WO2014013884A1 - Film de démoulage - Google Patents

Film de démoulage Download PDF

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Publication number
WO2014013884A1
WO2014013884A1 PCT/JP2013/068396 JP2013068396W WO2014013884A1 WO 2014013884 A1 WO2014013884 A1 WO 2014013884A1 JP 2013068396 W JP2013068396 W JP 2013068396W WO 2014013884 A1 WO2014013884 A1 WO 2014013884A1
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WIPO (PCT)
Prior art keywords
release film
release
base layer
layer
resin
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PCT/JP2013/068396
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English (en)
Japanese (ja)
Inventor
裕人 谷口
Original Assignee
住友ベークライト株式会社
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Application filed by 住友ベークライト株式会社 filed Critical 住友ベークライト株式会社
Priority to CN201380037570.1A priority Critical patent/CN104507680B/zh
Priority to KR20147034756A priority patent/KR20150035596A/ko
Publication of WO2014013884A1 publication Critical patent/WO2014013884A1/fr
Priority to PH12015500100A priority patent/PH12015500100A1/en

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
    • B32B27/302—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising aromatic vinyl (co)polymers, e.g. styrenic (co)polymers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
    • B32B27/308—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising acrylic (co)polymers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/06—Interconnection of layers permitting easy separation
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J7/00—Adhesives in the form of films or foils
    • C09J7/40—Adhesives in the form of films or foils characterised by release liners
    • C09J7/405—Adhesives in the form of films or foils characterised by release liners characterised by the substrate of the release liner
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2250/00—Layers arrangement
    • B32B2250/24—All layers being polymeric
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/50—Properties of the layers or laminate having particular mechanical properties
    • B32B2307/51—Elastic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/50—Properties of the layers or laminate having particular mechanical properties
    • B32B2307/54—Yield strength; Tensile strength
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/70—Other properties
    • B32B2307/748—Releasability
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2457/00—Electrical equipment
    • B32B2457/08—PCBs, i.e. printed circuit boards
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2301/00—Additional features of adhesives in the form of films or foils
    • C09J2301/30—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier
    • C09J2301/312—Additional features of adhesives in the form of films or foils characterized by the chemical, physicochemical or physical properties of the adhesive or the carrier parameters being the characterizing feature
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2423/00—Presence of polyolefin
    • C09J2423/006—Presence of polyolefin in the substrate
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2425/00—Presence of styrenic polymer
    • C09J2425/005—Presence of styrenic polymer in the release coating
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J2425/00—Presence of styrenic polymer
    • C09J2425/006—Presence of styrenic polymer in the substrate

Definitions

  • the present invention relates to a release film.
  • This application claims priority on July 17, 2012 based on Japanese Patent Application No. 2012-155854 for which it applied to Japan, and uses the content here.
  • a cover lay film is provided so as to cover an electrical wiring formed on the surface of an insulating base material such as a polyimide resin film, thereby insulating the electrical wiring. It is illustrated.
  • This coverlay film is disposed by press laminating on an insulating substrate.
  • the press laminating method is a method in which a cover lay film is pressed against an insulating substrate or electrical wiring by pressing a heating plate, but after pressing, the heating plate is easily released from the cover lay film or insulating substrate. A release film is inserted between the hot platen and the workpiece to be processed.
  • the release film has a cushioning property for evenly transmitting pressure and heat to the coverlay film, and a shape-following property for suppressing the bleeding of the adhesive from the end surface of the coverlay film.
  • Various characteristics such as (embeddability) are required.
  • a release film As such a release film, a cushion layer containing a polyolefin resin and a polystyrene resin having a syndiotactic structure (hereinafter also referred to as SPS resin), and a mold release mainly composed of the SPS resin.
  • SPS resin polystyrene resin having a syndiotactic structure
  • the thing which has a layer is proposed (for example, refer patent document 1).
  • the release film described in Patent Document 1 when it is attempted to sufficiently secure the embedding property of the release film, the peelability (release property) between the release film and the object to be processed decreases. As a result, workability of the press laminate may be reduced.
  • An object of the present invention is to provide a release film capable of satisfying both release properties and embedding properties.
  • a base layer comprising a polyolefin resin and a polystyrene resin having a syndiotactic structure
  • a first release layer that is provided on at least one surface side of the base layer and is made of a resin material mainly composed of a polystyrene-based resin having a syndiotactic structure
  • the tensile storage modulus E ′ measured under the measurement conditions of 1 minute and a measurement frequency of 1 Hz is 1.0 ⁇ 10 6 to 5.0 ⁇ 10 8 Pa at 120 ° C., and 1.0 ⁇ 10 7 to 170 ° C.
  • a second release layer that is provided on the surface of the base layer opposite to the first release layer and is made of a resin material mainly composed of a polystyrene resin having a syndiotactic structure.
  • the release film according to any one of (1) to (7) above.
  • FIG. 3 is a graph showing temperature dependence of tensile storage modulus E ′ measured for release films obtained in Examples 1 to 4.
  • FIG. 1 is a cross-sectional view showing an embodiment of a release film of the present invention.
  • a release film 1 shown in FIG. 1 is a laminate having a base layer 2 and a first release layer 3 provided on the base layer 2.
