TW526222B - Polyimide for high temperature adhesive - Google Patents

Abstract

Disclosed is polyimide useful as an adhesive for semiconductor assemblies. With excellency in thermal resistance and adhesive strength at high temperatures, the polyimide adhesive is based on the polyimide represented by the following formula II which can be prepared through the thermal or chemical imidization of the polyamic acid represented by the following formula I.

Description

526222 A7 B7 V. Description of the invention (丨) Field of the invention The tree of the present invention is a kind of polyhime_high temperature_, also refers to—H kinds of polyS imine 1 ¾ glue 'has excellent barrel temperature stability 丨 locking adhesive strength, and it has Good processability, and also a kind of insulation used as material for the electronics industry. The tape has high electrical insulation and thermal resistance, and can be bonded by hot melt. Meanwhile, the present invention relates to a lead holder and a semiconductor device using the tape. Background of the Invention Polyimide obtained by reacting a tetracarboxylic acid dianhydride with a diamine has various excellent properties and good thermal stability properties, and will be widely used in the field of high temperature stability thereafter. In addition to excellent high-temperature stability, 'Polyimine' also has good mechanical strength, dimensional stability in appearance, flame retardancy, and electrical insulation. Transportation machinery, also used in high temperature resistant adhesives of various high performance materials in these fields. However, the conventional polydrum is generally excellent in thermal stability, but has poor melting feasibility due to its high softening point. On the other hand, resins developed to improve the feasibility of melting have poor high temperature stability. Therefore, the performance of polyimide still has its advantages and disadvantages. Printed by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economic Affairs on the use of traditional polyimides, such as in the manufacture of film, line coating, panels, or adhesives, the linear linkage of traditional polyimides As a result, high tight bundle densities are generated between the chains, and the movement of the chains is restricted even at high temperatures. Therefore, the conventional polyimide has excellent thermal stability like a thermostat ', but its melting feasibility and adhesion are poor. In addition, the melting point and softening point of the meltable polyimide, which is particularly used for adhesion, is lower than that of the conventional polyimide. Therefore, the meltable polymer garden has poor thermal stability and high thermal expansion coefficient (C.T.E,). Polyimide adhesives or tapes used for various types of integrated circuit packaging tapes need to be subject to mass during the bonding process. 3 This paper size is applicable to China National Standard (CNS) A4 (210X 297 mm) 526222 Ministry of Economic Affairs A 7 __B7__ printed by the Central Standards Bureau's Consumer Cooperative. V. Description of the Invention (fork) Such as 1C wafer substrate, 1C wafer or protective layer on the lead holder has good feasibility of melting, and good humidification. After bonding, even in subsequent high-temperature procedures such as wire bonding and resin molding, the excellent adhesive properties and thermal stability of the adhesive are very important to ensure the reliability of the semiconductor package. The invention is implemented in order to obtain good melting feasibility and good stability. Another object of the present invention is to spread a kind of insulating tape using a polyimide adhesive, which tape can maintain excellent insulating properties for a long life. The insulating tape also has appropriate adhesive properties for high temperatures at a temperature of 450 degrees Celsius (45 ° C) (ie, the temperature at which the adhesive is applied), in a short time of not more than ten (10) seconds. Adhesive, and its adhesive strength is sufficient for different semiconductor materials. In addition, the insulating tape will not cause pollution and damage to the wire adhesion of the tag frame and the collective chip surface. The insulating tape has extremely high heat resistance enough to withstand wire adhesion The heating effect in the step can prevent any slight movement of the lead wire, so that the wire bonding strength is sufficient to obtain excellent electronic reliability. In order to meet the aforementioned various properties, a small amount of triamine or tetraamine is specifically used as a single Substituting diamines with polyacids or poly155 amines. Triamines or tetraamines are very useful in breaking the chain structure to reduce the inter-chain tight bundle density and increase the melting feasibility and adhesion properties of polyimide. The cross-linking effect of amines or tetraamines, in particular: ¾ wire bonding and the temperature in the resin molding process can increase the thermal stability of the polyimide. SUMMARY OF THE INVENTION It is to provide polyimide and its poly-precursor. In addition to the exceptionally high temperature stability inherent in polyimide, both have excellent feasibility of melting and excellent high-temperature adhesion. They are very suitable for many purposes. The present invention provides a polymer having recurrent individuals represented by the following molecular formula one: Please read the memorandum first. The matter is then written on the page of the book. The paper size is applicable to the Chinese National Standard (CMS) A4 specification ( 210X297) 526222 A7 B7 V. Description of the invention (3) HOOC COOH X ~ HNCO, XCONH—R1 HOOC COOH χ HNC〇 / CONH- HOOC X COOH 〆-m F -HNCO '\ CONH— R3- [Molecular formula one] Wherein R is a trivalent organic group; R1 is a divalent organic group; R2 is a trivalent or tetravalent organic group; R3 is a divalent organic group represented by the following formula:

Page CH0 CHa -Si—fO-Si-^ * T-R4-

ChU CH0 where R4 is an olefin group containing 0-20 carbon atoms; and V is the number of recurrent individuals; 1, m and η are in the range of 1 / (m + n) from 99.985 / 0.015 to 80/15 Expressed in molar ratios, and m / α + η) ranging from 1/2000 to 500/1, and the corresponding number of molars of recurrent individuals under the condition of expressed in molar ratios. The present invention further provides a rosin acid resin, wherein the carboxyl group in the polyacrylic acid resin is esterified, and the poly s acid resin or the corresponding rosin resin is dehydrated or dehydrated. A jujube resin was obtained from the alcohol ring box. The present invention also provides a polyacid resin of molecular formula one, which is prepared by reacting a diamine compound including a novel triamine compound or a tetraamine compound with a dianhydride in an organic solvent. The precursor polymer of the present invention is polyphosphatic acid, and its obtaining method is as follows: (1) A dianhydride having the following molecular formula 本: This paper size applies the Chinese National Standard (CNS) A4 specification (210X 297 mm).

Printed by the Central Labor Standards Cooperative of the Ministry of Economic Affairs% 526222 A7 B7 V. Description of the invention (if 0 0 ΛΛ 0 八 〆〇

'YY 〇〇 [Molecular Formula 贰] wherein R is a member selected from the group consisting of an aliphatic radical having two or more carbon atoms, a cycloaliphatic radical and a single aromatic radical, a condensation polyaromatic radical, and A tetravalent radical of a chemical group composed of a condensed polyaromatic radical, wherein the aromatic radicals are connected to each other by a chemical bond or a cross-linking action. Refer to the following examples as examples of the tetravalent radical R:

Printed by the Consumer Cooperative of the Central Bureau of Standards of the Ministry of Economic Affairs, a diamine with the following liver-type ginseng: h2n-ri-nh2 (ginseng) where R1 is selected from the group consisting of aliphatic radicals, cycloaliphatic radicals, and monoaromatics Free radicals, condensed polyaromatic paper This paper applies the Chinese National Standard (CNS) A4 specification (210X297 mm) 526222 A7 B7 V. Description of the invention (5) Chemical groups consisting of aromatic free radicals and uncondensed polyaromatic free radicals Divalent radicals, in which the aromatic radicals are connected to each other by a chemical bond or a cross-linking action. The following example can be referred to as an example of this divalent dissociation.

