Low dielectric resin composition, adhesiveness imparting agent, low dielectric adhesive composition, low dielectric adhesive molded article, low dielectric adhesive and multilayer body

Abstract

This low dielectric resin composition contains a polyolefin resin. The polyolefin resin contains a styrene elastomer (A) and a cyclic olefin polymer (B) that has an alicyclic ring in the main chain. The content ratio of the styrene elastomer (A) is 30 parts by mass to 89 parts by mass relative to a total of 100 parts by mass of the styrene elastomer (A) and the cyclic olefin polymer (B).

Description

Low dielectric resin composition, adhesion promoter, low dielectric adhesive composition, low dielectric adhesive molded product, low dielectric adhesive, and laminate

[0001] The present invention relates to a low dielectric resin composition, an adhesion promoter, a low dielectric adhesive composition, a low dielectric adhesive molded product, a low dielectric adhesive, and a laminate.

[0002] 2. Description of the Related Art Wired circuit boards include, for example, a resin layer (insulating layer) containing a thermosetting resin and a conductor layer containing a metal, and are widely used in various industrial fields.

[0003] In recent years, there has been a demand for direct adhesion between a resin layer (insulating layer) and a conductor layer in a wired circuit board, and therefore it has been proposed to add an adhesion promoter to the resin layer (insulating layer) to impart adhesiveness to the resin layer (insulating layer).

[0004] As the adhesion promoter, for example, a resin having a relatively high adhesive property and a relatively low dielectric constant is used. For example, the following low dielectric constant resin has been proposed as such a resin. This low dielectric constant resin includes a maleic anhydride-grafted modified resin. As the maleic anhydride-grafted modified resin, a maleic anhydride-grafted (styrene-ethylene-butylene-styrene) block copolymer is used alone, or a maleic anhydride-grafted cyclic olefin copolymer is used alone (see, for example, Patent Document 2 (Examples 1 and 4)).

[0005] Furthermore, in wired circuit boards, it is also required that the resin layer (insulating layer) and the conductor layer are not directly bonded to each other but are bonded to each other by an interlayer adhesive.

[0006] As the interlayer adhesive, for example, a resin having a relatively high adhesiveness and a relatively low dielectric constant is used. For example, the following resin has been proposed. That is, this resin contains a mixture of a maleic acid-modified propylene-1-butene copolymer and a maleic acid-modified styrene-ethylene-propylene-styrene copolymer. More specifically, the above resin is produced by modifying a mixture of a propylene-1-butene copolymer and a styrene-ethylene-propylene-styrene copolymer with maleic acid (see, for example, Patent Document 1 (Production Example 5 and Example 1)).

[0007] JP 2018-154823 A JP 2022-043966 A

[0008] On the other hand, tackifiers and interlayer adhesives are required to have better heat resistance.

[0009] The adhesion promoter is mixed with the thermosetting resin to form a resin layer (insulating layer), and therefore the adhesion promoter is required to have improved affinity (compatibility) with the thermosetting resin.

[0010] Furthermore, the interlayer adhesive is required to have excellent adhesion to the resin layer (insulating layer), and therefore, the interlayer adhesive is also required to have improved affinity (adhesion) to the thermosetting resin.

[0011] The present invention relates to a low dielectric resin composition, an adhesion promoter, a low dielectric adhesive composition, a low dielectric adhesive molded product, a low dielectric adhesive, and a laminate, which have excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity for thermosetting resins.

[0012] The present invention [1] is a low dielectric resin composition containing a polyolefin-based resin, wherein the polyolefin-based resin contains a styrene-based elastomer (A) and a cyclic olefin-based polymer (B) having an alicyclic ring in its main chain, and the content of the styrene-based elastomer (A) is 30 parts by mass or more and 89 parts by mass or less per 100 parts by mass of the total amount of the styrene-based elastomer (A) and the cyclic olefin-based polymer (B).

[0013] The present invention [2] includes the low dielectric resin composition according to the above [1], wherein the styrene-based elastomer (A) has a weight average molecular weight of 70,000 or more and 110,000 or less.

[0014] The present invention [3] includes the low dielectric resin composition according to the above [1] or [2], wherein the styrene-based elastomer (A) contains a structural unit derived from styrene, and the content of the structural unit derived from styrene is 10% by mass or more and 40% by mass or less relative to the total amount of the styrene-based elastomer (A).

[0015] The present invention [4] includes the low dielectric resin composition according to any one of the above [1] to [3], wherein the styrene-based elastomer (A) does not contain a structural unit derived from butylene.

[0016] The present invention [5] includes the low dielectric resin composition according to any one of the above [1] to [4], wherein the glass transition temperature of the cyclic olefin polymer (B) is 100°C or higher and 140°C or lower.

[0017] The present invention [6] includes the low dielectric resin composition according to any one of the above [1] to [5], wherein the polyolefin resin is modified with a functional group-containing monomer.

[0018] The present invention [7] includes the low dielectric resin composition according to the above [6], in which the functional group-containing monomer includes a carboxy group-containing monomer.

[0019] The present invention [8] includes an adhesion promoter containing the low dielectric resin composition according to any one of the above [1] to [7].

[0020] The present invention [9] includes a low dielectric adhesive composition containing a thermosetting resin and the adhesion promoter described in [8] above, wherein the thermosetting resin contains at least one selected from the group consisting of epoxy resin, polyphenylene ether resin, fluororesin, polyimide resin, phenolic resin, melamine resin, polyolefin resin having an unsaturated double bond, and liquid crystal polymer.

[0021] The present invention

[10] includes a low dielectric adhesive molded article comprising a cured product of the low dielectric adhesive composition described in [9] above.

[0022] The present invention

[11] includes a laminate comprising an insulating layer containing the low dielectric adhesive molding described in

[10] above, and a conductor layer disposed on at least one surface of the insulating layer.

[0023] The present invention

[12] includes a low dielectric adhesive containing the low dielectric resin composition according to any one of the above [1] to [7].

[0024] The present invention

[13] includes a laminate comprising an insulating layer, a conductor layer disposed opposite the insulating layer, and an adhesive layer disposed between the insulating layer and the conductor layer and adhering the insulating layer and the conductor layer, wherein the adhesive layer comprises the low dielectric adhesive described in

[12] above.

[0025] The present invention

[14] includes a laminate comprising a first conductor layer, a second conductor layer disposed opposite the first conductor layer, and an adhesive layer disposed between the first conductor layer and the second conductor layer and adhering the first conductor layer and the second conductor layer, wherein the adhesive layer comprises the low dielectric adhesive described in

[12] above.

[0026] The low dielectric resin composition of the present invention contains a polyolefin resin as a resin component. The polyolefin resin contains a styrene elastomer (A) and a cyclic olefin polymer (B) having an alicyclic ring in the main chain in specific proportions. Therefore, the low dielectric resin composition has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility and adhesion) with thermosetting resins.

[0027] The adhesion promoter, low dielectric adhesive composition, and low dielectric adhesive molded article of the present invention contain the above-mentioned low dielectric resin composition, and therefore have excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility and adhesion) for thermosetting resins.

[0028] The laminate of the present invention has an insulating layer. The insulating layer contains the low dielectric adhesive molded article. Therefore, in the laminate, the insulating layer has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility, adhesion) with thermosetting resins.

[0029] The low dielectric adhesive of the present invention includes the low dielectric resin composition described above. Therefore, the low dielectric adhesive has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility and adhesion) with thermosetting resins.

[0030] The laminate of the present invention also has an adhesive layer. The adhesive layer contains the low dielectric adhesive. Therefore, in the laminate, the adhesive layer has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility and adhesion) with thermosetting resins.

[0031] Fig. 1 is a schematic diagram showing a copper-clad laminate as a first embodiment of the laminate. Fig. 2 is a schematic diagram showing a circuit board as a second embodiment of the laminate. Fig. 3 is a schematic diagram showing a copper-clad laminate as a third embodiment of the laminate. Fig. 4 is a schematic diagram showing a circuit board as a fourth embodiment of the laminate. Fig. 5A is a process diagram for producing a circuit board as a fifth embodiment of the laminate, showing the step of preparing a carrier-attached copper foil, Fig. 5B is a process diagram for forming a first resist layer, and Fig. 5C is a process diagram for forming a first conductor layer. Fig. 6D is a process diagram for producing a circuit board following Fig. 5, showing the step of removing the first resist layer, Fig. 6E is a process diagram for removing the copper foil exposed from the first conductor layer, Fig. 6F is a process diagram for laminating an adhesive layer, and Fig. 6G is a process diagram for laminating the carrier-attached copper foil on the adhesive layer. Fig. 7H shows a step of peeling off the carrier layer in a process diagram for manufacturing a circuit board subsequent to Fig. 6, Fig. 7I shows a step of forming via holes, Fig. 7J shows a step of forming via fills, Fig. 7K shows a step of forming a second resist layer, Fig. 8L shows a step of forming a second conductor layer in a process diagram for manufacturing a circuit board subsequent to Fig. 7, Fig. 8M shows a step of removing the second resist layer, Fig. 8N shows a step of removing the copper foil exposed from the second conductor layer, and Fig. 8O shows a step of peeling off the carrier layer.

[0032] 1. Low dielectric resin composition The low dielectric resin composition is a resin composition contained in, for example, an insulating layer (described later) or an adhesive layer (described later) in the laminate described later. The low dielectric resin composition contains a polyolefin resin.