  • the base layer 2 contains a polyolefin resin and a polystyrene resin having a syndiotactic structure.
  • the 1st mold release layer 3 is comprised with the resin material which has as a main component the polystyrene-type resin which has a syndiotactic structure.
  • the release film 1 has a tensile storage modulus E ′ of 1.0 ⁇ 10 6 to 5.0 ⁇ 10 8 Pa at 120 ° C. measured by a method based on a test method defined in JIS K 7244. Yes, and configured to be 1.0 ⁇ 10 7 to 1.0 ⁇ 10 9 Pa at 170 ° C.
  • a release film 1 press laminates a coverlay film on an insulating substrate on which an electrical wiring is formed, for example, between the heating plate and the coverlay film (in a portion where the coverlay film is interrupted, Between the board and the insulating substrate).
  • the release film 1 can suppress deterioration of the release property while ensuring sufficient embedding property. That is, according to this invention, the release film 1 which can make embedding property and release property compatible is obtained.
  • the base layer 2 supports the first release layer 3 and imparts cushioning properties to the release film 1.
  • the constituent material of the base layer 2 is a resin mixture (resin blend) containing a polyolefin resin and a polystyrene resin having a syndiotactic structure.
  • resin mixture resin blend
  • polyolefin resin and the polystyrene resin having a syndiotactic structure will be sequentially described.
  • Polyolefin resin Since the polyolefin-based resin has a relatively high flexibility, it contributes to improving the cushioning property of the release film 1.
  • polystyrene resin examples include ethylene, propylene, 1-butene, isobutene, 1-pentene, 2-methyl-1-butene, 3-methyl-1-butene, 1-hexene and 3-methyl.
  • ⁇ -olefins such as 1-pentene, 4-methyl-1-pentene, 1-heptene, 1-octene, 1-decene, 1-dodecene, 1-tetradecene, 1-hexadecene, 1-octadecene, 1-icocene Homopolymers of the above, copolymers of at least two types of ⁇ -olefins, copolymers of ⁇ -olefins and other monomers, and the like. Good.
  • Other monomers are those copolymerizable with ⁇ -olefins, for example, unsaturated carboxylic acids such as acrylic acid and methacrylic acid, and unsaturated carboxylic acid esters such as acrylic acid esters and methacrylic acid esters.
  • Polybasic unsaturated carboxylic acids such as maleic acid, polybasic unsaturated carboxylic acid anhydrides, 1,3-butadiene, isoprene, 1,3-pentadiene, 1,3-hexadiene, dicyclopentadiene
  • Non-conjugated dienes such as conjugated dienes, dicyclopentadiene, 1,4-hexadiene, 1,9-decadiene, cyclooctadiene, norbornadiene, methylene norbornene, ethylidene norbornene, 7-methyl-1,6-octadiene, etc. Can be mentioned.
  • polyolefin resins include linear high density polyethylene, linear low density polyethylene, various polyethylenes such as high pressure method low density polyethylene, isotactic polypropylene, syndiotactic polypropylene, block polypropylene, Examples include various polypropylenes such as random polypropylene, ethylene-vinyl acetate copolymer (EVA), ethylene-methyl methacrylate copolymer (EMMA), and one or a mixture of two or more of ethylene-styrene copolymers. It is done.
  • EVA ethylene-vinyl acetate copolymer
  • EMMA ethylene-methyl methacrylate copolymer
  • the polyolefin resin is preferably any one of polypropylene, ethylene-methyl methacrylate copolymer, and ethylene-styrene copolymer, and more preferably a mixture of two or more of these.
  • the mechanical properties of the base layer 2 are optimized, and as a result, the tensile storage elastic modulus E ′ of the release film 1 at a predetermined temperature can be optimized.
  • polypropylene examples include a propylene homopolymer and a copolymer of propylene and an ⁇ -olefin having 2 to 20 carbon atoms other than propylene.
  • the polypropylene preferably has a melting point measured by a suggestive scanning calorimeter of 140 ° C. or higher, more preferably 150 to 170 ° C. Heat resistance can be imparted to the release film 1 by using such polypropylene.
  • the polypropylene preferably has a melt flow rate (MFR) measured at a load of 2.16 kg and a temperature of 230 ° C. of 0.1 to 2 g / 10 minutes, preferably 0.3 to 1.5 g / 10 minutes. Some are more preferred.
  • MFR melt flow rate
  • the ethylene-methyl methacrylate copolymer preferably contains 5 to 50% by mass of units derived from methyl methacrylate, more preferably 8 to 35% by mass.
  • the ethylene-methyl methacrylate copolymer preferably has a melt flow rate (MFR) measured at a load of 2.16 kg and a temperature of 190 ° C. of 0.25 to 50 g / 10 minutes, preferably 0.5 to What is 10 g / 10min is more preferable.
  • MFR melt flow rate
  • the ethylene-styrene copolymer may be any copolymer as long as it is a copolymer of a polyethylene structural unit and a polystyrene structural unit.
