Low dielectric resin composition having high glass transition temperature, prepreg, and metal laminate

Abstract

To provide a low dielectric resin composition having a high glass transition temperature which contains a resin system, a halogen-free flame retardant, a coupling agent and an inorganic filler.SOLUTION: A resin system contains a low dielectric resin formed of a monomer composition containing styrene, divinyl benzene and vinyl, which are added by specific wt.%, a crosslinking agent and polyindan. The glass transition temperature of a low dielectric resin composition having a high glass transition temperature is 200°C or higher, relative dielectric constant (Dk) at 10 GHz of the resin composition after curing is 3.0 to 3.2, and a dielectric loss tangent (Df) is less than 0.0013. There are provided a prepreg and a metal laminate which use the low dielectric resin composition having the high glass transition temperature.SELECTED DRAWING: Figure 1

Description

Technical Field

[0001] The present invention relates to a resin composition and its applications, and particularly to a resin composition having low dielectric properties and a high glass transition temperature, and a prepreg and a metal laminate manufactured from the resin composition.

Background Art

[0002] 5G communication realizes a faster and lower-latency transmission effect due to its high-frequency and short-wavelength characteristics. Currently, the most concerning properties in the application fields of 5G are the dielectric constant and dissipation factor of materials. Materials with low dielectric properties can reduce signal loss and heat generation in the application of 5G high-frequency signal transmission. Therefore, in the industry, the development of materials with required low dielectric properties is being actively carried out.

[0003] Among resin materials, polytetrafluoroethylene (PTFE) and polyphenylene ether (PPO / PPE) with low dielectric constants and loss factors have attracted particular attention. Among them, polytetrafluoroethylene not only has poor processability but also poor adhesion to copper foil, and is not suitable for the manufacture of circuit boards for multilayer wiring and high-density wiring design. Polyphenylene ether has very excellent processability compared to polytetrafluoroethylene and has become one of the main alternatives to polytetrafluoroethylene. Currently, low-dielectric materials mainly composed of polyphenylene ether developed are adopted by many manufacturers of copper-clad laminates (CCL).

[0004] In high-speed products such as high-end server products, dielectric loss of the substrate is emphasized. However, it is difficult to further reduce the loss factor (for example, dielectric tangent) to a lower level in low-dielectric materials mainly composed of polyphenylene ether. Although it is possible to reduce the loss factor by combining with different types of low-dielectric resins from polyphenylene ether, the glass transition temperature (Tg) is likely to decrease, so the applications are limited.

[0005] Therefore, a low dielectric constant material having a low dielectric constant, a low loss factor, and a high glass transition temperature is an important goal for those skilled in the art.

Summary of the Invention

Problems to be Solved by the Invention

[0006] One of the objects of the present invention is to provide a resin composition having a low dielectric constant and a high glass transition temperature in view of the deficiencies of the prior art. The resin composition having a low dielectric constant and a high glass transition temperature can be applied to a plate after curing, which is advantageous for high-frequency and high-speed signal transmission of the plate and the long-term reliability of the substrate. The present invention further provides a prepreg and a metal laminate using the resin composition.

Means for Solving the Problems

[0007] In order to achieve the object of the present invention, one technical means adopted by the present invention is to provide a resin composition having a low dielectric constant and a high glass transition temperature, which comprises (A) a resin system, (B) a halogen-free flame retardant, (C) a coupling agent, and (D) an inorganic filler. The (A) resin system comprises 10% to 40% by weight of a low dielectric resin formed of a monomer composition containing styrene, divinylbenzene, and vinyl, 5% to 20% by weight of a crosslinking agent, and 10% to 70% by weight of a polyindane resin, based on the total weight of the resin system. In the resin composition having a low dielectric constant and a high glass transition temperature, the amount of the (B) halogen-free flame retardant used is 20 parts to 45 parts by weight, the amount of the (C) coupling agent used is 0.05 part to 1 part by weight, and the amount of the (D) inorganic filler used is 50 parts to 120 parts by weight, based on 100 parts by weight of the (A) resin system. Further, the glass transition temperature of the resin composition having a low dielectric constant and a high glass transition temperature is 200 °C or higher, the relative dielectric constant (Dk) at 10 GHz after curing of the resin composition having a low dielectric constant and a high glass transition temperature is 3.0 to 3.2, and the dielectric tangent (Df) is less than 0.0013.

