JP6801659B2 - Epoxy resin composition, film epoxy resin composition and electronic device - Google Patents
Epoxy resin composition, film epoxy resin composition and electronic device Download PDFInfo
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- JP6801659B2 JP6801659B2 JP2017533061A JP2017533061A JP6801659B2 JP 6801659 B2 JP6801659 B2 JP 6801659B2 JP 2017533061 A JP2017533061 A JP 2017533061A JP 2017533061 A JP2017533061 A JP 2017533061A JP 6801659 B2 JP6801659 B2 JP 6801659B2
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- Prior art keywords
- epoxy resin
- resin composition
- film
- hydroxyl group
- sealing
- Prior art date
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- 239000003822 epoxy resin Substances 0.000 title claims description 268
- 229920000647 polyepoxide Polymers 0.000 title claims description 268
- 239000000203 mixture Substances 0.000 title claims description 151
- 229920005989 resin Polymers 0.000 claims description 83
- 239000011347 resin Substances 0.000 claims description 83
- 238000007789 sealing Methods 0.000 claims description 51
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 50
- 239000000843 powder Substances 0.000 claims description 38
- 229920001296 polysiloxane Polymers 0.000 claims description 34
- 125000003118 aryl group Chemical group 0.000 claims description 30
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 claims description 28
- 239000011256 inorganic filler Substances 0.000 claims description 22
- 229910003475 inorganic filler Inorganic materials 0.000 claims description 22
- 150000001875 compounds Chemical class 0.000 claims description 20
- 239000007788 liquid Substances 0.000 claims description 18
- 239000002904 solvent Substances 0.000 claims description 14
- 125000001624 naphthyl group Chemical group 0.000 claims description 13
- PXKLMJQFEQBVLD-UHFFFAOYSA-N bisphenol F Chemical compound C1=CC(O)=CC=C1CC1=CC=C(O)C=C1 PXKLMJQFEQBVLD-UHFFFAOYSA-N 0.000 claims description 10
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 claims description 8
- 125000004432 carbon atom Chemical group C* 0.000 claims description 8
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 8
- 125000003545 alkoxy group Chemical group 0.000 claims description 4
- 125000000217 alkyl group Chemical group 0.000 claims description 4
- 239000000047 product Substances 0.000 description 40
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- 238000011156 evaluation Methods 0.000 description 15
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- 238000012360 testing method Methods 0.000 description 10
- 239000004593 Epoxy Substances 0.000 description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 9
- 230000000052 comparative effect Effects 0.000 description 9
- 125000003055 glycidyl group Chemical group C(C1CO1)* 0.000 description 9
- 239000011241 protective layer Substances 0.000 description 9
- 239000007787 solid Substances 0.000 description 9
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- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 8
- RZPFVRFSYMUDJO-UHFFFAOYSA-N 2h-naphthalen-1-one Chemical compound C1=CC=C2C(=O)CC=CC2=C1 RZPFVRFSYMUDJO-UHFFFAOYSA-N 0.000 description 7
- 238000004519 manufacturing process Methods 0.000 description 7
- ZUOUZKKEUPVFJK-UHFFFAOYSA-N phenylbenzene Natural products C1=CC=CC=C1C1=CC=CC=C1 ZUOUZKKEUPVFJK-UHFFFAOYSA-N 0.000 description 7
- 239000003566 sealing material Substances 0.000 description 7
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 6
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 6
- 229910000831 Steel Inorganic materials 0.000 description 6
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- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 description 3
- QTWJRLJHJPIABL-UHFFFAOYSA-N 2-methylphenol;3-methylphenol;4-methylphenol Chemical compound CC1=CC=C(O)C=C1.CC1=CC=CC(O)=C1.CC1=CC=CC=C1O QTWJRLJHJPIABL-UHFFFAOYSA-N 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
- 239000006087 Silane Coupling Agent Substances 0.000 description 3
- 150000001299 aldehydes Chemical class 0.000 description 3
- 238000013329 compounding Methods 0.000 description 3
- 238000000748 compression moulding Methods 0.000 description 3
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- 239000000377 silicon dioxide Substances 0.000 description 3
- HECLRDQVFMWTQS-RGOKHQFPSA-N 1755-01-7 Chemical compound C1[C@H]2[C@@H]3CC=C[C@@H]3[C@@H]1C=C2 HECLRDQVFMWTQS-RGOKHQFPSA-N 0.000 description 2
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 description 2
- MEVBAGCIOOTPLF-UHFFFAOYSA-N 2-[[5-(oxiran-2-ylmethoxy)naphthalen-2-yl]oxymethyl]oxirane Chemical compound C1OC1COC(C=C1C=CC=2)=CC=C1C=2OCC1CO1 MEVBAGCIOOTPLF-UHFFFAOYSA-N 0.000 description 2
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 2
- 239000004642 Polyimide Substances 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- NBBJYMSMWIIQGU-UHFFFAOYSA-N Propionic aldehyde Chemical compound CCC=O NBBJYMSMWIIQGU-UHFFFAOYSA-N 0.000 description 2
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 2
- SMEGJBVQLJJKKX-HOTMZDKISA-N [(2R,3S,4S,5R,6R)-5-acetyloxy-3,4,6-trihydroxyoxan-2-yl]methyl acetate Chemical compound CC(=O)OC[C@@H]1[C@H]([C@@H]([C@H]([C@@H](O1)O)OC(=O)C)O)O SMEGJBVQLJJKKX-HOTMZDKISA-N 0.000 description 2
- 229940081735 acetylcellulose Drugs 0.000 description 2
- 150000001298 alcohols Chemical class 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- 125000003710 aryl alkyl group Chemical group 0.000 description 2
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Chemical compound [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 description 2
- 238000005452 bending Methods 0.000 description 2
- HUMNYLRZRPPJDN-UHFFFAOYSA-N benzaldehyde Chemical compound O=CC1=CC=CC=C1 HUMNYLRZRPPJDN-UHFFFAOYSA-N 0.000 description 2
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- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 2
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- SGUVLZREKBPKCE-UHFFFAOYSA-N 1,5-diazabicyclo[4.3.0]-non-5-ene Chemical compound C1CCN=C2CCCN21 SGUVLZREKBPKCE-UHFFFAOYSA-N 0.000 description 1
- GQHTUMJGOHRCHB-UHFFFAOYSA-N 2,3,4,6,7,8,9,10-octahydropyrimido[1,2-a]azepine Chemical compound C1CCCCN2CCCN=C21 GQHTUMJGOHRCHB-UHFFFAOYSA-N 0.000 description 1
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- 231100000419 toxicity Toxicity 0.000 description 1
- UKRDPEFKFJNXQM-UHFFFAOYSA-N vinylsilane Chemical compound [SiH3]C=C UKRDPEFKFJNXQM-UHFFFAOYSA-N 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 125000002256 xylenyl group Chemical class C1(C(C=CC=C1)C)(C)* 0.000 description 1
- 125000006839 xylylene group Chemical group 0.000 description 1
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- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G59/00—Polycondensates containing more than one epoxy group per molecule; Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups
- C08G59/18—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing
- C08G59/40—Macromolecules obtained by polymerising compounds containing more than one epoxy group per molecule using curing agents or catalysts which react with the epoxy groups ; e.g. general methods of curing characterised by the curing agents used
- C08G59/62—Alcohols or phenols
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- C08L83/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
- C08L83/04—Polysiloxanes
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L23/00—Details of semiconductor or other solid state devices
- H01L23/28—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection
- H01L23/29—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the material, e.g. carbon
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L23/00—Details of semiconductor or other solid state devices
- H01L23/28—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection
- H01L23/31—Encapsulations, e.g. encapsulating layers, coatings, e.g. for protection characterised by the arrangement or shape
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- Epoxy Resins (AREA)
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Description
本発明は、エポキシ樹脂組成物、フィルム状エポキシ樹脂組成物及び電子装置に関する。本発明は、電子部品又は電子デバイス（例えば、プリント配線基板に配置された電子部品又は電子デバイス）の埋め込み又は封止等を可能とするエポキシ樹脂組成物及びフィルム状エポキシ樹脂組成物、並びに、これらを用いた電子装置に関する。 The present invention relates to epoxy resin compositions, film-like epoxy resin compositions and electronic devices. The present invention provides an epoxy resin composition and a film-like epoxy resin composition capable of embedding or sealing an electronic component or an electronic device (for example, an electronic component or an electronic device arranged on a printed wiring board), and these. The present invention relates to an electronic device using.
電子機器の軽薄短小化に伴って、半導体装置の小型化及び薄型化が進んでいる。半導体素子とほぼ同じ大きさの半導体装置を用いる形態、又は、半導体装置の上に半導体装置を積む実装形態（パッケージ・オン・パッケージ）が盛んに行われており、今後、半導体装置の小型化及び薄型化が一段と進むと予想される。 As electronic devices become lighter, thinner, shorter, and smaller, semiconductor devices are becoming smaller and thinner. A form in which a semiconductor device having almost the same size as a semiconductor element is used, or a mounting form in which the semiconductor device is stacked on the semiconductor device (package-on-package) is being actively carried out. It is expected that the thickness will be further reduced.
半導体素子の微細化が進展し、端子数が増加してくると、半導体素子上にすべての外部接続端子（外部接続用の端子）を設けることが難しくなる。例えば、無理に外部接続端子を半導体素子上に設けた場合、端子間のピッチが狭くなると共に端子高さが低くなり、半導体装置を実装した後の接続信頼性の確保が難しくなる。そこで、半導体装置の小型化及び薄型化を実現するために、新たな実装方法が多々提案されている。 As the miniaturization of semiconductor elements progresses and the number of terminals increases, it becomes difficult to provide all external connection terminals (terminals for external connection) on the semiconductor element. For example, when the external connection terminals are forcibly provided on the semiconductor element, the pitch between the terminals becomes narrow and the terminal height becomes low, which makes it difficult to secure the connection reliability after mounting the semiconductor device. Therefore, many new mounting methods have been proposed in order to realize miniaturization and thinning of semiconductor devices.
例えば、半導体ウエハから個片化されて作製された半導体素子を、適度な間隔を有するように再配置した後、半導体素子を液状又は固形の樹脂封止材を用いて封止し、半導体素子を封止した部分に外部接続端子を更に設ける実装方法、及び、当該実装方法を用いて作製される半導体装置が提案されている（例えば、下記特許文献１〜４参照）。 For example, a semiconductor element produced by being separated from a semiconductor wafer is rearranged so as to have an appropriate interval, and then the semiconductor element is sealed with a liquid or solid resin encapsulant to form the semiconductor element. A mounting method in which an external connection terminal is further provided in the sealed portion and a semiconductor device manufactured by using the mounting method have been proposed (see, for example, Patent Documents 1 to 4 below).
再配置した半導体素子の封止は、例えば、液状又は固形の樹脂封止材を金型で成形するモールド成形で行われる。封止成形をモールド成形で行う場合、ペレット状の樹脂封止材を溶融させて得られる樹脂を金型内に流し込むことで封止するトランスファーモールド成形が使用されることがある。しかしながら、溶融させて得られる樹脂を流し込んで成形するため、大面積を封止する場合、未充填部が発生する可能性がある。そこで近年、あらかじめ金型又は被封止体に樹脂封止材を供給してから成形を行うコンプレッションモールド成形が使用され始めている。コンプレッションモールド成形では、樹脂封止材を金型又は被封止体に直接供給するため、大面積の封止でも未充填部が発生しにくい利点がある。コンプレッションモールド成形では、トランスファーモールド成形と同様に、液状又は固形の樹脂封止材が用いられる。 The rearranged semiconductor element is sealed, for example, by molding a liquid or solid resin sealing material with a mold. When the sealing molding is performed by molding, transfer molding may be used in which the resin obtained by melting the pellet-shaped resin sealing material is poured into a mold to seal the resin. However, since the resin obtained by melting is poured into the molding, an unfilled portion may be generated when a large area is sealed. Therefore, in recent years, compression molding molding, in which a resin sealing material is supplied to a mold or an object to be sealed in advance and then molding is performed, has begun to be used. In compression molding, since the resin encapsulant is directly supplied to the mold or the object to be sealed, there is an advantage that unfilled portions are less likely to occur even when encapsulating a large area. In the compression molding, a liquid or solid resin encapsulant is used as in the transfer molding.
ところで、近年、液状又は固形の樹脂封止材に代えてフィルム状の樹脂封止材を用いることにより、金型を必要としない成形方法（ラミネート、プレス等）により封止を行うことが検討されている。この場合、フィルム状の樹脂封止材が破損して封止を行うことが困難となることを避ける観点から、樹脂封止材に対しては、優れた取扱性（屈曲性等）が求められている。 By the way, in recent years, it has been studied to use a film-shaped resin encapsulant instead of a liquid or solid resin encapsulant to perform encapsulation by a molding method (laminate, press, etc.) that does not require a mold. ing. In this case, the resin encapsulant is required to have excellent handleability (flexibility, etc.) from the viewpoint of avoiding damage to the film-shaped resin encapsulant and making it difficult to encapsulate. ing.
また、大面積を封止する場合、一度に封止できる面積が増えるために作業時間が短縮できるものの、封止成形物に反りが生じる場合がある。封止成形物の反りは、後続の工程において不具合を誘引する要因となることから、封止成形物の反りを低減することが求められている。 Further, when sealing a large area, the working time can be shortened because the area that can be sealed at one time increases, but the sealed molded product may be warped. Since the warp of the sealed molded product is a factor that induces defects in the subsequent process, it is required to reduce the warp of the sealed molded product.
本発明は、前記課題を鑑みてなされたものであり、優れた取扱性（屈曲性等）を有するフィルム状エポキシ樹脂組成物（フィルム状の樹脂封止材）が得られると共に、封止後の反りを抑制することが可能なエポキシ樹脂組成物を提供することを目的とする。また、本発明は、優れた取扱性を有すると共に、封止後の反りを抑制することが可能なフィルム状エポキシ樹脂組成物を提供することを目的とする。さらに、本発明は、これらのエポキシ樹脂組成物若しくはその硬化物、又は、フィルム状エポキシ樹脂組成物を用いた電子装置を提供することを目的とする。 The present invention has been made in view of the above problems, and a film-like epoxy resin composition (film-like resin encapsulant) having excellent handleability (flexibility, etc.) can be obtained, and after encapsulation, the present invention can be obtained. An object of the present invention is to provide an epoxy resin composition capable of suppressing warpage. Another object of the present invention is to provide a film-like epoxy resin composition which has excellent handleability and can suppress warpage after sealing. Furthermore, an object of the present invention is to provide an electronic device using these epoxy resin compositions or cured products thereof, or film-shaped epoxy resin compositions.