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◎ CF CH; CH, CH: Grain content. · € π〇ά Printed by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economic Affairs

(3) —Triamine with the following molecular formula

H2N \ H2N V / NH2 R2—NH2 R2X h2n H2l · \ ίΗ2 1Ί This paper size is applicable to the Chinese National Standard (CNS) A4 specification (210X297 mm) 526222 A7 B7 V. Description of the invention (厶) where R2 is one selected from A trivalent or tetravalent radical having a chemical group consisting of an aliphatic radical, a cycloaliphatic radical, a single aromatic radical, a condensed polyaromatic radical, and a non-condensed polyaromatic radical. Group radicals are linked to each other by a chemical bond or cross-linking. The following examples can be referred to as examples of the trivalent or tetravalent radical R2:

Printed by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economic Affairs (4) A diamine containing the following SILOXANE® oxane fractions: 〒h3 ch0 —R4_S »_ ^ 〇-Si- ^ R4-CH3 CH0 where R4 is a For hydrocarbon storage groups containing 0-20 carbon atoms, y is the number of recurrent individuals. Specific examples of the di-acrylic acid include aromatic tetracarboxylic acid dianhydrides, such as tetraethyl carboxylic dianhydride, tetrabutyl carboxylic dianhydride-cyclopentabutylene dianhydride, cyanuric dianhydride, 3,3'4A-di Benzophenonetetracarboxylic dianhydride, 2,2 ', 3,3 ~ benzophenonetetracarboxylic dianhydride, 3,3f, 4, V-biphenyltetracarboxylic dianhydride, 2, Y3,3'-biphenyl Tetracarboxylic dianhydride, 2,2-bis (3,4-diphenylbenzene) propane, two paper sizes are applicable to China National Standard (CNS) A4 specification (210 × 297 mm) 526222 A 7 B7 V. Description of the invention (7 ) Printed Anhydride, 2,2-Bis (2,3-Di-Compound Benzene) Propane Dianhydride, Bis (3,4-Dicarboxybenzene) Ethyl Dianhydride, Bis (2, 3-dicarboxybenzene) ether dianhydride, bis (3,4-dicarboxybenzene dianhydride, bis (2,3 ~ dicarboxybenzene) stone dianhydride 'bis (2,3-dicarboxybenzene) methane di Anhydride, bis (3,4-dicarboxybenzene) methane dianhydride, U-bis (2, hudicarboxybenzene) ethane dianhydride, 1,1_bis (3,4-dicarboxybenzene) ethane dianhydride Bis (2,3, dicarboxybenzene) ethane dianhydride, 1,2-bis (3,4-dicarboxybenzene) ethane dianhydride, 1,3-bis (2,3-dicarboxyphenoxy) Phthalic anhydride, ls3-bis (3,4-dicarboxyphenoxy) phthalic anhydride, 1,4-bis (2,3-dicarboxyphenoxy) phthalic anhydride 'Μ- (3,4-Dicarboxyphenoxy) phthalic anhydride, 2,3,6,7-tetracarboxylic dianhydride, 1,4,5,8-tetracarboxylic dianhydride, 1,2,5,6-tetracarboxylic Dianhydride, 1,2,3,4-benzenetetraresidual dianhydride, 3,4,9 · 10-Tanjuku-Jinjiye, 2,3,6,7 · Tetrakis dianhydride, ι, 2,7 , 8-phenanthrenetetracarboxylic dianhydride, 2,2-bis (3,4-dicarboxybenzene) -1,1,1,3,3,3-pentafluoromethane dianhydride, 2,2-bis (2, 3-Di-cenebenzene) -1,1,1,3,3,3-pentafluoromethane dianhydride, 1,3-bis [4- (1,2-dicarboxy) phenoxy] phthalic anhydride, 1Λbis [4- (1,2-Dicarboxy) phenoxy] phthalic anhydride, 1,4-bis [3- (i, 2-dicarboxy) phenoxy] phthalic anhydride, 1,3-bis [4- ( 1,2-Dimethyl-α, α-dimethyl] phthalic anhydride, 1,3-bis [3- (1,2, -di-end) -α, □ -dimethyl] phthalic anhydride, 1 , 4-bis [3- (1,2Γ dicarboxy) -α, □ -dimethyl] phthalic anhydride, 1,4-bis [4 · (1,2, · di-residual) -α, □ -di Methyl] phthalic anhydride, 2,2-bis [4- (4- (1,2, -di-end) phenoxy) .yl] methane dianhydride, 2,2-bis [4Κ3- (1,2, Dicarboxy) benzene_yl] methane dianhydride, bis [4- (4- (U-dicarboxy) phenoxy) base dianhydride, bis [4- (3- (1,2Γ diresidual) phenoxy) group ] Ketone dianhydride, bis [4- (4- (1,2,2Γ di-end) phenoxy) yl] stone wind dianhydride, bis [4- (3 · (1,2,2Γ di-end) phenoxy) Toilet dianhydride, bis [4- (4- (1,2, -di-end) phenoxy) yl] thiodianhydride, bis [4- (3- (1,2, -di-end) phenoxy) yl] Sulfuric anhydride, bis [Zhong K1,2Γ dijun) benzenefanyl H, l, l, 3,3,3-hexachloromethane dianhydride and bis [4 · (3- (1,2, -dijun) benzene (Oxy) group] 4,1,1,3,3,3-hexachloromethane dianhydride, ethylene glycol bis (anhydrous-triphenylhexamethylene salt). In addition to the aromatic tetracarboxylic dianhydrides, aliphatic tetracarboxylic dianhydrides may be used as long as their use does not deteriorate the heat resistance. Preferred examples of such di-fields include aliphatic dicarboxylic acid difluorene, such as 5-2 (2,5-didioxytetrahydro); methyl-3 * cyclohexane-1,2-dicarboxylic dianhydride , 4- (2,5-dioxetane-3-yl) -tetrachloro 4,2-dicarboxylic dianhydride, bicyclic (2,2,2) -7-ene-2,3,5,6 -Tetracarboxylic dianhydride, 1,2,3, cyclopentane tetracarboxylic dianhydride. This paper size applies to Chinese National Standard (CNS) A4 specification (210X 297 mm) 526222 A7 B7 5. Description of the invention (?) These dianhydrides can be used alone or in combination. Diamines that can be used in combination include, for example, m-benzenedioxane, 0-benzenedioxane, p-benzenedioxane, m-aminoaniline, 0-aminoaniline printed by the Consumer Cooperatives of the Central Standardization Bureau of the Ministry of Economic Affairs, 3-Chloro-4, 2-benzene dimer, 4-chloro-1,2-benzene dioxane, 2,3-diaminotoluene, 2,4-diaminotoluene, 2,5-diaminotoluene, 2,6 · diaminotoluene, 3,4-diaminotoluene, 3,5-diaminotoluene, 2, -methoxybenzenedioxane, 4, -methoxy4,2-benzenedioxane , 4, -methoxy-1,3-benzidine, benzidine, 3,3 ~ dimethylbenzidine, 3,3f-dimethoxybenzidine, 3,3 ^ dichlorobenzidine, diamine Amino diphenyl ether, 3, 1-diamino diphenyl ether, 4, 4, diamino diphenyl ether, 3, 3 ^ diamino diphenyl sulfur, 3, 4'-diamino diphenyl sulfur, 4,3'-diaminodiphenylsulfan, 3,3 ^ diaminodiphenylsulfanfan, 3, -diaminodiphenylsulfanfan, 4, -diaminodiphenylsulfanfan, 3 , 3 ^ diaminodibenzene, 5,3,4f-diaminodibenzene, 5,4,4 diaminodiphenyl, 5,3,3 ^ diaminobenzophenone, 3,4 '-Diaminobenzophenone, 4,4'-Diaminobenzophenone, 3,3 ~ Diaminodiphenylmethane, 3,4 ~ Di Diphenylmethane, 4,4 ^ diaminodiphenylmethane, bis [4- (3-aminephenoxy) benzenemethane, bis [4- (4-aminephenoxy) phenyl] methane, bis [ 3- (3-aminophenoxy) phenyl] methane, U-bis [4- (4-aminephenoxy) phenyl] ethane, 1,2-bis [4- (4-aminephenoxy ) Phenyl] ethane, 1,1-bis [4- (3-aminephenoxy) phenyl] ethane, 