KR101274816B1 - Resin composition having high heat resistance, thermal conductivity and reflectivity and the method of the same - Google Patents

Abstract

The present invention relates to a method for producing a material having a high reflectivity of 90% or more and excellent thermal conductivity of 0.35 w / m.k or more and an excellent heat resistance of 260 ° C or more. The present invention is an additive material and glass fiber to improve the white inorganic material and thermal conductivity in a super-engineering plastic such as polyphenylene sulfide (PPS), liquid crystal polymer (LCP), polyphenylene amide (PPA) having a melting point of 270 ℃ or more ( Materials such as glass fiber) are kneaded using a twin screw extruder. Its main purpose can be used as LED package housing.

Heat Resistance, Reflectance, Thermal Conductivity, Light Emitting Diode Package (LED Package)

Description

RESIN COMPOSITION HAVING HIGH HEAT RESISTANCE, THERMAL CONDUCTIVITY AND REFLECTIVITY AND THE METHOD OF THE SAME}

The present invention relates to a composition of a material having a high reflectance of 90% or more and an excellent thermal conductivity of 0.35 w / m.k or more, and having an excellent heat resistance of 260 ° C or more, and a method of manufacturing the same. The present invention relates to a method for producing a material having high reflectance, excellent heat resistance and thermal conductivity. Its main use can be used for light emitting diode package housings.

Light emitting diodes have been widely used as indicators or light sources in household appliances such as lighting equipment and various appliances due to advantages such as low heat dissipation and long life, low size, and low power consumption. Recently, light emitting diodes have been developed to pursue the purpose of multi-color and high brightness, and thus the use range of such light emitting diodes has been extended to large outdoor display boards, traffic signals, automobile tail lights, mobile phone lamps, and the like. In the future, the LEDs are expected to replace tungsten filament lamps and mercury lamps as light emitting sources with power saving and environmental protection features, and the recently developed acriche has a longer lifespan than conventional LEDs. It does not require a long, alternating circuit that converts alternating current in series, saving cost and space. More importantly, it is not possible to replace existing building, luminaire, and mechanical lights that operate on AC alternating current directly with DC light emitting diodes. On the other hand, Acrichero is known to be replaceable immediately, and its utility is expected to extend to the entire lighting market. Referring to the operation principle of the light emitting diode package, when the light emitting diode chip of the light emitting diode package is driven by light and emits light, part of the light emitted by the chip is reflected by the white package housing and then away from the lead frame. Is released. Conventional light emitting diode package housing materials will reflect some of the light emitted when the chip is driven by a current to emit light and will also absorb some of the light. The heat generated by the absorbed light, the material is low thermal conductivity, so the heat transfer is not good, the temperature of the light emitting diode package housing has been increased, thereby reducing the lifetime and brightness of the light emitting diode. In addition, surface mount technology is used as a process of bonding the light emitting diodes to a PCB substrate. Due to environmental regulations, the transition to the lead removal process is compulsory, so that the material for the light emitting diode package housing has a heat resistance of more than 260 ° C. Was required. Looking at the state of the art, white polycarbonate is disclosed in U.S. Patent No. 5,837,757, Japanese Patent Application Laid-Open No. 7-242781, and Japanese Patent Application Laid-open No. 9-176471 for the fact that the reflectivity can be increased by adding a white inorganic material to a material such as PC. The technique regarding the reflectance and impact resistance of resin is disclosed. However, the patent for a material that satisfies all thermal conductivity properties of more than 0.35w / mk can be maintained at a low temperature by releasing heat absorbed heat of more than 260 ℃, reflectance of more than 90%, absorbed heat for the housing It has not been disclosed. The light emitting diode package housing manufactured by the above-mentioned conventional manufacturing technique is mainly obtained by adding a white powder inorganic material to a PC, or a resin having high heat resistance such as polyphenylene amide as the surface mounting temperature is increased due to environmental regulations. The material which added the mineral of white powder appeared. In this case, excellent heat resistance and reflectance performance can be obtained, but due to the gap between the inserted metal and the housing due to the dimensional change due to water absorption of polyphenylene amide, the life of the light emitting diode is shortened due to exposure to moisture. In addition to the role of reducing the heat absorption of the light emitting diode due to the failure to dissipate the heat absorbed due to low thermal conductivity, the fatal disadvantage has not yet been solved.