  • a copolymer By using such a copolymer, the affinity with the polystyrene resin having the syndiotactic structure contained in the base layer 2 and the polystyrene resin having the syndiotactic structure contained in the first release layer 3 is improved. To do. As a result, the mechanical strength of the base layer 2 can be improved and the adhesion between the base layer 2 and the first release layer 3 can be improved.
  • the ethylene-styrene copolymer is preferably a copolymer having a main chain composed of polyethylene structural units and a side chain composed of polystyrene structural units.
  • Such an ethylene-styrene copolymer has a polystyrene structural unit in the side chain, so that the above effect becomes more remarkable.
  • ethylene-styrene copolymer a copolymer having a polystyrene structural unit mass ratio of 5 to 15% by mass is preferably used.
  • a copolymer having a polystyrene structural unit mass ratio of 5 to 15% by mass is preferably used.
  • the mechanical strength of the base layer 2 and the adhesion between the base layer 2 and the first release layer 3 can be further enhanced.
  • the mass ratio of the polystyrene structural unit is lower than the lower limit, the affinity between the ethylene-styrene copolymer and the polystyrene resin having a syndiotactic structure is lowered. Therefore, the mechanical strength of the base layer 2 may be reduced, or the adhesion between the base layer 2 and the first release layer 3 may be reduced.
  • the mass ratio of the polystyrene structural unit in the ethylene-styrene copolymer can be calculated based on, for example, a peak integral value in a 1 H-NMR spectrum obtained by NMR analysis.
  • the NMR analyzer for example, a JNM-ECA400 superconducting FT-NMR apparatus manufactured by JEOL Ltd. is used.
  • the measurement nucleus is 1 H, 13 C
  • the measurement temperature is 125 ° C.
  • the measurement solvent is deuterated 1,2-dichlorobenzene
  • the number of integration is 16 for 1 H, 16384 for 13 C
  • the repetition waiting time is 1 H can be 5 seconds and 13 C can be 2 seconds.
  • the reference peak can be set to the peak of the measurement solvent
  • 1 H can be set to 7.40 ppm as an internal reference
  • 13 C can be set to 127.70 ppm as an internal reference.
  • a polystyrene-based resin (SPS resin) having a syndiotactic structure has a stereoregular structure (syndi) in which phenyl groups and substituted phenyl groups as side chains are alternately located in opposite directions with respect to the main chain composed of carbon-carbon sigma bonds. It is a resin having an tactic structure.
  • SPS resin used for the base layer 2 examples include those described in JP-A No. 2000-038461. Specifically, 75% or more, preferably 85% or more of racemic dyad, or 30% or more, preferably 50% or more of syndiotacticity of racemic pentad, polystyrene, poly (alkylstyrene), poly ( Aryl styrene), poly (halogenated styrene), poly (halogenated alkyl styrene), poly (alkoxy styrene), poly (vinyl benzoate), hydrogenated polymers thereof and mixtures thereof, or these as main components And the like.
  • poly (alkyl styrene) examples include poly (methyl styrene), poly (ethyl styrene), poly (isopropyl styrene), poly (t-butyl styrene), and the like.
  • poly (aryl styrene) examples include poly (phenyl styrene), poly (vinyl naphthalene), and poly (vinyl styrene).
  • poly (halogenated styrene) examples include poly (chlorostyrene), poly (bromostyrene), poly (fluorostyrene), and the like.
  • poly (halogenated alkylstyrene) examples include poly (chloromethylstyrene).
  • poly (alkoxystyrene) examples include poly (methoxystyrene) and poly (ethoxystyrene).
  • polystyrene poly (p-methylstyrene), poly (m-methylstyrene), poly (pt-butylstyrene), poly (p-chlorostyrene), poly (m-chlorostyrene) are particularly preferable.
  • Poly (p-fluorostyrene), hydrogenated polystyrene, and copolymers containing these structural units are preferably used.
  • Examples of other resins include various elastomer resins, polyester resins, polyamide resins, polyphenylene ether resins, polyphenylene sulfide resins, and the like, and one or a mixture of two or more of these are used.
  • elastomer resin for example, those described in JP 2011-161749 A are preferably used.
  • polyester-based resin examples include polycarbonate, polyethylene terephthalate, polybutylene terephthalate, and the like.
  • examples of the polyamide-based resin include nylon 6, nylon 66, and the like.
  • additives include an antiblocking agent, an antioxidant, a nucleating agent, an antistatic agent, a process oil, a plasticizer, a release agent, a flame retardant, and the like as described in JP-A-2011-161749.
  • flame retardant aids, pigments, etc. and one or a mixture of two or more of these is used.
  • antiblocking agent for example, those described in JP 2011-161749 A are preferably used.
  • antioxidants examples include phosphorus antioxidants, phenolic antioxidants, sulfur antioxidants, and the like.
  • nucleating agent examples include metal salts of carboxylic acids such as aluminum di (pt-butylbenzoate); metal salts of phosphoric acid such as methylene bis (2,4-di-tert-butylphenol) acid phosphate sodium.
