WO2025023631A1 - Layered composite filler sheet, manufacturing method therefor, and manufacturing apparatus therefor - Google Patents

Abstract

The present invention provides a layered composite filler sheet, a manufacturing method therefor, and a manufacturing apparatus therefor. The manufacturing method for a layered composite filler sheet according to one embodiment of the present invention comprises the steps of: providing a carrier sheet; forming a first polymer layer by providing a first polymer material on the carrier sheet; forming a filler layer by providing a filler material on the first polymer layer; forming a second polymer layer by providing a second polymer material on the filler layer; and curing at least one of the first polymer layer and the second polymer layer.

Description

Layered composite filler sheet, its manufacturing method and manufacturing device

The technical idea of the present invention relates to a filler sheet, and more specifically, to a layered composite filler sheet, a manufacturing method therefor, and a manufacturing apparatus therefor.

The present invention relates to the Excellent Corporate Research Institute Promotion Project (ATC+) (Project No. 20014176, Project Unique No. 1415187319) which was carried out with the support of the Korea Institute of Industrial Technology Planning and Evaluation with funds from the Ministry of Trade, Industry and Energy.

Next-generation technologies such as 5G communications are bringing about innovation in many application fields such as autonomous driving, virtual reality, medicine, healthcare, and the Internet of Things, and accordingly, development and research on material technologies are actively being conducted. In particular, the development of materials with low permittivity and low dielectric loss characteristics for next-generation communications is required, and composites using various materials such as polymers, metals, and ceramics are being applied as such materials. Conventional composites have a mixed structure in which ceramic fillers are added to a polymer matrix. Since polymer materials and ceramic materials are mixed, various problems such as differences in drying shrinkage, deterioration of uniformity due to deterioration of dispersibility, Bernard cell phenomenon, deterioration of bonding strength, and defects caused by fillers may occur, and therefore, there is a limit to the amount of ceramic filler added. It is possible to minimize the occurrence of defects by using fabric sheets and prevent surface defects by using additives such as leveling agents or slip agents, but there is a limit to the amount of filler added.

Therefore, a composite filler sheet that can prevent the above-described problems and easily control desired properties is required.

The technical problem to be achieved by the technical idea of the present invention is to provide a layered composite filler sheet, a manufacturing method therefor, and a manufacturing device therefor.

However, these tasks are exemplary and the technical idea of the present invention is not limited thereto.

According to one aspect of the present invention, a layered composite filler sheet, a manufacturing method therefor, and a manufacturing apparatus therefor are provided.

According to one embodiment of the present invention, the method for manufacturing the layered composite filler sheet may include the steps of: providing a carrier sheet; providing a first polymer material on the carrier sheet to form a first polymer layer; providing a filler material on the first polymer layer to form a filler layer; providing a second polymer material on the filler layer to form a second polymer layer; and curing at least one of the first polymer layer and the second polymer layer.

According to one embodiment of the present invention, the step of forming the first polymer layer can be performed by tape casting the first polymer material onto the carrier sheet to form the first polymer layer.

According to one embodiment of the present invention, the step of forming the filler layer can be accomplished by forming the filler layer by spraying or tape casting the filler material on the first polymer layer.

According to one embodiment of the present invention, the step of forming the filler layer may include the step of providing a first filler material on the first polymer layer to form a first filler layer; and the step of providing a second filler material on the first filler layer to form a second filler layer.

According to one embodiment of the present invention, the first filler material and the second filler material may include the same material or different materials.

According to one embodiment of the present invention, the step of forming the second polymer layer can be accomplished by forming the second polymer layer by spraying or tape casting the second polymer material onto the filler layer.

According to one embodiment of the present invention, the curing step can be performed by curing at least one of the first polymer layer and the second polymer layer by applying thermal energy or light energy.

According to one embodiment of the present invention, in the step of forming the first polymer layer, nanosheets can be provided so that the first polymer layer contains nanosheets.

According to one embodiment of the present invention, the step of providing the carrier sheet and the step of curing can be performed as a continuous process.

According to one embodiment of the present invention, the step of providing the carrier sheet and the step of curing can be performed in a roll-to-roll manner.

According to one embodiment of the present invention, the method for manufacturing the layered composite filler sheet may include: providing a carrier sheet; providing a first polymer material on the carrier sheet to form a first polymer layer; providing a filler material on the first polymer layer to form a filler layer; and curing the first polymer layer.

