CN105802563A - Flowing type chip-grade bottom filling adhesive and preparation method thereof - Google Patents

Flowing type chip-grade bottom filling adhesive and preparation method thereof Download PDF

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Publication number
CN105802563A
CN105802563A CN201610246981.7A CN201610246981A CN105802563A CN 105802563 A CN105802563 A CN 105802563A CN 201610246981 A CN201610246981 A CN 201610246981A CN 105802563 A CN105802563 A CN 105802563A
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parts
epoxy resin
reactor
mix homogeneously
type epoxy
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CN105802563B (en
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闫善涛
王建斌
陈田安
解海华
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Yantai Darbond Technology Co Ltd
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Yantai Darbond Technology Co Ltd
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Priority to CN201610246981.7A priority Critical patent/CN105802563B/en
Priority to PCT/CN2016/081230 priority patent/WO2017181447A1/en
Priority to TW105118641A priority patent/TW201738350A/en
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    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J163/00Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02Non-macromolecular additives
    • C09J11/04Non-macromolecular additives inorganic
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02Non-macromolecular additives
    • C09J11/06Non-macromolecular additives organic
    • CCHEMISTRY; METALLURGY
    • C09DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09JADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/08Macromolecular additives
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2203/00Applications
    • C08L2203/20Applications use in electrical or conductive gadgets
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/02Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group
    • C08L2205/025Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group containing two or more polymers of the same hierarchy C08L, and differing only in parameters such as density, comonomer content, molecular weight, structure
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/03Polymer mixtures characterised by other features containing three or more polymers in a blend
    • C08L2205/035Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)
  • Inorganic Chemistry (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Epoxy Resins (AREA)

Abstract

The invention belongs to the technical field of filling adhesive preparation and particularly relates to flowing type chip-grade bottom filling adhesive and a preparation method thereof. No diluents is adopted in the chip-grade bottom filling adhesive prepared through the method, the adhesive has the advantages of being high in flowing speed, high in reliability, low in thermal expansion coefficient, high in bending modulus, low in moisture absorbility and the like, through adding of wetting dispersant, the effects of effectively lowering viscosity and increasing flowing speed are remarkable, it is more effective to disperse the filling material uniformly, and reliability of a packaged component is guaranteed.

