Modified bismaleimide prepolymer, resin composition, and use of the resin composition

Abstract

The present invention provides a modified bismaleimide prepolymer, a resin composition and its use, the modified bismaleimide being obtained by reacting a prepolymer bismaleimide compound with an aminoorganic silicone resin A and an aminoorganic silicone resin B, wherein the amino equivalent Ea A is the amino equivalent Ea of the amino organic silicone resin B B Unlike the above, the ratio of the sum of the masses of the amino organic silicone resin A and the amino organic silicone resin B to the mass of the bismaleimide compound is (5 to 80): 100. In the present invention, the reactivity of the bismaleimide compound is improved, and the rheological properties in high temperature lamination are controlled when the modified bismaleimide prepolymer is used in the field of substrate materials such as package substrates.

Description

Technical Field

[0001] The present invention relates to the technical field of electronic materials, and particularly relates to a modified bismaleimide prepolymer, a resin composition containing the modified bismaleimide prepolymer, and the use of the resin composition.

Background Art

[0002] In recent years, electronic devices have been developing in the direction of miniaturization and high performance. As the wiring density and high integration on printed circuit boards continue to evolve, higher requirements are imposed on the heat resistance and reliability of copper-clad laminates. In particular, in semiconductor package substrates, due to the difference in the coefficient of thermal expansion between the chip and the organic substrate during package assembly, warpage problems occur.

[0003] The cured product of bismaleimide resin has excellent properties such as high temperature resistance, high humidity resistance, high elastic modulus, low CTE, and high strength, and is particularly suitable for use as a matrix resin for IC package substrates and substrate-like PCBs. However, due to disadvantages such as high brittleness and low processability, its large-scale use is limited.

[0004] In the prior art, in order to improve the above problems existing in the cured product of bismaleimide resin, silicone rubber powder is introduced into the bismaleimide resin. By introducing the silicone rubber powder, the water absorption rate and toughness of the cured product of bismaleimide resin are improved to a certain extent. However, the silicone rubber powder has a small density, is easy to aggregate, has low dispersibility, floats on the upper layer of the bismaleimide resin adhesive liquid, causes phase separation, and brings problems such as interlayer delamination to the cured product of bismaleimide resin. In addition, there is also a prior art in which silicone oil is directly added to the bismaleimide resin. In the lamination of the cured product, if the silicone oil does not react completely, it is very easy to exude from the system, affecting the production processability, and moreover, seriously affecting the comprehensive performance of the final cured product.

Summary of the Invention

Problems to be Solved by the Invention

[0005] An object of the present invention is to provide a modified bismaleimide prepolymer, a resin composition containing the modified bismaleimide prepolymer, and the use of the resin composition. The modified bismaleimide prepolymer is modified by reacting with an amino organic silicone resin having an amino equivalent different from that of a bismaleimide compound, and by controlling the masses of the amino organic silicone resin and the bismaleimide compound, the problem of high brittleness of the bismaleimide resin is improved, the reactivity of the bismaleimide resin and the rheological properties of the resin during high-temperature lamination are effectively controlled, and furthermore, the processing performance of the resin composition is improved.

Means for Solving the Problems

[0006] In order to achieve one of the above object of the invention, one embodiment of the present invention is obtained by reacting a bismaleimide compound, an amino organic silicone resin A, and an amino organic silicone resin B, and the amino equivalent Ea of the amino organic silicone resin A A is different from the amino equivalent Ea of the amino organic silicone resin B B and a modified bismaleimide prepolymer is provided, wherein the ratio of the sum of the masses of the amino organic silicone resin A and the amino organic silicone resin B to the mass of the bismaleimide compound is (5 to 80):100.

[0007] As a further improvement of one embodiment of the present invention, the ratio of the sum of the masses of the amino organic silicone resin A and the amino organic silicone resin B to the mass of the bismaleimide compound is (20 to 50):100.

[0008] As a further improvement of one embodiment of the present invention, the mass ratio of the amino organic silicone resin A to the amino organic silicone resin B is 1:(2 to 30).

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

[0010]

Chemical formula

[0011] In the formula, R and R' are C1-C5 alkyl groups, and m is an integer of 1-30.

[0012] As a further improvement of one embodiment of the present invention, the side chains in the amino organic silicone resin A and / or the amino organic silicone resin B contain at least one amino group.

