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Thermosetting resin composition, method for producing resin composition varnish, prepreg and laminate

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Thermosetting resin composition, method for producing resin composition varnish, prepreg and laminate


Discloses are a thermosetting resin composition containing a maleimide compound including an unsaturated maleimide compound having a specified chemical structure, a thermosetting resin, an inorganic filler, and a molybdenum compound; a laminate plate for wiring boards obtained by coating a base material with a thermosetting resin composition containing a thermosetting resin, silica, and a specified molybdenum compound and then performing semi-curing to form a prepreg, and laminating and molding the prepreg; and a method for manufacturing a resin composition varnish including specified steps. According to the present invention, electronic components having low thermal expansion properties and excellent drilling processability and heat resistance, for example, a prepreg, a laminate plate, an interposer, etc., can be provided.
Related Terms: Varnish

Browse recent Hitachi Chemical Company, Ltd. patents - Tokyo, JP
Inventors: Yoshihiro Takahashi, Yasuo Kamigata, Hikari Murai, Masahiro Aoshima, Shinji Tsuchikawa, Masato Miyatake, Tomohiko Kotake, Hiroyuki Izumi
USPTO Applicaton #: #20120276392 - Class: 428418 (USPTO) - 11/01/12 - Class 428 
Stock Material Or Miscellaneous Articles > Composite (nonstructural Laminate) >Of Epoxy Ether >Next To Metal

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The Patent Description & Claims data below is from USPTO Patent Application 20120276392, Thermosetting resin composition, method for producing resin composition varnish, prepreg and laminate.

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TECHNICAL FIELD

The present invention relates to a thermosetting resin composition which is especially low in thermal expansion properties and excellent in drilling processability and heat resistance and which is suitably used for electronic components, etc.; a prepreg and a laminate plate each using the same; a laminate plate for wiring boards requiring a drilling processing treatment at a manufacturing stage for wiring board; a manufacturing method of a resin composition varnish; and a prepreg and a laminate plate fabricated utilizing the subject manufacturing method, each of which is suitable for semiconductor packages and printed wiring boards.

BACKGROUND ART

In a wiring board to be used for semiconductor packages (hereinafter referred to as “interposer”), it is general to perform a large number of drilling processing for interlayer connection of wirings. In consequence, a laminate plate for interposers is required to have high drilling processability.

Now, for a laminate plate for semiconductor packages, there have hitherto been used a lot of curable resin compositions composed of a bismaleimide compound and a cyanate resin (for example, Patent Document 1). This is because in view of the fact that the subject resin compositions are excellent in heat resistance, the resin compositions were suitable as a resin composition for the laminate plate for semiconductor packages, which is frequently exposed to high temperatures in a reflow step or the like at the time of mounting.

However, in recent years, requirements for thinning and weight reduction of electronic appliances are increased, and associated with rapid progress of thinning and high density of semiconductor packages, laminate plates for semiconductor packages have also been required to have higher characteristics other than heat resistance over broad regions.

Above all, in order to suppress an increase of a warp at the time of mounting to be caused due to thinning of a semiconductor package, it is strongly required to make a coefficient of thermal expansion of a laminate plate for semiconductor packages close to that of a silicon chip, namely to realize low thermal expansion.

While there are considered a variety of techniques for realizing low thermal expansion of the laminate plate, it is effective to allow a resin per se for laminate plates to realize low thermal expansion, or to fill an inorganic filler in a high density in a resin composition. For that reason, a novolak type cyanate resin is used, or a content of the inorganic filler is increased (for example, Patent Document 2).

But, the use of a cyanate resin or the filling of an inorganic filler in a high density involved such a problem that cutting properties of the resin composition are lowered, thereby significantly impairing drilling processability of a laminate plate using such a resin composition.

Then, there was made an attempt to prevent a lowering of the drilling processability by adding a plate-shaped filler such as burnt talc, etc. as an inorganic filler or reducing a content the inorganic filler (for example, Patent Document 3). However, there were such inconveniences that the effect for preventing a lowering of the drilling processability is insufficient; the resin composition becomes low in elasticity, so that the effect for suppressing a warp of the semiconductor package is insufficient; and so on. Thus, satisfactory results have not been obtained yet.

In order to realize low thermal expansion of the laminate plate, it is effective to increase a content of a filler having a small coefficient of thermal expansion, such as silica, among inorganic fillers in the resin composition used in the laminate plate. But, if the content of a hard filler such as silica is increased, there was encountered such a problem that the drilling processability of the laminate plate is lowered.

Also, in order to enhance the drilling processability, there is made an attempt to add a metal dichalcogenide such as molybdenum disulfide as an inorganic solid lubricant particle (see, for example, Patent Document 4). But, if molybdenum disulfide is added, there is encountered such a problem that electrical insulating properties of the laminate plate are significantly lowered. Thus, satisfactory results have not been obtained yet.

Then, in order to solve this problem, the present inventors investigated additives which even when an inorganic filler is filled in high density, can inhibit the deterioration of the drilling processability and then found that a molybdenum compound has an excellent effect.

But, since the molybdenum compound has a large specific gravity, when added directly to a resin composition varnish to be used for the fabrication of a laminate plate, it easily precipitates to cause defective manufacture. For that reason, it is recommended to use a particle having a molybdenum compound supported on talc or the like (for example, KEMIGARD 911C, manufactured by Sherwin-Williams Company) (see, for example, Patent Document 5). However, there are such drawbacks that the resin composition varnish is thickened; aggregation of the molybdenum compound-supported particles with each other easily occurs; and so on. Thus, satisfactory results are not obtained.

