Modified bismaleimide prepolymer, resin composition and application of resin composition

Abstract

The present invention provides a modified bismaleimide prepolymer, a resin composition and an application thereof. The modified bismaleimide prepolymer is obtained by reacting a bismaleimide compound, an amino silicone resin A and an amino silicone resin B; wherein the amino equivalent Ea of the amino silicone resin A is A <Amino equivalent Ea of the amino silicone resin B B The present invention allows the modified bismaleimide compound to react with amino silicone resin A and amino silicone resin B having different amino equivalents, thereby improving the reactivity of the bismaleimide compound and controlling the rheological properties of the modified bismaleimide prepolymer during high-temperature lamination when the modified bismaleimide prepolymer is applied to the field of substrate materials such as packaging substrates.

Description

Technical Field

[0001] The present invention relates to the technical field of electronic materials, and in particular to a modified bismaleimide prepolymer, a resin composition containing the modified bismaleimide prepolymer, and applications of the resin composition. Background Art

[0002] In recent years, electronic equipment has developed towards miniaturization and high performance. The wiring density and high concentration in printed circuit boards have continued to develop, which has put forward higher requirements on the heat resistance and reliability of copper clad laminates, especially in semiconductor packaging substrates. The difference in thermal expansion coefficient between the chip and the organic substrate during packaging assembly leads to warping problems.

[0003] Bismaleimide resin cured products have excellent properties such as high temperature resistance, moisture and heat resistance, high modulus, low CTE, and high strength, and are suitable for use as the base resin of IC packaging substrates and similar substrates. However, they also have disadvantages such as high brittleness and poor processing performance, which limit their large-scale application.

[0004] In order to improve the above-mentioned problems of the cured product of bismaleimide resin in the prior art, silicone rubber powder is introduced into the bismaleimide resin. The introduction of silicone rubber powder improves the water absorption and toughness of the cured product of bismaleimide resin to a certain extent, but the silicone rubber powder has a small density, is easy to agglomerate, and has poor dispersibility. It floats on the upper layer of the bismaleimide resin glue to form a phase separation, resulting in the cured product of the bismaleimide resin being delaminated. In addition, the prior art also directly adds silicone oil to the bismaleimide resin, but in the process of curing the cured product, if the silicone oil does not react completely, it is very easy to seep out of the system, affecting the production processability and seriously affecting the comprehensive performance of the final cured product. Summary of the invention

[0005] The purpose of the present invention is to provide a modified bismaleimide prepolymer, a resin composition and an application of the resin composition. The bismaleimide compound is modified by reacting with an amino silicone resin with different amino equivalents, which not only improves the problem of high brittleness of the bismaleimide resin, but also better controls the reactivity of the bismaleimide resin and the rheological properties of the resin during high-temperature lamination.

[0006] In order to achieve one of the above-mentioned objects of the invention, one embodiment of the present invention provides a modified bismaleimide prepolymer obtained by reacting a bismaleimide compound, an amino silicone resin A and an amino silicone resin B; wherein the amino equivalent Ea of the amino silicone resin A is A <Amino equivalent Ea of the amino silicone resin B B .

[0007] As a further improvement of one embodiment of the present invention, the amino equivalent Ea of the amino silicone resin A is A 100g / mol≤Ea A ≤500g / mol, the amino equivalent Ea of the amino silicone resin B B The amino equivalent is 500g / mol<Ea B ≤1600g / mol.

[0008] As a further improvement of one embodiment of the present invention, the absolute value of the difference in amino equivalent between the amino silicone resin A and the amino silicone resin B is 100 g / mol to 600 g / mol.

[0009] As a further improvement of one embodiment of the present invention, the amino silicone resin A and the amino silicone resin B both contain the following structure:

[0010] Wherein R and R' are C1-C5 alkyl groups, and m is an integer of 1-30.

[0011] As a further improvement of one embodiment of the present invention, the amino silicone resin A and / or the amino silicone resin B contains at least one amino group on the side chain.

[0012] As a further improvement of one embodiment of the present invention, the amino silicone resin A and / or the amino silicone resin B contains at least one amino group at the terminal.

[0013] One embodiment of the present invention further provides a resin composition, comprising the following components by weight:

[0014] (a) modified bismaleimide prepolymer: 100 parts;

[0015] (b) maleimide resin: 0 to 100 parts;

[0016] (c) filler: 1 to 300 parts;

[0017] Wherein, the modified bismaleimide prepolymer is the aforementioned modified bismaleimide prepolymer.

