TWI612022B - Manufacturing method of glass for led - Google Patents
Manufacturing method of glass for led Download PDFInfo
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- TWI612022B TWI612022B TW105116693A TW105116693A TWI612022B TW I612022 B TWI612022 B TW I612022B TW 105116693 A TW105116693 A TW 105116693A TW 105116693 A TW105116693 A TW 105116693A TW I612022 B TWI612022 B TW I612022B
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- glass
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- sintering
- glass frit
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- 239000011521 glass Substances 0.000 title claims abstract description 389
- 238000004519 manufacturing process Methods 0.000 title claims description 19
- 238000005245 sintering Methods 0.000 claims abstract description 80
- 238000000034 method Methods 0.000 claims abstract description 41
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 claims abstract description 39
- 238000012545 processing Methods 0.000 claims abstract description 4
- 238000001035 drying Methods 0.000 claims abstract description 3
- 238000002844 melting Methods 0.000 claims description 145
- 230000008018 melting Effects 0.000 claims description 32
- 239000000758 substrate Substances 0.000 claims description 25
- 239000011148 porous material Substances 0.000 claims description 18
- 239000002002 slurry Substances 0.000 claims description 12
- 238000010030 laminating Methods 0.000 claims description 8
- 229920005989 resin Polymers 0.000 claims description 8
- 239000011347 resin Substances 0.000 claims description 8
- 238000010345 tape casting Methods 0.000 claims description 8
- 239000011230 binding agent Substances 0.000 claims description 6
- 239000002904 solvent Substances 0.000 claims description 6
- 238000002788 crimping Methods 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 238000007496 glass forming Methods 0.000 claims description 2
- 238000006243 chemical reaction Methods 0.000 description 16
- 238000002834 transmittance Methods 0.000 description 9
- 239000003795 chemical substances by application Substances 0.000 description 7
- 239000000463 material Substances 0.000 description 6
- 238000000605 extraction Methods 0.000 description 5
- JNDMLEXHDPKVFC-UHFFFAOYSA-N aluminum;oxygen(2-);yttrium(3+) Chemical compound [O-2].[O-2].[O-2].[Al+3].[Y+3] JNDMLEXHDPKVFC-UHFFFAOYSA-N 0.000 description 4
- 230000007547 defect Effects 0.000 description 4
- 230000006866 deterioration Effects 0.000 description 4
- 238000010438 heat treatment Methods 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 238000012805 post-processing Methods 0.000 description 4
- 229910019901 yttrium aluminum garnet Inorganic materials 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 3
- 238000009826 distribution Methods 0.000 description 3
- 239000005340 laminated glass Substances 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 239000004593 Epoxy Substances 0.000 description 2
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 2
- ULGYAEQHFNJYML-UHFFFAOYSA-N [AlH3].[Ca] Chemical compound [AlH3].[Ca] ULGYAEQHFNJYML-UHFFFAOYSA-N 0.000 description 2
- VEUACKUBDLVUAC-UHFFFAOYSA-N [Na].[Ca] Chemical compound [Na].[Ca] VEUACKUBDLVUAC-UHFFFAOYSA-N 0.000 description 2
- 229910000287 alkaline earth metal oxide Inorganic materials 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 238000000280 densification Methods 0.000 description 2
- 238000003475 lamination Methods 0.000 description 2
- 239000004973 liquid crystal related substance Substances 0.000 description 2
- 210000001161 mammalian embryo Anatomy 0.000 description 2
- 238000004806 packaging method and process Methods 0.000 description 2
- 150000003303 ruthenium Chemical class 0.000 description 2
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 1
- 229910003564 SiAlON Inorganic materials 0.000 description 1
- XWROSHJVVFETLV-UHFFFAOYSA-N [B+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O Chemical compound [B+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O XWROSHJVVFETLV-UHFFFAOYSA-N 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- 230000000903 blocking effect Effects 0.000 description 1
- 239000000919 ceramic Substances 0.000 description 1
- 239000003086 colorant Substances 0.000 description 1
- 239000012141 concentrate Substances 0.000 description 1
- 230000008602 contraction Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000002845 discoloration Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000003822 epoxy resin Substances 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- -1 liquid paraffin Substances 0.000 description 1
- 229940057995 liquid paraffin Drugs 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 239000005022 packaging material Substances 0.000 description 1
- 230000035515 penetration Effects 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 229910052698 phosphorus Inorganic materials 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 239000003566 sealing material Substances 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 150000003481 tantalum Chemical class 0.000 description 1
- 238000000870 ultraviolet spectroscopy Methods 0.000 description 1
- 239000001993 wax Substances 0.000 description 1
- 238000004383 yellowing Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03B—MANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
- C03B19/00—Other methods of shaping glass
- C03B19/01—Other methods of shaping glass by progressive fusion or sintering of powdered glass onto a shaping substrate, i.e. accretion, e.g. plasma oxidation deposition
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03B—MANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
- C03B19/00—Other methods of shaping glass
- C03B19/02—Other methods of shaping glass by casting molten glass, e.g. injection moulding
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03B—MANUFACTURE, SHAPING, OR SUPPLEMENTARY PROCESSES
- C03B19/00—Other methods of shaping glass
- C03B19/06—Other methods of shaping glass by sintering, e.g. by cold isostatic pressing of powders and subsequent sintering, by hot pressing of powders, by sintering slurries or dispersions not undergoing a liquid phase reaction
-
- C—CHEMISTRY; METALLURGY
- C03—GLASS; MINERAL OR SLAG WOOL
- C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
- C03C4/00—Compositions for glass with special properties
- C03C4/12—Compositions for glass with special properties for luminescent glass; for fluorescent glass
-
- 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
- H01L33/48—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 characterised by the semiconductor body packages
- H01L33/50—Wavelength conversion elements
Landscapes
- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Microelectronics & Electronic Packaging (AREA)
- Physics & Mathematics (AREA)
- Plasma & Fusion (AREA)
- Life Sciences & Earth Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Geochemistry & Mineralogy (AREA)
- Dispersion Chemistry (AREA)
- Computer Hardware Design (AREA)
- Power Engineering (AREA)
- Led Device Packages (AREA)
Abstract
Description
本發明涉及LED用玻璃的製備方法，更詳細地，涉及如下LED用玻璃的製備方法，將通過後加工的裂紋不良最小化，並提高透射率及光提取效率，在燒結過程中防止急劇的收縮，且無離型劑也可與基板進行分離。 The present invention relates to a method for producing a glass for LED, and more particularly to a method for preparing a glass for LED, which minimizes crack defects by post-processing, improves transmittance and light extraction efficiency, and prevents sharp shrinkage during sintering. And no release agent can be separated from the substrate.
LED(light emitting diode，發光二極體)作為由镓(Ga)、磷(P)、砷(As)等材料製備而成的半導體，當電流流動時，具有發光的性质。LED與以往的燈泡相比，不僅壽命長、回應速度快，而且可實現小型化、且發出顏色鮮明的光，因此廣泛利用為各種顯示裝置的光源。例如，包括LED晶片的LED封裝件使用為在液晶顯示裝置(liquid crystal display，LCD)的液晶畫面背面發光的背光模組(backlight unit，BLU)中的發光器件。 An LED (light emitting diode) is a semiconductor prepared from a material such as gallium (Ga), phosphorus (P), or arsenic (As), and has a light-emitting property when a current flows. LEDs are widely used as light sources for various display devices because they have a longer life and a faster response speed than conventional light bulbs, and can be made compact and emit bright colors. For example, an LED package including an LED chip uses a light-emitting device in a backlight unit (BLU) that emits light on the back surface of a liquid crystal display of a liquid crystal display (LCD).