  • Polyhydric alcohol derivatives such as dibenzylidene sorbitol, bis (methylbenzylidene) sorbitol, bis (p-ethylbenzylidene) sorbitol, bis (dimethylbenzylidene) sorbitol; N, N ′, N ′′ -tris [2-methylcyclohexyl] -1,2,3-propanetricarboxamide, N, N ', N "-tricyclohexyl 1,3,5-benzenetricarboximide, N, N'-dicyclohexyl-naphthalenedicarboxamide, 1,3,5- Of tri (dimethylisopropoylamino) benzene Una amide compound; talc, phthalocyanine derivatives and the like, and these can be used singly or in combination of two or more of them.
  • plasticizer examples include polyethylene glycol, polyamide oligomer, ethylene bisstearoamide, phthalate ester, polystyrene oligomer, polyethylene wax, silicone oil, etc., and one or more of these are combined. Can be used.
  • examples of the release agent include polyethylene wax, silicone oil, long chain carboxylic acid, long chain carboxylic acid metal salt, and the like, and one or more of them can be used in combination.
  • examples of the process oil include paraffinic oil, naphthenic oil, and aroma oil.
  • the amount of each of these additives is not particularly limited, but is preferably about 0.01 to 15 parts by mass, and 0.05 to 10 parts by mass with respect to 100 parts by mass in total of the polyolefin resin and the SPS resin. More preferably, it is about a part.
  • First release layer For example, when the coverlay film is press-laminated on an insulating substrate on which electrical wiring is formed, the first release layer 3 prevents adhesion between the release film 1 and the object to be processed and provides good release properties.
  • the constituent material of the first release layer 3 is a resin material mainly composed of the SPS resin described above.
  • the SPS resin included in the first release layer 3 and the SPS resin included in the base layer 2 may have different compositions, but are preferably configured to include the same composition. Thereby, the adhesiveness of the base layer 2 and the 1st mold release layer 3 can be improved. As a result, it is possible to prevent delamination between the base layer 2 and the first release layer 3 when the release film 1 is peeled after press lamination.
  • the average thickness of the first release layer 3 is not particularly limited, but is preferably 5 to 100 ⁇ m, and more preferably 10 to 80 ⁇ m. By making the thickness of the first release layer 3 within the above range, sufficient embedding property can be imparted to the release film 1 while ensuring the adhesion between the base layer 2 and the first release layer 3. it can.
  • the ratio of the SPS resin in the first release layer 3 is preferably 70% by mass or more, and more preferably 80% by mass or more. By setting the ratio of the SPS resin in the first release layer 3 within the above range, the release film 1 has good release properties.
  • FIG. 2 is a cross-sectional view showing another embodiment of the release film of the present invention.
  • the release film 1 shown in FIG. 2 will be described.
  • differences from FIG. 1 will be mainly described, and description of similar matters will be omitted.
  • the release film 1 shown in FIG. 2 has the second release layer 4 provided on the surface opposite to the surface on which the first release layer 3 of the base layer 2 is provided, except for the release film shown in FIG. The same as film 1.
  • the second release layer 4 for example, when the coverlay film is press-laminated on the insulating substrate on which the electrical wiring is formed, the releasability between the hot platen and the coverlay film can be improved.
  • the intermediate member is interposed between the hot platen and the cover lay film, the releasability between the intermediate member and the cover lay film can be enhanced. As a result, adhesion between the hot platen or the intermediate member and the release film 1 can be suppressed, and the workability of press lamination can be further improved.
  • the total thickness (average thickness) of the release film 1 is preferably about 20 to 300 ⁇ m, and more preferably about 20 to 200 ⁇ m.
  • the release film 1 having the above layer structure has an appropriate cushioning property.
  • This cushioning property influences the embedding property and releasing property of the release film 1, and is an important characteristic for the release film 1 to perform its function. Specifically, for example, when the release film 1 is subjected to press lamination, it is heated to a predetermined temperature. The release film 1 is softened with heating, and easily follows the surface shape of the object to be processed for press lamination. This phenomenon imparts embedding property to the release film 1, while causing the release property to deteriorate.
  • embedding property and releasability are characteristics that can be contradicted in principle. Therefore, it has been insufficient so far to achieve both of these characteristics, particularly when a press laminate is applied to a workpiece having a complicated surface shape.
  • the present inventor has intensively studied the conditions for achieving both embeddability and releasability.
  • the tensile storage elastic modulus E ′ of the release film 1 on the low temperature side is 1.0 ⁇ 10 6 to 5.0 ⁇ 10.
  • the tensile storage elastic modulus E ′ of the release film 1 on the high temperature side (170 ° C.) is 1.0 ⁇ 10 7 to 1.0 ⁇ 10 9 Pa at 8 Pa, the release film 1 is embedded.
  • the present invention has been completed by finding that the properties and releasability can be highly compatible.
  • the release film 1 satisfying such conditions is optimized for cushioning from the low temperature side to the high temperature side in the temperature rising process in the press laminating process and the like, and can be highly compatible with embedding property and mold release property. . Therefore, for example, when the coverlay film is press-laminated on the insulating substrate on which the electrical wiring is formed, it is possible to improve the release workability while suppressing the bleeding of the adhesive from the end face of the coverlay film. As a result, a high-quality FPC can be efficiently manufactured.
  • the tensile storage elastic modulus E ′ of the release film 1 is measured by a method based on the test method specified in JIS K 7244.
