KR20070089053A - Thermosetting resin compositions, resin films in b-stage and build-up multi-layer board - Google Patents

Abstract

Provided are a thermosetting resin composition which is excellent in the balance of elasticity, rupture strength and rupture elongation, a B-staged resin film prepared from the composition, and a multilayered build-up substrate containing the resin film. A thermosetting resin composition comprises an epoxy resin containing 50-100 wt% of a liquid epoxy resin having a viscosity of 1.0-120 Pa.s at 25 deg.C; a triazine-modified phenol novolac resin curing agent; and 10-250 parts by weight of a solvent-soluble polyimide resin based on 100 parts by weight of the epoxy resin and the triazine modified phenol novolac resin curing agent. Preferably the thermosetting resin composition comprises further at least one filler selected from silica, alumina, aluminum nitride, boron nitride and magnesium oxide.

Description

Thermosetting resin composition, wet-stage resin film and multilayer build-up substrate {THERMOSETTING RESIN COMPOSITIONS, RESIN FILMS IN B-STAGE AND BUILD-UP MULTI-LAYER BOARD}

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a B-staged resin film, which has a low expansion coefficient and is used for a low density-high adhesion strength, high heat resistance, high reliability, high density build-up printed wiring board, and the like. Here, B-stage refers to the state which semi-hardened the resin composition.

In recent years, package substrates for MPUs and ASICs require thinning, narrow pad pitches of small diameters, multilayering, shortening of connections, and low transmission loss. For this purpose, high-density build-up boards or high-density batch-forming boards are required for the substrate structure, and the subtractive method to the (semi) additive method is required for thinning, and the small diameter laser via is required for the narrow pad pitch of the small diameter. In addition, connection in the thickness direction also requires connection by a stack via or the like. For this reason, the main characteristics required for the substrate material are high peel strength due to the low coarsening corresponding to the (semi) additive method for thinning, laser processing and reliability improvement at small diameters, and low precision for improving the dimensional accuracy and position accuracy. It has balanced resin properties such as expansion coefficient, elastic modulus, breaking strength, and elongation at break, and has a low dielectric constant and low dielectric constant. Among them, the importance of low dielectric constant and low dielectric loss tangent is reduced because the method of improving the performance of the MPU has shifted from the higher frequency to the higher parallelism. As such a film product, the thing of patent documents 1-11 is known, for example.

(Patent Document 1) Japanese Patent Application Laid-Open No. 11-1547

(Patent Document 2) Japanese Patent Application Laid-Open No. 11-87927

(Patent Document 3) Japanese Patent Publication 2000-17148

(Patent Document 4) Japanese Patent Publication 2000-198907

(Patent Document 5) Japanese Patent Publication 2003-238772

(Patent Document 6) Japanese Patent Publication 2001-181375

(Patent Document 7) Japanese Patent Publication 2002-241590

(Patent Document 8) Japanese Patent Publication 2002-309200

(Patent Document 9) Japanese Patent Publication 2003-127313

(Patent Document 10) Japanese Patent Publication 2003-321607

(Patent Document 11) Japanese Patent Publication 2005-154727

However, no material currently satisfies these requirements, especially for interlayer insulating materials for build-up substrates. In other words, it has high heat resistance and low expansion coefficient and is excellent in peel strength at the surface roughness after roughening suitable for the (semi) additive method, and also has good balance of elasticity, breaking strength and elongation at break. Resin compositions are not known.

The problem of the present invention is high heat resistance and low expansion coefficient, excellent peel strength at the surface roughness after roughening suitable for the (semi) additive method, and balance of elastic modulus, breaking strength and elongation at break. It is to provide an interlayer insulating material of resin properties.

Moreover, the subject of this invention is providing the high density buildup printed wiring board manufactured using such a thermosetting resin composition as an interlayer insulation material.