[0033] The polyolefin resin contains a styrene elastomer (A) and a cyclic olefin polymer (B) having an alicyclic ring in the main chain.

[0034] (1) Styrene-Based Elastomers Examples of the styrene-based elastomer (A) include copolymers of styrene and chain olefins.

[0035] Examples of the chain olefin include chain olefins having 2 to 8 carbon atoms. Examples of the chain olefins having 2 to 8 carbon atoms include ethylene, propylene, butylene (butene), pentene, hexene, octene, and 3-methyl-1-pentene. These can be used alone or in combination of two or more. Preferred examples of the chain olefin include ethylene alone, propylene alone, and a combination of ethylene and propylene. More preferred examples of the chain olefin include a combination of ethylene and propylene.

[0036] The styrene-based elastomer (A) is produced by a known method. For example, styrene and a chain olefin are polymerized in the presence of a known initiator (e.g., an alkyllithium compound). This produces the styrene-based elastomer (A). The polymerization conditions are appropriately set depending on the purpose and application.

[0037] The styrene-based elastomer (A) contains structural units derived from styrene and structural units derived from a chain olefin. Preferably, the styrene-based elastomer (A) consists of structural units derived from styrene and structural units derived from a chain olefin.

[0038] From the viewpoint of affinity for thermosetting resins, the content of the structural units derived from styrene is, for example, 5% by mass or more, preferably 10% by mass or more, more preferably 15% by mass or more, based on the total amount of the styrene-based elastomer (A). From the viewpoint of low dielectric properties, the content of the structural units derived from styrene is, for example, 50% by mass or less, preferably 40% by mass or less, more preferably 30% by mass or less, based on the total amount of the styrene-based elastomer (A).

[0039] From the viewpoint of low dielectric properties, the content of the structural units derived from the chain olefin is, for example, 50% by mass or more, preferably 60% by mass or more, more preferably 70% by mass or more, based on the total amount of the styrene-based elastomer (A). From the viewpoint of affinity with thermosetting resins, the content of the structural units derived from the chain olefin is, for example, 95% by mass or less, preferably 90% by mass or less, more preferably 85% by mass or less, based on the total amount of the styrene-based elastomer (A).

[0040] The content ratio of the structural unit derived from styrene and the content ratio of the structural unit derived from the chain olefin are calculated based on the formulation of the polymerization raw materials of the styrene-based elastomer (A). More specifically, the content ratio of the structural unit derived from styrene is calculated as the ratio of styrene to the total amount of the polymerization raw materials (styrene and chain olefin). Furthermore, the content ratio of the structural unit derived from the chain olefin is calculated as the ratio of the chain olefin to the total amount of the polymerization raw materials (styrene and chain olefin).

[0041] The styrene-based elastomer (A) preferably contains a structural unit derived from ethylene as the structural unit derived from the chain olefin. The content of the structural unit derived from ethylene is appropriately set depending on the purpose and application.

[0042] The styrene-based elastomer (A) preferably contains a structural unit derived from propylene as the structural unit derived from the chain olefin, and the content of the structural unit derived from propylene is appropriately set depending on the purpose and application.

[0043] Furthermore, the styrene-based elastomer (A) may contain, as necessary, a structural unit derived from butylene as a structural unit derived from a chain olefin, and the content of the structural unit derived from butylene is appropriately set depending on the purpose and application.

[0044] On the other hand, when the content of structural units derived from styrene in the styrene-based elastomer (A) is relatively low, the content of structural units derived from butylene is preferably relatively low from the viewpoint of affinity with the thermosetting resin.

[0045] In other words, when the styrene-based elastomer (A) contains structural units derived from butylene, the content of structural units derived from styrene is preferably set to a relatively high level.

[0046] From the viewpoint of affinity for thermosetting resins, when the styrene-based elastomer (A) contains structural units derived from butylene, the content of the structural units derived from styrene is, for example, 10% by mass or more, preferably 20% by mass or more, particularly preferably 25% by mass or more, based on the total amount of the styrene-based elastomer (A), and preferably 90% by mass or less, more preferably 85% by mass or less, based on the total amount of the styrene-based elastomer (A).

[0047] It is particularly preferred that the styrene-based elastomer (A) does not contain a structural unit derived from butylene. More specifically, when the content of structural units derived from styrene in the styrene-based elastomer (A) is less than 25 mass%, the styrene-based elastomer (A) preferably does not contain a structural unit derived from butylene as a structural unit derived from a chain olefin.

[0048] In other words, when the content of structural units derived from styrene in the styrene-based elastomer (A) is relatively high (e.g., 25 mass% or more), the styrene-based elastomer (A) may contain structural units derived from butylene. Conversely, when the content of structural units derived from styrene is relatively high, the styrene-based elastomer (A) may not contain structural units derived from butylene.

[0049] From the viewpoint of affinity for thermosetting resins, the styrene-based elastomer (A) particularly preferably contains structural units derived from styrene in a proportion of 25% by mass or more and does not contain structural units derived from butylene, or contains structural units derived from styrene in a proportion of 25% by mass or more and contains structural units derived from butylene, or contains structural units derived from styrene in a proportion of less than 25% by mass and does not contain structural units derived from butylene.

[0050] More specific examples of the styrene-based elastomer (A) include styrene-ethylene-propylene copolymer (SEP), styrene-ethylene-propylene-styrene copolymer (SEPS), styrene-ethylene-ethylene-propylene-styrene block copolymer (SEEPS), styrene-butadiene-styrene copolymer (SBS), styrene-ethylene-butylene-styrene copolymer (SEBS), and styrene-isobutylene-styrene copolymer (SIBS). Examples of copolymers include random copolymers and block copolymers (the same applies hereinafter). These can be used alone or in combination of two or more types.

[0051] In view of affinity for thermosetting resins, preferred examples of the styrene elastomer (A) include styrene-ethylene-propylene copolymer (SEP), styrene-ethylene-propylene-styrene copolymer (SEPS), styrene-butadiene-styrene copolymer (SBS), and styrene-ethylene-butylene-styrene copolymer (SEBS).

[0052] From the viewpoints of heat resistance, low dielectric properties, and affinity for thermosetting resins, more preferred examples of the styrene-based elastomer (A) include styrene-ethylene-propylene-styrene copolymer (SEPS) and styrene-ethylene-butylene-styrene copolymer (SEBS).

[0053] From the viewpoints of heat resistance, low dielectric properties, and affinity for thermosetting resins, the styrene-based elastomer (A) is more preferably a styrene-based elastomer (A) that does not contain a structural unit derived from butylene, and more specifically, a styrene-ethylene-propylene-styrene copolymer (SEPS) is mentioned.

[0054] From the viewpoints of heat resistance, low dielectric properties, and affinity for thermosetting resins, the styrene-based elastomer (A) is more preferably a styrene-based elastomer (A) containing structural units derived from butylene and a relatively large amount of structural units derived from styrene. In such a case, the content of the structural units derived from butylene is preferably 20% by mass or more, particularly preferably 25% by mass or more, based on the total amount of the styrene-based elastomer (A), as described above.

[0055] That is, more preferred examples of the styrene-based elastomer (A) include a styrene-based elastomer (A) that does not contain structural units derived from butylene, and a styrene-based elastomer (A) that contains structural units derived from butylene and 25 mass% or more of structural units derived from styrene.

[0056] Furthermore, from the viewpoints of heat resistance, low dielectric properties, and affinity for thermosetting resins, particularly preferred is a styrene-based elastomer (A) that does not contain a structural unit derived from butylene, and more specifically, a styrene-ethylene-propylene-styrene copolymer (SEPS) is mentioned.

[0057] From the viewpoint of low dielectric properties, the weight average molecular weight of the styrene elastomer (A) is, for example, 10,000 or more, preferably 30,000 or more, more preferably 50,000 or more, even more preferably 70,000 or more, and particularly preferably 90,000 or more. From the viewpoint of low dielectric properties and the stability of the dilution liquid (varnish) described below, the weight average molecular weight of the styrene elastomer (A) is, for example, 500,000 or less, preferably 300,000 or less, more preferably 200,000 or less, even more preferably 110,000 or less, and particularly preferably 100,000 or less.

[0058] The weight average molecular weight of the styrene elastomer (A) is measured by gel permeation chromatography as a molecular weight converted into standard polystyrene.

[0059] The styrene-based elastomer (A) may be used alone or in combination of two or more kinds. Commercially available styrene-based elastomers may also be used as the styrene-based elastomer (A).

[0060] Commercially available styrene elastomers (A) include, for example, the SEPTON series (manufactured by Kuraray), the Kraton series (manufactured by Kraton Polymer Japan), and the Tuftec series (manufactured by Asahi Kasei).

[0061] (2) Cycloolefin Polymer Examples of the cycloolefin polymer (B) having an alicyclic ring in the main chain include polymers of cycloolefins and hydrogenated products thereof.