通常，用於背光模組等的LED封裝件通過將LED晶片安裝於印刷電路板上，並利用封裝材料進行封裝之後，附著鏡頭來形成。其中，封裝材料基本上起到保護LED晶片受到熱量、水分及外部衝擊的影響，並從LED晶片透射光，來向外部發光的作用。 Generally, an LED package for a backlight module or the like is formed by attaching an LED chip to a printed circuit board and packaging it with a packaging material, and attaching the lens. Among them, the encapsulating material basically protects the LED chip from heat, moisture and external impact, and transmits light from the LED chip to emit light to the outside.
作為封裝材料，通常主要使用矽系列樹脂和環氧系列樹脂，將這種樹脂與螢光體混合使用，從而起到轉換LED晶片中的發光顏色的功能。例如，眾所周知的有如下方法：當將發出藍色光的藍色LED利用為LED晶片時，使用由樹脂與黃色螢光體混合而成的封裝材料來轉換為白色光的顏色轉換方法。並且，以往的眾所周知的封裝方法有將這種樹脂形成為板狀之後，在LED晶片上進行加壓的方法。 As the encapsulating material, a ruthenium series resin and an epoxy series resin are generally mainly used, and this resin is used in combination with a phosphor to function to convert the luminescent color in the LED wafer. For example, it is known that when a blue LED emitting blue light is used as an LED wafer, a color conversion method of converting white light into a package material by mixing a resin and a yellow phosphor is used. Further, a conventionally known packaging method is a method in which such a resin is formed into a plate shape and then pressurized on an LED wafer.
然而，當使用矽系列樹脂中混合有螢光體的封裝材料時，因在高溫下顏色轉換的原材料之劣化而產生變黃現象，並且因氣體及水分的滲透而存在可靠性降低的問題，當使用環氧系列樹脂中混合有螢光體的封裝材料時，存在耐熱性低的問題。 However, when a package material in which a phosphor is mixed in a ruthenium series resin is used, yellowing occurs due to deterioration of a color-converted raw material at a high temperature, and reliability is lowered due to penetration of gas and moisture. When a sealing material in which a phosphor is mixed in an epoxy resin is used, there is a problem that heat resistance is low.
並且，當利用這種矽系列和環氧系列的樹脂來形成LED晶片的封裝材料時，因加壓而設置封裝結構而有可能留有晶片形狀的痕跡，由 此有可能產生發光品質降低的問題。 Further, when the package material of the LED wafer is formed by using the resin of the tantalum series and the epoxy series, the package structure is provided by pressurization, and there is a possibility that a trace of the wafer shape remains. This may cause a problem in that the illuminating quality is lowered.
眾所周知，為了解決如上所述的高溫劣化問題，並提高對於氣體及水分滲透的抵抗性，將在玻璃中分散螢光體的玻璃一螢光體混合物(phosphor in glass，PIG)用作顏色轉換原材料。 It is known that in order to solve the problem of high temperature deterioration as described above and to improve resistance to gas and moisture permeation, a glass-phosphor in glass (PIG) in which a phosphor is dispersed in glass is used as a color conversion raw material. .
在這種玻璃的情況下，存在光集中於LED光源前部面的中央部分，且其餘部分的亮度稍低的問題，因而通常，將擴散板等額外的部件配置於顏色轉換玻璃前部面來使用。但是，在將擴散板配置於玻璃前部面的情況下，存在如下問題：隨著使用額外的部件，不僅大大增加費用，而且隨著光通過擴散板，光的強度降低。 In the case of such a glass, there is a problem that light concentrates on the central portion of the front surface of the LED light source, and the brightness of the remaining portion is slightly lower. Therefore, in general, an additional member such as a diffusion plate is disposed on the front surface of the color conversion glass. use. However, in the case where the diffusing plate is disposed on the front surface of the glass, there is a problem that not only the cost is greatly increased as the additional member is used, but also the intensity of light is lowered as the light passes through the diffusing plate.
並且，在對包含玻璃料的混合物進行燒結的過程中，有可能產生因玻璃急劇收縮而翹起的現象，還存在螢光體因玻璃料的燒結溫度而劣化的問題。並且，以往，當在軟化點以上的溫度下進行燒結時，氣孔多的邊緣部分先熔融，從而消失開放的氣孔通道，因而在內部分佈有大量的閉合的氣孔，從而當燒結後進行加工時，導致裂紋不良。 Further, in the process of sintering the mixture containing the glass frit, there is a possibility that the glass is warped due to sharp shrinkage of the glass, and there is a problem that the phosphor is deteriorated by the sintering temperature of the glass frit. Further, conventionally, when sintering is performed at a temperature higher than the softening point, the edge portion having many pores is first melted, and the open pore passage is eliminated, so that a large number of closed pores are distributed inside, so that when processing is performed after sintering, Causes poor cracks.
另一方面，在製備玻璃的過程中，為了順暢地分離基板和玻璃片，通常，使用蠟、液體石蠟、矽類、氟類等的離型劑。但是，在使用這種離型劑來從基板分離玻璃片的情況下，根據玻璃片的組成所分離的程度不同，並形成額外的離型劑，或者需要利用離型劑覆蓋基板表面的工序。 On the other hand, in the process of preparing the glass, in order to smoothly separate the substrate and the glass piece, a release agent such as wax, liquid paraffin, hydrazine or fluorine is usually used. However, in the case where such a release agent is used to separate the glass piece from the substrate, the degree of separation depending on the composition of the glass piece is different, and an additional release agent is formed, or a process of covering the surface of the substrate with a release agent is required.
本發明的目的在於，解決如上所述的現有技術的問題。 It is an object of the present invention to solve the problems of the prior art as described above.
並且，本發明的目的在於，提供LED用玻璃的製備方法，可將通過後加工的裂紋不良最小化，並提高透射率及光提取效率，在燒結步驟中控制玻璃的急劇收縮，來可將翹起現象的產生最小化。 Further, an object of the present invention is to provide a method for producing a glass for LEDs, which can minimize crack defects by post-processing, improve transmittance and light extraction efficiency, and control the sharp shrinkage of the glass during the sintering step. The occurrence of the phenomenon is minimized.
並且，本發明的另一目的在於，提供LED用玻璃的製備方法，無離型劑也可與基板進行分離，並提高強度。 Further, another object of the present invention is to provide a method for producing a glass for LED, which can be separated from a substrate without a release agent and can be improved in strength.
用於實現上述目的的本發明的代表性結構如下。 A representative structure of the present invention for achieving the above object is as follows.
根據本發明的一實施例，可包括：步驟a，對添加有螢光體的玻璃漿料進行成形及加工之後，進行乾燥來形成玻璃成形體；以及步驟b，對玻璃成形體進行燒結。其中，對玻璃成形體進行燒結的步驟可包括：在小於軟化點的溫度下，進行第一次預燒結的步驟；以及在真空狀態下，以軟化點至比軟化點高20℃的溫度對預燒結的玻璃成形體進行第二次燒結的步驟。 According to an embodiment of the present invention, the method may include a step a of forming and processing a glass paste to which a phosphor is added, followed by drying to form a glass molded body, and a step b of sintering the glass formed body. Wherein, the step of sintering the glass formed body may include: performing a first pre-sintering step at a temperature lower than a softening point; and, in a vacuum state, a softening point to a temperature higher than a softening point by 20 ° C The sintered glass formed body is subjected to a second sintering step.
根據本發明的再一實施例，LED用玻璃的製備方法可包括：步驟a，形成包含了由低熔點玻璃料及高熔點玻璃料混合而成的玻璃料的玻璃生胚片；以及步驟b，對玻璃生胚片進行燒結。其中，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結，當進行燒結時，高熔點玻璃料的形狀可保持不變。 According to still another embodiment of the present invention, a method for preparing a glass for LED may include: step a, forming a glass green sheet comprising a glass frit mixed with a low-melting glass frit and a high-melting glass frit; and step b, The glass green sheets are sintered. Among them, sintering is performed at a softening temperature higher than the softening temperature of the low-melting glass frit and less than the high-melting glass frit, and the shape of the high-melting glass frit can be maintained when sintering is performed.
