KR20150023304A - Rolled sheet - Google Patents

Abstract

The roll-shaped sheet (60) contains particles and a resin component, and the mixing ratio of the particles exceeds 30% by volume. The roll-shaped sheet 60 is obtained by deforming the composition containing the particles and the resin component in the direction of the rotation axis of the gear 32 using the gear structure 4 having the pair of gears 32 After passing through the gap between the moving roll 51 and the protruding portion 63 while conveying the sheet 7 while the sheet 7 is supported by the moving roll 51 after the deforming conveying step and the deforming conveying step in which the sheet 7 is conveyed do.

Description

ROLLED SHEET [0002]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a roll-shaped sheet, and more particularly, to a roll-shaped sheet containing particles and a resin component.

Conventionally, various methods for producing a sheet from a composition containing particles and a resin component have been studied.

For example, there is a method in which a composition is prepared by mixing a boron nitride particle and a resin component in which the boron nitride particle is dispersed, and the resulting composition is heat-pressed by a flat plate to produce a press sheet and then laminated to obtain a thermally conductive sheet (For example, refer to Patent Document 1 below).

Japanese Patent Application Laid-Open No. 2007-039060

However, in the method described in Patent Document 1, since the batch production method in which the composition is pressed each time, the sheet to be produced becomes a flat sheet having one short side. When such a short sheet is stacked and stored in the form of a flat sheet, not only a large storage space is required but also a disadvantage in terms of transportability.

An object of the present invention is to provide a roll-shaped sheet containing particles at a high blending ratio and having excellent storability and transportability.

In order to achieve the above object, the roll-shaped sheet of the present invention contains particles and a resin component, and the mixing ratio of the particles exceeds 30% by volume.

Further, the sheet of the present invention is characterized in that it comprises a deformation carrying step of transferring a composition containing the particles and the resin component while deforming the gear structure with a pair of gears in the rotational axis direction of the gear, After the deforming and conveying step, the composition is transported while being supported by and supported by a movable support body, and is passed through the gap between the movable support body and the doctor arranged opposite to the movable support body so as to form a gap therebetween Is suitable.

In the sheet of the present invention, it is preferable that the composition passing through the gap passing step has a shearing stress of not more than 5.0 x 10 < ⁴ > Pa at a temperature range of 50 to 250 deg.

The sheet of the present invention preferably has a width of 200 mm or more.

The roll-shaped sheet of the present invention is a particle-containing roll-shaped sheet, which contains particles and a resin component, the blending ratio of the particles exceeds 30% by volume, and the resin component comprises an epoxy resin composition and / And is wound in a roll shape.

The roll-shaped sheet of the present invention preferably has a width of 200 mm or more.

In the roll-shaped sheet of the present invention, it is preferable that the average value of the maximum length of the particles is 0.1 탆 or more and 100 탆 or less.

In addition, the roll-shaped sheet of the present invention preferably has a tensile elastic modulus at 25 DEG C of not less than 0.1 GPa and not more than 20 GPa.

In the roll-shaped sheet of the present invention, it is preferable that the thickness of the sealing sheet is 100 mu m or more.

The roll-shaped sheet of the present invention is formed into a roll shape while containing particles at a high mixing ratio. As a result, it is possible to reduce the storage space while sufficiently exhibiting the specific physical properties possessed by the particles, and is excellent in transportability.

In addition, the roll-shaped sheet of the present invention, which is also a particle-containing roll-shaped sheet, contains the particles in a high mixing ratio while the sealing sheet is wound in a roll form. Therefore, it is possible to sufficiently exhibit the specific physical properties possessed by the particles while being manufactured with high production efficiency, and also to reduce the storage space, thereby being excellent in transportability.

BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 shows a partially cut-away plan view of an embodiment of a sheet manufacturing apparatus used for manufacturing the roll-shaped sheet of the present invention.
Fig. 2 shows a cross-sectional view taken along line AA of Fig.
Fig. 3 shows a schematic configuration diagram of a kneader used in the sheet producing apparatus shown in Fig. 1. Fig.
Fig. 4 is a plan sectional view of the knocking machine shown in Fig. 3 on the discharge port side.
Fig. 5 shows a top cross-sectional view of a feed portion, a gear structure and a sheet adjusting portion used in the sheet producing apparatus shown in Fig. 1. Fig.
Fig. 6 is a side cross-sectional view of the supply portion, the gear structure, and the sheet adjustment portion shown in Fig. 5, and shows a cross-sectional view along the line BB of Fig.
Fig. 7 is an exploded perspective view of a pair of gears of the gear structure shown in Fig. 5;
Fig. 8 is a side sectional view for explaining the engagement of the pair of gears shown in Fig. 7, wherein Fig. 8 (a) is a plan view showing a state in which the downstream side end portion of the convex surface of the oblique teeth of the first gear, (B) shows a state in which a midway portion of the convex surface of the oblique teeth of the first gear is engaged with the intermediate portion of the concave surface of the oblique teeth of the second gear, (c) The upstream side end portion of the convex surface of the tooth and the upstream side end portion of the concave surface of the oblique tooth of the second gear are engaged with each other.
Fig. 9 shows a partially cut-away plan view of another embodiment of the sheet producing apparatus of the present invention.
Fig. 10 shows a schematic configuration diagram of a kneader used in the sheet producing apparatus shown in Fig.
Fig. 11 shows a plan sectional view of the knocking machine shown in Fig. 10 on the discharge port side.

The roll-shaped sheet of the present invention is obtained by winding a sheet containing particles and a resin component.

The particles include powder, solid, powder, and powder, and examples of the material for forming the particles include inorganic materials and organic materials. An inorganic material is preferably used.

Examples of the inorganic material include carbides, nitrides, oxides, carbonates, sulfates, metals, clay minerals, and carbon-based materials.

Examples of the carbide include silicon carbide, boron carbide, aluminum carbide, titanium carbide, and tungsten carbide.

Examples of the nitride include silicon nitride, boron nitride (BN), aluminum nitride (AlN), gallium nitride, chromium nitride, tungsten nitride, magnesium nitride, molybdenum nitride and lithium nitride.

As the oxide, for example (including silica, spherical fused silica powder and crushed fused silica powder and the like), silicon oxide, aluminum oxide (alumina, Al ₂ O _3), magnesium oxide (magnesia), titanium, cerium, iron oxide , Beryllium oxide, and the like. Examples of the oxide include indium tin oxide and antimony tin oxide doped with metal ions. Silicon oxide is preferably used.

Examples of the carbonate include calcium carbonate and the like.

Examples of the sulfate include calcium sulfate (gypsum) and the like.

Examples of the metal include copper (Cu), silver, gold, nickel, chromium, lead, zinc, tin, iron, palladium or alloys thereof (solder and the like).

The clay minerals include, for example, montmorillonite, magnesian montmorillonite, iron montmorillonite, iron magnesium montmorillonite, beidellite, aluminian beellite, nontronite, aluminian nontronite, saponite, aluminian saponite, Light, sauconite, stevensite, and the like.

Examples of the carbon-based material include carbon black, graphite, diamond, fullerene, carbon nanotube, carbon nanofiber, nanohorn, carbon microcoil, and nanocoil. Preferably carbon black.

Preferable examples thereof include oxides and carbon-based materials.

Examples of the material include materials having specific physical properties. Examples of the material include a thermally conductive material (for example, a thermally conductive material selected from carbide, nitride, oxide and metal, specifically BN, AlN, Al ₂ O ₃ , , An electrically conductive material (e.g., an electrically conductive material selected from a metal and a carbon-based material, specifically, Cu), an insulating material (e.g., nitride and oxide such as BN and silica) Materials (e.g., oxides, metals, specifically, ferrites (soft magnetic ferrite, hard magnetic), iron, etc.). The material having specific physical properties may be overlapped with the materials exemplified above.

The thermal conductivity of the particles is, for example, 10 W / m · K or higher, preferably 30 W / m · K or higher, and is, for example, 2000 W / m · K or lower.

The electrical conductivity of the particles is, for example, 10 ⁶ S / m or more, preferably 10 ⁸ S / m or more, and usually 10 ¹⁰ S / m or less.

Further, the volume resistivity of the particles is, 1 × ¹⁰ 10 Ω · cm and, preferably at least 1 × 10 ¹² Ω · cm, also, for example, is also ²⁰ Ω · cm or less 10 × 1.

The magnetic permeability of the particles (mu "at a wavelength of 2.45 GHz) is, for example, 0.1 to 10.

The particles may be surface-treated with, for example, a silane coupling agent or the like.

The shape of the particles is not particularly limited and may be, for example, a plate shape, a scaly shape, a particle shape (indefinite shape), or a spherical shape.

The average value of the maximum length of the particles (average particle diameter in the case of a spherical shape) is 0.1 탆 or more, preferably 1 탆 or more, for example, 1000 탆 or less, preferably 100 탆 or less Do. Further, the average particle diameter is obtained, for example, as a d50 value.

When the average value of the maximum length of the particles is not more than the upper limit, it can be processed smoothly in the sealing sheet production apparatus. On the other hand, when the average value of the maximum lengths of the particles is not less than the above lower limit, Can be formed to have a wide width.

When the particle has a shape other than a spherical shape, the particle has an aspect ratio of, for example, 2 or more, preferably 10 or more, and for example, 10000 or less, preferably 5000 or less.

The density (true density) of the particles is, for example, 0.1 g / cm ³ or more, preferably 0.2 g / cm ³ or more and 20 g / cm ³ or less, preferably 10 g / ³ or less.

These particles may be used alone or in combination of two or more.

The resin component is a dispersion medium (matrix) in which particles can be dispersed, that is, a particle is dispersed. The resin component contains an insulating component and includes, for example, a resin component such as a thermosetting resin component or a thermoplastic resin component .

Examples of the thermosetting resin component include an epoxy resin, a thermosetting polyimide, a urea resin, a melamine resin, an unsaturated polyester resin, a diallyl phthalate resin, a silicone resin, and a thermosetting urethane resin.

Examples of the thermoplastic resin component include acrylic resin, polyolefin (e.g., polyethylene, polypropylene, ethylene-propylene copolymer, etc.), polyvinyl acetate, ethylene-vinyl acetate copolymer, polyvinyl chloride, polystyrene, A polyether sulfone, a polyether sulfone, a polyether sulfone, a polyaryl sulfone, a thermoplastic polyimide, a thermoplastic polyurethane, a polyether sulfone, a polysulfone, Polyamideimide, polyimide, polyamideimide, bismaleimide triazine resin, polymethylpentene, fluorinated resin, liquid crystal polymer, olefin-vinyl alcohol copolymer, ionomer, polyarylate, acrylonitrile -Ethylene-styrene copolymers, acrylonitrile-butadiene-styrene copolymers, And the like can be mentioned polyisobutylene copolymer-acrylonitrile-methacrylate-styrene copolymer, polystyrene.