  • the measurement conditions were as follows: test piece length 40 mm, test piece width 4 mm, test piece length 20 mm between clamps for fixing the test piece, measurement start temperature 25 ° C., measurement end temperature 250 ° C., heating rate 5
  • the measurement frequency is 1 ° C./min.
  • the tensile storage elastic modulus E ′ at 120 ° C. is set to the above-described value on the low temperature side
  • the tensile storage elastic modulus E ′ at 170 ° C. is set to the above-described value on the high temperature side.
  • the tensile storage elastic modulus E ′ of the release film 1 at 120 ° C. is preferably 3.0 ⁇ 10 6 to 3.0 ⁇ 10 8 Pa, more preferably 7.0 ⁇ 10 6 to 7.0 ⁇ . 10 7 Pa.
  • the tensile storage elastic modulus E ′ of the release film 1 at 170 ° C. is preferably 2.0 ⁇ 10 7 to 5.0 ⁇ 10 8 Pa, more preferably 3.0 ⁇ 10 7 to 3.0 ⁇ . 10 8 Pa.
  • the tensile storage elastic modulus E ′ of the release film 1 is preferably 1.0 ⁇ 10 6 to 5.0 ⁇ 10 8 Pa in the temperature range of 120 to 145 ° C., and preferably 3.0 ⁇ 10 6 to 3.0 ⁇ 10 8 Pa is more preferable, and 5.0 ⁇ 10 6 to 7.0 ⁇ 10 7 Pa is even more preferable.
  • the tensile storage modulus E ′ of the release film 1 at 185 ° C. which is higher than 170 ° C., is preferably 8.0 ⁇ 10 6 to 5.0 ⁇ 10 8 Pa, more preferably 1. 5 ⁇ 10 7 to 5.0 ⁇ 10 8 Pa, more preferably 2.0 ⁇ 10 7 to 3.0 ⁇ 10 8 Pa. If the tensile storage elastic modulus E ′ of the release film 1 at 185 ° C. is within the above range, the embedding property of the release film can be further improved. Therefore, the embedding property and the releasability can be made highly compatible. For example, even when the height difference of the surface of the FPC is large, it is possible to manufacture a high-quality FPC and prevent the workability of the press laminate from being lowered. .
  • the average thickness of the base layer 2 is not particularly limited, but is preferably about 10 to 200 ⁇ m, more preferably about 15 to 150 ⁇ m, and further preferably about 20 to 120 ⁇ m. By making the thickness of the base layer 2 within the above range, it is possible to suppress the deterioration of the mold release property while ensuring the sufficient embedding property of the mold release film 1. In addition, when the average thickness of the base layer 2 is less than the said lower limit, the adhesive force of the base layer 2 with respect to the 1st release layer 3 will fall.
  • the release film 1 when the release film 1 is peeled after press laminating a coverlay film on an insulating substrate on which electrical wiring is formed, there is a possibility that delamination may occur between the base layer 2 and the first release layer 3. is there. Moreover, when the average thickness of the base layer 2 is less than the said lower limit, there exists a possibility that the embedding property of the release film 1 may fall. On the other hand, when the average thickness of the base layer 2 exceeds the upper limit, the embedding property of the release film 1 becomes excessive, and the release property of the release film 1 may be lowered.
  • the average thickness of the base layer 2 is preferably 1.5 times or more, more preferably 2 to 10 times, more preferably 2.5 to 7 times the average thickness of the first release layer 3. Is more preferable.
  • the ratio of the SPS resin in the base layer 2 is preferably smaller than the ratio of the polyolefin resin. Specifically, it is preferably about 2 to 40% by mass, more preferably about 3 to 35% by mass. Thereby, sufficient embedding property can be imparted to the release film 1 while ensuring the adhesion between the base layer 2 and the first release layer 3.
  • the ratio of the polyolefin-based resin is preferably about 60 to 98% by mass, and more preferably about 65 to 97% by mass.
  • the ethylene-styrene copolymer is preferably set to be larger.
  • the mass ratio of the ethylene-styrene copolymer is preferably about 1.05 to 2.5 times the mass ratio of polypropylene, more preferably about 1.1 to 2 times.
  • the amount of the ethylene-methyl methacrylate copolymer is preferably increased.
  • the mass ratio of the ethylene-methyl methacrylate copolymer is preferably about 1.05 to 2.5 times, more preferably about 1.1 to 2 times the mass ratio of polypropylene.
  • the ethylene-styrene copolymer and the ethylene-methyl methacrylate copolymer are each preferably set to be larger than the SPS resin.
  • the mass ratio of the ethylene-styrene copolymer and the ethylene-methyl methacrylate copolymer is preferably about 1.05 to 2.5 times the mass ratio of the SPS resin. More preferably, it is about double.
  • the cushioning property of the base layer 2 is optimized, so that the embedding property and the releasability of the release film 1 can be made more highly compatible.
  • the base layer 2 contains, for example, SPS resin, polypropylene, ethylene-methyl methacrylate copolymer (EMMA) and ethylene-styrene copolymer
  • the ratio of SPS resin is 2 to 40 parts by mass
  • the ratio of polypropylene is 3 to It is preferable to set 40 parts by mass, the ratio of ethylene-methyl methacrylate copolymer to 10 to 50 parts by mass, and the ratio of ethylene-styrene copolymer to 10 to 50 parts by mass, respectively.
