CN114437503A - Epoxy resin composition suitable for halogen-free copper clad plate material and preparation method thereof - Google Patents
Epoxy resin composition suitable for halogen-free copper clad plate material and preparation method thereof Download PDFInfo
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Abstract
The invention provides an epoxy resin composition suitable for a halogen-free copper clad plate material, which is characterized by comprising the following components in percentage by weight: 10 to 40 percent of phosphorus-containing epoxy resin; 15% -45% of isocyanic acid modified epoxy resin; 1% -8% of benzoxazine resin; 2 to 12 percent of phosphorus-containing curing agent; dicyandiamide 0.5% -3%; 1% -10% of bisphenol A type phenolic resin; 1 to 10 percent of flame retardant; 0.05 to 1.00 percent of epoxy resin curing accelerator; 10% -40% of a first inorganic filler; 5-20% of second inorganic filler. The invention also discloses a preparation method of the composition. Compared with the comparative example, the copper clad laminate prepared by the invention has the characteristics of common glass transition temperature (Tg ≧ 138 ℃), excellent heat resistance, good peeling strength and the like, and is completely suitable for being applied to halogen-free and environment-friendly lead-free processes in the PCB industry and the manufacturing and processing of multilayer boards.
Description
Technical Field
The invention belongs to the technical field of new materials, and particularly relates to an epoxy resin composition suitable for a halogen-free copper clad plate material and a preparation method thereof.
Background
With the increasing environmental requirements of people and the gradual improvement of relevant laws and regulations, more environment-friendly products are needed to meet the requirements. At present, main FR-4 products in the copper-clad plate market often contain halogen elements harmful to organisms in order to achieve the product characteristics of relevant flame retardance and the like. Despite the excellent flame retardancy of bromine-containing halides, toxic chlorine is generated during combustion thereof.
Since halogen-containing substances can generate carcinogenic dioxins, the use of the molding device is extremely strictly controlled. Therefore, the industry demands the use of non-halogen flame retardant molded circuit substrates for flame retardancy, i.e., the use of halogen-free flame retardant printed circuit substrates and the use of such molded circuit substrates in the processes of detecting PCB processing, appliance fires, disposal (including recycling, burial, incineration), etc., and the molding
At present, non-halogen flame retardants blended in common epoxy resins, such as compositions containing nitrogen compounds, phosphorus compounds, inorganic substances, etc., have been developed in the industry. However, these flame retardant materials have disadvantages that the material is relatively hygroscopic, the material is likely to explode at high temperature, and the brittleness is large.
Disclosure of Invention
In view of the above problems, the present invention aims to provide an epoxy resin composition suitable for a halogen-free copper clad laminate material and an application thereof. The copper-clad plate material prepared from the epoxy resin composition has good heat resistance and good toughness (good peeling strength), and can be suitable for halogen-free and environment-friendly lead-free manufacturing processes and processing and manufacturing of multilayer plates.
In order to realize the purpose of the invention, the adopted technical scheme is as follows:
the epoxy resin composition suitable for the halogen-free copper clad plate material comprises the following components in percentage by weight:
in a preferred embodiment of the present invention, the epoxy resin composition is mixed with an organic solvent. The organic solvent is preferably any one or more of methyl ethyl ketone, toluene, xylene, methyl isobutyl ketone, propylene glycol methyl ether or cyclohexanone.
The amount of the organic solvent used is not particularly limited, but from the viewpoint of ease of impregnating the epoxy resin binder into the matrix in the case of producing the prepreg and good adhesion between the resin composition and the matrix, the organic solvent is preferably added so that the solid content of the dope is 55% or more, particularly preferably 55 to 75%.
In a preferred embodiment of the present invention, the epoxy resin composition comprises 60 to 75% by weight, and the balance is organic solvent.
In a preferred embodiment of the present invention, the physical property requirement of the phosphorus-containing epoxy resin is that the epoxy equivalent EEW (g/eq) is 290-340;
hydrolysable chlorine (dipropylene glycol methyl ether) 400 MAX;
the solid content (wt%) is 68-72;
the phosphorus content (wt%) is 3.0-3.5.
In a preferred embodiment of the present invention, the phosphorous epoxy resin is represented by the following formula 1, wherein n is 4-12:
the phosphorus-containing epoxy resin provides phosphorus-free materials needed for flame retardancy.