These resin components may be used alone or in combination of two or more.

Among the resin components, an epoxy resin is preferably used as the thermosetting resin component, and as the thermoplastic resin component, an acrylic resin is preferably used.

The epoxy resin is in a liquid, semi-solid or solid form at room temperature.

Specifically, examples of the epoxy resin include bisphenol type epoxy resins (e.g., bisphenol A type epoxy resins, bisphenol F type epoxy resins, bisphenol S type epoxy resins, hydrogenated bisphenol A type epoxy resins, (E.g., bisphenol type epoxy resin and the like), novolac type epoxy resin, naphthalene type epoxy resin, fluorene type epoxy resin (e.g., bisaryl fluorene type epoxy resin and the like), triphenylmethane type epoxy resin Aromatic epoxy resin such as hydroxyphenylmethane epoxy resin, etc.), and nitrogen-containing cyclic epoxy resin such as triepoxypropylisocyanurate and hydantoin epoxy resin, for example, aliphatic epoxy resin, alicyclic epoxy resin, Type epoxy resin, glycidyl ether type epoxy resin, glycidylamine type epoxy resin and the like. As the epoxy resin, for example, a bisphenol type epoxy resin is preferably used.

These epoxy resins may be used alone or in combination of two or more.

The epoxy equivalent of the epoxy resin is, for example, 100 g / eq. Or more, preferably 180 g / eq. For example, 1000 g / eq. Preferably 700 g / eq. Or less. When the epoxy resin is in a solid-state at room temperature, the softening point is, for example, 20 to 90 占 폚.

The mixing ratio of the resin component (particularly, epoxy resin) is, for example, 1 part by mass or more, preferably 2 parts by mass or more, and more preferably 3.5 parts by mass or more, relative to 100 parts by mass of the particles. Preferably 50 mass parts or less, more preferably 40 mass parts or less, further preferably 30 mass parts or less.

The roll-shaped sheet, together with the epoxy resin, preferably contains a curing agent.

The curing agent is a latent curing agent (epoxy resin curing agent) capable of curing the epoxy resin by heating, and examples thereof include phenol compounds, amine compounds, acid anhydride compounds, amide compounds, hydrazide compounds, imidazoline compounds and the like . In addition to the above, urea compounds and polysulfide compounds can also be used.

The phenolic compound includes a phenolic resin, for example, a novolak type phenol resin obtained by condensing phenol and formaldehyde under an acidic catalyst, for example, phenol and dimethoxyparaxylene or bis (methoxymethyl) biphenyl For example, biphenyl aralkyl resins such as dicyclopentadiene type phenol resins such as cresol novolak resins, such as resol resins, and the like. A phenol-aralkyl resin is preferably used.

The hydroxyl equivalent of the phenol compound is, for example, 80 g / eq. Or more, preferably 90 g / eq. More preferably 100 g / eq. And, for example, 2,000 g / eq. Preferably 1,000 g / eq. More preferably 500 g / eq. Or less.

Examples of the amine compound include polyamines such as ethylenediamine, propylenediamine, diethylenetriamine, triethylenetetramine and the like, or amine adducts thereof, for example, metaphenylenediamine, diaminodiphenylmethane, Aminodiphenylsulfone, and the like.

Examples of the acid anhydride compound include acid anhydride compounds such as phthalic anhydride, maleic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, 4-methylhexahydrophthalic anhydride, methylnadonic anhydride, pyromellitic anhydride, dodecenylsuccinic anhydride, Dichlorosuccinic anhydride, benzophenone tetracarboxylic acid anhydride, and chlorendic anhydride.

Examples of the amide compound include dicyandiamide, polyamide and the like.

Examples of the hydrazide compound include adipic acid dihydrazide and the like.

Examples of the imidazoline compound include methylimidazoline, 2-ethyl-4-methylimidazoline, ethylimidazoline, isopropylimidazoline, 2,4-dimethylimidazoline, phenylimidazoline, Undecylimidazoline, heptadecylimidazoline, 2-phenyl-4-methylimidazoline, and the like.

A phenol compound is preferably used.

The softening point of the curing agent is, for example, 50 DEG C or higher, preferably 60 DEG C or higher, and is 80 DEG C or lower, preferably 70 DEG C or lower.

These curing agents may be used alone or in combination of two or more.

The mixing ratio of the curing agent is, for example, not less than 1 part by mass, preferably not less than 5 parts by mass, more preferably not less than 10 parts by mass, and, for example, not more than 200 parts by mass based on 100 parts by mass of the epoxy resin , Preferably not more than 150 parts by mass. When the curing agent contains a phenol compound, the hydroxyl group of the phenol compound is added in an amount of, for example, 0.5 mol or more, preferably 0.8 mol or more, and, for example, 2.0 mol or less per mol of the epoxy group of the epoxy resin, Preferably 1.2 moles or less.

The roll-shaped sheet may contain a curing accelerator together with the epoxy resin.

The curing accelerator is a curing catalyst, for example, 2-phenylimidazole, 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenyl- Imidazole compounds such as imidazole, imidazole and the like, tertiary amine compounds such as triethylenediamine and tri-2,4,6-dimethylaminomethylphenol, for example, triphenylphosphine, tetraphenylphosphonium tetraphenylborate , And tetra-n-butylphosphonium-o, o-diethylphosphorodithioate, and quaternary ammonium salt compounds such as organic metal salt compounds such as derivatives thereof have.

Preferably an imidazole compound.

These curing accelerators may be used alone or in combination of two or more.

The mixing ratio of the curing accelerator is, for example, not less than 0.1 part by mass, preferably not less than 0.2 parts by mass, and not more than 10 parts by mass, preferably not more than 5 parts by mass, for example, based on 100 parts by mass of the epoxy resin It is also.

The above-mentioned curing agent and / or curing accelerator may be used as a solvent solution and / or a solvent dispersion prepared by dissolving and / or dispersing in a solvent, if necessary.

Examples of the solvent include ketones such as acetone and methyl ethyl ketone (MEK), esters such as ethyl acetate, and organic solvents such as amides such as N, N-dimethylformamide, etc. have. Examples of the solvent include water, for example, water-based solvents such as alcohols such as methanol, ethanol, propanol and isopropanol.

The acrylic resin includes an acrylic rubber, specifically, obtained by polymerization of a monomer containing a (meth) acrylic acid alkyl ester.

(Meth) acrylic acid alkyl ester is a methacrylic acid alkyl ester and / or an acrylic acid alkyl ester, and examples thereof include methyl (meth) acrylate, ethyl (meth) acrylate, butyl (meth) acrylate, hexyl (Meth) acrylate, isodecyl (meth) acrylate, undecyl (meth) acrylate, lauryl (meth) acrylate, (meth) acrylate, Linear or branched alkyl (meth) acrylates in which the alkyl moiety has not more than 30 carbon atoms, such as tridecyl (meth) acrylate, tetradecyl (meth) acrylate, octadecyl (meth) acrylate and octadecyl (Meth) acrylic acid alkyl ester having 1 to 18 carbon atoms in the alkyl moiety.

These alkyl (meth) acrylate esters may be used alone or in combination of two or more.

The proportion of the (meth) acrylic acid alkyl ester is, for example, not less than 50% by mass, preferably not less than 75% by mass, for example, not more than 99% by mass with respect to the monomer.

The monomer may also include a copolymerizable monomer polymerizable with the (meth) acrylic acid alkyl ester.

The copolymerizable monomer contains a vinyl group and is exemplified by a cyano group-containing vinyl monomer such as (meth) acrylonitrile, a glycidyl group-containing vinyl monomer such as (meth) acrylate glycidyl Vinyl monomers), aromatic vinyl monomers such as styrene, and the like.

The compounding ratio of the copolymerizable monomer is, for example, 50 mass% or less, preferably 25 mass% or less, for example, 1 mass% or more with respect to the monomer.

These copolymerizable monomers may be used alone or in combination of two or more.

When the copolymerizable monomer is a cyano group-containing vinyl monomer and / or an epoxy group-containing vinyl monomer, the acrylic resin to be obtained is preferably a functional group-modified acrylic resin having a functional group-modified acrylic resin ( Specifically, it is a cyano-modified acrylic resin, an epoxy-modified acrylic resin, a cyano-epoxy-modified acrylic resin).

The melt viscosity at 80 캜 of the resin component (the resin component in which the thermosetting resin component is in the A-stage state when the thermosetting resin component is contained) is, for example, 10 to 10,000 mPa · s, preferably 50 to 10000 mPa · s It is also.

The softening temperature (ring method) of the resin component is, for example, 80 占 폚 or lower, preferably 70 占 폚 or lower, and is, for example, 20 占 폚 or higher, preferably 35 占 폚 or higher.

These resin components may be used alone or in combination.

The thermosetting resin component and the thermoplastic resin component may be used in combination.

The resin component may contain known additives such as an elastomer, a flame retardant, a dispersant, a tackifier, a silane coupling agent, a fluorine surfactant, a plasticizer, an antioxidant and a colorant in an appropriate ratio. Preferably an elastomer and / or a flame retardant.

Examples of the elastomer include urethane rubber, silicone rubber, vinyl alkyl ether rubber, polyvinyl alcohol rubber, polyvinylpyrrolidone rubber, polyacrylamide rubber, cellulose rubber, natural rubber, butadiene rubber, chloroprene rubber, styrene / butadiene (SBR), acrylonitrile / butadiene rubber (NBR), isoprene rubber, polyisobutylene rubber, butyl rubber, styrene / ethylene / butadiene / styrene rubber, styrene / isoprene / styrene rubber, styrene / . And styrene-isobutylene rubber is preferable.

The styrene / isobutylene rubber is a synthetic rubber obtained by copolymerization of styrene and isobutylene, and examples thereof include styrene / isobutylene random copolymer, styrene / isobutylene block copolymer, and the like, Include styrene-isobutylene block copolymer.

Specific examples of the styrene / isobutylene block copolymer include styrene / isobutylene / styrene block copolymer (SIBS).

The content of the elastomer is, for example, not less than 1 part by mass, preferably not less than 2 parts by mass, and not more than 100 parts by mass, preferably not more than 50 parts by mass, And preferably 10 parts by mass or less.

As the flame retardant, for example, a phosphazene derivative and the like can be mentioned. The content of the flame retardant is, for example, not less than 0.1 part by mass, preferably not less than 1 part by mass, more preferably not less than 2 parts by mass, relative to 100 parts by mass of the particles, Or less, preferably 10 parts by mass or less, and more preferably 5 parts by mass or less.

As the flame retardant, for example, a phosphazene derivative and the like can be mentioned. The flame retardant may be blended at an appropriate ratio.