本発明は、（Ａ）エポキシ樹脂、（Ｂ）芳香環及び水酸基を有する樹脂、（Ｃ）シリコーンパウダー、（Ｄ）硬化促進剤、並びに、（Ｅ）無機充填剤を含有し、前記（Ａ）エポキシ樹脂が、２５℃で液状であるエポキシ樹脂を含み、前記（Ｂ）芳香環及び水酸基を有する樹脂が、ナフタレン環及び水酸基を有する樹脂を含み、前記２５℃で液状であるエポキシ樹脂の含有量が、前記（Ａ）エポキシ樹脂と前記（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として３２質量％以上であり、前記（Ｃ）シリコーンパウダーの含有量が、エポキシ樹脂組成物の全量（但し、エポキシ樹脂組成物が溶剤を含有する場合、溶剤を除く。以下同様。）を基準として０．８０〜７．３０質量％である、エポキシ樹脂組成物を提供する。 The present invention contains (A) an epoxy resin, (B) a resin having an aromatic ring and a hydroxyl group, (C) a silicone powder, (D) a curing accelerator, and (E) an inorganic filler. The epoxy resin contains an epoxy resin that is liquid at 25 ° C., and the resin having the aromatic ring and hydroxyl group (B) contains a resin having a naphthalene ring and a hydroxyl group, and the content of the epoxy resin that is liquid at 25 ° C. However, the content of the (C) silicone powder is 32% by mass or more based on the total amount of the (A) epoxy resin and the (B) resin having an aromatic ring and a hydroxyl group, and the content of the (C) silicone powder is the epoxy resin composition. Provided is an epoxy resin composition having an epoxy resin composition in an amount of 0.80 to 7.30% by mass based on the total amount (however, when the epoxy resin composition contains a solvent, the solvent is excluded. The same shall apply hereinafter).
本発明に係るエポキシ樹脂組成物によれば、当該エポキシ樹脂組成物をフィルム状に成形した場合において、優れた取扱性（屈曲性等）を有するフィルム状エポキシ樹脂組成物が得られる。また、本発明に係るエポキシ樹脂組成物によれば、封止後の反りを抑制することが可能であり、特に、大面積を封止する場合であっても封止後の反りを抑制することができる。さらに、本発明に係るエポキシ樹脂組成物は、優れた耐熱性及び難燃性を得ることもできる。 According to the epoxy resin composition according to the present invention, when the epoxy resin composition is molded into a film shape, a film-shaped epoxy resin composition having excellent handleability (flexibility, etc.) can be obtained. Further, according to the epoxy resin composition according to the present invention, it is possible to suppress the warp after sealing, and in particular, it is possible to suppress the warp after sealing even when sealing a large area. Can be done. Further, the epoxy resin composition according to the present invention can also obtain excellent heat resistance and flame retardancy.
前記ナフタレン環及び水酸基を有する樹脂は、下記一般式（Ｉ）で表される化合物を含んでもよい。
前記（Ｃ）シリコーンパウダーの含有量は、エポキシ樹脂組成物の全量を基準として２〜７質量％であってもよい。 The content of the silicone powder (C) may be 2 to 7% by mass based on the total amount of the epoxy resin composition.
前記（Ｃ）シリコーンパウダーは、シロキサン結合が三次元網目状に架橋した構造を有してもよい。 The silicone powder (C) may have a structure in which siloxane bonds are crosslinked in a three-dimensional network.
また、本発明は、前記エポキシ樹脂組成物又はその硬化物を含む、フィルム状エポキシ樹脂組成物を提供する。本発明に係るフィルム状エポキシ樹脂組成物は、優れた取扱性（屈曲性等）を有すると共に、封止後の反りを抑制することができ、且つ、優れた耐熱性及び難燃性を有している。 The present invention also provides a film-like epoxy resin composition containing the epoxy resin composition or a cured product thereof. The film-shaped epoxy resin composition according to the present invention has excellent handleability (flexibility, etc.), can suppress warpage after sealing, and has excellent heat resistance and flame retardancy. ing.
さらに、本発明は、電子部品及び電子デバイスからなる群より選ばれる少なくとも１種の被封止体と、前記被封止体を封止する封止部と、を備え、前記封止部が、前記エポキシ樹脂組成物若しくはその硬化物、又は、前記フィルム状エポキシ樹脂組成物を含む、電子装置を提供する。 Further, the present invention includes at least one type of sealed body selected from the group consisting of electronic components and electronic devices, and a sealing portion for sealing the sealed body, and the sealing portion comprises. An electronic device including the epoxy resin composition or a cured product thereof, or the film-shaped epoxy resin composition is provided.
本発明によれば、優れた取扱性（屈曲性等）を有するフィルム状エポキシ樹脂組成物が得られると共に、封止後の反りを抑制することができ、且つ、優れた耐熱性及び難燃性を有するエポキシ樹脂組成物を提供することができる。また、本発明によれば、優れた取扱性（屈曲性等）を有すると共に、封止後の反りを抑制することができ、且つ、優れた耐熱性及び難燃性を有するフィルム状エポキシ樹脂組成物を提供することができる。さらに、本発明によれば、これらのエポキシ樹脂組成物若しくはその硬化物又はフィルム状エポキシ樹脂組成物を用いた電子装置を提供することができる。 According to the present invention, a film-like epoxy resin composition having excellent handleability (flexibility, etc.) can be obtained, warpage after sealing can be suppressed, and excellent heat resistance and flame retardancy can be obtained. An epoxy resin composition having the above can be provided. Further, according to the present invention, a film-like epoxy resin composition having excellent handleability (flexibility, etc.), being able to suppress warpage after sealing, and having excellent heat resistance and flame retardancy. Can provide things. Further, according to the present invention, it is possible to provide an electronic device using these epoxy resin compositions or a cured product thereof or a film-shaped epoxy resin composition.
本発明に係るフィルム状エポキシ樹脂組成物は、電子部品又は電子デバイス（例えば、プリント配線基板に配置された電子部品又は電子デバイス）の埋め込み又は封止等に好適に用いることができる。また、本発明に係るフィルム状エポキシ樹脂組成物は、モールド成形に好適に用いることができることに加え、金型を必要としない成形方法（ラミネート、プレス等）にも好適に用いることができる。 The film-shaped epoxy resin composition according to the present invention can be suitably used for embedding or encapsulating an electronic component or an electronic device (for example, an electronic component or an electronic device arranged on a printed wiring board). Further, the film-shaped epoxy resin composition according to the present invention can be suitably used for molding, and can also be suitably used for a molding method (lamination, press, etc.) that does not require a mold.
本発明によれば、封止材としてのフィルム状エポキシ樹脂組成物の応用を提供することができる。本発明によれば、電子部品の埋め込み又は封止へのフィルム状エポキシ樹脂組成物の応用を提供することができる。本発明によれば、電子デバイスの埋め込み又は封止へのフィルム状エポキシ樹脂組成物の応用を提供することができる。本発明によれば、プリント配線基板に配置された電子部品又は電子デバイスの埋め込み又は封止へのフィルム状エポキシ樹脂組成物の応用を提供することができる。本発明によれば、モールド成形へのフィルム状エポキシ樹脂組成物の応用を提供することができる。本発明によれば、金型を必要としない成形方法（ラミネート、プレス等）へのフィルム状エポキシ樹脂組成物の応用を提供することができる。 According to the present invention, it is possible to provide an application of a film-like epoxy resin composition as a sealing material. According to the present invention, it is possible to provide an application of a film-like epoxy resin composition to embedding or encapsulating an electronic component. According to the present invention, it is possible to provide an application of a film-like epoxy resin composition to embedding or encapsulating an electronic device. According to the present invention, it is possible to provide an application of a film-like epoxy resin composition to embedding or encapsulating an electronic component or electronic device arranged on a printed wiring board. According to the present invention, it is possible to provide an application of a film-like epoxy resin composition to molding. According to the present invention, it is possible to provide an application of a film-like epoxy resin composition to a molding method (lamination, press, etc.) that does not require a mold.
以下、本発明を実施するための好適な形態について詳細に説明する。 Hereinafter, suitable embodiments for carrying out the present invention will be described in detail.
なお、本明細書において、「〜」を用いて示された数値範囲は、「〜」の前後に記載される数値をそれぞれ最小値及び最大値として含む範囲を示す。また、組成物中の各成分の量は、組成物中に各成分に該当する物質が複数存在する場合、特に断らない限り、組成物中に存在する当該複数の物質の合計量を意味する。さらに、本明細書において、エポキシ樹脂組成物の全量を基準とは、エポキシ樹脂組成物に含有される成分のうち、有機溶剤等の溶剤を除いた成分の総量（固形分の総量）を基準とすることを意味する。すなわち、エポキシ樹脂組成物が溶剤を含有する場合、溶剤を除いた成分の総量がエポキシ樹脂組成物の全量となる。 In the present specification, the numerical range indicated by using "~" indicates a range including the numerical values before and after "~" as the minimum value and the maximum value, respectively. In addition, the amount of each component in the composition means the total amount of the plurality of substances present in the composition when a plurality of substances corresponding to each component are present in the composition, unless otherwise specified. Further, in the present specification, the total amount of the epoxy resin composition is referred to as the total amount (total amount of solid content) of the components contained in the epoxy resin composition excluding the solvent such as an organic solvent. Means to do. That is, when the epoxy resin composition contains a solvent, the total amount of the components excluding the solvent is the total amount of the epoxy resin composition.
＜エポキシ樹脂組成物＞
本実施形態に係るエポキシ樹脂組成物は、（Ａ）エポキシ樹脂、（Ｂ）芳香環及び水酸基を有する樹脂、（Ｃ）シリコーンパウダー、（Ｄ）硬化促進剤、並びに、（Ｅ）無機充填剤を必須成分として含有している。本実施形態に係るエポキシ樹脂組成物において、前記（Ａ）エポキシ樹脂は、２５℃で液状であるエポキシ樹脂を含み、前記（Ｂ）芳香環及び水酸基を有する樹脂は、ナフタレン環及び水酸基を有する樹脂を含み、前記２５℃で液状であるエポキシ樹脂の含有量は、前記（Ａ）エポキシ樹脂と前記（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として３２質量％以上であり、前記（Ｃ）シリコーンパウダーの含有量は、エポキシ樹脂組成物の全量を基準として０．８０〜７．３０質量％である。但し、上記エポキシ樹脂組成物が溶剤を含有する場合、エポキシ樹脂組成物の全量は溶剤を除いた量を指す。<Epoxy resin composition>
The epoxy resin composition according to the present embodiment contains (A) an epoxy resin, (B) a resin having an aromatic ring and a hydroxyl group, (C) a silicone powder, (D) a curing accelerator, and (E) an inorganic filler. It is contained as an essential ingredient. In the epoxy resin composition according to the present embodiment, the (A) epoxy resin contains an epoxy resin that is liquid at 25 ° C., and the (B) resin having an aromatic ring and a hydroxyl group is a resin having a naphthalene ring and a hydroxyl group. The content of the epoxy resin which is liquid at 25 ° C. is 32% by mass or more based on the total amount of the (A) epoxy resin and the (B) resin having an aromatic ring and a hydroxyl group. The content of the silicone powder (C) is 0.80 to 7.30% by mass based on the total amount of the epoxy resin composition. However, when the epoxy resin composition contains a solvent, the total amount of the epoxy resin composition refers to the amount excluding the solvent.
本実施形態に係るエポキシ樹脂組成物の形状としては、フィルム状、液状、固形（顆粒、粉体等）などが挙げられる。本実施形態に係るエポキシ樹脂組成物は、モールド成形による封止、金型を必要としない成形方法（ラミネート、プレス等）による封止などに用いることができる。本実施形態に係るエポキシ樹脂組成物は、電子部品又は電子デバイスの埋め込み又は封止等に用いることができる。電子部品としては、例えば、ＳＡＷフィルタ等のフィルタ；センサ等の受動部品が挙げられる。電子デバイスとしては、例えば、半導体素子、集積回路、半導体デバイス等が挙げられる。なお、本実施形態に係るエポキシ樹脂組成物は、これら以外の被封止体の埋め込み又は封止に用いることもできる。「埋め込み」とは、隙間、段差等に封止材を供給することを意味する。「封止」とは、被封止体が外気に触れないように封止材で被封止体を被覆することを意味する。 Examples of the shape of the epoxy resin composition according to the present embodiment include film-like, liquid, solid (granule, powder, etc.) and the like. The epoxy resin composition according to the present embodiment can be used for sealing by molding, sealing by a molding method (lamination, press, etc.) that does not require a mold, and the like. The epoxy resin composition according to this embodiment can be used for embedding or sealing an electronic component or an electronic device. Examples of electronic components include filters such as SAW filters; passive components such as sensors. Examples of electronic devices include semiconductor elements, integrated circuits, semiconductor devices, and the like. The epoxy resin composition according to the present embodiment can also be used for embedding or sealing other objects to be sealed. "Embedding" means supplying a sealing material to a gap, a step, or the like. By "sealing" is meant covering the material to be sealed with a sealing material so that the material to be sealed is not exposed to the outside air.
以下、本実施形態に係るエポキシ樹脂組成物の各構成成分について説明する。 Hereinafter, each component of the epoxy resin composition according to the present embodiment will be described.
（（Ａ）エポキシ樹脂）
（Ａ）エポキシ樹脂は、フィルム状エポキシ樹脂組成物に柔軟性を付与するために、２５℃で液状であるエポキシ樹脂（以下、「エポキシ樹脂（ａ１）」という）を少なくとも１種含む。ここで、「２５℃で液状であるエポキシ樹脂」とは、２５℃に保持された当該エポキシ樹脂の粘度をＥ型粘度計又はＢ型粘度計を用いて測定した値が４００Ｐａ・ｓ以下であるエポキシ樹脂を示す。((A) Epoxy resin)
The epoxy resin (A) contains at least one type of epoxy resin (hereinafter, referred to as "epoxy resin (a1)") that is liquid at 25 ° C. in order to impart flexibility to the film-shaped epoxy resin composition. Here, the "epoxy resin liquid at 25 ° C." means that the value of the viscosity of the epoxy resin held at 25 ° C. measured with an E-type viscometer or a B-type viscometer is 400 Pa · s or less. Indicates an epoxy resin.
エポキシ樹脂（ａ１）としては、特に制限はなく、例えば、１分子中に２個以上のグリシジル基を有するエポキシ樹脂を用いることができる。エポキシ樹脂（ａ１）としては、ビスフェノールＡ型エポキシ樹脂、ビスフェノールＦ型エポキシ樹脂、ナフタレン型エポキシ樹脂等が挙げられる。エポキシ樹脂（ａ１）は、耐熱性付与の観点から、高いガラス転移温度（Ｔｇ）を得やすいナフタレン型エポキシ樹脂を含んでもよい。 The epoxy resin (a1) is not particularly limited, and for example, an epoxy resin having two or more glycidyl groups in one molecule can be used. Examples of the epoxy resin (a1) include bisphenol A type epoxy resin, bisphenol F type epoxy resin, naphthalene type epoxy resin and the like. The epoxy resin (a1) may contain a naphthalene-type epoxy resin that can easily obtain a high glass transition temperature (Tg) from the viewpoint of imparting heat resistance.
