JP5378276B2 - Method for manufacturing light emitting device - Google Patents

Description

  The present invention relates to a method for manufacturing a light emitting device having a structure in which a light emitting element is mounted on a package including a lead electrode and an electrode holding member, and the light emitting element is sealed with a sealing resin.

  In this type of light emitting device, various resins are employed as the material of the electrode holding member with emphasis on processability and lightness. In particular, liquid crystal polyester is excellent in heat resistance and thin-wall processability, and therefore can also have a function as a reflector. Further, since the light emitting element is sealed with the sealing resin, it is possible to reduce the impact from the outside and protect it from dust and moisture.

  When manufacturing such a light-emitting device, conventionally, a resin serving as an electrode holding member is integrally formed with a lead electrode by insert molding to produce a package, and the light-emitting element is electrically connected to the lead electrode and mounted on the package. Then, this light emitting element was sealed with sealing resin (for example, refer patent document 1).

Japanese Patent Laying-Open No. 2005-142236 (columns [0014] to [0016], FIG. 2)

  However, in the light emitting device manufactured in this way, the adhesion (adhesion) between the electrode holding member and the sealing resin is not always sufficient. Therefore, depending on the usage environment of the light emitting device, peeling occurs at the interface between the electrode holding member and the sealing resin, the luminance of the light emitting device is lowered, and the reliability as the light emitting device may be lowered.

  Therefore, in view of such circumstances, an object of the present invention is to provide a method for manufacturing a light-emitting device that can improve the reliability by improving the adhesion between an electrode holding member and a sealing resin.

  In order to achieve such an object, the present inventor heat-treats the electrode holding member at a stage before the light emitting element is sealed with the sealing resin in order to improve the adhesion between the electrode holding member and the sealing resin. The present invention was completed by paying attention to the above.

  That is, the invention according to claim 1 is a package manufacturing step of manufacturing a package by providing a resin electrode holding member on a lead electrode, an element mounting step of mounting a light emitting element on the lead electrode, and the electrode holding member And a device sealing process for sealing the light emitting element with the sealing resin in a form in which the sealing resin is in contact with the light emitting device. In this stage, a method of manufacturing a light emitting device in which at least the electrode holding member is heat-treated is used.

  According to a second aspect of the present invention, there is provided a package manufacturing step of manufacturing a package by providing a resin electrode holding member on a lead electrode, an element mounting step of mounting a light emitting element on the lead electrode, and the electrode holding member And a device sealing step of sealing the light emitting element with the sealing resin in a form in which the sealing resin is in contact with the light emitting device, wherein the device mounting step and the device sealing step include: In the intervening stage, at least the electrode holding member is manufactured by a method for manufacturing a light emitting device.

The invention described in claim 3 is characterized in that, in addition to the structure described in claim 1 or 2 , the electrode holding member is made of liquid crystal polyester.

In addition to the structure described in claim 3 , the invention described in claim 4 is characterized in that titanium oxide is blended in the liquid crystal polyester.

The invention described in claim 5 is characterized in that, in addition to the structure described in claim 3 or 4 , the temperature of the heat treatment for the electrode holding member is in the range of 80 to 250 ° C.

The invention according to claim 6 is characterized in that, in addition to the structure according to any one of claims 3 to 5 , the time for the heat treatment on the electrode holding member is in the range of 1 to 10 hours. To do.

Furthermore, the invention described in claim 7 is characterized in that, in addition to the structure described in any one of claims 1 to 6 , the sealing resin is a thermosetting silicone resin.

  According to the present invention, since the electrode holding member is heat-treated before the light emitting element is sealed with the sealing resin, the adhesion between the electrode holding member and the sealing resin can be enhanced. As a result, regardless of the usage environment of the light emitting device, the occurrence of a situation where peeling occurs at the interface between the electrode holding member and the sealing resin and the luminance of the light emitting device is reduced, and the reliability as the light emitting device is improved. It becomes possible.

It is a figure which shows the light-emitting device which concerns on Embodiment 1 of this invention, Comprising: (a) is the perspective view, (b) is the vertical sectional view. FIGS. 2A and 2B are process diagrams illustrating a manufacturing method of the light emitting device illustrated in FIG. 1, in which FIG. 1A is a vertical sectional view illustrating a package manufacturing process, FIG. 1B is a vertical sectional view illustrating an element mounting process, and FIG. It is a vertical sectional view showing the process. It is process drawing which shows the manufacturing method of the light-emitting device concerning a reference example , Comprising: (a) is a vertical sectional view which shows an element mounting process, (b) is a vertical sectional view which shows a package preparation process, (c) is element sealing It is a vertical sectional view showing the process.

Embodiments of the present invention will be described below.
Embodiment 1 of the Invention

  1 and 2 show Embodiment 1 of the present invention. In the first embodiment, in the method for manufacturing the light emitting device 1, the light emitting element 7 is mounted after the electrode holding member 3 is provided on the pair of lead electrodes 5 and 6.

  First, the configuration of the light emitting device 1 according to Embodiment 1 will be described, and then the method for manufacturing the light emitting device 1 will be described.

  As shown in FIG. 1, the light emitting device 1 includes a package 2, and the package 2 includes a pair of (positive and negative) lead electrodes 5 and 6 and an electrode holding member 3 made of liquid crystal polyester. Here, the electrode holding member 3 has a hexahedral body 3a, and an element mounting recess 3b is formed on the upper surface of the body 3a. Each of the lead electrodes 5 and 6 has an electrode holding member such that one end is exposed on the outer peripheral surface (side surface and bottom surface) of the main body 3a and the other end is exposed on the element mounting recess 3b. 3 is integrally formed in a form embedded in the body 3.