根據本發明的另一實施例，LED用玻璃的製備方法可包括：步驟a，形成包含高熔點玻璃料的第一玻璃生胚片；步驟b，形成包含低熔點玻璃料的第二玻璃生胚片；步驟c，交替地層疊第一玻璃生胚片及第二玻璃生胚片；以及步驟d，在對已層疊的第一玻璃生胚片及第二玻璃生胚片進行壓接之後，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結。其中，當進行燒結時，上述高熔點玻璃料的形狀可保持不變。 According to another embodiment of the present invention, a method for preparing a glass for LED may include: step a, forming a first glass green sheet containing a high-melting glass frit; and step b, forming a second glass green body containing a low-melting glass frit a step c, alternately laminating the first glass green sheet and the second glass green sheet; and step d, after crimping the laminated first glass green sheet and the second glass green sheet, Sintering is performed at a softening temperature of the low-melting glass frit above and below the softening temperature of the high-melting glass frit. Among them, when sintering is performed, the shape of the above-mentioned high-melting glass frit can be kept constant.
根據本發明的還一實施例，LED用玻璃的製備方法可包括：步驟a，在基板上形成包含高熔點玻璃料的高熔點玻璃生胚片；步驟b，在高熔點玻璃生胚片上層疊包含高熔點玻璃料及低熔點玻璃料的多個玻璃生胚片；步驟c，在對已層疊的多個玻璃生胚片進行壓接之後，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結；以及步驟d，從基板分離步驟c的結果物。 According to still another embodiment of the present invention, a method for preparing a glass for LED may include: step a, forming a high-melting glass green plate containing a high-melting glass frit on a substrate; and step b, laminating on the high-melting glass green plate a plurality of glass green sheets of a high melting point glass frit and a low melting point glass frit; step c, after crimping the plurality of laminated glass green sheets, above a softening temperature of the low melting glass frit and less than a high melting point frit Sintering at a softening temperature; and step d, separating the result of step c from the substrate.
根據本發明的一實施例，當製備LED用玻璃時，在小於軟化點的溫度下，進行預燒結，來使玻璃成形體收縮的比率減少到1至5%，從而將開放的氣孔通道(open pore channel)形成至上述玻璃成形體的內部，對於預燒結的玻璃成形體，將溫度維持在軟化點附近，或慢慢地提高溫度，並進行真空燒結，來在玻璃成形體的整個區域中製作均勻的溫度曲線，從而可控制在玻璃成形體的邊緣區域中的急劇的收縮，並阻隔由此在這部分中生成閉合的氣孔，從而可完全地去除氣孔。如上所述，根據本發明的一實施例，可具有無氣孔的無孔結構，從而可將通過後加工的裂紋不良最小化，並使透射率及光提取效率最大化。 According to an embodiment of the present invention, when the glass for LED is prepared, pre-sintering is performed at a temperature lower than the softening point to reduce the shrinkage ratio of the glass formed body to 1 to 5%, thereby opening the open pore passage (open The pore channel is formed in the inside of the glass molded body, and the pre-sintered glass molded body is maintained in the vicinity of the softening point, or the temperature is gradually increased, and vacuum sintering is performed to produce the entire glass molded body. A uniform temperature profile makes it possible to control a sharp contraction in the edge region of the glass shaped body and to thereby block the formation of closed pores in this portion, so that the pores can be completely removed. As described above, according to an embodiment of the present invention, it is possible to have a non-porous structure without pores, thereby minimizing crack defects by post-processing and maximizing transmittance and light extraction efficiency.
並且，根據本發明的一實施例，在混合低熔點玻璃料及高熔點玻璃料來形成玻璃生胚片的方法和交替地層疊包含高熔點玻璃料的第一玻璃生胚片和包含低熔點玻璃料的第二玻璃生胚片的方法中，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，對玻璃生胚片進行燒結，從而可通過將高熔點玻璃料的形狀保持不變，來將玻璃急劇收縮並翹起的現象最小化。並且，將高熔點玻璃料的形狀保持不變，從而可防止薄片的邊緣區域捲曲的捲曲現象(curling)。 Moreover, according to an embodiment of the present invention, a method of forming a glass green plate by mixing a low-melting glass frit and a high-melting glass frit, and alternately laminating a first glass green plate containing a high-melting glass frit and containing a low-melting glass frit In the method of the second glass green sheet, the glass green sheets are sintered at a softening temperature above the softening temperature of the low melting glass frit and less than the softening temperature of the high melting glass frit, thereby maintaining the shape of the high melting glass frit It does not change to minimize the phenomenon of sharp shrinkage and lifting of the glass. Further, the shape of the high-melting glass frit is kept constant, so that the curling of the curling of the edge portion of the sheet can be prevented.
並且，根據本發明的一實施例，在基板上形成包含高熔點玻璃料 的高熔點玻璃生胚片，從而無離型劑也可從基板容易地分離玻璃，並且，層疊由高熔點玻璃料及低熔點玻璃料混合而成的玻璃生胚片，從而可提高玻璃的強度。 And, according to an embodiment of the present invention, forming a high melting point glass frit on the substrate The high-melting glass raw green sheet can easily separate the glass from the substrate without a release agent, and laminate the glass green sheets mixed with the high-melting glass frit and the low-melting glass frit to increase the strength of the glass.
200‧‧‧真空加熱裝置 200‧‧‧Vacuum heating device
210‧‧‧真空腔室 210‧‧‧vacuum chamber
215‧‧‧閘閥 215‧‧‧ gate valve
220‧‧‧真空吸盤 220‧‧‧vacuum suction cup
230‧‧‧升降單元 230‧‧‧ Lifting unit
235‧‧‧頂升銷 235‧‧‧ top sales
240‧‧‧加熱器 240‧‧‧heater
250‧‧‧真空泵 250‧‧‧vacuum pump
S210~S230、S310~S340、S410~S440‧‧‧步驟 S210~S230, S310~S340, S410~S440‧‧‧ steps
圖1為依次表示本發明第一實施例的LED用玻璃的製備過程的流程圖。 Fig. 1 is a flow chart sequentially showing the preparation process of the glass for LED of the first embodiment of the present invention.
圖2為用於說明本發明第一實施例的真空燒結過程的工序示意圖。 Fig. 2 is a schematic view showing the steps of the vacuum sintering process of the first embodiment of the present invention.
圖3為依次表示本發明第二實施例的玻璃的製備過程的流程圖。 Fig. 3 is a flow chart sequentially showing the preparation process of the glass of the second embodiment of the present invention.
圖4為依次表示本發明第三實施例的LED用玻璃的製備過程的流程圖。 Fig. 4 is a flow chart sequentially showing the preparation process of the glass for LED of the third embodiment of the present invention.
以下，參照附圖詳細地說明本發明的優選實施例，以至於本發明所屬技術領域的普通技術人員可簡單地實施的程度。為了明確地說明本發明，省略了與本發明無關的部分，在說明書全文中，對於相同的結構要素，標註相同的附圖標記。並且，在說明各實施例的過程中，對於與其他實施例相同的結構，進行簡單說明或省略其說明。 DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the accompanying drawings, so that those skilled in the art to which the present invention pertains can be easily implemented. In order to clearly explain the present invention, parts that are not related to the present invention are omitted, and the same reference numerals are given to the same structural elements throughout the specification. Further, in the course of explaining the respective embodiments, the same configurations as those of the other embodiments will be briefly described or omitted.
在本說明書中，當記載為一個結構要素位於另一結構要素「上」時，不僅包括位於另一結構要素「正上方」的情況，還包括它們之間還存在其他結構要素的情況。並且，為了便於說明，附圖中出現的各個結構的大小等以任意的方式示出，因此本發明不一定局限於圖中所示。 In the present specification, when one structural element is referred to as being "on" another structural element, it is not only included in the case where the other structural element is "directly above" but also includes other structural elements. Also, for convenience of explanation, the sizes and the like of the respective structures appearing in the drawings are shown in an arbitrary manner, and thus the present invention is not necessarily limited to the drawings.
