JP2019019231A - Resin composition - Google Patents

Abstract

An object of the present invention is to provide a resin composition capable of suppressing aggregation of carbon black while maintaining properties such as color development, minimum melt viscosity and glass transition temperature. (A) an epoxy resin, (B) an inorganic filler, (C) a carbon black having a DBP absorption of 130 cm3 / 100 g or less, and (D) a polymer resin having a glass transition temperature of 30 ° C. or less. And a resin composition. [Selection diagram] Fig. 1

Description

  The present invention relates to a resin composition. Furthermore, this invention relates to the resin sheet, circuit board, and semiconductor chip package which are obtained using the said resin composition.

  In recent years, electronic devices are becoming smaller and higher performance. Along with this, in the semiconductor package substrate, the build-up layer is multilayered, and miniaturization and high density of wiring are required. In addition, with the spread of smartphones and tablet devices, there is an increasing demand for thinning. Therefore, there is a demand for a thin package substrate in which the core material is thinned or a coreless structure is adopted. In order to realize such a thin package substrate, the insulating layer is required to have high insulation properties even if it is thin.

  On the other hand, the insulating layer may be required to contain carbon black due to its coloring. For example, Patent Document 1 discloses a resin composition containing carbon black as a smear suppressing component. Patent Document 2 discloses a resin composition containing a polymer resin having a glass transition temperature of 30 ° C. or lower.

JP 2014-005464 A JP 2014-095047 A

  In order to increase the glass transition temperature of the insulating layer and improve the heat resistance, the present inventors tried to blend an inorganic filler into the resin composition. In addition, the present inventors formulated a polymer resin having a glass transition temperature of 30 ° C. or lower in the resin composition in order to improve the laminate property of the resin sheet by adjusting the melt viscosity of the resin composition to an appropriate value. Tried to do. And the present inventors examined in order to improve the physical property balance in the resin composition containing these inorganic fillers and polymer resins in combination.

  In this study, the present inventors have found that when such a resin composition is used for coloring with carbon black, carbon black may be aggregated. According to the study by the present inventors, the aggregation of carbon black as described above is considered to be caused by the difference in compatibility between the carbon black, the inorganic filler, and the polymer resin.

  When the carbon black aggregates, the color of the insulating layer is affected by the aggregation and a desired color tone may not be obtained. In addition, if carbon black defects are generated as aggregates that can be visually recognized due to aggregation of carbon black, even if there is no problem in the quality of the resin composition, the commercial value may be evaluated low.

  The present invention was devised in view of the above problems, and is a resin composition capable of suppressing the aggregation of carbon black while being balanced in characteristics such as color development, minimum melt viscosity, and glass transition temperature; A resin sheet having a resin composition layer containing a product; a circuit board including an insulating layer formed of a cured product of the resin composition; and a semiconductor chip package including a cured product of the resin composition; For the purpose.

The present inventors diligently studied to solve the above problems. As a result, (A) an epoxy resin, (B) an inorganic filler, (C) a carbon black having a DBP absorption amount of a predetermined value or less, and (D) a polymer resin having a glass transition temperature of 30 ° C. or less. The present inventors have found that a resin composition containing it can solve the above-mentioned problems, and have completed the present invention.
That is, the present invention is as follows.

[1] (A) an epoxy resin, (B) a mineral filler, (C) DBP absorption amount is less 130 cm ^3/100 g carbon black, and, (D) a glass transition temperature of 30 ° C. or less of the polymeric resin A resin composition comprising.
[2] The resin composition according to [1], wherein the amount of the component (B) is 30% by mass or more and 95% by mass or less with respect to 100% by mass of the nonvolatile component in the resin composition.
[3] The resin composition according to [1] or [2], wherein the amount of the component (B) is 75% by mass to 95% by mass with respect to 100% by mass of the nonvolatile component in the resin composition.
[4] The resin composition according to any one of [1] to [3], wherein the component (A) includes (A-1) a nitrogen-containing epoxy resin or an epoxy resin having a condensed ring structure.
[5] The component (D) is selected from the group consisting of a polybutadiene structure, a polysiloxane structure, a polyalkylene structure, a polyalkyleneoxy structure, a polyisoprene structure, a polyisobutylene structure, a polycarbonate structure, and a polyacrylic structure in the molecule. The resin composition according to any one of [1] to [4], which has one or more types of structures.
[6] The resin composition according to any one of [1] to [5], wherein the component (D) has a functional group capable of reacting with the component (A).
[7] The component (D) has one or more functional groups selected from the group consisting of a hydroxyl group, an acid anhydride group, a phenolic hydroxyl group, an epoxy group, an isocyanate group, and a urethane group. [6] The resin composition according to any one of [6].
[8] The resin composition according to any one of [1] to [7], wherein the number average molecular weight of the component (D) is from 4,000 to 100,000.
[9] Any one of [1] to [8], wherein the amount of the component (D) is 0.2% by mass or more and 20% by mass or less with respect to 100% by mass of the non-volatile component in the resin composition. The resin composition described in 1.
[10] Any one of [1] to [9], wherein the amount of the component (C) is 0.1% by mass or more and 3% by mass or less with respect to 100% by mass of the nonvolatile component in the resin composition. The resin composition described in 1.
[11] The resin composition according to any one of [1] to [10], which is a resin composition for an insulating layer of a semiconductor chip package.
[12] The resin composition according to any one of [1] to [11], which is a resin composition for semiconductor encapsulation.
[13] A resin sheet comprising a support and a resin composition layer comprising the resin composition according to any one of [1] to [12] provided on the support.
[14] The resin sheet according to [13], which is a resin sheet for an insulating layer of a semiconductor chip package.
[15] A circuit board comprising an insulating layer formed of a cured product of the resin composition according to any one of [1] to [12].
[16] A semiconductor chip package comprising the circuit board according to [15] and a semiconductor chip mounted on the circuit board.
[17] A semiconductor chip package comprising a semiconductor chip and a cured product of the resin composition according to any one of [1] to [12] for sealing the semiconductor chip.

  According to the present invention, a resin composition capable of suppressing aggregation of carbon black while being balanced in characteristics such as color development, minimum melt viscosity, and glass transition temperature; a resin having a resin composition layer containing the resin composition described above A sheet; a circuit board including an insulating layer formed of a cured product of the resin composition; and a semiconductor chip package including a cured product of the resin composition can be provided.

FIG. 1 is a cross-sectional view schematically showing a Fan-out type WLP as an example of a semiconductor chip package according to a second embodiment of the present invention.

  Hereinafter, the present invention will be described in detail with reference to embodiments and examples. However, the present invention is not limited to the following embodiments and exemplifications, and can be implemented with any modifications without departing from the scope of the claims of the present invention and the equivalents thereof.

[1. Outline of Resin Composition]
The resin composition of the present invention includes (A) an epoxy resin, (B) an inorganic filler, (C) carbon black having a DBP absorption amount of a predetermined value or less, and (D) a high glass transition temperature of 30 ° C. or less. Contains molecular resin. In the following description, “carbon black whose DBP absorption amount is a predetermined value or less” as the component (C) may be referred to as “(C) carbon black”. In the following description, “polymer resin having a glass transition temperature of 30 ° C. or lower” as component (D) may be referred to as “(D) polymer resin”.

  By including a combination of the above (A) epoxy resin, (B) inorganic filler, (C) carbon black and (D) polymer resin, the resin composition has a color development, minimum melt viscosity, glass transition temperature, etc. It is possible to obtain the desired effect of the present invention that the aggregation of carbon black can be suppressed while the properties are balanced. Such a cured product of the resin composition can be preferably used as an insulating layer and a sealing material of a semiconductor chip package, taking advantage of its excellent characteristics.

  Moreover, the said resin composition may contain arbitrary components further combining with (A) epoxy resin, (B) inorganic filler, (C) carbon black, and (D) polymer resin. Examples of the optional component include (E) a curing agent, (F) a curing accelerator, (G) a thermoplastic resin, (H) a flame retardant, and the like.

[2. (A) Epoxy resin]
The resin composition of the present invention contains an epoxy resin as the component (A). (A) The epoxy resin usually has an epoxy group in the molecule. (A) The number of epoxy groups per molecule of the epoxy resin is usually 1 or more, preferably 2 or more. From the viewpoint of remarkably obtaining the desired effect of the present invention, the ratio of the epoxy resin having two or more epoxy groups in one molecule with respect to 100% by mass of the nonvolatile component (A) of the epoxy resin is preferably 50 masses. % Or more, more preferably 60% by mass or more, and particularly preferably 70% by mass or more.

  (A) As an epoxy resin, for example, bixylenol type epoxy resin; fluorine-containing epoxy resin such as bisphenol AF type epoxy resin and perfluoroalkyl type epoxy resin; bisphenol A type epoxy resin; bisphenol F type epoxy resin; bisphenol S Type epoxy resin; bisphenol AF type epoxy resin; dicyclopentadiene type epoxy resin; trisphenol type epoxy resin; naphthol novolac type epoxy resin; phenol novolac type epoxy resin; tert-butyl-catechol type epoxy resin; naphthalene type epoxy resin; Type epoxy resin; anthracene type epoxy resin; glycidyl amine type epoxy resin; glycidyl ester type epoxy resin; cresol novolac type epoxy resin; Nyl type epoxy resin; Linear aliphatic epoxy resin; Epoxy resin having butadiene structure; Alicyclic epoxy resin; Heterocyclic epoxy resin; Spiro ring-containing epoxy resin; Cyclohexane type epoxy resin; Cyclohexane dimethanol type epoxy resin; Examples include renether type epoxy resins; trimethylol type epoxy resins; tetraphenylethane type epoxy resins; and phosphorus-containing epoxy resins. (A) An epoxy resin may be used individually by 1 type, and may be used in combination of 2 or more types.

  (A) The epoxy resin preferably includes (A-1) a nitrogen-containing epoxy resin or an epoxy resin having a condensed ring structure. As the component (A-1), only a nitrogen-containing epoxy resin may be used, only an epoxy resin having a condensed ring structure may be used, or a combination of a nitrogen-containing epoxy resin and an epoxy resin having a condensed ring structure is used. May be. When the (A) epoxy resin contains the component (A-1), the desired effect of the present invention can be remarkably exhibited, and in particular, the glass transition temperature of the cured product of the resin composition can be effectively increased. Thus, the effect | action which can raise a glass transition temperature is remarkable when (A-1) component and (D) polymeric resin are combined. Furthermore, the (A-1) component can usually improve the shear strength, break bending strain, and crackability of the cured product of the resin composition.

  The nitrogen-containing epoxy resin is an epoxy resin containing a nitrogen atom in the molecule. Examples of preferable nitrogen-containing epoxy resins include glycidylamine type epoxy resins and aminophenol type epoxy resins.

  Specific examples of the nitrogen-containing epoxy resin include “630” and “630LSD” (glycidylamine type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “EP-3950S”, “EP-3950L”, and “EP-3980S” manufactured by ADEKA. (Glycidylamine type epoxy resin); Nippon Kayaku Co., Ltd. “GAN”, “GOT” (glycidylamine type epoxy resin); Sumitomo Chemical Co., Ltd. “ELM-100” (glycidylamine type epoxy resin); It is done. These may be used alone or in combination of two or more.

  The epoxy resin having a condensed ring structure is an epoxy resin having a condensed ring structure in the molecule. Preferred epoxy resins having a condensed ring structure include, for example, naphthalene type epoxy resins, naphthalene type tetrafunctional epoxy resins, naphthol type epoxy resins, naphthylene ether type epoxy resins, anthracene type epoxy resins, and dicyclopentadiene type epoxy resins. It is done. Among these, naphthalene type epoxy resins, naphthalene type tetrafunctional epoxy resins, naphthol type epoxy resins, naphthylene ether type epoxy resins, and dicyclopentadiene type epoxy resins are more preferable, and naphthalene type epoxy resins and naphthol type epoxy resins are more preferable.

  Specific examples of the epoxy resin having a condensed ring structure include “HP4032” and “HP4032SS” (naphthalene type epoxy resin) manufactured by DIC; “HP-4700” and “HP-4710” (naphthalene type 4) manufactured by DIC. (Functional epoxy resin); “HP-7200H”, “HP-7200”, “HP-7200L” (dicyclopentadiene type epoxy resin) manufactured by DIC; “EXA7311”, “EXA7311-G3”, “made by DIC” "EXA7311-G4", "EXA7311-G4S", "HP6000" (naphthylene ether type epoxy resin); "NC7000L" (naphthol novolak type epoxy resin) manufactured by DIC; "ESN475V" (naphthol type manufactured by Nippon Steel & Sumikin Chemical Co., Ltd.) Epoxy resin); “ESN485 manufactured by Nippon Steel & Sumikin Chemical Co., Ltd. (Naphthol novolac type epoxy resin); “YX8800” (anthracene type epoxy resin) manufactured by Nippon Steel & Sumikin Chemical; “PG-100” and “CG-500” (fluorene type epoxy resin) manufactured by Osaka Gas Chemical; “YL7800” (fluorene type epoxy resin) manufactured by the company; “YX8800” (anthracene type epoxy resin) manufactured by Mitsubishi Chemical Corporation; and the like. These may be used alone or in combination of two or more.

  When the nitrogen-containing epoxy resin and the epoxy resin having a condensed ring structure are used in combination as the component (A-1), it is preferable that the quantitative ratio thereof falls within a predetermined range. Specifically, the mass ratio of “nitrogen-containing epoxy resin: epoxy resin having a condensed ring structure” is preferably 1: 0.1 to 1:10, more preferably 1: 0.3 to 1: 5, and further Preferably it is 1: 0.6-1: 2.5. By setting the amount ratio of the nitrogen-containing epoxy resin and the epoxy resin having a condensed ring structure in such a range, the heat resistance of the cured product of the resin composition can be effectively increased.

  The amount of the component (A-1) in the resin composition is preferably 0.5% by mass or more, more preferably 0.8% by mass or more, and particularly preferably with respect to 100% by mass of the nonvolatile component of the resin composition. 1.0 mass% or more, preferably 10 mass% or less, more preferably 8 mass% or less, and particularly preferably 5 mass% or less. When the amount of the component (A-1) is in the above range, the desired effect of the present invention can be remarkably obtained. Furthermore, usually, the shear strength, fracture bending strain, and crack resistance of the cured product of the resin composition can be improved.

  The (A) epoxy resin preferably further contains an epoxy resin that is liquid at 25 ° C. (A-2) other than the component (A-1) in combination with the component (A-1). The component (A-2) does not include a nitrogen-containing epoxy resin that is liquid at 25 ° C. and an epoxy resin that has a condensed ring structure that is liquid at 25 ° C. By using the component (A-2) in combination with the component (A-1), the desired effect of the present invention can be remarkably obtained.

  The epoxy resin that is liquid at 25 ° C. as the component (A-2) preferably has two or more epoxy groups in one molecule. The epoxy resin that is liquid at 25 ° C. as the component (A-2) is preferably an aromatic epoxy resin having an aromatic ring in the molecule. Here, the term “aromatic ring” includes not only a single aromatic ring but also a polycyclic aromatic ring and an aromatic heterocyclic ring.

  As the component (A-2), bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol AF type epoxy resin, glycidyl ester type epoxy resin, phenol novolac type epoxy resin, alicyclic epoxy resin having an ester skeleton, cyclohexane Type epoxy resin, cyclohexanedimethanol type epoxy resin, aliphatic epoxy resin, and epoxy resin having a butadiene structure. Among these, from the viewpoint of remarkably obtaining the desired effect of the present invention, bisphenol A type epoxy resin, bisphenol F type epoxy resin, and bisphenol AF type epoxy resin are preferable, and bisphenol A type epoxy resin and bisphenol F type epoxy resin are more preferable. .

