A dielectric composite material and a preparation method and application thereof

By employing 3D printing technology with alternating layers of barium titanate and boron nitride, combined with resin composition and organosilicon compound treatment, the problems of dielectric constant and breakdown strength of dielectric ceramic composite materials were solved, achieving high energy storage density and molding stability.

CN119798919BActive Publication Date: 2026-04-17FUJIAN INST OF RES ON THE STRUCTURE OF MATTER CHINESE ACAD OF SCI
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
FUJIAN INST OF RES ON THE STRUCTURE OF MATTER CHINESE ACAD OF SCI
Filing Date
2024-12-30
Publication Date
2026-04-17

AI Technical Summary

Technical Problem

While existing technologies can improve the dielectric constant of dielectric ceramic composites, the material properties deteriorate, especially the breakdown strength and energy storage density are limited, and there is also the problem of stress cracking after molding.

Method used

Alternating layers of barium titanate and boron nitride are used, with the barium titanate layer having a three-dimensional network structure. A resin composition is filled in and a ceramic skeleton is formed by 3D printing and sintering. Combined with surface treatment with organosilicon compounds, the interface continuity is improved.

Benefits of technology

It improves the dielectric constant and breakdown strength, enhances the energy storage density of the material, avoids stress cracking after molding, and simplifies the manufacturing process.

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Abstract

This invention relates to the field of energy storage dielectric materials technology, specifically to a dielectric composite material and its preparation method and application. It comprises alternating layers of barium titanate and boron nitride, wherein the barium titanate layers have a three-dimensional network structure, and the three-dimensional network structure is filled with a resin composition. The barium titanate and boron nitride layers are fixedly connected. This application utilizes photopolymerization 3D printing technology to simultaneously prepare a three-dimensional continuous dielectric ceramic that improves the dielectric constant and a boron nitride layer that enhances the dielectric strength, greatly improving the energy storage density of the composite material. Through hyperbranched polysiloxane modification of the skeleton surface and the introduction of a small amount of barium titanate into the resin matrix, defects caused by the large difference in thermal expansion coefficients between the skeleton and the resin matrix are improved from the interface structure and matrix perspectives.
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Description

Technical Field

[0001] This invention relates to the field of energy storage dielectric materials technology, specifically to a dielectric composite material, its preparation method, and its application. Background Technology

[0002] In the field of dielectric materials science, dielectric ceramics, with their superior high dielectric constant, have become a focus of research and application. These materials show great potential in enhancing the energy storage performance of polymer-based composites, particularly in capacitors, energy storage devices, and high-frequency electronic devices. The preparation process of dielectric ceramic-polymer composites typically involves uniformly dispersing fine dielectric ceramic powder within a polymer matrix. The aim is to effectively increase the overall dielectric constant of the composite material by introducing ceramic particles, thereby enhancing energy storage density. However, a key technical challenge lies in ensuring a high dielectric constant while avoiding the resulting degradation of material properties. To achieve even higher dielectric constants, a large amount of ceramic powder is often added to the polymer. The introduction of a large number of ceramic particles not only increases the processing difficulty but also easily leads to particle agglomeration and the formation of internal pores. This significantly weakens the material's breakdown strength—its ability to withstand the maximum electric field strength without being destroyed. The reduction in breakdown strength directly limits further increases in the energy storage density of composite materials.

[0003] Chinese invention patent CN105541389B uses polyurethane foam as a carrier to prepare ceramic / polymer composites by constructing a three-dimensional dielectric ceramic network. This not only solves the problem of poor molding process caused by high ceramic content, but also achieves high dielectric constants with lower ceramic content. However, the structure of this three-dimensional ceramic network depends on the carrier foam of the ceramic particles, making it difficult to prepare composites with high ceramic content, thus limiting the improvement in dielectric constant of the composite material. Furthermore, due to the difference in thermal expansion coefficients between the ceramic skeleton and the polymer (approximately 500 times different), stress cracking easily occurs after molding, forming defects that significantly reduce the dielectric strength of the final composite material. Summary of the Invention

[0004] The first aspect of the present invention provides a dielectric composite material comprising alternating layers of barium titanate and boron nitride, wherein the barium titanate layers have a three-dimensional network structure, the three-dimensional network structure is filled with a resin composition, and the barium titanate layers and boron nitride layers are fixedly connected.

