Epoxy plastic packaging material as well as preparation method and application thereof

Abstract

The invention relates to the field of electronic packaging materials, and discloses an epoxy plastic packaging material and a preparation method and application thereof. The small-particle-size inorganic filler is matched with the low-viscosity epoxy resin, and the toughening agent intermediate, the curing accelerator intermediate, the release agent intermediate, the coupling agent, the curing agent, the curing accelerator, the flame retardant, the release agent, the coloring agent and other auxiliaries are introduced, so that the epoxy plastic packaging material is prepared. The epoxy plastic packaging material has low viscosity, also can keep low adhesion, good fluidity, stable mechanical properties, good demoulding property and high reliability, and the preparation method is simple, efficient, green and environment-friendly, and has wide application prospects in the electronic semiconductor packaging process.

Description

Technical Field

[0001] The present invention relates to the field of electronic packaging materials, and in particular to an epoxy plastic packaging material and a preparation method and application thereof. Background Art

[0002] With the development of emerging applications such as 5G communications, artificial intelligence, smart cars, and data centers, the prosperity and market demand of the semiconductor industry have gradually increased, and the demand for semiconductor materials has therefore increased significantly. As one of the key materials in the field of electronic packaging, epoxy plastic encapsulation materials, along with the rising prosperity of the semiconductor industry, the overall market demand continues to grow, bringing good and huge development opportunities to the development of the domestic plastic encapsulation material industry, and the industrial structure has also quietly changed. Today, the world is in an era of electronic information technology with the Internet as the core, and electronic products are also developing in the direction of high performance, multi-function, high reliability, thinness, lightness, and portability. At the same time, electronic products are also required to have the characteristics of popularization, popularization, and low cost. This puts higher requirements on the electronic packaging industry, and it is urgent to develop products in the direction of lighter, thinner, higher density, higher reliability, and better performance-price ratio. Similarly, higher and newer requirements are also put forward for electronic packaging materials. Meeting the requirements of ultra-thin, miniaturized, high-performance, multi-functional, low-cost, and green and environmentally friendly packaging is the primary problem facing the development of current electronic packaging materials. Therefore, epoxy plastic encapsulation materials, as the main electronic packaging material, are also facing unprecedented opportunities and challenges.

[0003] With the development of the electronic semiconductor industry, the requirements for electronic packaging on integrated circuits are increasing. The reliability of epoxy molding compounds is affected by many factors, including ionic impurities, viscosity, and bonding strength. Ionic impurities will form electrolytes, corrode aluminum wiring, and affect the reliability of devices. Improving purity and reducing ionic impurities can significantly improve the reliability of epoxy molding compounds. Excessive viscosity will cause poor fluidity, and there will be a risk of leaks during the packaging process; materials with good fluidity can better fill the mold and reduce the formation of pores and voids. Excessive adhesion will make it difficult to remove the glue from electronic packaging, affecting product quality and efficiency. However, a decrease in viscosity will inevitably lead to an increase in adhesion.

[0004] Therefore, how to ensure low viscosity of epoxy molding compound while reducing the adhesion as much as possible to avoid problems such as leaking and difficulty in debonding caused by high viscosity and high adhesion, and to ensure good demolding and high reliability between epoxy molding compound and mold, is a technical problem that needs to be solved urgently in the field of epoxy molding compound. Summary of the invention

[0005] The purpose of the present invention is to overcome the problem that low viscosity and low adhesion cannot be taken into account at the same time in the prior art, and to provide an epoxy molding material and a preparation method and application thereof. The epoxy molding material has low viscosity and can maintain low adhesion, has good fluidity, stable mechanical properties, good demoulding properties and high reliability, and the epoxy molding material does not contain halogen compounds and antimony-containing compounds. The preparation method is simple, efficient, green and environmentally friendly, and has broad application prospects in the electronic semiconductor packaging process.

[0006] In order to achieve the above object, the present invention provides a method for preparing an epoxy molding material, which comprises the following steps: (1) mixing a first phenolic resin and a polyether epoxy co-modified silicone oil at a mass ratio of 2-4:1 at 140-160° C. to obtain a first toughening agent intermediate; (2) mixing the first epoxy resin and the modifier at a mass ratio of 6-8:1 at 140-160° C. to obtain a second toughening agent intermediate; (3) mixing the second phenolic resin and the first curing accelerator at a mass ratio of 6-8:1 at 140-160° C. to obtain a curing accelerator intermediate; (4) mixing the third phenolic resin and the first release agent at a mass ratio of 3-5:1 at 140-160° C. to obtain a release agent intermediate; (5) The coupling agent is mixed with the inorganic filler in a mist form, and then the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant are added in sequence and mixed, and then the obtained mixture is extruded, cooled, crushed and compression molded.

