TW201348425A - Rolled sheet - Google Patents

Abstract

This rolled sheet (60) contains particles and a resin component, the mixed proportion of the particles exceeding 30 vol%. The rolled sheet (60) is produced by a deformation and conveyance step in which a composition containing particles and a resin component is conveyed while being deformed in the direction of the axis of rotation of a pair of gears (32) using a gear structure (4) provided with the gears (32), and, after the deformation and conveyance step, a gap passage step in which a sheet (7) is passed through a gap between a moving roller (51) and a protruding section (63) while being supported and conveyed by the moving roller (51).

Description

Rolled sheet

The present invention relates to a roll-shaped sheet. In particular, the present invention relates to a roll-shaped sheet containing particles and a resin component.

Previously, the industry has studied various methods for producing sheets from compositions containing particles and resin components.

For example, a method is proposed in which a boron nitride particle is mixed with a resin component dispersed therein to prepare a composition, and a press sheet is produced by hot pressing the composition on a flat plate, and then laminated to obtain a thermally conductive sheet. (for example, refer to Patent Document 1 below).

[Previous Technical Literature] [Patent Literature]

[Patent Document 1] Japanese Patent Laid-Open Publication No. 2012-039060

However, since the method described in Patent Document 1 is a batch production method of pressing the composition each time, the sheet produced is a flat sheet having one side of a short side. When such a short-side sheet is downloaded and stored in the state of a flat sheet, a large storage space is required, and it is also disadvantageous in terms of portability.

An object of the present invention is to provide a roll-shaped sheet which contains particles at a high blending ratio and is excellent in storage property and portability.

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

Moreover, the sheet of the present invention is preferably produced by a deformation transport step of using a gear structure including a pair of gears so that the composition containing the particles and the resin component is in the direction of the rotation axis of the gear And a gap passing step, after the deformation transporting step, while supporting and transporting the composition by the moving support, passing the moving support and providing a gap with respect to the moving support The above gap of the doctor is arranged in the opposite direction.

Further, in the sheet of the present invention, the composition which passes through the gap passing step preferably has a shear stress of 5.0 × 10 ⁴ Pa or less in a temperature range of 50 to 250 °C.

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

The roll-shaped sheet of the present invention is characterized in that it is a sealing sheet which is wound into a roll shape, and the sealing sheet contains a particle roll-shaped sheet containing particles and a resin component, and the blending ratio of the above particles exceeds 30 5% by volume, the resin component contains an epoxy resin composition and/or a phenol resin.

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

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

Further, the roll-shaped sheet of the present invention preferably has a tensile modulus of elasticity of from 0.1 GPa to 20 GPa at 25 °C.

Moreover, it is preferable that the roll-shaped sheet of the present invention has a thickness of the sealing sheet of 100 μm or more.

The roll-shaped sheet of the present invention contains particles at a high blending ratio and is formed into a roll shape. Therefore, the specific physical properties of the particles can be fully utilized, and the storage space can be reduced. Excellent handling.

Further, the roll-shaped sheet of the present invention which is a particle-containing roll-shaped sheet is obtained by winding a sealing sheet into a roll shape and containing particles at a high blending ratio. Therefore, the production can be efficiently performed, and the specific physical properties of the particles can be sufficiently exhibited, and the storage space can be reduced, and the handling property is excellent.

1‧‧‧Sheet manufacturing equipment

2‧‧‧Machine

3‧‧‧Supply Department

4‧‧‧ Gear Construction

5‧‧‧Sheet Adjustment Department

6‧‧‧Winding Department

6a‧‧‧Moltening and mixing department

7‧‧‧Sheet

7a‧‧‧ Ventilation Department

8‧‧‧Substrate

8a‧‧‧Drive shaft

9‧‧‧Parts

9a‧‧‧feed screw

10‧‧‧Laminated sheets

10a‧‧‧Reverse screw section

11a‧‧‧Mixed Department

12a‧‧‧Pipe Department

13‧‧‧Mixed shaft

14‧‧‧Import

15‧‧‧Spray outlet

17‧‧‧Connected tube

18‧‧‧Supply entrance

19‧‧‧1st Storage Department

20‧‧‧ leaves

20a‧‧‧ spiral strip

21‧‧‧1st casing

21a‧‧‧ mixed leaves

22‧‧‧Supply screw

23‧‧‧1st screw

23a‧‧‧1st feeding department

24‧‧‧2nd screw

24a‧‧‧2nd feeding department

25‧‧‧1st axis

25a‧‧‧3rd feeding department

26‧‧‧2nd axis

26a‧‧‧4th feeding department

27‧‧‧First Storage Department

27a‧‧‧1st mixing department

28‧‧‧Second Storage Department

28a‧‧‧2nd mixing department

29‧‧‧ Rear

29a‧‧‧3rd mixing department

30‧‧‧ front

30a‧‧‧1st reversal

31‧‧‧2nd casing

31a‧‧‧2nd Reversal Department

32‧‧‧ Gears

32a‧‧‧3rd Reversal Department

33‧‧‧1st gear

34‧‧‧2nd gear

35‧‧‧ helical teeth

36‧‧‧1st helical tooth

37‧‧‧2nd helical tooth

38‧‧‧3rd helical tooth

39‧‧‧4th helical tooth

40‧‧‧2nd Storage Department

41‧‧‧ Surface

42‧‧‧ concave

43‧‧ ‧ convex

44‧‧‧Spout

45‧‧‧Spray wall

46‧‧‧ Gear spout

47‧‧‧lower side wall

48‧‧‧ upper side wall

50‧‧‧ gap

51‧‧‧Support roll

52‧‧‧ Tension roller

53‧‧‧Winding roller

54a‧‧‧1st Ventilation Department

55a‧‧‧2nd Ventilation Department

56‧‧‧Substrate feed roller

57‧‧‧Parts Laminating Roller

58‧‧‧Rotating roller

59‧‧‧Parts delivery roller

60‧‧‧Rolled sheet

61‧‧‧ lower

62‧‧‧ upper

63‧‧‧Protruding

70‧‧‧ material cylinder

X‧‧‧ composition

Y‧‧‧Machine

BRIEF DESCRIPTION OF THE DRAWINGS Fig. 1 is a partially cutaway plan view showing an embodiment of a sheet manufacturing apparatus for producing a roll-shaped sheet of the present invention.

Figure 2 is a cross-sectional view taken along line A-A of Figure 1.

Fig. 3 is a schematic block diagram showing a kneading machine used in the sheet manufacturing apparatus shown in Fig. 1;

Fig. 4 is a plan sectional view showing the discharge port side of the kneading machine shown in Fig. 3.

Fig. 5 is a plan sectional view showing a supply unit, a gear structure, and a sheet adjusting unit used in the sheet manufacturing apparatus shown in Fig. 1 .

Fig. 6 is a side cross-sectional view showing the supply unit, the gear structure, and the sheet adjusting unit shown in Fig. 5, and showing a cross-sectional view taken along line B-B of Fig. 5.

Fig. 7 is an exploded perspective view showing a pair of gears of the gear structure shown in Fig. 5;

Figure 8 is a side cross-sectional view showing the engagement of a pair of gears shown in Figure 7, (a) shows a state in which the downstream end portion of the convex surface of the helical tooth of the first gear meshes with the downstream end portion of the concave surface of the helical tooth of the second gear, (b) shows a state in which the middle portion of the convex surface of the helical tooth of the first gear meshes with the middle portion of the concave surface of the helical tooth of the second gear, (c) shows a state in which the upstream end portion of the convex surface of the helical tooth of the first gear meshes with the upstream end portion of the concave surface of the helical tooth of the second gear.

Fig. 9 is a partially cutaway plan view showing another embodiment of the sheet manufacturing apparatus of the present invention.

Fig. 10 is a schematic block diagram showing a kneading machine used in the sheet manufacturing apparatus shown in Fig. 9.

Fig. 11 is a plan sectional view showing the discharge port side of the kneading machine shown in Fig. 10.

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

The particles include powders, granules, powders, and powders, and examples of the material for forming the particles include inorganic materials and organic materials. Preferably, an inorganic material is listed.

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

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

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

Examples of the oxide include cerium oxide (including cerium oxide, spherical molten cerium oxide powder, crushed molten cerium oxide powder, etc.), alumina (alumina, Al ₂ O ₃ ), and magnesium oxide (magnesia). Titanium oxide, cerium oxide, iron oxide, cerium oxide, and the like. Further, examples of the oxide include indium tin oxide and antimony tin oxide doped with a metal ion. Preferably, cerium oxide is listed.

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, etc.).

As the clay mineral, for example, montmorillonite, magnesia montmorillonite, iron montmorillonite, iron-magnesium montmorillonite, beidelite, aluminum-aluminum bentonite, and smectite may be mentioned. (nontronite), aluminum smectite, saponite, aluminosilicate, hectorite, sauconite, stevensite, and the like.

Examples of the carbon-based material include carbon black, graphite, diamond, fullerene, carbon nanotube, nano carbon fiber, nano angle, carbon microcoil, and nanocoil. Preferably, carbon black is listed.

Preferably, an oxide or a carbon-based material is listed.

Further, examples of the material include materials having specific physical properties, and heat conductive materials (for example, thermally conductive materials selected from the group consisting of carbides, nitrides, oxides, and metals, specifically BN, AlN, and Al ₂ O). _3, etc., a conductive material (for example, a conductive material selected from a metal or a carbon-based material, specifically Cu or the like), an insulating material (for example, a nitride, an oxide, or the like, specifically BN, cerium oxide, etc.), magnetic Materials (for example, oxides, metals, specifically ferrite (soft magnetic ferrite, hard magnetic), iron, etc.). Materials having specific physical properties may also be repeated with the materials exemplified above.

Furthermore, the thermal conductivity of the particles is, for example, 10 W/m. K or more, preferably 30 W/m. K or more, and, for example, also 2000W/m. Below K.

Further, the 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.

Moreover, the volume resistance of the particles is 1 × 10 ¹⁰ Ω. Above cm, preferably 1 x 10 ¹² Ω. Above cm, again, for example, 1 × 10 ²⁰ Ω. Below cm.

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

Further, the particles may be surface-treated by, for example, a decane coupling agent or the like.

Further, the shape of the particles is not particularly limited, and examples thereof include a plate shape, a scaly shape, a particle shape (indefinite shape), and a spherical shape.

The average value of the maximum length of the particles (the average particle diameter in the case of a spherical shape) is, for example, 0.1 μm or more, preferably 1 μm or more, and is also, for example, 1000 μm or less, preferably 100 μm or less. Further, the average particle diameter is determined, for example, by a d50 value.

