Low dielectric resin compositions, adhesion promoters, low dielectric adhesive compositions, low dielectric adhesive molded products, low dielectric adhesives, and laminates

A low dielectric resin composition with a styrene-based elastomer and cyclic olefin polymer addresses the need for superior heat resistance and affinity with thermosetting resins, enhancing adhesion and dielectric properties in circuit board applications.

JP7856772B2Active Publication Date: 2026-05-11MITSUI CHEMICALS INC
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Patent Information

Authority / Receiving Office
JP · JP
Patent Type
Patents
Current Assignee / Owner
MITSUI CHEMICALS INC
Filing Date
2023-08-07
Publication Date
2026-05-11

AI Technical Summary

Technical Problem

Existing adhesives and interlayer adhesives in wiring circuit boards require superior heat resistance and improved affinity with thermosetting resins, while maintaining excellent adhesion and low dielectric properties.

Method used

A low dielectric resin composition containing a polyolefin resin with a specific ratio of styrene-based elastomer and cyclic olefin polymer, which includes a styrene-based elastomer and a cyclic olefin polymer with an alicyclic ring, optimized for adhesion, heat resistance, and compatibility with thermosetting resins.

Benefits of technology

The resin composition achieves excellent adhesion, low dielectric properties, and heat resistance, with enhanced affinity to thermosetting resins, resulting in improved bonding between resin and conductor layers in circuit boards.

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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).
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Description

[Technical Field]

[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. [Background technology]

[0002] A wiring circuit board comprises, for example, a resin layer (insulating layer) containing a thermosetting resin and a conductive layer containing a metal. Wiring circuit boards are widely used in various industrial fields.

[0003] In recent years, there has been a demand for direct bonding between the resin layer (insulating layer) and the conductor layer in wiring circuit boards. Therefore, it has been proposed to add an adhesion promoter to the resin layer (insulating layer) to impart adhesive properties to it.

[0004] As adhesion promoters, for example, resins having relatively high adhesion and relatively low dielectric constant are used. As such resins, for example, the following low dielectric constant resins have been proposed. These low dielectric constant resins include maleic anhydride graft-modified resins. As maleic anhydride graft-modified resins, maleic anhydride graft (styrene-ethylene-butylene-styrene) block copolymer is used alone, or maleic anhydride graft cyclic olefin copolymer is used alone (see, for example, Patent Document 2 (Examples 1 and 4)).

[0005] Furthermore, in wiring circuit boards, it is required that the resin layer (insulating layer) and the conductor layer be bonded together using an interlayer adhesive, rather than directly bonded together.

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

[0007] [Patent Document 1] Japanese Patent Publication No. 2018-154823 [Patent Document 2] Japanese Patent Publication No. 2022-043966 [Overview of the Initiative] [Problems that the invention aims to solve]

[0008] On the other hand, adhesives and interlayer adhesives require superior heat resistance.

[0009] Furthermore, the adhesion promoter is mixed with the thermosetting resin to form a resin layer (insulating layer). Therefore, improved affinity (compatibility) with the thermosetting resin is required for the adhesion promoter.

[0010] Furthermore, interlayer adhesives require excellent adhesion to the resin layer (insulating layer). Therefore, improved affinity (adhesion) to thermosetting resins is also required for interlayer adhesives.

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

Means for Solving the Problem

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

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

[0014] The present invention [3] includes the low dielectric resin composition according to [1] or [2] above, wherein the styrene-based elastomer (A) contains a structural unit derived from styrene, and the content ratio of the structural unit derived from styrene is 10% by mass or more and 40% by mass or less with respect 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 [1] to [3] above, 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 [1] to [4] above, wherein the glass transition temperature of the cyclic olefin polymer (B) is 100°C or more and 140°C or less.

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

[0018] The present invention [7] comprises the low dielectric resin composition described in [6] above, wherein the functional group-containing monomer includes a carboxyl group-containing monomer.

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

[0020] The present invention [9] includes a low-dielectric adhesive composition comprising a thermosetting resin and the adhesion agent described in [8] above, wherein the thermosetting resin comprises at least one selected from the group consisting of epoxy resins, polyphenylene ether resins, fluororesins, polyimide resins, phenolic resins, melamine resins, polyolefin resins having unsaturated double bonds, and liquid crystal polymers.

[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 molded product described in

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

[0023] The present invention

[12] includes a low-dielectric adhesive comprising a 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 to the insulating layer, and an adhesive layer disposed between the insulating layer and the conductor layer for bonding 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 to the first conductor layer, and an adhesive layer disposed between the first conductor layer and the second conductor layer for bonding the first conductor layer and the second conductor layer, wherein the adhesive layer contains the low dielectric adhesive described in

[12] above. [Effects of the Invention]

[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 its main chain in specific proportions. Therefore, the low-dielectric resin composition has excellent adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, excellent affinity (compatibility and adhesion) to thermosetting resins.

[0027] The adhesion promoter, low-dielectric adhesive composition, and low-dielectric adhesive molded product of the present invention include the above-mentioned low-dielectric resin composition. Therefore, the adhesion promoter, low-dielectric adhesive composition, and low-dielectric adhesive molded product have excellent adhesion and low dielectric properties, as well as excellent heat resistance and, in addition, excellent affinity (compatibility, adhesion) to thermosetting resins.

[0028] The laminate of the present invention has an insulating layer. The insulating layer includes the low-dielectric adhesive molded product described above. Therefore, in the laminate, the insulating layer has excellent adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, excellent affinity (compatibility, adhesion) to thermosetting resins.

[0029] The low-dielectric adhesive of the present invention comprises the above-mentioned low-dielectric resin composition. Therefore, the low-dielectric adhesive has excellent adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, excellent affinity (compatibility and adhesion) to thermosetting resins.

