CN102167886A - Epoxy resin composition and a method for preparing the same - Google Patents
Epoxy resin composition and a method for preparing the same Download PDFInfo
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- CN102167886A CN102167886A CN 201110007933 CN201110007933A CN102167886A CN 102167886 A CN102167886 A CN 102167886A CN 201110007933 CN201110007933 CN 201110007933 CN 201110007933 A CN201110007933 A CN 201110007933A CN 102167886 A CN102167886 A CN 102167886A
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Abstract
The invention relates to an epoxy resin composition with excellent electronic packaging manufacturability and a method for preparing the same. The epoxy resin composition includes at least following components: (A):epoxy resin of 100 amounts by weight, (B) linear phenolic resin of 10 to 100 amounts by weight, (C) curing accelerator of 0.01 to 15 amounts by weight, (D) silicon powder of 400 to 1600 amounts by weight, The curing accelerator includes more than two kinds of accelerators selected from imidazole compounds, minated compounds, organic phosphine compounds and latent accelerators. The invention provided epoxy resin composition is suitable for being used as packing material of chips or devices in industries of micro-electronics, electron and photoelectron, And the invention provided expoxy resin has excellent packaging properties,
Description
Technical field
The present invention relates to a kind of composition epoxy resin and preparation method thereof.Described composition epoxy resin is to be used for the matrix material that chip or device encapsulated in microelectronics, electronics and photoelectron industry.
Background technology
At electronics and microelectronic industry, protect the heat cured composition epoxy resin of common employing to encapsulate to electronic devices and components or chip.Along with the fast development of information industry, electronics miniaturization, lightweight and multifunctionality are irreversible trend, and for example, the unicircuit packing forms develops into many pins, extra-thin QFN, CSP, BGA etc. from few pin, large-sized DIP, SOP.For this reason, the composition epoxy resin material that is encapsulated in the chip outside is more and more thinner, so, more and more higher to the reliability requirement of packaged material.Simultaneously, in the encapsulation process process, the defective of profile becomes more obvious to the electronic devices and components Effect on Performance.
Composition epoxy resin as same with thermosetting compound material, the problem that always exists in scale operation and use is, because its production and encapsulation can only disposablely be finished, be difficult to do over again, so its production regulation and control difficulty is big, in addition, in use, the defective of packaging appearance can cause the scrap rate of electron device higher.
In the prior art, for example in patent documentation 1 (CN1233626A) and patent documentation 2 (US6822341B1), reported the method that adopts novel curing catalyst to improve packaging process respectively, but, the curing catalyst of its use speed when the composition package curing is slow, causes the problem that the fused sizing material overflows from die gap in the encapsulation process easily.The latent promotor of introducing in the patent documentation 3 (CN1600809A) has been improved curing speed, but, fast setting under its high temperature causes viscosity of material to increase fast, there are defectives such as pit, vestige on the electron device surface that causes encapsulation easily, simultaneously, this promotor poor stability, when producing composition epoxy resin, its difficult quality control.Patent documentation 4 (Japanese kokai publication hei 5-239321) has proposed the mobile way that improves of filler, but packaging process is not significantly improved.
Summary of the invention
The problem that The present invention be directed to is as above made.By concentrating on studies of the inventor, proposed to come the method for optimal control reactive behavior according to the difference of various curing catalyst catalytic activitys.Specifically, be by adopting the method that is used in combination and/or adopts non-latent promotor and latent promotor to be used in combination of multiple different types of curing catalyst, the curing speed of control composition epoxy resin in encapsulation process, regulate the said composition speed that viscosity increases under high temperature fused state, thereby the electronic devices and components of encapsulation or the surface imperfection of unicircuit finished product are reduced, yield rate significantly improves, and reaches the purpose of packaging process excellence.
The invention provides a kind of composition epoxy resin, it is characterized in that, have following component at least:
(A) Resins, epoxy: 100 weight parts,
(B) solidifying agent: 10～100 weight parts,
(C) curing catalyst: 0.01～15 weight part,
(D) mineral filler: 400～1600 weight parts,
Wherein, comprise the promotor more than 2 kinds that is selected from glyoxaline compound, tertiary amine compounds, organic phosphine compounds, the latent promotor in the described curing catalyst.
At least comprise a kind of latent promotor in the preferred described curing catalyst, the content of described latent promotor in whole curing catalysts is 5～99 weight %, more preferably 10～90 weight %.