[0007] Preferably, the total amount of the coupling agent, the inorganic filler, the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant is 100 parts by weight, the amount of the coupling agent is 0.3-1 parts by weight, the amount of the inorganic filler is 70-80 parts by weight, the amount of the second epoxy resin is 10-18 parts by weight, the amount of the curing agent is 3-10 parts by weight, the amount of the second curing accelerator is 0.01-0.2 parts by weight, the amount of the curing accelerator intermediate is 0.01-1.2 parts by weight, the amount of the first toughening agent intermediate is 0.5-1 parts by weight, the amount of the second toughening agent intermediate is 0.5-1.5 parts by weight, the amount of the flame retardant is 2-10 parts by weight, the amount of the second release agent is 0.1-2 parts by weight, the amount of the release agent intermediate is 1-5 parts by weight, and the amount of the colorant is 0.1-0.5 parts by weight.

[0008] Preferably, each of the first phenolic resin, the second phenolic resin and the third phenolic resin is at least one of a PN type phenolic resin, a XYLOK type phenolic resin and a MAR type phenolic resin.

[0009] Preferably, the viscosity of the first epoxy resin and the second epoxy resin is 0.5-4.5P respectively.

[0010] Preferably, the first epoxy resin and the second epoxy resin are each at least one of bisphenol A epoxy resin, bisphenol F epoxy resin, tetrafunctional epoxy resin, o-cresol epoxy resin, polyphenol glycidyl ether epoxy resin, aliphatic glycidyl ether epoxy resin, glycidyl ester epoxy resin, glycidyl amine epoxy resin, biphenyl epoxy resin, dicyclopentadiene epoxy resin, alicyclic epoxy resin and heterocyclic epoxy resin.

[0011] Preferably, the modifier is at least one of silicone rubber, silicone oil, polyether epoxy co-modified silicone oil, silicone copolymer and carboxyl-terminated polybutadiene acrylonitrile.

[0012] Preferably, the first curing accelerator and the second curing accelerator are each at least one of 2-ethyl-4-methylimidazole, triphenylphosphine, 2-methylimidazole, 1-(dimethylamino)cyclohexanecarbonitrile, 2-phenyl-4-methylimidazole and N,N-dimethylbenzylamine.

[0013] Preferably, each of the first release agent and the second release agent is at least one of carnauba wax, OP wax, S wax, polyethylene wax, ester wax, stearic acid polyamide wax and erucamide.

[0014] Preferably, the coupling agent is at least one of γ-glycidyloxypropyltrimethoxysilane, γ-mercaptopropyltrimethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane and bis-(3-triethoxysilylpropyl)-tetrasulfide.

[0015] Preferably, the maximum particle size of the inorganic filler is less than 200 μm.

[0016] Preferably, the inorganic filler is at least one of aluminum oxide, aluminum nitride, boron nitride, silicon nitride and silicon dioxide.

[0017] Preferably, the inorganic filler is at least one of crystalline angular silica, fused angular silica, fused spherical silica and fumed silica.

[0018] Preferably, the curing agent is at least one of a phenolic curing agent, a low water absorption curing agent and a DCP curing agent.

[0019] Preferably, the flame retardant is at least one of hexaphenylcyclotriphosphazene, triphenylphosphine oxide, zinc borate, magnesium hydroxide and aluminum hydroxide.

[0020] Preferably, the colorant is at least one of carbon black, titanium dioxide and zinc oxide.

[0021] A second aspect of the present invention provides an epoxy molding material prepared by the method described above.

[0022] A third aspect of the present invention provides an application of the epoxy molding material mentioned above in an electronic semiconductor packaging process.

[0023] Through the above technical scheme, inorganic fillers with small particle size and low viscosity epoxy resin are matched, and then toughening agent intermediates, curing accelerator intermediates and release agent intermediates, as well as coupling agents, curing agents, curing accelerators, flame retardants, release agents and colorants and other auxiliary agents are introduced. By adjusting and controlling the content ratio of each component, and then through extrusion, cooling, crushing and compression molding processes, an epoxy molding material can be prepared. The epoxy molding material not only has ultra-low viscosity, so that it has better fluidity during injection molding, can better fill the mold, and reduce the formation of voids and defects, but also the material mechanics has low adhesion, can well meet the high requirements of electronic packaging for degumming, and improve the production quality and efficiency of products. At the same time, the material has stable performance, good reliability, and does not contain halogen compounds and antimony compounds. The preparation method is simple and efficient, green and environmentally friendly, and has broad application prospects in the electronic semiconductor packaging process. DETAILED DESCRIPTION

[0024] The specific embodiments of the present invention are described in detail below. It should be understood that the specific embodiments described herein are only used to illustrate and explain the present invention, and are not used to limit the present invention.

[0025] The endpoints and any values ​​of the ranges disclosed in this article are not limited to the precise ranges or values, and these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of each range, the endpoint values ​​of each range and the individual point values, and the individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed in this article.

