Epoxy resin composition and preparation method thereof

Abstract

The present invention relates to an epoxy resin composition, wherein, based on the total weight of the epoxy resin composition, the epoxy resin composition comprises: (a) 1-12 weight % of epoxy resin, (b) 1-8 weight % of phenolic resin, (c) 0.1-1 weight % of curing accelerator, (d) 30-95 weight % of high dielectric filler, (e) 0-35 weight % of low dielectric filler; the high dielectric filler comprises titanate. The present invention also relates to a preparation method of the epoxy resin composition and its use in molded packaging.

Description

Technical Field

[0001] The present invention belongs to the technical field of microelectronic packaging materials, and specifically relates to an epoxy resin composition. The present invention and its preparation method also relate to a preparation method of the epoxy resin composition and its use in molding packaging. Background Art

[0002] With the rapid development of information technology, wireless communication has become a necessity in life. The wireless communication system consists of transmission, reception and antenna. The antenna is responsible for the conversion of electromagnetic energy values ​​between the circuit and the air. It is one of the indispensable basic equipment of the communication system. The circuit design related to the antenna will rely on passive components such as capacitors or inductors to match the antenna. With the demand for high frequency and high speed of signal transmission in 5G and the future 6G, the antenna size needs to be reduced to the package size, and AiP (Antenna in package) came into being. The advantage of AiP is that the system design is simple, which is conducive to the miniaturization and low cost of the equipment. High dielectric packaging materials are the best choice for the materials required for the design and packaging of such antenna equipment.

[0003] CN 106280275 A relates to a high dielectric epoxy molding compound and a preparation method and application thereof, wherein the filler is graphene-coated silicon dioxide particles with a particle size of 50nm-5μm. The prepared high dielectric epoxy molding compound has low expansion coefficient, low stress, high dielectric constant, small dielectric loss, and good dielectric performance frequency stability, and can be used in the field of fingerprint sensor packaging. Summary of the invention

[0004] In one aspect, the present invention relates to an epoxy resin composition, wherein, based on the total weight of the epoxy resin composition, the epoxy resin composition comprises: (a) 1-12 wt % of an epoxy resin, (b) 1-8 wt % of a phenolic resin, (c) 0.1-1 wt % of a curing accelerator, (d) 30-95 wt % of a high dielectric filler, and (e) 0-35 wt % of a low dielectric filler; the high dielectric filler comprises titanate.

[0005] In one embodiment, in the epoxy resin composition of the present invention, the titanate is selected from barium titanate, strontium titanate, calcium titanate, lead titanate and combinations thereof.

[0006] In a preferred embodiment, in the epoxy resin composition of the present invention, the titanate is barium titanate.

[0007] In another embodiment, in the epoxy resin composition of the present invention, the high dielectric filler further comprises a transition metal oxide.

[0008] In a preferred embodiment, in the epoxy resin composition of the present invention, the transition metal oxide is selected from iron oxide, titanium oxide and a combination thereof.

[0009] In one embodiment, in the epoxy resin composition of the present invention, the content of the titanate is 25-95 wt % based on the total weight of the epoxy resin composition.

[0010] In another embodiment, in the epoxy resin composition of the present invention, the content of the transition metal oxide is 0.1-17 wt % based on the total weight of the epoxy resin composition.

[0011] In yet another embodiment, in the epoxy resin composition of the present invention, the ratio of the weight of the titanate to the weight of the transition metal oxide is greater than 3 based on the total weight of the epoxy resin composition.

[0012] In one embodiment, in the epoxy resin composition of the present invention, the content of titanium oxide in the transition metal oxide is 0.1-12 wt % based on the total weight of the epoxy resin composition.

[0013] In another embodiment, in the epoxy resin composition of the present invention, the content of iron oxide in the transition metal oxide is 0.1-7 wt % based on the total weight of the epoxy resin composition.

[0014] In one embodiment, in the epoxy resin composition of the present invention, the total content of the high dielectric filler and the low dielectric filler is 75-95 wt % based on the total weight of the epoxy resin composition.

[0015] In another embodiment, in the epoxy resin composition of the present invention, the ratio of the weight of the high dielectric filler to the weight of the low dielectric filler is 2 or more.

[0016] In another aspect, the present invention also relates to a method for preparing the epoxy resin composition of the present invention, comprising the steps of: (1) weighing each component and mixing them to obtain a premixed powder, and (2) heating and mixing the premixed powder and extruding it to obtain a product.

[0017] In another aspect, the present invention also relates to the use of the epoxy resin composition of the present invention in a molded package. In a preferred embodiment, in the use of the epoxy resin composition, the molded package is a package using package antenna technology. DETAILED DESCRIPTION

[0018] General Definitions and Terminology

[0019] Unless otherwise indicated, all publications, patent applications, patents, and other references mentioned herein are incorporated by reference in their entirety.

[0020] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. In the event of a conflict, the definitions provided herein shall prevail.

[0021] Unless otherwise indicated, all percentages, parts, ratios, etc. are by weight.

[0022] When quantity, concentration or other value or parameter is given as range, preferred range or preferred upper limit and lower limit or specific value, it should be understood as specifically disclosing all ranges formed by paired values ​​from any upper limit range or preferred value and any lower limit range or preferred value, regardless of whether the range is disclosed separately. Unless otherwise stated, when numerical range is quoted herein, the range refers to including its endpoints and integers and fractions within all such ranges. The scope of the present invention is not limited to the specific numerical value quoted when defining the range. For example, "1-8" covers 1, 2, 3, 4, 5, 6, 7, 8 and any sub-range consisting of any two values ​​therein, such as 2-6, 3-5.

[0023] The terms "about" and "approximately" when used with a numerical variable generally refer to the value of that variable and all values ​​of that variable are within experimental error (e.g., within a 95% confidence interval for the mean) or within ±10% of the specified value, or a wider range.

[0024] The terms "comprises", "includes", "has", "contains" or "involves" and other variations thereof herein are inclusive or open-ended and do not exclude other unlisted elements or method steps. It will be understood by those skilled in the art that the above terms such as "comprising" encompass the meaning of "consisting of". The expression "consisting of" excludes any element, step or ingredient not specified. The expression "consisting essentially of" means that the scope is limited to the specified elements, steps or ingredients, plus the optional presence of elements, steps or ingredients that do not substantially affect the basic and novel features of the claimed subject matter. It will be understood that the expression "comprising" encompasses the expressions "consisting essentially of" and "consisting of".

[0025] The term "selected from..." means that one or more elements in the group listed later are independently selected and may include combinations of two or more elements.

[0026] When values ​​or end-points of a range are described herein, it should be understood that the disclosure includes the specific value or end-point cited.

[0027] As used herein, the terms "one or more" or "at least one" refer to one, two, three, four, five, six, seven, eight, nine or more.

[0028] Unless otherwise specified, the terms "combination thereof" and "mixture thereof" refer to a multi-component mixture of the elements, such as a two-component mixture, a three-component mixture, a four-component mixture and the maximum possible multi-component mixture.