The mixing ratio of the particles and the resin component is adjusted so as to be in a desired range in a roll-shaped sheet to be described later.

Next, a method of manufacturing the roll-shaped sheet will be described with reference to Figs. 1 to 8. Fig.

1, the right side of the paper is referred to as "right side", the left side of the paper is referred to as "left side", the lower side of the paper is referred to as "front side", the upper side of the paper is referred to as " Quot; lower side ". 1, the right side shows one side in the direction of the rotation axis of the pair of gears (described later), the left side shows the other side in the direction of the rotation axis, the front side shows one side in the cross direction Direction is the other side. Note that the directions of FIG. 2 and the subsequent drawings are the same as those of FIG. 1.

1, the sheet manufacturing apparatus 1 is constructed so as to produce a rolled sheet 60 from a composition (X) containing particles and a resin component. For example, Respectively. The sheet manufacturing apparatus 1 is provided with a kneader 2, a feeding section 3, a gear structure 4, a sheet adjusting section 5 and a winding section 6. The kneader 2, the feeding section 3, the gear structure 4, the sheet adjusting section 5 and the winding section 6 are arranged and arranged in a substantially L shape in plan view in the sheet manufacturing apparatus 1 have. That is, the sheet manufacturing apparatus 1 is configured to convey the composition X or the sheet 7 (see FIG. 2) in a substantially L shape when viewed from the top.

The kneader 2 is provided on the left side of the sheet manufacturing apparatus 1. [

As shown in Figs. 3 and 4, the kneader 2 is a continuous biaxial kneader, which is provided with a cylinder 70 and two kneading shafts 13.

The cylinder 70 is formed in a substantially elliptical cylinder shape extending in the left-right direction. On the left end side (one end side), as shown in Fig. 2, a composition X containing particles and a resin component, An introduction port 14 is formed as an introduction port for introducing the gas into the inside of the reaction chamber 70. A discharge port 15 serving as a discharge section for discharging the kneaded product Y kneaded with the composition X onto the outside of the cylinder 70 is formed on the right end side (the other end side).

As shown in Fig. 3, the inlet 14 is formed to penetrate the upper wall of the left end of the cylinder 70 and to open upward.

The discharge port 15 is formed at the right end of the cylinder 70 so as to open in the right direction.

As the sectional shape of the discharge port 15, for example, there can be mentioned a rectangular shape, an elliptical shape, a circular shape and the like, preferably an elliptic shape or a circular shape.

The sectional area of the discharge port 15 is 15% or more, preferably 25% or more, for example, 50% or less, preferably 45% or less, Do.

Between the introduction port 14 and the discharge port 15 in the cylinder 70 is formed a melt-kneading section 6a for melt-kneading the composition X.

The melt-kneading portion 6a has a plurality of (two) bent portions 7a for discharging the gas in the melt-kneading portion 6a in the middle of its axial direction.

Each of the bent portions 7a is formed so as to penetrate the upper wall of the cylinder 70. That is, the bent portions 7a and the introduction ports 14 are formed so as to be parallel to each other in the axial direction of the kneading shaft 13.

Further, each of the bent portions 7a is always closed, and can be properly opened as needed.

More specifically, the plurality of vent portions 7a are provided in the left and right direction of the cylinder 70 in such a manner that the first vent portion 54a (located on the side of the introduction port 14) And a second vent portion 55a (a vent portion 7a on the side of the discharge port 15) provided in the vicinity of the left side of the discharge port 15. [

The second vent portion 55a is disposed on the left side of the pipe portion 12a (to be described later) and connected to a pump (not shown). By the suction force of the pump , The gas in the molten kneading section 6a is sucked.

The melt kneading section 6a is provided with a heater (not shown), and the temperature of the melt kneading section 6a is appropriately adjusted in a block unit in the left-right direction of the cylinder 70. [

The kneading shaft 13 is inserted (disposed) inside the cylinder 70. The kneading shaft 13 is a rotary shaft for mixing and shearing the composition X and has a drive shaft 8a, a feed screw portion 9a, a reverse screw portion 10a, a paddle portion 11a as a kneading portion, And a pipe section 12a as a low-shear section are integrally formed.

More specifically, the kneading shaft 13 is provided with a driving shaft 8a, a plurality of (four) feed screw portions 9a, a plurality of (two) reverse screw portions 10a, A paddle portion 11a, and a pipe portion 12a.

The feed screw portion 9a, the reverse screw portion 10a, the paddle portion 11a, and the pipe portion 12a can appropriately change the axial length or the number of installed pipes as required.

A plurality of (four) feed screw portions 9a are portions for conveying the composition X toward the discharge port 15. Specifically, the first feed portion 23a, the second feed portion 24a, A third feed portion 25a and a fourth feed portion 26a, which are arranged at an interval from each other in the axial direction of the drive shaft 8a.

The first feed portion 23a is disposed at the left end of the kneading shaft 13 and when the introduction port 14 and the first vent portion 54a are projected in the radial direction of the drive shaft 8a, As shown in Fig. The length of the first feed portion 23a in the axial direction of the drive shaft 8a is longer than that of other feed portions.

The fourth feed portion 26a is disposed on the most discharge port 15 side among the four feed portions and when the second bent portion 55a is projected in the radial direction of the drive shaft 8a, Respectively. The fourth feed portion 26a is formed such that the axial length of the drive shaft 8a is approximately 1/2 of the first feed portion 23a.

The second feed portion 24a and the third feed portion 25a are disposed between the first feed portion 23a and the fourth feed portion 26a and the axial length of the drive shaft 8a is smaller than the axial length of the drive shaft 8a, Is approximately 1/10 of the first feed portion 23a.

As shown in Fig. 4, the feed screw portion 9a is provided with a spiral screw 20a protruding from the outer peripheral surface of the drive shaft 8a.

More specifically, the screw 20a is formed in a spiral shape in the same direction as the rotational direction (described later) of the drive shaft 8a. That is, the feed screw portion 9a has the screw 20a on the right side.

The pitch interval of the screw 20a in the feed screw portion 9a is, for example, 0.6 cm or more, preferably 1.5 cm or more, and is, for example, 2.0 cm or less.

A plurality of (two) reverse-screw portions 10a are formed by the first reverse portion 30a and the second reverse portion 31a as shown in Fig. 3, As shown in Fig.

The first reverse portion 30a is disposed between the first feed portion 23a and the second feed portion 24a and adjacent to the left side of the second feed portion 24a.

The second reverse portion 31a is disposed between the second feed portion 24a and the third feed portion 25a and adjacent to the left side of the third feed portion 25a.

The first reverse portion 30a and the second reverse portion 31a are formed so that the axial length of the drive shaft 8a is substantially the same. The axial length thereof is approximately 1/20 of the first feed portion 23a.

Like the feed screw portion 9a, the reverse screw portion 10a also has a spiral screw groove 20a protruding from the outer circumferential surface of the drive shaft 8a, as shown in Fig.

The screw groove 20a of the reverse screw portion 10a is formed in a spiral shape opposite to the screw groove 20a of the feed screw portion 9a. That is, the reverse screw portion 10a has the screw 20a on the left side.

The pitch interval of the screw 20a in the reverse screw portion 10a is, for example, not less than 0.6 cm, preferably not less than 1.0 cm, and is not more than 1.5 cm, for example.

3, the plurality of (three) paddle portions 11a are portions for kneading the composition X, specifically, the first paddle portion 27a, the second paddle portion 28a, And a third paddle portion 29a, which are arranged at an interval from each other in the axial direction of the kneading shaft 13. [

The first paddle portion 27a is disposed between the first feed portion 23a and the first reverse portion 30a.

The second paddle portion 28a is disposed between the second feed portion 24a and the second reverse portion 31a.

The third paddle portion 29a is disposed between the third feed portion 25a and the fourth feed portion 26a.

The first paddle portion 27a, the second paddle portion 28a and the third paddle portion 29a have the same length in the axial direction of the drive shaft 8a, Approximately 1/3.

The paddle portion 11a has a plurality of substantially elliptical paddle wings 21a arranged in parallel along the axial direction of the drive shaft 8a as shown in Fig.

More specifically, the plurality of paddle wings 21a are arranged in parallel so that the long diameters of the paddle wings 21a adjacent to each other in the axial direction of the drive shaft 8a are displaced by about 90 占 from each other.

The pipe portion 12a is formed in a substantially cylindrical shape along the axial direction of the drive shaft 8a, and is formed so as not to have irregularities over the entire circumferential surface.

The pipe section 12a is disposed at the right end of the kneading shaft 13 and adjacent to the right side of the fourth feed section 26a. The axial length of the drive shaft 8a of the pipe section 12a is formed to be approximately 1/2 of the first feed section 23a.

3, the kneading shaft 13 is provided with a first feed portion 23a, a first paddle portion 27a, and a second feed portion 23b sequentially from the left end side to the right end side of the drive shaft 8a, The first reverse portion 30a, the second feed portion 24a, the second paddle portion 28a, the second reverse portion 31a, the third feed portion 25a, the third paddle portion 29a, A feed section 26a, and a pipe section 12a.

That is, the kneading shaft 13 is repeatedly arranged with units including a feed portion, a paddle portion, and a reverse portion from the left end side to the right end side of the drive shaft 8a repeatedly. In the unit on the right end side, A feed section and a pipe section are disposed.

The two kneading shafts 13 are disposed along the axial direction of the cylinder 70 in the cylinder 70 as shown in Fig. 4, and are disposed in parallel with each other along the radial direction.

The two kneading shafts 13 are arranged so as not to interfere with each other's rotational drive in the respective portions (the feed screw portion 9a, the reverse screw portion 10a, and the paddle portion 11a).

Both ends of the drive shaft 8a of the kneading shaft 13 protrude outward in the axial direction of the cylinder 70. [ The right end side of the protruded both end portions is connected to a driving source (not shown) in a relatively non-rotatable manner, and the left end side is supported so as to be rotatable relative to a supporting wall (not shown). That is, the kneading shaft 13 is rotationally driven around the axis of the drive shaft 8a by transmitting a drive force from a drive source (not shown) to the drive shaft 8a. More specifically, the kneading shaft 13 rotates clockwise from the inlet 14 side toward the outlet 15 side in the axial direction of the drive shaft 8a.

4, the inner peripheral surface of the cylinder 70, the feed screw portion 9a, the reverse screw portion 10a (see Fig. 3), and the paddle portion 11a of the kneading shaft 13, Are disposed so as to face each other with a slight gap in the radial direction of the kneading shaft 13. [ On the other hand, the inner circumferential surface of the cylinder 70 and the pipe section 12a are arranged at a larger distance in the radial direction of the kneading shaft 13 than in the other parts.