[0013] As a further improvement of one embodiment of the present invention, the terminals in the amino organic silicone resin A and / or the amino organic silicone resin B contain at least one amino group.

[0014] One embodiment of the present invention is, by weight, (a) 30-100 parts of a modified bismaleimide prepolymer, and (b) 3-50 parts of a cyanate resin, and (c) 5-60 parts of an elastomer, and A resin composition is further provided, which comprises the above composition components, and the modified bismaleimide prepolymer is the modified bismaleimide prepolymer described above.

[0015] As a further improvement of one embodiment of the present invention, the cyanate resin is selected from one or more of bisphenol A cyanate resin, bisphenol F cyanate resin, bisphenol S type cyanate resin, bisphenol E type cyanate resin, bisphenol M type cyanate resin, double bond-containing cyanate resin, phosphorus-containing cyanate resin, phenol type cyanate resin, biphenyl type cyanate resin, naphthalene ring type cyanate resin, dicyclopentadiene type cyanate resin.

[0016] As a further improvement of one embodiment of the present invention, the cyanate resin is a naphthalene type cyanate resin and / or a phenol type cyanate resin represented by the following structure.

[0017] [Chemical formula]

[0018] However, R6 is hydrogen, a methyl group or an ethyl group, and n2 is an integer from 1 to 10.

[0019]

Chemical formula

[0020] However, n is an integer from 1 to 10.

[0021] As a further improvement of one embodiment of the present invention, the elastomer is selected from at least one of styrene-based elastomers, methacrylate-based elastomers, and organosilicon-based elastomers.

[0022] As a further improvement of one embodiment of the present invention, it further contains a silane coupling agent and a dispersant.

[0023] As a further improvement of one embodiment of the present invention, the silane coupling agent is an epoxy silane coupling agent, the dispersant is a phosphate ester-based dispersant and / or a modified polyurethane-based dispersant, and the weight ratio of the silane coupling agent to the dispersant is 2:1 to 10:1.

[0024] One embodiment of the present invention further provides the use of the resin composition described above for prepregs, laminates, insulating films, insulating boards, copper-clad boards, circuit boards, and electronic devices.

Advantages of the Invention

[0025] One or more technical solutions provided by the present invention have at least the following technical effects or advantages. The modified bismaleimide prepolymer provided by the present invention is obtained by reacting a bismaleimide compound with an amino-functional organosilicon resin having a different amino equivalent weight, which improves the reactivity and brittleness of the bismaleimide compound. By controlling the masses of the amino-functional organosilicon resin and the bismaleimide compound, the rheological reaction window of the resin composition is effectively adjusted, and the risk of defects such as wrinkles or white patterns occurring on the substrate due to the reaction being too fast during the crimping of the resin composition is reduced.

Brief Description of the Drawings

[0026]

Figure 1

Modes for Carrying Out the Invention

[0027] The present invention will be described in detail below in connection with specific embodiments, but these embodiments do not limit the present invention, and any changes made by those skilled in the art to the reaction conditions, reactants or raw material usage amounts based on these embodiments are all included within the protection scope of the present invention.

[0028] Examples of the present invention are obtained by reacting a bismaleimide compound with an amino-functional organosilicon resin A and an amino-functional organosilicon resin B, and the amino equivalent weight Ea of the amino-functional organosilicon resin A A is different from the amino equivalent weight Ea of the amino-functional organosilicon resin B B and a modified bismaleimide prepolymer is provided in which the ratio of the sum of the masses of the amino-functional organosilicon resin A and the amino-functional organosilicon resin B to the mass of the bismaleimide compound is (5 - 80):100.

[0029] Preferably, the ratio of the sum of the masses of the amino-functional organosilicon resin A and the amino-functional organosilicon resin B to the mass of the bismaleimide compound is (20 - 50):100.

[0030] Furthermore, the mass ratio of the amino-functional organosilicon resin A to the amino-functional organosilicon resin B is 1:(2 - 30).

[0031] The specific reaction of the bismaleimide compound, amino organosilicone resin A, and amino organosilicone resin B is as follows. First, the bismaleimide compound is reacted with amino organosilicone resin A at 60-90 °C for 0.5-1.5 hours. Then, the temperature is raised to 90-130 °C, and then amino organosilicone resin B is added and the reaction is continued for 0.5-2 hours.

