WO2018218597A1

WO2018218597A1 - High temperature resistant and aging resistant led packaging material

Info

Publication number: WO2018218597A1
Application number: PCT/CN2017/086813
Authority: WO
Inventors: 朱桂林
Original assignee: 苏州佳亿达电器有限公司
Priority date: 2017-06-01
Filing date: 2017-06-01
Publication date: 2018-12-06
Also published as: CN107980052A

Abstract

A high temperature resistant and aging resistant LED packaging material, comprising the following raw materials in parts by weight: 40-80 parts by weight of an epoxy resin, 20-60 parts by weight of a silicone resin, 20-60 parts by weight of a silicone oil, 10-40 parts by weight of octafluorobiphenyl diglycidyl ether, 10-50 parts by weight of a polyphenylene sulfide, 10-50 parts by weight of poly(1,4-cyclohexanedimethylene terephthalate), 2-20 parts by weight of a sericite powder, 5-30 parts by weight of a silica gel powder, 2-20 parts by weight of isobutyltriethoxysilane, 2-20 parts by weight of a butadienyl triethoxysilane, 5-25 parts by weight of an antioxidant, 10-50 parts by weight of a filler, 20-50 parts by weight of a diluent, and 5-40 parts of a curing agent. The LED packaging material has greatly increased aging and high temperature resistance, and has a broad market prospects.

Description

LED packaging material with high temperature resistance and aging resistance

Technical field

The invention relates to the technical field of LED luminaire materials, in particular to an LED packaging material with high temperature resistance and aging resistance.

Background technique

The choice of LED packaging methods, materials, structures, and processes is primarily determined by factors such as chip structure, optoelectronic/mechanical characteristics, specific applications, and cost. After more than 40 years of development, LED packaging has experienced the development stages of stent (LampLED), SMD (SMDLED), and power LED (PowerLED). With the increase of chip power, especially the development of solid-state lighting technology, new and higher requirements are put forward for the optical, thermal, electrical and mechanical structures of LED packages. In order to effectively reduce the thermal resistance of the package and improve the light extraction efficiency, a new technical idea must be adopted for the package design. In order to improve the reliability of the LED package, the potting compound is required to have low hygroscopicity, low stress, and aging resistance. Currently used potting compounds include epoxy resin and silica gel. The performance of packaging materials has a great effect on the use of LEDs. Today's LED packaging materials generally suffer from defects such as poor high temperature resistance, poor aging resistance and short service life.

Summary of the invention

The technical problem to be solved by the present invention is to provide an LED packaging material having high temperature resistance and aging resistance in view of the above deficiencies in the prior art.

In order to solve the above technical problems, the technical solution adopted by the present invention is: an LED packaging material having high temperature resistance and aging resistance, including the following raw materials by weight:

An LED packaging material having high temperature resistance and aging resistance, comprising the following parts by weight:

Preferably, the epoxy resin is a mixture of a glycidylamine epoxy resin and an alicyclic epoxy resin.

Preferably, the silicone oil is ethyl silicone oil, phenyl silicone oil, methyl hydrogen silicone oil, methyl phenyl silicone oil, methyl chlorophenyl silicone oil, methyl ethoxy silicone oil, methyl trifluoropropyl silicone oil, a mixture of one or more of methyl vinyl silicone oil, methyl hydroxy silicone oil, ethyl hydrogen siloxane oil.

Preferably, the antioxidant is a mixture of bisphenol A, triphenyl phosphite and phenyl diisooctyl phosphite.

Preferably, the filler is a mixture of nano zinc oxide powder, nano calcium carbonate powder, nano aluminum hydroxide powder, nano silicon carbide powder and glass fiber powder.

Preferably, the diluent is one of diglycidyl ether, propylene oxide butyl ether, propylene oxide phenyl ether, dipropylene oxide ethyl ether, tripropylene oxide propyl ether, and xylene. Or a mixture of multiples.

A method for preparing an LED packaging material having high temperature resistance and aging resistance, comprising the following steps:

1) Weigh 40-80 parts by weight of epoxy resin, 20-60 parts by weight of silicone resin, 20-60 parts by weight of silicone oil, 10-40 parts by weight of octafluorobiphenyl diglycidyl ether, and polyphenylene sulfide 10 by weight. 50 parts by weight, polybutylene terephthalate 1,4-cyclohexanedimethyl ester 10-50 parts by weight, isobutyl triethoxysilane 2-20 parts by weight, butadiene triethoxysilane 2 -20 parts by weight, 20-50 parts by weight of the diluent; heated and mechanically stirred until homogeneously mixed to obtain a mixture A;

2) adding the mixture A obtained in the step 1) and 2-20 parts by weight of the sericite powder, 5-30 parts by weight of the silica gel powder, and 10-50 parts by weight of the filler to the high temperature reaction kettle, heating and stirring 2-8 hours, obtaining a mixture B;

3) adding 5-25 parts by weight of the antioxidant, 5-40 parts by weight of the curing agent to the mixture B obtained in the step 2) by weight, and stirring uniformly;

4) The mixture obtained in the step 3) is placed in a vacuum defoaming machine for defoaming, and the defoaming time is 1-4.5 hours;

5) The mixture treated in the step 4) is added to a mold for curing, the curing temperature is 130 ° C - 155 ° C, and after curing, it is cooled to room temperature to prepare an LED packaging material having high temperature resistance and aging resistance.