[0026] The preparation method of the epoxy molding material of the present invention comprises the following steps: (1) mixing a first phenolic resin and a polyether epoxy co-modified silicone oil at a mass ratio of 2-4:1 at 140-160° C. to obtain a first toughening agent intermediate; (2) mixing the first epoxy resin and the modifier at a mass ratio of 6-8:1 at 140-160° C. to obtain a second toughening agent intermediate; (3) mixing the second phenolic resin and the first curing accelerator at a mass ratio of 6-8:1 at 140-160° C. to obtain a curing accelerator intermediate; (4) mixing the third phenolic resin and the first release agent at a mass ratio of 3-5:1 at 140-160° C. to obtain a release agent intermediate; (5) The coupling agent is mixed with the inorganic filler in a mist form, and then the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant are added in sequence and mixed, and then the obtained mixture is extruded, cooled, crushed and compression molded.

[0027] According to the method described in the present invention, the first toughening agent intermediate, the second toughening agent intermediate, the curing accelerator intermediate and the release agent intermediate are first prepared, and some of the materials are preferentially melt-mixed at high temperature, so that the materials can be better dispersed, mixed more evenly in the subsequent mixing process, and the prepared materials have better uniformity.

[0028] According to the method of the present invention, the total amount of the coupling agent, the inorganic filler, the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant is 100 parts by weight, the amount of the coupling agent can be 0.3-1 parts by weight, the amount of the inorganic filler can be 70-80 parts by weight, the amount of the second epoxy resin can be 10-18 parts by weight, the amount of the curing agent can be 3-10 parts by weight, the amount of the second curing accelerator can be 0.01-0.2 parts by weight, the amount of the curing accelerator intermediate can be 0.01-1.2 parts by weight, the amount of the first toughening agent intermediate can be 0.5-1 parts by weight, the amount of the second toughening agent intermediate can be 0.5-1.5 parts by weight, the amount of the flame retardant can be 2-10 parts by weight, the amount of the second release agent can be 0.1-2 parts by weight, the amount of the release agent intermediate can be 1-5 parts by weight, and the amount of the colorant can be 0.1-0.5 parts by weight.

[0029] In a preferred embodiment, the total amount of the coupling agent, the inorganic filler, the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant is 100 parts by weight, the amount of the coupling agent is 0.5-0.7 parts by weight, the amount of the inorganic filler is 72-78 parts by weight, the amount of the second epoxy resin is 10-15 parts by weight, the amount of the curing agent is The amount of the second curing accelerator is 3-6 parts by weight, the amount of the second curing accelerator is 0.05-0.15 parts by weight, the amount of the curing accelerator intermediate is 0.1-0.2 parts by weight, the amount of the first toughening agent intermediate is 0.6-0.8 parts by weight, the amount of the second toughening agent intermediate is 0.8-1.3 parts by weight, the amount of the flame retardant is 2-5 parts by weight, the amount of the second release agent is 0.2-0.4 parts by weight, the amount of the release agent intermediate is 2-4 parts by weight, and the amount of the colorant is 0.2-0.4 parts by weight.

[0030] According to the method of the present invention, each of the first phenolic resin, the second phenolic resin and the third phenolic resin can be a phenolic resin commonly used in the art, preferably at least one of a PN type phenolic resin, a XYLOK type phenolic resin and a MAR type phenolic resin. The first phenolic resin, the second phenolic resin and the third phenolic resin can be selected from different types of phenolic resins, or the same type of phenolic resins, or a mixture of different types of phenolic resins.

[0031] According to the method of the present invention, the viscosity of the first epoxy resin and the second epoxy resin can each be an epoxy resin with lower viscosity in the art. In a preferred case, the viscosity of the first epoxy resin and the second epoxy resin is 0.5-4.5P respectively. In a more preferred case, the viscosity of the first epoxy resin and the second epoxy resin is 0.8-4.2P respectively. The viscosity is measured under standard conditions of a temperature of 150°C and a frequency of 400Hz. In the method of the present invention, the second epoxy resin can be selected from epoxy resins of different viscosities, or a single viscosity epoxy resin can be selected.

[0032] In a more preferred case, the first epoxy resin and the second epoxy resin are each at least one of bisphenol A epoxy resin, bisphenol F epoxy resin, tetrafunctional epoxy resin, o-cresol epoxy resin, polyphenol glycidyl ether epoxy resin, aliphatic glycidyl ether epoxy resin, glycidyl ester epoxy resin, glycidyl amine epoxy resin, biphenyl epoxy resin, dicyclopentadiene epoxy resin, alicyclic epoxy resin and heterocyclic epoxy resin.

[0033] According to the method of the present invention, the modifier may be at least one of organic silicone rubber, silicone oil, polyether epoxy co-modified silicone oil, organic silicone copolymer and carboxyl-terminated polybutadiene acrylonitrile.

[0034] According to the method described in the present invention, the first curing accelerator and the second curing accelerator can each be at least one of 2-ethyl-4-methylimidazole, triphenylphosphine, 2-methylimidazole, 1-(dimethylamino)cyclohexanecarbonitrile, 2-phenyl-4-methylimidazole and N,N-dimethylbenzylamine.