[0005] The number of barium titanate layer and boron nitride layer is 2-10.

[0006] Preferably, the number of barium titanate layer and boron nitride layer is 2-5.

[0007] The resin composition comprises epoxy resin, barium titanate, and epoxy curing agent.

[0008] The amount of barium titanate added to the resin composition is 2-10 wt%.

[0009] Preferably, the amount of barium titanate added to the resin composition is 3-8 wt%.

[0010] Preferably, the epoxy resin comprises bisphenol A type epoxy resin.

[0011] This application research found that by 3D printing alternating layers of barium titanate and boron nitride, wherein the barium titanate layers form a three-dimensional network structure and are filled with a resin composition, the dielectric constant can be improved, and its breakdown strength can be enhanced. Further research revealed that the resin composition comprises epoxy resin, barium titanate, and an epoxy curing agent, and is further enhanced by surface treatment of the ceramic skeleton using an organosilicon compound. This improves the interfacial continuity of the dielectric composite material and avoids the formation of defects. It is possible that the specific barium titanate and surface treatment address internal defects caused by the difference in thermal expansion coefficients between the skeleton and the resin matrix, thereby preventing stress cracking and subsequent defect formation after molding.

[0012] The epoxy curing agent includes amine curing agents, including diethylenetriamine, ethylenediamine, triethylenetetramine, 1,6-hexanediamine, tetraethylenepentamine, 4-amino-α,α-4-trimethylcyclohexanemethylamine, 5-amino-1,3,3-trimethylcyclohexanemethylamine, bis(4-amino-3-methylcyclohexyl)methane, bis(4-aminocyclohexyl)methane, 3,3'-dimethyl-4,4-diaminodicyclohexylmethane, 4,4'-diaminodicyclohexylmethane, 4,4'-methylenebis( At least one of 2-methyl-6-ethylaniline, m-phenylenediamine, m-phenylenediamine, 4,4-diaminodiphenyl sulfone, 4,4-diaminodiphenylmethane, diethyltoluenediamine, dimethylthiotoluenediamine, 3-chloro-3'-ethyl-4,4'-diaminodiphenylmethane, 4,4'-methylenebis(2,6-diethylaniline), 4,4'-methylenebis(2-ethyl)aniline, 4,4'-bis-sec-butylaminodiphenylmethane, and 4,4'-methylenebis(3-chloro-2,6-diethylaniline).

[0013] The raw materials for preparing the barium titanate layer include micron-sized barium titanate and nano-sized barium titanate, and the weight ratio of micron-sized barium titanate to nano-sized barium titanate is 1:(1.5-6).

[0014] Preferably, the weight ratio of the micron-sized barium titanate to the nano-sized barium titanate is 1:(1.5-4).

[0015] More preferably, the weight ratio of the micron-sized barium titanate to the nano-sized barium titanate is 1:(1.5-2).

[0016] Preferably, the particle size of the barium titanate is not higher than 10 μm.

[0017] More preferably, the particle size of the barium titanate is no higher than 5 μm.

[0018] Preferably, the particle size of the nano-barium titanate is not higher than 500 nm.

[0019] Further preferably, the particle size of the nano-barium titanate is not higher than 200 nm.

[0020] The raw materials for preparing the boron nitride layer include boron nitride with a particle size of no more than 500 nm.

[0021] Preferably, the raw materials for preparing the boron nitride layer include boron nitride with a particle size of no more than 300 nm.

[0022] Preferably, the raw materials for preparing the barium titanate layer and the boron nitride layer also include a photosensitive resin mixture and an organosilicon compound.