[0018] As a further improvement of one embodiment of the present invention, the maleimide resin is selected from at least one of the following structures:

[0019]

[0020] wherein n is an integer from 1 to 10, R2 is hydrogen, methyl or ethyl, R1 is methylene, ethylene or

[0021]

[0022] Wherein, n is an integer from 1 to 10; Wherein n is an integer from 1 to 10; Wherein, n is an integer from 1 to 10;

[0023]

[0024] R is hydrogen, methyl or ethyl, and n is an integer of 1-10.

[0025] As a further improvement of one embodiment of the present invention, the filler includes an inorganic filler, an organic filler, and a composite filler. The inorganic filler is selected from at least one of fused silica, crystalline silica, spherical silica, hollow silica, aluminum hydroxide, aluminum oxide, talc, aluminum nitride, boron nitride, silicon carbide, barium sulfate, barium titanate, strontium titanate, calcium carbonate, calcium silicate, mica, and glass fiber powder; the organic filler is selected from at least one of polytetrafluoroethylene powder, polyphenylene sulfide powder, and polyether sulfone powder.

[0026] As a further improvement of one embodiment of the present invention, the filler is surface treated with a silane coupling agent, and the silane coupling agent is at least one of an aminosilane coupling agent, a carbon-carbon double bond-containing silane coupling agent, or an epoxy silane coupling agent.

[0027] As a further improvement of one embodiment of the present invention, the resin composition further comprises 5 to 50 parts of an elastomer, and the elastomer is selected from at least one of styrene elastomers, methacrylate elastomers, and silicone elastomers.

[0028] As a further improvement of one embodiment of the present invention, the resin composition also includes a flame retardant, and the flame retardant contains 5 to 50 parts by weight; the flame retardant is selected from bromide flame retardants, phosphorus flame retardants, nitrogen flame retardants, silicone flame retardants, and organic metal salt flame retardants.

[0029] One embodiment of the present invention further provides a use of the above-mentioned resin composition in a prepreg, a laminate, an insulating film, an insulating board, a copper-clad board, a circuit substrate and an electronic device.

[0030] One or more technical solutions provided by the present invention have at least the following technical effects or advantages:

[0031] The modified bismaleimide prepolymer provided by the present invention is prepared by reacting a bismaleimide compound with an amino silicone resin A having a lower amino equivalent and an amino silicone resin B having a higher amino equivalent, wherein the amino silicone resin A having a lower amino equivalent consumes part of the amino groups, slowing down the reaction rate of the bismaleimide compound and the amino silicone resin B having a higher amino equivalent, thereby improving the brittleness and reactivity of the bismaleimide compound; and controlling the rheological properties of the modified bismaleimide prepolymer during high-temperature lamination when the prepolymer is applied to the field of substrate materials such as packaging substrates. BRIEF DESCRIPTION OF THE DRAWINGS

[0032] Figure 1 The rheological curves of Example 1 and Comparative Example 2 of the present invention are shown in FIG. DETAILED DESCRIPTION

[0033] The present invention will be described in detail below in conjunction with specific embodiments, but these embodiments do not limit the present invention, and changes in reaction conditions, reactants or raw material amounts made by ordinary technicians in the field according to these embodiments are all included in the protection scope of the present invention.

[0034] The embodiment of the present invention provides a modified bismaleimide prepolymer, which is obtained by reacting a bismaleimide compound, an amino silicone resin A and an amino silicone resin B. The amino equivalent Ea of the amino silicone resin A is A <Amino equivalent Ea of amino silicone resin B B .

[0035] Specifically, the amino equivalent Ea of the amino silicone resin A is A 100g / mol≤Ea A ≤500g / mol, amino equivalent Ea of amino silicone resin B B The amino equivalent is 500g / mol<Ea B ≤1600g / mol.

[0036] The specific reaction between the bismaleimide compound, the amino silicone resin A and the amino silicone resin B is as follows:

[0037] First, the bismaleimide compound and the amino silicone resin A are reacted at 60-90° C. for 0.5-1.5 hours, and then the temperature is raised to 90-130° C., and then the amino silicone resin B is added and the reaction is continued for 0.5-2 hours.