[0008] In one embodiment of the present invention, the number average molecular weight of the polyindan resin is 300 g / mol to 1000 g / mol.

[0009] In one embodiment of the present invention, the polyindan resin has reactive functional groups having two or more of an acrylic group, a styrene group, and a maleimide group.

[0010] In one embodiment of the present invention, the number average molecular weight of the low dielectric resin is 4500 g / mol to 6500 g / mol.

[0011] In one embodiment of the present invention, taking all monomer units in the low dielectric resin as 100 mol%, the content of styrene units is 10 mol% to 40 mol%, the content of divinylbenzene units is 10 mol% to 40 mol%, and the content of vinyl units is 10 mol% to 20 mol%.

[0012] In one embodiment, the inorganic filler is silica prepared by a synthesis method, and the average particle diameter D50 of the silica is 2.0 μm to 3.0 μm.

[0013] In one embodiment of the present invention, the specific gravity of the silica is 2.0 to 2.5 g / cm 3 is.

[0014] In one embodiment of the present invention, the halogen-free flame retardant is a compound having a structure represented by the following formula (I).

Chemical formula

Chemical formula

Chemical formula

Chemical formula

[0015] In one embodiment of the present invention, the crosslinking agent is selected from the group consisting of 1,3,5-triallyl cyanurate (TAC), triallyl isocyanurate (TAIC), trimethallyl isocyanurate (TMAIC), diallyl phthalate, divinylbenzene, and 1,2,4-triallyl trimellitate.

[0016] Another object of the present invention is to provide a prepreg. The prepreg is obtained by applying or impregnating the resin composition having low dielectric constant and high glass transition temperature to the reinforcing material.

[0017] Another object of the present invention is to provide a metal laminate. The metal laminate is manufactured by laminating the prepreg and a metal layer, or by applying the resin composition having low dielectric constant and high glass transition temperature to a metal layer. [Advantages of the Invention]

[0018] Generally speaking, the resin composition with low dielectric constant and high glass transition temperature according to the present invention has technical features such as "10 wt% - 40 wt% of a low dielectric resin formed of a monomer composition containing styrene, divinylbenzene, and vinyl, 5 wt% - 20 wt% of a crosslinking agent, and 10 wt% - 70 wt% of a polyindan resin, based on the total weight of the resin system". Due to excellent high-frequency low dielectric characteristics (low Dk / low Df), especially the characteristic of Df < 0.0013, it can maintain stable low transmission loss for a long time and keep the glass transition temperature (Tg) at 200 °C or higher, so that the desired sheet material characteristics (such as water absorption, heat resistance, peeling strength, etc.) in practical applications can be improved.

Brief Description of the Drawings

[0019]

Figure 1

Figure 2

Figure 3

Figure 4

Figure 5

Embodiments for Carrying Out the Invention

[0020] For a better understanding of the features and technical content of the present invention, please refer to the following detailed description of the present invention and the accompanying drawings. However, the provided accompanying drawings are only for reference and explanation, and are not for limiting the scope of the claims of the present invention.

[0021] Hereinafter, embodiments of the present invention will be described by the "resin composition, prepreg, and metal laminate having low dielectric constant and high glass transition temperature" according to certain specific embodiments, and those skilled in the art can understand the advantages and effects of the present invention based on the content disclosed herein. The present invention can be implemented or applied by other different specific embodiments, and for each detail in this specification, various modifications and changes can be made based on different viewpoints and applications without departing from the concept of the present invention. Also, as explained in advance, the accompanying drawings of the present invention are simple schematic illustrations and are not drawn based on actual sizes. The technical content of the present invention will be described in more detail based on the following embodiments, but the disclosed content does not limit the protection scope of the present invention.