When the average value of the maximum length of the particles is equal to or less than the above upper limit, the sealing sheet manufacturing apparatus can be processed flat. On the other hand, if the average length of the particles is the average When the thickness is more than the above lower limit, it is possible to suppress the increase in viscosity during the production of the sheet, and to form the sheet stably and in a wide range.

Further, when the particles have a shape other than the spherical shape, the aspect ratio thereof is, for example, 2 or more, preferably 10 or more, and is also, for example, 10,000 or less, preferably 5,000 or less.

Further, 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 is also, for example, 20 g/cm ³ or less, preferably 10 g/cm 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 the particles are dispersed, and the insulating component is contained, and examples thereof include a resin component such as a thermosetting resin component and 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 polyoxyxylene resin, and the like. A thermosetting urethane resin or the like.

Examples of the thermoplastic resin component include acrylic resins, polyolefins (for example, polyethylene, polypropylene, and ethylene-propylene copolymers), polyvinyl acetate, ethylene-vinyl acetate copolymer, polyvinyl chloride, and poly. Styrene, polyacrylonitrile, polyamide, polycarbonate, polyacetal, polyethylene terephthalate, polyphenylene ether, polyphenylene sulfide, polyfluorene, polyether oxime, polyether ether ketone, poly Aryl sulfonium, thermoplastic polyimine, thermoplastic urethane resin, polyamine bismaleimide, polyamidimide, polyetherimine, bismaleimide Resin, polymethylpentene, fluorinated resin, liquid crystal polymer, olefin-vinyl alcohol copolymer, ionic polymer, polyarylate, acrylonitrile-ethylene-styrene copolymer, acrylonitrile-butadiene-styrene Copolymer, acrylonitrile-styrene copolymer, polystyrene-polyisobutylene copolymer, and the like.

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

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

The epoxy resin is in any form of a liquid state, a semi-solid shape, and a solid shape at normal temperature.

Specifically, examples of the epoxy resin include, for example, a bisphenol type epoxy resin (for example, Bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, hydrogenated bisphenol A type epoxy resin, dimer acid modified bisphenol type epoxy resin, etc.), novolak type Epoxy resin, naphthalene type epoxy resin, bismuth type epoxy resin (for example, bisaryl fluorene type epoxy resin, etc.), triphenylmethane type epoxy resin (for example, trishydroxyphenylmethane type epoxy resin, etc.) An aromatic epoxy resin; for example, an epoxy resin containing a nitrogen ring such as a triglycidyl isocyanurate or an ethyl carbendazole epoxy resin; for example, an aliphatic epoxy resin or an alicyclic epoxy resin; A glycidyl ether type epoxy resin, a glycidylamine type epoxy resin, or 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. or more, and is also, for example, 1000 g/eq. or less, preferably 700 g/eq. or less. Further, when the epoxy resin is in a normal temperature solid state, the softening point is, for example, 20 to 90 °C.

The blending ratio of the resin component (especially the epoxy resin) is, for example, 1 part by mass or more, preferably 2 parts by mass or more, more preferably 3.5 parts by mass or more, and further preferably 50 parts by mass, based on 100 parts by mass of the particles. The amount is preferably 40 parts by mass or less, more preferably 30 parts by mass or less.

The roll-shaped sheet preferably contains a hardener together with the epoxy resin.

The curing agent is a latent curing agent (epoxy resin curing agent) which can cure the epoxy resin by heating, and examples thereof include a phenol compound, an amine compound, an acid anhydride compound, a guanamine compound, an anthraquinone compound, an imidazoline compound, and the like. . Further, in addition to the above, a urea compound, a polysulfide compound, or the like may be mentioned.

The phenol compound contains a phenol resin, and examples thereof include a novolac type phenol resin obtained by condensing phenol with formaldehyde under an acidic catalyst, for example, a combination of phenol and dimethoxy-p-xylene or bis(methoxymethyl). A phenol-aralkyl resin synthesized by benzene, for example, a biphenyl-aralkyl resin, for example, a dicyclopentadiene type phenol resin, for example, a cresol novolak resin, for example, a resol resin. Preference is given to phenol-aralkyl resins.

The hydroxyl group equivalent of the phenol compound is, for example, 80 g/eq. or more, preferably 90 g/eq. or more, more preferably 100 g/eq. or more, and further, for example, 2,000 g/eq. or less, preferably 1,000 g/eq. The following is further preferably 500 g/eq. or less.

The amine compound may, for example, be a polyamine such as ethylenediamine, propylenediamine, diethylenetriamine or triethylenetetramine or an amine adduct thereof; for example, m-phenylenediamine or diaminodiphenyl Methane, diaminodiphenyl hydrazine, and the like.

Examples of the acid anhydride compound include phthalic anhydride, maleic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, 4-methyl-hexahydrophthalic anhydride, and methylation resistance. Anic anhydride, pyromellitic anhydride, dodecenyl succinic anhydride, dichlorosuccinic anhydride, diphenyl ketone tetracarboxylic anhydride, chlorinic anhydride, and the like.

Examples of the guanamine compound include dicyandiamide and polyamidamine.

Examples of the ruthenium compound include diammonium adipate and the like.

Examples of the imidazoline compound include methyl imidazoline, 2-ethyl-4-methylimidazoline, ethyl imidazoline, isopropyl imidazoline, 2,4-dimethylimidazoline, and phenylimidazole. Porphyrin, undecyl imidazoline, heptadecyl imidazoline, 2-phenyl-4-methylimidazoline and the like.

Preference is given to phenolic compounds.

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

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

The blending ratio of the curing agent is, for example, 1 part by mass or more, preferably 5 parts by mass or more, more preferably 10 parts by mass or more, and further preferably 200 parts by mass or less, more preferably 100 parts by mass or less, based on 100 parts by mass of the epoxy resin. It is 150 parts by mass or less. Further, when the curing agent contains a phenol compound, the hydroxyl group of the phenol compound is, for example, 0.5 mol or more, preferably 0.8 mol or more, relative to the epoxy group of the epoxy resin, and is, for example, 2.0. The adjustment is performed in the following manner, preferably below 1.2 m.

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

The hardening accelerator is a hardening catalyst, and examples thereof include 2-phenylimidazole, 2-methylimidazole, 2-ethyl-4-methylimidazole, and 2-phenyl-4-methyl-5-hydroxymethyl group. An imidazole compound such as imidazole; a tertiary amine compound such as triethylenediamine or tris-2,4,6-dimethylaminomethylphenol; for example, triphenylphosphine, tetraphenylphosphonium tetraphenylborate, o, a phosphorus compound such as tetra-n-butylphosphonium diethyldithiophosphate; for example, a quaternary ammonium salt compound; for example, an organometallic salt compound; for example, such a derivative or the like.

Preferably, an imidazole compound is listed.

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

The blending ratio of the curing accelerator is, for example, 0.1 parts by mass or more, preferably 0.2 parts by mass or more, and is also, for example, 10 parts by mass or less, preferably 5 parts by mass or less, based on 100 parts by mass of the epoxy resin.

The above-mentioned curing agent and/or curing accelerator may be used as a solvent solution and/or a solvent dispersion which is dissolved and/or dispersed by 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 decylamine such as N,N-dimethylformamide. Further, examples of the solvent include water; for example, an aqueous solvent such as an alcohol such as methanol, ethanol, propanol or isopropanol.

The acrylic resin contains an acrylic rubber, and is specifically obtained by polymerization of a monomer containing an alkyl (meth)acrylate.

Examples of the alkyl (meth)acrylate-based alkyl methacrylate and/or alkyl acrylate include methyl (meth)acrylate, ethyl (meth)acrylate, and butyl (meth)acrylate. , (meth) hexyl acrylate, 2-ethylhexyl (meth) acrylate, decyl (meth) acrylate, isodecyl (meth) acrylate, decyl (meth) acrylate, (methyl) Isodecyl acrylate, undecyl (meth) acrylate, dodecyl (meth) acrylate, tridecyl (meth) acrylate, tetradecyl (meth) acrylate, ( The alkyl moiety such as octadecyl methyl methacrylate or octadecyl (meth) acrylate is a linear or branched chain having a carbon number of 30 or less (A The alkyl acrylate is preferably a linear alkyl (meth) acrylate having an alkyl group of 1 to 18 carbon atoms.

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

The blending ratio of the alkyl (meth)acrylate is, for example, 50% by mass or more, preferably 75% by mass or more, and is, for example, 99% by mass or less based on the monomer.

The monomer may also contain a copolymerizable monomer polymerizable with an alkyl (meth)acrylate.

The copolymerizable monomer contains a vinyl group, and examples thereof include a cyano group-containing vinyl monomer such as (meth)acrylonitrile; and a glycidyl group-containing vinyl monomer such as glycidyl (meth)acrylate (including An epoxy group-based vinyl monomer); for example, an aromatic vinyl monomer such as styrene.

The blending ratio of the copolymerizable monomer is, for example, 50% by mass or less, preferably 25% by mass or less, and is, for example, 1% by mass or more based on 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 obtained acrylic resin is introduced into the end of the main chain or in the middle thereof. A functional group-modified acrylic resin having a functional group such as an epoxy group and/or a cyano group (specifically, a cyano-modified acrylic resin, an epoxy-modified acrylic resin, or a cyano-epoxy-modified acrylic resin).

The resin component (in the case where the thermosetting resin component is contained, the thermosetting resin component is a resin component in the A-stage state) has a melt viscosity at 80 ° C of, for example, 10 to 10000 mPa. s, preferably 50~10000mPa. s.

Further, the softening temperature (ring and ball method) of the resin component is, for example, 80 ° C or lower, preferably 70 ° C or lower, and is also, for example, 20 ° C or higher, preferably 35 ° C or higher.

These resin components may be used singly or in combination.

Further, a thermosetting resin component and a thermoplastic resin component may be used in combination.

Further, it is also possible to contain an elastomer, a flame retardant, and a dispersion in an appropriate ratio among the resin components. A known additive such as a agent, an adhesion-imparting agent, a decane coupling agent, a fluorine-based surfactant, a plasticizer, an anti-aging agent, and a coloring agent. It is preferred to contain an elastomer and/or a flame retardant.

Examples of the elastomer include urethane rubber, polyoxyethylene rubber, vinyl alkyl ether rubber, polyvinyl alcohol rubber, polyvinylpyrrolidone rubber, polypropylene polyamide rubber, cellulose rubber, and natural. Rubber, butadiene rubber, chloroprene rubber, styrene-butadiene rubber (SBR), acrylonitrile-butadiene rubber (NBR), isoprene rubber, polyisobutylene rubber, butyl rubber, benzene Ethylene-ethylene-butadiene-styrene rubber, styrene-isoprene-styrene rubber, styrene-isobutylene rubber, and the like. A styrene-isobutylene rubber is preferred.