The consumption of described curing catalyst is preferably 0.1～10 weight part with respect to 100 parts by weight of epoxy resin.
And then, the invention provides a kind of preparation method of composition epoxy resin, it comprises the steps: that the composition material metering that will have said components adds in the super mixer, carries out high speed dispersion and mixes; Subsequently, mix, be rolled into sheet after the discharging, after overcooling, be ground into powder, make finished product by screw extrusion press and/or double roller plastic-making device heating.
According to composition epoxy resin of the present invention, be used in combination and/or the adopt non-latent promotor and the latent promotor of different types of curing catalyst is used in combination more than 2 kinds owing to having adopted, can come curing catalyst in the optimal control composition epoxy resin solidification process to the reactive behavior of active group according to hope, can suppress simultaneously the composition epoxy resin product store and transportation in curing catalyst to the reactive behavior of active group, cause the defective of electron device thereby reduced when encapsulation is used, and help improving composition epoxy resin operability in the use.
In addition, manufacture method according to composition epoxy resin of the present invention, owing to adopted the above-mentioned raw materials component, in the process that said composition is used for encasing electronic components, has higher flowability when on die material, flowing, and when reaching the temperature of reaction of regulation, can promote epoxy composite to solidify fast, the electronic devices and components of encapsulation or the yield rate of unicircuit are significantly improved.
Embodiment
Composition epoxy resin of the present invention has following component at least:
(A) Resins, epoxy: 100 weight parts,
(B) solidifying agent: 10～100 weight parts,
(C) curing catalyst: 0.01～15 weight part,
(D) mineral filler: 400～1600 weight parts.
Above-mentioned Resins, epoxy can use this area Resins, epoxy commonly used, and preferred the use is selected from least a in o-cresol formaldehyde epoxy resin, biphenyl type epoxy resin, naphthalene type Resins, epoxy, dicyclopentadiene type Resins, epoxy, heterocyclic-type epoxy resin, bisphenol f type epoxy resin, the bisphenol A type epoxy resin.
Above-mentioned solidifying agent can use this area solidifying agent commonly used, preferably uses at least a in resol, dicyclopentadiene type resol, amino phenol urea formaldehyde, melamine resin, penylene type resol and the biphenyl type resol that is selected from phenol lacquer resins, phenyl methylcarbamate lacquer resins, monohydroxy or dihydroxy naphthlene resol, p-Xylol and phenol or naphthols polycondensation.
Above-mentioned mineral filler can be used this area inorganic filler commonly used, and preferred the use is selected from least a in powdered quartz powder, fusion SiO 2 powder, preparing spherical SiO 2 powder, the ball-aluminium oxide powder.
Comprise the promotor more than 2 kinds that is selected from glyoxaline compound, tertiary amine compounds, organic phosphine compounds, the latent promotor in the curing catalyst of the present invention, that is to say that curing catalyst of the present invention is the compound accelerant that different types of promotor combines more than 2 kinds.
In composition epoxy resin of the present invention, by adopting the combination of the different promotor more than 2 kinds, can the optimal control curing catalyst as a whole for the reactive behavior of said composition resin solidification reaction, and then the curing speed of control composition epoxy resin in encapsulation process, regulate the said composition speed that viscosity increases under high temperature fused state, improve liquidity, thereby the electronic devices and components of encapsulation or the surface imperfection of unicircuit finished product are reduced, yield rate significantly improves.
The inventor has studied the response characteristic of above-mentioned various promotor, discovery begins the difference of temperature and speed of reaction according to the reaction of different types of promotor, can design the particular combinations of promotor different more than 2 kinds, it has and is not reaching reactive behavior effect low, that reactive behavior uprises when reaching the regulation temperature of reaction before the temperature of reaction of regulation, thereby has finished the present invention.
Glyoxaline compound as curing catalyst of the present invention is not particularly limited, it can be the normally used general glyoxaline compound in this area, preferably be selected from glyoxal ethyline, 2, at least a in 4-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, the 2-heptadecyl imidazoles, glyoxal ethyline, 2 more preferably, 4-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, be preferably glyoxal ethyline, 2 especially, the 4-methylimidazole.