[0062] Examples of cyclic olefins include cyclic hydrocarbon compounds containing an ethylenically unsaturated bond. Examples of cyclic hydrocarbon compounds include cyclic hydrocarbon compounds having 6 to 30 carbon atoms. More specific examples of cyclic olefins include bicyclo[2.2.1]-hept-2-ene (also known as norbornene) and its derivatives, tricyclo[4.3.0.1]-hept-2-ene, and the like. ２．５ ]-3-decene and its derivatives, tricyclo[4.4.0.1 ２．５ ]-3-decene and its derivatives, tetracyclo[4.4.0.1 ２，５ .1 ７，１０ ]-3-dodecene and its derivatives, pentacyclo[6.5.1.1 ３．６ .0 ２．７ .0 ９．１３ ]-4-pentadecene and its derivatives, hexacyclo[6.6.1.1 ３．６ .1 １０．１３ .0 ２．７ .0 ９．１４ ]-4-heptadecene and its derivatives, and heptacyclo[8.7.0.1 ２．９ .1 ４．７ .1 １１．１７ .0 ３．８ .0 １２．１６]-5-eicosene and its derivatives. These can be used alone or in combination of two or more. Preferably, bicyclo[2.2.1]-hept-2-ene (also known as norbornene) is used.

[0063] The cyclic olefin polymer is produced by a known method. For example, the cyclic olefin is subjected to ring-opening metathesis polymerization by a known method. This results in a ring-opening metathesis polymer of the cyclic olefin. The polymerization conditions are appropriately set depending on the purpose and application.

[0064] If necessary, the ring-opening metathesis polymer of cyclic olefin can be hydrogenated by a known method to obtain a hydrogenated product of the ring-opening metathesis polymer of cyclic olefin.

[0065] The cyclic olefin polymer and its hydrogenated product can be used alone or in combination of two or more kinds.

[0066] Examples of the cycloolefin polymer (B) having an alicyclic ring in the main chain include copolymers of cycloolefins and chain olefins (cycloolefin copolymers), and hydrogenated products thereof.

[0067] Examples of the cyclic olefin include the above-mentioned cyclic hydrocarbon compounds, and preferred are tetracyclo[4.4.0.1 ２，５ .1 ７，１０ ]-3-dodecene and its derivatives, and more preferably tetracyclo[4.4.0.1 ２，５ .1 ７，１０ ]-3-dodecene.

[0068] Examples of the chain olefin include the chain olefins having 2 to 8 carbon atoms described above, and preferably ethylene.

[0069] The copolymer of a chain olefin and a cyclic olefin is produced by a known method. For example, the chain olefin and the cyclic olefin are polymerized in the presence of a known catalyst (e.g., a vanadium-based catalyst, an aluminum-based catalyst, or a metallocene catalyst). This results in a copolymer of a chain olefin and a cyclic olefin. The polymerization conditions are appropriately set depending on the purpose and application.

[0070] If necessary, the copolymer of the chain olefin and the cyclic olefin can be hydrogenated by a known method, thereby obtaining a hydrogenated copolymer of the chain olefin and the cyclic olefin.

[0071] The copolymer of a chain olefin and a cyclic olefin and its hydrogenated product can be used alone or in combination of two or more kinds.

[0072] The cyclic olefin polymer (B) is preferably a copolymer of a chain olefin and a cyclic olefin. In other words, the cyclic olefin polymer (B) preferably contains structural units derived from a chain olefin and structural units derived from a cyclic olefin. More preferably, the cyclic olefin polymer (B) is composed of structural units derived from a chain olefin and structural units derived from a cyclic olefin.

[0073] The content ratio of the structural unit derived from the chain olefin and the content ratio of the structural unit derived from the cyclic olefin are appropriately set depending on the purpose and application. For example, in order to adjust the weight average molecular weight and glass transition temperature of the cyclic olefin polymer (B), the content ratio of the structural unit derived from the chain olefin and the content ratio of the structural unit derived from the cyclic olefin are appropriately set.

[0074] From the viewpoint of heat resistance, the weight average molecular weight of the cyclic olefin polymer (B) is, for example, 10,000 or more, preferably 50,000 or more, more preferably 80,000 or more, even more preferably 100,000 or more, particularly preferably 112,000 or more. The weight average molecular weight of the cyclic olefin polymer (B) is, for example, 500,000 or less, preferably 300,000 or less, more preferably 200,000 or less, even more preferably 150,000 or less, particularly preferably 118,000 or less.

[0075] The weight average molecular weight of the cyclic olefin polymer (B) is measured by gel permeation chromatography as a molecular weight converted into standard polystyrene.

[0076] From the viewpoint of heat resistance, the glass transition temperature of the cyclic olefin polymer (B) is, for example, 60° C. or higher, preferably 70° C. or higher, more preferably 80° C. or higher, even more preferably 90° C. or higher, and particularly preferably 100° C. or higher. Furthermore, from the viewpoint of the stability of the dilution liquid (varnish) described below and the affinity (compatibility) with the thermosetting resin, the glass transition temperature of the cyclic olefin polymer (B) is, for example, 200° C. or lower, preferably 175° C. or lower, more preferably 150° C. or lower, even more preferably 140° C. or lower, even more preferably 130° C. or lower, still more preferably 120° C. or lower, and particularly preferably 110° C. or lower.

[0077] The glass transition temperature of the cyclic olefin polymer (B) is measured in accordance with JIS K 7122 (2012).

[0078] The cyclic olefin polymer (B) may be used alone or in combination of two or more kinds. Commercially available cyclic olefin polymers may also be used as the cyclic olefin polymer (B).

[0079] Commercially available cyclic olefin polymers (B) include, for example, the ZEONEX series (hydrogenated cyclic monomer polymers, manufactured by Zeon Corporation), the ZEONOR series (hydrogenated cyclic monomer polymers, manufactured by Zeon Corporation), and the APEL series (copolymers of chain olefins and cyclic olefins, manufactured by Mitsui Chemicals).

[0080] (3) Blending ratio The polyolefin resin can be obtained by mixing the styrene elastomer (A) and the cyclic olefin polymer (B) by a known method. Preferably, the polyolefin resin can be obtained by melt-kneading the styrene elastomer (A) and the cyclic olefin polymer (B) in a twin-screw extruder.

[0081] In the polyolefin resin, the blending ratio of the styrene elastomer (A) and the cyclic olefin polymer (B) is adjusted to fall within a specific range.

[0082] More specifically, from the viewpoint of affinity for thermosetting resins, the content of the styrene elastomer (A) is 30 parts by mass or more, preferably 35 parts by mass or more, more preferably 40 parts by mass or more, and even more preferably 45 parts by mass or more, per 100 parts by mass of the total of the styrene elastomer (A) and the cyclic olefin polymer (B). Also, from the viewpoint of heat resistance, the content of the styrene elastomer (A) is 89 parts by mass or less, preferably 85 parts by mass or less, more preferably 80 parts by mass or less, even more preferably 70 parts by mass or less, and particularly preferably 60 parts by mass or less, per 100 parts by mass of the total of the styrene elastomer (A) and the cyclic olefin polymer (B).

[0083] That is, from the viewpoint of heat resistance, the content of the cyclic olefin polymer (B) is 11 parts by mass or more, preferably 15 parts by mass or more, more preferably 20 parts by mass or more, even more preferably 30 parts by mass or more, and particularly preferably 40 parts by mass or more, per 100 parts by mass of the total of the styrene elastomer (A) and the cyclic olefin polymer (B). Also, from the viewpoint of affinity for thermosetting resins, the content of the cyclic olefin polymer (B) is 70 parts by mass or less, preferably 65 parts by mass or less, more preferably 60 parts by mass or less, and even more preferably 55 parts by mass or less, per 100 parts by mass of the total of the styrene elastomer (A) and the cyclic olefin polymer (B).

[0084] When the polyolefin resin contains the styrene elastomer (A) and the cyclic olefin polymer (B) having an alicyclic ring in the main chain in the above-mentioned specific ratio, the low dielectric resin composition has excellent adhesiveness and low dielectric properties, as well as excellent heat resistance and, in addition, excellent affinity (compatibility, adhesion) for thermosetting resins.

[0085] The content of the cyclic olefin polymer (B) relative to 100 parts by mass of the styrene elastomer (A) is, for example, 12 parts by mass or more, preferably 25 parts by mass or more, more preferably 50 parts by mass or more, and the content of the cyclic olefin polymer (B) relative to 100 parts by mass of the styrene elastomer (A) is, for example, 235 parts by mass or less, preferably 185 parts by mass or less, more preferably 150 parts by mass or less.

[0086] When the ratio of the styrene-based elastomer (A) to the cyclic olefin-based polymer (B) is within the above range, the low dielectric resin composition has excellent adhesiveness and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility, adhesion) with thermosetting resins.

[0087] (4) Other Olefin-Based Polymers The polyolefin-based resin may contain other olefin-based polymers (C) as needed. The other olefin-based polymers (C) are known olefin polymers excluding the styrene-based elastomer (A) and the cyclic olefin-based polymer (B).

[0088] Examples of other olefin-based polymers (C) include polyethylene, polypropylene, polyisobutylene, poly-1-butene, poly-4-methylpentene, ethylene-propylene copolymer, propylene-butene copolymer, ethylene-butene copolymer, ethylene-4-methyl-1-pentene copolymer, propylene-4-methyl-1-pentene copolymer, butylene-4-methyl-1-pentene copolymer, ethylene-hexene copolymer, and ethylene-vinyl acetate copolymer. These can be used alone or in combination of two or more. The content ratio of the other olefin-based polymers can be appropriately set within a range that does not impair the excellent effects of the present invention.

