Composition set and film

Abstract

A composition set comprising a first film-like composition and a second film-like composition that contain a polymerizable compound, wherein the first film-like composition contains (A) a borate anion, the second film-like composition contains (B) a phosphorus compound having a P=O(OH) structure, and at least one selected from the group consisting of the first film-like composition and the second film-like composition contains (X) at least one selected from the group consisting of aromatic carboxylic acids having two or more hydroxy groups, salts of said aromatic carboxylic acids, and hydrates of said aromatic carboxylic acids.

Description

Composition Set and Film

[0001] The present disclosure relates to composition sets, films, and the like.

[0002] In recent years, films containing polymerizable compounds have been used to bond various components in the manufacture of various devices. For example, Patent Document 1 listed below describes a thermosetting film containing a polymerizable compound.

[0003] JP 2014-156522 A

[0004] With the recent miniaturization and high performance of various devices, there are cases where a film containing a polymerizable compound is heat-cured near a member that should be avoided from being exposed to high heat, or where a film is heat-cured in contact with a member that should be avoided from being exposed to high heat, etc. In these cases, from the viewpoint of avoiding deterioration of the member by performing heat-curing at a low temperature, it is required to lower the reaction initiation temperature of the film containing a polymerizable compound.

[0005] An object of one aspect of the present disclosure is to provide a composition set for obtaining a film containing a polymerizable compound, the composition set being capable of lowering the reaction initiation temperature of the film.An object of another aspect of the present disclosure is to provide a film containing a polymerizable compound, the film being capable of lowering the reaction initiation temperature.

[0006] In some aspects, the present disclosure relates to the following items [1] to

[12] . [1] A composition set comprising a first film-like composition and a second film-like composition each containing a polymerizable compound, wherein the first film-like composition contains (A) a borate anion, the second film-like composition contains (B) a phosphorus compound having a P=O(OH) structure, and at least one selected from the group consisting of the first film-like composition and the second film-like composition contains (X) at least one selected from the group consisting of an aromatic carboxylic acid having two or more hydroxy groups, a salt of the aromatic carboxylic acid, and a hydrate of the aromatic carboxylic acid. [2] The composition set described in [1], wherein the aromatic carboxylic acid includes dihydroxybenzoic acid. [3] The composition set described in [1] or [2], wherein the component (A) includes a borate anion having a naphthalene ring. [4] The composition set described in any one of [1] to [3], wherein the component (B) includes a (meth)acrylate compound having a P=O(OH) structure. [5] The composition set according to any one of [1] to [4], wherein the content of the component (B) is 0.01 to 10.00 mass% based on the total mass of the second film-like composition. [6] The composition set according to any one of [1] to [5], wherein at least one selected from the group consisting of the first film-like composition and the second film-like composition has a thickness of 1 to 50 μm. [7] A film having a first region and a second region containing a polymerizable compound, wherein the first region contains (A) a borate anion, the second region contains (B) a phosphorus compound having a P═O(OH) structure, and at least one selected from the group consisting of the first region and the second region contains (X) at least one selected from the group consisting of an aromatic carboxylic acid having two or more hydroxy groups, a salt of the aromatic carboxylic acid, and a hydrate of the aromatic carboxylic acid. [8] The film according to [7], wherein the aromatic carboxylic acid includes dihydroxybenzoic acid. [9] The film according to [7] or [8], wherein the component (A) contains a borate anion having a naphthalene ring.

[10] The film according to any one of [7] to [9], wherein the component (B) contains a (meth)acrylate compound having a P═O(OH) structure.

[11] The film according to any one of [7] to

[10] , wherein the content of the component (B) is 0.01 to 10.00 mass% based on the total mass of the second region.

[12] The film according to any one of [7] to

[11] , wherein the thickness is 1 to 100 μm.

[0007] According to one aspect of the present disclosure, there is provided a composition set for obtaining a film containing a polymerizable compound, the composition set being capable of lowering the reaction initiation temperature of the film. According to another aspect of the present disclosure, there is provided a film containing a polymerizable compound, the composition set being capable of lowering the reaction initiation temperature of the film.

[0008] Hereinafter, embodiments of the present disclosure will be described in detail, but the present disclosure is not limited to the following embodiments.

[0009] In this specification, numerical ranges indicated using "to" indicate a range that includes the numerical values ​​before and after "to" as the minimum and maximum values, respectively. A numerical range "A or greater" means a range exceeding A and A. A numerical range "A or less" means a range less than A and A. In numerical ranges described in stages in this specification, the upper or lower limit of a numerical range in a certain stage can be arbitrarily combined with the upper or lower limit of a numerical range in another stage. In numerical ranges described in this specification, the upper or lower limit of the numerical range may be replaced with a value shown in the examples. "A or B" may include either A or B, or may include both. Unless otherwise specified, the materials exemplified in this specification can be used alone or in combination of two or more. When multiple substances corresponding to each component are present in the composition, the content of each component in the composition refers to the total amount of the multiple substances present in the composition, unless otherwise specified. "(Meth)acrylate" means at least one of acrylate and the corresponding methacrylate. The same applies to other similar expressions such as "(meth)acrylic." The content of (meth)acrylate compounds means the total amount of acrylate compounds and methacrylate compounds. Unless otherwise specified, "alkyl groups" may be linear, branched, or cyclic. "Hydroxy groups" do not include OH groups contained in carboxy groups.

[0010] In this specification, the "weight average molecular weight" can be measured by gel permeation chromatography (GPC) under the following measurement conditions, by conversion from a calibration curve using standard polystyrene. (Measurement conditions) Apparatus: GPC-8020, manufactured by Tosoh Corporation Detector: RI-8020, manufactured by Tosoh Corporation Column: Gelpack GL-A-160-S + GL-A150, manufactured by Resonaq Corporation Sample concentration: 120 mg / 3 mL Solvent: tetrahydrofuran Injection volume: 60 μL Pressure: 294 × 10 ６ Pa (30kgf / cm ２ ) Flow rate: 1.00mL / min

[0011] The composition set according to the present embodiment includes a first film-like composition and a second film-like composition each containing a polymerizable compound, the first film-like composition containing (A) a borate anion, the second film-like composition containing (B) a phosphorus compound having a P=O(OH) structure, and at least one selected from the group consisting of the first film-like composition and the second film-like composition containing (X) at least one selected from the group consisting of an aromatic carboxylic acid having two or more hydroxy groups, a salt of the aromatic carboxylic acid, and a hydrate of the aromatic carboxylic acid. The film according to the present embodiment includes a first region and a second region each containing a polymerizable compound, the first region containing (A) a borate anion, and the second region containing (B) a phosphorus compound having a P=O(OH) structure, and at least one selected from the group consisting of the first region and the second region containing (X) at least one selected from the group consisting of an aromatic carboxylic acid having two or more hydroxy groups, a salt of the aromatic carboxylic acid, and a hydrate of the aromatic carboxylic acid. The film according to this embodiment can be obtained as a film containing a polymerizable compound by laminating the first film-like composition and the second film-like composition of the composition set according to this embodiment on each other. The film manufacturing method according to this embodiment includes a step of laminating the first film-like composition and the second film-like composition of the composition set according to this embodiment on each other.

[0012] Hereinafter, (A) borate anion will sometimes be referred to as "component (A)," (B) phosphorus compound having a P═O(OH) structure will sometimes be referred to as "component (B)," (X) at least one selected from the group consisting of aromatic carboxylic acids having two or more hydroxy groups, salts of aromatic carboxylic acids, and hydrates of aromatic carboxylic acids will sometimes be referred to as "component (X)," and aromatic carboxylic acids having two or more hydroxy groups will sometimes be referred to as "aromatic carboxylic acid x." Hereinafter, the first and second film-like compositions of the composition set according to this embodiment will sometimes be referred to simply as the "first film-like composition" and the "second film-like composition," respectively, and the first and second regions of the film according to this embodiment will sometimes be referred to simply as the "first region" and the "second region," respectively.

[0013] The first film-like composition, the second film-like composition, the first region, and the second region each contain at least one polymerizable compound, and the polymerizable compound may be at least one selected from the group consisting of a compound containing component (A), component (B), and component (X), or may contain a polymerizable compound other than a compound containing component (A), component (B), or component (X). When the at least one compound selected from the group consisting of a compound containing component (A), component (B), and component (X) is a polymerizable compound, the first film-like composition, the second film-like composition, the first region, and the second region may contain a compound containing component (A), component (B), or a polymerizable compound other than a compound containing component (X).

[0014] The first film-like composition and the second film-like composition of the composition set according to this embodiment can be used as thermosetting film-like compositions. The film according to this embodiment can be used as a thermosetting film.

[0015] The composition set and film according to this embodiment can lower the reaction initiation temperature of the film, and can lower the reaction initiation temperature of the film immediately after production. The composition set and film according to this embodiment can achieve a reaction initiation temperature T1 of, for example, 81°C or lower (preferably, 80°C or lower, 79°C or lower, 78°C or lower, 77°C or lower, etc.) in the evaluation method described in the Examples below.