Tertiary amine compounds as curing catalyst of the present invention is not particularly limited, it can be the normally used general tertiary amine compounds in this area, preferably be selected from triethylamine Bian Ji dimethylamine, Alpha-Methyl Bian Ji dimethylamine, 2-(dimethylamino methyl) phenol, 2,4,6-three (dimethylamino methyl) phenol, 1, at least a in 8-diazabicyclo (5.4.0) undecylene-7 (DBU).More preferably triethylamine Bian Ji dimethylamine, 2-(dimethylamino methyl) phenol, 1,8-diazabicyclo (5.4.0) undecylene-7 (DBU) is preferably triethylamine Bian Ji dimethylamine, 1 especially, 8-diazabicyclo (5.4.0) undecylene-7 (DBU).
Organic phosphine compounds as curing catalyst of the present invention is not particularly limited, can be the normally used general organic phosphine compounds in this area, preferably be selected from least a in triphenylphosphine, trimethyl-phosphine, triethyl phosphine, tributylphosphine, three (p-methylphenyl) phosphine, three (nonyl phenyl) phosphine.More preferably triphenylphosphine, tributylphosphine, three (p-methylphenyl) phosphine are preferably triphenylphosphine, tributylphosphine especially.
Latent promotor as curing catalyst of the present invention is not particularly limited, can be the normally used general latent promotor in this area, preferably be selected from least a in boron trifluoride mono aminoethane, boron trifluoride quadrol, boron trifluoride aniline, boron trifluoride o-toluidine, boron trifluoride xylidine, boron trifluoride benzylamine, boron trifluoride ethylaniline, boron trifluoride pyridine, triphenylphosphine-benzoquinones affixture, tetraphenyl phosphine-adjacent dinaphthyl borate, the tetraphenyl phosphine-adjacent dinaphthyl silicate.More preferably boron trifluoride mono aminoethane, boron trifluoride aniline, boron trifluoride benzylamine, triphenylphosphine-benzoquinones affixture, tetraphenyl phosphine-adjacent dinaphthyl borate, tetraphenyl phosphine-adjacent dinaphthyl silicate are preferably boron trifluoride mono aminoethane, triphenylphosphine-benzoquinones affixture especially.
Particular combinations (compound accelerant) as curing catalyst of the present invention, can from above-mentioned promotor of enumerating, select two or more arbitrarily, as long as selected two or more promotor has different response characteristic (for example the response characteristic curve under reaction beginning temperature, speed of reaction, the high low temperature etc.), just can carry out arbitrary combination as required, to adapt to the specific requirement of composition epoxy resin in different curing reactions.For example, when the curing reaction of composition epoxy resin needs slowly stablely at low temperatures carry out but when at high temperature finishing fast, can adopt to have the promotor of stable speed of reaction at high temperature has the promotor of high reaction rate with not reacting at low temperatures combination in wide temperature range.In addition, can the kind and the array mode thereof of promotor suitably be selected according to needed viscosity of composition epoxy resin and mobile requirement.
Specifically, above-mentioned selected promotor more than 2 kinds can belong to the compound of same kind, for example all belong to glyoxaline compound, tertiary amine compounds, organic phosphine compounds or latent promotor, also can belong to different types of compound, for example the promotor more than 2 kinds belongs to glyoxaline compound, tertiary amine compounds, organic phosphine compounds or latent promotor respectively.Object lesson as the combination of curing catalyst of the present invention for example can list: the combination of glyoxal ethyline and triphenylphosphine, the combination of glyoxal ethyline and DBU, the combination of triphenylphosphine-benzoquinones affixture and DBU, the combination of triphenylphosphine-benzoquinones affixture and glyoxal ethyline, the combination of triphenylphosphine-benzoquinones affixture and triphenylphosphine, the combination of 2-phenyl-4-methylimidazole and DBU, the combination of 2-phenyl-4-methylimidazole and triphenylphosphine-benzoquinones affixture, the combination of boron trifluoride mono aminoethane and DBU, the combination of boron trifluoride mono aminoethane and glyoxal ethyline, the combination of boron trifluoride mono aminoethane and triphenylphosphine etc.
The consumption of described curing catalyst (i.e. the total amount of the promotor more than 2 kinds) is 0.01～15 weight part with respect to 100 parts by weight of epoxy resin.If the consumption of curing catalyst is lower than 0.01 weight part, problem insufficient or that curing reaction is long then might appear solidifying, if be higher than 15 weight parts, might occur then solidifying that defective increases, encapsulates problems such as scrap rate is big in too fast, the packaged device, be 0.1～10 weight part preferably with respect to 100 parts by weight of epoxy resin, more preferably 1～8 weight part is preferably 1.5～5 weight parts especially.