[0089] The content of the other olefin polymer (C) relative to the total amount of the polyolefin resin is, for example, 30% by mass or less, preferably 20% by mass or less, more preferably 10% by mass or less, and particularly preferably 0% by mass. In other words, the polyolefin resin preferably does not contain the other olefin polymer (C). In other words, the polyolefin resin preferably comprises a styrene elastomer (A) and a cyclic olefin polymer (B).

[0090] (5) Modified Polyolefin Resin The polyolefin resin may be an unmodified polyolefin resin or a modified polyolefin resin.

[0091] The unmodified polyolefin resin is a polyolefin resin that contains a styrene elastomer (A) and a cyclic olefin polymer (B) and is not modified with a modifier (described later). The modified polyolefin resin is a polyolefin resin that contains a styrene elastomer (A) and a cyclic olefin polymer (B) and is modified with a modifier (described later). From the viewpoint of adhesion to metals (for example, the conductor layer described later), modified polyolefin resins are preferred.

[0092] The modified polyolefin resin can be obtained, for example, by modifying a polyolefin resin with a known modifying agent.

[0093] Examples of the modifying agent include functional group-containing monomers. Examples of the functional group-containing monomer include carboxy group-containing monomers, sulfonyl group-containing monomers, amino group-containing monomers, hydroxyl group-containing monomers, glycidyl group-containing monomers, and halogen-containing monomers. These can be used alone or in combination of two or more. From the viewpoint of adhesion to metals (e.g., the conductor layer described below), preferred examples of the functional group-containing monomer include carboxy group-containing monomers.

[0094] Examples of the carboxyl group-containing monomer include unsaturated acids. Examples of the unsaturated acids include maleic acid, fumaric acid, itaconic acid, and (meth)acrylic acid. Examples of the unsaturated acids include anhydrides of these acids. These can be used alone or in combination of two or more. Examples of the carboxyl group-containing monomer include preferably maleic acid and its anhydride, more preferably maleic anhydride.

[0095] That is, examples of modified polyolefin resins include acid-modified polyolefin resins. Examples of acid-modified polyolefin resins include (anhydride) maleic acid-modified polyolefin resins, (anhydride) fumaric acid-modified polyolefin resins, (anhydride) itaconic acid-modified polyolefin resins, and (meth)acrylic acid-modified polyolefin resins. These can be used alone or in combination of two or more. Preferred modified polyolefin resins include maleic anhydride-modified polyolefin resins.

[0096] The method for obtaining the modified polyolefin resin is not particularly limited. For example, an unmodified polyolefin resin is reacted with a modifier by a known method. For example, the modifier is added when the styrene elastomer (A) and the cyclic olefin polymer (B) are mixed. Alternatively, for example, the modifier is added to the styrene elastomer (A) and / or the cyclic olefin polymer (B) before the above mixing, and the styrene elastomer (A) and / or the cyclic olefin polymer (B) are reacted with the modifier. Preferably, the modifier is added when the styrene elastomer (A) and the cyclic olefin polymer (B) are mixed.

[0097] The amount of the modifier to be added is appropriately determined depending on the purpose and application. For example, when a carboxyl group-containing monomer is used as the modifier, the amount of the carboxyl group-containing monomer is, for example, 0.1 parts by mass or more, preferably 0.5 parts by mass or more, per 100 parts by mass of the styrene elastomer (A) and the cyclic olefin polymer (B). Furthermore, the amount of the carboxyl group-containing monomer is, for example, 20 parts by mass or less, preferably 10 parts by mass or less, more preferably 5 parts by mass or less, per 100 parts by mass of the styrene elastomer (A) and the cyclic olefin polymer (B).

[0098] In addition, when a carboxyl group-containing monomer is used as a modifying agent, a modifying initiator is added as necessary.The modifying initiator can be, for example, a known graft catalyst, more specifically, a known peroxide and a known azo compound.The mixing ratio of the modifying initiator can be appropriately set according to the purpose and application.

[0099] The styrene elastomer (A), the cyclic olefin polymer (B), and the modifier are mixed and reacted to obtain a modified polyolefin resin. The reaction conditions are not particularly limited and are appropriately set depending on the type and amount of the modifier.

[0100] The modified polyolefin resin contains a styrene elastomer (A) modified with a modifier (modified styrene elastomer) and a cyclic olefin polymer (B) modified with a modifier (modified cyclic olefin polymer). The modified polyolefin resin can improve adhesion to metals (e.g., the conductor layer described below).

[0101] When a carboxyl group-containing monomer is used as the modifier, the acid value of the modified polyolefin resin is, for example, 0.1 mgKOH / g or more, preferably 0.5 mgKOH / g or more. The acid value of the modified polyolefin resin is, for example, 100 mgKOH / g or less, preferably 60 mgKOH / g or less. The acid value is measured in accordance with JIS K 2501 (2003).

[0102] (6) Non-polyolefin resin In the low dielectric resin composition, the resin component may contain a non-polyolefin resin in addition to the polyolefin resin described above. The non-polyolefin resin is a known resin other than the polyolefin resin. Examples of the non-polyolefin resin include (meth)acrylic resins. These may be used alone or in combination of two or more.

[0103] From the viewpoint of affinity with thermosetting resins, the resin component in the low dielectric resin composition preferably does not contain a non-polyolefin resin, i.e., the resin component in the low dielectric resin composition preferably consists of the above-mentioned polyolefin resin.

[0104] (7) Organic Solvent The low dielectric resin composition may be diluted with an organic solvent. More specifically, the low dielectric resin composition may be dissolved and / or dispersed in an organic solvent. That is, a diluted solution (solution and / or dispersion) of the low dielectric resin composition may be prepared.

[0105] The solid content concentration of the diluted solution (solution and / or dispersion) of the low dielectric resin composition is, for example, 5% by mass or more, preferably 10% by mass or more, and the solid content concentration of the diluted solution (solution and / or dispersion) of the low dielectric resin composition is, for example, 50% by mass or less, preferably 30% by mass or less.

[0106] (8) Additives The low dielectric resin composition and / or its diluted solution may contain known additives. Examples of additives include plasticizers, antifoaming agents, leveling agents, mildew inhibitors, rust inhibitors, matting agents, flame retardants, thixotropic agents, tackifiers, thickeners, lubricants, antistatic agents, surfactants, reaction retarders, antioxidants, UV absorbers, hydrolysis inhibitors, weathering stabilizers, heat stabilizers, dyes, inorganic pigments, organic pigments, curing agents, crosslinking agents, thermal initiators (thermal radical polymerization initiators), silane coupling agents, anti-tack agents, inorganic particles, and organic particles. These additives may be used alone or in combination of two or more. The proportion and timing of the additives may be appropriately determined depending on the purpose and application.

[0107] (9) Effects The low dielectric resin composition contains a polyolefin resin as a resin component. The polyolefin resin contains a styrene elastomer (A) and a cyclic olefin polymer (B) having an alicyclic ring in the main chain in specific proportions. Therefore, the low dielectric resin composition has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility and adhesion) with thermosetting resins.

[0108] The low dielectric resin composition (solid content) has a relative dielectric constant (measurement condition: 10 GHz) of, for example, 1.5 or more, preferably 1.9 or more. The low dielectric resin composition (solid content) has a relative dielectric constant (measurement condition: 10 GHz) of, for example, 3.0 or less, preferably 2.5 or less. The relative dielectric constant is measured in accordance with the examples described later (the same applies hereinafter).

[0109] The dielectric loss tangent (measurement condition: 10 GHz) of the low dielectric adhesive composition (solid content) is, for example, 0.0001 or more, preferably 0.0003 or more. The dielectric loss tangent (measurement condition: 10 GHz) of the low dielectric adhesive composition (solid content) is, for example, 0.004 or less, preferably 0.002 or less. The relative dielectric constant is measured in accordance with the examples described later.

[0110] Such a low dielectric resin composition is suitably used as an adhesion promoter and / or a low dielectric adhesive in the production of laminates.

[0111] 2. Laminate A laminate is a circuit board or a circuit board material. A circuit board is, for example, a laminate including a conductor layer (circuit layer) having a circuit pattern. A circuit board material is a laminate that can be processed into a circuit board. More specifically, a circuit board material is, for example, a laminate including a conductor layer (non-circuit layer) that does not have a circuit pattern and that can be processed to form a circuit pattern. An example of a circuit board material is a copper-clad laminate.

[0112] The laminate is produced by using a low dielectric resin composition. A method for producing a circuit board or a circuit board material as a laminate using the low dielectric resin composition will be described in detail below.

[0113] (1) First Embodiment Fig. 1 is a schematic cross-sectional view showing a copper-clad laminate as a first embodiment of the laminate. In the first embodiment, the low dielectric resin composition described above is used as an adhesion promoter.

[0114] More specifically, in FIG. 1 , the copper-clad laminate 1 comprises an adhesive insulating layer (hereinafter referred to as an adhesive insulating layer) 2 and a conductor layer 4 disposed on at least one side of the adhesive insulating layer 2.

[0115] The adhesive insulating layer 2 contains a resin molded product having low dielectric properties and adhesive properties (hereinafter referred to as a low dielectric adhesive molded product). The adhesive insulating layer 2 is preferably made of a low dielectric adhesive molded product or an impregnated base material and a low dielectric adhesive molded product.

[0116] The low dielectric adhesive molded product is, for example, a molded and cured product of the following low dielectric adhesive composition (molding material).