  Further, as shown in FIG. 1, a light emitting element 7 such as a light emitting diode is mounted on the package 2 in a form of being placed in the element placement recess 3 b of the electrode holding member 3. As shown in FIG. 1B, the light emitting element 7 has a pair of electrodes 7a and 7b, and the electrodes 7a and 7b are electrically connected to the lead electrodes 5 and 6, respectively. Further, the light emitting element 7 is sealed with a translucent sealing resin 9.

  The sealing resin 9 can be formed using various resins. Specifically, thermosetting resins and glass having excellent weather resistance and translucency such as epoxy resin, urea resin, and silicone resin are preferably used, and in terms of heat resistance, particularly thermosetting silicone resin. Is preferred. The type of this thermosetting silicone resin is not limited, but because it cures in a short time by heating, it is highly productive and encapsulates addition reaction curable silicone rubber using hydrosilylation that does not generate by-products during curing Agents are particularly preferred.

The sealing resin 9 is preferably added with a platinum group metal catalyst for the purpose of accelerating its curing. Platinum group metal-based catalysts include platinum-based, palladium-based, and rhodium-based catalysts. From the viewpoint of cost and the like, platinum-based catalysts such as platinum, platinum black, and chloroplatinic acid, such as H ₂ PtCl ₆ · mH ₂ O, K ₂ PtCl ₆ , KHPtCl ₆ · mH ₂ O, K ₂ PtCl ₄ , K ₂ PtCl ₄ · mH ₂ O, PtO ₂ · mH ₂ O (m is a positive integer), etc., and olefins And a complex with a hydrocarbon, alcohol, or vinyl group-containing organopolysiloxane. These catalysts may be used alone or in combination of two or more. The compounding amount of these catalysts may be a so-called catalytic amount, and is usually used in the range of 0.1 to 1000 ppm, preferably 0.5 to 200 ppm in terms of platinum group metal (mass) with respect to the silicone resin component. .

  Furthermore, it is preferable that an aluminum metal polymerization catalyst is added. The aluminum metal-based polymerization catalyst polymerizes the functional groups of the adhesion-imparting component described later such as epoxy group and alkoxy group in the adhesion-imparting component. Specifically, as the aluminum metal-based polymerization catalyst, aluminum trihydroxide Alternatively, an organoaluminum compound selected from the group consisting of aluminum alcoholate, aluminum acylate, aluminum acylate salt, aluminosyloxy compound and aluminum metal chelate compound is exemplified, and aluminum metal chelate compound is particularly preferable.

As the catalyst comprising such an aluminum metal chelate compound, a commercially available product can be used, and examples thereof include catalysts “ACS” and “Kelope EB-2” manufactured by Hope Pharmaceutical Co., Ltd.

By the way, the liquid crystal polyester which is a material of the electrode holding member 3 is a polyester called a thermotropic liquid crystal polymer, and forms a melt that exhibits optical anisotropy at a temperature of 450 ° C. or lower. Specifically, for example,
(1) What is obtained by polymerizing a combination of an aromatic hydroxycarboxylic acid, an aromatic dicarboxylic acid and an aromatic diol,
(2) What is obtained by polymerizing plural kinds of aromatic hydroxycarboxylic acids,
(3) What is obtained by polymerizing a combination of an aromatic dicarboxylic acid and an aromatic diol,
(4) Examples include those obtained by reacting a crystalline polyester such as polyethylene terephthalate with an aromatic hydroxycarboxylic acid.

  In addition, instead of aromatic hydroxycarboxylic acid, aromatic dicarboxylic acid or aromatic diol, those ester-forming derivatives can be used for the production of liquid crystal polyester, and if this ester-forming derivative is used, liquid crystal There exists an advantage that manufacture of polyester becomes easy.

  Here, the ester-forming derivative will be briefly described.

  An ester-forming derivative of an aromatic hydroxycarboxylic acid and aromatic dicarboxylic acid having a carboxyl group in the molecule is one obtained by converting the carboxyl group into a group such as a highly reactive acid halogen group or acid anhydride, Examples include those in which an ester is formed with an alcohol or ethylene glycol that forms a polyester by transesterification of a carboxyl group. In the case of an aromatic hydroxycarboxylic acid or aromatic diol having a phenolic hydroxyl group (phenolic hydroxyl group) in the molecule, a phenolic hydroxyl group is formed so that the phenolic hydroxyl group is produced by a transesterification reaction. May form an ester with a lower carboxylic acid.

  Furthermore, the aromatic hydroxycarboxylic acid, the aromatic dicarboxylic acid or the aromatic diol has a halogen atom such as a chlorine atom or a fluorine atom on its aromatic ring; An alkyl group such as a group; an aryl group such as a phenyl group may be substituted.

  The following can be illustrated as a structural unit which comprises liquid crystalline polyester.

Structural units derived from aromatic hydroxycarboxylic acids:

  The above structural unit may have a halogen atom, an alkyl group or an aryl group as a substituent.

Structural units derived from aromatic dicarboxylic acids:

  The above structural unit may have a halogen atom, an alkyl group or an aryl group as a substituent.

Structural units derived from aromatic diols:

  The above structural unit may have a halogen atom, an alkyl group or an aryl group as a substituent.