エポキシ樹脂（ａ１）としては市販品を用いてもよい。エポキシ樹脂（ａ１）の市販品としては、三菱化学株式会社製の商品名「ｊＥＲ８２５」（ビスフェノールＡ型エポキシ樹脂、エポキシ当量：１７５）、三菱化学株式会社製の商品名「ｊＥＲ８０６」（ビスフェノールＦ型エポキシ樹脂、エポキシ当量：１６０）、ＤＩＣ株式会社製の商品名「ＨＰ−４０３２Ｄ」（２官能ナフタレン型エポキシ樹脂）等が挙げられる。エポキシ樹脂（ａ１）は、１種を単独で用いてもよく、２種以上を併用してもよい。 A commercially available product may be used as the epoxy resin (a1). Commercially available epoxy resin (a1) includes the product name "jER825" (bisphenol A type epoxy resin, epoxy equivalent: 175) manufactured by Mitsubishi Chemical Corporation and the product name "jER806" (bisphenol F type) manufactured by Mitsubishi Chemical Corporation. Epoxy resin, epoxy equivalent: 160), trade name "HP-4032D" (bifunctional naphthalene type epoxy resin) manufactured by DIC Corporation, and the like can be mentioned. As the epoxy resin (a1), one type may be used alone, or two or more types may be used in combination.
エポキシ樹脂（ａ１）の含有量は、優れた取扱性（屈曲性等）を得る観点から、（Ａ）エポキシ樹脂と（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として３２質量％以上である。エポキシ樹脂（ａ１）の含有量は、更に優れた取扱性（屈曲性等）を得る観点から、３５質量％以上であってもよく、４０質量％以上であってもよく、４５質量％以上であってもよく、５０質量％以上であってもよい。エポキシ樹脂（ａ１）の含有量は、保護層を設けた封止シートとして用いる場合に保護層の剥離性が良好である観点から、７０質量％以下であってもよく、６５質量％以下であってもよい。エポキシ樹脂（ａ１）の含有量は、優れた取扱性（屈曲性等）を維持しつつ、保護層を設けた封止シートとして用いる場合に保護層の剥離性が良好である観点から、３２〜７０質量％であってもよく、３２〜６５質量％であってもよい。 The content of the epoxy resin (a1) is 32% by mass based on the total amount of (A) epoxy resin and (B) resin having an aromatic ring and a hydroxyl group from the viewpoint of obtaining excellent handleability (flexibility, etc.). That is all. The content of the epoxy resin (a1) may be 35% by mass or more, 40% by mass or more, or 45% by mass or more from the viewpoint of obtaining more excellent handleability (flexibility, etc.). It may be present, and may be 50% by mass or more. The content of the epoxy resin (a1) may be 70% by mass or less, and 65% by mass or less, from the viewpoint of good peelability of the protective layer when used as a sealing sheet provided with a protective layer. You may. The content of the epoxy resin (a1) is 32 to 32 from the viewpoint that the protective layer has good peelability when used as a sealing sheet provided with a protective layer while maintaining excellent handleability (flexibility, etc.). It may be 70% by mass, or 32 to 65% by mass.
エポキシ樹脂（ａ１）の含有量は、更に優れた取扱性（屈曲性等）を得る観点から、（Ａ）エポキシ樹脂の全量を基準として、６０質量％以上であってもよく、６５質量％以上であってもよく、７０質量％以上であってもよい。エポキシ樹脂（ａ１）の含有量は、更に優れた取扱性（屈曲性等）を得る観点から、（Ａ）エポキシ樹脂の全量を基準として、１００質量％以下であってもよく、９５質量％以下であってもよく、９０質量％以下であってもよい。 The content of the epoxy resin (a1) may be 60% by mass or more, or 65% by mass or more, based on the total amount of the epoxy resin (A) from the viewpoint of obtaining more excellent handleability (flexibility, etc.). It may be 70% by mass or more. The content of the epoxy resin (a1) may be 100% by mass or less, or 95% by mass or less, based on the total amount of the (A) epoxy resin, from the viewpoint of obtaining more excellent handleability (flexibility, etc.). It may be 90% by mass or less.
（Ａ）エポキシ樹脂は、２５℃で液状であるエポキシ樹脂（ａ１）以外のエポキシ樹脂（以下、「エポキシ樹脂（ａ２）」という。例えば、２５℃で液状ではないエポキシ樹脂）を更に含んでいてもよい。エポキシ樹脂（ａ２）としては、ナフタレン型エポキシ樹脂（４官能ナフタレン型エポキシ樹脂、３官能ナフタレン型エポキシ樹脂等）、アントラセン型エポキシ樹脂、トリスフェニルメタン型エポキシ樹脂、ジシクロペンタジエン型エポキシ樹脂、ビフェニルアラルキル型エポキシ樹脂、フェノールノボラック型エポキシ樹脂、クレゾールノボラック型エポキシ樹脂（ｏ−クレゾールノボラック型エポキシ樹脂等）、ジヒドロキシベンゼンノボラック型エポキシ樹脂、グリシジルエステル型エポキシ樹脂、グリシジルアミン型エポキシ樹脂、ヒダントイン型エポキシ樹脂、イソシアヌレート型エポキシ樹脂などが挙げられる。エポキシ樹脂（ａ２）としては、更に優れた耐熱性及び難燃性を得る観点から、ナフタレン型エポキシ樹脂であってもよい。エポキシ樹脂（ａ２）は、１種を単独で用いてもよく、２種以上を併用してもよい。 The epoxy resin (A) further contains an epoxy resin other than the epoxy resin (a1) that is liquid at 25 ° C. (hereinafter referred to as "epoxy resin (a2)", for example, an epoxy resin that is not liquid at 25 ° C.). May be good. Examples of the epoxy resin (a2) include naphthalene type epoxy resin (tetrafunctional naphthalene type epoxy resin, trifunctional naphthalene type epoxy resin, etc.), anthracene type epoxy resin, trisphenylmethane type epoxy resin, dicyclopentadiene type epoxy resin, and biphenyl aralkyl. Type epoxy resin, phenol novolac type epoxy resin, cresol novolac type epoxy resin (o-cresol novolac type epoxy resin, etc.), dihydroxybenzene novolac type epoxy resin, glycidyl ester type epoxy resin, glycidylamine type epoxy resin, hidden in type epoxy resin, Isocyanurate type epoxy resin and the like can be mentioned. The epoxy resin (a2) may be a naphthalene-type epoxy resin from the viewpoint of obtaining more excellent heat resistance and flame retardancy. As the epoxy resin (a2), one type may be used alone, or two or more types may be used in combination.
エポキシ樹脂（ａ２）としては市販品を用いてもよい。エポキシ樹脂（ａ２）の市販品としては、ＤＩＣ株式会社製の商品名「ＨＰ−４７００」（４官能ナフタレン型エポキシ樹脂）、商品名「ＨＰ−４７５０」（３官能ナフタレン型エポキシ樹脂）、商品名「ＨＰ−４７１０」（４官能ナフタレン型エポキシ樹脂）、商品名「エピクロンＮ−７７０」（フェノールノボラック型エポキシ樹脂）、商品名「エピクロンＮ−６６０」（クレゾールノボラック型エポキシ樹脂）及び商品名「エピクロンＨＰ−７２００Ｈ」（ジシクロペンタジエン型エポキシ樹脂）、日本化薬株式会社製の商品名「ＥＰＰＮ−５０２Ｈ」（トリスフェニルメタン型エポキシ樹脂）及び商品名「ＮＣ−３０００」（ビフェニルアラルキル型エポキシ樹脂）、新日鉄住金化学株式会社製の商品名「ＥＳＮ−３５５」（ナフタレン型エポキシ樹脂）、三菱化学株式会社製の商品名「ＹＸ−８８００」（アントラセン型エポキシ樹脂）、住友化学株式会社製の商品名「ＥＳＣＮ−１９０−２」（ｏ−クレゾールノボラック型エポキシ樹脂）等が挙げられる。 A commercially available product may be used as the epoxy resin (a2). As commercial products of the epoxy resin (a2), the trade name "HP-4700" (tetrafunctional naphthalene type epoxy resin), the trade name "HP-4750" (trifunctional naphthalene type epoxy resin), and the trade name manufactured by DIC Co., Ltd. "HP-4710" (tetrafunctional naphthalene type epoxy resin), product name "Epicron N-770" (phenol novolac type epoxy resin), product name "Epicron N-660" (cresol novolac type epoxy resin) and product name "Epicron" HP-7200H "(dicyclopentadiene type epoxy resin), product name" EPPN-502H "(trisphenylmethane type epoxy resin) and product name" NC-3000 "(biphenyl aralkyl type epoxy resin) manufactured by Nippon Kayaku Co., Ltd. , Nippon Steel & Sumitomo Metal Chemical Co., Ltd. product name "ESN-355" (naphthalene type epoxy resin), Mitsubishi Chemical Co., Ltd. product name "YX-8800" (anthracene type epoxy resin), Sumitomo Chemical Co., Ltd. product name Examples thereof include "ESCN-190-2" (o-cresol novolac type epoxy resin).
（Ａ）エポキシ樹脂は、耐熱性、難燃性、及び、Ｂステージ（半硬化）のフィルム状エポキシ樹脂組成物の取扱性（屈曲性等）が更に向上する観点から、エポキシ樹脂（ａ２）の中でも、下記一般式（ＩＩＩ）で表されるエポキシ樹脂を含んでもよい。式（ＩＩＩ）において、ｎ３１＋ｎ３２＋ｎ３３＋ｎ３４は、更に優れた耐熱性を得る観点から、２以上であってもよく、３以上であってもよい。ｎ３１＋ｎ３２＋ｎ３３＋ｎ３４は、更に優れた取扱性（屈曲性等）を得る観点から、４以下であってもよく、３以下であってもよい。 The epoxy resin (A) is the epoxy resin (a2) from the viewpoint of heat resistance, flame retardancy, and the handleability (flexibility, etc.) of the B-stage (semi-cured) film-shaped epoxy resin composition. Among them, an epoxy resin represented by the following general formula (III) may be contained. In the formula (III), n31 + n32 + n33 + n34 may be 2 or more, or 3 or more, from the viewpoint of obtaining more excellent heat resistance. n31 + n32 + n33 + n34 may be 4 or less, or 3 or less, from the viewpoint of obtaining more excellent handleability (flexibility, etc.).
式（ＩＩＩ）で表されるエポキシ樹脂としては、下記式（ＩＶ）で表されるエポキシ樹脂、下記式（Ｖ）で表されるエポキシ樹脂等が挙げられる。式（ＩＩＩ）で表されるエポキシ樹脂としては、市販品を用いてもよい。式（ＩＶ）で表されるエポキシ樹脂の市販品としては、例えば、ＤＩＣ株式会社製の商品名「ＨＰ−４７５０」（エポキシ当量：１８２）が挙げられる。式（Ｖ）で表されるエポキシ樹脂の市販品としては、例えば、ＤＩＣ株式会社製の商品名「ＨＰ−４７００」（エポキシ当量：１６６）が挙げられる。 Examples of the epoxy resin represented by the formula (III) include an epoxy resin represented by the following formula (IV), an epoxy resin represented by the following formula (V), and the like. As the epoxy resin represented by the formula (III), a commercially available product may be used. Examples of commercially available products of the epoxy resin represented by the formula (IV) include the trade name “HP-4750” (epoxy equivalent: 182) manufactured by DIC Corporation. Examples of commercially available products of the epoxy resin represented by the formula (V) include the trade name “HP-4700” (epoxy equivalent: 166) manufactured by DIC Corporation.
エポキシ樹脂（ａ２）の含有量は、更に優れた耐熱性を得る観点から、（Ａ）エポキシ樹脂の全量を基準として、１０質量％以上であってもよく、１５質量％以上であってもよく、２０質量％以上であってもよい。エポキシ樹脂（ａ２）の含有量は、更に優れた取扱性（屈曲性等）を得る観点から、（Ａ）エポキシ樹脂の全量を基準として、４５質量％以下であってもよく、４２質量％以下であってもよく、４０質量％以下であってもよい。 The content of the epoxy resin (a2) may be 10% by mass or more, or 15% by mass or more, based on the total amount of the epoxy resin (A), from the viewpoint of obtaining more excellent heat resistance. , 20% by mass or more. The content of the epoxy resin (a2) may be 45% by mass or less, or 42% by mass or less, based on the total amount of the (A) epoxy resin, from the viewpoint of obtaining more excellent handleability (flexibility, etc.). It may be 40% by mass or less.
（（Ｂ）芳香環及び水酸基を有する樹脂）
（Ｂ）芳香環及び水酸基を有する樹脂は、ナフタレン環（ナフタレン骨格）及び水酸基を有する樹脂（以下、「樹脂（ｂ１）」という）を少なくとも１種含む。樹脂（ｂ１）を用いることにより、（Ａ）エポキシ樹脂と（Ｂ）芳香環及び水酸基を有する樹脂との反応によって生じる収縮（反応収縮）を小さくすることが可能であることから、封止後の反りを抑制できると推測される。また、燃焼時にナフタレン骨格が炭化層を形成することで、難燃性を付与することができる。（Ｂ）芳香環及び水酸基を有する樹脂における水酸基としては、例えば、フェノール性水酸基（芳香環に直接結合している水酸基）等が挙げられる。フェノール性水酸基としては、例えば、ナフタレン環に直接結合している水酸基、ベンゼン環に直接結合している水酸基等が挙げられる。((B) Resin having an aromatic ring and a hydroxyl group)
(B) The resin having an aromatic ring and a hydroxyl group contains at least one kind of a naphthalene ring (naphthalene skeleton) and a resin having a hydroxyl group (hereinafter referred to as “resin (b1)”). By using the resin (b1), it is possible to reduce the shrinkage (reaction shrinkage) caused by the reaction between the (A) epoxy resin and the (B) resin having an aromatic ring and a hydroxyl group. It is presumed that warpage can be suppressed. Further, the naphthalene skeleton forms a carbonized layer at the time of combustion, so that flame retardancy can be imparted. (B) Examples of the hydroxyl group in the resin having an aromatic ring and a hydroxyl group include a phenolic hydroxyl group (a hydroxyl group directly bonded to the aromatic ring). Examples of the phenolic hydroxyl group include a hydroxyl group directly bonded to the naphthalene ring, a hydroxyl group directly bonded to the benzene ring, and the like.
樹脂（ｂ１）は、封止後の反りを更に抑制する観点から、下記一般式（Ｉ）で表される化合物を含んでもよい。 The resin (b1) may contain a compound represented by the following general formula (I) from the viewpoint of further suppressing warpage after sealing.
