TW466265B - High-performance adhesive compositions - Google Patents

Abstract

An improved epoxy based adhesive composition contains: (1) a barbituric acid modified bismaleimide; (2) an epoxy resin selected from the group consisting of tetraglycidylmethylenedianiline, diglycidyl ortho-phthalate, diblycidyl ether of bisphenol A, glycidyl ether of novolac, and epoxy cresol novolac; (3) a carboxylated acrylontrile rubber containing between 19 and 41 wt% of acrylontrile; (4) a hardening agent and (5) a catalyst.

Description

Printed by Shellfish Consumer Cooperative of Central Bureau of Standards, Ministry of Economic Affairs A7 B7 V. Description of Invention (1) Inventive Jaw Field This invention relates to a composition based on epoxy resin, which can be used as a high-performance adhesive. In particular, the present invention relates to an adhesive composition containing a special epoxy resin composition, which has excellent chemical and thermal stability and can be effectively applied to high-density 1C packaging processes. The present invention also provides an improved 1C package 'that includes a special epoxy composition to provide improved chemical and thermal stability. BACKGROUND OF THE INVENTION Due to the improvement of the high-function and high-efficiency quality of life in the world, electronic products tend to be light, thin, short, small, and have the characteristics of high density and high functionality. These are the goals pursued by electronic products in recent years. To achieve the above-mentioned goal, the choice of its construction materials and methods occupies a decisive and important position. Among them, Tape Automated Bonding (TAB) is used in large computers, consumer electronics, liquid crystal displays and IC cards; flexible Flexible printed circuit board (FPC) applications in the automotive industry, communications industry, notebook computers, and lead frame tape are one of the important ways to meet the above-mentioned requirements. Regardless of the various electronic components of the tape-and-reel automatic bonding or flexible printed circuit board, the solder is adhered to the copper foil of the printed circuit board. The electronic components generate heat when used, and the greater the component density (assembly density) The more layers of flexible printed circuit boards, the more heat generated and the higher the temperature, so the adhesive used in the laminated material must be able to withstand high temperatures and not deteriorate at high temperatures. The three-layer flexible printed circuit board or three-layer tape-and-tape automatic bonding (TAB) is mostly used in acrylic or epoxy resin series, but the heat resistance and chemical resistance of the two are higher than the base paper. Standards (CNS) M specifications (2 丨 0X 297 mm) 83.110,000 (please read the note on the back before filling in this page) Order the Ministry of Economic Affairs t Mabeong Consumer Cooperatives Printing crack d 6 6 2 6 a7 ^ _B7_ V. Description of the invention (2) Polyimide (PI) is very low or worse. When the density of electronic components is increasing, it limits the use of such resins in advanced The possibility of multilayer printed circuit boards. In order to improve the lack of application of epoxy resin and the like, bismaleimide (BMI) resin is added to the resin to improve the heat resistance and drug resistance of the entire formula resin. After the bismaleimide resin is hardened, because the reaction mode is crosslinking, the product after the reaction is hard and brittle, and it is very easy to be brittle. * It is not conducive to the addition of soft boards: t; The epoxy resin is mixed with bismaleimide resin, and a rubber with appropriate toughness needs to be added to the resin material to reduce its brittleness in order to facilitate the work. However, it may be found that the obtained resin material has a phase separation phenomenon, and Disadvantages of not being able to achieve a uniform coating layer US Patent No. 4,294,877 discloses the use of bismaleimide to improve heat resistance and Tg to meet the requirement that the Tg of the materials used in printed circuit board production must be higher than 180 ° C. Otherwise deformation will occur during high temperature operation. The disadvantage is that the resin becomes very brittle after hardening and is not suitable for processing of soft substrates). British Patent No. 1190718 discloses that using a material with a soft molecular structure such as rubber to improve the brittleness of the resin has the disadvantages that it easily causes phase separation, the physical properties of the adhesive are deteriorated, and Tg is reduced. US Patent No. J, 〇41,519 shows an improved epoxy resin composition -----.......