According to one embodiment of the present invention, the layered composite filler sheet may include: a first polymer layer; and a filler layer disposed on the first polymer layer and including a filler material.

According to one embodiment of the present invention, the first polymer layer may further include a carrier sheet formed of a metal sheet, a polymer sheet, a ceramic sheet, glass, or copper foil.

According to one embodiment of the present invention, the first polymer layer may include at least one of polyamic acid, polyimide, modified polyimide, polytetrafluoroethylene, polyphenyl ether, polyphenyl oxide, polyphenyl sulfide, polystyrene, polyacrylic acid, epoxy, polyvinyl butyral, polyvinyl pyrrolidone, ethylene carbonate, polyvinyl alcohol, polyvinyl chloride, polyethylene, polypropylene, and liquid crystal polymer.

According to one embodiment of the present invention, the filler layer may include at least one of a dielectric material, a piezoelectric material, a heat-dissipating material, and a magnetic material.

According to one embodiment of the present invention, the filler layer may include at least one of a ceramic material, a metal material, and a carbon-based material.

According to one embodiment of the present invention, the filler layer may include a first filler layer including a first filler material; and a second filler layer including a second filler material and disposed on the first filler layer.

According to one embodiment of the present invention, a second polymer layer may be further included disposed on the filler layer.

According to one embodiment of the present invention, the second polymer layer may include at least one of polyamic acid, polyimide, modified polyimide, polytetrafluoroethylene, polyphenyl ether, polyphenyl oxide, polyphenyl sulfide, polystyrene, polyacrylic acid, epoxy, polyvinyl butyral, polyvinyl pyrrolidone, ethylene carbonate, polyvinyl alcohol, polyvinyl chloride, polyethylene, polypropylene, and liquid crystal polymer.

According to one embodiment of the present invention, the first polymer layer may contain nanosheets.

According to one embodiment of the present invention, the device for manufacturing the layered composite filler sheet may include a first polymer layer forming unit that forms a first polymer layer by providing a first polymer material on a carrier sheet; a filler layer forming unit that forms a filler layer on the first polymer layer; a second polymer layer forming unit that forms a second polymer layer by providing a second polymer material on the filler layer; and a curing unit that cures at least one of the first polymer layer and the second polymer layer.

According to the technical idea of the present invention, the layered composite filler sheet, its manufacturing method, and its manufacturing apparatus have a layered structure composed of a polymer layer and a filler layer, and thus can prevent defects caused by mixing of different materials, easily control the content of the filler, and particularly increase it, and can manufacture a filler sheet with a layered structure according to required characteristics. In addition, a filler suitable for required characteristics such as dielectric properties, heat dissipation properties, piezoelectric properties, magnetic properties, and surface control can be easily used to form a filler sheet. In addition, since the layered composite filler sheet can be manufactured in one step, such as by a roll-to-roll method, it can provide the effects of process simplification and cost reduction. The layered composite filler sheet can be applied to a circuit board or a high-frequency electronic component.

The effects of the present invention described above are described as examples, and the scope of the present invention is not limited by these effects.

FIGS. 1 and 2 are flow charts illustrating a method for manufacturing a layered composite filler sheet according to one embodiment of the present invention.

FIG. 3 is a schematic diagram illustrating a manufacturing device for a layered composite filler sheet that performs a method for manufacturing a layered composite filler sheet according to one embodiment of the present invention.

FIGS. 4 to 9 are cross-sectional views showing a layered composite filler sheet manufactured by a method for manufacturing a layered composite filler sheet according to one embodiment of the present invention.

Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the attached drawings. The embodiments of the present invention are provided to more completely explain the technical idea of the present invention to those skilled in the art, and the following embodiments may be modified in various different forms, and the scope of the technical idea of the present invention is not limited to the following embodiments. Rather, these embodiments are provided to more faithfully and completely convey the technical idea of the present invention to those skilled in the art. Like reference numerals throughout this specification denote like elements. Furthermore, various elements and areas in the drawings are schematically drawn. Therefore, the technical idea of the present invention is not limited by the relative sizes or intervals drawn in the attached drawings.

In this specification, a layer formed "on" another layer may refer to a layer formed directly on the other layer, or may refer to a layer formed on an intermediate layer or intermediate layers formed on the other layer. It should be noted that the meanings of "upper" and "lower" in this specification are relative, and the direction upward from the substrate is described as "upper", and the direction downward is described as "lower."