  • the release film 1 shown in FIG. 1 can be produced by a coextrusion method or an extrusion lamination method.
  • FIG. 3 is a diagram for explaining an example of a method for producing the release film 1.
  • the release film 1 is manufactured by extruding the raw material of the base layer 2 and the raw material of the first release layer 3 simultaneously using a feed block and a multi-manifold die.
  • the raw material of the base layer 2 and the raw material of the first release layer 3 are each melt-kneaded by a known method, and granulated or pulverized as necessary to obtain a melt.
  • a blender such as a V blender, a ribbon blender, a Henschel hexar, or a tumbler blender, a single screw extruder, a twin screw extruder, a kneader, a Banbury mixer, or the like is used.
  • the melt that is the raw material of the base layer 2 and the melt that is the raw material of the first release layer 3 are simultaneously extruded in layers from the die 210.
  • a single screw extruder, a twin screw extruder, or the like is used for this extrusion.
  • the extruded melt M is guided between the first roll 230 and the touch roll 220, and until the melt M is separated from the first roll 230, the melt M is pushed by the touch roll 220 and the first roll 230. To be cooled. Thereby, the release film 1 is obtained.
  • the manufactured release film 1 is sent to the downstream side in the film feeding direction (see the arrow in FIG. 3) by the second roll 240 and is finally taken up by a take-up roll (not shown).
  • the temperature of the first roll 230 is preferably about 30 to 100 ° C.
  • the temperature of the touch roll 220 is preferably about 50 to 120 ° C.
  • the temperature of the second roll 240 relative to the first roll 230 is The peripheral speed ratio is preferably about 0.990 to 0.998.
  • the release film 1 is manufactured by extruding the raw material of the base layer 2 and the raw material of the first release layer 3 and then laminating them.
  • the temperature of the extruder cylinder is set to 270 to 300 ° C., and the melt as the raw material of the first release layer 3 is extruded in layers, and as shown in FIG. 3, the first roll 230 and the touch roll Lead to 220.
  • the induced melt M is cooled by the touch roll 220 and the first roll 230 until the melt M is separated from the first roll 230. Thereby, the release layer film 30 is obtained.
  • the melt which is the raw material of the base layer 2
  • the release layer film 30 (not shown).
  • the release film 1 is obtained by cooling this.
  • the manufactured release film 1 is finally wound up on a winding roll (not shown).
  • the tensile storage elastic modulus E ′ of the release film 1 can be appropriately adjusted by changing the cooling rate of the melt that is the raw material of the base layer 2 and the first release layer 3.
  • the cooling rate is appropriately set according to the composition and thickness of the base layer 2, the composition and thickness of the first release layer 3, the layer configuration of the release film 1, and the like. For example, it is preferably set to about 0.1 to 20 ° C./second, more preferably about 0.3 to 15 ° C./second.
  • the crystallinity of the crystalline resin eg, SPS resin, polypropylene, etc.
  • the crystallinity of the crystalline resin eg, SPS resin, polypropylene, etc.
  • the crystallinity of the crystalline resin contained in the base layer 2 and the first release layer 3 is reduced, or the crystal size is reduced, and the mold release
  • the tensile storage elastic modulus E ′ of the film 1 is lowered.
  • the crystallinity of the crystalline resin contained in the base layer 2 and the first release layer 3 is increased, or the crystal size is increased, and the tensile storage modulus E of the release film 1 is increased. 'Will rise.
  • the crystallinity of the constituent material of the base layer 2 and the first release layer 3 is preferably 5 to 50%, more preferably 10 to 40%, as measured by a differential scanning calorimeter (DSC). preferable.
  • DSC differential scanning calorimeter
  • the tensile storage elastic modulus E ′ of the release film 1 on the low temperature side (120 ° C.) and the tensile storage elastic modulus E ′ of the release film 1 on the high temperature side (170 ° C.) are respectively the base layer 2 and the first release layer. It can adjust suitably by changing the composition of 3.
  • the ratio of resins having a softening point (melting point or glass transition point) close to 170 ° C. hereinafter referred to as “high softening point resin” is increased and the softening point is close to 120 ° C.
  • the tensile storage modulus E ′ of the release film 1 By lowering the ratio of the resin (hereinafter referred to as “low softening point resin”), the characteristics occupied by the high softening point resin in the tensile storage modulus E ′ of the release film 1 become more obvious. As a result, the tensile storage modulus E ′ on the high temperature side can be selectively adjusted. Similarly, the tensile storage modulus E ′ on the low temperature side can be selectively adjusted by decreasing the ratio of the high softening point resin and increasing the ratio of the low softening point resin. In this way, the release film 1 having the tensile storage elastic modulus E ′ on the low temperature side and the high temperature side within the above ranges can be produced.
  • the tensile storage elastic modulus E ′ can also be adjusted by adding the above-described additives to the base layer 2 and the first release layer 3.
  • a step of adjusting the crystallinity of the SPS resin or polyolefin resin of the release film 1 obtained as described above may be provided.