更に優れた難燃性を得る観点から、Ｒ１１、Ｒ１２、Ｒ１３、Ｒ１４及びＲ１５の少なくとも一つが水素原子であってもよく、Ｒ１１、Ｒ１２、Ｒ１３、Ｒ１４及びＲ１５の全てが水素原子であってもよい。封止後の反りを更に抑制する観点から、ｍ１、ｍ２、ｍ３、ｍ４、ｍ５、ｍ６、ｍ７及びｍ８の少なくとも一つが１であってもよく、ｍ１、ｍ２、ｍ３、ｍ４、ｍ５、ｍ６、ｍ７及びｍ８の全てが１であってもよい。耐熱性に更に優れる観点から、ｍ１、ｍ２、ｍ３、ｍ４、ｍ５、ｍ６、ｍ７及びｍ８の少なくとも一つが２であってもよく、ｍ１、ｍ２、ｍ３、ｍ４、ｍ５、ｍ６、ｍ７及びｍ８の全てが２であってもよい。ｎ１は、成形性、流動性及び難燃性に更に優れる観点から、０〜１０の整数であってもよく、０〜６の整数であってもよい。From the viewpoint of obtaining more excellent flame retardancy, at least one of R 11 , R 12 , R 13 , R 14 and R 15 may be a hydrogen atom, and R 11 , R 12 , R 13 , R 14 and R may be obtained. All 15 may be hydrogen atoms. From the viewpoint of further suppressing warpage after sealing, at least one of m1, m2, m3, m4, m5, m6, m7 and m8 may be 1, and m1, m2, m3, m4, m5, m6, All of m7 and m8 may be 1. From the viewpoint of further excellent heat resistance, at least one of m1, m2, m3, m4, m5, m6, m7 and m8 may be 2, and of m1, m2, m3, m4, m5, m6, m7 and m8. All may be 2. n1 may be an integer of 0 to 10 or an integer of 0 to 6 from the viewpoint of further excellent moldability, fluidity and flame retardancy.
式（Ｉ）で表される化合物は、封止後の反りを更に抑制する観点、及び、更に優れた耐熱性を得る観点から、水酸基が１位及び６位に結合したナフタレン環を有していてもよい。水酸基がナフタレン環の１位及び６位に結合していることで、（Ａ）エポキシ樹脂と効率的に反応できる。式（Ｉ）で表される化合物は、封止後の反りを更に抑制する観点、及び、更に優れた耐熱性を得る観点から、下記一般式（ＩＩ）で表される化合物を含んでもよい。 The compound represented by the formula (I) has a naphthalene ring in which a hydroxyl group is bonded at the 1-position and a 6-position from the viewpoint of further suppressing warpage after sealing and obtaining more excellent heat resistance. You may. Since the hydroxyl group is bonded to the 1-position and the 6-position of the naphthalene ring, it can efficiently react with the epoxy resin (A). The compound represented by the formula (I) may contain a compound represented by the following general formula (II) from the viewpoint of further suppressing warpage after sealing and obtaining further excellent heat resistance.
また、更に優れた難燃性を得る観点から、Ｒ２１、Ｒ２２及びＲ２３の少なくとも一つが水素原子であってもよく、Ｒ２１、Ｒ２２及びＲ２３の全てが水素原子であってもよい。ｎ２は、成形性、流動性及び難燃性に更に優れる観点から、０〜１０の整数であってもよく、０〜６の整数であってもよい。Further, from the viewpoint of obtaining more excellent flame retardancy, at least one of R 21, R 22 and R 23 may be hydrogen atoms, also all of R 21, R 22 and R 23 is a hydrogen atom Good. n2 may be an integer of 0 to 10 or an integer of 0 to 6 from the viewpoint of further excellent moldability, fluidity and flame retardancy.
式（Ｉ）で表される化合物としては、市販品を用いてもよい。式（Ｉ）で表される化合物の市販品としては、新日鉄住金化学株式会社製の商品名「ＳＮ−１８０」、「ＳＮ−３９５」、「ＳＮ−４７５Ｎ」、「ＳＮ−４８５」等が挙げられる。式（Ｉ）で表される化合物は、１種を単独で用いてもよく、２種以上を併用してもよい。 As the compound represented by the formula (I), a commercially available product may be used. Examples of commercially available products of the compound represented by the formula (I) include trade names "SN-180", "SN-395", "SN-475N", "SN-485", etc. manufactured by Nippon Steel & Sumikin Chemical Co., Ltd. Be done. As the compound represented by the formula (I), one type may be used alone, or two or more types may be used in combination.
式（Ｉ）で表される化合物としては、吸水及び封止後の反りを更に抑制する観点から、下記一般式（ＶＩ）で表される構造を有する化合物（ｎ６は１以上の整数を示す。例えば、新日鉄住金化学株式会社製の商品名「ＳＮ−１８０」）、及び、下記一般式（ＶＩＩ）で表される構造を有する化合物（ｎ７は１以上の整数を示す。例えば、新日鉄住金化学株式会社製の商品名「ＳＮ−４７５Ｎ」）であってもよい。 As the compound represented by the formula (I), a compound having a structure represented by the following general formula (VI) (n6 represents an integer of 1 or more) from the viewpoint of further suppressing water absorption and warpage after sealing. For example, the product name "SN-180" manufactured by Nippon Steel & Sumikin Chemical Co., Ltd.) and a compound having a structure represented by the following general formula (VII) (n7 represents an integer of 1 or more. For example, Nippon Steel & Sumikin Chemical Co., Ltd. It may be a company-made product name "SN-475N").
（Ｂ）芳香環及び水酸基を有する樹脂は、樹脂（ｂ１）以外の樹脂として、ナフタレン環を有していない樹脂（以下、「樹脂（ｂ２）」という）を更に含んでいてもよい。樹脂（ｂ２）としては、封止用エポキシ樹脂組成物に一般に使用されている樹脂等が挙げられ、特に制限はない。 (B) The resin having an aromatic ring and a hydroxyl group may further contain a resin having no naphthalene ring (hereinafter referred to as "resin (b2)") as a resin other than the resin (b1). Examples of the resin (b2) include resins generally used in sealing epoxy resin compositions, and are not particularly limited.
樹脂（ｂ２）としては、ノボラック型フェノール樹脂（フェノール類とアルデヒド類とを酸性触媒下で縮合又は共縮合させて得られる樹脂等）；トリスフェニルメタン型フェノール樹脂；ポリパラビニルフェノール樹脂；フェノール・アラルキル樹脂（フェノール類及びジメトキシパラキシレンから合成される、キシリレン基を有するフェノール・アラルキル樹脂等）；ビフェニル骨格を有するフェノール樹脂（ビフェニルアラルキル型フェノール樹脂等）などが挙げられる。前記フェノール類としては、フェノール、クレゾール、キシレノール、レゾルシン、カテコール、ビスフェノールＡ、ビスフェノールＦ等が挙げられる。前記アルデヒド類としては、ホルムアルデヒド、アセトアルデヒド、プロピオンアルデヒド、ベンズアルデヒド、サリチルアルデヒド等が挙げられる。樹脂（ｂ２）は、更に優れた難燃性を得る観点から、ビフェニルアラルキル型フェノール樹脂であってもよく、更に優れた耐熱性を得る観点から、ノボラック型フェノール樹脂であってもよい。樹脂（ｂ２）は、１種を単独で用いてもよく、２種以上を併用してもよい。 The resin (b2) includes novolak-type phenolic resin (resin obtained by condensing or co-condensing phenols and aldehydes under an acidic catalyst, etc.); trisphenylmethane-type phenolic resin; polyparavinylphenolic resin; phenol. Examples thereof include aralkyl resins (phenols and aralkyl resins having a xylylene group synthesized from phenols and dimethoxyparaxylene); phenolic resins having a biphenyl skeleton (biphenyl aralkyl type phenol resins, etc.). Examples of the phenols include phenol, cresol, xylenol, resorcin, catechol, bisphenol A, bisphenol F and the like. Examples of the aldehydes include formaldehyde, acetaldehyde, propionaldehyde, benzaldehyde, salicylaldehyde and the like. The resin (b2) may be a biphenyl aralkyl type phenol resin from the viewpoint of obtaining more excellent flame retardancy, or may be a novolak type phenol resin from the viewpoint of obtaining further excellent heat resistance. As the resin (b2), one type may be used alone, or two or more types may be used in combination.
市販の樹脂（ｂ２）としては、旭有機材工業株式会社製の商品名「ＰＡＰＳ−ＰＮ２」（ノボラック型フェノール樹脂）、エア・ウォーター株式会社製の商品名「ＳＫレジンＨＥ２００Ｃ−７」（ビフェニルアラルキル型フェノール樹脂）及び商品名「ＨＥ９１０−１０」（トリスフェニルメタン型フェノール樹脂）、明和化成株式会社製の商品名「ＤＬ−９２」、「Ｈ−４」及び「ＨＦ−１Ｍ」、群栄化学工業株式会社製の商品名「ＬＶＲ−８２１０ＤＬ」、「ＥＬＰ」シリーズ及び「ＮＣ」シリーズ、日立化成株式会社製の商品名「ＨＰ−８５０Ｎ」（ノボラック型フェノール樹脂）等が挙げられる。 As commercially available resin (b2), the product name "PAPS-PN2" (novolac type phenol resin) manufactured by Asahi Organic Materials Industry Co., Ltd. and the product name "SK Resin HE200C-7" (biphenyl aralkyl) manufactured by Air Water Co., Ltd. Type phenol resin) and product name "HE910-10" (trisphenylmethane type phenol resin), product names "DL-92", "H-4" and "HF-1M" manufactured by Meiwa Kasei Co., Ltd., Gunei Kagaku Examples thereof include the trade name "LVR-8210DL", "ELP" series and "NC" series manufactured by Kogyo Co., Ltd., and the trade name "HP-850N" (novolak type phenol resin) manufactured by Hitachi Kasei Co., Ltd.
（Ａ）エポキシ樹脂のグリシジル基の当量（エポキシ当量）の、（Ｂ）芳香環及び水酸基を有する樹脂における前記グリシジル基と反応する官能基（例えばフェノール性水酸基）の当量（例えば水酸基当量）に対する比率（（Ａ）エポキシ樹脂のグリシジル基の当量／（Ｂ）芳香環及び水酸基を有する樹脂における前記グリシジル基と反応する官能基の当量）は、未反応の（Ｂ）芳香環及び水酸基を有する樹脂を少なく抑える観点から、０．７以上であってもよく、０．８以上であってもよく、０．９以上であってもよい。前記比率は、未反応の（Ａ）エポキシ樹脂を少なく抑える観点から、２．０以下であってもよく、１．８以下であってもよく、１．７以下であってもよい。前記比率は、未反応の（Ａ）エポキシ樹脂、並びに、未反応の（Ｂ）芳香環及び水酸基を有する樹脂を少なく抑える観点から、０．７〜２．０であってもよく、０．８〜１．８であってもよく、０．９〜１．７であってもよい。 Ratio of (A) glycidyl group equivalent (epoxy equivalent) of the epoxy resin to (B) equivalent of the functional group (for example, phenolic hydroxyl group) that reacts with the glycidyl group in the resin having an aromatic ring and a hydroxyl group (for example, hydroxyl group equivalent). ((A) Equivalent of glycidyl group of epoxy resin / (B) Equivalent of functional group reacting with glycidyl group in resin having aromatic ring and hydroxyl group) is the unreacted resin having (B) aromatic ring and hydroxyl group. From the viewpoint of keeping the amount low, it may be 0.7 or more, 0.8 or more, or 0.9 or more. The ratio may be 2.0 or less, 1.8 or less, or 1.7 or less from the viewpoint of suppressing the amount of the unreacted (A) epoxy resin. The ratio may be 0.7 to 2.0, and may be 0.8, from the viewpoint of suppressing the amount of the unreacted (A) epoxy resin and the unreacted (B) resin having an aromatic ring and a hydroxyl group. It may be ~ 1.8 or 0.9 to 1.7.
（Ａ）エポキシ樹脂のグリシジル基の当量（エポキシ当量）の、樹脂（ｂ２）における前記グリシジル基と反応する官能基（例えばフェノール性水酸基）の当量（例えば水酸基当量）に対する比率（（Ａ）エポキシ樹脂のグリシジル基の当量／樹脂（ｂ２）における前記グリシジル基と反応する官能基の当量）は、未反応の樹脂（ｂ２）を少なく抑える観点から、０．７以上であってもよく、０．８以上であってもよく、０．９以上であってもよい。前記比率は、未反応の（Ａ）エポキシ樹脂を少なく抑える観点から、２．０以下であってもよく、１．８以下であってもよく、１．７以下であってもよい。前記比率は、未反応の（Ａ）エポキシ樹脂及び未反応の樹脂（ｂ２）を少なく抑える観点から、０．７〜２．０であってもよく、０．８〜１．８であってもよく、０．９〜１．７であってもよい。 The ratio of the equivalent of the glycidyl group (epoxy equivalent) of the (A) epoxy resin to the equivalent (for example, hydroxyl group equivalent) of the functional group (for example, phenolic hydroxyl group) that reacts with the glycidyl group in the resin (b2) ((A) epoxy resin The equivalent of the glycidyl group / the equivalent of the functional group that reacts with the glycidyl group in the resin (b2)) may be 0.7 or more, and may be 0.8 or more, from the viewpoint of suppressing the unreacted resin (b2) to be small. It may be more than or equal to 0.9 or more. The ratio may be 2.0 or less, 1.8 or less, or 1.7 or less from the viewpoint of suppressing the amount of the unreacted (A) epoxy resin. The ratio may be 0.7 to 2.0 or 0.8 to 1.8 from the viewpoint of suppressing the unreacted (A) epoxy resin and the unreacted resin (b2) to a small extent. It may be 0.9 to 1.7.
（（Ｃ）シリコーンパウダー）
本実施形態に係るエポキシ樹脂組成物は、（Ｃ）シリコーンパウダーを含有することにより、封止後の反り（例えばパッケージの反り量）及びパッケージクラックを効果的に低減することができ、優れた耐熱性及び難燃性を得ることができる。((C) Silicone powder)
By containing (C) silicone powder, the epoxy resin composition according to the present embodiment can effectively reduce warpage after sealing (for example, the amount of warpage of the package) and package cracks, and has excellent heat resistance. Sexuality and flame retardancy can be obtained.
（Ｃ）シリコーンパウダーの粒子形状は、流動性に優れる観点から、球状（真球状又は略球状）であってもよい。（Ｃ）シリコーンパウダーとしては、例えば、粒子形状が球状のシリコーンゴムパウダーの表面をシリコーンレジンで被膜して粉末化したもの等を用いることができる。このような（Ｃ）シリコーンパウダーは、シリコーンレジンで被膜することで凝集しにくく、樹脂への分散、封止後の反りの抑制及び耐熱性に優れた特徴を有する。（Ｃ）シリコーンパウダーは、シロキサン結合が三次元網目状に架橋した構造を有することで、耐熱性及び難燃性に更に優れたエポキシ樹脂組成物を得ることができる。（Ｃ）シリコーンパウダーは、ジメチルポリシロキサンが架橋した構造を有してもよい。 The particle shape of the silicone powder (C) may be spherical (true spherical or substantially spherical) from the viewpoint of excellent fluidity. As the silicone powder (C), for example, a silicone rubber powder having a spherical particle shape coated on the surface with a silicone resin and powdered can be used. Such a silicone powder (C) is hard to aggregate by being coated with a silicone resin, and has excellent characteristics of dispersion in a resin, suppression of warpage after sealing, and heat resistance. The silicone powder (C) has a structure in which siloxane bonds are crosslinked in a three-dimensional network, so that an epoxy resin composition having further excellent heat resistance and flame retardancy can be obtained. The silicone powder (C) may have a structure in which dimethylpolysiloxane is crosslinked.