As shown in Fig. 1, the supply unit 3 is provided on the right side of the kneader 2 and extends in the left and right direction. The feeding section 3 is connected to the kneading machine 2 by a connecting pipe 17.

The connecting tube 17 is formed in a substantially cylindrical shape having an axis common to the axis of the cylinder 70. The left end of the connection pipe 17 is connected to the discharge port 15 of the cylinder 70 and the right end of the connection pipe 17 is connected to the supply portion inlet 18 (described later) of the supply unit 3 .

As shown in Figs. 5 and 6, the supply unit 3 includes a first casing 21 and a supply screw 22. [

The first casing 21 has a rectangular shape as viewed in a plane extending in the left-right direction, and the front side is opened across the right-left direction. A supply inlet 18 is formed at the left end of the first housing 21 and a first storage portion 27 is formed at the front end of the first housing 21. [ The first housing 21 is provided with a first accommodating portion 19 for accommodating the supply screw 22 described below. The first accommodating portion 19 is provided with a rear portion 29 and a front portion 30 communicating with the front side of the rear portion 29. Each of the rear portion 29 and the front portion 30 has a substantially circular shape when viewed from the side end face, and is formed across the first housing 21 in the left and right direction.

The supply portion inlet 18 is in communication with the first accommodating portion 19 (the rear portion 29 and the front portion 30).

The first storage portion 27 is formed in a substantially tapered shape when viewed from the side end face that becomes larger toward the front.

The supply screw 22 is housed in the first accommodating portion 19 and includes a first screw 23 and a second screw 24 which extend in the left and right direction and mesh with each other.

The first screw 23 is housed in the rear portion 29 and has a blade 20 which is inclined with respect to the rotational direction R1 of the first screw 23. [ The pitch interval in the direction of the rotation axis of the blade 20 of the first screw 23 is, for example, 5 mm or more, preferably 10 mm or more, and for example, 50 mm or less, preferably 30 mm or less.

The second screw 24 is accommodated in the front portion 30 and has the same configuration and the same dimensions as the first screw 23 and is engaged with the first screw 23 and is rotated in the same direction as the first screw 23 As shown in FIG.

The length of the feed screw 22 (the first screw 23 and the second screw 24) in the direction of the rotational axis is smaller than the width W0 of the first casing 21 by a minute amount of clearance (not shown) As shown in Fig.

The supply section 3 is provided with a motor (not shown) connected to the supply screw 22 on the right side of the first casing 21.

The supply unit 3 is configured to supply the kneaded product Y to the rear side of the kneading machine 2 so as to have a width W0 (that is, a width W0 of the first casing 21) along the discharge direction (lateral direction) To the gear structure 4, as shown in Fig.

As shown in Figs. 6 and 7, the gear structure 4 includes a second casing 31 and a pair of gears 32. As shown in Fig. The gear structure 4 has a structure in which the length W2 of the pair of gears 32 in the direction of the axis of rotation A1 is long and the kneaded material Y supplied from the feeding portion 3 is fed to the sheet adjusting portion 5 It is also a gear pump that carries it.

As shown in Figs. 5 and 6, the second housing 31 is continuously formed on the front side of the first housing 21, and has a rear portion and a front portion opened in the left-right direction, As shown in FIG. A second accommodating portion 40 for accommodating the pair of gears 32 is provided at the rear end portion of the second casing 31 and a gear ejection port 46 is formed at the front end portion. A second storage portion 28 and a discharge passage 44 are formed between the second housing portion 40 and the gear discharge opening 46 so as to communicate with the second housing portion 40 and the gear discharge opening 46.

The second accommodating portion 40 has a lower portion 61 and an upper portion 62 that communicates with the first storing portion 27 and communicates with the upper side of the lower portion 61. Each of the lower portion 61 and the upper portion 62 has a substantially circular shape when viewed from the side end face and is formed to extend in the left and right direction in the second housing 31. [

The gear ejection openings 46 are defined by two ejection walls 45 formed to be spaced apart from each other in the vertical direction and are formed to open forward. The discharge wall 45 is provided at the front end portion of the second casing 31 and has a lower wall 47 and an upper wall 48.

The lower wall 47 has a thick flat plate shape extending in the left-right direction and the up-and-down direction, and each of the front face and the upper face is formed in a flat shape.

The upper side wall 48 has a flat bottom surface. The upper side wall 48 has a substantially L shape as viewed from the side end surface, and the front end portion of the lower portion is formed so as to protrude forward with respect to the front surface of the upper portion. That is, in the upper side wall 48, the front end portion of the lower portion is formed as a protruding portion 63 as a doctor having a substantially rectangular shape when viewed from the side end face. The protruding length of the protruding portion 63 (for example, the length in forward and backward directions) is, for example, 2 mm or more, and is 150 mm or less, for example, 50 mm or less. The thickness of the protruding portion 63 (i.e., the length in the up-down direction) is, for example, 2 mm or more, and is, for example, 100 mm or less, preferably 50 mm or less. The front surface of the projecting portion 63 and the front surface of the lower wall 47 are formed so as to be in the same position when projected in the vertical direction.

The second storage portion 28 communicates with the front side of the second accommodating portion 40 and is formed in a substantially U shape as viewed from the side end surface in which the rear portion is opened.

The discharge passage 44 communicates with the front side of the second storage portion 28 and communicates with the rear side of the gear discharge port 46. The discharge passage 44 is formed in a substantially linear shape extending in the forward direction as viewed from the side end face.

As shown in Fig. 7, the pair of gears 32 is, for example, a double helical gear, specifically, a first gear 33 and a second gear 34, respectively.

The first shaft 25 which is the rotation shaft of the first gear 33 is provided so as to extend in the left and right direction in the second casing 31 (see Fig. 6).

The second shaft 26 as the rotation shaft of the second gear 34 is provided so as to extend in parallel with the first shaft 25 in the second casing 31 (see Fig. 6). Further, the second shaft 26 is arranged to face upward with respect to the first shaft 25.

The first gear 33 and the second gear 34 are housed in the lower portion 61 and the upper portion 62, respectively.

Each of the first gear 33 and the second gear 34 has, specifically, inclined teeth 35 that mesh with each other.

The sawtooth pattern of the warp teeth 35 of the first gear 33 is shifted from the downstream side of the rotational direction R2 of the first gear 33 toward the upstream side of the rotational direction R2, And is inclined outward in the direction A1. The inclined teeth 35 integrally include first inclined teeth 36 and second inclined teeth 37 having different sawtooth patterns. In the first gear 33, the first tilted tooth 36 is formed from the center in the axial direction of the first gear 33 to the right side, and the second tilted tooth 37 is formed in the center of the first gear 33 And is formed from the center in the axial direction to the left.

More specifically, the sawtooth pattern of the first warp teeth 36 is shifted from the left side (the center side) to the right side (the right side end side) from the downstream side of the rotation direction R2 toward the upstream side of the rotation direction R2, . On the other hand, the sawtooth pattern of the second warp tooth 37 is symmetrically formed with respect to the sawtooth pattern of the first warp tooth 36 in the lateral direction centering portion of the first gear 33. Specifically, (Toward the left end side) from the right side (the center side) as it goes from the downstream side of the rotation direction R2 to the upstream side of the rotation direction R2.

The second gear 34 is formed so as to be vertically symmetrical with respect to the first gear 33 so as to be engaged with the first gear 33. Concretely, the second gear 34 is engaged with the first inclined teeth 36 The third tilted tooth 38 and the fourth tilted tooth 39 engaged with the second tilted tooth 37 integrally.

As shown in Fig. 8, the pair of gears 32 is configured such that the engaging portion indicated by a black circle is in contact with the first gear 33 and the second gear 34 in a point shape as viewed from the side end surface , It is a side cross-sectional point contact type. The pair of gears 32 are arranged in such a manner that the engaging portion is formed in a spiral shape of the first gear 33 and the second gear 34 along the sawtooth pattern of the pair of gears 32, Line contact type.

Each of the oblique teeth 35 of the pair of gears 32 has a concave surface 42 provided to be spaced apart in the rotational direction R2 and curved inward in the radial direction, And a curved surface 41 integrally provided with a convex surface 43 curved outwardly in the radial direction from both end portions in the peripheral direction of the concave surface 42.

Next, the engagement of the pair of gears 32 on the curved surface 41 will be described with reference to Figs. 8 (a) to 8 (c).

8A, the downstream end of the convex surface 43 of the first gear 33 in the rotational direction R2 and the concave surface 42 of the second gear 34 are engaged with each other, The first gear 33 and the second gear 34 are engaged with each other as shown in the arrows in Fig. 8 (a) and Fig. 8 (b) The intermediate portion of the rotational direction R2 of the convex surface 43 of the first gear 33 and the intermediate portion of the rotational direction R2 of the concave surface 42 of the second gear 34, As shown in Fig. 8 (b) and 8 (c), when the first gear 33 and the second gear 34 rotate in the rotation direction R2, the first gear 33 The upstream end of the convex surface 43 of the second gear 34 is engaged with the upstream end of the rotational direction R2 of the concave surface 42 of the second gear 34. [ In other words, the convex surface 43 of the first gear 33 and the engagement portion of the concave surface 42 of the second gear 34 are located at the downstream side end portion, And the upstream side end portion.

The engaging portion of the concave surface 42 of the first gear 33 and the convex surface 43 of the second gear 34 is formed on the downstream side of the rotational direction R2 on each surface End portion, midway portion, and upstream side end portion.

Therefore, the curved surface 41 of the first gear 33 and the engaging portion of the curved surface 41 of the second gear 34 continuously move along the rotational direction R2. The movement of the engagement portion prevents the storage portion in which the kneaded product (Y) is stored in the transportation of the kneaded product (Y).

The gear structure 4 is provided with a motor (not shown) connected to the first shaft 25 and the second shaft 26 of the pair of gears 32 on the right side of the supply screw 22 Is installed.

5 and 6, the seat adjustment portion 5 is provided so as to include the projection portion 63 of the upper side wall 48 on the front side of the gear structure 4, and, for example, A protrusion 63 in the structure 4, and a support roll 51 as a moving support. 2, the sheet forming portion 5 is provided with a substrate feed roll 56, a separator laminate roll 57, a rolling roll 58 and a separator feed roll 59 .

The projecting portion 63 serves as a wall for partitioning the gear discharge port 46 of the second casing 31 in the gear structure 4 as shown in Figs. 2 and 6, (Or knife) that adjusts the thickness of the sheet 7 discharged from the gear discharging port 46 of the camshaft.