即，說明書中記載的特徵形狀、結構及特性應理解為在不脫離本發明的思想及範圍的情況下，能夠以從一實施例變更為另一實施例的方式實現，且個別結構要素的位置或配置也可在不脫離本發明的思想及範圍的情況下，進行變更。因此，如下所述的詳細的說明不應解釋為局限性的意思，本發明的範圍應接受為包括發明要求保護範圍中的方案所請求的範圍及與其等同的所有範圍。 In other words, the features, structures, and characteristics of the present invention are to be understood as being changed from one embodiment to another, and the position of the individual structural elements can be changed without departing from the spirit and scope of the invention. Changes may be made without departing from the spirit and scope of the invention. Therefore, the following detailed description is not to be construed as a limitation, and the scope of the invention
進行預燒結的LED用玻璃的製備方法 Method for preparing pre-sintered LED glass
圖1作為依次表示本發明第一實施例的LED用玻璃的製備過程的流程圖，本實施例的LED用玻璃的製備方法包括玻璃成形體形成步驟S210、預燒結步驟S220及真空燒結步驟S230。 1 is a flow chart sequentially showing a process of preparing a glass for LED according to a first embodiment of the present invention. The method for producing a glass for LED of the present embodiment includes a glass formed body forming step S210, a pre-sintering step S220, and a vacuum sintering step S230.
首先，進行玻璃成形體形成步驟S210，對添加有螢光體的玻璃漿料進行成形及加工之後，進行乾燥來形成玻璃生胚片等玻璃成形體。 First, the glass molded body forming step S210 is performed, and the glass paste to which the phosphor is added is molded and processed, and then dried to form a glass molded body such as a glass green sheet.
接著，進行預燒結步驟S220，在小於軟化點的溫度下，對玻璃成形體進行第一次燒結。像這樣，進行預燒結來使玻璃成形體僅收縮1 ~5%，從而將開放的氣孔通道形成至上述玻璃成形體的內部。 Next, a pre-sintering step S220 is performed to sinter the glass formed body at a temperature lower than the softening point. In this way, pre-sintering is performed to shrink the glass molded body only 1 ~5%, thereby forming an open pore passage into the inside of the above glass formed body.
在本實施例中，玻璃成形體的軟化點根據玻璃料的含量略不同，但可將黏度為107.6泊(poise)的溫度定義為軟化點，優選地，可在500~750℃溫度下，進行預燒結。這是因為在預燒結溫度小於500℃的情況下，玻璃成形體的收縮無法滿足目標值的擔憂多，在預燒結溫度大於750℃的情況下，因過度的收縮而使開放的氣孔通道崩潰的擔憂多。 In the present embodiment, the softening point of the glass formed body is slightly different depending on the content of the glass frit, but a temperature at which the viscosity is 10 7.6 poise can be defined as a softening point, and preferably, at a temperature of 500 to 750 ° C. Pre-sintering is carried out. This is because, in the case where the pre-sintering temperature is less than 500 ° C, there is a concern that the shrinkage of the glass formed body cannot satisfy the target value, and in the case where the pre-sintering temperature is more than 750 ° C, the open pore passage collapses due to excessive shrinkage. Worried.
其次，進行真空燒結步驟S230，在真空狀態下，以軟化點至比軟化點高約20℃的溫度對預燒結的玻璃成形體進行第二次燒結，具體地，能夠以600~850℃進行燒結。其中，在燒結溫度低於軟化點溫度的情況下，在燒結的玻璃料中產生大量的氣泡，從而有可能降低透光率及光提取效率，相反，在燒結溫度比軟化點大20℃來過高的情況下，有可能在螢光體上發生變色。 Next, a vacuum sintering step S230 is performed to secondarily sinter the pre-sintered glass molded body at a temperature from a softening point to a softening point of about 20 ° C in a vacuum state, specifically, sintering at 600 to 850 ° C. . Wherein, in the case where the sintering temperature is lower than the softening point temperature, a large amount of bubbles are generated in the sintered glass frit, which may lower the light transmittance and the light extraction efficiency, and conversely, the sintering temperature is 20 ° C higher than the softening point. In the high case, it is possible to cause discoloration on the phosphor.
圖2作為用於說明真空燒結過程的工序示意圖，參照圖2，預燒結的玻璃成形體G借助真空加熱裝置200來實現真空燒結。此時，預燒結的玻璃成形體G安裝於真空吸盤220上，上述真空吸盤220安裝於以真空狀態維持的真空腔室210的內部。這種玻璃成形體G通過閘閥215移送至真空腔室210的內部來安裝於真空吸盤220上。 2 is a schematic view showing a process of a vacuum sintering process. Referring to FIG. 2, the pre-sintered glass molded body G is vacuum sintered by means of a vacuum heating device 200. At this time, the pre-sintered glass molded body G is attached to the vacuum chuck 220, and the vacuum chuck 220 is attached to the inside of the vacuum chamber 210 maintained in a vacuum state. This glass molded body G is transferred to the inside of the vacuum chamber 210 through the gate valve 215 to be mounted on the vacuum chuck 220.
在這種真空吸盤220的內部安裝有加熱器240，上述加熱器240用於以燒結溫度對玻璃成形體G進行加熱。這種加熱器240能夠以分割成多個的方式設計而成，使得這種加熱器240可實現局部性的加熱，但並不局限於此。並且，在真空吸盤220的下部安裝有升降單元230，上述升降單元230具有用於控制玻璃成形體G的高度的頂升銷235。並且，在真空腔室210的一側下端設置有用於調節真空腔室210內部的真空度的真空泵250。 Inside the vacuum chuck 220, a heater 240 for heating the glass formed body G at a sintering temperature is attached. Such a heater 240 can be designed in a plurality of divisions such that the heater 240 can achieve localized heating, but is not limited thereto. Further, a lifting unit 230 is attached to a lower portion of the vacuum chuck 220, and the lifting unit 230 has a jacking pin 235 for controlling the height of the glass forming body G. Further, a vacuum pump 250 for adjusting the degree of vacuum inside the vacuum chamber 210 is provided at a lower end of one side of the vacuum chamber 210.
如上所述，在本發明中，對於預燒結的玻璃成形體G，以軟化點至比軟化點高約20℃的溫度，即，在將溫度維持為軟化點附近，或以1℃/min以下的升溫速度逐漸提高溫度來進行燒結，因而在玻璃成形體G的整個區域中可製作均勻的溫度曲線。由此，可控制在玻璃成形體G的邊緣區域中的急劇的收縮，且可阻斷閉合氣孔的生成，因而可完全地去除氣孔。 As described above, in the present invention, the pre-sintered glass formed body G has a softening point to a temperature higher than the softening point by about 20 ° C, that is, the temperature is maintained near the softening point, or at 1 ° C/min or less. The temperature rise rate is gradually increased by temperature to perform sintering, so that a uniform temperature profile can be produced in the entire region of the glass formed body G. Thereby, sharp shrinkage in the edge region of the glass formed body G can be controlled, and generation of the closed pores can be blocked, so that the pores can be completely removed.
另一方面，在本發明中，可使用由熔融點不同的兩種以上混合而成的玻璃料，尤其，可使用玻璃料相互間的熔融點的差異大的玻璃料。像這樣，若利用由熔融點不同的兩種以上混合而成的玻璃料來進行真空燒結，則玻璃料相互間的熔融點不同，從而可防止急劇收縮。 On the other hand, in the present invention, a glass frit in which two or more kinds of different melting points are mixed can be used, and in particular, a glass frit having a large difference in melting points between the glass frits can be used. In this manner, when vacuum sintering is performed by using a glass frit in which two or more kinds of melting points are mixed, the melting points of the glass frits are different from each other, and rapid shrinkage can be prevented.