Wherein, preferably in described curing catalyst, comprise a kind above-mentioned latent promotor at least.The content of latent promotor in whole curing catalysts is 0～99 weight %, is preferably 5～99 weight %, more preferably 10～90 weight %.By in whole curing catalysts, containing the latent promotor more than the 10 weight %, can make full use of latent promotor is quickened curing reaction under the temperature of reaction of regulation characteristics, further control reactive behavior effectively, the progress of control curing reaction.From the balance angle of activity control, the content of latent promotor in whole curing catalysts is preferably 40～80 weight % especially.
If be used in combination two kinds of different latent promotor, begin the difference of temperature according to reaction separately, can be under different temperature of reaction piecewise control extent of reaction.And when being used in combination non-latent promotor and latent promotor, compare with the situation of the latent promotor of independent use more than 2 kinds, though the reactive behavior that can effectively avoid latent promotor to exist insufficient the regulation temperature of reaction under the also lower shortcoming of speed of reaction.
Non-latent promotor described in the present invention can be to be selected from above-mentioned glyoxaline compound, tertiary amine compounds, the organic phosphine compounds any.
In addition, can further comprise fire retardant in the composition epoxy resin of the present invention, described fire retardant is combination, aluminium hydroxide, the magnesium hydroxide, 9 that is selected from brominated epoxy resin and antimonous oxide, the 10-dihydro-9-oxy is assorted-assorted luxuriant and rich with fragrance, the 2-(6-oxygen-6-hydrogen-phosphine is assorted luxuriant and rich with fragrance) 1 of 10-phosphine, and at least a in 4-Resorcinol, the zinc borate.
In the present invention, can add the known coupling agent of the industry as required, for example be selected from γ-(2, the 3-glycidoxy) at least a in the group formed of propyl trimethoxy silicane, 2-(3,4 epoxycyclohexyl) ethyl trimethoxy silane, anilino propyl trimethoxy silicane, γ-Qiu Jibingjisanjiayangjiguiwan.
In addition, in the present invention, can add the known releasing agent of the industry as required, for example be selected from least a in carnauba wax, S wax, OP wax, 161P wax, Ployethylene Wax, the stearic acid etc.
And then, in the present invention, can add the known tinting material of the industry as required, for example be selected from carbon black, phthalein green grass or young crops, the titanium dioxide etc. any one.
According to the present invention, be used in combination and/or the adopted non-latent promotor and the latent promotor of different types of promotor is used in combination more than 2 kinds owing to having adopted as curing catalyst, can come curing catalyst in the optimal control composition epoxy resin solidification process to the reactive behavior of active group according to hope, therefore relaxed consumption to curing catalyst in the composition epoxy resin, the restriction of solidification value and set time, help prolonging mixing time and/or improve melting temperature, make between component and to mix more fully, reduced the defective that causes electron device when the inhomogeneous encapsulation that causes of product is used.Simultaneously, can suppress composition epoxy resin product curing catalyst in storing and transporting the reactive behavior of active group is helped improving composition epoxy resin product operability in the use.
The preparation method of composition epoxy resin of the present invention can adopt industry usual method, comprises the steps: the composition material metering with composition of the invention described above is added in the super mixer, carries out high speed dispersion and mixes; Subsequently, mix, be rolled into sheet after the discharging, after overcooling, be ground into powder, make finished product by screw extrusion press and/or double roller plastic-making device heating.In addition, also it can be pressed into cylindrical product by the moulding pancake making machine as required.
In manufacture method of the present invention, the Heating temperature in the described screw extrusion press is preferably 90～135 ℃, and the Heating temperature in the described double roller plastic-making device is preferably 80～98 ℃.Under the said temperature condition, composition epoxy resin of the present invention is being used for the process of encasing electronic components, has higher flowability when on die material, flowing, and when reaching temperature of reaction, the speed of response of composite curing promotor of the present invention is very fast, can effectively promote epoxy composite to solidify, the defective (as: overlap, pit, pore etc.) of the electronic devices and components or the unicircuit finished product of encapsulation is reduced, yield rate significantly improves.
[embodiment]
Adopt embodiment that the present invention is specifically described below, yet only otherwise exceed purport of the present invention, the present invention is not limited to following disclosed specific embodiment.