[0022] Unless otherwise specified, the terms used in the present invention have meanings generally understood by those skilled in the art. The materials used in the following embodiments are commercially available materials unless otherwise specified. The operations or instruments used in the following examples are common operations or instruments in the technical field unless otherwise specified.

[0023] Conventional low dielectric constant materials mainly have difficulty in further reducing the loss coefficient (e.g., dielectric tangent) to a lower level by using polyphenylene ether as the main component (main composition). By combining with a new low dielectric resin, polydivinylbenzene (PDVB), the loss coefficient can be reduced, but the glass transition temperature (Tg) decreases simultaneously, so there are limitations in applications. Therefore, the present invention proposes a new idea that by combining a low dielectric resin containing styrene, divinylbenzene, and vinyl monomer units with a polyindene resin, it is possible to satisfy a low dielectric loss coefficient while maintaining a sufficient glass transition temperature (Tg).

[0024] Specifically, in the embodiments of the present invention, the concept of the invention is realized to provide a resin composition having low dielectric constant and high glass transition temperature. The composition having low dielectric constant and high glass transition temperature comprises (A) a resin system, (B) a halogen-free flame retardant, (C) a coupling agent, and (D) an inorganic filler. Each component will be described in detail below.

[0025] [(A) Resin system] The resin system constituting the resin composition having low dielectric constant and high glass transition temperature according to the present invention comprises, based on the total weight of the resin system, 10% to 40% by weight of a low dielectric resin, 5% to 20% by weight of a crosslinking agent, and 10% to 70% by weight of a polyindane resin.

[0026] In one embodiment of the present invention, the low dielectric resin is a copolymer essentially containing olefin-based monomers and is formed of a monomer composition containing styrene, divinylbenzene, and vinyl. Here, when divinylbenzene is a monomer unit in the low dielectric resin, it can play a role in improving the glass transition temperature (Tg). When vinyl is a monomer unit in the low dielectric resin, it can play a role in reducing the dielectric tangent (Df). When styrene is a monomer unit in the low dielectric resin, it can play a role in maintaining good heat resistance.

[0027] Preferably, taking all monomer units in the low dielectric resin as 100 mol%, the content of styrene units is 10 mol% to 40 mol%, the content of divinylbenzene units is 10 mol% to 40 mol%, and the content of vinyl units is 10 mol% to 20 mol%. Thereby, it is possible to balance the low dielectric characteristics and the glass transition temperature of the applied plate material.

[0028] In actual application, taking the total weight of the resin system as 100% by weight, the content of the low dielectric resin may be 10% by weight, 15% by weight, 20% by weight, 25% by weight, 30% by weight, 35% by weight, or 40% by weight. The number average molecular weight of the low dielectric resin is 4500 g / mol to 6000 g / mol.

[0029] In an embodiment of the present invention, the polyindane indane resin exhibits a synergistic effect with the low dielectric resin so as to reduce the dissipation factor (Df) while maintaining the glass transition temperature (Tg) at 200 °C or higher. It is particularly noteworthy that the polyindane indane resin can improve the processability, stability, thermal properties, viscoelasticity, rheology, adhesion and / or mechanical properties of the resin composition as a modifier. For example, compared with a conventional resin composition mainly composed of a polyphenylene ether resin, in the resin composition according to the present invention, by using the polyindane indane resin as the main component, the peel strength of the applied sheet material can be improved.

[0030] Preferably, the polyindane indane resin has reactive functional groups having two or more of an acrylic group, a styrene group and a maleimide group, thereby forming a three-dimensional network structure and achieving desired physicochemical properties (e.g., high glass transition temperature, low water absorption, and good heat resistance).