[0016] According to one aspect of the composition set and film of this embodiment, it is possible to suppress changes in the reaction initiation temperature over time after film production, and to obtain excellent storage stability with respect to the reaction initiation temperature. According to one aspect of the composition set and film of this embodiment, in the evaluation method described in the Examples below, the absolute value |T2-T1| of the temperature difference between the reaction initiation temperature T1 and the reaction initiation temperature T2 can be obtained to be, for example, 20°C or less (preferably, 16°C or less, 15°C or less, 12°C or less, 10°C or less, etc.).

[0017] The applications of the composition set and film according to this embodiment are not particularly limited, and examples thereof include display devices, semiconductor devices, electronic device components, etc. The composition set and film according to this embodiment may be used in micro LEDs (light emitting diodes), micro OLEDs (organic light emitting diodes), etc.

[0018] The film according to this embodiment has a first region and a second region containing a polymerizable compound. The film according to this embodiment may be configured such that the first region is located on one side of the film and the second region is located on the other side of the film. The first region and the second region may be adjacent to each other, or another region may be present between the first region and the second region. When the first region and the second region are adjacent to each other, a visible boundary may or may not exist between the first region and the second region. The first region and the second region may be layered, and the film according to this embodiment may be a laminate film having a first layer and a second layer containing a polymerizable compound.

[0019] In the film according to this embodiment, the content of the component (A) in the first region may be greater than the content of the component (A) in the second region, and the second region may not contain the component (A). In the film according to this embodiment, the content of the component (B) in the second region may be greater than the content of the component (B) in the first region, and the first region may not contain the component (B).

[0020] In the composition set according to this embodiment, the thickness of at least one selected from the group consisting of the first film-like composition and the second film-like composition may be within the following ranges. The thickness may be 0.1 μm or more, 0.5 μm or more, 1 μm or more, 3 μm or more, 5 μm or more, 8 μm or more, or 10 μm or more. The thickness may be 250 μm or less, 200 μm or less, 150 μm or less, 100 μm or less, 80 μm or less, 50 μm or less, 30 μm or less, 20 μm or less, 15 μm or less, or 10 μm or less. From these perspectives, the thickness may be 0.1 to 250 μm, 0.1 to 50 μm, 0.1 to 25 μm, 1 to 250 μm, 1 to 50 μm, 1 to 25 μm, 5 to 250 μm, 5 to 50 μm, or 5 to 25 μm. The thickness of the first film composition and the second film composition may be the average thickness measured at 10 points.

[0021] The thickness (total thickness) of the film according to this embodiment may be in the following ranges. The thickness may be 1 μm or more, 3 μm or more, 5 μm or more, 8 μm or more, 10 μm or more, 12 μm or more, 15 μm or more, 18 μm or more, or 20 μm or more. The thickness may be 500 μm or less, 300 μm or less, 200 μm or less, 100 μm or less, 80 μm or less, 50 μm or less, 30 μm or less, or 20 μm or less. From these viewpoints, the thickness may be 1 to 500 μm, 1 to 100 μm, 1 to 50 μm, 5 to 500 μm, 5 to 100 μm, 5 to 50 μm, 10 to 500 μm, 10 to 100 μm, or 10 to 50 μm. The thickness (total thickness) of the film according to this embodiment may be the average thickness at 10 locations.

[0022] The first film-like composition and the first region contain a borate anion as component (A). The first film-like composition and the first region may contain a boron salt containing a borate anion (a salt of component (A) and a counter cation of component (A); hereinafter referred to as "component (a1)"). Component (A) may be bound to a counter cation, or may be free and not bound to a counter cation.

[0023] In component (A), the number of boron atoms (number per molecule) may be 1 to 4, 1 to 3, or 1 to 2, from the viewpoint of making it easier to lower the reaction initiation temperature.

[0024] From the viewpoint of easily lowering the reaction initiation temperature, the component (A) may include a borate anion having a naphthalene ring (a substituted or unsubstituted naphthyl group), may include a borate anion having a naphthalene ring (a substituted or unsubstituted naphthyl group) bonded to a boron atom, may include at least one anion selected from the group consisting of an alkyltriarylborate anion and a tetraarylborate anion, may include an alkyltriarylborate anion, may include an alkyltrinaphthylborate anion, or may include a butyltrinaphthylborate anion.

[0025] In component (A), the number of naphthalene rings (the number per molecule) or the number of naphthalene rings bonded to boron atoms (the number per molecule) may be 1 to 4, 1 to 3, 2 to 4, 2 to 3, or 3 to 4, or may be 3, from the viewpoint of making it easier to lower the reaction initiation temperature.

[0026] Component (A) may have an unsubstituted naphthalene ring or a naphthalene ring having a substituent, such as a halogen atom, an alkyl group, an aryl group, or an alkoxy group.

[0027] From the viewpoint of easily lowering the reaction initiation temperature, component (A) may have alkyl groups bonded to boron atoms. From the viewpoint of easily lowering the reaction initiation temperature, the number of alkyl groups bonded to boron atoms in component (A) (the number per molecule) may be 1 to 3, or 1 to 2.

[0028] The number of carbon atoms in the alkyl group bonded to the boron atom may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The number of carbon atoms in the alkyl group may be 1 or more, 2 or more, 3 or more, or 4 or more. The number of carbon atoms in the alkyl group may be 12 or less, 10 or less, 8 or less, 6 or less, 5 or less, or 4 or less. From these viewpoints, the number of carbon atoms in the alkyl group may be 1 to 12, 1 to 8, 1 to 4, 2 to 12, 2 to 8, 2 to 4, 3 to 12, 3 to 8, 3 to 4, 4 to 12, or 4 to 8.

[0029] Component (A) may have a functional group bonded to the boron atom other than a naphthalene ring (naphthyl group) or an alkyl group, such as an aryl group other than a naphthyl group (e.g., a phenyl group).

[0030] Examples of the counter cation in component (a1) include quaternary ammonium ions, tertiary ammonium ions, secondary ammonium ions, primary ammonium ions, ammonium ions, imidazolium ions, imidazolinium ions, pyridinium ions, alkali metal ions (sodium ions, potassium ions, etc.), phosphonium cations, sulfonium cations, and iodonium cations. Component (a1) may or may not contain a metal ion. Examples of the metal ion include alkali metal ions (sodium ions, potassium ions, etc.). Component (a1) may contain a quaternary ammonium ion as a counter cation, from the viewpoint of easily lowering the reaction initiation temperature.

[0031] In the quaternary ammonium ion, examples of the substituent bonded to the nitrogen atom include an alkyl group, an aryl group (e.g., a phenyl group), etc. From the viewpoint of easily lowering the reaction initiation temperature, component (a1) may contain, as a counter cation, a quaternary ammonium ion having an alkyl group bonded to the nitrogen atom, or may contain a quaternary ammonium ion having at least one alkyl group selected from the group consisting of a linear alkyl group bonded to the nitrogen atom and a branched alkyl group bonded to the nitrogen atom.

[0032] The number of carbon atoms in the alkyl group bonded to the nitrogen atom may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The number of carbon atoms in the alkyl group may be 1 or more, 2 or more, 3 or more, or 4 or more. The number of carbon atoms in the alkyl group may be 18 or less, 16 or less, 14 or less, 12 or less, 10 or less, 8 or less, 6 or less, 5 or less, or 4 or less. From these viewpoints, the number of carbon atoms in the alkyl group may be 1 to 18, 1 to 8, 1 to 4, 2 to 6, 4 to 18, or 4 to 8.

[0033] Examples of quaternary ammonium ions include tetraalkylammonium ions, trialkylammonium ions, dialkylammonium ions, monoalkylammonium ions, tetraarylammonium ions, triarylammonium ions, diarylammonium ions, monoarylammonium ions, etc. Component (a1) may contain a tetraalkylammonium ion as a counter cation, from the viewpoint of easily lowering the reaction initiation temperature.

[0034] Examples of tetraalkylammonium ions include tetramethylammonium ion, tetraethylammonium ion, tetrapropylammonium ion, tetrabutylammonium ion, tetrahexylammonium ion, triethylmethylammonium ion, tributylethylammonium ion, trimethyldecylammonium ion, etc. Component (a1) may contain a tetrabutylammonium ion as a counter cation, from the viewpoint of easily lowering the reaction initiation temperature.