According to the technical idea of the present invention, the layered composite filler sheet and its manufacturing method can control the filler input content without limitation and form a defect-free sheet or film. In addition, the layered composite filler sheet can be manufactured into a layered structure according to required characteristics, and for example, a heat-radiating layer, a dielectric layer, and a surface control layer can be formed.

Key terms related to the present invention may include low dielectric, low dielectric loss, 5G communication/next generation 5G communication/6G communication (5G/beyond 5G/6G), polymer-ceramic composites, composite films, composite sheets, ceramic fillers, and roll-to-roll manufacturing devices.

In addition, element technologies related to the present invention may include a one step hybrid casting system, a one step polymer film process, and a multi-function composite sheet/film.

FIGS. 1 and 2 are flow charts illustrating a method for manufacturing a layered composite filler sheet according to one embodiment of the present invention.

Referring to FIG. 1, a method for manufacturing a layered composite filler sheet (S100) includes a step of providing a carrier sheet (S110); a step of providing a first polymer material on the carrier sheet to form a first polymer layer (S120); a step of providing a filler material on the first polymer layer to form a filler layer (S130); a step of providing a second polymer material on the filler layer to form a second polymer layer (S140); and a step of curing the first polymer layer and the second polymer layer (S150).

A layered composite filler sheet having a filler layer interposed between the first polymer layer and the second polymer layer can be manufactured by a method for manufacturing a layered composite filler sheet according to FIG. 1 (S100).

The steps of providing the carrier sheet (S110) to the curing step (S150) may be performed as a continuous process. For example, the roll-to-roll process may be performed from the carrier sheet as a raw material to the layered composite filler sheet as a final product. However, this is exemplary, and the technical idea of the present invention is not limited thereto, and the technical idea of the present invention also includes a case where each of the steps or some of the steps are performed in a batch type.

Referring to FIG. 2, a method for manufacturing a layered composite filler sheet (S200) includes a step of providing a carrier sheet (S210); a step of providing a first polymer material on the carrier sheet to form a first polymer layer (S220); a step of providing a filler material on the first polymer layer to form a filler layer (S230); and a step of curing the first polymer layer (S250).

A layered composite filler sheet having a filler layer formed on the first polymer layer can be manufactured by the method for manufacturing a layered composite filler sheet (S200) according to FIG. 2.

The step of providing the carrier sheet (S210) to the step of curing (S250) may be performed as a continuous process. For example, it may be performed as a roll-to-roll process from the carrier sheet as a raw material to the layered composite filler sheet as a final product. However, this is exemplary, and the technical idea of the present invention is not limited thereto, and the technical idea of the present invention also includes a case where each of the steps or some of the steps are performed in a batch type.

FIG. 3 is a schematic diagram illustrating a manufacturing device for a layered composite filler sheet that performs a method for manufacturing a layered composite filler sheet according to one embodiment of the present invention.

Referring to FIG. 3, a manufacturing device (1000) for a layered composite filler sheet includes a first polymer layer forming unit (20) that forms a first polymer layer by providing a first polymer material on a carrier sheet, a filler layer forming unit (30) that forms a filler layer on the first polymer layer, a second polymer layer forming unit (40) that forms a second polymer layer by providing a second polymer material on the filler layer; and a curing unit (50) that cures at least one of the first polymer layer and the second polymer layer.

Hereinafter, a method for manufacturing the layered composite filler sheet will be described with reference to FIGS. 1 to 3.

The step (S110) of providing the carrier sheet can be performed by providing the carrier sheet (110) to the first polymer layer forming portion (20).

The carrier sheet (110) can perform the function of receiving a first polymer material on its surface. The carrier sheet (110) can include various materials and can be made of, for example, a cured polymer sheet, a ceramic sheet, or a metal sheet.

The step (S120) of forming the first polymer layer may be performed by the first polymer layer forming unit (20), and may be performed by providing a first polymer material on a carrier sheet (110) to form the first polymer layer (120). For example, the step (S120) of forming the first polymer layer may be performed by tape casting the first polymer material on a carrier sheet (110) using a doctor blade or the like to form the first polymer layer (120).

In the step (S120) of forming the first polymer layer, nanosheets may be provided so that the first polymer layer contains nanosheets. The nanosheets may be provided together with the first polymer material, or may be provided separately. Accordingly, a first polymer layer containing nanosheets may be formed.