Materials, with high glass transition temperature and good flexibility. The epoxy resin composition includes a special epoxy resin, a pair of maleimide and barbitur. However, although the improved physical and electrical properties provided by the composition can be used for 1C ----- 4- The paper ruler A applies the Chinese national standard (CNS) A4 size (210X297 mm) 83.3.10,000 (谙 Please read the precautions on the back before filling out this page) Order printed by the Ministry of Economic Affairs, China Standards Bureau, Shellfisher Consumer Cooperatives 46 626 A7 ______B7________ V. Description of the invention (3) The substrate of the package, but it is not suitable for use as an adhesive. US Patent No. 5,268,432 discloses the use of bismaleimide and barbituric acid with polyamide imidate and Epoxy resin to improve Tg and heat resistance and reduce brittleness without phase separation. Its disadvantages are that many high-boiling solvents are used, it is not easy to process, it does not contain hardeners and catalysts, it is not easy to do B-stage control, and high temperature pressure is required. The high heat-resistant adhesive disclosed in Japanese Patent No. 61-98782 is based on polyamidoamine (PAI) and bismaleimide to increase Tg and improve heat resistance. Its disadvantages will cause the surface The shrinkage and flatness are deteriorated. Known resins are not conducive to the production of flexible printed circuit boards, and are prone to shortcomings such as brittleness, heat resistance and chemical resistance. They have developed a flexible printed circuit board that can produce good toughness, high heat resistance and high chemical resistance and is easy to process. The main purpose of the present invention is to provide an improved adhesive composition for high-density 1C packaging processes, and in particular to provide an improved epoxy resin-based adhesive composition, which can increase Thermal and chemical stability 'make it resistant to thermal dispersion in the manufacture of high density and / or multilayer integrated circuit boards. Another object of the present invention is to provide an improved epoxy resin-based adhesive composition, which After coating on the substrate and hardening, it has strong adhesion to the substrate and good product flatness. The adhesive composition based on the improved epoxy resin according to the present invention is a national standard (CNS specification (CNS specification ( 210 > < 297 mm) 83. 3.10,000 I ^ J: Order alone, /, '(Please read the back · t note the negative items before filling out this page) Α7 Β7 4.6 62 6 2 | > It is stated (4) that the bismaleimide resin is firstly introduced into barbituric acid (BTA) or its derivative, dissolved in a co-solvent, and then mixed with epoxy resin and carboxylated propionitrile (carboxylated). acrylonitrile rubber (CTBN) methyl ethyl acetone solution of softener, catalyst and hardener is mixed and agitated to obtain strong toughness, no cracking and brittle resin material, excellent processability, high heat resistance and high drug resistance Properties, which is conducive to manufacturing high-quality multilayer flexible printed circuit boards. The improved epoxy resin-based adhesive composition includes the following components: (1) bismaleimide and its derivatives, the structural formula is: (Please fill in the notes on the back before filling in this page) 0 〇

-丁 " '•' Printed by the Ministry of Economic Affairs and the Central Bureau of China Bureau, Beigong Consumer Cooperatives, where R can be-< CH2) 2-, 4CH2) r, one (CHi qcwhr-,