[0035] According to the method of the present invention, the first release agent and the second release agent can each be at least one of carnauba wax, OP wax, S wax, polyethylene wax, ester wax, stearic acid polyamide wax and erucamide. In a specific embodiment, the second release agent is a combination of carnauba wax and ester wax, and the mass ratio of the carnauba wax to the ester wax is 1-2:1.

[0036] According to the method of the present invention, the coupling agent can be a coupling agent commonly used in the art, preferably at least one of γ-glycidyloxypropyltrimethoxysilane, γ-mercaptopropyltrimethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane and bis-(3-triethoxysilylpropyl)-tetrasulfide. In a specific embodiment, the coupling agent is a combination of γ-glycidyloxypropyltrimethoxysilane and γ-mercaptopropyltrimethoxysilane, and the mass ratio of the γ-glycidyloxypropyltrimethoxysilane to the γ-mercaptopropyltrimethoxysilane is 2-3:1.

[0037] According to the method of the present invention, the maximum particle size of the inorganic filler can be less than 200 μm. In a preferred case, the maximum particle size of the inorganic filler is less than 180 μm. In a further preferred case, the inorganic filler is at least one of aluminum oxide, aluminum nitride, boron nitride, silicon nitride and silicon dioxide. In a further preferred case, the inorganic filler is at least one of crystalline angular silica, fused angular silica, fused spherical silica and fumed silica.

[0038] In some specific embodiments, the inorganic filler is a combination of fused angular silica, crystalline angular silica, fused spherical silica and fumed silica, and the mass ratio of the fused angular silica, the crystalline angular silica, the fused spherical silica and the fumed silica is 80-200:24-34:8-18:1.

[0039] In some other specific embodiments, the inorganic filler is a combination of fused angular silica and fumed silica, and the mass ratio of the fused angular silica to the fumed silica is 145-155:1.

[0040] In other specific embodiments, the inorganic filler is a combination of fused angular silica, crystalline angular silica and fumed silica, and the mass ratio of the fused angular silica, the crystalline angular silica and the fumed silica is 130-140:13-15:1.

[0041] According to the method of the present invention, the curing agent can be a curing agent commonly used in the art, preferably at least one of a phenolic curing agent, a low water absorption curing agent and a DCP curing agent.

[0042] According to the method of the present invention, the flame retardant can be at least one of hexaphenylcyclotriphosphazene, triphenylphosphine oxide, zinc borate, magnesium hydroxide and aluminum hydroxide. In a specific embodiment, the flame retardant is a combination of zinc borate and hexaphenylcyclotriphosphazene, and the mass ratio of the zinc borate to the hexaphenylcyclotriphosphazene is 1:3-5.

[0043] According to the method of the present invention, the colorant may be at least one of carbon black, titanium dioxide and zinc oxide.

[0044] According to the method of the present invention, in step (5), the extrusion process includes: kneading the mixture obtained by mixing, melting and mixing at a temperature of 100-140°C to uniformly form a black mud-like material, and then extruding at a temperature of 10-110°C.

[0045] According to the method of the present invention, the mixing process can be carried out in a high-speed mixer, and the extrusion process can be carried out in a twin-screw extruder. In a preferred case, the extrusion conditions include: the screw speed is 100-200rpm.

[0046] The present invention also provides an epoxy molding material prepared by the method described above. The epoxy molding material does not contain halogen compounds and antimony-containing compounds and has good green environmental protection effects.

[0047] The present invention also provides the application of the epoxy molding material described above in the electronic semiconductor packaging process. Since the epoxy molding material described in the present invention has low viscosity and can maintain low adhesion, its low viscosity property makes it more fluid during the injection molding process, reduces the formation of voids and defects, and is easier to demold; and the low adhesion can avoid the problems of leaking seals and difficulty in removing glue caused by high viscosity and high adhesion, and the epoxy molding material also has good reliability, so it has broad application prospects in the electronic semiconductor packaging process.

[0048] The following examples further illustrate the epoxy molding material and its preparation method and application of the present invention. The examples are implemented based on the technical solution of the present invention, and provide detailed implementation methods and specific operation processes, but the protection scope of the present invention is not limited to the following examples.

[0049] The experimental methods in the following examples, unless otherwise specified, are all conventional methods in the art. The experimental materials used in the following examples, unless otherwise specified, are all commercially available.

[0050] Example 1 The sources of materials in this embodiment are shown in Table 1. Table 1