1,2, bis [4- (3-aminephenoxy) phenyl] ethane , 1,1-bis [4- (4-aminephenoxy) phenyl] propane, 1,2-bis [4- (4-aminephenoxy) phenyl] propane, 1,3-bis [4 -(4-aminephenoxy) phenyl] propane, 2,2-bis [4, (4-aminephenoxy) phenyl] propane, 1, l.bis [4- (3-aminephenoxy ) Phenyl] propane, 1,2-bis [4〇aminephenoxy) phenyl] propane, 1,3-bis [4- (3-aminephenoxy) phenyl] propane, 2, -2 [ 4- (3-aminephenoxy) phenyl] propane, 1,1-bis [4- (4-linoxy) phenyl] butane, i, 2-bis [Longanphenoxy) phenyl ] Butane, 1,3 hetero (4-aminephenoxy) phenyl] butane, 2,2-bis [4- (4-aminephenoxy) phenyl] butane, 2,3-bis [ 4 < 4-aminephenoxy) phenyl] butane, 1,1-bis [M3-aminephenoxy) phenyl] butane, 1,2-bis [4K3-aminephenoxy) phenyl] Butane, 1,3-bis [4- (3 · amine (Oxy) phenyl] butane, 1,4-bis [4- (3-aminephenoxy) phenyl] butane, bis [4- (3-aminephenoxy) phenylbutane, 2,3- Bis [4- (3-aminephenoxy) phenyl] butane, 2- [4- (fluorenaminephenoxy) phenyl] -2- [4-sunaminephenoxy) each tolyl] methane, 2-2-Bis [4- (4-aminebenzene-10] This paper size applies to Chinese National Standard (CNS) A4 specification (210X297 mm) 526222 A7 B7 V. Description of the invention (7) Oxy) each tolyl] methane , 2- [4- (4-aminephenoxy) phenyl] -2- [4- (4-aminephenoxy) -3,5f-xylyl] methane, 2.2-bis [4- (4 -Aminephenoxy) -3,5-xylyl] methane, 2,2-bis [4- (4-aminephenoxy) -1,1,1,3,3,3-hexafluoromethane, 2.2- bis [3- (4-aminephenoxy H, l, l, 3,3,3-hexafluoromethane, 2,2-bis [4 > (3-aminephenoxy) -1,1, 1,3,3,3-Hexafluoromethane, printed by 2.2-Bis [3- (3-aminephenoxy) -1,1,1,3,3,3- Hexafluoromethane, 1,3-bis (3-aminephenoxy) benzene, 1,3-bis (4-aminephenoxy) benzene, 1,4-bis (4-aminephenoxy) benzene, 1 4,4-bis (3-aminephenoxy) benzene, 4, -bis (3-aminephenoxy) diphenyl, 3,3 ~ bis (3-aminephenoxy) di Group, bis! ≫ (4-aminephenoxy) phenyl] ketone, bis [4- (4-aminephenoxy) phenyl] ketone, bis [4 ((3-aminephenoxy) phenyl) ] Ketone, bis [3- (3-aminephenoxy) phenyl] one, bis [4- (4-aminephenoxy) phenyl] sulfur, bis [3- (4-aminephenoxy) benzene Yl] sulfur, bis [3- (3-aminephenoxy) phenyl] sulfur, bis [4- (3-aminephenoxy) phenyl] sulfur, bis [4- (4-aminephenoxy) Phenyl] stone wind, bis [3- (4-aminephenoxy) phenyl] stone wind, bis [3- (3-aminephenoxy) phenyl] stone wind, bis [4- (3-amine Phenoxy) phenyl] phenyl, bis [4- (3-aminephenoxyphenyl) ether, bis [4- (4-aminephenoxy) phenyl] ether, bis [3- (3-aminebenzene Oxy) phenyl] ether, bis [3- (4-aminephenoxy) phenyl] ether, 1,4-bis [4- (3-aminephenoxy) phenyl] benzene, 1,3- Bis [4- (3-aminephenoxy) phenyl] benzene, 1,4-bis [4- (4-aminephenoxy) phenyl] benzene., 1,3-bis ['(4-amine (Phenoxy) phenyl] benzene, 4,4f-bis (3-aminephenoxy) winter methyl diphenyl, 4,4 '· bis (3-aminephenoxy) -3,3'-dimethyl Diphenyl, 4, -bis (3-aminephenoxy) -3,5-dimethyldibenzene, 4,4 ~ bis (3-aminephenoxy) -3,3,5,5 ~ tetra Methyldiphenyl, 4,4 ~ bis (3-aminephenoxy) -3,3 ~ dichlorodibenzene, 4,4 ~ bis (3-aminephenoxy) -3,5-dichlorodiphenyl, 4,4'-bis (3-aminephenoxy) -3,3% 5,5'-tetrachlorodiphenyl Benzene, 4,4 \ bis (3-aminephenoxy) -3,3 ~ dibromobiphenyl, 4,4'-bis (3-aminephenoxy) -3,5, dibromodiphenyl, 4 , -Bis (3-aminephenoxy > 3,3'5,5 ~ tetrabromodiphenyl, bis [4- (3 · aminophenoxy) -3-tolyl] sulfur, [4- (3 -Aminephenoxy)] [4- (3-aminephenoxy) -3,5-dimethoxyphenyl] sulfur, bis [4 (3-aminephenoxy) -3,5-dimethoxy Phenyl] sulfur, and 1,3- [4- (4-aminophenoxy), alpha., .Alpha.-dimethoxyphenyl] benzene. These diamines can be used alone or as a mixture. Triamines or tetraamines that can be used in combination, including, for example, U3-triamine benzene, 1,2,4-triamine benzene, 1,2,4,5- -Ί1 This paper size applies Chinese national standards ( CNS) A4 specification (210X 297 mm) 526222 A7 B7 printed by the Consumer Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs 5. Description of the invention U〇) Tetraamine, 3-aminobenzidine, 3,3'-diamine Aniline, 3,4,4 \ triaminodiphenyl ether, 3,3M, 4'tetraaminodiphenyl ether, 3,4,4 ^ triaminobenzophenone, 3,4, f-triamine Diphenylmethane, 3,3 M, 4'-tetraaminodiphenylmethane '3,4,4, -triaminodiphenylsulfide, 3,3M, 4'-tetraaminodiphenylsulfide, 3, 4,4, -triamine diphenyl stone, 3,3 'tetraamino diphenyl stone, 2,2-bis (3,4-diaminephenyl) -propane, 4,4, bis (3 , 4-diaminephenoxy) diphenyl, 2,2-bis [4- (3,4-diaminephenoxy) phenyl] -propane, 2,2-bis [3,4-diaminebenzene [Yl] -hexachloropropane, 2,2-bis (3,4-diaminephenoxy) phenyl] -hexachloropropane. These triamines or tetraamines can be used alone or as a mixture. Generally, polymers can be prepared by reacting di and triamine or tetraamine with dianhydride in an organic solvent. Organic solvents used in this reaction include, for example, N, NN-dimethylformamide, N, N-dimethylacetamide, N, N-diethylacetamide, N, N-dimethyl -Methoxyacetamidamine, N-methyl: hydrazone, 1,3-dimethyl-2-imidazolidine, N-methyl-caprolactam, 1,2-dimethoxyethyl Alkane, bis (2-methoxyethyl) ether, 1,2-bis (2-methoxyethoxy) ethane, tetrahydrofuran, 1,3-epoxyhexane, 1A epoxyhexane , Pyridine, methyl, pyridine, dimethylmethylene, dimethyl, tetramethyl, hexamethylphosphamide, m-methoxycresol, p-chloroamidine, and anisole. These solvents may be used singly or in combination of two or more. The manufacturing process of polyisocyanate lacquer is as follows: First, the preparation method of polyisocyanate lacquer which belongs to the precursor of polyimide is to place monodiamine and triamine or tetraamine as N-methyl hydrazone. After the pyridine is dissolved in the polar solvent, a tetrameric carboxylic anhydride is added for reaction, and the addition range is 90 to 110% according to the equivalent ratio. The equivalent ratio should be selected in the range of 95-103%. When measured using an N, N-dimethylacetamide solvent medium with a purity of 0.5 g / 100 m at 30 ° C, the Gu'an acid polymer has a logarithmic viscosity of 0.05 to 3 dl / g. , The 値 should be between 0.1 and 1.5 dl / g. During the formation of brain-cooling, the reaction temperature generally does not exceed 80 ° C, preferably not higher than 50 ° C. 〇For the reaction pressure, this paper size applies the Chinese National Standard (CNS) A4 specification (21 × 297 mm). (Please read the notes on the back before this page)