  Specific examples of the component (A-2) include “828US” and “jER828EL” (bisphenol A type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “JER806” and “jER807” (bisphenol F type epoxy resin manufactured by Mitsubishi Chemical Corporation). ); “JER152” (phenol novolac type epoxy resin) manufactured by Mitsubishi Chemical Corporation; “ZX1059” (mixed product of bisphenol A type epoxy resin and bisphenol F type epoxy resin) manufactured by Nippon Steel & Sumikin Chemical Co., Ltd .; manufactured by Nagase ChemteX Corporation “EX-721” (glycidyl ester type epoxy resin); “Celoxide 2021P” (alicyclic epoxy resin having an ester skeleton) manufactured by Daicel; “ZX1658”, “ZX1658GS” (liquid 1) manufactured by Nippon Steel Chemical Co., Ltd. , 4-glycidylcyclohexane); “YX740” manufactured by Mitsubishi Chemical Corporation "(Epoxy resin having a flexible aliphatic backbone); and the like. These may be used alone or in combination of two or more.

  (A) When an epoxy resin contains the (A-1) component and the (A-2) component in combination, it is preferable that those quantitative ratios fall in a predetermined range. Specifically, the mass ratio of “component (A-1): component (A-2)” is preferably 1: 0.1 to 1:10, more preferably 1: 0.1 to 1: 8. More preferably, it is 1: 0.1 to 1: 6. By setting the mass ratio of the component (A-1) to the component (A-2) within such a range, the desired effect of the present invention can be remarkably obtained. Moreover, normally, the shear strength of the hardened | cured material of a resin composition, breaking bending distortion, and crackability can be made favorable.

  When the (A) epoxy resin contains the component (A-2), the amount of the component (A-2) is preferably 0.5% by mass or more, more preferably 100% by mass of the nonvolatile component of the resin composition. Is 1% by mass or more, more preferably 2% by mass or more, preferably 10% by mass or less, more preferably 8% by mass or less, and further preferably 6% by mass or less. When the amount of the component (A-2) is in the above range, the desired effect of the present invention can be remarkably obtained. Furthermore, the crack resistance of the cured product of the resin composition can usually be improved.

  (A) The epoxy resin is combined with the component (A-1) and the component (A-2), and (A-3) any epoxy resin other than the component (A-1) and the component (A-2). May be included. As such component (A-3), a solid epoxy resin at 20 ° C. is preferable. The epoxy resin that is solid at 20 ° C. preferably has three or more epoxy groups in one molecule. Furthermore, the component (A-3) is preferably an aromatic epoxy resin having an aromatic ring in the molecule.

  Preferred examples of the component (A-3) include a cresol novolac type epoxy resin, a trisphenol type epoxy resin, a biphenyl type epoxy resin, a bisphenol A type epoxy resin, a bisphenol AF type epoxy resin, and a tetraphenylethane type epoxy resin. . Among these, biphenyl type epoxy resins are preferable from the viewpoint of remarkably obtaining the desired effect of the present invention.

  Specific examples of the component (A-3) include “N-690” (cresol novolac type epoxy resin) and “N-695” (cresol novolak type epoxy resin) manufactured by DIC; “EPPN” manufactured by Nippon Kayaku Co., Ltd. -502H "(trisphenol type epoxy resin)," YX4000HK "(bixylenol type epoxy resin)," YL7760 "(bisphenol AF type epoxy resin)," NC3000L "(biphenyl type epoxy resin);" jER1010 "manufactured by Mitsubishi Chemical Corporation (Solid bisphenol A type epoxy resin), “jER1031S” (tetraphenylethane type epoxy resin), “157S70” (bisphenol novolac type epoxy resin), “jER1031S” (tetraphenylethane type epoxy resin); . These may be used alone or in combination of two or more.

  When the (A) epoxy resin contains the component (A-3), the amount of the component (A-3) is preferably 0.5% by mass or more with respect to 100% by mass of the nonvolatile component in the resin composition. Preferably it is 1 mass% or more, More preferably, it is 2 mass% or more, Preferably it is 10 mass% or less, More preferably, it is 8 mass% or less, More preferably, it is 6 mass% or less. When the amount of the component (A-3) is in the above range, the desired effect of the present invention can be remarkably obtained. Furthermore, normally, the mechanical strength and insulation reliability of the cured product of the resin composition can be improved.

  The amount of the whole (A) epoxy resin including the components (A-1) to (A-3) described above is preferably 0.5% by mass or more with respect to 100% by mass of the nonvolatile component of the resin composition. Preferably it is 1 mass% or more, Especially preferably, it is 3 mass% or more, Preferably it is 30 mass% or less, More preferably, it is 20 mass% or less, More preferably, it is 15 mass% or less. (A) When the amount of the epoxy resin is within the above range, the desired effect of the present invention can be remarkably obtained.

  (A) The epoxy equivalent of an epoxy resin becomes like this. Preferably it is 50-5000, More preferably, it is 50-3000, More preferably, it is 80-2000, More preferably, it is 110-1000. By becoming this range, the crosslinked density of the hardened | cured material of a resin composition becomes enough, and when using hardened | cured material as an insulating layer, an insulating layer with small surface roughness can be brought about. In addition, the epoxy equivalent of (A) component can be measured according to JISK7236, and is the mass of resin containing 1 equivalent of epoxy groups.

  (A) The weight average molecular weight of an epoxy resin becomes like this. Preferably it is 100-5000, More preferably, it is 250-3000, More preferably, it is 400-1500. Here, the weight average molecular weight of the liquid epoxy resin is a weight average molecular weight in terms of polystyrene measured by a gel permeation chromatography (GPC) method.

  (A) The number average molecular weight of an epoxy resin becomes like this. Preferably it is less than 4000, More preferably, it is 3500 or less, More preferably, it is 3000 or less. The lower limit is preferably 500 or more, more preferably 1000 or more, and further preferably 1500 or more. The number average molecular weight (Mn) is a number average molecular weight in terms of polystyrene measured using a gel permeation chromatography method.

[3. (B) Inorganic filler]
The resin composition of the present invention contains an inorganic filler as the component (B). (B) By using an inorganic filler, the heat resistance of the resin composition can be improved. Furthermore, since the thermal expansion coefficient of the cured product of the resin composition can be normally reduced by using the (B) inorganic filler, warpage can be suppressed. Furthermore, (B) the inorganic filler can usually improve the insulating performance and sealing performance of the cured product of the resin composition.

  As the material for the inorganic filler, an inorganic material is usually used, and an inorganic compound is preferably used. (B) Examples of inorganic filler materials include silica, alumina, glass, cordierite, silicon oxide, barium sulfate, barium carbonate, talc, clay, mica powder, zinc oxide, hydrotalcite, boehmite, and water. Aluminum oxide, magnesium hydroxide, calcium carbonate, magnesium carbonate, magnesium oxide, boron nitride, aluminum nitride, manganese nitride, aluminum borate, strontium carbonate, strontium titanate, calcium titanate, magnesium titanate, bismuth titanate, titanium oxide , Zirconium oxide, barium titanate, barium zirconate titanate, barium zirconate, calcium zirconate, zirconium phosphate, and zirconium tungstate phosphate. Among these, silica is particularly preferable from the viewpoint of remarkably obtaining the desired effect of the present invention. As silica, spherical silica is preferable. Moreover, (B) inorganic filler may be used individually by 1 type, and may be used in combination of 2 or more types.

  Usually, the (B) inorganic filler is contained in the resin composition in the form of particles. (B) The average particle size of the inorganic filler is preferably 0.01 μm or more, more preferably 0.05 μm or more, still more preferably 0.1 μm or more, and preferably 5 μm or less, more preferably 2.5 μm. Hereinafter, it is further preferably 2.2 μm or less, particularly preferably 2 μm or less. (B) When the average particle diameter of the inorganic filler is in the above range, the desired effect of the present invention can be remarkably obtained, and more usually, an insulating layer having a low surface roughness can be obtained.

  (B) The average particle diameter of the inorganic filler can be measured by a laser diffraction / scattering method based on Mie scattering theory. Specifically, the particle size distribution of (B) inorganic filler is created on a volume basis by a laser diffraction scattering type particle size distribution measuring device, and the average particle size can be measured as the median diameter from the particle size distribution. As the measurement sample, (B) an inorganic filler dispersed in a solvent such as water by ultrasonic waves can be preferably used. As the laser diffraction / scattering particle size distribution measuring apparatus, “LA-500” manufactured by Horiba, Ltd. or the like can be used.

  Examples of the inorganic filler (B) described above include “YC100C”, “YA050C”, “YA050C-MJE”, “YA010C” manufactured by Admatechs Corporation; “UFP-30” manufactured by Denki Kagaku Kogyo Co., Ltd .; “Silfil NSS-3N”, “Silfil NSS-4N”, “Silfil NSS-5N” manufactured by Admatechs Co., Ltd. “SC2500SQ”, “SO-C6”, “SO-C4”, “SO-C2”, “SO” -C1 "; and the like.

  (B) It is preferable that the inorganic filler is surface-treated with an appropriate surface treatment agent. By performing the surface treatment, the moisture resistance and dispersibility of the inorganic filler (B) can be enhanced. Examples of surface treatment agents include fluorine-containing silane coupling agents, aminosilane coupling agents, epoxysilane coupling agents, mercaptosilane coupling agents, silane coupling agents, alkoxysilane compounds, organosilazane compounds, and titanates. System coupling agents and the like.

  Examples of commercially available surface treatment agents include “KBM22” (dimethyldimethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., “KBM403” (3-glycidoxypropyltrimethoxysilane) manufactured by Shin-Etsu Chemical Co., Ltd., and manufactured by Shin-Etsu Chemical Co., Ltd. "KBM803" (3-mercaptopropyltrimethoxysilane), Shin-Etsu Chemical "KBE903" (3-aminopropyltriethoxysilane), Shin-Etsu Chemical "KBM573" (N-phenyl-3-aminopropyltrimethoxy) Silane), Shin-Etsu Chemical Co., Ltd. “SZ-31” (hexamethyldisilazane), Shin-Etsu Chemical Co., Ltd. “KBM103” (phenyltrimethoxysilane), Shin-Etsu Chemical Co., Ltd. “KBM-4803” (long-chain epoxy type) Silane coupling agent). Moreover, a surface treating agent may be used individually by 1 type, and may be used in combination of 2 or more types.

  The amount of the (B) inorganic filler in the resin composition is preferably 30% by mass or more, more preferably 50% by mass or more, and still more preferably 75% by mass with respect to 100% by mass of the nonvolatile component in the resin composition. It is above, Preferably it is 95 mass% or less, More preferably, it is 93 mass% or less, More preferably, it is 90 mass% or less. (B) When the quantity of an inorganic filler exists in the said range, the desired effect of this invention can be acquired notably. Moreover, normally, the amount of the inorganic filler (B) is not less than the lower limit value of the above range, so that the thermal expansion coefficient of the cured product of the resin composition can be lowered, and is not more than the upper limit value of the above range. As a result, the mechanical strength of the resin composition, particularly the elongation, can be improved.

[4. (C) Carbon black]
The resin composition of the present invention contains carbon black having a DBP absorption amount of a predetermined value or less as the component (C). (C) Specific DBP absorption of carbon black is usually 130 cm ^3/100 g or less, preferably 100 cm ^3/100 g or less, particularly preferably not more than 80 cm ^3/100 g. As described above, (C) carbon black having a small DBP absorption amount suppresses aggregation of the (C) carbon black when combined with (A) an epoxy resin, (B) an inorganic filler, and (D) a polymer resin. it can. Further, the properties of the resin composition containing (C) carbon black and the cured product thereof (the minimum melt viscosity of the resin composition, the color of the cured product of the resin composition, the glass transition temperature, etc.) The characteristics of the resin composition obtained by combining black with (A) an epoxy resin, (B) an inorganic filler, and (D) a polymer resin are excellent to the same extent or more. Therefore, by using (C) carbon black, it is possible to realize a resin composition capable of suppressing the aggregation of carbon black while being balanced in characteristics such as color development, minimum melt viscosity and glass transition temperature. In view of the tendency that carbon black generally tends to aggregate in a resin composition containing (B) an inorganic filler and (D) a polymer resin, the above action is surprising to those skilled in the art. (C) the lower limit of the DBP absorption of carbon black is no particular restriction is not, for ^example, 10 cm 3/100 g or ^more, 20 cm 3/100 g or ^more, may be 40 cm 3/100 g or more.

  (C) The DBP absorption amount of carbon black can be measured by the method defined in JIS K 6217-4: 2017. The DBP absorption amount is a physical property value affected by factors such as the type and amount of functional groups on the surface of carbon black and the specific surface area of carbon black, and this DBP absorption amount is determined by (B) inorganic filler and ( D) It has not been known in the past that there is a correlation between the dispersibility of (C) carbon black mixed with a polymer resin.

  (C) The average particle diameter of carbon black is preferably 5 nm or more, more preferably 10 nm or more, particularly preferably 15 nm or more, preferably 300 nm or less, more preferably 100 nm or less, and particularly preferably 50 nm or less. Generally, carbon black having a small average particle size tends to cause aggregation. However, in the resin composition of the present invention, aggregation can usually be suppressed even when (C) carbon black is small. Therefore, from the viewpoint of effectively utilizing the effects of the present invention, it is preferable to use (C) carbon black having a small average particle diameter as described above. Further, by using (C) carbon black having a small average particle diameter as described above, the color of the cured product of the resin composition can be easily adjusted.

  The average particle diameter of the (C) carbon black represents not the average particle diameter of the secondary particles in which a plurality of (C) carbon blacks are collected, but the average particle diameter of primary particles of the individual (C) carbon black. The average particle diameter of (C) carbon black can be determined as the arithmetic average diameter of (C) carbon black observed with an electron microscope.

  The pH of (C) carbon black is preferably 1.0 or more, more preferably 2.0 or more, particularly preferably 3.0 or more, preferably 7.0 or less, more preferably 6.0 or less, particularly Preferably it is 4.0 or less. By using (C) carbon black having a pH in such a range, the desired effect of the present invention can be remarkably obtained, and in particular, aggregation of (C) carbon black can be effectively suppressed.

  (C) The pH of carbon black can be measured by the method prescribed | regulated to JISK5101-17-2: 2004.

  (C) As the carbon black, commercially available carbon black may be used as it is, or a plurality of commercially available products may be appropriately mixed so that physical property values such as DBP absorption amount are within a predetermined range. Commercially available products of carbon black can be obtained from, for example, Mitsubishi Chemical Corporation, Tokai Carbon Co., Asahi Carbon Co., Ltd., Nippon Chemical Co., Ltd., Nippon Pigment Co., Toyocolor Co., Ltd., and Gokoku Color Co., Ltd.

  The amount of (C) carbon black in the resin composition is preferably 0.1% by mass or more, more preferably 0.15% by mass or more, particularly preferably 100% by mass of the nonvolatile component in the resin composition. It is 0.2% by mass or more, preferably 3% by mass or less, more preferably 2.5% by mass or less, and particularly preferably 2% by mass or less. (C) When the amount of carbon black is within the above range, the desired effect of the present invention can be remarkably obtained. In particular, when the amount of (C) carbon black is not less than the lower limit of the above range, the cured product of the resin composition can be appropriately colored, and the amount of (C) carbon black is not more than the upper limit of the above range. (C) Aggregation of carbon black can be particularly effectively suppressed.