[0029] In addition, if the number of parts or components of the present invention is not indicated before, it means that there is no limit to the number of occurrences (or existence) of the parts or components. Therefore, it should be interpreted as including one or at least one, and the singular form of the parts or components also includes the plural form, unless the numerical value obviously represents the singular.

[0030] As used herein, the term "optional" or "optionally" means that the subsequently described event or circumstance may or may not occur, and that the description includes both occurring and not occurring of said event or circumstance.

[0031] The term "alkyl" refers to a straight or branched saturated aliphatic hydrocarbon group consisting of carbon atoms and hydrogen atoms, which is connected to the rest of the molecule by a single bond. The alkyl group described herein generally has about 1-20 carbon atoms, preferably about 1-10 carbon atoms, and more preferably about 1-3 carbon atoms. Non-limiting examples thereof include, but are not limited to, methyl, ethyl, propyl, isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, n-pentyl, n-hexyl, etc.

[0032] The term "substituted" means that any one or more hydrogen atoms on a particular atom are replaced by a substituent, as long as the valence state of the particular atom is normal and the substituted compound is stable. The groups or structures herein may be optionally substituted by one or more substituents, for example, by one, two or three substituents. The substituents may be, for example, halogen, alkyl, aryl, cycloalkyl, heteroaryl, etc.

[0033] The term "repeating unit" refers to a combination of atoms linked in a certain manner on a polymer or oligomer chain, which is a basic unit constituting the polymer chain or oligomer.

[0034] The term "epoxy molding compound" used herein refers to epoxy resin molding compound and epoxy molding compound. In this article, the epoxy resin composition is used as a molding compound, so the "epoxy molding compound" is also referred to as an "epoxy resin composition".

[0035] As used herein, the term "room temperature (RT)" refers to about 25°C.

[0036] The term "molded package" means that epoxy molding compound is squeezed into the mold cavity by transfer molding, and the chip is embedded therein, and cross-linked and cured to form a semiconductor device with a certain structural appearance. Epoxy molding compound needs to have good operability, sealing and insulation properties to protect the chip and electronic circuit from damage such as external heat, cold, moisture, and chemical corrosion.

[0037] Unless otherwise defined, all terms used in the disclosure of the present invention, including technical and scientific terms, have the meanings commonly understood by those skilled in the art to which the present invention belongs. By way of further example, term definitions are included herein to better understand the teachings of the present invention.

[0038] Hereinafter, each component in the epoxy resin composition of the present invention will be described in detail.

[0039] (a) Epoxy resin

[0040] As used herein, epoxy resins contain two or more epoxy groups per molecule.

[0041] Selecting a suitable type of epoxy resin helps the product to obtain desired properties, such as suitable Tg, lower shrinkage and thermal expansion coefficient, etc. The epoxy resin of the present invention includes multifunctional epoxy resin and other epoxy resins.

[0042] Adding a multifunctional epoxy resin increases the cross-linked structure network of the epoxy resin, helps to increase the glass transition temperature of the product and give the cured product low warpage at high temperatures. In the repeating unit of the multifunctional epoxy resin, there are multiple functional group substitutions. The position of the functional group substitution can be on the main chain or the side chain, such as on the aromatic ring in the main chain, on the methylene group in the main chain, etc. The types of functional groups include but are not limited to: aromatic groups, substituted aromatic groups, epoxy groups, etc. The total number of functional groups in the repeating unit should be more than two, for example: two, three, four, etc. The functional groups in the repeating unit can be the same or different.

[0043] In one embodiment, the multifunctional epoxy resin is an epoxy resin having two or more epoxy groups in a repeating unit.

[0044] In a preferred embodiment, the multifunctional epoxy resin has the structure of the following formula (1):

[0045] Wherein, n is an integer of 3-20.

[0046] In a more preferred embodiment, the multifunctional epoxy resin has a structure as shown in the above formula (1), and n is an integer of 3-10.

[0047] Other epoxy resins contribute to the cross-linking process of the epoxy resin composition, so that the cured product has better properties, such as mechanical properties, electrical properties, etc. Other epoxy resins include, but are not limited to: o-cresol epoxy resins, bisphenol epoxy resins, biphenyl epoxy resins, dicyclopentadiene phenol epoxy resins, aralkylphenol epoxy resins, naphthol epoxy resins or combinations thereof. In one embodiment, the other epoxy resins are a combination of biphenyl epoxy resins, bisphenol epoxy resins, and dicyclopentadiene phenol epoxy resins.

[0048] The content of multifunctional epoxy resin and other epoxy resins should be maintained within a suitable range so that the product has a high Tg, a low thermal expansion coefficient, good continuous formability, etc. If the content of multifunctional epoxy resin or other epoxy resins is too high, the spiral flow length of the product will be reduced and the fluidity will be poor; if the content is too low, the glass transition temperature of the product will be reduced and the degree of warping will increase. Based on the total weight of the epoxy resin composition, the content of multifunctional epoxy resin is about 0.01-4% by weight, for example: about 1.00% by weight, about 1.50% by weight, about 2.00% by weight. Based on the total weight of the epoxy resin composition, the content of other epoxy resins is about 0.01-6% by weight, for example: about 3.50% by weight, about 5.16% by weight, about 6.00% by weight.

[0049] The total content of the epoxy resin should be maintained within a certain range to help give the product suitable fluidity, wettability, adhesion, water resistance and mechanical properties, etc. Based on the total weight of the epoxy resin composition, the total content of the epoxy resin in the epoxy resin composition of the present invention can be about 1-12% by weight, preferably about 4-10% by weight, such as about 4.50% by weight, about 6.76% by weight, about 8% by weight.

[0050] The multifunctional epoxy resin and other epoxy resins should each have a relatively low viscosity, so as to help increase the amount of filler that can be added, especially the amount of high dielectric filler that can be added, while ensuring that the epoxy resin composition has sufficient fluidity and wettability, thereby increasing the dielectric constant of the epoxy resin composition. In one embodiment, the viscosity of the multifunctional epoxy resin is about 0.2-2P, for example, 0.2-1P. In another embodiment, the viscosity of the other epoxy resins is about 0.01-1.5P, for example, about 0.01-1P, about 0.1-1P.

[0051] (b) Phenolic resin

[0052] The phenolic resin used in the epoxy resin composition of the present invention contains at least two hydroxyl groups per molecule. The phenolic resin of the present invention is mainly used as a curing agent and has a linear chain structure. The hydroxyl group can react with the epoxy resin to form a cross-linked network structure. The phenolic resin of the present invention includes biphenyl type phenolic resin and other phenolic resins.

[0053] Other phenolic resins that can be used in the present invention include, but are not limited to, phenol formaldehyde type phenolic resins, o-cresol type resins, aralkylphenol type phenolic resins, hydroxybenzaldehyde type phenolic resins, multifunctional phenolic resins, and combinations thereof.