[0023] A second aspect of the present invention provides a method for preparing a dielectric composite material, comprising the following steps:

[0024] Barium titanate of micron size and barium titanate of nano size are mixed with a photosensitive resin mixture to obtain barium titanate slurry; boron nitride is mixed with a photosensitive resin mixture to obtain boron nitride slurry.

[0025] 3D printing was performed using barium titanate slurry and boron nitride slurry to obtain alternating layers of barium titanate green body and boron nitride green body;

[0026] Alternating layers of barium titanate green body and boron nitride green body are sintered to obtain a ceramic framework;

[0027] Silane-modified ceramic frameworks are obtained by surface treatment of ceramic frameworks with organosilicon compounds.

[0028] A dielectric composite material is obtained by mixing a silane-modified ceramic framework with components of a resin composition and then curing it.

[0029] The amount of barium titanate added in the barium titanate slurry is 50-80 wt%.

[0030] Preferably, the amount of barium titanate added to the barium titanate slurry is 60-80 wt%.

[0031] The amount of boron nitride added in the boron nitride slurry is 30-60 wt%.

[0032] Preferably, the amount of boron nitride added to the boron nitride slurry is 40-50 wt%.

[0033] The organosilicon compounds include silane coupling agents.

[0034] Preferably, the silane coupling agent includes at least one of the following grades: KH-550, KH-551, KH-560, KH-570, A-151, and A-171.

[0035] The photosensitive resin mixture includes: photosensitive resin, initiator, and additives.

[0036] The photosensitive resin includes bifunctional acrylates, hydroxy acrylate monomers, trifunctional acrylates, and phosphate acrylates.

[0037] The phosphate acrylate includes phosphate methacrylate, hydroxyethyl phosphate methacrylate, and 2-methyl-2-hydroxyethyl acrylate phosphate ester.

[0038] The hydroxyacrylate monomer includes at least one of ethoxylated trimethylolpropane triacrylate, trimethylolpropane triacrylate, hydroxypropyl acrylate, and hydroxybutyl acrylate.

[0039] The bifunctional acrylates include at least one of 1,6-hexanediol diacrylate, triethylene glycol dimethacrylate, and tripropylene glycol diacrylate.

[0040] The trifunctional acrylates include SR9051 NS (Sartoma).

[0041] The additives include leveling agents and thickeners.

[0042] Preferably, the leveling agent includes BYK307; the thickener includes SA-6000.

[0043] The initiator includes one or more of the following: benzoin dimethyl ether, benzophenone, 1-hydroxycyclohexylphenyl ketone (abbreviated as: 184 photoinitiator), 2-hydroxy-2-methyl-1-phenyl-1-propanone (abbreviated as: 1173 photoinitiator), 2-methyl-1-(4-methylthio)phenyl-2-morpholinopropyl-1-one (IRGACURE 907), 2,4,6-trimethylbenzoyl-diphenylphosphine oxide (abbreviated as: TPO photoinitiator), 2,4,6-trimethylbenzoylphosphonate ethyl phenyl (abbreviated as: TPO-L photoinitiator), and bis(2,4,6-trimethylbenzoyl)phosphine oxide (IRGACURE 819).

[0044] The sintering temperature is 1100-1400℃, and the sintering time is 2-5h.

[0045] Preferably, the sintering temperature is 1250-1350℃ and the sintering time is 2-4h.

[0046] The surface treatment steps include: reacting the ceramic skeleton with hydrogen peroxide, impregnating it with an organic solvent, and then modifying it with a silane coupling agent.

[0047] The third aspect of this invention provides an application of a method for preparing dielectric composite materials, which is used in the preparation of capacitors.

[0048] Beneficial effects

[0049] 1. By 3D printing alternating layers of barium titanate and boron nitride, wherein the barium titanate layer is a three-dimensional network structure and the three-dimensional network structure is filled with a resin composition, the dielectric constant can be improved and its breakdown strength can be enhanced.