[0051] (1) mixing PN phenolic resin-2 and polyether epoxy co-modified silicone oil at a mass ratio of 3:1 at 150° C. to obtain a first toughening agent intermediate; (2) mixing o-cresol epoxy resin-2 and silicone copolymer at a mass ratio of 7:1 at 150° C. to obtain a second toughening agent intermediate; (3) mixing PN phenolic resin-2 and 1-(dimethylamino)cyclohexanecarbonitrile at a mass ratio of 7:1 at 150° C. to obtain a curing accelerator intermediate; (4) mixing PN phenolic resin-2 and OP wax at a mass ratio of 4:1 at 150° C. to obtain a release agent intermediate; (5) 50.68 kg of silica powder-2, 15 kg of silica powder-3, 8 kg of silica powder-4 and 0.6 kg of fumed silica were added to a high-speed mixer and mixed for 15 minutes; then 0.43 kg of γ-glycidyloxypropyltrimethoxysilane and 0.17 kg of γ-mercaptopropyltrimethoxysilane-1 were slowly sprayed into the high-speed mixer in a mist form through a high-pressure nozzle and mixed for another 4 minutes; then 3.19 kg of o-cresol epoxy resin-1, 10 kg of o-cresol epoxy resin-2, 4.2 1kg of PN phenolic resin-1, 0.1kg of 2-methylimidazole, 0.74kg of the first toughening agent intermediate, 1.11kg of the second toughening agent intermediate, 0.17kg of the curing accelerator intermediate, 0.5kg of zinc borate, 2kg of hexaphenylcyclotriphosphazene, 2.43kg of the release agent intermediate, 0.21kg of carnauba wax, 0.13kg of ester wax and 0.33kg of carbon black were sequentially put into a high-speed mixer and mixed for 45 minutes to make them fully mixed and uniform; finally, the extrusion temperature of the twin-screw extruder was set to 100°C and the screw speed was 100rpm, and the uniformly mixed powder was put into the twin-screw extruder to obtain an extruded product, which was crushed into powder after cooling, and finally the powder was compressed into cakes of the required size by a forming cake making machine to obtain the epoxy plastic encapsulation material L1.

[0052] Example 2 The source of materials in this embodiment is the same as that in Example 1.

[0053] (1) mixing PN phenolic resin-2 and polyether epoxy co-modified silicone oil at a mass ratio of 2:1 at 140° C. to obtain a first toughening agent intermediate; (2) mixing o-cresol epoxy resin-2 and silicone copolymer at a mass ratio of 6:1 at 140° C. to obtain a second toughening agent intermediate; (3) mixing PN phenolic resin-2 and 1-(dimethylamino)cyclohexanecarbonitrile at a mass ratio of 6:1 at 140° C. to obtain a curing accelerator intermediate; (4) mixing PN phenolic resin-2 and OP wax at a mass ratio of 3:1 at 140° C. to obtain a release agent intermediate; (5) 50 kg of silica powder-2, 13.5 kg of silica powder-3, 6 kg of silica powder-4 and 0.5 kg of fumed silica were added to a high-speed mixer and mixed for 10 minutes; then 0.4 kg of γ-glycidyloxypropyltrimethoxysilane and 0.1 kg of γ-mercaptopropyltrimethoxysilane-1 were slowly sprayed into the high-speed mixer in a mist form through a high-pressure nozzle and mixed for 3 minutes; then 5 kg of o-cresol epoxy resin-1, 13 kg of o-cresol epoxy resin-2, 4 kg of PN phenolic resin-1, 0.2 kg of 2-methylimidazole, 0.9 kg of the first toughening agent intermediate, and 1.3 kg of The second toughening agent intermediate, 0.2 kg of the curing accelerator intermediate, 0.1 kg of zinc borate, 1.9 kg of hexaphenylcyclotriphosphazene, 2 kg of the release agent intermediate, 0.1 kg of carnauba wax, 0.3 kg of ester wax and 0.5 kg of carbon black were put into a high mixer in sequence and mixed for 40 minutes to make them fully mixed; finally, the extrusion temperature of the twin-screw extruder was set to 100°C and the screw speed was 100 rpm, and the evenly mixed powder was put into the twin-screw extruder to obtain the extruded product, which was crushed into powder after cooling, and finally the powder was compressed into cakes of the required size by a forming cake making machine to obtain the epoxy molding material L2.

[0054] Example 3 The source of materials in this embodiment is the same as that in Example 1.

[0055] (1) mixing PN phenolic resin-2 and polyether epoxy co-modified silicone oil at a mass ratio of 4:1 at 160° C. to obtain a first toughening agent intermediate; (2) mixing o-cresol epoxy resin-2 and silicone copolymer at a mass ratio of 8:1 at 160° C. to obtain a second toughening agent intermediate; (3) mixing PN phenolic resin-2 and 1-(dimethylamino)cyclohexanecarbonitrile at a mass ratio of 8:1 at 160° C. to obtain a curing accelerator intermediate; (4) mixing PN phenolic resin-2 and OP wax at a mass ratio of 5:1 at 160° C. to obtain a release agent intermediate; (5) 51 kg of silica powder-2, 16 kg of silica powder-3, 8.3 kg of silica powder-4 and 0.7 kg of fumed silica were added to a high-speed mixer and mixed for 20 minutes; then 0.6 kg of γ-glycidyloxypropyltrimethoxysilane and 0.1 kg of γ-mercaptopropyltrimethoxysilane-1 were slowly sprayed into the high-speed mixer in a mist form through a high-pressure nozzle and mixed for 5 minutes; then 2 kg of o-cresol epoxy resin-1, 8 kg of o-cresol epoxy resin-2, 4.5 kg of PN phenolic resin-1, 0.05 kg of 2-methylimidazole, 0.65 kg of the first toughening agent intermediate, and 1 kg of The second toughening agent intermediate, 0.1 kg of the curing accelerator intermediate, 1 kg of zinc borate, 2.5 kg of hexaphenylcyclotriphosphazene, 2.9 kg of the release agent intermediate, 0.3 kg of carnauba wax, 0.1 kg of ester wax and 0.2 kg of carbon black were put into a high mixer in sequence and mixed for 50 minutes to make them fully mixed; finally, the extrusion temperature of the twin-screw extruder was set to 100°C and the screw speed was 100 rpm, and the evenly mixed powder was put into the twin-screw extruder to obtain the extruded product, which was crushed into powder after cooling, and finally the powder was compressed into cakes of the required size by a forming cake making machine to obtain the epoxy molding material L3.