[0117] The low dielectric adhesive composition (molding material) contains, for example, a thermosetting resin (uncured thermosetting resin) and an adhesion promoter (additive).

[0118] Examples of thermosetting resins include epoxy resins, polyphenylene ether resins, fluororesins, polyimide resins, phenolic resins, melamine resins, polyolefin resins having unsaturated double bonds, and liquid crystal polymers. These may be used alone or in combination of two or more. A preferred example of the thermosetting resin is polyphenylene ether resin.

[0119] In other words, the thermosetting resin includes at least one selected from the group consisting of epoxy resin, polyphenylene ether resin, fluororesin, polyimide resin, phenolic resin, melamine resin, polyolefin resin having an unsaturated double bond, and liquid crystal polymer. The thermosetting resin preferably includes a polyphenylene ether resin. The thermosetting resin preferably consists of a polyphenylene ether resin.

[0120] The adhesion promoter (additive) contains the above-mentioned low dielectric resin composition, and preferably consists of the above-mentioned low dielectric resin composition.

[0121] The low dielectric adhesive composition (molding material) is prepared, for example, by mixing a thermosetting resin and an adhesion promoter by a known method.

[0122] The blending ratio of the thermosetting resin and the adhesion promoter is not particularly limited, but is, for example, 1 part by mass or more, preferably 5 parts by mass or more, of the adhesion promoter per 100 parts by mass of the thermosetting resin, and for example, 400 parts by mass or less, preferably 150 parts by mass or less, of the adhesion promoter per 100 parts by mass of the thermosetting resin.

[0123] The amount of the thermosetting resin relative to the total amount of the thermosetting resin and the adhesion promoter is, for example, 20 mass% or more, or preferably 40 mass% or more, and the amount of the thermosetting resin relative to the total amount of the thermosetting resin and the adhesion promoter is, for example, 99 mass% or less, or preferably 95 mass% or less.

[0124] The amount of the adhesion imparter relative to the total amount of the thermosetting resin and the adhesion imparter is, for example, 1 mass % or more, or preferably 5 mass % or more, and the amount of the adhesion imparter relative to the total amount of the thermosetting resin and the adhesion imparter is, for example, 80 mass % or less, or preferably 60 mass % or less.

[0125] In addition to the thermosetting resin and adhesion promoter, the low dielectric adhesive composition (molding material) may contain additives. Examples of additives include plasticizers, antifoaming agents, leveling agents, mildew inhibitors, rust inhibitors, matting agents, flame retardants, thixotropic agents, tackifiers, thickeners, lubricants, antistatic agents, surfactants, reaction retarders, antioxidants, UV absorbers, hydrolysis inhibitors, weathering stabilizers, heat stabilizers, dyes, inorganic pigments, organic pigments, curing agents, crosslinking agents, thermal initiators (thermal radical polymerization initiators), silane coupling agents, anti-tack agents, inorganic particles, and organic particles. These additives can be used alone or in combination. The proportion and timing of additive addition can be determined appropriately depending on the purpose and application.

[0126] From the viewpoint of thermosetting properties, the low dielectric adhesive composition (molding material) preferably contains a thermal initiator. Examples of thermal initiators include organic peroxides. Examples of organic peroxides include dicumyl peroxide, 1-(2-t-butylperoxyisopropyl)-1-isopropylbenzene, 1-(2-t-butylperoxyisopropyl)-3-isopropylbenzene, 1,3-bis(t-butylperoxyisopropyl)benzene, 2,5-dimethyl-2.5-bis(t-butylperoxy)hexane, and 2,5-dimethyl-2,5-(tert-butylperoxy)hexyne-3. These can be used alone or in combination of two or more.

[0127] The amount of the thermal initiator added is, for example, 0.1 parts by mass or more, preferably 1.0 part by mass or more, relative to 100 parts by mass of the total amount of the resin components of the adhesion promoter (low dielectric resin composition). The amount of the thermal initiator added is, for example, 10 parts by mass or less, preferably 5 parts by mass or less, relative to 100 parts by mass of the total amount of the resin components of the adhesion promoter (low dielectric resin composition).

[0128] For example, when the adhesive insulating layer 2 is made of a low dielectric adhesive molding, the adhesive insulating layer 2 is formed by molding and curing a low dielectric adhesive composition (molding material) by a known method.

[0129] For example, the low dielectric adhesive composition (molding material) is applied to a known substrate (e.g., a copper plate and a release liner) and dried as necessary to obtain a coating film of the low dielectric adhesive composition (molding material). The coating film is then cured (thermocured) by heating.

[0130] This results in a low dielectric adhesive molded product (adhesive insulating layer 2) made of a cured product of the low dielectric adhesive composition (molding material).

[0131] Also, for example, when the adhesive insulating layer 2 consists of an impregnated base material and a low dielectric adhesive molding, the adhesive insulating layer 2 is formed by impregnating the impregnated base material with a low dielectric adhesive composition (molding material), drying and curing the composition.

[0132] For example, a low dielectric adhesive composition (molding material) is impregnated into a glass cloth as an impregnation substrate, and dried as necessary. Then, the glass cloth and the low dielectric adhesive composition (molding material) impregnated into the glass cloth are cured (thermoset) by heating.

[0133] This results in a low dielectric adhesive molded product (adhesive insulating layer 2) containing the glass cloth and the cured product of the low dielectric adhesive composition (molding material).

[0134] The shape and size of the low dielectric adhesive molding (adhesive insulating layer 2) are appropriately determined depending on the purpose and application.

[0135] The conductor layer 4 is a thin film made of a known conductive material. An example of the conductive material is copper. The conductor layer 4 is formed by a known film formation method. The thickness of the conductor layer 4 is adjusted to be, for example, relatively thin. This allows the circuit pattern to be formed by a subtractive method. The thickness of the conductor layer 4 is, for example, 50 μm or less.

[0136] The conductor layer 4 is disposed on at least one surface of the adhesive insulating layer 2. The conductor layer 4 is preferably disposed on both surfaces of the adhesive insulating layer 2. In FIG.

[0137] More specifically, the conductor layer 4 is formed by a known method so as to be in contact with the surface of the adhesive insulating layer 2. In this way, the conductor layer 4 is adhered to the adhesive insulating layer 2. As a result, a copper-clad laminate 1 comprising the adhesive insulating layer 2 and the conductor layer 4 is obtained.

[0138] The method for obtaining the copper-clad laminate 1 is not limited to the above. For example, first, a conductor layer 4 made of a metal foil is prepared. Next, a low dielectric adhesive composition (molding material) is applied to the conductor layer 4, and dried as necessary. The low dielectric adhesive composition (molding material) is then thermally cured. This allows the adhesive insulating layer 2 to be formed on the surface of the conductor layer 4. As a result, a copper-clad laminate 1 is obtained, which includes the adhesive insulating layer 2 and the conductor layer 4 in contact with the surface of the adhesive insulating layer 2.

[0139] The copper-clad laminate 1 has an insulating layer 2. The insulating layer 2 contains the low-dielectric adhesive molding. Therefore, in the copper-clad laminate 1, the insulating layer 2 has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility, adhesion) with thermosetting resins, thereby providing excellent strength.

[0140] The adhesion promoter (additive), low dielectric adhesive composition (molding material), and low dielectric adhesive molded product (adhesive insulating layer 2) contain the low dielectric resin composition. Therefore, the adhesion promoter (additive), low dielectric adhesive composition (molding material), and low dielectric adhesive molded product (adhesive insulating layer 2) have excellent adhesiveness and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility) with thermosetting resins, and therefore excellent strength.

[0141] (2) Second Embodiment Fig. 2 is a schematic cross-sectional view showing a circuit board as a second embodiment of the laminate. In the second embodiment, similarly to the first embodiment, the low dielectric resin composition described above is used as an adhesion promoter.

[0142] More specifically, the copper clad laminate 1 of the first embodiment described above can be processed to form a circuit board 11. That is, the conductor layer 4 of the copper clad laminate 1 can be etched by a known method to form a circuit 14. As a result, as shown in FIG. 2, a circuit board 11 is formed as a second embodiment of the laminate.

[0143] In such a circuit board 11, the adhesive insulating layer 2 contains a low dielectric adhesive molding. Therefore, in the circuit board 11, the adhesive insulating layer 2 has excellent adhesiveness and low dielectric properties, as well as excellent heat resistance and excellent affinity (compatibility, adhesion) with thermosetting resins, and therefore has excellent strength.

[0144] (3) Third Embodiment Fig. 3 is a schematic cross-sectional view showing a copper-clad laminate as a third embodiment of the laminate. In the third embodiment, the above-mentioned low dielectric resin composition is used as a low dielectric adhesive.

[0145] 3, copper-clad laminate 21 includes insulating layer 22, conductor layer 24 disposed opposite insulating layer 22, and adhesive layer 23 disposed between insulating layer 22 and conductor layer 24 to bond insulating layer 22 and conductor layer 24. In copper-clad laminate 21, adhesive layer 23 is formed from the low-dielectric adhesive described above.

[0146] The insulating layer 22 is, for example, an insulating layer that does not have adhesive properties (a non-adhesive insulating layer). The insulating layer 22 contains, for example, the above-mentioned thermosetting resin. The insulating layer 22 is preferably made of the above-mentioned thermosetting resin.