[0035] The content of component (a1) in the first film-like composition (based on the total mass of the first film-like composition) or the content of component (a1) in the first region (based on the total mass of the first region) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature: The content of component (a1) may be 0.01% by mass or more, 0.05% by mass or more, 0.10% by mass or more, 0.20% by mass or more, 0.30% by mass or more, 0.40% by mass or more, 0.50% by mass or more, 0.60% by mass or more, 0.70% by mass or more, or 0.80% by mass or more. The content of component (a1) is 20.00% by mass or less, 15.00% by mass or less, 10.00% by mass or less, 8.00% by mass or less, 7.00% by mass or less, 6.00% by mass or less, 5.00% by mass or less, 4. 00 mass% or less, 3.00 mass% or less, 2.00 mass% or less, 1.50 mass% or less, 1.20 mass% or less, 1.10 mass% or less, 1.00 mass% or less, or 0.90 mass% or less. From these viewpoints, the content of the (a1) component may be 0.01 to 20.00 mass%, 0.30 to 20.00 mass%, 0.50 to 20.00 mass%, 0.01 to 2.00 mass%, 0.30 to 2.00 mass%, 0.50 to 2.00 mass%, 0.01 to 1.00 mass%, 0.30 to 1.00 mass%, or 0.50 to 1.00 mass%.

[0036] The second film-like composition and the second region contain, as component (B), a phosphorus compound having a P=O(OH) structure (excluding compounds corresponding to component (a1)). In the phosphorus compound having a P=O(OH) structure, as shown in the following general formula (b1), an oxygen atom is bonded to a phosphorus atom via a double bond, and a hydroxy group is bonded to the phosphorus atom via a single bond. In component (B), the number of P=O(OH) structures (the number per molecule) may be 1, from the viewpoint of easily lowering the reaction initiation temperature.

[0037] [In the formula, b11 represents an integer of 1 to 3, b12 represents an integer of 0 to 2, b11+b12 is 3, and R ｂ１ represents a monovalent group.

[0038] b11 may be 1 to 2, or 2 to 3, from the viewpoint of easily lowering the reaction initiation temperature.

[0039] The component (B) has a monovalent group other than a hydroxy group (R in general formula (b1)) as a functional group bonded to a phosphorus atom. ｂ１ ) Examples of the monovalent group include a substituted or unsubstituted alkyl group, a substituted or unsubstituted aryl group (e.g., a phenyl group), and a (meth)acryloyl group-containing group. The (meth)acryloyl group-containing group is a group having at least one group selected from the group consisting of an acryloyl group and a methacryloyl group.

[0040] From the viewpoint of easily lowering the reaction initiation temperature, the component (B) may include at least one selected from the group consisting of a (meth)acrylate compound having a P═O(OH) structure, phosphoric acid, and phenylphosphonic acid, or may include a (meth)acrylate compound having a P═O(OH) structure, or may include a compound represented by the following general formula (b2):

[0041] [In the formula, b21 represents an integer of 1 or 2, b22 represents an integer of 1 or 2, b21 + b22 is 3, b23 and b24 each independently represent an integer of 1 or more, and R ｂ２ represents a hydrogen atom or a methyl group.

[0042] From the viewpoint of easily lowering the reaction initiation temperature, b23 may be 1 to 8, 1 to 6, 1 to 5, 3 to 8, 3 to 6, 3 to 5, 5 to 8, or 5 to 6. From the viewpoint of easily lowering the reaction initiation temperature, b24 may be 1 to 4, 2 to 4, 1 to 3, or 1 to 2.

[0043] From the viewpoint of easily lowering the reaction initiation temperature, the content of component (B) may be 50.00 mass% or more, more than 50.00 mass%, 70.00 mass% or more, 80.00 mass% or more, 90.00 mass% or more, 92.00 mass% or more, 95.00 mass% or more, 97.00 mass% or more, 98.00 mass% or more, 99.00 mass% or more, or substantially 100.00 mass% based on the total mass of the phosphorus-containing compound (compound containing a phosphorus atom) contained in the second film-like composition or the second region.

[0044] From the viewpoint of easily lowering the reaction initiation temperature, the content of component (B) in the second film-like composition (based on the total mass of the second film-like composition) or the content of component (B) in the second region (based on the total mass of the second region) may be within the following ranges: The content of component (B) may be 0.01% by mass or more, 0.05% by mass or more, 0.10% by mass or more, 0.20% by mass or more, 0.30% by mass or more, 0.40% by mass or more, 0.50% by mass or more, 0.60% by mass or more, 0.70% by mass or more, 0.80% by mass or more, 0.85% by mass or more, or 0.90% by mass or more. The content of component (B) may be 10.00% by mass or less, 8.00% by mass or less, 6.00% by mass or less, 5.00% by mass or less, 4.00% by mass or less, 3.00% by mass or less, 2.00% by mass or less, 1.80% by mass or less, 1.50% by mass or less, 1.20% by mass or less, or 1.00% by mass or less. From these viewpoints, the content of component (B) may be 0.01 to 10.00% by mass, 0.01 to 3.00% by mass, 0.01 to 1.00% by mass, 0.30 to 10.00% by mass, 0.30 to 3.00% by mass, 0.30 to 1.00% by mass, 0.50 to 10.00% by mass, 0.50 to 3.00% by mass, or 0.50 to 1.00% by mass.

[0045] The mass ratio R1 (component (B) / component (a1)), which is the mass ratio of the content of component (B) in the second film-like composition to the content of component (a1) in the first film-like composition, or the mass ratio of the content of component (B) in the second region to the content of component (a1) in the first region, may be within the following ranges from the viewpoint of easily lowering the reaction initiation temperature: Mass ratio R1 may be 0.01 or more, 0.05 or more, 0.10 or more, 0.30 or more, 0.50 or more, 0.60 or more, 0.70 or more, 0.80 or more, 0.90 or more, 1.00 or more, or 1.10 or more. The mass ratio R1 may be 10.00 or less, 8.00 or less, 6.00 or less, 5.00 or less, 4.00 or less, 3.00 or less, 2.80 or less, 2.50 or less, 2.30 or less, 2.00 or less, 1.80 or less, 1.50 or less, or 1.20 or less. From these viewpoints, the mass ratio R1 may be 0.01 to 10.00, 0.01 to 5.00, 0.01 to 2.00, 0.50 to 10.00, 0.50 to 5.00, 0.50 to 2.00, 1.00 to 10.00, 1.00 to 5.00, or 1.00 to 2.00.

[0046] At least one selected from the group consisting of the first film-like composition and the second film-like composition of the composition set according to this embodiment contains, as the component (X), at least one selected from the group consisting of aromatic carboxylic acid x, a salt of aromatic carboxylic acid x, and a hydrate of aromatic carboxylic acid x (excluding compounds corresponding to component (a1) or component (B)). The first and second regions of the film according to this embodiment contain, as the component (X), at least one selected from the group consisting of aromatic carboxylic acid x, a salt of aromatic carboxylic acid x, and a hydrate of aromatic carboxylic acid x (excluding compounds corresponding to component (a1) or component (B)). It is presumed that the reaction initiation temperature is lowered by accelerating the reaction due to the interaction between component (X) having a carboxy group or a group derived from a carboxy group (a group related to a salt, hydrate, etc.) and component (A) or (B). However, the cause of the lowered reaction initiation temperature is not limited to this.

[0047] From the viewpoint of easily lowering the reaction initiation temperature, the first film-like composition may contain the component (X), and the first region may contain the component (X). From the viewpoint of easily obtaining excellent storage stability (easy to suppress changes in the reaction initiation temperature over time after film production: the same applies below), only one of the first film-like composition and the second film-like composition may contain the component (X), or only the second film-like composition of the first film-like composition and the second film-like composition may contain the component (X), and the content of the component (X) in the second film-like composition may be higher than the content of the component (X) in the first film-like composition. From the viewpoint of easily obtaining excellent storage stability, only one of the first region and the second region may contain the component (X), or only the second region of the first region and the second region may contain the component (X), and the content of the component (X) in the second region may be higher than the content of the component (X) in the first region.

[0048] Examples of the salt of aromatic carboxylic acid x include alkali metal salts such as sodium salts and potassium salts. From the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability, the component (X) may contain at least one selected from the group consisting of aromatic carboxylic acid x and a hydrate of aromatic carboxylic acid x, and may contain aromatic carboxylic acid x.

[0049] The aromatic carboxylic acid x has at least one aromatic ring. The number of aromatic rings (the number in one molecule) may be 1, from the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability. Examples of the aromatic ring include a benzene ring and a naphthalene ring. The aromatic carboxylic acid x may contain an aromatic carboxylic acid having a benzene ring, from the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability.

[0050] The aromatic carboxylic acid x has a carboxy group bonded to an aromatic ring. From the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability, the aromatic carboxylic acid x may include an aromatic carboxylic acid having a hydroxy group (phenolic hydroxy group) bonded to the aromatic ring. From the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability, the aromatic carboxylic acid x may have a hydroxy group bonded to the para position relative to the carboxy group bonded to the aromatic ring, or may have one or two hydroxy groups bonded to the meta position relative to the carboxy group bonded to the aromatic ring.