[0032] Preferably, at least one of aminophenol, carboxylic acid, or carboxylic anhydride is added during the reaction in a content of 0.1-10 parts by weight, and any of the phenolic hydroxyl group, carboxyl group, and acid anhydride group in aminophenol, carboxylic acid, or carboxylic anhydride reacts with the bismaleimide compound to improve the reactivity.

[0033] Furthermore, the amino equivalent Ea of amino organosilicone resin A A is 100 g / mol ≤ Ea A ≤ 500 g / mol, and the amino equivalent Ea of amino organosilicone resin B B has an amino equivalent of 500 g / mol < Ea B ≤ 1600 g / mol.

[0034] Preferably, the absolute value of the difference in amino equivalents between organosilicone resin A and organosilicone resin B is 100 g / mol to 600 g / mol.

[0035] Both amino organosilicone resin A and amino organosilicone resin B contain the following structure.

[0036]

Chemical formula

[0037] In the formula, R and R' are C1-C5 alkyl groups, and m is an integer of 1-30.

[0038] Furthermore, at least one amino group is contained in the side chain of the amino organic silicone resin A and / or the amino organic silicone resin B.

[0039] Furthermore, at least one amino group is contained in the terminal of the amino organic silicone resin A and / or the amino organic silicone resin B.

[0040] Furthermore, the aforementioned bismaleimide compound may be selected from at least one of the following structures.

[0041]

Chemical formula

[0042]

Chemical formula

[0043]

Chemical formula

[0044]

Chemical formula

[0045] However, R2 is hydrogen, a methyl group or an ethyl group, R1 is a methylene group or an ethylene group, and n is an integer from 1 to 10.

[0046]

Chemical formula

[0047]

Chemical formula

[0048] However, n is an integer from 1 to 10.

[0049] [Chemical formula]

[0050] However, n is an integer from 1 to 10.

[0051] [Chemical formula]

[0052] However, n is an integer from 1 to 10.

[0053] [Chemical formula]

[0054] [Chemical formula]

[0055] However, R is hydrogen, a methyl group or an ethyl group, and n is an integer from 1 to 10.

[0056] The present invention further provides a resin composition comprising, by weight, (a) 30 to 100 parts of a modified bismaleimide prepolymer, (b) 3 to 50 parts of a cyanate resin, (c) 5 to 60 parts of an elastomer, wherein the modified bismaleimide prepolymer is the aforementioned modified bismaleimide prepolymer.

[0057] Furthermore, the cyanate resin is selected from one or more of bisphenol A type cyanate resin, bisphenol F type cyanate resin, bisphenol S type cyanate resin, bisphenol E type cyanate resin, bisphenol M type cyanate resin, double bond-containing cyanate resin, phosphorus-containing cyanate resin, phenol type cyanate resin, biphenyl type cyanate resin, naphthalene ring type cyanate resin, dicyclopentadiene type cyanate resin.

[0058] Preferably, the cyanate resin is a naphthalene ring type cyanate resin and / or a phenol type cyanate resin represented by the following structure.

[0059]

Chemical formula

[0060] However, R6 is hydrogen, a methyl group or an ethyl group, and n2 is an integer from 1 to 10.

[0061]

Chemical formula

[0062] However, n is an integer from 1 to 10.

[0063] Furthermore, the elastomer is selected from at least one of styrene-based elastomers, methacrylate-based elastomers, and organosilicon-based elastomers.

[0064] Among them, the styrene-based elastomers are selected from H1041, H1043, H1051, H1052, H1053, H1221, P1500, P2000, M1911, or M1913 of Asahi Kasei Corporation, 8004, 8006, 8076, 8104, V9827, 2002, 2005, 2006, 2007, 2104, 7125, 4033, 4044, 4055, 4077, or 4099 of Kuraray Co., Ltd.

[0065] The methacrylates are selected from M51, M52, M22, or D51N of Arkema, LA-2330 of Kuraray Co., Ltd., and the SG-P3 series or SG-80 series of Nagase Co., Ltd.

[0066] The organosilicon-based elastomer is selected from Shin-Etsu Chemical's X-40-2670, R-170S, X-40-2705, X-40-2701, KMP-600, KMP-605, X-52-7030, Dow's AY-42-119, EP-2600, EP-2601, EP-2720, TMS-2670, EXL-2315, EXL-2655, etc.