The thermosetting resin composition according to the present invention comprises (a) an epoxy resin containing 50 to 100% by weight of a liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C, (b) a triazine-modified phenol novolak resin curing agent, (c) an epoxy resin containing a solvent-soluble polyimide resin and (a) 50 to 100% by weight of a liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C; and (b) a triazine-modified phenol. When the total amount of the novolak resin curing agent is 100 parts by weight, the amount of the solvent-soluble polyimide resin (c) is 10 to 250 parts by weight.

The present invention also relates to a B-staged resin film produced from the thermosetting resin composition. Moreover, this invention relates to the multilayer buildup board | substrate containing this B-staged resin film.

In the present invention, 50 to 100% by weight of the epoxy resin (a) is composed of a liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C. Examples of liquid epoxy resins having a viscosity of 1.0 to 120 Pa · s at 25 ° C include bis-A epoxy resins, bis-F epoxy resins, hydrogenated bis-A epoxy resins, novolac phenol epoxy resins, naphthalene epoxy resins, and t. -Butyl catechol type epoxy resins, and the like, and can be used alone or in combination of two or more thereof. This viscosity is defined by the value measured using the E-type viscosity meter.

(a) Epoxy resin may contain or may not contain epoxy resins other than "liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C", but the content is 50% by weight or less. Epoxy resins other than "liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C '' may be used as long as they are epoxy resins having two or more glycidyl groups, but preferably novolacs that are solid resins at 25 ° C. A phenol type epoxy resin, a biphenyl type epoxy resin, a naphthalene type epoxy resin, a dicyclopentadiene type epoxy resin, etc. can be used individually or in combination of 2 or more types.

The following effects are obtained by using 50% by weight or more of the liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C in the entire (a) epoxy resin. That is, in order to cope with thinning, specifically, in order that L / S is 20/20 micrometers or less, it shifts from the subtractive method to the (semi) additive method, and it is low Ra (0.3 micrometer or less), and high peeling strength (0.7 kN) / m or more) is a requirement. However, the flatness of the insulating layer at the time of entering the roughening step in the (semi) additive process also greatly influences this. In other words, the surface roughness before the roughening process affects the Ra at low roughness. In order to prevent this, it is necessary that the surface is flattened before the roughening step, that is, after the first hardening step of vacuum lamination flattening. Although the standard of this planarization changes with various process conditions, in the experiment of this invention, it is necessary that the difference (step difference) of each pattern saw and its etching surface saw is 1.5 micrometer or less, regardless of the pattern density of surface irregularities. It was proved.

In order to realize such a high flatness, in addition to the optimization of the respective process conditions, proper fluidity during the vacuum lamination planarization step and the first curing is required, and the viscosity at 25 ° C. is 1.0 to 120 Pa · s. It was found that 50% or more of the phosphorus liquid epoxy resin was most effective. If the amount is less than 50% by weight, high flatness cannot be realized. Moreover, although the liquid epoxy resin whose viscosity in 25 degreeC is 120 Pa * s or more is effective in this flatness, the effect is remarkably reduced. Moreover, heat resistance does not satisfy | fill with the liquid epoxy resin whose viscosity in 25 degreeC is less than 1.0 Pa * s.

From the viewpoint of the present invention, the proportion of the liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C in the epoxy resin (a) is preferably 50 to 100% by weight, more preferably 60% by weight or more.

In the present invention, the triazine-modified phenol novolak resin curing agent (b) is a benzoguanamine-modified bisphenol-A novolak resin, a benzoguanamine-modified cresol novolak-type phenol resin, a benzoguanamine-modified phenol novolak-type phenol resin, Melamine-modified bisphenol A novolac resins, melamine-modified cresol novolac-type phenol resins, melamine-modified phenol novolac-type phenol resins, and the like.