In a preferred embodiment of the present invention, the physical properties of the isocyanate-modified epoxy resin are required to be as follows:
the epoxy equivalent EEW (g/eq) is 260-320;
hydrolysable chlorine (dipropylene glycol methyl ether) 300 MAX;
the solid content (wt%) is 73-77.
In a preferred embodiment of the present invention, the isocyanate-modified epoxy resin is any one or more of aromatic diphenylmethane diisocyanate (MDI) modified epoxy resin or Toluene Diisocyanate (TDI) modified epoxy resin.
The purpose is to impart the essential mechanical and thermal properties required for the cured resin and laminates made therewith, as well as good toughness and excellent copper peel strength.
In a preferred embodiment of the present invention, the benzoxazine resin is a bisphenol a type benzoxazine resin. LZ8290 resin, produced by hensmei, usa, is preferred.
In a preferred embodiment of the present invention, the physical properties of the phosphorus-containing curing agent are as follows:
hydroxyl equivalent (g/eq) is 330-560;
hydrolysable chlorine (dipropylene glycol methyl ether) 300 MAX;
the phosphorus content (wt%) is 8-10;
the solid content (wt%) is 54-60.
In a preferred embodiment of the present invention, the phosphorus-containing curing agent is prepared by reacting a phosphorus-containing compound with a bisphenol A type epoxy resin. A Dow chemical-produced resin, trade name XZ-92741, is preferred.
In a preferred embodiment of the present invention, the bisphenol A type phenolic resin is preferably SH-2120 resin of Shandong Shengquan chemical industry.
In a preferred embodiment of the invention, the flame retardant parameters are as follows:
phosphorus content (wt%): 25-33;
average particle diameter (μm): 0.9-1.5;
the water content (percent) is less than or equal to 0.2;
density @25 ℃ (g/cm 3): 1.9.
in a preferred embodiment of the present invention, the epoxy resin curing accelerator is any one or more of 2-ethyl-4-methylimidazole or 1-benzyl-2-methylimidazole. 2-ethyl-4-methylimidazole is preferred.
In a preferred embodiment of the present invention, the inorganic filler is any one or more of talc, quartz powder, ceramic powder, aluminum hydroxide, metal oxide particles such as silica, clay, boron nitride.
The chemical and electrical properties of the cured resin can be improved, such as lowering the Coefficient of Thermal Expansion (CTE), increasing the modulus, increasing heat transfer, and assisting in flame retardancy. Preferably silica or aluminium hydroxide.
A preparation method of an epoxy resin composition suitable for a halogen-free copper clad plate material comprises the following steps:
1) adding part of organic solvent, dicyandiamide and a fire retardant into a stirring tank, starting a stirrer, continuously stirring for 2-3 hours at the rotation speed of 500-;
then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90-120 minutes after the addition is finished;
2) sequentially adding the phosphorus-containing epoxy resin, the isocyanic acid modified epoxy resin, the benzoxazine resin, the phosphorus-containing curing agent and the bisphenol A type phenolic resin into a stirring tank, stirring at the rotation speed of 800-;
3) and adding the epoxy resin curing accelerator into the rest organic solvent, adding the solution into a stirring tank after the epoxy resin curing accelerator is completely dissolved, and continuously stirring for 5-12 hours at 1000-1500 rpm to obtain the epoxy resin composition.
The invention has the beneficial effects that:
the copper-clad plate material prepared from the epoxy resin composition has good heat resistance and good toughness (good peeling strength), and can be suitable for halogen-free and environment-friendly lead-free manufacturing processes and processing and manufacturing of multilayer plates.
Detailed Description
The invention is further illustrated by the following examples and comparative examples.
The characteristics of the copper clad laminates of examples 1 to 4 and comparative example were measured by the following method (see IPC-TM-650).
(1) Glass transition temperature (Tg)
Glass transition temperature:
the detection method comprises the following steps: differential Scanning Calorimetry (DSC) is used to refer to the temperature (. degree. C.) at which the sheet changes from a glassy state to a highly elastic (rubbery) state when heated.
(2) Thermal stratification time (T-288):
the T-288 thermal delamination time is the time that the sheet material is delaminated due to the action of heat at a set temperature of 288 ℃, and the time is kept before.
The detection method comprises the following steps: thermomechanical analysis (TMA) was used.
(3) Peel strength:
the test was carried out according to the IPC-TM-650-2.4.8C method.