The step (S130) of forming the filler layer may be performed by a filler layer forming unit (30), and may be performed by providing a filler material on the first polymer layer (120) to form the filler layer (130). For example, the step (S130) of forming the filler layer may be performed by spraying or tape casting the filler material on the first polymer layer (120) to form the filler layer (130).

The step (S130) of forming the filler layer may be composed of a step of forming a plurality of filler layers, and may include, for example, a step of providing a first filler material (31) on a first polymer layer (120) to form a first filler layer (130_1); and a step of providing a second filler material (32) on the first filler layer (130_1) to form a second filler layer (130_2). To this end, the filler layer forming unit (30) may be composed of a first filler layer forming unit (30_1) and a second filler layer forming unit (30_2). The first filler material (31) and the second filler material (32) may include the same material, or may include different materials. In addition, the first filler material (31) and the second filler material (32) may have different diameters.

In addition, the case where the filler layer forming portion (30) is composed of three or more filler layer forming portions and three or more filler layers are formed is also included in the technical idea of the present invention.

Since the filler layer forming section (30) is composed of multiple parts and the filler layer is formed in multiple stages, the height of the filler layer can be easily controlled, and filler layers having fillers with different characteristics can be formed by stacking them.

The step (S140) of forming the second polymer layer may be performed by the second polymer layer forming unit (40), and may be performed by providing a first polymer material on a filler layer (130) to form the second polymer layer (140). For example, the step (S140) of forming the second polymer layer may be performed by spraying or tape casting the second polymer material on a filler layer (130) to form the second polymer layer (140).

The above-mentioned curing step (S150) can be performed by a curing unit (50), and can be performed by curing at least one of the first polymer layer (120) and the second polymer layer (130). For example, the above-mentioned curing step (S150) can be performed by applying thermal energy or light energy to cure at least one of the first polymer layer (120) and the second polymer layer (130). The above-mentioned curing can be performed by cross linking of the polymer material.

Here, the first polymer material, the second polymer material, and the filler material may have a viscosity suitable for spraying or casting, and for this purpose, a binder or a solvent may be included. The solvent may include a water-soluble material, an alcohol-based material, an ether-based material, or an ester-based material, and may be polar or nonpolar.

After the filler layer (130) is formed, the solvent can be evaporated and removed by natural drying or artificial drying by heating to a temperature ranging from 50° C. to 100° C. using a heater or the like, and thus the filler layer (130) can be solidified. The filler layer (130) can be bound to each other by a binder included in the filler layer (130). The binder can include at least one of, for example, polyamic acid, polyimide varnish, polyester, polyurethane, polyolefin, acrylic resin, and silicate resin. However, this is exemplary and the technical idea of the present invention is not limited thereto.

The first polymer layer (120) and the second polymer layer (140) can be solidified to a certain level by natural drying after being formed. In addition, the first polymer layer (120) and the second polymer layer (140) can be further solidified by a curing step.

FIGS. 4 to 9 are cross-sectional views showing a layered composite filler sheet manufactured by a method for manufacturing a layered composite filler sheet according to one embodiment of the present invention.

Referring to FIG. 4, the layered composite filler sheet (100) includes a carrier sheet (110), a first polymer layer (120), a filler layer (130), and a second polymer layer (140).

Referring to FIG. 5, the layered composite filler sheet (200) includes a carrier sheet (110), a first polymer layer (120), a filler layer (130), and a second polymer layer (140).

Referring to FIG. 6, the layered composite filler sheet (300) includes a carrier sheet (110), a first polymer layer (120a) containing nanosheets, a filler layer (130), and a second polymer layer (140).

Referring to FIG. 7, the layered composite filler sheet (400) includes a carrier sheet (110), a first polymer layer (120a) containing nanosheets, and a filler layer (130).

Referring to FIG. 8, the layered composite filler sheet (500) includes a carrier sheet (110), a first polymer layer (120a) containing nanosheets, a filler layer (130), and a second polymer layer (140a) containing nanosheets.

Referring to FIG. 9, the layered composite filler sheet (500) includes a carrier sheet (110), a first polymer layer (120), a filler layer (130), and a second polymer layer (140a) containing nanosheets.

Hereinafter, the components of the layered composite filler sheet illustrated in FIGS. 4 to 9 will be described in detail.