The support rolls 51 are disposed so as to face each other so that the gaps 50 are formed with respect to the projecting portions 63. The rotation axis of the support roll 51 is parallel to the first axis 25 and the second axis 26 of the pair of gears 32 and concretely, Extended. 6, the rotation axis of the support roll 51 is arranged so as to overlap the gear ejection orifice 46 and the protrusion 63 when projected in the forward and backward directions. Further, the support rolls 51 are configured to support and convey the sheet 7.

Therefore, the support roll 51 is configured to allow the sheet 7 to pass through the gap 50.

As shown in Fig. 2, the substrate feed rolls 56 are provided below the support rolls 51 with an interval therebetween. The rotation axis of the substrate feed roll 56 extends in the left and right direction and the substrate 8 is wound on the circumferential surface of the substrate feed roll 56 in the form of a roll.

The separator laminate roll 57 and the rolling rollers 58 are provided in front of the support rollers 51 at intervals. The rotation axes of the separator laminate roll 57 and the rolling roll 58 are arranged so as to extend in the left-right direction. The separator laminate roll 57 is arranged on the upper side with respect to the rolling roll 58 and is configured to be pressurizable with respect to the rolling roll 58.

The rolling roll 58 is configured so as to be capable of rolling with respect to the sheet 7 and the base material 8 under the pressure of the separator laminate roll 57. When the upper end portion is projected in the forward and backward directions, And is disposed at the same position as the upper end of the support roll 51.

The separator feed rolls 59 are provided at an interval obliquely above the separator laminate rolls 57 at intervals. The rotation axis of the separator feed roll 59 extends in the left and right direction and the separator 9 is wound on the circumferential surface of the separator feed roll 59 in the form of a roll.

The winding portion 6 is provided in front of the sheet adjusting portion 5 and includes a tension roll 52 and a winding roll 53. [

More specifically, the upper end portion of the tension roll 52 is located at the upper end of the rolling roll 58 when the rollers 52 are projected in the forward and backward directions, As shown in FIG. The rotation axis of the tension roll 52 is formed to extend in the left-right direction.

The take-up rolls 53 are arranged obliquely downward and opposed to the tension rolls 52 with a gap therebetween. The rotation axis of the winding roll 53 extends in the left and right direction and the laminated sheet 10 is rolled up (wound) on the circumferential surface of the winding roll 53, 60 can be obtained.

The dimensions of the sheet manufacturing apparatus 1 are appropriately set corresponding to the types and blending ratios of particles and resin components to be used and the width W1 and thickness T1 of the intended roll-shaped sheet 60.

5, the width W0 of the first housing 21 is set to, for example, the relationship between the length W2 in the axial direction of the pair of gears 32 and the following formula (1) Is set to satisfy the relationship of the following formula (2), more preferably the relation of the following formula (3).

W2-100 (mm)? W0? W2 + 150 (mm) (1)

W2? 50 (mm)? W0? W2 + 100 (mm) (2)

W2-20 (mm)? W0? W2 + 50 (mm) (3)

7, the length W2 in the axial direction of the pair of gears 32 can be appropriately selected in accordance with the width W1 of the sheet 7 or the roll sheet 60 to be manufactured, Concretely, it is similar to the width W0 of the first casing 21 described above and is set to, for example, 70% or more, for example, the width W1 of the sheet 7 or the roll- , Preferably 80% or more, and for example, 100% or less.

Specifically, the length W2 in the direction of the axis of rotation of the pair of gears 32 is, for example, 200 mm or more, preferably 300 mm or more, and is, for example, 2000 mm or less.

The gear diameter of the pair of gears 32 (the diameter of the gear 32 (specifically, the diameter of the blade), specifically, the diameter of the blade) is set so that the pair of gears 32 are not distorted Concretely, for example, 10 mm or more, preferably 20 mm or more, and for example, 200 mm or less, preferably 80 mm or less.

The tooth length of the pair of gears 32 is, for example, not less than 1 mm, preferably not less than 3 mm, and is, for example, not more than 30 mm, preferably not more than 20 mm.

The pitch interval in the direction of the axis of rotation A1 of the oblique teeth 35 is, for example, 5 mm or more, preferably 10 mm or more, and is, for example, 30 mm or less, preferably 25 mm or less. The angle (inclination angle) of the sawtooth streaks of the oblique saw teeth 35 with respect to the axis of rotation of the pair of gears 32 is, for example, 5 degrees or more, preferably 10 degrees or more, more preferably 15 And is, for example, less than 90 degrees, preferably 85 degrees or less, more preferably 80 degrees or less.

5 and 6, the distance L1 in the front-rear direction of the gap 50 is appropriately set in accordance with the desired thickness, and more specifically, the total thickness of the sheet 7 and the base material 8 For example, 10 mu m or more, preferably 30 mu m or more, more preferably 100 mu m or more, and, for example, 1000 mu m or less, preferably 800 mu m or less, Or less.

The outer diameter of the winding roll 53 is, for example, 76 mm or more, preferably 152 mm or more, and is, for example, 500 mm or less.

Hereinafter, a method for producing the roll-shaped sheet 60 from the composition (X) containing particles and a resin component will be described using this sheet production apparatus 1. Fig.

First, as shown in Fig. 2, a composition (X) containing particles and a resin component is introduced into an introduction port (14).

In the sheet manufacturing apparatus 1, the kneader 2, the supply unit 3, and the gear structure 4 are adjusted to a predetermined temperature and rotational speed. The temperatures of the kneader 2, the feeding section 3 and the gear structure 4 are set such that the temperature of the kneading machine 2 is higher than the softening temperature when the resin component contains a thermoplastic resin component, When the resin component (for example, an epoxy resin) is contained, the curing temperature is lower than the curing temperature, specifically, for example, 200 占 폚 or lower, preferably 150 占 폚 or lower, Component, it is at least the softening temperature thereof, and specifically, it is, for example, at least 50 캜, preferably at least 70 캜.

Further, the substrate 8 is previously wound on the substrate feed roll 56.

Examples of the base material 8 include plastic films such as a polypropylene film, an ethylene-propylene copolymer film, a polyester film (PET or the like) and polyvinyl chloride, for example, paper such as kraft paper, Woven fabrics such as polyester nonwoven fabric and vinylon nonwoven fabric, for example, metal foil, and the like. The thickness of the base material 8 is appropriately selected according to its purpose and application, and is, for example, 10 to 500 탆. The surface of the substrate 8 may also be subjected to a releasing treatment.

Further, the separator 9 is wound around the separator feed roll 59 in advance.

The separator 9 may be the same as that of the base material 8, and the surface of the separator 9 may be surface-treated. The thickness of the separator 9 is appropriately selected according to its purpose and purpose, and is, for example, 10 to 500 mu m.

Subsequently, the composition (X) is introduced into the cylinder (70) through the introduction port (14) of the cylinder (70).

In the kneader 2, the particles and the resin component contained in the composition (X) are kneaded and extruded by the rotation of the kneading shaft 13 while being heated by a heater (not shown) The kneaded product Y reaches the supply portion inlet 18 of the supply portion 3 through the connection pipe 17 from the discharge port 15 as shown in Fig. 5 (kneading and extruding step).

3, when a driving force is transmitted from a driving source (not shown) to the driving shaft 8a, the kneading shaft 13 is rotationally driven so that the composition X is fed to the first feed portion 23a while being conveyed toward the first paddle portion 27a.

At this time, the cylinder 70 (melt-kneaded portion 6a) located outside the first feed portion 23a is adjusted to, for example, 15 to 20 占 폚 by a heater (not shown). With the introduction of the composition X, the air or the like which has entered the inside of the cylinder 70 is released to the outside of the cylinder 70 by opening the first vent portion 54a.

Subsequently, the conveyed composition X is kneaded in the first padding portion 27a.

At this time, the melt kneading portion 6a located outside the first paddle portion 27a is adjusted to, for example, 40 to 80 占 폚 by a heater (not shown).

The kneaded composition X is extruded toward the first reverse portion 30a by the pressure output of the composition X conveyed by the rotational driving of the first feed portion 23a.

Most of the composition X extruded toward the first reverse portion 30a passes through the first reverse portion 30a and reaches the second feed portion 24a. On the other hand, a part of the extruded composition X is returned to the first paddle portion 27a by rotational driving of the first reverse portion 30a, and is kneaded again.

Thereby, the kneading of the composition (X) is accelerated and the conveying speed of the composition (X) is adjusted.

Subsequently, the composition X that has passed through the first reverse portion 30a is transported toward the second paddle portion 28a and the second reverse portion 31a by the second feed portion 24a.

Thereby, the composition X passes through the second paddle portion 28a and the second reverse portion 31a while being kneaded like the first paddle portion 27a and the first reverse portion 30a.

At this time, the melt kneading portion 6a located outside the second paddle portion 28a is adjusted to, for example, 60 to 120 占 폚 by a heater (not shown).

Subsequently, the composition X having passed through the second reverse portion 31a is conveyed to the third paddle portion 29a by the succeeding third feed portion 25a, and is conveyed again at the third paddle portion 29a Kneaded. Thereby, the composition (X) is produced as a kneaded product (Y).

At this time, the melt kneading portion 6a located outside the third paddle portion 29a is adjusted to, for example, 80 to 140 占 폚 by a heater (not shown).

Then, the kneaded product Y is extruded by rotational drive of the kneading shaft 13 and reaches the fourth feed portion 26a.

At this time, by driving a pump (not shown) connected to the second vent portion 55a, moisture and volatile components in the kneaded product Y are discharged to the outside of the molten kneading portion 6a.

Thereby, pores in the kneaded product (Y) can be reduced.

Subsequently, the kneaded product (Y) is conveyed to the pipe section (12a) by the fourth feed section (26a).

In the pipe section 12a, as described above, the entire circumferential surface is formed so as not to have irregularities. Thus, in the pipe section 12a, the kneaded product Y is smoothly moved along the axial direction of the pipe section 12a by suppressing the front end in the direction intersecting the axial direction of the kneading shaft 13 .

Then, the kneaded product (Y) is discharged from the discharge port (15).

As described above, the kneaded product (Y) in which the generation of pores is suppressed is produced from the composition (X).

As shown in Fig. 1, the kneaded product Y is fed in the feeding section 3 along the feeding direction of the kneader 2, that is, in the left-right direction by the rotation of the feeding screw 22 In the direction intersecting with the discharge direction (specifically, in the direction orthogonal to the discharge direction) so as to have the width W0 (the width W0 of the first housing 21) (Supply step). That is, the kneaded product (Y) that has been extruded to the right from the kneader (2) through the connecting pipe (17) and reaches the supply unit (3) is changed in the feeding direction by 90 degrees in the feeding unit (3). Concretely, the kneaded product Y is supplied to the gear structure 4 through the first storage portion 27 so as to have a width W0 along the left-right direction while the carrying direction is changed forward from the right direction . That is, in the supply unit 3, the discharge in the discharge direction (lateral direction) of the kneaded product Y (that is, the transport in the delivery direction of the supply screw 22) ) Simultaneously.