[0056] Example 4 The source of materials in this embodiment is the same as that in embodiment 1.

[0057] An epoxy molding material was prepared according to the method of Example 1, except that in step (5), the amount of silicon micropowder-2 was increased to 55.78 kg, the amount of silicon micropowder-3 was reduced to 13 kg, the amount of silicon micropowder-4 was reduced to 5 kg, and the amount of fumed silica was reduced to 0.5 kg, to obtain epoxy molding material L4.

[0058] Example 5 The sources of the inorganic filler and the second epoxy resin in this embodiment are shown in Table 2, and the sources of the remaining materials are the same as those in Embodiment 1.

[0059] Table 2

[0060] Based on the method of Example 1, step (5) is as follows: 59.47 kg of silicon powder-1, 10 kg of silicon powder-3, 5 kg of silicon powder-4 and 0.3 kg of fumed silica are put into a high-speed mixer and mixed for 15 minutes; then 0.43 kg of γ-glycidyloxypropyltrimethoxysilane and 0.17 kg of γ-mercaptopropyltrimethoxysilane-1 are slowly sprayed into the high-speed mixer in a mist form through a high-pressure nozzle, and mixing is continued for 4 minutes; then 12.87 kg of o-cresol epoxy resin-2, 4.05 kg of PN phenolic resin-1, 0.1 kg of 2-methylimidazole, 0.74 kg of the first toughening agent intermediate, 1.1 1 kg of the second toughening agent intermediate, 0.16 kg of the curing accelerator intermediate, 0.5 kg of zinc borate, 2 kg of hexaphenylcyclotriphosphazene, 2.43 kg of the release agent intermediate, 0.21 kg of carnauba wax, 0.13 kg of ester wax and 0.33 kg of carbon black are sequentially put into a high mixer and mixed for 45 minutes to make them fully mixed; finally, the extrusion temperature of the twin-screw extruder is set to 100°C and the screw speed is 100 rpm, and the evenly mixed powder is put into the twin-screw extruder to obtain an extruded product, which is crushed into powder after cooling, and finally the powder is compressed into cakes of the required size by a forming cake making machine to obtain epoxy molding material L5.

[0061] Example 6 The sources of the inorganic filler in this example are shown in Table 3, and the sources of the remaining materials are the same as those in Example 1.

[0062] Table 3

[0063] Based on the method of Example 1, step (5) is as follows: 67.28 kg of silicon powder-1, 7 kg of silicon powder-3 and 0.49 kg of fumed silica are put into a high-speed mixer and mixed for 15 minutes; then 0.43 kg of γ-glycidyloxypropyltrimethoxysilane and 0.17 kg of γ-mercaptopropyltrimethoxysilane-1 are slowly sprayed into the high-speed mixer in a mist form through a high-pressure nozzle, and the mixture is mixed for 4 minutes; then 6.5 kg of o-cresol epoxy resin-1, 6.37 kg of o-cresol epoxy resin-2, 4.05 kg of PN phenolic resin-1, 0.1 kg of 2-methylimidazole, 0.74 kg of the first toughening agent intermediate, 1.11 kg of the second toughening agent intermediate, 0.16 kg of the curing accelerator intermediate, 0.5 kg of zinc borate, 2 kg of hexaphenylcyclotriphosphazene, 2.43 kg of the release agent intermediate, 0.21 kg of carnauba wax, 0.13 kg of ester wax and 0.33 kg of carbon black were successively put into a high mixer and mixed for 45 minutes to make them fully mixed; finally, the extrusion temperature of the twin-screw extruder was set to 100 ° C, and the screw speed was 100 rpm, and the evenly mixed powder was put into the twin-screw extruder to obtain an extruded product, which was crushed into powder after cooling, and finally the powder was compressed into cakes of the required size by a forming cake making machine to obtain epoxy plastic encapsulation material L6.

[0064] Example 7 The sources of the inorganic filler, the second epoxy resin, the coupling agent and the curing agent in this embodiment are shown in Table 4, and the sources of the remaining materials are the same as those in Embodiment 1.