As more suitable liquid crystalline polyester, the combination of the structural unit can mention the following (a)-(f).
(A): a combination consisting of (A ₁ ), (B ₁ ) and (C ₁ ), or a combination consisting of (A ₁ ), (B ₁ ), (B ₂ ) and (C ₁ ) (b ): A combination consisting of (A ₂ ), (B ₃ ) and (C ₂ ), or a combination consisting of (A ₂ ), (B ₁ ), (B ₃ ) and (C ₂ ) (c): A combination comprising (A ₁ ) and (A ₂ ).
In combination with structural units of (d) :( a), in combination with structural units (A ₁₎ of some or all (those replaced with _{A 2) (e) :( a} ), (B 1) in combination with structural units of the part or the whole (B ₃₎ with those obtained by replacing (f) :( a) of, those replaced by (C ₁₎ of some or all (C ₃₎ (g): in combination with structural units of (b), a part or all of (a ₂₎ to a combination of structural units of those replaced with _{(a 1) (h) :(} c), and (B ₁₎ (C ₂ )

As in the above (a) to (f), the liquid crystal polyester used as the component (A) includes (A ₁ ) and / or (A ₂ ) as a structural unit derived from aromatic hydroxycarboxylic acid, aromatic As structural units derived from dicarboxylic acids, any one or more of (B ₁ ), (B ₂ ) and (B ₃ ), and as structural units derived from aromatic diols, (C ₁ ), (C ₂ ) and preferably those having a (C ₃₎ any one or more.

  The liquid crystalline polyester used for the electrode holding member 3 of the present invention preferably has a flow temperature of 270 to 400 ° C, more preferably 300 to 380 ° C. When a liquid crystal polyester having a flow temperature of less than 270 ° C. is used, the resulting molded body (electrode holding member 3) is used in a light-emitting device 1 having LEDs as light-emitting elements 7, and is used in a high-temperature environment in the LED module assembly process or the like However, there is an inconvenience that the molded body itself is easily deformed and blisters (blowing abnormality) are likely to occur. On the other hand, in the case of liquid crystalline polyester having a flow temperature exceeding 400 ° C., the melt processing temperature becomes high, so that there is an inconvenience that it is relatively difficult to produce a molded product.

  The flow temperature referred to here uses a capillary rheometer having a nozzle with an inner diameter of 1 mm and a length of 10 mm, and extrudes the heated melt from the nozzle at a heating rate of 4 ° C./min at a load of 9.8 MPa. Sometimes, it means a temperature at which the melt viscosity is 4800 Pa · s, and this flow temperature is an index representing the molecular weight of a liquid crystal polyester well known in the art (for example, “Liquid Crystal Polymer— Synthesis, molding, and application- "see pages 95-105, CMC, issued on June 5, 1987).

Various known methods can be employed as a method for producing the liquid crystalline polyester used for the electrode holding member 3 of the present invention. For example, JP 2004-256673 A discloses a resin composition for high reflectivity. As suggested, a method that can produce a liquid crystal polyester having a YI value of 32 or less is preferred. In addition, YI value means the value obtained by measuring this test piece using a color difference meter, when the test piece which consists of liquid crystalline polyester is obtained. The YI value is an index representing the yellowness of an object, and is a value defined in ASTM (American Material Testing Association) D1925. Specifically, it can be obtained by the following equation.
YI = [100 (1.28X-1.06Z) / Y]
(Here, the X value, Y value, and Z value are the tristimulus values of the light source color in the XYZ color system, respectively.)

  Specifically, a preferred method for producing a liquid crystal polyester disclosed in JP-A-2004-256673 will be described.

  By mixing a fatty acid anhydride with a mixture of an aromatic hydroxycarboxylic acid, an aromatic diol, and an aromatic dicarboxylic acid, and reacting at 130 to 180 ° C. in a nitrogen atmosphere, the hydroxyl group of the aromatic hydroxycarboxylic acid and the aromatic diol After acylating with fatty acid anhydride, the obtained acylated products (aromatic hydroxycarboxylic acid acylated products and aromatic diol acylated products) were obtained, and the reaction by-products were distilled out of the reaction system by raising the temperature. However, this is a method for producing a liquid crystal polyester by polycondensation of the acyl group of the acylated product and the carboxyl group of the aromatic hydroxycarboxylic acid acylated product and the aromatic dicarboxylic acid so as to cause transesterification.

  The molar ratio of the phenolic hydroxyl group to the carboxyl group in the mixture of aromatic hydroxycarboxylic acid, aromatic diol and aromatic dicarboxylic acid is preferably 0.9 to 1.1.

  0.95-1.2 times equivalent is preferable and, as for the usage-amount of the fatty acid anhydride with respect to the sum total of the phenolic hydroxyl group of aromatic diol and aromatic hydroxycarboxylic acid, 1.00-1.15 times equivalent is more preferable.

  If the amount of fatty acid anhydride used is small, coloration of the liquid crystal polyester tends to be suppressed, but if the amount used is too small, unreacted aromatic diol or aromatic dicarboxylic acid is likely to sublime at the time of polycondensation. The system may be blocked. On the other hand, when the usage-amount of a fatty acid anhydride exceeds 1.2 times equivalent, coloring of the obtained liquid crystal polyester may generate | occur | produce and there exists a possibility of deteriorating the color tone of a molded object.