（Ｃ）シリコーンパウダーの市販品としては、信越化学工業株式会社製の商品名「ＫＭＰ５９７」、「ＫＭＰ５９０」、「ＫＭＰ６００」、「ＫＭＰ６０１」、「ＫＭＰ６０２」、「ＫＭＰ６０５」、「ＫＭＰ７０１」、「Ｘ−５２−７０４２」等が挙げられる。（Ｃ）シリコーンパウダーは、１種を単独で用いてもよく、２種以上を併用してもよい。 (C) Commercially available silicone powder products include the trade names "KMP597", "KMP590", "KMP600", "KMP601", "KMP602", "KMP605", "KMP701", and "X" manufactured by Shin-Etsu Chemical Co., Ltd. -52-7042 "and the like. (C) One type of silicone powder may be used alone, or two or more types may be used in combination.
（Ｃ）シリコーンパウダーの平均粒子径の下限値は、０．０５μｍ以上であってもよく、０．１μｍ以上であってもよく、２μｍ以上であってもよく、２．５μｍ以上であってもよく、３μｍ以上であってもよい。また、（Ｃ）シリコーンパウダーの平均粒子径の上限値は、５０μｍ以下であってもよく、４５μｍ以下であってもよく、３０μｍ以下であってもよく、２０以下μｍであってもよく、１０μｍ以下であってもよい。すなわち、（Ｃ）シリコーンパウダーの平均粒子径は、０．０５〜５０μｍであってもよく、０．１〜４５μｍであってもよく、２〜３０μｍであってもよく、２．５〜２０μｍであってもよく、３〜１０μｍであってもよい。（Ｃ）シリコーンパウダーの平均粒子径がこれらの範囲であることにより、溶融時の樹脂組成物の流動性が低下することを抑制することができる。（Ｃ）シリコーンパウダーの平均粒子径は、粒度分布測定装置により測定することができる。 (C) The lower limit of the average particle size of the silicone powder may be 0.05 μm or more, 0.1 μm or more, 2 μm or more, or 2.5 μm or more. It may be 3 μm or more. Further, the upper limit of the average particle size of the (C) silicone powder may be 50 μm or less, 45 μm or less, 30 μm or less, 20 or less μm, or 10 μm. It may be as follows. That is, the average particle size of the (C) silicone powder may be 0.05 to 50 μm, 0.1 to 45 μm, 2 to 30 μm, or 2.5 to 20 μm. It may be 3 to 10 μm. When the average particle size of the silicone powder (C) is in these ranges, it is possible to suppress a decrease in the fluidity of the resin composition at the time of melting. (C) The average particle size of the silicone powder can be measured by a particle size distribution measuring device.
（Ｃ）シリコーンパウダーの含有量は、エポキシ樹脂組成物の全量を基準として０．８０〜７．３０質量％である。（Ｃ）シリコーンパウダーの含有量がこのような範囲であることにより、フィルムの取扱性（屈曲性等）が良好であり、封止後の反りを効果的に低減し、且つ、燃焼時に優れた難燃性を発揮することができる。（Ｃ）シリコーンパウダーの含有量は、フィルムの取扱性（屈曲性等）が更に良好であり、封止後の反りを更に効果的に低減し、且つ、燃焼時に更に優れた難燃性を発揮する観点から、２〜７質量％であってもよく、３〜６質量％であってもよい。 The content of the silicone powder (C) is 0.80 to 7.30% by mass based on the total amount of the epoxy resin composition. (C) When the content of the silicone powder is in such a range, the handleability (flexibility, etc.) of the film is good, the warp after sealing is effectively reduced, and the film is excellent at the time of combustion. Can exhibit flame retardancy. The content of the silicone powder (C) is such that the handleability (flexibility, etc.) of the film is further improved, the warp after sealing is further effectively reduced, and the flame retardancy is further improved during combustion. From the viewpoint of the above, it may be 2 to 7% by mass or 3 to 6% by mass.
樹脂（ｂ１）と（Ｃ）シリコーンパウダーとの併用により、燃焼時には、優れた難燃性を更に効果的に発揮することができる。これは、燃焼時において、樹脂（ｂ１）の縮合芳香環であるナフタレン環によって生成される炭化層と、（Ｃ）シリコーンパウダーを含むシロキサンの複合体による無機系燃焼残渣との複合層により、優れた断熱効果及び酸素遮断効果を示すために高い難燃効果が発揮されると考えられる。 By using the resin (b1) and the silicone powder (C) in combination, excellent flame retardancy can be more effectively exhibited at the time of combustion. This is excellent due to the composite layer of the carbonized layer formed by the naphthalene ring, which is the condensed aromatic ring of the resin (b1), and the inorganic combustion residue of the composite of siloxane containing (C) silicone powder during combustion. It is considered that a high flame retardant effect is exhibited because it exhibits a heat insulating effect and an oxygen blocking effect.
また、近年、環境保護の観点からダイオキシンの問題に端を発し、デカブロムをはじめとしたハロゲン化樹脂についての規制の動きがあり、同様にアンチモン化合物（アンチモン含有化合物）も毒性面から規制の動きがあることから、樹脂封止材に対してノンハロゲン化（ノンブロム化等）及びノンアンチモン化の要求が出てきている。また、プラスチック封止ＩＣの高温放置特性にブロム化合物（ブロム含有化合物）が悪影響を及ぼすことが知られており、ブロム化合物の低減が望まれている。本実施形態に係るエポキシ樹脂組成物は、難燃性に優れることから、ノンハロゲン化及びノンアンチモン化の要求を満たす封止材に適用できる。そのため、本実施形態に係るエポキシ樹脂組成物は、ノンハロゲン化及びノンアンチモン化の難燃性封止材への応用を提供することができる。 In recent years, there has been a movement to regulate halogenated resins such as decabrom, which originated from the problem of dioxins from the viewpoint of environmental protection, and similarly, antimony compounds (antimony-containing compounds) have also been regulated from the viewpoint of toxicity. For this reason, there are demands for non-halogenation (non-bromination, etc.) and non-antimonyization of resin encapsulants. Further, it is known that a brom compound (brom-containing compound) has an adverse effect on the high-temperature standing characteristics of a plastic-sealed IC, and reduction of the brom compound is desired. Since the epoxy resin composition according to the present embodiment is excellent in flame retardancy, it can be applied to a sealing material that satisfies the requirements for non-halogenation and non-antimonyization. Therefore, the epoxy resin composition according to the present embodiment can provide a non-halogenated and non-antimonized flame-retardant encapsulant application.
（（Ｄ）硬化促進剤）
（Ｄ）硬化促進剤としては、特に制限されるものではないが、例えば、アミン系の硬化促進剤、イミダゾール系の硬化促進剤、尿素系の硬化促進剤及びリン系の硬化促進剤からなる群より選ばれる少なくとも１種であってもよい。アミン系の硬化促進剤としては、１，８−ジアザビシクロ［５．４．０］−７−ウンデセン、１，５−ジアザビシクロ［４．３．０］−５−ノネン等が挙げられる。イミダゾール系の硬化促進剤としては、２−フェニル−４−メチルイミダゾール、２−エチル−４−メチルイミダゾール、１−シアノエチル−２−エチル−４−メチルイミダゾール等が挙げられる。尿素系の硬化促進剤としては、３−フェニル−１，１−ジメチルウレア等が挙げられる。リン系の硬化促進剤としては、トリフェニルホスフィン及びその付加反応物、（４−ヒドロキシフェニル）ジフェニルホスフィン、ビス（４−ヒドロキシフェニル）フェニルホスフィン、トリス（４−ヒドロキシフェニル）ホスフィン等が挙げられる。((D) Curing accelerator)
The (D) curing accelerator is not particularly limited, but is, for example, a group consisting of an amine-based curing accelerator, an imidazole-based curing accelerator, a urea-based curing accelerator, and a phosphorus-based curing accelerator. It may be at least one selected from the above. Examples of the amine-based curing accelerator include 1,8-diazabicyclo [5.4.0] -7-undecene and 1,5-diazabicyclo [4.3.0] -5-nonene. Examples of the imidazole-based curing accelerator include 2-phenyl-4-methylimidazole, 2-ethyl-4-methylimidazole, 1-cyanoethyl-2-ethyl-4-methylimidazole and the like. Examples of the urea-based curing accelerator include 3-phenyl-1,1-dimethylurea and the like. Examples of the phosphorus-based curing accelerator include triphenylphosphine and its addition reaction product, (4-hydroxyphenyl) diphenylphosphine, bis (4-hydroxyphenyl) phenylphosphine, tris (4-hydroxyphenyl) phosphine and the like.
（Ｄ）硬化促進剤としては、誘導体の種類が豊富であり、所望の活性温度を得やすい観点から、イミダゾール系の硬化促進剤であってもよい。イミダゾール系の硬化促進剤としては、市販品を用いてもよい。イミダゾール系の硬化促進剤の市販品としては、例えば、四国化成工業株式会社製の商品名「キュアゾール ２ＰＨＺ−ＰＷ」及び「キュアゾール２Ｐ４ＭＺ」等が挙げられる。（Ｄ）硬化促進剤は、１種を単独で用いてもよく、２種以上を併用してもよい。 The curing accelerator (D) may be an imidazole-based curing accelerator from the viewpoint that a wide variety of derivatives are available and a desired active temperature can be easily obtained. A commercially available product may be used as the imidazole-based curing accelerator. Examples of commercially available imidazole-based curing accelerators include trade names "Curesol 2PHZ-PW" and "Curesol 2P4MZ" manufactured by Shikoku Chemicals Corporation. (D) As the curing accelerator, one type may be used alone, or two or more types may be used in combination.
（Ｄ）硬化促進剤の含有量は、充分な硬化促進効果を容易に得ることができる観点、並びに、フィルム状エポキシ樹脂組成物を作製する際の工程（塗工及び乾燥等）中、又は、フィルム状エポキシ樹脂組成物の保管中に硬化が進行することを抑制することができると共に、フィルム状エポキシ樹脂組成物の割れ、及び、溶融粘度の上昇に伴う成形不良を防止しやすい観点から、下記の範囲であってもよい。（Ｄ）硬化促進剤の含有量は、（Ａ）エポキシ樹脂と（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として、０．０１質量％以上であってもよく、０．１質量％以上であってもよく、０．３質量％以上であってもよい。（Ｄ）硬化促進剤の含有量は、（Ａ）エポキシ樹脂と（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として、５質量％以下であってもよく、３質量％以下であってもよく、１．５質量％以下であってもよい。これらの観点から、（Ｄ）硬化促進剤の含有量は、（Ａ）エポキシ樹脂と（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として、０．０１〜５質量％であってもよく、０．１〜３質量％であってもよく、０．３〜１．５質量％であってもよい。 (D) The content of the curing accelerator is determined from the viewpoint that a sufficient curing promoting effect can be easily obtained, and during the steps (coating, drying, etc.) when producing the film-shaped epoxy resin composition, or. From the viewpoint that it is possible to suppress the progress of curing during storage of the film-shaped epoxy resin composition, and it is easy to prevent cracking of the film-shaped epoxy resin composition and molding defects due to an increase in melt viscosity, the following It may be in the range of. The content of (D) curing accelerator may be 0.01% by mass or more based on the total amount of (A) epoxy resin and (B) resin having an aromatic ring and a hydroxyl group, and may be 0.1. It may be mass% or more, and may be 0.3 mass% or more. The content of the curing accelerator (D) may be 5% by mass or less, or 3% by mass or less, based on the total amount of the (A) epoxy resin and (B) the resin having an aromatic ring and a hydroxyl group. It may be present, and may be 1.5% by mass or less. From these viewpoints, the content of (D) the curing accelerator is 0.01 to 5% by mass based on the total amount of (A) epoxy resin and (B) resin having an aromatic ring and a hydroxyl group. It may be 0.1 to 3% by mass, or 0.3 to 1.5% by mass.
（（Ｅ）無機充填剤）
（Ｅ）無機充填剤としては、従来公知の無機充填剤が使用でき、特定に限定されない。（Ｅ）無機充填剤としては、硫酸バリウム；チタン酸バリウム；無定形シリカ、結晶性シリカ、溶融シリカ、球状シリカ等のシリカ類；タルク；クレー；炭酸マグネシウム；炭酸カルシウム；酸化アルミニウム；水酸化アルミニウム；窒化ケイ素；窒化アルミニウムなどが挙げられる。（Ｅ）無機充填剤は、表面改質等により、樹脂中への分散性の向上効果及びワニス中での沈降抑制効果が得られやすい観点、並びに、比較的小さい熱膨張率を有するために所望の硬化膜特性が得られやすい観点から、シリカ類であってもよい。（Ｅ）無機充填剤は、１種を単独で用いてもよく、２種以上を併用してもよい。((E) Inorganic filler)
As the inorganic filler (E), a conventionally known inorganic filler can be used and is not particularly limited. (E) Examples of the inorganic filler include barium sulfate; barium titanate; silicas such as amorphous silica, crystalline silica, fused silica, and spherical silica; talc; clay; magnesium carbonate; calcium carbonate; aluminum oxide; aluminum hydroxide. ; Silicon nitride; aluminum nitride and the like. The inorganic filler (E) is desirable because it has a viewpoint that it is easy to obtain an effect of improving dispersibility in a resin and an effect of suppressing sedimentation in a varnish by surface modification or the like, and it has a relatively small coefficient of thermal expansion. From the viewpoint that the cured film characteristics of the above can be easily obtained, silica may be used. (E) As the inorganic filler, one type may be used alone, or two or more types may be used in combination.
（Ｅ）無機充填剤は、表面改質されていてもよい。表面改質の手法としては、特に限定されないが、簡便であり、官能基の種類が豊富であり、所望の特性を付与しやすいことから、シランカップリング剤を用いた表面改質であってもよい。シランカップリング剤としては、アルキルシラン、アルコキシシラン、ビニルシラン、エポキシシラン、アミノシラン、アクリルシラン、メタクリルシラン、メルカプトシラン、スルフィドシラン、イソシアネートシラン、サルファーシラン、スチリルシラン、アルキルクロロシラン等が挙げられる。シランカップリング剤は、１種を単独で用いてもよく、２種以上を併用してもよい。 (E) The inorganic filler may be surface-modified. The surface modification method is not particularly limited, but is simple, has a wide variety of functional groups, and is easy to impart desired properties. Therefore, even surface modification using a silane coupling agent is possible. Good. Examples of the silane coupling agent include alkylsilane, alkoxysilane, vinylsilane, epoxysilane, aminosilane, acrylicsilane, methacrylsilane, mercaptosilane, sulfidesilane, isocyanatesilane, sulfasilane, styrylsilane, and alkylchlorosilane. One type of silane coupling agent may be used alone, or two or more types may be used in combination.