Description

A kind of flow model chip-level bottom filling adhesive and preparation method thereof
Technical field
The invention belongs to filling glue preparing technical field, particularly relate to a kind of flow model chip-level bottom filling adhesive and preparation method thereof.
Background technology
Along with the development that Electronic Packaging industry is maked rapid progress, electronic package material be it is also proposed harsher requirement.The chip CTE made due to silicon materials is far below substrate, and in order to protect chip, stannum ball and solder joint and strengthen the reliability of chip, underfill is widely used in electronic package material.Underfill generally selects epoxy-resin systems to be material, and it has that toughness is high, corrosion-resistant, viscosity is high and the premium properties such as good insulating.But all there is the shortcomings such as fragility is big, reliability is low, internal stress is big, poor heat resistance, moisture resistance difference in major part underfill at present, is only capable of meeting tier 2 encapsulation requirement.
Summary of the invention
The present invention is directed to the deficiency that above-mentioned prior art exists, it is provided that a kind of flow model chip-level bottom filling adhesive and preparation method thereof.
The technical scheme is that a kind of flow model chip-level bottom filling adhesive, its component is by following weight portion composition: epoxy resin 18 parts~30 parts, toughener 1 part~3 parts, wetting dispersing agent 0.1 part~1 part, coupling agent 0.1 part~1 part, white carbon black 0.1 part~0.5 part, filler 50 parts~70 parts and 8 parts~15 parts of firming agent.
Further, described epoxy resin is the two or more mixing in bisphenol A type epoxy resin, bisphenol f type epoxy resin, Ppolynuclear aromatic epoxy resin, phenol aldehyde type epoxy resin.
Further, described bisphenol A type epoxy resin is E51, E44 or EPON825;Described bisphenol f type epoxy resin is EPIKOTE862 or EPIKOTE983U;Described Ppolynuclear aromatic epoxy resin is EPICLONHP4700, EPICLONHP4500 or EPICLONHP4032;Described phenol aldehyde type epoxy resin is DEN431, DEN438 or DEN439.
Adopt above-mentioned further scheme to provide the benefit that, select different types of epoxy resin to coordinate, it is possible to the advantage of the various epoxy resin of more effective performance so that heat stability, thermal coefficient of expansion etc. reach an equilibrium point, thus obtaining the combination property of excellence.
Further, described toughener is liquid nbr carboxyl terminal, methyl vinyl silicone rubber, dimethylvinylsiloxy silicone rubber, methyl phenyl vinyl silicone rubber or methyldiphenyl base vinyl silicone gum.
Adopting above-mentioned further scheme to provide the benefit that, the addition of toughener can regulate the toughness of solidfied material, effectively increases elastic modelling quantity, reduces thermal coefficient of expansion, meets shock proof requirement.
Further, described wetting dispersing agent is fatty alcohol-polyoxyethylene ether, aliphatic amine polyoxyethylene ether or alkylphenol polyoxyethylene.
Adopting above-mentioned further scheme to provide the benefit that, the addition of wetting dispersing agent effectively reduces system viscosity, increases system flowing wettability.
Further, described coupling agent is one or more mixing of β-(3,4-epoxycyclohexyl) ethyl trimethoxy silane, γ-glycidoxypropyltrimewasxysilane or γ mercaptopropyitrimethoxy silane.
Further, described white carbon black is high-carbon black pigment.
Further, described filler is that particle diameter is less than 15 μm and the ball-shaped silicon micro powder that mean diameter is 1.5 μm~7.5 μm.
Adopting above-mentioned further scheme to provide the benefit that, silicon powder maximum particle diameter 15 μm and mean diameter are between 1.5 μm~7.5 μm, it is ensured that the filling that small-gap suture chip can be quickly good, choose ball-shaped silicon micro powder so that resin reaches consistent with the mobility of filler.
Further, described firming agent is modified amine compound or anhydrides compound.
Further, described modified amine compound is modified aromatic amine, modified polyamide or modified dicyandiamine;Described anhydrides compound is THPA, HHPA, methyl tetrahydro phthalic anhydride or methyl hexahydrophthalic anhydride.
Second purpose of the present invention is in that the preparation method providing a kind of flow model chip-level bottom filling adhesive, and step is as follows:
(1) weigh epoxy resin 18 parts~30 parts and white carbon black 0.1 part~0.5 part, put into stirring 0.5~1h in reactor, after mix homogeneously, put in reactor after grinding;
(2) weigh toughener 1 part~3 parts, wetting dispersing agent 0.1 part~1 part and coupling agent 0.1 part~1 part, put into stirring 1~2h, mix homogeneously in reactor;