、 1T line 526222 Employees' Cooperatives of the Central Standards Bureau of the Ministry of Economic Affairs of the People's Republic of China printed A7 B7 V. Description of invention (\\) W is not intentionally limited, and atmospheric pressure is sufficient. The reaction time depends on the type of solvent used and the reaction temperature. However, it is generally required to be sufficient to complete the poly-an acid represented by formula one. A normal response time of four to twenty-four hours is sufficient. According to the reaction under the aforementioned conditions, the polyamic acid can have recurrent individuals represented by the following molecular formula one: HOOC COOH V HOOC COOH " v-气 HOOC COOH \ / —HNCO ^ CONH—R1- -HNC 〇y 'c〇NH —R2 R% -HNCO ^ CONH —R3_--1 tn where R is a tetravalent organic group; R1 is a divalent organic group;: R2 is a trivalent or tetravalent organic group; R3 Is a divalent organic group represented by the following fraction: ^ CH0 —R4——Si — (-O-Si- ^ τ—R4 — CHa CH〇 where R4 is an olefin group containing 0 »20 carbon atoms; and y is the number of recurrent individuals; 1, n ^ n is expressed in a molar ratio between l / (m + n) from 99.985 / 0.015 to 80/15, and m / (l + n ) Range from 1/2000 to 500/1 The number of moles of their respective recurrent individuals under the same conditions expressed in mole ratio. If the polyamine compound used is a monoamine, the polyamine compound is The molar ratio of the anhydride should be adjusted to 0.7 / 1.5 to 1.3 / 1.5, especially 1.0 / 1.5. In addition, if the polyamine compound is a tetraamine, the molar ratio of the polyamine compound to the dianhydride should be adjusted. To 0.7 / 10 to 1.3 / 2.0, especially Adjusted to 1.0 / 10 〇 In the next step, the polyhuanamic acid is between one hundred and four hundred degrees Celsius, preferably between one hundred and three hundred Baidu-i3. This paper size applies Chinese National Standard (CNS) A4 specifications ( 210X297 mm) (Please read the notes on the back before filling this page)

1T line 526222 A7 B7 V. Description of the invention (The hot water cooperation between them, or the chemical hydrolysis by treating with an amination agent such as acetic anhydride, etc., can provide the corresponding polymer of the following molecular formula.醯 imine: _ 0 0-Λ Λ, " 0 0 'person Λ -〇〇-ΛΛ R3-NR N-R1-YY _ 0 0 _ 1 _W—R2_ 0 0 m ′ yY—R3 0 o where R Is a tetravalent organic group; R1 is a divalent organic group; R2 is a trivalent or tetravalent organic group; R3 is a divalent organic group represented by the following fraction: CHa CH3 R4—Si-f. —Si卞 i-R4-ch3 chq where R4 is an olefin group containing 0-20 carbon atoms; and n 'is the number of recurrent individuals; 1, m and n are at l / (m + n) from 99.985 / 0.015 It is expressed in a molar ratio from 80 to 15 / m, and m / G + n) ranges from 1/2000 to 500/1, and the corresponding number of moles of a recurrent individual is also expressed under a molar ratio. Printed by the Consumers Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs? Water (please read the precautions on the back first, then this page) M (l + n) is less than 0.005 / 99.985, the cross-linking effect leads to an increase in thermal resistance, especially an increase in thermal reliability, and the non-linearity of the molecular chain causes the molecular chain The reduction of the encapsulation density between them and the increase of the feasibility of melting are not enough to provide a poly-an acid adhesive with good feasibility of melting and good thermal resistance. In addition, if it is higher than 2/17, the cross-linking effect that can provide appropriate melting and feasible 14 for adhesive applications will be excessive. According to the present invention, the standard adhesive is summarized as follows: -Ί4 This paper size is applicable to the Chinese National Standard (CNS) A4 specification (210X297 mm) 526222 A7 B7 V. Description of the invention (v5) 1 · The poly 1 imine adhesive Formation of structural individuals with molecular expressions like land. 2 · The precursor of the polyimide viscose includes a polyamidic acid or a polyether ether, which can be condensed into a molecular polyimide of molecular formula by thermal or chemical action. The standard insulating tape is summarized as follows: An insulating tape composed of a base supporting film and a layer of polyimide having a structure expressed in terms of molecular formula on at least one side of the supporting film. The standard insulating tape can be made in the following ways: 1. Coating the polyimide paint (i.e., the lacquer-type land to form a polyimide adhesive that can be dissolved in an organic solvent) on at least one of the supporting film On the side, the solvent is dried at 25CTC, especially at a temperature not lower than 3 ° C to eliminate residual solvents. 2. The polyanhydride varnish or polypentamate diethyl ether varnish (including a Polyurethane dissolved in organic solvents or a precursor of polyimide adhesive consisting of polyammonium ether) is coated on at least one side of the support film, so that the solvent is dried at a temperature not lower than 25 (TC, In particular, it is dried at a temperature of not less than 30rc to eliminate residual solvents and aminate the adhesive layer. A polymer having a fluorene imine bond can be used as a material for the insulating film. Central Standards Bureau, Ministry of Economic Affairs Printed by the Employee Consumer Cooperative, the material can be illustrated as follows: One includes Regulus (registered trademark of Mitsui Toatsu Chemical Co., Ltd.), Kapton H, V, E, K, and ZT (respectively registered trademarks of DuPont >, Upikx M, S, SGA, SGAPA (respective registrars of Ube Industries Ltd. ), Apical AH, NPI, HP (respectively registered trademarks of Kanegafuchi Chemical Industry Co., Ltd.), or polySimine membranes such as Aramica (registered trademark of AsaM Chemical Industry Co., Ltd.) '-, ... In the material, it is recommended to use a wave with a low CTE (coefficient of thermal expansion), especially if it belongs to Upilex s, SGA type, -15 This paper size is applicable to Chinese National Standard (CNS) A4 specification (210X297 mm) 526222 A7, B7 V. Description of the invention (\ Ll ·)