[0067] Furthermore, the resin composition further contains 0.01 to 5 parts by weight of a catalyst, and the catalyst is at least one of an imidazole-based catalyst, a pyridine-based catalyst, and an organometallic salt-based catalyst. Preferably, the catalyst is at least one of 4-dimethylaminopyridine, 2-methylimidazole, 2-methyl-4-ethylimidazole, 2-phenylimidazole, modified imidazole, and zinc caprylate.

[0068] The modified imidazole is as shown by the following structure.

[0069]

Chemical formula

[0070] In the formula, R3, R4, R5, and R6 are the same or different, and each is a methyl group, an ethyl group, or a tert-butyl group, B is a methylene group, an ethylene group, a dimethylmethylene group, a sulfide group, or a sulfonyl group, and P200F50 manufactured by JER can be used.

[0071]

Chemical formula

[0072] In the formula, R3, R4, R5, and R6 are the same or different, and each is a methyl group, an ethyl group, or a tert-butyl group, A is a methylene group, an ethylene group, a dimethylmethylene group, a sulfide group, a sulfonyl group, or an aromatic hydrocarbon group, and G8009L manufactured by Dai-ichi Kogyo Seiyaku Co., Ltd. can be used.

[0073] Furthermore, the resin composition further contains 20 to 200 parts by weight of a filler. The filler includes an inorganic filler, an organic filler, and a 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 powder, 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 polyethersulfone powder.

[0074] Preferably, the filler is spherical silica, aluminum oxide, or aluminum hydroxide, and more preferably spherical silica.

[0075] Preferably, the content of the filler is 30 to 150 parts by weight.

[0076] Furthermore, 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. Preferably, the silane coupling agent is selected from one or more of product number KBM-573 manufactured by Shin-Etsu Chemical Co., Ltd., Z-6883 manufactured by Dow Corning, product number KBM-1003 manufactured by Shin-Etsu Chemical Co., Ltd., and product number KBM-1403 manufactured by Shin-Etsu Chemical Co., Ltd.

[0077] Furthermore, the resin composition further contains a silane coupling agent and a dispersant. The silane coupling agent is an epoxy silane coupling agent, the dispersant is phosphoric esters or / and modified polyurethanes, and the weight ratio of the silane coupling agent to the dispersant is 2:1 to 10:1.

[0078] Furthermore, the resin composition further contains 5 to 50 parts by weight of a flame retardant based on 100 parts by weight of the resin composition, and the flame retardant is selected from brominated flame retardants, phosphorus-based flame retardants, nitrogen-based flame retardants, organosilicon flame retardants, organic metal salt flame retardants, and the like.

[0079] Preferably, the flame retardant is selected from phosphazenes with product numbers SPB-100, modified phosphazenes with product numbers BP-PZ, PP-PZ, SPCN-100, SPV-100, and SPB-100L manufactured by Otsuka Chemical Co., Ltd. of Japan.

[0080] Furthermore, a dye may be further added to the resin composition, and a fluorescent dye or a black dye may be selected. Specifically, a pyrazoline-based compound may be selected as the fluorescent dye, and specifically, liquid or powdered carbon black, a pyridine complex, an azo complex, a quinone-based compound, zirconium nitride, titanium oxide, titanium nitride, black talc powder, cobalt chromium chromium metal oxide, azine, or phthalocyanine may be selected as the black dye.

[0081] The present invention further provides the use of the above resin composition for prepregs, laminates, insulating films, insulating boards, circuit boards, and electronic devices, and the specific description is as follows.

[0082] The present invention further provides a prepreg containing a reinforcing material and the aforementioned resin composition. The manufacturing method of the prepreg is to dissolve the resin composition as an adhesive solution with a solvent, then immerse the reinforcing material in the above adhesive solution, take out the immersed reinforcing material, and bake it at 100 to 180°C for 1 to 15 minutes, and a prepreg can be obtained by drying.

[0083] Here, the solvent is selected from at least one of acetone, butanone, toluene, methyl isobutyl ketone, N,N-dimethylformamide, N,N-dimethylacetamide, ethylene glycol monomethyl ether, propylene glycol monomethyl ether, benzene, toluene, xylene, and cyclohexane.

[0084] The reinforcing material is selected from at least one of natural fibers, synthetic organic fibers, organic fabrics, and inorganic fabrics. Preferably, a glass fiber cloth is used as the reinforcing material. Among the glass fiber cloths, it is preferable to use an open filament fiber cloth or a plain woven fiber cloth. The glass fiber cloth is preferably an E glass fiber cloth, an S glass fiber cloth, or a Q glass fiber cloth.