(4) Solder heat resistance:
solder heat resistance refers to the duration of time during which the sheet is immersed in molten solder at 288 ℃ without delamination and blistering.
The detection method comprises the following steps: cutting the etched substrate into 5.0cm × 5.0cm, sequentially polishing the edges of the substrate with 120-mesh and 800-mesh abrasive paper, cooking for a certain time with a pressure cooker, putting into a tin melting furnace at 288 ℃, and observing whether layering occurs or not.
(5) Water absorption:
the test was carried out according to the IPC-TM-650-2.6.2.1 method.
Example 1
The resin composition comprises 70% by mass of a solid content and the balance of an organic solvent (such as dimethylformamide), wherein the formula of the solid content is shown in the following table 1 (by weight):
TABLE 1
| Raw material | Solid weight (g) |
| Phosphorus-containing epoxy resin | 20 |
| Isocyanic acid modified epoxy resin | 30 |
| Benzoxazine resins | 2 |
| Phosphorus-containing curing agent | 6 |
| Dicyandiamide | 1 |
| Bisphenol A type phenolic resin | 5 |
| Flame retardant | 3 |
| Epoxy resin curing accelerator | 0.08 |
| First inorganic filler | 22 |
| Second inorganic filler | 8 |
2. The preparation method of the epoxy resin composition comprises the following steps:
(1) adding 41 g of organic solvent dimethylformamide, a flame retardant and dicyandiamide into a stirring tank according to the weight, starting a stirrer, rotating at 1000 rpm, and continuously stirring for 120 minutes until the dicyandiamide and the flame retardant are completely dissolved;
(2) sequentially adding phosphorus-containing epoxy resin, isocyanic acid modified epoxy resin, benzoxazine resin, a phosphorus-containing curing agent and bisphenol A type phenolic resin into a stirring tank according to the formula amount, and stirring at the rotating speed of 1000 revolutions per minute in the feeding process;
(3) then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90 minutes after the addition is finished;
(4) weighing the epoxy resin curing accelerator according to the formula ratio of 1: 10 and the organic solvent dimethylformamide, the solution was added to a stirring tank and stirred for 2 hours while maintaining 1000 rpm, to obtain a resin composition.
3. Preparation of copper clad laminate
The resin adhesive prepared by the method is continuously coated or impregnated with glass fiber cloth, the glass fiber cloth is dried under the baking condition of 170 ℃ to obtain prepregs, 8 prepregs are stacked, 1 piece of high-temperature extending copper foil with the thickness of 35 mu m is respectively placed on the upper part and the lower part of the prepreg, and the prepreg is heated and pressurized for 50 minutes under the pressure of 190 ℃ and 350PSI to obtain the copper-clad laminate with the thickness of 1.5 mm.
4. The performance parameters of the copper clad laminate prepared in this example are shown in table 2 below:
TABLE 2
| Item | Test results |
| Glass transition temperature (DSC,. degree.C.) | 142 |
| Copper foil peel strength (1oz, lb/in) | 10.8 |
| T288(TMA,min) | >60 |
| Solder heat resistance (288 ℃ tin, min) | >10 |
| Water absorption (%) | 0.13 |
| Flame retardancy | V0 |
Example 2
1. The resin composition comprises 68% by mass of solids and the balance of an organic solvent (e.g., dimethylformamide), wherein the formulation of the solids is shown in table 3 below (by weight):
TABLE 3
| Raw material | Solid weight (g) |
| Phosphorus-containing epoxy resin | 15 |
| Isocyanic acid modified epoxy resin | 35 |
| Benzoxazine resins | 5 |
| Phosphorus-containing curing agent | 10 |
| Dicyandiamide | 0.8 |
| Bisphenol A type phenolic resin | 7 |
| Flame retardant | 5 |
| Epoxy resin curing accelerator | 0.08 |
| First inorganic filler | 28 |
| Second inorganic filler | 5 |
2. The preparation method of the epoxy resin composition comprises the following steps:
(1) adding 52 g of organic solvent dimethylformamide, a flame retardant and dicyandiamide into a stirring tank according to the weight, starting a stirrer, rotating at 1000 rpm, and continuously stirring for 120 minutes until the dicyandiamide and the flame retardant are completely dissolved;
(2) sequentially adding phosphorus-containing epoxy resin, isocyanic acid modified epoxy resin, benzoxazine resin, a phosphorus-containing curing agent and bisphenol A type phenolic resin into a stirring tank according to the formula amount, and stirring at the rotating speed of 1000 revolutions per minute in the feeding process;
(3) then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90 minutes after the addition is finished;
(4) weighing the epoxy resin curing accelerator according to the formula ratio of 1: 10 and the organic solvent dimethylformamide, the solution was added to a stirring tank and stirred for 2 hours while maintaining 1000 rpm, to obtain a resin composition.