（Ｅ）無機充填剤の平均粒子径は、無機充填剤の凝集が容易に抑制されて充分な分散が可能であると共に、フィルム状エポキシ樹脂組成物の作製においてワニス中での粒子の沈降が容易に抑制される観点から、下記の範囲であってもよい。（Ｅ）無機充填剤の平均粒子径は、０．０１μｍ以上であってもよく、０．１μｍ以上であってもよく、０．３μｍ以上であってもよい。（Ｅ）無機充填剤の平均粒子径は、５０μｍ以下であってもよく、２５μｍ以下であってもよく、１０μｍ以下であってもよい。これらの観点から、（Ｅ）無機充填剤の平均粒子径は、０．０１〜５０μｍであってもよく、０．１〜２５μｍであってもよく、０．３〜１０μｍであってもよい。 (E) The average particle size of the inorganic filler is such that the aggregation of the inorganic filler is easily suppressed and sufficient dispersion is possible, and the particles are easily settled in the varnish in the production of the film-shaped epoxy resin composition. The range may be as follows from the viewpoint of being suppressed. The average particle size of the inorganic filler (E) may be 0.01 μm or more, 0.1 μm or more, or 0.3 μm or more. The average particle size of the inorganic filler (E) may be 50 μm or less, 25 μm or less, or 10 μm or less. From these viewpoints, the average particle size of the (E) inorganic filler may be 0.01 to 50 μm, 0.1 to 25 μm, or 0.3 to 10 μm.
（Ｅ）無機充填剤の含有量は、被封止体（半導体素子等の電子デバイスなど）と封止部との熱膨張率の差によって電子装置（半導体装置等）の反りが大きくなることを容易に防止できると共に、フィルム状エポキシ樹脂組成物の作製の際に乾燥工程において割れが生じること、及び、フィルム状エポキシ樹脂組成物の溶融粘度の上昇により被封止体が充分に封止できなくなる不具合を容易に抑制できる観点から、下記の範囲であってもよい。（Ｅ）無機充填剤の含有量は、エポキシ樹脂組成物の全量を基準として、５０質量％以上であってもよく、６０質量％以上であってもよく、７０質量％以上であってもよい。（Ｅ）無機充填剤の含有量は、エポキシ樹脂組成物の全量を基準として、９５質量％以下であってもよく、９０質量％以下であってもよい。これらの観点から、（Ｅ）無機充填剤の含有量は、エポキシ樹脂組成物の全量を基準として、５０質量％以上であってもよく、６０〜９５質量％であってもよく、７０〜９０質量％であってもよい。 (E) The content of the inorganic filler is such that the warp of the electronic device (semiconductor device, etc.) increases due to the difference in the coefficient of thermal expansion between the object to be sealed (electronic device such as a semiconductor element) and the sealing portion. In addition to being easily prevented, cracks occur in the drying step during the production of the film-shaped epoxy resin composition, and the material to be sealed cannot be sufficiently sealed due to an increase in the melt viscosity of the film-shaped epoxy resin composition. From the viewpoint that defects can be easily suppressed, the range may be as follows. The content of the inorganic filler (E) may be 50% by mass or more, 60% by mass or more, or 70% by mass or more based on the total amount of the epoxy resin composition. .. The content of the inorganic filler (E) may be 95% by mass or less, or 90% by mass or less, based on the total amount of the epoxy resin composition. From these viewpoints, the content of the (E) inorganic filler may be 50% by mass or more, 60 to 95% by mass, or 70 to 90% based on the total amount of the epoxy resin composition. It may be% by mass.
（その他の成分）
本実施形態に係るエポキシ樹脂組成物は、他の添加剤を更に含有していてもよい。このような添加剤としては、顔料、染料、離型剤、酸化防止剤、応力緩和剤、カップリング剤、表面張力調整剤、イオン交換体、着色剤、難燃剤等を挙げることができる。但し、添加剤はこれらに限定されるものではなく、本実施形態に係るエポキシ樹脂組成物は、必要に応じて当技術分野で周知の各種添加剤を含有していてもよい。(Other ingredients)
The epoxy resin composition according to the present embodiment may further contain other additives. Examples of such additives include pigments, dyes, mold release agents, antioxidants, stress relaxation agents, coupling agents, surface tension modifiers, ion exchangers, colorants, flame retardants and the like. However, the additives are not limited to these, and the epoxy resin composition according to the present embodiment may contain various additives well known in the art, if necessary.
＜フィルム状エポキシ樹脂組成物＞
本実施形態に係るフィルム状エポキシ樹脂組成物は、本実施形態に係るエポキシ樹脂組成物又はその硬化物を含んでいる。本実施形態に係るフィルム状エポキシ樹脂組成物は、モールド成形による封止、金型を必要としない成形方法（ラミネート、プレス等）による封止などに用いることができる。<Film epoxy resin composition>
The film-shaped epoxy resin composition according to the present embodiment contains the epoxy resin composition according to the present embodiment or a cured product thereof. The film-shaped epoxy resin composition according to the present embodiment can be used for sealing by molding, sealing by a molding method (lamination, press, etc.) that does not require a mold, and the like.
本実施形態に係るフィルム状エポキシ樹脂組成物によれば、被封止体が大型化した場合であっても、液状又は固形（顆粒、粉体等）の樹脂封止材と比較して、被封止体上へ封止樹脂を均一に供給することが可能であり、被封止体を容易に良好に封止することができる。また、顆粒又は粉体である樹脂封止材を用いた場合には、樹脂封止材が発塵源となり、装置又はクリーンルームが汚染されることがあるのに対し、本実施形態に係るフィルム状エポキシ樹脂組成物によれば、発塵の問題を低減しつつ封止成形物を大型化することができる。 According to the film-shaped epoxy resin composition according to the present embodiment, even when the object to be sealed is enlarged, it is covered as compared with a liquid or solid (granule, powder, etc.) resin encapsulant. The sealing resin can be uniformly supplied onto the sealing body, and the sealed body can be easily and satisfactorily sealed. Further, when a resin encapsulant which is a granule or a powder is used, the resin encapsulant becomes a dust generation source and may contaminate the apparatus or the clean room, whereas the film-like material according to the present embodiment. According to the epoxy resin composition, the size of the sealed molded product can be increased while reducing the problem of dust generation.
モールド成形では、封止樹脂を金型内で成形するため、封止成形物を大型化するには、金型の大型化が必要となる。金型の大型化は、高い金型精度が求められることから技術面での難易度が上がると共に、金型の製造コストが大幅に増加する場合がある。これに対し、本実施形態に係るフィルム状エポキシ樹脂組成物は、従来の封止成形方法であるモールド成形のみならず、金型を必要としない成形方法（ラミネート、プレス等）にも好適に用いることができる。 In mold molding, since the sealing resin is molded in the mold, it is necessary to increase the size of the mold in order to increase the size of the sealed molded product. Since high mold accuracy is required to increase the size of the mold, the technical difficulty increases and the manufacturing cost of the mold may increase significantly. On the other hand, the film-shaped epoxy resin composition according to the present embodiment is suitably used not only for molding, which is a conventional sealing molding method, but also for molding methods (lamination, press, etc.) that do not require a mold. be able to.
本実施形態に係るフィルム状エポキシ樹脂組成物の厚みは、フィルム状エポキシ樹脂組成物が割れることを防ぎやすい観点から、２５μｍ以上であってもよく、５０μｍ以上であってもよい。本実施形態に係るフィルム状エポキシ樹脂組成物の厚みは、フィルム状エポキシ樹脂組成物の厚みのばらつきを抑える観点から、５００μｍ以下であってもよく、３００μｍ以下であってもよい。 The thickness of the film-shaped epoxy resin composition according to the present embodiment may be 25 μm or more, or 50 μm or more, from the viewpoint of easily preventing the film-shaped epoxy resin composition from cracking. The thickness of the film-shaped epoxy resin composition according to the present embodiment may be 500 μm or less, or 300 μm or less, from the viewpoint of suppressing variations in the thickness of the film-shaped epoxy resin composition.
本実施形態に係るフィルム状エポキシ樹脂組成物は、例えば、本実施形態に係るエポキシ樹脂組成物又はその硬化物をフィルム状に成形することにより得ることができる。第１実施形態に係るフィルム状エポキシ樹脂組成物の製造方法は、ワニス塗工法であり、例えば、少なくとも（Ａ）エポキシ樹脂、（Ｂ）芳香環及び水酸基を有する樹脂、（Ｃ）シリコーンパウダー、（Ｄ）硬化促進剤、並びに、（Ｅ）無機充填剤を含有するワニスを用いて塗膜を支持体上に形成する工程と、前記塗膜を加熱乾燥してフィルム状エポキシ樹脂組成物を得る工程と、を備える。第２実施形態に係るフィルム状エポキシ樹脂組成物の製造方法は、少なくとも（Ａ）エポキシ樹脂、（Ｂ）芳香環及び水酸基を有する樹脂、（Ｃ）シリコーンパウダー、（Ｄ）硬化促進剤、並びに、（Ｅ）無機充填剤を含有する固形樹脂組成物をシート状に成形してフィルム状エポキシ樹脂組成物を得る工程を備える。厚みを簡便に制御できる観点から、前記ワニス塗工法であってもよい。 The film-shaped epoxy resin composition according to the present embodiment can be obtained, for example, by molding the epoxy resin composition according to the present embodiment or a cured product thereof into a film shape. The method for producing the film-shaped epoxy resin composition according to the first embodiment is a varnish coating method, for example, (A) epoxy resin, (B) resin having an aromatic ring and a hydroxyl group, (C) silicone powder, ( D) A step of forming a coating film on a support using a varnish containing a curing accelerator and (E) an inorganic filler, and a step of heating and drying the coating film to obtain a film-like epoxy resin composition. And. The method for producing the film-shaped epoxy resin composition according to the second embodiment is as follows: (A) epoxy resin, (B) resin having an aromatic ring and hydroxyl group, (C) silicone powder, (D) curing accelerator, and (E) The present invention comprises a step of molding a solid resin composition containing an inorganic filler into a sheet to obtain a film-shaped epoxy resin composition. The varnish coating method may be used from the viewpoint that the thickness can be easily controlled.
本実施形態に係るフィルム状エポキシ樹脂組成物は、例えば、（Ａ）エポキシ樹脂、（Ｂ）芳香環及び水酸基を有する樹脂、（Ｃ）シリコーンパウダー、（Ｄ）硬化促進剤、（Ｅ）無機充填剤、並びに、必要に応じて用いられる各種任意成分を混合することにより作製することができる。混合方法としては、各配合成分が分散混合できれば特に限定されないが、ミル、ミキサー、撹拌羽根等が使用できる。必要に応じて、各配合成分を溶剤等に溶解して得られるワニスを用いるワニス塗工法により製膜することができる。また、本実施形態に係るフィルム状エポキシ樹脂組成物は、ニーダー、二本ロール、連続混練装置等で各配合成分を混練することにより作製した固形樹脂組成物をシート状に押し出して製膜することにより得ることもできる。 The film-shaped epoxy resin composition according to the present embodiment is, for example, (A) epoxy resin, (B) resin having an aromatic ring and a hydroxyl group, (C) silicone powder, (D) curing accelerator, and (E) inorganic filling. It can be prepared by mixing an agent and various optional components used as needed. The mixing method is not particularly limited as long as each compounding component can be dispersed and mixed, but a mill, a mixer, a stirring blade or the like can be used. If necessary, a film can be formed by a varnish coating method using a varnish obtained by dissolving each compounding component in a solvent or the like. Further, the film-shaped epoxy resin composition according to the present embodiment is formed by extruding a solid resin composition prepared by kneading each compounding component with a kneader, a double roll, a continuous kneading device or the like into a sheet shape. Can also be obtained by.
溶剤としては、従来公知の有機溶剤が使用できる。有機溶剤としては、脂肪族炭化水素類、芳香族炭化水素類、テルペン類、ハロゲン類、エステル類、ケトン類、アルコール類、アルデヒド類等が挙げられる。有機溶剤は、１種を単独で用いてもよく、２種以上を併用してもよい。 As the solvent, a conventionally known organic solvent can be used. Examples of the organic solvent include aliphatic hydrocarbons, aromatic hydrocarbons, terpenes, halogens, esters, ketones, alcohols, aldehydes and the like. As the organic solvent, one type may be used alone, or two or more types may be used in combination.
有機溶剤としては、環境負荷が小さい観点、及び、（Ａ）エポキシ樹脂並びに（Ｂ）芳香環及び水酸基を有する樹脂を溶解しやすい観点から、エステル類、ケトン類及びアルコール類であってもよい。有機溶剤としては、（Ａ）エポキシ樹脂並びに（Ｂ）芳香環及び水酸基を有する樹脂を特に溶解しやすい観点から、ケトン類であってもよい。有機溶剤としては、室温（２５℃）での揮発が少なく乾燥時に除去しやすい観点から、アセトン、メチルエチルケトン及びメチルイソブチルケトンであってもよい。 The organic solvent may be esters, ketones and alcohols from the viewpoint of having a small environmental load and from the viewpoint of easily dissolving (A) an epoxy resin and (B) a resin having an aromatic ring and a hydroxyl group. The organic solvent may be ketones from the viewpoint of particularly easily dissolving (A) an epoxy resin and (B) a resin having an aromatic ring and a hydroxyl group. The organic solvent may be acetone, methyl ethyl ketone or methyl isobutyl ketone from the viewpoint of less volatilization at room temperature (25 ° C.) and easy removal during drying.
フィルム状エポキシ樹脂組成物の製造に用いるワニスにおける有機溶剤の含有量は、当該ワニスの全量を基準として、２〜３０質量％であってもよく、５〜２５質量％であってもよい。このような範囲であることにより、フィルム割れ等の不具合を容易に防止できると共に、充分な最低溶融粘度が得られやすい。また、粘着性が強くなりすぎて取扱性が低下する不具合、及び、熱硬化時における有機溶剤の揮発に伴う発泡等の不具合を容易に防止することができる。 The content of the organic solvent in the varnish used for producing the film-shaped epoxy resin composition may be 2 to 30% by mass or 5 to 25% by mass based on the total amount of the varnish. Within such a range, defects such as film cracking can be easily prevented, and a sufficient minimum melt viscosity can be easily obtained. In addition, it is possible to easily prevent a problem that the adhesiveness becomes too strong and the handleability is lowered, and a problem such as foaming due to volatilization of the organic solvent during thermosetting.
ワニス塗工法においては、支持体にワニスを塗布して得られた塗膜を熱風吹き付け等によって加熱乾燥させることにより、フィルム状エポキシ樹脂組成物を作製することができる。塗布に使用するコーティング方法としては、特に限定されないが、ダイコート、コンマコート等が挙げられる。 In the varnish coating method, a film-like epoxy resin composition can be produced by applying varnish to a support and heating and drying the coating film obtained by blowing hot air or the like. The coating method used for coating is not particularly limited, and examples thereof include die coating and comma coating.