[0031] In actual application, assuming the total weight of the resin system is 100% by weight, the content of the polyindane indane resin may be 10% by weight, 15% by weight, 20% by weight, 25% by weight, 30% by weight, 35% by weight, 40% by weight, 45% by weight, 50% by weight, 55% by weight, 60% by weight, 65% by weight or 70% by weight. The main molecular chain backbone of the polyindane indane resin may contain 90% or more of indane repeating units. Also, the number average molecular weight of the polyindane indane resin is 300 g / mol to 1000 g / mol. Further, the polyindane indane resin can be partially or completely hydrogenated to control the aromaticity, which is advantageous for improving the compatibility.

[0032] In an embodiment of the present invention, the crosslinking agent is a component having an unsaturated functional group containing a double bond or a triple bond, which can cause crosslinking to form a three-dimensional network structure. For example, a monofunctional crosslinking agent (having only one unsaturated functional group in the molecule) or a polyfunctional crosslinking agent (having two or more unsaturated functional groups in the molecule) can be mentioned, but the present invention is not limited thereto. The type of the crosslinking agent is not particularly limited, and preferably, it has good compatibility with the resin component.

[0033] Specifically, the crosslinking agent in the (A) resin system may be selected from the group consisting of 1,3,5-triallyl cyanurate (TAC), triallyl isocyanurate (TAIC), trimethallyl isocyanurate (TMAIC), diallyl phthalate, 1,2,4-triallyl trimellitate, and divinylbenzene. The crosslinking agent may be used alone or in combination.

[0034] Taking the total weight of the resin system as 100% by weight, the content of the crosslinking agent may be 5% by weight, 10% by weight, 15% by weight, 20% by weight, 25% by weight, or 30% by weight.

[0035] In an embodiment of the present invention, the (A) resin system may further contain a polyphenylene ether resin. The terminal of the molecular structure of the polyphenylene ether resin contains an unsaturated functional group. Examples of the unsaturated functional group include a hydroxyl group, a vinyl group, a styrene group, a vinylbenzyl group, an allyl group, an acryloyl group, a methacrylate group, an epoxy group, and a maleimide group, but the present invention is not limited thereto. The unsaturated functional group is a group capable of undergoing an addition polymerization reaction with a component having another unsaturated functional group. The addition polymerization reaction can be caused by light or heat in the presence of a polymerization initiator.

[0036] Specifically, the polyphenylene ether resin in the resin system may be selected from the group consisting of a polyphenylene ether resin having a hydroxyl group at the end, a polyphenylene ether resin having a vinyl group at the end, a polyphenylene ether resin having a styrene group at the end, a polyphenylene ether resin having a vinylbenzyl group at the end, a polyphenylene ether resin having an allyl group at the end, a polyphenylene ether resin having an acryloyl group at the end, a polyphenylene ether resin having a methacrylate group at the end, a polyphenylene ether resin having an epoxy group at the end, and a polyphenylene ether resin having a maleimide group at the end. The polyphenylene ether resin may be used alone or in combination.

[0037] Taking the total weight of the resin system as 100% by weight, the content of the polyphenylene ether resin may be 20% to 60% by weight. It should be noted that in the presence of the polyindane resin, the content of the polyphenylene ether resin in the resin system may be significantly reduced or even set to 0% (without addition).

[0038] The weight average molecular weight of the polyphenylene ether resin may be 1000 g / mol to 20000 g / mol, and preferably 1000 g / mol to 10000 g / mol. If the molecular weight of the polyphenylene ether resin is too large, the fluidity of the polyphenylene ether resin and the solubility in the solvent may deteriorate. If the molecular weight of the polyphenylene ether resin is too small, it may have an adverse effect on the electrical properties and thermal stability of the resin composition.