When (a) epoxy equivalent (total value of (a)) of epoxy resin is 1, (b) the amount of triazine-modified phenol novolak resin used is 0.35 to 0.80 hydroxyl group equivalent of triazine-modified phenol novolak resin. Is optimal. If the usage-amount (equivalent) of a hardening | curing agent is less than 0.35, the composition of a suitable thermal expansion coefficient will not be obtained. If the amount (equivalent) of the curing agent exceeds 0.80, a good breaking strength and elongation at break cannot be obtained.

In this invention, (c) solvent soluble polyimide resin is polyimide resin soluble in the organic solvent used for manufacture of a composition. For example, NMP (N-methylpyrrolidone), DMF (dimethylformamide), DMAC (dimethylacetamide) can be illustrated. It is preferable that this resin has the characteristics of high Tg, low CTE, excellent film properties, and high adhesion strength. As the molecular weight, the number average molecular weight (Mn) is preferably 10,000 to 50,000, and more preferably 12,000 to 20,000. .

(c) Solvent As a soluble polyimide resin, there exist fully imidized soluble polyimide resin (1 type) etc. which are obtained, for example by making diamino trimethylphenyl indane react with benzophenone tetracarboxylic dianhydride.

When the total amount of (a) epoxy resin and (b) hardener is 100 parts by weight, the amount of (c) solvent-soluble polyimide resin is preferably in the range of 10 to 250 parts by weight. By setting it as 10 weight part or more, adhesive strength and flexibility can be provided. It is more preferable to set it as 15 weight part or more from this viewpoint. Moreover, when this exceeds 250 weight part, since the breaking strength as a film falls, it is preferable to set it as 250 weight part or less.

In the composition of this invention, a (d) filler can be added. Specifically, the filler (d) is preferably silica, alumina, aluminum nitride, boron nitride, magnesium oxide, or the like. Moreover, when the total amount of (a) epoxy resin, (b) hardening | curing agent, and (c) solvent-soluble polyimide resin is 100 weight part, it is preferable to make the amount of (d) filler 0-150 weight part. In the case of adding a low expansion coefficient, silica is preferred. In this case, silica may use the surface-treated silica (epoxy silane treatment, amino silane treatment, vinyl silane treatment, etc.). As the particle diameter, spherical particles having an average particle diameter of 0.5 µm or less are preferable from the viewpoint of narrow pitch response (L / S? 20/20 µm) and reduction of surface roughness (Ra? 0.3 µm). Moreover, in order to make the peeling strength of 0.5 kN / m or more into Ra <= 0.3micrometer, it is good to add 10 weight part or more of silica addition amounts. Moreover, since adding 150 weight part or more worsens workability, peeling strength, etc., such as laser workability, it is preferable to set it as 150 weight part or less. In addition, fillers, such as alumina, aluminum nitride, boron nitride, and magnesium oxide, can be used similarly.

Moreover, the hardening accelerator can be used together in the composition of this invention as needed. As a hardening accelerator, general things, such as various imidazoles and an organic phosphine type compound, can be used. It is mainly selected from the viewpoint of reaction rate (curing rate) and potlife. For example, 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-phenyl-4- Methylimidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole, 1,2-dimethylimidazole, 1-cyanoethyl-2-ethyl-4-methyl Midazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6- [2'-methyl Imidazolyl- (1 ')]-ethyl-s-triazine, 2,4-diamino-6- [2'-undecylimidazolyl- (1')]-ethyl-s-triazine, 2 , 4-diamino-6- [2'-methylimidazolyl- (1 ')]-ethyl-s-triazineisocyanuric 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] benz Imidazole, 4,4'-methylenebis (2-ethyl-5-methylimidazole), TPP, and the like.

In addition, a flame retardant may be added to the component of the present invention for imparting flame retardancy. In particular, as the halogen-free flame retardant, condensed phosphate esters, phosphazenes, polyphosphates, and HCA (9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide) derivatives are preferable. .

Although the solvent which can be used for the thermosetting resin composition of this invention is not specifically limited, It is especially preferable to combine high boiling point solvents, such as NMP and diethylene glycol monomethyl ether acetate, and a low boiling point solvent, such as cyclohexanone and MEK.