The carrier sheet (110) may have a first polymer layer (120) arranged on its surface. The carrier sheet (110) may include a material to which the first polymer material is attached so that the first polymer layer (120) can be formed and maintained while moving, and may be formed of, for example, a metal sheet, a polymer sheet, a ceramic sheet, glass, or a copper foil. However, this is exemplary and the technical idea of the present invention is not limited thereto. In addition, the carrier sheet (110) may be surface-treated using oxygen or argon gas plasma to control adhesive strength, or a silicon-based material, etc. may be formed on the surface. The carrier sheet (110) may be removed later or may remain to maintain its function.

The first polymer layer (120) can be placed on the carrier sheet (110).

The first polymer layer (120) can form a relatively weak bond, such as an electrostatic bond or a van der Waals bond, with the carrier sheet (110). Accordingly, the first polymer layer (120) can be fixed on the carrier sheet (110).

The first polymer layer (120) may include a polymer material that is curable by heat or light, for example, polyamic acid (PAA), polyimide (PI), modified polyimide (MPI), polytetrafluoro ethylene (PTFE), polyphenylene ether (PPE), polyphenylene oxide (PPO), polyphenylene sulfide (PPS), polystyrene (PS), polyacrylic acid (PA), epoxy, polyvinyl butyral (PVB), polyvinyl pyrrolidone (PVP), ethylene carbonate (EC), polyvinyl alcohol (PVA), polyvinyl chloride (PVC), polyethylene (PE), It may include at least one of polypropylene (PP), and a liquid crystal polymer (LCP). However, this is exemplary and the technical idea of the present invention is not limited thereto.

The filler layer (130) is disposed on the first polymer layer (120) and may include a filler material.

The filler layer (130) may include various materials suitable for desired characteristics as the filler material. That is, desired electrical characteristics and physical characteristics may be controlled by the filler material. For example, the filler material may be controlled to have characteristics such as low dielectric characteristics, low dielectric loss characteristics, high heat dissipation characteristics, and low thermal expansion coefficient.

The filler layer (130) may include, as the filler material, at least one of a dielectric material, a piezoelectric material, a heat-dissipating material, and a magnetic material. The filler layer (130) may include, as the filler material, at least one of a ceramic material, a metal material, and a carbon-based material.

The dielectric material described above is used as an electrical insulator and can be applied to various fields such as electronic devices, communication equipment, and energy storage devices. The dielectric material may include various materials according to characteristics such as dielectric constant, dielectric loss, insulating characteristics, and thermal stability. The dielectric material may include ceramic materials such as, for example, magnesium silicon oxide (Mg ₂ SiO ₄ ), titanium oxide (TiO ₂ ), barium titanium oxide (BaTiO ₃ ), strontium titanium oxide (SrTiO ₃ ), aluminum oxide (Al ₂ O ₃ ), magnesium oxide (MgO), aluminum nitride (AlN), tantalum oxide (Ta ₂ O ₅ ), and cerium oxide (CeO ₂ ). In addition, the dielectric material may include a polymer material, such as, for example, polytetrafluoroethylene (PTFE, Teflon), polyethylene, polypropylene, polyimide, polycarbonate, polyacrylate, and polyurethane. In addition, the dielectric material may include a carbon-based material, such as carbon nanotube composites and graphene.

The piezoelectric material is a material that generates an electric potential when mechanical pressure is applied, and conversely, causes mechanical deformation when an electric potential is applied. The piezoelectric material can be applied to various fields such as sensors, actuators, and electronic devices. The dielectric material can include ceramic materials such as, for example, quartz (SiO ₂ ), PZT (Pb-Zr-Ti oxide), barium titanium oxide (BaTiO ₃ ), zinc oxide (ZnO), potassium niobium oxide (KNbO ₃ ), lithium niobium oxide (LiNbO ₃ ), lithium tantalum oxide (LiTaO ₃ ), sodium niobium oxide (NaNbO ₃ ), gadolinium molybdenum oxide (Gd(MoO ₃ ) ₃ ), gallium nitride (GaN), and aluminum nitride (AlN). In addition, the dielectric material may include a polymer material, such as polyvinylidene fluoride (PVDF), polyvinylidene fluoride-trifluoroethylene (PVDF-TrFE), polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP), and Nylon 11. In addition, the piezoelectric material may include a carbon-based material, such as carbon nanotube composites and graphene oxide.