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

Further, specific examples of the styrene-isobutylene block copolymer include styrene-isobutylene-styrene block copolymer (SIBS).

The content ratio of the elastomer is, for example, 1 part by mass or more, preferably 2 parts by mass or more, and is also, for example, 100 parts by mass or less, preferably 50 parts by mass or less, more preferably 10% by mass, based on 100 parts by mass of the particles. The following.

Examples of the flame retardant include a phosphazene derivative and the like. The content ratio of the flame retardant is, for example, 0.1 part by mass or more, preferably 1 part by mass or more, more preferably 2 parts by mass or more, and further preferably 100 parts by mass or less, preferably 100 parts by mass or less, per 100 parts by mass of the particles. 10 parts by mass or less, more preferably 5 parts by mass or less.

Examples of the flame retardant include a phosphazene derivative and the like. The flame retardant can be formulated in an appropriate ratio.

The blending ratio of the particles and the resin component is adjusted to a desired range in the following roll-shaped sheet.

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

In Fig. 1, the right side of the paper is set to "right side", the left side of the paper is set to "left side", the lower side of the paper is set to "front side", and the upper side of the paper is set to "back side", indicated by a directional arrow, and the paper surface is closer. The front side is set to "upper side" and the back side of the paper is set to "lower side". Further, in Fig. 1, the right side is on the side of the rotation axis direction of the pair of gears (described below), the left side is on the other side in the direction of the rotation axis, the front side is in the direction of intersection (described below), and the rear side is in the direction of intersection side. Further, the orientation of the drawings of Fig. 2 and Fig. 2 is based on the orientation illustrated in Fig. 1.

In FIG. 1, the sheet manufacturing apparatus 1 is configured to manufacture the roll-shaped sheet 60 from the composition X containing particles and a resin component, and is formed, for example, in a substantially L shape in plan view. The sheet manufacturing apparatus 1 includes a kneading machine 2, a supply unit 3, a gear structure 4, a sheet adjusting unit 5, and a winding unit 6. The kneading machine 2, the supply unit 3, the gear structure 4, the sheet adjusting unit 5, and the winding unit 6 are arranged in a line in the sheet manufacturing apparatus 1 so as to have a substantially L shape in plan view. In other words, the sheet manufacturing apparatus 1 is configured to convey the composition X or the sheet 7 (see FIG. 2) in a substantially L shape in plan view.

The kneading machine 2 is disposed on the left side of the sheet manufacturing apparatus 1.

As shown in FIGS. 3 and 4, the kneading machine 2 is a continuous two-axis kneading machine, and includes a cylinder 70 and two kneading shafts 13.

The cylinder 70 is formed in a substantially elliptical cylindrical shape extending in the left-right direction, and is provided on the left end side (one end side) thereof as shown in FIG. 2 as a composition for introducing the composition X containing the particles and the resin component into the cylinder 70. The inlet 14 of the lead-in portion of the inside. Further, a discharge port 15 as a discharge portion for discharging the kneaded material Y kneaded with the composition X to the outside of the cylinder 70 is provided on the right end side (the other end side).

As shown in FIG. 3, the introduction port 14 is formed so as to penetrate the upper wall of the left end portion of the cylinder 70 and open upward.

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

Examples of the cross-sectional shape of the discharge port 15 include a rectangular shape, an elliptical shape, and a circular shape. Preferably, an elliptical shape or a circular shape is used.

Further, the cross-sectional area of the discharge port 15 is, for example, 15% with respect to the cross-sectional area of the cylinder 70. The above is preferably 25% or more, and is also, for example, 50% or less, preferably 45% or less.

Further, a melt kneading portion 6a for melting and kneading the composition X is formed between the introduction port 14 and the discharge port 15 in the cylinder 70.

The melt kneading portion 6a includes a plurality of (two) vent portions 7a for discharging the gas in the melt kneading portion 6a at the middle portion in the axial direction.

Each of the vent portions 7a is formed to penetrate the upper wall of the cylinder 70. In other words, each of the ventilating portion 7a and the inlet port 14 is formed in parallel with each other in the axial direction of the kneading shaft 13.

Moreover, each ventilation part 7a is normally closed, and it can open suitably as needed.

More specifically, the plurality of venting portions 7a include a first venting portion 54a (a venting portion 7a on the side of the introduction port 14) provided in the vicinity of the right side of the introduction port 14 in the left-right direction of the cylinder 70, and a discharge port 15 provided in the discharge port 15 The second ventilation portion 55a (the ventilation portion 7a on the discharge port 15 side) in the vicinity of the left side.

Further, the second ventilation portion 55a is disposed on the left side of the duct portion 12a (described later), is connected to a pump (not shown), and is sucked into the melt kneading portion 6a by the suction force of the pump (not shown). Gas.

Further, a heater (not shown) is provided in the melt kneading section 6a, and the melt kneading section 6a is appropriately temperature-controlled 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 rotating shaft in which the composition X is mixed and sheared, and the drive shaft 8a, the feed screw portion 9a, the reverse screw portion 10a, the kneading portion 11a as a kneading portion, and the low shear are integrally formed. Part of the pipe portion 12a.

Specifically, the kneading shaft 13 includes one drive shaft 8a, a plurality of (four) feed screw portions 9a, a plurality of (two) reverse screw portions 10a, a plurality of (three) mixing portions 11a, and One duct portion 12a.

Further, the feed screw portion 9a, the reverse screw portion 10a, the kneading portion 11a, and the duct portion 12a may be appropriately changed in the axial direction length or the number of installations as needed.

A plurality of (four) feed screw portions 9a are portions that convey the composition X to the discharge port 15, specifically, the first feed portion 23a, the second feed portion 24a, the third feed portion 25a, and the 4 feeding department 26a is formed, and these are arranged at intervals in the axial direction of the drive shaft 8a.

The first feeding portion 23a is disposed at the left end portion of the kneading shaft 13, and is disposed so as to overlap the projection surfaces when the introduction port 14 and the first ventilation portion 54a are projected in the radial direction of the drive shaft 8a. Further, the length of the drive shaft 8a of the first feed portion 23a in the axial direction is formed to be the longest compared to the other feed portions.

The fourth feeding portion 26a is disposed on the side closest to the discharge port 15 among the four feeding portions, and is disposed so as to overlap the projection surface when the second ventilation portion 55a is projected in the radial direction of the drive shaft 8a. . Further, the length of the drive shaft 8a of the fourth feed portion 26a in the axial direction is formed to be substantially 1/2 of the first feed portion 23a.

Further, the second feeding portion 24a and the third feeding portion 25a are disposed between the first feeding portion 23a and the fourth feeding portion 26a, and the length of the driving shaft 8a in the axial direction is formed as the first feeding portion 23a. About 1/10.

Further, as shown in Fig. 4, the feed screw portion 9a includes a spiral spiral strip 20a that protrudes from the outer peripheral surface of the drive shaft 8a.

Specifically, the spiral strip 20a is formed in a spiral shape in the same direction as the rotation direction (described later) of the drive shaft 8a. That is, the feed screw portion 9a includes a right spiral spiral strip 20a.

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

As shown in FIG. 3, a plurality of (two) reversing screw portions 10a are formed by the first reversing portion 30a and the second reversing portion 31a, and are arranged at intervals in the axial direction of the kneading shaft 13 on.

The first reversing portion 30a is located between the first feeding portion 23a and the second feeding portion 24a, and is disposed adjacent to the left side of the second feeding portion 24a.

Further, the second reversing portion 31a is located between the second feeding portion 24a and the third feeding portion 25a, and is disposed adjacent to the left side of the third feeding portion 25a.

Further, the longitudinal direction of the drive shaft 8a of the first reversing portion 30a and the second reversing portion 31a is long. It becomes roughly the same. The length in the axial direction is approximately 1/20 of the first feeding portion 23a.

Further, similarly to the feed screw portion 9a, the reverse screw portion 10a includes a spiral spiral strip 20a that protrudes from the outer peripheral surface of the drive shaft 8a as shown in Fig. 4 .

Further, the spiral strip 20a of the reverse screw portion 10a is formed in a spiral shape in a direction opposite to the spiral strip 20a of the feed screw portion 9a. That is, the inverting screw portion 10a includes the left spiral spiral strip 20a.

The pitch of the pitch of the spiral strip 20a in the inverting screw portion 10a is, for example, 0.6 cm or more, preferably 1.0 cm or more, and is also, for example, 1.5 cm or less.

As shown in FIG. 3, a plurality of (three) kneading sections 11a are portions in which the composition X is kneaded, specifically, the first kneading portion 27a, the second kneading portion 28a, and the third kneading portion 29a. These are formed and arranged at intervals in the axial direction of the kneading shaft 13.

The first kneading portion 27a is disposed between the first feeding portion 23a and the first reversing portion 30a.

The second kneading portion 28a is disposed between the second feeding portion 24a and the second reversing portion 31a.

The third kneading portion 29a is disposed between the third feeding portion 25a and the fourth feeding portion 26a.

Further, the axial lengths of the drive shafts 8a of the first kneading portion 27a, the second kneading portion 28a, and the third kneading portion 29a are substantially the same length, and are formed approximately 1/ of the first feeding portion 23a. 3.

Further, as shown in Fig. 4, the kneading portion 11a includes a plurality of mixed elliptical plates 21a which are substantially elliptical in shape so as to be aligned in the axial direction of the drive shaft 8a.

More specifically, the plurality of mixed blades 21a are arranged side by side in the axial direction of the drive shaft 8a so that the long diameters of the adjacent mixed blades 21a are shifted by 90 degrees from each other.

The duct 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 circumference.

Further, the duct portion 12a is disposed at the right end portion of the kneading shaft 13, and is disposed adjacent to the right side of the fourth feeding portion 26a. Further, the length of the drive shaft 8a of the duct portion 12a in the axial direction is formed to be substantially 1/2 of the first feed portion 23a.

That is, in the kneading shaft 13, as shown in Fig. 3, from the left end side to the right end side of the drive shaft 8a The first feeding unit 23a, the first mixing unit 27a, the first reversing unit 30a, the second feeding unit 24a, the second mixing unit 28a, the second reversing unit 31a, and the third feeding unit are disposed in this order. 25a, a third mixing portion 29a, a fourth feeding portion 26a, and a duct portion 12a.

In other words, in the kneading shaft 13, the unit including the feeding portion, the kneading portion, and the reversing portion is repeatedly disposed from the left end side to the right end side of the drive shaft 8a, and the feeding portion and the pipe portion are disposed in the unit on the right end side. Instead of the inversion section.

Further, as shown in FIG. 4, the two kneading shafts 13 are disposed inside the cylinder 70 in the axial direction thereof, and are arranged side by side in the radial direction thereof.