[0030] Furthermore, the laminate of the present invention has an adhesive layer. The adhesive layer contains the low-dielectric adhesive described above. Therefore, in the laminate, the adhesive layer has excellent adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, excellent affinity (compatibility, adhesion) to thermosetting resins. [Brief explanation of the drawing]

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

[0032] 1. Low-dielectric resin composition The low dielectric resin composition is, for example, a resin composition included in an insulating layer (described later) or an adhesive layer (described later) in a 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 its main chain.

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

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

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

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

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

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

[0040] The proportion of structural units derived from styrene and the proportion of structural units derived from linear olefins are calculated based on the formulation of the polymerization raw materials for styrene-based elastomer (A). More specifically, the proportion of structural units derived from styrene is calculated as the ratio of styrene to the total amount of polymerization raw materials (styrene and linear olefins). Similarly, the proportion of structural units derived from linear olefins is calculated as the ratio of linear olefins to the total amount of polymerization raw materials (styrene and linear olefins).

[0041] The styrene-based elastomer (A) preferably contains structural units derived from ethylene as structural units derived from a chain-like olefin. The proportion of structural units derived from ethylene is appropriately set according to the purpose and application.

[0042] Furthermore, the styrene-based elastomer (A) preferably contains structural units derived from propylene as structural units derived from the chain-like olefin. The proportion of structural units derived from propylene is appropriately set according to the purpose and application.

[0043] Furthermore, the styrene-based elastomer (A) may, if necessary, contain structural units derived from butylene as structural units derived from the chain olefin. The proportion of structural units derived from butylene will be appropriately set according to the purpose and application.

[0044] On the other hand, in the styrene-based elastomer (A), if the content of structural units derived from styrene is relatively low, it is preferable, from the viewpoint of affinity to thermosetting resins, that the content of structural units derived from butylene is also relatively low.

[0045] In other words, if the styrene-based elastomer (A) contains structural units derived from butylene, it is preferable that the proportion of structural units derived from styrene is set to a relatively high level.

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

[0047] Particularly preferably, the styrene-based elastomer (A) does not contain structural units derived from butylene. More specifically, in the case where the content of structural units derived from styrene in the styrene-based elastomer (A) is less than 25% by mass, preferably, the styrene-based elastomer (A) does not contain structural units derived from butylene as structural units derived from the chain olefin.

[0048] In other words, in styrene-based elastomer (A), if the content of structural units derived from styrene is relatively high (for example, 25% by mass or more), styrene-based elastomer (A) may also contain structural units derived from butylene. Conversely, if the content of structural units derived from styrene is relatively high, styrene-based elastomer (A) does not need to contain structural units derived from butylene.

[0049] From the viewpoint of affinity to thermosetting resins, the styrene-based elastomer (A) is particularly preferably one that contains 25% by mass or more of structural units derived from styrene and no structural units derived from butylene, or one that contains 25% by mass or more of structural units derived from styrene and also contains structural units derived from butylene, or one that contains less than 25% by mass of structural units derived from styrene and does not contain structural units derived from butylene.

[0050] More specifically, examples of styrene-based elastomers (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 individually or in combination of two or more types.

[0051] From the viewpoint of affinity to thermosetting resins, preferred styrene-ethylene-propylene copolymers (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 viewpoint of heat resistance, low dielectric properties, and affinity to thermosetting resins, styrene-ethylene-propylene-styrene copolymer (SEPS) and styrene-ethylene-butylene-styrene copolymer (SEBS) are more preferred as styrene-based elastomer (A).

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

[0054] Furthermore, from the viewpoint of heat resistance, low dielectric properties, and affinity to thermosetting resins, a styrene-based elastomer (A) that contains structural units derived from butylene and a relatively large amount of structural units derived from styrene can also be mentioned. In such a case, structural units derived from butylene of As described above, the content ratio is preferably 20% by mass or more, and particularly preferably 25% by mass or more, relative to the total amount of styrene-based elastomer (A).

[0055] In other words, as the styrene-based elastomer (A), more preferably, there is 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 also contains 25% by mass or more of structural units derived from styrene.

[0056] Furthermore, from the viewpoint of heat resistance, low dielectric properties, and affinity to thermosetting resins, particularly preferred are styrene-based elastomers (A) that do not contain structural units derived from butylene, and more specifically, styrene-ethylene-propylene-styrene copolymers (SEPS) are mentioned.

[0057] The weight-average molecular weight of the styrene-based elastomer (A) is, from the viewpoint of low dielectric properties, 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. Furthermore, the weight-average molecular weight of the styrene-based elastomer (A) is, from the viewpoint of low dielectric properties and the stability of the diluent (varnish) described later, 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 styrene-based elastomer (A) is measured as the molecular weight equivalent to standard polystyrene by gel permeation chromatography.

[0059] Styrene elastomer (A) can be used alone or in combination of two or more types. Commercially available styrene elastomers (A) can also be used.

[0060] Examples of commercially available styrene-based elastomers (A) include the SEPTON series (manufactured by Kuraray), the Kraton series (manufactured by Kraton Polymer Japan), and the ToughTec series (manufactured by Asahi Kasei).

[0061] (2) Cyclic olefin polymers Examples of cyclic olefin polymers (B) having an alicyclic ring in the main chain include polymers of cyclic olefins and their hydrides.

[0062] Examples of the cyclic olefin include cyclic hydrocarbon compounds containing ethylenically unsaturated bonds. Examples of the cyclic hydrocarbon compounds include cyclic hydrocarbon compounds having 6 to 30 carbon atoms. More specifically, examples of the cyclic olefin include, for example, bicyclo[2.2.1]-hepta-2-ene (alias norbornene) and its derivatives, tricyclo[4.3.0.1 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]-hepta-2-ene (alias norbornene) is mentioned.

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

[0064] Also, if necessary, the ring-opening metathesis polymer of the cyclic olefin can be hydrogenated by a known method. Thereby, a hydride of the ring-opening metathesis polymer of the cyclic olefin is obtained.

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

[0066] Examples of cyclic olefin polymers (B) having an alicyclic ring in the main chain include copolymers of cyclic olefins and linear olefins (cyclic olefin copolymers), and their hydrides.