(2) The structural formula of barbituric acid and its derivatives is: 0

II 0 = C \ c ^ C = 0 This paper size is applicable to China National Standards (CNS > A4 Grid (21 OX297)) 83. 3.10,000 Printed by Shelley Consumer Cooperative, Shenyang quasi bureau, Ministry of Economic Affairs Α7 Β7 V. Description of the invention (5) Its center and R2 may be -Η '-CH3, -C6H5, -CH (CH3) 2, -CH2CH (CH3) 2, -CH2CH2CH (CH3) 2 »—— (CH2) 2CH3 CH, the method of preparing bismaleimide modified by barbituric acid or its derivative is: mixing barbituric acid or its derivative with bismaleimide in a molar ratio of 1: 20 ~ 1: 3 was added to a co-solvent (mixture of methyl ethyl acetone and 7 · butyrolactone) so that the solid content was 30 to 60 weight percent, and then the barbituric acid and the bismaleimide were mixed at about The reaction is performed at 100 ~ 130 ° C for about 1 ~ 6 hours to form the bismaleimide modified by barbituric acid. (3) The epoxy resin may be: ① Tetragly cedyl methyl enedi aniline) ② diglycidyl ortho-phthalate ③ diglycidyl ether of bisphenol A ④ glycidyl ether of novolac ⑤ epoxy Toluene (epoxy cresol novolac) (4) Carboxylated acrylonitrile (CTBN). (5) Hardener: it can be ethylene diamine, m-diamine benzene, trimellitic acid ethanol, polythiol or methyl Tetrahydrophthalic anhydride mixed with ethylene glycol and so on.

(6) Catalyst: may be 1-benzyl-2-methylimidazo or cyanomethylethyl imidazo D (7) methyl ethyl ketone (MEK) 〇 (8) 7 -T-bytyrolactone. The paper size is in accordance with the Chinese National Standard (CNS) A4 scale (210 X 297 mm) 83. 3.10,000 (please read the precautions on the back of the product first to write this page) Order

" V 46 626 ^ 4s A7 B7 V. Description of the invention (6) (9) Surfactant. Other additives such as a coupling agent, a defoaming agent, and a UV stabilizer may also be added to the adhesive composition of the present invention. The final adhesive composition preferably has a total solid content of 40-50% by weight. Detailed description of the preferred embodiment (1) Preparation of bismaleimide modified by barbituric acid: The structural formula of bismaleimide used in the present invention is: 0 0

Where R can be-< CH2) plant, gas CH2V, one (CH2 ·) plant, CH, —CH2—C—CH2—CH —ch2—ch2— CH,

(Please read the notes on the back before filling in this K.) The structural formula of the barbituric acid and its derivatives used to modify bismaleimide to be printed by the male workers' consumer cooperative in the Ministry of Economic Affairs is as follows. 0 II 0 = C, / C = 0 Its center and ruler 2 can be -Η, -CH3, -C6H5, -CH (CH3) 2, -CH2CH (CH3) 2, -CH2CH2CH (CH3) 2 '— CH, This paper size applies Chinese National Standard (CNS) A4 specification (210X297 mm) 81 3.10,000 Printed by the Shellfish Consumer Cooperative of the Central Bureau of Standards of the Ministry of Economic Affairs 6 626 5. Description of the invention (7) Preparation of barbituric acid or its derivatives The modification method of bismaleimide is to add barbituric acid or its derivative and bismaleimide in a molar ratio of 1: 20 ~ 1: 3 to a co-solvent (methyl ethyl acetone). Mixed with τ-butyrolactone) so that the solid content is 30 to 60 weight percent, and then the barbituric acid and the bismaleimide are reacted at about 100 to 130 ° C for about 1 to 6 hours to form The barbituric acid modified bismaleimide. (2) Preparation of epoxy resin adhesive composition: A methyl ethyl acetone solution having a solid content of 30 to 70% by weight is prepared. The solid composition comprises 7 to 25 weight percent of carboxylated acrylonitrile (CTBN) containing 19 to 41 weight percent acrylonitrile, and 45 to 70 weight percent of epoxy resin, hardener, and catalyst as described above. The equivalent ratio of the hardener to the epoxy resin is 0.9 to 1.1, and the content of the added catalyst is about 3 to 7 phr (parts per 100 parts of the resin). The methyl ethyl acetone solution is mixed with (1) to form a final epoxy resin-based adhesive composition having a solid content of about 40 to 50 weight percent. The hardening agent may be a mixture of methyltetrahydrophthalic anhydride and ethylene glycol, and ethylenediamine, m-diamined apple, trimellitic acid ethanol or polythiol; and the catalyst may be 1-benzyl-2-methyl Imidazo (l-B2Mz) or cyanomethylethylimidazo (2-E4Mn-CN). Other additives such as a coupling agent, a defoaming agent, and a UV stabilizer may also be added to the adhesive composition of the present invention. The foregoing and other objects and features of the present invention will be more prominent through the following descriptions of the preferred embodiments. It should be understood that these descriptions are only used to illustrate the operation results of the present invention under better conditions, rather than Attempt to apply this paper size to the Chinese national standard (CNS) A4 (210X297mm) 83. 3 · 10,000 (please read the note on the back before filling this page)