By B-stageting the thermosetting resin composition of the present invention, a resin film can be obtained. In other words, the resin composition of the present invention described above is, if necessary, diluted with a preferred mixed organic solvent such as NMP, (diethylene glycol monomethyl ether acetate) / MEK, (cyclohexanone), etc. The thermosetting resin film of B state can be manufactured by the conventional method of apply | coating with a die coater etc. on the polyethylene terephthalate film (PET film) which carried out the mold release process, and heating.

Moreover, the metal foil with an adhesive agent can be manufactured by apply | coating the thermosetting resin composition of this invention to metal foil with a die coater. As this metal foil, although surface roughened copper foil and aluminum foil can be illustrated, copper foil is especially preferable.

The product with a film of this invention can be used for the printed wiring board which has non-through via holes, such as a laser via, as HDI material, such as a buildup multilayer board which has a rigid core.

(Example)

Below, an Example demonstrates this invention.

Example 1

141 parts by weight of naphthalene type epoxy resin epicron HP-4032D (product made by Dainippon Ink & Chemicals Co., Ltd., epoxy equivalent 141, viscosity 23Pa · s / 25 ° C), 95 parts by weight of melamine-modified cresol novolac resin EXB-9854 (Dainippon Ink Kagaku Kogyo Co., Ltd., hydroxy group 151, 80 weight% of resin solid content), 360 weight part of soluble polyimide resin Q-VR-X0163 (made by Phi Gijutsu Kenkyu Sho Co., Ltd., 20 weight% resin), 0.7 weight of 2-ethyl- A mixture consisting of 4methylimidazole and 192 parts by weight of epoxysilane-treated spherical silica (average particle size 0.3 μm) was prepared to adjust a resin varnish having a resin solid content of 61% by weight.

Example 2

180 parts by weight of phenol novolac-type epoxy resin epicron N-730A (product made by Dainippon Ink, Kagaku Kogyo Co., Ltd., epoxy equivalent 180, viscosity 95 Pa · s / 25 ° C), 95 parts by weight of melamine-modified cresol novolac resin EXB-9854 (die Nippon Ink Kagaku Kogyo Co., Ltd., hydroxyl value 151, resin 80% by weight resin), 420 parts by weight of soluble polyimide resin Q-VR-X0163 (manufactured by Pei Gijutsu Kenkyu Sho Co., Ltd., 20% by weight resin), 0.7 parts by weight of 2- A mixture consisting of ethyl-4 methylimidazole and 220 parts by weight of epoxy silane-treated spherical silica (average particle size 0.3 µm) was prepared to adjust a resin varnish having a resin solid content of 63% by weight.

Example 3

141 parts by weight of naphthalene type epoxy resin epiclon HP-4032D (manufactured by Dainippon Ink & Chemicals Co., Ltd., epoxy equivalent 141, viscosity 23Pa · s / 25 ° C), 63 parts by weight of dicyclopentadiene type epoxy resin HP-7200H (Dinipon Ink made by Kagaku Kogyo Co., Ltd., epoxy equivalent 283, resin 80% by weight), 112 parts by weight of melamine-modified cresol novolac resin EXB-9854 (manufactured by Dainippon Ink, Kagaku Kogyo Co., Ltd., hydroxyl group 151, resin 80% by weight), 470 Parts by weight of soluble polyimide resin Q-VR-X0163 (manufactured by Piaget Kyushu, Ltd., 20% by weight of resin solid content), 0.7 parts by weight of 2-ethyl-4methylimidazole, 250 parts by weight of epoxysilane-treated spherical silica (average particle diameter 0.3 micrometer) was prepared, and the resin varnish of 60 weight% of resin solid content was adjusted.