Therefore, the inventors of the present invention by extruder to a material including a super engineering plastic and a white inorganic material, a filler to impart thermal conductivity and a glass fiber in the thermoplastic resin in order to have excellent reflectivity and thermal conductivity and excellent heat resistance and mechanical strength As a result of studying the extrusion process, it was confirmed that a material having excellent reflectance, thermal conductivity, and mechanical strength could be obtained, and the present invention was reached.

The present invention provides a resin composition having heat resistance, excellent thermal conductivity and light reflection characteristics for use in a light emitting diode package housing or the like. In particular, the present invention provides a resin composition having a reflectance of 90% or more, excellent thermal conductivity of 0.35 w / m.k or more, and excellent heat resistance of 260 ° C or more.

Still another object of the present invention is to provide a method of manufacturing a material for a light emitting dide package housing having excellent mechanical rigidity by mixing glass fibers.

In addition, an object of the present invention is to mass-produce a composition of a material for a light emitting diode package housing by a specific method using a twin screw extruder, thereby providing an economical and excellent resin production method and a manufacturing method thereof.

The above and other objects of the present invention can be achieved by the configuration of the present invention described below.

In order to achieve the above object, the present invention provides a light emitting diode packaging composition comprising a high heat resistance thermoplastic resin, a white inorganic material and glass fiber described below:

(a) 40 to 70% by weight of the crystalline resin having a melting point of at least 270 ° C,

(b) 5 to 50% by weight of white minerals

(c) 1 to 40 wt% of the thermally conductive filler and

(d) 5 to 30 weight percent of stiffness increasing agent

In addition, the light emitting diode packaging composition may optionally include additives such as hygroscopic resins, antioxidants, light stabilizers, mold release agents, plasticizers, nucleating agents, pigments, crosslinking agents, optical brighteners, or the like.

In particular, syndiotactic polystyrene or polyamide 12 may be additionally included for the hygroscopicity. In this case, the syndiotactic polystyrene or polyamide 12 may be included in a ratio of 97: 3 to 50:50 with respect to the crystalline resin.

In addition, the present invention is 40 to 70% by weight of the crystalline resin having a melting point of 270 ℃ or more, 5 to 50% by weight of the white inorganic material, 1 to 40% by weight of the thermally conductive filler and 5 to 30% by weight of the rigidity increasing agent barrel temperature of 280 to Provided is a method of manufacturing a light emitting diode packaging material comprising the step of manufacturing in pellet form through extrusion mixing in a twin screw extruder at 360 ℃.

As described above, the resin composition according to the present invention has excellent heat resistance, excellent thermal conductivity and light reflectance, and is excellent in processability such as thin film molding, and can be used in a light emitting diode package housing of a notebook computer, an LCD TV, a mobile phone, and the like. Applicable to all parts with Pb-free SMT.

Although described in detail above with reference to the specific embodiments of the present invention, it will be apparent to those skilled in the art that various changes and modifications can be made within the scope of the present invention and the technical spirit, and such modifications and modifications fall within the scope of the appended claims. It is also natural.

In the light emitting diode packaging composition excellent in heat resistance, reflectance, and thermal conductivity according to the present invention, the crystalline resin having a melting point of 270 ° C. or higher may be polyphenylene amide, polyphenylene sulfide, or liquid crystal. Liquid crystalline polymer can be used.

The polyphenylene amide may be a resin having a melting point ranging from 270 ° C. to 350 ° C. In addition, the polyphenylene sulfide is a linear type having a similar white color to implement a reflectance of 90% or more, a melting point of 270 ℃ to 290 ℃ range of resin can be used. Liquid crystal polymer can also be used that has a heat resistance of 270 ℃ or more.