與此又不同，在本發明中，在進行真空燒結過程時，還可通過在起始溫度附近維持燒結溫度曲線之後，以1℃/min以下的速度升溫來 逐漸地實現收縮，從而阻斷閉合氣孔的生成，由此，完全去除氣孔。 In contrast to this, in the present invention, when the vacuum sintering process is performed, the temperature can be raised at a rate of 1 ° C/min or less after maintaining the sintering temperature profile near the initial temperature. Shrinkage is gradually achieved, thereby blocking the formation of closed pores, thereby completely removing the pores.
像這樣，LED用玻璃具有無氣孔的無孔結構，從而可將通過後加工的裂紋不良最小化，並使透射率及光提取效率最大化。 As such, the glass for LED has a non-porous, non-porous structure, thereby minimizing crack defects through post-processing, and maximizing transmittance and light extraction efficiency.
以下，通過具體實驗例對本實施例的結構及作用進行更詳細的說明。 Hereinafter, the structure and action of the present embodiment will be described in more detail by way of specific experimental examples.
實驗例1 Experimental example 1
對在表1中記載的玻璃料中以相同的量添加螢光體而製成的玻璃漿料進行成形及加工之後，在50℃溫度下，進行乾燥來形成玻璃成形體。其次，在620℃溫度下，將玻璃成形體預燒結30分鐘之後，在維持成3Torr的真空腔室內部中，在830℃溫度下，將真空燒結進行80分鐘，來製備了顏色轉換玻璃。 The glass paste prepared by adding a phosphor in the same amount to the glass frit described in Table 1 was molded and processed, and then dried at a temperature of 50 ° C to form a glass molded body. Next, the glass molded body was pre-sintered at a temperature of 620 ° C for 30 minutes, and then vacuum-sintered at a temperature of 830 ° C for 80 minutes in a vacuum chamber maintained at 3 Torr to prepare a color conversion glass.
實驗例2 Experimental example 2
對在表1中記載的玻璃料中以相同的量添加螢光體而製成的玻璃漿料進行成形及加工之後，在50℃溫度下，進行乾燥來形成玻璃成形體。其次，在680℃溫度下，將玻璃成形體預燒結30分鐘之後，在維持成4Torr的真空腔室內部中，在820℃溫度下，將真空燒結進行80分鐘，來製備了顏色轉換玻璃。 The glass paste prepared by adding a phosphor in the same amount to the glass frit described in Table 1 was molded and processed, and then dried at a temperature of 50 ° C to form a glass molded body. Next, the glass molded body was pre-sintered at a temperature of 680 ° C for 30 minutes, and then vacuum-sintered at a temperature of 820 ° C for 80 minutes in a vacuum chamber maintained at 4 Torr to prepare a color conversion glass.
實驗例3 Experimental example 3
對在表1中記載的玻璃料中以相同的量添加螢光體而製成的玻璃漿料進行成形及加工之後，在50℃溫度下，進行乾燥來形成玻璃成形體。其次，在650℃溫度下，將玻璃成形體預燒結40分鐘之後，在維持成6Torr的真空腔室內部中，在830℃溫度下，將真空燒結進行110分鐘，來製備了顏色轉換玻璃。 The glass paste prepared by adding a phosphor in the same amount to the glass frit described in Table 1 was molded and processed, and then dried at a temperature of 50 ° C to form a glass molded body. Next, the glass molded body was pre-sintered at a temperature of 650 ° C for 40 minutes, and then vacuum-sintered at a temperature of 830 ° C for 110 minutes in a vacuum chamber maintained at 6 Torr to prepare a color conversion glass.
實驗例4 Experimental example 4
對在表1中記載的玻璃料中以相同的量添加螢光體而製成的玻璃漿料進行成形及加工之後，在45℃溫度下，進行乾燥來形成玻璃成形體。其次，在710℃溫度下，將玻璃成形體預燒結50分鐘之後，在維持成7Torr的真空腔室內部中，在810℃溫度下，將真空燒結進行100分鐘，來製備了顏色轉換玻璃。 The glass paste prepared by adding a phosphor in the same amount to the glass frit described in Table 1 was molded and processed, and then dried at a temperature of 45 ° C to form a glass molded body. Next, the glass molded body was pre-sintered at a temperature of 710 ° C for 50 minutes, and then vacuum-sintered at a temperature of 810 ° C for 100 minutes in a vacuum chamber maintained at 7 Torr to prepare a color conversion glass.
比較例1 Comparative example 1
對在表1中記載的玻璃料中以相同的量添加螢光體而製成的玻璃漿料進行成形及加工之後，在45℃溫度下，進行乾燥來形成玻璃成形體。其次，在760℃溫度下，將玻璃成形體預燒結20分鐘之後，在維持成4Torr的真空腔室內部中，在830℃溫度下，將真空燒結進行90分鐘，來製備了顏色轉換玻璃。 The glass paste prepared by adding a phosphor in the same amount to the glass frit described in Table 1 was molded and processed, and then dried at a temperature of 45 ° C to form a glass molded body. Next, the glass molded body was pre-sintered at a temperature of 760 ° C for 20 minutes, and then vacuum-sintered at a temperature of 830 ° C for 90 minutes in a vacuum chamber maintained at 4 Torr to prepare a color conversion glass.
表1
表2表示實施例1至實施例4及比較例1的顏色轉換玻璃的物性評價結果，通過紫外線/可見光光譜測定(紫外可見吸收光譜測定儀(UV-vis meter)，凱瑞(cary)公司)來測定了波長為400nm~800nm的透光度。 Table 2 shows the results of physical property evaluation of the color conversion glasses of Examples 1 to 4 and Comparative Example 1, which were measured by ultraviolet/visible spectroscopy (UV-vis meter, cary company) The transmittance at a wavelength of 400 nm to 800 nm was measured.
參照表1及表2，可知在實施例1至實施例4的顏色轉換玻璃的情況下，透射率均為95%以上，這是因為氣孔完美地得到去除。相反，在比較例1的顏色轉換玻璃的情況下，透射率測定為85.7%，可知未達到目標值，這是因為預燒結溫度超過在本發明中公開的溫度範圍，從而因過度收縮而使開放的氣孔通道崩潰，進而生成閉合氣孔而導致透射率降低。 Referring to Tables 1 and 2, it is understood that in the case of the color conversion glass of Examples 1 to 4, the transmittance is 95% or more because the pores are perfectly removed. In contrast, in the case of the color conversion glass of Comparative Example 1, the transmittance was measured to be 85.7%, and it was found that the target value was not reached because the pre-sintering temperature exceeded the temperature range disclosed in the present invention, and was opened due to excessive shrinkage. The stomata channel collapses, which in turn creates closed pores resulting in reduced transmission.
用於將翹起現象的產生最小化的玻璃的製備方法 Method for preparing glass for minimizing the occurrence of lift-up phenomenon
根據本發明的第二實施例涉及在製備玻璃的過程中控制在燒結步驟中的急劇的收縮來將翹起現象的產生最小化的方法。本實施例的玻璃的製備方法與上述的方法類似地，包括形成玻璃成形體，即，玻璃生胚片之後，對玻璃生胚片進行燒結的步驟。 A second embodiment according to the present invention relates to a method of controlling the sharp shrinkage in the sintering step to minimize the occurrence of the lift-up phenomenon in the process of preparing the glass. The method for producing the glass of the present embodiment is similar to the above-described method, and includes the step of sintering the glass green sheets after forming the glass shaped body, that is, the glass green sheets.
在本實施例中，混合低熔點玻璃料及高熔點玻璃料來形成玻璃生胚片。 In this embodiment, a low-melting glass frit and a high-melting glass frit are mixed to form a glass green sheet.