Further, the two kneading shafts 13 are disposed such that the respective portions (the feed screw portion 9a, the reverse screw portion 10a, and the kneading portion 11a) are driven to rotate without interfering with each other.

Further, both end portions of the drive shaft 8a of the kneading shaft 13 project outward in the axial direction of the cylinder 70. Among the protruding end portions, the right end side is not rotatably coupled to a drive source (not shown), and the left end side is rotatably supported by a support wall (not shown). That is, the kneading shaft 13 is rotationally driven around the axis of the drive shaft 8a by transmitting a driving force from a drive source (not shown) on the drive shaft 8a. Specifically, when viewed from the side of the introduction port 14 toward the discharge port 15 side, the kneading shaft 13 is rotated rightward in the axial direction of the drive shaft 8a.

Further, as shown in Fig. 4, the inner circumferential surface of the cylinder 70 is opposed to the feeding screw portion 9a, the reverse screw portion 10a (see Fig. 3), and the mixing portion 11a of the kneading shaft 13 at a minute interval. The manner is arranged in the diameter direction of the kneading shaft 13. On the other hand, the inner circumferential surface of the cylinder 70 and the duct portion 12a are arranged in the radial direction of the kneading shaft 13 at a large interval from the other portions.

As shown in Fig. 1, the supply unit 3 is provided on the right side of the kneading machine 2, and is formed to extend in the left-right direction. The supply unit 3 is connected to the kneading machine 2 via a connecting pipe 17.

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

As shown in FIGS. 5 and 6, the supply unit 3 includes a first sleeve 21 and a supply screw 22.

The first sleeve 21 is formed in a rectangular shape in a plan view extending in the left-right direction, and the front side is opened in the left-right direction. A supply portion inlet 18 is formed at a left end portion of the first sleeve 21, and a first reservoir portion 27 is formed at an end portion of the first sleeve 21. Moreover, the first housing portion 19 that houses the supply screw 22 described below is provided in the first sleeve 21. The first housing portion 19 includes a rear portion 29 and a front portion 30 that communicates with the front portion of the rear portion 29 . The rear portion 29 and the front portion 30 are formed in a substantially circular cross-sectional view, and are formed in the first sleeve 21 in the left-right direction.

The supply unit inlet 18 communicates with the first storage unit 19 (the rear portion 29 and the front portion 30).

The first storage portion 27 is formed in a substantially conical shape in a side cross section that is enlarged toward the front.

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

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

The second screw 24 is housed in the front portion 30 and has the same configuration and size as the first screw 23, and is configured to rotate in the same direction as the first screw 23 while being engaged with the first screw 23.

The length of the supply screw 22 (the first screw 23 and the second screw 24) in the direction of the rotation axis is set to be slightly shorter than the width W0 of the first sleeve 21 (not shown).

Further, the supply unit 3 is provided with a motor (not shown) connected to the supply screw 22 on the right side of the first sleeve 21.

The supply unit 3 is configured to supply the kneaded material Y from the rear to the gear so as to have a width W0 (that is, the width W0 of the first sleeve 21) in the discharge direction (left-right direction) of the kneading machine 2 Structure 4.

As shown in FIGS. 6 and 7, the gear structure 4 includes a second sleeve 31 and a pair of gears 32. Further, the gear structure 4 is also long in the length W2 of the rotation axis direction A1 of the pair of gears 32, The kneaded material Y supplied from the supply unit 3 is conveyed to the gear pump of the sheet adjusting unit 5.

As shown in FIG. 5 and FIG. 6 , the second sleeve 31 is continuously formed on the front side of the first sleeve 21 , and the rear and the front are opened in the left-right direction, and are formed in a substantially rectangular shape in plan view extending in the left-right direction. A second housing portion 40 that houses the pair of gears 32 is provided at an end portion of the second sleeve 31, and a gear discharge port 46 is formed at the distal end portion. Further, a second storage portion 28 and a discharge passage 44 that communicate with the second storage portion 40 and the gear discharge port 46 are formed.

The second housing portion 40 includes a lower portion 61 and a upper portion 62 that communicates with the first storage portion 27 and communicates with the upper portion 61 of the lower portion 61. Each of the lower portion 61 and the upper portion 62 is formed in a substantially circular cross-sectional view, and is formed in the second sleeve 31 in the left-right direction.

The gear discharge port 46 is defined by two discharge walls 45 which are formed at intervals in the vertical direction, and are formed to open toward the front. The discharge wall 45 is disposed at a front end portion of the second sleeve 31 and includes a lower side wall 47 and an upper side wall 48.

The lower side wall 47 is formed in a flat plate shape having a thick wall extending in the left-right direction and the up-and-down direction, and the front surface and the upper surface are formed in a flat shape.

The lower surface of the upper side wall 48 is formed in a flat shape. Further, the upper side wall 48 is formed in a substantially L-shaped side cross section, and the lower end portion of the lower portion is formed to protrude forward with respect to the upper front surface. In other words, in the upper side wall 48, the lower end portion of the lower portion is a protruding portion 63 of the blade which is a substantially rectangular shape as viewed in a side cross section. The protruding length of the protruding portion 63 (that is, the length in the front-rear direction) is, for example, 2 mm or more, and is also, for example, 150 mm or less and 50 mm or less. Further, the thickness of the protruding portion 63 (that is, the length in the vertical direction) is, for example, 2 mm or more, and is also, for example, 100 mm or less, preferably 50 mm or less. The front surface of the protruding portion 63 and the front surface of the lower side wall 47 are formed so as to be at the same position when projected in the vertical direction.

The second storage portion 28 communicates with the front side of the second storage portion 40, and is formed in a substantially U-shaped cross section that is open rearward.

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 as a substantially straight line extending forward as viewed from a side cross section. shape.

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

The first shaft 25 as the rotation shaft of the first gear 33 is provided to extend in the left-right direction in the second sleeve 31 (see FIG. 6).

The second shaft 26 as the rotation shaft of the second gear 34 is provided to extend parallel to the first shaft 25 in the second sleeve 31 (see FIG. 6). Further, the second shaft 26 is disposed 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.

Further, specifically, the first gear 33 and the second gear 34 respectively include helical teeth 35 that mesh with each other.

In the first gear 33, the tooth ribs of the helical teeth 35 are inclined to the outside of the rotation axis direction A1 in the upstream side from the downstream side in the rotation direction R2 of the first gear 33 toward the rotation direction R2. Further, the helical teeth 35 integrally include the first helical teeth 36 and the second helical teeth 37 having different tooth ribs. In the first gear 33, the first helical gear 36 is formed from the center in the axial direction of the first gear 33 to the right side, and the second helical gear 37 is formed from the center in the axial direction of the first gear 33 to the left side.

Specifically, the tooth rib of the first helical gear 36 is inclined from the left side (center portion side) to the right side (right end side) in the upstream side from the rotation direction R2 toward the upstream side in the rotation direction R2. On the other hand, the tooth rib of the second helical tooth 37 is formed bilaterally symmetrically with respect to the tooth rib of the first helical tooth 36 with respect to the central portion of the first gear 33 in the left-right direction, and specifically, is downstream from the rotation direction R2. The side faces the upstream side of the rotation direction R2 and is inclined from the right side (center portion side) to the left side (left end side).

The second gear 34 is formed to be vertically symmetrical with respect to the first gear 33, and is configured to mesh with the first gear 33. Specifically, the third gear 34 integrally includes the third helical gear 38 that meshes with the first helical gear 36, and 2 The fourth helical tooth 39 meshed by the helical tooth 37.

As shown in FIG. 8, in the pair of gears 32, the meshing portion indicated by the black dot is used for the side section. When the first gear 33 and the second gear 34 are in contact with each other in a point-like manner, the side cross-point contact type is obtained. Further, in the pair of gears 32, the meshing portion of the pair of gears 32 is formed in a spiral shape of the first gear 33 and the second gear 34 along the pair of gears 32, and thus is also in a line contact type.

The respective helical teeth 35 of the pair of gears 32 include a curved surface 41 that integrally includes a concave surface 42 that is formed in the rotational direction R2 at intervals and that is curved inward in the diametrical direction, and that connects the concave surfaces 42 is a convex surface 43 formed so that both ends of the concave surface 42 in the circumferential direction are curved outward in the radial direction.

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

First, as shown in FIG. 8(a), when the downstream end portion of the convex surface 43 of the first gear 33 in the rotational direction R2 meshes with the downstream end portion of the rotational direction R2 of the concave surface 42 of the second gear 34, As shown in FIG. 8(a) and FIG. 8(b), when the first gear 33 and the second gear 34 rotate in the rotational direction R2, the rotational direction R2 of the convex surface 43 of the first gear 33 is intermediate and The middle of the rotation direction R2 of the concave surface 42 of the gear 34 is engaged. Then, as shown by the arrows in FIG. 8(b) and FIG. 8(c), when the first gear 33 and the second gear 34 rotate in the rotational direction R2, the upstream side of the rotational direction R2 of the convex surface 43 of the first gear 33 is provided. The end portion is engaged with the upstream end portion of the concave direction 42 of the second gear 34 in the rotational direction R2. In other words, the nip portion of the convex surface 43 of the first gear 33 and the concave surface 42 of the second gear 34 sequentially moves in the downstream end portion, the intermediate portion, and the upstream end portion of the rotation direction R2 of each surface.

Then, although not shown, the nip portion of the concave surface 42 of the first gear 33 and the convex surface 43 of the second gear 34 is continuously continuous on the downstream side end portion, the intermediate portion, and the upstream side end of the rotation direction R2 of each surface. Department moves.

Therefore, the nip portion of the curved surface 41 of the first gear 33 and the curved surface 41 of the second gear 34 continuously moves in the rotational direction R2. The movement of the kneading portion prevents the formation of the storage portion of the retained kneaded material Y during the conveyance of the kneaded material Y.

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

As shown in FIGS. 5 and 6, the sheet adjusting portion 5 is provided on the front side of the gear structure 4 so as to include the protruding portion 63 of the upper side wall 48, and includes, for example, the protruding portion 63 in the gear structure 4, and as a movement. The support roller 51 of the support body. Further, as shown in FIG. 2, the sheet adjusting portion 5 includes a substrate feeding roller 56, a separator laminating roller 57, a rotating roller 58, and a separator feeding roller 59.

As shown in FIGS. 2 and 6, the protruding portion 63 has a function of dividing the wall of the gear discharge port 46 of the second sleeve 31 of the gear structure 4, and is adjusted to be ejected from the gear discharge port 46 in the sheet adjusting portion 5. Both of the functions of the blade (or knife) of the thickness of the sheet 7 are used.