In the light emitting diode packaging composition according to the present invention, a white inorganic material may be used, such as titanium oxide (TiO ₂ ), an average particle diameter of 0.1 to 10 microns may be used, and the surface may be used at high temperature. Preference is given to using titanium oxide treated with a tolerable coating.

In the light emitting diode packaging composition according to the present invention, a white thermally conductive filler may be used to improve the ability of dissipating heat transferred to the surface, and such thermally conductive fillers may include talc, wollastonite, and boron nitride. , Mica, graphite, etc. can be applied, the size of the filler is preferably 1 to 100 microns in size.

 In the light emitting diode packaging composition according to the present invention, glass fibers, milled glass fibers, glass beads, and the like may be used to increase heat resistance and rigidity, and the content may increase heat resistance. Limit the minimum quantity from 5% to 30%.

Hereinafter, preferred examples are provided to help the understanding of the present invention, but the following examples are merely for exemplifying the present invention, and various changes and modifications within the scope and spirit of the present invention are apparent to those skilled in the art. It is natural that such variations and modifications fall within the scope of the appended claims.

First, the measurement and evaluation methods necessary for the explanation of the present invention were performed under the following conditions.

[Test Example]

(1) Heat resistance

    It measured according to ASTM D648 method.

(2) mechanical strength

Flexural Strength - Determined according to the ASTM D790 method.

Flexural modulus-measured according to ASTM D790 method.

* Tensile strength - Measured according to ASTM D638 method.

* Impact strength-measured according to ASTM D256 method.

(3) water absorption

    It measured according to ASTM D-570, Karl Fischer method.

(4) reflectance

   Spectrophotometer, Gretagmacbeth, Color-Eye

550nm wavelength at 10 ° viewing angle using D65 light source

The total reflectance of was measured.

(5) thermal conductivity

    Data within 10% error was used in the measurement methods such as the plate method (LG Chem Tech Center) and the laser flash method (ASTM E-1461).

 (6) liquidity

    It measured according to ASTM D1238.

 (7) Coefficient of linear expansion

    The coefficient of linear expansion was measured according to ASTM D696.

Example  One

54% by weight of PPA resin (melting point: 295 ° C) by BASF as polyphenylene amide, 5% by weight of boron nitride as a thermally conductive filler, and antioxidants, lubricants, UV stabilizers and fluorescent brighteners in the same direction (co- Rotating Into the main inlet, the beginning of the screw of the twin screw extruder, 10% by weight of titanium oxide (TiO ₂ ), white powder, is inserted into the first inlet of the side of the extruder, and the glass fiber ) 30% by weight was added to the second inlet of the side of the extruder, and the processing conditions were prepared in a pellet state using an extruder at 300 ℃, 250rpm. The obtained pellet was sufficiently dehumidified and dried to obtain a specimen for measuring physical properties, a heat resistance, a thermal conductivity, and a light reflectance using an injection molding machine, and the results are shown in Table 2. main

Example  2

54 wt% of polyphenylene amide resin (melting point: 295 ° C.), 5 wt% of a thermally conductive filler boron nitride, 20 wt% of titanium oxide (TiO ₂ ), and 20 wt% of glass fiber were used. Pellet preparation and injection specimens were prepared in the same manner as in Example 1, the results are shown in Table 2.

Example  3

54% by weight of polyphenylene amide resin (melting point: 295 ° C), 5% by weight of boron nitride, a thermally conductive filler, 30% by weight of titanium oxide (TiO ₂ ), and 10% by weight of glass fiber Except for the preparation of pellets and injection specimens in the same manner as in Example 1, the results are shown in Table 2.

Example  4

Except for using 49% by weight of polyphenylene amide resin (melting point: 295 ° C.), 10% by weight of boron nitride as a thermally conductive filler, 30% by weight of titanium oxide (TiO ₂ ), and 10% by weight of glass fiber. Pellet preparation and injection specimens were prepared in the same manner as in Example 1, the results are shown in Table 2.