[0038] During the reaction of the bismaleimide compound with the amino silicone resin A and the amino silicone resin B, at least one of aminophenol, carboxylic acid or carboxylic anhydride is added in an amount of 0.1 to 10 parts by weight. The phenolic hydroxyl group, carboxyl group and anhydride group in the aminophenol, carboxylic acid or carboxylic anhydride can react with the bismaleimide compound, thereby improving the reactivity.

[0039] The modified bismaleimide prepolymer provided in an embodiment of the present invention first reacts a bismaleimide compound with an amino silicone resin A with a low amino equivalent, consumes part of the amino group and the maleimide group, and forms a prepolymer with a certain molecular weight; then, an amino silicone resin B with a high amino equivalent is added to make the overall reaction proceed slowly, so that the reactivity of the bismaleimide compound and the rheological properties during high-temperature lamination can be better controlled, and a modified bismaleimide prepolymer with high heat resistance, low CTE, high Tg, low water absorption and excellent processability is obtained.

[0040] Preferably, the absolute value of the difference in amino equivalent between the silicone resin A and the silicone resin B is 100 g / mol to 600 g / mol.

[0041] Furthermore, both the amino silicone resin A and the amino silicone resin B contain the following structure:

[0042] Wherein R and R' are C1-C5 alkyl groups, and m is an integer of 1-30.

[0043] Furthermore, the amino silicone resin A and / or the amino silicone resin B contain at least one amino group on the side chain.

[0044] Furthermore, the amino silicone resin A and / or the amino silicone resin B contain at least one amino group at the terminal.

[0045] The present invention also provides a resin composition, which comprises the following components by weight:

[0046] (a) modified bismaleimide prepolymer: 100 parts;

[0047] (b) maleimide resin: 0 to 100 parts;

[0048] (c) filler: 1 to 300 parts;

[0049] Wherein, the modified bismaleimide prepolymer is the aforementioned modified bismaleimide prepolymer.

[0050] Furthermore, the maleimide resin and the bismaleimide compound in the aforementioned modified bismaleimide prepolymer can be selected from at least one of the following structures:

[0051]

[0052] R2 is hydrogen, methyl or ethyl, R1 is methylene, ethylene or n is an integer from 1 to 10;

[0053]

[0054] n is an integer from 1 to 10;

[0055] n is an integer from 1 to 10;

[0056] n is an integer from 1 to 10;

[0057]

[0058] R is hydrogen, methyl or ethyl, and n is an integer of 1-10.

[0059] The filler includes inorganic filler, organic filler and composite filler. Among them, the inorganic filler is selected from at least one of fused silica, crystalline silica, spherical silica, hollow silica, aluminum hydroxide, aluminum oxide, talc, aluminum nitride, boron nitride, silicon carbide, barium sulfate, barium titanate, strontium titanate, calcium carbonate, calcium silicate, mica and glass fiber powder. The organic filler is selected from at least one of polytetrafluoroethylene powder, polyphenylene sulfide powder and polyether sulfone powder.

[0060] Preferably, the filler content is 30 to 150 parts by weight.

[0061] Preferably, the filler is spherical silica, alumina or aluminum hydroxide, more preferably spherical silica.

[0062] Further, the filler is surface treated with a silane coupling agent, and the silane coupling agent is at least one of an aminosilane coupling agent, a carbon-carbon double bond-containing silane coupling agent, or an epoxysilane coupling agent. Preferably, the silane coupling agent is selected from the following structures:

[0063] The grades are KBM-573 manufactured by Shin-Etsu Chemical and Z-6883 manufactured by Dow Corning;

[0064] The brand name is KBM-1003 manufactured by Shin-Etsu Chemical;

[0065] The brand name is KBM-1403 manufactured by Shin-Etsu Chemical.

[0066] Furthermore, the resin composition also includes a silane coupling agent and a dispersant, the silane coupling agent is an epoxy silane coupling agent, the dispersant is a phosphate dispersant and / or a modified polyurethane dispersant, and the weight ratio of the silane coupling agent to the dispersant is 2:1 to 10:1.

[0067] Furthermore, the resin composition also includes 5 to 50 parts by weight of an elastomer, and the elastomer is selected from at least one of styrene elastomers, methacrylate elastomers, and silicone elastomers.

[0068] Among them, the styrene elastomer is selected from H1041, H1043, H1051, H1052, H1053, H1221, P1500, P2000, M1911 or M1913 of Asahi Chemical Industry of Japan; 8004, 8006, 8076, 8104, V9827, 2002, 2005, 2006, 2007, 2104, 7125, 4033, 4044, 4055, 4077 or 4099 of Kuraray.

