Classifications

• • 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
• • 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
  • C09J125/00—Adhesives based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring; Adhesives based on derivatives of such polymers
  • C09J125/02—Homopolymers or copolymers of hydrocarbons
  • C09J125/04—Homopolymers or copolymers of styrene
  • C09J125/08—Copolymers of styrene
  • C09J125/10—Copolymers of styrene with conjugated dienes
• • 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
  • C09J153/00—Adhesives based on block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Adhesives based on derivatives of such polymers
  • C09J153/02—Vinyl aromatic monomers and conjugated dienes
• • 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
  • C09J163/00—Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
• • 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
  • C09J163/00—Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
  • C09J163/10—Epoxy resins modified by unsaturated compounds

Definitions

• the present invention relates to an adhesive composition. More specifically, the present invention relates to an adhesive composition that can be used for adhesive applications such as electronic components.
• FPC flexible printed wiring board
• a base material having a small loss even in the millimeter wave band of 28 GHz in order to efficiently transmit signals having frequencies in the 3.5 GHz and 28 GHz bands used in the 5th generation mobile communication system (hereinafter, also referred to as 5G), a base material having a small loss even in the millimeter wave band of 28 GHz. Films and adhesives are becoming more important.
• the low-dielectric adhesive has poor reactivity with the curing agent because the main agent molecule has few reactive groups. Further, when an epoxy resin is used as the curing agent, the dielectric loss tangent tends to be high. Due to these factors, it is extremely difficult to achieve both curability and low dielectric resistance, which affect the adhesiveness, heat resistance, and chemical resistance (solvent resistance) of the adhesive composition.
• the present invention exhibits good adhesion to a low-dielectric base film having poor adhesion while having good electrical characteristics (dielectric characteristics) compatible with 5G, and has heat resistance and chemical resistance (resistance to chemicals). It is an object of the present invention to provide an adhesive composition for forming a low-dielectric adhesive layer having a solvent-like property.
• the present invention includes the following aspects.
• R 1 , R 2 , R 3 and R 4 independently represent hydrogen or an organic group, respectively. However, at least one of R 1 and R 2 is an organic group, and R 3 and R 4 have an organic group. At least one of them is an organic group.
• R 5 and R 6 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 5 in the formula (2) may be the same or different
• R 6 in each formula (2) may be the same or different. * Represents a binding group. .)
• [7] The adhesive composition according to any one of [1] to [6], wherein the epoxy-modified resin contains an unsaturated bond other than an aromatic ring.
• [8] The adhesive composition according to [7], wherein the epoxy-modified resin has a structure represented by the following formula (3).
• R 7 and R 8 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 7 in the formula (3) may be the same or different, and R 8 in each formula (3) may be the same or different.
• * represents a binding group. .) [9] Any of [1] to [8], wherein the epoxy-modified resin has at least one of a structure represented by the following formula (4) and a structure represented by the following formula (5).
• the adhesive composition according to. (R 9 and R 10 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 9 in the formula (4) may be the same or different, and R 10 in each formula (4) may be the same or different.
• * Represents a binding group. .) R 11 and R 12 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms. When a plurality of structures represented by the formula (5) are present in the epoxy-modified resin, R 11 in each formula (5) may be the same or different, and each formula (5) may be different. R 12 in) may each be the same or different.
• [15] The adhesive composition according to any one of [1] to [14], wherein the epoxy-modified resin has a weight average molecular weight (Mw) of 30,000 or more and 200,000 or less.
• Mw weight average molecular weight
• [16] The adhesive composition according to any one of [1] to [15], wherein the adhesive composition contains a filler.
• [18] The adhesive composition according to any one of [1] to [17], wherein the adhesive composition contains an organic peroxide.
• the relative permittivity of the adhesive layer measured at a frequency of 28 GHz with respect to the adhesive layer obtained by curing the adhesive composition according to any one of [1] to [18] is 3 or less.
• PEEK polyetheretherketone
• a copper-clad laminate comprising the laminate according to [20] or [21].
• the present invention while having good electrical characteristics (dielectric characteristics) compatible with 5G, it also exhibits good adhesion to a low-dielectric base film having poor adhesion, and has heat resistance and chemical resistance (resistance to chemicals). It is possible to provide an adhesive composition for forming a low-dielectric adhesive layer having a solvent-like property.
• the adhesive composition of the present invention the laminated body including the adhesive layer made of the adhesive composition, and the constituent members related to the electronic parts including the laminated body will be described in detail, but the constituent requirements described below will be described.
• the description of the above is an example as an embodiment of the present invention, and is not specified in these contents.
• the adhesive composition of the present invention contains a styrene-based elastomer and an epoxy-modified resin having a structure represented by the following formula (1).
• the adhesive composition of the present invention may contain other components, if necessary.
• the adhesive composition of the present invention containing a styrene-based elastomer and an epoxy-modified resin having a structure represented by the above formula (1) exhibits good adhesion even with a low-dielectric adhesive composition. It is an adhesive composition having excellent heat resistance and chemical resistance (solvent resistance).
• the styrene-based elastomer is a copolymer mainly composed of a block of a conjugated diene compound and an aromatic vinyl compound and a random structure, and a hydrogenated product thereof. There are few highly polar bonding groups in the molecule, and good electrical properties (dielectric properties) can be imparted to the composition. Further, as compared with other types of elastomers, it is easy to control the molecular weight, and it is also an advantage that the characteristics of the adhesive composition can be stably produced.
• aromatic vinyl compound examples include styrene, t-butylstyrene, ⁇ -methylstyrene, divinylbenzene, 1,1-diphenylethylene, N, N-diethyl-p-aminoethylstyrene, vinyltoluene and the like.
• conjugated diene compound examples include butadiene, isoprene, 1,3-pentadiene, 2,3-dimethyl-1,3-butadiene and the like.
• styrene-based elastomer examples include a styrene-butadiene block copolymer, a styrene-ethylene propylene block copolymer, a styrene-butadiene-styrene block copolymer, a styrene-isoprene-styrene block copolymer, and a styrene-ethylene butylene.