Example  5

Except for using 49% by weight of polyphenylene amide resin (melting point: 295 ° C), 20% by weight of boron nitride as a thermally conductive filler, 20% by weight of titanium oxide (TiO ₂ ), and 10% by weight of glass fiber. Pellet preparation and injection specimens were prepared in the same manner as in Example 1, the results are shown in Table 2.

Example  6

Except for using 49% by weight of polyphenylene amide resin (melting point: 295 ℃), 10% by weight of talc, 30% by weight of titanium oxide (TiO ₂ ) and 10% by weight of glass fiber (glass fiber) in the same manner as in Example 1 Pellets were prepared and injection specimens were prepared, and the results are shown in Table 2.

Example  7

34 wt% BASF's PPA resin (melting point: 295 ° C.) with polyphenylene amide A and 20 wt% Degusa's PPA resin (melting point 330 ° C.) with polyphenyleneamide B having another high heat resistance %, Boron nitride 5% by weight, titanium oxide (TiO ₂ ) 30% by weight, glass fiber (Glass fiber) 10% by weight except using a pellet and injection specimens were prepared in the same manner as in Example 1, the results are shown in Table 2 is shown.

Example  8

20 wt% of BASF's PPA resin (melting point: 295 ° C.) with polyphenylene amide A and 34 wt% of Degusa's PPA resin (melting point 330 ° C.) with polyphenyleneamide B having another high heat resistance %, Boron nitride 5% by weight, titanium oxide (TiO ₂ ) 30% by weight, glass fiber (Glass fiber) 10% by weight except using a pellet and injection specimens were prepared in the same manner as in Example 1, the results are shown in Table 2 is shown.

Example  9

Polyphenylene sulfide resin with 54% by weight of linear type PPS resin (melting point: 280 ℃), 5% by weight of boron nitride, 30% by weight of titanium oxide (TiO ₂ ), 10% by weight of glass fiber Pellets and injection specimens were prepared in the same manner as in Example 1 except for using the results, and the results are shown in Table 2.

Comparative example  One

Pellets were manufactured in the same manner as in Example 1, except that 60% by weight of PPA resin (melting point: 295 ° C), 30% by weight of TiO ₂ , and 10% by weight of glass fiber were used as polyphenylene amide A. And an injection specimen was prepared, the results are shown in Table 4.

Comparative example  2

In the same manner as in Example 1, except that 60% by weight of Deggusa's PPA resin (melting point: 330 ° C), 20% by weight of TiO _{2, and} 20% by weight of glass fiber were used as polyphenylene amide B. Pellets and injection specimens were prepared, and the results are shown in Table 4.

Comparative example  3

45 wt% of Deggusa's PPA resin (melting point: 330 ° C) with polyphenylene amide B, 15 wt% of PA6.6 (melting point: 255 ° C) from Rhodia, 30 wt% TiO _{2 with} Polyamide 6.6 %, Except that 10% by weight glass fiber (Glass fiber) was used to prepare pellets and injection specimens in the same manner as in Example 1, the results are shown in Table 4.

Table 1 below shows the composition ratio of the constituents of the components of the present invention.

Example 1 Example 2 Example 3 Example 4 Example
5 Example
6 Example
7 Example
8 Example
9 PPA A 54 54 54 49 49 49 34 20 PPA B 20 34 PPS 54 TiO ₂ 10 20 30 30 20 30 30 30 30 Boron nitride 5 5 5 10 20 5 5 5 Talc 10 Fiberglass 30 20 10 10 10 10 10 10 10