在玻璃料的總重量中，高熔點玻璃料的含量優選為50~90%。在高熔點玻璃料的含量小於50%的情況下，與低熔點玻璃料的含量相比，高熔點玻璃料的含量相對地降低，從而基於低熔點玻璃料確定玻璃的特性。即，在燒結步驟中，低熔點玻璃料熔融，且玻璃急劇地收縮，從而可產生捲曲現象及翹起現象。相反，在高熔點玻璃料的含量大於90%的情況下，基於低熔點玻璃料的緻密化有可能不足。 The content of the high-melting glass frit is preferably from 50 to 90% in the total weight of the glass frit. In the case where the content of the high-melting glass frit is less than 50%, the content of the high-melting glass frit is relatively lowered as compared with the content of the low-melting glass frit, thereby determining the characteristics of the glass based on the low-melting glass frit. That is, in the sintering step, the low-melting glass frit is melted, and the glass is sharply shrunk, so that a curling phenomenon and a lifting phenomenon can be generated. On the contrary, in the case where the content of the high-melting glass frit is more than 90%, the densification based on the low-melting glass frit may be insufficient.
低熔點玻璃料的燒結作業的溫度為約500~800℃，可包含含有鹼土族氧化物(MgO、CrO及BaO)的玻璃成分，但並不局限於此。作為高熔點玻璃料，可使用燒結作業的溫度為約800℃以上的玻璃，更具體地，優選地，使用屬於硼矽酸鹽的硼矽酸鹽(borosilicate)類成分。硼矽酸鹽類成分可適用於高熔點，並具有強度及耐久性優秀的優點，可將鈣鋁硼矽酸鹽、鈣鈉硼矽酸鹽等單獨使用或混合兩種以上來使用。 The sintering temperature of the low-melting glass frit is about 500 to 800 ° C, and may include a glass component containing an alkaline earth oxide (MgO, CrO, and BaO), but is not limited thereto. As the high-melting-point glass frit, a glass having a sintering operation temperature of about 800 ° C or higher can be used, and more specifically, a borosilicate-based component belonging to the borosilicate is preferably used. The borosilicate component can be used for a high melting point and has excellent strength and durability. Calcium aluminum borosilicate, calcium sodium borosilicate, or the like can be used alone or in combination of two or more.
為了使用於LED的封裝部件等，玻璃生胚片還可包含螢光體。作為螢光體可利用公知的多種螢光體，例如，可利用釔鋁石榴石(YAG)類、鑥鋁石榴石(LuAg)類、鋱鋁石榴石(TAG)類、矽酸鹽類、賽隆(SiAlON)類、正矽酸鋇(BOS)類、氮氧化物((oxy)nitride)類等的螢光體。相對於100重量百分比的漿料，可混合大致10~50重量百分比左右的螢光體，但並不是必須限定於此的，可考慮顏色轉換程度等來調節其含量。並且，上述螢光體的直徑可以為5~30μm，但並不是必須限定於此的。 In order to be used for a package member or the like of an LED, the glass green sheet may further contain a phosphor. As the phosphor, various known phosphors can be used. For example, yttrium aluminum garnet (YAG), yttrium aluminum garnet (LuAg), yttrium aluminum garnet (TAG), silicate, and race can be used. Phosphors such as SiAlON, BOS, and oxynitride. The phosphor may be mixed in an amount of about 10 to 50% by weight with respect to 100% by weight of the slurry, but it is not necessarily limited thereto, and the content thereof may be adjusted in consideration of the degree of color conversion or the like. Further, the diameter of the phosphor may be 5 to 30 μm, but it is not necessarily limited thereto.
在層疊包含螢光體的玻璃生胚片的情況下，可判別螢光體的含量分佈圖之後，均勻地組合螢光體的含量分佈圖來進行層疊。通常，螢光體無法在玻璃生胚片中均勻地分散，因而在玻璃生胚片的中央部分和邊緣部分中的螢光體的分佈圖有可能不均勻。能夠以使玻璃生胚片的相同的面朝向一個方向的方式進行層疊，還能夠以使薄片的上部面或下部面錯開一次以上的方式進行層疊。 When the glass green sheets containing the phosphors are laminated, the content distribution map of the phosphors can be discriminated, and then the content distribution map of the phosphors can be uniformly combined and laminated. In general, the phosphor cannot be uniformly dispersed in the glass green sheets, and thus the distribution map of the phosphors in the central portion and the edge portion of the glass green sheets may be uneven. It is also possible to laminate the same surface of the glass green sheets in one direction, and to laminate the upper surface or the lower surface of the sheet one or more times.
像這樣，形成玻璃生胚片之後，對玻璃生胚片進行燒結。在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結。例如，燒結溫度可以為大致500~800℃，進行燒結的時間可以為大致10~100分鐘，但並不局限於此。 In this manner, after the glass green sheets are formed, the glass green sheets are sintered. Sintering is carried out at a softening temperature above the softening temperature of the low melting glass frit and less than the high melting glass frit. For example, the sintering temperature may be approximately 500 to 800 ° C, and the sintering time may be approximately 10 to 100 minutes, but is not limited thereto.
這種情況下，當進行燒結時，高熔點玻璃料的形狀保持不變，從而可抑制玻璃急劇地收縮，且可將翹起現象的產生最小化。並且，當進行燒結時，可隨著低熔點玻璃料熔融，通過緻密化填充氣孔，由此，用肉眼看不出高熔點玻璃料，從而可呈現玻璃的透明性。 In this case, when sintering is performed, the shape of the high-melting glass frit remains unchanged, so that the glass can be suppressed from being sharply shrunk, and the occurrence of the lift-up phenomenon can be minimized. Further, when sintering is performed, the low-melting glass frit can be melted, and the pores can be filled by densification, whereby the high-melting glass frit can be seen with the naked eye, and the transparency of the glass can be exhibited.
在燒結溫度低於低熔點玻璃料的軟化溫度的情況下，由於燒結體的緻密性不足，隨著氣孔率增加，可產生使玻璃的強度及透射率降低的問題，相反，在燒結溫度為上述高熔點玻璃料的軟化溫度以上的情況下，可發生螢光體粉末的劣化或者玻璃的翹起。 When the sintering temperature is lower than the softening temperature of the low-melting glass frit, since the compactness of the sintered body is insufficient, as the porosity increases, a problem of lowering the strength and transmittance of the glass may occur. On the contrary, the sintering temperature is as described above. When the softening temperature of the high-melting glass frit is equal to or higher than the softening temperature of the glass frit, the deterioration of the phosphor powder or the lifting of the glass may occur.
另一方面，在層疊玻璃生胚片的情況下，可使層疊體壓接之後進行燒結。壓接的薄片可縮小成大致15%以下的厚度，並在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結之後，形成為一個單片(monolithic)。此時，單片成為向寬度方向收縮成大致15~25%，並向厚度方向收縮成大致10%以下的形態。 On the other hand, in the case of laminating the glass green sheets, the laminate may be pressure-bonded and then sintered. The pressure-bonded sheet can be reduced to a thickness of approximately 15% or less and formed into a monolithic shape after sintering at a softening temperature of the low-melting glass frit and less than the softening temperature of the high-melting glass frit. At this time, the single piece shrinks to approximately 15 to 25% in the width direction and shrinks to approximately 10% or less in the thickness direction.
在本實施例中，還能夠以如下方式製備玻璃：分別形成包含低熔點玻璃料的玻璃生胚片和包含高熔點玻璃料的玻璃生胚片，並層疊玻璃生胚片之後進行燒結。 In the present embodiment, it is also possible to prepare a glass by separately forming a glass green sheet containing a low-melting glass frit and a glass green sheet containing a high-melting glass frit, and sintering the glass green sheets.