The above heat-dissipating material is a material that has high heat capacity and thermal conductivity and effectively dissipates heat generated in electronic devices or mechanical devices. The heat-dissipating material may include a metal material such as copper, aluminum, silver, gold, titanium, magnesium, and stainless steel, for example. The heat-dissipating material may include a ceramic material such as aluminum oxide (Al ₂ O ₃ ), aluminum nitride (AlN), beryllium oxide (BeO), boron nitride (BN), and silicon carbide (SiC), for example. In addition, the dielectric material may include a carbon-based material such as graphite, carbon nanotubes, and graphene.

The above magnetic property material is a material that forms a magnetic field or is affected by it, and may include a ferromagnetic material, an antiferromagnetic material, a ferrimagnetic material, a paramagnetic material, or a diamagnetic material.

The above ferromagnetic material is a material that maintains a strong magnetic field even in the absence of an external magnetic field, and may include, for example, iron (Fe), nickel (Ni), cobalt (Co), gadolinium (Gd), neodymium (Nd), markensite, ferrichrome, silicon steel, and alloys thereof.

The above antiferromagnetic material is a material in which the magnetic moments of adjacent atoms are aligned in opposite directions so that the overall magnetism is canceled out, and may include, for example, manganese (Mn), chromium (Cr), nickel oxide (NiO), manganese oxide (MnO), chromium oxide (Cr ₂ O ₃ ), and iron oxide (FeO).

The above ferrimagnet is a material that is magnetic overall due to incomplete cancellation, but in which adjacent atoms are aligned in opposite directions, similar to an antiferromagnet, and may include, for example, magnetite (Fe ₃ O ₄ ), ferrite, and garnet.

The above paramagnetic material is a material that has weak magnetism only when an external magnetic field is present and loses magnetism when the external magnetic field disappears, and may include, for example, aluminum (Al), tungsten (W), platinum (Pt), and magnesium (Mg).

The above diamagnetic material is a material that has a weak opposite magnetism when an external magnetic field is present and loses magnetism when the external magnetic field disappears, and may include, for example, copper (Cu), gold (Au), silver (Ag), lead (Pb), carbon (C), and bismuth (Bi).

The filler layer (130) may include a first filler material (31) and a second filler material (32). The filler layer (130) may be composed of multiple layers including a layer including the first filler material (31) and a layer including the second filler material (32). The first filler material (31) and the second filler material (32) may include the same material or may include different materials. In addition, the first filler material (31) and the second filler material (32) may have different diameters.

The second polymer layer (140) may be disposed on the filler layer (130). The second polymer layer (140) is exemplary and may be omitted.

The second polymer layer (140) may include a polymer material that is curable by heat or light, for example, polyamic acid (PAA), polyimide (PI), modified polyimide (MPI), polytetrafluoro ethylene (PTFE), polyphenylene ether (PPE), polyphenylene oxide (PPO), polyphenylene sulfide (PPS), polystyrene (PS), polyacrylic acid (PA), epoxy, polyvinyl butyral (PVB), polyvinyl pyrrolidone (PVP), ethylene carbonate (EC), polyvinyl alcohol (PVA), polyvinyl chloride (PVC), polyethylene (PE), It may include at least one of polypropylene (PP), and a liquid crystal polymer (LCP). However, this is exemplary and the technical idea of the present invention is not limited thereto.

The first polymer layer (120) and the second polymer layer (140) may contain the same material or may contain different materials.

The first polymer layer (120a) containing nanosheets may contain nanosheets (190) therein. In addition, the second polymer layer (140a) containing nanosheets may contain nanosheets (190) therein. As illustrated, the nanosheets (190) may be contained in both the first polymer layer and the second polymer layer, only in the first polymer layer, or only in the second polymer layer.

The nanosheet (190) may include a heat-radiating material having excellent heat transfer properties. Since the nanosheet (190) releases heat generated from a heat source through a passage with high thermal conductivity when conducted, it may perform the function of facilitating heat release by increasing the contact area using a filler such as a ceramic having a higher thermal conductivity than a polymer.

Nanosheets (190) can create a heat transfer path within the nanosheet-containing first polymer layer (120a) or the nanosheet-containing second polymer layer (140a), thereby facilitating heat dissipation. Accordingly, the heat dissipation characteristics of the nanosheet-containing first polymer layer (120a) or the nanosheet-containing second polymer layer (140a) can be improved.