[0054] In one embodiment, the other phenolic resin is a multifunctional phenolic resin. Adding a multifunctional phenolic resin can increase the cross-linked structure network of the epoxy resin, help to increase the glass transition temperature of the product and give the cured product low warpage at high temperatures. In the repeating unit of the multifunctional phenolic resin, there are multiple functional group substitutions. The position of the functional group substitution can be on the main chain or the side chain, such as on the aromatic ring in the main chain, on the methylene in the main chain, etc. The types of functional groups include but are not limited to: aryl, substituted aryl, phenolic hydroxyl, etc. The total number of functional groups in the repeating unit should be two or more, for example: two, three, four, etc. The functional groups in the repeating unit may be the same or different. In one embodiment, the multifunctional phenolic resin is a phenolic resin having more than two phenolic hydroxyl groups in the repeating unit.

[0055] In a preferred embodiment, the multifunctional phenolic resin is a phenolic resin having the following formula (2):

[0056]

[0057] Wherein, n is an integer of 3-20, preferably 3-10; m is an integer of 3-20, preferably 3-10.

[0058] The content of biphenyl phenolic resin and other phenolic resins should be maintained within a suitable range so that the product has a high Tg, a low thermal expansion coefficient, good curing properties, etc. If the content of biphenyl phenolic resin or its phenolic resin is too high, the spiral flow length of the product is reduced and the fluidity is deteriorated; if the content is too low, the glass transition temperature of the product is reduced. Based on the total weight of the epoxy resin composition, the content of biphenyl phenolic resin is about 0.01-4% by weight, for example: about 1.00% by weight, about 1.50% by weight, about 2.00% by weight. Based on the total weight of the epoxy resin composition, the content of other phenolic resins is about 0.01-4% by weight, for example: about 0.40% by weight, about 0.60% by weight, about 0.80% by weight.

[0059] The total content of the phenolic resin should be maintained within a certain range so that the obtained composition has good curing properties. Too high a total amount of the phenolic resin will reduce the gelation time and fluidity, and too low a total amount of the phenolic resin will not easily obtain the desired effect. In one embodiment, based on the total weight of the epoxy resin composition, the total content of the phenolic resin is about 1-8% by weight, preferably about 1-5% by weight, such as about 1.40% by weight, about 2.10% by weight, about 2.80% by weight.

[0060] The biphenyl type phenolic resin and other phenolic resins should each have a relatively low viscosity, so as to help increase the amount of filler that can be added, especially the amount of high dielectric filler that can be added, while ensuring that the phenolic resin composition has good curing properties, thereby increasing the dielectric constant of the epoxy resin composition. In one embodiment, the viscosity of the biphenyl type phenolic resin is about 0.5-2P. In another embodiment, the viscosity of the other phenolic resins is about 0.2-10P, for example, about 0.5-8P.

[0061] By regulating the composition, viscosity and content of epoxy resin and phenolic resin, the obtained product can maintain a low content of low dielectric filler, increase the addition amount of high dielectric filler, and at the same time maintain good flow properties of the product. The increase in the content of high dielectric filler can give the product a higher dielectric constant, which is beneficial to the subsequent use of the product.

[0062] (c) Curing accelerator

[0063] As used herein, the term "curing accelerator" has the same meaning as "catalyst", which can catalyze or promote the cross-linking reaction between epoxy resin and phenolic resin to form a spatial network structure without affecting the curing performance.

[0064] The preferred curing accelerator of the present invention helps to achieve a suitable curing speed of the epoxy resin composition to meet a sufficient degree of curing while taking into account the necessary fluidity and wettability during injection molding and filling. The curing accelerator of the present invention can be selected from, including but not limited to, organophosphorus compounds, amines, amidine compounds, imidazole compounds or combinations thereof, preferably organophosphorus compounds.

[0065] Based on the total weight of the epoxy resin composition, the content of the curing accelerator is about 0.1-1 wt %, for example, about 0.27 wt %, about 0.24 wt %, or about 0.21 wt %.

[0066] filler

[0067] Fillers added to epoxy resin compositions help improve the properties of epoxy resin compositions, such as thermal expansion, wear resistance, moisture resistance, thermal conductivity, electrical properties, etc. The type, content, and size of fillers can be selected to impart appropriate properties to the product.

[0068] According to the difference in dielectric constant of filler materials, fillers can be divided into high dielectric fillers and low dielectric fillers. Generally, when the dielectric constant of fillers is higher than the dielectric constant of Si3N4 (about 7), it is called high dielectric filler; when the dielectric constant of fillers is lower than the dielectric constant of SiO2 (about 3.9), it is called high dielectric filler.

[0069] The particle size of the filler should meet certain requirements to ensure the fluidity of the epoxy resin composition and the coating of the surface filler particles by the resin. Adding a small-sized filler helps to obtain a product with low warpage. If the filler size is too large, the coating of the filler by the resin will deteriorate, affecting the use of the final product. The maximum particle size of the high dielectric filler should be about 5-20 μm, preferably about 20 μm. The maximum particle size of the low dielectric filler should be about 1-20 μm, preferably about 20 μm.

[0070] Selecting a suitable amount of filler is beneficial to improving product performance. If the filler content is too high, the flowability of the product will deteriorate, which is not conducive to subsequent processing; if the filler content is too low, the thermal expansion coefficient of the product will increase, the shrinkage rate will increase, the low warpage will be lost, and the water absorption rate will increase. In one embodiment, based on the total weight of the epoxy resin composition, the total content of the high dielectric filler and the low dielectric filler is about 75-95% by weight, for example, about 85% by weight, about 86% by weight, about 86.5% by weight, about 88% by weight, about 87% by weight, about 90% by weight, about 93% by weight.

[0071] (d) High dielectric filler

[0072] Adding high dielectric fillers can significantly improve the electrical properties of products and increase the dielectric constant of products. The selection of the appropriate type and content of high dielectric constant can be combined with other components in the epoxy resin composition (such as epoxy resin, phenolic resin, curing accelerator, low dielectric filler, etc.) to achieve products with high dielectric, high wear resistance, moisture resistance, and high thermal conductivity.

[0073] In the present invention, the high dielectric material may be titanate, including but not limited to: barium titanate, strontium titanate, calcium titanate, magnesium titanate or a combination thereof. In a preferred embodiment, the high dielectric filler is barium titanate.

[0074] The content of titanate needs to be maintained within a suitable range to give the product excellent performance. If the content of added titanate is too high, the flow properties of the product will deteriorate, which is not conducive to subsequent processing and the cost will increase significantly; if the content of titanate is too low, the dielectric constant of the product will decrease, and the high dielectric properties will be lost, which is not conducive to use in the AiP field. In the present invention, based on the total weight of the epoxy resin composition, the content of titanate is 25-95% by weight, preferably 40-90% by weight, and more preferably 45-75% by weight, for example: about 50% by weight, about 70% by weight, about 80% by weight, about 90% by weight, about 93% by weight.