[0147] The conductor layer 24, like the conductor layer 4, is a thin film made of a known conductive material. Examples of the conductive material include copper. The conductor layer 24 is formed by a known film formation method. The thickness of the conductor layer 24 is adjusted to be relatively thin, for example. This allows the circuit pattern to be formed by a subtractive method. The thickness of the conductor layer 24 is, for example, 50 μm or less.

[0148] The adhesive layer 23 is interposed between the insulating layer 22 and the conductor layer 24. The adhesive layer 23 is a dried product of a low dielectric adhesive. The low dielectric adhesive includes, for example, the above-mentioned low dielectric resin composition. The low dielectric adhesive is preferably a diluted solution of the above-mentioned low dielectric resin composition.

[0149] When manufacturing the copper-clad laminate 21, for example, first, the insulating layer 22 and the conductor layer 24 are prepared. Next, a low-dielectric adhesive is applied to one side of the insulating layer 22. After that, the conductor layer 24 is bonded to one side of the low-dielectric adhesive, and the low-dielectric adhesive is dried. In this way, the copper-clad laminate 21 is obtained. Note that the copper-clad laminate 21 can also be manufactured in the reverse order described above. That is, in this method, the low-dielectric adhesive is applied to one side of the conductor layer 24. Then, the insulating layer 22 is bonded to one side of the low-dielectric adhesive, and the low-dielectric adhesive is dried. In this way, the copper-clad laminate 21 is obtained.

[0150] In the copper-clad laminate 21, the insulating layer 22 and the conductor layer 24 are bonded together by an adhesive layer 23 (low-dielectric adhesive). That is, the copper-clad laminate 21 has the adhesive layer 23. The adhesive layer 23 (low-dielectric adhesive) contains the low-dielectric resin composition. Therefore, in the copper-clad laminate 21, the adhesive layer 23 (low-dielectric adhesive) has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (adhesion) with thermosetting resins.

[0151] In the copper-clad laminate 21 of the third embodiment described above, the adhesive layer 23 and the conductor layer 24 are formed only on one side of the insulating layer 22, but the adhesive layer 23 and the conductor layer 24 may be formed on both sides of the insulating layer 22. In such a case, the copper-clad laminate 21 does not need to have the insulating layer 22. That is, the conductor layer 24 may be formed on both sides of the adhesive layer 23. In other words, two conductor layers 24 may be bonded by the adhesive layer 23. In such a case, the adhesive layer 23 also serves as the insulating layer 22.

[0152] (4) Fourth Embodiment Fig. 4 is a schematic cross-sectional view showing a circuit board as a fourth embodiment of the laminate. In the fourth embodiment, similarly to the third embodiment, the above-described low dielectric resin composition is used as a low dielectric adhesive.

[0153] More specifically, the copper-clad laminate 21 of the third embodiment described above can be processed to form a circuit board 31. More specifically, the conductor layer 24 of the copper-clad laminate 21 can be etched by a known method to form a circuit 34. As a result, as shown in FIG. 4, a circuit board 31 is formed as a fourth embodiment of the laminate.

[0154] In such a circuit board, an insulating layer 22 and a circuit 34 made of a conductor layer are bonded together by an adhesive layer 23 .

[0155] In this circuit board 31, the insulating layer 22 and the circuit 34 made of a conductor layer are bonded together by an adhesive layer 23 (low dielectric adhesive). The adhesive layer 23 (low dielectric adhesive) contains the low dielectric resin composition described above. Therefore, in the circuit board 31, the adhesive layer 23 (low dielectric adhesive) has excellent adhesive properties and low dielectric properties, as well as excellent heat resistance and excellent affinity (adhesion) with thermosetting resins.

[0156] In the circuit board 31 of the fourth embodiment described above, the adhesive layer 23 and the circuit 34 are formed only on one side of the insulating layer 22, but the adhesive layer 23 and the circuit 34 may be formed on both sides of the insulating layer 22. In such a case, the circuit board 31 does not need to have the insulating layer 22. That is, the circuit 34 may be formed on both sides of the adhesive layer 23. In other words, two circuits 34 may be bonded by the adhesive layer 23. In such a case, the adhesive layer 23 also serves as the insulating layer 22.

[0157] 5 to 8 are cross-sectional views showing steps for manufacturing a circuit board as a fifth embodiment of the laminate. In the fifth embodiment, the low dielectric resin composition described above is used as a low dielectric adhesive.

[0158] 5 to 8, the circuit board 41 is a multilayer circuit board having at least two conductor layers. More specifically, as shown in FIG. 8O, the circuit board 41 includes a first conductor layer 40, a second conductor layer 50 disposed opposite the first conductor layer 40, and an adhesive layer 51 disposed between the first conductor layer 40 and the second conductor layer 50 and adhering the first conductor layer 40 and the second conductor layer 50 together. In the circuit board 41, the adhesive layer 51 is formed from the low dielectric adhesive (preferably a diluted solution of a low dielectric resin composition).

[0159] 5A, a carrier-attached copper foil 442 is first prepared. The carrier-attached copper foil 442 includes a carrier layer 43 and a copper foil 44 laminated on one side of the carrier layer 43.

[0160] The carrier layer 43 is not particularly limited, and may be a known release sheet. The copper foil 44 is laminated on the carrier layer 43 by a known method. The thickness of the copper foil 44 is appropriately set depending on the purpose and application. Furthermore, the copper foil 44 may be surface-treated as needed. Examples of surface treatments include roughening treatment.

[0161] 5B, a first resist layer 45 having a predetermined shape is formed on one surface of the copper foil 44. The first resist layer 45 is formed, for example, by applying a known resist liquid, exposing it to light, and developing it. Alternatively, the first resist layer 45 can be formed by exposing and etching a dry film resist.

[0162] Next, in this method, as shown in FIG. 5C , a first plating layer 46 is formed. The first plating layer 46 is formed, for example, by electrolytic plating. In electrolytic plating, for example, the carrier layer 43, copper foil 44, and first resist layer 45 are immersed in an electrolytic plating solution, and then a current is supplied to the copper foil 44. As a result, the first plating layer 46 is formed on one surface of the copper foil 44 in the reverse pattern of the first resist layer 45. In other words, the first plating layer 46 has a circuit pattern.

[0163] Next, in this method, as shown in Fig. 6D, the first resist layer 45 is removed by a known method. Next, in this method, as shown in Fig. 6E, the copper foil 44 exposed from the first plating layer 46 is removed by a known method. This forms the first conductor layer 40, which includes the copper foil 44 that remains unremoved and the first plating layer 46 laminated on the copper foil 44. In other words, the first conductor layer 40 includes the copper foil 44 and the first plating layer 46. The first conductor layer 40 is preferably made of the copper foil 44 and the first plating layer 46.

[0164] Next, the method involves laminating an adhesive layer 51 made of a low dielectric adhesive to the carrier layer 43, the first plating layer 46, and the copper foil 44, as shown in FIG. 6F.

[0165] More specifically, in this method, for example, a cast film of a low-dielectric adhesive is prepared. The cast film is then pressure-bonded to the carrier layer 43, the first plating layer 46, and the copper foil 44. As a result, the cast film covers the first plating layer 46 and the copper foil 44. The cast film also forms an adhesive layer 51.

[0166] On the other hand, in this method, a carrier-attached copper foil 52 is separately prepared. The carrier-attached copper foil 52 includes a carrier layer 53 and a copper foil 54 laminated on the other side of the carrier layer 53. Then, in this method, the copper foil 54 of the carrier-attached copper foil 52 is laminated on an adhesive layer 51, as shown in Fig. 6G.

[0167] Next, in this method, as shown in Fig. 7H, the carrier layer 53 of the carrier-attached copper foil 52 is peeled off. Next, as shown in Fig. 7I, the copper foil 54 and the adhesive layer 51 are opened by a known method to form via holes 58. Furthermore, the first plating layer 46 is exposed from the via holes 58. Next, in this method, as shown in Fig. 7J, the via holes 58 are filled with a conductive material to form via fills 59. Note that examples of the conductive material include copper.

[0168] 7K, a second resist layer 55 having a predetermined shape is then formed on one surface of the copper foil 54. The second resist layer 55 is formed, for example, by applying a known resist liquid, exposing it to light, and developing it. Similarly to the first resist layer 45, the second resist layer 55 can also be formed from a dry film resist.

[0169] 8L, the second plating layer 56 is then formed. The second plating layer 56 is formed, for example, by electrolytic plating. As a result, the second plating layer 56 is formed on one surface of the copper foil 54 in the reverse pattern of the second resist layer 55. In other words, the second plating layer 56 has a circuit pattern.

[0170] Next, in this method, as shown in Fig. 8M, the second resist layer 55 is removed by a known method. Next, in this method, as shown in Fig. 8N, the copper foil 54 exposed from the second plating layer 56 is removed by a known method. This forms the second conductor layer 50, which includes the copper foil 54 that remains unremoved and the first plating layer 56 laminated on the copper foil 54. In other words, the second conductor layer 50 includes the copper foil 54 and the second plating layer 56. The second conductor layer 50 is preferably made of the copper foil 54 and the second plating layer 56.

[0171] 8O, the method then includes peeling off the carrier layer 43, thereby exposing the copper foil 44. As a result, the circuit board 1 is formed.

[0172] In the circuit board 41, the first conductor layer 40 and the second conductor layer 50 are bonded together by an adhesive layer 51 (low dielectric adhesive). That is, the circuit board 41 has the adhesive layer 51. The adhesive layer 51 (low dielectric adhesive) contains the low dielectric resin composition. Therefore, in the circuit board 41, the adhesive layer 51 (low dielectric adhesive) has excellent adhesive properties and low dielectric properties, and also has excellent heat resistance.