[5. (D) Polymer resin]
The resin composition of the present invention contains a polymer resin having a glass transition temperature of 30 ° C. or lower as the component (D). By using the component (D), the minimum melt viscosity of the resin composition can be lowered. Therefore, normally, the laminating property of the resin sheet provided with the resin composition layer can be improved. Specifically, the glass transition temperature of (D) the polymer resin is usually 30 ° C. or lower, preferably 20 ° C. or lower, more preferably 10 ° C. or lower. Although the lower limit of a glass transition temperature is not specifically limited, For example, it may be -30 degreeC or more. Moreover, since the elastic modulus of the cured product of the resin composition can usually be lowered by using the polymer resin (D), the peel strength of the sealing layer and the insulating layer formed of the cured product can be improved. . In addition, (D) the polymer resin usually has a linear thermal expansion coefficient that hardly changes in a wide temperature range of 25 ° C. to 220 ° C., so that the dimensional stability of the cured product of the resin composition can be enhanced.

  (D) The polymer resin is selected from the group consisting of polybutadiene structure, polysiloxane structure, polyalkylene structure, polyalkyleneoxy structure, polyisoprene structure, polyisobutylene structure, polycarbonate structure, and polyacrylic structure in the molecule. Preferred are compounds having one or more structures. By using the (D) polymer resin having such a structure, the desired effect of the present invention can be remarkably obtained. Moreover, since the (D) polymer resin having such a structure is usually excellent in flexibility, the minimum melt viscosity of the resin composition can be effectively reduced. Furthermore, when combined with the (D) polymer resin having such a structure, carbon black generally tends to aggregate, but the above-mentioned (C) carbon black hardly causes aggregation. Therefore, from the viewpoint of utilizing the effect that (C) the aggregation of carbon black can be effectively suppressed, (D) the polymer resin preferably has a compound having the above structure in its molecule. Among these, from the viewpoint of more effectively exerting the above-described effects, a polybutadiene structure, a polysiloxane structure, a polyisoprene structure, a polyisobutylene structure, a polycarbonate structure, and a polyacrylic structure are preferable, and a polybutadiene structure, a polyisoprene structure, and a polycarbonate structure are preferable. More preferred are a polybutadiene structure and a polycarbonate structure.

  The polybutadiene structure includes not only a structure formed by polymerizing butadiene but also a structure formed by hydrogenating the structure. Moreover, only a part of the butadiene structure may be hydrogenated, or all of it may be hydrogenated. Furthermore, the polybutadiene structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. Hereinafter, the resin having a polybutadiene structure in the molecule may be referred to as a “butadiene resin”. The butadiene resin is preferably a butadiene resin that is liquid at 25 ° C. or has a glass transition temperature of 25 ° C. or lower.

  The polysiloxane structure is a structure including a siloxane bond, and is included in, for example, silicone rubber. The polysiloxane structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. Hereinafter, a resin having a polysiloxane structure in the molecule may be referred to as a “siloxane resin”.

  The polyalkylene structure preferably has a predetermined number of carbon atoms. The specific number of carbon atoms of the polyalkylene structure is preferably 2 or more, more preferably 3 or more, particularly preferably 5 or more, preferably 15 or less, more preferably 10 or less, and particularly preferably 6 or less. The polyalkylene structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. The resin having a polyalkylene structure in the molecule may be hereinafter referred to as “alkylene resin”.

  The polyalkyleneoxy structure preferably has a predetermined number of carbon atoms. The specific number of carbon atoms of the polyalkyleneoxy structure is preferably 2 or more, preferably 3 or more, more preferably 5 or more, preferably 15 or less, more preferably 10 or less, and particularly preferably 6 or less. The polyalkyleneoxy structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. The resin having a polyalkyleneoxy structure in the molecule may be hereinafter referred to as “alkyleneoxy resin”.

  The polyisoprene structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. Hereinafter, a resin having a polyisoprene structure in the molecule may be referred to as an “isoprene resin”.

  The polyisobutylene structure may be contained in the main chain or the side chain in the molecule (D) of the polymer resin. Hereinafter, a resin having a polyisobutylene structure in the molecule may be referred to as an “isobutylene resin”.

  The polycarbonate structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. Hereinafter, a resin having a polycarbonate structure in the molecule may be referred to as a “carbonate resin”. As the carbonate resin, a carbonate resin having a glass transition temperature of 25 ° C. or lower is preferable.

  The polyacrylic structure is a structure formed by polymerizing a compound (acrylate, methacrylate, etc.) containing at least one of acryloyl group and methacryloyl group with the acryloyl group or methacryloyl group. The polyacrylic structure may be contained in the main chain or in the side chain in the molecule (D) of the polymer resin. Hereinafter, the resin having a polyacrylic structure in the molecule may be referred to as “acrylic resin”. As the acrylic resin, an acrylic resin having a glass transition temperature of 25 ° C. or lower is preferable.

  The (D) polymer resin preferably has a functional group capable of reacting with the (A) epoxy resin. This functional group includes a reactive group that appears upon heating. (D) When the polymer resin has the functional group, the mechanical strength of the cured product of the resin composition can be improved.

  Examples of the functional group include a hydroxy group, a carboxy group, an acid anhydride group, a phenolic hydroxyl group, an epoxy group, an isocyanate group, and a urethane group. Among these, from the viewpoint of remarkably obtaining the effects of the present invention, the functional group is one or more selected from the group consisting of a hydroxyl group, an acid anhydride group, a phenolic hydroxyl group, an epoxy group, an isocyanate group, and a urethane group. Are preferred, and phenolic hydroxyl groups are particularly preferred.

  (D) The polymer resin preferably has an imide structure. By having an imide structure, the heat resistance of the (D) polymer resin can be effectively increased.

  (D) A preferred example of the polymer resin is a butadiene resin. Preferred examples of butadiene resins include hydrogenated polybutadiene skeleton-containing resins, hydroxy group-containing butadiene resins, phenolic hydroxyl group-containing butadiene resins, carboxy group-containing butadiene resins, acid anhydride group-containing butadiene resins, epoxy group-containing butadiene resins, and isocyanate groups. Butadiene resin containing, urethane group-containing butadiene resin. Among these, phenolic hydroxyl group-containing butadiene resins are more preferable. Here, the “hydrogenated polybutadiene skeleton-containing resin” refers to a resin in which at least a part of the polybutadiene skeleton is hydrogenated, and is not necessarily a resin in which the polybutadiene skeleton is completely hydrogenated. Examples of the hydrogenated polybutadiene skeleton-containing resin include a hydrogenated polybutadiene skeleton-containing epoxy resin. Examples of the phenolic hydroxyl group-containing butadiene resin include resins having a polybutadiene structure and having a phenolic hydroxyl group.

  Specific examples of the butadiene resin include “Ricon 657” (epoxy group-containing polybutadiene), “Ricon 130MA8”, “Ricon 130MA13”, “Ricon 130MA20”, “Ricon 131MA5”, “Ricon 131MA10”, “Ricon 131MA10” manufactured by Clay Valley. “Ricon 131MA17”, “Ricon 131MA20”, “Ricon 184MA6” (anhydride-containing polybutadiene), “JP-100”, “JP-200” (epoxidized polybutadiene), “GQ-1000” (manufactured by Nippon Soda Co., Ltd.) Hydroxyl group, carboxyl group-introduced polybutadiene), "G-1000", "G-2000", "G-3000" (both end hydroxyl group polybutadiene), "GI-1000", "GI-2000", "GI-3000" Hydroxylated polybutadiene at both ends), “PB3600”, “PB4700” (polybutadiene skeleton epoxy compound), “Epofriend A1005”, “Epofriend A1010”, “Epofriend A1020” (styrene, butadiene and styrene block) manufactured by Daicel (Epoxy compound of copolymer), “FCA-061L” (hydrogenated polybutadiene skeleton epoxy compound) manufactured by Nagase ChemteX Corporation, “R-45EPT” (polybutadiene skeleton epoxy compound), and the like.

  Examples of preferred butadiene resins include linear polyimides made from hydroxyl-terminated polybutadiene, diisocyanate compounds and tetrabasic acid anhydrides (polyimides described in JP 2006-37083 A and WO 2008/153208 A). ). The content of the polybutadiene structure in the polyimide resin is preferably 60% by mass to 95% by mass, and more preferably 75% by mass to 85% by mass. Details of the polyimide resin can be referred to the descriptions in JP-A-2006-37083 and International Publication No. 2008/153208, the contents of which are incorporated herein.

  (D) Another preferred example of the polymer resin is a siloxane resin. Specific examples of the siloxane resin include “SMP-2006”, “SMP-2003PGMEA”, “SMP-5005PGMEA” manufactured by Shin-Etsu Silicone Co., Ltd., linear polyimide using amine group-terminated polysiloxane and tetrabasic acid anhydride (raw material). International Publication No. 2010/053185).

  (D) Still another preferable example of the polymer resin includes an alkylene resin and an alkyleneoxy resin. Specific examples of the alkylene resin and alkyleneoxy resin include “PTXG-1000” and “PTXG-1800” manufactured by Asahi Kasei Fibers, Inc. and “YX-7180” manufactured by Mitsubishi Chemical Corporation (resins containing an alkylene structure having an ether bond). ), “EXA-4850-150”, “EXA-4816”, “EXA-4822” manufactured by DIC Corporation, “EP-4000”, “EP-4003”, “EP-4010”, “EP-4010” manufactured by ADEKA EP-4011 ”,“ BEO-60E ”,“ BPO-20E ”manufactured by Shin Nippon Rika Co., Ltd.,“ YL7175 ”,“ YL7410 ”manufactured by Mitsubishi Chemical Corporation, and the like.

  (D) Another preferred example of the polymer resin is an isoprene resin. Specific examples of the isoprene resin include “KL-610” and “KL-613” manufactured by Kuraray Co., Ltd.

  (D) Another preferred example of the polymer resin is isobutylene resin. Specific examples of the isobutylene resin include “SIBSTAR-073T” (styrene-isobutylene-styrene triblock copolymer) and “SIBSTAR-042D” (styrene-isobutylene diblock copolymer) manufactured by Kaneka Corporation.

  (D) Still another preferred example of the polymer resin is a carbonate resin. Preferred examples of the carbonate resin include hydroxy group-containing carbonate resin, phenolic hydroxyl group-containing carbonate resin, carboxy group-containing carbonate resin, acid anhydride group-containing carbonate resin, epoxy group-containing carbonate resin, isocyanate group-containing carbonate resin, urethane group-containing A carbonate resin etc. are mentioned.

  Specific examples of the carbonate resin include "T6002", "T6001" (polycarbonate diol) manufactured by Asahi Kasei Chemicals, "C-1090", "C-2090", "C-3090" (polycarbonate diol) manufactured by Kuraray. Etc.

  Examples of preferred carbonate resins also include linear polyimides made from hydroxyl group-terminated polycarbonates, diisocyanate compounds and tetrabasic acid anhydrides. The content of the polycarbonate resin in the polycarbonate structure is preferably 60% by mass to 95% by mass, and more preferably 75% by mass to 85% by mass. Details of the polyimide resin can be referred to the description of International Publication No. 2016/129541, the contents of which are incorporated herein.

  (D) Another preferable example of the polymer resin is an acrylic resin. Preferred examples of the acrylic resin include hydroxy group-containing acrylic resin, phenolic hydroxyl group-containing acrylic resin, carboxy group-containing acrylic resin, acid anhydride group-containing acrylic resin, epoxy group-containing acrylic resin, isocyanate group-containing acrylic resin, urethane group-containing An acrylic resin etc. are mentioned.

  Specific examples of acrylic resins include Teissan resin “SG-70L”, “SG-708-6”, “WS-023”, “SG-700AS”, “SG-280TEA” (carboxy group) manufactured by Nagase ChemteX Corporation. -Containing acrylic ester copolymer resin, acid value of 5 to 34 mg KOH / g, weight average molecular weight of 400,000 to 900,000, Tg-30 ° C to 5 ° C), "SG-80H", "SG-80H-3", " SG-P3 "(epoxy group-containing acrylate copolymer resin, epoxy equivalent 4761-14285 g / eq, weight average molecular weight 350,000-850,000, Tg 11 ° C-12 ° C)," SG-600TEA "," SG-790 (Hydroxy group-containing acrylate copolymer resin, hydroxyl value 20 to 40 mg KOH / g, weight average molecular weight 500,000 to 1,200,000, Tg-37 ° C. 32 ° C), “ME-2000”, “W-116.3” (carboxy group-containing acrylate copolymer resin), “W-197C” (hydroxyl group-containing acrylate copolymer resin) manufactured by Negami Kogyo Co., Ltd. ), “KG-25”, “KG-3000” (epoxy group-containing acrylate copolymer resin), and the like.

  (D) Other preferable examples of the polymer resin include acrylic rubber particles, polyamide fine particles, and silicone particles. Specific examples of the acrylic rubber particles include resin fine particles obtained by subjecting a resin exhibiting rubber elasticity, such as acrylonitrile butadiene rubber, butadiene rubber, and acrylic rubber, to a chemical cross-linking treatment so as to be insoluble and infusible in an organic solvent. Specific examples of the acrylic rubber particles include XER-91 (manufactured by Nippon Synthetic Rubber Co., Ltd.); Staphyloid AC3355, AC3816, AC3832, AC4030, AC3364, IM101 (above, manufactured by Ganz Kasei Co., Ltd.); Chemical Industry Co., Ltd.); As the polyamide fine particles, aliphatic polyamides such as nylon and those having a flexible skeleton such as polyamideimide can be used. Specific examples of the polyamide fine particles include VESTOSINT 2070 (manufactured by Daicel Huls); SP500 (manufactured by Toray Industries, Inc.); and the like.

  (D) One type of polymer resin may be used alone, or two or more types may be used in combination.

  The polymer resin (D) preferably has a high molecular weight from the viewpoint of exhibiting excellent flexibility. (D) The specific number average molecular weight Mn of the polymer resin is preferably 4000 or more, more preferably 4500 or more, further preferably 5000 or more, particularly preferably 5500 or more, preferably 100000 or less, more preferably 95000. Hereinafter, it is particularly preferably 90000 or less. (D) When the number average molecular weight Mn of the polymer resin is in the above range, the desired effect of the present invention can be remarkably obtained. (D) The number average molecular weight Mn of the polymer resin is a polystyrene-equivalent number average molecular weight measured using GPC (gel permeation chromatography).

  When the (D) polymer resin has a functional group, the functional group equivalent of the (D) polymer resin is preferably 100 or more, more preferably 200 or more, still more preferably 1000 or more, particularly preferably 2500 or more, Preferably it is 50000 or less, More preferably, it is 30000 or less, More preferably, it is 10,000 or less, Most preferably, it is 5000 or less. Functional group equivalent is the number of grams of resin containing 1 gram equivalent of functional group. For example, the epoxy group equivalent can be measured according to JIS K7236. Further, for example, the hydroxyl equivalent can be calculated by dividing the molecular weight of KOH by the hydroxyl value measured according to JIS K1557-1.

  The amount of the (D) polymer resin in the resin composition is preferably 0.2% by mass or more, more preferably 0.3% by mass or more, and particularly preferably with respect to 100% by mass of the nonvolatile component of the resin composition. It is 0.4 mass% or more, preferably 20 mass% or less, more preferably 15 mass% or less, and particularly preferably 10 mass% or less. (D) When the amount of the polymer resin is within the above range, the desired effect of the present invention can be remarkably obtained. In particular, when the amount of the (D) polymer resin is not less than the lower limit value of the above range, the minimum melt viscosity of the resin composition can be effectively lowered, and by being not more than the upper limit value of the above range, Heat resistance can be improved by raising the glass transition temperature of the cured product of the resin composition.

[6. (E) Curing agent]
The resin composition may contain (E) a curing agent in addition to the components described above as an optional component. (E) The curing agent usually has a function of reacting with the epoxy resin (A) to cure the resin composition. (E) A hardening | curing agent may be used individually by 1 type, and may be used in combination of 2 or more types.