[0067] Examples of cyclic olefins include the cyclic hydrocarbon compounds mentioned above, preferably tetracyclo[4.4.0.1 2.5 .1 7.10 Examples include ]-3-dodecene and its derivatives, more preferably tetracyclo[4.4.0.1 2.5 .1 7.10 ]-3-dodecene is one example.

[0068] Examples of chain-like olefins include the chain-like olefins having 2 to 8 carbon atoms as described above, and ethylene is preferred.

[0069] Copolymers of linear olefins and cyclic olefins are produced by known methods. For example, linear olefins and cyclic olefins are polymerized in the presence of known catalysts (e.g., vanadium-based catalysts, aluminum-based catalysts, and metallocene catalysts). This yields a copolymer of linear olefins and cyclic olefins. The polymerization conditions are set appropriately according to the purpose and application.

[0070] Furthermore, if necessary, the copolymer of the linear olefin and the cyclic olefin can be hydrogenated by known methods. This yields a hydride of the copolymer of the linear olefin and the cyclic olefin.

[0071] Copolymers of linear olefins and cyclic olefins, and their hydrides, can be used individually or in combination of two or more types.

[0072] Preferably, the cyclic olefin polymer (B) is 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) consists of structural units derived from a chain olefin and structural units derived from a cyclic olefin.

[0073] The proportion of structural units derived from linear olefins and the proportion of structural units derived from cyclic olefins are set as appropriate according to 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 proportion of structural units derived from linear olefins and the proportion of structural units derived from cyclic olefins are set as appropriate.

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

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

[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 diluent (varnish) described later, and 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, even 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] Cyclic olefin polymer (B) can be used alone or in combination of two or more types. Commercially available cyclic olefin polymers (B) can also be used.

[0079] Examples of commercially available cyclic olefin polymers (B) include the ZEONEX series (hydrogenated cyclic monomer polymers, manufactured by Nippon Zeon), the ZEONOR series (hydrogenated cyclic monomer polymers, manufactured by Nippon Zeon), and the APEL series (polymers of linear olefins and cyclic olefins, manufactured by Mitsui Chemicals).

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

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

[0082] More specifically, from the viewpoint of affinity to thermosetting resins, the content ratio of styrene-based 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 amount of styrene-based elastomer (A) and cyclic olefin polymer (B). Furthermore, from the viewpoint of heat resistance, the content ratio of styrene-based 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 amount of styrene-based elastomer (A) and cyclic olefin polymer (B).

[0083] In other words, from the viewpoint of heat resistance, the content ratio 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, relative to 100 parts by mass of the total amount of styrene elastomer (A) and cyclic olefin polymer (B). Furthermore, from the viewpoint of affinity to thermosetting resins, the content ratio 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, relative to 100 parts by mass of the total amount of styrene elastomer (A) and cyclic olefin polymer (B).

[0084] If the polyolefin resin contains a styrene elastomer (A) and a cyclic olefin polymer (B) having an alicyclic ring in its main chain in the specified proportions described above, the low-dielectric resin composition will have excellent adhesion and low dielectric properties, as well as excellent heat resistance and, in addition, excellent affinity (compatibility and adhesion) to thermosetting resins.

[0085] Furthermore, the content ratio of the cyclic olefin polymer (B) per 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, and more preferably 50 parts by mass or more. Also, the content ratio of the cyclic olefin polymer (B) per 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, and more preferably 150 parts by mass or less.

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

[0087] (4) Other olefin polymers Polyolefin resins may optionally contain other olefin polymers (C). These other olefin polymers (C) are known olefin polymers, excluding styrene elastomers (A) and cyclic olefin polymers (B).

[0088] Other olefin polymers (C) include, for example, 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 individually or in combination of two or more. The content ratio of the other olefin polymers is set appropriately within a range that does not hinder the excellent effects of the present invention.

[0089] The content of other olefin polymers (C) 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, relative to the total amount of polyolefin resin. In other words, the polyolefin resin preferably does not contain other olefin polymers (C). To put it another way, the polyolefin resin preferably consists of a styrene elastomer (A) and a cyclic olefin polymer (B).

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

[0091] Unmodified polyolefin resin is a polyolefin resin containing a styrene elastomer (A) and a cyclic olefin polymer (B), and which has not been modified by a modifying agent (described later). Modified polyolefin resin is a polyolefin resin containing a styrene elastomer (A) and a cyclic olefin polymer (B), and which has been modified by a modifying agent (described later). From the viewpoint of adhesion to metals (for example, the conductive layer described later), modified polyolefin resins are preferred as polyolefin resins.

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

[0093] Examples of modifying agents include functional group-containing monomers. Examples of functional group-containing monomers include carboxyl 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 individually or in combination of two or more. From the viewpoint of adhesion to metals (for example, the conductive layer described later), carboxyl group-containing monomers are preferred as functional group-containing monomers.

[0094] Examples of carboxyl group-containing monomers include unsaturated acids. Examples of unsaturated acids include maleic acid, fumaric acid, itaconic acid, and (meth)acrylic acid. Anhydrides of these unsaturated acids can also be used. These can be used alone or in combination of two or more. Preferably, maleic acid and its anhydride are used as carboxyl group-containing monomers, and more preferably, maleic anhydride is used.

[0095] In other words, examples of modified polyolefin resins include acid-modified polyolefin resins. Examples of acid-modified polyolefin resins include (anhydrous) maleic acid-modified polyolefin resins, (anhydrous) fumaric acid-modified polyolefin resins, (anhydrous) itaconic acid-modified polyolefin resins, and (meth)acrylic acid-modified polyolefin resins. These can be used individually or in combination of two or more types. Preferably, as a modified polyolefin resin, maleic anhydrous-modified polyolefin resin is used.

[0096] The method for obtaining a modified polyolefin resin is not particularly limited. For example, an unmodified polyolefin resin and a modifying agent can be reacted by a known method. For example, the modifying agent can be added when mixing a styrene elastomer (A) and a cyclic olefin polymer (B). Alternatively, for example, the modifying agent can be 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) can be reacted with the modifying agent. Preferably, the modifying agent is added when mixing the styrene elastomer (A) and the cyclic olefin polymer (B).