(3) weigh filler 50 parts~70 parts, put in reactor and stir 2~4 hours, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls at 20~25 DEG C, weighs 8 parts~15 parts of firming agent, is put into evacuation stirring 1~2h, mix homogeneously in reactor, obtains filling glue.
Further, the speed of agitator in step (1)-(3) is 1000rpm;Speed of agitator in step (4) is 300rpm.
Adopt above-mentioned further scheme to provide the benefit that, step (4) reduces mixing speed after adding firming agent, it is possible to reduce the heat that stirring produces.
Further, after the filler in step (3) is mixed homogeneously with other raw materials in a kettle., add in reactor after three-roll grinder grinds, 40~80 DEG C of standings.
Adopting above-mentioned further scheme to provide the benefit that, hot conditions is conducive to resin and the abundant wetting and dispersing of filler.
Further, in step (4), the vacuum of evacuation is less than-0.095MPa, need to pass into nitrogen protection during reactor pressure release.
The invention has the beneficial effects as follows: the chip-level bottom filling adhesive that the present invention prepares, do not adopt any kind of diluent and there is the features such as flowing velocity is fast, reliability is high, thermal coefficient of expansion is low, bending modulus is high, hygroscopicity is low, the addition of wetting dispersing agent effectively reduces viscosity, the effect increasing flowing velocity is notable, significantly more efficient filler is uniformly dispersed, it is ensured that the reliability of encapsulation components and parts.
Detailed description of the invention
Below in conjunction with example, principles of the invention and feature being described, example is served only for explaining the present invention, is not intended to limit the scope of the present invention.
The present invention is further illustrated by embodiment and comparative example.The product that following embodiment and comparative example are obtained is tested, and tests its viscosity, mobile performance, water absorption rate, curing performance, thermal coefficient of expansion, elastic modelling quantity, seven performance indications of shear strength respectively.
Viscosity is tested, and uses TA company of U.S. flow graph, rotating speed 1.5s-1, temperature 25 DEG C, unit Pa s.
Mobile performance is tested, spacer shims and coverslip, microscope slide form the device that gap is 50 μm (simulation encapsulation components and parts gaps), test product flowing 10mm required time, unit s when 100 DEG C.
Water absorption rate is tested, and uses saturated vapor test (PCT), temperature 121 DEG C, humidity 100%R.H., time 20h.
Curing performance is tested, and uses differential scanning calorimetry (DSC), and 150 DEG C of products of constant temperature are fully cured required hardening time, unit min.
Thermal coefficient of expansion test (CTE), according to U.S.'s ASTMD696 standard, uses thermomechanical analysis (TMA) test, unit μm/m DEG C.
Elastic modelling quantity is tested, and according to U.S.'s ASTME1142 standard, uses dynamic mechanical analyzer (DMA) test, unit GPa.
Shear strength is tested, and condition of cure is solidification 90min at 150 DEG C, according to China's GB/T7124-1986 method of testing, measures AL/AL shear strength, units MPa.
Embodiment 1
A kind of preparation method of flow model chip-level bottom filling adhesive, step is as follows:
(1) weigh bisphenol A type epoxy resin E5180g, phenol aldehyde type epoxy resin DEN431100g and white carbon black 5g, put in reactor and stir 0.5~1h with the speed of 1000rpm, after mix homogeneously, put in reactor after grinding;
(2) weigh liquid nbr carboxyl terminal 20g, fatty alcohol-polyoxyethylene ether 10g and γ mercaptopropyitrimethoxy silane 5g, put in reactor and stir 1~2h, mix homogeneously with the speed of 1000rpm;
(3) weigh the silicon powder 700g of mean diameter 7.5 μm, put in reactor and stir 2~4 hours with the speed of 1000rpm, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls at 20~25 DEG C, weighs methyl four benzonitrile acid anhydride 80g, is put into evacuation in reactor, stirs 1~2h, mix homogeneously with the speed of 300rpm, obtains filling glue.
Embodiment 2
A kind of preparation method of flow model chip-level bottom filling adhesive, step is as follows:
(1) weigh bisphenol f type epoxy resin EPIKOTE983U120g, Ppolynuclear aromatic epoxy resin ICLONHP4700100g and white carbon black 5g, put in reactor and stir 0.5~1h with the speed of 1000rpm, after mix homogeneously, put in reactor after grinding;
(2) weigh methyl phenyl vinyl silicone rubber 30g, aliphatic amine polyoxyethylene ether 10g and β-(3,4-epoxycyclohexyl) ethyl trimethoxy silane 5g, put into stirring 1~2h, mix homogeneously in reactor;
(3) weigh the silicon powder 630g of mean diameter 1.5 μm, put in reactor and stir 2~4 hours with the speed of 1000rpm, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls, at 20~25 DEG C, to weigh modified aromatic amine 100g, is put into evacuation in reactor, stirs 1~2h, mix homogeneously with the speed of 300rpm, obtains filling glue.