• -Styrene block copolymer, styrene-ethylene propylene-styrene block copolymer and the like can be mentioned.
• the styrene-based elastomer may be a modified styrene-based elastomer or an unmodified styrene-based elastomer, and may be selected according to the intended purpose without any particular limitation.
• a modified styrene-based elastomer such as the styrene-based elastomer containing a carboxy group or a styrene-based elastomer containing an amino group described below is preferable, and the adhesion by laminating and each temperature are different.
• an unmodified styrene-based elastomer is preferable.
• styrene-based elastomer Only one type of styrene-based elastomer may be used, or two or more types may be used in combination.
• a modified styrene-based elastomer with good surface adhesion to the adherend and an unmodified styrene-based elastomer whose elastic modulus can be adjusted for each temperature of the adhesive composition high adhesion can be achieved. It is possible to control the fluidity.
• styrene-ethylene from the viewpoint that adhesiveness and electrical properties (dielectric properties) can be imparted to the adhesive composition, the control of the molecular structure is relatively simple, and the properties of the adhesive composition can be easily adjusted.
• Butylene-styrene block copolymers and styrene-ethylenepropylene-styrene block copolymers are preferred.
• the mass ratio of styrene / ethylenebutylene in the styrene-ethylenebutylene-styrene block copolymer and the mass ratio of styrene / ethylenepropylene in the styrene-ethylenepropylene-styrene block copolymer are 10/90 to 50/50. It is preferably 20/80 to 40/60, and more preferably 20/80 to 40/60. When the mass ratio is within this range, an adhesive composition having excellent adhesive properties can be obtained.
• the styrene-based elastomer containing a carboxy group has high adhesion, can impart flexibility to the cured product, and is effective as a component that imparts good electrical characteristics. Since the styrene-based elastomer containing a carboxy group is contained in the adhesive composition, the adhesive composition is flexible even for an adherend such as a base film or a metal foil having good electrical characteristics and low polarity. Since the object can sufficiently follow the surface of the adherend, the highly polar carboxy group can develop the adhesiveness, so that the adhesiveness of the adhesive layer is improved.
• the styrene-based elastomer containing a carboxy group is reactive, the heat resistance and chemical resistance of the adhesive layer are improved by epoxy curing. Further, the inclusion of the carboxy group improves the dispersibility of the filler in the dispersion liquid.
• the styrene-based elastomer containing a carboxy group is a copolymer mainly composed of a block of a conjugated diene compound and an aromatic vinyl compound and a random structure, and a hydrogenated product thereof modified with an unsaturated carboxylic acid. .. Specific examples of the types of aromatic vinyl compounds and conjugated diene compounds and styrene-based elastomers are as described in the above section ⁇ Styrene-based elastomer>.
• Modification of the styrene-based elastomer containing a carboxy group can be performed, for example, by copolymerizing an unsaturated carboxylic acid at the time of polymerizing the styrene-based elastomer. It can also be carried out by heating and kneading a styrene-based elastomer and an unsaturated carboxylic acid in the presence of an organic peroxide.
• the unsaturated carboxylic acid include acrylic acid, methacrylic acid, maleic acid, itaconic acid, fumaric acid, maleic anhydride, and itaconic anhydride.
• the amount of modification with unsaturated carboxylic acid is preferably 0.1 to 10% by mass.
• the acid value of the styrene-based elastomer containing a carboxy group is preferably 0.1 to 25 mgKOH / g, and more preferably 0.5 to 23 mgKOH / g.
• this acid value is 0.1 mgKOH / g or more, the adhesive composition is sufficiently cured, and good adhesiveness and heat resistance can be obtained.
• the acid value is 30 mgKOH / g or less, the cohesive force of the adhesive composition is suppressed, so that the adhesiveness is excellent and the electrical characteristics are also excellent.
• the weight average molecular weight of the styrene-based elastomer containing a carboxy group is preferably 10,000 to 500,000, more preferably 30,000 to 300,000, and even more preferably 50,000 to 200,000.
• the weight average molecular weight is at least the above lower limit, excellent adhesiveness can be exhibited, and the coatability when dissolved in a solvent and coated is also improved.
• the weight average molecular weight is not more than the above upper limit, the compatibility with the epoxy resin is improved.
• the weight average molecular weight is a value obtained by converting the molecular weight measured by gel permeation chromatography (hereinafter, also referred to as “GPC”) into polystyrene.
• the content of the styrene-based elastomer containing a carboxy group is preferably 15 to 90 parts by mass with respect to 100 parts by mass of the solid content of the adhesive composition. When the content is within this range, an adhesive composition having excellent adhesive properties can be obtained.
• Styrene-based elastomer containing amino groups Since the styrene-based elastomer containing an amino group is contained in the adhesive composition, the amino group exhibits a strong interaction with the low-dielectric base film, and the reactivity of the adhesive composition becomes high. The adhesion of the adhesive layer is improved. Further, since the styrene-based elastomer containing an amino group is reactive, the heat resistance and chemical resistance of the adhesive layer are improved by epoxy curing. Since it contains an amino group, the adhesion to the metal is improved.
• the styrene-based elastomer containing an amino group is a copolymer of a conjugated diene compound and an aromatic vinyl compound mainly having a block and a random structure, and an amine-modified product thereof.
• Specific examples of the types of aromatic vinyl compounds and conjugated diene compounds and styrene-based elastomers are as described in the above section ⁇ Styrene-based elastomer>.
• the method for modifying the styrene-based elastomer with an amine is not particularly limited, and a known method can be used.
• an amine is polymerized by polymerizing a (hydrogenated) block copolymer using a polymerization initiator having an amino group.
• the weight average molecular weight of the styrene-based elastomer containing an amino group is preferably 10,000 to 500,000, more preferably 30,000 to 300,000, and further preferably 50,000 to 200,000.
• the weight average molecular weight is at least the above lower limit, excellent adhesiveness can be exhibited, and the coatability when dissolved in a solvent and coated is also improved.
