescence.
  • an irreversible layer is formed on the fluorescent compound, leading to complexity and radiation wavelength infringement in the formation of the phosphor layer.
  • the distance ⁇ of the two emission wavelength peaks emitted from the phosphor will depend on the partial equilibrium of the cation lattice of Gd, Y, Lu and Tb.
  • the other peak depends on the parity of Gd / Y + Lu + Tb, so that the distance between the spectral peaks by ⁇ / ⁇ + Lu + Tb ( ⁇ ). ) May be changed to 25-50 nm, which may change the color coordinates of the color temperature and radiation wavelength.
  • XRD X-ray diffraction
  • the phosphor has a garnet structure showing a cubic crystal structure, and the lattice parameter is reduced by a small concentration of F- 1 ions.
  • Table 1 is a table showing the wavelength, illuminance, color temperature and color rendering index for each phosphor structure in which the cation lattice structure and the anion lattice structure are changed in the present invention.

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  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Luminescent Compositions (AREA)

Abstract

La présente invention concerne une diode électroluminescente blanche ayant un luminophore monophasique. La diode électroluminescente blanche ayant le luminophore monophasique est caractérisée en ce qu'elle comprend un luminophore sous la forme d'un composé monophasique à base de gadolinium (Gd) des ions de métal terre rare correspondant à un type de grenaille activée par cérium (Ce), les ions inclus dans le luminophore étant composés de matériaux des Groupes I, III et VII de la table périodique des éléments et étant exprimés dans la formule chimique suivante. <Formule chimique> (ΣLn)A(Al1-xMeIx/2MeVx/2)2[AlO4-xFy/2Ny/2]3, où ΣLn=Gd, Y, Lu, Тb, Ce, Pr, et Sm, les constantes A, x, et y sont des rapports molaires, 0,25 ≤ A ≤ 3,5, 0,001 ≤ x ≤ 0,1, MeI= Li ou Na ou K, 0,001 ≤ y ≤ 0,05, MeV= V ou Nb ou Ta. La présente invention peut émettre une lumière blanche ayant un indice de rendu de couleur élevé par l'intermédiaire du luminophore monophasique à base de gadolinium des ions de métal terre rare correspondant à la grenaille.
PCT/KR2011/003675 2011-04-20 2011-05-18 Diode électroluminescente blanche ayant un luminophore monophasique Ceased WO2012144686A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR10-2011-0036498 2011-04-20
KR1020110036498A KR101337999B1 (ko) 2011-04-20 2011-04-20 단일상 형광체를 포함하는 백색 발광 다이오드

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WO2012144686A1 true WO2012144686A1 (fr) 2012-10-26

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Publication number Priority date Publication date Assignee Title
RU2619318C2 (ru) * 2015-08-17 2017-05-15 Акционерное общество "Научно-исследовательский институт "Платан" с заводом при НИИ" Фотолюминофор нейтрально-белого цвета свечения со структурой граната и светодиод на его основе

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1429397A2 (fr) * 1996-07-29 2004-06-16 Nichia Chemical Industries, Ltd. Dispositif electroluminescent
US20090105065A1 (en) * 2006-03-23 2009-04-23 Koninklijke Philips Electronics N.V. Light emitting device with a ceramic garnet material
US20090289545A1 (en) * 2008-05-26 2009-11-26 Soshchin Naum Warm-White Light-Emitting Diode and Its Phosphor Powder
US20090315449A1 (en) * 2008-06-20 2009-12-24 Soshchin Naum Warm-white light-emitting diode and its orange phosphor powder
US20100044729A1 (en) * 2008-08-22 2010-02-25 Soshchin Naum Warm-white light emtitting diode and its halide phosphor powder

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7094362B2 (en) * 2003-10-29 2006-08-22 General Electric Company Garnet phosphor materials having enhanced spectral characteristics

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP1429397A2 (fr) * 1996-07-29 2004-06-16 Nichia Chemical Industries, Ltd. Dispositif electroluminescent
US20090105065A1 (en) * 2006-03-23 2009-04-23 Koninklijke Philips Electronics N.V. Light emitting device with a ceramic garnet material
US20090289545A1 (en) * 2008-05-26 2009-11-26 Soshchin Naum Warm-White Light-Emitting Diode and Its Phosphor Powder
US20090315449A1 (en) * 2008-06-20 2009-12-24 Soshchin Naum Warm-white light-emitting diode and its orange phosphor powder
US20100044729A1 (en) * 2008-08-22 2010-02-25 Soshchin Naum Warm-white light emtitting diode and its halide phosphor powder

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KR101337999B1 (ko) 2013-12-06
KR20120118873A (ko) 2012-10-30

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