  Examples of the curing agent as the component (E) include an active ester curing agent, a phenol curing agent, a naphthol curing agent, a benzoxazine curing agent, a cyanate ester curing agent, and a carbodiimide curing agent. Among these, from the viewpoint of remarkably obtaining the desired effect of the present invention, the (E) curing agent is preferably a phenol curing agent, a naphthol curing agent, an active ester curing agent, or a cyanate ester curing agent, and a phenol curing An agent and an active ester curing agent are more preferable.

  As the active ester curing agent, a compound having one or more active ester groups in one molecule can be used. Among them, as the active ester curing agent, two or more ester groups having high reaction activity such as phenol esters, thiophenol esters, N-hydroxyamine esters, and heterocyclic hydroxy compound esters in one molecule are used. The compound which has is preferable. The active ester curing agent is preferably obtained by a condensation reaction between a carboxylic acid compound and / or a thiocarboxylic acid compound and a hydroxy compound and / or a thiol compound. In particular, from the viewpoint of improving heat resistance, an active ester curing agent obtained from a carboxylic acid compound and a hydroxy compound is preferable, and an active ester curing agent obtained from a carboxylic acid compound and a phenol compound and / or a naphthol compound is more preferable. .

  Examples of the carboxylic acid compound include benzoic acid, acetic acid, succinic acid, maleic acid, itaconic acid, phthalic acid, isophthalic acid, terephthalic acid, and pyromellitic acid.

  Examples of the phenol compound or naphthol compound include hydroquinone, resorcin, bisphenol A, bisphenol F, bisphenol S, phenolphthaline, methylated bisphenol A, methylated bisphenol F, methylated bisphenol S, phenol, o-cresol, m- Cresol, p-cresol, catechol, α-naphthol, β-naphthol, 1,5-dihydroxynaphthalene, 1,6-dihydroxynaphthalene, 2,6-dihydroxynaphthalene, dihydroxybenzophenone, trihydroxybenzophenone, tetrahydroxybenzophenone, phloroglucin, Benzenetriol, dicyclopentadiene type diphenol compound, phenol novolac and the like can be mentioned. Here, the “dicyclopentadiene type diphenol compound” refers to a diphenol compound obtained by condensing two molecules of phenol with one molecule of dicyclopentadiene.

  Preferable specific examples of the active ester curing agent include an active ester compound containing a dicyclopentadiene type diphenol structure, an active ester compound containing a naphthalene structure, an active ester compound containing an acetylated product of phenol novolac, and a benzoylated product of phenol novolac. The active ester compound containing is mentioned. Of these, active ester compounds containing a naphthalene structure and active ester compounds containing a dicyclopentadiene type diphenol structure are more preferred. The “dicyclopentadiene type diphenol structure” represents a divalent structure composed of phenylene-dicyclopentylene-phenylene.

  As a commercial product of an active ester type curing agent, for example, as an active ester compound containing a dicyclopentadiene type diphenol structure, “EXB9451”, “EXB9460”, “EXB9460S”, “HPC-8000-65T”, “HPC-” "8000H-65TM", "EXB-8000L-65TM" (manufactured by DIC); "EXB9416-70BK" (manufactured by DIC) as an active ester compound containing a naphthalene structure; "DC808" as an active ester compound containing an acetylated product of phenol novolac (Mitsubishi Chemical Co., Ltd.); “YLH1026” (Mitsubishi Chemical Co., Ltd.) as an active ester compound containing a benzoylated phenol novolac; “DC808” (Mitsubishi Chemical Co., Ltd.) as an active ester curing agent which is an acetylated product of phenol novolac Examples of active ester curing agents that are benzoylated phenol novolaks include “YLH1026” (manufactured by Mitsubishi Chemical), “YLH1030” (manufactured by Mitsubishi Chemical), “YLH1048” (manufactured by Mitsubishi Chemical); .

  As a phenol type hardening | curing agent and a naphthol type | system | group hardening | curing agent, what has a novolak structure from a heat resistant and water-resistant viewpoint is preferable. Moreover, from a viewpoint of adhesiveness with a conductor layer, a nitrogen-containing phenol type hardening | curing agent is preferable and a triazine frame | skeleton containing phenol type hardening | curing agent is more preferable.

  Specific examples of the phenol-based curing agent and naphthol-based curing agent include “MEH-7700”, “MEH-7810”, “MEH-7785” manufactured by Meiwa Kasei Co., Ltd .; “NHN”, “CBN” manufactured by Nippon Kayaku Co., Ltd. “SN170”, “SN180”, “SN190”, “SN475”, “SN485”, “SN495V”, “SN375”, “SN395” manufactured by Nippon Steel & Sumikin Co., Ltd .; “TD-” manufactured by DIC 2090 "," LA-7052 "," LA-7054 "," LA-1356 "," LA-3018-50P "," EXB-9500 "," HPC-9500 "," KA-1160 "," KA- " 1163 "," KA-1165 ";" GDP-6115L "," GDP-6115H "manufactured by Gunei Chemical Co., Ltd., and the like.

  Specific examples of the benzoxazine-based curing agent include “HFB2006M” manufactured by Showa Polymer Co., Ltd. and “Pd” and “Fa” manufactured by Shikoku Kasei Kogyo Co., Ltd.

  Examples of the cyanate ester curing agent include bisphenol A dicyanate, polyphenol cyanate, oligo (3-methylene-1,5-phenylene cyanate), 4,4′-methylenebis (2,6-dimethylphenyl cyanate), 4,4. '-Ethylidene diphenyl dicyanate, hexafluorobisphenol A dicyanate, 2,2-bis (4-cyanate) phenylpropane, 1,1-bis (4-cyanatephenylmethane), bis (4-cyanate-3,5-dimethyl) Bifunctional cyanate resins such as phenyl) methane, 1,3-bis (4-cyanatephenyl-1- (methylethylidene)) benzene, bis (4-cyanatephenyl) thioether, and bis (4-cyanatephenyl) ether; Phenol novolac and Polyfunctional cyanate resin derived from resol novolac; prepolymer these cyanate resin is partially triazine of; and the like. Specific examples of the cyanate ester curing agent include “PT30” and “PT60” (both phenol novolac polyfunctional cyanate ester resins), “BA230”, “BA230S75” (part of bisphenol A dicyanate) manufactured by Lonza Japan. Or a prepolymer which is all triazine-modified into a trimer).

  Specific examples of the carbodiimide curing agent include “V-03” and “V-07” manufactured by Nisshinbo Chemical Co., Ltd.

  When the resin composition contains (E) a curing agent, the amount of the (E) curing agent is preferably 0.5% by mass or more, more preferably 1.% by mass with respect to 100% by mass of the nonvolatile component in the resin composition. It is 0% by mass or more, particularly preferably 2.0% by mass or more, preferably 20% by mass or less, more preferably 15% by mass or less, and particularly preferably 10% by mass or less. When the amount of the component (E) is in the above range, the desired effect of the present invention can be remarkably obtained.

  When the number of epoxy groups in the (A) epoxy resin is 1, the number of active groups in the (E) curing agent is preferably 0.10 or more, more preferably 0.15 or more, still more preferably 0.20 or more, preferably Is 2 or less, more preferably 1.5 or less, and still more preferably 1.0 or less. Here, “(A) the number of epoxy groups of the epoxy resin” is a value obtained by adding up all the values obtained by dividing the mass of the nonvolatile component of the (A) epoxy resin present in the resin composition by the epoxy equivalent. Further, “(B) the number of active groups of the curing agent” is a value obtained by adding all values obtained by dividing the mass of the non-volatile component of the (E) curing agent present in the resin composition by the active group equivalent. (A) When the number of active groups of (E) curing agent when the number of epoxy groups of the epoxy resin is 1, the desired effect of the present invention can be remarkably obtained, and more usually, the resin composition The heat resistance of the cured product of the physical layer is further improved.

[7. (F) Curing accelerator]
The resin composition may contain (F) a curing accelerator as an optional component in addition to the components described above. (F) By using a curing accelerator, curing can be accelerated when the resin composition is cured.

  Examples of the curing accelerator as the component (F) include phosphorus-based curing accelerators, amine-based curing accelerators, imidazole-based curing accelerators, guanidine-based curing accelerators, metal-based curing accelerators, and the like. A curing accelerator, an amine curing accelerator, an imidazole curing accelerator, and a metal curing accelerator are preferred. Among these, amine-based curing accelerators, imidazole-based curing accelerators, and metal-based curing accelerators are preferable, and imidazole-based curing accelerators are particularly preferable from the viewpoint of remarkably exhibiting the effects of the present invention. A hardening accelerator may be used individually by 1 type, and may be used in combination of 2 or more types.

  Examples of phosphorus curing accelerators include triphenylphosphine, phosphonium borate compounds, tetraphenylphosphonium tetraphenylborate, n-butylphosphonium tetraphenylborate, tetrabutylphosphonium decanoate, (4-methylphenyl) triphenylphosphonium thiocyanate. , Tetraphenylphosphonium thiocyanate, butyltriphenylphosphonium thiocyanate, and the like. Of these, triphenylphosphine and tetrabutylphosphonium decanoate are preferable.

  Examples of amine curing accelerators include trialkylamines such as triethylamine and tributylamine, 4-dimethylaminopyridine, benzyldimethylamine, 2,4,6, -tris (dimethylaminomethyl) phenol, 1,8-diazabicyclo. (5, 4, 0) -undecene and the like. Of these, 4-dimethylaminopyridine and 1,8-diazabicyclo (5,4,0) -undecene are preferable.

  Examples of the imidazole curing accelerator include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2- Phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2- Ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6 -[2 -Methylimidazolyl- (1 ')]-ethyl-s-triazine, 2,4-diamino-6- [2'-undecylimidazolyl- (1')]-ethyl-s-triazine, 2,4-diamino- 6- [2′-Ethyl-4′-methylimidazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6- [2′-methylimidazolyl- (1 ′)]-ethyl-s -Triazine isocyanuric acid adduct, 2-phenylimidazole isocyanuric acid adduct, 2-phenyl-4,5-dihydroxymethylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2,3-dihydro-1H- Pyrrolo [1,2-a] benzimidazole, 1-dodecyl-2-methyl-3-benzylimidazolium chloride, 2-methylimidazoline, - adduct of an imidazole compound and an imidazole compound and an epoxy resin of the phenyl imidazoline, and the like. Of these, 2-ethyl-4-methylimidazole and 1-benzyl-2-phenylimidazole are preferable.

  Commercially available products may be used as the imidazole curing accelerator, and examples thereof include “P200-H50” manufactured by Mitsubishi Chemical Corporation; “1B2PZ” manufactured by Shikoku Kasei Kogyo Co., Ltd.

  Examples of the guanidine curing accelerator include dicyandiamide, 1-methylguanidine, 1-ethylguanidine, 1-cyclohexylguanidine, 1-phenylguanidine, 1- (o-tolyl) guanidine, dimethylguanidine, diphenylguanidine, trimethylguanidine, Tetramethylguanidine, pentamethylguanidine, 1,5,7-triazabicyclo [4.4.0] dec-5-ene, 7-methyl-1,5,7-triazabicyclo [4.4.0] Deca-5-ene, 1-methyl biguanide, 1-ethyl biguanide, 1-n-butyl biguanide, 1-n-octadecyl biguanide, 1,1-dimethyl biguanide, 1,1-diethyl biguanide, 1-cyclohexyl biguanide, 1 -Allyl biguanide, 1-phenyl biguanide, 1- ( - tolyl) biguanide, and the like. Of these, dicyandiamide and 1,5,7-triazabicyclo [4.4.0] dec-5-ene are preferred.

  As a metal type hardening accelerator, the organometallic complex or organometallic salt of metals, such as cobalt, copper, zinc, iron, nickel, manganese, tin, is mentioned, for example. Specific examples of the organometallic complex include organic cobalt complexes such as cobalt (II) acetylacetonate and cobalt (III) acetylacetonate, organic copper complexes such as copper (II) acetylacetonate, and zinc (II) acetylacetonate. Organic zinc complexes such as iron (III) acetylacetonate, organic nickel complexes such as nickel (II) acetylacetonate, and organic manganese complexes such as manganese (II) acetylacetonate. Examples of the organic metal salt include zinc octylate, tin octylate, zinc naphthenate, cobalt naphthenate, tin stearate, and zinc stearate.

  When the resin composition contains (F) a curing accelerator, the amount of (F) the curing accelerator is based on 100% by mass of the nonvolatile component of the resin composition from the viewpoint of remarkably obtaining the desired effect of the present invention. Preferably it is 0.01% by mass or more, more preferably 0.03% by mass or more, particularly preferably 0.05% by mass or more, preferably 3% by mass or less, more preferably 1.5% by mass or less, particularly preferably. Is 1% by mass or less.

[8. (G) Thermoplastic resin]
The resin composition may contain (G) a thermoplastic resin as an optional component in addition to the components described above.

  Examples of the thermoplastic resin as the component (G) include phenoxy resin, polyvinyl acetal resin, polyolefin resin, butadiene resin, siloxane resin, alkylene resin, alkyleneoxy resin, isoprene resin, isobutylene resin, carbonate resin, acrylic resin, and polyimide. Examples thereof include resins, polyamideimide resins, polyetherimide resins, polysulfone resins, polyethersulfone resins, polyphenylene ether resins, polyetheretherketone resins, and polyester resins.

  Examples of the phenoxy resin include bisphenol A skeleton, bisphenol F skeleton, bisphenol S skeleton, bisphenolacetophenone skeleton, novolac skeleton, biphenyl skeleton, fluorene skeleton, dicyclopentadiene skeleton, norbornene skeleton, naphthalene skeleton, anthracene skeleton, adamantane skeleton, terpene Examples thereof include a phenoxy resin having one or more skeletons selected from the group consisting of a skeleton and a trimethylcyclohexane skeleton. The terminal of the phenoxy resin may be any functional group such as a phenolic hydroxyl group or an epoxy group.

  Specific examples of the phenoxy resin include “1256” and “4250” (both bisphenol A skeleton-containing phenoxy resins) manufactured by Mitsubishi Chemical; “YX8100” (bisphenol S skeleton-containing phenoxy resin) manufactured by Mitsubishi Chemical; "YX6954" (bisphenolacetophenone skeleton-containing phenoxy resin) manufactured by Nippon Steel & Sumitomo Chemical Co., Ltd. "FX280" and "FX293" manufactured by Nippon Steel & Sumikin Chemical Co., Ltd .; “YL7769BH30”, “YL6794”, “YL7213”, “YL7290”, “YL7891BH30”, “YL7482” and the like.

  (G) The weight average molecular weight Mw of the thermoplastic resin is preferably 8,000 or more, more preferably 10,000 or more, and particularly preferably 20,000 or more from the viewpoint of remarkably obtaining the desired effect of the present invention. , Preferably 70,000 or less, more preferably 60,000 or less, particularly preferably 50,000 or less. (G) The weight average molecular weight Mw of a thermoplastic resin is the number average molecular weight of polystyrene conversion measured using GPC.

  When the resin composition contains (G) a thermoplastic resin, the amount of the (G) thermoplastic resin in the resin composition is 100 masses of the non-volatile component in the resin composition from the viewpoint of remarkably obtaining the desired effect of the present invention. %, Preferably 0.01% by mass or more, more preferably 0.1% by mass or more, further preferably 0.3% by mass or more, preferably 20% by mass or less, more preferably 10% by mass or less. More preferably, it is 5 mass% or less.

[9. (H) Flame retardant]
The resin composition may contain a flame retardant (H) as an optional component in addition to the components described above.

  Examples of (H) flame retardants include organic phosphorus flame retardants, organic nitrogen-containing phosphorus compounds, nitrogen compounds, silicone flame retardants, and metal hydroxides. A flame retardant may be used individually by 1 type and may use 2 or more types together.