[0039] When actually applied, two kinds of polyphenylene ether resins may be used in combination in the (A) resin system. For example, a polyphenylene ether resin having a bismaleimide group at the end of the molecular main chain and a polyphenylene ether resin having a hydroxyl group, a styrene group, a methacrylate group or an epoxy group at the end of the molecular main chain may be used in combination, but the present invention is not limited thereto. Alternatively, three kinds of polyphenylene ether resins may be used in combination in the (A) resin system. For example, a polyphenylene ether resin having a bismaleimide group at the end of the molecular main chain, a polyphenylene ether resin having a styrene group at the end of the molecular main chain, and a polyphenylene ether resin having a methacrylate group at the end of the molecular main chain may be used in combination, but the present invention is not limited thereto.

[0040] The method for producing the polyphenylene ether resin having an unsaturated functional group is not the core technology of the present invention and can be obtained or completed by those skilled in the art based on the disclosure content of this specification and the general knowledge they possess.

[0041] [(B) Halogen-free flame retardant] The halogen-free flame retardant constituting the resin composition having low dielectric and high glass transition temperature of the present invention may employ a phosphorus-based flame retardant so as to improve the flame retardancy of the produced electronic material and meet the requirement of being halogen-free. When actually applied, the phosphorus-based flame retardant may be selected from the group consisting of phosphate ester-based flame retardants, phosphazene-based flame retardants, phosphine oxide-based flame retardants, ammonium polyphosphate, melamine polyphosphate, melamine phosphate, and 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO). The halogen-free flame retardant may be used alone or in combination, but the present invention is not limited thereto.

[0042] Specific examples of phosphate-based halogen-free flame retardants include triphenyl phosphate (TPP), tetraphenyl resorcinol bis(diphenylphosphate) (RDP), bisphenol A bis(diphenyl phosphate) (BDP), and Resorcinol bis(di-2,6-xylyl phosphate) (RXP).

[0043] Specific examples of phosphazene-based halogen-free flame retardants include cyclic phosphazene compounds and linear phosphazene compounds.

[0044] Specific examples of phosphine oxide-based halogen-free flame retardants include tris(4-methoxyphenyl)phosphine oxide, diphenylphosphine oxide, triphenylphosphine oxide, and the phosphine oxide compound represented by the following formula (I) (PQ-60 manufactured by Shin-ichi Chemical Industry Co., Ltd.). It should be noted that the phosphine oxide compound having the structure represented by formula (I) has well-known flame retardancy and imparts low dielectric properties to the resin composition, which is advantageous for applications in the high-frequency field.

Chemical formula

Chemical formula

Chemical formula

Chemical formula

Chemical formula

Chemical formula

[0045] (A) With respect to 100 parts by weight of the resin-based material, the usage amount of (B) the halogen-free flame retardant is 20 to 45 parts by weight. For example, it may be 20 parts by weight, 25 parts by weight, 30 parts by weight, 35 parts by weight, 40 parts by weight, or 45 parts by weight, but the present invention is not limited thereto. If the usage amount of the halogen-free flame retardant is less than the above range, the electronic material manufactured from the resin composition cannot achieve the desired flame retardancy. If the usage amount of the halogen-free flame retardant exceeds the above range, it may adversely affect the desired properties such as electrical properties, water absorption, and peel strength.

[0046] [(C) Coupling agent] The coupling agent constituting the resin composition having low dielectric and high glass transition temperature according to the present invention may employ at least one selected from a silane compound and a siloxane compound so as to improve the interfacial bonding strength between the resin and the reinforcing material (for example, fiber cloth) and to improve the compatibility between the resin and the reinforcing material (for example, fiber cloth) and the inorganic powder.

[0047] Specific examples of the silane compound include amino silane, vinyl silane, acrylic silane, and epoxy silane. Specific examples of the siloxane compound include amino siloxane, vinyl siloxane, acrylic siloxane, and epoxy siloxane.