Example 1 Example 2 Example 3 Example 4 Example 5 Example
6 Example
7 Example
8 Example
9 Tensile strength (Kg / cm ² ) 1,430 1,220 1,000 950 920 890 980 960 900 Tensile elongation
(%) 8.3 7.9 6.5 4.0 3.8 3.7 5.5 5.2 2.0 Flexural strength
(Kg / cm ² ) 2,070 1,750 1,500 1,350 1,320 1,290 1,490 1,420 1,300 Flexural modulus (Kg / cm ² ) 91,000 72,000 55,000 69,000 67,000 65,000 67,000 70,000 74,000 Impact strength
(kJ / m ² ) 4.2 3.3 3.2 2.8 2.9 2.5 3.1 3.0 1.9 Linear expansion
Coefficient (MD) 15.9 21 29 - - - - - - MI
(g / 10 min) 13.1 16.9 24.2 17.5 16.1 16.9 18.3 13.1 - reflectivity
(%) 90.1 91.5 93 92 91 92.6 92.2 92.1 90.3 moisture
Absorption rate (%) 1.91 2.4 2.5 - - - - - Thermal conductivity
(w / mk) 0.35 0.38 0.40 0.45 0.50 0.42 0.40 0.40 0.52 Heat resistance
(℃) 273 269 261 262 262 261 265 290 262

Table 3 below shows the composition ratio of the contents of the constituents of the comparative examples.

Comparative Example 1 Comparative Example
2 Comparative Example
3 PPA A 60 PPA B 60 45 PA 6.6 15 TiO ₂ 30 20 30 Fiberglass 10 20 10

Comparative Example 1 Comparative Example 2 Comparative Example 3 Tensile strength (Kg / cm ² ) 1,000 1,250 830 Tensile elongation
(%) 6.5 7.7 4.1 Flexural strength
(Kg / cm ² ) 1,500 1,810 1,390 Flexural modulus (Kg / cm ² ) 55,000 73,000 53,000 Impact strength
(kJ / m ² ) 3.2 3.4 2.6 Linear expansion
Coefficient (MD) - - - MI
(g / 10 min) 24.2 - 110 reflectivity
(%) 93 91.2 91.9 moisture
Absorption rate (%) - - - Thermal conductivity
(w / mk) 0.34 0.32 0.33 Heat resistance
(℃) 261 295 230

As shown in the above embodiment, the resin composition according to the present invention is a material having a characteristic of light reflectivity of 92%, thermal conductivity of 0.5w / m.k, heat resistance of 260 ° C or more. In addition, as can be seen in Table 4, in the case of Comparative Example 3 using PA 6.6 having a melting point of 255 ℃, it can be seen that the physical properties are very poor compared to the Example.

Claims (11)

(a) 40 to 70% by weight of polyphenylene amide, which is a crystalline resin having a melting point of 270 ° C. or more, (b) 5 to 50 weight percent of titanium oxide (TiO ₂ ), (c) 1 to 40% by weight of thermally conductive fillers selected from the group consisting of boron nitride, talc, mica and wollastonite and (d) light emission comprising 5 to 30% by weight of a stiffness increasing agent selected from the group consisting of glass fibers, glass beads, and milled glass fibers Diode packaging composition. delete delete The composition of claim 1, wherein the polyphenylene amide has a melting point in the range of 270 ° C to 350 ° C. delete delete delete The composition of claim 1, wherein the composition further comprises syndiotactic polystyrene or polyamide 12.  The light emitting diode packaging composition of claim 1, further comprising an antioxidant, a UV light stabilizer, a fluorescent brightener, or a lubricant. 40-70% by weight of polyphenyleneamide, a crystalline resin having a melting point of at least 270 ° C, and 1-40% by weight of a thermally conductive filler selected from the group consisting of boron nitride, talc, mica or wollastonite Injected into the main inlet, and 5 to 50% by weight of titanium oxide (TiO ₂ ) to the first secondary inlet, glass fiber (glass glass), glass beads (glass bead) and milled glass fiber (Milled Glass fiber) 5 to 30% by weight of at least one stiffness increasing agent selected from the group consisting of a method for producing a light emitting diode packaging material, characterized in that the extruded after injection. The method of claim 10, wherein the main inlet is further added with syndiotactic polystyrene or polyamide 12 in addition to the crystalline resin.