圖3為依次表示利用以如上方式分別形成的多個玻璃生胚片製備玻璃的過程的流程圖，參照圖3，首先形成包含高熔點玻璃料的第一玻璃生胚片(步驟S310)。 3 is a flow chart sequentially showing a process of preparing glass by using a plurality of glass green sheets formed separately in the above manner. Referring to FIG. 3, first glass green sheets containing a high-melting glass frit are first formed (step S310).
第一玻璃生胚片可從包含高熔點玻璃料、黏結劑及溶劑的漿料通過流延成形法來製備而成，厚度優選為100μm以下。在厚度大於100μm的情況下，由於玻璃的厚度，有可能限制層疊的薄片的數量，且有可能降低玻璃的透明度。 The first glass green plate can be prepared by a tape casting method from a slurry containing a high-melting glass frit, a binder, and a solvent, and has a thickness of preferably 100 μm or less. In the case where the thickness is more than 100 μm, it is possible to limit the number of laminated sheets due to the thickness of the glass, and it is possible to lower the transparency of the glass.
另一方面，為了用作LED用顏色轉換玻璃，第一玻璃生胚片還可包含螢光體。在後述的燒結過程中，由於低熔點玻璃料，有可能使螢光體劣化，因而為了將劣化現象最小化，優選地，螢光體與高熔點玻璃料混合而成。螢光體的種類及重量等如上所述。 On the other hand, in order to be used as a color conversion glass for LEDs, the first glass green sheets may further contain a phosphor. In the sintering process to be described later, the phosphor may be deteriorated by the low-melting glass frit. Therefore, in order to minimize the deterioration phenomenon, it is preferable that the phosphor is mixed with the high-melting glass frit. The type and weight of the phosphor are as described above.
其次，形成包含低熔點玻璃料的第二玻璃生胚片(步驟S320)。第二玻璃生胚片可從包含低熔點玻璃料、黏結劑及溶劑的漿料通過流延成形法來製備而成，其厚度優選為第一玻璃生胚片的厚度的1/2以下。在厚度大於第一玻璃生胚片厚度的1/2的情況下，有可能降低捲曲防止效果，當螢光體混合於第一玻璃生胚片時，在燒結過程中，與低熔點玻璃料、螢光體進行反應來可使螢光體劣化。 Next, a second glass green sheet containing a low-melting glass frit is formed (step S320). The second glass green plate can be prepared by a tape casting method from a slurry containing a low-melting glass frit, a binder, and a solvent, and the thickness thereof is preferably 1/2 or less of the thickness of the first glass green plate. In the case where the thickness is greater than 1/2 of the thickness of the first glass green sheet, it is possible to reduce the curl prevention effect, when the phosphor is mixed with the first glass green sheet, during the sintering process, with the low melting glass frit, The phosphor reacts to deteriorate the phosphor.
像這樣，形成第一玻璃生胚片和第二玻璃生胚片之後，交替地層疊第一玻璃生胚片和第二玻璃生胚片(步驟S330)。可在第一玻璃生胚片上形成第二玻璃生胚片，並在上述第二玻璃生胚片上形成第一玻璃 生胚片來進行層疊。並且，還可交替地層疊一個以上的第一玻璃生胚片和一個以上的第二玻璃生胚片，可考慮第一玻璃生胚片及第二玻璃生胚片的厚度來調節層疊的薄片的數量。 After the first glass green sheets and the second glass green sheets are formed as described above, the first glass green sheets and the second glass green sheets are alternately laminated (step S330). Forming a second glass green sheet on the first glass green sheet and forming a first glass on the second glass green sheet The embryonic sheets are stacked for lamination. Moreover, one or more first glass green sheets and one or more second glass green sheets may be alternately laminated, and the thickness of the first glass green sheets and the second glass green sheets may be adjusted to adjust the laminated sheets. Quantity.
最終，在壓接層疊的薄片之後，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結(步驟S340)。 Finally, after the laminated sheets are pressure-bonded, sintering is performed at a softening temperature higher than the softening temperature of the low-melting glass frit and less than the softening temperature of the high-melting glass frit (step S340).
如上所述，在本實施例中，混合低熔點玻璃料及高熔點玻璃料來形成玻璃生胚片，或分別形成包含低熔點玻璃料的玻璃生胚片和包含高熔點玻璃料的玻璃生胚片來層疊之後，對玻璃生胚片進行燒結來製備玻璃，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結，從而通過將高熔點玻璃料的形狀保持不變，來可控制玻璃急劇地收縮的現象和翹起的現象。像這樣，將高熔點玻璃料的形狀保持不變，從而可防止薄片的邊緣區域捲曲的捲曲現象。 As described above, in the present embodiment, the low-melting glass frit and the high-melting glass frit are mixed to form a glass green sheet, or a glass green sheet containing a low-melting glass frit and a glass green sheet containing a high-melting glass frit, respectively. After lamination, the glass green sheets are sintered to prepare glass, which is sintered at a softening temperature above the softening temperature of the low melting glass frit and less than the high melting glass frit, thereby maintaining the shape of the high melting glass frit. To control the phenomenon of sharp shrinkage of the glass and the phenomenon of lifting. In this manner, the shape of the high-melting glass frit is kept constant, so that the curling phenomenon of the curling of the edge portion of the sheet can be prevented.
與基板的分離容易的LED用玻璃的製備方法 Method for preparing glass for LED which is easy to separate from substrate
圖4為依次表示本發明第三實施例的LED用玻璃的製備過程的流程圖，參照圖4，本實施例的LED用玻璃的製備方法包括：步驟S410，在基板上形成高熔點玻璃生胚片；步驟S420，對多個玻璃生胚片進行層疊；步驟S430，對已層疊的薄片進行燒結；以及步驟S440，從基板分離玻璃。 4 is a flow chart sequentially showing a process for preparing a glass for LED according to a third embodiment of the present invention. Referring to FIG. 4, a method for preparing a glass for LED of the present embodiment includes: step S410, forming a high-melting glass green embryo on a substrate. a sheet; step S420, laminating a plurality of glass green sheets; step S430, sintering the stacked sheets; and step S440, separating the glass from the substrate.
首先，在基板上形成包含高熔點玻璃料的高熔點玻璃生胚片(步驟S410)。高熔點玻璃生胚片可從包含高熔點玻璃料、黏結劑及溶劑的漿料通過流延成形法來製備而成，漿料的組成可以為40~50重量百分比的高熔點玻璃料、5~10重量百分比的黏結劑、40~55重量百分比的溶劑，但並不局限於此。在漿料中還可包含螢光體，這種情況下，可混合約5~30重量百分比左右的螢光體，但考慮顏色轉換程度而可調節其含量。 First, a high-melting glass green plate containing a high-melting glass frit is formed on a substrate (step S410). The high-melting glass green sheet can be prepared by a tape casting method from a slurry containing a high-melting glass frit, a binder and a solvent, and the composition of the slurry can be 40 to 50% by weight of a high-melting glass frit, 5~ 10% by weight of the binder, 40 to 55% by weight of the solvent, but is not limited thereto. A phosphor may also be included in the slurry. In this case, about 5 to 30% by weight of the phosphor may be mixed, but the content may be adjusted in consideration of the degree of color conversion.
在本實施例中的高熔點玻璃料作為燒結作業的溫度為約900℃以上的玻璃，可適用於高熔點，只要是強度及耐久性優秀的玻璃料，就可無限制地使用，例如，可將鈣鋁硼矽酸鹽、鈣鈉硼矽酸鹽等單獨使用或混合兩種以上來使用。 The high-melting-point glass frit in the present embodiment can be applied to a glass having a temperature of about 900 ° C or higher for sintering, and can be applied to a high melting point. As long as it is a glass frit having excellent strength and durability, it can be used without limitation, for example, Calcium aluminum borosilicate, calcium sodium borosilicate, or the like may be used alone or in combination of two or more.