  Examples of fatty acid anhydrides include acetic anhydride, propionic anhydride, butyric anhydride, isobutyric anhydride, valeric anhydride, pivalic anhydride, 2-ethylhexanoic anhydride, monochloroacetic anhydride, dichloroacetic anhydride, trichloroacetic anhydride, monobromo anhydride Specific examples include acetic acid, dibromoacetic anhydride, tribromoacetic anhydride, monofluoroacetic anhydride, difluoroacetic anhydride, trifluoroacetic anhydride, glutaric anhydride, maleic anhydride, succinic anhydride, β-bromopropionic anhydride, etc. It is not what is done. You may use these in mixture of 2 or more types. From the viewpoint of price and handleability, acetic anhydride, propionic anhydride, butyric anhydride, and isobutyric anhydride are preferably used, and acetic anhydride is more preferably used.

  The transesterification (polycondensation) reaction is preferably carried out while raising the temperature at a rate of 0.1 to 50 ° C./min in the range of 130 to 400 ° C., and 0.3 to 5 ° C. in the range of 150 to 350 ° C. It is more preferable to carry out the reaction while raising the temperature at a rate of / min.

  And in order to make a transesterification (polycondensation) reaction smoother, the reaction by-product is distilled off out of the system.

  The transesterification (polycondensation) reaction is a heterocyclic organic base compound containing two or more nitrogen atoms (nitrogen-containing) from the viewpoint of facilitating the production of liquid crystal polyester and the viewpoint of sufficiently suppressing coloring of the obtained liquid crystal polyester. It is preferably carried out in the presence of a heterocyclic organic base compound). Examples of the nitrogen-containing heterocyclic organic base compound include imidazole compounds, triazole compounds, dipyridyl compounds, phenanthroline compounds, diazaphenanthrene compounds, and the like. Among these, from the viewpoint of reactivity, an imidazole compound is preferably used, and 1-methylimidazole and 1-ethylimidazole are more preferably used because they are easily available.

  In addition, a catalyst other than the heterocyclic organic base compound may be used for the purpose of further promoting the transesterification (polycondensation) reaction and increasing the polycondensation rate. However, when a metal salt or the like is used as a catalyst, the metal salt remains as an impurity in the liquid crystal polyester, which may adversely affect an electronic component such as the electrode holding member 3. Also in this respect, use of the nitrogen-containing heterocyclic organic base compound is a particularly preferable embodiment in producing the liquid crystalline polyester used for the electrode holding member 3 of the present invention.

  As a method of further increasing the degree of polymerization by further proceeding the transesterification (polycondensation) reaction, a method of reducing the pressure inside the reaction vessel of the transesterification (polycondensation) reaction (vacuum polymerization), or a powder after cooling and solidifying the reaction product And a method of subjecting the obtained powder to solid phase polymerization at 250 to 350 ° C. for 2 to 20 hours. By increasing the degree of polymerization by such a method, it becomes easy to produce a liquid crystal polyester having a suitable flow temperature. In view of simple equipment, it is preferable to use solid phase polymerization.

  The polycondensation by the acylation and transesterification reactions and the low-pressure polymerization or solid phase polymerization carried out for the purpose of increasing the degree of polymerization are preferably carried out in an inert gas atmosphere such as nitrogen gas.

  The liquid crystal polyester thus produced is a liquid crystal polyester having a YI value of 32 or less, and is particularly preferable as the liquid crystal polyester used for the electrode holding member 3 of the present invention.

  A liquid crystal polyester obtained by the production method using the nitrogen-containing heterocyclic organic base compound and having a YI value of 32 or less is particularly preferable for the electrode holding member 3 of the present invention. A liquid crystal polyester mixture having a YI value of 32 or less by mixing polyester can also be used for the electrode holding member 3 of the present invention. In this case as well, a liquid crystal polyester mixture suitable for the electrode holding member 3 of the present invention can be selected if a plurality of types of liquid crystal polyesters are mixed and the YI value of the liquid crystal polyester mixture is determined by the method using the chromaticity meter. You can also.

  The liquid crystalline polyester used for the electrode holding member 3 of the present invention can be filled with various inorganic fillers. Examples of the inorganic filler include pigments such as iron oxide, ultramarine, zinc oxide, zinc sulfide, lead white, and titanium oxide; glass fiber, carbon fiber, metal fiber, alumina fiber, boron fiber, titanate fiber, and wollast. Inorganic fibers such as knight and asbestos; silicon dioxide, calcium carbonate, alumina, aluminum hydroxide, kaolin, talc, clay, mica, glass flakes, glass beads, hollow glass beads, dolomite, various metal powders, barium sulfate, titanic acid Examples thereof include powders such as potassium and calcined gypsum; powdered, plate-like, and whisker-like inorganic compounds such as silicon carbide, alumina, boron nitrite, aluminum borate and silicon nitride.

  In order to impart practical mechanical strength without significantly reducing the physical properties of the resulting resin composition, inorganic fibers such as glass fiber, titanic acid fiber and wollastonite, silicon dioxide, aluminum borate and silica nitride are used. Preference is given to an inorganic compound such as elemental powder, plate, whisker, or talc. In order to improve the whiteness of the resin composition, pigments such as zinc oxide, zinc sulfide, lead white and titanium oxide, silica, glass beads, hollow glass beads, talc, silicon dioxide, calcium carbonate, alumina, hydroxide It is preferable to use a white inorganic filler such as aluminum, and titanium oxide is more preferable.

  20-200 mass parts is preferable with respect to 100 mass parts of liquid crystalline polyester, as for the compounding quantity of this inorganic filler, it is more preferable that it is 25-150 mass parts, and 40-100 mass parts is further more preferable. If the amount is less than 20 parts by mass, the sufficient effect of the present invention may not be obtained. On the other hand, when the amount exceeds 200 parts by mass, the production itself tends to be difficult.