[0085] Also, when a glass fiber cloth is used as the reinforcing material, the glass fiber cloth is chemically treated with a coupling agent in order to improve the interfacial bonding between the resin composition and the glass fiber cloth. In order to provide high water resistance and heat resistance, it is preferable to use an epoxy silane coupling agent or an amino silane coupling agent as the coupling agent.

[0086] Examples of the present invention further provide a laminate including one of the aforementioned prepregs and a metal foil provided on at least one surface of the prepreg, or a combined sheet formed by stacking a plurality of the aforementioned prepregs on top of each other, and a metal foil provided on at least one surface of the combined sheet.

[0087] The laminate is manufactured by the following method. Coating a metal foil on one or both surfaces of one prepreg, or stacking at least two prepregs as a combined sheet, coating a metal foil on one or both surfaces of the combined sheet, and obtaining a metal foil laminate by thermocompression molding. The pressure conditions for thermocompression are 0.2 - 2 MPa, and pressurize at 150 - 250 °C for 2 - 4 hours.

[0088] Preferably, the metal foil is selected from a copper foil or an aluminum foil. The thickness of the metal foil is 5 microns, 8 microns, 12 microns, 18 microns, 35 microns, or 70 microns.

[0089] Examples of the present invention further provide an insulating board including at least one of the aforementioned prepregs.

[0090] Examples of the present invention further provide an insulating thin film including a carrier film and the aforementioned resin composition coated thereon, with a significantly improved heat index.

[0091] The insulating thin film is manufactured by the following method. The above resin composition is dissolved with a solvent to form an adhesive liquid, and then the adhesive liquid is applied onto a carrier film. When the carrier film coated with the adhesive liquid is heated and dried, an insulating thin film is obtained.

[0092] The above-mentioned solvent is selected from at least one of acetone, butanone, toluene, methyl isobutyl ketone, N,N-dimethylformamide, N,N-dimethylacetamide, ethylene glycol monomethyl ether, propylene glycol monomethyl ether, benzene, toluene, xylene, and cyclohexane.

[0093] The carrier film is selected from at least one of a PET film, a PP film, a PE film, and a PVC film.

[0094] Embodiments of the present invention further provide a circuit board including one or more of the above-mentioned prepreg, laminate, insulating board, and insulating thin film.

[0095] Embodiments of the present invention further provide an electronic device including the above-mentioned circuit board. Since the heat resistance of the circuit board is greatly improved, the safety of the electronic device is significantly improved.

[0096] The technical solution of the present application will be further described below in connection with several specific synthesis examples and comparative examples.

[0097] Synthesis Example 1 Modified Bismaleimide Prepolymer Y1 100 g of bismaleimide resin (manufactured by Daiwa Chemical Co., Ltd., BMI-2300) and 10 g of amino organic silicone resin A (amino equivalent 450 g / mol, DOWSIL TMAdd 100 g of bismaleimide resin (manufactured by Nippon Kayaku Co., Ltd., MIR-3000), 5 g of amino organic silicone resin A (amino equivalent 430 g / mol, KF-8010 manufactured by Shin-Etsu Chemical Co., Ltd.) and an appropriate amount of organic solvent to a beaker, react at 80°C for 60 min, raise the temperature to 100°C, and then add another 30 g of amino organic silicone resin B (amino equivalent 800 g / mol, X-22-161A manufactured by Shin-Etsu Chemical Co., Ltd.). Continue the reaction for 90 min and discharge to obtain modified bismaleimide prepolymer Y2.

[0098] Synthesis Example 2 Modified Bismaleimide Prepolymer Y2 Add 100 g of bismaleimide resin (manufactured by Nippon Kayaku Co., Ltd., MIR-3000), 5 g of amino organic silicone resin A (amino equivalent 430 g / mol, KF-8010 manufactured by Shin-Etsu Chemical Co., Ltd.) and an appropriate amount of organic solvent to a beaker, react at 80°C for 60 min, raise the temperature to 100°C, and then add another 30 g of amino organic silicone resin B (amino equivalent 800 g / mol, X-22-161A manufactured by Shin-Etsu Chemical Co., Ltd.). Continue the reaction for 90 min and discharge to obtain modified bismaleimide prepolymer Y2.