其次，在高熔點玻璃生胚片上層疊包含高熔點玻璃料及低熔點玻璃料的多個玻璃生胚片(步驟S420)。這可從包含高熔點玻璃料及低熔點玻璃料的漿料通過流延成形法來製備而成，漿料的組成可以為40~50重量百分比的高熔點玻璃料及低熔點玻璃料、5~10重量百分比的黏結劑、40~55重量百分比的溶劑，但並不局限於此。在包含高熔點玻璃料及低熔點玻璃料的漿料中，考慮顏色轉換程度等來還可包含螢光體。 Next, a plurality of glass green sheets including a high-melting glass frit and a low-melting glass frit are laminated on the high-melting glass green sheets (step S420). This can be prepared by a tape casting method from a slurry containing a high melting point glass frit and a low melting point glass frit. The composition of the slurry can be 40 to 50 weight percent of high melting glass frit and low melting point glass frit, 5 to 10 weight. A percentage of the binder, 40 to 55 weight percent of the solvent, but is not limited thereto. In the slurry containing the high-melting glass frit and the low-melting glass frit, a phosphor may be contained in consideration of the degree of color conversion or the like.
在本實施例中的低熔點玻璃料作為燒結作業的溫度為約600~800℃的玻璃，可包含含有鹼土族氧化物(MgO、CrO及BaO)的玻璃成分，但並不局限於此。 The low-melting glass frit in the present embodiment may contain a glass component containing an alkaline earth oxide (MgO, CrO, and BaO) as a glass having a temperature of about 600 to 800 ° C in the sintering operation, but is not limited thereto.
在本實施例中，優選地，在形成於高熔點玻璃生胚片的上部表面的玻璃生胚片的高熔點玻璃料及低熔點玻璃料的總重量中，包含50重量百分比以上的高熔點玻璃料。更優選地，包含80重量百分比以上的高熔點玻璃料，對此，依次層疊的玻璃生胚片包含70重量百分比以上的高熔點玻璃料，在接著層疊的玻璃生胚片中，高熔點玻璃料的含量為50重量百分比以上。 In the present embodiment, preferably, the high-melting glass frit of 50% by weight or more is contained in the total weight of the high-melting glass frit and the low-melting glass frit of the glass green sheet formed on the upper surface of the high-melting glass green sheet. . More preferably, it contains 80% by weight or more of a high-melting glass frit, and the glass green sheets which are sequentially laminated comprise 70% by weight or more of a high-melting glass frit, and in the subsequently laminated glass green sheets, a high-melting glass frit The content is 50% by weight or more.
像這樣，在各玻璃生胚片中，從基板越遠，高熔點玻璃料的含量越少，在形成層疊的多個玻璃生胚片的高熔點玻璃料含量為50重量百分比以上的玻璃生胚片的情況下，從上述基板可容易分離玻璃。並且，混合使用高熔點玻璃料及低熔點玻璃料，從而可提高玻璃的強度。 As described above, in each of the glass green sheets, the farther from the substrate, the smaller the content of the high-melting glass frit, the glass green embryo having a high-melting glass frit content of 50% by weight or more in forming the plurality of laminated glass green sheets. In the case of a sheet, the glass can be easily separated from the above substrate. Further, a high-melting glass frit and a low-melting glass frit are used in combination to increase the strength of the glass.
在高熔點玻璃生胚片上層疊包含高熔點玻璃料及低熔點玻璃料的多個玻璃生胚片之後，對層疊的薄片進行壓接及燒結(步驟S430)。若對已層疊的薄片進行壓接，則縮小成大致25%以下的厚度，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結之後，形成為一個單片。此時，單片成為向寬度方向收縮成大致15~22%，並向厚度方向收縮成大致10%以下的形態。 After laminating a plurality of glass green sheets including a high-melting glass frit and a low-melting glass frit on the high-melting glass green sheets, the laminated sheets are pressure-bonded and sintered (step S430). When the laminated sheet is pressure-bonded, it is reduced to a thickness of approximately 25% or less, and after sintering at a softening temperature of the low-melting glass frit or less and less than the softening temperature of the high-melting glass frit, it is formed into a single sheet. At this time, the single piece shrinks to approximately 15 to 22% in the width direction and shrinks to approximately 10% or less in the thickness direction.
燒結溫度優選為大致600~800℃，進行燒結的時間可以為大致10~100分鐘，但並不局限於此。只是，在燒結溫度大於900℃的情況下，由於超過高熔點玻璃料的軟化溫度，因而高熔點玻璃料可進行燒結來與基板進行黏結，有可能難以與所要製備的玻璃進行分離。並且，在漿料中包含螢光體的情況下，由於大於900℃的熱，有可能存在螢光體劣化的問題。 The sintering temperature is preferably approximately 600 to 800 ° C, and the sintering time may be approximately 10 to 100 minutes, but is not limited thereto. However, in the case where the sintering temperature is higher than 900 ° C, the high-melting glass frit may be sintered to adhere to the substrate due to the softening temperature exceeding the high-melting glass frit, which may be difficult to separate from the glass to be prepared. Further, in the case where the phosphor is contained in the slurry, there is a possibility that the phosphor is deteriorated due to heat of more than 900 °C.
在對已層疊的薄片進行壓接及燒結之後，從基板分離玻璃(步驟S440)。基板可由在800℃以上的高溫條件下，幾乎無變形，並對熱衝擊強的陶瓷或金屬物質形成，優選地，作為基板可使用硝酸硼(boron nitrate)或氧化鋁(aluminum oxide)。從基板分離的玻璃可用作適用於LED的玻璃或顏色轉換原材料。 After the laminated sheets are pressure-bonded and sintered, the glass is separated from the substrate (step S440). The substrate may be formed of a ceramic or a metal substance having a strong thermal shock under high temperature conditions of 800 ° C or higher, and preferably, boron nitrate or aluminum oxide may be used as the substrate. The glass separated from the substrate can be used as a glass or color conversion raw material suitable for LEDs.
如上所述，在本實施例中，在基板上形成包含高熔點玻璃料的高熔點玻璃生胚片，並層疊包含高熔點玻璃料及低熔點玻璃料的多個玻璃生胚片之後，在低熔點玻璃料的軟化溫度以上且小於高熔點玻璃料的軟化溫度下，進行燒結，從而可利用高熔點玻璃生胚片容易地分離基板和玻璃。並且，在利用包含高熔點玻璃料及低熔點玻璃料的玻璃生胚片製備玻璃的情況下，可提高玻璃的強度。 As described above, in the present embodiment, a high-melting glass green sheet containing a high-melting glass frit is formed on a substrate, and a plurality of glass green sheets including a high-melting glass frit and a low-melting glass frit are laminated, and a low melting point is formed. Sintering is performed at a softening temperature of the glass frit or less and less than the softening temperature of the high-melting glass frit, whereby the substrate and the glass can be easily separated by the high-melting glass green sheets. Further, in the case where glass is prepared from a glass green sheet containing a high-melting glass frit and a low-melting glass frit, the strength of the glass can be improved.
以上，參照附圖對本發明的優選實施例進行了說明，然而只要是本發明所屬技術領域的普通技術人員可理解在不變更本發明的技術思想或必要特徵的情況下，能夠以其他具體形態來實施本發明。因此，要理解的是，以上所述的實施例在所有方面均為例示性的，而非限定。 The preferred embodiments of the present invention have been described above with reference to the accompanying drawings. However, as those skilled in the art to which the present invention pertains, it can be understood that the present invention can be embodied in other specific forms without changing the technical spirit or essential features of the present invention. The invention is implemented. Therefore, the embodiments described above are to be considered in all respects as illustrative and not limiting.
S210~S230‧‧‧步驟 S210~S230‧‧‧Steps
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| KR1020150088934A KR101787381B1 (en) | 2015-06-23 | 2015-06-23 | Method for manufacturing the glass for light emitting diode |
| KR1020150088933A KR101722464B1 (en) | 2015-06-23 | 2015-06-23 | Manufacturing method of poreless structure phosphor in glass for light emitting diode |
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