3. Preparation of copper clad laminate
The resin adhesive prepared by the method is continuously coated or impregnated with glass fiber cloth, the glass fiber cloth is dried under the baking condition of 170 ℃ to obtain prepregs, 8 prepregs are stacked, 1 piece of high-temperature extending copper foil with the thickness of 35 mu m is respectively placed on the upper part and the lower part of the prepreg, and the prepreg is heated and pressurized for 50 minutes under the pressure of 190 ℃ and 350PSI to obtain the copper-clad laminate with the thickness of 1.5 mm.
4. The performance parameters of the copper clad laminate prepared in this example are shown in table 4 below:
TABLE 4
| Item | Test results |
| Glass transition temperature (DSC,. degree.C.) | 144 |
| Copper foil peel strength (1oz, lb/in) | 11.2 |
| T288(TMA,min) | >60 |
| Solder heat resistance (288 ℃ tin, min) | >10 |
| Water absorption (%) | 0.14 |
| Flame retardancy | V0 |
Example 3
1. The resin composition contains 65% by mass of a solid content and the balance of an organic solvent (for example, propylene glycol methyl ether), wherein the formulation of the solid content is shown in table 5 below (by weight):
TABLE 5
| Raw material | Solid weight (g) |
| Phosphorus-containing epoxy resin | 25 |
| Isocyanic acid modified epoxy resin | 20 |
| Benzoxazine resins | 7 |
| Phosphorus-containing curing agent | 4 |
| Dicyandiamide | 1.3 |
| Bisphenol A type phenolic resin | 9 |
| Flame retardant | 8 |
| Epoxy resin curing accelerator | 0.1 |
| First inorganic filler | 18 |
| Second inorganic filler | 18 |
2. The preparation method of the epoxy resin composition comprises the following steps:
(1) adding 59 g of organic solvent dimethylformamide, a flame retardant and dicyandiamide into a stirring tank according to the weight, starting a stirrer, rotating at 1000 rpm, and continuously stirring for 120 minutes until the dicyandiamide and the flame retardant are completely dissolved;
(2) sequentially adding phosphorus-containing epoxy resin, isocyanic acid modified epoxy resin, benzoxazine resin, a phosphorus-containing curing agent and bisphenol A phenolic resin into a stirring tank according to the formula amount, and stirring at the rotating speed of 1000 revolutions per minute in the feeding process;
(3) then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90 minutes after the addition is finished;
(4) weighing the epoxy resin curing accelerator according to the formula ratio of 1: 10 and the organic solvent dimethylformamide, the solution was added to a stirring tank and stirred for 2 hours while maintaining 1000 rpm, to obtain a resin composition.
3. Preparation of copper clad laminate
The resin adhesive prepared by the method is continuously coated or impregnated with glass fiber cloth, the glass fiber cloth is dried under the baking condition of 170 ℃ to obtain prepregs, 8 prepregs are stacked, 1 piece of high-temperature extending copper foil with the thickness of 35 mu m is respectively placed on the upper part and the lower part of the prepreg, and the prepreg is heated and pressurized for 60 minutes under the pressure of 190 ℃ and 350PSI to obtain the copper-clad laminate with the thickness of 1.5 mm.