  Specific examples of the (H) flame retardant include “HCA-HQ” manufactured by Sanko Co., Ltd. and “PX-200” manufactured by Daihachi Chemical Industry Co., Ltd. As the flame retardant, those which are difficult to hydrolyze are preferable, and for example, 10- (2,5-dihydroxyphenyl) -10-hydro-9-oxa-10-phosphaphenanthrene-10-oxide and the like are preferable.

  When the resin composition contains (H) a flame retardant, the amount of (H) the flame retardant is preferably 0.01% by mass or more, more preferably 0, with respect to 100% by mass of the nonvolatile component in the resin composition. 0.1% by mass or more, more preferably 0.3% by mass or more, preferably 20% by mass or less, more preferably 10% by mass or less, more preferably 5% by mass or less.

[10. (I) Optional additive]
The resin composition may further contain an additive as an optional component in addition to the components described above. Examples of such additives include organic metal compounds such as organic copper compounds, organic zinc compounds, and organic cobalt compounds; resin additives such as binders, thickeners, antifoaming agents, leveling agents, and adhesion-imparting agents; Etc. These additives may be used alone or in combination of two or more.

[11. Method for producing resin composition]
A resin composition can be manufactured by the method of stirring a compounding component using stirring apparatuses, such as a rotary mixer, for example.

[12. Characteristics of resin composition]
According to the resin composition described above, the minimum melt viscosity can be lowered. Therefore, the laminating property of the resin sheet using the resin composition can be improved. (B) According to the inorganic filler, the insulating performance and sealing performance of the cured product of the resin composition can be improved. Generally, however, the composition containing the inorganic filler (B) has a high melt viscosity and is laminated. Tend to be impaired. On the other hand, in the resin composition mentioned above, since (D) the polymer resin is used, the melt viscosity can be lowered while using the inorganic filler (B), and therefore, good laminating properties can be achieved. The specific minimum melt viscosity of the resin composition is preferably 30000 poise or less, more preferably 20000 poise or less, and still more preferably 12000 poise or less. The lower limit of the minimum melt viscosity of the resin composition is not particularly limited, but may be, for example, 100 poise or more. The minimum melt viscosity of the resin composition can be measured by the method described in Examples.

  According to the resin composition described above, a cured product having a high glass transition temperature can be obtained. Therefore, since the heat resistance of the hardened | cured material of a resin composition can be made favorable, the insulating layer and sealing layer excellent in heat resistance can be obtained. For example, the specific glass transition temperature of the cured product obtained by thermosetting the resin composition under the conditions described in the examples is preferably 140 ° C. or higher, more preferably 145 ° C. or higher, particularly preferably 150 ° C. or higher. is there. The upper limit of the glass transition temperature of the cured product of the resin composition is not particularly limited, but may be, for example, 300 ° C. or lower. The glass transition temperature of the cured product of the resin composition can be measured by the method described in the examples.

According to the above-described resin composition, since carbon black functions as a colorant, it is possible to obtain an appropriate color depending on the application using the carbon black. Usually, since carbon black functions as a black pigment, the color of the cured product of the resin composition can be black or a color close thereto. For example, when an insulating layer is formed by a cured product of the resin composition by the method described in the examples, a black insulating layer is obtained. Specifically, the coordinates ^{L *} in ^{the L} * ^a * ^{b *} color system of the insulating layer, and the coordinates ^{L *} in ^{the L} * ^a * ^{b *} color system of the aluminum oxide white plate as a white standard plate The difference ΔL ^* is preferably −100 or more, preferably −40 or less, more preferably −50 or less, and particularly preferably −60 or less. Furthermore, the coordinate ^{b *} in ^{the L} * ^a * ^{b *} color system of the insulating layer, of aluminum oxide white plate as a white standard plate ^L * ^a * ^{b *} difference Δb between the coordinate ^{b *} in the color system ^* Is preferably −20 or more, more preferably −15 or more, particularly preferably −10 or more, preferably 20 or less, more preferably 15 or less, and particularly preferably 10 or less.

  The resin composition described above can suppress the aggregation of carbon black. Conventionally, in a resin composition containing (B) an inorganic filler and (D) a polymer resin, carbon black generally tends to agglomerate, so that excellent characteristics such as color development, minimum melt viscosity, glass transition temperature, and the like are obtained. It has been difficult to achieve both the suppression of aggregation. On the other hand, according to the above-described resin composition, (C) aggregation of carbon black can be suppressed even when combined with (B) inorganic filler and (D) polymer resin. Therefore, the occurrence of defects due to the aggregation of (C) carbon black can be suppressed while the characteristics such as color development, minimum melt viscosity and glass transition temperature are balanced as described above. Specifically, when the resin composition layer is formed, it is possible to reduce the frequency of occurrence of (C) carbon black aggregates exceeding the maximum length of 100 μm.

  The cured product of the resin composition described above usually has excellent insulating performance. (B) In addition to obtaining an excellent insulating performance by the inorganic filler, it is possible to suppress the aggregation of carbon black, and thus it is possible to suppress a decrease in insulation due to the aggregate of carbon black. Moreover, since generation | occurrence | production of the aggregate of carbon black can be suppressed, it is possible to use a resin composition as a material of a thin insulating layer.

  The cured product of the resin composition described above usually has excellent sealing performance. (B) In addition to obtaining excellent sealing performance by the inorganic filler, it is possible to suppress the aggregation of carbon black, so it is possible to suppress the occurrence of cracks starting from the aggregate of carbon black, and the sealing performance by cracks Reduction can be suppressed.

[13. Application of resin composition]
The sealing layer and the insulating layer can be formed from the cured product of the resin composition by utilizing the advantages described above. Therefore, this resin composition can be used as a resin composition for semiconductor encapsulation or insulating layer.

  For example, the resin composition includes a resin composition for forming an insulating layer of a semiconductor chip package (resin composition for an insulating layer of a semiconductor chip package) and an insulation of a circuit board (including a printed wiring board). The resin composition for forming a layer (resin composition for an insulating layer of a circuit board) can be suitably used.

  For example, the resin composition can be suitably used as a resin composition for sealing a semiconductor chip (a resin composition for sealing a semiconductor chip).

  As a semiconductor chip package to which a sealing layer or an insulating layer formed of a cured product of the resin composition can be applied, for example, FC-CSP, MIS-BGA package, ETS-BGA package, Fan-out type WLP (Wafer) Level-Package), Fan-in type WLP, Fan-out type PLP (Panel Level Package), and Fan-in type PLP.

  The resin composition may be used as an underfill material. For example, the resin composition may be used as a MUF (Molding Under Filling) material used after a semiconductor chip is connected to a substrate.

  Furthermore, the resin composition can be used in a wide range of applications in which the resin composition is used, such as a sheet-like laminated material such as a resin sheet or prepreg, a solder resist, a die bonding material, a hole-filling resin, or a component-embedded resin.

[14. Resin sheet]
The resin sheet of this invention has a support body and the resin composition layer provided on this support body. A resin composition layer is a layer containing the resin composition of this invention, and is normally formed with the resin composition.

  The thickness of the resin composition layer is preferably 200 μm or less, more preferably 150 μm or less, still more preferably 100 μm or less, 80 μm or less, 60 μm or less, 50 μm or less, or 40 μm or less from the viewpoint of thinning. The minimum of the thickness of a resin composition layer is not specifically limited, For example, it may be 1 micrometer or more, 5 micrometers or more, 10 micrometers or more, etc.

  Examples of the support include a film made of a plastic material, a metal foil, and a release paper, and a film made of a plastic material and a metal foil are preferable.

  When a film made of a plastic material is used as the support, examples of the plastic material include polyethylene terephthalate (hereinafter sometimes abbreviated as “PET”) and polyethylene naphthalate (hereinafter abbreviated as “PEN”). Polyester) such as polycarbonate; acrylic polymer such as polymethyl methacrylate (hereinafter sometimes abbreviated as “PMMA”); cyclic polyolefin; triacetyl cellulose (hereinafter referred to as “PMMA”). May be abbreviated as “TAC”); polyether sulfide (hereinafter may be abbreviated as “PES”); polyether ketone; polyimide; Among these, polyethylene terephthalate and polyethylene naphthalate are preferable, and inexpensive polyethylene terephthalate is particularly preferable.

  When metal foil is used as the support, examples of the metal foil include copper foil and aluminum foil. Among these, copper foil is preferable. As the copper foil, a foil made of a single metal of copper may be used, and a foil made of an alloy of copper and another metal (for example, tin, chromium, silver, magnesium, nickel, zirconium, silicon, titanium, etc.). It may be used.

  The support may be subjected to a treatment such as a mat treatment, a corona treatment, a charge suppression treatment, or the like on the surface bonded to the resin composition layer.

  Moreover, as a support body, you may use the support body with a release layer which has a release layer in the surface joined to a resin composition layer. Examples of the release agent used for the release layer of the support with a release layer include one or more release agents selected from the group consisting of alkyd resins, polyolefin resins, urethane resins, and silicone resins. . Examples of commercially available release agents include “SK-1”, “AL-5”, and “AL-7” manufactured by Lintec Corporation as alkyd resin release agents. Examples of the support with a release layer include “LUMIRROR T60” manufactured by Toray Industries, “Purex” manufactured by Teijin Limited, and “Unipeel” manufactured by Unitika.

  As a thickness of a support body, the range of 5 micrometers-75 micrometers is preferable, and the range of 10 micrometers-60 micrometers is more preferable. In addition, when using a support body with a release layer, it is preferable that the thickness of the whole support body with a release layer is the said range.

  The resin sheet is prepared by, for example, preparing a resin varnish in which a resin composition is dissolved in an organic solvent, applying the resin varnish on a support using a coating device such as a die coater, and drying the resin varnish. Can be produced.

  Examples of organic solvents include ketone solvents such as acetone, methyl ethyl ketone (MEK), and cyclohexanone; acetate solvents such as ethyl acetate, butyl acetate, cellosolve acetate, propylene glycol monomethyl ether acetate, and carbitol acetate; cellosolve and butyl carbitol Carbitol solvents of the following: aromatic hydrocarbon solvents such as toluene and xylene; amide solvents such as dimethylformamide, dimethylacetamide (DMAc) and N-methylpyrrolidone; One organic solvent may be used alone, or two or more organic solvents may be used in combination.

  Drying may be performed by a known method such as heating or hot air blowing. Drying is performed so that the content of the organic solvent in the resin composition layer is usually 10% by mass or less, preferably 5% by mass or less. Depending on the boiling point of the organic solvent in the resin varnish, for example, when using a resin varnish containing 30% by mass to 60% by mass of the organic solvent, the resin composition is dried at 50 ° C. to 150 ° C. for 3 minutes to 10 minutes. A physical layer can be formed.

  The resin sheet may contain arbitrary layers other than a support body and a resin composition layer as needed. For example, in the resin sheet, a protective film according to the support may be provided on the surface of the resin composition layer that is not bonded to the support (that is, the surface opposite to the support). The thickness of the protective film is, for example, 1 μm to 40 μm. By the protective film, it is possible to suppress adhesion or scratches of dust or the like to the surface of the resin composition layer. When the resin sheet has a protective film, the resin sheet can be used by peeling off the protective film. The resin sheet can be stored in a roll.

  The resin sheet can be suitably used for forming an insulating layer in the manufacture of a semiconductor chip package (resin sheet for an insulating layer of a semiconductor chip package). For example, a resin sheet can be suitably used for forming an insulating layer of a circuit board (resin sheet for an insulating layer of a circuit board), and an interlayer insulating layer on which a conductor layer is formed by plating is formed thereon Therefore, it can be more suitably used (for an interlayer insulating layer of a circuit board on which a conductor layer is formed by plating). Examples of a package using such a substrate include FC-CSP, MIS-BGA package, and ETS-BGA package.

  The resin sheet can be suitably used for sealing a semiconductor chip (semiconductor chip sealing resin sheet) or for forming a wiring on a semiconductor chip (semiconductor chip wiring forming resin sheet). . Examples of applicable semiconductor chip packages include Fan-out type WLP (Wafer Level Package), Fan-in type WLP, Fan-out type PLP (Panel Level Package), Fan-in type PLP, and the like.

  Moreover, you may use a resin sheet for the material of MUF used after connecting a semiconductor chip to a board | substrate.

  Furthermore, the resin sheet can be used for a wide variety of other applications that require high insulation reliability. For example, the resin sheet can be suitably used for forming an insulating layer of a circuit board such as a printed wiring board.

[15. Circuit board]
The circuit board of the present invention includes an insulating layer formed of a cured product of the resin composition of the present invention. This circuit board can be manufactured, for example, by a manufacturing method including the following step (1) and step (2).
(1) The process of forming a resin composition layer on a base material.
(2) A step of thermosetting the resin composition layer to form an insulating layer.

  In step (1), a substrate is prepared. Examples of the substrate include glass epoxy substrates, metal substrates (stainless steel, cold rolled steel plate (SPCC), etc.), polyester substrates, polyimide substrates, BT resin substrates, thermosetting polyphenylene ether substrates, and the like. Moreover, the base material may have metal layers, such as copper foil, on the surface as a part of the said base material. For example, you may use the base material which has the 1st metal layer and the 2nd metal layer which can peel on both surfaces. When such a base material is used, a conductor layer as a wiring layer that can function as circuit wiring is usually formed on the surface of the second metal layer opposite to the first metal layer. As a base material having such a metal layer, for example, an ultrathin copper foil with a carrier copper foil “Micro Thin” manufactured by Mitsui Mining & Mining Co., Ltd.) may be mentioned.

  Moreover, the conductor layer may be formed in the surface of one or both of a base material. In the following description, a member including a base material and a conductor layer formed on the surface of the base material may be referred to as a “base material with a wiring layer”. The conductive material contained in the conductive layer is, for example, one selected from the group consisting of gold, platinum, palladium, silver, copper, aluminum, cobalt, chromium, zinc, nickel, titanium, tungsten, iron, tin, and indium. Examples include materials containing the above metals. The conductor material may be a single metal or an alloy. Examples of the alloy include alloys of two or more kinds of metals selected from the above group (for example, nickel / chromium alloy, copper / nickel alloy, and copper / titanium alloy). Above all, from the viewpoint of versatility of conductor layer formation, cost, easiness of patterning, etc., chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper as single metal; and nickel-chromium alloy, copper -Nickel alloy, copper-titanium alloy; Among them, chromium, nickel, titanium, aluminum, zinc, gold, palladium, silver or copper single metal; and nickel-chromium alloy; are more preferable, and copper single metal is more preferable.

  The conductor layer may be patterned in order to function as a wiring layer, for example. At this time, the line (circuit width) / space (inter-circuit width) ratio of the conductor layer is not particularly limited, but is preferably 20/20 μm or less (that is, the pitch is 40 μm or less), more preferably 10/10 μm or less, The thickness is preferably 5/5 μm or less, more preferably 1/1 μm or less, and particularly preferably 0.5 / 0.5 μm or more. The pitch need not be the same throughout the conductor layer. The minimum pitch of the conductor layer may be, for example, 40 μm or less, 36 μm or less, or 30 μm or less.

  The thickness of the conductor layer is preferably 3 μm to 35 μm, more preferably 5 μm to 30 μm, still more preferably 10 to 20 μm, and particularly preferably 15 to 20 μm, although it depends on the design of the circuit board. In addition, when the insulating layer is polished or ground after the insulating layer is formed and the conductor layer is exposed to perform the interlayer connection of the conductor layer, the thickness of the conductor layer that performs the interlayer connection and the conductor layer that does not perform the interlayer connection has a thickness. Preferably they are different. Among the conductor layers, the thickness of the thickest conductor layer (conductive pillar) is preferably 2 μm or more and 100 μm or less, although it depends on the desired design of the wiring board. The thickness of the conductor layer can be adjusted by repeating the pattern formation described above. Moreover, the conductor layer connected between layers may be a convex type.