Thereafter, the kneaded product Y is deformed in the rotational axis direction A1 of the pair of gears 32 in the gear structure 4, and is formed as a sheet 7 and is transported forward Transformation conveying step).

Concretely, the kneaded product Y is formed as a sheet 7 by being widened from the central portion in the direction of the axis of rotation A1 to both ends by the engagement of the pair of gears 32. Then, it is transported forward.

6, the kneaded product Y is transferred from the upper end and the lower end of the front portion of the first storage portion 27 to the lower portion 61 of the second storage portion 40, 1 gear 33 and the upper portion 62 of the second accommodating portion 40 and the second gear 34 in the forward direction along the rotational direction R2 of the pair of gears 32 And reaches the second storage portion 28.

At this time, the kneaded product Y of the second storage portion 28 is returned (backward) to the first storage portion 27 through the engagement portion of the oblique saw tooth 35 (see FIG. 8) (Formed) by the engagement portion of the oblique saw tooth 35 while being prevented by the pair of gears 32 and spreading in the lateral direction.

More specifically, as shown in Fig. 7, at the right side portion of the gear structure 4, by engaging the first tilted tooth 36 and the third tilted tooth 38, the pair of gears 32 To the right end portion in the direction of the rotation axis line A1. On the other hand, in the left portion of the gear structure 4, the engagement of the second warp tooth 37 and the fourth warp tooth 39 causes the pair of gears 32 to extend from the center of the rotation axis direction A1 And widen toward the left end.

Thus, the sheet 7 can be obtained from the kneaded product (Y).

5 and 6, the obtained sheet 7 reaches the gear discharge port 46 through the second storage portion 28 and the discharge passage 44, and subsequently, 46 to the support roll 51. The support rolls 51,

Specifically, a substrate 8 fed from a substrate feed roll 56 (see Fig. 2) is laminated on the circumferential surface of the support roll 51, and the sheet 7 is conveyed through the substrate 8 And is conveyed in the rotating direction of the support roll 51 while being supported by the support roll 51.

The sheet 7 conveyed from the gear ejection port 46 is once conveyed through the base material 8 to the rear of the support roll 51 and immediately transferred to the peripheral surface of the support roll 51 Thereby adjusting the thickness. Concretely, the excess kneaded product Y is scraped off by the projecting portion 63 on the surface of the base material 8 supported by the support roll 51, and the desired thickness T1 and the desired width W1 ) Sheet 7 (gap passing step).

The speed (coating speed) of the sheet 7 passing through the gap 50 between the protruding portion 63 and the circumferential surface of the support roll 51 is, for example, 0.01 m / min or more, Min or more, for example, 1.0 m / min or less, preferably 0.35 m / min or less.

The thickness T1 of the sheet 7 is substantially equal to the distance L1 in the front and rear direction of the gap 50 and is concretely 50 mu m or more, preferably 100 mu m or more, For example, 1000 mu m or less, preferably 800 mu m or less, and more preferably 750 mu m or less.

Further, the composition (sheet-modified composition) which is passed through the gap passing process is, for example, at a temperature range of 50 to 250 ° C, for example, at most 5.0 x 10 ⁴ Pa, preferably at most 4.0 x 10 ⁴ Pa, Is 3.0 x 10 < ⁴ > Pa or less, and has a shear stress of 1.0 x 10 < ³ > Pa or more, for example. The shear zone only needs to have a shear stress of the above value at a temperature of at least part of the above temperature range (i.e., 50 to 250 DEG C, preferably 60 to 150 DEG C, more preferably 80 to 100 DEG C) Preferably has a shear stress of the above value over the entire temperature range.

If the shear stress is 5 x 10 < ⁴ > Pa or less, the width of the sheet 7 after the gap passing process is easily formed into a predetermined width, On the other hand, when the shear stress is 1.0 x 10 < ³ > Pa or more,

The shear rate can be appropriately determined from the gap 50 and the application speed.

The method of measuring shear stress and shear rate will be described in detail in the following embodiments.

The temperature in the gap passing step is, for example, 50 DEG C or higher, preferably 60 DEG C or higher, more preferably 80 DEG C or higher, and further, for example, 250 DEG C or lower, preferably 150 DEG C or lower, More preferably 100 DEG C or less.

Subsequently, as shown in Fig. 2, the base material 8 on which the sheet 7 is laminated is conveyed from the support roll 51 toward the separator laminate roll 57 and the rolling roll 58, and the separator laminate Between the roll 57 and the rolling roll 58, the separator 9 is laminated on the upper surface of the sheet 7. Thereby, the sheet 7 is obtained as the laminated sheet 10 in which the base material 8 and the separator 9 are laminated on both surfaces (lower surface and upper surface).

Thereafter, the laminated sheet 10 is passed through a tension roll 52 and then wound up in a roll by a winding roll 53 to produce a rolled sheet 60 (winding step).

At this time, in the roll-shaped sheet 60, the separator 9, the sheet 7 and the base material 8 are repeatedly laminated in the radially outward direction of the take-up roll 53 in this order.

In the case where the resin component contains a thermosetting resin component in the sheet manufacturing apparatus 1, the sheet 7 is heated in the kneader 2 until it is wound on the winding roll 53 The thermosetting resin component of the sheet 7 wound around the take-up roll 53 is also in the B-stage state.

The roll-shaped sheet 60 produced by the above-described production method has flexibility at room temperature (25 캜).

When the resin contains an epoxy resin in the roll-shaped sheet 60, the tensile modulus of elasticity of the B-stage sealing sheet 7 (excluding the base material 8 and the separator 9) at 25 캜 is, for example, For example, not more than 20 GPa, preferably not more than 10 GPa, more preferably not more than 5 GPa, for example, not less than 0.1 GPa, preferably not less than 0.5 Gaa, more preferably not less than 1.0 GPa. The method of measuring the tensile modulus of the sealing sheet 7 of the B stage will be described in detail in the evaluation of the following embodiments.

When the tensile elastic modulus is not more than the upper limit, the sealing object to be sealed can be improved by embedding the sealing object described later reliably. On the other hand, when the tensile elastic modulus is equal to or lower than the lower limit, sagging of the sealing sheet 7 before being wound (wound) on the winding roll 53 is prevented, and workability can be improved.

The volume ratio of the particles in the roll-shaped sheet 60 is, for example, more than 30% by volume, preferably not less than 35% by volume, preferably not less than 40% by volume, more preferably not less than 60% More preferably, it is at least 70 vol%, for example, at most 98 vol%, preferably at most 95 vol%.

If the volume ratio of the particles is less than the above lower limit, the specific physical properties of the particles can not be sufficiently exerted. On the other hand, when the volume ratio of the particles is less than the upper limit, the flexibility of the sealing sheet 7 is ensured and the roll-shaped sheet 60 can be reliably obtained.

The thickness of each sheet 7 of the roll-shaped sheet 60 is, for example, 10 占 퐉 or more, preferably 30 占 퐉 or more, more preferably 100 占 퐉 or more, particularly preferably 200 占 퐉 or more, For example, it is 800 μm or less.

When the thickness is equal to or smaller than the lower limit, the thickness of the roll-shaped sheet 60 containing particles in a desired ratio can be sufficiently secured, and the object to be sealed can be reliably covered and embedded.

The width (length orthogonal to the longitudinal direction and thickness direction) of the roll-shaped sheet 60 is, for example, 200 mm or more, preferably 500 mm or more, more preferably 1000 mm, and, for example, It is also. When the width of the roll-shaped sheet 60 is not less than the above-mentioned lower limit, various sealing objects are covered / embedded by one sheet of the sealing sheet 7 drawn out from one roll-like sheet 60, can do.

The inner diameter of the roll-shaped sheet 60 is the same as the outer diameter of the winding roll 53. The outer diameter of the roll-shaped sheet 60 is, for example, 76 mm or more, preferably 152 mm or more, and is, for example, 500 mm or less.

According to the roll-shaped sheet 60, the particles are formed into a roll shape while containing a high proportion of the particles. As a result, it is possible to reduce the storage space while sufficiently exhibiting the specific physical properties possessed by the particles, and is excellent in transportability.

According to the production method of the roll-shaped sheet 60, after the composition X containing the particles and the resin component is transported while being deformed in the axial direction A1 thereof by using the gear structure 4, The sheet (composition) deformed in the direction A1 is passed through the gap 50 with the projecting portion 63 while being supported and supported by the support roll 51 via the base material 8 in the sheet adjusting portion 5, The mixing ratio of the particles exceeds 30% by volume, whereby the long sheet 7 can be produced. As a result, in the subsequent winding step, since the long sheet 7 can be easily wound on the winding roll 53, the roll-shaped sheet 60 can be obtained.

Further, since the kneaded product (Y) is deformed by using the gear structure (4), the particles can be formed into a sheet shape by containing the particles in a resin component at a high blending ratio.

As a result, the roll-shaped sheet 60 in which the particles are dispersed in the resin component at a high mixing ratio can be produced.

Further, the shear stress of the composition passing through the gap passing step is 5.0 x 10 < ⁴ > Pa or less in the temperature range of 50 to 250 deg. Therefore, it is easy to form the sheet width after the gap passing process to a predetermined width, and a roll-shaped sheet having a desired width can be produced.

Also, in the case where the roll-shaped sheet 60 is used as a heat-radiating sheet to form a composite with a flexible circuit board (a composite circuit board), the heat-radiating sheet produced in the form of a roll is easily rolled, Cost, a composite circuit board can be manufactured.

In addition, since the mixing ratio of the particles in the roll-shaped sheet 60 exceeds 30% by volume, the roll-shaped sheet 60 is excellent in the physical properties (for example, heat conductivity (thermal conductivity) (Conductivity), insulation, magnetism, etc.) can be sufficiently exhibited.

Thus, when the roll-shaped sheet 60 is fed from the winding roll 53, it is possible to use a thermally conductive sheet such as a heat-radiating sheet, for example, a conductive sheet such as an electrode material or a current collector, Sheet, for example, a magnetic sheet and the like.

The roll-shaped sheet 60 produced by the production apparatus shown in Fig. 1 has a substrate and a separator laminated on both surfaces in the thickness direction of the sheet (layer) including the composition containing the particles and the resin component, A base material or a separator may be laminated only on one side in the thickness direction, or a sheet not laminated on both sides (that is, a single layer only of a sheet containing a composition containing particles and resin components).

7, when the length W2 of the pair of gears 32 in the direction of the axis of rotation is 200 mm or more, the sheet W having a large width W1 7), and can be suitably used for a wide range of applications.