[0069] The methacrylate is selected from M51, M52, M22 or D51N of Arkema; ​​LA-2330 of Kuraray; SG-P3 series or SG-80 series of Nagase.

[0070] Silicone elastomers include X-40-2670, R-170S, X-40-2705, X-40-2701, KMP-600, KMP-605, X-52-7030 from Xinyue Chemical; AY-42-119, EP-2600, EP-2601, EP-2720, TMS-2670, EXL-2315, EXL-2655 from DOW, etc.

[0071] Furthermore, the resin composition further comprises 0.001-5 parts by weight of a catalyst, selected from at least one of 2-methylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2-undecylimidazole, 1-benzyl-2-methylimidazole, 2-heptadecylimidazole, 2-isopropylimidazole, 2-phenyl-4-methylimidazole, 2-dodecylimidazole, 1-cyanoethyl-2-methylimidazole or a modified imidazole shown in the following structure:

[0072] Wherein R3, R4, R5 and R6 are the same or different and are methyl, ethyl or tert-butyl respectively; B is methylene, ethylene, P200F50, made by JER, can be used.

[0073] Wherein R3, R4, R5 and R6 are the same or different and are methyl, ethyl or tert-butyl respectively; A is methylene, ethylene, Or aromatic hydrocarbon group, G8009L, made by the first industry, can be used.

[0074] Furthermore, the resin composition also includes a flame retardant, which contains 5 to 50 parts by weight. The flame retardant is selected from bromine flame retardants, phosphorus flame retardants, nitrogen flame retardants, organosilicon flame retardants, organic metal salt flame retardants, and the like.

[0075] Specifically, the brominated flame retardant is selected from decabromodiphenyl ether, decabromodiphenyl ethane, brominated styrene or tetrabromophthalamide.

[0076] The phosphorus flame retardant is selected from inorganic phosphorus, phosphate ester, phosphoric acid, hypophosphorous acid, phosphorus oxide, 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO), 10-(2,5-dihydroxyphenyl)-9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO-HQ), (m is an integer from 1 to 5), Organic phosphorus-containing compounds such as 10-phenyl-9,10-dihydro-9-oxa-10-phosphatren-10-oxide, tri(2,6-dimethylphenyl)phosphine, phosphazene, modified phosphazene, etc.

[0077] The nitrogen-based flame retardant is selected from triazine compounds, cyanuric acid compounds, isocyanic acid compounds, phenothiazine and the like.

[0078] The organic silicon flame retardant is selected from organic silicon oil, organic silicon rubber, organic silicon resin and the like.

[0079] The organic metal flame retardant is selected from ferrocene, acetylacetone metal complex, organic metal carbonyl compound and the like.

[0080] Preferably, the flame retardant is selected from phosphazene with the brand name SPB-100 produced by Otsuka Chemical of Japan; modified phosphazenes with the brands BP-PZ, PP-PZ, SPCN-100, SPV-100 and SPB-100L.

[0081] Furthermore, a dye, such as a fluorescent dye or a black dye, may be added to the resin composition.

[0082] Preferably, the fluorescent dye is a pyrazoline compound, and the black dye is liquid or powdered carbon black, pyridine complex, azo complex, quinone compound, zirconium nitride, titanium oxide, titanium nitride, black talc, cobalt chromium chromium metal oxide, azine or phthalocyanine.

[0083] The present invention also provides the use of the resin composition in prepregs, laminates, insulating boards, insulating films, circuit substrates and electronic devices, which are specifically described as follows:

[0084] The present invention also provides a prepreg, comprising a reinforcing material and the above-mentioned resin composition. The preparation method of the prepreg is: dissolving the resin composition with a solvent to prepare a glue solution, then immersing the reinforcing material in the above-mentioned glue solution, taking out the immersed reinforcing material and baking it at 100-180°C for 1-15 minutes; after drying, the prepreg is obtained.

[0085] The solvent is selected from at least one of acetone, butanone, toluene, methyl isobutyl ketone, N,N-dimethylformamide, N,N-dimethylacetamide, ethylene glycol methyl ether, propylene glycol methyl ether, benzene, toluene, xylene and cyclohexane.