• the weight average molecular weight is not more than the above upper limit, the compatibility with the epoxy resin is improved.
• the content of the styrene-based elastomer containing an amino group is preferably 15 to 90 parts by mass with respect to 100 parts by mass of the solid content of the adhesive composition. When the content is within this range, an adhesive composition having excellent adhesive properties can be obtained.
• the total amount of nitrogen in the styrene-based elastomer containing an amino group is preferably 50 to 5000 ppm. More preferably, it is 200 to 3000 ppm. When the total amount of nitrogen is at least the above lower limit, excellent adhesion can be exhibited. When the total amount of nitrogen is not more than the above upper limit, the electrical characteristics are excellent.
• the total amount of nitrogen in the styrene-based elastomer containing an amino group can be determined according to JIS-K2609 using a trace nitrogen analyzer ND-100 (manufactured by Mitsubishi Chemical Corporation).
• the epoxy-modified resin having the structure represented by the above formula (1) has an epoxy structure and the styrene containing the carboxy group and the amino group in the styrene-based elastomer containing the carboxy group, as compared with the ordinary epoxy resin.
• the reaction with the amino group in the system elastomer or the reaction rate of self-polymerization is fast, and it is effective as a component that develops high adhesiveness to the adherend and heat resistance of the cured adhesive.
• a preferred embodiment of the epoxy-modified resin is an epoxy-modified resin having a structure represented by the following formula (2).
• R 5 and R 6 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 5 in (2) may be the same or different
• R 6 in each formula (2) may be the same or different.
• * Represents a binding group.
• the epoxy-modified resin preferably contains an unsaturated bond other than an aromatic ring, such as an olefin skeleton or a vinyl group.
• unsaturated bonds other than aromatic rings such as olefin skeletons and vinyl groups, can be incorporated into reactions involving epoxy groups to accelerate reaction rates and increase crosslink density. As a result, heat resistance and chemical resistance can be improved even with a small blending amount.
• unsaturated bonds other than aromatic rings can be crosslinked by radical polymerization to increase the crosslink density of the epoxy-modified resin, and to improve heat resistance and chemical resistance.
• a preferred embodiment of the epoxy-modified resin is an epoxy-modified resin having a structure represented by the following formula (3).
• R 7 and R 8 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 7 in (3) may be the same or different
• R 8 in each formula (3) may be the same or different. * Represents a binding group.
• the epoxy-modified resin is preferably an epoxy-modified resin having a structure represented by the above formula (1) and a structure represented by the above formula (3), and the structure represented by the above formula (2) and the above formula. It is more preferable that the epoxy-modified resin has the structure represented by (3).
• Preferred embodiments of the epoxy-modified resin include an epoxy-modified resin having at least one of a structure represented by the following formula (4) and a structure represented by the following formula (5). It is also preferable to have both a structure represented by the following formula (4) and a structure represented by the following formula (5).
• R 9 and R 10 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 9 in (4) may be the same or different
• R 10 in each formula (4) may be the same or different. * Represents a binding group.
• R 11 and R 12 each independently represent hydrogen or an alkyl group having 10 or less carbon atoms.
• R 11 in (5) may be the same or different
• R 12 in each formula (5) may be the same or different. * Represents a binding group.
• the epoxy-modified resin has an epoxy-modified structure having a structure represented by the above formula (1), a structure represented by the above formula (4), and at least one of the structures represented by the above formula (5).
• a resin is preferable, and an epoxy having at least one of a structure represented by the above formula (2), a structure represented by the above formula (4), and a structure represented by the above formula (5). More preferably with a modified resin. Further, the structure represented by the above formula (1) and the above formula (2), the structure represented by the above formula (3), the structure represented by the above formula (4), and the above formula (5). Epoxy-modified resins having at least one of the structures represented are also preferred.
• the epoxy-modified resin is preferably an epoxy-modified organic compound obtained by modifying an organic compound containing an unsaturated bond.
• the structure represented by the above formula (1) and the unsaturated bond can coexist in the molecule depending on the modification rate, and the olefin skeleton or the reaction of the epoxy structure can be carried out. It is easy to impart the effect of unsaturated bonds other than aromatic rings such as vinyl groups.
• a reaction in which an epoxy skeleton is formed by a peroxide is effective.
• the epoxy-modified resin is preferably an epoxy-modified elastomer modified from an elastomer containing an unsaturated bond.
• the epoxy-modified elastomer can impart flexibility to the cured product, and by suppressing the decrease in toughness of the cured product due to epoxy curing, it is possible to maintain the adhesiveness when the laminate is bent, and to improve heat resistance and chemical resistance. Do not lower.
• the epoxy-modified resin is preferably a styrene-based elastomer.
• the epoxy-modified resin having the structure represented by the above formula (1) or the above formula (2) it is also preferable to have a structural unit of styrene in addition to the structures represented by the above formulas (3) to (5). .. Since the epoxy-modified resin is also a styrene-based elastomer together with the styrene-based elastomer contained in the adhesive resin composition of the present invention, compatibility is improved when both are mixed, and the styrene-based elastomer containing the carboxy group is used. This is because the reaction with the carboxy group in the elastomer and the amino group in the styrene-based elastomer containing the amino group can be efficiently proceeded.
• the epoxy-modified resin examples include an alicyclic epoxy compound having an alicyclic epoxy group such as epoxycyclohexane, an epoxidized polybutadiene, and an epoxy compound of a styrene-butadiene block copolymer. Above all, an epoxy compound of a styrene-butadiene block copolymer is more preferable. Since the styrene-butadiene block copolymer contains an unsaturated bond, the structure represented by the above formula (1) and the unsaturated bond can coexist in the molecule, and the olefin skeleton or vinyl can be involved in the reaction of the epoxy structure. It is easy to impart the effect of unsaturated bonds other than aromatic rings such as groups.
• epoxy-modified resin a commercially available epoxy compound can also be used.