Although not shown in Fig. 1, the composition X may be directly supplied to the supply portion 3 or the gear structure 4, for example, without forming the kneader 2 in the sheet manufacturing apparatus 1 .

Preferably, the kneader 2 is provided in the sheet manufacturing apparatus 1 as in the embodiment of Fig.

Thus, the kneaded product (Y) reaching the feed part (3) or the gear structure (4) is preliminarily kneaded and extruded by the kneader (2), so that the dispersibility of the particles in the resin component can be further improved.

Although not shown in Fig. 1, for example, the sheet 7 is wound on the take-up roll 53 without forming the separator laminate roll 57 and the separator feed roll 59 in the sheet manufacturing apparatus 1 And the separator 9 may not be laminated. At this time, in the roll-shaped sheet 60, the sheet 7 and the base material 8 are repeatedly laminated in the radially outward direction of the take-up roll 53. Preferably, the base material 8 subjected to the release treatment at least on its back side is used.

Generally, when a sealing sheet is used, it is necessary to carry the sealing sheet prepared in the shape of a piece separately, or to arrange the sealing sheet in a sealed object one by one. As a result, the tact time is long, and when the sealing sheet is taken out from a tray or the like, scratches may occur on the sealing sheet, which may be disadvantageous in handling properties. Further, in order to mass-produce the sealing sheet, a number of sheet producing apparatuses are required.

On the other hand, since the roll-shaped sheet 60 obtained by the sheet manufacturing apparatus 1 is produced in a roll shape, the object to be sealed can be continuously sealed by the sheet 7 like this. In addition, the above-described handling property can be improved, and a sheet 7 having a small number of sheets can be produced in a large quantity in the sheet production apparatus 1 required. Further, the cost required for sealing can be reduced. That is, it is possible to shorten the tact time, improve the handling property, and reduce the investment cost.

Further, in the case where the particles are formed of an insulating material and the resin component contains an insulating thermosetting resin component, the roll-shaped sheet 60 may be a thermosetting insulating resin sheet such as a thermosetting resin sheet , A sealing sheet).

Next, an embodiment in which the roll-shaped sheet 60 is made into a particle-containing roll-shaped sheet will be described in detail.

In the following description, description of the same configuration as that of the above embodiment will be omitted.

As the particle, a nitride and an oxide are preferably used from the viewpoint of reinforcing property.

As the material, an insulating material is preferably used. Examples of the insulating material include nitride, oxide and the like. Specifically, BN, silica and the like can be mentioned.

The resin component contains an epoxy resin and / or a phenolic resin.

Further, the epoxy resin is preferably used in combination with a curing agent and / or a curing accelerator and is produced as an epoxy resin composition and contained in the resin component.

The above-mentioned curing agent and / or curing accelerator may be used as a solvent solution and / or a solvent dispersion prepared by dissolving and / or dispersing in a solvent, if necessary.

The resin component may further contain a thermosetting resin component or a thermoplastic resin component other than the epoxy resin, if necessary.

Examples of the thermosetting resin component other than the epoxy resin include thermosetting polyimide, urea resin, melamine resin, unsaturated polyester resin, diallyl phthalate resin, silicone resin, and thermosetting urethane resin.

The phenol resin is a resin contained in the above-mentioned phenolic compound, and can be used in combination with an epoxy resin as a curing agent. When used in combination with an epoxy resin, the compounding ratio of the phenol resin is, for example, not less than 1 part by mass, preferably not less than 5 parts by mass, more preferably not less than 10 parts by mass based on 100 parts by mass of the epoxy resin, , For example, 200 parts by mass or less, preferably 150 parts by mass or less.

The roll-shaped sheet 60 is obtained by winding a sealing sheet formed as a thermosetting insulating resin sheet in the form of a roll by the same method as above by the sheet manufacturing apparatus 1 shown in Figs. 1 to 8 Loses.

Next, a method for producing the roll-shaped sheet 60 which is a particle-containing roll-shaped sheet will be described with reference to Figs. 1 to 8. Fig.

1, a sheet manufacturing apparatus (a particle-containing roll-shaped sheet producing apparatus) 1 is configured to produce a roll-shaped sheet 60 (see Fig. 2) from a composition X containing particles and a resin component A kneader 2, a feeding portion 3, a gear structure 4, a sheet adjusting portion (sealing sheet adjusting portion) 5, and a winding portion 6.

Either the separator (9) or the substrate (8) is removed from the sealing sheet (7). Thereafter, the sealing sheet 7 is placed on the object to be sealed so as to cover / embed the object to be sealed.

Examples of the sealing target include a semiconductor device, a hard disk, an LED device (television, light, display, etc.), an EL device (organic EL display, organic EL light, etc.), a capacitor, , Surface acoustic wave (SAW) filters, and various sensor devices.

Subsequently, the other of the separator 9 and the substrate 8 is removed from the sealing sheet 7.

Thereafter, the sealing sheet 7 is heated to completely cure the sealing sheet 7 (C-stage). The heating conditions for fully curing the sealing sheet 7 include heating temperatures of, for example, 100 ° C or higher, preferably 120 ° C or higher, and for example, 180 ° C or lower, preferably 160 ° C or lower It is also. The heating time is, for example, 30 minutes or longer, preferably 60 minutes or longer, and is, for example, 120 minutes or shorter, preferably 70 minutes or shorter.

Thereby, the object to be sealed is sealed by the sealing sheet 7.

The tensile elastic modulus of the sealing sheet 7 of the C stage at 25 캜 is preferably 0.1 GPa or more, preferably 1 GMPa or more, more preferably 2 GPa or more, for example, 20 GPa or less, Preferably 8 GPa or less, more preferably 5 GPa or less. The method of measuring the tensile modulus of elasticity of the sealing sheet 7 of the C stage will be described in detail in the evaluation of the following embodiments.

If the tensile elastic modulus at 25 deg. C of the sealing sheet 7 of the C stage is not less than the above lower limit, there is an advantage that the dicing property of the resin is excellent, and if it is not more than the upper limit, the warpage can be reduced.

Conventionally, a method for producing a sealing sheet from a composition containing particles and a resin component has been frequently studied.

For example, the following method has been proposed (see, for example, Japanese Patent Laid-Open Publication No. 2011-32434).

That is, a coating varnish obtained by dispersing and mixing silica powder, an epoxy resin, a phenol resin, and methyl ethyl ketone was prepared. Subsequently, a varnish for application and coating was applied on the exfoliated surface of the polyester film and dried , The sheet is formed on the polyester film. Thereafter, they are cut into a predetermined shape to prepare a plurality of sheets. Subsequently, each of the plurality of sheets is peeled off from the polyester film, and a plurality of peeled sheets are laminated, I'm getting a sheet.

However, in the method described in Patent Document 1, there is a problem in that a plurality of sheets are peeled off each time from the polyester film, and then the sheets are stacked to produce a sheet, the number of manufacturing steps is large and the manufacturing efficiency is low have.

Further, the sheet obtained by the method described in Japanese Patent Laid-Open Publication No. 2011-32434 is a flat sheet having a short side. When such a short sheet is stacked and stored in the form of a flat sheet, not only a large storage space is required but also a disadvantage in terms of transportability.

However, the roll-shaped sheet 60, which is also the particle-containing roll-shaped sheet, contains the particles in a high mixing ratio while the sealing sheet 7 is rolled. Therefore, it is possible to sufficiently exhibit the specific properties possessed by the particles, specifically, the insulating property and the reinforcing property, while reducing the storage space, and being excellent in transportability, while being produced with good production efficiency.

According to the production method of the roll-shaped sheet 60, after the composition X containing the particles and the resin component is transported while being deformed in the axial direction A1 thereof by using the gear structure 4, The sheet (composition) deformed in the direction A1 is passed through the gap 50 with the projecting portion 63 while being supported and supported by the support roll 51 via the base material 8 in the sheet adjusting portion 5, The mixing ratio of the particles exceeds 30% by volume, whereby the long sealing sheet 7 can be produced. As a result, in the subsequent winding step, since the long sealing sheet 7 can be easily wound around the winding roll 53, the roll-shaped sheet 60 can be obtained.

Further, since the kneaded product (Y) is deformed by using the gear structure (4), the particles can be molded into a sheet form by containing the particles in a resin component at a high blending ratio.

As a result, the roll-shaped sheet 60 in which the particles are dispersed in the resin component at a high mixing ratio can be produced.

In general, when the sealing sheet 7 is used, it is necessary to carry the sealing sheet 7 prepared in the shape of an individual piece, or to arrange the sealing sheet 7 one by one in the sealing object. As a result, the tact time is long, and when the sealing sheet 7 is taken out from a tray or the like, scratches may occur on the sealing sheet 7, which may result in deteriorated handling properties. Further, in order to mass-produce the sealing sheet 7, a plurality of sheet manufacturing apparatuses 1 are required.

On the other hand, since the roll-shaped sheet 60 obtained by the sheet manufacturing apparatus 1 is manufactured in a roll shape, the object to be sealed can be continuously sealed by such a sealing sheet 7. In addition, the above-described handling property can be improved, and the sheet-producing apparatus 1 required can also mass-produce the roll-shaped sheet 60 from the small-sized, long-shaped sealing sheet 7. Further, the cost required for sealing can be reduced. That is, it is possible to shorten the tact time, improve the handling property, and reduce the investment cost.

The roll-shaped sheet 60 produced by the production apparatus shown in Fig. 1 is formed on both surfaces in the thickness direction of the sealing sheet (layer) 7 including the composition containing the particles and the resin component, The base material 8 or the separator 9 may be laminated only on one side in the thickness direction and the sealing sheet 8 (or the separator 9) may be laminated on both sides of the substrate 8 or the separator 9 7) (that is, a single layer of only the sealing sheet 7 including the composition containing the particles and the resin component).

Next, another embodiment of the sheet producing apparatus of the present invention will be described with reference to Figs. 9 to 11. Fig. In each of the subsequent drawings, the same reference numerals are given to the members corresponding to the above-mentioned respective parts, and detailed description thereof will be omitted.

In the embodiment of Fig. 1, the kneader 2 is disposed so as to extend in the left-right direction on the left side of the sheet manufacturing apparatus 1. However, as shown in Fig. 9, 1 in the front and rear direction.

In the embodiment of Fig. 9, the cylinder 70 is formed so as to extend in the front-rear direction as shown in Fig.

The introduction port 14 is formed so as to penetrate the upper end wall of the cylinder 70 and to open upward.

As shown in Figs. 9 and 10 (broken lines in Fig. 10), the discharge port 15 is formed so as to pass through the front end right wall of the cylinder 70 and to open in the right direction, And is arranged so as to be continuous with the pipe (17).

10, the kneading shaft 13 includes a driving shaft 8a, a plurality of (four) feed screw portions 9a, a plurality of (three) reverse screw portions 10a, A plurality of (three) paddle portions 11a, and one pipe portion 12a.