[0086] The reinforcing material is selected from at least one of natural fibers, organic synthetic fibers, organic fabrics, and inorganic fabrics. Preferably, the reinforcing material is glass fiber cloth; among the glass fiber cloth, open fiber cloth or flat cloth is preferably used; and the glass fiber cloth is preferably E glass fiber cloth, S glass fiber cloth, or Q glass fiber cloth.

[0087] In addition, when the reinforcing material is glass fiber cloth, the glass fiber cloth is chemically treated with a coupling agent to improve the interface bonding between the resin composition and the glass fiber cloth. The coupling agent is preferably an epoxy silane coupling agent or an amino silane coupling agent to provide good water resistance and heat resistance.

[0088] An embodiment of the present invention further provides a laminate comprising a piece of the aforementioned prepreg and a metal foil disposed on at least one side of the prepreg; or comprising a composite sheet formed by overlapping a plurality of the aforementioned prepregs and a metal foil disposed on at least one side of the composite sheet.

[0089] The laminate is prepared by the following method: a metal foil is coated on one or both sides of a prepreg, or at least two prepregs are stacked to form a composite sheet, a metal foil is coated on one or both sides of the composite sheet, and the composite sheet is hot pressed to obtain a metal foil laminate. The hot pressing conditions are: pressing at 0.2-2MPa and 150-250°C for 2-4 hours.

[0090] Preferably, the metal foil is selected from copper foil or aluminum foil. The thickness of the metal foil is 5 micrometers, 8 micrometers, 12 micrometers, 18 micrometers, 35 micrometers or 70 micrometers.

[0091] An embodiment of the present invention further provides an insulating board, comprising at least one of the aforementioned prepreg sheets.

[0092] The embodiment of the present invention further provides an insulating film, comprising a carrier film and the above-mentioned resin composition coated thereon, and the thermal index of the insulating film is significantly improved.

[0093] The insulating film is prepared by the following method: the resin composition is dissolved in a solvent to prepare a glue solution, the glue solution is then coated on a carrier film, and the carrier film coated with the glue solution is heated and dried to obtain the insulating film.

[0094] The aforementioned solvent is selected from at least one of acetone, butanone, toluene, methyl isobutyl ketone, N, N-dimethylformamide, N, N-dimethylacetamide, ethylene glycol methyl ether, propylene glycol methyl ether, benzene, toluene, xylene, and cyclohexane.

[0095] The carrier film is selected from at least one of PET film, PP film, PE film and PVC film.

[0096] An embodiment of the present invention further provides a circuit substrate, comprising one or more of the aforementioned prepreg, laminate, insulating plate, and insulating film.

[0097] An embodiment of the present invention further provides an electronic device, comprising the aforementioned circuit substrate; since the heat resistance of the circuit substrate is greatly improved, the safety of the electronic device is significantly improved.

[0098] The technical solution of the present application is further described below in conjunction with some specific synthesis examples and comparative examples.

[0099] Synthesis Example 1: Modified bismaleimide prepolymer Y1

[0100] Add 100 g of bismaleimide resin (BMI-2300 manufactured by Yamato Chemical), 10 g of amino silicone resin A (amino equivalent of 450 g / mol, DOWSILTM BY 16-853) and an appropriate amount of organic solvent into a beaker, react at 80°C for 60 min, heat to 100°C, add 25 g of amino silicone resin B (amino equivalent of 800 g / mol, X-22-161A manufactured by Shin-Etsu Chemical), continue the reaction for 90 min, and obtain modified bismaleimide prepolymer Y1.

[0101] Synthesis Example 2: Modified bismaleimide prepolymer Y2

[0102] Add 100g of bismaleimide resin (made by Nippon Kayaku, MIR-3000), 5g of amino silicone resin A (amino equivalent is 430g / mol, KF-8010 made by Shin-Etsu Chemical) and an appropriate amount of organic solvent into a beaker, react at 80°C for 60min, raise the temperature to 100°C, add 30g of amino silicone resin B (amino equivalent is 800g / mol, X-22-161A made by Shin-Etsu Chemical), continue the reaction for 100min, and obtain the modified bismaleimide prepolymer Y2.

[0103] Synthesis Example 3: Modified bismaleimide prepolymer Y3

[0104] Add 100 g of bismaleimide resin (BMI-2300 manufactured by Yamato Chemical), 10 g of amino silicone resin A (amino equivalent is 450 g / mol, DOWSILTM BY 16-853), 1 g of aminophenol and an appropriate amount of organic solvent into a beaker, react at 80°C for 60 min, heat to 100°C, add 25 g of amino silicone resin B (amino equivalent is 800 g / mol, X-22-161A manufactured by Shin-Etsu Chemical), continue the reaction for 90 min, and obtain modified bismaleimide prepolymer Y3.