• seroxide 2021P, seroxide 2081, seroxide 2000 manufactured by Daicel
• Eporide GT401, Epolide PB3600, Eporide PB4700 manufactured by Daicel
• Friend AT501 and Epofriend CT310 manufactured by Daicel
• the weight average molecular weight (Mw) of the epoxy-modified resin is preferably 30,000 or more, and more preferably 50,000 or more. When the weight average molecular weight is 30,000 or more, softening of the adhesive composition can be suppressed, and resin flow during heat pressure bonding can be prevented. When the weight average molecular weight is 50,000 or more, the flexibility of the epoxy-modified resin is improved and the toughness of the cured product is improved.
• the weight average molecular weight (Mw) of the epoxy-modified resin is preferably 200,000 or less, and more preferably 160,000 or less. When the weight average molecular weight is 200,000 or less, the compatibility with the styrene-based elastomer is further improved. When the weight average molecular weight is 160,000 or less, the elastic modulus of the adhesive composition can be lowered and the shape of the adherend can be followed.
• the content of the epoxy-modified resin is preferably 0.5 parts by mass or more, more preferably 1 part by mass or more, and further preferably 2 parts by mass or more with respect to 100 parts by mass of the resin composition. preferable.
• the content of the epoxy-modified resin is 0.5 parts by mass or more, epoxy curing with the modified styrene-based elastomer is possible, and the adhesiveness is improved.
• the content of the epoxy-modified resin is 1 part by mass or more, the adhesive composition is sufficiently cured and good heat resistance can be ensured.
• the content of the epoxy-modified resin is 2 parts by mass or more, the adhesive composition can further proceed with the crosslinking reaction, and good chemical resistance can be ensured.
• the content of the epoxy-modified resin is preferably 50 parts by mass or less, more preferably 25 parts by mass or less, and further preferably 15 parts by mass or less with respect to 100 parts by mass of the resin composition. ..
• the content of the epoxy-modified resin is 50 parts by mass or less, it is possible to achieve both low dielectric constant, heat resistance, and chemical resistance.
• the content of the epoxy-modified resin is 25 parts by mass or less, the flexibility of the adhesive composition after curing can be ensured and the adhesiveness is improved.
• the content of the epoxy-modified resin is 15 parts by mass or less, the dielectric can be further reduced.
• the epoxy equivalent of the epoxy-modified resin is 200 g / eq.
• the above is preferable, and 350 g / eq.
• the above is more preferable, and 900 g / eq.
• the above is more preferable.
• the epoxy equivalent of the epoxy-modified resin is 200 g / eq.
• the epoxy skeleton does not become too dense in the epoxy-modified resin, the reaction with the modified elastomer proceeds, and the adhesive composition forms a matrix, so that heat resistance and chemical resistance are improved.
• the epoxy equivalent of the epoxy-modified resin is 350 g / eq.
• the epoxy equivalent of the epoxy-modified resin is 900 g / eq. With the above, the adhesive composition becomes flexible and the adhesiveness is improved.
• the epoxy equivalent of the epoxy-modified resin is 20,000 g / eq. It is preferably 16,000 g / eq. It is more preferably 10,000 g / eq. The following is more preferable.
• the epoxy equivalent of the epoxy-modified resin is 20,000 g / eq. If the following, the adhesive composition can be epoxy-cured and the adhesiveness is improved.
• the epoxy equivalent of the epoxy-modified resin is 16,000 g / eq. If the following, the crosslink density of the cured adhesive composition is increased, and the heat resistance and chemical resistance are improved.
• the epoxy equivalent of the epoxy-modified resin is 10,000 g / eq. If the following is the case, even if the blending amount of the epoxy-modified resin is small, the matrix can be formed with the modified elastomer, so that the electrical characteristics can be improved while maintaining the heat resistance and chemical resistance.
• the adhesive composition of the present invention can contain other resin components in addition to the above-mentioned styrene-based elastomer and epoxy-modified resin.
• resin components for example, a thermoplastic resin other than the styrene-based elastomer can be contained to such an extent that the function of the adhesive composition is not affected.
• thermoplastic resins examples include phenoxy resin, polyamide resin, bismaleimide resin, polyester resin, polycarbonate resin, polyphenylene oxide resin, polyurethane resin, polyacetal resin, polyethylene resin, polypropylene resin, polyvinyl resin and the like. Can be mentioned. These thermoplastic resins may be used alone or in combination of two or more.
• the adhesive composition of the present invention includes fillers, radical polymerization initiators, tackifiers, flame retardants, curing agents, curing accelerators, coupling agents, heat aging inhibitors, and the like.
• a leveling agent, a defoaming agent, an inorganic filler, a pigment, a solvent and the like can be contained to such an extent that the function of the adhesive composition is not affected.
• the adhesive composition of the present invention preferably contains a filler.
• a filler for example, an inorganic filler is preferable from the viewpoint of heat resistance and mechanical property control of the adhesive composition, and as the inorganic filler, a silicon-based inorganic filler and boron nitride are used from the viewpoint of electrical properties. preferable.
• the silicon-based inorganic filler for example, mica and talc, which can control the mechanical properties of the adhesive composition even in a small amount and have excellent electrical characteristics, are preferable.
• an organic filler is preferable from the viewpoint of dispersibility and brittleness
• a styrene-based spherical filler is preferable from the viewpoint of electrical characteristics
• a styrene-based hollow filler is preferable. More preferred. These may be used alone or in combination of two or more.
• the content of the filler contained in the adhesive composition of the present invention is preferably 0.5 to 25 parts by volume with respect to 100 parts by volume of the resin composition, and 1 to 15 parts by volume with respect to 100 parts by volume of the resin composition. Is more preferable.
• the shape of the filler is not particularly limited and may be appropriately selected depending on the intended purpose.
• the inorganic filler may be a spherical inorganic filler or a non-spherical inorganic filler, but a non-spherical inorganic filler is preferable from the viewpoint of thermal expansion coefficient (CTE) and film strength.