[0050] 2. The resin composition comprises epoxy resin, barium titanate, and epoxy curing agent, and is further surface-treated with an organosilicon compound. This improves the interfacial continuity of the dielectric composite material and prevents defects from forming.

[0051] 3. The raw materials for preparing the barium titanate layer include micron-sized barium titanate and nano-sized barium titanate, and the weight ratio of micron-sized barium titanate to nano-sized barium titanate is 1:(1.5-6), which can further improve the energy storage density of the dielectric composite material.

[0052] 4. The weight ratio of micron-sized barium titanate to nano-sized barium titanate is 1:(1.2-4), and the energy storage density can exceed 12 J / cm³. 3 This meets the requirements for capacitor usage.

[0053] 5. The preparation process of this application is simple and the raw materials are readily available. Attached Figure Description

[0054] Figure 1 The dielectric composite material was prepared as in Example 1.

[0055] Figure 2 The dielectric composite material was prepared in Example 2.

[0056] Figure 3 A dielectric composite material was prepared for Comparative Example 1.

[0057] Figure 4 The image shows an electron microscope (EM) image of the interface (interlayer bonding) of the dielectric composite material prepared in Example 1.

[0058] Figure 5 The image shows an electron microscope (EM) image of the interface (interlayer bonding) of the dielectric composite material prepared for Comparative Example 1. Detailed Implementation

[0059] Example 1

[0060] A dielectric composite material, such as Figure 1 As shown, there are alternating layers of barium titanate and boron nitride (5-layer structure, from top to bottom: boron nitride layer-barium titanate layer-boron nitride layer-barium titanate layer-boron nitride layer). The barium titanate layer has a three-dimensional network structure, which is filled with a resin composition. The barium titanate layer and the boron nitride layer are fixedly connected by sintering.

[0061] A method for preparing a dielectric composite material comprises the following steps:

[0062] 35g of 1μm barium titanate (Shanghai Aladdin Biochemical Technology Co., Ltd.) and 105g of 100nm barium titanate (Shanghai Maclean Biochemical Technology Co., Ltd.) were added to 60g of photosensitive resin mixture and ball-milled for 2 hours to obtain barium titanate slurry; 45g of boron nitride (200nm, Shanghai Maclean Biochemical Technology Co., Ltd.) were added to 55g of photosensitive resin mixture and ball-milled for 1 hour to obtain boron nitride slurry.

[0063] 3D printing was performed using barium titanate slurry and boron nitride slurry (commercial DLP 3D printer), with a layer thickness of 20 μm and a single-layer exposure time of 10 s, to obtain alternating layers of barium titanate green body and boron nitride green body.

[0064] Alternating layers of barium titanate green and boron nitride green were sintered (muffle furnace, heated to 1300℃ at a rate of 1℃ / min and held for 3 hours) to obtain a ceramic skeleton.

[0065] The ceramic framework was immersed in a 30 wt% hydrogen peroxide solution and refluxed at 80 °C for 3 h. After the reaction, it was washed with deionized water and then immersed in n-propanol. 0.2 mol of KH560 and 0.26 mol of deionized water were added, and the mixture was stirred at 60 °C for 1 h. The pH of the mixture was then adjusted to 10 with a 1 wt% NaOH solution in n-propanol, and the reaction was continued at this temperature for 6 h. After thorough washing with ethanol and drying, the hyperbranched polysiloxane-modified ceramic framework was obtained.

[0066] The hyperbranched polysiloxane-modified ceramic skeleton was mixed with components of a resin composition (5 wt% barium titanate, 10 wt% triethylenetetramine, and 85 wt% epoxy resin NPEL-128 (Nan Ya Epoxy Resin Kunshan Co., Ltd.)) and repeatedly degassed in a vacuum oven until no bubbles were generated. Finally, it was cured at room temperature for 24 hours and then transferred to a 100°C forced-air drying oven for 4 hours to obtain the dielectric composite material.