46 626 4? Λ7 ________B7 5. The description of the invention (“) does not limit the scope of the invention, and other modifications and changes made without departing from the spirit of the invention are the intention of the present invention. Example 1 56.1 g of bismaleimide and 7 "g of barbituric acid were dissolved in a co-solvent of 20.7 g of methyl ethyl acetone and 83.0 1-butyrolactone. After 3 hours of reaction with not: 20 grams with 14.2 grams of epoxy resin, 2.65 grams of methyltetrahydroanhydride (MTHPA), 0.09 grams of cyanomethylethylimidazo (2E4Mn-CN), and 42.24 grams of carboxylated acrylonitrile (CTBN) solution (20% The methyl ethyl acetone solution) 'After fully stirring and mixing, an epoxy resin-based adhesive composition is formed. All the above components are uniformly coated on a polyimide (PI) film, and placed in an oven to bake at 150 ° C for 2 to 4 minutes. Thereafter, the polyurethane film coated with the modified epoxy resin was laminated with a copper foil, and laminated at a rate of 100 cm / min at 100 ° C. The final product is cured at 180 ° C for 1 to 4 hours to form a sandwich product of polyimide (PI) / adhesive / copper foil. The product was then subjected to hot-pressing dry film 'exposure, development, etching, and film drying to obtain copper wires with a line width of 1/8 inch, and then tested for strength, heat resistance, and chemical resistance. Peel strength refers to the bonding strength between polyimide (PI) / adhesive / copper foil layer, using a Shimadzu AG5000A tensile machine to perform a peel test at a peel speed of 25mm / niin; the heat resistance test uses a tin furnace test (solciemg iest), The method is to immerse polyimide (PI) / adhesive / copper foil in a tin furnace at 288 ° C for 1 to 5 minutes, then take it out, and then dry and test the strength of the adhesive; Imide (PI) / adhesive / copper foil is immersed in 25t methyl ethyl acetone. It is taken out after 50 ~ 50 minutes, and dried after _10_ sheets. Applicable to Chinese national standards (CNS > A4 specifications (210X297 &)) ( Please read the notes on the back before filling out this page) Equipment · i Ministry of Economic Affairs t Central Standards Bureau W: printed by industrial and consumer cooperatives A7 B7 4 6 626 ^ The explanation is clearer than the formula t 9 Same as in Example 1 and Process, but the formulation does not contain bismaleimide and barbituric acid modifiers, the polyimide / adhesive / copper foil laminate material prepared, and the adhesive strength, heat resistance and drug resistance The results are shown in Table 1. Table 1. Test conditions Peel Strength {! Mnj 实Example 1 Comparative Example 1 Dip tin at 288 ° C for 0 minutes 9.8 10.1 Dip tin at 288 ° C for 1 minute 9.7 7.6 Dip tin at 288 ° C for 2 minutes 9.2 5.3 Dip tin at 288 ° C for 3 minutes 8.9 3.7 Dip at 288 ° C Tin 4 minutes 8.3 2.1 Immersion tin at 288 ° C for 5 minutes 7.1 1.1 Immersion in methyl ethyl acetone 0 minutes 9.8 10.1 Immersion in methyl ethyl acetone for 1 minute 9.8 7.0 f Man in methyl ethyl acetone for 2 minutes 9.4 5.1 Immersion in methyl ethyl acetone for 3 minutes 8.6 3.2 Immersion in methyl ethyl acetone for 4 minutes 7.8 2.0 Immersion in methyl ethyl acetone for 5 minutes 6.9 1.0 Ministry of Economic Affairs, Central Bureau of Commerce, Industrial and Commercial Cooperatives, India (Please read the note on the back and then fill in the "This page")-Table 1 clearly shows that the improved epoxy resin-based adhesive composition of the present invention has excellent efficacy, especially related to In terms of drug resistance and heat resistance, it should be noted that if different epoxy resins or other ingredients that do not contain the composition of the present invention, such as bismaleimide, etc., have poor peel strength. In addition, the present The composition of the invention can also be applied to other systems. For example, the copper foil used in the invention can be aluminum Chromium, titanium, nickel, gold, silver, etc. are substituted; and in addition to polyimide, it is also suitable for other polymers. 4J- This paper ruler applies the national national standard (CNS) A4 specification (2 丨 〇 X 297 mm) 83.3.10,000