  • the crystallinity can be adjusted, for example, by subjecting the release film 1 to heat treatment. Specifically, a method of heat-setting the release film 1 in a drier using a tenter device or a method of heat-treating at about 50 to 220 ° C. using a heat treatment roll can be mentioned.
  • the manufacturing method of the release film 1 is not limited to the above-mentioned thing, Other methods may be used.
  • FIG. 4 is a diagram for explaining an example of use of the release film 1.
  • the release film 1 according to the present invention is, for example, when a coverlay film is press-laminated on a surface having an elevation difference of an insulating substrate on which electric wiring is formed (between a hot platen and a coverlay film). In the interrupted portion, it is inserted between the hot platen and the insulating substrate) and used to ensure the release property after press lamination.
  • an unbonded body 340 having a coverlay film temporarily fixed on an insulating substrate on which electrical wiring is formed is sandwiched between two release films 1. Further, these are sandwiched between two fluororesin sheets 330, two rubber cushions 320, and two stainless steel plates 310. And these are pressed with the hot platen 300 as shown by the arrow in FIG.
  • FIG. 5 is a diagram showing an example of a temperature profile in press lamination. Note that the origin of the horizontal axis of the temperature profile corresponds to the time when the object to be processed is started to be pressed by the heating plate 300.
  • the temperature of the hot platen 300 is rapidly raised from room temperature to 185 ° C. within 10 seconds after starting to pressurize the workpiece, and then maintained at that temperature for 60 seconds. Thereafter, when pressurization of the object to be processed by the hot platen 300 is finished, press lamination is completed.
  • the press pressure of the object to be processed by the hot platen 300 is preferably set to about 5 to 15 MPa.
  • the release film 1 In press laminating, the release film 1 is deformed so as to be embedded along the end face of the coverlay film, so that bleeding of the adhesive from the end face of the coverlay film is suppressed.
  • the base layer 2 since the base layer 2 has appropriate mechanical properties, the release film 1 is quickly separated from the end face of the coverlay film when the applied pressure is released after press lamination. Thereby, the embedding property and release property of the release film 1 in the press laminate can be made compatible, and the workability of the press laminate can be improved.
  • the bleeding of the adhesive is prevented at the portion where the cover lay film is interrupted, the electrical wiring can be surely exposed at the portion to achieve electrical connection.
  • the fluororesin sheet 330, the rubber cushion 320, and the stainless steel plate 310 may be omitted.
  • the release film 1 may be used for the purpose of separating the molding die and the member so as not to adhere to each other when the member is molded, in addition to the above-described use examples.
  • release film for FRP (Fiber Reinforced Plastics) and CFRP (Carbon Fiber Reinforced Plastics) molding release film for advanced composite materials (ACM: Advanced Composites Material), release film for rubber sheet curing, epoxy and phenolic It can be used as a release film for semiconductor sealing materials such as, a release film for special adhesive tape, and the like.
  • the present invention is intermediate between the base layer 2 and the first release layer 3 and between the base layer 2 and the second release layer 4. You may make it interpose a layer.
  • the intermediate layer is used, for example, for the purpose of increasing the adhesion between the layers, and specifically includes an anchor layer, a primer layer, and the like.
  • Example 1 Production of release film (Example 1) (1) Raw materials for first release layer and second release layer First, SPS resins (Zarek S104 manufactured by Idemitsu Kosan Co., Ltd.) were prepared as raw materials for the first release layer and the second release layer.
  • SPS resins Zarek S104 manufactured by Idemitsu Kosan Co., Ltd.
  • Base layer raw materials The following resins were prepared as base layer raw materials.
  • the polyolefin resin is a mixture of a plurality of resins, and the breakdown is as follows.
  • the ethylene-methyl methacrylate copolymer is represented as EMMA, the ethylene-styrene copolymer as AD, and the polypropylene as PP.
  • EMMA Suditomo Chemical Co., Ltd. ACLIFT WD106
  • AD Mitsubishi Chemical Co., Ltd. Modic F502
  • PP Part 1 of PP
  • the methyl methacrylate derived unit content in EMMA is 5% by mass, and the melt flow rate is 2 g / 10 min.
  • the polyethylene structural unit content rate in AD is 91.4 mass%
  • the polystyrene structural unit content rate is 8.6 mass%
  • the melt flow rate is 1 g / 10 min.
  • the melt flow rate of PP is 0.5 g / 10 minutes.
  • the raw materials were simultaneously extruded so that the first release layer, the base layer, and the second release layer were laminated to produce a release film.
  • the temperature of the raw material melt was 285 ° C., respectively.
  • the apparatus shown in FIG. 3 is used, the temperature of the first roll 230 is 30 ° C., the temperature of the touch roll 220 is 70 ° C., and the peripheral speed ratio of the second roll 240 to the first roll 230. was set to 0.990.
  • the peripheral speed etc. of each roll were adjusted so that the cooling rate of a release film might be 5 degree-C / sec.
  • the total thickness (average thickness) of the produced release film was 120 ⁇ m.
  • the average thickness of the base layer was 70 ⁇ m, and the average thickness of the first release layer and the second release layer was 25 ⁇ m.