4. The performance parameters of the copper clad laminate prepared in this example are shown in table 6 below:
TABLE 6
| Item | Test results |
| Glass transition temperature (DSC,. degree.C.) | 139 |
| Copper foil peel strength (1oz, lb/in) | 10.1 |
| T288(TMA,min) | >60 |
| Solder heat resistance (288 ℃ tin, min) | >10 |
| Water absorption (%) | 0.12 |
| Flame retardancy | V0 |
Comparative example 1
1. The resin composition comprises 66% by mass of solids and the balance of an organic solvent (e.g., dimethylformamide), wherein the formulation of the solids is shown in table 7 below (by weight):
TABLE 7
| Raw material | Solid weight (g) |
| Phosphorus-containing epoxy resin | 57 |
| Isocyanic acid modified epoxy resin | 18 |
| Dicyandiamide | 3 |
| Epoxy resin curing accelerator | 0.1 |
| First inorganic filler | 10 |
| Second inorganic filler | 20 |
2. The preparation method of the epoxy resin composition comprises the following steps:
(1) adding 56 g of organic solvent dimethylformamide and dicyandiamide into a stirring tank according to the weight, starting a stirrer at the rotating speed of 1000 rpm, and continuously stirring for 120 minutes until the dicyandiamide and the flame retardant are completely dissolved;
(2) sequentially adding phosphorus-containing epoxy resin and isocyanic acid modified epoxy resin into a stirring tank according to the formula amount, and stirring at the rotating speed of 1000 revolutions per minute in the feeding process;
(3) then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90 minutes after the addition is finished;
(4) weighing the epoxy resin curing accelerator according to the formula ratio of 1: 10 and the organic solvent dimethylformamide, the solution was added to a stirring tank and stirred for 2 hours while maintaining 1000 rpm, to obtain a resin composition.
3. Preparation of copper clad laminate
The resin adhesive prepared by the method is continuously coated or impregnated with glass fiber cloth, the glass fiber cloth is dried under the baking condition of 170 ℃ to obtain prepregs, 8 prepregs are stacked, 1 piece of high-temperature extending copper foil with the thickness of 35 mu m is respectively placed on the upper part and the lower part of the prepreg, and the prepreg is heated and pressurized for 60 minutes under the pressure of 190 ℃ and 350PSI to obtain the copper-clad laminate with the thickness of 1.5 mm.
4. The performance parameters of the copper clad laminate prepared in this example are shown in table 8 below:
TABLE 8
| Item | Test results |
| Glass transition temperature (DSC,. degree.C.) | 137 |
| Copper foil peel strength (1oz, lb/in) | 10.5 |
| T288(TMA,min) | 12 |
| Solder heat resistance (288 ℃ tin, min) | 2 |
| Water absorption (%) | 0.15 |
| Flame retardancy | V0 |
Comparative example 2
1. The resin composition comprises 68% by mass of solids and the balance of an organic solvent (such as dimethylformamide), wherein the formulation of the solids is shown in table 9 below (by weight):
TABLE 9
| Raw material | Solid weight (g) |
| Phosphorus-containing epoxy resin | 46 |
| Isocyanic acid modified epoxy resin | 15 |
| Phosphorus-containing curing agent | 7 |
| Bisphenol A type phenolic resin | 17 |
| Epoxy resin curing accelerator | 0.1 |
| First inorganic filler | 19 |
| Second inorganic filler | 11 |
2. The preparation method of the epoxy resin composition comprises the following steps:
(1) adding 55 g of organic solvent dimethylformamide, a flame retardant and dicyandiamide into a stirring tank according to the weight, starting a stirrer, rotating at 1000 rpm, and continuously stirring for 120 minutes until the dicyandiamide is completely dissolved;
(2) sequentially adding phosphorus-containing epoxy resin, isocyanic acid modified epoxy resin, a phosphorus-containing curing agent and bisphenol A type phenolic resin into a stirring tank according to the formula amount, and stirring at the rotating speed of 1000 revolutions per minute in the feeding process;
(3) then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90 minutes after the addition is finished;
(4) weighing the epoxy resin curing accelerator according to the formula ratio of 1: 10 and the organic solvent dimethylformamide, the solution was added to a stirring tank and stirred for 2 hours while maintaining 1000 rpm, to obtain a resin composition.
3. Preparation of copper clad laminate
The resin adhesive prepared by the method is continuously coated or impregnated with glass fiber cloth, the glass fiber cloth is dried under the baking condition of 170 ℃ to obtain prepregs, 8 prepregs are stacked, 1 piece of high-temperature extending copper foil with the thickness of 35 mu m is respectively placed on the upper part and the lower part of the prepreg, and the prepreg is heated and pressurized for 60 minutes under the pressure of 190 ℃ and 350PSI to obtain the copper-clad laminate with the thickness of 1.5 mm.