Claims (1)

46626 ^ A8 B8 C8 D8 VI. Application for patent repairs mx The Ministry of Economic Affairs Bureau of the Ministry of Economic Affairs, Machining and Consumer Cooperatives printed a policy !. An adhesive composition, including: (1) The weight percentage is 3% to 30% of the total solids content % Of bismaleimide modified with barbhuric acid; (2) weight percentage of epoxy resin with a total solid content of 30% to 70%; (3) weight percentage of ^ 19% ~ 41% carboxylated acrylonitrile rubber of propylene navel; (4) hardener is selected from ethylenediamine, m-diamined benzene, trimellitic acid ethanol, polythiol and formazan The number of equivalent groups of epoxy tetrahydrophthalic anhydride and ethylene glycol is 0.9 to 1.1 times the equivalent number of epoxy resins; and (5) catalysts with a weight percentage of 0.1% to 3% of the total solid content It may be 1-;: hexyl-2-methylimidazo or cyanomethylethylimidazo;-wherein the epoxy resin is selected from the group consisting of tetraglycidyl methylidene diamine and diacid glycerol o-benzene A group of diacids, bisphenol A glycidyl ether, phenol glycidyl ether, epoxy cresol aldehyde, and the aforementioned derivatives. 2. The adhesive composition according to item 1 in the scope of the patent application, wherein the bismaleimide modified by barbituric acid is bismaleimide and barbituric acid or barbituric acid. The derivative is prepared by reaction, and the structural formula of the bismaleimide is: 0 0 people. Human N -R -N γ0 〇0 where R can be-(CH2h,-(CH2V, -ΘΗ2ν •, -(CH2b CH, ChL -CH: —C—CH2—CH —CH2—CH ^ -CH, (Please read the precautions on the back before filling this page) 袈 · Ϊ The paper size is in accordance with China National Standards (CNS) A4 (210 × 29 ^ >%) 4 6 626 ^ Α8 Β8 C8 D8 Scope of patent application- < 〇 > -0- < 〇 >-'^ -7〇) _CH2- < p And the structural formula of the barbituric acid or its derivative is 0 'NH 〇 = c- ^ c ^ c = 〇Rr where & and 112 can be -Η, -ch3, -c6h5, -ch (ch3) 2 , -Ch2ch (ch3) 2 -ch2ch2ch (ch3) 2, or one— (ch2) 2ch3 CH, (Please read the note on the back before filling in this page) "Installation · 3. As the second scope of the patent application The adhesive composition described above, wherein the step of modifying the bis-maleimide with barbituric acid or its derivative is: (1) combining barbituric acid or its derivative with bismaleic acid The imine is added to the co-solvent at a molar ratio of 1: 20 ~ 1: 3; (2) reacting the barbituric acid with the bismaleimide to form the barbituric acid-modified shuangma Laimidine. 4. The adhesive composition as described in item 3 of the patent application, wherein (1) the co-solvent is a mixture of methyl ethyl acetone and r-butyrolactone, and the barbiturate The solid content of the acid and the bismaleimide is 30 to 60% by weight: and (2) the barbituric acid reacts with the bismaleimide at a temperature of 100 to 130 ° C for 6 hours. 5. The adhesive composition as described in item 1 of the scope of patent application, wherein the total The solid content is 40 to 50% by weight. 