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

[0098] Furthermore, when a carboxyl group-containing monomer is used as a modifying agent, a modification initiator may be added as needed. Examples of modification initiators include known graft catalysts, and more specifically, known peroxides and known azo compounds. The proportion of the modification initiator is set appropriately according to the purpose and application.

[0099] Then, a styrene-based elastomer (A) and a cyclic olefin polymer (B) are mixed with a modifier, and a modified polyolefin resin is obtained by reaction. The reaction conditions are not particularly limited and are set appropriately depending on the type and amount of the modifier.

[0100] Such modified polyolefin resins include a styrene elastomer (A) (modified styrene elastomer) modified with a modifying agent and a cyclic olefin polymer (B) (modified cyclic olefin polymer) modified with a modifying agent. of It contains. Modified polyolefin resins can improve adhesion to metals (for example, the conductive layer described later).

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

[0102] (6) Non-polyolefin resins In a low-dielectric resin composition, the resin component may include 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 non-polyolefin resins include (meth)acrylic resins. These can be used individually or in combination of two or more types.

[0103] From the viewpoint of affinity to thermosetting resins, in low dielectric resin compositions, the resin component preferably does not contain non-polyolefin resins. In other words, in low dielectric resin compositions, the resin component preferably consists of the polyolefin resin described above.

[0104] (7) Organic solvents 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. In other words, a diluted solution (solution and / or dispersion) of the low dielectric resin composition may be prepared.

[0105] The solid content concentration of the diluent (solution and / or dispersion) of the low dielectric resin composition is, for example, 5% by mass or more, preferably 10% by mass or more. Alternatively, the solid content concentration of the diluent (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 Low dielectric resin compositions and / or their dilutions may contain known additives. Examples of additives include plasticizers, defoamers, leveling agents, antifungal agents, rust inhibitors, matting agents, flame retardants, thixotropes, tackifiers, thickeners, lubricants, antistatic agents, surfactants, reaction retarders, antioxidants, UV absorbers, hydrolysis inhibitors, weather stabilizers, heat stabilizers, dyes, inorganic pigments, organic pigments, curing agents, crosslinking agents, thermal initiators (thermal radical polymerization initiators), silane coupling agents, tack inhibitors, inorganic particles, and organic particles. These can be used individually or in combination of two or more. The proportion and timing of additive addition are appropriately determined according to the purpose and application.

[0107] (9) Effects The low-dielectric resin composition described above 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 its main chain in specific proportions. Therefore, the low-dielectric resin composition has excellent adhesion and low dielectric properties, as well as excellent heat resistance and, in addition, excellent affinity (compatibility and adhesion) to thermosetting resins.

[0108] The relative permittivity (measurement conditions; 10 GHz) of the low dielectric resin composition (solid content) is, for example, 1.5 or higher, preferably 1.9 or higher. Alternatively, the relative permittivity (measurement conditions; 10 GHz) of the low dielectric resin composition (solid content) is, for example, 3.0 or lower, preferably 2.5 or lower. The relative permittivity is measured in accordance with the examples described later (the same applies hereafter).

[0109] The dielectric loss tangent (measurement conditions; 10 GHz) of the low dielectric adhesive composition (solid content) is, for example, 0.0001 or higher, preferably 0.0003 or higher. Furthermore, the dielectric loss tangent (measurement conditions; 10 GHz) of the low dielectric adhesive composition (solid content) is, for example, 0.004 or lower, preferably 0.002 or lower. The relative permittivity is measured according to the examples described later.

[0110] Such low-dielectric resin compositions are suitably used as adhesion promoters and / or low-dielectric adhesives in the manufacture of laminates.

[0111] 2. Laminate A laminate is a circuit board or a circuit board material. A circuit board is, for example, a laminate comprising a conductive 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 comprising a conductive layer (non-circuit layer) that does not have a circuit pattern, and into which a circuit pattern can be formed by processing. An example of a circuit board material is a copper-clad laminate.

[0112] The laminate is manufactured using a low-dielectric resin composition. The following describes in detail a method for manufacturing a circuit board or circuit board material as a laminate using a low-dielectric resin composition.

[0113] (1) First Embodiment Figure 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 Figure 1, the copper-clad laminate 1 comprises an adhesive insulating layer (hereinafter referred to as the 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 includes a resin molded product having low dielectric properties and adhesive properties (hereinafter referred to as a low-dielectric adhesive molded product). Preferably, the adhesive insulating layer 2 consists of a low-dielectric adhesive molded product, or consists of an impregnated substrate and a low-dielectric adhesive molded product.

[0116] Low dielectric adhesive molded products are, for example, molded and cured products of the following low dielectric adhesive compositions (molding materials).

[0117] A 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 can be used individually or in combination of two or more. Polyphenylene ether resins are preferred as thermosetting resins.

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

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

[0121] Low dielectric adhesive compositions (molding materials) are prepared, for example, by mixing a thermosetting resin and an adhesion promoter in a known manner.

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

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

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

[0125] Furthermore, low-dielectric adhesive compositions (molding materials) may include additives in addition to thermosetting resins and adhesion promoters. Examples of additives include plasticizers, defoamers, leveling agents, antifungal agents, rust inhibitors, matting agents, flame retardants, thixotropes, tackifiers, thickeners, lubricants, antistatic agents, surfactants, reaction retarders, antioxidants, UV absorbers, hydrolysis inhibitors, weather stabilizers, heat stabilizers, dyes, inorganic pigments, organic pigments, curing agents, crosslinking agents, thermal initiators (thermal radical polymerization initiators), silane coupling agents, tack inhibitors, inorganic particles, and organic particles. These can be used individually or in combination of two or more. The proportion and timing of additive addition are set appropriately according to the purpose and application.