支持体としては、特に限定されるものではないが、高分子フィルム、金属箔等が挙げられる。高分子フィルムとしては、ポリエチレンフィルム、ポリプロピレンフィルム等のポリオレフィンフィルム；ポリエチレンテレフタレートフィルム等のポリエステルフィルム；ポリ塩化ビニルフィルム；ポリカーボネートフィルム；アセチルセルロースフィルム；ポリイミドフィルム；ポリアミドフィルム；テトラフルオロエチレンフィルムなどが挙げられる。金属箔としては、銅箔、アルミニウム箔等が挙げられる。 The support is not particularly limited, and examples thereof include a polymer film and a metal foil. Examples of the polymer film include polyolefin films such as polyethylene film and polypropylene film; polyester film such as polyethylene terephthalate film; polyvinyl chloride film; polycarbonate film; acetyl cellulose film; polyimide film; polyamide film; tetrafluoroethylene film and the like. .. Examples of the metal foil include copper foil and aluminum foil.
支持体の厚みは、特に限定されるものではないが、作業性及び乾燥性に優れる観点から、２〜２００μｍであってもよい。このような厚みであると、支持体が塗工時に切れる不具合、及び、ワニスの重さによって支持体が塗工時にたわむ不具合を防止できる。また、塗工面及び裏面の両面から熱風が吹き付けられる乾燥機を用いる場合にワニス中の溶剤乾燥が妨げられる不具合の発生を抑制することもできる。 The thickness of the support is not particularly limited, but may be 2 to 200 μm from the viewpoint of excellent workability and dryness. With such a thickness, it is possible to prevent a problem that the support is cut at the time of coating and a problem that the support is bent at the time of coating due to the weight of the varnish. Further, when a dryer in which hot air is blown from both the coated surface and the back surface is used, it is possible to suppress the occurrence of a problem that the solvent drying in the varnish is hindered.
前記塗膜の加熱乾燥としては、全乾燥時間の２５％以上の時間において、有機溶剤の沸点の±１０℃の温度で塗膜を加熱することができる。加熱乾燥は、加熱温度が異なる２段階以上の工程で行うことができる。この場合、低い温度から加熱乾燥を行ってもよく、次段階の加熱温度は、前段階の加熱温度の＋３０℃以内に設定することができる。 As the heating and drying of the coating film, the coating film can be heated at a temperature of ± 10 ° C., which is the boiling point of the organic solvent, for a time of 25% or more of the total drying time. The heat drying can be performed in two or more steps having different heating temperatures. In this case, heating and drying may be performed from a low temperature, and the heating temperature of the next stage can be set within + 30 ° C. of the heating temperature of the previous stage.
本実施形態においては、支持体上に設けられたフィルム状エポキシ樹脂組成物上に、保護を目的とした保護層（例えば保護フィルム）を配置してもよい。保護層を配置することで、取扱性が更に向上し、巻き取りした場合において支持体の裏面にフィルム状エポキシ樹脂組成物が張り付く不具合を回避することができる。 In the present embodiment, a protective layer (for example, a protective film) for the purpose of protection may be arranged on the film-like epoxy resin composition provided on the support. By arranging the protective layer, the handleability is further improved, and it is possible to avoid the problem that the film-like epoxy resin composition sticks to the back surface of the support when it is wound up.
保護層としては、特に限定されるものではないが、高分子フィルム、金属箔等が挙げられる。高分子フィルムとしては、ポリエチレンフィルム、ポリプロピレンフィルム等のポリオレフィンフィルム；ポリエチレンテレフタレートフィルム等のポリエステルフィルム；ポリ塩化ビニルフィルム；ポリカーボネートフィルム；アセチルセルロースフィルム；テトラフルオロエチレンフィルムなどが挙げられる。金属箔としては、銅箔、アルミニウム箔等が挙げられる。 The protective layer is not particularly limited, and examples thereof include a polymer film and a metal foil. Examples of the polymer film include a polyolefin film such as a polyethylene film and a polypropylene film; a polyester film such as a polyethylene terephthalate film; a polyvinyl chloride film; a polycarbonate film; an acetyl cellulose film; and a tetrafluoroethylene film. Examples of the metal foil include copper foil and aluminum foil.
保護層の厚みは、特に限定されるものではないが、充分な保護効果を得る観点、及び、フィルム状エポキシ樹脂組成物をロール状に巻き取った際の厚みを低減する観点から、１２〜１００μｍであってもよい。 The thickness of the protective layer is not particularly limited, but is 12 to 100 μm from the viewpoint of obtaining a sufficient protective effect and reducing the thickness when the film-shaped epoxy resin composition is wound into a roll. It may be.
本実施形態によれば、支持体と、当該支持体上に配置されたフィルム状エポキシ樹脂組成物と、を備える封止シートを提供することができる。封止シートは、フィルム状エポキシ樹脂組成物の支持体側とは反対側に保護層を更に備えていてもよい。 According to the present embodiment, it is possible to provide a sealing sheet including a support and a film-like epoxy resin composition arranged on the support. The sealing sheet may further be provided with a protective layer on the side opposite to the support side of the film-shaped epoxy resin composition.
＜電子装置＞
本実施形態に係る電子装置は、電子部品及び電子デバイスからなる群より選ばれる少なくとも１種の被封止体と、前記被封止体を封止する封止部と、を備え、前記封止部が、本実施形態に係るエポキシ樹脂組成物若しくはその硬化物、又は、本実施形態に係るフィルム状エポキシ樹脂組成物を含む。本実施形態に係る電子装置は、エポキシ樹脂組成物若しくはその硬化物、又は、フィルム状エポキシ樹脂組成物を用いて被封止体が封止されてなる。電子デバイスを備える電子装置としては、例えば、半導体素子を備える半導体装置が挙げられる。<Electronic equipment>
The electronic device according to the present embodiment includes at least one type of object to be sealed selected from the group consisting of electronic components and electronic devices, and a sealing portion for sealing the sealed body, and the sealing portion is provided. The unit includes the epoxy resin composition according to the present embodiment or a cured product thereof, or the film-shaped epoxy resin composition according to the present embodiment. The electronic device according to the present embodiment is formed by sealing the sealed body with an epoxy resin composition or a cured product thereof, or a film-shaped epoxy resin composition. Examples of the electronic device including the electronic device include a semiconductor device including a semiconductor element.
本実施形態に係る電子装置の製造方法は、本実施形態に係るエポキシ樹脂組成物（フィルム状エポキシ樹脂組成物等）により、電子部品及び電子デバイスからなる群より選ばれる少なくとも１種の被封止体を封止する封止工程と、前記エポキシ樹脂組成物を硬化させて封止部を得る工程と、を備えてもよい。封止工程は、例えば、エポキシ樹脂組成物（フィルム状エポキシ樹脂組成物等）を加熱下で押圧することにより、被封止体（例えば、基板上に設けられた被封止体）を封止する工程である。本実施形態に係る電子装置の製造方法は、例えば、加熱下でフィルム状エポキシ樹脂組成物を被封止体に押圧することにより、フィルム状エポキシ樹脂組成物により被封止体を封止する工程と、被封止体が封止されたフィルム状エポキシ樹脂組成物を硬化させて封止部を得る工程と、を備えてもよい。 The method for manufacturing an electronic device according to the present embodiment is that the epoxy resin composition (film-like epoxy resin composition or the like) according to the present embodiment is used to seal at least one type selected from the group consisting of electronic parts and electronic devices. A sealing step of sealing the body and a step of curing the epoxy resin composition to obtain a sealed portion may be provided. In the sealing step, for example, the epoxy resin composition (film-like epoxy resin composition or the like) is pressed under heating to seal the sealed body (for example, the sealed body provided on the substrate). It is a process to do. The method for manufacturing an electronic device according to the present embodiment is, for example, a step of sealing the sealed body with the film-shaped epoxy resin composition by pressing the film-shaped epoxy resin composition against the sealed body under heating. And a step of curing the film-like epoxy resin composition in which the material to be sealed is sealed to obtain a sealed portion may be provided.
以上、本発明の好適な実施形態について説明したが、本発明は、上述した実施形態に限定されるものではなく、その趣旨を逸脱しない範囲で適宜変更を行ってもよい。 Although the preferred embodiment of the present invention has been described above, the present invention is not limited to the above-described embodiment, and modifications may be made as appropriate without departing from the spirit of the present invention.
以下、実施例により本発明を更に具体的に説明するが、本発明の範囲はこれらの実施例に限定されるものではない。 Hereinafter, the present invention will be described in more detail with reference to Examples, but the scope of the present invention is not limited to these Examples.
＜実施例１〜５及び比較例１〜４、６＞
（フィルム状エポキシ樹脂組成物の作製）
フィルム状エポキシ樹脂組成物を構成する成分として、表１及び表２に示す化合物を準備した。各成分の詳細を下記に示す。<Examples 1 to 5 and Comparative Examples 1 to 4, 6>
(Preparation of film-shaped epoxy resin composition)
The compounds shown in Tables 1 and 2 were prepared as components constituting the film-shaped epoxy resin composition. Details of each component are shown below.
（Ａ）エポキシ樹脂
［２５℃で液状である成分］
Ａ１：ビスフェノールＦ型エポキシ樹脂（エポキシ当量：１６０、三菱化学株式会社製、商品名「ｊＥＲ８０６」）
Ａ２：２官能ナフタレン型エポキシ樹脂（エポキシ当量：１４１、ＤＩＣ株式会社製、商品名「ＨＰ−４０３２Ｄ」、下記式で表される化合物）
Ａ３：３官能ナフタレン型エポキシ樹脂（エポキシ当量：１８２、ＤＩＣ株式会社製、商品名「ＨＰ−４７５０」、式（ＩＶ）で表される化合物）(A) Epoxy resin [components that are liquid at 25 ° C]
A1: Bisphenol F type epoxy resin (epoxy equivalent: 160, manufactured by Mitsubishi Chemical Corporation, trade name "jER806")
A2: Bifunctional naphthalene type epoxy resin (epoxy equivalent: 141, manufactured by DIC Corporation, trade name "HP-4032D", compound represented by the following formula)
A3: Trifunctional naphthalene type epoxy resin (epoxy equivalent: 182, manufactured by DIC Corporation, trade name "HP-4750", compound represented by formula (IV))
（Ｂ）芳香環及び水酸基を有する樹脂
［ナフタレン環及び水酸基を有する樹脂］
Ｂ１：下記式で表される化合物（水酸基当量：１１０、新日鉄住金化学株式会社製、商品名「ＳＮ−３９５」）
Ｂ２：式（ＶＩＩ）で表される構造を有する化合物（水酸基当量：２０５、新日鉄住金化学株式会社製、商品名「ＳＮ−４７５Ｎ」）
［ナフタレン環を有していないフェノール樹脂］
Ｂ３：ノボラック型フェノール樹脂（水酸基当量：１０４、旭有機材工業株式会社製、商品名「ＰＡＰＳ−ＰＮ２」）(B) Resin having an aromatic ring and a hydroxyl group [Resin having a naphthalene ring and a hydroxyl group]
B1: Compound represented by the following formula (hydroxyl equivalent: 110, manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., trade name "SN-395")
B2: Compound having a structure represented by the formula (VII) (hydroxyl equivalent: 205, manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., trade name "SN-475N")
[Phenolic resin without naphthalene ring]
B3: Novolac type phenolic resin (hydroxyl equivalent: 104, manufactured by Asahi Organic Materials Industry Co., Ltd., trade name "PAPS-PN2")
（Ｃ）シリコーンパウダー
Ｃ１：信越化学工業株式会社製、商品名「ＫＭＰ６０５」、平均粒子径：２μｍ
Ｃ２：信越化学工業株式会社製、商品名「ＫＭＰ６００」、平均粒子径：５μｍ
Ｃ３：信越化学工業株式会社製、商品名「ＫＭＰ７０１」、平均粒子径：３．５μｍ(C) Silicone powder C1: Manufactured by Shin-Etsu Chemical Co., Ltd., trade name "KMP605", average particle size: 2 μm
C2: Manufactured by Shin-Etsu Chemical Co., Ltd., trade name "KMP600", average particle size: 5 μm
C3: Made by Shin-Etsu Chemical Co., Ltd., trade name "KMP701", average particle size: 3.5 μm
（Ｄ）硬化促進剤
四国化成工業株式会社製、商品名「キュアゾール ２Ｐ４ＭＺ」(D) Curing accelerator, manufactured by Shikoku Kasei Kogyo Co., Ltd., trade name "Curesol 2P4MZ"
（Ｅ）無機充填剤
シリカ（株式会社アドマテックス製、商品名「ＳＸ−Ｅ２」、フェニルアミノシラン処理、平均粒子径：５．８μｍ）(E) Inorganic filler silica (manufactured by Admatex Co., Ltd., trade name "SX-E2", phenylaminosilane treatment, average particle size: 5.8 μm)
有機溶剤
メチルエチルケトン（株式会社ゴードー製）Organic solvent Methyl ethyl ketone (manufactured by Gordo Co., Ltd.)
表１及び表２に示す配合量（単位：質量部）の各成分を１Ｌのポリエチレン容器に仕込んだ後、３時間攪拌して分散及び混合することにより混合液を得た。この混合液をナイロン製の＃２００メッシュ（開口径：７５μｍ）でろ過し、ろ液をワニス状エポキシ樹脂組成物として採取した。塗工機を使用して支持体（３８μｍ厚のポリエチレンテレフタレート、王子エフテックス株式会社製）上にこのワニス状エポキシ樹脂組成物を塗布した後に乾燥させることで、支持体及びフィルム状エポキシ樹脂組成物の積層体（全厚：１８８μｍ、樹脂組成物層の厚み：１５０μｍ）を作製した。なお、塗布及び乾燥の条件は下記のとおりである。
・塗布方法：コンマコート
・乾燥速度：１ｍ／分
・乾燥条件（温度／炉長）：１１０℃／３．３ｍ、１３０℃／３．３ｍ、１４０℃／３．３ｍEach component in the blending amounts (unit: parts by mass) shown in Tables 1 and 2 was charged into a 1 L polyethylene container, and then stirred for 3 hours to disperse and mix to obtain a mixed solution. This mixed solution was filtered through a nylon # 200 mesh (opening diameter: 75 μm), and the filtrate was collected as a varnish-like epoxy resin composition. By applying this varnish-like epoxy resin composition on a support (38 μm thick polyethylene terephthalate, manufactured by Oji F-Tex Co., Ltd.) using a coating machine and then drying it, the support and film-like epoxy resin composition (Total thickness: 188 μm, thickness of resin composition layer: 150 μm) was prepared. The conditions for application and drying are as follows.
-Applying method: Comma coat-Drying speed: 1 m / min-Drying conditions (temperature / furnace length): 110 ° C / 3.3 m, 130 ° C / 3.3 m, 140 ° C / 3.3 m
＜比較例５＞
表２に示す化合物を用いて、実施例１と同様にワニス状エポキシ樹脂組成物を支持体上に塗布した後に乾燥させたが、樹脂組成物のフィルム化ができず、フィルム状エポキシ樹脂組成物が得られなかった。<Comparative example 5>
Using the compounds shown in Table 2, the varnish-like epoxy resin composition was applied onto the support and then dried in the same manner as in Example 1, but the resin composition could not be formed into a film, and the film-like epoxy resin composition was not formed. Was not obtained.