The support roller 51 is disposed opposite to the protruding portion 63 so as to provide the gap 50 therebetween. The rotation axis of the support roller 51 is parallel to the first axis 25 and the second axis 26 of the pair of gears 32, and specifically extends in the left-right direction as shown in FIG. Further, as shown in FIG. 6, the rotation axis of the support roller 51 is disposed such that the gear discharge port 46 overlaps the protruding portion 63 when projected in the front-rear direction. Further, the support roller 51 is configured to support and convey the sheet 7.

Therefore, the support roller 51 is configured such that the sheet 7 passes through the gap 50.

As shown in FIG. 2, the substrate feed roller 56 is provided below the support roller 51 at intervals. The rotation axis of the substrate feeding roller 56 extends in the left-right direction, and the substrate 8 is wound into a roll shape on the circumferential surface of the substrate feeding roller 56.

The separator laminating roller 57 and the rotating roller 58 are disposed in front of the support roller 51 at intervals. The respective rotation axes of the separator laminating roller 57 and the rotating roller 58 are arranged to extend in the left-right direction. The separator laminating roller 57 is disposed on the upper side with respect to the rotating roller 58 and can be configured to press the rotating roller 58.

The rotating roller 58 is pressed against the sheet laminating roller 57, and is rotatable with respect to the sheet 7 and the substrate 8, and its upper end portion is formed to be the same as the upper end portion of the support roller 51 when projected in the front-rear direction. Location configuration.

The separator feeding roller 59 is provided on the upper side of the separator laminating roller 57 at an upper side with a space therebetween. The rotation axis of the separator feeding roller 59 extends in the left-right direction and is sent out at the partition On the circumferential surface of the roller 59, the separator 9 is wound into a roll shape.

The take-up portion 6 is provided in front of the sheet adjusting portion 5 and includes a tension roller 52 and a take-up roller 53.

The tension roller 52 is disposed in front of the rotating roller 58 at intervals, and specifically, the upper end portion of the tension roller 52 is disposed so as to be at the same position as the upper end portion of the rotating roller 58 when projected in the front-rear direction. The rotation axis of the tension roller 52 is formed to extend in the left-right direction.

The take-up roller 53 is disposed opposite to the tension roller 52 at an interval obliquely downward from the front side. Further, the rotation axis of the take-up roller 53 is configured to extend in the left-right direction, and the laminated sheet 10 is wound (wound) into a roll shape on the circumferential surface of the take-up roller 53, and a roll-shaped sheet can be obtained. Material 60.

The size of the sheet manufacturing apparatus 1 is appropriately set in accordance with the type and blending ratio of the particles and resin components to be used, and the width W1 and the thickness T1 of the target roll sheet 60.

As shown in FIG. 5, the width W0 of the first sleeve 21 and the length W2 of the pair of gears 32 in the rotation axis direction satisfy the relationship of the following formula (1), and preferably satisfy the relationship of the following formula (2). More preferably, it is set so as to satisfy the relationship 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)

As shown in Fig. 7, the length W2 of the rotational direction of the pair of gears 32 can be appropriately selected depending on the width W1 of the manufactured sheet 7 or the roll-shaped sheet 60, specifically, the width of the first sleeve 21 described above. Similarly to W0, the width W1 of the produced sheet 7 or the roll-shaped sheet 60 is, for example, 70% or more, preferably 80% or more, and is also, for example, 100% or less.

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

The gear diameter of a pair of gears 32 (the diameter (outer diameter) of the gear 32, in detail, the straight edge of the tool tip The diameter is set so as not to deform the pair of gears 32 under the pressure at the time of conveyance of the kneaded material, and specifically, for example, 10 mm or more, preferably 20 mm or more, and for example, 200 mm or less, preferably Below 80mm.

The tooth height of the pair of gears 32 is, for example, 1 mm or more, preferably 3 mm or more, and is also, for example, 30 mm or less, preferably 20 mm or less.

The pitch interval in the rotation axis direction A1 of the helical teeth 35 is, for example, 5 mm or more, preferably 10 mm or more, and is also, for example, 30 mm or less, preferably 25 mm or less. Further, the angle (inclination angle) of the tooth ribs of the helical teeth 35 with respect to the rotation axis of the pair of gears 32 is, for example, 5 degrees or more, preferably 10 degrees or more, more preferably 15 degrees or more, and, for example, less than 90 degrees. The degree is preferably 85 degrees or less, more preferably 80 degrees or less.

Further, as shown in FIGS. 5 and 6, the gap 50 in the front-rear direction distance L1 can be appropriately set according to the required thickness, and in detail, is the same distance (length) as the total thickness of the sheet 7 and the substrate 8. For example, it is 10 μm or more, preferably 30 μm or more, and more preferably 100 μm or more, and is also, for example, 1000 μm or less, preferably 800 μm or less, and more preferably 750 μm or less.

The outer diameter of the take-up roller 53 is, for example, 76 mm or more, preferably 152 mm or more, and is also, for example, 500 mm or less.

Hereinafter, a method of manufacturing the roll-shaped sheet 60 from the composition X containing particles and a resin component using the sheet manufacturing apparatus 1 will be described.

First, as shown in FIG. 2, the composition X containing a particle and a resin component is added to the inlet port 14.

Moreover, in the sheet manufacturing apparatus 1, the kneading machine 2, the supply unit 3, and the gear structure 4 are adjusted to a specific temperature and a rotation speed. In addition, when the temperature of the kneading machine 2, the supply unit 3, and the gear structure 4 is, for example, when the resin component contains a thermoplastic resin component, the temperature is equal to or higher than the softening temperature, and the resin component contains a thermosetting resin component (for example, a ring). In the case of an oxy-resin, the curing temperature is not reached, specifically, for example, 200 ° C or lower, preferably 150 ° C. In the case where the resin component further contains a thermoplastic resin component, the softening temperature is more than or equal to, and specifically, it is, for example, 50 ° C or higher, preferably 70 ° C or higher.

Further, the substrate 8 is preliminarily wound on the substrate feed roller 56.

Examples of the substrate 8 include a polypropylene film, an ethylene-propylene copolymer film, a polyester film (PET (polyethylene terephthalate), etc.), and a plastic film such as polyvinyl chloride; for example; Paper such as kraft paper; cloth such as cotton cloth or staple fiber cloth; non-woven fabric such as polyester non-woven fabric and vinylon non-woven fabric; for example, metal foil. The thickness of the substrate 8 is appropriately selected depending on the purpose, use, and the like, and is, for example, 10 to 500 μm. Further, the surface of the substrate 8 may be subjected to a release treatment.

Further, the separator 9 is wound on the separator feeding roller 59 in advance.

The separator 9 may be the same as the substrate 8, or may be surface-treated. The thickness of the separator 9 is appropriately selected depending on the purpose, use, and the like, and is, for example, 10 to 500 μm.

Then, the composition X is introduced into the cylinder 70 from the inlet 14 of the cylinder 70.

In the kneading machine 2, the particles and the resin component contained in the composition X are heated by a heater (not shown), and kneaded by the rotation of the kneading shaft 13 to disperse the particles in the resin component. The kneaded material Y reaches the supply unit inlet 18 in the supply unit 3 from the discharge port 15 via the connection pipe 17 as shown in Fig. 5 (kneading extrusion step).

Specifically, as shown in FIG. 3, when the driving force from the driving source (not shown) is transmitted to the drive shaft 8a, the kneading shaft 13 is rotationally driven, and the composition X is stirred by the first feeding portion 23a while The first mixing unit 27a is conveyed.

At this time, the cylinder 70 (melt kneading portion 6a) located on the outer side of the first feeding portion 23a is adjusted to, for example, 15 to 20 ° C by a heater (not shown). Further, the air or the like that has entered the inside of the cylinder 70 while introducing the composition X is released to the outside of the cylinder 70 by opening the first vent portion 54a.

Then, the conveyed composition X is kneaded in the first kneading section 27a.

At this time, the melt kneading portion 6a located on the outer side of the first kneading portion 27a is adjusted to, for example, 40 to 80 ° C by a heater (not shown).

Then, the kneaded composition X is extruded to the first inverting portion 30a by the extrusion force of the composition X conveyed by the rotation of the first feeding portion 23a.

Most of the composition X extruded to the first inverting portion 30a reaches the second feeding portion 24a through the first inverting portion 30a. On the other hand, part of the extruded composition X is returned to the first kneading portion 27a by the rotation of the first reversing portion 30a, and the kneading is performed again.

Thereby, the promotion of the kneading of the composition X is sought, and the conveying speed of the composition X is adjusted.

Then, the composition X that has passed through the first inverting portion 30a is transported to the second mixing portion 28a and the second inverting portion 31a by the second feeding portion 24a.

In the same manner as in the case of the first mixing unit 27a and the first reversing unit 30a, the composition X passes through the second mixing unit 28a and the second reversing unit 31a.

At this time, the melt kneading portion 6a located on the outer side of the second kneading portion 28a is adjusted to, for example, 60 to 120 ° C by a heater (not shown).

Then, the composition X that has passed through the second inverting portion 31a is conveyed to the third mixing portion 29a by the next third feeding portion 25a, and further kneaded in the third mixing portion 29a. Thereby, the composition X was prepared as the kneaded material Y.

At this time, the melt kneading portion 6a located on the outer side of the third kneading portion 29a is adjusted to, for example, 80 to 140 ° C by a heater (not shown).

Then, the kneaded material Y is extruded by the rotation of the kneading shaft 13 to reach the fourth feeding portion 26a.

At this time, by driving a pump (not shown) connected to the second ventilating portion 55a, moisture or volatile components in the kneaded material Y are discharged to the outside of the melt kneading portion 6a.

Thereby, the reduction of the pores in the kneaded material Y can be achieved.

Then, the kneaded material Y is conveyed to the duct portion 12a by the fourth feeding portion 26a.

As described above, the duct portion 12a is formed so as not to have irregularities over the entire circumference. Therefore, in the duct portion 12a, the kneaded material Y is prevented from shearing in the direction intersecting the axial direction of the kneading shaft 13, and smoothly moves in the axial direction of the duct portion 12a.

Then, the kneaded material Y ejects the kneaded material Y from the discharge port 15.

According to the above, the kneaded material Y which suppresses the generation of pores was prepared from the composition X.

Then, as shown in FIG. 1, the kneading material Y is rotated by the supply screw 22 in the supply unit 3 so as to have a width W0 (width W0 of the first sleeve 21) which is a direction in which the kneading machine 2 is ejected, that is, in the left-right direction. In the intersecting direction with respect to the discharge direction (specifically, the direction orthogonal to the discharge direction), the method is supplied to the gear structure 4 in the front direction in detail (supply step). In other words, the kneaded material Y that has been extruded from the kneading machine 2 to the right side and reaches the supply unit 3 via the connecting pipe 17 is converted into a direction of 90 degrees in the supply unit 3 by the kneading direction. Specifically, the kneaded material Y is supplied to the gear structure 4 via the first storage portion 27 so as to have a width W0 in the left-right direction while changing the conveyance direction from the right to the front. In other words, in the supply unit 3, the kneading material Y is ejected in the discharge direction (left-right direction) (that is, conveyed in the conveying direction of the supply screw 22) and the kneaded material Y is supplied to the gear structure 4.