Kapton E and Apical HP materials. However, the thickness range is preferably between 1 and 500 μm, especially between 3 and 50 μm. Before the bottom film forms a viscous polymer layer containing polySimine, the surface of a base layer should be treated with plasma or ozone. The conventional technique is to physically saccharify the surface of a base layer through these treatments, or to form a functional group such as a carboxylated radical on the surface of the base layer according to chemical methods. This can greatly improve and stabilize the adhesion strength of the substrate. In order to implement the present invention, it is important that the adhesive polymer forming the layer has a glass transition temperature ranging from 135 ° to 280 ° (:), and has a wire junction in a temperature range of 150 ° C to 300 ° C. At temperature, the storage modulus is 102 to 109 dyne / cm2 (dyne per square centimeter). If the glass transition temperature is lower than 135 ° C, or the storage modulus at the first-line consolidation temperature is lower than 10 2 dyne / cm2 , There will be problems that the internal lead will move during the wire consolidation process, or the energy cannot be properly converted to the internal lead during ultrasonic heating. Conversely, the glass transition temperature exceeds 280 ° C or the storage mold at this consolidation temperature If the amount exceeds 100dyne / cin2, it takes a long time to perform the thermal junction between the lead holder and the integrated circuit chip, so it is difficult to perform short-term consolidation (rapid or short-term consolidation). Printed by the Consumer Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs. In order to implement the present invention, it is necessary that the amount of the solvent contained in the adhesive layer formed on the base film should not exceed one percent (1%). The amidation reaction of amines must have been specifically completed. This can prevent the volatilization of the solvent, or the volatile contamination of the water generated by the amination reaction during the short-time high temperature hot-melt and junction process (generally at 27 (TC or more)) to the lead base or the integrated circuit chip Cavities are formed on the surface or in the adhesive layer. The ionic impurities such as sodium, potassium, chlorine and sulfate ions in the existing polyimide are trace amounts or about 1 to 16 This paper is in accordance with Chinese national standards (CNS ) A4 specification (2i0'x 297 mm) 526222 A 7 _B7_ printed by the Consumer Cooperatives of the Central Standards Bureau of the Ministry of Economic Affairs 5. Description of the invention (ι5ι Ug / g (using hydrothermal extraction method, and according to the temperature of 121 Calculate the amount of ions extracted from a water for 24 hours at ° C.) For these reasons, the electronic circuit around the insulating tape used for adhesion has not been caused by ionic impurities in the tape invading uranium or metal migration. Short circuit situation. Because the amount of uranium and plutonium radioactive elements that will cause the semiconductor memory software to malfunction is lower than the detection limit of radiochemical analysis, that is, less than 0.6 ppb, the semiconductor memory can be used for a long time It maintains a fairly high level of reliability. · The water absorption of the adhesive layer is less than L8% (soaked in pure water at 23 ° C for 24 hours). Because it is generally used as polyetheramide and polyether Triammine-imidimide is three-quarters to three-tenths · It can greatly reduce the formation of cavitation, which may be caused by water vapor generated during the high temperature adhesion process. Polyimide The adhesive polymer film can be formed by coating a polyimide lacquer or a polyamic acid or a polyamic acid ether (as the precursor of the polyimide) or a mixture of the foregoing lacquers. 'Before applying thorium lacquer to the base film, if necessary, the thorium varnish can be mixed with a filter containing no radioactive elements such as uranium and thorium, such as silicon. The content of viscous polyimide must not be less than fifty percent (50%) by weight. 'It is preferably not less than seventy-five percent (75%) by weight. More preferably, it is based on Not less than 90% (90%) by weight, and most desirably not less than 95% (95%) by weight. Each adhesive polymer layer is not particularly affected by its thickness. limit. However, it is necessary to control the thickness in a range of 1 μm to less than 100 μm, and more preferably in a range higher than 3 mm and lower than 50 μm. Conventional equipment such as tip-tailed, trifurcated and tail-type brushes can be used for painting. In the method of drying and polyamine, if the viscous polymer is formed on one side of the base film or on the quotient of the base film, the traditional drum dryer is formed. If a viscous polymerization system is formed on both sides of the base film, Jian-Tu 7 paper size is applicable to Chinese National Standards (CNs) A4 (210X297 mm) (Please read the precautions on the back before going to this page) Hold