[0126] Low dielectric adhesive compositions (molding materials) preferably contain a thermal initiator from the viewpoint of thermosetting properties. 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-butylperoxy-isopropyl)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 thermal initiator added is, for example, 0.1 parts by mass or more, preferably 1.0 part by mass or more, per 100 parts by mass of the total amount of resin components in the adhesion promoter (low dielectric resin composition). Alternatively, the amount of thermal initiator added is, for example, 10 parts by mass or less, preferably 5 parts by mass or less, per 100 parts by mass of the total amount of resin components in the adhesion promoter (low dielectric resin composition).

[0128] For example, if the adhesive insulating layer 2 is made of a low-dielectric adhesive molded product, the adhesive insulating layer 2 is formed by molding and curing a low-dielectric adhesive composition (molding material) in a known manner.

[0129] For example, a 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. This yields a coating of the low-dielectric adhesive composition (molding material). The coating is then cured by heating (thermosetting).

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

[0131] Furthermore, for example, if the adhesive insulating layer 2 consists of an impregnated substrate and a low-dielectric adhesive molded product, the adhesive insulating layer 2 is formed by impregnating the impregnated substrate with a low-dielectric adhesive composition (molding material), drying and curing it.

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

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

[0134] The shape and size of the low-dielectric adhesive molded product (adhesive insulating layer 2) are set as appropriate according to the purpose and application.

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

[0136] The conductor layer 4 is disposed on at least one side of the adhesive insulating layer 2. Preferably, the conductor layer 4 is disposed on both sides of the adhesive insulating layer 2. In Figure 1, the conductor layer 4 is disposed on both sides of the adhesive insulating layer 2.

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

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

[0139] The copper-clad laminate 1 described above has an insulating layer 2. The insulating layer 2 includes the low-dielectric adhesive molded product described above. Therefore, in the copper-clad laminate 1, the insulating layer 2 has excellent adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, it has excellent affinity (compatibility, adhesion) to thermosetting resins, and therefore has excellent strength.

[0140] Furthermore, the above-mentioned adhesion promoter (additive), low-dielectric adhesive composition (molding material), and low-dielectric adhesive molded product (adhesive insulating layer 2) include the above-mentioned 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 adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, excellent affinity (compatibility) with thermosetting resins, and therefore have excellent strength.

[0141] (2) Second Embodiment Figure 2 is a schematic cross-sectional view showing a circuit board as a second embodiment of the laminate. In the second embodiment, as in 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 conductive layer 4 of the copper-clad laminate 1 can be etched by a known method to form a circuit 14. As a result, a circuit board 11 as a second embodiment of the laminate is formed, as shown in Figure 2.

[0143] In such a circuit board 11, the adhesive insulating layer 2 contains a low-dielectric adhesive molded product. Therefore, in the circuit board 11, the adhesive insulating layer 2 has excellent adhesion and low dielectric properties, as well as excellent heat resistance, and in addition, it has excellent affinity (compatibility and adhesion) to thermosetting resins, and thus has excellent strength.

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

[0145] In Figure 3, the copper-clad laminate 21 comprises an insulating layer 22, a conductive layer 24 positioned opposite the insulating layer 22, and an adhesive layer 23 positioned between the insulating layer 22 and the conductive layer 24 to bond them together. In the copper-clad laminate 21, the 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 (non-adhesive insulating layer). The insulating layer 22 includes, for example, the thermosetting resin described above. Preferably, the insulating layer 22 is made of the thermosetting resin described above.

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

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

[0149] When manufacturing a copper-clad laminate 21, for example, first, an insulating layer 22 and a conductive layer 24 are prepared. Next, a low-dielectric adhesive is applied to one side of the insulating layer 22. Then, the conductive layer 24 is bonded to one side of the low-dielectric adhesive, and the low-dielectric adhesive is dried. This yields a copper-clad laminate 21. It can also be manufactured in the reverse order of the above. That is, in this method, a low-dielectric adhesive is applied to one side of the conductive layer 24. Then, the insulating layer 22 is bonded to one side of the low-dielectric adhesive, and the low-dielectric adhesive is dried. This yields a copper-clad laminate 21.

[0150] In the copper-clad laminate 21 described above, the insulating layer 22 and the conductive layer 24 are bonded together by an adhesive layer 23 (low dielectric adhesive). In other words, the copper-clad laminate 21 has an adhesive layer 23. The adhesive layer 23 (low dielectric adhesive) contains the low dielectric resin composition described above. Therefore, in the copper-clad laminate 21, the adhesive layer 23 (low dielectric adhesive) has excellent adhesion and low dielectric properties, as well as excellent heat resistance and, in addition, excellent affinity (adhesion) to 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. However, 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 may not have an 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 together by the adhesive layer 23. In such a case, the adhesive layer 23 also serves as the insulating layer 22.

[0152] (4) Fourth Embodiment Figure 4 is a schematic cross-sectional view showing a circuit board as a fourth embodiment of the laminate. In the fourth embodiment, as in the third embodiment, the low dielectric resin composition described above 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 conductive layer 24 of the copper-clad laminate 21 can be etched by a known method to form a circuit 34. As a result, a circuit board 31 as a fourth embodiment of the laminate is formed, as shown in Figure 4.

[0154] In such a circuit board, the insulating layer 22 and the circuit 34, which consists of a conductive layer, are bonded together by an adhesive layer 23.

[0155] In such a circuit board 31, the insulating layer 22 and the circuit 34, which consists of a conductive 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 adhesion and low dielectric properties, as well as excellent heat resistance and, in addition, excellent affinity (adhesion) to 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 may not have an 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 together by the adhesive layer 23. In such a case, the adhesive layer 23 also serves as the insulating layer 22.