Embodiment 3
A kind of preparation method of flow model chip-level bottom filling adhesive, step is as follows:
(1) weigh bisphenol A type epoxy resin E44160g, Ppolynuclear aromatic epoxy resin ICLONHP4500100g and white carbon black 5g, put in reactor and stir 0.5~1h with the speed of 1000rpm, after mix homogeneously, put in reactor after grinding;
(2) weigh 3,5-dimethylphenyl vinyl silicone gum 20g, aliphatic amine polyoxyethylene ether 5g and β-(3,4-epoxycyclohexyl) ethyl trimethoxy silane 10g, put in reactor and stir 1~2h, mix homogeneously with the speed of 1000rpm;
(3) weigh the silicon powder 560g of mean diameter 5 μm, put in reactor and stir 2~4 hours with the speed of 1000rpm, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls, at 20~25 DEG C, to weigh modified dicyandiamine 140g, is put into evacuation in reactor, stirs 1~2h, mix homogeneously with the speed of 300rpm, obtains filling glue.
Embodiment 4
A kind of preparation method of flow model chip-level bottom filling adhesive, step is as follows:
(1) weigh bisphenol f type epoxy resin EPIKOTE862 epoxy resin 150g, phenol aldehyde type epoxy resin DEN439150g and white carbon black 5g, put in reactor and stir 0.5~1h with the speed of 1000rpm, after mix homogeneously, put in reactor after grinding;
(2) weigh methyl phenyl vinyl silicone rubber 30g, alkylphenol polyoxyethylene 5g and γ-glycidoxypropyltrimewasxysilane 10g, put in reactor and stir 1~2h, mix homogeneously with the speed of 1000rpm;
(3) weigh the silicon powder 500g of mean diameter 3 μm, put in reactor and stir 2~4 hours with the speed of 1000rpm, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls, at 20~25 DEG C, to weigh HHPA 150g, is put into evacuation in reactor, stirs 1~2h, mix homogeneously with the speed of 300rpm, obtains filling glue.
Comparative example 1
A kind of preparation method of chip-level bottom filling adhesive, step is as follows:
(1) weigh bisphenol f type epoxy resin EPIKOTE983U120g, Ppolynuclear aromatic epoxy resin ICLONHP4700100g and white carbon black 5g, put in reactor and stir 0.5~1h with the speed of 1000rpm, after mix homogeneously, put in reactor after grinding;
(2) weigh methyl phenyl vinyl silicone rubber 30g and β-(3,4-epoxycyclohexyl) ethyl trimethoxy silane 5g, put in reactor and stir 1~2h, mix homogeneously with the speed of 1000rpm;
(3) weigh 1.5 μm of silicon powder 630g of mean diameter, put in reactor and stir 2~4 hours with the speed of 1000rpm, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls, at 20~25 DEG C, to weigh HHPA 150g, is put into evacuation in reactor, stirs 1~2h, mix homogeneously with the speed of 300rpm, obtains filling glue.
Comparative example 2
A kind of preparation method of chip-level bottom filling adhesive, step is as follows:
(1) 3 are weighed, 4-epoxycyclohexyl-methyl-3,4-epoxycyclohexyl formic acid esters 400g, double; two (7-oxabicyclo [4.1.0] 3-methyl in heptan) adipate ester 400g and hexafluoro antimonate 5g, put in reactor and stir 0.5~1h with the speed of 1000rpm, after mix homogeneously, put in reactor after grinding;
(2) temperature is controlled at 15 DEG C~20 DEG C, weigh acrylic acid epoxy resin 100g, butyl acrylate 50g, 1,4-butanediol 30g, β-(3,4-epoxycyclohexyl) ethyl trimethoxy silane 10g, benzoyl peroxide 3g and white carbon black 2g put into evacuation in reactor, stir 2~4h with the speed of 500rpm, mix homogeneously, obtains filling glue.
The glue of filling prepared by above-described embodiment 1-4 carries out testing performance index with the comparative example 1-2 filling glue prepared, and data result is as shown in table 1.
Table 1 performance indications compare
From the data of table 1 it can be seen that the chip-level bottom filling adhesive for preparing of the present invention, it is longer than two grades of underfills, faster than two grades of underfills on flowing time hardening time so that glue is being filled and formed less internal flaw in solidification process;In thermal coefficient of expansion, water absorption rate, bending modulus, shear strength etc., relatively second level package underfill all has a clear superiority in.This just determines the chip-level bottom filling adhesive that the present invention prepares and has higher reliability, meets the requirement of one-level superchip level encapsulation.It addition, the addition of wetting dispersing agent in the present invention, effectively reducing viscosity, the effect increasing flowing velocity is notable.Owing to this chip-level bottom filling adhesive does not use any diluent, there is higher reliability.
The foregoing is only presently preferred embodiments of the present invention, not in order to limit the present invention, all within the spirit and principles in the present invention, any amendment of making, equivalent replacement, improvement etc., should be included within protection scope of the present invention.