[0099] Synthesis Example 3 Modified Bismaleimide Prepolymer Y3 Add 100 g of bismaleimide resin (manufactured by Daiwa Chemical Co., Ltd., BMI-2300), 10 g of amino organic silicone resin A (amino equivalent 450 g / mol, DOWSIL TM BY 16-853), 1 g of aminophenol and an appropriate amount of organic solvent to a beaker, react at 80°C for 60 min, raise the temperature to 100°C, and then add another 25 g of amino organic silicone resin B (amino equivalent 800 g / mol, X-22-161A manufactured by Shin-Etsu Chemical Co., Ltd.). Continue the reaction for 90 min and discharge to obtain modified bismaleimide prepolymer Y3.

[0100] Synthesis Example 4 Modified Bismaleimide Prepolymer Y4 Add 100 g of bismaleimide resin (manufactured by Nippon Kayaku Co., Ltd., BMI-2300), 10 g of amino organic silicone resin A (amino equivalent 430 g / mol, manufactured by Shin-Etsu Chemical Co., Ltd., KF-8010), 1 g of aminophenol and an appropriate amount of organic solvent to a beaker, react at 80 °C for 60 min, raise the temperature to 100 °C, and further add 25 g of amino organic silicone resin B (amino equivalent 1500 g / mol, manufactured by Shin-Etsu Chemical Co., Ltd., X-22-161B), continue the reaction for 100 min, and discharge to obtain modified bismaleimide prepolymer Y4.

[0101] Synthesis Comparative Example 1 Modified bismaleimide prepolymer Y5 Add 100 g of bismaleimide resin (manufactured by Daiwa Kasei Co., Ltd., BMI-2300), 35 g of amino organic silicone resin A (amino equivalent 450 g / mol, DOWSIL TM BY 16-853) and an appropriate amount of organic solvent to a beaker, react at 100 °C for 120 min, and discharge to obtain modified bismaleimide prepolymer Y5.

[0102] Synthesis Comparative Example 2 Modified bismaleimide prepolymer Y6 Add 100 g of bismaleimide resin (manufactured by Nippon Kayaku Co., Ltd., MIR-3000), 35 g of amino organic silicone resin B (amino equivalent 800 g / mol, manufactured by Shin-Etsu Chemical Co., Ltd., X-22-161A), 1 g of aminophenol and an appropriate amount of organic solvent to a beaker, react at 100 °C for 120 min, and discharge to obtain modified bismaleimide prepolymer Y6.

[0103] Weigh the corresponding solids according to the data in Table 1, adjust each weighed solid with a solvent so that the solid content of the adhesive solution becomes 60%, apply the adhesive solution onto an E-glass fiber cloth, after infiltration, place it in a hot air drying oven at 160 °C, bake for 3 - 6 min, and manufacture prepreg.

[0104] Cut the prepreg into 300×300 mm, place one electrolytic copper foil on each side of the prepreg, stack them in a certain stacking structure, feed them into a vacuum press and press them to obtain a metal foil laminate (or copper-clad laminate). The specific performance detection is as shown in Table 2.

[0105]

Table 1

[0106]

Table 2

[0107] Perform performance tests on the prepregs and copper-clad laminates manufactured in all of the above Examples 1 to 5 and Comparative Examples 1 to 2.

[0108] 1) For the glass transition temperature, adopt DMA (Thermomechanical Analysis), and the heating rate is 10°C / min. 2) For the PCT 2HR water absorption measurement, take 3 samples with a size of 10 cm×10 cm and a thickness of 0.40 mm, and remove the metal foils on both sides. Dry them at 100°C for 2 hours, weigh them as W1. Subsequently, process them in a Pressure Cooker test machine at 121°C and 2 atmospheres for 2 hours, weigh them as W2, and measure the water absorption as (W2 - W1) / W1×100%. 3) For the measurement of the X / Y coefficient of thermal expansion (CTE), adopt TMA (Thermomechanical Analysis), the heating rate is 10°C / min, and the test temperature range is 30 to 100°C. 4) For the secondary defects in appearance, test them by the standard method specified in IPC-TM-650, and judge the presence or absence of defects such as wrinkles and white patterns in the base material by visual inspection or slicing method.

[0109] As can be seen from the above experimental data, Examples 1 to 3 have excellent properties such as high Tg, low water absorption rate, low CTE value, and high appearance quality. Among them, Example 1 has a higher Tg value and lower CTE than Comparative Example 1, and Example 2 has a higher Tg value and lower CTE than Comparative Example 2.