4. The performance parameters of the copper clad laminate prepared in this example are shown in table 10 below:
watch 10
| Item | Test results |
| Glass transition temperature (DSC,. degree.C.) | 137 |
| Copper foil peel strength (1oz, lb/in) | 7.9 |
| T288(TMA,min) | >60 |
| Solder heat resistance (288 ℃ tin, min) | >10 |
| Water absorption (%) | 0.12 |
| Flame retardancy | V0 |
As can be seen from tables 1 to 9, compared with the comparative examples, the copper clad laminate prepared according to the present invention has the characteristics of a common glass transition temperature (Tg ≧ 138 ℃), excellent heat resistance, good peeling strength, and the like, and is completely suitable for application in the PCB industry to halogen-free and environment-friendly lead-free processes and manufacturing and processing of multilayer boards.
Claims (10)
1. The epoxy resin composition suitable for the halogen-free copper clad plate material is characterized by comprising the following components in percentage by weight:
2. the epoxy resin composition suitable for halogen-free copper clad laminate material according to claim 1, wherein the organic solvent is preferably any one or more of methyl ethyl ketone, toluene, xylene, methyl isobutyl ketone, propylene glycol methyl ether or cyclohexanone.
3. The epoxy resin composition suitable for halogen-free copper clad laminate material according to claim 1, wherein the physical property of the phosphorus-containing epoxy resin is required to have an epoxy equivalent EEW (g/eq) of 290-340;
hydrolysable chlorine (dipropylene glycol methyl ether) 400 MAX;
the solid content (wt%) is 68-72;
the phosphorus content (wt%) is 3.0-3.5;
the phosphorus-containing epoxy resin is shown as the following structural formula 1, wherein n is 4-12:
4. the epoxy resin composition suitable for the halogen-free copper clad plate material according to claim 1, wherein the physical properties of the isocyanic acid modified epoxy resin are as follows:
the epoxy equivalent EEW (g/eq) is 260-320;
hydrolysable chlorine (dipropylene glycol methyl ether) 300 MAX;
the solid content (wt%) is 73-77.
5. The epoxy resin composition suitable for the halogen-free copper clad plate material according to claim 1, wherein the isocyanate modified epoxy resin is any one or more of aromatic diphenylmethane diisocyanate (MDI) modified epoxy resin or Toluene Diisocyanate (TDI) modified epoxy resin.
6. The epoxy resin composition suitable for halogen-free copper clad laminate material according to claim 1, wherein the benzoxazine resin is bisphenol a benzoxazine resin.
7. The epoxy resin composition suitable for halogen-free copper clad plate material according to claim 1, wherein the phosphorus-containing curing agent has the following physical property requirements:
hydroxyl equivalent (g/eq) is 330-560;
hydrolysable chlorine (dipropylene glycol methyl ether) 300 MAX;
the phosphorus content (wt%) is 8-10;
the solid content (wt%) is 54-60;
the phosphorus-containing curing agent is prepared by reacting a phosphorus-containing compound with bisphenol A epoxy resin.
8. The epoxy resin composition suitable for the halogen-free copper clad plate material according to claim 1, wherein the flame retardant has the following parameters:
phosphorus content (wt%): 25-33;
average particle diameter (μm): 0.9-1.5;
the water content (percent) is less than or equal to 0.2;
density @25 ℃ (g/cm 3): 1.9.
9. the epoxy resin composition suitable for halogen-free copper clad laminate material according to claim 1, wherein the first or second inorganic filler is any one or more of talc, quartz powder, ceramic powder, aluminum hydroxide, metal oxide particles such as silica, clay, boron nitride.
10. The method for preparing the epoxy resin composition suitable for the halogen-free copper clad plate material according to any one of claims 1 to 9, comprising the following steps:
1) adding part of organic solvent, dicyandiamide and a fire retardant into a stirring tank, starting a stirrer, continuously stirring for 2-3 hours at the rotation speed of 500-;
then adding the first inorganic filler and the second inorganic filler, and continuously stirring for 90-120 minutes after the addition is finished;
2) sequentially adding the phosphorus-containing epoxy resin, the isocyanic acid modified epoxy resin, the benzoxazine resin, the phosphorus-containing curing agent and the bisphenol A type phenolic resin into a stirring tank, stirring at the rotation speed of 800-;
3) and adding the epoxy resin curing accelerator into the rest organic solvent, adding the solution into a stirring tank after the epoxy resin curing accelerator is completely dissolved, and continuously keeping stirring at 1000-1500 rpm for 5-12 hours to obtain the epoxy resin composition.
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