CN105001649A

CN105001649A - High-performance organic silicon resin-polymethyl methacrylate composite material mixed with nanometer silicon nitride for LED package, and preparation method of high-performance organic silicon resin-polymethyl methacrylate composite material

Info

Publication number: CN105001649A
Application number: CN201510500340.5A
Authority: CN
Inventors: 朱志
Original assignee: Individual
Current assignee: Individual
Priority date: 2015-08-16
Filing date: 2015-08-16
Publication date: 2015-10-28

Abstract

The invention discloses a high-performance organic silicon resin-polymethyl methacrylate composite material mixed with nanometer silicon nitride for LED package. The composite material is a high-performance material which is formed by polymerization and curing of vinylphenyl silicone oil, hydrogen containing silicon resin, vinyl silicone resin and methyl methacrylate and has the hybrid advantages of organic silicon resin and polymethyl methacrylate; besides, powder formed by compounding nanometer silicon nitride which is mixed in the composite material, surface-treated with a silane coupling agent and wrapped by silica sol, magnesium sulfate whiskers and grapheme is good in compatibility with resin, and high in surface activity, after the powder is uniformly dispersed in the resin, the refractive index, the heat-conducting property, the heat dissipation performance, the high-temperature oxidation resistance, the insulation performance and other performance of the composite material can be improved greatly, and the prepared material is high in mechanical property, long in service life, high in transparency, and excellent in optical performance.

Description

High performance organo-silicon resin-composite material of polymethyl methacrylate of a kind of LED blending nano-silicon nitride and preparation method thereof

Technical field

The present invention relates to LED encapsulation material technical field, particularly relate to high performance organo-silicon resin-composite material of polymethyl methacrylate of a kind of LED blending nano-silicon nitride and preparation method thereof.

Background technology

LED refers to the encapsulation of luminescence chip; it works the keying action of forming a connecting link in LED industry chain; the packaged material that it uses changes to component parameter from factors such as envrionment temperature, humidity, external mechanical vibrations, surging forces for fixing and protect IC on the one hand; be on the other hand reduce chip and air refraction gap to increase light efficiency, and in time the heat of generation to be distributed.Conventional packaged material mainly contains the materials such as epoxy resin, modified epoxy and silicone resin, redix is mainly used in lower powered LED encapsulation material, it is restricted in high-power LED application, and silicone resin possesses the excellent advantage such as heat-proof aging, ultraviolet aging resistance, high permeability, low-stress, be well suited for as high-power LED encapsulation material.

The performance requriements of existing market high-power LED to packaged material mainly contains: high refractive index, high transmission rate, high thermal conductivity, resistance to ultraviolet, heat-proof aging and low thermal expansivity etc., domestic market is to the main dependence on import product of this high performance organosilicon encapsulating material, and these products also exist many defects, such as physical strength is lower, dispersiveness in silicone resin of ultraviolet light resistant poor performance, specific refractory power, transmittance, thermal conductivity and modified filler and consistency, stability etc. after encapsulation all need further lifting.

Summary of the invention

The object of the invention is exactly the defect in order to make up prior art, provides high performance organo-silicon resin-composite material of polymethyl methacrylate of a kind of LED blending nano-silicon nitride and preparation method thereof.

The present invention is achieved by the following technical solutions:

A kind of high performance organo-silicon resin-composite material of polymethyl methacrylate of LED blending nano-silicon nitride, this matrix material is prepared by the raw material of following weight part: phenyltrimethoxysila,e 70-80, organosilicon vinyl double-seal head agent 0.4-0.5, organosilicon hydrogeneous double-seal head agent 0.2-0.3, tetramethyl tetraphenyl cyclotetrasiloxane 10-12, Tetramethylammonium hydroxide 0.2-0.3, octamethylcyclotetrasiloxane 12-15, 2-phenyl-3-butyne-2-alcohol 3-5, erucicamide 0.1-0.2, toluene 50-60, platinum catalyst 0.01-0.02, concentration is the dilute hydrochloric acid 0.5-0.8 of 30%, deionized water 5-10, methyl methacrylate 12-15, solid content is the silicon sol 10-12 of 20-25%, Graphene 0.1-0.2, silane coupling agent kh550 0.1-0.2, nano-silicon nitride 2-3, magnesium sulfate crystal whisker 2-3, dibenzoyl peroxide 0.01-0.02.