In following embodiment or comparative example, feed composition as composition epoxy resin, adopted biphenyl type epoxy resin (YX4000H as Resins, epoxy, epoxy equivalent (weight) 193,102 ℃ of softening temperatures), linear phenolic resin (TD2131 as solidifying agent, hydroxyl equivalent 103,80 ℃ of softening temperatures), ball-shaped silicon micro powder (SS-0183R as mineral filler, meso-position radius is 16.3 μ m), coupling agent (KH560), glyoxal ethyline (2-MZ) as curing catalyst, triphenylphosphine-benzoquinones affixture (TPP-BQ), 1,8-diazabicyclo (5.4.0) undecylene-7 (DBU), triphenylphosphine (TPP), fire retardant (aluminium hydroxide), releasing agent (carnauba wax), tinting material (carbon black) etc.Above-mentioned each material is commercially available reagent.
The preparation method of the composition epoxy resin sample of each embodiment and comparative example is as follows:
(embodiment 1)
Ball-shaped silicon micro powder (SS-0183R) 800 weight parts are joined in the super mixer, spray into KH560 coupling agent 5 weight parts, add biphenyl type epoxy resin (YX4000H) 100 weight parts, linear phenolic resin (TD2131) 100 weight parts, triphenylphosphine-benzoquinones affixture (TPP-BQ) 1 weight part, DBU promotor 0.8 weight part then, carnauba wax 1 weight part, aluminium hydroxide 20 weight parts, carbon black 0.2 weight part in batches.In super mixer, mixed then 20 minutes, and took out powder was heated mixing 5 minutes being preheated on 85～90 ℃ the double roller plastic-making device, the material after mixing is taken off be cooled to normal temperature, pulverize the sample powder that makes composition epoxy resin.
(embodiment 2)
As curing catalyst, use glyoxal ethyline 0.4 weight part to replace DBU promotor 0.8 weight part, in addition, other component is identical with embodiment 1, and the preparation method is also identical with embodiment 1.
(embodiment 3)
As curing catalyst, use triphenylphosphine 1.1 weight parts to replace DBU promotor 0.8 weight part, in addition, other component is identical with embodiment 1, and the preparation method is also identical with embodiment 1.
(embodiment 4)
As curing catalyst, use glyoxal ethyline 0.4 weight part and DBU promotor 0.8 weight part, in addition, other component is identical with embodiment 1, and the preparation method is also identical with embodiment 1.
(comparative example 1)
As curing catalyst, do not use triphenylphosphine-benzoquinones affixture (TPP-BQ), and change the consumption of DBU promotor into 1.3 weight parts, in addition, other component is identical with embodiment 1, and the preparation method is also identical with embodiment 1.
(comparative example 2)
As curing catalyst, do not use triphenylphosphine-benzoquinones affixture (TPP-BQ), and change the consumption of glyoxal ethyline into 0.8 weight part, in addition, other component is identical with embodiment 1, and the preparation method is also identical with embodiment 1.
Rerum natura (gelation time, helicoidal flow length, water-intake rate, encapsulation scrap rate, flame retardant properties) to the composition epoxy resin that obtains in each embodiment and the comparative example is measured.Concrete detection method is as follows.
Gelation time: hot plate method, it is 175 ± 1 ℃ that hot plate is heated temperature control, gets 0.3～0.5g powdered sample and is placed on the hot plate, and powder smelting is that fluid solidifies again, and record becomes the required time of solidified colloidal state from fluid.
Helicoidal flow length: adopt EMMI-1-66 helicoidal flow metal die to measure on the transfer mould press, 175 ± 1 ℃ of die temperatures are transmitted pressure 70 ± 2kg/cm
2, get powdered sample 20 ± 5g.
Water-intake rate: solidified 125mm * 13mm * 3.2mm sample is measured 121 ± 2 ℃ of temperature, air pressure 2atm, 24hr, the percentage that the weight before and after the mensuration boiling increases by steaming and decocting under high pressure (PCT) method.
Encapsulation scrap rate: adopt pie sample encapsulation TO-3P type triode, take out 100, check various surface imperfection, comprise vestige, excessive glue, pit, space, pore, crackle etc., calculate scrap rate.
Flame retardant properties: measure by national GB/T2408-1996 plastics combustibility test method, adopt horizontal vertical burning instrument.
The measurement result of above-mentioned every rerum natura is shown in table 1.Each components contents unit in the table is a weight part.
Table 1:
From above-mentioned table as can be seen, be used in combination among the embodiment 1～4 of the promotor more than 2 kinds as curing catalyst of the present invention, used the flowability of the embodiment 1～3 that contains latent promotor (TPP-BQ), the effect of water-absorbent aspect to be better than not using the embodiment 4 of latent promotor to a certain extent, but compare with an independent comparative example 1～2 of a kind of promotor that adopts, under the roughly the same situation of gelation time, any embodiment has obtained mobile significantly improvement, water-intake rate reduces and encapsulate the excellent effect that scrap rate declines to a great extent.
Claims (10)
1. a composition epoxy resin is characterized in that, has following component at least:
(A) Resins, epoxy: 100 weight parts,
(B) solidifying agent: 10～100 weight parts,
(C) curing catalyst: 0.01～15 weight part,
(D) mineral filler: 400～1600 weight parts,
Wherein, comprise the promotor more than 2 kinds that is selected from glyoxaline compound, tertiary amine compounds, organic phosphine compounds, the latent promotor in the described curing catalyst.
2. composition epoxy resin according to claim 1 wherein, comprises a kind of latent promotor at least in the described curing catalyst, the content of described latent promotor in whole curing catalysts is 5～99 weight %.
3. composition epoxy resin according to claim 1 and 2, wherein, described glyoxaline compound is to be selected from glyoxal ethyline, 2, at least a in 4-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4-methylimidazole, the 2-heptadecyl imidazoles;
Described tertiary amine compounds is to be selected from triethylamine Bian Ji dimethylamine, Alpha-Methyl Bian Ji dimethylamine, 2-(dimethylamino methyl) phenol, 2,4,6-three (dimethylamino methyl) phenol, 1, at least a in 8-diazabicyclo (5.4.0) undecylene-7;
Described organic phosphine compounds is to be selected from least a in triphenylphosphine, trimethyl-phosphine, triethyl phosphine, tributylphosphine, three (p-methylphenyl) phosphine, three (nonyl phenyl) phosphine;
Described latent promotor is to be selected from least a in boron trifluoride mono aminoethane, boron trifluoride quadrol, boron trifluoride aniline, boron trifluoride o-toluidine, boron trifluoride xylidine, boron trifluoride benzylamine, boron trifluoride ethylaniline, boron trifluoride pyridine, triphenylphosphine-benzoquinones affixture, tetraphenyl phosphine-adjacent dinaphthyl borate, the tetraphenyl phosphine one adjacent dinaphthyl silicate.
4. composition epoxy resin according to claim 1 and 2, wherein, the consumption of described curing catalyst is 0.1～10 weight part with respect to 100 parts by weight of epoxy resin.
5. composition epoxy resin according to claim 1 and 2, wherein, described Resins, epoxy is to be selected from least a in o-cresol formaldehyde epoxy resin, biphenyl type epoxy resin, naphthalene type Resins, epoxy, dicyclopentadiene type Resins, epoxy, heterocyclic-type epoxy resin, bisphenol f type epoxy resin, the bisphenol A type epoxy resin.
6. composition epoxy resin according to claim 1 and 2, wherein, described solidifying agent is at least a in resol, dicyclopentadiene type resol, amino phenol urea formaldehyde, melamine resin, penylene type resol and the biphenyl type resol that is selected from phenol lacquer resins, phenyl methylcarbamate lacquer resins, monohydroxy or dihydroxy naphthlene resol, p-Xylol and phenol or naphthols polycondensation.
7. composition epoxy resin according to claim 1 and 2, wherein, described mineral filler is to be selected from least a in powdered quartz powder, fusion SiO 2 powder, preparing spherical SiO 2 powder, the ball-aluminium oxide powder.
8. composition epoxy resin according to claim 1 and 2, it further comprises fire retardant, described fire retardant is combination, aluminium hydroxide, the magnesium hydroxide, 9 that is selected from brominated epoxy resin and antimonous oxide, the 10-dihydro-9-oxy is assorted-assorted luxuriant and rich with fragrance, the 2-(6-oxygen-6-hydrogen-phosphine is assorted luxuriant and rich with fragrance) 1 of 10-phosphine, and at least a in 4-Resorcinol, the zinc borate.
9. the preparation method of a composition epoxy resin is characterized in that, comprises the steps: the composition material metering with each described component in the claim 1～8 is added in the super mixer, carries out high speed dispersion and mixes; Subsequently, mix, be rolled into sheet after the discharging, after overcooling, be ground into powder, make finished product by screw extrusion press and/or double roller plastic-making device heating.
10. preparation method according to claim 9, wherein, the Heating temperature in the described screw extrusion press is 90～135 ℃, the Heating temperature in the described double roller plastic-making device is 80～98 ℃.
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