  For example, the conductive layer is a pattern dry process in which a dry film (photosensitive resist film) is laminated on a substrate, a pattern is formed by exposing and developing the dry film under predetermined conditions using a photomask. It can be manufactured by a method including a step of obtaining a film, a step of forming a conductor layer by a plating method such as an electrolytic plating method using the developed pattern dry film as a plating mask, and a step of peeling the pattern dry film. As the dry film, a photosensitive dry film made of a photoresist composition can be used. For example, a dry film formed of a resin such as a novolac resin or an acrylic resin can be used. The lamination conditions of the base material and the dry film can be the same as those of the base material and the resin sheet to be described later. Peeling of the dry film can be performed using, for example, an alkaline peeling solution such as a sodium hydroxide solution. If necessary, unnecessary wiring patterns may be removed by etching or the like.

  After preparing the base material, a resin composition layer is formed on the base material. When the conductor layer is formed on the surface of the substrate, the resin composition layer is preferably formed so that the conductor layer is embedded in the resin composition layer.

  Formation of a resin composition layer is normally performed by laminating | stacking a resin sheet and a base material. This lamination can be performed, for example, by attaching the resin composition layer to the substrate by removing the protective film from the resin sheet and then heat-pressing the resin sheet to the substrate from the support side. Examples of the member that heat-presses the resin sheet to the base material (hereinafter sometimes referred to as “heat-pressing member”) include a heated metal plate (SUS end plate, etc.) or a metal roll (SUS roll). . In addition, it is preferable not to press the thermocompression bonding member directly on the resin sheet, but to press it through an elastic material such as heat-resistant rubber so that the resin sheet sufficiently follows the surface irregularities of the base material.

  Lamination of the base material and the resin sheet may be performed by, for example, a vacuum laminating method. In the vacuum laminating method, the thermocompression bonding temperature is preferably in the range of 60 ° C to 160 ° C, more preferably 80 ° C to 140 ° C. The thermocompression bonding pressure is preferably in the range of 0.098 MPa to 1.77 MPa, more preferably 0.29 MPa to 1.47 MPa. The thermocompression bonding time is preferably in the range of 20 seconds to 400 seconds, more preferably 30 seconds to 300 seconds. Lamination is preferably performed under reduced pressure conditions with a pressure of 13 hPa or less.

  After lamination, the laminated resin sheets may be smoothed under normal pressure (atmospheric pressure), for example, by pressing a thermocompression bonding member from the support side. The pressing conditions for the smoothing treatment can be the same conditions as the thermocompression bonding conditions for the laminate. In addition, you may perform lamination | stacking and a smoothing process continuously using a vacuum laminator.

  After forming the resin composition layer on the substrate, in step (2), the resin composition layer is thermally cured to form an insulating layer. The thermosetting conditions of the resin composition layer vary depending on the type of the resin composition, but the curing temperature is usually in the range of 120 ° C to 240 ° C (preferably in the range of 150 ° C to 220 ° C, more preferably in the range of 170 ° C to 200 ° C. C.) and the curing time is usually in the range of 5 minutes to 120 minutes (preferably 10 minutes to 100 minutes, more preferably 15 minutes to 90 minutes).

  Prior to thermosetting the resin composition layer, the resin composition layer may be subjected to a preheating treatment in which the resin composition layer is heated at a temperature lower than the curing temperature. For example, prior to thermosetting the resin composition layer, the resin composition layer is usually at a temperature of 50 to 120 ° C. (preferably 60 to 110 ° C., more preferably 70 to 100 ° C.). May be preheated for usually 5 minutes or longer (preferably 5 minutes to 150 minutes, more preferably 15 minutes to 120 minutes).

As described above, a circuit board having an insulating layer can be manufactured. The circuit board manufacturing method may further include an optional step.
The method for manufacturing a circuit board may include, for example, a step of peeling the support of the resin sheet. The support may be peeled off before the thermosetting of the resin composition layer, or may be peeled off after the thermosetting of the resin composition layer.

  The method for manufacturing a circuit board may include, for example, a step of polishing the surface of the insulating layer after forming the insulating layer. The polishing method is not particularly limited. For example, the surface of the insulating layer can be polished using a surface grinder.

  The circuit board manufacturing method may include, for example, a step (3) of interconnecting conductor layers. In this step (3), usually, a conductor layer provided on one side of the insulating layer (for example, a conductor layer formed on the surface of the base material) is conducted to the other side of the conductor layer. This step (3) may include forming a via hole in the insulating layer, further forming a conductor layer at an appropriate position on the insulating layer including the position where the via hole is formed, and performing interlayer connection. . Further, the step (3) may include performing interlayer connection by polishing or grinding the insulating layer to expose the conductor layer formed on one side of the insulating layer.

  When performing interlayer connection using a via hole, for example, after forming a via hole in an insulating layer formed on a substrate with a wiring layer, a conductor layer is formed on the opposite side of the insulating layer from the substrate, I do. Examples of the method for forming the via hole include laser irradiation, etching, mechanical drilling, and the like. Among these, laser irradiation is preferable. This laser irradiation can be performed using an appropriate laser processing machine using an arbitrary light source such as a carbon dioxide laser, a YAG laser, or an excimer laser. For example, laser irradiation may be performed on the support side of the resin sheet to form a via hole that penetrates the support and the insulating layer and exposes the conductor layer on the substrate surface.

  Laser irradiation can be performed by an appropriate process according to the selected laser beam machine. The shape of the via hole is not particularly limited, but is generally circular or substantially circular. The shape of the via hole refers to the shape of the outline of the opening when viewed in the extending direction of the via hole.

  After forming the via hole, it is preferable to perform a step of removing smear in the via hole. This process is sometimes called a desmear process. For example, when the conductor layer is formed on the insulating layer by a plating process, wet desmear treatment may be performed on the via hole. In addition, when the conductor layer is formed on the insulating layer by a sputtering process, a dry desmear process such as a plasma treatment process may be performed. Furthermore, a roughening process may be performed on the insulating layer by a desmear process.

  Further, before the conductor layer is formed on the insulating layer, a roughening treatment may be performed on the insulating layer. According to this roughening treatment, the surface of the insulating layer including the inside of the via hole is generally roughened. As the roughening treatment, either dry or wet roughening treatment may be performed. Examples of the dry roughening treatment include plasma treatment. Moreover, as an example of a wet roughening process, the method of performing the swelling process by a swelling liquid, the roughening process by an oxidizing agent, and the neutralization process by a neutralization liquid in this order is mentioned.

  The surface roughness Ra of the surface of the insulating layer after the roughening treatment is preferably 350 nm or more, more preferably 400 nm or more, further preferably 450 nm or more, preferably 700 nm or less, more preferably 650 nm or less, and further preferably 600 nm or less. It is. The surface roughness Ra can be measured using a non-contact type surface roughness meter.

  After forming the via hole, a conductor layer is formed on the insulating layer. By forming the conductor layer at the position where the via hole is formed, the newly formed conductor layer and the conductor layer on the surface of the substrate are electrically connected, and interlayer connection is performed. Examples of the method for forming the conductor layer include a plating method, a sputtering method, a vapor deposition method, and the like, and among them, the plating method is preferable. In a preferred embodiment, the surface of the insulating layer is plated by an appropriate method such as a semi-additive method or a full additive method to form a conductor layer having a desired wiring pattern. Moreover, when the support body in a resin sheet is metal foil, the conductor layer which has a desired wiring pattern can be formed by a subtractive method. The material of the conductor layer to be formed may be a single metal or an alloy. Moreover, this conductor layer may have a single layer structure, or may have a multilayer structure including two or more layers of different kinds of materials.

  Here, the example of embodiment which forms a conductor layer on an insulating layer is demonstrated in detail. A plating seed layer is formed on the surface of the insulating layer by electroless plating. Next, a mask pattern for exposing a part of the plating seed layer is formed on the formed plating seed layer corresponding to a desired wiring pattern. An electrolytic plating layer is formed on the exposed plating seed layer by electrolytic plating. At this time, the filled via may be formed by filling the via hole by electrolytic plating together with the formation of the electrolytic plating layer. After the electrolytic plating layer is formed, the mask pattern is removed. Thereafter, an unnecessary plating seed layer can be removed by a process such as etching to form a conductor layer having a desired wiring pattern. In addition, when forming a conductor layer, the dry film used for formation of a mask pattern is the same as the said dry film.

  The conductor layer can include not only a linear wiring but also an electrode pad (land) on which an external terminal can be mounted, for example. Moreover, the conductor layer may be comprised only from the electrode pad.

  The conductor layer may be formed by forming an electrolytic plating layer and a filled via without using a mask pattern after the formation of the plating seed layer, and then performing patterning by etching.

  When interlayer connection is performed by polishing or grinding the insulating layer, for example, the insulating layer formed on the substrate with the wiring layer is polished or ground, and the conductor layer formed on the substrate is replaced with the insulating layer substrate. Expose to the opposite side. As the method for polishing and grinding the insulating layer, any method that can expose the conductor layer on the substrate surface can be used. Among them, a method in which a polished surface or a cut surface parallel to the layer plane of the insulating layer is obtained by polishing or grinding is preferable. Examples thereof include a chemical mechanical polishing method using a chemical mechanical polishing apparatus, a mechanical polishing method such as buffing, and a surface grinding method by rotating a grindstone. In addition, when performing interlayer connection by polishing or grinding the insulating layer, the process of removing smear, roughening, and forming a conductor layer on the insulating layer is performed in the same manner as when performing interlayer connection using via holes. May be. Moreover, it is not necessary to expose all the conductor layers on the surface of the base material, and a part thereof may be exposed.

  The circuit board manufacturing method may include, for example, a step (4) of removing the base material. By removing the base material, a circuit board having an insulating layer and a conductor layer embedded in the insulating layer can be obtained. This step (4) can be performed, for example, when a substrate having a peelable first metal layer and a second metal layer is used. A preferred example will be described below. A conductor layer is formed on the surface of the second metal layer of the substrate having the first metal layer and the second metal layer. Furthermore, a resin composition layer is formed on the second metal layer so that the conductor layer is embedded in the resin composition layer, and is thermally cured to obtain an insulating layer. Then, after performing interlayer connection as needed, parts other than the 2nd metal layer of a base material are peeled. Then, the second metal layer is removed by etching with an etchant such as an aqueous copper chloride solution. Thereby, the substrate is removed. Under the present circumstances, you may remove a base material in the state which protected the conductor layer with the protective film as needed.

  In other embodiments, the circuit board can be manufactured using a prepreg. The prepreg is obtained by impregnating a sheet-like fiber base material with a resin composition by a method such as a hot melt method or a solvent method. Examples of the sheet-like fiber base material include glass cloth, aramid nonwoven fabric, and liquid crystal polymer nonwoven fabric. From the viewpoint of thinning, the thickness of the sheet-like fiber substrate is preferably 900 μm or less, more preferably 800 μm or less, further preferably 700 μm or less, particularly preferably 600 μm or less, and preferably 1 μm or more. 1.5 μm or more and 2 μm or more. The thickness of this prepreg may be in the same range as the resin composition layer in the resin sheet described above. A method of manufacturing a circuit board using such a prepreg is basically the same as that using a resin sheet.

[16. Semiconductor chip package]
A semiconductor chip package according to the first embodiment of the present invention includes the circuit board described above and a semiconductor chip mounted on the circuit board. This semiconductor chip package can be manufactured by bonding a semiconductor chip to a circuit board.

  As a bonding condition between the circuit board and the semiconductor chip, any condition that allows the conductor connection between the terminal electrode of the semiconductor chip and the circuit wiring of the circuit board can be adopted. For example, conditions used in flip chip mounting of a semiconductor chip can be adopted. Further, for example, the semiconductor chip and the circuit board may be bonded via an insulating adhesive.

  As an example of the bonding method, there is a method in which a semiconductor chip is pressure-bonded to a circuit board. As the crimping conditions, the crimping temperature is usually in the range of 120 ° C to 240 ° C (preferably in the range of 130 ° C to 200 ° C, more preferably in the range of 140 ° C to 180 ° C), and the crimping time is usually in the range of 1 second to 60 seconds. (Preferably 5 to 30 seconds).

  Another example of the bonding method is a method in which a semiconductor chip is reflowed and bonded to a circuit board. Reflow conditions are good also as the range of 120 to 300 degreeC.

  After the semiconductor chip is bonded to the circuit board, the semiconductor chip may be filled with a mold underfill material. As the mold underfill material, the above-described resin composition may be used, or the above-described resin sheet may be used.

  The semiconductor chip package according to the second embodiment of the present invention includes a semiconductor chip and a cured product of the resin composition that seals the semiconductor chip. In such a semiconductor chip package, the cured product of the resin composition usually functions as a sealing layer. As a semiconductor chip package according to the second embodiment, for example, a Fan-out type WLP can be cited.

  FIG. 1 is a cross-sectional view schematically showing a Fan-out type WLP as an example of a semiconductor chip package according to a second embodiment of the present invention. A semiconductor chip package 100 as a fan-out type WLP includes, for example, a semiconductor chip 110; a sealing layer 120 formed so as to cover the periphery of the semiconductor chip 110; and a sealing layer of the semiconductor chip 110, as shown in FIG. A rewiring layer 130 as an insulating layer; a rewiring layer 140 as a conductor layer; a solder resist layer 150; and a bump 160 are provided on the surface opposite to 120.

A manufacturing method of such a semiconductor chip package is as follows:
(A) Laminating a temporary fixing film on a substrate;
(B) a step of temporarily fixing the semiconductor chip on the temporary fixing film;
(C) forming a sealing layer on the semiconductor chip;
(D) The process of peeling a base material and a temporary fixing film from a semiconductor chip,
(E) a step of forming a rewiring forming layer as an insulating layer on the surface of the semiconductor chip substrate and the temporarily fixed film peeled off,
(F) forming a rewiring layer as a conductor layer on the rewiring formation layer; and
(G) forming a solder resist layer on the rewiring layer;
including. Further, the manufacturing method of the semiconductor chip package is as follows.
(H) A step of dicing a plurality of semiconductor chip packages into individual semiconductor chip packages and separating them into individual pieces may be included. Hereinafter, this manufacturing method will be described in detail.

(Process (A))
Step (A) is a step of laminating a temporary fixing film on a base material. The lamination conditions of the base material and the temporary fixing film may be the same as the lamination conditions of the base material and the resin sheet in the circuit board manufacturing method.

  Examples of base materials include silicon wafers; glass wafers; glass substrates; metal substrates such as copper, titanium, stainless steel, cold rolled steel plate (SPCC); Examples include a substrate subjected to thermosetting treatment; a substrate made of bismaleimide triazine resin such as BT resin; and the like.

  The temporary fixing film can be made of any material that can be peeled off from the semiconductor chip and can temporarily fix the semiconductor chip. Examples of commercially available products include “Riva Alpha” manufactured by Nitto Denko Corporation.

(Process (B))
Step (B) is a step of temporarily fixing the semiconductor chip on the temporary fixing film. The temporary fixing of the semiconductor chip can be performed by using a device such as a flip chip bonder or a die bonder, for example. The layout and number of semiconductor chips can be appropriately set according to the shape and size of the temporarily fixed film, the number of target semiconductor packages produced, and the like. For example, the semiconductor chips may be aligned and temporarily fixed in a matrix of a plurality of rows and a plurality of columns.

(Process (C))
Step (C) is a step of forming a sealing layer on the semiconductor chip. The sealing layer is formed by a cured product of the resin composition described above. The sealing layer is usually formed by a method including a step of forming a resin composition layer on a semiconductor chip and a step of thermosetting the resin composition layer to form a sealing layer.