[0105] Synthesis Example 4: Modified bismaleimide prepolymer Y4

[0106] Add 100g of bismaleimide resin (BMI-2300 manufactured by Yamato Chemical), 10g of amino silicone resin A (amino equivalent is 430g / mol, KF-8010 manufactured by Shin-Etsu Chemical), 1g of aminophenol and an appropriate amount of organic solvent into a beaker, react at 80°C for 60min, heat to 100°C, add 25g of amino silicone resin B (amino equivalent is 1500g / mol, X-22-161B manufactured by Shin-Etsu Chemical), continue the reaction for 100min, and obtain modified bismaleimide prepolymer Y4.

[0107] Comparative Synthesis Example 1: Modified Bismaleimide Prepolymer Y5

[0108] Add 100 g of bismaleimide resin (BMI-2300 manufactured by Yamato Chemical Industry Co., Ltd.), 35 g of amino silicone resin A (amino equivalent of 450 g / mol, DOWSILTM BY 16-853) and an appropriate amount of organic solvent into a beaker, react at 100° C. for 120 min, and obtain modified bismaleimide prepolymer Y5.

[0109] Comparative Synthesis Example 2: Modified Bismaleimide Prepolymer Y6

[0110] Add 100 g of bismaleimide resin (made by Nippon Kayaku, MIR-3000), 35 g of amino silicone resin B (amino equivalent is 800 g / mol, X-22-161A made by Shin-Etsu Chemical), 1 g of aminophenol and an appropriate amount of organic solvent into a beaker, react at 100°C for 120 min, and obtain modified bismaleimide prepolymer Y6.

[0111] According to the data in Table 1, the corresponding solid substances are weighed, and the glue solution is adjusted to a solid content of 60% by a solvent. The glue solution is applied to E glass fiber cloth, taken out after infiltration, placed in a 160°C forced air drying oven, and baked for 3 to 6 minutes to form a semi-cured sheet.

[0112] The prepreg was cut to 300×300 mm, and an electrolytic copper foil was placed on each side of the prepreg to form a certain stacking structure, and then sent to a vacuum press for pressing to obtain a metal foil laminate (or copper-clad laminate). The specific performance tests are shown in Table 2.

[0113] Table 1 Resin composition composition

[0114]

[0115] Table 2 Performance table

[0116]

[0117] The performance tests were conducted on the prepregs and copper-clad laminates prepared in all the above Examples 1 to 5 and Comparative Examples 1 to 2.

[0118] (1) Glass transition temperature was measured by DMA (thermomechanical analysis) at a heating rate of 10°C / min;

[0119] (2) PCT 2HR water absorption rate determination: Take 3 samples of 10 cm × 10 cm, 0.40 mm thick, with metal foil removed from both sides, dry them at 100°C for 2 hours, weigh them, and record the weight as W1. Then, treat them in a pressure cooker tester at 121°C and 2 atmospheres for 2 hours, weigh them, and record the weight as W2. The water absorption rate is determined as (W2-W1) / W1×100%;

[0120] (3) X / Y thermal expansion coefficient (CTE) determination: TMA (thermomechanical analysis) was used, with a heating rate of 10°C / min and a test temperature range of 30 to 100°C;

[0121] (4) Secondary surface defects: The standard test method specified in IPC-TM-650 is used to determine whether the substrate has defects such as dried flowers and white lines by visual inspection or slicing.

[0122] It can be seen from the above experimental data that Examples 1 to 5 have excellent high Tg, low water absorption and low CTE values, and the substrates of Examples 1 to 5 have no white lines. Compared with Comparative Example 1, Example 1 has a higher Tg value and low water absorption, and compared with Comparative Example 2, Example 2 has a higher Tg value, low CTE and no white lines on the substrate.

[0123] In addition, it can be seen from the rheological curves of Comparative Example 2 and Example 1 that the rheological window of Example 1 is wider and the minimum melt viscosity is lower, indicating that the resin reacts slowly, which is conducive to controlling processability.

[0124] It should be understood that although this specification is described according to implementation modes, not every implementation mode contains only one independent technical solution. This description of the specification is only for the sake of clarity. Those skilled in the art should regard the specification as a whole. The technical solutions in each implementation mode may also be appropriately combined to form other implementation modes that can be understood by those skilled in the art.