[0075] Adding different types of high dielectric fillers can better improve the performance of the epoxy resin composition, such as moisture resistance, wear resistance, mechanical properties, etc. after curing. Selecting different types of high dielectric fillers for combined use can better balance the various properties of the product to meet actual needs and reduce production costs. In one embodiment, the high dielectric filler also contains a transition metal oxide. Adding a transition metal oxide can obtain a product with high dielectric properties under the premise of a lower total addition amount of the high dielectric filler, and can reduce production costs. In a preferred embodiment, the transition metal oxide selected by the high dielectric filler of the present invention is iron oxide, titanium oxide or a combination thereof.

[0076] The content of transition metal oxide needs to be maintained within a suitable range. If the content of transition metal oxide is too high, the fluidity of the product will be significantly reduced, which is not conducive to subsequent processing and use. The content of transition metal oxide is 0.1-17% by weight, for example: about 5% by weight, about 10% by weight, about 15% by weight.

[0077] The content of titanium oxide and iron oxide in the transition metal oxide should be maintained within a suitable range. When the content of titanium oxide or iron oxide is too high, the flowability of the product will be significantly reduced. Based on the total weight of the epoxy resin composition, the content of titanium oxide is 0.1-12% by weight, for example, about 5% by weight, 10% by weight. Based on the total weight of the epoxy resin composition, the content of iron oxide is 0.1-7% by weight, for example, about 5% by weight.

[0078] In a high dielectric filler, when the ratio of the weight of the titanate to the weight of the transition metal oxide is too low, the content of the transition metal oxide is relatively too high, the fluidity of the product is significantly reduced, the viscosity is increased, the gelation time is shortened, and the spiral flow length is reduced, which is not conducive to the subsequent processing and use of the product. In the present invention, the ratio of the weight of the titanate to the weight of the transition metal oxide is above 3, for example: about 3.33, about 5, about 6, about 14. When the ratio of the weight of the titanate to the weight of the transition metal oxide is too high, the production cost will increase. The ratio of the weight of the titanate to the weight of the transition metal oxide can be below 15, preferably below 10.

[0079] The total content of the high dielectric filler needs to be maintained within a reasonable range to achieve high dielectric properties of the product. In one embodiment, based on the total weight of the epoxy resin composition, the content of the high dielectric filler is about 30-95% by weight, preferably 45-95% by weight, more preferably 55-75% by weight, for example, about 60% by weight, about 65% by weight, about 75% by weight, about 80% by weight, about 90% by weight, about 93% by weight.

[0080] (e) Low dielectric filler

[0081] The low dielectric filler can be one or more selected from the following: silicon dioxide, aluminum hydroxide, magnesium hydroxide, aluminum oxide, fumed silicon powder, etc. In one embodiment, the filler is silicon dioxide. The shape of the inorganic filler includes but is not limited to spherical, rod-shaped, angular, polygonal, irregular shapes, etc., preferably spherical. The preferred shape contributes to good compatibility between the inorganic filler and the epoxy resin, thereby obtaining a suitable spiral flow length. In a preferred embodiment, the filler is spherical silicon dioxide.

[0082] The content of low dielectric filler should be within a suitable range. If the content of low dielectric filler added is too high, due to the requirements of maintaining the fluidity and viscosity of the product, the total content of filler cannot be too high. Accordingly, the content of high dielectric filler that can be added will decrease, and the high dielectric properties of the product cannot be achieved. By rationally regulating the properties such as the type, content, and viscosity of epoxy resin and phenolic resin, it is possible to achieve the good fluidity of the product while adding a relatively low content of low dielectric filler. In one embodiment of the present invention, based on the gross weight of the epoxy resin composition, the content of the low dielectric filler component is 0-35% by weight, preferably 0-30% by weight, such as about 27% by weight, about 21.5% by weight, about 11.5% by weight, about 5% by weight. In a preferred embodiment, low dielectric filler may not be added.

[0083] The ratio of the weight of the high dielectric filler to the weight of the low dielectric filler should also be maintained within a suitable range so that the product has high dielectric, good fluidity and other properties (e.g., mechanical properties, flame retardancy, etc.). In one embodiment, the ratio of the weight of the high dielectric filler to the weight of the low dielectric filler is above 2, preferably 2-20, more preferably 2-10. For example, about 2.2, about 3.0, about 6.8, about 16.

[0084] (f) Other additives

[0085] The epoxy resin composition of the present invention may also optionally contain one or more other additives, including but not limited to ion capture agents, release agents, flame retardants, colorants, coupling agents, toughening agents. Based on the total weight of the epoxy resin composition, the content of the additives is about 0.6-9 weight %.

[0086] Ion trapping agents can be used to reduce the mobility of free ions in the epoxy resin composition. Suitable ion trapping agents are selected from metal acid salts, hydrated oxides and combinations thereof. In the present invention, the ion trapping agents include but are not limited to: Bi2O3, Al2O3, MgO, Sb2O5, ZrO and combinations thereof, preferably Al2O3, MgO or combinations thereof. Based on the total weight of the epoxy resin composition, the content of the ion trapping agent is about 0.1-1% by weight, for example, about 0.20% by weight.

[0087] The preferred release agent of the present invention helps to obtain an epoxy resin composition with sufficient fluidity, good anti-delamination performance and moisture absorption resistance. The release agent of the present invention includes but is not limited to montan wax, fatty acid ester wax, fatty acid wax, aliphatic ester wax, polyethylene wax, polypropylene wax, alkyl oligomer wax, amide wax or a combination thereof, preferably fatty acid ester wax. Based on the total weight of the epoxy resin composition, the content of the release agent is about 0.1-0.5 weight%, for example, about 0.20%.

[0088] The flame retardant is a functional auxiliary agent that can impart flame retardancy to the epoxy resin composition having a polymer matrix, including organic flame retardants and inorganic flame retardants. The flame retardant of the present invention is one or more selected from the following: metal hydroxide, zinc borate, phosphine-containing compounds, preferably metal hydroxide. Based on the total weight of the epoxy resin composition, the content of the flame retardant is about 0.1-5% by weight, such as about 1.0% by weight, about 1.5% by weight, about 2.0% by weight, about 3.0% by weight.

[0089] The coupling agent can improve the compatibility between the components of the epoxy resin composition on the one hand, and also provide a function of promoting bonding on the other hand. The coupling agent of the present invention is selected from trimethoxysilane, mercaptopropyl trimethoxysilane, phenylaminopropyl trimethoxysilane, glycidyl ether propyl trimethoxysilane and a combination thereof. Based on the total weight of the epoxy resin composition, the content of the coupling agent is about 0.1-1% by weight, for example, about 0.20% by weight.

[0090] Colorant is a substance that imparts color to the epoxy resin composition, and it should have good dispersibility, weather resistance, thermal stability, and chemical stability. The colorant of the present invention is selected from carbon black, iron yellow, and a combination thereof. Based on the total weight of the epoxy resin composition, the content of the colorant is about 0.1-0.5 weight %, such as about 0.2 weight %, about 0.23 weight %, about 0.24 weight %.