The preparation method of the high performance organo-silicon resin-composite material of polymethyl methacrylate of described a kind of LED blending nano-silicon nitride, described preparation method is:

(1) first the double-seal head agent of organosilicon vinyl and the Tetramethylammonium hydroxide of 0.2-0.3 weight part will be added after tetramethyl tetraphenyl cyclotetrasiloxane, octamethylcyclotetrasiloxane under agitation vacuum hydro-extraction, be heated to 90-100 DEG C under nitrogen atmosphere, 160-180 DEG C is warming up to after reaction 6-8h, after constant temperature 20-30min, be decompressed to 0.05-0.095MPa, obtain vinyl phenyl silicone oil after steaming low boilers completely for subsequent use;

(2) dilute hydrochloric acid of hydrogeneous to the phenyltrimethoxysila,e of 20-30 weight part and organosilicon double-seal head agent, 0.1-0.2 weight part, the deionized water of 1-2 weight part are mixed, be heated to 70-80 DEG C, stirring reaction 4-5h, add the toluene of 15-20 weight part subsequently and be warming up to 100 DEG C, unnecessary deionized water is evaporated completely, finally be decompressed to 0.05-0.1MPa again, steam low-boiling point material completely, obtain Silicon Containing Hydrogen resin for subsequent use;

(3) by the phenyltrimethoxysila,e of residue part, the agent of organosilicon vinyl double-seal head, dilute hydrochloric acid, deionized water mixing, be heated to 70-80 DEG C, the toluene of residue part is added after stirring reaction 3-4h, and be progressively warming up to 100 DEG C and evaporate unnecessary deionized water, finally be decompressed to 0.05-0.1MPa again, steam low-boiling point material completely, obtain vinyl polysiloxane for subsequent use;

(4) drop in silicon sol by nano-silicon nitride, magnesium sulfate crystal whisker, Graphene, carry out heated drying after ultrasonic disperse is even, remove moisture completely, subsequently by the powder of gained and silane coupling agent kh550 mixing and stirring, gained material is for subsequent use;

(5) successively step (1), (2), (3), (4) and other leftover materials are added in reaction vessel, through deaeration process after being uniformly mixed, be heated to 70-80 DEG C of solidification 1.5-2h subsequently, after being finally warming up to 140-150 DEG C with the speed of 5 DEG C/min again, isothermal curing 0.5-1h, obtains described matrix material.

Advantage of the present invention is: the present invention utilizes vinyl phenyl silicone oil, Silicon Containing Hydrogen resin, vinyl polysiloxane and methyl methacrylate polymerization solidify to form a kind of high performance material having silicone resin concurrently and mix advantage with poly-methyl esters methyl acrylate, simultaneously blending wherein through silane coupling agent surface-treated, through the nano-silicon nitride that silicon sol is coated, the consistency of magnesium sulfate crystal whisker and graphene composite powder and resin is good, surfactivity is high, specific refractory power and the heat conduction of material is can greatly improve wherein after dispersed, heat radiation, resistance to high temperature oxidation, the performances such as insulation, the mechanical property of materials prepared is good, long service life, transparency is high, excellent optical performance.

Embodiment

The matrix material of the present embodiment is prepared by the raw material of following weight part: phenyltrimethoxysila,e 70, organosilicon vinyl double-seal head agent 0.4, the hydrogeneous double-seal head agent 0.2 of organosilicon, tetramethyl tetraphenyl cyclotetrasiloxane 10, Tetramethylammonium hydroxide 0.2, octamethylcyclotetrasiloxane 12, 2 phenylbutynol 3, erucicamide 0.1, toluene 50, platinum catalyst 0.01, concentration is the dilute hydrochloric acid 0.5 of 30%, deionized water 5, methyl methacrylate 12, solid content is the silicon sol 10 of 20%, Graphene 0.1, silane coupling agent kh550 0.1, nano-silicon nitride 2, magnesium sulfate crystal whisker 2, dibenzoyl peroxide 0.01.