[0173] Next, the present invention will be described based on examples and comparative examples, but the present invention is not limited thereto. Note that "parts" and "%" are by mass unless otherwise specified. Furthermore, specific numerical values ​​such as blending ratios (content ratios), physical property values, parameters, etc. used in the following description can be substituted with the corresponding upper limit values ​​(numerical values ​​defined as "equal to or less than") or lower limit values ​​(numerical values ​​defined as "equal to or more than" or "exceeding") of the blending ratios (content ratios), physical property values, parameters, etc. described in the above "Modes for Carrying Out the Invention."

[0174] 1. Preparation of Raw Materials Preparation Example 1-1 (Styrene-based elastomer) As shown in Tables 1 to 4, the following commercially available products were prepared as styrene-based elastomers. SEPTON 2063: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 13% by mass, weight average molecular weight (Mw) 100,000 SEPTON 2002: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 30% by mass, weight average molecular weight (Mw) 55,000 Kraton G1730: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 20% by mass, weight average molecular weight (Mw) 93,000 Kraton G1652: styrene-ethylene-butylene-styrene copolymer (SEBS), styrene unit content 30% by mass, weight average molecular weight (Mw) 75,000 SEPTON 1020: styrene-ethylene-propylene copolymer (SEP), styrene unit content 36% by mass, weight average molecular weight (Mw) 120,000 SEPTON 4033: Styrene-ethylene-ethylene-propylene-styrene copolymer (SEEPS), styrene unit content 30% by mass, weight average molecular weight (Mw) 88,000 SEPTON 2104: Styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 65% by mass, weight average molecular weight (Mw) 60,000

[0175] Preparation Example 2-1 (Cyclic Olefin Polymer (B-1)) (1) Catalyst Preparation Step VO(OC ２ H ５ ) Cl ２The vanadium catalyst solution was diluted with cyclohexane to obtain a vanadium catalyst solution having a vanadium concentration of 6.7 mmol / L.

[0176] Also, ethyl aluminum sesquichloride (Al(C ２ H ５ ) １．５ Cl １．５ ) was diluted with cyclohexane to obtain an aluminum catalyst solution having an aluminum concentration of 107 mmol / L.

[0177] (2) Polymerization step: Using a stirred polymerization vessel (inner diameter 500 mm, reaction volume 100 L), ethylene and tetracyclo[4.4.0.12,5.17,10]-3-dodecene were continuously fed and copolymerized. The glass transition temperature (Tg) of the cyclic olefin polymer was adjusted by adjusting the ratio of ethylene to tetracyclo[4.4.0.12,5.17,10]-3-dodecene.

[0178] The vanadium catalyst solution was supplied to the polymerization reactor so that the vanadium catalyst concentration relative to cyclohexane in the polymerization reactor was 0.6 mmol / L. The aluminum catalyst solution was supplied to the polymerization reactor so that the molar ratio of aluminum to vanadium (Al / V) was 12.0. The polymerization temperature was 12°C. The polymerization pressure was 3.1 kg / cm. ２ G (gauge pressure).

[0179] This results in the formation of ethylene and tetracyclo[4.4.0.1 ２，５ .1 ７，１０ ]-3-dodecene (cyclic olefin polymer (B-1)). The copolymer was obtained as a solution in cyclohexane (solvent).

[0180] (3) Decalcification Step The copolymer solution was extracted from the polymerization reactor. A 25% by mass NaOH solution was added to the copolymer solution to terminate the reaction. This also removed catalyst residue from the copolymer solution (decalcification treatment). The copolymer concentration in the solution was 7.7% by mass.

[0181] To the copolymer solution, pentaerythritol-tetrakis[3-(3,5-di-t-butyl-4-hydroxyphenyl)propionate] was added as a stabilizer in an amount of 0.4 parts by mass relative to 100 parts by mass of the copolymer.

[0182] Then, a stirring tank (effective volume 1.0 cm ３ The copolymer solution was stirred for 1 hour using a stirring rod. The solid content of the copolymer was 5% by mass.

[0183] (4) Solvent removal process Double tube heater (outer tube diameter 2B, inner tube diameter 3 / 4B, length 21m, heat source 20kg / cm ２ A copolymer solution (solid content concentration: 5% by mass) was supplied to the reactor (G steam) and heated to 180° C. The supply rate was 150 kg / H.

[0184] Next, a double-tube flash dryer (outer tube diameter 2B, inner tube diameter 3 / 4B, length 27 m, heat source 20 kg / cm ２ Cyclohexane was removed from the copolymer solution using a steam (G steam) and a flash hopper (volume 200 L). Unreacted monomers were also removed along with the cyclohexane.

[0185] This resulted in a molten cyclic olefin polymer (B-1). The glass transition temperature (Tg) of the cyclic olefin polymer (B-1) was measured in accordance with JIS K 7122 (2012). As a result, the glass transition temperature (Tg) of the cyclic olefin polymer (B-1) was 105°C. The weight average molecular weight of the cyclic olefin polymer (B-1) (polystyrene equivalent, measured by gel permeation chromatography) was 113,000.

[0186] Preparative Example 2-2 (Cyclic Olefin Polymer (B-2)) A cyclic olefin polymer (B-2) was obtained in the same manner as in Preparative Example 2-1, except that ethylene and tetracyclo[4.4.0.1 ２，５ .1 ７，１０ The composition ratio of cycloolefin polymer to cycloolefin-3-dodecene was changed to adjust the glass transition temperature (Tg) of the cycloolefin polymer.

[0187] The glass transition temperature (Tg) of the cyclic olefin polymer (B-2) was 125° C. The weight average molecular weight of the cyclic olefin polymer (B-2) (measured by gel permeation chromatography in terms of polystyrene) was 116,000.

[0188] Preparative Example 2-3 (Cyclic Olefin Polymer (B-3)) A cyclic olefin polymer (B-3) was obtained in the same manner as in Preparative Example 2-1, except that ethylene and tetracyclo[4.4.0.1 ２，５ .1 ７，１０ The composition ratio of cycloolefin polymer to cycloolefin-3-dodecene was changed to adjust the glass transition temperature (Tg) of the cycloolefin polymer.

[0189] The glass transition temperature (Tg) of the cyclic olefin polymer (B-3) was 65° C. The weight average molecular weight of the cyclic olefin polymer (B-3) (measured by gel permeation chromatography in terms of polystyrene) was 110,000.

[0190] Preparation Example 3-1 (Other Olefin Polymer (C-1)) 900 mL of hexane and 90 g of 1-butene were placed in a 2-liter autoclave whose atmosphere had been replaced with nitrogen. 1 mmol of triisobutylaluminum was also added to the autoclave. The temperature inside the autoclave was raised to 70°C.

[0191] Next, 0.30 mmol of methylaluminoxane and 0.001 mmol of rac-dimethylsilylene-bis{1-(2-methyl-4-phenylindenyl)}zirconium dichloride (calculated as Zr) were added to the autoclave.

[0192] Then, propylene was continuously supplied to the autoclave, and the total pressure was kept at 7 kg / cm. ２ While maintaining the temperature at G, 1-butene and propylene were polymerized for 30 minutes to obtain a random copolymer of 1-butene and propylene (another olefin polymer (C-1)).

[0193] The autoclave was degassed, and the copolymer (other olefin-based polymer (C-1)) was recovered with methanol, followed by drying under reduced pressure at 110°C for 12 hours.

[0194] The melting point (Tm) of the other olefin-based polymer (C-1) was measured in accordance with JIS K 7122 (2012). As a result, the melting point (Tm) of the other olefin-based polymer (C-1) was 78.3° C. The weight average molecular weight (Mw) of the other olefin-based polymer (C-1) was 300,000.

[0195] Preparation Example 3-2 (Other Olefin-Based Polymer (C-2)) The following commercially available product was prepared as other olefin-based polymer (C-2): Trade name Vistamaxx 6102: propylene-ethylene copolymer (PER), styrene unit content 0 mass%, weight average molecular weight (Mw) 320,000, melting point 107°C, manufactured by ExxonMobil Japan LLC

[0196] Preparation Example 3-3 (Other Olefin-Based Polymer (C-3)) The following commercially available product was prepared as other olefin-based polymer (C-3): Trade name Vistamaxx 3020FL; propylene-ethylene copolymer (PER), styrene unit content 0 mass%, weight average molecular weight (Mw) 370,000, melting point 64°C, manufactured by ExxonMobil Japan LLC

[0197] 2. Preparation of Resin Composition Example 1 (Low Dielectric Resin Composition (D-1)) As resin components, 50 parts by mass of SEPTON 2063 (SEPS, Mw 100,000, styrene unit content 13%) and 50 parts by mass of cyclic olefin polymer (B-1) were prepared.

[0198] Maleic anhydride (MAH) was added as a modifier to the resin component in an amount of 1 part by mass per 100 parts by mass of the total amount of the resin component.

[0199] Furthermore, 2,5-dimethyl-2,5-bis(t-butylperoxy)hexane (peroxide, modified initiator) was added to the resin component. The amount of 2,5-dimethyl-2,5-bis(t-butylperoxy)hexane added was 0.6 parts by mass per 100 parts by mass of the total amount of the resin component.