[0051] In the aromatic carboxylic acid x, the number of carboxy groups bonded to the aromatic ring (the number per molecule) may be 1, from the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability. In the aromatic carboxylic acid x, the number of hydroxy groups (the number per molecule) or the number of hydroxy groups bonded to the aromatic ring (the number per molecule) may be 2 to 4 or 2 to 3, or may be 2, from the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability.

[0052] The aromatic ring of the aromatic carboxylic acid x may have a substituent other than a carboxy group and a hydroxy group, or may not have a substituent other than a carboxy group and a hydroxy group. Examples of the substituent include an alkyl group and an alkoxy group.

[0053] Examples of aromatic carboxylic acid x include protocatechuic acid (also known as 3,4-dihydroxybenzoic acid), α-resorcylic acid (also known as 3,5-dihydroxybenzoic acid), β-resorcylic acid, γ-resorcylic acid, 2-pyrocatechuic acid, gentisic acid, orsellinic acid, gallic acid, phloroglucinol carboxylic acid, etc. From the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability, aromatic carboxylic acid x may include dihydroxybenzoic acid, may include at least one selected from the group consisting of protocatechuic acid and α-resorcylic acid, or may include protocatechuic acid.

[0054] The content of component (X) in the first film-like composition (criteria: the total amount of aromatic carboxylic acid (aromatic carboxylic acid x and aromatic carboxylic acid not corresponding to aromatic carboxylic acid x; the same applies hereinafter), aromatic carboxylic acid salt, and aromatic carboxylic acid hydrate contained in the first film-like composition), the content of component (X) in the second film-like composition (criteria: the total amount of aromatic carboxylic acid, aromatic carboxylic acid salt, and aromatic carboxylic acid hydrate contained in the second film-like composition), the content of component (X) in the first region (criteria: the total amount of aromatic carboxylic acid, aromatic carboxylic acid salt, and aromatic carboxylic acid contained in the first region), From the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability, the content of the (X) component in the second region (criterion: the total amount of the aromatic carboxylic acid, the salt of the aromatic carboxylic acid, and the hydrate of the aromatic carboxylic acid contained in the second region) may be 50.00% by mass or more, more than 50.00% by mass, 70.00% by mass or more, 80.00% by mass or more, 90.00% by mass or more, 92.00% by mass or more, 95.00% by mass or more, 97.00% by mass or more, 98.00% by mass or more, 99.00% by mass or more, or substantially 100.00% by mass.

[0055] The content of the component (X) in the first film-like composition (based on the total mass of the first film-like composition), the content of the component (X) in the second film-like composition (based on the total mass of the second film-like composition), the content of the component (X) in the first region (based on the total mass of the first region), or the content of the component (X) in the second region (based on the total mass of the second region) may be within the following ranges, from the viewpoints of easily lowering the reaction initiation temperature and easily achieving excellent storage stability: The content of the component (X) may be 0.01% by mass or more, 0.05% by mass or more, 0.10% by mass or more, 0.30% by mass or more, 0.50% by mass or more, 0.80% by mass or more, 1.00% by mass or more, 1.20% by mass or more, or 1.30% by mass or more. The content of the (X) component may be 10.00% by mass or less, 8.00% by mass or less, 6.00% by mass or less, 5.00% by mass or less, 4.00% by mass or less, 3.00% by mass or less, 2.00% by mass or less, 1.80% by mass or less, 1.60% by mass or less, 1.50% by mass or less, 1.40% by mass or less, or 1.30% by mass or less. From these viewpoints, the content of the (X) component may be 0.01 to 10.00% by mass, 0.01 to 5.00% by mass, 0.01 to 2.00% by mass, 0.10 to 10.00% by mass, 0.10 to 5.00% by mass, 0.10 to 2.00% by mass, 1.00 to 10.00% by mass, 1.00 to 5.00% by mass, or 1.00 to 2.00% by mass.

[0056] The content of the component (X) in film-like composition X1, one of the first film-like composition and the second film-like composition, may be higher than the content of the component (X) in the other film-like composition X2. The content of the component (X) in one of the first region and the second region, region X1, may be higher than the content of the component (X) in the other region X2. In these cases, the content of the component (X) in film-like composition X2 (based on the total mass of film-like composition X2) or the content of the component (X) in region X2 (based on the total mass of region X2) may be 1.20 mass% or less, 1.00 mass% or less, 0.80 mass% or less, 0.50 mass% or less, 0.30 mass% or less, 0.10 mass% or less, 0.05 mass% or less, or 0.01 mass% or less, and film-like composition X2 or region X2 may not contain the component (X).

[0057] The mass ratio R2 of the content of the component (X) to the content of the component (a1) (component (X) / component (a1)) may be in the following range, from the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability. The mass ratio R2 may be 10 or more, 30 or more, 50 or more, 80 or more, 100 or more, 120 or more, 140 or more, 150 or more, or 160 or more. The mass ratio R2 may be 500 or less, 400 or less, 350 or less, 300 or less, 250 or less, 200 or less, 180 or less, or 170 or less. From these viewpoints, the mass ratio R2 may be 10 to 500, 10 to 300, 10 to 200, 50 to 500, 50 to 300, 50 to 200, 100 to 500, 100 to 300, or 100 to 200.

[0058] The mass ratio R3 of the content of the component (X) to the content of the component (B) (component (X) / component (B)) may be in the following range, from the viewpoint of easily lowering the reaction initiation temperature and easily obtaining excellent storage stability. The mass ratio R3 may be 10 or more, 30 or more, 50 or more, 80 or more, 100 or more, 110 or more, 120 or more, 130 or more, or 140 or more. The mass ratio R3 may be 500 or less, 400 or less, 350 or less, 300 or less, 250 or less, 200 or less, 180 or less, 160 or less, 150 or less, or 140 or less. From these viewpoints, the mass ratio R3 may be 10 to 500, 10 to 300, 10 to 200, 50 to 500, 50 to 300, 50 to 200, 100 to 500, 100 to 300, or 100 to 200.

[0059] The first film-like composition and the second film-like composition of the composition set according to this embodiment may contain a polymerizable compound (excluding compounds corresponding to component (a1), component (B), or component (X)) as component (C). The first region and the second region of the film according to this embodiment may contain a polymerizable compound (excluding compounds corresponding to component (a1), component (B), or component (X)) as component (C).

[0060] Examples of the component (C) include a radical polymerizable compound, a cationically polymerizable compound, an anionically polymerizable compound, etc. The component (C) may contain a radical polymerizable compound from the viewpoint of easily lowering the reaction initiation temperature.

[0061] Examples of the component (C) include (meth)acrylate compounds, maleimide compounds, vinyl ether compounds, allyl compounds, styrene compounds, (meth)acrylamide compounds, nadimide compounds, natural rubber, isoprene rubber, butyl rubber, nitrile rubber, butadiene rubber, styrene-butadiene rubber, acrylonitrile-butadiene rubber, carboxylated nitrile rubber, epoxy compounds, oxetane compounds, lactone compounds, etc. At least one component (C) selected from the group consisting of the first film-like composition and the second film-like composition, or at least one component (C) selected from the group consisting of the first region and the second region, may contain a compound having an ethylenically unsaturated bond and may contain a (meth)acrylate compound, from the viewpoint of easily lowering the reaction initiation temperature.

[0062] Examples of the (meth)acrylate compound include (poly)urethane (meth)acrylate, epoxy (meth)acrylate, methyl (meth)acrylate, polyether (meth)acrylate, polyester (meth)acrylate, polybutadiene (meth)acrylate, silicone (meth)acrylate, ethyl (meth)acrylate, 2-cyanoethyl (meth)acrylate, 2-(2-ethoxyethoxy)ethyl (meth)acrylate, 2-ethoxyethyl (meth)acrylate, 2-ethylhexyl (meth)acrylate, and n-hexyl (meth)acrylate. acrylate, 2-hydroxyethyl (meth)acrylate, isopropyl (meth)acrylate, hydroxypropyl (meth)acrylate, isobutyl (meth)acrylate, isobornyl (meth)acrylate, isodecyl (meth)acrylate, isooctyl (meth)acrylate, n-lauryl (meth)acrylate, 2-methoxyethyl (meth)acrylate, 2-phenoxyethyl (meth)acrylate, tetrahydrofurfuryl (meth)acrylate, N,N-dimethylaminoethyl (meth)acrylate, N,N-dimethylaminopropyl (meth)acrylate, ethylene glycol di(meth)acrylate, diethylene glycol di(meth)acrylate, trimethylolpropane tri(meth)acrylate, tetramethylolmethane tetra(meth)acrylate, polyethylene glycol di(meth)acrylate, polyalkylene glycol di(meth)acrylate, cyclohexyl (meth)acrylate, dicyclopentenyl (meth)acrylate, dicyclopentenyloxyethyl (meth)acrylate, neopentyl glycol di(meth)acrylate, pentaerythritol (meth)acrylate

[0033] Examples of the alkylene oxide-modified isocyanuric acid tri(meth)acrylate include 2-hydroxy-1,3-di(meth)acryloxypropane, 2,2-bis[4-((meth)acryloxymethoxy)phenyl]propane, and 2,2-bis[4-((meth)acryloxypolyethoxy)phenyl]propane.“Polyurethane (meth)acrylate” and “urethane (meth)acrylate” are collectively referred to as “(poly)urethane (meth)acrylate.” The component (C) may contain a difunctional (meth)acrylate compound.