[0091] Tougheners can reduce the brittleness and cracking of materials, and improve their toughness, fatigue resistance and bearing strength. Commonly used epoxy resin tougheners can be reactive tougheners or non-reactive tougheners. Tougheners of the present invention include, but are not limited to, epoxy silane epoxy resins, epoxy silicone glycidyl resins, carboxyl-terminated nitrile rubbers or combinations thereof. Based on the gross weight of the epoxy resin composition, the content of the toughener is about 0.1-1% by weight, for example, about 0.15% by weight.

[0092] Epoxy resin composition

[0093] The present invention relates to an epoxy resin composition, which comprises, based on the total weight of the epoxy resin composition:

[0094] (a) 1-12% by weight of epoxy resin,

[0095] (b) 1-8% by weight of phenolic resin,

[0096] (c) 0.1-1% by weight of a curing accelerator,

[0097] (d) 30-95% by weight of a high dielectric filler,

[0098] (e) 0-60 wt% of a low dielectric filler, and

[0099] (f) 0.6-9 wt% of one or more additives selected from the following: 0.1-1 wt% ion capture agent; 0.1-0.5 wt% release agent; 0.1-5 wt% flame retardant; 0.1-0.5 wt% colorant; 0.1-1 wt% coupling agent; 0.1-1 wt% toughening agent.

[0100] It should be understood that the content of each component should be reasonably selected so that the sum of all components in the product is 100%.

[0101] For example, in a preferred embodiment, based on the total weight of the epoxy resin composition, the epoxy resin composition contains: 4.0 wt% of MAR epoxy resin, 1.0 wt% of BP epoxy resin, 1.0 wt% of DCPD epoxy resin, 2.0 wt% of multifunctional epoxy resin, 2.0 wt% of MAR phenolic resin, 0.8 wt% of multifunctional phenolic resin, 0.21 wt% of curing accelerator, 27.00 wt% of spherical silica A, 5.0 wt% of iron oxide, 5.0 wt% of titanium oxide, 50.00 wt% of barium titanate, 0.20 wt% of ion capture agent, 0.20 wt% of release agent, 1.0 wt% of flame retardant, 0.20 wt% of coupling agent, 0.24 wt% of colorant, and 0.15 wt% of toughening agent.

[0102] In another preferred embodiment, based on the total weight of the epoxy resin composition, the epoxy resin composition contains: 4.0 wt% of MAR epoxy resin, 1.0 wt% of BP epoxy resin, 1.0 wt% of DCPD epoxy resin, 2.0 wt% of multifunctional epoxy resin, 2.0 wt% of MAR phenolic resin, 0.8 wt% of multifunctional phenolic resin, 0.21 wt% of curing accelerator, 21.50 wt% of spherical silica A, 5.0 wt% of iron oxide, 10.0 wt% of titanium oxide, 50.00 wt% of barium titanate, 0.20 wt% of ion capture agent, 0.20 wt% of release agent, 1.5 wt% of flame retardant, 0.20 wt% of coupling agent, 0.24 wt% of colorant, and 0.15 wt% of toughening agent.

[0103] In another preferred embodiment, based on the total weight of the epoxy resin composition, the epoxy resin composition contains: 4.0 wt% of MAR epoxy resin, 1.0 wt% of BP epoxy resin, 1.0 wt% of DCPD epoxy resin, 2.0 wt% of multifunctional epoxy resin, 2.0 wt% of MAR phenolic resin, 0.8 wt% of multifunctional phenolic resin, 0.21 wt% of curing accelerator, 11.00 wt% of spherical silica A, 5.0 wt% of titanium oxide, 70.00 wt% of barium titanate, 0.20 wt% of ion capture agent, 0.20 wt% of release agent, 2.00 wt% of flame retardant, 0.20 wt% of coupling agent, 0.24 wt% of colorant, and 0.15 wt% of toughening agent.

[0104] In another preferred embodiment, based on the total weight of the epoxy resin composition, the epoxy resin composition contains: 4.0 wt% of MAR epoxy resin, 1.0 wt% of BP epoxy resin, 1.0 wt% of DCPD epoxy resin, 2.0 wt% of multifunctional epoxy resin, 2.0 wt% of MAR phenolic resin, 0.8 wt% of multifunctional phenolic resin, 0.21 wt% of curing accelerator, 5.00 wt% of spherical silica A, 80.00 wt% of barium titanate, 0.20 wt% of ion capture agent, 0.20 wt% of release agent, 3.0 wt% of flame retardant, 0.20 wt% of coupling agent, 0.24 wt% of colorant, and 0.15 wt% of toughening agent.

[0105] In another preferred embodiment, based on the total weight of the epoxy resin composition, the epoxy resin composition contains: 3.76 wt % of MAR epoxy resin, 1.0 wt % of BP epoxy resin, 0.5 wt % of DCPD epoxy resin, 1.5 wt % of multifunctional epoxy resin, 1.5 wt % of MAR phenolic resin, 0.6 wt % of multifunctional phenolic resin, 0.19 wt % of curing accelerator, 90.00 wt % of barium titanate, 0.20 wt % of ion capture agent, 0.20 wt % of release agent, 0.20 wt % of coupling agent, 0.20 wt % of colorant, and 0.15 wt % of toughening agent.

[0106] In another preferred embodiment, based on the total weight of the epoxy resin composition, the epoxy resin composition contains: 2.50 wt% of MAR epoxy resin, 0.50 wt% of BP epoxy resin, 0.50 wt% of DCPD epoxy resin, 1.00 wt% of multifunctional epoxy resin, 1.00 wt% of MAR phenolic resin, 0.4 wt% of multifunctional phenolic resin, 0.15 wt% of curing accelerator, 93.00 wt% of barium titanate, 0.20 wt% of ion capture agent, 0.20 wt% of release agent, 0.20 wt% of coupling agent, 0.20 wt% of colorant, and 0.15 wt% of toughening agent.

[0107] It will be understood by those skilled in the art that for a composition, the sum of all ingredients thereof may be 100%.

[0108] Preparation method

[0109] The present invention also relates to a method for preparing the epoxy resin composition, which comprises the following steps:

[0110] (1) weigh each component and mix them to obtain a premixed powder,

[0111] (2) The premixed powder is heated, mixed and extruded to obtain the product.

[0112] Step (1) may also include grinding each component to a smaller size by a grinding device, such as a ball mill.

[0113] The equipment for mixing in step (1) should allow the components to be uniformly mixed. In one embodiment, a high-speed stirrer is used for mixing. The speed of mixing in step (1) is generally about 200-300 rpm. The mixing time is generally about 20-50 minutes, preferably about 30 minutes.

[0114] In step (1), the components can be added together or one by one into the mixing device.

[0115] The equipment for heating and mixing in step (2) needs to allow each component to be evenly heated and mixed. In one embodiment, an extruder is used for mixing. The extruder includes but is not limited to a single-screw extruder and a twin-screw extruder, preferably a twin-screw extruder. In one embodiment, the extrusion temperature of step (2) is about 90-110° C., and the screw speed is about 220 rpm.

[0116] In one embodiment, step (2) further comprises cooling, crushing and post-mixing after extrusion. In another embodiment, a crusher is used for crushing. In another embodiment, a post-mixing is used for post-mixing.