[0067] Preparation of the photosensitive resin mixture: Under light-protected conditions, 1,6-ethylene glycol diacrylate, trimethylolpropane triacrylate, trifunctional ester SR9051 NS (Sartoma, Shengkai Enterprise Co., Ltd.), 2-methyl-2-acrylate hydroxyethyl phosphate, BYK307, SA-6000, and phenyl bis(2,4,6-trimethylbenzoyl)phosphine oxide were mixed in a ratio of 63wt%:21.2wt%:6.5wt%:2wt%:3wt%:2.5wt%:1.8wt%.

[0068] Example 2

[0069] A dielectric composite material, such as Figure 2 As shown, there are alternating layers of barium titanate and boron nitride (7-layer structure, from top to bottom: barium titanate layer-boron nitride layer-barium titanate layer-boron nitride layer-barium titanate layer-boron nitride layer-barium titanate layer-barium titanate layer). The barium titanate layer has a three-dimensional network structure, which is filled with a resin composition. The barium titanate layer and the boron nitride layer are fixedly connected by sintering.

[0070] A method for preparing a dielectric composite material comprises the following steps:

[0071] 50g of 1μm barium titanate (Shanghai Aladdin Biochemical Technology Co., Ltd.) and 90g of 100nm barium titanate (Shanghai Maclean Biochemical Technology Co., Ltd.) were added to 60g of photosensitive resin mixture and ball-milled for 2 hours to obtain barium titanate slurry; 45g of boron nitride (200nm, Shanghai Maclean Biochemical Technology Co., Ltd.) were added to 55g of photosensitive resin mixture and ball-milled for 1 hour to obtain boron nitride slurry.

[0072] 3D printing was performed using barium titanate slurry and boron nitride slurry (commercial DLP 3D printer), with a layer thickness of 20 μm and a single-layer exposure time of 10 s, to obtain alternating layers of barium titanate green body and boron nitride green body.

[0073] Alternating layers of barium titanate green and boron nitride green were sintered (muffle furnace, heated to 1300℃ at a rate of 1℃ / min and held for 3 hours) to obtain a ceramic skeleton.

[0074] The ceramic framework was immersed in a 30 wt% hydrogen peroxide solution and refluxed at 80 °C for 3 h. After the reaction, it was washed with deionized water and then immersed in n-propanol. 0.2 mol of KH560 and 0.26 mol of deionized water were added, and the mixture was stirred at 60 °C for 1 h. The pH of the mixture was then adjusted to 10 with a 1 wt% NaOH solution in n-propanol, and the reaction was continued at this temperature for 6 h. After thorough washing with ethanol and drying, the hyperbranched polysiloxane-modified ceramic framework was obtained.

[0075] The hyperbranched polysiloxane-modified ceramic skeleton was mixed with components of a resin composition (5 wt% barium titanate, 10 wt% triethylenetetramine, and 85 wt% epoxy resin NPEL-128 (Nan Ya Epoxy Resin Kunshan Co., Ltd.)) and repeatedly degassed in a vacuum oven until no bubbles were generated. Finally, it was cured at room temperature for 24 hours and then transferred to a 100°C forced-air drying oven for 4 hours to obtain the dielectric composite material.

[0076] Preparation of the photosensitive resin mixture: Under light-protected conditions, 1,6-ethylene glycol diacrylate, trimethylolpropane triacrylate, trifunctional ester SR9051 NS (Sartoma, Shengkai Enterprise Co., Ltd.), 2-methyl-2-acrylate hydroxyethyl phosphate, BYK307, SA-6000, and phenyl bis(2,4,6-trimethylbenzoyl)phosphine oxide were mixed in a ratio of 63wt%:21.2wt%:6.5wt%:2wt%:3wt%:2.5wt%:1.8wt%.