The invention has the beneficial effects that the LED packaging material with high temperature resistance and aging resistance of the invention greatly improves the aging resistance and high temperature resistance of the LED packaging material by optimizing the raw material formulation and the material preparation method, and at the same time has good The refractive index, bond strength and light transmittance improve the stability of the material, improve the use effect of the produced LED products, extend the service life of the LED products, and have broad market prospects.

detailed description

The present invention will be further described in detail below with reference to the embodiments, so that those skilled in the art can refer to the description.

It is to be understood that the terms "having", "comprising" and "comprising" are used in the <RTIgt;

In order to solve the above technical problems, the technical solution adopted by the present invention provides: an LED packaging material having high temperature resistance and aging resistance, including the following raw materials by weight:

Wherein the epoxy resin is a mixture of a glycidylamine epoxy resin and an alicyclic epoxy resin. The glycidylamine epoxy resin has good heat resistance, and the alicyclic epoxy resin has good ultraviolet aging resistance. The glycidylamine epoxy resin and the alicyclic epoxy resin are compounded to improve the resistance of the material. Aging and heat resistance.

Among them, silicone is a highly crosslinked network structure of polyorganosiloxane, usually with methyltrichlorosilane, dimethyldichlorosilane, phenyltrichlorosilane, diphenyldichlorosilane or methyl Various mixtures of phenyldichlorosilane, silicone resin has low surface tension, small viscosity coefficient, high compressibility, etc. Nature, and has high temperature resistance and oxidation resistance. Silicone and glycidylamine epoxy resins and cycloaliphatic epoxy resins can produce synergistic effects, resulting in high hardness, high transparency, high aging resistance and heat resistance of the material, so that it can remain high at high temperatures. transparency.

Among them, octafluorobiphenyl diglycidyl ether is added to the glycidylamine epoxy resin and the alicyclic epoxy resin system, which can significantly improve the heat resistance of the material; polyphenylene sulfide can improve the material forming property and mechanical strength. Poly(1,4-cyclohexanedimethylene terephthalate) can improve the transparency of the material and improve the high temperature resistance of the material. Isobutyltriethoxysilane has strong anti-ultraviolet radiation properties, butadiene-based triethoxysilane can improve the bond strength of the material and increase the hardness of the material. Octafluorobiphenyl diglycidyl ether, polyphenylene sulfide, poly(1,4-cyclohexanedimethylene terephthalate), isobutyltriethoxysilane, butadiene-triethoxysilane When used, the heat resistance, transparency, ultraviolet aging resistance and mechanical strength of the obtained material can be effectively improved.

Among them, the sericite powder has a polarizing effect and has a strong absorption and shielding effect on ultraviolet rays, which can improve the mechanical properties of the material and improve its aging and ultraviolet resistance. The silica gel powder is made of high-quality silica gel with high transparency and has good thermal stability, chemical stability and high mechanical strength. The addition of silica gel improves the stability and heat resistance of the material.

Wherein, the silicone oil is ethyl silicone oil, phenyl silicone oil, methyl hydrogen silicone oil, methyl phenyl silicone oil, methyl chlorophenyl silicone oil, methyl ethoxy silicone oil, methyl trifluoropropyl silicone oil, methyl a mixture of one or more of vinyl silicone oil, methyl hydroxy silicone oil, ethyl hydrogen hydride oil. Silicone oil can further improve the stability, weather resistance and high temperature resistance of the material, and promote the uniform mixing of the components to improve the overall performance of the material.

Wherein, the antioxidant is a mixture of bisphenol A, triphenyl phosphite and phenyl diisooctyl phosphite. Bisphenol A, triphenyl phosphite and phenylisooctyl phosphite can produce synergistic effects and can significantly improve the aging resistance of materials.