[0117] performance

[0118] The epoxy resin composition of the present invention has a suitable spiral flow length so that the product has good fluidity and filling properties. The spiral flow length can be tested using a spiral flow measurement mold. According to EMI-1-66, a spiral flow measurement mold is used at a molding temperature of 175°C and a pressure of 70 kg / cm 2 The measurement is carried out under the conditions of injection molding pressure and 90 seconds curing time. The flow ability during injection molding is characterized by the length of the resin flowing along the path of the spiral cavity. In one embodiment, the epoxy resin composition of the present invention is cured at 175° C. for about 90 seconds with a spiral flow length of about 40 inches or more, for example, about 47 inches, about 45 inches, about 46 inches, about 50 inches, or about 43 inches.

[0119] The epoxy resin composition of the present invention has a suitable gelation time. The gelation time can be determined by measuring the time from when the powder sample of the epoxy molding compound is placed on a heating plate to gelation by a timer. The epoxy resin composition is placed on a curing plate heated to a certain temperature, and a stopwatch is used for timing. The sample is stirred evenly using the front section of a scraper. The stopwatch is stopped when the sample gels, and the time is recorded as the gelation time at the temperature. In one embodiment, the gelation time of the epoxy resin composition of the present invention at 175° C. is 30-50 seconds, for example, about 38 seconds, about 37 seconds, about 36 seconds, or about 33 seconds.

[0120] The epoxy resin composition of the present invention has a high thermal hardness, so that the epoxy resin composition can be easily separated from the mold, and has good continuous molding performance and can be injection molded at a higher temperature. The test method for thermal hardness is to measure the cured sample using a hardness meter. Shore hardness, Brinell hardness, Rockwell hardness, etc. can be used. In one embodiment, the thermal hardness of the epoxy resin composition of the present invention is about Shore 60-90 when cured at about 175°C for about 90s, for example, about Shore 81, 80, 76, 77, 79.

[0121] The epoxy resin composition of the present invention has a suitable viscosity. The viscosity test can be measured, for example, by the following method: using a capillary rheometer, model Shimadzu CFT-500D, at 175±2°C, with a load of 10 kgf. In one embodiment, the viscosity of the epoxy resin composition of the invention is below 30 Pa.s, preferably below 20 Pa.s, for example, about 17 Pa.s, about 20 Pa.s, about 9 Pa.s, about 16 Pa.s, about 25 Pa.s, about 12 Pa.s.

[0122] The epoxy resin composition of the present invention has high dielectric properties and has a relatively high dielectric constant. At room temperature, the dielectric constant is measured using a dielectric constant tester. In one embodiment, the dielectric constant of the epoxy resin composition of the present invention is 8 or more, preferably 10 or more, such as about 12, about 15, about 18, about 20, about 26, about 28.

[0123] The epoxy resin composition of the present invention has good flame retardancy. The test is performed using a vertical combustion apparatus of model CZF-01, and the sample thickness can be selected as 0.25 inches or 0.125 inches as required. In one embodiment, the test sample thickness is 0.125 inches, and the epoxy resin composition of the present invention can pass the UL-94 standard, and the flame retardancy grade is V-0.

[0124] Beneficial Effects

[0125] In the present invention, the dielectric constant of epoxy resin can be increased by adding high dielectric fillers. For example, by adding titanate, the dielectric constant of the product is increased. By adding transition metal oxides, the cost can be reduced while maintaining a high dielectric constant.

[0126] On the other hand, by adding a low-viscosity resin, the amount of high-dielectric filler that can be added can be increased, and the dielectric constant of the obtained high-dielectric epoxy resin composition is high. In addition, the composition of the present invention has good fluidity and high hardness, which meets the requirements of AiP. The epoxy resin composition of the present invention has the advantages of high dielectric constant, flame retardancy and environmental protection, simple process, and easy industrial application, and can be used for AiP packaging.

[0127] Example

[0128] The solution of the present invention is further described in detail below in conjunction with specific embodiments.

[0129] It should be noted that the following examples are merely examples for clearly illustrating the technical solutions of the present invention, and are not intended to limit the present invention. For those skilled in the art, other different forms of changes or modifications can be made based on the above description, and it is not necessary and impossible to exhaustively list all the embodiments here, and the obvious changes or modifications derived therefrom are still within the scope of protection of the present invention. Unless otherwise specified, the instruments, equipment, and reagents used herein are all commercially available.

[0130] Epoxy resin:

[0131] Multifunctional epoxy resin: epoxy resin (MFN), having the following structure (2):

[0132]

[0133] Wherein n is an integer of 3-10; viscosity 0.2-1P;

[0134] Other epoxy resins: biphenyl type (MAR) epoxy resin, viscosity 0.01-1P;

[0135] Bisphenol (BP) epoxy resin, viscosity 0.01-1P;

[0136] Dicyclopentadiene phenol type (DCPD) epoxy resin, viscosity 0.1-1P.

[0137] Phenolic resin:

[0138] Multifunctional phenolic resin: phenolic resin (MFN), having the following structure (2):

[0139]

[0140] Wherein n is an integer of 3-10; m is an integer of 3-10; viscosity is 0.5-8P;

[0141] Biphenyl type phenolic resin (MAR), viscosity 0.5-2P.

[0142] Low dielectric filler: spherical silica A, maximum particle size 20μm, D90 particle size 10μm;

[0143] Spherical silica B, D90 particle size is 1-2μm.

[0144] High dielectric fillers: iron oxide, titanium oxide, barium titanate, with a maximum particle size of 20μm.

[0145] Ion scavenger: combination of Al2O3 and MgO.

[0146] Release agent: a combination of montan wax and fatty acid ester wax, purchased from Klein Company.

[0147] Flame retardant: metal hydroxide.

[0148] Coupling agent: trimethoxysilane, mercaptopropyltrimethoxysilane, phenylaminopropyltrimethoxysilane.

[0149] Colorant: Carbon black, purchased from Orion.

[0150] Toughening agent: carboxyl-terminated nitrile rubber, purchased from Corning;

[0151] composition

[0152] The compositions of Comparative Examples 1-3 are shown in Table 1, and the compositions of Examples 1-7 are shown in Table 2. The content of each component is based on the total weight of the epoxy resin composition.