1T line 526222 Α7 Β7 V. Description of the invention (/ L) It is also possible to use a floating dryer. Drying conditions generally depend on the thickness of the adhesive polymer layer, the concentration of the lacquer, and the drying method used. For example, the concentration of lacquer is 25 percent (25%) and the thickness is 25 μm after drying. The drying can be performed at 8CTC ~ 15CTC, 150 ° 0200 ° C, 200 ° C ~ 250 ° C, or 25 ( TC ~ 300 ° C for 30 minutes. If the temperature range exceeds 300.400 ° C, the drying time can be reduced to less than ten minutes, so that the residual solvent can be completely eliminated and a complete viscose polyimide can be achieved. The present invention can be further understood through the description of the following examples, but these examples are for illustration only and do not constitute a limitation on the implementation of the present invention. Example 1: 13.851 g (0.0376 Moj 4,4'-Double (Double 4-aminophenoxy) diphenyl, 0.057 g (0.0002 mol) of 3,3% 4,4f-tetraamine diphenyl, 0.497 g (0.0020 mol) of 1,3 · bis (4-aminopropyl) Esters> Tetramethyldisilazane and 156.8 g of N, N-dimethylacetamide were introduced into a container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 4.296 Grams (0.012 moles) of 3,3 ', 4,4, -diphenyl stone wind tetracarboxylic dianhydride and 8.686 grams (0.028 moles) of 4,4 ~ oxodiacetic acid dianhydride are divided into four portions under nitrogen pressure Add to the container at room temperature and stir the mixture for twenty (20) hours at room temperature. As a result, the logarithmic viscosity of the polyamic acid 7? Is 0.85 dl / g. Example 2 Central Ministry of Economic Affairs 13.851 grams (0.0376 moles) of 4,4, -bis (4-aminophenoxy) diphenyl and 0.62 grams (0.00027 moles) of 353,4,4, -triamine di printed by the Consumer Bureau of Standards Bureau Phenyl sulfide, 0.497 g (like 0020 mole) of D double-piece aminopropyl ester) -tetramethyldisilazane, and 156.8 g of N, N-dimethylacetamide were introduced into a mixer equipped with a reflux A condenser and a nitrogen gas introduction tube. Then 4.296 g (0.012 mol) of 3,3,4,4, -diphenyl stone tetracarboxylic dianhydride and 8.686 g (0.028 mol) The 4,4, -oxodiphthalic dianhydride is divided into four parts and added under the conditions of nitrogen pressure and room temperature -48 This paper is suitable for Chinese National Standards (CNS) A4 specifications (210 × 297 Gongchu :) 526222 A7 B7 Five 2. Description of the invention (丨 " 7) into the container and stir the mixture for twenty (20) hours at room temperature. The logarithmic viscosity C of the polyamic acid was 0.80dl / g. Example 3 13,8 51 grams (0.0376 moles) of 4,4, bis (4-aminophenoxy) diphenyl, 0.043 grams (0.00027 moles) of 3,3 ', 4,4, triamine diphenyl ether, 0.497 grams (0.0020 mol) of 1,3-bis < 4-aminopropyl ester) -tetramethyldioxane and 155.9 g of N, N-dimethylacetamide were introduced into a A condenser and a container with a nitrogen introduction tube. Next, 4.296 g (0.012 mol) of 3,3,4,4 ^ diphenyl stone wind tetracarboxylic dianhydride and 8.886 g (0.028 mol) of 4,4 ~ oxodiphthalic dianhydride were divided into four portions under nitrogen. Add pressure and room temperature to the container and stir the mixture for twenty (20) hours at room temperature. Results The logarithmic viscosity of polyamic acid 7 was 0.90 dl / g. Comparative Example 1 14.736 g (0.040 moles of 4,4'bis (benzaminophenoxy) diphenyl) and 155.9 g of N, N-di Methylacetamidine was introduced into a container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 4.296 g (0.012 mol) of 3,3'4,4f-diphenylstone tetracarboxyl Anhydride and 8.686 g (0.028 mol) of 4,4, -oxodiphthalic dianhydride were added in four portions under nitrogen pressure and room temperature and the mixture was stirred at room temperature for twenty (20) Hours. Results The logarithmic viscosity of polyamidic acid was 0.70 dl / g. Comparative Example 2 13.262 grams (0.0360 moles) of bis (4-aminophenoxy) diphenyl, 0.857 grams (0.0020 moles of tetraamine diphenyl, and 156.8 grams of N) were printed by the Consumer Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs. NC methylacetamide was introduced into a container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 4.296 g (0.012 mol) of 3,3,4 4,4-diphenyl stone wind tetracarboxylic dianhydride and 8.686 g (0.028 mol) of 4,4, -oxodiphthalic dianhydride are divided into four portions under nitrogen pressure and room temperature and added to the container at room temperature The mixture was stirred for twenty (20) hours. As a result, the logarithmic viscosity of the polyamic acid was-• 19. This paper is a suitable paper size _ home standard (CNS) A4 size (2 like 297 Gongchu) 526222 A7 B7 V. Description of the invention (丨 Mod) L05 dl / g 0 Apply the above five polyan acid lacquers on the glass plate and Upilex-S film, and respectively at 80 ° C, 150 ° c, Heating at 200 ° C and 3 ° C for one hour each. According to the DMTA extension method, the glass transition temperature and storage modulus of the polyimide film were obtained. Measuring temperature. Adhesive tape consisting of polyimide adhesive and Upilx-SGA film is bonded to a copper plate, a nickel-iron alloy plate, and a coating at 400 ° c and a pressure of 10 kg / cm2 for one second. The board with PIX-3000 (Hitachi Chemical Co., Ltd.) was obtained at room temperature. The T-peel strength (measured using a tensile force of 50 mm / min) of the bonded specimen was obtained at room temperature. 0 The results are shown in Table 1 below (please first Read the notes on the back of this page and reheat this page) — Equipment-Printed in Table 1 by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economy Example Tg (° C) 5% Weight Loss Storage Modulus Active Strength (kg / cm) 25 ° C 230〇C Copper-nickel iron PIX-3000 _ .: 231 | 523 L7 X 1010 2.8 X 109 1.10 1.20: L30 two 227 521 1.7 1.7 X 1010 1.9 X 109 L15 L20 1.35 three 225 521 1.7 X 1010 3.1 X 109 1.20 L30 1.30 Comparison 1 231 517 1.7 X 1〇10 6 · 7 X 109 0.75 0.75 0.60 Comparison 2 242 525 2.8 X 1〇10 7.9 X 1010 0.60 0 * 65 0.50 Alignment This paper size is applicable to China National Standard (CNS) A4 specifications ( 210X297 male t) 526222 A7 _ B7_ V. Description of the invention () 13.925 g (0.0378 mol) of 4,4f-bis (4-aminophenoxy) diphenyl Group, 0.029 g (0.0001 mol) of 3,3f, 4,4'tetraaminediphenyl, 0.497 g (0.0020 mol) of 1,3-bis (4-aminopropyl) -tetramethyldisiloxane Alkanes and 175.8 grams of N-methyl-2-pyridine were introduced into a container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 3.867 g (0.012 mol) of 3,3 \ 4,4 ^ benzophenone tetracarboxylic dianhydride and 12.493 g (0.028 mol) of 4,4M hexafluoroisopropylidene) dianhydride were divided into four Portions were added to the vessel under nitrogen pressure and room temperature and the mixture was stirred for twenty (20) hours at room temperature. Results The logarithmic viscosity of the polyamidic acid was 0.65 dl / g. Example 5 13.925 g (0.0378 mol) of 4,4 bis (4 * aminophenoxy) diphenyl, 0.031 g (0.00015 mol) of 3,3,, 4f-triaminediphenylsulfide, 0.497 g (like 0,020 moles) of 1,3-bis (4-aminopropyl ester). Methyldisilaxane and 176.7 g of N-methyl- 