6. The adhesive composition 1 described in item 1 of the scope of the patent application, wherein the paper size is further changed to the Chinese National Standard (CNS) M specification (21OX: 20mm) * tT Printed by the Central Bureau of Standards, Ministry of Economic Affairs, Consumer Cooperatives, Central Standards of the Ministry of Economics, Employees' Cooperatives, printed A8 BS C8 m A, the scope of patent application includes a coupling agent, defoaming agent and UV stabilizer in one step. A method for combining a metal film and a polymer substrate, including: (A) preparing an adhesive agent> comprising: (1) a weight percentage of 3% to 30% by weight of barbituric acid (barbituric acid :); Bismaleimide; (2) Epoxy resin with a total solid content of 30% to 70%; (3) Carboxylated acrylonitrile containing 19% to 41% acrylonitrile by weight (carboxylated acrylonitrile rubber)-(4) The hardener is selected from the group consisting of ethylenediamine, m-diamined benzene, trimellitic acid ethanol, polythiol, and methyltetrahydrophthalic anhydride mixed with ethylene glycol. Ethnic groups, the equivalent number of epoxy equivalent equivalent number is 0.9 ~ 1. 1 times; and (5) a catalyst with a weight percentage of 0.1% to 3% of the total solid content, which may be 1-fluorenyl-2-methylimidazo or cyanomethylethylimidazo; wherein the epoxy The resin is selected from the group consisting of tetraglycidylidene diphenylamine, diglycidyl phthalic acid, bisphenol + A glycidyl ether, novolac glycidyl ether, epoxycresol aldehyde, and the aforementioned derivatives. (B) applying the adhesive of (A) between the metal film and the polymer substrate; and (C) laminating and heating to form a sandwich-shaped product. 8. The method of combining a metal film and a polymer substrate as described in item 7 of the scope of the application for patent. The method 'wherein the bismaleimide modified by barbituric acid is based on the Shuangma ^ paper standard in China搮 芈 (CNS) A4 specification (210X29 ^ cent) (Please read the precautions on the back before filling out this page) Binding-Binding. 4 G G26 4. A8 B8 C8 D8 Patent application scope for aramide and barbitur It is prepared by the reaction of acid or a derivative of barbituric acid, and the structural formula of the bismaleimide is: 0 0 ιΑ 入 V, γ 0 0, φψ where R may be ~ (CH2h '— (CH2) ^ , A 1-(CH2) j2 CH, ch3 ch3I f —CH2—C —CH2— (I ch3 ~ " < \ ^ / > ~ o ~~, and / or the barbituric acid or its derivative, the structural formula of the organism is: 0 -C \ 丽 I 〆0 = 0 ΰσ〇 \ (Please read the notes on the back before filling in this page),? Τ Printed by the Central Consumers ’Bureau of the Ministry of Economic Affairs and the Consumer Cooperatives, where Gen and 112 can be -Η, -CH3,- C6H5, -CH (CH3) 2, -CH2CH (CH3) 2, -CH2CH2CH (CH3) 2, or a γΗ _ (ch2) 2ch3 ch3 <? \ C 9. Combination as described in item 7 of the scope of patent application A method for metal film and polymer substrate, wherein the step of modifying bismaleimide with barbituric acid or its derivative is: (1) combining barbituric acid or its derivative with bismaleic acid Lamine is added to the co-solvent at a molar ratio of 1:20 to 1: 3; (2) reacting the barbituric acid with the bismaleimide to form the barbituric acid i. L · / This paper has been re-used in China (CMS) A4 size (210X297 丨 roll) α2 6 φ issued < _§__ VI. The bismaleimide modified by the scope of patent application. Ί 0. Such as Method for combining metal film and polymer substrate as described in claim 9 U) The co-solvent is a mixture of methyl ethyl acetone and 7-butyrolactone, and the solid content of the barbituric acid and the bismaleimide: 30% by weight; and (2 ) The barbituric acid reacts with the bismaleimide at a temperature of 100 to 0 ° C for 1 to 6 hours. Π. The combination of a metal film and a polymer base as described in item 7 of the scope of patent application Wood method, wherein the total solids content is 40 to 50 weight percent. 