  In addition, when using multiple types of inorganic fillers as an inorganic filler, the total amount should just be the said range with respect to liquid crystalline polyester resin.

  The titanium oxide filler suitably used as this inorganic filler is mainly composed of titanium oxide. If it is called “titanium oxide” in the art and is commercially available as a resin filler, it can be used as an inorganic filler. In addition, what is called a titanium oxide and marketed as a resin filler can be used as it is, and does not exclude the impurity contained unintentionally. Further, as the titanium oxide filler, those subjected to surface treatment as described later can be used.

  This titanium oxide filler is not particularly limited in the crystal form of the titanium oxide itself contained, and a rutile type, anatase type, or a mixture of both may be used. From the standpoint that the electrode holding member 3 having a higher degree of reflectance is obtained and the weather resistance of the electrode holding member 3 is good, it is preferable to use a titanium oxide filler containing rutile type titanium oxide. It is more preferable to use a titanium oxide filler made of titanium oxide.

  Although the average particle diameter of the titanium oxide filler is not particularly limited, the average particle diameter is 0.10 to 1 μm from the viewpoint of the reflectance of the obtained electrode holding member 3 and the filler dispersibility in the electrode holding member 3. It is preferably 0.15 to 0.50 μm, more preferably 0.18 to 0.40 μm. The average particle diameter of such a titanium oxide filler can be used in consideration of the thickness of the electrode holding member 3 to be manufactured.

  Here, the average particle diameter of the titanium oxide filler means that the appearance of the titanium oxide filler is measured with a scanning electron microscope (SEM), and the obtained SEM photograph is used as an image analysis device (for example, image analysis manufactured by Nireco Corporation). Using a device "Luzex IIIU"), plot the particle amount (%) in each particle size section of the primary particles to obtain a distribution curve, and obtain a cumulative degree of 50% (average particle size) from the accumulated distribution curve. The volume average particle diameter.

  The titanium oxide filler may be subjected to a surface treatment for the purpose of improving characteristics such as dispersibility. Such surface treatment is not particularly limited, but from the viewpoint of improving dispersibility and weather resistance, surface treatment with an inorganic metal oxide is preferred, and aluminum oxide (alumina) is preferred as the inorganic metal oxide. However, if there is no aggregation or the like and it is easy to handle, a titanium oxide filler that is not surface-treated is preferable from the viewpoint of heat resistance and strength.

  The method for producing the titanium oxide filler is preferable as long as it satisfies the above range of the average particle diameter, but is more preferably a titanium oxide filler containing titanium oxide produced by a chlorine method. Briefly explaining the chlorine method here, ore (synthetic rutile obtained from rutile or ilmenite ore) as a titanium source is reacted with chlorine at around 1000 ° C. to obtain crude titanium tetrachloride. Is purified by rectification, and then titanium tetrachloride obtained is oxidized with oxygen to obtain titanium oxide. According to this chlorine method, it becomes easy to obtain rutile type titanium oxide which is a suitable crystal type. And, by optimizing the conditions in the step of oxidizing with oxygen (oxidation step), it is easy to obtain titanium oxide having relatively high whiteness, and the titanium oxide filler containing such titanium oxide is particularly suitable as the present invention. Is preferred. In addition, by optimizing the conditions in the oxidation step, there is an advantage that generation of coarse particles is suppressed and it becomes easy to obtain a titanium oxide filler having an average particle diameter suitable for the present invention.

  As a commercial item of the titanium oxide filler, for example, “TIPAQUE CR-60, TIPAQUE CR-58” manufactured by Ishihara Sangyo Co., Ltd., which is made of titanium oxide manufactured by the chlorine method, was manufactured by a manufacturing method called a sulfuric acid method. Examples thereof include “TITANIX JR-301, WP0042” manufactured by Teika Co., Ltd. and “SR-1, SR-1R, D-2378” manufactured by Sakai Chemical Industry Co., Ltd., which are made of titanium oxide.

  In the liquid crystal polyester resin composition produced in the present invention, an inorganic filler other than the titanium oxide filler is used for the purpose of improving the mechanical properties of the electrode holding member 3 within a range that does not significantly impair the properties of the resulting composition. It can also be used together.

  In addition, the liquid crystal polyester resin composition includes a mold release improver such as a fluororesin, a higher fatty acid ester compound, and a fatty acid metal soap; a colorant such as a dye and a pigment; an antioxidant within a range not impairing the object of the present invention. Normal additives such as a heat stabilizer, a fluorescent brightener, an ultraviolet absorber, an antistatic agent, and a surfactant may be added. In addition, additives having an external lubricant effect such as higher fatty acid, higher fatty acid ester, higher fatty acid metal salt, and fluorocarbon surfactant may be added.

  When manufacturing the light emitting device 1 having the above-described configuration, the following procedure is used.

  First, in the package manufacturing process, as shown in FIG. 2A, the electrode holding member 3 is integrally formed with the pair of lead electrodes 5 and 6 to manufacture the package 2. At this time, as an integral molding method of the electrode holding member 3, for example, insert molding can be used.

  Next, the process proceeds to a heat treatment step, and the electrode holding member 3 is heat treated. For this purpose, the package 2 is placed in an oven (not shown) and subjected to heat treatment under predetermined heating conditions (temperature and time).