Example 4

126 parts by weight of phenol novolak type epoxy resin epicron N-730A (manufactured by Dainippon Ink & Chemicals Co., Ltd., epoxy equivalent 180, viscosity 95Pa · s / 25 ° C), 54 parts by weight of naphthalene type polyfunctional epoxy resin epiclon HP4700 (die Nippon Ink Kagaku Kogyo Co., Ltd., epoxy equivalent 162), 109 parts by weight of melamine-modified cresol novolak resin EXB-9854 (manufactured by Dainippon Ink, Kagaku Kogyo Co., Ltd., hydroxy group 151, resin 80% by weight), 420 parts by weight of soluble polyimide Made of resin Q-VR-X0163 (manufactured by Pia Gijutsu Kenkyu Sho Co., Ltd., 20% by weight resin), 0.7 parts by weight of 2-ethyl-4methylimidazole, 220 parts by weight of epoxysilane-treated spherical silica (average particle size 0.3 탆) The resin varnish of 61 weight% of resin solid content was prepared by preparing the mixture.

(Comparative Example 1)

1,300 parts by weight of cresol novolac type epoxy resin YDCN-704P (manufactured by Tokasei Co., Ltd., epoxy equivalent 210: 70% by weight of resin solid content: solid at 25 ° C), 140 parts by weight of bisphenol A type epoxy resin epicoat 1001 (manufactured by JER Corporation, epoxy Equivalent 456, 70% by weight of resin solid content: solid at 25 ° C), 327 parts by weight of phenoxy resin YP-55 (manufactured by Totokasei Co., Ltd.), 925 parts by weight of melamine-modified phenol novolak resin LA-7054 (Dainippon Ink & Chemicals Co., Ltd.) Manufactured, the hydroxyl value is 125, 60 weight% of resin solid content), 240 weight part of condensation type phosphate ester PX-200 (made by Daihachi Kagaku Co., Ltd.), 0.7 weight part of 2-ethyl-4 methylimidazole, 320 weight part of epoxidation Polybutadiene resin E-1800-6.5 (manufactured by Nippon Sekiyu Kagaku Co., Ltd.) and 1050 parts by weight of epoxysilane-treated spherical silica (average particle size 0.3 µm) was added as a solvent to give a propylene glycol monomethyl ether (PGM) as a solid resin. 65% by weight of epoxy resin varnish The.

(Comparative Example 2)

600 parts by weight of brominated epoxy resin epicoat 5045 (manufactured by JER, epoxy equivalent 480 resin high solids content: 80% by weight: solid at 25 ° C), 85 parts by weight of phenoxy resin YP-55 (manufactured by Totokasei Co., Ltd.), 13 parts by weight of dicyandiamide And 0.5 parts by weight of 2-ethyl-4methylimidazole, 100 parts by weight of epoxidized polybutadiene resin E-1800-6.5 (manufactured by Nippon Sekiyu Kagaku Co., Ltd.), 291 parts by weight of epoxysilane-treated spherical silica (average particle size 0.3 탆) Propylene glycol monomethyl ether (PGM) and dimethylformamide were added as a solvent to the mixture which consists of a) and the epoxy resin varnish of 65 weight% of resin solid content was adjusted.

(Comparative Example 3)

126 parts by weight of phenol novolac-type epoxy resin epicron N-740 (manufactured by Dainippon Ink, Kagaku Kogyo Co., Ltd., epoxy equivalent 180, viscosity of 50 Pa at 75 Pa, semisolid at 25 ° C), 54 parts by weight of naphthalene type polyfunctional epoxy resin Epiclon HP4700 (product made by Dainippon Ink & Chemicals Co., Ltd., epoxy equivalent 162), 109 weight part of melamine modified cresol novolak resin EXB-9854 (product made by Dainippon Ink & Chemicals Kagaku Kogyo Co., Ltd., hydroxyl value 151, resin 80% by weight), 420 Parts by weight of soluble polyimide resin Q-VR-X0163 (manufactured by Piaget Kyushu Co., Ltd., 20% by weight of resin solid content), 0.7 parts by weight of 2-ethyl-4methylimidazole, 220 parts by weight of epoxysilane-treated spherical silica (average particle diameter 0.3 micrometer) was prepared, and the resin varnish of 61 weight% of resin solid content was adjusted.