  Formation of the resin composition layer on the semiconductor chip is usually performed using the above-described resin sheet. Specifically, the resin composition layer is formed on the semiconductor chip by laminating the resin composition layer of the resin sheet and the semiconductor chip. Since the resin composition described above usually has a low minimum melt viscosity, the semiconductor chip can be satisfactorily sealed by the above lamination.

  Lamination of the semiconductor chip and the resin sheet is performed by, for example, bonding the resin composition layer to the semiconductor chip by removing the protective film of the resin sheet and then heat-pressing the resin sheet to the semiconductor chip from the support side. Can do. Examples of the thermocompression bonding member for thermocompression bonding the resin sheet to the semiconductor chip include a heated metal plate (SUS mirror plate or the like), a metal roll (SUS roll), or the like. Note that it is preferable that the thermocompression-bonding member is not pressed directly on the resin sheet, but is pressed via an elastic material such as heat-resistant rubber so that the resin sheet sufficiently follows the surface irregularities of the semiconductor chip.

  Further, the lamination of the semiconductor chip and the resin sheet may be performed by, for example, a vacuum laminating method after removing the protective film of the resin sheet. The lamination conditions in the vacuum laminating method can be the same as the lamination conditions of the base material and the resin sheet in the circuit board manufacturing method.

  The support of the resin sheet may be peeled off before laminating the resin sheet on the semiconductor chip, or may be peeled off after laminating the semiconductor chip and the resin sheet and before thermosetting the resin composition layer. Alternatively, the semiconductor chip and the resin sheet may be laminated and the resin composition layer may be thermally cured and then peeled off.

  Moreover, you may perform formation of the resin composition layer on a semiconductor chip using the resin composition mentioned above. Specifically, you may carry out by apply | coating a resin composition on a semiconductor chip. The application conditions for the resin composition may be the same as the application conditions for forming the resin composition layer in the method for producing a resin sheet.

  After forming the resin composition layer on the semiconductor chip, the resin composition layer is thermally cured to obtain a sealing layer that covers the semiconductor chip. Thereby, the semiconductor chip is sealed with the cured product of the resin composition. The thermosetting conditions for the resin composition layer may be the same as the thermosetting conditions for the resin composition layer in the method for manufacturing a circuit board. Furthermore, before the resin composition layer is thermally cured, the resin composition layer may be subjected to a preheating treatment in which the resin composition layer is heated at a temperature lower than the curing temperature. The processing conditions for the preheating process may be the same as the preheating process in the circuit board manufacturing method.

(Process (D))
A process (D) is a process of peeling a base material and a temporary fixing film from a semiconductor chip. As the peeling method, it is desirable to adopt an appropriate method according to the material of the temporarily fixed film. As a peeling method, the method of peeling by heating, foaming, or expanding a temporarily fixed film is mentioned, for example. Moreover, as a peeling method, the method of irradiating a temporarily fixed film with an ultraviolet-ray through a base material and reducing the adhesive force of a temporarily fixed film and peeling is mentioned, for example.

In the method in which the temporarily fixed film is peeled by heating, foaming or expanding, the heating condition is usually 100 ° C. to 250 ° C. for 1 second to 90 seconds or 5 minutes to 15 minutes. Further, in the method for peeling by reducing the adhesive strength of the temporary fixing film by ultraviolet irradiation, irradiation amount of ultraviolet rays is ^{usually, 10mJ / cm 2 ~1000mJ / cm} 2.

(Process (E))
The step (E) is a step of forming a rewiring forming layer as an insulating layer on the surface from which the base material and the temporary fixing film of the semiconductor chip are peeled off.

  As the material of the rewiring formation layer, any material having an insulating property when the rewiring formation layer is formed can be used. Among these, a photosensitive resin and a thermosetting resin are preferable from the viewpoint of easy manufacture of the semiconductor chip package. Moreover, you may use the resin composition of this invention as this thermosetting resin.

  After forming the rewiring layer, via holes may be formed in the rewiring layer in order to connect the semiconductor chip and the rewiring layer.

  In the method of forming a via hole when the material of the rewiring layer is a photosensitive resin, normally, the surface of the rewiring layer is irradiated with active energy rays through a mask pattern, and the rewiring layer in the irradiated portion is irradiated with light. Harden. Examples of active energy rays include ultraviolet rays, visible rays, electron beams, X-rays and the like, and ultraviolet rays are particularly preferable. The irradiation amount and irradiation time of ultraviolet rays can be appropriately set according to the photosensitive resin. As an exposure method, for example, a contact exposure method in which a mask pattern is brought into close contact with the rewiring formation layer and exposed, a non-contact exposure method in which the mask pattern is exposed using parallel rays without being brought into close contact with the rewiring formation layer, etc. Is mentioned.

  After the rewiring formation layer is photocured, the rewiring formation layer is developed, the unexposed portion is removed, and a via hole is formed. Development may be either wet development or dry development. Examples of the developing method include a dip method, a paddle method, a spray method, a brushing method, a scraping method, and the like, and the paddle method is preferable from the viewpoint of resolution.

  Examples of a method for forming a via hole when the material of the rewiring forming layer is a thermosetting resin include laser irradiation, etching, and mechanical drilling. Among these, laser irradiation is preferable. Laser irradiation can be performed using an appropriate laser processing machine using a light source such as a carbon dioxide laser, a UV-YAG laser, or an excimer laser.

  The shape of the via hole is not particularly limited, but is generally circular or substantially circular. The top diameter of the via hole is preferably 50 μm or less, more preferably 30 μm or less, further preferably 20 μm or less, preferably 3 μm or more, preferably 10 μm or more, more preferably 15 μm or more. Here, the top diameter of the via hole means the diameter of the opening of the via hole on the surface of the rewiring formation layer.

(Process (F))
Step (F) is a step of forming a rewiring layer as a conductor layer on the rewiring formation layer. The method for forming the rewiring layer on the rewiring formation layer can be the same as the method for forming the conductor layer on the insulating layer in the method for manufacturing a circuit board. Alternatively, the step (E) and the step (F) may be repeated to build up the rewiring layer and the rewiring forming layer alternately (build up).

(Process (G))
Step (G) is a step of forming a solder resist layer on the rewiring. As a material for the solder resist layer, any material having an insulating property when the solder resist layer is formed can be used. Among these, a photosensitive resin and a thermosetting resin are preferable from the viewpoint of easy manufacture of the semiconductor chip package. Moreover, you may use the resin composition of this invention as a thermosetting resin.

  Further, in the step (G), a bumping process for forming bumps may be performed as necessary. The bumping process can be performed by a method such as solder ball or solder plating. In addition, the via hole can be formed in the bumping process in the same manner as in the step (E).

(Process (H))
The manufacturing method of the semiconductor chip package may include a step (H) in addition to the steps (A) to (G). Step (H) is a step of dicing a plurality of semiconductor chip packages into individual semiconductor chip packages and dividing them into individual pieces. A method for dicing the semiconductor chip package into individual semiconductor chip packages is not particularly limited.

  The semiconductor chip package according to the third embodiment of the present invention includes, for example, a rewiring layer 130 or a solder resist layer 150 as a cured product of the resin composition of the present invention in a semiconductor chip package 100 as shown in FIG. The semiconductor chip package formed in

[17. Semiconductor device]
Examples of the semiconductor device on which the above-described semiconductor chip package is mounted include, for example, electrical products (for example, computers, mobile phones, smartphones, tablet devices, wearable devices, digital cameras, medical devices, and televisions) and vehicles (for example, , Various semiconductor devices used for motorcycles, automobiles, trains, ships, airplanes, and the like).

  Hereinafter, the present invention will be specifically described with reference to examples. However, the present invention is not limited to the following examples. In the following description, “parts” and “%” representing amounts mean “parts by mass” and “% by mass”, respectively, unless otherwise specified. Further, the operations described below were performed in an environment of normal temperature and pressure unless otherwise specified.

[Synthesis Example 1]
In a reaction vessel, 69 g of a bifunctional hydroxy group-terminated polybutadiene (“G-3000” manufactured by Nippon Soda Co., Ltd., number average molecular weight = 3000, hydroxy group equivalent = 1800 g / eq.) And an aromatic hydrocarbon mixed solvent (Idemitsu Petroleum) 40 g of “Ipsol 150” manufactured by Kagaku Co., Ltd. and 0.005 g of dibutyltin laurate were added and mixed to dissolve uniformly. When it became uniform, the temperature was raised to 50 ° C., and 8 g of isophorone diisocyanate (“IPDI” manufactured by Evonik Degussa Japan, isocyanate group equivalent = 113 g / eq.) Was added while stirring, and the reaction was carried out for about 3 hours.

The resulting reaction was then cooled to room temperature. To the cooled reaction product, 23 g of cresol novolak resin (“KA-1160” manufactured by DIC, hydroxyl group equivalent = 117 g / eq.) And 60 g of ethyl diglycol acetate (manufactured by Daicel) were added and stirred at 80 ° C. The reaction was continued for about 4 hours. The disappearance of the NCO peak at 2250 cm ⁻¹ was confirmed by FT-IR. The confirmation of the disappearance of the NCO peak was regarded as the end point of the reaction, and the reaction was cooled to room temperature. Then, the reaction product was filtered through a 100-mesh filter cloth to obtain an elastomer A having a butadiene structure and a phenolic hydroxyl group (phenolic hydroxyl group-containing butadiene resin: nonvolatile component 50% by mass). The number average molecular weight of the elastomer A was 5500, and the glass transition temperature was −5 ° C.

[Synthesis Example 2]
To a flask equipped with a stirrer, a thermometer, and a condenser, 368.41 g of ethyl diglycol acetate and 368.41 g of an aromatic solvent (“Solvesso 150” manufactured by ExxonMobil) were charged as a solvent. Furthermore, 100.1 g (0.4 mol) of diphenylmethane diisocyanate and polycarbonate diol (“C-2015N” manufactured by Kuraray Co., Ltd., number average molecular weight: about 2000, hydroxyl group equivalent = 1000 g / eq., Nonvolatile component: 100%) 400 g (0.2 mol) was charged and reacted at 70 ° C. for 4 hours.

Next, 195.9 g (0.2 mol) of nonylphenol novolak resin (hydroxyl equivalent = 229.4 g / eq, average 4.27 functional, average calculated molecular weight 979.5 g / mol) and ethylene glycol bis Anhydrotrimellitate 41.0 g (0.1 mol) was charged, heated to 150 ° C. over 2 hours, and allowed to react for 12 hours. The disappearance of the NCO peak at 2250 cm ⁻¹ was confirmed by FT-IR. The confirmation of the disappearance of the NCO peak was regarded as the end point of the reaction, and the reaction was cooled to room temperature. And it filtered with the filter cloth of 100 meshes, and obtained the elastomer B (nonvolatile component 50 mass%) which has a carbonate structure. The number average molecular weight of the elastomer B was 6100, and the glass transition temperature was 5 ° C.

[Example 1]
Liquid epoxy resin (“ZX1059” manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., 1: 1 mixture (mass ratio) of bisphenol A type epoxy resin and bisphenol F type epoxy resin, epoxy equivalent: 169 g / eq.) 25 parts at 25 ° C. , 5 parts of glycidylamine type epoxy resin (“ELM-100” manufactured by Sumitomo Chemical Co., Ltd., epoxy equivalent 107 g / eq.), 20 parts of biphenyl type epoxy resin (“NC3000L” manufactured by Nippon Kayaku Co., Ltd., 269 g / eq. Of epoxy equivalent) , Spherical silica surface treated with 3 parts of amphiphilic polyether block copolymer (“Fortegra 100” manufactured by Dow Chemical Co., number average molecular weight 6700), phenylaminosilane coupling agent (“KBM573” manufactured by Shin-Etsu Chemical Co., Ltd.) Particle size 0.5μm, “SO-C2” manufactured by Admatechs 380 parts, active ester compound (“HPC-8000-65T” manufactured by DIC, toluene solution of 65% by mass of non-volatile component having an active group equivalent of about 223 g / eq.) 7.7 parts, phenol novolac-based curing agent containing triazine skeleton ("LA-7054" manufactured by DIC, hydroxyl group equivalent of about 125 g / eq., MEK solution with 60% nonvolatile component), 8.3 parts, phenoxy resin ("YX7553BH30" manufactured by Mitsubishi Chemical Corporation), cyclohexanone with 30% by mass nonvolatile component: 16.6 parts of a methyl ethyl ketone (MEK) 1: 1 solution), flame retardant (“HCA-HQ” manufactured by Sanko Co., Ltd., 10- (2,5-dihydroxyphenyl) -10-hydro-9-oxa-10-phosphor phenanthrene-10-oxide, average particle diameter 2 [mu] m) 5 parts carbon black A (DBP absorption 120 cm ^3/10 0 g, pH = 6.5, average particle size 20 nm) 1.5 parts, curing accelerator (“1B2PZ” manufactured by Shikoku Kasei Kogyo Co., Ltd., 1-benzyl-2-phenylimidazole) 0.3 part, methyl ethyl ketone 25 parts, and Then, 25 parts of cyclohexanone was mixed and dispersed uniformly using a high-speed rotary mixer to obtain a mixture. The mixture was filtered through a cartridge filter (“SHP050” manufactured by ROKITECHNO) to prepare resin varnish 1.

  The amphiphilic polyether block copolymer (“Fortegra 100” manufactured by Dow Chemical Co.) is a liquid resin at room temperature of about 25 ° C., and therefore its glass transition temperature is 30 ° C. or less.

[Example 2]
The amount of carbon black A was changed from 1.5 parts to 1.0 part. A resin varnish 2 was prepared in the same manner as in Example 1 except for the above items.

[Example 3]
At 25 ° C., 10 parts of a liquid epoxy resin (“ZX1059” manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., 1: 1 mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin (mass ratio), epoxy equivalent: 169 g / eq), 5 parts of glycidylamine type epoxy resin (“ELM-100” manufactured by Sumitomo Chemical Co., Ltd., epoxy equivalent 107 g / eq.), 7 parts of naphthalene type epoxy resin (“HP4032SS” manufactured by DIC, 151 g / eq. Of epoxy equivalent), synthesis example 16 parts of elastomer A (non-volatile component 50% by mass) prepared in 1 and spherical silica (average particle size 0.5 μm, Admatechs) surface-treated with a phenylaminosilane coupling agent (“KBM573” manufactured by Shin-Etsu Chemical Co., Ltd.) "SO-C2") 310 parts, active ester compound (DIC Corporation "HPC-8000-6" T ”, active group equivalent of about 223 g / eq., 7.7 parts of toluene solution of 65% by mass of non-volatile components, triazine skeleton-containing phenol novolac-based curing agent (“ LA-7054 ”manufactured by DIC, hydroxyl group equivalent of about 125 g / eq. , 60% MEK solution) 25 parts of non-volatile components, carbon black a (DBP absorption 120cm ³ /100g,pH=6.5, average particle size 20 nm) 4 parts, the curing accelerator (Shikoku Chemicals Corporation, "1B2PZ" , 1-benzyl-2-phenylimidazole) and 20 parts of methyl ethyl ketone were mixed and dispersed uniformly with a high-speed rotary mixer to obtain a mixture. This mixture was filtered through a cartridge filter (“SHP050” manufactured by ROKITECHNO) to prepare a resin varnish 3.

[Example 4]
The amount of carbon black A was changed from 4 parts to 2 parts. The amount of methyl ethyl ketone was changed from 20 parts to 25 parts. A resin varnish 4 was prepared in the same manner as in Example 3 except for the above items.

[Example 5]
Instead of carbon black A 1.5 parts of carbon black B were used (DBP absorption 70cm ³ /100g,pH=3.5, average particle size 20 nm) 4 parts. A resin varnish 5 was prepared in the same manner as in Example 1 except for the above items.