[0157] (5) Fifth embodiment Figures 5 to 8 are cross-sectional process views 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] In Figures 5 to 8, the circuit board 41 is a multilayer circuit board having at least two conductive layers. More specifically, as shown in Figure 8O, the circuit board 41 comprises a first conductive layer 40, a second conductive layer 50 positioned opposite the first conductive layer 40, and an adhesive layer 51 positioned between the first conductive layer 40 and the second conductive layer 50 to bond them 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] To manufacture such a circuit board 41, first, as shown in Figure 5A, a copper foil with a carrier is prepared. 42 Prepare the following: Copper foil with carrier 42It comprises 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 includes known release sheets. The copper foil 44 is laminated onto the carrier layer 43 by a known method. The thickness of the copper foil 44 is set as appropriate depending on the purpose and application. The copper foil 44 is also surface-treated as necessary. Examples of surface treatments include roughening treatment.

[0161] Next, in this method, a first resist layer 45 of a predetermined shape is formed on one surface of the copper foil 44, as shown in Figure 5B. The first resist layer 45 is formed, for example, by applying a known resist solution, exposing it to light, and developing it. Alternatively, the first resist layer 45 can also be formed by exposing and etching a dry film resist.

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

[0163] Next, in this method, the first resist layer 45 is removed by a known method, as shown in Figure 6D. Then, in this method, the copper foil 44 exposed from the first plating layer 46 is removed by a known method, as shown in Figure 6E. This forms a first conductive layer 40 comprising the remaining copper foil 44 and the first plating layer 46 laminated on the copper foil 44. In other words, the first conductive layer 40 comprises the copper foil 44 and the first plating layer 46. Preferably, the first conductive layer 40 consists of the copper foil 44 and the first plating layer 46.

[0164] Next, in this method, as shown in Figure 6F, an adhesive layer 51 made of a low-dielectric adhesive is laminated onto the carrier layer 43, the first plating layer 46, and the copper foil 44.

[0165] More specifically, this method involves, for example, creating a cast film of a low-dielectric adhesive. The cast film is then pressed onto the carrier layer 43, the first plating layer 46, and the copper foil 44. This causes the cast film to cover 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 prepared separately. The carrier-attached copper foil 52 comprises a carrier layer 53 and a copper foil 54 laminated on the other side of the carrier layer 53. In this method, as shown in Figure 6G, the copper foil 54 of the carrier-attached copper foil 52 is laminated onto the adhesive layer 51.

[0167] Next, in this method, as shown in Figure 7H, the carrier layer 53 of the carrier-attached copper foil 52 is peeled off. Next, in this method, as shown in Figure 7I, the copper foil 54 and the adhesive layer 51 are opened in a known manner to form via holes 58. The first plating layer 46 is also exposed through the via holes 58. Next, in this method, as shown in Figure 7J, a conductive material is filled into the via holes 58 to form via fills 59. Copper is an example of the conductive material.

[0168] Next, in this method, a second resist layer 55 of a predetermined shape is formed on one surface of the copper foil 54, as shown in Figure 7K. The second resist layer 55 is formed, for example, by applying a known resist solution, exposing it to light, and developing it. Alternatively, the second resist layer 55 can also be formed from a dry film resist, similar to the first resist layer 45.

[0169] Next, in this method, a second plating layer 56 is formed as shown in Figure 8L. The second plating layer 56 is formed, for example, by electroplating. As a result, the second plating layer 56 is formed on one side surface of the copper foil 54 in the reverse pattern of the second resist layer 55. That is, the second plating layer 56 has a circuit pattern.

[0170] Next, in this method, the second resist layer 55 is removed by a known method, as shown in Figure 8M. Then, in this method, the copper foil 54 exposed from the second plating layer 56 is removed by a known method, as shown in Figure 8N. This forms a second conductive layer 50 comprising the remaining copper foil 54 and the first plating layer 56 laminated on the copper foil 54. In other words, the second conductive layer 50 comprises the copper foil 54 and the second plating layer 56. Preferably, the second conductive layer 50 consists of the copper foil 54 and the second plating layer 56.

[0171] Subsequently, in this method, the carrier layer 43 is peeled off as shown in Figure 8O. This exposes the copper foil 44. As a result, the circuit board 1 is formed.

[0172] In the circuit board 41 described above, the first conductor layer 40 and the second conductor layer 50 are bonded together by an adhesive layer 51 (low dielectric adhesive). In other words, the circuit board 41 has an adhesive layer 51. The adhesive layer 51 (low dielectric adhesive) contains the low dielectric resin composition described above. Therefore, in the circuit board 41, the adhesive layer 51 (low dielectric adhesive) has excellent adhesion and low dielectric properties, and furthermore, excellent heat resistance. [Examples]

[0173] Next, the present invention will be described based on examples and comparative examples, but the present invention is not limited thereto. Unless otherwise specified, "parts" and "%" refer to mass. Furthermore, specific numerical values ​​such as blending ratios (content percentages), physical properties, and parameters used in the following description may be replaced with the corresponding upper limits (numerical values ​​defined as "less than or equal to" or "less than") or lower limits (numerical values ​​defined as "greater than or equal to" or "greater than") of the blending ratios (content percentages), physical properties, and parameters described in the "Modes for Carrying Out the Invention" above.

[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) 55000 Kraton G1730; Styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 20% by mass, weight-average molecular weight (Mw) 93000 Kraton G1652; Styrene-ethylene-butylene-styrene copolymer (SEBS), styrene unit content 30% by mass, weight-average molecular weight (Mw) 75000 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) 88000 SEPTON 2104; Styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 65% by mass, weight-average molecular weight (Mw) 60000

[0175] Preparation Example 2-1 (Cyclic Olefin Polymer (B-1)) (1) Catalyst preparation process VO(OC2H5)Cl2 was diluted with cyclohexane to obtain a vanadium catalyst solution. The vanadium concentration in the catalyst solution was 6.7 mmol / L.

[0176] Also, ethylaluminum sesquichloride (Al(C2H5) 1.5 Cl 1.5 The solution was diluted with cyclohexane to obtain an aluminum catalyst solution. The aluminum concentration of the catalyst solution was 107 mg. Ri It was moles / L.