[0048] (A) For 100 parts by weight of the resin system, the amount of the (C) coupling agent used may be 0.05 to 1 part by weight, preferably 0.3 to 0.7 part by weight.

[0049] In one embodiment, for 100 parts by weight of the (A) resin system, the amount of the (C) coupling agent used may be 0.05 part, 0.1 part, 0.2 part, 0.3 part, 0.4 part, 0.5 part, 0.6 part, 0.7 part, 0.8 part, 0.9 part or 1 part by weight.

[0050] [(D) Inorganic filler] The inorganic filler constituting the resin composition having low dielectric constant and high glass transition temperature according to the present invention may be selected from the group consisting of silica, aluminum oxide, zinc oxide, titanium oxide, magnesium oxide, antimony oxide, beryllium oxide, aluminum nitride, boron nitride, calcium carbonate, potassium titanate, glass fiber, barium titanate, barium sulfate, aluminum hydroxide, and magnesium hydroxide. The inorganic filler may be used alone or in combination, but the present invention is not limited thereto. Thereby, while maintaining the relative dielectric constant and dielectric tangent at a low level, properties such as the mechanical strength, thermal conductivity, and heat resistance of the resin composition can be improved, but the present invention is not limited thereto.

[0051] Preferably, the (D) inorganic filler is spherical silica produced by a synthetic method. Also, the spherical silica has a specific gravity of 2.0 to 2.5 g / cm 3 and an average particle diameter D50 of 2.0 to 3.0 μm. The specific gravity of the spherical silica is preferably 2.2 g / cm 3 Moreover, the spherical silica may be surface-modified with at least one functional group among acrylic group and vinyl group so as to give better compatibility with the (A) resin system, not impairing the desired properties in practical use, and being added to the resin composition in a larger amount.

[0052] (A) For 100 parts by weight of the resin system, the amount of (D) inorganic filler used may be 50 to 120 parts by weight, preferably 80 to 110 parts by weight, and more preferably 90 to 110 parts by weight.

[0053] In one embodiment, for 100 parts by weight of the resin system (A), the amount of the inorganic filler (D) used may be 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 105, 110, 115 or 120 parts by weight.

[0054] [Prepreg and Metal Laminate] As shown in FIGS. 1 and 2, the present invention further provides a prepreg 1 and a metal laminate using the resin composition having low dielectric constant and high glass transition temperature. Specifically, the prepreg 1 is obtained by applying or impregnating a resin composition 12 having low dielectric constant and high glass transition temperature to a reinforcing material 11, attaching the resin composition 12 having low dielectric constant and high glass transition temperature to the reinforcing material 11, and further heating at a high temperature to a semi-cured state. The reinforcing material 11 may be, for example, an electronic-grade glass fiber cloth, but the present invention is not limited thereto.

[0055] As shown in FIGS. 3 to 5, the metal laminate may be manufactured by the following method. That is, the prepreg 1 and at least one metal layer 2 (for example, a copper foil layer) are laminated and bonded by hot pressing, or the resin composition 12 having low dielectric constant and high glass transition temperature is applied to the metal layer 2 and dried and cured sufficiently. In a specific example of laminating the prepreg 1 and at least one metal layer 2 (for example, a copper foil layer), a predetermined number of prepregs 1 may be laminated, and the metal layer 2 may be laminated on at least one outer side of the formed laminate 1'.

[0056] In actual application, a printed circuit board can be manufactured by patterning the metal layer 2 on the outside of the metal laminate by a conventional process step.