Claims (9)

1. a flow model chip-level bottom filling adhesive, it is characterized in that, its component is by following weight portion composition: epoxy resin 18 parts~30 parts, toughener 1 part~3 parts, wetting dispersing agent 0.1 part~1 part, coupling agent 0.1 part~1 part, white carbon black 0.1 part~0.5 part, filler 50 parts~70 parts and 8 parts~15 parts of firming agent.
2. filling glue according to claim 1, it is characterised in that described epoxy resin is the two or more mixing in bisphenol A type epoxy resin, bisphenol f type epoxy resin, Ppolynuclear aromatic epoxy resin, phenol aldehyde type epoxy resin.
3. filling glue according to claim 2, it is characterised in that described bisphenol A type epoxy resin is E51, E44 or EPON825;Described bisphenol f type epoxy resin is EPIKOTE862 or EPIKOTE983U;Described Ppolynuclear aromatic epoxy resin is EPICLONHP4700, EPICLONHP4500 or EPICLONHP4032;Described phenol aldehyde type epoxy resin is DEN431, DEN438 or DEN439.
4. filling glue according to claim 1, it is characterised in that described toughener is liquid nbr carboxyl terminal, methyl vinyl silicone rubber, dimethylvinylsiloxy silicone rubber, methyl phenyl vinyl silicone rubber or methyldiphenyl base vinyl silicone gum;
Described wetting dispersing agent is fatty alcohol-polyoxyethylene ether, aliphatic amine polyoxyethylene ether or alkylphenol polyoxyethylene;
Described coupling agent is one or more mixing of β-(3,4-epoxycyclohexyl) ethyl trimethoxy silane, γ-glycidoxypropyltrimewasxysilane or γ mercaptopropyitrimethoxy silane;
Described white carbon black is high-carbon black pigment;
Described filler is that particle diameter is less than 15 μm and the ball-shaped silicon micro powder that mean diameter is 1.5 μm~7.5 μm.
5. filling glue according to claim 1, it is characterised in that described firming agent is modified amine compound or anhydrides compound.
6. filling glue according to claim 5, it is characterised in that described modified amine compound is modified aromatic amine, modified polyamide or modified dicyandiamine;Described anhydrides compound is THPA, HHPA, methyl tetrahydro phthalic anhydride or methyl hexahydrophthalic anhydride.
7. the preparation method of the flow model chip-level bottom filling adhesive described in a claim 1, it is characterised in that step is as follows:
(1) weigh epoxy resin 18 parts~30 parts and white carbon black 0.1 part~0.5 part, put into stirring 0.5~1h in reactor, mix homogeneously, put in reactor after grinding;
(2) weigh toughener 1 part~3 parts, wetting dispersing agent 0.1 part~1 part and coupling agent 0.1 part~1 part, put into stirring 1~2h, mix homogeneously in reactor;
(3) weigh filler 50 parts~70 parts, put in reactor and stir 2~4 hours, mix homogeneously, polished put into again in reactor, temperature controls at 40~80 DEG C, stands 3~8h;
(4) temperature controls at 20~25 DEG C, weighs 8 parts~15 parts of firming agent, is put into evacuation stirring 1~2h, mix homogeneously in reactor, obtains filling glue.
8. preparation method according to claim 7, it is characterised in that the speed of agitator in step (1)-(3) is 1000rpm;Speed of agitator in step (4) is 300rpm.
9. preparation method according to claim 7, it is characterised in that in step (4), the vacuum of evacuation is less than-0.095MPa, passes into nitrogen protection during reactor pressure release.
CN201610246981.7A 2016-04-20 2016-04-20 A kind of flow model chip-level bottom filling adhesive and preparation method thereof Active CN105802563B (en)

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CN201610246981.7A CN105802563B (en) 2016-04-20 2016-04-20 A kind of flow model chip-level bottom filling adhesive and preparation method thereof
PCT/CN2016/081230 WO2017181447A1 (en) 2016-04-20 2016-05-06 Fluid chip-level underfill resin and manufacturing method thereof
TW105118641A TW201738350A (en) 2016-04-20 2016-06-14 A kind of flow type chip level underfill and its preparation method

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