[0177] (2) Polymerization process Using a stirred polymerizer (inner diameter 500 mm, reaction volume 100 L), ethylene and tetracyclo[4.4.0.1 2.5 .1 7.10 ]-3-dodecene was continuously supplied and copolymerized. Note that ethylene and tetracyclo[4.4.0.1 2.5 .1 7.10 The glass transition temperature (Tg) of the cyclic olefin polymer was adjusted by controlling the ratio with ]-3-dodecene.

[0178] Furthermore, the vanadium catalyst solution was supplied to the polymerizer so that the vanadium catalyst concentration in the cyclohexane within the polymerizer was 0.6 mmol / L. The aluminum catalyst solution was also supplied to the polymerizer so that the molar ratio of aluminum to vanadium (Al / V) was 12.0. The polymerization temperature was set to 12°C. The polymerization pressure was set to 3.1 kg / cm². 2 G (gauge pressure) was used.

[0179] This results in ethylene and tetracyclo[4.4.0.1 2.5 .1 7.10 A copolymer with ]-3-dodecene (cyclic olefin polymer (B-1)) was obtained. The copolymer was obtained as a solution in cyclohexane (solvent).

[0180] (3) Decalcification process The copolymer solution was removed from the polymerizer. A 25% by mass NaOH solution was added to the copolymer solution to stop the reaction. This also removed the catalyst residue from the copolymer solution (damine treatment). The copolymer concentration in the solution was 7.7% by mass.

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

[0182] After that, a stirring tank (effective volume 1.0 cm³) 3 The copolymer solution was stirred for 1 hour using [a specific method / tool]. The solid content concentration of the copolymer was 5% by mass.

[0183] (4) Desolvent step Double pipe heater (outer pipe diameter 2B, inner pipe diameter 3 / 4B, length 21m, heat source 20kg / cm 2 A copolymer solution (solid content concentration 5% by mass) was supplied to steam (G) 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 27m, heat source 20kg / cm²) 2 Cyclohexane was removed from the copolymer solution using steam (G) and a flash hopper (200 L volume). Unreacted monomers were also removed along with the cyclohexane.

[0185] This yielded 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. Furthermore, the weight-average molecular weight (polystyrene equivalent, measured by gel permeation chromatography) of the cyclic olefin polymer (B-1) was 113,000.

[0186] Preparation Example 2-2 (Cyclic Olefin Polymer (B-2)) A cyclic olefin polymer (B-2) was obtained using the same method as in Preparation Example 2-1. However, ethylene and tetracyclo[4.4.0.1 2.5 .1 7.10 The glass transition temperature (Tg) of the cyclic olefin polymer was adjusted by changing the composition ratio with ]-3-dodecene.

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

[0188] Preparation Example 2-3 (Cyclic Olefin Polymer (B-3)) A cyclic olefin polymer (B-3) was obtained using the same method as in Preparation Example 2-1. However, ethylene and tetracyclo[4.4.0.1 2.5 .1 7.10 The glass transition temperature (Tg) of the cyclic olefin polymer was adjusted by changing the composition ratio with ]-3-dodecene.

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

[0190] Preparation Example 3-1 (Other Olefin Polymers (C-1)) 900 mL of hexane and 90 g of 1-butene were added to a 2-liter autoclave that had been purged 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 was added to the autoclave. Additionally, 0.001 mmol of rac-dimethylsilylene-bis{1-(2-methyl-4-phenylindenyl)}zirconium dichloride (Zr equivalent) was added to the autoclave.

[0192] Subsequently, propylene was continuously supplied to the autoclave. The total pressure was then set to 7 kg / cm². 2 While maintaining a temperature of G, 1-butene and propylene were polymerized for 30 minutes. A random copolymer of 1-butene and propylene (other olefin polymers (C-1)) was obtained.

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

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

[0195] Preparation Example 3-2 (Other Olefin Polymers (C-2)) The following commercially available products were prepared as other olefin polymers (C-2). Product name Vistamaxx 6102; Propylene-ethylene copolymer (PER), Styrene unit amount 0% by mass, Weight-average molecular weight (Mw) 320,000, Melting point 107°C, Manufactured by ExxonMobil Japan G.K.

[0196] Preparation Example 3-3 (Other Olefin Polymers (C-3)) The following commercially available products were prepared as other olefin polymers (C-3). Product name: Vistamaxx 3020FL; Propylene-ethylene copolymer (PER), Styrene unit amount: 0% by mass, Weight-average molecular weight (Mw): 370,000, Melting point: 64°C, Manufactured by ExxonMobil Japan G.K.

[0197] 2. Preparation of the 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), used as a modifier, was added to the resin component at a ratio of 1 part by mass per 100 parts by mass of the total amount of the resin component.

[0199] In addition, 2,5-dimethyl-2,5-bis(t-butylperoxy)hexane (peroxide, modification 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] Then, the resin components were melt-kneaded at 230°C using a twin-screw compounding extruder with vents. This yielded a low-dielectric resin composition (D-1). Hereinafter, the low-dielectric resin composition will simply be referred to as the resin composition.

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

[0202] Example 2~ 10, Reference Example 11, Example 12, Reference Example13 and Comparative Examples 1-9 (Resin Compositions (D-2)-(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 permittivity and measurement of dielectric loss tangent A solution of the resin composition was applied to a release film (polyethylene terephthalate film, 100 μm thick) and dried at 100°C for 1 minute. This yielded a dried coating of the resin composition (film thickness approximately 60 μm).

[0204] The dried coating film was formed into strips, and the relative permittivity and dielectric loss tangent of the dried coating film were measured in accordance with JIS R1641 (2007). A cavity resonator (vector network analyzer HP8510B (Keysight Technologies)) was used for the measurement. The measurement frequency was set to 10 GHz.

[0205] (2) Compatibility (affinity for thermosetting resins) Polyphenylene ether (hereinafter referred to as PPE) was prepared as the thermosetting resin. The PPE was dissolved in toluene to obtain a PPE solution.

[0206] A solution of PPE and a solution of the above-mentioned resin composition were mixed to obtain a mixed solution. The mass ratio of PPE to the resin composition (PPE:resin composition) was set to 7:3.