Then, the kneaded material Y is deformed in the rotation axis direction A1 of the pair of gears 32 in the gear structure 4, and is formed into the sheet 7 and conveyed forward (deformation conveyance step).

Specifically, the kneaded material Y is formed into a sheet 7 by the meshing of the pair of gears 32 and extending from the central portion of the rotation axis direction A1 to both end portions. Then, move forward.

Specifically, referring to Fig. 6, the kneaded material Y is extruded forward from the upper end portion and the lower end portion of the front side portion of the first storage portion 27 in the rotation direction R2 of the pair of gears 32, and passes through the lower portion 61 of the second housing portion 40. The second storage portion 28 is reached between the first gear 33 and between the upper portion 62 of the second housing portion 40 and the second gear 34.

At this time, the kneaded material Y of the second storage portion 28 is prevented from flowing backward (returning to the rear) to the first storage portion 27 via the meshing portion (see FIG. 8) of the helical teeth 35 by the pair of gears 32, while being inclined by the pair of gears The engaging portion of the teeth 35 is expanded in the left-right direction to be deformed (formed) into the sheet 7.

Specifically, as shown in FIG. 7, in the right side portion of the gear structure 4, the first helical gear 36 meshes with the third helical gear 38, and the central portion of the pair of gears 32 in the direction of the rotational axis A1 The right end is expanded. On the other hand, on the left side of the gear structure 4, the second helical tooth The engagement with the fourth helical teeth 39 extends from the central portion of the pair of gears 32 in the direction of the rotational axis A1 toward the left end.

Thereby, the sheet 7 can be obtained from the kneaded material Y.

Then, as shown in FIGS. 5 and 6, the obtained sheet 7 reaches the gear discharge port 46 via the second reservoir portion 28 and the discharge passage 44, and then ejects (transports) from the gear discharge port 46 to the support roller 51.

Specifically, the base material 8 fed from the substrate feed roller 56 (see FIG. 2) is laminated on the circumferential surface of the support roller 51, and the sheet 7 is supported by the support roller 51 via the base material 8 while supporting the roller. 51 in the direction of rotation.

The sheet 7 conveyed from the gear discharge port 46 is temporarily conveyed via the base material 8 after the support roller 51, and then the thickness is adjusted by the projection 63 and the circumferential surface of the support roller 51. Specifically, the excess kneaded material Y is adjusted to a sheet 7 having a desired thickness T1 and a desired width W1 by the surface of the substrate 8 supported on the support roller 51 being removed by the projection 63 (the gap is passed) step).

The speed (coating speed) of the sheet 7 passing through the gap 50 between the protruding portion 63 and the peripheral surface of the support roller 51 is, for example, 0.01 m/min or more, preferably 0.05 m/min or more, and is also, for example, 1.0. It is m/min or less, preferably 0.35 m/min or less.

The thickness T1 of the sheet 7 is substantially the same as the distance L1 between the front and the rear direction of the gap 50, and specifically, for example, 50 μm or more, preferably 100 μm or more, more preferably 300 μm or more, and for example, 1000 μm or less, preferably 800 μm or less, more preferably 750 μm or less.

Further, the shear stress in the temperature range of 50 to 250 ° C of the composition (deformed into a composition of the sheet) passed through the gap passage is, for example, 5.0 × 10 ⁴ Pa or less, preferably 4.0 × 10 ⁴ Pa. The following is further preferably 3.0 × 10 ⁴ Pa or less, and further has a shear stress of 1.0 × 10 ³ Pa or more. The shearing region may have a shear stress of the above value at a temperature of at least a part of the temperature range (ie, 50 to 250 ° C, preferably 60 to 150 ° C, more preferably 80 to 100 ° C). It is preferred to have a shear stress of the above value over the entire temperature range.

If the shear stress is 5 × 10 ⁴ Pa or less, the gap can be easily formed into a predetermined width by the width of the sheet 7 after the step, and the desired wide roll-shaped sheet 60 can be obtained. On the other hand, when the shear stress is 1.0 × 10 ³ Pa or more, it is good in terms of prevention of dripping.

Further, the shear rate may be adjusted so that the shear stress is within the above range, and may be appropriately determined depending on the gap 50 and the coating speed.

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

The temperature in the gap passage step is, for example, 50 ° C or higher, preferably 60 ° C or higher, more preferably 80 ° C or higher, and is also, for example, 250 ° C or lower, preferably 150 ° C or lower, and more preferably 100 ° C or lower. .

Then, as shown in FIG. 2, the substrate 8 on which the sheet 7 is laminated is conveyed from the support roller 51 to the separator laminating roller 57 and the rotating roller 58, between the separator laminating roller 57 and the rotating roller 58, the sheet The upper surface area layer 7 has a separator 9. Thereby, the sheet 7 can be obtained as a laminated sheet 10 in which the base material 8 and the separator 9 are laminated on both surfaces (the lower surface and the upper surface).

Thereafter, the laminated sheet 10 is passed through a tension roller 52, and then wound up by a take-up roll 53 into a roll shape to manufacture a roll-shaped sheet 60 (winding step).

At this time, in the roll-shaped sheet 60, the separator 9 , the sheet 7 , and the substrate 8 are sequentially laminated on the outer side in the diameter direction of the winding roller 53 .

In the sheet manufacturing apparatus 1, when the resin component contains a thermosetting resin component, it is thermally hardened in the sheet 7 after being heated by the kneading machine 2 until it is wound up on the winding roller 53. The resin component is in a B-stage state, and the thermosetting resin component wound in the sheet 7 on the take-up roll 53 is also in a B-stage state.

Further, the roll-shaped sheet 60 produced by the above production method has flexibility at normal temperature (25 ° C).

In the roll-shaped sheet 60, if the resin contains an epoxy resin, the B-stage sealing sheet 7 (base) The tensile modulus at 25 ° C of the material 8 and the separator 9 is, for example, 0.1 GPa or more, preferably 0.5 Ga or more, more preferably 1.0 GPa or more, and is also, for example, 20 GPa or less, preferably 10 GPa. The following is more preferably 5 GPa or less. The method for measuring the tensile elastic modulus of the sealing sheet 7 of the B stage is described in detail in the evaluation of the examples below.

When the tensile elastic modulus is equal to or less than the above upper limit, the following sealing target can be reliably embedded, and the sealing property against the sealing target can be improved. On the other hand, when the tensile elastic modulus is at least the above lower limit, the collapse of the sealing sheet 7 wound up on the take-up roll 53 can be 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 35% by volume or more, preferably 40% by volume or more, more preferably 60% by volume or more, and still more preferably 70% by volume or more. For example, it is 98% by volume or less, preferably 95% by volume or less.

When the volume ratio of the particles does not reach the above lower limit, the specific physical properties of the particles cannot be sufficiently exhibited. On the other hand, when the volume ratio of the particles is equal to or less than the above upper limit, the flexibility of the sealing sheet 7 can be ensured, and the roll-shaped sheet 60 can be surely obtained.

The thickness of each of the sheets 7 of the roll-shaped sheet 60 is, for example, 10 μm or more, preferably 30 μm or more, more preferably 100 μm or more, and particularly preferably 200 μm or more, and is also, for example, 800 μm or less.

When the thickness is at least the above lower limit, the thickness of the roll-shaped sheet 60 containing particles in a desired ratio can be sufficiently ensured, and the object to be sealed can be reliably covered and embedded.

The width of the roll-shaped sheet 60 (the length orthogonal to the longitudinal direction and the thickness direction) is, for example, 200 mm or more, preferably 500 mm or more, more preferably 1000 mm, and is also, for example, 10000 mm or less. When the width of the roll-shaped sheet 60 is not less than the above-described lower limit, it is possible to easily seal the sealed object by covering/embedding various sealing objects by one of the sealing sheets 7 taken out from the one roll-shaped sheet 60.

The inner diameter of the roll-shaped sheet 60 is the same as the outer diameter of the take-up 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 also, for example, 500 mm or less.

Further, according to the roll-shaped sheet 60, particles are contained at a high blending ratio and formed into a roll shape. Therefore, the specific physical properties of the particles can be sufficiently exhibited, and the storage space can be reduced, and the handling property is excellent.

In the method of manufacturing the roll-shaped sheet 60, the gear structure 4 is used, and the composition X containing the particles and the resin component is transferred while being deformed in the axial direction A1, and then the sheet adjusting unit 5 is used. The support roller 51 supports and conveys the sheet (composition) deformed in the axial direction A1 via the substrate 8, and passes it through the gap 50 with the protruding portion 63, so that the blending ratio of the particles exceeds 30% by volume, and the strip can be manufactured. Sheet 7. As a result, in the subsequent winding step, the long sheet 7 can be easily taken up on the take-up roll 53, so that the roll-shaped sheet 60 can be obtained.

Moreover, since the kneaded material Y is deformed by using the gear structure 4, it is possible to form a sheet shape by containing particles in the 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 blending ratio can be produced.

Further, the shear stress of the composition passed through the gap passage step is 5.0 × 10 ⁴ Pa or less in a temperature range of 50 to 250 °C. Therefore, the gap can be easily formed into a predetermined width by the width of the sheet after the step, and a desired wide roll-shaped sheet can be produced.

In the case where the roll-shaped sheet 60 is used as a heat-dissipating sheet and is combined with a flexible circuit board (composite circuit board), the heat-dissipating sheet which is formed into a roll shape can be continuously wound ( Roll to roll) is manufactured as a composite circuit substrate simply and at a low manufacturing cost.

In addition, since the blending ratio of the particles in the roll-shaped sheet 60 exceeds 30% by volume, the roll-shaped sheet 60 can sufficiently exhibit the specific physical properties of the particles (for example, heat dissipation (thermal conductivity), conductivity (conductivity) ), insulation, magnetic, etc.).

Therefore, when the roll-shaped sheet 60 is fed out from the take-up roll 53, it can be preferably used as a heat conductive sheet such as a heat-dissipating sheet, for example, an electroconductive sheet such as an electrode material or a current collector, for example, an insulating sheet. For example, a magnetic sheet or the like.

Further, the roll-shaped sheet 60 produced by the manufacturing apparatus shown in Fig. 1 is formed by laminating a substrate and a separator on both sides in the thickness direction of a sheet (layer) containing a composition containing particles and a resin component, or only A substrate or a separator may be laminated on one side in the thickness direction, or a sheet in which the substrate is not laminated on both sides (that is, a single layer including only a sheet containing a composition of particles and a resin component).