[0063] From the viewpoint of easily lowering the reaction initiation temperature, the component (C) may include a urethane (meth)acrylate compound having a polycarbonate skeleton (hereinafter referred to as "component (c1)"), may include a urethane (meth)acrylate compound having a structure derived from a polycarbonate polyol, or may include a compound represented by the following general formula (c1):

[0064] [In the formula, R １ represents a hydrogen atom or a methyl group, j represents an integer of 1 to 3, k represents an integer of 2 to 7, m represents an integer of 1 to 8, and n represents an integer of 5 to 7.

[0065] In general formula (c1), from the viewpoint of easily lowering the reaction initiation temperature, j may be 1 to 2 or 2 to 3, k may be 2 to 3 or 3 to 5, m may be 1 to 6, 1 to 4, or 1 to 2, and n may be 5 to 6 or 6 to 7.

[0066] From the viewpoint of easily lowering the reaction initiation temperature, the weight average molecular weight of the component (c1) may be 1,000 or more, 3,000 or more, 5,000 or more, 8,000 or more, 10,000 or more, 12,000 or more, 13,000 or more, 14,000 or more, or 15,000 or more. From the viewpoint of easily lowering the reaction initiation temperature, the weight average molecular weight of the component (c1) may be 100,000 or less, 50,000 or less, 30,000 or less, 25,000 or less, 20,000 or less, 18,000 or less, or 15,000 or less. From these viewpoints, the weight average molecular weight of the component (c1) may be 1,000 to 100,000, 5,000 to 50,000, or 10,000 to 30,000.

[0067] In the first film-like composition, the second film-like composition, the first region, or the second region, the content of component (c1) may be within the following ranges based on the total mass of component (C), from the viewpoint of easily lowering the reaction initiation temperature. The content of component (c1) may be 10.00 mass% or more, 15.00 mass% or more, 20.00 mass% or more, 25.00 mass% or more, 30.00 mass% or more, 35.00 mass% or more, 40.00 mass% or more, 45.00 mass% or more, 50.00 mass% or more, or 55.00 mass% or more. The content of component (c1) may be 90.00 mass% or less, 85.00 mass% or less, 80.00 mass% or less, 75.00 mass% or less, 70.00 mass% or less, 65.00 mass% or less, or 60.00 mass% or less. From these viewpoints, the content of the (c1) component may be 10.00 to 90.00 mass%, 10.00 to 80.00 mass%, 10.00 to 70.00 mass%, 20.00 to 90.00 mass%, 20.00 to 80.00 mass%, 20.00 to 70.00 mass%, 40.00 to 90.00 mass%, 40.00 to 80.00 mass%, or 40.00 to 70.00 mass%.

[0068] The content of component (c1) in the first film-like composition (based on the total mass of the first film-like composition), the content of component (c1) in the second film-like composition (based on the total mass of the second film-like composition), the content of component (c1) in the first region (based on the total mass of the first region), or the content of component (c1) in the second region (based on the total mass of the second region) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The content of component (c1) may be 5.00% by mass or more, 10.00% by mass or more, 15.00% by mass or more, or 20.00% by mass or more. The content of component (c1) may be 50.00% by mass or less, 45.00% by mass or less, 40.00% by mass or less, 35.00% by mass or less, 30.00% by mass or less, or 25.00% by mass or less. From these viewpoints, the content of the (c1) component may be 5.00 to 50.00 mass%, 5.00 to 40.00 mass%, 5.00 to 30.00 mass%, 10.00 to 50.00 mass%, 10.00 to 40.00 mass%, 10.00 to 30.00 mass%, 20.00 to 50.00 mass%, 20.00 to 40.00 mass%, or 20.00 to 30.00 mass%.

[0069] From the viewpoint of easily lowering the reaction initiation temperature, the component (C) may contain an isocyanuric acid alkylene oxide-modified di(meth)acrylate (excluding compounds corresponding to the component (c1); hereinafter referred to as "component (c2)") or an isocyanuric acid ethylene oxide-modified di(meth)acrylate.

[0070] In the first film-like composition, the second film-like composition, the first region, or the second region, the content of component (c2) may be within the following ranges based on the total mass of component (C), from the viewpoint of easily lowering the reaction initiation temperature. The content of component (c2) may be 1.00 mass% or more, 5.00 mass% or more, 10.00 mass% or more, 15.00 mass% or more, or 20.00 mass% or more. The content of component (c2) may be 50.00 mass% or less, 45.00 mass% or less, 40.00 mass% or less, 35.00 mass% or less, 30.00 mass% or less, or 25.00 mass% or less. From these viewpoints, the content of the (c2) component may be 1.00 to 50.00 mass%, 1.00 to 40.00 mass%, 1.00 to 30.00 mass%, 10.00 to 50.00 mass%, 10.00 to 40.00 mass%, 10.00 to 30.00 mass%, 20.00 to 50.00 mass%, 20.00 to 40.00 mass%, or 20.00 to 30.00 mass%.

[0071] The content of component (c2) in the first film-like composition (based on the total mass of the first film-like composition), the content of component (c2) in the second film-like composition (based on the total mass of the second film-like composition), the content of component (c2) in the first region (based on the total mass of the first region), or the content of component (c2) in the second region (based on the total mass of the second region) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The content of component (c2) may be 1.00% by mass or more, 3.00% by mass or more, 5.00% by mass or more, or 8.00% by mass or more. The content of component (c2) may be 30.00% by mass or less, 25.00% by mass or less, 20.00% by mass or less, 15.00% by mass or less, or 10.00% by mass or less. From these viewpoints, the content of the (c2) component may be 1.00 to 30.00 mass%, 1.00 to 20.00 mass%, 1.00 to 10.00 mass%, 5.00 to 30.00 mass%, 5.00 to 20.00 mass%, 5.00 to 10.00 mass%, 7.00 to 30.00 mass%, 7.00 to 20.00 mass%, or 7.00 to 10.00 mass%.

[0072] From the viewpoint of making it easier to lower the reaction initiation temperature, the component (C) may include a di(meth)acrylate compound having at least one selected from the group consisting of a dicyclopentanyl structure and a dicyclopentenyl structure (excluding compounds corresponding to the component (c1) or the component (c2); hereinafter referred to as "component (c3)"), and may include at least one selected from the group consisting of dimethylol tricyclodecane di(meth)acrylate and tricyclodecane diol di(meth)acrylate.

[0073] In the first film-like composition, the second film-like composition, the first region, or the second region, the content of component (c3) may be within the following ranges based on the total mass of component (C), from the viewpoint of easily lowering the reaction initiation temperature. The content of component (c3) may be 1.00 mass% or more, 5.00 mass% or more, 10.00 mass% or more, 15.00 mass% or more, or 20.00 mass% or more. The content of component (c3) may be 50.00 mass% or less, 45.00 mass% or less, 40.00 mass% or less, 35.00 mass% or less, 30.00 mass% or less, or 25.00 mass% or less. From these viewpoints, the content of the (c3) component may be 1.00 to 50.00 mass%, 1.00 to 40.00 mass%, 1.00 to 30.00 mass%, 10.00 to 50.00 mass%, 10.00 to 40.00 mass%, 10.00 to 30.00 mass%, 20.00 to 50.00 mass%, 20.00 to 40.00 mass%, or 20.00 to 30.00 mass%.

[0074] The content of component (c3) in the first film-like composition (based on the total mass of the first film-like composition), the content of component (c3) in the second film-like composition (based on the total mass of the second film-like composition), the content of component (c3) in the first region (based on the total mass of the first region), or the content of component (c3) in the second region (based on the total mass of the second region) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The content of component (c3) may be 1.00% by mass or more, 3.00% by mass or more, 5.00% by mass or more, or 8.00% by mass or more. The content of component (c3) may be 30.00% by mass or less, 25.00% by mass or less, 20.00% by mass or less, 15.00% by mass or less, or 10.00% by mass or less. From these viewpoints, the content of the (c3) component may be 1.00 to 30.00 mass%, 1.00 to 20.00 mass%, 1.00 to 10.00 mass%, 5.00 to 30.00 mass%, 5.00 to 20.00 mass%, 5.00 to 10.00 mass%, 7.00 to 30.00 mass%, 7.00 to 20.00 mass%, or 7.00 to 10.00 mass%.