PRIOR ART DOCUMENTS Patent Documents

Patent Document 1: JP-A-3-52773

Patent Document 2: Japanese Patent No. 4132703

Patent Document 3: JP-A-2005-162787

Patent Document 4: JP-T-2002-527538

Patent Document 5: JP-A-2000-264986

DISCLOSURE OF THE INVENTION

Under such circumstances, the present invention has been made. A first object of the present invention is to provide a thermoplastic resin composition which is especially low in thermal expansion properties and excellent in drilling processability and heat resistance and which is suitably used for electronic components, etc., and a prepreg and a laminate plate each using the same; and a second object thereof is to provide a laminate plate for wiring boards, which is very excellent in drilling processability at the time of fabricating a wiring board and which also has favorable electrical insulating properties and low thermal expansion properties.

Furthermore, a third object of the present invention is to provide a method for manufacturing a resin composition varnish, in which precipitation or aggregation of a molybdenum compound hardly occurs, and a prepreg and a laminate plate each having a low coefficient of thermal expansion and high drilling processability.

The present inventors made extensive and intensive investigations. As a result, it has been found that the foregoing first object can be achieved by a thermosetting resin composition containing an unsaturated maleimide compound having an acidic substituent composed of a specified chemical formula, a thermosetting resin, an inorganic filler, and a molybdenum compound; the foregoing second object can be achieved by forming a laminate plate by using a thermosetting resin composition containing a thermosetting resin, a specified amount of silica, and a specified molybdenum compound; and furthermore, the foregoing third object can be achieved by manufacturing a resin composition varnish by a method in which after a molybdenum compound is dispersed and mixed in a slurry having a specified silica particle dispersed therein, this slurry is added to a varnish containing a thermosetting resin, and thereafter, an inorganic filler is blended therewith. The present invention has been accomplished on the basis of such knowledge.

That is, the present invention provides the following.

(1) A thermosetting resin composition comprising (A) a maleimide compound containing an unsaturated maleimide compound having an acidic substituent, as represented by the following general formula (I) or (II), (B) a thermosetting resin, (C) an inorganic filler, and (D) a molybdenum compound:

(In the formulae, R1 represents a hydroxyl group, a carboxyl group, or a sulfonic acid group, each of which is the acidic substituent; each of R2, R3, R4, and R5 independently represents a hydrogen atom, an aliphatic hydrocarbon group having a carbon number of from 1 to 5, or a halogen atom; A represents an alkylene group, an alkylidene group, an ether group, a sulfonyl group, or a group represented by the following formula (III); x represents an integer of from 1 to 5; y represents an integer of from 0 to 4; and a sum of x and y is 5.)

(2) The thermosetting resin composition as set forth above in (1), wherein the molybdenum compound (D) is at least one member selected from a molybdenum oxide and a molybdic acid compound, and a content of the molybdenum compound is from 0.02 to 20% by volume of the whole of the resin composition. (3) The thermosetting resin composition as set forth above in (1) or (2), wherein the thermosetting resin (B) is an epoxy resin; a total sum content of the component (A) and the component (B) is from 30 to 80% by volume of the whole of the resin composition; and a mass ratio of the component (A) and the component (B) is from 20 to 90 parts by mass in terms of the component (A) based on 100 parts by mass of the total sum content of the component (A) and the component (B). (4) The thermosetting resin composition as set forth above in any one of (1) to (3), wherein the inorganic filler (C) is fused spherical silica, and a content of the inorganic filler is from 10 to 60% by volume of the whole of the resin composition. (5) A prepreg obtained by impregnating or coating a base material with the thermosetting resin composition as set forth above in any one of (1) to (4) and then performing B-staging. (6) A laminate plate obtained by laminating and molding the prepreg as set forth above in (5). (7) The laminate plate as set forth above in (6), which is a metal clad laminate plate obtained by superimposing a metal foil on at least one surface of the prepreg and then performing heat pressure molding. (8) A laminate plate for wiring boards, obtained by coating a thermosetting resin composition containing (E) a thermosetting resin, (F) silica, and (G) at least one molybdenum compound selected from zinc molybdate, calcium molybdate, and magnesium molybdate, with a content of the silica (F) being 20% by volume or more and not more than 60% by volume, on a base material in a film form or fiber form, then performing semi-curing to form a prepreg, and laminating and molding the prepreg. (9) The laminate plate for wiring boards as set forth above in (8), wherein the silica (F) is fused spherical silica having an average particle size of 0.1 μm or more and not more than 1 μm, and a content of the molybdenum compound (G) is from 0.1% by volume or more and not more than 10% by volume of the whole of the resin composition. (10) The laminate plate for wiring boards as set forth above in (8) or (9), wherein the thermosetting resin composition is varnished. (11) The laminate plate for wiring boards as set forth above in any one of (8) to (10), wherein the base material in a film form or fiber form is a glass cloth. (12) A method for manufacturing a resin composition varnish comprising



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stats Patent Info
Application #
US 20120276392 A1
Publish Date
11/01/2012
Document #
13518578
File Date
12/24/2010
USPTO Class
428418
Other USPTO Classes
524105, 523455, 156 60, 427 58, 428457
International Class
/
Drawings
0


Varnish


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