• the shape of the non-spherical inorganic filler may be a three-dimensional shape other than a spherical shape (substantially a perfect circular spherical shape), and examples thereof include a plate shape, a scale shape, a columnar shape, a chain shape, and a fibrous shape. Among them, a plate-shaped or scaly inorganic filler is preferable, and a plate-shaped inorganic filler is more preferable, from the viewpoint of the coefficient of thermal expansion (CTE) and the film strength.
• the adhesive composition of the present invention preferably contains a radical polymerization initiator.
• Unsaturated bonds other than aromatic rings such as the above-mentioned olefin skeleton and vinyl group can crosslink the resin component even by radical polymerization, and further improve the adhesion (adhesiveness), heat resistance and chemical resistance of the adhesive layer. Can be improved.
• the type of the radical polymerization initiator is not particularly limited and may be appropriately selected depending on the intended purpose. For example, a peroxide capable of crosslinking at a temperature equivalent to that of epoxy curing, without proceeding with epoxy curing. Examples thereof include a photopolymerization initiator capable of pre-crosslinking.
• more preferable embodiments include, for example, organic peroxides.
• organic peroxides By containing an organic peroxide, the crosslink density of the adhesive composition is improved without containing a highly polar functional group, and the adhesive layer has more adhesiveness (adhesiveness), heat resistance and chemical resistance. Can be improved.
• the organic peroxide include benzoyl peroxide, lauroyl peroxide, t-butyl peroxypivalate, t-butyl peroxyethyl hexanoate, 1,1'-bis- (t-butyl peroxy) cyclohexane, and t-amyl.
• organic peroxides such as peroxy-2-ethylhexanoate and t-hexylperoxy-2-ethylhexanoate.
• tackifier examples include kumaron-inden resin, terpene resin, terpene-phenol resin, rosin resin, pt-butylphenol-acetylene resin, phenol-formaldehyde resin, xylene-formaldehyde resin, petroleum hydrocarbon resin, and the like. Examples thereof include hydrogenated hydrocarbon resins and terepine resins. These tackifiers may be used alone or in combination of two or more.
• the flame retardant may be either an organic flame retardant or an inorganic flame retardant.
• organic flame retardant include melamine phosphate, melamine polyphosphate, guanidine phosphate, guanidine polyphosphate, ammonium phosphate, ammonium polyphosphate, ammonium phosphate amide ammonium, polyphosphate amide ammonium, phosphate carbamate, and polyphosphate carbamate.
• Aluminum Trisdiphenylphosphite Aluminum Trismethylethylphosphinate, Aluminum Trisdiphenylphosphinate, Zinc bisdiethylphosphinate, Zinc bismethylethylphosphinate, Zinc bisdiphenylphosphite, Titanyl bisdiphenylphosphite, Titanium tetrakisdiethylphosphinate , Phosphate-based flame retardants such as titanyl bismethylethylphosphinate, titanium tetrakismethylethylphosphinate, titanyl bisdiphenylphosphinate, titanium tetrakisdiphenylphosphinate; , Isocyanuric acid compound, triazole compound, tetrazole compound, diazo compound, urea and other nitrogen-based flame retardant; silicone compound, silane compound and other silicon-based flame retardant.
• Examples of the inorganic flame retardant include metal hydroxides such as aluminum hydroxide, magnesium hydroxide, zirconium hydroxide, barium hydroxide, and calcium hydroxide; tin oxide, aluminum oxide, magnesium oxide, zirconium oxide, and zinc oxide.
• Metal oxides such as molybdenum oxide and nickel oxide; zinc carbonate, magnesium carbonate, barium carbonate, zinc borate, hydrated glass and the like can be mentioned. Two or more of these flame retardants can be used in combination.
• Examples of the above-mentioned curing agent include, but are not limited to, amine-based curing agents and acid anhydride-based curing agents.
• Examples of the amine-based curing agent include melamine resins such as methylated melamine resin, butylated melamine resin, and benzoguanamine resin, dicyandiamide, and 4,4'-diphenyldiaminosulfone.
• Examples of the acid anhydride include aromatic acid anhydrides and aliphatic acid anhydrides. These curing agents may be used alone or in combination of two or more.
• the curing accelerator is used, for example, for the purpose of accelerating the reaction between a styrene-based elastomer, particularly a modified styrene-based elastomer and an epoxy resin, and is a tertiary amine-based curing accelerator or a tertiary amine salt-based curing. Accelerators, imidazole-based curing accelerators, and the like can be used.
• tertiary amine-based curing accelerator examples include benzyldimethylamine, 2- (dimethylaminomethyl) phenol, 2,4,6-tris (dimethylaminomethyl) phenol, tetramethylguanidine, triethanolamine, N, N'. -Dimethylpiperazine, triethylenediamine, 1,8-diazabicyclo [5.4.0] undecene and the like can be mentioned.
• imidazole-based curing accelerator examples include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-methyl-4-ethylimidazole, 2-phenylimidazole, and 2-phenyl-.
• Examples of the coupling agent include vinyltrimethoxysilane, 3-glycidoxypropyltrimethoxysilane, p-styryltrimethoxysilane, 3-methacryloxypropylmethyldimethoxysilane, 3-acryloxypropyltrimethoxysilane, and N.
• heat antiaging agent examples include 2,6-di-tert-butyl-4-methylphenol and n-octadecyl-3- (3', 5'-di-tert-butyl-4'-hydroxyphenyl) propione.
• tetrakis [methylene-3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionate] methane, pentaerythritol tetrakis [3- (3,5-di-t-butyl-4-)
• Phenol-based antioxidants such as hydroxyphenol, triethylene glycol-bis [3- (3-t-butyl-5-methyl-4-hydroxyphenyl) propionate; dilauryl-3,3'-thiodipropionate, dimyristyl Sulfur-based antioxidants such as -3,3'-dithiopropionate; phosphorus-based antioxidants such as trisnonylphenylphosphite and tris (2,4-di-tert-butylphenyl) phosphite can be mentioned. These may be used alone or in combination of two or more.
• examples of the inorganic filler include powders made of titanium oxide, aluminum oxide, zinc oxide, carbon black, silica, copper, silver and the like. These may be used alone or in combination of two or more.