Further, in the method of manufacturing the roll-shaped sheet 60, as shown in Fig. 7, when the length W2 of the pair of gears 32 in the rotational axis direction is 200 mm or more, the sheet 7 having a wide width W1 is preferably used. For a wide range of uses.

In FIG. 1, although not shown, the composition X may be directly supplied to the supply unit 3 or the gear structure 4 without providing the kneading machine 2 in the sheet manufacturing apparatus 1.

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

As a result, the kneaded material Y that has reached the supply unit 3 or the gear structure 4 is preliminarily kneaded by the kneading machine 2, so that the dispersibility of the particles with respect to the resin component can be further improved.

In FIG. 1, although not shown, for example, the separator laminating roller 57 and the separator feeding roller 59 are not provided in the sheet manufacturing apparatus 1, and the sheet 7 is taken up to the winding roller 53. The roll-shaped sheet 60 of the separator 9 is not laminated. At this time, in the roll-shaped sheet 60, the laminated sheet 7 and the substrate 8 are sequentially repeated in the outer diameter direction of the winding roller 53. It is preferred to use the substrate 8 which is subjected to mold release treatment at least on the inner surface.

Further, in general, when the sealing sheet is used, it is necessary to separately transport the sealing sheets prepared in a single sheet shape or to arrange the sealing sheets one by one on the sealing target. Therefore, there is a case where the working time is long, and when the sealing sheet is taken out from a tray or the like, the sealing sheet or the like is damaged and the operability is disadvantageous. Further, in order to mass-produce a sealing sheet, a plurality of sheet manufacturing apparatuses 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 sealing object can be continuously sealed by the sheet 7. Moreover, the above-described operability can be improved, and the necessary sheet manufacturing apparatus 1 is also small in size, and a large number of sheets can be manufactured in a large amount. 7. Further, the cost required for the sealing can be reduced. That is, it is possible to shorten the working time, improve the operability, and reduce the investment cost.

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 can be preferably used as a thermosetting insulating resin such as a thermosetting resin sheet. Sheet (specifically a sealing sheet).

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

In the following description, the same configurations as those of the above-described embodiment will be omitted.

As the particles, from the viewpoint of reinforcement, nitrides and oxides are preferably cited.

In addition, as the material, an insulating material is preferable, and examples of such an insulating material include a nitride, an oxide, and the like. Specific examples thereof include BN and cerium oxide.

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

Further, the epoxy resin is preferably used in combination with a curing agent and/or a curing accelerator to prepare an epoxy resin composition and is 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 which is dissolved and/or dispersed by a solvent, if necessary.

Further, the resin component may further contain a thermosetting resin component other than the epoxy resin or a thermoplastic resin component, 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, and polyoxymethylene resin. , thermosetting urethane resin, and the like.

The phenol resin is a resin containing a phenol compound carried in the front, and can be used as a curing agent in combination with an epoxy resin. When the ratio of the phenol resin is used in combination with the epoxy resin, the amount is, for example, 1 part by mass or more, preferably 5 parts by mass or more, and more preferably 10 parts by mass or more, based on 100 parts by mass of the epoxy resin. For example, it is 200 parts by mass or less, preferably 150 parts by mass or less.

Further, the roll-shaped sheet 60 can be wound into a roll shape by using the sheet manufacturing apparatus 1 shown in FIGS. 1 to 8 in the same manner as described above in the sealing sheet formed as a thermosetting insulating resin sheet. And get.

Next, a method of manufacturing the roll-shaped sheet 60 as a particle-containing roll-shaped sheet will be described with reference to Figs. 1 to 8 .

In Fig. 1, a sheet manufacturing apparatus (particle roll-containing sheet manufacturing apparatus) 1 is configured by manufacturing a roll-shaped sheet 60 (see Fig. 2) from a composition X containing particles and a resin component, and includes kneading. The machine 2, the supply unit 3, the gear structure 4, the sheet adjusting unit (sealing sheet adjusting unit) 5, and the winding unit 6.

Any one of the separator 9 and the substrate 8 is peeled off from the sealing sheet 7. Thereafter, the sealing sheet 7 is placed on the sealing target so as to cover/embed the sealing object.

Examples of the sealing target include a semiconductor device, a hard disk, an LED (Light Emitting Diode) device (such as a television, an illumination, and a display), and an EL (Electroluminescence) device (an organic EL display or an organic device). EL illumination, etc., capacitors, batteries (lithium ion batteries, etc.), power modules, surface acoustic wave (SAW) filters, various sensor devices, and the like.

Then, the other of the separator 9 and the substrate 8 is peeled off from the sealing sheet 7.

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

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

Further, the tensile modulus of the C-stage sealing sheet 7 at 25 ° C is, for example, 0.1 GPa or more, preferably 1 GMPa or more, more preferably 2 GPa or more, and is also, for example, 20 GPa or less, preferably 8 GPa. The following is more preferably 5 GPa or less. C-stage sealing sheet 7 pull The method for determining the modulus of elasticity is described in detail in the evaluation of the examples below.

When the tensile modulus at 25° C of the sealing sheet 7 of the C-stage is at least the above lower limit, there is an advantage that the cutting property of the resin is excellent, and if it is at most the above upper limit, there is an advantage that warpage can be reduced.

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

For example, the following method is proposed (for example, refer to Japanese Laid-Open Patent Publication No. 2011-32434).

In other words, a coating varnish in which a cerium oxide powder, an epoxy resin, a phenol resin, and methyl ethyl ketone are dispersed and mixed is prepared, and then a coating varnish is applied onto a release-treated surface of the polyester film. Drying, thereby producing a sheet on the polyester film. Thereafter, the pieces are cut into a specific shape, and a plurality of sheets are prepared, and then the plurality of sheets are peeled off from the polyester film, and the peeled plurality of sheets are laminated to obtain electrons having a specific thickness. Sheet for parts sealing.

However, in the method described in Patent Document 1, since a plurality of sheets are peeled off from the polyester film, and then the sheets are laminated to produce a sheet, the number of manufacturing steps is large, and thus the production efficiency is low. Bad situation.

In addition, the sheet obtained by the method described in Japanese Laid-Open Patent Publication No. 2011-32434 is a flat sheet having one side as a short side. When such a short-side sheet is downloaded and stored in the state of a flat sheet, a large storage space is required, and it is also disadvantageous in terms of portability.

However, as the roll-shaped sheet 60 containing the particle-shaped roll sheet, the sealing sheet 7 is wound into a roll shape, and the particles are contained at a high blending ratio. Therefore, it is possible to manufacture efficiently and efficiently, and to exhibit the specific physical properties of the particles, specifically, the insulating property and the reinforcing property, and the storage space can be reduced, and the handling property is excellent.

Further, according to the method of manufacturing the roll-shaped sheet 60, the gear structure 4 is used to contain After the composition X of the particle and the resin component is conveyed while being deformed in the axial direction A1, the sheet adjusting portion 5 supports and conveys the sheet deformed in the axial direction A1 via the substrate 8 via the support roller 51 ( The composition) is passed through the gap 50 with the projection 63, so that the blending ratio of the particles exceeds 30% by volume, and the long sealing sheet 7 can be produced. As a result, in the subsequent winding step, the long sealing sheet 7 can be easily wound up on the take-up roll 53, so that the roll-shaped sheet 60 can be obtained.

Moreover, since the kneaded material Y is deformed by using the gear structure 4, it is possible to form a sheet shape by containing particles in the 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 blending ratio can be produced.

Moreover, in general, when the sealing sheet 7 is used, it is necessary to separately transport the sealing sheets 7 prepared in a single sheet or to arrange the sealing sheets 7 one by one on the sealing target. Therefore, there is a case where the working time is long, and the sealing sheet 7 is damaged when the sealing sheet 7 is taken out from the tray or the like, which is disadvantageous in terms of operability. 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 sealing sheet 7 can be continuously sealed by the sealing sheet 7. Moreover, the above-described operability can be improved, and the necessary sheet manufacturing apparatus 1 is also small, and the roll-shaped sheet 60 can be mass-produced from the long-length sealing sheet 7. Further, the cost required for the sealing can be reduced. That is, it is possible to shorten the working time, improve the operability, and reduce the investment cost.

Further, the roll-shaped sheet 60 manufactured by the manufacturing apparatus shown in Fig. 1 is formed by laminating a substrate 8 and a separator on both sides in the thickness direction of a sealing sheet (layer) 1 containing a composition containing particles and a resin component. 9. The substrate 8 or the separator 9 may be laminated only on one side in the thickness direction, or may be formed as a sealing sheet 7 which does not laminate the substrate 8 or the separator 9 on both sides (ie, contains only particles) And a single layer of the sealing sheet 7 of the composition of the resin component).

Next, another embodiment of the sheet manufacturing apparatus of the present invention will be described with reference to FIGS. 9 to 11. State is explained. In the following drawings, the same reference numerals will be given to the components corresponding to the respective components, and the detailed description thereof will be omitted.

In the embodiment of Fig. 1, the kneading machine 2 is disposed on the left side of the sheet manufacturing apparatus 1 so as to extend in the left-right direction, and may be disposed on the sheet so as to extend in the front-rear direction as shown in Fig. 9, for example. The rear side of the device 1 is manufactured.

In the embodiment of Fig. 9, the cylinder 70 is formed to extend in the front-rear direction as shown in Fig. 10 .

The inlet 14 is formed to open upward through the upper end wall of the rear end of the cylinder 70.

As shown in FIG. 9 and FIG. 10 (dotted line in FIG. 10), the discharge port 15 is formed so as to open to the right side through the right wall of the front end portion of the cylinder 70, and is connected to the left-right direction. The tube 17 is configured in a continuous manner.

As shown in Fig. 10, the kneading shaft 13 includes one drive shaft 8a, a plurality of (four) feed screw portions 9a, a plurality of (three) reverse screw portions 10a, and a plurality of (three) mixing portions 11a. And one pipe portion 12a.

Specifically, the kneading shaft 13 of the embodiment of Fig. 3 includes two reversing screw portions 10a. In contrast, the kneading shaft 13 of the embodiment of Fig. 9 further includes one reversing screw portion 10a, the reversing screw As shown in FIGS. 10 and 11, the portion 10a is disposed adjacent to the duct portion 12a on the front side of the duct portion 12a.

In other words, the plurality of (three) reversing screw portions 10a are formed by the first reversing portion 30a, the second reversing portion 31a, and the third reversing portion 32a, and are arranged at intervals with respect to the axis of the kneading shaft 13 In the direction, the third reversing portion 32a is disposed at the end portion on the side of the discharge port 15 side.

The length of the drive shaft 8a of the third inverting portion 32a in the axial direction is formed to be the longest compared to the other inverting portions. The length of the drive shaft 8a in the axial direction is approximately 1/4 of the first feed portion 23a.