[0075] From the viewpoint of easily lowering the reaction initiation temperature, the content of component (C) in the first film-like composition (based on the total mass of the first film-like composition), the content of component (C) in the second film-like composition (based on the total mass of the second film-like composition), the content of component (C) in the first region (based on the total mass of the first region), or the content of component (C) in the second region (based on the total mass of the second region) may be within the following ranges: The content of component (C) may be 10.00% by mass or more, 15.00% by mass or more, 20.00% by mass or more, 25.00% by mass or more, 30.00% by mass or more, 35.00% by mass or more, 38.00% by mass or more, or 40.00% by mass or more. The content of the (C) component may be 80.00% by mass or less, 75.00% by mass or less, 70.00% by mass or less, 65.00% by mass or less, 60.00% by mass or less, 55.00% by mass or less, 50.00% by mass or less, or 45.00% by mass or less. From these viewpoints, the content of the (C) component may be 10.00 to 80.00% by mass, 10.00 to 60.00% by mass, 10.00 to 50.00% by mass, 30.00 to 80.00% by mass, 30.00 to 60.00% by mass, 30.00 to 50.00% by mass, 35.00 to 80.00% by mass, 35.00 to 60.00% by mass, or 35.00 to 50.00% by mass.

[0076] In the first film-like composition or the first region, the mass ratio R4 of the content of the component (C) to the content of the component (a1) (component (C) / component (a1)) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R4 may be 1.00 or more, 5.00 or more, 10.00 or more, 20.00 or more, 30.00 or more, 35.00 or more, 40.00 or more, 45.00 or more, or 50.00 or more. The mass ratio R4 may be 300.00 or less, 250.00 or less, 200.00 or less, 150.00 or less, 120.00 or less, 100.00 or less, 80.00 or less, 60.00 or less, or 55.00 or less. From these viewpoints, the mass ratio R4 may be 1.00 to 300.00, 1.00 to 150.00, 1.00 to 80.00, 20.00 to 300.00, 20.00 to 150.00, 20.00 to 80.00, 35.00 to 300.00, 35.00 to 150.00, or 35.00 to 80.00.

[0077] In the second film-like composition or the second region, the mass ratio R5 of the content of the component (C) to the content of the component (B) (component (C) / component (B)) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R5 may be 1.00 or more, 5.00 or more, 10.00 or more, 20.00 or more, 30.00 or more, 40.00 or more, or 45.00 or more. The mass ratio R5 may be 300.00 or less, 250.00 or less, 200.00 or less, 150.00 or less, 120.00 or less, 100.00 or less, 90.00 or less, 80.00 or less, 70.00 or less, 60.00 or less, 50.00 or less, or 45.00 or less. From these viewpoints, the mass ratio R5 may be 1.00 to 300.00, 1.00 to 100.00, 1.00 to 60.00, 10.00 to 300.00, 10.00 to 100.00, 10.00 to 60.00, 30.00 to 300.00, 30.00 to 100.00, or 30.00 to 60.00.

[0078] In the first film-like composition, the second film-like composition, the first region, or the second region, the mass ratio R6 of the content of the component (C) to the content of the component (X) (component (C) / component (X)) may be within the following ranges from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R6 may be 1.00 or more, 5.00 or more, 10.00 or more, 15.00 or more, 20.00 or more, 25.00 or more, or 30.00 or more. The mass ratio R6 may be 300.00 or less, 250.00 or less, 200.00 or less, 150.00 or less, 120.00 or less, 100.00 or less, 80.00 or less, 60.00 or less, 50.00 or less, or 40.00 or less. From these viewpoints, the mass ratio R6 may be 1.00 to 300.00, 1.00 to 100.00, 1.00 to 50.00, 10.00 to 300.00, 10.00 to 100.00, 10.00 to 50.00, 30.00 to 300.00, 30.00 to 100.00, or 30.00 to 50.00.

[0079] At least one selected from the group consisting of the first film-like composition and the second film-like composition of the composition set according to this embodiment may contain a polymerization initiator as component (D) (excluding compounds corresponding to component (a1), component (B), component (X), or component (C)). At least one selected from the group consisting of the first region and the second region of the film according to this embodiment may contain a polymerization initiator as component (D) (excluding compounds corresponding to component (a1), component (B), component (X), or component (C)). The component (D) may contain a thermal polymerization initiator. Examples of the component (D) include a radical polymerization initiator, a cationic polymerization initiator, and an anionic polymerization initiator. The component (D) may contain a radical polymerization initiator from the viewpoint of easily lowering the reaction initiation temperature.

[0080] Examples of the component (D) include ketone peroxides such as methyl ethyl ketone peroxide, cyclohexanone peroxide, and methylcyclohexanone peroxide; peroxyketals such as 1,1-bis(tert-butylperoxy)cyclohexane, 1,1-bis(tert-butylperoxy)-2-methylcyclohexane, 1,1-bis(tert-butylperoxy)-3,3,5-trimethylcyclohexane, 1,1-bis(tert-hexylperoxy)cyclohexane, and 1,1-bis(tert-hexylperoxy)-3,3,5-trimethylcyclohexane; hydroperoxides such as p-menthane hydroperoxide; α,α'-bis(t dialkyl peroxides such as diisopropylbenzene (tert-butylperoxy), dicumyl peroxide, tert-butylcumyl peroxide, and di-tert-butyl peroxide; diacyl peroxides such as dioctanoyl peroxide, dilauroyl peroxide (for example, NOF Corporation's trade name "PEROIL L"), distearyl peroxide, and dibenzoyl peroxide; peroxycarbonates such as bis(4-tert-butylcyclohexyl) peroxydicarbonate, di-2-ethoxyethyl peroxydicarbonate, di-2-ethylhexyl peroxydicarbonate, and di-3-methoxybutyl peroxycarbonate;tert-butyl peroxypivalate, tert-hexyl peroxypivalate, 1,1,3,3-tetramethylbutylperoxy-2-ethylhexanoate, 2,5-dimethyl-2,5-bis(2-ethylhexanoylperoxy)hexane (for example, trade name "Perhexa 25O" of NOF Corporation), tert-hexylperoxy-2-ethylhexanoate (for example, trade name "Perhexyl O" of NOF Corporation), tert-butylperoxy-2-ethylhexanoate, tert-butylperoxyisobutyl ester, tert-hexylperoxyisopropyl monocarbonate, tert-butylperoxy-3,5,5-trimethylhexanoate, tert-butylperoxylaurate, tert-butylperoxyisopropyl monocarbonate, tert-butylperoxy-2-ethylhexyl monocarbonate, tert-butylperoxybenzoate, tert-hexylperoxybenzoate, 2,5-dimethyl-2,5-bis(benzoylperoxy)hexane, tert-butylperoxyacetate peroxyesters such as phthalic anhydride, maleic anhydride, trimellitic anhydride, hexahydrophthalic anhydride, tetrahydrophthalic anhydride, methylnadic anhydride, nadic anhydride, glutaric anhydride, dimethylglutaric anhydride, diethylglutaric anhydride, succinic anhydride, methylhexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, 1,2,3,4-cyclobutanetetracarboxylic dianhydride, 4,4'-biphthalic anhydride, 4,4'-carbonyldiphthalic anhydride, 4,4'-sulfonyldiphthalic anhydride, 4,4 acid anhydrides such as 4,4'-(hexafluoroisopropylidene)diphthalic anhydride, 4,4'-oxydiphthalic anhydride, 9,9-bis(3,4-dicarboxyphenyl)fluorene dianhydride, and 2,3,6,7-naphthalenetetracarboxylic dianhydride; azo compounds such as 2,2'-azobisisobutyronitrile, 2,2'-azobis(2,4-dimethylvaleronitrile), and 2,2'-azobis(4-methoxy-2'-dimethylvaleronitrile); iodonium salts; sulfonium salts; phosphonium salts; and imidazole compounds.

[0081] The component (D) may contain a peroxide, an organic peroxide, or a diacyl peroxide, from the viewpoint of making it easier to lower the reaction initiation temperature.

[0082] From the viewpoint of easily lowering the reaction initiation temperature, the content of component (D) in the first film-like composition (based on the total mass of the first film-like composition), the content of component (D) in the second film-like composition (based on the total mass of the second film-like composition), the content of component (D) in the first region (based on the total mass of the first region), or the content of component (D) in the second region (based on the total mass of the second region) may be within the following ranges: The content of component (D) may be 0.10% by mass or more, 0.50% by mass or more, 1.00% by mass or more, 1.50% by mass or more, 2.00% by mass or more, 2.50% by mass or more, 3.00% by mass or more, 3.50% by mass or more, or 4.00% by mass or more. The content of component (D) may be 20.00% by mass or less, 15.00% by mass or less, 10.00% by mass or less, 9.00% by mass or less, 8.00% by mass or less, 7.00% by mass or less, 6.00% by mass or less, or 5.00% by mass or less. From these viewpoints, the content of component (D) may be 0.10 to 20.00% by mass, 0.10 to 10.00% by mass, 0.10 to 5.00% by mass, 1.00 to 20.00% by mass, 1.00 to 10.00% by mass, 1.00 to 5.00% by mass, 3.00 to 20.00% by mass, 3.00 to 10.00% by mass, or 3.00 to 5.00% by mass.