[0200] The resin components were then melt-kneaded at 230°C using a vented twin-screw kneading extruder. This gave a low dielectric resin composition (D-1). Hereinafter, the low dielectric resin composition will be simply referred to as the resin composition.

[0201] The resin composition (D-1) was cooled and pelletized. Then, 100 parts by mass of the resin composition (D-1) pellets were dissolved in 400 parts by mass of toluene under a heated environment. This gave a solution of the resin composition (D-1) (solid content concentration: 20% by mass).

[0202] Examples 2 to 13 and Comparative Examples 1 to 9 (Resin Compositions (D-2) to (D-22)) Resin compositions (D-2) to (D-21) were obtained in the same manner as in Example 1, except that the formulations were changed as shown in Tables 1 to 4. Solutions of resin compositions (D-2) to (D-21) (solid content concentration 20% by mass) were also obtained in the same manner as in Example 1. In Example 12, no modifier was added.

[0203] 3. Evaluation (1) Measurement of relative dielectric constant and dielectric loss tangent A solution of the resin composition was applied to a release film (polyethylene terephthalate film, thickness 100 μm) and dried for 1 minute at 100° C. This gave a dried coating film of the resin composition (film thickness approximately 60 μm).

[0204] The dried coating film was molded into a strip, and the relative permittivity and dielectric loss tangent of the dried coating film were measured in accordance with JIS R1641 (2007). The measurement was performed using a cavity resonator (Vector Network Analyzer HP8510B (manufactured by Keysight Technologies)) at a measurement frequency of 10 GHz.

[0205] (2) Compatibility (affinity with thermosetting resin) Polyphenylene ether (hereinafter, PPE) was prepared as a thermosetting resin, and the PPE was dissolved in toluene to obtain a PPE solution.

[0206] The PPE solution and the resin composition solution were mixed to obtain a mixed solution, where the mass ratio of the PPE to the resin composition (PPE:resin composition) was 7:3.

[0207] The mixed solution was applied to a glass plate and dried for 1 minute at 100° C. This gave a dried coating film of the mixed resin (film thickness: approximately 30 μm).

[0208] The haze of the dried coating film was measured in accordance with JIS K7136 (2000). A haze meter (NDH 4000, manufactured by Nippon Denshoku Industries Co., Ltd.) was used for the measurement. The transparency of the dried coating film was evaluated by the haze value and visual observation. The evaluation criteria are as follows:

[0209] 5: The entire coating film is homogeneous. The haze is less than 25. 4: The entire coating film is homogeneous. The haze is 25 or more. 3: The coating film is phase-separated. The phase-separated portions are uniformly distributed throughout the coating film. 2: The coating film is phase-separated. The phase-separated portions are non-uniform. The maximum length of the non-uniform portions is less than 1 cm. 1: The coating film is phase-separated. The phase-separated portions are non-uniform. The maximum length of the non-uniform portions is 1 cm or more.

[0210] If the affinity of the resin composition for the thermosetting resin is improved, the adhesiveness is also improved, and if the affinity of the resin composition for the thermosetting resin is improved, the strength of the molded product is also improved.

[0211] (3) Heat Resistance To a solution of the resin composition, 2,5-dimethyl-2,5-bis(t-butylperoxy)hexane (trade name: Perhexyne 25B, manufactured by NOF Corporation) was added as a thermal initiator. The solid content of the thermal initiator was 3 parts by mass per 100 parts by mass of the total solid content of the resin components of the resin composition.

[0212] Next, the solution of the resin composition to which the thermal initiator had been added was placed in a Teflon (registered trademark) Petri dish and dried at 100° C. for 1 minute, thereby obtaining a dried coating film of the resin composition (film thickness: approximately 100 μm).

[0213] The dried coating film of the resin composition was heat-treated at 200°C for 3 hours. Thereafter, the shear storage modulus (G') of the dried coating film of the resin composition was measured. The measurement was performed using a viscoelasticity measuring device (MCR302 (manufactured by Anton Paar Japan)). The measurement conditions were as follows:

[0214] Temperature range: 0°C to 200°C Heating rate: 2°C / min Operating conditions: Shear mode Frequency: 1 Hz

[0215] The heat resistance of the dried coating film was evaluated based on the shear storage modulus (G'). The evaluation criteria are as follows:

[0216] ◯: The shear storage modulus (G') at 200°C is 1500 Pa or more. Δ: The shear storage modulus (G') at 200°C is 1000 Pa or more and less than 1500 Pa. ×: The shear storage modulus (G') at 200°C is less than 1000 Pa.

[0217] (4) Solubility in Solvent A solution of the resin composition (solid content concentration 20% by mass, toluene solution) was visually inspected to evaluate the solubility of the resin composition in toluene. The evaluation criteria are as follows:

[0218] ◯: When the resin composition and the solvent are stirred and allowed to stand, the solution is in a uniform liquid state. Δ: The mixture of the resin composition and the solvent is in a uniform gel state. ×: Precipitates are observed in the mixture of the resin composition and the solvent. In addition, the entire mixture is heterogeneous.

[0219]

[0220]

[0221]

[0222]

[0223] Details of the abbreviations in the table are as follows. Styrene unit content: content ratio (mass%) of structural units derived from styrene SEPTON 2063: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 13% by mass, weight average molecular weight (Mw) 100,000, manufactured by Kuraray SEPTON 2002: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 30% by mass, weight average molecular weight (Mw) 55,000, manufactured by Kuraray Kraton G1730: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 20% by mass, weight average molecular weight (Mw) 93,000, manufactured by Kraton Polymer Japan Kraton G1652: styrene-ethylene-butylene-styrene copolymer (SEBS), styrene unit content 30% by mass, weight average molecular weight (Mw) 75,000, manufactured by Kraton Polymer Japan SEPTON 1020: styrene-ethylene-propylene copolymer (SEP), styrene unit content 36% by mass, weight average molecular weight (Mw) 120,000, manufactured by Kuraray SEPTON 4033: styrene-ethylene-ethylene-propylene-styrene copolymer (SEEPS), styrene unit content 30% by mass, weight average molecular weight (Mw) 88,000, manufactured by Kuraray SEPTON 2104: styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 65% by mass, weight average molecular weight (Mw) 60,000, manufactured by Kuraray MAH: modifier, carboxy group-containing monomer maleic anhydride

[0224] The above invention is provided as an exemplary embodiment of the present invention, but it is merely an example and should not be interpreted as being limiting. Modifications of the present invention that are obvious to those skilled in the art are intended to be included in the scope of the following claims.

[0225] The low dielectric resin composition, adhesion promoter, low dielectric adhesive composition, low dielectric adhesive molded product, low dielectric adhesive, and laminate of the present invention are suitably used in the field of circuit boards.

Claims

1. A low dielectric resin composition containing a polyolefin resin, wherein the polyolefin resin contains a styrene elastomer (A) and a cyclic olefin polymer (B) having an alicyclic ring in its main chain, and the content of the styrene elastomer (A) is 30 parts by mass or more and 89 parts by mass or less per 100 parts by mass of the total of the styrene elastomer (A) and the cyclic olefin polymer (B).

2. The low dielectric resin composition according to claim 1, wherein the weight average molecular weight of the styrene elastomer (A) is 70,000 or more and 110,000 or less.

3. The low dielectric resin composition according to claim 1, wherein the styrene-based elastomer (A) contains structural units derived from styrene, and the content of the structural units derived from styrene is 10% by mass or more and 40% by mass or less relative to the total amount of the styrene-based elastomer (A).

4. The low dielectric resin composition according to claim 1, wherein the styrene elastomer (A) does not contain a structural unit derived from butylene.

5. The low dielectric resin composition according to claim 1, wherein the glass transition temperature of the cyclic olefin polymer (B) is 100°C or higher and 140°C or lower.

6. The low dielectric resin composition according to claim 1, wherein the polyolefin resin is modified with a functional group-containing monomer.

7. The low dielectric resin composition according to claim 6, wherein the functional group-containing monomer comprises a carboxy group-containing monomer.

8. An adhesion promoter comprising the low dielectric resin composition according to claim 1.

9. A low dielectric adhesive composition comprising a thermosetting resin and the adhesion promoter according to claim 8, wherein the thermosetting resin comprises at least one selected from the group consisting of epoxy resin, polyphenylene ether resin, fluororesin, polyimide resin, phenolic resin, melamine resin, polyolefin resin having an unsaturated double bond, and liquid crystal polymer.

10. A low dielectric adhesive molded article comprising a cured product of the low dielectric adhesive composition according to claim 9.

11. A laminate comprising an insulating layer containing the low dielectric adhesive molding according to claim 10, and a conductor layer disposed on at least one surface of the insulating layer.

12. A low dielectric adhesive comprising the low dielectric resin composition of claim 1.

13. A laminate comprising: an insulating layer; a conductor layer disposed opposite the insulating layer; and an adhesive layer disposed between the insulating layer and the conductor layer and adhering the insulating layer and the conductor layer, wherein the adhesive layer comprises the low dielectric adhesive according to claim 12.

14. A laminate comprising: a first conductor layer; a second conductor layer disposed opposite the first conductor layer; and an adhesive layer disposed between the first conductor layer and the second conductor layer and adhering the first conductor layer and the second conductor layer, wherein the adhesive layer comprises the low dielectric adhesive according to claim 12.