Wherein, the filler is a mixture of nano zinc oxide powder, nano calcium carbonate powder, nano aluminum hydroxide powder, nano silicon carbide powder and glass fiber powder. The filler is prepared by grinding nano-zinc oxide powder, nano-calcium carbonate powder, nano-aluminum hydroxide powder, nano-silicon carbide powder and glass fiber powder into fine powder and then uniformly mixing. Nano zinc oxide powder can improve the UV radiation resistance of the material. The nanometer calcium carbonate powder can effectively improve the fluidity, smoothness and bending strength of the material; improve the stability of the material, heat resistance, aging resistance and toughness. Nano-aluminum hydroxide powder can improve the high temperature resistance of the material. Nano silicon carbide powder and The addition of glass fiber powder can greatly improve the hardness and mechanical strength of the material and prolong the service life of the material. A mixture of nano zinc oxide powder, nano calcium carbonate powder, nano aluminum hydroxide powder, nano silicon carbide powder and glass fiber powder is added as a filler to the raw material, and the components are synergistically combined to greatly improve the high temperature resistance of the material. Aging resistance, hardness and toughness improve the overall performance of the material.

Wherein the diluent is one or more of diglycidyl ether, propylene oxide butyl ether, propylene oxide phenyl ether, dipropylene oxide ethyl ether, tripropylene oxide propyl ether, and xylene. Kind of mixture.

The invention also provides a preparation method of the above LED packaging material with high temperature resistance and aging resistance, comprising the following steps:

The present invention will be further described in detail below in conjunction with specific embodiments.

Example 1:

The preparation method comprises the following steps: 1) weighing epoxy resin, silicone resin, silicone oil, octafluorobiphenyl diglycidyl ether, polyphenylene sulfide, and poly(1,4-cyclohexane) polybutylene terephthalate according to the above weight parts. Ester, isobutyltriethoxysilane, butadiene triethoxysilane, diluent; heated and mechanically stirred until homogeneously mixed to obtain a mixture A; 2) the mixture A obtained in the step 1) and The weighed sericite powder, silica gel powder, and filler are added to a high temperature reaction kettle, heated and stirred for 4 hours to obtain a mixture B; 3) an antioxidant is added to the mixture B obtained in the step 2) according to the above parts by weight, The curing agent is stirred uniformly; 4) the mixture obtained in the step 3) is subjected to defoaming in a vacuum defoaming machine, and the defoaming time is 3.5 hours; 5) the mixture after the step 4) is added to the mold for curing, The curing temperature is 145 ° C, and after cooling, it is cooled to room temperature to prepare an LED packaging material having high temperature resistance and aging resistance.

Example 2:

Example 3:

The preparation method comprises the following steps: 1) weighing epoxy resin, silicone resin, silicone oil, octafluorobiphenyl diglycidyl ether, polyphenylene sulfide, and poly(1,4-cyclohexane) polybutylene terephthalate according to the above weight parts. Ester, isobutyltriethoxysilane, butadiene triethoxysilane, diluent; heated and mechanically stirred until homogeneously mixed to obtain a mixture A; 2) the mixture A obtained in the step 1) and The weighed sericite powder, silica gel powder, and filler are added to a high temperature reaction kettle, heated and stirred for 4 hours to obtain a mixture B; 3) an antioxidant is added to the mixture B obtained in the step 2) according to the above parts by weight, The curing agent is stirred uniformly; 4) the mixture obtained in the step 3) is subjected to defoaming in a vacuum defoaming machine, and the defoaming time is 3 hours; 5) the mixture after the step 4) is added to the mold for curing, The curing temperature is 140 ° C, and after cooling, it is cooled to room temperature to prepare an LED packaging material having high temperature resistance and aging resistance.

Example 4:

Example 5:

The LED aging materials with high temperature resistance and aging resistance prepared by the above examples were subjected to ultraviolet aging test. The surface temperature of the sample was 60 ° C, and the UVB 313 UV lamp was selected. The irradiation intensity was 1.5 Kwh/m 2 , and the ultraviolet ray was irradiated. The test time was 0h, 720h, 1500h, 2000h, and the yellowing index (ΔYI) and the change of visible light transmittance (ΔT) of the corresponding time were sequentially measured.

UV aging: UV irradiation aging test was carried out in accordance with the requirements of the International Electrotechnical Commission standard IEC61345.

Test conditions: sample surface temperature 60 ± 5 ° C, ultraviolet light wavelength: 280 nm ~ 400 nm range, irradiation intensity is 0.5 ~ 2 Kwh / m2. The ultraviolet irradiation test time is 0 to 2000 h.

The yellowing index (△YI) is analyzed according to GB2409-80 "Plastic Yellow Index Test Method".

The change in transmittance of visible light (ΔT) was measured using an Agilengt 8453 UV-visible Spectroscopy System UV-Vis spectrophotometer.

The evaluation results of the LED package materials obtained in the above examples after testing by the above test methods are shown in Table 1 below.

Among them, Table 1 shows the change of the yellow index (ΔYI) and the change of the transmittance to visible light (ΔT) of the LED package material before and after UV aging.