• the adhesive layer according to the present invention comprises the above-mentioned adhesive composition of the present invention.
• the adhesive composition forming the adhesive layer can be cured.
• the curing method is not particularly limited and may be appropriately selected depending on the intended purpose. Examples thereof include thermosetting.
• the thickness of the adhesive layer is not particularly limited and may be appropriately selected depending on the intended purpose. For example, the thickness is preferably 3 to 100 ⁇ m, more preferably 3 to 50 ⁇ m, and 5 to 30 ⁇ m. Is even more preferable.
• An adhesive layer can be produced by forming the above adhesive composition into a film.
• the adhesive composition can be produced by mixing a styrene-based elastomer, a resin composition containing an epoxy-modified resin having a structure represented by the above formula (1), and other components as necessary. ..
• the mixing method is not particularly limited, and the adhesive composition may be uniform. Since the adhesive composition is preferably used in the state of a solution or a dispersion, a solvent is also usually used.
• the solvent examples include alcohols such as methanol, ethanol, isopropyl alcohol, n-propyl alcohol, isobutyl alcohol, n-butyl alcohol, benzyl alcohol, ethylene glycol monomethyl ether, propylene glycol monomethyl ether, diethylene glycol monomethyl ether, and diacetone alcohol.
• alcohols such as methanol, ethanol, isopropyl alcohol, n-propyl alcohol, isobutyl alcohol, n-butyl alcohol, benzyl alcohol, ethylene glycol monomethyl ether, propylene glycol monomethyl ether, diethylene glycol monomethyl ether, and diacetone alcohol.
• Ketones such as acetone, methyl ethyl ketone, methyl isobutyl ketone, methyl amyl ketone, cyclohexanone, isophorone; aromatic hydrocarbons such as toluene, xylene, ethylbenzene, mesitylene; methyl acetate, ethyl acetate, butyl acetate, ethylene glycol monomethyl ether acete -Esters such as 3-methoxybutyl acetate; aliphatic hydrocarbons such as hexane, heptane, cyclohexane, methylcyclohexane and the like can be mentioned.
• the adhesive composition is a solution containing a solvent or a dispersion (resin varnish), coating on the base film and formation of the adhesive layer can be smoothly performed, and an adhesive layer having a desired thickness can be obtained. It can be easily obtained.
• the adhesive composition contains a solvent, the solid content concentration is preferably in the range of 3 to 80% by mass, more preferably 10 to 50% by mass, from the viewpoint of workability including formation of the adhesive layer. When the solid content concentration is 80% by mass or less, the viscosity of the solution is appropriate and it is easy to apply the solution uniformly.
• a resin varnish containing the adhesive composition and a solvent is applied to the surface of a base film to form a resin varnish layer, and then the resin varnish is formed.
• a B-stage-like adhesive layer can be formed.
• the B-staged adhesive layer means an uncured state or a semi-cured state in which a part of the adhesive composition has begun to be cured, and the adhesive composition is further cured by heating or the like. The state of doing.
• the method of applying the resin varnish on the base film is not particularly limited and may be appropriately selected depending on the intended purpose. For example, a spray method, a spin coat method, a dip method, a roll coat method, etc.
• the B-stage-shaped adhesive layer can be further heated or the like to form a cured adhesive layer.
• the relative permittivity ( ⁇ r) of the adhesive layer obtained by curing the adhesive composition of the present invention at a frequency of 28 GHz is preferably 3 or less, and more preferably 2.7 or less.
• the dielectric loss tangent (tan ⁇ ) of the adhesive layer at a frequency of 28 GHz is preferably 0.004 or less, more preferably 0.0025 or less, still more preferably 0.002 or less. If the relative permittivity is 3 or less and the dielectric loss tangent is 0.004 or less, it can be used for high-frequency FPC-related products with strict electrical characteristics requirements.
• the relative permittivity is 2.7 or less and the dielectric loss tangent is 0.0025 or less
• the electrical characteristics expected for the components of 5G-compatible high-frequency FPC-related products can be satisfied, which is equivalent to LCP. It has the electrical characteristics of the above, and can be suitably used for 5G high-frequency FPC-related products, which have strict requirements for electrical characteristics.
• the dielectric loss tangent is 0.002 or less, a high frequency FPC-related product having further improved transmission characteristics can be manufactured.
• the laminate of the present invention includes a base film and the adhesive layer on at least one surface of the base film.
• the base film used in the present invention can be selected depending on the intended use of the laminate.
• examples thereof include a polyimide film, a polyether ether ketone film, a polyphenylene sulfide film, an aramid film, a polyethylene naphthalate film, and a liquid crystal polymer film. ..
• a polyimide film, a polyetheretherketone (PEEK) film, a polyethylene naphthalate film, and a liquid crystal polymer film are preferable from the viewpoint of adhesiveness and electrical properties.
• the base film When the laminate of the present invention is used as a bonding sheet, the base film must be a releasable film, for example, polyethylene terephthalate film, polyethylene film, polypropylene film, silicone releasable paper, and polyolefin resin. Examples thereof include coated paper, TPX (polymethylpentene) film, and fluororesin film.
• the base film When the laminate of the present invention is used as a shield film, the base film needs to be a film having an electromagnetic wave shielding ability, and examples thereof include a laminate of a protective insulating layer and a metal foil.
• Coverlay film A coverlay film is mentioned as a preferable embodiment of the laminate according to the present invention.
• a laminate having an adhesive layer called a "coverlay film” is usually used to protect the wiring portion.
• This coverlay film includes an insulating resin layer and an adhesive layer formed on the surface thereof.
• the coverlay film is a laminate in which the adhesive layer is formed on at least one surface of the base film, and it is generally difficult to peel off the base film and the adhesive layer.
• the thickness of the base film contained in the coverlay film is preferably 5 to 100 ⁇ m, more preferably 5 to 50 ⁇ m, and even more preferably 5 to 30 ⁇ m.