[0065] Table 4

[0066] Based on the method of Example 1, step (5) is as follows: 74.2 kg of silicon powder-1 and 0.49 kg of fumed silica are added to a high-speed mixer and mixed for 15 minutes; 0.43 kg of γ-glycidyloxypropyltrimethoxysilane and 0.17 kg of γ-mercaptopropyltrimethoxysilane-2 are then slowly sprayed into the high-speed mixer in a mist form through a high-pressure nozzle, and the mixture is mixed for 4 minutes; 12.8 kg of o-cresol epoxy resin-2, 4.05 kg of PN phenolic resin-2, 0.1 kg of 2-methylimidazole, 0.74 kg of the first toughening agent intermediate, and 1.11 kg of the second toughening agent intermediate are then added. The epoxy resin L7 was prepared by mixing 0.16 kg of curing accelerator intermediate, 0.5 kg of zinc borate, 2 kg of hexaphenylcyclotriphosphazene, 2.43 kg of release agent intermediate, 0.21 kg of carnauba wax, 0.13 kg of ester wax and 0.33 kg of carbon black in a high-speed mixer for 45 minutes to make them fully mixed. Finally, the extrusion temperature of the twin-screw extruder was set to 100 ° C and the screw speed was set to 100 rpm. The evenly mixed powder was put into the twin-screw extruder to obtain an extruded product, which was crushed into powder after cooling. Finally, the powder was compressed into cakes of the required size by a forming cake making machine to obtain the epoxy molding material L7.

[0067] Comparative Example 1 The sources of materials in this comparative example are the same as those in Example 1.

[0068] Directly add 50.68kg of silicon powder-2, 15kkg of silicon powder-3, 8kkg of silicon powder-4, 0.6kg of fumed silica, 0.43kg of γ-glycidyloxypropyltrimethoxysilane, 0.17kg of γ-mercaptopropyltrimethoxysilane-1, 3.19kg of o-cresol epoxy resin-1, 10.971kg of o-cresol epoxy resin-2, 4.21kg of PN phenolic resin-1, 2.649kg of PN phenolic resin-2, 0.1kg of 2-methylimidazole, 0.02kg of 1-(dimethylamino)cyclohexanecarbonitrile, 0.5kg 2kg of zinc borate, 2kg of hexaphenylcyclotriphosphazene, 0.21kg of carnauba wax, 0.13kg of ester wax, 0.486kg of OP wax, 0.324kg of polyether epoxy co-modified silicone oil and 0.33kg of carbon black were put into a high mixer in sequence and mixed for 65 minutes to make them fully mixed; finally, the extrusion temperature of the twin-screw extruder was set to 100°C and the screw speed was 100rpm, and the evenly mixed powder was put into the twin-screw extruder to obtain an extruded product, which was crushed into powder after cooling, and finally the powder was compressed into cakes of the required size by a forming cake making machine to obtain the epoxy molding material M1.

[0069] Comparative Example 2 An epoxy molding material was prepared according to the method of Example 1, except that the second epoxy resin used was o-cresol epoxy resin-3, brand CNE195XL-8, purchased from Changchun Artificial Resin Factory Co., Ltd., with a viscosity of 4.5-6p, to obtain epoxy molding material M2.

[0070] Comparative Example 3 An epoxy molding material was prepared according to the method of Example 1, except that the organic filler used was silica powder-5 with a brand name of RST-11 purchased from Ristar Company and a maximum particle size of 250 μm, to obtain epoxy molding material M3.

[0071] Test Case The epoxy molding materials L1-L7 prepared in Examples 1-7 and the epoxy molding materials M1-M3 prepared in Comparative Examples 1-3 were performance tested. Referring to the test standard of "Test Method for Epoxy Resins for Electronic Packaging" (kgB / T40564-2021), the following performance indicators were tested: gelation time, spiral flow length, 90s / 120s hot hardness, viscosity, Cu adhesion before curing, and Cu adhesion after curing. The test results are shown in Table 5.

[0072] Table 5

[0073] It can be seen from the results in Table 1 that the epoxy molding material prepared by the method of the present invention has a longer gelation time and a longer spiral flow length, indicating that the epoxy molding material has better fluidity; its 90s / 120s thermal hardness changes little, indicating that the mechanical properties of the epoxy molding material are stable and it has excellent reliability; in a preferred case, the viscosity of the epoxy molding material can be as low as 33.7Pa·s, and the Cu adhesion before and after curing is close to zero, fully demonstrating that the epoxy molding material can maintain low viscosity while maintaining low adhesion; while the epoxy molding material M1 in Comparative Example 1 has good fluidity, its viscosity is large, and the adhesion before and after curing is also high, and it is not suitable for packaging material production, and the high viscosity and high adhesion of the epoxy molding materials in Comparative Examples 2-3 are even more unsuitable for electronic packaging materials.

[0074] The preferred embodiments of the present invention are described in detail above, but the present invention is not limited thereto. Within the technical concept of the present invention, the technical solution of the present invention can be subjected to a variety of simple modifications, including the combination of various technical features in any other suitable manner, and these simple modifications and combinations should also be regarded as the contents disclosed by the present invention and belong to the protection scope of the present invention.