The nanosheet (190) may be a two-dimensional sheet separated from a layered material such as, for example, kaolinite (Al ₂ Si ₂ O ₅ (OH) ₄ ), mica (KAl ₂ (Si ₃ AlO ₁₀ )(OH) ₂ ), or a ceramic material having high thermal conductivity such as aluminum oxide (Al ₂ O ₃ ), aluminum nitride (AlN), silicon nitride (Si ₃ N ₄ ), and may have a shape of powder, plate, line, fiber, rod, or wire. In addition, the nanosheet (190) may include graphene oxide, graphene nanoplate, graphite and expanded graphite, carbon nanotube, etc. However, this is exemplary and the technical idea of the present invention is not limited thereto.

The layered composite filler sheet according to the present invention has a multilayered structure, so that it has less influence on the interface properties between different materials and can have high flexibility in material selection. The layered composite filler sheet can complement the disadvantages of a mixed structure because the polymer and ceramic materials form separate layers.

Experimental example

Hereinafter, preferred experimental examples are presented to help understand the present invention. However, the following experimental examples are provided only to help understand the present invention, and the present invention is not limited to the following experimental examples.

Considering the possibility that the properties may vary depending on various factors such as the physical properties and thickness of the layered structure of the layered composite filler sheet according to the present invention, the properties were compared with those of the mixed structure.

In the example, a first polymer layer composed of polyimide and a filler layer composed of forsterite (Mg ₂ SiO ₄ ), a ceramic material, were formed. In the comparative example, a mixed layer was formed by mixing polyimide and forsterite. The example and comparative example were completed by drying at 70° C. for 30 minutes. The filler content was varied from 0 vol% to 50 vol%. The dielectric constant and dielectric loss were measured using a SPDR (Split Post Dielectric Resonator).

For reference, the forsterite (Mg2SiO4) is an important silicate mineral belonging to the olivine group, and its dielectric properties play an important role in various applications, especially in ceramic materials, high-temperature insulators, and electronic components. The dielectric constant of the forsterite is generally about 6 to 7, and it has a relatively low dielectric constant and excellent electrical insulation properties. In addition, the forsterite has a very low dielectric loss, which is an important property in high-frequency applications. The low dielectric loss minimizes the loss of electrical energy and enables efficient transmission. The forsterite has a high insulation resistance, which allows it to be used as an electrical insulator in a high-voltage environment. Since the forsterite maintains excellent dielectric properties even at high temperatures, it can be used as a stable insulator in a high-temperature environment. The forsterite is applied in various ways in the field of electronic ceramics, and in particular, due to its low dielectric constant and dielectric loss properties, it can be applied to high-frequency ceramics, electronic devices, and radio frequency components, and in particular, it is used as a high-frequency filter and insulator. In addition, since the forsterite has high temperature stability and insulating properties, it is used as a high-temperature insulator. In addition, the forsterite is used as a substrate material for electronic components, which has advantages in applications requiring high insulation resistance and thermal stability. In addition, since the forsterite has low dielectric loss and stable dielectric constant, it can be used in microwave communication devices and radar systems.

Table 1 is a table showing the characteristics of examples of layered composite filler sheets according to the technical idea of the present invention and comparative examples of mixed structures.

division Filler amount
(volume%) genetic constant
(ε') Genetic loss
(tanδ) Crosscut
attachment Comparative Example 1 0 2.78 0.0024 - Comparative Example 2 10 2.80 0.0018 - Comparative Example 3 20 3.28 0.0029 - Comparative Example 4 30 2.39 0.0021 - Comparative Example 5 40 4.04 0.0035 - Comparative Example 6 50 - - - Example 1 0 2.75 0.0023 5B Example 2 10 2.90 0.0022 4B Example 3 20 2.84 0.0014 4B Example 4 30 2.94 0.0024 4B Example 5 40 3.02 0.0031 2B Example 6 50 3.22 0.0037 2B

Referring to Table 1, the comparative example could not be manufactured when the filler content was 50% by volume, but the example could be manufactured. Both the comparative example and the example showed a tendency for the dielectric constant and dielectric loss to increase as the filler content increased.

Throughout the filler content range, the dielectric constant and dielectric loss of the examples and comparative examples showed almost similar trends. However, while the comparative examples showed a large deviation in the change trends of the dielectric constant and dielectric loss, the examples showed a gradual change trend. Therefore, it can be seen that the examples can predict the dielectric constant and dielectric loss according to the filler content.

The desirable filler content considering both the dielectric constant and the dielectric loss was 10 vol% for the comparative example and 20 vol% for the exemplary embodiment. Therefore, the exemplary embodiment can further increase the filler content.