[0057] [Characteristic Evaluation] Using toluene, the resin compositions shown in Tables 1 and 2 were used to prepare a thermosetting resin varnish. Next, using a glass fiber cloth made by Nanya Plastics (NE1078 made by Nanya Plastics) as a reinforcing material, the thermosetting varnish was impregnated at room temperature and dried at 130 °C for several minutes to obtain a prepreg having a resin content of 70% by weight. Next, four prepregs were sandwiched between two copper foils with a thickness of 35 μm, and hot pressing was performed to obtain a sample of a copper foil substrate with a thickness of 0.4 mm. The hot pressing was first held at a temperature of 85 °C and a pressure of 25 kg / cm 2 for 20 minutes, then heated to 210 °C at a heating rate of 3 °C / min, held for 120 minutes, and then slowly cooled to 130 °C. The obtained samples of copper foil substrates were evaluated for characteristics as described below.

[0058] Glass transition temperature (°C): The glass transition temperature was measured using a Dynamic Mechanical Analyzer (DMA).

[0059] Water absorption rate (%): After heating the sample in a pressure cooker at 2 atm for 120 °C for 120 minutes, the weight change before and after heating was determined.

[0060] T288 solder resistance test (heat resistance): After heating the sample in a pressure cooker at 2 atm for 120 °C for 120 minutes, it was immersed in a solder bath at 288 °C and observed for 1 / 2 hour and 2 hours respectively. If popcorn phenomenon or delamination (layer separation) occurred on the sample substrate, it was rated as "NG". On the other hand, if no popcorn phenomenon or delamination (layer separation) occurred on the sample substrate, it was rated as "PASS".

[0061] Relative dielectric constant (Dk) and dielectric dissipation factor (Df): After removing the copper foil from the sample, it was baked in an oven at 105 °C for 30 minutes, and the relative dielectric constant and dielectric dissipation factor at 10 GHz were measured using an analyzer (E4991A) manufactured by Agilent.

[0062] Peel strength: A copper foil substrate sample of 1 cm × 10 cm was manufactured, and the peel strength between the copper foil and the substrate was measured with a universal testing machine.

[0063] The detailed information of each component in Table 1 and Table 2 is as follows. Low dielectric resin: Poly-DVB manufactured by DENKA. Polyindane resin: NE-X-9480 manufactured by Nippon DIC Corporation. Polyphenylene ether resin: MX9000 manufactured by SABIC. BMI resin-1: MIR-3000-70MT manufactured by Nippon Kayaku Co., Ltd. BMI resin-2: MIR-5000-60T manufactured by Nippon Kayaku Co., Ltd. Crosslinking agent: TAIC manufactured by Evonik. Flame retardant: PQ-60 manufactured by Jin Yi Chemical Industry. Silica produced by the synthetic method: EQ2410-SMC manufactured by China Sanshiji Co., Ltd. Coupling agent: Z-6030 manufactured by Dow Corning. Peroxide: Luperox F manufactured by ARKEMA.

[0064]

Table 1

[0065]

Table 2

[0066] According to Table 1 and Table 2 above, in the resin compositions according to Comparative Examples 1 to 3, only a combination of a polyphenylene ether resin and a low dielectric resin is added, and no polyindan resin is added. Therefore, the Df of the manufactured plate material cannot be reduced to a level lower than 0.0014 or 0.0013, that is, the desired low dielectric characteristics (Low Dk / Low Df) cannot be achieved. In the resin compositions according to Comparative Examples 2 and 3, by further adding a BMI resin, the Tg of the manufactured plate material was improved, but its Df also increased, and there is a risk of an increase in transmission loss. In contrast, in the resin compositions according to Examples 1 to 3, by combining a low dielectric resin and a polyindan resin, a level lower than the desired relative dielectric constant and dielectric tangent can be achieved, and the glass transition temperature (Tg) is maintained at 200 °C or higher, and further, the characteristics required in practical use such as water absorption and heat resistance are not impaired. In addition, the resin compositions according to Examples 1 to 3 were given excellent peel strength to the applied plate material by using a polyindan resin.