12. The method for combining a metal film and a polymer substrate according to item 7 of the scope of the patent application, wherein the polymer substrate is selected from the group consisting of polyimide, polyimide, and polyimide A group of amine ethers, polyamides, and polyamides. (Please read the precautions on the back before filling this page) Binding. Ordering. 1- i- Printed by the Consumers' Cooperative of the Central Bureau of Standards of the Ministry of Economic Affairs This paper is printed in accordance with Chinese Painting National Standards (CNS) A4 (210 × 29%) ) Bulletin L— —---- Application date contains η and case number category (the above columns are filled out by this bureau) A4 C4 Collection Patent Specification Chinese Invention New Name High Performance Adhesive Compositions English High-Performance Adhesive Compositions Name Nationality Chen Zhiqiang, Pan Jinping, Liu Shufen Chinese National Costume Invention Creator, Residence, Residence, Hsinchu County, No. 41, Chengbei Street, Hsinchu City No. 52, Lane 76, Dongming Guangming Road, Hsinchu City, Section 1, Guangfu Road, Hsinchu City, No. 7, Lane 1, Lane 7, Q4, 4th Floor. Name (name). Sanju, Residence (Office) Name of Representative No. 195, Section 4, Zhongxing Road, Zhudong Township, Hsinchu County Government Paper Size Applicable to Chinese National Standard (CNS) A4 Specification (210X 297 mm > 46 626 4? Λ7 ________B7 5. The description of the invention (“) does not limit the scope of the invention, and other modifications and changes made without departing from the spirit of the invention are the intention of the present invention. Example 1 56.1 g of bismaleimide and 7 "g of barbituric acid were dissolved in a co-solvent of 20.7 g of methyl ethyl acetone and 83.0 1-butyrolactone. After 3 hours of reaction with not: 20 grams with 14.2 grams of epoxy resin, 2.65 grams of methyltetrahydroanhydride (MTHPA), 0.09 grams of cyanomethylethylimidazo (2E4Mn-CN), and 42.24 grams of carboxylated acrylonitrile (CTBN) solution (20% The methyl ethyl acetone solution) 'After fully stirring and mixing, an epoxy resin-based adhesive composition is formed. All the above components are uniformly coated on a polyimide (PI) film, and placed in an oven to bake at 150 ° C for 2 to 4 minutes. Thereafter, the polyurethane film coated with the modified epoxy resin was laminated with a copper foil, and laminated at a rate of 100 cm / min at 100 ° C. The final product is cured at 180 ° C for 1 to 4 hours to form a sandwich product of polyimide (PI) / adhesive / copper foil. The product was then subjected to hot-pressing dry film 'exposure, development, etching, and film drying to obtain copper wires with a line width of 1/8 inch, and then tested for strength, heat resistance, and chemical resistance. Peel strength refers to the bonding strength between polyimide (PI) / adhesive / copper foil layer, using a Shimadzu AG5000A tensile machine to perform a peel test at a peel speed of 25mm / niin; the heat resistance test uses a tin furnace test (solciemg iest), The method is to immerse polyimide (PI) / adhesive / copper foil in a tin furnace at 288 ° C for 1 to 5 minutes, then take it out, and then dry and test the strength