The duct portion 12a is formed between the fourth feeding portion 26a and the third reversing portion 32a, and is disposed to include the discharge port 15 when projected in the left-right direction.

Further, as shown in the imaginary line of FIG. 9, the kneading machine 2 shown in FIG. 10 may be disposed after the supply unit 3 via the connecting pipe 17 so that the axial direction of the kneading shaft 13 is parallel to the axial direction of the supply screw 22. side.

Thereby, the generation of the pores in the kneaded material Y can be suppressed similarly to the embodiment of Fig. 4 described above.

Further, in the present invention, the sheet contains the concept of a belt or a film.

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

[Examples]

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

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 (particles), 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 mixture of semi-solid shapes (composition X) ). The blending ratio of the particles was 78.8 vol%.

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

Extruder 2: extrusion speed 42 mL / min, temperature 120 ° C

Supply unit 3: the supply screw 22 is a twin screw, the length in the direction of the rotation axis (WO) is 500 mm, the supply speed is 42 mL/min, the screw rotation speed is 5 rpm, and the temperature is 90 ° C.

Gear structure 4: tooth height 8.8 mm, inclination angle of helical teeth 35 (with respect to the direction of the rotation axis (A1)) 17.7 degrees, pitch interval 18.84 mm, length of the rotation axis direction of the gear 32 (A1) (W2) 500 mm The width of the first sleeve 21 (W0) is 500.2 mm, the gear diameter (outer diameter) is 42 mm, the gear rotation speed is 0.15 rpm, and the temperature is 90 ° C.

Sheet adjusting portion 5: gap 50 before and after the gap 50 (L1) 200 μm, coating speed 0.05 (m/min), temperature 80 ° C

Winding portion 6: diameter (outer diameter) of the take-up roller 53: 200 mm

Substrate 8: PET, thickness 38 μm

Separator 9: PET, thickness 38μm

Then, the sheet manufacturing apparatus 1 was operated under the above-described conditions, and the sealing sheet 7 of the B stage and having a thickness of 200 μm was taken up (wound) by the winding unit 6, whereby the particle-containing roll-shaped sheet 60 was obtained.

Hereinafter, the components to be formulated will be described in detail.

̇Epoxy resin: bisphenol F type epoxy resin, trade name "YSLV-80XY", manufactured by Nippon Steel Chemical Co., Ltd., epoxy equivalent 200g/eq., softening point 80 °C

Tantalum hardener: phenol-aralkyl resin, trade name "MEH7851SS", manufactured by Minghe Chemical Co., Ltd., hydroxyl equivalent 203g/eq., softening point 67 °C

̇ Filler: 矽 偶 coupling agent (KBM403, Shin-Etsu) is added to 100 parts by mass of particles, inorganic filler (melted cerium oxide) (FB-9454, spherical shape, density 2.2 g/cm ³ , manufactured by Denki Kagaku Kogyo Co., Ltd.) 0.1 part by mass produced by Chemical Industry Co., Ltd. and subjected to surface treatment.

̇ Flame retardant: phosphazene derivative, trade name "Rabitle FP-100", manufactured by Fushimi Pharmaceutical Co., Ltd.

̇ Elastomer: styrene-isobutylene block copolymer, trade name "SIBSTAR 072T", manufactured by Kaneka

Example 2~16

The roll-shaped sheet 60 was obtained in the same manner as in Example 1 except that the setting conditions of the sheet adjusting portion were changed to the conditions described in Table 1.

Example 17

A sheet-like sheet-like sheet 60 was obtained in the same manner as in Example 1 except that the sheet manufacturing apparatus 1 having the apparatus configuration of FIG. 9 was prepared and used in place of the sheet manufacturing apparatus 1 having the apparatus configuration of FIG. .

Comparative example 1 (roll coating + laminating machine)

In the same formulation as in Example 1, each component (particles and resin component) and further MEK were blended and stirred to prepare a liquid varnish (composition, solid content concentration: 50% by mass).

In addition, a roll coater was prepared.

Then, the varnish was applied using a roll coater to produce a sealing sheet.

Specifically, the coating film was applied to the PET film subjected to the release treatment, and the coating gap was adjusted so that the thickness of the sealing sheet after the solvent was dried was 50 μm, and the coating speed was 1.0 m/min. . Further, the drying furnace was set to a drying temperature of 120 ° C and a drying time of 3 minutes.

The obtained sheet having a thickness of 50 μm was formed into a sealing sheet having a thickness of 100 μm at a conveying speed of 1.0 m/min at a temperature of 90 ° C using a laminator.

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

Further, in Comparative Example 1, in order to obtain a laminated sealing sheet having a desired thickness (500 μm) having a high blending ratio of particles (78.8% by volume), a plurality of sealing sheets (50 μm, 100 μm) were laminated in plural times. The trouble.

(Evaluation)

̇ shear stress

The shear stress was calculated based on the following.

Use the measuring instrument name CAPILOGRRAPH. E 3B (manufactured by Toyo Seiki Seisakusho Co., Ltd.), based on the capillary length: 10 mm, capillary diameter: 1.0 mm, the shear load is calculated at a piston speed of 0.5, 1.0, 2.0, 5.0, 7.0, 10.0 mm/min. The shear stress is further calculated based on the capillary diameter and the piston speed, and a graph of shear rate-shear stress is prepared. The curve obtained in the graph was used, and the shear rate calculated from the GAP (gap) and the coating speed at the time of evaluation was applied to the formula, and the shear stress at each shear rate was calculated.

Cutting speed

The shear rate was calculated based on the following.

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

Coating property

For the coating width of 500 mm, the case where the coatable region is about 100% is ○, the case where the coatable region is 99 to 50% is Δ, and the coatable region is less than 50%. The situation is set to ×. The results are shown in Table 1.

Roller shape

The case where the sheet was in the form of a roll was evaluated as ○, and the case where the sheet was cracked or broken was evaluated as ×. The results are shown in Table 1.

密封 Sealing test of Example 1 and Example 17

The sealing sheet 7 is taken out from each of the particle-containing roll sheets 60 of the first embodiment and the seventeenth embodiment, and the sealing sheet 7 is placed on the flip chip and the flip chip type device. The FR-4 substrate (Flame Retardant Type 4, size 150 mm × 150 mm × 0.5 mm) of the wafer type device.

Thereafter, the sealing sheet 7 was completely cured by heating at 150 ° C for 60 minutes. Thereby, the flip chip type device is covered with the sealing sheet 7.

密封Comparative 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 × 150 mm × 0.5 mm) in which a flip chip type device to be sealed was mounted so as to cover and embed a flip chip type device. )on.

Thereafter, the sealing sheet 7 was completely cured by heating at 150 ° C for 60 minutes. Thereby, the flip chip type device is coated with the laminated sealing sheet.

Determination of tensile modulus of elasticity

The B-stage sealing sheet was taken out from the particle-containing roll sheets of Examples 1 and 17, and was obtained by the DMA method (calculating the storage elastic modulus value at a temperature increase rate of 10 ° C/min at a measurement frequency of 1 Hz). Its tensile modulus at 25 ° C. Then, the B-stage sealing sheet The material was heated at 150 ° C for 60 minutes, and the fully cured (C-staged) sealing sheet was obtained at 25 ° C by the DMA method (calculating the storage elastic modulus value at a temperature increase rate of 10 ° C/min at a measurement frequency of 1 Hz). The tensile modulus of elasticity.

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

In addition, the invention is described as an exemplified embodiment of the invention, and is merely illustrative and not limited by the disclosure. The scope of the patent application described below is intended to be a modification of the invention to those skilled in the art.

[Industrial availability]

The roll-shaped sheet can be used as a semiconductor device, a hard disk, an LED device (television, illumination, display, etc.), an EL device (organic EL display, organic EL illumination, etc.), a capacitor, a battery (lithium ion battery, etc.), and a power mode. Sealed particle-containing roll sheets such as groups, surface acoustic wave (SAW) filters, various sensor devices, and the like.

1‧‧‧Sheet manufacturing equipment

2‧‧‧Machine

3‧‧‧Supply Department

4‧‧‧ Gear Construction

5‧‧‧Sheet Adjustment Department

6‧‧‧Winding Department

7‧‧‧Sheet

8‧‧‧Substrate

9‧‧‧Parts

10‧‧‧Laminated sheets

13‧‧‧Mixed shaft

14‧‧‧Import

15‧‧‧Spray outlet

17‧‧‧Connected tube

20‧‧‧ leaves

21‧‧‧1st casing

22‧‧‧Supply screw

24‧‧‧2nd screw

27‧‧‧First Storage Department

28‧‧‧Second Storage Department

29‧‧‧ Rear

31‧‧‧2nd casing

32‧‧‧ Gears

33‧‧‧1st gear

34‧‧‧2nd gear

45‧‧‧Spray wall

46‧‧‧ Gear spout

47‧‧‧lower side wall

48‧‧‧ upper side wall

51‧‧‧Support roll

52‧‧‧ Tension roller

53‧‧‧Winding roller

56‧‧‧Substrate feed roller

57‧‧‧Parts Laminating Roller

58‧‧‧Rotating roller

59‧‧‧Parts delivery roller

60‧‧‧Rolled sheet

63‧‧‧Protruding

70‧‧‧ material cylinder

Claims (9)

A roll-shaped sheet comprising particles and a resin component, wherein the blending ratio of the particles exceeds 30% by volume, and the sheet is wound into a roll shape. The roll-shaped sheet of claim 1, which is produced by a deformation transport step of using a gear structure including a pair of gears to cause a composition containing the particles and the resin component to be on a rotation axis of the gear And the gap passing step, after the deformation transporting step, is supported by the moving support and transporting the composition, and passing through the moving support and the moving support The gap is the opposite of the above-described gap of the disposed blade. The roll-shaped sheet of claim 2, wherein the composition having passed through the gap passing step has a shear stress of 5.0 × 10 ⁴ Pa or less in a temperature range of 50 to 250 °C. The roll-shaped sheet according to any one of claims 1 to 3, which has a width of 200 mm or more. The roll-shaped sheet according to claim 1, wherein the roll-shaped sheet is a particle-containing roll-shaped sheet, and the resin component contains an epoxy resin composition and/or a phenol resin. The roll-shaped sheet of claim 5 has a width of 200 mm or more. The roll-shaped sheet of claim 5, wherein an average value of the maximum length of the particles is 0.1 μm or more and 1000 μm or less. The roll-shaped sheet of claim 5, which has a tensile modulus at 25 ° C of 0.1 GPa or more and 20 GPa or less. The roll-shaped sheet of claim 5, wherein the sealing sheet has a thickness of 100 μm or more.