[0110] Also, from the rheology curves of Comparative Example 2 and Example 2 in Figure 1, it can be seen that the rheology window of Example 2 is wider and the minimum melt viscosity is lower, which indicates that the reaction of the resin is slow and contributes to the control of processability.

[0111] Although this specification has been described in terms of embodiments, each embodiment does not necessarily include only one independent technical solution. Such a description method in the specification is merely for clarification purposes. Those skilled in the art should regard the specification as a whole, and the technical solutions in each embodiment can be appropriately combined to form other embodiments that can be understood by those skilled in the art.

[0112] The above series of detailed descriptions are merely specific descriptions of the feasible embodiments of the present invention and do not limit the protection scope of the present invention. Equivalent embodiments or modifications that do not deviate from the technical spirit of the present invention are all included in the protection scope of the present invention.

Claims

1. A modified bismaleimide prepolymer obtained by reacting a bismaleimide compound with an amino organic silicone resin A and an amino organic silicone resin B, wherein the amino equivalent weight Ea of the amino organic silicone resin A Ａ is different from the amino equivalent weight Ea of the amino organic silicone resin B Ｂ and the ratio of the sum of the masses of the amino organic silicone resin A and the amino organic silicone resin B to the mass of the bismaleimide compound is (5 to 80):100, and the absolute value of the difference between the amino equivalent weight Ea A of the amino organic silicone resin A and the amino equivalent weight Ea B of the amino organic silicone resin B is 100 g / mol to 600 g / mol.

2. The modified bismaleimide prepolymer according to claim 1, wherein the ratio of the sum of the masses of the amino organic silicone resin A and the amino organic silicone resin B to the mass of the bismaleimide compound is (20 to 50):

100.

3. The modified bismaleimide prepolymer according to claim 1 or 2, wherein the mass ratio of the amino organic silicone resin A to the amino organic silicone resin B is 1:(2 to 30).

4. Both the amino organic silicone resin A and the amino organic silicone resin B contain the following structure: 【Chemical Formula 1】 However, R and R' are C1-C5 alkyl groups, and m is an integer from 1 to 30. The modified bismaleimide prepolymer according to claim 1.

5. The modified bismaleimide prepolymer according to claim 1, wherein the side chain in the amino organic silicone resin A and / or the amino organic silicone resin B contains at least one amino group.

6. The modified bismaleimide prepolymer according to claim 1, wherein the terminal in the amino organic silicone resin A and / or the amino organic silicone resin B contains at least one amino group.

7. By weight, (a)30 to 100 parts of a modified bismaleimide prepolymer, (b)3 to 50 parts of a cyanate resin, (c)5 to 60 parts of an elastomer, The resin composition characterized in that the modified bismaleimide prepolymer is the modified bismaleimide prepolymer according to claim 1.

8. The resin composition according to claim 7, wherein the cyanate resin is selected from one or more of bisphenol A type cyanate resin, bisphenol F type cyanate resin, bisphenol S type cyanate resin, bisphenol E type cyanate resin, bisphenol M type cyanate resin, double bond-containing cyanate resin, phosphorus-containing cyanate resin, phenol type cyanate resin, biphenyl type cyanate resin, naphthalene ring type cyanate resin, dicyclopentadiene type cyanate resin.

9. The cyanate resin is a naphthalene type cyanate resin and / or a phenol type cyanate resin represented by the following structure: 【Chemical Formula 2】 However, R6 is hydrogen, a methyl group or an ethyl group, and n ２ is an integer from 1 to 10, 【Chemical Formula 3】 However, n is an integer from 1 to 10. The resin composition according to claim 8.

10. The resin composition according to claim 7, wherein the elastomer is selected from at least one of a styrene-based elastomer, a methacrylate-based elastomer, and an organosilicon-based elastomer.

11. The resin composition according to claim 7, further comprising a silane coupling agent and a dispersant.

12. The resin composition according to claim 11, wherein the silane coupling agent is an epoxy silane coupling agent, the dispersant is a phosphate ester-based dispersant and / or a modified polyurethane-based dispersant, and the weight ratio of the silane coupling agent to the dispersant is 2:1 to 10:

1.

13. Use of the resin composition according to claim 7 for prepregs, laminates, insulating films, insulating boards, copper-clad boards, circuit boards, and electronic devices.

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