(Comparative Example 4)

126 parts by weight of liquid epoxy resin decoration EX321L (manufactured by Nagase Chemtex Co., Ltd., epoxy equivalent 160, viscosity 0.8 Pa · s at 25 ° C.), 54 parts by weight of naphthalene type polyfunctional epoxy resin epiclon HP4700 (manufactured by Dainippon Ink & Chemical Co., Ltd.) , Epoxy equivalent 162), 109 parts by weight of melamine modified cresol novolac resin EXB-9854 (manufactured by Dainippon Ink & Chemicals Co., Ltd., hydroxyl value of 151, 80% by weight resin), 420 parts by weight of soluble polyimide resin Q-VR-X0163 (Pia Gijutsu Kenkyu Sho Co., Ltd., 20% by weight of resin solid content), a mixture of 0.7 parts by weight of 2-ethyl-4methylimidazole and 220 parts by weight of epoxysilane-treated spherical silica (average particle size 0.3㎛) to prepare a resin 61 weight% resin varnish was adjusted.

The resin varnish of each said example was well disperse | distributed with three rolls. This was apply | coated with the die coater on the 25 micrometer polyethylene terephthalate film (PET film) which carried out the mold release process as needed, and it dried at the temperature of 120 degreeC, and manufactured the thermosetting resin film (A) of B state of thickness 40micrometer. Volatilization was adjusted to 3.0 wt%. Moreover, the polyethylene film (PE film) was laminated as a protective film.

This was made to overlap with 18 micrometers surface-treated copper foil, and it put in the vacuum press, and it shape | molded by 180 Mx120 minutes and heating and pressurization (vacuum degree 5torr) at 4 Mpa. (Molded object (1)).

Similarly, in order to improve the adhesion before coating, the sheet was overlapped with a copper foil subjected to a process of making small irregularities with paper, put into a vacuum press, and heated and pressurized (vacuum degree of 5torr) at 180 ° C for 120 minutes and 4 Mpa. ))

On the other hand, a circuit was formed on a high Tg halogen-free FR-4 double-sided copper clad laminate (18 µm of copper foil) (trade name TLC-W-552Y, manufactured by Kyocera Chemical Co., Ltd.) having a thickness of 0.6 mm, and then subjected to a black copper oxide treatment on a conductor with a vacuum laminator. The film A is peeled off from the protective film on this surface, and lamination is performed on both surfaces, and the film A is flattened through a flattening press process. This is hardened by the 1st stage of 190 degreeC * 30 minutes in a tunnel drying furnace. After cooling out, a blind via having a predetermined pore size (60 µm, 100 µm) was formed by a C0 ₂ laser.

The surface roughening was performed with the permanganic acid desmear solution, and at the same time, the remaining resin in the bottom of the hole was also dissolved and removed. Electroless copper plating 0.8 micrometer and electrolytic copper plating 20 micrometer were attached to this, and after-baking of 180 degreeC * 60 minutes was performed. This was repeated to produce a six-layer build-up multilayer printed wiring board I having a two-sided build-up layer (no built-up pattern formation, but beta-copper portion that can be measured).

Each parameter of each said example is put together in Table 1, and is shown. In addition, the evaluation results of the characteristics of each example are shown in Tables 2 and 3. PWB (II) in Table 2 is a test pattern substrate of JPCA-HD01 produced according to the manufacturing method of PWB (I).

Table 1

Table 2

Table 3

The evaluation method is as follows.

Flatness: Difference between each pattern saw and its etched surface saw with surface irregularities after PWB (II) planarization press

(Step); (by laser microscope)

Surface roughness: by laser microscope

PWB (II): A test pattern substrate of JPCA-HD01 produced according to the manufacturing method of PWB (I).