The preparation method of the high performance organo-silicon resin composite material of polymethyl methacrylate of described a kind of LED blending nano-silicon nitride is:

(1) first the double-seal head agent of organosilicon vinyl and the Tetramethylammonium hydroxide of 0.2 weight part will be added after tetramethyl tetraphenyl cyclotetrasiloxane, octamethylcyclotetrasiloxane under agitation vacuum hydro-extraction, be heated to 90 DEG C under nitrogen atmosphere, 160 DEG C are warming up to after reaction 6h, after constant temperature 20min, be decompressed to 0.05MPa, obtain vinyl phenyl silicone oil after steaming low boilers completely for subsequent use;

(2) dilute hydrochloric acid of hydrogeneous to the phenyltrimethoxysila,e of 20 weight parts and organosilicon double-seal head agent, 0.1 weight part, the deionized water of 1 weight part are mixed, be heated to 70 DEG C, stirring reaction 4h, add the toluene of 15 weight parts subsequently and be warming up to 100 DEG C, unnecessary deionized water is evaporated completely, finally be decompressed to 0.05MPa again, steam low-boiling point material completely, obtain Silicon Containing Hydrogen resin for subsequent use;

(3) by the phenyltrimethoxysila,e of residue part, the agent of organosilicon vinyl double-seal head, dilute hydrochloric acid, deionized water mixing, be heated to 70 DEG C, the toluene of residue part is added after stirring reaction 3h, and be progressively warming up to 100 DEG C and evaporate unnecessary deionized water, finally be decompressed to 0.05MPa again, steam low-boiling point material completely, obtain vinyl polysiloxane for subsequent use;

(5) successively step (1), (2), (3), (4) and other leftover materials are added in reaction vessel, through deaeration process after being uniformly mixed, be heated to 70 DEG C of solidification 1.5h subsequently, after being finally warming up to 140 DEG C with the speed of 5 DEG C/min again, isothermal curing 0.5h, obtains described matrix material.

The thick sample of 3mm made by matrix material obtained by the present embodiment, and relevant criterion followed by this sample, and measured performance index are as follows:

Transmittance >=95% under 400-800nm visible light conditions; Specific refractory power is 1.735; The yellowness index of ultraviolet resistance burn-in test is 25; Hardness: 90A; Thermotolerance: toast 24h material without considerable change under 150 DEG C of conditions.

Claims

1. the LED high performance organo-silicon resin-composite material of polymethyl methacrylate of blending nano-silicon nitride, it is characterized in that, this matrix material is prepared by the raw material of following weight part: phenyltrimethoxysila,e 70-80, organosilicon vinyl double-seal head agent 0.4-0.5, organosilicon hydrogeneous double-seal head agent 0.2-0.3, tetramethyl tetraphenyl cyclotetrasiloxane 10-12, Tetramethylammonium hydroxide 0.2-0.3, octamethylcyclotetrasiloxane 12-15, 2-phenyl-3-butyne-2-alcohol 3-5, erucicamide 0.1-0.2, toluene 50-60, platinum catalyst 0.01-0.02, concentration is the dilute hydrochloric acid 0.5-0.8 of 30%, deionized water 5-10, methyl methacrylate 12-15, solid content is the silicon sol 10-12 of 20-25%, Graphene 0.1-0.2, silane coupling agent kh550 0.1-0.2, nano-silicon nitride 2-3, magnesium sulfate crystal whisker 2-3, dibenzoyl peroxide 0.01-0.02.

2. the preparation method of the high performance silicone resin-composite material of polymethyl methacrylate of a kind of LED blending nano-silicon nitride as claimed in claim 1, it is characterized in that, described preparation method is: