TW201144376A - Epoxy resin based molding material for use in sealing, and electronic components and devices - Google Patents

Abstract

Provided are: an epoxy resin composition for use in sealing, which exhibits excellent moldability and reflow resistance; and electronic components and devices which are provided with elements sealed with the resin composition. An epoxy resin composition for use in sealing, which comprises (A) an epoxy resin, (B) a curing agent, (C) a cure accelerator, (D) an inorganic filler, and (E) a silicon-containing polymer, said silicon -containing polymer (E) having a three-dimensional crosslinked structure and a weight-average molecular weight of 1500 to 7000.

Description

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an electronic component device for packaging an epoxy resin molding material molding material. [Prior Art] In recent years, with the miniaturization and light weight of electronic equipment, the installation has been progressing toward higher density, and the electronic component device has been developed into a surface mount type package. In order to increase the mounting density and lower the mounting height, the package is mounted so that the area occupied by the component with respect to the package becomes extremely thin. In addition, these packages are different from past pin insertion methods. That is, when mounted on a wiring board, the past pin is inserted into the wiring board, and since the wiring is self-wiring, the package is not directly exposed to high temperatures. However, Table \ is directly exposed to the soldering temperature (reflow temperature) due to the solder bath or reflow soldering device as a whole. As a result, the moisture absorbing moisture rapidly expands during welding, and peeling stress acts, which causes peeling between the component and the lead frame package, which causes the package crack to occur. Therefore, it is expected to develop solder heat resistance (resistance material). In order to meet these requirements, various epoxy resins have been reviewed so far, but only epoxy, and this has been used to improve the performance. The IC and the LSI for the pin-inserted type are thin and small, and the package-thickness type is mounted on the back side of the package-inserted package board for the solder-surface-mounted package. Therefore, the package that absorbs moisture in the package becomes an insert. It is a change from the main material resin which is excellent in electrical properties and electrical properties. -201144376 Good's heat resistance decreases with low moisture absorption, and the hardenability decreases with the improvement of adhesion. It is difficult to balance the physical properties. In view of the above, various epoxy resin modifiers have been reviewed, and one of them is a sulfur atom-containing compound which has been attracting attention in terms of adhesion to an insert such as a component or a lead frame (see, for example, Patent Documents 1 and 2). And a sulfonium coupling agent containing a sulfur atom (refer to, for example, Patent Document 3) or a styrene styrene phenol copolymer oligomer (see, for example, Patent Document 4). [PRIOR ART DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT PATENT DOCUMENT [Problem to be Solved by the Invention] However, when the sulfane coupling agent containing a sulfur atom described in the above Patent Document 3 is used, the adhesion to a noble metal such as Ag or Au is lacking. Increasing the effect' and using the sulfur atom-containing compound described in Patent Documents 1 and 2, even if the amount disclosed in the literature is added, the adhesion to the noble metal cannot be sufficiently improved, and depending on the case, it is considered that the sulfur is caused by the sulfur in the compound. The condition is worse. When the styrene-phenol-copolymerized oligomer described in Patent Document 4 is used, the other characteristics are not deteriorated, but the reflow-reducing effect is not obtained. As described above, in the past, it has not been possible to obtain a weld-return-resistant property, and the present invention has been completed in view of the above circumstances, and an object thereof is to provide an excellent reflow resistance without lowering moldability or flame retardancy. An epoxy resin molding material for encapsulation, and an electronic component device having components packaged using the material. [Means for Solving the Problem] The present invention relates to an epoxy resin molding material containing a specific cerium-containing compound and an electronic component device including the component encapsulated by the epoxy resin molding material for packaging. More specifically, it is as follows. (!) The present invention relates to an epoxy resin molding material for encapsulation comprising (A) an epoxy resin, (B) a hardener, (c) a hardening accelerator, (D) an inorganic filler, and (E) The ruthenium-containing polymer, (E) ruthenium-containing polymer has any two or all of the structures represented by the following general formula (I), the following general formula (II), and the following general formula (111)' ( E) The weight average molecular weight of the ruthenium-containing polymer is 15 Å or more and 7,000 or less, [Chemical Formula 1] R1 - O-Si - Ο - (I) Ο

I (In the formula (I), R 1 represents a substituted or unsubstituted hydrocarbon group having a carbon number of 丨 1-6, and at least one of the oxygen atoms is an oxygen atom constituting a siloxane coupling, and the oxygen atom other than the oxygen atom Hydrogen atom bonding), 201144376 [Chemical 2] R1

I - O - Si - Ο - (II) R1 (in the formula (II), R1 represents a substituted or unsubstituted hydrocarbon group having 1 to 6 carbon atoms" wherein R1 may be the same or different, and an oxygen atom At least one of them is an oxygen atom constituting a siloxane chain, and an oxygen atom other than the oxygen atom is bonded to a hydrogen atom), % - olsiloI I ο 11 (at least one of the oxygen atoms in the formula (III) is a siloxane The oxygen atom of the alkane bond 'and the oxygen atom other than the oxygen atom is bonded to the hydrogen atom). (2) The present invention relates to the epoxy resin molding material for encapsulation according to (1), wherein (E) the content of the ruthenium-containing polymer is 2.5 with respect to the (A) epoxy resin in the epoxy resin molding material for encapsulation. The mass% is more than 4% by mass. (3) The present invention relates to the epoxy resin molding material for encapsulation according to (1) or (2), wherein the (E) ytterbium-containing polymer in the encapsulating epoxy resin molding material is substituted in all of R1 Or the unsubstituted phenyl group is 4〇201144376 /〇 or more and 1 〇0 mole% or less. (4) The epoxy resin molding material for encapsulation according to any one of (1) to (3) further comprising a fluorene oligomer. (5) The epoxy resin molding material for encapsulation according to any one of (1) to (4) further comprising a decane compound (a) represented by the following formula (IV), R1 —(CH2)q—Si (OR')p (ιν) (R2)3-p (in the formula (IV), R1 represents a cycloalkyl or cycloalkenyl group having 5 to 8 carbon atoms, and R2 is the same as R1. Or a hydrocarbon group having a carbon number of 丨6, R3 represents a hydrocarbon group having 1 to 6 carbon atoms, and a part of a hydrogen atom represented by R1 to R3 may be substituted, p represents an integer of 1 to 3, and q represents 〇~3. Integer). (6) The present invention relates to an electronic component device comprising the component encapsulated by the epoxy resin molding material for encapsulation according to any one of (1) to (5). [Effects of the Invention] According to the epoxy resin molding material for encapsulation obtained by the present invention, an electronic component device having high reliability and excellent reflow resistance without lowering the formability and flame retardancy can be obtained, and the industrial price is large. [Embodiment] The present invention is an encapsulating epoxy resin comprising (A) an epoxy resin, (B) a curing agent, (c) a curing promoting 201144376 agent, (D) an inorganic chelating agent, and (E) a cerium-containing polymer. Forming material. The invention is described in detail below. [(E) cerium-containing polymer] The (E) cerium-containing polymer used in the present invention must have any or all of the structures represented by the following general formula (1), general formula (II), and general formula (III). Constructed ruthenium containing polymer. These polymers are three-dimensionally crosslinked ruthenium-containing polymers having a branched polyoxyalkylene, an oxime resin or an intermediate for oxime resin modification, and do not contain a linear polyoxyalkylene. R1 ο ά ο - ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( ( An oxygen atom of an alkane bond, the oxygen atom other than the oxygen atom is bonded to a hydrogen atom), [Chemical 6] R1

I —〇—Si-o— (II)

IJ R1 (In the formula (II), R1 represents a substituted or unsubstituted hydrocarbon group having a carbon number of 1 to 6-10-201144376, wherein R1 may be the same or different from the 'oxygen atom' to the constituent sand. Oxygen atom of the oxygen bond, and the oxygen atom other than the oxygen atom circulates the stomach to bond), [Chem. 7]

I 〇

I - 〇 - Si - o - (III) Ο (In the formula (III), at least one of the oxygen atoms is an oxygen atom constituting a bond of a sand oxide and the oxygen atom other than the oxygen atom is bonded to a hydrogen atom). The ruthenium-containing polymer of the present invention has a structure of any one or both of the structures represented by the above formula (I), formula (Π), and formula (III), but in the case of both, it is difficult to ignite From the viewpoint of the nature, R1 in the above formula (I) and (Π) is preferably a methyl group, an ethyl group, a propyl group, a butyl group or an isopropyl group. An alkyl group such as a group, an isobutyl group, a tert-butyl group, a pentyl group or a hexyl group; an alkenyl group such as a vinyl group, an allyl group, a butenyl group, a pentenyl group or a hexenyl group; a phenyl group; The methyl group, the propyl group and the phenyl group are preferred, and the phenyl group is more preferable from the viewpoint of fluidity and flame retardancy. Most of the compounds which can be obtained by linear polyoxyalkylene represented by fluorenone oil are liquid, have poor handleability, and are not able to obtain sufficient effects related to reflow resistance, and are polluting and flame retardant to the surface of the cured product. Sex also worsened. Further, even if the branched polyoxyalkylene has a structure different from the present invention, the example -11 - 201144376 such as a branched polyoxyalkylene containing an epoxy group has insufficient effect of lowering the modulus of elasticity, and is not obtained. The full effect of reflow resistance. Further, the weight average molecular weight (Mw) of the (E) ruthenium-containing polymer needs to be 1,500 or more and 7,000 or less. Further, it is preferably 2,000 or more and 5,500 or less, more preferably 2,000 or more and 3,500 or less. When the weight average molecular weight (Mw) is less than 1500, the ruthenium-containing polymer becomes liquid or semi-liquid at room temperature, and the handleability is deteriorated. At the same time, due to the low molecular component, the volatile content is increased, so the reflow-reduction cannot be sufficiently improved. Sex, and thus can not fully obtain flame retardancy. On the other hand, when the weight average molecular weight (Mw) is as large as more than 7,000 Å, the effect of lowering the modulus of elasticity in a high temperature region is insufficient, and the reflow resistance tends to be insufficiently improved. Further, from the viewpoint of fluidity, it is preferably from 2,000 to 3,500, and further, even if the molecular weight is low in this range, there is a tendency to be excellent in fluidity and flame retardancy. Here, 'M w is obtained by gel permeation chromatography (G pc ) using a calibration curve using standard polystyrene. The above Mw is used as a pump for GPC (manufactured by Hitachi, Ltd.). Model l-6200), pipe column (TSKgel-G5000HXL + TSKgel-G2000HXL, all manufactured by TOSHO Co., Ltd.), detector (L-3 00RI type manufactured by Hitachi, Ltd.), with tetrahydrofuran The result of the measurement was carried out as a solution at a temperature of 30 ° C and a flow rate of 1.0 ml/min. Further, in terms of formability, reflow resistance, and flame retardancy, (E) ratio of substituted or unsubstituted phenyl groups in all of R 1 in the sand-containing polymer (proportion of Ph groups) It is preferably 40 mol% or more and 丨〇〇 mol% or less, more preferably 50 mol% or more and 90 mol% or less. When the amount is 4% or more, -12- 201144376 'The compatibility with the epoxy resin or the hardener is good, and it does not easily penetrate the surface of the cured material' and it is not easy to cause poor appearance. Further, the effect of reducing the modulus of elasticity in the room temperature region or the high temperature region can be easily sufficiently obtained, and the reflow resistance can be sufficiently improved. In addition, there is also a tendency to improve the flame retardancy. In particular, g is preferably 50 mol% or more from the viewpoint of reflow resistance and flame retardancy. Further, from the viewpoint of easiness of production of the sand-containing polymer and difficulty in obtaining the ruthenium-containing polymer, it is preferably 90 mol% or less. Further, even in this range, the higher the ratio of the Ph group, the more excellent the flame retardancy. Here, the ratio of the 'P h group can be calculated from the Η NMR of the ruthenium-containing polymer to calculate the Si atom of the 'Si-0-Si bond, and the phenyl group relative to the substituent on the Si atom (phenyl, alkoxy) is calculated. The molar ratio of the base, hydroxyl group, etc., as the ratio of the Ph group. Further, in the present invention, attention is paid to dividing the ratio of the substituted or unsubstituted phenyl group (the ratio of Ρ1 to the base) in all of R 1 in the above (E) ruthenium-containing polymer by the molecular weight (Ph/). At Mw), Ph/Mw is considered to be the ratio of the simple phenyl group to the ruthenium-containing polymer as a whole. The higher the Ph/Mw, the more excellent the fluidity, and the superior the reflow resistance in the high-temperature region, which is excellent in the effect of reducing the modulus of elasticity. The (E) ruthenium-containing polymer can be obtained by the following production method, but as a commercial product, it can be obtained from T矽ray Dow Corning Co., Ltd., an oxime resin or an oxime resin modification intermediate SH- 6018, 217 FLAKE, 220 FLAKE, 23 3 FLAKE and other commercial products. (E) The method for producing the sand-containing polymer can be produced by a conventional method without particular limitation. For example, a hydrolyzed condensation reaction can be used to form an organochlorodecane, an organoalkoxydecane, a decane which is a unit represented by the above formula -13- 201144376 (I), formula (II), and formula (ΠΙ). Or a partial hydrolysis condensate is obtained by mixing a mixture of an organic solvent capable of dissolving a raw material and a reaction product with water in an amount which can hydrolyze all of the hydrolyzable groups of the raw material, by a hydrolysis condensation reaction. In order to reduce the amount of chlorine contained as an impurity in the epoxy resin forming material for encapsulation, it is preferred to use an organic alkoxy decane and/or a decane as a raw material. In this case, an acid, a base or an organometallic compound is preferably added as a catalyst for promoting the reaction. Further, the molecular weight (Mw) of the ruthenium-containing polymer and the ratio of the phenyl group can be adjusted depending on the feed ratio of the raw material for production, the organic solvent, water, the reaction catalyst, or the like, or the reaction temperature, the reaction time, and the like. The molecular weight is mainly susceptible to the concentration or feed ratio of the raw materials in the organic solvent, and the proportion of the phenyl group is mainly affected by the feed ratio of the raw materials. The organoalkoxydecane and/or oxime which is a raw material of the (E) ruthenium-containing polymer is exemplified by methyltrimethoxydecane, methyltriethoxydecane, ethyltrimethoxydecane, and ethyltriphenyl. Ethoxy decane, vinyl trimethoxy decane, vinyl triethoxy decane, phenyl trimethoxy decane, phenyl triethoxy decane 'dimethyl dimethoxy decane, methyl phenyl dimethyl Oxy decane, methyl vinyl dimethoxy decane, phenyl vinyl dimethoxy decane, diphenyl dimethoxy decane, methyl phenyl diethoxy decane, methyl vinyl diethoxy Decane, phenylethylene fluorene diethoxy decane, diphenyl bis oxy decane, dimethyl diethoxy decane, tetramethoxy decane, tetraethoxy decane, dimethoxy diethoxy The content of the above-mentioned (E) ruthenium-containing polymer, such as decane, and the like, may be as long as the content of the above-mentioned (E) ruthenium-containing polymer is up to the range of the invention -14,044,376, which is not particularly limited 'but as the content increases', there will be room temperature, The elastic modulus in the high temperature region is reduced, 'the reflow resistance is improved', and the high tendency is 'reducing the amount of blending' The hardness is increased in the case of heat, and it is preferably 2.5% by mass or more and 40% by mass or less, more preferably 30% by mass or less, more preferably 1 〇 by mass, based on the λ fat in the epoxy resin molding material for encapsulation. More than %. [(A) Epoxy Resin] The epoxy resin used in the present invention is not particularly limited as long as it is one or more epoxy groups, and is exemplified by, for example, a lacquer epoxy resin or an o-cresol novolak type. Epoxy resin, methane skeleton epoxy resin represented by phenol, cresol, dimethyl cresol, catechol, bisphenol A, bisphenol F and other phenols and / or naphthol, dihydroxy naphthalene and other naphthols The phenolic varnish resin obtained by condensation of a compound having an aldehyde group such as formaldehyde, acetaldehyde or salicylic acid salicylaldehyde under an acidic catalyst is epoxidized, substituted or unsubstituted bisphenol A or double with an alkyl ring Polyglycidyl ethers such as phenol F and bisphenol glutarylene glycol, bismuth type epoxy resins, hydrogen lipids, phthalic acid, dimer acid and the like, and epichlorohydrin-glycidyl ester type epoxy resin, Aminodiphenylmethane, a polyglycidylamine type obtained by the reaction of a polyamine with epichlorohydrin, an epoxide of a cyclopentadiene and a phenolic co-condensation resin, from an oxy-resin, a phenol, and/or a naphthalene The tendency of the phenolic and dimethoxy-dimethyl groups to be elastic and flame retardant is also mentioned. The bismuth (Α) epoxy tree is preferably 5 mass% and 20% by mass, and the phenolic phenolic aldehyde is substituted with triphenylphenol, isophthaloyl-naphthol, β-, benzaldehyde, or co-condensation. Aromatic; bisphenol, thiophene type epoxy tree should be obtained by oxygenating resin such as cyanuric acid, cyclopentene having two naphthalene rings or bisphenol synthesized by bis(methoxy-15- 201144376 methyl)biphenyl An epoxide of an aralkyl type phenol resin such as an aralkyl resin or a naphthol/aralkyl resin, a trimethylolpropane type epoxy resin or a terpene-modified epoxy resin, which is a peracid such as peracetic acid A linear aliphatic epoxy resin, an alicyclic epoxy resin, or the like obtained by oxidizing an olefin bond may be used alone or in combination of two or more. Among them, in view of both fluidity and hardenability, a biphenyl type epoxy resin preferably containing a bis-glycidyl ether of an alkyl group, an aromatic ring substituted or an unsubstituted biphenol is hardenable. From the viewpoint of low hygroscopicity, a dicyclopentadiene type epoxy resin is preferable, and it is preferable to contain a dicyclopentadiene type epoxy resin from the viewpoint of heat resistance and low warpage. The naphthalene type epoxy resin preferably contains a bisphenol F type ring of a bisglycidyl ether of bisphenol F substituted by an alkyl group, an aromatic ring or an unsubstituted one from the viewpoint of both fluidity and flame retardancy. Oxygen resin, in terms of both fluidity and reflowability, a thiodiphenol type epoxy preferably containing a diglycidyl ether of an alkyl substituted, an aromatic ring substituted or an unsubstituted thiodiphenol The resin preferably contains an alkyl group-substituted, aromatic ring-substituted or unsubstituted phenol and dimethoxy-p-xylene or bis(methoxymethyl) from the viewpoint of both hardenability and flame retardancy. ) epoxide of phenol/aralkyl resin synthesized by biphenyl, which is stable and difficult to store The viewpoint of both is preferably substituted by a group containing an aromatic ring, a substituted or unsubstituted naphthols of the dimethoxyparaxylene • synthesis of naphthol aralkyl epoxy resin. The biphenyl type epoxy resin is exemplified by an epoxy resin represented by the following general formula (V). -16- 201144376 [Chem. 8] 〇-CH2-CH*CH2 (V) (wherein R1 to R8 are selected from a hydrogen atom and a substituted or unsubstituted one-valent hydrocarbon group having 1 to 10 carbon atoms; All the same or different, η represents an integer of 0 or 1 to 3). The biphenyl type epoxy resin represented by the above formula (V) is obtained by reacting epichlorohydrin with a biphenol compound by a known method. R1 to R8 in the formula (V) are exemplified by an alkyl group having 1 to 10 carbon atoms such as a hydrogen atom, a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group or a t-butyl group; The alkenyl group having 1 to 10 carbon atoms such as a vinyl group, an allyl group and a butenyl group is preferably a hydrogen atom or a methyl group. These epoxy resins are exemplified by, for example, 4,4'-bis(2,3-epoxypropoxy)biphenyl or 4,4'.bis(2,3-epoxypropoxy)-3. , 3',5,5'-tetramethylbiphenyl as the main component of epoxy resin, making epichlorohydrin and 4,4'-biphenol or 4,4'-(3,3',5,5' -Epoxy resin obtained by the reaction of -tetramethyl)biphenol. Among them, an epoxy resin containing 4,4'-bis(2,3-epoxypropoxy)-3,3',5,5'-tetramethylbiphenyl as a main component is preferred. These epoxy resins are commercially available from the Japan Epoxy Resin Co., Ltd. under the trade names of ΥΧ-4000 and YL-6121H. The biphenyl type epoxy resin is preferably used in an amount of 20% by mass or more, more preferably 30% by mass or more, and still more preferably 50% by mass or more based on the total amount of the epoxy resin. The thiodiphenol type epoxy resin is exemplified by an epoxy resin represented by the following formula (VI). -17- (VI) (VI)201144376 [Chemical 9] R' R2 R^R6 〇HR' R2 RJ R6 CH2-CH-CH2-^〇-^-S-^-〇-CHj-CH-CH2j〇- ^-S-^-〇-CH2-CH-CH2 (wherein R1 to R8 are selected from a hydrogen atom and a substituted or unsubstituted one-valent hydrocarbon group having a carbon number of 1 to 10, and all may be the same or different' η represents an integer of 0 or 1 to 3). The thiodiphenol type epoxy resin represented by the above formula (VI) is obtained by reacting epichlorohydrin with a thiodiphenol compound by a known method. R1 to R8 in the formula (VI) are exemplified by an alkyl group having 1 to 10 carbon atoms such as a hydrogen atom, a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group or a t-butyl group; The alkenyl group having 1 to 10 carbon atoms such as a vinyl group, an allyl group and a butenyl group is preferably a hydrogen atom, a methyl group or a tributyl group. These epoxy resins are exemplified by, for example, an epoxy resin having a diglycidyl ether of 4,4'-dihydroxydiphenyl sulfide as a main component, and 2,2',5,5'-tetramethyl-4 , 4'-dihydroxydiphenyl sulfide diglycidyl ether as the main component of the epoxy resin, 2,2'-dimethyl-4,4'-dihydroxy-5,5'- two third Epoxy resin or the like as a main component of diglycidyl ether of butyl diphenyl sulfide, preferably 2,2'-dimethyl-4,4'-dihydroxy-5,5'-di The diglycidyl ether of tributyldiphenyl sulfide is used as a main component of the epoxy resin. These epoxy resins are commercially available from the trade name YSLV-120TE manufactured by Shinco Steel Chemical Co., Ltd. In order to exhibit the performance, the thiodiphenol type epoxy resin is preferably used in an amount of 20% by mass or more based on the total amount of the epoxy resin, more preferably 30% by mass or more, and still more preferably 50% by mass or more. -18- 201144376 Bisphenol F-type epoxy resin is exemplified by, for example, the following general formula (VII) _ $ epoxy resin. [Chem. 10] c^ch-Ch2^ch^〇^^ (wherein R1 to R8 are selected by a hydrogen atom and a substituted or unsubstituted one-valent hydrocarbon group having a carbon number of 1 to 1 Å, which may all be the same Different, n means 〇 or an integer of 1 to 3). The bisphenol F type epoxy resin represented by the above formula (VII) is obtained by reacting epichlorohydrin with a bisphenol F compound by a conventional method. R1 to R8 in the formula (VII) are exemplified by an alkyl group having 1 to 10 carbon atoms such as a hydrogen atom, a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group, an isobutyl group or a t-butyl group; The alkenyl group having 1 to 10 carbon atoms such as a vinyl group, an allyl group and a butenyl group is preferably a hydrogen atom or a methyl group. These epoxy resins are exemplified by, for example, an epoxy resin having a diglycidyl ether of 4,4'-methylbis(2,6-dimethylphenol) as a main component, and a 4,4'-methyl group. Epoxy resin containing bis(2,3,6-trimethylphenol) diglycidyl ether as a main component, epoxy resin having 4,4′-methyl bisphenol diglycidyl ether as a main component, etc. Among them, an epoxy resin having a diglycidyl ether of 4,4'-methyl bis(2,6-dimethylphenol) as a main component is preferred. These epoxy resins are commercially available from the trade name YSLV-80XY manufactured by Nippon Steel Chemical Co., Ltd. In order to exhibit the performance, the bisphenol F-type epoxy resin is preferably formulated in an amount of 20% by mass to -19 to 201144376, more preferably 30% by mass or more, and even more preferably 50% by mass. the above. The novolac type epoxy resin is exemplified by an epoxy resin represented by the following formula (VIII). [化11]

(VIII) (wherein 'R is selected from a hydrogen atom and a substituted or unsubstituted one-valent hydrocarbon group having 1 to 1 carbon number, and η represents an integer of 〇~1〇)" expressed by the above formula (VIII) The novolac type epoxy resin can be easily obtained by reacting epichlorohydrin with a novolac type phenol resin. Wherein R in the above formula (VIII) is preferably an alkyl group having a carbon number of 1 to 1 Å such as a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group or an isobutyl group; a methoxy group; The alkoxy group having a carbon number of 1 to 1 Å, such as an oxy group, a propoxy group or a butoxy group, more preferably a hydrogen atom or a methyl group η is preferably an integer of 0 to 3. The furfural varnish type epoxy resin represented by the above formula (νιπ) is preferably an o-cresol novolac type epoxy resin. These epoxy resins are commercially available from Sumitomo Chemical Industries Co., Ltd. under the trade name · · ESCN-190 » When using novolak-type epoxy resin, 'in order to exert its performance', the blending amount is preferably epoxy resin. More than 20% by mass of the total amount is more preferably 3% by mass or more. The dicyclopentadiene-type epoxy resin is exemplified by an epoxy resin represented by the following formula (Ιχ). -20- (IX) (IX) 201144376 [Chem. 12]

(wherein 'R1 is selected from a hydrogen atom and a substituted or unsubstituted one-valent hydrocarbon group having a carbon number of 1 to 1 Å, 'R2 is a substituted or unsubstituted one-valent hydrocarbon group having a carbon number of 1 to 1 Å, respectively. Selected, η represents an integer of 〇~10, and m represents an integer of 〇~6). R1 in the above formula (IX) is exemplified by an alkyl group such as a hydrogen atom, a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group or a tributyl group; a vinyl group, an allyl group, a butenyl group or the like. Alkenyl; a halogenated alkyl group, an amine-substituted alkyl group, a mercapto-substituted alkyl group, etc., a substituted or unsubstituted one-valent hydrocarbon group having 1 to 10 carbon atoms, preferably an alkyl group such as a methyl group or an ethyl group. And a hydrogen atom, more preferably a methyl group and a hydrogen atom. R2 is exemplified by an alkyl group such as a hydrogen atom, a methyl group, an ethyl group, a propyl group, a butyl group, an isopropyl group or a tributyl group; an alkenyl group such as a vinyl group, an allyl group or a butenyl group; An amine-substituted alkyl group, a mercapto-substituted alkyl group, or the like, a substituted or unsubstituted one-valent hydrocarbon group having 1 to 1 carbon atom, preferably a hydrogen atom. When the dicyclopentadiene type epoxy resin is used, the amount thereof is preferably 20% by mass or more, more preferably 30% by mass or more based on the total amount of the epoxy resin. The naphthalene type epoxy resin is exemplified by an epoxy resin represented by the following formula (X). -21 - (X) 201144376 [Chem. 13] r CH2-CHJ0H2 (R^j ^R2)k CH2.qi>CH2 0) a

CH〇- (R3)i CHj-CH^CHj O , _ ; R')j (R2)k ^X (R3)i (1-P) (wherein R1 to R3 are based on carbon numbers l~12 Substituted or unsubstituted - valence hydrocarbon group selected 'these may all be the same or different' P is 1 or 〇' m, η is an integer of 0 to 11, respectively, and (m + n) is an integer of 1 to 11 And (m + p) is an integer of 1 to 12, i represents an integer of 〇 3, j represents an integer of 0 to 2, and k represents an integer of 0 to 4). The naphthalene type epoxy resin represented by the above formula (X) is exemplified by a random copolymer containing a plurality of constituent units and η constituent units, and an alternating copolymer which is contained in an alternating manner, a copolymer containing a regularity, and a block. The block copolymer is contained. Any of these may be used alone or in combination of two or more. These epoxy resins are commercially available from Nippon Kayaku Co., Ltd. under the trade name of NC-7300. When these naphthalene type epoxy resins are used, in order to exhibit the performance, the blending amount is preferably 20% by mass or more, more preferably 30% by mass or more, and more preferably 50% by mass or more in the total amount of the epoxy resin. . The epoxide of the phenolic aralkyl resin is exemplified by an epoxy resin represented by the following formula (XI) or (XII). -22- (XI)201144376 [Chemistry 14] ch2-ch--ch CH,-CH-CH, 0 _ '〇 " R!R2R5 R6 (R9)i R3 R4 R7 R8 CH,—CH two CH,

9 r'r2r5 r6 ? ^CH2M^CH2^〇(R' R3 M R7 R* n ;R9). (wherein R1 to R9 are a hydrogen atom, one substituted or unsubstituted by a carbon number of 1 to 12; The valence hydrocarbon group is selected, and all may be the same or different, i represents 〇 or an integer of 1 to 3, and η represents 0 or an integer of 1 to 10). [化15]

Ir05 (Rs)i ch2-ch-ch2 〇(XII) (wherein R1 to R4 are a hydrogen atom 'selected by a substituted or unsubstituted one of the carbon number 1 to 12', all may be the same or different R5 is selected from a substituted or unsubstituted one-valent hydrocarbon group having 1 to 12 carbon atoms, and i represents 〇 or an integer of 1 to 3' η represents an integer of 〇 or 1 to 1 以 in the above formula (XI) The epoxide of the phenolic aralkyl resin having a biphenyl skeleton can be obtained by a known method by using epichlorohydrin with a phenol and a bisphenol substituted by an alkyl group, an aromatic ring or an unsubstituted group. The phenolic arylalkyl resin synthesized by oxymethyl)biphenyl is obtained by reacting. R|~R9 in the formula (ΧΙ) is exemplified by, for example, methyl, ethyl 'propyl 'isopropyl, n-butyl' Chain -23- 201144376 alkyl, cyclopentyl, cyclohexyl, cyclobutyl, cyclopentenyl, etc. An alkyl group substituted with a cyclic alkyl group such as a cyclohexenyl group, a benzyl group such as a phenethyl group, an alkyl group substituted with a methoxy group, an alkyl group substituted with an ethoxy group, or an alkyl group substituted with a butoxy group. Oxyl group An alkyl group substituted with an amino group such as an alkyl group, an aminoalkyl group, a dimethylaminoalkyl group or a diethylaminoalkyl group, an alkyl group substituted with a hydroxy group, a phenyl group, a naphthyl group, a biphenyl group or the like, which is unsubstituted. An alkyl group-substituted aryl group such as aryl, tolyl, dimethylphenyl, ethylphenyl, butylphenyl, tert-butylphenyl or dimethylnaphthyl, methoxyphenyl, ethoxy An alkoxy-substituted aryl group such as a phenyl group, a butoxyphenyl group, a second butoxyphenyl group or a methoxynaphthyl group, an aryl group substituted with an amine group such as a dimethylamino group or a diethylamino group, and a hydroxy group. The substituted aryl group or the like is preferably a hydrogen atom or a methyl group, and the η in the formula (XI) is preferably 6 or less on average, and the epoxy resins are commercially available from Nippon Kay Co., Ltd. The product name is NC-3000S. In terms of flame retardancy, reflow resistance, and fluidity, it is preferably used in combination with the epoxy resin represented by the above formula (V). R1 to R8 in the above formula (XI) are a hydrogen atom, and R1 to R8 in the above formula (V) are a hydrogen atom, and η = 0 ^ In addition, in particular, the blending quality is preferably (V) / (XI) = 50/50 5/95, more preferably 40/60 to 10/90, and even more preferably 30/70 to 15/85. Compounds satisfying these blending quality ratios are commercially available as CER-3000L (Nippon Chemical Co., Ltd.) The trade name of the product is commercially available. The epoxide of the aromatic resin based on the above formula (XII) is replaced by an epicyclic chlorohydrin with an alkyl group substituted by an aromatic ring by a conventional method. The substituted phenol and dimethoxy-p-xylene synthesized phenol. Aralkyl resin anti-24- 201144376 should be obtained. R1 R R5 in the formula (ΧΠ) is exemplified by, for example, methyl, ethyl, propyl. , isopropyl, n-butyl, t-butyl, tert-butyl, pentyl, hexyl, octyl, decyl, dodecyl and other chain alkyl groups, cyclopentyl, cyclohexyl, cycloheptyl a cyclic alkyl group such as a cyclopentenyl group or a cyclohexenyl group; an alkyl group substituted with an aryl group such as a benzyl group or a phenethyl group; a methoxy-substituted alkyl group, an ethoxy-substituted alkyl group, and a butoxy group. An alkyl group substituted with an alkoxy group such as an alkyl group, an alkyl group substituted with an amine group such as an aminoalkyl group, a dimethylaminoalkyl group or a diethylaminoalkyl group, a hydroxy-substituted alkyl group, a phenyl group, a naphthyl group, Biphenyl An unsubstituted aryl group, an alkyl group-substituted aryl group such as tolyl, dimethylphenyl, ethylphenyl, butylphenyl, tert-butylphenyl or dimethylnaphthyl, methoxy Alkoxy-substituted aryl group such as phenyl, ethoxyphenyl, butoxyphenyl, tert-butoxyphenyl 'methoxynaphthyl, etc., amine such as dimethylamino or diethylamino A group-substituted aryl group, a hydroxy-substituted aryl group or the like, wherein a hydrogen atom or a methyl group is preferred. Further, the average η in the general formula (XII) is preferably 6 or less. The epoxy resins are commercially available from Nippon Chemical Co., Ltd. under the trade name NC-2000L. The epoxide of the naphthol. aralkyl resin is exemplified by an epoxy resin represented by the following formula - (XIII). CHi-CH^CHz CH2-CH^.CH2 (^-CH2-X-CH2f-(^J-CH2-X-CH2 CHrCH-CH2 (XIII)

Ri (wherein R is selected by a substituted or unsubstituted one-valent hydrocarbon group having a carbon number of 1 to 12, all of which may be the same or different '' denotes an integer of 0 or 1 to 3, -25- 201144376 X represents a divalent organic group containing an aromatic ring, η represents an integer of 0 or 1 to 10) 〇X is exemplified by an alkyl group such as a stretching phenyl group, a stretching phenyl group, a stretching naphthyl group, or an alkyl group such as a tolyl group. An aryl group, an alkoxy-substituted aryl group, an aralkyl-substituted aryl group, a divalent group obtained from an aralkyl group such as a benzyl group or a phenethyl group, or a divalent group containing an exoaryl group such as a xylyl group. Among them, in view of both flame retardancy and storage stability, it is preferred to extend the phenyl group and extend the biphenyl group. The epoxide of a naphthol aralkyl resin represented by the above formula (XIII) can be obtained by a known method by using epichlorohydrin with naphthol substituted by an alkyl group, an aromatic ring or an unsubstituted group. Obtained by reacting a methoxy-p-xylene or a bis(methoxymethyl)biphenyl synthesized naphthol aralkyl resin. R in the formula (XIII) is exemplified by, for example, methyl, ethyl, propyl, isopropyl, n-butyl, t-butyl, t-butyl, pentyl, hexyl, octyl, decyl, ten a chain alkyl group such as a dialkyl group, a cyclic alkyl group such as a cyclopentyl group, a cyclohexyl group, a cyclobutyl group, a cyclopentenyl group or a cyclohexenyl group; an alkyl group substituted with an aryl group such as a benzyl group or a phenethyl group; An alkoxy-substituted alkyl group such as an oxy-substituted alkyl group, an ethoxy-substituted alkyl group or a butoxy-substituted alkyl group, an aminoalkyl group, a dimethylaminoalkyl group, a diethylaminoalkyl group, etc. An amino-substituted alkyl group, a hydroxy-substituted alkyl group, an unsubstituted aryl group such as a phenyl group, a naphthyl group or a biphenyl group, a tolyl group, a dimethylphenyl group, an ethylphenyl group, a butylphenyl group, An alkyl-substituted aryl group such as tributylphenyl or dimethylnaphthyl, methoxyphenyl, ethoxyphenyl, butoxyphenyl, tert-butoxyphenyl, methoxynaphthyl An alkoxy-substituted aryl group, an aryl group substituted with an amine group such as a dimethylamino group or a diethylamino group, an aryl group substituted with a hydroxy group, or the like, wherein a hydrogen atom or a methyl group is preferably used, for example, by the following formula (XIV) -26- 2011443 76 or (XV) indicates that the naphthoic acid • Fangyuan resin epoxide. η represents 〇 or an integer of 1 to 10, and the average is preferably 6 or less. The epoxy tree s which is represented by the following general formula (χιν) is exemplified by the epoxy resin represented by the following general formula (χν), which is commercially available from Nippon Steel Chemical Co., Ltd. under the trade name ESN-3 75 '. It is listed as a commercial item ESN-1 75 manufactured by Nippon Steel Chemical Co., Ltd. as a commercial item. The amount of the epoxide of the naphthol aralkyl resin is preferably 20% by mass or more, more preferably 30% by mass or more, and still more preferably 50% by mass in order to exhibit the performance. Above" [Chem. 17] iH2"C^/CH2 CH2-CH-CH2 CH2-〇-Cf

Ch2-ch-ch2 o , 〇 ch2—〇-ch2-V0(S (XIV) (where 'n represents an integer of 0 or 1 to 10) [Chem. 18]

CH,-C -CH-/CH2

CHz-CH^CHz CH2-CHHCH2 (XV) (where n represents 0 or an integer from 1 to 10). Further, an epoxy resin having the following structural formula (XVI) can also be used as the (A) epoxy resin. -27- (XVI) (XVI) 201144376 [Chem. 19]

Ch2-ch-ch, (R1 in the formula (XVI) is selected from a substituted or unsubstituted hydrocarbon group having a carbon number i to 12 and a substituted or unsubstituted alkoxy group having a carbon number of 1 to 12; All may be the same or different, η represents an integer of 0 to 4, and R 2 is a substituted or unsubstituted hydrocarbon group having 1 to 12 carbon atoms and a substituted or unsubstituted carbon number of 1 to 12 The oxy group selection 'all may be the same or different, and m represents an integer of 0 to 2). The epoxy resin represented by the above formula (XVI) is exemplified by an epoxy resin represented by the following formula (XVII) to (XXXV). -28 - 201144376 [Chem. 20]

ο 〇 ? ch2-ch-ch2 , 〇’ ch2-ch-ch2 h3c〇 9 rVS I

Ch7-ch-ch2 \ / A ch2-ch-ch2 CH3?

I :i :i 1; o ch2-ch-ch2 , 0 (XVn〇

HiCxx^o 0 1 ch2-ch-ch- (XIX) 2

(XXI) 0 1 ch2-ch-ch2 ο I ch2-ch-ch2

(XXIII) h3c〇 9 ch2-ch-ch2

Ch7-ch-ch2 _, 〇 / ch, -ch-ch2 —, d ch,9 (ΧΧϊν> h3co*

(XXV) ch2-ch-ch2, 〇’

Ch2-ch*ch2 1 V»/ O 0 , CH ch2*ch-ch2o OCH, οφσ'brain οφσ ο I ch2-ch-ch, ο I ch2-<ch;ch2 (XXVII)

(XXVIII) CH,, CH-.CH: -29 - 201144376 [Chem. 21] ch,-ch-ch2 I ' ch,? 0

(XXIX)

(XXX) ch2-ch-ch2

(XXXI)

(XXXII) CH, -ch-ch2

(ΧΧΧΙΠ) ch2-ch-ch, ch2-ch-ch2 h3c〇 o 0 ’ .och3

(XXXIV)

(XXXV) The epoxy resin represented by the above formula (XVI) is preferably an epoxy resin represented by the above formula (XVII) from the viewpoint of flame retardancy and formability. These compounds are commercially available as YX-8800 (trade name manufactured by Nippon Epoxy Resin Co., Ltd.). In order to exert the performance of the above-mentioned epoxy resin, the blending amount is preferably 30% by mass or more, more preferably 50% -30 to 201144376% or more, and more preferably 60% by mass based on the total amount of the epoxy resin. the following. The (Β) hardener used in the present invention is not particularly limited as long as it is a general oxygen resin molding material, and is exemplified by phenols such as metacresol, catechol, bisphenol A, bisphenol F, phenol, and aminophenol. And/or α-naphthol, β-naphthol quinones and formaldehyde, benzaldehyde, salicylaldehyde, etc., which have been condensed or co-condensed by an aldehyde-based catalyst, and/or naphthols and dimethoxy a para-xylene or bis(A; phenol/aralkyl resin, naphthol arylalkyl resin grease 'phenolic phenolic varnish structure and phenolic aralkyl structure cross-repeated phenolic aromatic a phenol resin modified with an alkylene resin, a phenol resin modified with melamine, a phenol resin modified with dicyclopentadiene, a phenol resin, a phenol resin modified with a polycyclic aromatic ring, etc. The above is used. Among them, the phenolic aralkyl resin and the naphthol aralkyl resin are preferred in terms of fluidity, flame retardancy and reflow resistance, and are preferably dicyclopentadiene type phenol resins. The novolac type phenol resin is preferably contained, and the phenolic aralkyl resin is exemplified by, for example, the following a resin used for encapsulating rings such as phenol, cresol, phenylphenol, thiodi, dihydroxynaphthalene, etc. in an acid phenol resin, from a phenolic high methyl group, a biphenyl aryl group, etc. The phenolic tree is preferably used in the form of random, block or p-xylene and/or phenol resin, decene-modified cyclopentadiene, or the like, and is preferably low in hygroscopicity. From the viewpoint, at least one formula (XXXVI) of the phenol resin means -31 - (XXXVI) 201144376 [Chem. 22]

(wherein R is selected from a hydrogen atom, a substituted carbon number of 1 to 12 or a monovalent hydrocarbon group, all of which may be the same or different, i represents an integer, X represents a divalent organic group containing an aromatic ring, and η represents 1〇 integer). The r in the above formula (xxxvi) is exemplified by a chain such as a methyl group, a benzyl group, an isopropyl group, a n-butyl group, a second butyl group, a tert-butyl group, a pentyl group, an octyl group, a decyl group or a dodecyl group. a cyclic alkyl group such as an alkyl group, a cyclopentyl group, a cyclobutyl group, a cyclopentenyl group or a cyclohexenyl group; an alkyl group substituted with an aryl group such as a benzyl group; a methoxy group substituted alkyl group, an ethoxy group, and a butyl group; An alkoxy-substituted alkyl group such as an oxy-substituted alkyl group, an alkyl group substituted with an amine group such as a dimethylaminoalkyl group or a diethylaminoalkyl group, an alkyl group substituted with an alkane, a phenyl group, a naphthyl group, or a biphenyl group. An unsubstituted aryl group such as phenyl, dimethylphenyl, ethylphenyl, butylphenyl, or dimethylphenylnaphthyl, methoxyphenyl, phenyl, butoxy a phenyl group, a tert-butoxyphenyl group, a methoxynaphthyl-substituted aryl group, an amino group substituted with an amino group such as a dimethylamino group or a diethylamino group, and the like, wherein a hydrogen atom or a methyl group is used. Preferably. Further, X represents a group containing an aromatic ring, and is exemplified by an alkyl group such as a stretched phenyl group, an extended naphthyl group, an alkyl group substituted with a tolyl group, an alkoxy substituted aryl group, a benzyl group, or a phenethyl group. Isoaryl-32-substituted 0 or 1~3 0 or 1~ethyl, propyl, hexylcyclohexyl, phenethyl substituted alkylaminoalkyl, hydroxyaryl, methyl butyl The alkoxyaryl group such as ethoxybenzene, the hydroxyphenyl group, and the extended aryl group are obtained as a divalent group having an extended aryl group such as a aryl group, a diphenyl group, or the like. Among them, a substituted or unsubstituted biphenyl group is preferred from the viewpoint of both flame retardancy and reflow resistance, and is exemplified by, for example, a phenolic aralkyl represented by the following formula (XXX VII). The base resin is preferably a substituted or unsubstituted phenylene group from the viewpoints of both flame retardancy, fluidity and hardenability, and is exemplified by a phenolic aralkyl group represented by the following formula (XXXVΙΠ). Resin. η represents an integer of 〇 or 丨 丨 , ^, preferably averaging below 6.

(where η represents 〇 or an integer from 1 to 1〇)

(where η represents 0 or an integer of 1 to 10). The phenolic aralkyl resin containing the extended biphenyl skeleton represented by the above formula (XXX VII) is exemplified by a commercial product manufactured by Minghe Chemical Co., Ltd. as a commercial product] ^£^1-7 8 5 1, The phenolic aralkyl resin represented by the formula (乂 乂乂 111) is exemplified by a commercially available product from the trade name XLC manufactured by Mitsui Chemicals, Inc. The blending amount of the above phenolic aralkyl resin is preferably 20% by mass or more, more preferably more, more preferably 50% by mass or more based on the total amount of the hardener. The naphthol aralkyl resin is exemplified by a resin represented by the following formula. [Chem. 25]

(wherein R is selected from a hydrogen atom, a substituted carbon number of 1 to 12 or a monovalent hydrocarbon group, all of which may be the same or different, i represents an integer of the month, X represents a divalent organic group containing an aromatic ring, and η : an integer of 10). R in the above formula (XXXIX) is exemplified by a chain alkyl group such as a methyl group, an isopropyl group, a n-butyl group, a second butyl group, a tert-butyl group, an octyl group, a decyl group or a dodecyl group. a cyclic alkyl group such as a cyclopentylcycloheptyl group, a cyclopentenyl group or a cyclohexenyl group; an alkyl group substituted with an aryl group such as benzyl; a methoxy-substituted alkyl group, an ethoxy group, a butoxy-substituted alkane An alkyl group substituted with an alkoxy group, an alkyl group substituted with an amine group such as a dimethylaminoalkyl group or a diethylaminoalkyl group, an unsubstituted group such as a phenyl group, a naphthyl group or a biphenyl group; An alkyl-substituted aryl group such as dimethylphenyl, ethylphenyl, butylphenyl or tert-dimethylnaphthyl, methoxyphenyl, butoxyphenyl, tert-butoxybenzene , methoxynaphthyl, 30% by mass (XXXIX), (XXXIX) unsubstituted e 0 or 1 to 3 and 0 or 1 to , ethyl, propylpentyl, hexyl, cyclohexyl, phenyl, phenyl The alkyl group-substituted alkylamino group, the group, the hydroxy group, the aryl group, the tolyl phenyl group, the ethoxyphenyl group, and the like are taken from the group - 34- 201144376 aryl group 'dimethylamino group, diethylamine Amino group substituted aryl group, hydroxyl group Instead aryl group, preferably wherein the hydrogen atom or a methyl group. And 'X represents a divalent organic group containing an aromatic ring, and is exemplified by an alkyl group-substituted aryl group such as a phenyl group, a phenylene group, a phenylene group, an alkyl group, or an alkoxy group. a divalent group obtained by an aryl group, an aralkyl group-substituted aryl group, an aralkyl group derived from a benzyl group or a phenethyl group, a divalent group containing an exoaryl group, and the like. Among them, from the viewpoint of storage stability and flame retardancy, a substituted or unsubstituted phenyl group and a phenyl group are preferred, and a phenyl group is more preferred, for example, by the following formula (XXXX) And (χχχχΐ) denote naphthol. Fangyuan resin. η represents an integer of 0 or 1 to 10, more preferably an average of 6 or less. OH OH ΟΗ (XXXX) (where η represents an integer of 0 or 1 to 10). [^ 27] (^-cu2-Q-ch2L^0-ch2-^)-cu2

(XXXXI)

PH (where η represents 0 or an integer of 1 to 10). The naphthol aralkyl resin represented by the above formula (ΧΧΧΧ) is exemplified by the trade name SN-47 5 manufactured by Nippon Steel Chemical Co., Ltd., commercially available as -35- 201144376, with the above formula (XXXXI). The naphthol/aralkyl resin represented by the product is commercially available as a commercial product SN-170 manufactured by Nippon Steel Chemical Co., Ltd. The blending amount of the naphthol/aralkyl resin is preferably 20% by mass or more, more preferably 30% by mass or more, and still more preferably 50% by mass or more based on the total amount of the curing agent. The naphthol aralkyl resin represented by the above formula (XXXVI) and the naphthol aralkyl resin represented by the formula (XXXIX) are preferably partially or wholly in view of flame retardancy. Pre-mixed with acenaphthylene. Dangerous can be obtained by dehydrogenation of hydrazine, but commercially available products can also be used. Further, a terpene polymer or a polymer of a terpene and another aromatic olefin may be used instead of terpene. A method of obtaining a polymer of a terpene or a polymer of a terpene and another aromatic olefin is exemplified by radical polymerization, cationic polymerization, anionic polymerization, and the like. Further, in the case of polymerization, a conventional catalyst can be used, but it is also possible to carry out heating only without using a catalyst. At this time, the polymerization temperature is preferably from 80 to 160 ° C, more preferably from 90 to 150 ° C. The polymer of the obtained terpene or the polymer of the terpene and the other aromatic olefin preferably has a softening point of 60 to 150 ° C, more preferably 70 to 1301. When the temperature is lower than 60 ° C, the moldability tends to decrease due to bleeding during molding. When the temperature is higher than 150 ° C, the compatibility with the resin tends to decrease. Other aromatic olefins copolymerized with terpenes are exemplified by styrene, ?-methylstyrene, anthracene, benzothiophene, benzofuran, vinylnaphthalene, ethylenebiphenyl or such alkyl substituents. Further, in addition to the above aromatic olefin, an aliphatic olefin may be used insofar as it does not impair the effects of the present invention. The aliphatic olefins are exemplified by (meth)acrylic acid and such esters, maleic anhydride, itaconic anhydride, fumaric acid-36-201144376, and the like. The amount of the aliphatic olefin to be used is preferably 20% by mass or less, more preferably 9% by mass or less based on the total amount of the polymerizable monomers. a method of premixing a part or all of the hardener with decene to directly mix the hardener and the decene in a finely pulverized solid state; and to dissolve the solvent after dissolving the solvent in the solvent; The method of melt-mixing and mixing the two at a temperature equal to or higher than the softening point of the curing agent and/or the terpene is preferable, but a melt mixing method in which a homogeneous mixture is obtained and impurities are less mixed is preferable. A premix (terpene modified hardener) was produced by the aforementioned method. The melt mixing is not limited as long as it is at least the softening point of the hardener and/or the terpene, but is preferably from 100 to 25 Torr, more preferably from 120 to 200 °C. Further, the mixing time is not limited as long as the melt mixing can be uniformly mixed, but it is preferably from 1 to 20 hours, more preferably from 2 to 15 hours. When premixing the hardener with the terpene, it is also possible to polymerize the terpene in the mixture or react with the hardener. The dicyclopentadiene type phenol resin is exemplified by a phenol resin represented by the following formula (χχχχπ).

(wherein R1 and R2 are independently selected from a hydrogen atom and a substituted or unsubstituted one-valent hydrocarbon group having 1 to 10 carbon atoms, η represents an integer of 〇10, and m represents an integer of 0 to 6). -37- 201144376 The above compound in which R1 and R2 are a hydrogen atom can be obtained from a commercially available product DPP (trade name manufactured by Shin-Nippon Petrochemical Co., Ltd.). The novolak-type phenol resin is exemplified by a novolac type phenol resin such as a phenol resin represented by the following formula (χχχχΐΠ), a cresol novolak resin, and the like. Among them, a novolac type phenol resin represented by the following formula (χχχχΐ II) is preferred. [化29]

(XXXXIII) (wherein R is selected from a hydrogen atom and a substituted or unsubstituted valent hydrocarbon group having 1 to 10 carbon atoms; 'i represents an integer of 0 to 3, and η represents an integer of 0 to 10) 〇 R in (ΧΧΧΧΙΠ) is exemplified by an alkyl group such as a hydrogen atom, a methyl group, an ethyl group, a propyl 'butyl group, an isopropyl group or a t-butyl group, or an alkenyl group such as a vinyl group, an allyl group or a butenyl group. a halogenated alkyl group, an amine-substituted alkyl group, a mercapto-substituted alkyl group, or the like, a substituted or unsubstituted one-valent hydrocarbon group having a carbon number of 1 to 10, wherein an alkyl group such as a methyl group or an ethyl group and a hydrogen atom are compared. Preferably, the average of the hydrogen atoms 'η is preferably from 0 to 8. The novolac type phenol resin represented by the above formula (XXXXIII) is commercially available from the product name: H-4 manufactured by Minghe Chemical Co., Ltd. When the novolac type phenol resin is used, the amount thereof is preferably from 30% by mass or more, more preferably from 50% by mass to 38% to 201144376, in terms of the total amount of the curing agent. The above-mentioned hardening agent may be used singly or in combination of two or more. The compounding amount in the case of using two or more kinds of the sizing agents is preferably 50% by mass or more, more preferably 60% by mass or more. It is better to be 80% by mass or more. In the present invention, the equivalent ratio of (A) epoxy resin to (B) hardener, that is, the ratio of the number of hydroxyl groups in the hardener to the epoxy group (the number of hydroxyl groups in the hardener / the number of epoxy groups in the epoxy resin) There is no particular limitation, but in order to suppress each unreacted component to a small amount, it is preferably set in the range of 0.5 to 2, more preferably in the range of 0.6 to 1.3. In order to obtain a molding epoxy resin molding material excellent in moldability and solder reflow resistance, it is preferably set in the range of 0.8 to 1.2. [(C) Hardening accelerator] The (C) hardening accelerator used in the present invention can be used. The epoxy resin molding material for encapsulation is generally not particularly limited as long as it is used by a user. Listed as, for example, 1,8-diazabicyclo[5.4.0]undecene-7, 1,5-diazabicyclo[4.3.0]nonene-5,5,6-dibutylamino group -1,8-diazabicyclo[5.4.0]undecene-7 and other Cycloami dine compounds and addition of maleic anhydride, 1,4-benzoquinone, 2,5 to these compounds -Toluene, 1,4-naphthoquinone, 2,3-dimethylphenylhydrazine, 2,6-dimethylphenylhydrazine, 2,3-dimethoxy-5-methyl-1,4-benzene An antimony compound such as hydrazine, 2,3-dimethoxy-I,4-benzoquinone or phenyl-1,4-benzoquinone, which has a compound having a π bond, such as a diazo phenyl group or a hydrazine resin. a compound of internal polarization, a tertiary amine such as benzyldimethylamine, triethanolamine, dimethylaminoethanol, ginseng (dimethylaminomethyl)phenol, and the like, 2-methylimidazole-39- 201144376, imidazoles such as 2-phenylimidazole, 2-phenyl-4-methylimidazole, 2-heptadecylimidazole, and the likes, 'tributylphosphine, methyldiphenylphosphine, triphenyl Organophosphines such as phosphine, ginseng (4-methylphenyl)phosphine, diphenylphosphine, phenylphosphine, and the like, and the addition of maleic anhydride, the above hydrazine compound, and diazophenyl to the phosphines a phosphorus compound having an intramolecular polarization, such as an alkane or a phenol resin, having a π bond, tetraphenylphosphinium tetraphenylborate, tetraphenyl iron ethyltriphenylborate, tetrabutyltetradecyltetrabutyl a tetraphenylborate such as a tetra-substituted scale such as a borate, a tetra-substituted borate, a 2-ethyl-4-methylimidazole tetraphenylborate, a fluorenyl-methylmorpholine or a tetraphenylborate These derivatives and the like may be used alone or in combination of two or more. Among them, from the viewpoint of hardenability and fluidity, an adduct of a tertiary phosphine and a ruthenium compound is preferred, and an adduct of triphenylphosphine and benzoquinone or tributylphosphine and benzoquinone is preferred. Additives. From the viewpoint of storage stability, it is preferably an adduct of a cyclic hydrazine compound and a phenol resin, more preferably a novolac type phenol resin salt of diazabicyclohexadecene. The blending amount of the hardening accelerator is preferably 60% by mass or more, more preferably 80% by mass or more based on the total amount of the hardening accelerator. The tertiary phosphine used in the adduct of the tertiary phosphine and the ruthenium compound is not particularly limited 'exemplified as, for example, tributylphosphine, dibutylphenylphosphine, butyldiphenylphosphine, ethyldiphenylphosphine, Triphenylphosphine, ginseng (4-methylphenyl)phosphine, ginseng (4-ethylphenyl)phosphine, ginseng (4-propylphenyl)phosphine, ginseng (4-butylphenyl)phosphine, ginseng Isopropylphenyl)phosphine, ginseng (t-butylphenyl)phosphine, ginseng (2,4-dimethylphenyl)phosphine, ginseng (2,6-dimethylphenyl)phosphine, ginseng (2 ,4,6-trimethylphenyl)phosphine, ginseng (2,6-dimethyl-4-cycloethoxyphenyl)phosphine, ginseng (4-methoxyphenyl)phosphine, ginseng-40- 201144376 A tertiary phosphine having an aryl group such as (4-ethoxyphenyl)phosphine is preferably triphenylphosphine or tributylphosphine in terms of moldability. Further, the ruthenium compound used for the adduct of the tertiary phosphine and the ruthenium compound is not particularly limited, and examples thereof include o-benzoquinone, p-benzoquinone, diphenylguanidine, 1,4-naphthoquinone, anthracene, etc. From the viewpoint of moisture resistance or storage stability, p-benzoquinone is preferred. The amount of the curing accelerator is not particularly limited as long as it can achieve the curing-promoting effect, but it is preferably 0.1 to 10 parts by mass based on 100 parts by mass of the total of the (A) epoxy resin and the (B) curing agent. It is preferably 0.3 to 5 parts by mass. When it is less than 1 part by mass, it is difficult to harden in a short time, and if it exceeds 10 parts by mass, the curing rate is too early and there is a tendency that a good molded article cannot be obtained. [(D) Inorganic Titanium Filler] The (D) inorganic chelating agent used in the present invention is formulated in a molding material for the purpose of reducing hygroscopicity, reducing linear expansion coefficient, improving thermal conductivity, and improving strength, and is only a package. The epoxy resin molding material is usually not particularly limited, and is exemplified by, for example, molten cerium oxide, crystalline cerium oxide, aluminum oxide, vermiculite, calcium silicate, calcium carbonate, potassium titanate, strontium carbide, and nitriding.矽, aluminum nitride, boron nitride, cerium oxide, chromium oxide, zircon 'Forsterite, talc (Steatite), spinel, mullite (Mullite), titanium oxide, etc., or These spheroidized beads, glass fibers, etc. may be used alone or in combination of two or more. Among them, from the viewpoint of reducing the coefficient of linear expansion, molten cerium oxide is preferred, and from the viewpoint of high thermal conductivity, alumina is preferred, and the shape of the sputum is in the form of -41 - 201144376. From the viewpoint of mold wearability, it is preferably spherical. It is preferable to be spherical molten cerium oxide from the viewpoint of balance cost and performance. The amount of the inorganic chelating agent is not particularly limited as long as it is within the scope of the invention, but it is preferably used for packaging from the viewpoints of flame retardancy, formability, hygroscopicity, reduction in coefficient of linear expansion, and strength. 70 to 95% by mass in the epoxy resin molding material, more preferably 85 to 95% by mass in terms of hygroscopicity and coefficient of linear expansion, and when it is less than 70% by mass, it is flame retardant and reflow resistant. When the tendency to decrease is more than 95% by mass, there is a tendency that the fluidity is insufficient. The molding material of the present invention preferably contains a fluorene oligomer, and the oxime oligomer is a hydrazine such as hydrazine or alkyl hydrazine, and a styrene such as styrene or alkyl styrene. And a phenolic copolymer resin. As for the production method, a Lewis acid, a Brensted acid, and a solid acid are used as a catalyst to obtain a cationic polymerization of the monomers. The proportion of the oxime is preferably 60% by mass or more based on the total amount of the copolymerized resin component, and may include an aromatic olefin such as coumarone as the other constituent monomers. The oxime oligomer is not particularly limited, and has a number average molecular weight of 300 to 1 000 and a softening point of 50 to 16 (the TC is the best. These specific examples are listed as the trade name I-1 manufactured by Dongdu Chemical Co., Ltd.). The amount of the oxime oligomer to be added is not particularly limited, but is preferably from 1 to 20 parts by mass based on 100 parts by mass of the epoxy resin of the component (A). [Expressed by the formula (IV) The decane compound (a) of the present invention is preferably a decane compound (a) represented by the following formula (IV) from the viewpoint of improving the reflow resistance. The compound represented by the formula (I) is not particularly limited, and may be used singly or in combination of two or more. (IV) R1-(CH2)q-Si-(〇R3)p (R2) 3-p (In the formula (IV), R1 represents a cycloalkyl group or a cycloalkenyl group having 5 to 8 carbon atoms, R2 is the same as R1 or a hydrocarbon group having 1 to 6 carbon atoms, and R3 represents a carbon number of 1 to 6 The hydrocarbon group, a part of a hydrogen atom represented by R1 to R3 may be substituted, p represents an integer of 1 to 3, and q represents an integer of 0 to 3.) R1 in the above formula (IV) is exemplified by, for example, a cyclopentyl group. Cyclohexyl, cycloheptyl, cyclooctyl, cyclohexenyl, cyclopentenyl, etc., preferably cyclopentyl and cyclohexyl. R2 is exemplified by methyl, ethyl, propyl, butyl, pentyl, Hexyl, isopropyl, isobutyl, tert-butyl, phenyl, cyclopentyl, cyclohexyl, cycloheptyl, cyclooctyl, cyclohexenyl, cyclopentenyl, etc., preferably methyl, Ethyl, cyclopentyl and cyclohexyl. R3 is exemplified by methyl, ethyl, propyl, butyl, pentyl, hexyl, isopropyl, isobutyl, tert-butyl, phenyl, cyclopentyl, The cyclohexyl group or the like is preferably a methyl group or an ethyl group. Further, the group may be substituted. Specific examples of the preferred structure of the decane compound represented by the above formula (IV) are exemplified by the following compounds. 43- 201144376 [Chem. 31] Q-Si(OCH3)3 (XXXXIV) 〇-Si(OCH3)3 (XXXXVI) 〇-Si(OCH,), (xxxxyjj!) CHj 〇-Si(OCH3)2 (XXXXX) Ch2ch3 ch3 〇-SiOCH3 (XXXXXII) CH3 Q-SKOCHOj (XXXXXIV) Q-(CH2)3-Si(OCHj)3 (XXXXXVI) 〇-(CH2)2-Si(OCH3)3 (XXXXXVin) Q-Si(OCH2CH3 )3 (XXXXV) 〇-Si(OCH,CH3)j (XXXXVII) 〇-Si(OCH2CH3)2 (χχχχιχ) CH, 〇- Si(OCH2CH3)2 (XXXXXJ) ch2ch3 ch3 〇-SiOCH2CH3 (XXXXXII I) ch3 Q-Si(OCH2CH3)3 (XXXXXV) J)-(CH2)3-Si(OCH2CH3)3 (XXXXXVII) 〇-(CH2)2 -Si(OCH2CH3)3 (XXXXXIX) 〇^〇CH3h (XXXXXX) [>^i(〇CH2CH3)2 (XXXXXXi) Among them, the balance between fluidity, formability and reflow resistance is excellent. It is preferably a compound represented by the above formula (xxxxvm) and (xxxxxx). Compounds represented by the formula (xxxxvm) are commercially available from commercial products.

Trade name manufactured by Toray Dow Corning Co., Ltd.: Z6187' The compound represented by the formula (xxxxxx) is commercially available from T〇ray.

Trade name manufactured by Dow Corning Co., Ltd.: Z6228. Further, a decane compound having a hydrolyzable group such as an alkoxyalkyl group or a phenoxyalkyl group is known to be hydrolyzed by moisture or the like in the air to form a decane-44- 201144376 alcohol group to produce a dehydration condensate of stanol groups. . The decane compound (a) represented by the above formula (IV) used in the present invention may further contain a stanol group and a dehydrated condensate obtained by hydrolyzing a decane compound. The total amount of the decane compound (a) represented by the above formula (IV) is not particularly limited as long as it is within the range of the effect of the invention, but from the viewpoints of fluidity, formability and reflow resistance, It is preferably 0.03 to 0.80% by mass in the epoxy resin molding material for encapsulation, more preferably 〇.〇4 to 0.75 mass%, and more preferably 0.05 to 0.7% by mass. When the amount is less than 3% by mass, the effect of the present invention tends to be small, and when it exceeds 0.8% by mass, the fluidity is improved, but the moldability and the reflow resistance tend to be greatly lowered. The molding material of the present invention preferably contains a decane compound (b) from the viewpoint of improving the adhesion between the resin component and the inorganic component in the molding material. The decane compound (b) is various decane-based compounds such as epoxy decane, decyl decane, amino decane, alkyl decane, ureido decane, and vinyl decane. Further, the decane compound (b) is excluded from the aforementioned decane compound ( a) Repeated decane-based compounds. When exemplified, vinyl trichloromethane, vinyl trimethoxy decane, vinyl triethoxy decane, vinyl ginseng (β-methoxyethoxy) decane, γ-methyl propylene oxime Propyltrimethoxydecane, γ-methylpropenyloxypropyltriethoxy oxime, γ-methylallyloxypropylmethyldimethoxydecane, γ-methylpropene oxime Oxypropylmethyldiethoxydecane, γ-methylpropenyloxypropyldimethylmethoxydecane, γ-methylpropenyloxypropyldimethylethoxydecane, γ- Propylene methoxypropyltrimethoxydecane, γ-propyleneoxypropyltriethoxydecane, β-(3,4-epoxycyclo-45- 201144376 hexyl)ethyltrimethoxydecane, γ - glycidoxypropyltrimethoxydecane, γ-glycidoxypropyltriethoxydecane, γ-glycidoxypropylmethyldimethoxydecane, γ-glycidoxypropyl Methyl diethoxy decane, γ-glycidoxypropyl dimethyl methoxy decane, γ-glycidoxy propyl dimethyl ethoxy decane, vinyl triethoxy methoxy Alkane, γ-mercaptopropyltrimethoxydecane, γ-mercaptopropyltriethoxydecane, bis(triethoxydecylpropyl)tetrasulfide, γ-aminopropyltrimethoxydecane , γ-aminopropyltriethoxydecane, γ-[bis(β-hydroxyethyl)]aminopropyltriethoxydecane, Ν-β-(aminoethyl)-γ-amino group Propyltriethoxydecane, fluorenyl-(trimethoxydecylpropyl)ethylenediamine, isocyanatepropyltrimethoxydecane,isoacylatepropyltriethoxydecane,methyltrimethoxy Decane, methyltriethoxydecane, dimethyldimethoxydecane, dimethyldiethoxydecane, phenyltrimethoxydecane, phenyltriethoxydecane, diphenyldimethoxy Decane, diphenyldiethoxydecane, diphenyldecanediol, triphenylmethoxydecane, triphenylethoxydecane, triphenylstanol, Ν-β-(Ν-vinylbenzyl Amino-ethyl)-γ-aminopropyltrimethoxydecane, γ-chloropropyltrimethoxydecane, hexamethyldioxane, γ-anilinopropyltrimethoxydecane, γ-anilinopropyl Triethoxy decane , 2·triethoxydecyl-indole-(1,3-dimethyl-butylene)propylamine, 3-triethoxydecyl-N-(l,3-dimethyl-butylene) Propylamine, Ν-(3-triethoxydecylpropyl)phenylimine, 3-(3-(triethoxydecyl)propylamino)-indole, fluorenyl-dimethyl Propylamine, N-triethoxydecylpropyl-β-alanine methyl ester, 3-(triethoxydecylpropyl)dihydro-3,5-furandione, bis(trimethoxy) a nonanezane compound such as a decyl benzene group, a hydrazine compound such as 1 Η-imidazole, 2-alkylimidazole, -46- 201144376 2,4-dialkylimidazole, 4-vinylimidazole, and γ-glycidoxypropyltrimethyl An imidazole-based decane compound of a reaction product of γ-glycidoxypropyl alkoxydecane such as oxydecane or γ-glycidoxypropyltriethoxydecane. When the decane compound (b) can be used alone or in combination of two or more kinds, the total amount of the compound is preferably 0.06 in the epoxy resin molding material for packaging, from the viewpoint of formability and adhesion. 2% by mass is more preferably 0.1 to 0.75 mass%, and more preferably 〇.2 to 0.7 mass%. When it is less than 0.06 mass%, the adhesion improving effect is hard to be exhibited, and when it exceeds 2 mass%, molding defects such as voids tend to occur. The epoxy resin molding material for encapsulation of the present invention improves the resin component and the inorganic material in the molding material. From the viewpoint of the adhesion of the components and the like, a conventional coupling agent other than the above-described decane compound (b) may be blended. Listed as, for example, isopropyl triisostearate titanate, isopropyl cis (dioctyl pyrophosphate) titanate, isopropyl tris(N-aminoethyl-aminoethyl) titanium Acid ester, tetraoctyl bis(di-tridecylphosphonate) titanate, tetrakis(2,2-diallyloxymethyl-1-butyl)bis(di-tridecyl) Phosphonate titanate, bis(dioctylpyrophosphate)oxyacetate titanate, bis(dioctyl pyrophosphate) extended ethyl titanate, isopropyl trioctylide titanate, Isopropyl dimethyl propylene isostearyl decyl titanate, isopropyl isostearyl decyl dipropylene titanate, isopropyl tris(dioctyl phosphate) titanate, isopropyl A titanate coupling agent such as tricumylphenyl titanate or tetraisopropylbis(dioctylphosphonate) titanate, an aluminum chelating agent, an aluminum/zirconium compound, or the like, which can be used alone. One type may be used in combination of two or more types. When the coupling agent is blended, the total amount of the coupling agent is preferably from 0.06 to 2% by mass, more preferably from 0.1% to 2% by mass, from the viewpoint of moldability and adhesion. 0.75 mass%, more preferably 0.2 to 0.7 mass%. When the amount is less than 5% by mass, the adhesion to various package members tends to decrease, and when it exceeds 2% by mass, molding defects such as voids tend to occur. Further, the epoxy resin molding material for encapsulation of the present invention may be formulated with an anion exchanger as needed to improve the moisture resistance and high-temperature placement characteristics of 1C. The anion exchanger is not particularly limited, and may be, for example, a hydrotalcite or an aqueous oxide of an element selected from magnesium, aluminum, titanium, pin, or ruthenium, etc., which may be used alone. It is also possible to combine two or more types. Among them, hydrotalcite represented by the following composition formula (XXXXXXIV) is preferred. xAIx (OH) a (C03) χ/2 *mHa〇 (XXXXXXIV) (in the formula (XXXXXXIV), 0 < Χ$〇·5, m is a positive number). The amount of the anion exchanger is not particularly limited as long as it can capture an anion such as a halogen ion, but is preferably 0.1 to 30 parts by mass, more preferably 1 to 1 part by mass based on the (A) epoxy resin. 5 parts by mass. The epoxy resin molding material for encapsulation of the present invention uses a further accelerator in order to further improve the adhesion. The promoters are listed as derivatives such as imidazole, triazole, tetrazole, triazine, ortho-aminobenzoic acid, gallic acid, malonic acid, malic acid, maleic acid, aminophenol, porphyrin, etc. Such derivatives as -48- 201144376, aliphatic acid amide compounds, dithiocarbamate, thio-n-spin derivatives, etc. may be used alone or in combination of two or more. A mold release agent may also be used as needed for the epoxy resin molding material for encapsulation. The release agent is preferably used in an amount of 0.01 to 10 parts by mass based on 1 part by mass of the (A) epoxy resin, and more preferably 0.1 to 5 parts by mass. If the amount is less than 1 part by mass, there is a tendency for the mold release property to be insufficient, and if it exceeds 10 parts, the adhesiveness tends to decrease. The oxidized or non-oxidized polyolefin is exemplified by the trade name H4 or PE, PED series manufactured by Hoechst Co., Ltd., and the like, and the low molecular weight polyethylene having an average molecular weight of about 5 Å to loooo. Further, the release agent other than the above is exemplified by carnauba wax, montanic acid vinegar, montanic acid, stearic acid, etc., and these may be used alone or in combination of two or more. When other mold release agents are used in addition to the oxidized or non-oxidized polyolefin, the total amount of the compounding agent is preferably 〇" to parts by mass, more preferably 0%, based on 1 part by mass of the (A) epoxy resin. 5 to 3 parts by mass. The epoxy resin molding material for encapsulation of the present invention may be formulated with a conventional flame retardant as needed to improve the flame retardancy of the molding material. Examples thereof include inorganic substances such as brominated epoxy resin, cerium oxide, red phosphorus, aluminum hydroxide, magnesium hydroxide, and zinc oxide, and/or phosphorus such as red phosphorus or ortho-acid ester coated with a thermosetting resin such as a bismuth resin. a compound, a melamine, a melamine derivative, a melamine-modified phenol resin, a compound having a triazine ring, a cyanuric acid derivative, an isocyanuric acid derivative, a nitrogen-containing compound, a phosphorus compound, and a nitrogen-containing compound. And aluminum hydroxide, magnesium hydroxide, and a composite metal hydroxide represented by the following composition formula -49-201144376 (XXXXXXV). p (M'.O,,) -q (M*c〇d) - Γ (Μ3.0|) -mHaO (XXXXXXV) (In the formula (XXXXXXV), M1, M2, and M3 are different from each other. The metal elements, a, b, c, d' e, f, ρ, q, and m represent a positive number, and r represents a zero or a positive number. In the above composition formula (XXXXXXV), Μ1, Μ2, and Μ3 are not particularly limited as long as they are mutually different metal elements, but in terms of flame retardancy, Μ1 is preferably a metal element of the third period, II 之Alkaline earth metal elements, metal elements belonging to group IVB, group IIB, group VIII, group IB, group IIIA and group IVA are selected, and M2 is preferably selected from transition metal elements of group IIIB to IIB, and Μ1 is more preferably made of magnesium, Calcium, aluminum, tin, titanium, iron, cobalt, nickel, copper and zinc are selected, and Μ2 is more preferably selected from iron, cobalt, nickel, copper and zinc. From the viewpoint of fluidity, Μ1 is preferably magnesium, and Μ2 is preferably zinc or nickel ’ r = 0. The molar ratio of p, q and r is not particularly limited, · When 0, p/q is preferably W99~1/1. Furthermore, the classification of metal elements is a periodic table with a typical element as the A subfamily and a transitional element of the B subfamily (Source: Kyoritsu Publishing Co., Ltd. issued "Chemical Dictionary 4" February 15, 1987 The condensed version of the 30th brush) is subject to approval. Further, examples thereof include compounds containing a metal element such as zinc oxide, zinc stannate, zinc borate, iron oxide, molybdenum oxide, zinc molybdate, and dicyclopentadienyl iron. These may be used alone or in combination of two or more. use. The blending amount of the flame retardant is not particularly limited, but -50 to 201144376 is preferably 1 to μ part by mass, more preferably 2 to 15 parts by mass, per 100 parts by mass of the (A) epoxy resin. Further, the epoxy resin molding material for encapsulation of the present invention may be a coloring agent such as carbon black, an organic dye, an organic pigment, titanium oxide, a tetraoxide, or a red iron oxide (Bengala). Further, as a further additive, a stress relieving agent such as an oxime oil or a ruthenium rubber powder may be blended as needed. The epoxy resin molding material for encapsulation of the present invention may be prepared by uniformly dispersing and mixing various components, and may be prepared by various methods. However, in general, a method in which a component of a specific blending amount is sufficiently mixed by a kneading machine or the like is used, and mixing is carried out. After melting and kneading, such as a roll or an extruder, it is cooled and pulverized. For example, a specific amount of the above components may be uniformly stirred and mixed, preheated to 70 to 14 ° C, and obtained by kneading, cooling, pulverization, or the like by a kneader, a roll, an extruder, or the like. It is easily granulated by the size and quality of the molding conditions. The electronic component device having the component encapsulated by the epoxy resin molding material obtained by the present invention is provided with a semiconductor die and a transistor on a support member such as a lead frame, a tape carrier, a wiring board, a glass, or a germanium wafer. An elemental device such as a passive element such as a thyristor (Thyristor), such as a passive element such as a capacitor, a resistor, or a coil, and an electronic component device in which a necessary portion is encapsulated by the epoxy resin molding material for packaging of the present invention. The electronic component device is exemplified by, for example, fixing a semiconductor element to a lead frame to connect a terminal portion and a lead portion of an element such as a wire or a jumper to the lead wire, and then using the epoxy resin molding material for encapsulation of the present invention by transferring Forming and other packages 'DIP (dual-wire package), PLCC (plastic wire die carrier), QFp (-51 - 201144376 quad flat package) 'SOP (small package), SOJ (small package J-lead package) , TSOP (thin small package), TQFP (thin quad flat package), etc. - the general resin package type 1C, which is packaged with the epoxy resin molding material of the present invention and is jumpered to the semiconductor die of the tape carrier. a TCP (tape-bearing package), a semiconductor die, a transistor, a diode, which is connected to a wiring board or a wiring formed on a glass by wire bonding, flip chip bonding, soldering, etc., by using the epoxy resin molding material for encapsulation of the present invention. COB (substrate flip-chip) module made up of active components such as body and thyristor, and/or passive components such as capacitors, resistors, and coils, mixed 1C, polycrystalline modules, and terminals for connecting wiring boards on the back side A BGA (Ball Grid Array) is mounted on the surface of the substrate, and the component is connected to the wiring formed on the organic substrate by jumper or wire bonding, and the component is packaged with the epoxy resin molding material of the present invention. ), c SP (grain size package), etc. Further, the epoxy resin encapsulating material of the present invention can be effectively used in the printed circuit board. The method of encapsulating an element using the epoxy resin molding material for encapsulation of the present invention is most commonly used in a low pressure transfer molding method, but an injection molding method, a compression molding method, or the like can also be used. EXAMPLES Hereinafter, the present invention will be described by way of Examples, but the scope of the present invention is not limited to the Examples "Preparation of the epoxy resin molding material for encapsulation of the present invention] (Examples 1 to 26, Comparative Example 1) ～13) -52- 201144376 The following components were prepared in the following parts 1 to 3, and the kneading was carried out under the conditions of a kneading temperature of 80 ° C and a kneading time of 10 minutes. Preparation Examples 1 to 26 and comparison Examples 1 to 13 are epoxy resin molding materials for encapsulation. The blank column in the table indicates that it is not deployed. (A) The following epoxy resins are used: o-cresol novolac type epoxy resin having an epoxy equivalent of 200 and a softening point of 67 t (epoxy resin 1 'sell name ESCN· 1 90 manufactured by Sumitomo Chemical Co., Ltd.), ring Ethylene equivalent of 196, biphenyl type epoxy resin (epoxy resin 2, trade name YX-4000H manufactured by Nippon Epoxy Resin Co., Ltd.), melting point 242' melting point of 118 ° C sulfur Diphenol-based epoxy resin (epoxy resin 3, trade name YS LV -120TE, manufactured by Nippon Steel Chemical Co., Ltd.), epoxy equivalent 24] softening point 96 °C containing phenyl group of the extended biphenyl skeleton Aralkyl type epoxy resin (epoxy resin 4, trade name CER-3000L, manufactured by Nippon Kayaku Co., Ltd.), epoxy equivalent 23S, softening point 52 ° C phenol. aralkyl resin epoxide ( Epoxy resin 5 'trade name NC-2000L manufactured by Nippon Kayaku Co., Ltd.), bisphenol A type brominated epoxy resin (epoxy resin with epoxy equivalent 375' softening point 80 °C, bromine content 48% by mass) 6). -53- 201144376 (B) The hardener is the following: a phenolic/aralkyl resin having a hydroxyl equivalent of 199 and a softening point of 8 9 ° C (hardener 1, trade name MEH-78 5 1 manufactured by Minghe Chemical Co., Ltd.) a phenolic aralkyl resin having a hydroxyl equivalent of 176 and a softening point of 70 ° C (hardener 2, trade name Mi rex XLC manufactured by Mitsui Chemicals, Inc.), a hydroxyl equivalent of 106, and a softening point of 64 ° C of novolak-type phenol Resin (hardener 3, 'trade name H-4' manufactured by Minghe Chemical Co., Ltd.). (C) A hardening accelerator is a betaine-type adduct of triphenylphosphine and p-benzoquinone (hardening accelerator 1), a betaine-type adduct of tributylphosphine and p-benzoquinone (hardening promotion) The agent 2), (D) inorganic chelating agent is a spherical molten cerium oxide having an average particle diameter of 17.5 μm and a specific surface area of 3.8 m 2 /g. The cerium-containing polymer of the component (E) is the following: Weight average molecular weight (Mw) 2150, (E) Proportion of substituted or unsubstituted phenyl groups (Ph-based ratio) of all R1 in the ruthenium-containing polymer 75 Ear %, Ph base ratio divided by Mw (Ph/Mw) is 0. 〇 349 containing cerium polymer (sand polymer 1, manufactured by Toray Dow Corning Co., Ltd. under the trade name 2 1 7FLAKE),

Mw3 700 - Ph ratio of 46 mol%, Ph/Mw 0.0124 containing sand polymer (sand polymer 2, trade name 23 3 FLAKE manufactured by Toray Dow Corning Co., Ltd.),

Mw5350, Ph base ratio of 67% by mole, Ph/Mw 0.0125 containing sand polymer (sand polymer 3, manufactured by Toray Dow Corning Co., Ltd. under the trade name 220FLAKE), -54- 201144376

Mw3500, Ph base ratio of 52% by mole, Ph/Mw 0.0149 containing bismuth polymer (containing bismuth polymer 4, trade name SH6018 manufactured by Toray Dow Corning Co., Ltd.). Further, the ruthenium containing polymers 1 and 3 have a structure represented by the general formula (I) and the general formula (Π), and the ruthenium containing polymers 2 and 4 have a structure represented by the general formula (I) to (ΠΙ). In addition to the component (E), that is, the cerium-containing polymer other than the preferred range for achieving the present invention, the following are used:

Mw 8 5 0 'Ph ratio of 15 mol%, Ph/Mw 0.0177 containing sand polymer (including polymer 5, manufactured by Toray Dow Corning Co., Ltd. under the trade name DC3 03 7),

Mwl350, the ratio of Ph base is 33%, and the composition of Ph/Mw 0.0244 is ruthenium polymer (containing ruthenium polymer 6, manufactured by Toray Dow Corning Co., Ltd. under the trade name DC3 074).

Mw7900, Ph base ratio of 34% by mole, Ph/Mw 0.0043 containing cerium polymer (containing cerium polymer 7, manufactured by Toray Dow Corning Co., Ltd. under the trade name 249FLAKE), viscosity at room temperature 4 〇〇 mPa. P-phenylmethyl fluorenone of S (containing bismuth polymer 8, trade name KF54 manufactured by Shin-Etsu Chemical Co., Ltd.), epoxy equivalent of 1660, softening point of 80 ° C polyoxane (containing ruthenium polymer 9, Toray Dow Corning Co., Ltd. trade name AY42-119). Further, the ruthenium-containing polymers 5 and 6 have a structure in which each of the structures represented by the general formulae (I) to (ΠΙ) has a structure in which a hydrogen atom bonded to an oxygen atom is substituted with a methyl group, and -55-201144376, The cerium-containing polymer 7 has all of the structures represented by the general formulae (I) to (III), and the cerium-containing polymer 8 has only the structure represented by the general formula (II), and the cerium-containing polymer 9 contains epoxy in the structure. base. The oxime oligomer is a trade name of 1-100 ° decane compound (a) manufactured by Tohto Kasei Co., Ltd., and bis-cyclopentyldimethoxy decane (trade name: Z6228, manufactured by Toray Dow Corning Co., Ltd.) is used. The decane compound (b) is γ-glycidoxypropyltrimethoxydecane (decane compound (b)-1), γ-anilinopropyltrimethoxydecane (decane compound (b)-2), γ. - Mercaptopropyltrimethoxydecane (decane compound (b)_3). Other additions were carried out using Brazilian palm lanthanum, osmium tetroxide, and carbon black β [Evaluation of a molded material for encapsulating epoxy resin] Next, the examples were evaluated by the following characteristic tests of (1) to (5)! ～26 and Comparative Examples 1 to 1 3 The characteristics of the epoxy resin molding material for packaging. The evaluation results are shown in Tables 1 to 3 below. Further, unless otherwise specified, the molding of the epoxy resin molding material for encapsulation is carried out by a transfer molding machine at a mold temperature of 180 ° C, a molding pressure of 6 · 9 Μ P a , and a curing time of 90 seconds. Further, the hardening was carried out at 1880 ° C for 5 hours as needed. (1) Spiral flow According to EMMI-1-66, a mold for spiral flow measurement was used, and an epoxy molding material for encapsulation was molded under the above conditions to obtain a flow distance (cm). -56- 201144376 (2) Thermal hardness The encapsulating epoxy resin molding material is formed into a German material with a diameter of 5 mm and a thickness of 3 mm, and a Sh〇re D type hardness tester is used immediately after forming. ) HD-1120 (D type) manufactured by Ueshima Manufacturing Co., Ltd.). (3) Flexural modulus at room temperature and flexural modulus at 260 °C The epoxy resin molding material for encapsulation was molded into 丨0 mm x 70 mm x 3 mm under the above conditions, and post-hardened to prepare a test piece, using Tensilon manufactured by A&D, according to JIS -K-6911, a 3-point support bending test was carried out in a constant temperature bath at room temperature and 260 °C, and the room temperature bending modulus (GPa) and the bending modulus (MPa) at 260 °C were obtained. (4) Reflow-resistance The epoxy resin molding material for encapsulation is used in an 80-pin flat package (QFP) with a size of 20 mm x 14 mm x 2 mm of 8 mm x 10 mm x 4 mm x 2 mm under the above conditions (wire frame material: copper Alloy, wafer solder joints and silver-plated handles on the front end of the wire are formed and post-hardened to 'wet at 85 ° C, 85% RH for 168 hours, at a specific temperature (2 3 5 ° C, Reflow soldering at 24 ° C, 25 5 ° C, 265 ° C) for 10 seconds to visually observe whether there is crack inside the package. Ultrasonic flaw detection device (HYE manufactured by Hitachi Construction Machinery Co., Ltd.) -FOCUS) It was observed whether or not peeling occurred inside the package, and the total number of packages of cracks and peeling was evaluated with respect to the number of test packages (10). -57- 201144376 (5) Flame-retardant molds of test pieces having a forming thickness of 1 /1 6 inches (about 1.6 mm) were molded under the above conditions to form epoxy resin molding materials for packaging and post-hardening according to UL-94 Test method for evaluation of flame retardancy ° [Table 1] Project implementation " 1 2 3 4 5 6 7 8 9 10 11 12 13 1 85 Epoxy resin for encapsulation 2 100 Epoxy resin T 100 ~ 100 100 100 100 100 100 100 100 100 100 6 15 1 82.2 Hardener 2 89.8 72.7 72.7 72.7 72.7 72.7 72.7 72.7 72.7 72.7 72.7 Grease 49.3 Toluene-containing polymer 1 10.0 10.0 10.0 10.0 2.5 5.0 10.0 20.0 30.0 40.0 10.0 10.0 10.0 Form decane compound (a) 5.0 With decane Compound (b) 1 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 Miscellaneous materials 2. 7.5 Hardening accelerator 1 2.8 3.8 3.0 30 3.0 3.0 3.0 3.0 3,0 3.0 3.0 2 4.5 3.0 8l>u Polymer 10.0 10.0 Three gasification 锑 6.0 into Brazil 蟋 蟋 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2. 0 2.0 2.0 2.0 2.0 Carbon black 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 Fused cerium oxide 1254 1615 1481 1512 1388 1406 1443 15^6 1589 1663 1443 1516 1553 The amount of cerium-containing polymer relative to epoxy resin ( Mass %) 10.0 10.0 10.0 10.0 2.5 5.0 10.0 20.0 30.0 40.0 10.0 10.0 10.0 Spiral flow 78 100 97 97 87 91 92 94 92 90 92 93 120 Thermal hardness 82 81 81 81 82 82 81 79 77 75 83 80 79 Room temperature bending Elasticity (GPa) 21.6 27.5 27.5 26.0 28.3 27.2 26.0 24.B 24.0 23.5 26.1 26.0 26.0 Juvenile TC bending elastic modulus (MPa 1 800 640 630 550 680 640 620 590 570 550 660 530 450 fixed resistance to dryness _ sex 235 » C 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 Item ____________________245°C 0/10 0/ 10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 ~o/To 0/10 0/10 One hundred 4/1D 1/10 0/ 10 0/10 1/10 0/10 0/10 0/10 0/10 ό/Ί"ο 0/10 265eC 5/10 4/10 3/10 3/10 9/10 4/10 3/10 2 /10 2/10 2/10 4/10 2/10 Τ/ίό Flame retardant total residual time (seconds 15 46 44 19 40 36 32 32 32 31 28 34 34 judge V-0 V-0 V -0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 -58- 201144376 [Table 2] Example " 14 15 16 17 18 19 20 21 22 23 24 25 26 2 too Epoxy 3 100 Seal 4 100 100 too 100 Pack 5 100 100 100 100 100 100 too Hardener J - 82.2 Epoxy 2 73.9 73.9 73.9 73.9 72.7 73.9 89.8 72.7 72.7 73.9 72.7 73.9 1 10.0 10.0 10.0 10.0 Bismuth polymer_2_ 10.0 10.0 B曰3 10.0 10,0 10.0 10.0 10.0 hk Form 4 10.0 \oxt J\y Materials decane compound fa, 5.0 Brothel compound (b) 1 7.5 7.5 7.5 7 -5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 Material 2 7.5 Hardening Accelerator 1 3.0 3.0 3.0 3.0 3.0 3.0 3.8 3.0 3,0 3.0 3.0 Tune 2 4.5 3.0 Pre-Polymer 10.0 10.0 Group Carnauba Wax 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 Carbon black 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1'5 1.5 1.5 1.5 1.5 1.5 Melt two gasification cut 1419 1419 1490 1526 1443 1419 1615 1481 1512 144 3 1419 1443 1419 Phase 5 矽; Discuss the amount of the thief contained in the epoxy resin. 10.0 10.0 10.0 10.0 10.0 10.0 10.0 10.0 10,0 10.0 \0JQ 10.0 10.0 93 93 95 120 86 87 94 91 91 86 B7 88 89 Thermal hardness 80 82 79 79 81 80 81 81 81 81 80 81 80 Room temperature bending rate (GPa) 24.5 24.5 ZA.S 24.5 25.8 24.2 27.5 27^ 26.0 25.8 24.0 26.0 24.5 Judging item hundred MVT, 蛮曲蹓# S(MPa 590 640 490 420 650 630 640 630 550 650 630 640 610 kneading resistance 2353⁄4 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 o/to o/ To 0/10 0/10 0/10 245°C 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 0 /10 255°C 0/10 0/10 0/10 0/10 0/10 1/10 1/10 0/10 0/10 0/10 0/10 0/10 0/10 265°C 4/10 4/10 3/10 2/10 5/10 5/10 5/10 4/10 4/10 4/10 5/10 3/10 4/10 Total residual fire time for flame retardant parts (& 35 31 37 37 41 42 48 48 22 39 39 39 41 萣V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 v-o" V-0 V-0 V- 0 -59- 201144376 [Table 3] Comparative Example Item 1 2 3 4 5 6 7 8 9 10 11 12 13 1 85 2 100 Epoxy Resin 3 100 4 100 100 100 100 100 100 100 100 100 seal 5 100 pack 6 15 with ring gas resin 1 82.2 hardener 2 89.8 72.7 72.7 73.9 72.7 72.7 72.7 72.7 72.7 72.7 72.7 3 49.3 5 10.0 into 6 10.0 Shape material containing bismuth polymer 7 10.0 8 10.0 9 10.0 decane compound (a) Adjust 1 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 7.5 Complex decane compound (b) 2 Composition 3 5.0 Hardening accelerator 1 2.8 3.8 3.0 3.0 3.0 3.0 3.0 3.0 3.0 3.0 3.0 2 4.5 3.0 茚 oligomer 10.0 three gasification 锑 6.0 Brazilian palm 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 2.0 Carbon black 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 1.5 Melt two gasification矽1184 1540 1406 1439 1369 1347 M43 1406 1443 1443 1443 1443 1443 The most bismuth-containing polymer relative to epoxy resin (0.0% 0.0 0.0 0.0 0.0 0.0 0.0 10.0 10.0 10.0 10.0 10.0 Spiral flow (cm) 73 95 92 92 87 88 88 83 92 92 80 78 90 Thermal hardness 82 81 81 B1 82 80 81 84 80 80 80 80 80 Room temperature flexural modulus (GPa) 24.0 30.6 30.6 28.9 28.9 27.2 28.9 28.9 28.3 28.3 25.5 28.2 27.5 Judgment of 2601 bending modulus (MPa) 880 700 690 600 690 660 620 730 600 620 710 630 690 Fixed reflow resistance 235eC 0/10 0/10 0/10 0/10 0/10 0 /10 0/10 0/10 0/10 0/10 0/10 0/10 0/10 Item 245°C 1/10 0/10 0/10 0/10 0/10 0/10 0/10 2/ 10 1/10 1/10 1/10 1/10 0/10 255°C 5/10 5/10 4/10 4/10 4/10 4/10 2/10 8/10 5/10 5/10 6/10 6/10 5/10 265ffC 10/10 10/10 10/10 I0/1C I0/1C 10/10 6/10 10/10 10/10 0/10 0/10 0/1C 10/10 Difficult Total flammability time (seconds) 15 48 48 22 40 41 41 41 67 60 46 70 33 Determination V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-0 V-1 V-1 V-0 V-1 V-0 From Tables 1 to 3, it is understood that Comparative Examples 1 to 13 in which the compound of the component (E) was not formulated were inferior in reflow resistance. Comparative Example 1 in which linear polyoxyalkylene was blended 2 Insufficient flame retardancy 'Comparative Example 1 in which a branched polyoxyalkylene group containing an epoxy group was blended 4 4 The bending elastic modulus was not sufficiently lowered. Comparative Examples 9 to 1 in which the weight average molecular weight of the compound of the component (E) was outside the range of the present invention were inferior in reflow resistance, and Comparative Examples 9 and 10 were inferior in difficulty and UL-94 V-0 could not be achieved. On the other hand, in the range of the present invention, the compound of the component (E) is prepared in a range of -60 to 201144376, which is different from the composition of the cerium-containing polymer other than the component (E) and the oxirane compound (b). The comparative examples of the same resin composition were better than those of Examples 1 to 26, and all of them were UL-94 V-0, and the flame retardancy was good, and the moldability was also good. Further, in Examples 1 2 and 16 of the ruthenium-containing oligomer, the examples 13 and 17 containing the decane compound (a) were particularly excellent in reflow resistance.

Claims (1)

201144376 VII. Patent application scope: 1 · A sealing epoxy resin molding material containing (A) epoxy resin, (B) hardener, (C) hardening accelerator, (D) inorganic filler, and E) a polymer containing ruthenium, (E) a ruthenium-containing polymer having any two or all of the structures represented by the following general formula (1), the following general formula (11), and the following general formula (ΠΙ) (E) The weight average molecular weight of the sand-containing polymer is 15 Å or more and 7 Å or less, [Chem. 1] R1 - Ο - Si - 〇 - (I) Ο (In the formula (I), R1 represents a substituted or unsubstituted hydrocarbon group having 1 to 6 carbon atoms, at least one of which is an oxygen atom constituting a siloxane chain, and an oxygen atom other than the oxygen atom is bonded to a hydrogen atom), [Chem. 2] R1 I —〇—Si—O— (II) R1 (wherein R1 represents a substituted or unsubstituted hydrocarbon group having 1 to 6 carbon atoms in the formula (II), wherein R1 may be the same or different, and at least an oxygen atom One is -62- 201144376 The oxygen atom constituting the siloxane chain and the oxygen atom other than the oxygen atom is bonded to the hydrogen atom, [Chemical 3] I 〇 - Ο - Si - O - (I II) Ο (In the formula (III), at least one of the oxygen atoms is an oxygen atom constituting a siloxane chain, and an oxygen atom other than the oxygen atom is bonded to a hydrogen atom). 2. $0 靑 靑 靑 靑 靑 靑 之 之 之 ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' ' % or more and 4% by mass or less. 3. The epoxy resin molding material for encapsulation of claim 2 or 2, wherein (E) of the epoxy resin molding material for encapsulation is substituted or unsubstituted in all R1 in the ruthenium-containing polymer The proportion of the phenyl group is 4 〇 mol% or more and 1 〇〇 mol. /. the following. 4. The epoxy resin molding material for encapsulation as described in claim i or 2, which further contains a fluorene oligomer. 5. The epoxy resin molding material for encapsulation of claim i or 2, which further contains a decane compound (a) represented by the following formula (IV), -63- (IV) 201144376 [Chemical 4] R1 -(CH2)q-Si-(OR3)p (R2)3-p (In the formula (IV), R1 represents a hydrocarbon group having the same carbon number of 5 to 8 or a hydrocarbon group having a carbon number of 1 to 6, R group, R1 to R3 represent a hydrogen atom of the group - an integer of 1 to 3, and q represents an integer of 0 to 3. 6. An electronic component device having an epoxy resin for encapsulation of any one of five items Alkyl or cycloalkenyl, R2 and 3 represent a hydrocarbon having a carbon number of 1 to 6 - a moiety may be substituted, P. An element encapsulated in a patented size 1st material. -64- 201144376 Four designated representative drawings: (1) The representative representative of the case is: No (2) The symbol of the representative figure is simple: No 201144376 If there is a chemical formula in the case, please disclose the chemical formula that best shows the characteristics of the invention: no