Claims

1. A method for preparing an epoxy molding material, characterized in that: The method comprises the following steps: (1) mixing a first phenolic resin and a polyether epoxy co-modified silicone oil at a mass ratio of 2-4:1 at 140-160° C. to obtain a first toughening agent intermediate; (2) mixing the first epoxy resin and the modifier at a mass ratio of 6-8:1 at 140-160° C. to obtain a second toughening agent intermediate; (3) mixing the second phenolic resin and the first curing accelerator at a mass ratio of 6-8:1 at 140-160° C. to obtain a curing accelerator intermediate; (4) mixing the third phenolic resin and the first release agent at a mass ratio of 3-5:1 at 140-160° C. to obtain a release agent intermediate; (5) The coupling agent is mixed with the inorganic filler in a mist form, and then the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant are added in sequence and mixed, and then the obtained mixture is extruded, cooled, crushed and compression molded.

2. The method according to claim 1, characterized in that The total amount of the coupling agent, the inorganic filler, the second epoxy resin, the curing agent, the second curing accelerator, the curing accelerator intermediate, the first toughening agent intermediate, the second toughening agent intermediate, the flame retardant, the second release agent, the release agent intermediate and the colorant is 100 parts by weight, the amount of the coupling agent is 0.3-1 parts by weight, the amount of the inorganic filler is 70-80 parts by weight, the amount of the second epoxy resin is 10-18 parts by weight, the amount of the curing agent is 3- 10 parts by weight, the amount of the second curing accelerator is 0.01-0.2 parts by weight, the amount of the curing accelerator intermediate is 0.01-1.2 parts by weight, the amount of the first toughening agent intermediate is 0.5-1 parts by weight, the amount of the second toughening agent intermediate is 0.5-1.5 parts by weight, the amount of the flame retardant is 2-10 parts by weight, the amount of the second release agent is 0.1-2 parts by weight, the amount of the release agent intermediate is 1-5 parts by weight, and the amount of the colorant is 0.1-0.5 parts by weight.

3. The method according to claim 1 or 2, characterized in that: Each of the first phenolic resin, the second phenolic resin, and the third phenolic resin is at least one of a PN type phenolic resin, a XYLOK type phenolic resin, and a MAR type phenolic resin.

4. The method according to claim 1 or 2, characterized in that: The viscosity of the first epoxy resin and the second epoxy resin is 0.5-4.5P respectively; Preferably, the first epoxy resin and the second epoxy resin are each at least one of bisphenol A epoxy resin, bisphenol F epoxy resin, tetrafunctional epoxy resin, o-cresol epoxy resin, polyphenol glycidyl ether epoxy resin, aliphatic glycidyl ether epoxy resin, glycidyl ester epoxy resin, glycidyl amine epoxy resin, biphenyl epoxy resin, dicyclopentadiene epoxy resin, alicyclic epoxy resin and heterocyclic epoxy resin.

5. The method according to claim 1 or 2, characterized in that: The modifier is at least one of organic silicone rubber, silicone oil, polyether epoxy co-modified silicone oil, organic silicone copolymer and carboxyl-terminated polybutadiene acrylonitrile.

6. The method according to claim 1 or 2, characterized in that: The first curing accelerator and the second curing accelerator are each at least one of 2-ethyl-4-methylimidazole, triphenylphosphine, 2-methylimidazole, 1-(dimethylamino)cyclohexanecarbonitrile, 2-phenyl-4-methylimidazole and N,N-dimethylbenzylamine.

7. The method according to claim 1 or 2, characterized in that: The first mold release agent and the second mold release agent are each at least one of carnauba wax, OP wax, S wax, polyethylene wax, ester wax, stearic acid polyamide wax and erucamide.

8. The method according to claim 1 or 2, characterized in that: The coupling agent is at least one of γ-glycidyloxypropyltrimethoxysilane, γ-mercaptopropyltrimethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane and bis-(3-triethoxysilylpropyl)-tetrasulfide.

9. The method according to claim 1 or 2, characterized in that: The maximum particle size of the inorganic filler is less than 200 μm; Preferably, the inorganic filler is at least one of aluminum oxide, aluminum nitride, boron nitride, silicon nitride and silicon dioxide; More preferably, the inorganic filler is at least one of crystalline angular silica, fused angular silica, fused spherical silica and fumed silica.

10. The method according to claim 1 or 2, characterized in that: The curing agent is at least one of a phenolic curing agent, a low water absorption curing agent and a DCP curing agent; and / or The flame retardant is at least one of hexaphenylcyclotriphosphazene, triphenylphosphine oxide, zinc borate, magnesium hydroxide and aluminum hydroxide; and / or The colorant is at least one of carbon black, titanium dioxide and zinc oxide.

11. An epoxy molding material prepared by the method according to any one of claims 1 to 10.

12. Use of the epoxy molding material according to claim 11 in an electronic semiconductor packaging process.

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