[0077] Comparative Example 1

[0078] A dielectric composite material, such as Figure 3 As shown, it is formed by sintering stacked barium titanate layers (4-layer structure), wherein the barium titanate layers have a three-dimensional network structure and the three-dimensional network structure is filled with a resin composition.

[0079] A method for preparing a dielectric composite material comprises the following steps:

[0080] 50g of 1μm barium titanate (Shanghai Aladdin Biochemical Technology Co., Ltd.) and 90g of 100nm barium titanate (Shanghai McLean Biochemical Technology Co., Ltd.) were added to 60g of photosensitive resin mixture, and the mixture was ball-milled for 2 hours to obtain barium titanate slurry.

[0081] 3D printing was performed using barium titanate slurry (commercial DLP 3D printer), with a layer thickness of 20μm and a single-layer exposure time of 10s, to obtain stacked barium titanate green layers.

[0082] The stacked barium titanate green layers were sintered (in a muffle furnace, the temperature was increased to 1300℃ at a rate of 1℃ / min and held for 3 hours) to obtain a ceramic skeleton.

[0083] The ceramic framework was immersed in a 30 wt% hydrogen peroxide solution and refluxed at 80 °C for 3 h. After the reaction, it was washed with deionized water and then immersed in n-propanol. 0.2 mol of KH560 and 0.26 mol of deionized water were added, and the mixture was stirred at 60 °C for 1 h. The pH of the mixture was then adjusted to 10 with a 1 wt% NaOH solution in n-propanol, and the reaction was continued at this temperature for 6 h. After thorough washing with ethanol and drying, the hyperbranched polysiloxane-modified ceramic framework was obtained.

[0084] The hyperbranched polysiloxane-modified ceramic skeleton was mixed with components of a resin composition (5 wt% barium titanate, 10 wt% triethylenetetramine, and 85 wt% epoxy resin NPEL-128 (Nan Ya Epoxy Resin Kunshan Co., Ltd.)) and repeatedly degassed in a vacuum oven until no bubbles were generated. Finally, it was cured at room temperature for 24 hours and then transferred to a 100°C forced-air drying oven for 4 hours to obtain the dielectric composite material.

[0085] Preparation of the photosensitive resin mixture: Under light-protected conditions, 1,6-ethylene glycol diacrylate, trimethylolpropane triacrylate, trifunctional ester SR9051 NS (Sartoma, Shengkai Enterprise Co., Ltd.), 2-methyl-2-acrylate hydroxyethyl phosphate, BYK307, SA-6000, and phenyl bis(2,4,6-trimethylbenzoyl)phosphine oxide were mixed in a ratio of 63wt%:21.2wt%:6.5wt%:2wt%:3wt%:2.5wt%:1.8wt%.

[0086] Comparative Example 2

[0087] A dielectric composite material is formed by sintering stacked barium titanate layers (4-layer structure), wherein the barium titanate layers have a three-dimensional network structure and the three-dimensional network structure is filled with a resin composition.

[0088] A method for preparing a dielectric composite material comprises the following steps:

[0089] 50g of 1μm barium titanate (Shanghai Aladdin Biochemical Technology Co., Ltd.) and 90g of 100nm barium titanate (Shanghai McLean Biochemical Technology Co., Ltd.) were added to 60g of photosensitive resin mixture, and the mixture was ball-milled for 2 hours to obtain barium titanate slurry.

[0090] 3D printing was performed using barium titanate slurry (commercial DLP 3D printer), with a layer thickness of 20μm and a single-layer exposure time of 10s, to obtain stacked barium titanate green layers.

[0091] The stacked barium titanate green layers were sintered (in a muffle furnace, the temperature was increased to 1300℃ at a rate of 1℃ / min and held for 3 hours) to obtain a ceramic skeleton.

[0092] The ceramic skeleton was mixed with components of a resin composition (5 wt% barium titanate, 10 wt% triethylenetetramine, and 85 wt% epoxy resin NPEL-128 (Nan Ya Epoxy Resin Kunshan Co., Ltd.)) and degassed repeatedly in a vacuum oven until no bubbles were generated. Finally, it was cured at room temperature for 24 hours and then transferred to a 100°C forced-air drying oven for 4 hours to obtain the dielectric composite material.