[0083] In the first film-like composition or the first region, the mass ratio R7 of the content of the component (D) to the content of the component (a1) (component (D) / component (a1)) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R7 may be 0.10 or more, 0.50 or more, 1.00 or more, 2.00 or more, 3.00 or more, 4.00 or more, or 5.00 or more. The mass ratio R7 may be 50.00 or less, 30.00 or less, 20.00 or less, 15.00 or less, 10.00 or less, 9.00 or less, 8.00 or less, 7.00 or less, or 6.00 or less. From these viewpoints, the mass ratio R7 may be 0.10 to 50.00, 0.10 to 20.00, 0.10 to 10.00, 1.00 to 50.00, 1.00 to 20.00, 1.00 to 10.00, 4.00 to 50.00, 4.00 to 20.00, or 4.00 to 10.00.

[0084] In the second film-like composition or the second region, the mass ratio R8 of the content of the component (D) to the content of the component (B) (component (D) / component (B)) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R8 may be 0.10 or more, 0.50 or more, 1.00 or more, 2.00 or more, 3.00 or more, 4.00 or more, or 5.00 or more. The mass ratio R8 may be 50.00 or less, 30.00 or less, 20.00 or less, 15.00 or less, 10.00 or less, 9.00 or less, 8.00 or less, 7.00 or less, 6.00 or less, or 5.00 or less. From these viewpoints, the mass ratio R8 may be 0.10 to 50.00, 0.10 to 15.00, 0.10 to 8.00, 1.00 to 50.00, 1.00 to 15.00, 1.00 to 8.00, 3.00 to 50.00, 3.00 to 15.00, or 3.00 to 8.00.

[0085] In the first film-like composition, the second film-like composition, the first region, or the second region, the mass ratio R9 of the content of the component (D) to the content of the component (X) (component (D) / component (X)) may be within the following ranges, from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R9 may be 0.10 or more, 0.50 or more, 1.00 or more, 1.50 or more, 2.00 or more, 2.50 or more, or 3.00 or more. The mass ratio R9 may be 50.00 or less, 30.00 or less, 20.00 or less, 15.00 or less, 10.00 or less, 9.00 or less, 8.00 or less, 7.00 or less, 6.00 or less, 5.00 or less, or 4.00 or less. From these viewpoints, the mass ratio R9 may be 0.10 to 50.00, 0.10 to 20.00, 0.10 to 5.00, 1.00 to 50.00, 1.00 to 20.00, 1.00 to 5.00, 2.00 to 50.00, 2.00 to 20.00, or 2.00 to 5.00.

[0086] In the first film-like composition, the second film-like composition, the first region, or the second region, the mass ratio R10 of the content of the component (D) to the content of the component (C) (component (D) / component (C)) may be within the following range, from the viewpoint of easily lowering the reaction initiation temperature. The mass ratio R10 may be 0.01 or more, 0.03 or more, 0.05 or more, 0.08 or more, or 0.10 or more. The mass ratio R10 may be 5.00 or less, 3.00 or less, 1.00 or less, 0.50 or less, 0.30 or less, 0.20 or less, or 0.15 or less. From these viewpoints, the mass ratio R10 may be 0.01 to 5.00, 0.01 to 1.00, 0.01 to 0.50, 0.05 to 5.00, 0.05 to 1.00, 0.05 to 0.50, 0.10 to 5.00, 0.10 to 1.00, or 0.10 to 0.50.

[0087] At least one selected from the group consisting of the first film-like composition and the second film-like composition of the composition set according to this embodiment may contain a thermoplastic resin as component (E). At least one selected from the group consisting of the first region and the second region of the film according to this embodiment may contain a thermoplastic resin as component (E).

[0088] Examples of the component (E) include phenoxy resin, polyester, polyurethane (excluding polyesterurethane), polyesterurethane, ethylene-vinyl acetate copolymer, butyral resin, etc. From the viewpoint of easily lowering the reaction initiation temperature, the component (E) may contain at least one selected from the group consisting of polyesterurethane and ethylene-vinyl acetate copolymer.

[0089] From the viewpoint of easily lowering the reaction initiation temperature, the content of component (E) in the first film-like composition (based on the total mass of the first film-like composition), the content of component (E) in the second film-like composition (based on the total mass of the second film-like composition), the content of component (E) in the first region (based on the total mass of the first region), or the content of component (E) in the second region (based on the total mass of the second region) may be within the following ranges: The content of component (E) may be 10.00% by mass or more, 15.00% by mass or more, 20.00% by mass or more, 25.00% by mass or more, 30.00% by mass or more, 35.00% by mass or more, 40.00% by mass or more, 45.00% by mass or more, or 50.00% by mass or more. The content of component (E) may be 90.00% by mass or less, 85.00% by mass or less, 80.00% by mass or less, 75.00% by mass or less, 70.00% by mass or less, 65.00% by mass or less, 60.00% by mass or less, or 55.00% by mass or less. From these viewpoints, the content of component (E) may be 10.00 to 90.00% by mass, 10.00 to 70.00% by mass, 10.00 to 60.00% by mass, 30.00 to 90.00% by mass, 30.00 to 70.00% by mass, 30.00 to 60.00% by mass, 40.00 to 90.00% by mass, 40.00 to 70.00% by mass, or 40.00 to 60.00% by mass.

[0090] At least one selected from the group consisting of the first film-like composition and the second film-like composition of the composition set according to this embodiment may contain components other than those described above. At least one selected from the group consisting of the first region and the second region of the film according to this embodiment may contain components other than those described above. Examples of such components include water, organic solvents, coupling agents, fillers, softeners, accelerators, anti-degradants, colorants, flame retardants, thixotropic agents, etc. At least one selected from the group consisting of the first film-like composition and the second film-like composition, or at least one selected from the group consisting of the first region and the second region, may contain at least one of these components, or may not contain at least one of these components.

[0091] The present disclosure will be further described below using examples and comparative examples, but the present disclosure is not limited to the following examples.

[0092] <Synthesis of urethane acrylate (UA1)> 2,500 parts by mass (2.50 mol) of poly(1,6-hexanediol carbonate) (trade name: Duranol T5652, manufactured by Asahi Kasei Chemicals Corporation) and 666 parts by mass (3.00 mol) of isophorone diisocyanate (manufactured by Sigma-Aldrich Co.) were uniformly added dropwise over 3 hours to a reaction vessel equipped with a stirrer, a thermometer, a reflux condenser with a calcium chloride drying tube, and a nitrogen gas inlet tube. Next, nitrogen gas was sufficiently introduced into the reaction vessel, and the reaction vessel was then heated to 70 to 75°C to allow the mixture to react. Next, 0.53 parts by mass (4.3 mmol) of hydroquinone monomethyl ether (Sigma-Aldrich) and 5.53 parts by mass (8.8 mmol) of dibutyltin dilaurate (Sigma-Aldrich) were added to the reaction vessel, followed by the addition of 238 parts by mass (2.05 mol) of 2-hydroxyethyl acrylate (Sigma-Aldrich), and the mixture was allowed to react at 70°C for 6 hours in an air atmosphere. This yielded a urethane acrylate (UA1) having a polycarbonate skeleton. The weight-average molecular weight of the urethane acrylate (UA1) was 15,000.

[0093] <Synthesis of Polyester Urethane (EU1)> 48 parts by mass of isophthalic acid and 37 parts by mass of neopentyl glycol were added to a heated stainless steel autoclave equipped with a stirrer, thermometer, condenser, vacuum generator, and nitrogen gas inlet tube, followed by 0.02 parts by mass of tetrabutoxy titanate as a catalyst. The mixture was then heated to 220°C under a nitrogen stream and stirred for 8 hours. The pressure was then reduced to atmospheric pressure (760 mmHg) and cooled to room temperature. This resulted in the deposition of a white precipitate, which was then removed. The precipitate was washed with water and vacuum-dried to obtain a polyester polyol. After thoroughly drying the polyester polyol, it was dissolved in MEK (methyl ethyl ketone) and added to a four-neck flask equipped with a stirrer, a dropping funnel, a reflux condenser, and a nitrogen gas inlet tube. Furthermore, 0.05 parts by mass of dibutyltin dilaurate (catalyst) was added relative to 100 parts by mass of the polyester polyol, and 50 parts by mass of 4,4'-diphenylmethane diisocyanate was dissolved in MEK relative to 100 parts by mass of the polyester polyol and added using a dropping funnel. The mixture was then stirred at 80°C for 4 hours to obtain a polyester urethane (EU1).