• the coverlay film When the thickness of the base film is not more than the above upper limit, the coverlay film can be thinned. When the thickness of the base film is at least the above lower limit, the printed wiring board can be easily designed and handled well.
• a resin varnish containing the adhesive composition and a solvent is applied to the surface of the base film to form a resin varnish layer, and then a solvent is used from the resin varnish layer. By removing the above, it is possible to produce a coverlay film on which a B-stage-like adhesive layer is formed.
• the drying temperature at the time of removing the solvent is preferably 40 to 250 ° C, more preferably 70 to 170 ° C.
• Drying is performed by passing the laminate coated with the adhesive composition through a furnace in which hot air drying, far-infrared heating, high-frequency induction heating and the like are performed.
• a releasable film may be laminated on the surface of the adhesive layer for storage or the like.
• known films such as polyethylene terephthalate film, polyethylene film, polypropylene film, silicone releasable paper, polyolefin resin coated paper, TPX film, and fluororesin film are used. Since the coverlay film according to the present invention uses the low-dielectric adhesive composition of the present invention, high-speed transmission of electronic devices is possible, and the adhesive stability with electronic devices is also excellent. Become.
• a bonding sheet is mentioned as a preferred embodiment of the laminate according to the present invention.
• the bonding sheet is one in which the adhesive layer is formed on the surface of a releasable film (base film). Further, the bonding sheet may have an aspect in which an adhesive layer is provided between the two releasable films.
• the release film is peeled off before use.
• the releasable film the same one as described in the above (Coverlay film) column can be used.
• the thickness of the base film contained in the bonding sheet is preferably 5 to 100 ⁇ m, more preferably 25 to 75 ⁇ m, and even more preferably 38 to 50 ⁇ m.
• the bonding sheet can be easily manufactured and handled well.
• a method for producing the bonding sheet for example, there is a method in which a resin varnish containing the adhesive composition and the solvent is applied to the surface of the release film and dried in the same manner as in the case of the coverlay film. Since the bonding sheet according to the present invention uses the low-dielectric adhesive composition of the present invention, high-speed transmission of electronic devices is possible, and the adhesive stability with electronic devices is also excellent. ..
• a preferred embodiment of the laminate according to the present invention is a copper-clad laminate in which a copper foil is bonded to an adhesive layer in the laminate of the present invention.
• a copper foil is bonded to the copper-clad laminate using the above-mentioned laminate, and for example, a base film, an adhesive layer, and a copper foil are configured in this order.
• the adhesive layer and the copper foil may be formed on both sides of the base film.
• the adhesive composition used in the present invention is also excellent in adhesiveness to articles containing copper. Since the copper-clad laminate according to the present invention uses the low-dielectric adhesive composition of the present invention, it enables high-speed transmission of electronic devices and has excellent adhesive stability.
• the adhesive layer of the laminate is brought into surface contact with a copper foil, heat laminating is performed at 80 ° C to 200 ° C, and the adhesive layer is further cured by aftercure.
• the aftercure conditions can be, for example, 100 ° C. to 200 ° C., 30 minutes to 4 hours in an atmosphere of an inert gas.
• the copper foil is not particularly limited, and electrolytic copper foil, rolled copper foil, and the like can be used.
• a preferred embodiment of the laminate according to the present invention is a printed wiring board in which copper wiring is bonded to an adhesive layer in the laminate of the present invention.
• the printed wiring board is obtained by forming an electronic circuit on the copper-clad laminate.
• the base film and the copper wiring are bonded to each other using the above laminated body, and the base film, the adhesive layer, and the copper wiring are configured in this order.
• the adhesive layer and the copper wiring may be formed on both sides of the base film.
• a printed wiring board is manufactured by attaching a coverlay film to a surface having a wiring portion via an adhesive layer using a hot press or the like.
• the printed wiring board according to the present invention uses the low-dielectric adhesive composition of the present invention, it enables high-speed transmission of electronic devices and has excellent adhesive stability.
• a method for manufacturing a printed wiring board according to the present invention for example, the adhesive layer of the laminate is brought into contact with copper wiring, heat laminating is performed at 80 ° C to 200 ° C, and the adhesive layer is further subjected to aftercure. There is a way to cure.
• the aftercure conditions can be, for example, 100 ° C. to 200 ° C., 30 minutes to 4 hours.
• the shape of the copper wiring is not particularly limited, and the shape or the like may be appropriately selected as desired.
• the shield film is a film for shielding various electronic devices in order to cut electromagnetic noise that affects various electronic devices such as computers, mobile phones and analytical devices and causes malfunctions. Also called an electromagnetic wave shield film.
• the electromagnetic wave shielding film is formed by laminating, for example, an insulating resin layer, a metal layer, and an adhesive layer according to the present invention in this order. Since the shield film according to the present invention uses the low-dielectric adhesive composition of the present invention, high-speed transmission of electronic devices is possible, and the adhesive stability with electronic devices is also excellent. ..
• a preferred embodiment of the laminate according to the present invention is a printed wiring board with a shield film.
• the printed wiring board with a shield film is a printed wiring board provided with a printed circuit on at least one side of the substrate, on which the electromagnetic wave shielding film is attached.
• the printed wiring board with a shield film has, for example, a printed wiring board, an insulating film adjacent to the surface of the printed wiring board on the side where the printed circuit is provided, and the electromagnetic wave shielding film. Since the printed wiring board with a shield film according to the present invention uses the low-dielectric adhesive composition of the present invention, it enables high-speed transmission of electronic devices and has excellent adhesive stability.
• the acid value of this copolymer is 0 mgKOH / g, the styrene / ethylene butylene ratio is 30/70, and the weight average molecular weight is 67,000.
• the trade name "Clayton G1651" styrene-ethylenebutylene-styrene block copolymer manufactured by Clayton Co., Ltd. was used.
• the acid value of this copolymer is 0 mgKOH / g, the styrene / ethylene butylene ratio is 33/67, and the weight average molecular weight is 136,700.