[0153] Table 1

[0154] Material Type Comparative Example 1 Comparative Example 2 Comparative Example 3 Comparative Example 4 Epoxy resin (MAR) 4.00 4.00 4.00 4.00 Epoxy resin (BP) 1.00 1.00 1.00 1.00 Epoxy resin (DCPD) 1.00 1.00 1.00 1.00 Epoxy resin (MFN) 2.00 2.00 2.00 2.00 Phenolic resin (MAR) 2.00 2.00 2.00 2.00 Phenolic resin (MFN) 0.80 0.80 0.80 0.80 Curing accelerator 0.25 0.25 0.21 0.22 Spherical Silica A 83.00 10 16.50 53.00 Spherical Silica B 5.00 - - - Alumina 78 - Iron Oxide - - 5 - Titanium oxide - - 15.00 5.00 Barium Titanate - - 50.00 30.00 Ion Scavenger 0.20 0.20 0.20 0.20 Release agent 0.20 0.20 0.20 0.20 Flame retardants - - 1.50 - Coupling agent 0.20 0.20 0.20 0.20 Colorants 0.20 0.20 0.24 0.23 Toughening agent 0.15 0.15 0.15 0.15

[0155] Table 2

[0156] Material Type Example 1 Example 2 Example 3 Example 4 Example 5 Example 6 Epoxy resin (MAR) 4.00 4.00 4.00 4.00 3.76 2.50 Epoxy resin (BP) 1.00 1.00 1.00 1.00 1.00 0.50 Epoxy resin (DCPD) 1.00 1.00 1.00 1.00 0.50 0.50 Epoxy resin (MFN) 2.00 2.00 2.00 2.00 1.50 1.00 Phenolic resin (MAR) 2.00 2.00 2.00 2.00 1.50 1.00 Phenolic resin (MFN) 0.80 0.80 0.80 0.80 0.60 0.40 Curing accelerator 0.21 0.21 0.21 0.21 0.19 0.15 Spherical Silica A 27.00 21.50 11.00 5.00 - - Iron Oxide 5.00 5.00 - - - - Titanium oxide 5.00 10.00 5.00 - - - Barium Titanate 50.00 50.00 70.00 80.00 90.00 93.00 Ion Scavenger 0.20 0.20 0.20 0.20 0.20 0.20 Release agent 0.20 0.20 0.20 0.20 0.20 0.20 Flame retardants 1.00 1.50 2.00 3.00 - - Coupling agent 0.20 0.20 0.20 0.20 0.20 0.20 Colorants 0.24 0.24 0.24 0.24 0.20 0.20 Toughening agent 0.15 0.15 0.15 0.15 0.15 0.15

[0157] preparation

[0158] Comparative Example 1

[0159] 83 parts of spherical silica A, 5 parts of spherical silica B and 0.2 parts of colorant are poured into a high-speed mixer and stirred for 10 minutes. 0.2 parts of coupling agent are slowly added and stirred for 10 minutes. Then, 4 parts of epoxy resin (MAR), 1 part of epoxy resin (BP), 1 part of epoxy resin (DCPD), 2 parts of epoxy resin (MFN), 2 parts of phenolic resin (MAR), 0.8 parts of phenolic resin (MFN), 0.25 parts of curing accelerator, 0.2 parts of ion capture agent and 0.2 parts of release agent are added and stirred for 3 minutes. Then, 0.15 parts of toughening agent are added and stirred for 30 minutes to obtain a premix. The premix is ​​heated, mixed and extruded by an extruder at a set temperature (80° C., 100° C., 100° C., 60° C., 80° C.), a feeding speed of 9 rpm, a main engine speed of 220 rpm and a blade pair of 26 pairs, and is rapidly cooled and crushed to obtain a powdery product.

[0160] Comparative Examples 2-4 were obtained according to their respective compositions by the same preparation operation as the above Comparative Example 1.

[0161] Example 1

[0162] 27 parts of spherical silica A, 5 parts of titanium oxide, 5 parts of iron oxide, 50 parts of barium titanate, and 0.24 parts of colorant were poured into a high-speed mixer and stirred for 10 minutes. 0.2 parts of coupling agent were slowly added and stirred for 10 minutes. Then, 4 parts of epoxy resin (MAR), 1 part of epoxy resin (BP), 1 part of epoxy resin (DCPD), 2 parts of epoxy resin (MFN), 2 parts of phenolic resin (MAR), 0.8 parts of phenolic resin (MFN), 0.21 The premix was prepared by mixing 0.15 parts of a curing accelerator, 0.2 parts of an ion capture agent, 0.2 parts of a release agent, and 1.00 parts of a flame retardant, and stirring for 3 minutes, then adding 0.15 parts of a toughening agent and stirring for 30 minutes to obtain a premix; the premix was heated, mixed, and extruded through an extruder at set temperatures (80°C, 100°C, 100°C, 60°C, 80°C), a feeding speed of 9 rpm, a main engine speed of 220 rpm, and 26 pairs of blades, and quickly cooled and crushed to obtain a powdery product.

[0163] Examples 2-6 were obtained according to their respective compositions by adopting the same preparation operation as the above-mentioned Example 1.

[0164] test

[0165] The various properties of the epoxy resin composition obtained were tested according to the following test methods, and the results are shown in Table 3 below.

[0166] Spiral flow length: According to EMI-1-66, spiral flow measurement mold is used at 175℃ molding temperature and 70kg / cm 2 The measurements were performed under injection pressure and 90 s curing time.

[0167] Gel time: Place the epoxy resin composition on a curing plate heated to 175°C, use a stopwatch to time, use the front end of a scraper to evenly stir the sample, and stop the stopwatch when the sample gels. This time is the gel time.

[0168] Shore D hardness: The sample cured at 175°C for about 90 seconds was measured using a hardness tester.

[0169] Viscosity: A Shimadzu capillary rheometer, model CFT 500D, was used with measurement parameters of 175°C and a load of 10 kgf.

[0170] Dielectric constant: Use dielectric constant tester, model QBG-3D, test frequency: 25KHz ~ 50MHz.

[0171] Flame retardancy: The flame retardancy test was conducted using the UL-94 method, with the sample thickness set to 0.125 inches. The test instrument was a vertical combustion instrument, model CZF-01.

[0172] Table 3

[0173]

[0174] Adding high dielectric fillers can increase the dielectric constant of the product, making the product have high dielectric properties. Compared with comparative example 1, the dielectric constants of the samples of Examples 1-6 are significantly increased with the use of high dielectric fillers, all of which are above 12.

[0175] From the test results of Comparative Example 2, it can be seen that after adding alumina, the dielectric properties of Comparative Example 2 are improved compared with Comparative Example 1, but are still below 6.5. When the addition amount of alumina is 78% by weight, the dielectric properties of the product are still lower than the product with a lower addition amount of high dielectric filler of the present invention.

[0176] Adding titanate can improve the dielectric constant of the product, and increasing its content can significantly improve the dielectric constant of the product. In Examples 1-6, as the barium titanate content increases from 50 wt % to 93 wt %, the dielectric constant of the product increases to 28.

[0177] Adding an appropriate amount of oxide can maintain the high dielectric properties and good fluidity of the product and reduce the production cost. In Example 1-2, by adding iron oxide and titanium oxide, the content of barium titanate is reduced compared to Example 3-6, but the dielectric constant of the product is still above 12, and the spiral flow length is above 45 inches, and the viscosity is below 20 Pa.s, which has both high dielectric properties and good fluidity, while reducing production costs.

[0178] In Comparative Example 3, the content of titanium oxide in the high dielectric filler is too high, and the weight ratio of barium titanate to metal oxide is 2.5. The viscosity of the product increases to 32 Pa.s, and the fluidity becomes poor, which is not conducive to subsequent use.