  • Example 2 A release film was produced in the same manner as in Example 1 except that the layer configuration and production conditions of the release film were changed as shown in Table 1.
  • N, N ′, N ′′ -tris [2-methylcyclohexyl] -1,2,3-propanetricarboxamide was used as the nucleating agent.
  • FIG. 6 is a graph showing the temperature dependence of the tensile storage modulus E ′ measured for the release films obtained in Examples 1 to 4.
  • a coverlay film was formed on an insulating substrate (FPC) on which an electrical wiring having an L / S of 150/150 ⁇ m was formed. Press laminated.
  • press lamination stainless steel plate, rubber cushion, fluororesin sheet, release film, coverlay film, FPC, release film, fluororesin sheet, rubber cushion, stainless steel are stacked in this order, and this is a one-stage press Pressed by machine.
  • pressing the temperature was raised to 185 ° C. at a rate of temperature rise of 10 ° C./min while being pressurized at a pressure of 10 MPa, then held for 1 minute, and then cooled to room temperature. This obtained the sample which carried out the press lamination of the coverlay film on FPC.
  • the embedding property of the coverlay film was evaluated for the obtained sample.
  • the extent of the coverlay film adhesive exuding from the end face is determined by “7.5. Of JPCA Standard, Single-sided and Double-sided Flexible Printed Circuit Board JPCA-DG02 issued by the Japan Electronic Circuits Association.
  • the evaluation was made based on the following evaluation criteria.
  • the release film obtained in each example can achieve both embedding and release properties when the cover lay film is press-laminated on the insulating substrate.
  • the release film obtained in each example by optimizing the layer structure of the base layer, even when press laminating a coverlay film on a rough surface, according to the release film obtained in each example, embedding and releasing properties It was recognized that the above can be made highly compatible.
  • the present invention it is possible to obtain a release film that can achieve both release properties and embedding properties by optimizing the structure of the base layer. Therefore, the present invention can be suitably used for a release film and is extremely important in industry.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Laminated Bodies (AREA)

Abstract

La présente invention concerne un film de démoulage ayant à la fois des propriétés de démoulage et une performance d'incorporation. Le film de démoulage (1) selon la présente invention comprend : une couche de base (2) qui comprend une résine de polyoléfine et une résine de polystyrène ayant une structure syndiotactique ; et une première couche de démoulage (3) qui est disposée sur la surface supérieure de la couche de base (2) et est composée d'une matière de résine contenant une résine de polystyrène ayant une structure syndiotactique comme composant principal. Le film de démoulage (1) a un module élastique de stockage à la traction (E') de 1,0 × 106 à 5,0 × 108 Pa à 120°C et 1,0 x 107 à 1,0 × 109 Pa à 170°C tel que mesuré par une méthode d'essai conformément à JIS K 7244 dans des conditions telles que la longueur d'une pièce d'essai est de 40 mm, la largeur de la pièce d'essai est de 4 mm, la longueur de la pièce d'essai entre des pinces est de 20 mm, la température de départ de mesure est de 25°C, la température de fin de mesure est de 250°C, la vitesse d'élévation de température est de 5°C/min, et la fréquence de mesure est de 1 Hz.
PCT/JP2013/068396 2012-07-17 2013-07-04 Film de démoulage WO2014013884A1 (fr)

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PH12015500100A PH12015500100A1 (en) 2012-07-17 2015-01-14 Mold release film

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JP6398221B2 (ja) * 2014-02-26 2018-10-03 住友ベークライト株式会社 樹脂封止半導体装置製造用離型フィルム、樹脂封止半導体装置製造用離型フィルムの製造方法及び樹脂封止半導体装置の製造方法
JP6303727B2 (ja) * 2014-03-31 2018-04-04 住友ベークライト株式会社 離型フィルム
JP6467800B2 (ja) * 2014-07-30 2019-02-13 住友ベークライト株式会社 離型フィルム
JP6648400B2 (ja) * 2014-11-10 2020-02-14 凸版印刷株式会社 端子用樹脂フィルム、それを用いたタブ及び蓄電デバイス
CN110461594B (zh) * 2017-03-22 2021-02-12 住友电木株式会社 脱模膜及挠性印刷电路基板的制造方法
EP3904090A4 (fr) * 2018-12-28 2022-09-14 Kuraray Co., Ltd. Film de base pour film décoratif et film décoratif le comprenant
JP7281381B2 (ja) * 2019-10-04 2023-05-25 出光興産株式会社 低誘電材用樹脂積層体
CN114080866B (zh) * 2020-10-21 2022-09-16 住友电木株式会社 脱模膜及成型品的制造方法
CN113924825B (zh) * 2020-10-21 2022-10-25 住友电木株式会社 脱模膜及成型品的制造方法
JP6870775B1 (ja) * 2020-10-21 2021-05-12 住友ベークライト株式会社 離型フィルムおよび成型品の製造方法

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JP5895755B2 (ja) 2016-03-30
PH12015500100A1 (en) 2015-03-02
TW201406518A (zh) 2014-02-16
CN104507680A (zh) 2015-04-08
CN104507680B (zh) 2016-10-19
TWI554375B (zh) 2016-10-21
JP2014019017A (ja) 2014-02-03

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