Table 1

It can be seen from the above table that the LED packaging material with high temperature resistance and aging resistance of the present invention has low yellowing index after continuous 2,000 hours of testing in terms of ultraviolet aging resistance, and the transmittance of visible light. The change is also low, so the LED packaging material with high temperature resistance and aging resistance produced by the invention can ensure the long service life of the assembly.

Other performance tests of the LED package materials with high temperature resistance and aging resistance prepared in Examples 1-5 are carried out. The test items include Shore hardness, refractive index, bond strength (MPa), light transmittance, and heat resistance. Properties 200 ° C / 60 min. Among them, Shore hardness: measured according to GB/T2411-2008; refractive index measured according to GB/T6488-2008; light transmittance: measured according to GB/T2410-2008.

The test results are shown in Table 2 below:

Table 2

It can be seen from the test results that the LED package material with high temperature resistance and aging resistance of the invention has excellent heat resistance, hardness, refractive index and bond strength are suitable, and has excellent comprehensive performance, and can effectively improve the use of LED. Effect and service life.

Although the embodiments of the present invention have been disclosed as above, they are not limited to the specification and the implementation. The use of the applications listed in the specification can be applied to a variety of suitable fields for the present invention, and other modifications can be easily made by those skilled in the art, and therefore, without departing from the scope of the claims and the equivalents. The invention is not limited to the specific details.

Claims

An LED packaging material having high temperature resistance and aging resistance, characterized in that it comprises the following raw materials by weight:
The LED package material having high temperature resistance and aging resistance according to claim 1, comprising the following raw materials by weight:
The LED package material having high temperature resistance and aging resistance according to claim 1, comprising the following raw materials by weight:
The LED package material having high temperature resistance and aging resistance according to claim 1, comprising the following raw materials by weight:
LED seal with high temperature resistance and aging resistance according to any one of claims 1-4 The material is characterized in that the epoxy resin is a mixture of a glycidylamine epoxy resin and an alicyclic epoxy resin.
The LED package material with high temperature resistance and aging resistance according to any one of claims 1 to 4, wherein the silicone oil is ethyl silicone oil, phenyl silicone oil, methyl hydrogen silicone oil, methylbenzene. a mixture of one or more of silicone oil, methyl chlorophenyl silicone oil, methyl ethoxy silicone oil, methyl trifluoropropyl silicone oil, methyl vinyl silicone oil, methyl hydroxy silicone oil, ethyl hydrogen silicone oil .
The LED package material having high temperature resistance and aging resistance according to any one of claims 1 to 4, wherein the antioxidant is bisphenol A, triphenyl phosphite, and bisphosphonium phosphite. a mixture of octyl esters.
The LED package material with high temperature resistance and aging resistance according to any one of claims 1 to 4, wherein the filler is nano zinc oxide powder, nano calcium carbonate powder, nano aluminum hydroxide powder, nanometer. a mixture of silicon carbide powder and glass fiber powder.
The LED package material having high temperature resistance and aging resistance according to any one of claims 1 to 4, wherein the diluent is diglycidyl ether, propylene oxide butyl ether or propylene oxide benzene. A mixture of one or more of a group ether, dipropylene oxide ethyl ether, tripropylene oxide propyl ether, and xylene.
A method for preparing an LED package material having high temperature resistance and aging resistance according to claim 1, comprising the steps of:

1) Weigh 40-80 parts by weight of epoxy resin, 20-60 parts by weight of silicone resin, 20-60 parts by weight of silicone oil, 10-40 parts by weight of octafluorobiphenyl diglycidyl ether, and polyphenylene sulfide 10 by weight. 50 parts by weight, polybutylene terephthalate 1,4-cyclohexanedimethyl ester 10-50 parts by weight, isobutyl triethoxysilane 2-20 parts by weight, butadiene triethoxysilane 2 -20 parts by weight, 20-50 parts by weight of diluent; heated and mechanically stirred Mix until homogeneously mixed to obtain a mixture A;

2) adding the mixture A obtained in the step 1) and 2-20 parts by weight of the sericite powder, 5-30 parts by weight of the silica gel powder, and 10-50 parts by weight of the filler to the high temperature reaction kettle, heating and stirring 2-8 hours, obtaining a mixture B;

3) adding 5-25 parts by weight of the antioxidant, 5-40 parts by weight of the curing agent to the mixture B obtained in the step 2) by weight, and stirring uniformly;

4) The mixture obtained in the step 3) is placed in a vacuum defoaming machine for defoaming, and the defoaming time is 1-4.5 hours;

5) The mixture treated in the step 4) is added to a mold for curing, the curing temperature is 130 ° C - 155 ° C, and after curing, it is cooled to room temperature to prepare an LED packaging material having high temperature resistance and aging resistance.