Film Properties: By Autograph

Reliability: According to JPCA-BU01

(a) Thermal shock test 150 ℃ × 30min↔-65 ℃ × 30min (1 cycle)

(b) High temperature and high humidity bias test 85 ℃ × 85% RH, DC = 50V

(Measured in the premise)

As described above, according to Examples 1 to 4 of the present invention, a resin composition for a high-density build-up printed wiring board having a low expansion coefficient and low roughness-high adhesive strength, high heat resistance, and high reliability can be provided. And the printed wiring board which provided these various characteristics can be used for semiconductor plastic packages, etc.

Although the low expansion coefficient of a thermosetting resin composition can be implement | achieved to some extent by adding an inorganic filler on the premise of the low expansion coefficient in a base resin, there exists a limit in the case of not reducing the thermal expansion coefficient of a base resin itself. In order to reduce the thermal expansion coefficient of an epoxy resin, selection of a hardening | curing agent is important. However, although only the selection of the curing agent is limited, it has been found that further reduction in the coefficient of thermal expansion can be achieved by using a specific solvent-soluble polyimide resin in combination. It was also found that this modification can improve film physical properties without imparting flexibility to the cured product and lowering Tg. In addition, the adhesive strength of the resin composition itself was improved by the addition of the solvent-soluble polyimide resin, and thus, the present invention was found to achieve a rough surface formation of high peel strength due to a low profile by the (semi) additive process. .

According to the thermosetting resin composition of the present invention, for example, high heat resistance (Tg: 150 ° C. or more), low expansion coefficient (40 ppm / ° C. or less at 25 ° C. to 150 ° C.), and a roughened surface suitable for the (semi) additive process It is possible to provide an interlayer insulating material of a resin property which is excellent in peeling strength at a part with a low roughness (Ra 0.3 µm or less) and in which a balance of elastic modulus, breaking strength and elongation at break is achieved.

Claims (8)

(a) an epoxy resin containing 50 to 100% by weight of a liquid epoxy resin having a viscosity of 1.0 to 120 Pa · s at 25 ° C, (b) a triazine-modified phenol novolak resin curing agent, and (c) a solvent-soluble polyimide resin. The amount of the solvent-soluble polyimide resin (c) when the total amount of the (a) epoxy resin and the (b) triazine-modified phenol novolak resin curing agent is 100 parts by weight is 10 to 250 parts by weight. Thermosetting resin composition to be. The total amount of the (a) epoxy resin, the (b) triazine-modified phenol novolak resin curing agent, and the (c) solvent-soluble polyimide resin is 100 parts by weight. A thermosetting resin composition, wherein the amount of the filler (d) is 150 parts by weight or less. The hydroxyl equivalent ratio of the said (b) triazine-modified phenol novolak resin hardener when the epoxy equivalent of said (a) epoxy resin is 1 is 0.35-0.80, The thermosetting of Claim 1 or 2 characterized by the above-mentioned. Resin composition. The (b) triazine-modified phenol novolak resin curing agent is a melamine-modified phenol novolak resin, melamine-modified cresol novolak resin, benzoguanamine-modified phenol novolak resin according to any one of claims 1 to 3; A thermosetting resin composition, which is selected from the group consisting of benzoguanamine-modified cresol novolak resins. The fully imidized soluble polyimide resin according to any one of claims 1 to 4, wherein (c) the solvent-soluble polyimide resin is obtained by reacting a diaminotrimethylphenyl group with benzophenone tetracarboxylic dianhydride. A thermosetting resin composition characterized in that the. The thermosetting resin composition according to any one of claims 2 to 5, wherein the (d) filler is one or two or more fillers selected from silica, alumina, aluminum nitride, boron nitride, and magnesium oxide. The B-staged resin film produced from the thermosetting resin composition of any one of Claims 1-6. A multilayer build-up substrate comprising the B-staged resin film according to claim 7.