[0125] The series of detailed descriptions listed above are only specific descriptions of feasible implementation methods of the present invention. They are not intended to limit the scope of protection of the present invention. Any equivalent implementation methods or changes that do not deviate from the technical spirit of the present invention should be included in the scope of protection of the present invention.

Claims

1. A modified bismaleimide prepolymer, characterized in that: The bismaleimide compound, amino silicone resin A and amino silicone resin B are reacted to obtain the bismaleimide compound; the specific reaction between the bismaleimide compound, amino silicone resin A and amino silicone resin B is as follows: the bismaleimide compound and amino silicone resin A are reacted at 60-90°C for 0.5-1.5 hours, the temperature is raised to 90-130°C, the amino silicone resin B is added and the reaction is continued for 0.5-2 hours; Wherein, the amino equivalent Ea of the amino silicone resin A is A <Amino equivalent Ea of the amino silicone resin B B ; The amino equivalent Ea of the amino silicone resin A A 100 g / mol≤Ea A ≤500g / mol, the amino equivalent Ea of the amino silicone resin B B The amino equivalent is 500 g / mol<Ea B ≤1600g / mol; The absolute value of the difference in amino equivalent between the amino silicone resin A and the amino silicone resin B is 100 g / mol to 600 g / mol.

2. The modified bismaleimide prepolymer according to claim 1, characterized in that The amino silicone resin A and the amino silicone resin B both contain the following structure: ; wherein R and R' are C1~C5 alkyl groups, and m is an integer of 1~30.

3. The modified bismaleimide prepolymer according to claim 1, characterized in that: The amino silicone resin A and / or the amino silicone resin B contain at least one amino group on the side chain.

4. The modified bismaleimide prepolymer according to claim 1, characterized in that: The amino silicone resin A and / or the amino silicone resin B contain at least one amino group at the terminal.

5. A resin composition, characterized in that By weight, it includes the following components: (a) modified bismaleimide prepolymer: 100 parts; (b) maleimide resin: 0-100 parts; (c) Filler: 1-300 parts; Wherein, the modified bismaleimide prepolymer is the modified bismaleimide prepolymer according to any one of claims 1 to 4.

6. The resin composition according to claim 5, characterized in that The maleimide resin is selected from at least one of the following structures: Structural formula (1); Structural formula (2); Structural formula (3); Structural formula (4), wherein n is an integer of 1 to 10, R2 is hydrogen, methyl or ethyl, and R1 is methylene, ethylene or ; Structural formula (5); Structural formula (6), wherein n is an integer from 1 to 10; Structural formula (7), wherein n is an integer from 1 to 10; Structural formula (8); Structural formula (9); In the structural formula (10), R is hydrogen, methyl or ethyl, and n is an integer of 1 to 10.

7. The resin composition according to claim 5, characterized in that The filler includes inorganic filler, organic filler and composite filler. The inorganic filler is selected from at least one of fused silica, crystalline silica, spherical silica, hollow silica, aluminum hydroxide, aluminum oxide, talc, aluminum nitride, boron nitride, silicon carbide, barium sulfate, barium titanate, strontium titanate, calcium carbonate, calcium silicate, mica and glass fiber powder; the organic filler is selected from at least one of polytetrafluoroethylene powder, polyphenylene sulfide powder and polyether sulfone powder.

8. The resin composition according to claim 7, characterized in that The filler is surface treated with a silane coupling agent, and the silane coupling agent is at least one of an aminosilane coupling agent, a carbon-carbon double bond-containing silane coupling agent, or an epoxy silane coupling agent.

9. The resin composition according to claim 5, characterized in that The resin composition further comprises 5 to 50 parts by weight of an elastomer, wherein the elastomer is selected from at least one of styrene elastomers, methacrylate elastomers, and silicone elastomers.

10. The resin composition according to claim 5, characterized in that The resin composition also includes a flame retardant, and the flame retardant contains 5 to 50 parts by weight; The flame retardant is selected from bromine flame retardants, phosphorus flame retardants, nitrogen flame retardants, organosilicon flame retardants, and organic metal salt flame retardants.

11. Use of the resin composition according to any one of claims 5 to 10 in prepregs, laminates, insulating films, insulating boards, copper-clad boards, circuit substrates and electronic devices.

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