Additionally, it can be expected that the occurrence of process defects is lower in the example than in the comparative example.

It will be apparent to a person skilled in the art that the technical idea of the present invention described above is not limited to the above-described embodiments and the attached drawings, and that various substitutions, modifications, and changes are possible within a scope that does not depart from the technical idea of the present invention.

Claims (20)

Step of providing a carrier sheet; A step of providing a first polymer material on the carrier sheet to form a first polymer layer; A step of forming a filler layer by providing a filler material on the first polymer layer; A step of providing a second polymer material on the filler layer to form a second polymer layer; and Comprising a step of curing at least one of the first polymer layer and the second polymer layer, A method for manufacturing a layered composite filler sheet. In paragraph 1, The step of forming the first polymer layer is: The first polymer layer is formed by tape casting the first polymer material on the carrier sheet. A method for manufacturing a layered composite filler sheet. In paragraph 1, The step of forming the above filler layer is: The filler layer is formed by spraying or tape casting the filler material on the first polymer layer. A method for manufacturing a layered composite filler sheet. In paragraph 1, The step of forming the above filler layer is: A step of providing a first filler material on the first polymer layer to form a first filler layer; and Comprising a step of providing a second filler material on the first filler layer to form a second filler layer. A method for manufacturing a layered composite filler sheet. In paragraph 4, The first filler material and the second filler material contain the same material or contain different materials. A method for manufacturing a layered composite filler sheet. In paragraph 1, The step of forming the second polymer layer is: The second polymer layer is formed by spraying or tape casting the second polymer material on the filler layer. A method for manufacturing a layered composite filler sheet. In paragraph 1, The above hardening step is, By applying heat energy or light energy to cure at least one of the first polymer layer and the second polymer layer, A method for manufacturing a layered composite filler sheet. In paragraph 1, In the step of forming the first polymer layer, Providing nanosheets so that the first polymer layer contains nanosheets, A method for manufacturing a layered composite filler sheet. In paragraph 1, The step of providing the carrier sheet or the step of curing, carried out as a continuous process, A method for manufacturing a layered composite filler sheet. In paragraph 1, The step of providing the carrier sheet or the step of curing, Performed in a roll-to-roll manner, A method for manufacturing a layered composite filler sheet. Step of providing a carrier sheet; A step of providing a first polymer material on the carrier sheet to form a first polymer layer; A step of forming a filler layer by providing a filler material on the first polymer layer; and Comprising a step of curing the first polymer layer, A method for manufacturing a layered composite filler sheet. a first polymer layer; and Comprising a filler layer disposed on the first polymer layer and including a filler material, Layered composite filler sheets. In Article 12, The first polymer layer is disposed, and further comprises a carrier sheet made of a metal sheet, a polymer sheet, a ceramic sheet, glass, or a copper foil. Layered composite filler sheets. In Article 12, The above first polymer layer, Comprising at least one of polyamic acid, polyimide, modified polyimide, polytetrafluoroethylene, polyphenyl ether, polyphenyl oxide, polyphenyl sulfide, polystyrene, polyacrylic acid, epoxy, polyvinyl butyral, polyvinyl pyrrolidone, ethylene carbonate, polyvinyl alcohol, polyvinyl chloride, polyethylene, polypropylene, and liquid crystal polymer. Layered composite filler sheets. In Article 12, The above filler layer, Comprising at least one of a dielectric material, a piezoelectric material, a heat-dissipating material, and a magnetic material, Layered composite filler sheets. In Article 12, The above filler layer, Comprising at least one of a ceramic material, a metallic material, and a carbon-based material, Layered composite filler sheets. In Article 12, The above filler layer, a first filler layer comprising a first filler material; and A second filler layer comprising a second filler material and disposed on the first filler layer, Layered composite filler sheets. In Article 12, Further comprising a second polymer layer disposed on the filler layer, Layered composite filler sheets. In Article 18, The second polymer layer is, Comprising at least one of polyamic acid, polyimide, modified polyimide, polytetrafluoroethylene, polyphenyl ether, polyphenyl oxide, polyphenyl sulfide, polystyrene, polyacrylic acid, epoxy, polyvinyl butyral, polyvinyl pyrrolidone, ethylene carbonate, polyvinyl alcohol, polyvinyl chloride, polyethylene, polypropylene, and liquid crystal polymer. Layered composite filler sheets. In Article 12, The above first polymer layer, Containing nano sheets, Layered composite filler sheets.

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