[0093] Preparation of the photosensitive resin mixture: Under light-protected conditions, 1,6-ethylene glycol diacrylate, trimethylolpropane triacrylate, trifunctional ester SR9051 NS (Sartoma, Shengkai Enterprise Co., Ltd.), 2-methyl-2-acrylate hydroxyethyl phosphate, BYK307, SA-6000, and phenyl bis(2,4,6-trimethylbenzoyl)phosphine oxide were mixed in a ratio of 63wt%:21.2wt%:6.5wt%:2wt%:3wt%:2.5wt%:1.8wt%.

[0094] Performance testing methods

[0095] The energy storage density of the dielectric composite materials prepared in the examples and comparative examples was tested, and the test data are listed in Table 1.

[0096] The energy storage density is calculated by testing the hysteresis loop of the material according to GB / T 6426-1999 (Quasi-static test method for hysteresis loop of ferroelectric ceramic materials).

[0097] Electron microscopy was performed on the interface of the dielectric composite materials prepared in Example 1 and Comparative Example 1. Figure 4 As shown, the interface integration is good, and Figure 5 Cracks appeared at the interface.

[0098] Performance test data

[0099] Table 1

[0100] sample <![CDATA[Energy storage density (J / cm 3 )]]> Example 1 12.21 Example 2 16.85 Comparative Example 1 2.42 Comparative Example 2 2.16

Claims

1. A dielectric composite material, characterized by, It includes alternating layers of barium titanate and boron nitride, wherein the barium titanate layer has a three-dimensional network structure, the three-dimensional network structure is filled with a resin composition, and the barium titanate layer and boron nitride layer are fixedly connected by sintering; The number of barium titanate layer and boron nitride layer is 2-10; The raw materials for preparing the barium titanate layer include micron-sized barium titanate, nano-sized barium titanate, organosilicon compounds and photosensitive resin mixtures, wherein the weight ratio of micron-sized barium titanate to nano-sized barium titanate is 1:(1.5-6). The raw materials for preparing the boron nitride layer include a mixture of boron nitride with a particle size not exceeding 500 nm, organosilicon compounds, and photosensitive resin. The alternating layers of barium titanate and boron nitride are surface-treated with an organosilicon compound.

2. The dielectric composite of claim 1, wherein, The resin composition comprises epoxy resin, barium titanate, and epoxy curing agent.

3. The dielectric composite material according to claim 2, characterized in that, The amount of barium titanate added to the resin composition is 2-10 wt%.

4. A method for preparing the dielectric composite material according to claim 3, characterized in that, Includes the following steps: Barium titanate of micron size and barium titanate of nano size are mixed with a photosensitive resin mixture to obtain barium titanate slurry; boron nitride is mixed with a photosensitive resin mixture to obtain boron nitride slurry. 3D printing was performed using barium titanate slurry and boron nitride slurry to obtain alternating layers of barium titanate green body and boron nitride green body; Alternating layers of barium titanate green body and boron nitride green body are sintered to obtain a ceramic framework; Silane-modified ceramic frameworks are obtained by surface treatment of ceramic frameworks with organosilicon compounds. A dielectric composite material is obtained by mixing a silane-modified ceramic framework with components of a resin composition and then curing it.

5. The method for preparing the dielectric composite material according to claim 4, characterized in that, The organosilicon compounds include silane coupling agents.

6. The method for preparing the dielectric composite material according to claim 5, characterized in that, The surface treatment steps include: reacting the ceramic skeleton with hydrogen peroxide, impregnating it with an organic solvent, and then modifying it with a silane coupling agent.

7. An application of a method for preparing a dielectric composite material according to any one of claims 4-6, characterized in that, It is used in the manufacture of capacitors.

Citation Information

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