  At this time, the temperature of the heat treatment is preferably in the range of 80 to 250 ° C, and more preferably in the range of 100 to 200 ° C. When this temperature is less than 100 ° C., the time required for the heat treatment is prolonged and the productivity is lowered, and when this temperature is less than 80 ° C., the adhesion between the electrode holding member 3 and the sealing resin 9 is reduced. Improvement is limited. Conversely, if this temperature exceeds 200 ° C, the liquid crystal polyester may be discolored (yellowing, blackening, etc.), and if this temperature exceeds 250 ° C, the liquid crystal polyester may deteriorate with heating. There is.

  The time for the heat treatment is not particularly limited as long as the liquid crystal polyester does not deteriorate, but is preferably within a range of 1 to 10 hours. When this time is less than 1 hour, the improvement in adhesion between the electrode holding member 3 and the sealing resin 9 is limited, and conversely, when this time exceeds 10 hours, the productivity is lowered.

  Here, it is not necessary to heat the entire package 2, and at least the electrode holding member 3 may be heated.

  Thereafter, the process proceeds to an element mounting process. As shown in FIG. 2B, the light emitting element 7 is placed in the element mounting recess 3b of the electrode holding member 3, and the light emitting element 7 is placed in a pair of lead electrodes 5, 6. Solder to the mounting. Then, the light emitting element 7 is in a state where the electrodes 7a and 7b are electrically connected to the lead electrodes 5 and 6, respectively.

  At this time, the light emitting element 7 may be bonded and fixed to the package 2 with a thermosetting resin or the like. Specific examples of the thermosetting resin include an epoxy resin, an acrylic resin, and an imide resin. Further, when Ag paste, carbon paste, ITO paste, metal bump, or the like is used, the light emitting element 7 can be fixed to the package 2 and at the same time, the electrodes 7 a and 7 b of the light emitting element 7 can be electrically connected to the lead electrodes 5 and 6.

  Finally, the process proceeds to an element sealing step, and the light emitting element 7 is sealed with a sealing resin 9 as shown in FIG. For this purpose, the curing temperature of the thermosetting resin constituting the sealing resin 9 (the “curing temperature of the thermosetting resin” in the present specification means that the solid thermosetting resin material is liquefied and further fixed. The sealing resin 9 is injected and filled into the element mounting recess 3b of the electrode holding member 3 under the condition that the solidification is completed after a lapse of time. Alternatively, after potting the liquid sealing resin 9 at room temperature, it is held for a certain period of time at the thermosetting temperature in an electric furnace. Then, the sealing resin 9 comes into contact with the element mounting recess 3 b of the electrode holding member 3.

  Here, the manufacturing method of the light emitting device 1 is finished, and the light emitting device 1 is completed.

  Thus, in this manufacturing method, the electrode holding member 3 is heat-treated before the light emitting element 7 is sealed with the sealing resin 9. For this reason, the adhesion between the electrode holding member 3 and the sealing resin 9 is enhanced. This is presumed to be because an insoluble component that may hinder the adhesion between the electrode holding member 3 and the sealing resin 9 evaporates from the electrode holding member 3 due to the heat treatment of the electrode holding member 3.

As a result, regardless of the usage environment of the light emitting device 1, it is possible to suppress the occurrence of a situation in which peeling occurs at the interface between the electrode holding member 3 and the sealing resin 9 and the luminance of the light emitting device 1 decreases. Therefore, the reliability as the light emitting device 1 can be improved.
[ Reference example ]

FIG. 3 shows a reference example . In this reference example , the configuration of the light emitting device 1 is the same as that of the first embodiment described above, and only the manufacturing method is different. That is, in this reference example , in the method for manufacturing the light emitting device 1, as described below, the electrode holding member 3 is provided after the light emitting element 7 is mounted on the pair of lead electrodes 5 and 6.

  First, in the element mounting step, the light emitting element 7 is soldered and mounted on the pair of lead electrodes 5 and 6 as shown in FIG. Then, the light emitting element 7 is in a state where the electrodes 7a and 7b are electrically connected to the lead electrodes 5 and 6, respectively.

  Thereafter, the process proceeds to a package production process, and as shown in FIG. 3B, the electrode holding member 3 is integrally formed with the pair of lead electrodes 5 and 6 to produce the package 2. At this time, as an integral molding method of the electrode holding member 3, for example, insert molding can be used.

  Next, the process proceeds to a heat treatment step, and the electrode holding member 3 is heat treated. For this purpose, the package 2 on which the light emitting element 7 is mounted is placed in an oven (not shown), and heat treatment is performed under predetermined heating conditions (temperature and time). The heating conditions at this time are the same as those in the first embodiment.

  Here, it is not necessary to heat the light emitting element 7 and the lead electrodes 5 and 6, and at least the electrode holding member 3 may be heated.

  Finally, the process proceeds to the element sealing step, and the light emitting element 7 is sealed with the sealing resin 9 as shown in FIG. Then, the sealing resin 9 comes into contact with the element mounting recess 3 b of the electrode holding member 3.

  Here, the manufacturing method of the light emitting device 1 is finished, and the light emitting device 1 is completed.