＜評価＞
実施例１〜５及び比較例１〜４、６のフィルム状エポキシ樹脂組成物を用いて以下の評価を行った。なお、比較例３については、反り量及び耐熱性の評価を行わなかった。フィルム状エポキシ樹脂組成物が得られていない比較例５については、取扱性を表中「Ｂ」と表記した。<Evaluation>
The following evaluations were carried out using the film-like epoxy resin compositions of Examples 1 to 5 and Comparative Examples 1 to 4 and 6. In Comparative Example 3, the amount of warpage and heat resistance were not evaluated. For Comparative Example 5 in which a film-like epoxy resin composition was not obtained, the handleability was indicated as "B" in the table.
（取扱性（屈曲性）の評価）
フィルム状エポキシ樹脂組成物の屈曲性は、屈曲試験機を用いて次の手順で評価した。試験機として、ヨシミツ精機株式会社製の屈曲試験機（ＪＩＳ型タイプ１、円筒型マンドレル法）を準備した。支持体及びフィルム状エポキシ樹脂組成物の積層体を５ｃｍ角にカットして試験片を準備した。直径２ｍｍの円筒形マンドレルに試験片の支持体側を接触させ、試験片を１８０°曲げたときのフィルム状エポキシ樹脂組成物の割れの有無を評価した。割れが発生しない場合を屈曲性良好として、表中「Ａ」と表記した。割れが発生した場合を屈曲性不良として、表中「Ｂ」と表記した。取扱性（屈曲性）の評価結果を表１及び表２に示す。(Evaluation of handleability (flexibility))
The flexibility of the film-shaped epoxy resin composition was evaluated by the following procedure using a bending tester. As a testing machine, a bending testing machine (JIS type type 1, cylindrical mandrel method) manufactured by Yoshimitsu Seiki Co., Ltd. was prepared. A test piece was prepared by cutting the support and the laminated body of the film-shaped epoxy resin composition into 5 cm squares. The support side of the test piece was brought into contact with a cylindrical mandrel having a diameter of 2 mm, and the presence or absence of cracks in the film-like epoxy resin composition when the test piece was bent by 180 ° was evaluated. The case where cracks do not occur is defined as good flexibility and is indicated as "A" in the table. The case where cracks occur is defined as poor flexibility and is indicated as "B" in the table. The evaluation results of handleability (flexibility) are shown in Tables 1 and 2.
（反り量の評価）
［評価サンプルの作製］
長さ２００ｍｍ×幅２００ｍｍ×厚み１．０ｍｍのニチアス株式会社製ナフロンシート（商品名：ＴＯＭＢＯ ９０００−Ｓ）を準備した。ナフロンシートの中心部を長さ１２０ｍｍ×幅１０ｍｍ×厚み１．０ｍｍにカットして、図１に示すように、開口１０ａを有する試験片１０を得た。開口１０ａの中に長さ１２０ｍｍ×幅１０ｍｍ×厚み０.７２５ｍｍのシリコン（Ｓｉ）基板を入れ、シリコン基板が動かないように、長さ１４０ｍｍ×幅２５ｍｍ×厚み０.０２５ｍｍにカットしたニチバン株式会社製のポリイミドテープでシリコン基板の全面及びナフロンシートをナフロンシートの下面から固定した。ポリイミドテープで固定していない上面に、厚み１５０μｍのフィルム状エポキシ樹脂組成物（長さ１２０ｍｍ×幅１０ｍｍにカットしたフィルムを使用）を、シリコン基板上の全面が覆われるように２枚配置した。配置したフィルム状エポキシ樹脂組成物を真空下（０．１ｋＰａ）、温度１１０℃、圧力０．１ＭＰａで５分間プレスした。次に、プレスの圧力を常圧に戻し、シリコン基板上に接着したフィルム状エポキシ樹脂組成物を得た。シリコン基板とフィルム状エポキシ樹脂組成物との積層体の全厚が１．００ｍｍとなるようにフィルム状エポキシ樹脂組成物を研磨した。全厚１．００ｍｍの積層体を１４０℃のオーブンで２時間硬化させた後、２５℃まで自然冷却させることで、反り評価用サンプルを得た。(Evaluation of warpage amount)
[Preparation of evaluation sample]
A naphthon sheet (trade name: TOMBO 9000-S) manufactured by Nichias Corporation having a length of 200 mm, a width of 200 mm and a thickness of 1.0 mm was prepared. The central portion of the naphthon sheet was cut into a length of 120 mm, a width of 10 mm, and a thickness of 1.0 mm to obtain a
［反り量の測定方法］
三次元レーザー形状測定装置（株式会社キーエンス製、商品名：ＬＫ−０３０）を用いて、前記で得られた反り評価用サンプルの室温（２５℃）における最大反り量を測定した。スキャン範囲を１４０ｍｍ×２０ｍｍ、スキャンピッチを１．０ｍｍ、スキャン速度を２０ｍｍ／ｓに設定して測定を行った。測定結果を表１及び表２に示す。[Measurement method of warpage amount]
Using a three-dimensional laser shape measuring device (manufactured by KEYENCE CORPORATION, trade name: LK-030), the maximum amount of warpage of the warp evaluation sample obtained above at room temperature (25 ° C.) was measured. The measurement was performed by setting the scan range to 140 mm × 20 mm, the scan pitch to 1.0 mm, and the scan speed to 20 mm / s. The measurement results are shown in Tables 1 and 2.
（耐熱性の評価）
支持体及びフィルム状エポキシ樹脂組成物の積層体を長さ３０ｍｍ×幅５ｍｍ×厚み０．１８ｍｍにカットした。次に、株式会社名機製作所製の真空加圧ラミネータＭＶＬＰ−５００を用いて、温度９０℃、真空引き時間３０秒、圧力０．５ＭＰａ、加圧時間４０秒の条件で、フィルム状エポキシ樹脂組成物面を長さ１００ｍｍ×幅１００ｍｍ×厚み２ｍｍのニチアス株式会社製ナフロンシート（商品名：ＴＯＭＢＯ ９０００−Ｓ）面に合わせてラミネートした。その後、フィルム状エポキシ樹脂組成物を支持する支持体を剥がした後、ナフロンシート及びフィルム状エポキシ樹脂組成物からなる積層体を１４０℃のオーブンに２時間入れて硬化させて、ナフロンシートに積層された硬化フィルムを得た。次に、ナフロンシートから硬化フィルムを剥がし、測定用サンプルを得た。動的粘弾性測定装置Ｅ−４０００（株式会社ＵＢＭ製）を用い、引張りモード、チャック間距離２０ｍｍ、周波数１０Ｈｚ、昇温速度５／ｍｉｎの条件で測定したときのｔａｎδのピーク値をガラス転移温度（Ｔｇ）として得た。耐熱性（ガラス転移温度［℃］）の評価結果を表１及び表２に示す。(Evaluation of heat resistance)
The support and the laminate of the film-shaped epoxy resin composition were cut into a length of 30 mm, a width of 5 mm, and a thickness of 0.18 mm. Next, using a vacuum pressurizing laminator MVLP-500 manufactured by Meiki Co., Ltd., a film-like epoxy resin composition was used under the conditions of a temperature of 90 ° C., a vacuuming time of 30 seconds, a pressure of 0.5 MPa, and a pressurizing time of 40 seconds. The surface of the object was laminated to match the surface of a Naflon sheet (trade name: TOMBO 9000-S) manufactured by Nichias Corporation having a length of 100 mm, a width of 100 mm, and a thickness of 2 mm. Then, after peeling off the support supporting the film-shaped epoxy resin composition, the laminate composed of the naphthon sheet and the film-shaped epoxy resin composition was placed in an oven at 140 ° C. for 2 hours to be cured, and then laminated on the naphthon sheet. A cured film was obtained. Next, the cured film was peeled off from the naphthon sheet to obtain a sample for measurement. The peak value of tan δ when measured using a dynamic viscoelasticity measuring device E-4000 (manufactured by UBM Co., Ltd.) under the conditions of tension mode, distance between chucks 20 mm,
（難燃性の評価）
支持体及びフィルム状エポキシ樹脂組成物の積層体から支持体を剥がして得られたフィルム状エポキシ樹脂組成物を、厚み１／８インチの試験片を成形するための金型を使用して、トランスファープレスにて金型温度１４０℃、成形圧力１．０ＭＰａ、成形時間１０分の条件で成形した。その後、金型から硬化物を取り出した。さらに、１４０℃のオーブンで２時間硬化を行い、厚み１／８インチの試験片を得た。評価方法はＵＬ−９４試験法に従った。評価結果が「Ｖ−１」に達している場合を表中「Ａ」と表記し、評価結果が「Ｖ−１」に達していない場合を表中「Ｂ」と表記した。難燃性の評価結果を表１及び表２に示す。(Evaluation of flame retardancy)
The film-like epoxy resin composition obtained by peeling the support from the support and the laminate of the film-like epoxy resin composition is transferred to the film-like epoxy resin composition using a mold for molding a test piece having a thickness of 1/8 inch. Molding was performed by a press under the conditions of a mold temperature of 140 ° C., a molding pressure of 1.0 MPa, and a molding time of 10 minutes. Then, the cured product was taken out from the mold. Further, it was cured in an oven at 140 ° C. for 2 hours to obtain a test piece having a thickness of 1/8 inch. The evaluation method was according to the UL-94 test method. The case where the evaluation result reaches "V-1" is described as "A" in the table, and the case where the evaluation result does not reach "V-1" is described as "B" in the table. The evaluation results of flame retardancy are shown in Tables 1 and 2.
前記の結果から、実施例のエポキシ樹脂組成物は、取扱性、反り量、耐熱性及び難燃性のいずれも良好であった。これに対して、比較例１、２及び６では、取扱性には優れているが、樹脂封止後の基板の反りが大きく、反り量が劣ると共に、難燃性も劣っていた。比較例３では、難燃性には優れているが、柔軟性が低く取扱性が劣っていた。比較例４では、取扱性及び難燃性には優れているが、樹脂封止後の基板の反りが大きく、反り量が劣っていた。比較例５では、フィルム化ができておらず、取扱性が劣っていた。 From the above results, the epoxy resin composition of the example was good in all of handleability, warpage amount, heat resistance and flame retardancy. On the other hand, in Comparative Examples 1, 2 and 6, although the handleability was excellent, the warpage of the substrate after resin encapsulation was large, the amount of warpage was inferior, and the flame retardancy was also inferior. In Comparative Example 3, the flame retardancy was excellent, but the flexibility was low and the handleability was inferior. In Comparative Example 4, although it was excellent in handleability and flame retardancy, the warpage of the substrate after resin sealing was large and the amount of warpage was inferior. In Comparative Example 5, the film was not formed and the handleability was inferior.
１０…試験片、１０ａ…開口。 10 ... Test piece, 10a ... Aperture.
Claims (5)
前記（Ａ）エポキシ樹脂が、２５℃で液状であるエポキシ樹脂を含み、
前記（Ｂ）芳香環及び水酸基を有する樹脂が、ナフタレン環及び水酸基を有する樹脂を含み、
前記２５℃で液状であるエポキシ樹脂の含有量が、前記（Ａ）エポキシ樹脂と前記（Ｂ）芳香環及び水酸基を有する樹脂との合計量を基準として３２質量％以上であり、
前記（Ｃ）シリコーンパウダーの含有量が、エポキシ樹脂組成物の全量（但し、前記エポキシ樹脂組成物が溶剤を含有する場合、前記溶剤を除く。）を基準として０．８０〜７．３０質量％であり、
前記（Ａ）エポキシ樹脂が、ビスフェノールＡ型エポキシ樹脂、ビスフェノールＦ型エポキシ樹脂及びナフタレン型エポキシ樹脂からなる群より選ばれる少なくとも１種であり、
前記（Ｃ）シリコーンパウダーが、シロキサン結合が三次元網目状に架橋した構造を有する、エポキシ樹脂組成物。 It contains (A) epoxy resin, (B) resin having aromatic rings and hydroxyl groups, (C) silicone powder, (D) curing accelerator, and (E) inorganic filler.
The epoxy resin (A) contains an epoxy resin that is liquid at 25 ° C.
The resin having the aromatic ring and the hydroxyl group (B) contains a resin having a naphthalene ring and a hydroxyl group.
The content of the epoxy resin liquid at 25 ° C. is 32% by mass or more based on the total amount of the (A) epoxy resin and the (B) resin having an aromatic ring and a hydroxyl group.
The content of the silicone powder (C) is 0.80 to 7.30% by mass based on the total amount of the epoxy resin composition (however, when the epoxy resin composition contains a solvent, the solvent is excluded). der is,
The (A) epoxy resin is at least one selected from the group consisting of bisphenol A type epoxy resin, bisphenol F type epoxy resin and naphthalene type epoxy resin.
An epoxy resin composition in which the silicone powder (C) has a structure in which siloxane bonds are crosslinked in a three-dimensional network .
［式（Ｉ）中、Ｒ１１、Ｒ１２、Ｒ１３、Ｒ１４及びＲ１５は、それぞれ独立に水素原子、炭素数１〜６のアルキル基又は炭素数１〜２のアルコキシ基を示し、ｍ１、ｍ２、ｍ３、ｍ４、ｍ５、ｍ６、ｍ７及びｍ８は、それぞれ独立に０〜２の整数を示し（但し、ｍ１、ｍ２、ｍ３、ｍ４、ｍ５、ｍ６、ｍ７及びｍ８の全てが０である場合を除く）、ｎ１は、０〜１０の整数を示す。］ The epoxy resin composition according to claim 1, wherein the resin having a naphthalene ring and a hydroxyl group contains a compound represented by the following general formula (I).
[In formula (I), R 11 , R 12 , R 13 , R 14 and R 15 each independently represent a hydrogen atom, an alkyl group having 1 to 6 carbon atoms or an alkoxy group having 1 to 2 carbon atoms, and m1 , M2, m3, m4, m5, m6, m7 and m8 each independently indicate an integer of 0 to 2 (provided that m1, m2, m3, m4, m5, m6, m7 and m8 are all 0s. (Except for cases), n1 represents an integer from 0 to 10. ]
前記封止部が、請求項１〜３のいずれか一項に記載のエポキシ樹脂組成物若しくはその硬化物、又は、請求項４に記載のフィルム状エポキシ樹脂組成物を含む、電子装置。
A sealed body of at least one selected from the group consisting of electronic components and electronic devices, and a sealing portion for sealing the sealed body are provided.
An electronic device in which the sealing portion includes the epoxy resin composition according to any one of claims 1 to 3 or a cured product thereof, or the film-shaped epoxy resin composition according to claim 4 .
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| TWI728992B (en) | 2021-06-01 |
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