2-Pyridine was introduced into a container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 3.867 g (0.012 mol) of 3,3M, 4'-benzophenone tetracarboxylic dianhydride and 12.439 g (0.028 mol) of 4,44 hexaoxoisophthalic acid) diphthalic dianhydride were divided into four portions It was added to the container under nitrogen pressure and room temperature, and the mixture was stirred for twenty (20) hours at room temperature. As a result, the logarithmic viscosity Θ of the polyamic acid was 0.85 dl / g. Example 6 Printed by the Consumer Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs ^ 13.925 g (0.0378 mols of 4,4, -bis (4-aminophenoxy) diphenyl, 0.021 g (0.00015 mol) of 3,3 ', 4'-triamine diphenyl ether, 0.497 g (0.0020 mol) of 1,3-bis (benzylaminopropyl) -tetramethyldisilazane, and 175.3 g of N-methyl winter pyrene were introduced. A container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 3.867 g (0.012 mol) of 3,3'4,4 ^ benzophenone tetracarboxylic anhydride and 12.439 g (0.028 Mol) of 4,4 ~ (hexafluoroisopropylidene) dipic acid dianhydride is divided into four portions and added to the container under nitrogen pressure and room temperature, and the mixture is stirred for twenty (20) at room temperature Hours. The logarithmic viscosity of the polyamic acid was 0.85 dl / g. 1 This paper size is in accordance with the Chinese National Standard (CNS). (210 parent 297 male 11 '~ 526222 A7 _B7 V. Description of the invention (> 〇) Comparison Example 3. 14.736 grams (0.040 moles) of 4, # · bis (4-aminophenoxy) diphenyl and 5.8 grams of N-methyl-2-fluorene B were introduced into a mixer, equipped with a reflux Condenser, with a nitrogen channel Tube container. Then 3.867 g (0.012 mol) of 3,3f, 4,4f-benzophenone tetracarboxylic dianhydride and 12.439 g (0.028 mol) of 4,4,-(hexafluoroisopropylidene) Diperoxy dianhydride was added to the container in four portions under nitrogen pressure and room temperature, and the mixture was stirred for twenty (20) hours at room temperature. As a result, the logarithmic viscosity of the polyamino acid was π. % dl / g. Comparative Example 4 13.262 g (0.0360 moles of 4 # -bis (4-aminophenoxy) diphenyl, 0.857 g (G.0020 moles) of 3,3,4,4 , -Tetraamine diphenyl and 175.8 g of N-methyl-2-fluorene were introduced into a container equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube. Then 3.867 g φ.012 Mol) of 3,3,4,4, -diphenyl stone tetracarboxylic dianhydride and 8.686 g (0.028 mol) of 4,4 ^ benzophenone tetracarboxylic dianhydride were divided into four portions under nitrogen pressure and Added to the container at room temperature and stirred the mixture for twenty to twenty hours at room temperature. As a result, the logarithmic viscosity of the polyamic acid 7? Was 0.80dl / g. Paint on the glass plate and Upilex_s film, and divide Heat at 80.0, 150 ° C, 200 ° C, and 300 ° C for one hour each. According to the DMTA extension method, obtain the polyimide film-glass transition temperature and storage modulus, and according to dta-Ministry of Economics Central Standard Bureau employee consumer cooperative prints 5% weight loss temperature in TG air. The adhesive tape composed of polydispersimide adhesive and Upilx-SGA adhesive film is at 400. (: Bonded under a pressure of 10 kg / cm2 for one second into a copper plate, a nickel-iron alloy plate, and a plate coated with PZχ-300 (X Hitachi Chemical Co., Ltd.). The bonded test was obtained at room temperature. Sample T-peel strength (measured using a tensile force at a rate of 50 mm / min). The results are shown in Table 2 below.-• 22 This paper size applies to China National Standard (CNS) A4 specification (21 × 297 mm) 526222 A7 --_ B7 V. Explanation of the invention (> \) Example ΓΤΠ Tg (° 〇5% Weight loss) Γ'-Storage modulus ^ Active strength (kg / cm) 25 ° C 230t: Copper-nickel-iron PIX-3000 Four 233 r \ r \ λ 517 2.1 X 1〇10 7.3 X 1〇9 1.50 1.65 1.20 5-221 516 2.1 X 1〇10 6.1 X 1〇9 1.45 L50 1.25 /, UUAtV- 233 515 " " " ι __ 2.2 X 1〇10 7.7 X 10 ^ 1.60 1.45 1.30 Comparison 2 236 r \ ar \ 511 2.0 X 1〇]. 23 X 1〇9 0.65 0.75 0.55 Comparison 4 242 522 2.3 X 1〇10 5.2 X 1〇 10 0.70 0.60 0.55 Example VII ... 19.496 grams (0,0376 moles) of 2,3-double M day consultation! Basically oxygen for every stupid woman) Basic] /, Fluoropropanein and 〇57 grams ( 〇〇〇〇 2 Festival of 353Ά4 ^ 0 $ Ι1 «^ α497 ^ 〇〇〇２００Ｍ） ^ 13 ^ (« ^ 186.6 grams of N-duck-2-pyridine printed by the Staff Consumer Cooperative of the Central Bureau of Standards of the Ministry of Economic Affairs was introduced into a equipped-mixer, a reflux The condenser and the trough with a nitrogen introduction tube were stirred and dissolved at room temperature under nitrogen pressure. Then, 7.28 g of 28 mole) of 5_ (2,5 • dioxotetrahydro) -3-methyl-3- Cyclohexane-1,2-diphenylcarboxylic dianhydride and 4.92 g (0.22 mol) of ethylene glycol bis (anhydrous-triphenylhexacarboxylate) were slowly added to the container in small amounts. The resulting mixture was warmed to 50 ° C and then stirred for another three hours. Then at 50 ° C, 37.24 g (0.04 mol) of Y-methylpyridine was added to the resulting polyamic acid solution The medium is heated while being stirred in a nitrogen stream. During the heating, the water produced by the daimidization reaction is discharged out of the system. The paper size of the mixture is applicable to China National Standard (CNS) A4 specifications (210X297 male fl 526222 A7 ___ B7__ V. Description of the invention (>) The temperature of the compound is maintained at 185 ° C for six hours to carry out the thermal ammonium salinization, and it will be produced by carrying a nitrogen stream. Part of the water and the reacted solvent are discharged out of the system. Then stop heating. Allow the finished product to cool to room temperature for about two hours while stirring. Then continue stirring the finished product for another three hours. Results The logarithmic viscosity of polyimide was 7? 0.45 dl / g. Example 8 19.496 g (0.0376 mol) of 2,3-bis [4 · (4-aminophenoxy) phenyl] hexafluoropropane And 0.062 g (0.00027 moles) of 3,3f, 4r-triaminediphenylsulfide, and 0.497 g (0.0020 moles) of 1,3-bis (4-S-aminopropyl) -tetramethyldisilazide Alkanes and 186.6 g of N-methyl-2-hydrazone were introduced into a vessel equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube, and dissolved by stirring at room temperature under nitrogen pressure. Next, 7.398 g (0.028 moles) of each of 5- (2,5-dioxotetrahydro) methyl-3-cyclohexane-1,2-diphenyl dianhydride, and 4.920 g (0.012 moles) of ethyl A small amount of diol bis (anhydrous-triphenylhexacarboxylate); added slowly to the container. The resulting mixture was warmed to 50 ° C and then stirred for another three hours. Then, at 50 ° C, 37.24 g (0.04 mol) of Y-methylpyridine was added to the resultant polyamic acid solution while heating under a stream of nitrogen. During the heating, the water produced by the imidization reaction is discharged outside the system. While maintaining the temperature of the mixture at 185 ° C for six hours for the thermal salinization, the water produced by the nitrogen stream and the reacted solvent were partially discharged out of the system. Then stop heating. Finished product · Allow to cool to room temperature for about two hours while stirring. Then continue printing by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economic Affairs for three hours. Results The logarithmic viscosity of polyiminic acid was 0.55 dl / g. Example 9. 