[0067] [Advantageous Effects According to Embodiments] The resin composition having low dielectric and high glass transition temperature according to the present invention has, "based on the total weight of the resin system, 10% to 40% by weight of a low dielectric resin formed of a monomer composition containing styrene, divinylbenzene, and vinyl, 5% to 20% by weight of a crosslinking agent, and 10% to 70% by weight of a polyindan resin", and due to the excellent high-frequency low dielectric characteristics (low Dk / low Df), particularly the characteristic of Df < 0.0013, it can maintain a stable low transmission loss for a long time and maintain the glass transition temperature (Tg) at 200 °C or higher. Therefore, the plate material characteristics desired in practical use (such as water absorption, heat resistance, peeling strength, etc.) can be improved.

[0068] The content disclosed above is only a preferred executable embodiment of the present invention, and the scope of the claims of the present invention is not limited thereto. Therefore, all equivalent technical changes made using the content of the specification and drawings of the present invention are included in the scope of the claims of the present invention.

Explanation of Reference Numerals

[0069] 1... Prepreg 11... Reinforcing material 12... Resin composition having low dielectric constant and high glass transition temperature 2... Metal layer

Claims

1. A resin composition comprising (A) a resin system, (B) a halogen-free flame retardant, (C) a coupling agent, and (D) an inorganic filler, wherein: The (A) resin system comprises 10% to 40% by weight of a low dielectric resin formed from a monomer composition containing styrene, divinylbenzene, and vinyl, 5% to 20% by weight of a crosslinking agent, and 10% to 70% by weight of a polyindene resin, based on the total weight of the resin system; Based on 100 parts by weight of the (A) resin system, the amount of the (B) halogen-free flame retardant used is 20 to 45 parts by weight, the amount of the (C) coupling agent used is 0.05 to 1 part by weight, and the amount of the (D) inorganic filler used is 50 to 120 parts by weight; The resin composition has a glass transition temperature of 200 °C or higher, a relative dielectric constant (Dk) at 10 GHz after curing of the resin composition of 3.0 to 3.2, and a dielectric tangent (Df) of less than 0.0013.

2. The resin composition according to Claim 1, wherein the number average molecular weight of the polyindene resin is 300 g / mol to 1000 g / mol.

3. The resin composition according to Claim 2, wherein the polyindene resin has reactive functional groups having two or more of an acrylic group, a styrene group, and a maleimide group.

4. The resin composition according to Claim 1, wherein the number average molecular weight of the low dielectric resin is 4500 g / mol to 6500 g / mol.

5. Based on 100 mol% of all monomer units in the low dielectric resin, the content of styrene units is 10 mol% to 40 mol%, the content of divinylbenzene units is 10 mol% to 40 mol%, and the content of vinyl units is 10 mol% to 20 mol%.

6. The resin composition according to Claim 1, wherein the inorganic filler is silica prepared by a synthetic method, and the average particle diameter D50 of the silica is 2.0 μm to 3.0 μm.

7. The specific gravity of the silica is 2.0 to 2.5 g / cm ３ The resin composition according to claim 6, which is such that.

8. The resin composition according to Claim 1, wherein the halogen-free flame retardant is a compound having a structure represented by the following formula (I). 【Chemical Formula 1】 Here, R １ is a covalent bond, -CH ２ -, 【Chemical 2】 【Chemical Formula 3】 【Chemical 4】 【Chemical Formula 5】 wherein: Here, R ２ , R ３ , R ４ , R ５ are independently H, an alkyl group or [Chemical Formula 6] wherein:

9. The crosslinking agent of the resin composition according to claim 1 is selected from the group consisting of 1,3,5-triallyl cyanurate (TAC), triallyl isocyanurate (TAIC), trimethylallyl isocyanurate (TMAIC), diallyl phthalate, divinylbenzene, and 1,2,4-triallyl trimellitate.

10. A prepreg, characterized in that the resin composition according to claim 1 is applied to or impregnated in the reinforcing material.

11. A metal laminate, characterized in that it is manufactured by laminating the prepreg according to claim 10 and a metal layer, or by applying the resin composition according to claim 1 to a metal layer.

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