• the styrene / ethylene butylene ratio of this copolymer is 40/60, the weight average molecular weight is 92,000, and the epoxy equivalent is 1055 g / eq. Is. (Epoxy modified resin)
• Epoxy modified resin The trade name "Epofriend CT310" (epoxydated product of styrene-butadiene block copolymer) manufactured by Daicel Corporation was used.
• the styrene / ethylene butylene ratio of this copolymer is 40/60, the weight average molecular weight is 93,000, and the epoxy equivalent is 2125 g / eq. Is.
• epoxy resin As the epoxy resin, a trade name "YX7700" (softening point 65 ° C.) manufactured by Mitsubishi Chemical Corporation, which is a novolak type epoxy resin, was used. The epoxy equivalent is 270 g / eq. Is. (Epoxy resin) As the epoxy resin, a trade name "HP-7200" (epoxy resin, softening point 56-66 ° C.) manufactured by DIC Corporation, which is a novolak type epoxy resin, was used. The epoxy equivalent is 259 g / eq. Is. (Perbutyl E) As the organic peroxide, the trade name "Perbutyl E", which is a peroxy ester manufactured by NOF CORPORATION, was used.
• MK-100DS The trade name "MK-100DS", which is a mica with an average particle diameter of 3 ⁇ m manufactured by Katakura Corp. Agri Co., Ltd., was used.
• UHP-S2 The trade name "UHP-S2", which is a scaly boron nitride manufactured by Showa Denko KK and has an average particle diameter of 0.7 ⁇ m, was used.
• OP935 The trade name "OP935", which is a flame retardant manufactured by Clariant Chemicals Co., Ltd., was used.
• the surface roughness of the glossy surface is a value obtained by measuring the roughness curve using a laser microscope and obtaining from this roughness curve based on JIS B 0601: 2013 (ISO 4287: 1997 Amd.1: 2009). .. (Release film)
• As the release film NP75SA (silicone release PET film, 75 ⁇ m) manufactured by Panac Co., Ltd. was used.
• the total amount of nitrogen contained in the amino group-containing styrene-based elastomer used in the examples was determined by the following method. ⁇ Measurement method> It was determined according to JIS-K2609 using a trace nitrogen analyzer ND-100 (manufactured by Mitsubishi Chemical Corporation).
• Example 1 Each component constituting the adhesive layer shown in Table 1 was contained in the ratio shown in Table 1, and these components were dissolved in a solvent to prepare a resin varnish having a solid content concentration of 20% by mass.
• the surface of the base film was corona-treated.
• the resin varnish was applied to the surface of the base film and dried in an oven at 110 ° C. for 4 minutes to volatilize toluene to form an adhesive layer, and a base film with an adhesive was obtained.
• the adhesive layer of the adhesive laminate was laminated so as to be in contact with the glossy surface of the electrolytic copper foil, and heat laminating was performed at 120 ° C. to obtain a pre-cured adhesive laminate.
• the adhesive layer was cured by after-curing the pre-cured adhesive laminate to obtain a post-cured adhesive laminate.
• the adhesion (N / cm) between the electrolytic copper foil of the cured adhesive laminate of Example 1 and the base film was measured.
• Adhesion (N / cm) After curing, the adhesive laminate was cut into a test piece with a width of 25 mm, and the adhesion was measured in accordance with JIS Z0237: 2009 (adhesive tape / adhesive sheet test method), with a peeling speed of 0.3 m / min and a peeling angle of 180.
• the adhesive force was measured by measuring the peeling strength when peeling the electrolytic copper foil from the base film with an adhesive fixed to the support at °.
• the relative permittivity and dielectric loss tangent at a frequency of 28 GHz were also measured for the adhesive layer in the cured adhesive laminate of Example 1.
• the adhesive layers were heat-laminated at 120 ° C. so that the adhesive surfaces were in contact with each other to form a pre-curing adhesive film (thickness 100 ⁇ m).
• This pre-curing adhesive film (thickness 100 ⁇ m) was allowed to stand in an oven and heat-cured at 150 ° C. for 60 minutes to prepare a post-curing adhesive film (100 mm ⁇ 100 mm).
• the release film was peeled off from the adhesive film, and the relative permittivity and dielectric loss tangent of the adhesive layer were measured.
• the heat resistance of the adhesive layer in the laminate of Example 1 was evaluated by a solder heat resistance test.
• solder heat resistance test In the solder heat resistance test, the adhesive laminate was floated in a solder bath at 288 ° C. for 10 seconds x 3 times with the base film surface facing up, and abnormal appearance such as swelling and peeling of the adhesive layer was confirmed. The heat resistance of the laminate was evaluated according to the following evaluation criteria. ⁇ No abnormality (no dissolution). ⁇ There is no abnormality in the end, but softening of the adhesive layer is observed during the test. ⁇ Although it was not peeled off, the adhesive layer was softened and a “stain pattern” was formed. ⁇ It is peeling off.
• Table 3 shows the results of each measurement.
• Example 2 to 15 In Example 1, the laminates of Examples 2 to 15 were prepared in the same manner as in Example 1 except that the types and blending amounts of the components constituting the adhesive layer were changed as shown in Table 1. .. The prepared laminate was evaluated in the same manner as in Example 1. The results are shown in Table 3.
• Example 1 Comparative Example 1 to Comparative Example 11
• Example 2 the laminates of Comparative Examples 1 to 11 were prepared in the same manner as in Example 1 except that the types and blending amounts of the components constituting the adhesive layer were changed as shown in Table 2. ..
• the prepared laminate was evaluated in the same manner as in Example 1. The results are shown in Table 4.
• the adhesive layer made of the adhesive composition of the present invention exhibits good electrical properties (dielectric properties) compatible with 5G, and is also excellent in adhesion, heat resistance, and solvent resistance. ing.
• the laminate having an adhesive layer made of the adhesive composition of the present invention is suitable for manufacturing FPC-related products for electronic devices such as smartphones, mobile phones, optical modules, digital cameras, game machines, notebook computers, and medical appliances. Can be used for.

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• 2021
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