More specifically, in the kneading shaft 13 of the embodiment shown in Fig. 3, the kneading shaft 13 of the embodiment of Fig. 9 is provided with two reverse screw portions 10a, one for each of the two reverse screw portions 10a And the reverse screw portion 10a is disposed adjacent to the pipe portion 12a on the front side of the pipe portion 12a as shown in Figs.

That is, a plurality of (three) reverse screw portions 10a are formed by the first reverse portion 30a, the second reverse portion 31a and the third reverse portion 32a, And the third reverse portion 32a is disposed at the front end of the discharge port 15 side.

The third reverse portion 32a has the longest axial length of the drive shaft 8a as compared with the other reverse portion. The axial length of the drive shaft 8a is approximately 1/4 of the first feed portion 23a.

The pipe section 12a is formed between the fourth feed section 26a and the third reverse section 32a and is arranged so as to include the discharge port 15 when projected in the left and right direction.

The kneader 2 shown in Fig. 10 is connected to the connecting pipe 17 (see Fig. 9) so that the axial direction of the kneading shaft 13 and the axial direction of the feed screw 22 become parallel (Not shown in the drawings).

This also makes it possible to suppress generation of pores in the kneaded product (Y) as in the embodiment of Fig.

Further, in the present invention, the sheet includes the concept of tape or film.

The present invention can combine a plurality of the above-described embodiments.

Example

The numerical values of the examples and comparative examples shown below can be replaced with the numerical values described in the above embodiments (that is, the upper limit value or the lower limit value).

Example 1

338.3 parts by mass of an epoxy resin, 357.8 parts by mass of a curing agent, 8800 parts by mass of a filler (particle), 303.5 parts by mass of an elastomer and 178.5 parts by mass of a flame retardant were mixed and stirred to prepare a semi-solid mixture (composition (X)). The mixing ratio of the particles was 78.8% by volume.

Separately, a sheet manufacturing apparatus 1 having the apparatus configuration of Fig. 1 was prepared. Specific dimensions and conditions are as follows.

Extruder (2): extrusion rate 42 mL / min, temperature 120 DEG C

Feeder 3: The feed screw 22 is a twin-screw screw, having a length (WO) of 500 mm in the direction of the axis of rotation, a feed rate of 42 mL / min, a screw rotation of 5 rpm,

The gear structure 4 has a saw tooth length of 8.8 mm and an inclination angle of 17.7 degrees with respect to the rotational axis direction A1 and a pitch interval of 18.84 mm and a length W2 of the gear 32 in the rotational axis direction A1 A width W0 of the first housing 21 of 500.2 mm, a gear diameter (outer diameter) of 42 mm, a gear rotation number of 0.15 rpm, a temperature of 90 DEG C

Sheet adjustment section 5: distance L1 in the front-rear direction of gap 50: 200 占 퐉, coating speed 0.05 (m / min), temperature 80 占 폚

Winding section 6: Diameter (outer diameter) of winding roll 53: 200 mm

Substrate (8): PET, thickness 38 탆

Separator 9: PET, 38 탆 thick

Subsequently, under the above conditions, the sheet manufacturing apparatus 1 is operated to wind (wind) the sealing sheet 7 having a thickness of 200 mu m in the B-stage in the winding unit 6, (60).

The compounded components are described in detail below.

Epoxy resin: Bisphenol F type epoxy resin, trade name "YSLV-80XY", manufactured by Shinnitsu Tetsu Chemical Co., Ltd., epoxy equivalent weight 200 g / eq., Softening point 80 ° C.

· Hardener: phenol · Aralkyl resin, trade name "MEH7851SS", manufactured by Meiwa Kasei Co., Ltd., hydroxyl equivalent: 203 g / eq., Softening point: 67 ° C.

Filler: 100 parts by mass of particles, an inorganic filler (fused silica) (FB-9454, spherical shape, density 2.2 g / cm ³ , manufactured by Denki Kagaku K.K.), 100 parts by mass of a silane coupling agent (KBM403, Shinetsu Chemical Co., Manufactured by Tatsuo Co., Ltd.).

Flame retardant: phosphazene derivative, product name "Ravitol FP-100", manufactured by Fushimi Seiyakusho Co., Ltd.

· Elastomer: styrene · isobutylene block copolymer, trade name "SIBSTAR072T", manufactured by Kaneka Corporation

Examples 2 to 16

A roll-like sheet (60) was obtained in the same manner as in Example 1 except that the setting conditions of the sheet adjusting section were changed to the conditions described in Table 1.

Example 17

9 was prepared and used instead of the sheet manufacturing apparatus 1 having the apparatus configuration shown in Fig. 1 to prepare a sheet-forming apparatus 1 having the apparatus configuration shown in Fig. To obtain a shape sheet 60.

Comparative Example 1

(Roll coating + laminator)

Each component (particle and resin component) and MEK were mixed and stirred in the same formulation as in Example 1 to prepare a liquid varnish (composition, solid concentration 50 mass%).

Separately, a roll coating machine was prepared.

Subsequently, the varnish was applied to the sealing sheet using a roll coating machine.

Specifically, on the PET film subjected to the releasing treatment, the application gap was adjusted so that the thickness of the sealing sheet after solvent drying was adjusted to 50 占 퐉 by using a roll coating construction apparatus, and coating was carried out at a conveying speed of 1.0 m / min. The drying furnace was set at a drying temperature of 120 캜 and a drying time of 3 minutes.

A sheet having a thickness of 50 占 퐉 obtained was formed into a sealing sheet having a thickness of 100 占 퐉 at a temperature of 90 占 폚 and a conveying speed of 1.0 m / min using a laminator.

Thereafter, five sheets of sealing sheets having a thickness of 100 mu m were prepared, and they were bonded (laminated) under the same conditions to obtain a laminated sealing sheet having a thickness of 500 mu m.

In this Comparative Example 1, in order to obtain a laminated sealing sheet having a desired thickness (500 μm) in which the mixing ratio of the particles was high (78.8% by volume), a plurality of sealing sheets (50 μm and 100 μm) It was necessary to carry out the lamination work.

(evaluation)

·shear

The shear stress was calculated as follows.

The piston speed was set at 0.5, 1.0, 2.0, 5.0, 7.0, and 10.0 mm / min with a capillary length of 10 mm and a capillary diameter of 1.0 mm using a measuring instrument name CAPILOGRAPH · E3B (manufactured by Toyo Seiki Seisakusho) Shear stress was calculated from the load at the time when the shear stress was applied and the shear rate was calculated from the capillary diameter and the piston speed to create a graph of shear rate-shear stress. The curves obtained in the graph were edited, and shear rates calculated from the GAP (gap) and the application speed at the time of evaluation were applied to the formulas, and shear stresses at respective shear rates were calculated.

· Shear rate

Shear rate was calculated as follows.

Shear rate (1 / s) = GAP (mm) / coating speed (mm / s)

· Application workability

The area where the applied area was about 100% was rated as?, The area with 99 to 50% as?, And the area with less than 50% as x with respect to the coating width of 500 mm. The results are shown in Table 1.

· Roll shape

The case where the sheet was roll-shaped was evaluated as & cir & and the case where the sheet was cracked or the sheet was broken was evaluated as " x ". The results are shown in Table 1.

Sealing tests of Examples 1 and 17

The sealing sheet 7 was taken out from each of the particle-containing roll-shaped sheets 60 of Example 1 and Example 17 and the FR-4 substrate (Flame) on which such a sealing sheet 7 was mounted, Retardant Type 4, size 150 mm x 150 mm x 0.5 mm) were placed so as to cover and embed a flip-chip type device.

Thereafter, they were heated at 150 캜 for 60 minutes to completely harden the sealing sheet 7. Thus, the flip-chip type device was covered with the sealing sheet 7.

Sealing test of Comparative Example 1

The laminated sealing sheet of Comparative Example 1 was placed on a FR-4 substrate (Flame Retardant Type 4, size: 150 mm x 150 mm x 0.5 mm) for mounting a flip-chip type device to be sealed.

Thereafter, they were heated at 150 캜 for 60 minutes to completely harden the sealing sheet 7. Thus, the flip-chip type device was covered with the laminated sealing sheet.

· Measurement of tensile modulus

The B-stage sealing sheet was taken out from the particle-containing roll-shaped sheet of Example 1 and Example 17, and the tensile elastic modulus at 25 캜 was measured by the DMA method (the storage elastic modulus value at a heating rate of 1 Hz at a heating rate of 10 캜 / ). ≪ / RTI > Subsequently, such a B-stage sealing sheet was heated at 150 占 폚 for 60 minutes to give a fully-cured (C-staged) sealing sheet a tensile modulus at 25 占 폚 by the DMA method (heating rate at 1 Hz, Min.). ≪ tb > < TABLE >

As a result, the sealing sheet of any of the B-stage of Example 1, Example 17, and Comparative Example 1 was 3 GPa and the sealing sheet of the C-stage was 4 GPa.

The above-mentioned invention is provided as an example of the present invention, but this is merely an example, and should not be construed as limiting. Variations of the invention that are apparent to those skilled in the art are within the scope of the following claims.

[Industrial applicability]

The roll-shaped sheet can be used in various applications such as a semiconductor device, a hard disk, an LED device (television, illumination, display, etc.), an EL device (organic EL display, organic EL light), a capacitor, (SAW) filter, various sensor devices, and the like.

Claims (9)

Particles and a resin component,
The mixing ratio of the particles exceeds 30% by volume,
Shaped sheet is wound in a roll shape. The method according to claim 1,
A deformation conveying step of conveying the composition containing the particles and the resin component while deforming the deformation of the composition in the rotation axial direction of the gear using a gear structure having a pair of gears; Passing through the gap between the moving support body and a doctor disposed so as to be spaced from the moving support body while being supported and supported by the moving support body, . 3. The method of claim 2,
Wherein the composition passed through the gap passing step has a shearing stress of not more than 5.0 x 10 < ⁴ > Pa at a temperature range of 50 to 250 deg. 4. The method according to any one of claims 1 to 3,
And a width of at least 200 mm. The method according to claim 1,
The roll-shaped sheet is a particle-containing roll-shaped sheet,
Wherein the resin component comprises an epoxy resin composition and / or a phenolic resin. 6. The method of claim 5,
And a width of at least 200 mm. 6. The method of claim 5,
Wherein the maximum length average value of the particles is 0.1 占 퐉 or more and 1000 占 퐉 or less. 6. The method of claim 5,
And a tensile elastic modulus at 25 DEG C of not less than 0.1 GPa and not more than 20 GPa. 6. The method of claim 5,
Wherein the thickness of the sealing sheet is 100 占 퐉 or more.

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