Thus, in this manufacturing method, the adhesion between the electrode holding member 3 and the sealing resin 9 is increased for the same reason as in the first embodiment. As a result, regardless of the usage environment of the light emitting device 1, it is possible to suppress the occurrence of a situation in which peeling occurs at the interface between the electrode holding member 3 and the sealing resin 9 and the luminance of the light emitting device 1 is reduced. The reliability as 1 can be improved.
[Other Embodiments of the Invention]

  In the above-described first embodiment, the case where the heat treatment process is provided between the package manufacturing process and the element mounting process in the method for manufacturing the light emitting device 1 has been described. A heat treatment step may be provided between the two. Also in this case, since the electrode holding member 3 is heat-treated before the light emitting element 7 is sealed with the sealing resin 9, the same effects as those of the first embodiment described above can be obtained.

In the first embodiment and the reference example described above, the light emitting device 1 in which the light emitting element 7 is sealed with the sealing resin 9 has been described. However, by including a diffusing agent in the sealing resin 9, the directivity from the light emitting element 7 can be relaxed and the viewing angle can be increased. Further, the sealing resin 9 can contain various colorants. Furthermore, the sealing resin 9 can be formed into convex lens shapes, concave lens shapes, and the like of various sizes in consideration of the light distribution and light condensing properties of light entering and exiting the light emitting element 7. Further, for the purpose of improving the light distribution in a predetermined direction with respect to the light emitting device 1, the sealing resin 9 is used as a lens so that the longitudinal section when the mold member is viewed from the light emitting direction is elliptical. It is also possible to mold. Alternatively, a phosphor can be used to obtain a desired emission color by converting the wavelength of light emitted from the light emitting element 7. Such a phosphor is contained in the mold member, or is fixed on the surface of the light emitting element 7 with a binder such as a translucent inorganic member. By using the phosphor, the light emitting device 1 capable of emitting various emission colors can be obtained.

Furthermore, in the first embodiment and the reference example described above, the light emitting device 1 including the electrode holding member 3 made of liquid crystal polyester has been described. However, the material of the electrode holding member 3 is not limited to liquid crystal polyester, and various thermoplastic resins can be used. Specific examples of this thermoplastic resin include polystyrene, polymethylpentene-1, polyethylene, polypropylene, polyamide 12, acrylonitrile-butadiene-styrene copolymer, acrylonitrile-ethylenepropylene-styrene copolymer, polyamide 6, polyamide 66. , Aromatic polyamide, 9T polyamide, polyacetal, polymethyl methacrylate, polyvinylidene fluoride, polyvinyl fluoride, polyhexafluoroethylene propylene, polytrifluoride ethylene, poly (ethylene-tetrafluoroethylene), polyacrylonitrile, polyarylate, Polyethylene terephthalate, polybutylene terephthalate, polyphenylene sulfide, polycarbonate, polyether ketone, polyether ether ketone, polyether Bromide, polysulfone polyethersulfone, polyester, polyethylene terephthalate, polyphenylene oxide and its modified products, polysulfone, polyarylate, polyester amides.

In the first embodiment and the reference example described above, the package 2 is constituted by the pair of lead electrodes 5 and 6 and the electrode holding member 3, and the light emitting element 7 is mounted on the pair of lead electrodes 5 and 6. As described above, a package may be constituted by a plurality of pairs (for example, two pairs or three pairs) of lead electrodes and an electrode holding member, and a light emitting element may be mounted on each of the plurality of pairs of lead electrodes.

Experimental example

  Hereinafter, although the experiment example of this invention is demonstrated, this invention is not limited to an experiment example.

In addition, based on the idea that the adhesion between the electrode holding member and the sealing resin does not depend on the presence or absence of the lead electrode or the light emitting element, in this experimental example, the electrode holding member alone (that is, In a state in which the pair of lead electrodes and the light emitting element are omitted, the adhesion with the sealing resin was evaluated.
<Experimental example 1>

  In a reactor equipped with a stirrer, a torque meter, a nitrogen gas inlet tube, a thermometer and a reflux condenser, 994.5 g (7.2 mol) of p-hydroxybenzoic acid, 446.9 g of 4,4′-dihydroxybiphenyl ( 2.4 mol), 299.0 g (1.8 mol) of terephthalic acid, 99.7 g (0.6 mol) of isophthalic acid, and 1347.6 g (13.2 mol) of acetic anhydride. .2 g was added and the inside of the reactor was sufficiently replaced with nitrogen gas, and then the temperature was raised to 150 ° C. over 30 minutes under a nitrogen gas stream, and the mixture was refluxed for 1 hour while maintaining the temperature.

  Thereafter, 0.9 g of 1-methylimidazole was added and the by-product acetic acid distilled and unreacted acetic anhydride was distilled off, and the temperature was raised to 320 ° C. over 2 hours and 50 minutes. A prepolymer was obtained as a reaction end point.

  Next, the prepolymer was cooled to room temperature, pulverized with a coarse pulverizer, then heated from room temperature to 250 ° C. over 1 hour in a nitrogen gas atmosphere, and then heated from 250 ° C. to 285 ° C. over 5 hours. And it hold | maintained at 285 degreeC for 3 hours, liquid crystal polyester was obtained by advancing a polymerization reaction by a solid layer. The liquid crystal polyester had a flow start temperature of 330 ° C.

  Thus, 55 parts by mass of titanium oxide “TIPAQUE CR-58” manufactured by Ishihara Sangyo Co., Ltd., chopped glass fiber manufactured by Owens Corning Japan Co., Ltd. with respect to 100 parts by mass of the liquid crystalline polyester thus obtained. After blending 27 parts by mass of “CS03JAPX-1”, a liquid crystal polyester resin composition was obtained using a twin screw extruder “PCM-30” manufactured by Ikegai Co., Ltd. The liquid crystal polyester resin composition thus obtained was molded at 330 ° C. with an injection molding machine “PS40E5ASE type” manufactured by Nissei Plastic Industry Co., Ltd. to obtain a liquid crystal polyester molded body (electrode holding member) of 64 mm × 64 mm × 3 mm. It was. Further, this liquid crystal polyester molded body was heat-treated at 120 ° C. for 2 hours.