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

[0208] The haze of the dried paint 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 paint film was evaluated based on the haze value and visual inspection. The evaluation criteria are as follows.

[0209] 5. The entire coating is homogeneous. Also, the haze is less than 25. 4. The entire coating is homogeneous. Also, the haze is 25 or higher. 3. The coating film is undergoing phase separation. The phase-separated areas are uniformly distributed throughout the coating film. 2. The coating film is undergoing phase separation. The phase-separated portion is non-uniform. The maximum length of the non-uniform portion is less than 1 cm. 1. The coating film is undergoing phase separation. The phase-separated area is non-uniform. The maximum length of the non-uniform area is 1 cm or more.

[0210] Furthermore, improving the affinity of the resin composition to the thermosetting resin will also improve the adhesion. In addition, improving the affinity of the resin composition to the thermosetting resin will also improve the strength of the molded product.

[0211] (3) Heat resistance 2,5-dimethyl-2,5-bis(t-butylperoxy)hexane (trade name Perhexine 25B, manufactured by Nippon Oil & Fats Co., Ltd.) was added as a thermal initiator to a solution of the resin composition. 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® petri dish and dried at 100°C for 1 minute. This yielded 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. Subsequently, the shear storage modulus (G') of the dried coating film was measured. A viscoelasticity measuring device (MCR302 (Anton Paar Japan)) was used for the measurement. The measurement conditions were as follows:

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

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

[0216] ○; The shear storage modulus (G') at 200°C is 1500 Pa or higher. △; The shear storage modulus (G') at 200℃ is between 1000 Pa and 1500 Pa. ×; The shear storage modulus (G') at 200°C is less than 1000 Pa.

[0217] (4) Solubility in solvents The solubility of the resin composition in toluene was evaluated by visual inspection of a solution of the resin composition (solid content concentration 20% by mass, toluene solution). The evaluation criteria are as follows.

[0218] ○; When the resin composition and solvent are stirred and allowed to stand, the solution is a uniform liquid. △; The mixture of the resin composition and the solvent is in a uniform gel-like state. ×; Precipitates are observed in the mixture of the resin composition and the solvent. Furthermore, the mixture as a whole is non-uniform.

[0219] [Table 1]

[0220] [Table 2]

[0221] [Table 3]

[0222] [Table 4]

[0223] Details of the abbreviations in the table are as follows. Styrene unit content; percentage (by 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) 55000, manufactured by Kuraray. Kraton G1730; Styrene-ethylene-propylene-styrene copolymer (SEPS), styrene content 20% by mass, weight-average molecular weight (Mw) 93000, manufactured by Kraton Polymers Japan. Kraton G1652; Styrene-ethylene-butylene-styrene copolymer (SEBS), styrene content 30% by mass, weight-average molecular weight (Mw) 75,000, manufactured by Kraton Polymers 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) 88000, manufactured by Kuraray. SEPTON 2104; Styrene-ethylene-propylene-styrene copolymer (SEPS), styrene unit content 65% by mass, weight-average molecular weight (Mw) 60000, manufactured by Kuraray. MAH; denaturant, carboxyl group-containing monomer, maleic anhydride

[0224] The above invention is provided as an illustrative embodiment of the present invention, but this is merely illustrative and should not be interpreted restrictively. Modifications of the present invention that are obvious to those skilled in the art are included in the claims below. [Industrial applicability]

[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, The aforementioned polyolefin resin Styrene-based elastomer (A) and It contains a cyclic olefin polymer (B) having an alicyclic ring in its main chain, With respect to 100 parts by mass of the total amount of the styrene-based elastomer (A) and the cyclic olefin polymer (B), the content ratio of the styrene-based elastomer (A) is 30 parts by mass or more and 89 parts by mass or less. The styrene-based elastomer (A) contains structural units derived from styrene, and the proportion of structural units derived from styrene relative to the total amount of the styrene-based elastomer (A) is 5% by mass or more and 90% by mass or less. The weight-average molecular weight of the styrene-based elastomer (A) is between 10,000 and 500,000. A low-dielectric resin composition in which the glass transition temperature of the cyclic olefin polymer (B) is 70°C or higher and 120°C or lower.

2. The weight-average molecular weight of the styrene-based elastomer (A) is between 70,000 and 110,000. The low dielectric resin composition according to claim 1.

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 ratio of the structural units derived from styrene relative to the total amount of the styrene-based elastomer (A) is 10% by mass or more and 40% by mass or less.

4. The low dielectric resin composition according to claim 1, wherein the styrene-based elastomer (A) does not contain structural units 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.

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 includes a carboxyl group-containing monomer.

8. An adhesion promoter comprising the low dielectric resin composition described in claim 1.

9. It contains a thermosetting resin and the adhesion agent described in claim 8, A low-dielectric adhesive composition wherein the thermosetting resin comprises at least one selected from the group consisting of epoxy resins, polyphenylene ether resins, fluororesins, polyimide resins, phenolic resins, melamine resins, polyolefin resins having unsaturated double bonds, and liquid crystal polymers.

10. A low-dielectric adhesive molded article comprising a cured product of the low-dielectric adhesive composition described in claim 9.

11. An insulating layer comprising the low dielectric adhesive molded product described in claim 10, A conductive layer disposed on at least one side of the insulating layer A laminate comprising the above.

12. A low-dielectric adhesive comprising the low-dielectric resin composition described in claim 1.

13. Insulating layer and, A conductor layer positioned opposite the insulating layer, An adhesive layer is disposed between the insulating layer and the conductor layer and adheres the insulating layer and the conductor layer together. Equipped with, A laminate in which the adhesive layer comprises the low-dielectric adhesive described in claim 12.

14. The first conductor layer, A second conductor layer is disposed opposite to the first conductor layer, An adhesive layer is disposed between the first conductor layer and the second conductor layer to bond the first conductor layer and the second conductor layer. Equipped with, A laminate in which the adhesive layer comprises the low-dielectric adhesive described in claim 12.