of the adhesive; Imide (PI) / adhesive / copper foil is immersed in 25t methyl ethyl acetone. It is taken out after 50 ~ 50 minutes, and dried after _10_ sheets. Applicable to Chinese national standards (CNS > A4 specifications (210X297 &)) ( Please read the notes on the back before filling in this page.) Equipment · i Ministry of Economic Affairs t Central Standards Bureau W: Printed by Industrial and Consumer Cooperatives 1 6 626 ^ 1 Chinese Abstract (The name of the invention is a high-performance adhesive composition. This invention is about An adhesive composition based on an improved epoxy resin, comprising (I) bismaleimide modified with barbituric acid; (2) an epoxy resin selected from tetraglycidyl forked Diphenylamine, diacid glycerol, phthalic acid, diphenyl Groups of phenol A glycidyl ether, phenolic glycidyl ether, epoxy cresol aldehyde, and the aforementioned derivatives; (3) carboxylated acrylonitrile containing 19 to 41 acrylonitrile by weight; rhenium hardener; and (5) Catalyst. Abstract of the English invention (Name of the invention: High-Performance Adhesive Compositions An improved epoxy based adhesive composition contains: (1) a barbituric acid modified bismaleimide; (2) an epoxy resin selected from the group consisting of tetraglycidylraethylenedianiline, diglycidyl ortho-phthalate, diblycidyl ether of bisphenol A. glycidyl ether of novolac, and epoxy cresol novolac; (3) a oarboxylated acrylontrile rubber containing between 19 and 41 wt% of acrylontrile; (4) a hardening agent and (5) a catalyst. Economy Lang Zhongshi 嚷 L.cr h J (Please read Ϊ-Notes on the previous page and fill in each page on this page 櫊) This paper size is applicable to China National Standard (CNS) A4 specification (21 OX297 mm) 46626 ^ A8 B8 C8 D8 VI. Application for patent scope repair mx The Ministry of Economic Affairs Bureau of Standards and Labor Bureau Consumers Cooperatives printed a policy! The agent composition comprises: (1) a weight percentage of 3% to 30% of a total solid content of bismaleimide modified with barbhuric acid; (2) a weight percentage of the total Epoxy resin with a solid content of 30% to 70%; (3) Contains ^ 19% to 41% by weight of carboxylated acrylonitrile rubber; (4) The hardener is selected from ethylene glycol A group of amines, m-diamined benzenes, trimellitic acid ethanol, polythiols, and methyl tetrahydrophthalic anhydride mixed with ethylene glycol. The number of equivalents is 0.9 to 1.1. And (5) a catalyst with a weight percentage of 0.1% to 3% of the total solid content, which may be 1-:: eyl-2-methylimidazo or cyanomethylethylimidazo;-wherein the ring The oxyresin is selected from tetraglycidyl methylidene dianiline, diacid glycerol phthalic acid, bisphenol A glycidyl ether, phenolic glycidyl A group of oleyl ether, epoxycresol aldehyde, and the aforementioned derivatives. 2. The adhesive composition according to item 1 in the scope of the patent application, wherein the bismaleimide modified by barbituric acid is bismaleimide and barbituric acid or barbituric acid. The derivative is prepared by reaction, and the structural formula of the bismaleimide is: 0 0 people. Human N -R -N γ0 〇0 where R can be-(CH2h,-(CH2V, -ΘΗ2ν •, -(CH2b CH, ChL -CH: —C—CH2—CH —CH2—CH ^ -CH, (Please read the precautions on the back before filling out this page) 袈 · Ϊ The size of this paper is in accordance with China National Standards (CNS) A4 (210 × 29 ^ >)