  Then, a thermosetting silicone resin “EG6301” containing a platinum-based catalyst manufactured by Shin-Etsu Chemical Co., Ltd. was used as a sealing resin, and a liquid crystal polyester molded body after heat treatment and a tensile manufactured by Honda Business Systems Co., Ltd. An adhesion piece (20 mm dolly) for the type adhesion tester “PosiTest AT” was brought into close contact. Thereafter, after the thermosetting silicone resin is cured under conditions of a temperature of 60 ° C. for 3 hours and a temperature of 150 ° C. for 3 hours, the adhesive is formed into a liquid crystal polyester when a predetermined tensile force is applied to the adhesive. It was observed whether it peeled off from the body and caused poor adhesion. And the ratio (adhesion failure rate) of the number of adhesion failures to the evaluation number (total number) was calculated.

The results are shown in Table 1.
<Experimental example 2>

As the sealing resin, except that the thermosetting silicone resin “XJR-9022 X-5” containing a platinum-based catalyst manufactured by Shin-Etsu Chemical Co., Ltd. was substituted, in the same manner as in Experimental Example 1 described above, The adhesion between the sealing resin and the liquid crystal polyester resin was evaluated. The results are shown in Table 1.
<Comparative Experimental Example 1>

The adhesiveness between the sealing resin and the liquid crystal polyester resin was evaluated in the same manner as in Experimental Example 1 except that the heat treatment for the liquid crystal polyester molded body was omitted. The results are shown in Table 1.
<Comparative Experiment Example 2>

＜封止樹脂と液晶ポリエステル樹脂との密着性の評価＞ The adhesiveness between the sealing resin and the liquid crystal polyester resin was evaluated in the same manner as in Experimental Example 2 described above except that the heat treatment for the liquid crystal polyester molded body was omitted. The results are shown in Table 1.

<Evaluation of adhesion between sealing resin and liquid crystal polyester resin>

  For each of Experimental Examples 1 and 2 and Comparative Experimental Examples 1 and 2, the adhesion between the sealing resin and the liquid crystal polyester resin was evaluated based on the adhesion failure rate.

  As a result, as is clear from Table 1, in Comparative Experimental Example 1, 8 out of 16 (that is, 50%) adhesion failure occurred, and in Comparative Experimental Example 2, 4 out of 8 (In other words, adhesion failure occurred at 50%). Therefore, Comparative Experiment Examples 1 and 2 resulted in poor adhesion between the sealing resin and the liquid crystal polyester resin.

  On the other hand, in Experimental Example 1, none of the 16 pieces had poor adhesion, and in Experimental Example 2, none of the eight pieces had poor adhesion. Therefore, about Experimental example 1, 2, the result excellent in the adhesiveness of sealing resin and liquid crystal polyester resin was obtained.

  The present invention is a light-emitting device used as a light source for various display devices (for example, liquid crystal display devices, projectors, information display terminals, traffic signal lights, automobile stop lamps and turn signals), and various illumination devices (for example, The present invention can be widely applied when manufacturing light-emitting devices and other light-emitting devices that are used as light sources for indoor illumination lamps, outdoor illumination lamps, interior lights, exterior lights, emergency lights, LED surface light sources, and the like.

DESCRIPTION OF SYMBOLS 1 ... Light-emitting device 2 ... Package 3 ... Electrode holding member 3a ... Main body 3b ... Element mounting recessed part 5, 6 ... Lead electrode 7 ... Light-emitting element 7a, 7b ... Electrode 9 ... Sealing resin

Claims (7)

A package manufacturing process in which a lead electrode is provided with a resin electrode holding member to manufacture a package; an element mounting process in which a light emitting element is mounted on the lead electrode; and the light emission in a form in which a sealing resin is in contact with the electrode holding member. A method of manufacturing a light-emitting device including an element sealing step of sealing an element with the sealing resin,
A method of manufacturing a light emitting device, wherein at least the electrode holding member is heat-treated in a stage between the package manufacturing process and the element mounting process. A package manufacturing process in which a lead electrode is provided with a resin electrode holding member to manufacture a package; an element mounting process in which a light emitting element is mounted on the lead electrode; and the light emission in a form in which a sealing resin is in contact with the electrode holding member. A method of manufacturing a light-emitting device including an element sealing step of sealing an element with the sealing resin,
A method of manufacturing a light emitting device, wherein at least the electrode holding member is heat-treated at a stage between the element mounting process and the element sealing process. The method for manufacturing a light emitting device according to claim 1 , wherein the electrode holding member is made of liquid crystal polyester . The method for manufacturing a light emitting device according to claim 3 , wherein titanium oxide is blended in the liquid crystal polyester . 5. The method for manufacturing a light emitting device according to claim 3 , wherein the temperature of the heat treatment for the electrode holding member is in a range of 80 to 250 ° C. 6 . The method for manufacturing a light-emitting device according to claim 3, wherein the heat treatment time for the electrode holding member is within a range of 1 to 10 hours . Said sealing resin, the method of manufacturing the light emitting device according to any one of claims 1 to 6, characterized in that a thermosetting silicone resin.

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