[0179] By selecting appropriate components and contents in the epoxy resin, when the addition amount of the low dielectric filler silicon dioxide is below 30 weight %, the obtained product still has very good fluidity and high dielectric properties.

[0180] By selecting the appropriate composition type and content, the epoxy resin composition of the present invention has excellent performance, and has the advantages of high dielectric and good fluidity. By adding a suitable content of high dielectric filler, the dielectric constant of the product is increased, and it has high dielectric properties. By adding a low-viscosity resin, the amount of ultrafine high dielectric filler that can be added is increased, and the dielectric constant of the obtained high dielectric epoxy resin composition is high, meeting the requirements of AiP. The epoxy resin composition of the present invention has the advantages of high dielectric constant, flame retardant and environmental protection, simple process, and easy industrial application, and can be used for AiP packaging.

[0181] Those skilled in the art will recognize or be able to determine many equivalents of the specific embodiments of the invention described herein using no more than routine experimentation. The appended claims are intended to cover such equivalents. It will be clear to those skilled in the art that many modifications and variations of the present invention may be made without departing from its spirit and scope. The specific embodiments described herein are provided by way of example only and are not intended to be limited in any way. The true scope and spirit of the present invention are shown by the appended claims, and the description and examples are exemplary only.

Claims

1. An epoxy resin composition, wherein Based on the total weight of the epoxy resin composition, the epoxy resin composition comprises: (a) 1-12% by weight of epoxy resin, (b) 1-8% by weight of a phenolic resin, (c) 0.1-1% by weight of a curing accelerator, (d) 30-95% by weight of a high dielectric filler, (e) 5-35 wt % of a low dielectric filler; The high dielectric filler comprises titanate and transition metal oxide; in, The titanate is selected from barium titanate, strontium titanate, calcium titanate, lead titanate and combinations thereof; The transition metal oxide is selected from iron oxide, titanium oxide and combinations thereof; The ratio of the weight of the titanate to the weight of the transition metal oxide is 3-15; The spiral flow length of the epoxy resin composition is greater than 40 inches.

2. The epoxy resin composition according to claim 1, wherein The titanate is barium titanate.

3. The epoxy resin composition according to claim 1, wherein Based on the total weight of the epoxy resin composition, The content of the titanate is 25-95% by weight; and / or The content of the transition metal oxide is 0.1-17 wt %.

4. The epoxy resin composition according to claim 1, wherein Based on the total weight of the epoxy resin composition, The content of titanium oxide in the transition metal oxide is 0.1-12% by weight; and / or The content of iron oxide in the transition metal oxide is 0.1-7% by weight.

5. The epoxy resin composition according to claim 1, wherein The epoxy resin comprises a multifunctional epoxy resin and other epoxy resins, wherein the other epoxy resins are selected from o-cresol epoxy resins, bisphenol epoxy resins, biphenyl epoxy resins, dicyclopentadiene phenol epoxy resins, aralkylphenol epoxy resins, naphthol epoxy resins and combinations thereof; and / or The phenolic resin comprises biphenyl phenolic resin and other phenolic resins, wherein the other phenolic resins are selected from phenol formaldehyde phenolic resin, o-cresol phenolic resin, aralkylphenol phenolic resin, hydroxybenzaldehyde phenolic resin, multifunctional phenolic resin and combinations thereof; and / or The low dielectric filler is selected from silicon dioxide, aluminum hydroxide, magnesium hydroxide, aluminum oxide, fumed silicon powder and combinations thereof; and / or The curing accelerator is selected from organic phosphorus compounds, amines, amidine compounds, imidazole compounds and combinations thereof.

6. The epoxy resin composition according to claim 5, wherein The low dielectric filler is silicon dioxide.

7. The epoxy resin composition according to claim 5, wherein The low dielectric filler is spherical silica.

8. The epoxy resin composition according to claim 5, wherein Based on the total weight of the epoxy resin composition, The content of the multifunctional epoxy resin is 0.01-4% by weight; and / or The content of the other epoxy resin is 0.01-8% by weight; and / or The content of the biphenyl phenolic resin is 0.01-4% by weight; and / or The other phenolic resin is 0.01-4% by weight.

9. The epoxy resin composition according to claim 5, wherein The viscosity of the multifunctional epoxy resin is 0.2-2 P; and / or The viscosity of the other epoxy resin is 0.01-1.5 P; and / or The viscosity of the biphenyl phenolic resin is 0.5-2 P; and / or The viscosity of the other phenolic resin is 0.5-10 P.

10. The epoxy resin composition according to claim 1, wherein The maximum particle size of the high dielectric filler is 5-20 μm; and / or The maximum particle size of low dielectric fillers is 1-20 μm.

11. The epoxy resin composition according to claim 1, wherein Based on the total weight of the epoxy resin composition, the total content of the high dielectric filler and the low dielectric filler is 75-95% by weight; and / or The ratio of the weight of the high dielectric filler to the weight of the low dielectric filler is 2 or more.

12. The epoxy resin composition according to claim 1, wherein The epoxy resin composition further comprises one or more (f) additives selected from the following: ion capture agent, mold release agent, flame retardant, coupling agent, colorant, toughening agent; wherein, The ion capture agent is selected from: Bi2O3, Al2O3, MgO, Sb2O5, ZrO and combinations thereof; and / or The release agent is selected from the group consisting of: montan wax, fatty acid ester wax, fatty acid wax, aliphatic ester wax, polyethylene wax, polypropylene wax, alkyl oligomer wax, amide wax and combinations thereof; and / or The flame retardant is selected from: metal hydroxides, zinc borates, phosphine-containing compounds and combinations thereof; and / or The coupling agent is selected from: trimethoxysilane, mercaptopropyl trimethoxysilane, phenylaminopropyl trimethoxysilane, glycidyl ether propyl trimethoxysilane and combinations thereof; and / or The colorant is selected from: carbon black, iron yellow and combinations thereof; and / or The toughening agent is selected from the group consisting of epoxy silane epoxy resin, epoxy silicone glycidyl resin, carboxyl-terminated nitrile rubber and combinations thereof.

13. The epoxy resin composition according to claim 12, wherein The ion capture agent is Al2O3, MgO or a combination thereof; and / or The release agent is aliphatic ester wax; and / or The flame retardant is a metal hydroxide; and / or The colorant is carbon black; and / or The toughening agent is carboxyl-terminated nitrile rubber.

14. The epoxy resin composition according to any one of claims 1 to 13, wherein The epoxy resin composition has one or more of the following properties: (1) Dielectric constant is greater than 8; (2) Viscosity below 30 Pa.s.

15. The epoxy resin composition according to any one of claims 1 to 13, wherein The epoxy resin composition has one or more of the following properties: (1) The dielectric constant is greater than 10; (2) The viscosity is below 20 Pa.S.

16. A method for preparing the epoxy resin composition according to any one of claims 1 to 15, comprising the following steps: (1) weigh each component and mix them to obtain a premixed powder, (2) The premixed powder is heated, mixed and extruded to obtain a product.

17. Use of the epoxy resin composition according to any one of claims 1 to 15 in molded packaging.

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