[0094] <Preparation of polymerizable composition> (Polymerizable composition A1) Polymerizable composition A1 was prepared by mixing a methyl ethyl ketone solution (solids content: 20% by mass) of a boron salt (tetrabutylammonium = butyltrinaphthyl borate, manufactured by Resonac Corporation, trade name: Karenz N3B), a urethane acrylate (UA1), an isocyanuric acid ethylene oxide-modified diacrylate (manufactured by Toagosei Co., Ltd., trade name: M-215), dimethylol tricyclodecane diacrylate (manufactured by Kyoeisha Chemical Co., Ltd., trade name: Light Acrylate DCP-A), a toluene solution (solids content: 20% by mass) of a polymerization initiator (diacyl peroxide, manufactured by NOF Corporation, trade name: Perloyl L), a methyl ethyl ketone / toluene mixed solution (mass ratio: 1 / 1, solids content: 40% by mass) of polyester urethane (EU1), and a toluene solution (solids content: 30% by mass) of an ethylene vinyl acetate copolymer (manufactured by DuPont Co., Ltd., trade name: EV40W). The amount of boron salt used (solid content) was 0.86 parts by mass, the amount of urethane acrylate (UA1) used was 25.00 parts by mass, the amount of ethylene oxide isocyanurate-modified diacrylate used was 10.00 parts by mass, the amount of dimethyloltricyclodecane diacrylate used was 10.00 parts by mass, the amount of polymerization initiator used (solid content) was 5.00 parts by mass, the amount of polyester urethane (EU1) used (solid content) was 47.50 parts by mass, the amount of ethylene vinyl acetate copolymer used (solid content) was 7.50 parts by mass, and the amount of toluene used was 10.00 parts by mass.

[0095] (Polymerizable Composition A2) Polymerizable composition A2 was prepared in the same manner as polymerizable composition A1, except that 1.40 parts by mass of protocatechuic acid (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.) was further mixed.

[0096] (Polymerizable Composition A3) Polymerizable composition A3 was prepared in the same manner as polymerizable composition A1, except that 1.40 parts by mass of α-resorcylic acid (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.) was further mixed.

[0097] (Polymerizable composition B1) A polymerizable composition B1 was prepared in the same manner as for polymerizable composition A1, except that 0.86 parts by mass of the boron salt was changed to 1.00 parts by mass of a phosphorus compound (a phosphorus compound having a P═O(OH) structure, a methacryloyl group-containing phosphate, manufactured by Nippon Kayaku Co., Ltd., product name: PM-21).

[0098] (Polymerizable Composition B2) Polymerizable composition B2 was prepared in the same manner as polymerizable composition B1, except that 1.40 parts by mass of protocatechuic acid (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.) was further mixed.

[0099] (Polymerizable Composition B3) Polymerizable Composition B3 was prepared in the same manner as for Polymerizable Composition B1, except that 1.40 parts by mass of α-resorcylic acid (manufactured by Fujifilm Wako Pure Chemical Industries, Ltd.) was further mixed.

[0100] <Preparation of Evaluation Film> (Comparative Example 1) The polymerizable composition A1 described above was applied to a PET film (manufactured by Toyobo Co., Ltd., product name: Purex A3100, with release treatment, thickness: 25 μm) using a bar coater (manufactured by Yasui Seiki Co., Ltd., product name "KNIFE COATER SNC-300"), and then dried in an oven at 60°C for 3 minutes to prepare a laminated film A1 including the film-like composition A1 arranged on the PET film and having a thickness of 10 μm (average thickness at 10 locations).

[0101] The polymerizable composition B1 described above was applied to a PET film (manufactured by Toyobo Co., Ltd., product name: Purex A3100, with release treatment, thickness: 25 μm) using a bar coater (manufactured by Yasui Seiki Co., Ltd., product name "KNIFE COATER SNC-300"), and then dried in an oven at 60°C for 3 minutes to produce a laminated film B1 comprising the film-like composition B1 with a thickness of 10 μm (average thickness at 10 locations) arranged on the PET film.

[0102] With the film-like composition A1 in the laminated film A1 and the film-like composition B1 in the laminated film B1 in contact with each other, they were heated and pressed at 40°C and 0.5 MPa for 30 seconds using a thermocompression bonding device (manufactured by Takahashi Kogyo Co., Ltd.) to obtain an evaluation film comprising a film-like composition formed by integrating the film-like composition A1 and the film-like composition B1.

[0103] (Example 1) The same procedure as in Comparative Example 1 was carried out except that the polymerizable composition B1 was changed to the polymerizable composition B2, thereby obtaining an evaluation film having a film-like composition formed by integrating the film-like composition A1 and the film-like composition B2.

[0104] (Example 2) The same procedure as in Comparative Example 1 was carried out except that the polymerizable composition B1 was changed to the polymerizable composition B3, thereby obtaining an evaluation film having a film-like composition formed by integrating the film-like composition A1 and the film-like composition B3.

[0105] (Example 3) The same procedure as in Comparative Example 1 was carried out except that the polymerizable composition A1 was changed to the polymerizable composition A2, thereby obtaining an evaluation film having a film-like composition formed by integrating the film-like composition A2 and the film-like composition B1.

[0106] (Example 4) The same procedure as in Example 3 was carried out except that polymerizable composition B1 was changed to polymerizable composition B2, thereby obtaining an evaluation film having a film composition formed by integrating film composition A2 and film composition B2.

[0107] (Example 5) The same procedure as in Comparative Example 1 was carried out except that the polymerizable composition A1 was changed to the polymerizable composition A3, thereby obtaining an evaluation film having a film-like composition formed by integrating the film-like composition A3 and the film-like composition B1.

[0108] (Example 6) The same procedure as in Example 5 was carried out except that polymerizable composition B1 was changed to polymerizable composition B3, thereby obtaining an evaluation film having a film composition formed by integrating film composition A3 and film composition B3.

[0109] <Evaluation: Reaction Initiation Temperature> After peeling the PET film from the evaluation film immediately after production, the curing exothermic behavior of the film-like composition was measured by differential scanning calorimetry (DSC), and the onset temperature of the exothermic peak was obtained as an index of the polymerization reaction initiation temperature. The DSC measurement was performed under the following conditions to obtain the reaction initiation temperature T1. The evaluation film immediately after production was placed in a nylon plastic bag (manufactured by Fukusuke Kogyo Co., Ltd., product name "Nylon Poly S Type"), and the bag was then sealed using a vacuum degassing sealer to enclose the evaluation film. This bag was then placed in an aluminum light-shielding bag. The evaluation film was left in this state at 25°C for 7 days (168 hours), after which the evaluation film was removed from the light-shielding bag, and the reaction initiation temperature T2 was obtained using the same procedure as described above. The absolute value of the temperature difference between the reaction initiation temperature T1 and the reaction initiation temperature T2, |T2 - T1|, was then calculated. The results are shown in Table 1.

[0110] [DSC measurement conditions] Measurement device: PerkinElmer Japan Co., Ltd., product name "DSC8500" Sample amount: 10.0±0.2 mg Measurement temperature range: 30 to 200°C Heating rate: 30°C / min Measurement atmosphere: nitrogen

[0111]

Claims

1. A composition set comprising a first film-like composition and a second film-like composition each containing a polymerizable compound, wherein the first film-like composition contains (A) a borate anion, the second film-like composition contains (B) a phosphorus compound having a P=O(OH) structure, and at least one selected from the group consisting of the first film-like composition and the second film-like composition contains (X) at least one selected from the group consisting of an aromatic carboxylic acid having two or more hydroxy groups, a salt of the aromatic carboxylic acid, and a hydrate of the aromatic carboxylic acid.

2. The set of compositions of claim 1, wherein said aromatic carboxylic acid comprises a dihydroxybenzoic acid.

3. The composition set according to claim 1, wherein component (A) contains a borate anion having a naphthalene ring.

4. The composition set according to claim 1, wherein the component (B) comprises a (meth)acrylate compound having a P=O(OH) structure.

5. The composition set according to claim 1, wherein the content of component (B) is 0.01 to 10.00 mass % based on the total mass of the second film-like composition.

6. The composition set described in any one of claims 1 to 5, wherein at least one selected from the group consisting of the first film-like composition and the second film-like composition has a thickness of 1 to 50 μm.

7. A film having a first region and a second region each containing a polymerizable compound, wherein the first region contains (A) a borate anion, and the second region contains (B) a phosphorus compound having a P=O(OH) structure, and at least one member selected from the group consisting of the first region and the second region contains (X) at least one member selected from the group consisting of an aromatic carboxylic acid having two or more hydroxy groups, a salt of the aromatic carboxylic acid, and a hydrate of the aromatic carboxylic acid.

8. The film of claim 7, wherein the aromatic carboxylic acid comprises a dihydroxybenzoic acid.

9. The film according to claim 7, wherein the component (A) contains a borate anion having a naphthalene ring.

10. The film according to claim 7, wherein the component (B) comprises a (meth)acrylate compound having a P=O(OH) structure.

11. The film according to claim 7, wherein the content of the component (B) is 0.01 to 10.00% by mass based on the total mass of the second region.

12. The film according to any one of claims 7 to 11, having a thickness of 1 to 100 µm.

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