19.496 g (0.0376 mol) of 2,3-bis [4- (4-aminophenoxy) phenyl] hexafluoropropane And 0.043 g (0.00027 moles) of 3,3,, 4. Triamine diphenyl ether, 0.497 g (0.0020 mol) of 1,3-bis (4-S propylpropyl) -tetramethyldisilaxane and 185.3 g of N-methyl-2-fluorene were introduced A container equipped with a stirrer, a reflux condenser, and a nitrogen inlet tube-£ 4 This paper is sized for the Chinese National Standard (CNS) A4 (210X 297 mm) 526222 A7 B7 V. Description of the invention) Nitrogen in the container Dissolve under pressure and room temperature with stirring. Then 7.398 g (0.028 mol) of 5- (2,5-dioxotetrahydro), each methyl, each cyclohexane-1,2-diphenylcarboxylic dianhydride, and 4.920 g (0.012 mol) of ethylene glycol bis (anhydrous-triphenylhexacarboxylate) was slowly added to the container in small amounts. The resulting mixture was warmed to 50 ° C and then stirred for another three hours. Then, at 50 ° C, 37.24 g (0.04 mol) of Y-methylpyridine was added to the resultant polyamic acid solution and heated while stirring in a stream of nitrogen. During the heating, the water produced by the ammonium amidation reaction was discharged out of the system. The temperature of the mixture was maintained at 185 ° C for six hours to perform thermal samarization, while the water produced by the nitrogen stream and the reacted solvent were partially discharged from the system. Then stop heating. Allow the finished product to cool to room temperature for about two hours while stirring. Then continue stirring the finished product for another three hours. Results The logarithmic viscosity of polySimine was 0.45 dl / g. Comparative Example 5 20.74 g (0.040 mol) of 2,3-bis [4- (4-aminophenoxy) phenyl] hexafluoropropane and 186.6 grams of N-methyl-2-pyridine was introduced-a vessel equipped with a stirrer, a reflux condenser, and a nitrogen introduction tube was dissolved by stirring at room temperature under nitrogen pressure. Next, 7.398 g (0.028 mol) of 5- (2,5-dioxotetrahydro) -3-methyl-3-cyclohexane-1,2-diphenylcarboxanhydride 'and 4.920 g (0.012 A small amount of ethylene glycol bis (anhydrous-triphenylhexacarboxylate) was slowly added to the container. The resulting mixture was warmed to 50 ° C and then stirred for another three hours. Then at 50 ° C, 37.24 g (0.04 moles) of Y-methylpyridine was added to the synthetic polyamic acid solution. One side was printed in a nitrogen stream printed by the Consumers Cooperative of the Central Standards Bureau of the Ministry of Economy and Economy. Heat while stirring. During the heating, the water produced by the acid imidization reaction is discharged out of the system. While maintaining the temperature of the mixture at 185t for six hours for the thermal salinization, the water generated by the nitrogen gas stream and the reacted solvent were partially discharged out of the system. Then stop heating. Allow the finished product to cool to room temperature for about two hours while stirring. Then continue stirring the finished product for another three hours. As a result, the logarithmic viscosity of polyimide was a35dl / g. This paper size applies the Chinese National Standard (CNS) A4 specification (210X297 mm) 526222 A7 B7 V. Description of the invention (&f; f) Comparative Example 6 18.666 g (0.0360 mol) of 2,3-bis [4 孙 aminobenzene Oxy) phenyl] hexafluoropropane and 0,857 g (0.00020 mols of 3,3M, 4f-triaminediphenyl and 186.6 g of N-methyl-2-hydrazone) were introduced into a stirrer and refluxed for condensation The container and a nitrogen introduction tube were stirred and dissolved under nitrogen pressure and room temperature. Then 7.398 g (0.028 mol) of 5- (2,5 · dioxytetrahydro) each methyl each cyclohexane-1 , 2.Diphenylcarboxylic dianhydride, and 4.920 g (0.012 moles of ethylene glycol bis (anhydrous-triphenylhexacarboxylate)) were slowly added to the container in small amounts. The resulting mixture was warmed to 5 CTC, followed by stirring. Three hours. Then at 50 ° C, 37.24 g (0.04 mol) of fluorene-methylpyridine was added to the resulting polyamic acid solution while heating in a nitrogen stream while heating. During the heating, Huanya The water produced by the amination reaction is drained out of the system. The temperature of the mixture is maintained at 185 ° C for six hours for thermal 醯 imine salinization At the same time, the water produced by the nitrogen flow and the reacted solvent are partly discharged out of the system. Then stop watching. The product is stirred and allowed to cool to room temperature for about two hours. Then the product is continuously disturbed for three hours. Result The logarithmic viscosity of polyimide was 7? 0.65 dl / g. The above five polyimide lacquers were coated on a glass plate and Upilex-S film, and were at 80 ° C, 150 ° C, 200 ° C, and 300 ° C for 40 minutes each. According to the DMTA extension method, the glass transition temperature and storage modulus of the polytimide film were obtained, and according to the 5% weight loss in DTA-TG air. Printed by the Consumers' Cooperative of the Central Standards Bureau of the Ministry of Economic Affairs, a tape composed of polyimide adhesive and Upilx-SGA adhesive film is bonded to the board for one second under the pressure of 40TC and 10 kg / cm2, a nickel-iron alloy HX-3000 (Hitachi Chemical Co., Ltd.) coated plate. Obtain the T-strip of the bonded sample at room temperature. Strength (using a tensile force measurement at a rate of 50 mm / min). The results are shown in the following table. 3-0-£ 6 This paper size applies to China National Standard (CNS) A4 (210X 297 mm) 526222 A7 B7 V. Description of the invention (> f) Table: Example Tg 5% Storage modulus activity is one degree stronger (° C) Weight loss (kg / cm) Brewing 25 ° C 230. Copper nickel iron PIX-3000 7227 461 L3 X 1010 1.3 X 109 1.25 1.25 1.30 Eight 228 462 1 1.3 X 1010 1.2 xltfl L40 1.25 1.30 Nine 226 460 1.3 X 1010 1.0 X 109 1.25 L30 L30 Compare five 232 457 1.3 X 1010 7.3 X 1.08 0.65 0.60 0.45 Comparison Six 245 463 2.3 X 101Q 5.8 X 1〇10 0.60 0.50 0.40 (Please read the precautions on the back before this page) The contents of the present invention are fabricated. In view of the foregoing teachings, many changes and improvements to the present invention are likely to occur. Therefore, within the scope of the patent claims, the present invention can still be implemented in ways other than the specified description. .Online printed by the Consumer Cooperatives of the Central Bureau of Standards of the Ministry of Economic Affairs -27

Claims (1)

526222 A8 B8 C8 D8 VI. Scope of patent application Printed by the Consumer Cooperatives of the Central Standards Bureau of the Ministry of Economic Affairs. ο-α R2 is a trivalent or tetravalent organic group selected from the group consisting of: 2 This paper size applies to China National Standard (CNS) Α4 specification (210 × 297 mm) (Please read the precautions on the back before filling this page)