[Example 6]
Instead of carbon black A 4 parts of carbon black B were used (DBP absorption 70cm ³ /100g,pH=3.5, average particle diameter 20 nm) 2.5 parts. The amount of methyl ethyl ketone was changed from 20 parts to 25 parts. A resin varnish 6 was prepared in the same manner as in Example 3 except for the above items.

[Example 7]
Instead of 16 parts of elastomer A (non-volatile component 50% by mass) prepared in Synthesis Example 1, 16 parts of elastomer B (non-volatile content 50% by mass) prepared in Synthesis Example 2 was used. Also, the amount of carbon black A was changed from 4 parts to 2 parts. Further, the amount of methyl ethyl ketone was changed from 20 parts to 25 parts. A resin varnish 7 was prepared in the same manner as in Example 3 except for the above items.

[Example 8]
The amount of liquid epoxy resin (“ZX1059” manufactured by Nippon Steel & Sumikin Chemical Co., Ltd.) was changed from 25 parts to 22 parts. In place of the carbon black A 1.5 parts of carbon black B were used (DBP absorption 70cm ³ /100g,pH=3.5, average particle size 20 nm) 4 parts. Furthermore, 3 parts of a rubber elastic epoxy resin (“YX7400” manufactured by Mitsubishi Chemical Corporation, epoxy equivalent 410 g / eq.) Was further added as a material for the resin varnish. Except for the above, the same operation as in Example 1 was performed to prepare a resin varnish 8.

[Comparative Example 1]
An active ester compound (“HPC-8000-65T” manufactured by DIC) was not used. In addition, the amount of triazine skeleton-containing phenol novolac curing agent (“LA-7054” manufactured by DIC, non-volatile content 60%) was changed from 8.3 parts to 16.6 parts. Further, instead of the carbon black A 1.5 parts were used carbon black C a (DBP absorption ^{140cm 3 / 100g, pH = 8} , average particle size 20 nm) 1.5 parts. Except for the above, the same operation as in Example 1 was performed to prepare a resin varnish 9.

[Comparative Example 2]
An active ester compound (“HPC-8000-65T” manufactured by DIC) was not used. The amount of the triazine skeleton-containing phenol novolac curing agent (“LA-7054” manufactured by DIC, non-volatile content 60%) was changed from 25 parts to 33.3 parts. Further, instead of the carbon black A 4 parts, was used carbon black C a (DBP absorption ^{140cm 3 / 100g, pH = 8} , average particle size 20 nm) 4 parts. The amount of methyl ethyl ketone was changed from 20 parts to 25 parts. A resin varnish 10 was prepared in the same manner as in Example 3 except for the above items.

[Comparative Example 3]
The active ester compound (“HPC-8000-65T” manufactured by DIC) was not used. Changed from 3 parts to 16.6 parts. Further, instead of the carbon black A 1.5 parts were used carbon black C a (DBP absorption ^{140cm 3 / 100g, pH = 8} , average particle size 20 nm) 0.6 parts. Further, the amount of the curing accelerator (“1B2PZ” manufactured by Shikoku Kasei Kogyo Co., Ltd.) was changed from 0.3 part to 0.7 part. A resin varnish 11 was prepared in the same manner as in Example 1 except for the above items.

[Comparative Example 4]
An active ester compound (“HPC-8000-65T” manufactured by DIC) was not used. The amount of the triazine skeleton-containing phenol novolac curing agent (“LA-7054” manufactured by DIC, non-volatile content 60%) was changed from 25 parts to 33.3 parts. Further, instead of the carbon black A 4 parts, was used carbon black C a (DBP absorption ^{140cm 3 / 100g, pH = 8} , average particle size 20 nm) 1.3 parts. The amount of methyl ethyl ketone was changed from 20 parts to 25 parts. A resin varnish 12 was prepared in the same manner as in Example 3 except for the above items.

[Comparative Example 5]
Instead of carbon black A 1.5 parts were used carbon black C a (DBP absorption ^{140cm 3 / 100g, pH = 8} , average particle size 20 nm) 1.5 parts. Except for the above, the same operation as in Example 1 was performed to prepare a resin varnish 13.

[Evaluation of carbon black defects in resin composition layer]
A polyethylene terephthalate film (“PET501010” manufactured by Lintec Corporation, thickness 50 μm) having a release treatment on the surface was prepared as a support. The resin varnishes prepared in Examples and Comparative Examples were uniformly applied to the release surface of this support so that the thickness of the resin composition layer after drying was 50 μm, and 80 ° C. to 120 ° C. (average 100 ° C. ) For 5 minutes to obtain a resin sheet having a width of 30 cm and a length of 30 cm.

  While applying a light source, the resin sheet was observed from the support side using a digital microscope (“VH-Z20R” manufactured by Keyence Corporation) to examine the presence or absence of carbon black aggregates. The case where there was an aggregate having a maximum aggregate length exceeding 100 μm was determined as “x”, and the case where there was no aggregate was determined as “◯”.

[Measurement of ΔL * and Δb * of insulating layer]
A polyethylene terephthalate film (“PET501010” manufactured by Lintec Corporation, thickness 50 μm) having a release treatment on the surface was prepared as a support. The resin varnishes prepared in Examples and Comparative Examples were uniformly applied to the release surface of this support so that the thickness of the resin composition layer after drying was 100 μm, and 80 ° C. to 120 ° C. (average 100 ° C. ) For 5 minutes to obtain a resin sheet.

  Using the batch-type vacuum pressure laminator (“MVLP-500” manufactured by Meiki Co., Ltd.), the resin composition layer of the resin sheet is brought into contact with both surfaces of the copper-clad laminate. Laminated. Lamination was performed by reducing the pressure for 30 seconds to a pressure of 13 hPa or less, and then pressure bonding at 100 ° C. and a pressure of 0.74 MPa for 30 seconds. After lamination, the support was removed. Thereafter, the resin composition layer was cured by heating at 100 ° C. for 30 minutes and then at 180 ° C. for 30 minutes to form an insulating layer.

Between the obtained insulating layer ^L * ^a * ^{b *} coordinates in color system ^{L *} and ^{b *,} the difference [Delta] L ^* and the coordinates ^{L *} and ^{b *} in ^{the L} * ^a * ^{b *} color system of the white standard plate Δb ^* was measured using a color difference meter (“CR-10” manufactured by Konica Minolta Japan). An aluminum oxide white plate was used as the white standard plate.

[Measurement of glass transition temperature of cured product of resin composition]
A polyethylene terephthalate film (“PET501010” manufactured by Lintec Corporation, thickness 50 μm) having a release treatment on the surface was prepared as a support. The resin varnishes prepared in Examples and Comparative Examples were uniformly applied to the release surface of this support so that the thickness of the resin composition layer after drying was 100 μm, and 80 ° C. to 120 ° C. (average 100 ° C. ) For 5 minutes to obtain a resin sheet.

  The resin sheet was heated in an oven at 180 ° C. for 90 minutes to thermally cure the resin composition layer, thereby obtaining a cured product layer of the resin composition. The support was peeled from the cured product layer, and the cured product layer was cut to obtain a test piece having a width of about 5 mm and a length of about 15 mm. About this test piece, the thermomechanical analysis was performed with the tension | pulling load method using the thermo equipment analyzer ("Thermo Plus TMA8310" by Rigaku). Specifically, after the test piece was mounted on the thermomechanical analyzer, the measurement was continuously performed twice under the measurement conditions of a load of 1 g and a heating rate of 5 ° C./min. In the second measurement, the glass transition temperature Tg (° C.) was calculated.

[Measurement of minimum melt viscosity of resin composition]
A polyethylene terephthalate film (“PET501010” manufactured by Lintec Corporation, thickness 50 μm) having a release treatment on the surface was prepared as a support. The resin varnishes prepared in Examples and Comparative Examples were uniformly applied to the release surface of this support so that the thickness of the resin composition layer after drying was 100 μm, and 80 ° C. to 120 ° C. (average 100 ° C. ) For 5 minutes to obtain a resin sheet.

  After peeling the support, the resin composition layer was compressed with a mold to prepare measurement pellets (diameter 18 mm, 1.2 g to 1.3 g). Then, about this pellet for a measurement, the minimum melt viscosity was measured using the dynamic viscoelasticity measuring apparatus ("Rhesol-G3000" by BM company). Specifically, for 1 g of measurement pellets, using a parallel plate with a diameter of 18 mm, the dynamic viscoelastic modulus was measured by raising the temperature in a temperature range from 60 ° C. to 200 ° C., and the minimum melt viscosity ( (poise) was calculated. The measurement conditions were a temperature increase rate of 5 ° C./min, a measurement temperature interval of 2.5 ° C., a frequency of 1 Hz, and a strain of 1 deg.

[result]
The results of the above-described examples and comparative examples are shown in the following table. In the following table, the amount of each component represents parts by mass of the non-volatile component. In the table below, the meanings of the abbreviations are as follows.
ZX1059: Liquid epoxy resin (“ZX1059” manufactured by Nippon Steel & Sumikin Chemical Co., Ltd., 1: 1 mixture of bisphenol A type epoxy resin and bisphenol F type epoxy resin (mass ratio), epoxy equivalent: 169 g / eq.).
ELM-100: Glycidylamine type epoxy resin (“ELM-100” manufactured by Sumitomo Chemical Co., Ltd., epoxy equivalent of 107 g / eq.).
HP4032SS: Naphthalene type epoxy resin (“HP4032SS” manufactured by DIC, epoxy equivalent 151 g / eq.).
YX7400: Rubber elastic epoxy resin (“YX7400” manufactured by Mitsubishi Chemical Corporation, epoxy equivalent 410 g / eq.).
NC3000L: biphenyl type epoxy resin (“NC3000L” manufactured by Nippon Kayaku Co., Ltd., epoxy equivalent: 269 g / eq.).
SO-C2: Spherical silica surface treated with a phenylaminosilane coupling agent (“KBM573” manufactured by Shin-Etsu Chemical Co., Ltd.) (average particle size 0.5 μm, “SO-C2” manufactured by Admatechs).
CB-A: Carbon black A (DBP absorption 120cm ³ /100g,pH=6.5, average particle size 20 nm).
CB-B: Carbon black B (DBP absorption 70cm ³ /100g,pH=3.5, average particle size 20 nm).
CB-C: Carbon Black C (DBP absorption ^{140cm 3 / 100g, pH = 8} , average particle size 20 nm).
Elastomer A: Elastomer having a butadiene structure and a phenolic hydroxyl group produced in Synthesis Example 1 (nonvolatile content 50 mass%, number average molecular weight 5500, glass transition temperature −5 ° C.).
Elastomer B: Elastomer having a carbonate structure produced in Synthesis Example 2 (non-volatile content 50 mass%, number average molecular weight 6100, glass transition temperature 5 ° C.).
fortegra 100: Amphiphilic polyether block copolymer that is liquid at 20 ° C. (“Fortegra 100” manufactured by Dow Chemical Co., number average molecular weight 6700).
HPC-8000: Active ester compound (“HPC-8000-65T” manufactured by DIC, toluene solution with a non-volatile content of 65% by mass with an active group equivalent of about 223 g / eq.).
LA-7054: Triazine skeleton-containing phenol novolac curing agent (“LA-7054” manufactured by DIC, hydroxyl equivalent of about 125 g / eq., Methyl ethyl ketone solution having a nonvolatile content of 60%).
1B2PZ: curing accelerator (“1B2PZ”, 1-benzyl-2-phenylimidazole, manufactured by Shikoku Kasei Kogyo Co., Ltd.).
YX7553BH30: Phenoxy resin (“YX7553BH30” manufactured by Mitsubishi Chemical Corporation, 1: 1 solution of cyclohexanone: methyl ethyl ketone (MEK) having a nonvolatile content of 30% by mass).
HCA-HQ: flame retardant (“HCA-HQ” manufactured by Sanko Co., Ltd., 10- (2,5-dihydroxyphenyl) -10-hydro-9-oxa-10-phosphaphenanthrene-10-oxide, average particle diameter 2 μm).
CB defect: Carbon black defect.

[Consideration]
As can be seen from Tables 1 and 2, in the examples using (C) carbon black having a DBP absorption amount within a predetermined range, (C) comparable to or more than the comparative examples using carbon black other than carbon black. Excellent color development, minimum melt viscosity and glass transition temperature can be obtained, and furthermore, the occurrence of defects due to carbon black aggregation can be suppressed. From this result, it was confirmed that the present invention can realize a resin composition capable of suppressing the aggregation of carbon black while being balanced in characteristics such as color development, minimum melt viscosity and glass transition temperature.

  In addition, the present inventors repeated the above-described experiments of Examples 1 to 8 until carbon black aggregates were generated. As a result, in Examples 5, 6 and 8 using carbon black B, the number of experiments to be performed before carbon black aggregates was larger than in Examples 1 to 4 and 7 using carbon black A. It was. This result indicates that the use of carbon black B more effectively suppresses the aggregation of carbon black and the frequency of occurrence of aggregates can be lowered than the use of carbon black A.

DESCRIPTION OF SYMBOLS 100 Semiconductor chip package 110 Semiconductor chip 120 Sealing layer 130 Rewiring formation layer 140 Rewiring layer 150 Solder resist layer 160 Bump

Claims (17)

(A) an epoxy resin, (B) a mineral filler comprises (C) DBP absorption amount is less 130 cm ^3/100 g carbon black, and, (D) a glass transition temperature of 30 ° C. or less of the polymer resin, the resin Composition.   (B) The resin composition of Claim 1 whose quantity of a component is 30 to 95 mass% with respect to 100 mass% of non-volatile components in a resin composition.   (B) The resin composition of Claim 1 or 2 whose quantity of a component is 75 to 95 mass% with respect to 100 mass% of non-volatile components in a resin composition.   The resin composition according to any one of claims 1 to 3, wherein the component (A) comprises (A-1) a nitrogen-containing epoxy resin or an epoxy resin having a condensed ring structure.   The component (D) is selected from the group consisting of a polybutadiene structure, a polysiloxane structure, a polyalkylene structure, a polyalkyleneoxy structure, a polyisoprene structure, a polyisobutylene structure, a polycarbonate structure, and a polyacrylic structure in the molecule. The resin composition of any one of Claims 1-4 which has the above structure.   (D) The resin composition of any one of Claims 1-5 in which a component has a functional group which can react with (A) component.   The component (D) has one or more types of functional groups selected from the group consisting of a hydroxyl group, an acid anhydride group, a phenolic hydroxyl group, an epoxy group, an isocyanate group, and a urethane group. 2. The resin composition according to item 1.   (D) The resin composition of any one of Claims 1-7 whose number average molecular weights of a component are 4000-100000.   (D) The resin composition of any one of Claims 1-8 whose quantity of a component is 0.2 mass% or more and 20 mass% or less with respect to 100 mass% of non-volatile components in a resin composition. object.   (C) The resin composition of any one of Claims 1-9 whose quantity of a component is 0.1 to 3 mass% with respect to 100 mass% of non-volatile components in a resin composition. object.   The resin composition according to claim 1, which is a resin composition for an insulating layer of a semiconductor chip package.   The resin composition as described in any one of Claims 1-11 which is a resin composition for semiconductor sealing.   The resin sheet which has a support body and the resin composition layer containing the resin composition of any one of Claims 1-12 provided on this support body.   The resin sheet according to claim 13, which is a resin sheet for an insulating layer of a semiconductor chip package.   The circuit board containing the insulating layer formed with the hardened | cured material of the resin composition of any one of Claims 1-12.   A semiconductor chip package comprising the circuit board according to claim 15 and a semiconductor chip mounted on the circuit board.   The semiconductor chip package containing a semiconductor chip and the hardened | cured material of the resin composition of any one of Claims 1-12 which seals the said semiconductor chip.

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