CN114656635A - Preparation method of polyimide printed circuit board with high peel strength and low dielectric constant - Google Patents
Preparation method of polyimide printed circuit board with high peel strength and low dielectric constant Download PDFInfo
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- H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
- H05K2201/01—Dielectrics
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Abstract
The invention belongs to the technical field of printed circuit boards, and particularly relates to a preparation method of a polyimide printed circuit board with high peel strength and low dielectric constant. The method synthesizes novel siloxane-containing fluorine-containing diamine 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine, and utilizes the siloxane-containing diamine to modify polyimide to realize the functionalization and fluorine-containing of polyimide silicon oxide, so that the material and a copper foil have higher cohesiveness, and the prepared flexible printed circuit board has good peeling strength, and simultaneously adopts a fluorine-containing monomer with low electronic polarizability to ensure that the obtained material has lower dielectric constant. The printed circuit board prepared by the invention belongs to a glue-free printed circuit board, and can be applied to the field of high-frequency high-speed communication.
Description
Technical Field
The invention belongs to the technical field of printed circuit boards, and particularly relates to a preparation method of a polyimide printed circuit board with high peel strength and low dielectric constant.
Background
In recent years, the 5G technology has been rapidly advanced. The market demand for printed circuit boards as the main body of signal transmission structures is growing explosively, and the core of the printed circuit boards used in the field of high-frequency and high-speed communication such as 5G is that the insulating materials used have lower dielectric constant and dielectric loss on the basis of keeping the performance of the traditional materials. Polyimide has the advantages of excellent thermal stability, outstanding mechanical properties, lower dielectric constant and the like, and is a common material for preparing flexible printed circuit boards. Meanwhile, fluorine has the characteristics of large volume and low electronic polarizability, the dielectric constant and the dielectric loss of the polyimide material can be further reduced (the dielectric constant is less than 3.0, and the dielectric loss factor is less than 0.001) by introducing the fluorine, and the requirements of high frequency and high speed of 5G communication are met. Compared with the traditional glue type printed circuit board, the glue-free printed circuit board is lighter and thinner, is easier to fold, is more environment-friendly, has better dimensional stability, has higher processing difficulty, limits the development of the glue-free printed circuit board in the field of the glue-free printed circuit board due to poorer cohesiveness between the polyimide material and the copper foil, and particularly leads the cohesiveness to be worse after fluorine is introduced into the polyimide. Therefore, the development of polyimide materials with high adhesion and low dielectric properties is of great importance in the application of flexible printed circuit boards in the electronic industry.
Disclosure of Invention
Aiming at the requirements of low dielectric property, high peel strength and no gelatinization in the field of high-frequency and high-speed communication substrates, the invention provides a preparation method of a non-colloid polyimide printed circuit board with high peel strength and low dielectric constant.
The technical scheme adopted by the invention is as follows:
the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant comprises the following steps: synthesizing a novel silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine by using 4-bromo-N, N-bis (trimethylsilyl) aniline, dissolving the diamine monomer and other diamine monomers in a polar aprotic solvent at normal temperature, and adding 4,4' -hexafluoroisopropyl phthalic anhydride and other dianhydride monomers in five times according to a one-half feeding method, wherein the molar ratio of the 4,4' -hexafluoroisopropyl phthalic anhydride to the other dianhydride monomers is 2: 1, regulating the temperature to 5-10 ℃ in ice water bath, polymerizing for 12 hours at low temperature to obtain precursor polyamic acid solution containing siloxane and fluorine with certain viscosity, removing bubbles in vacuum for 0.5 hour, coating the polyamic acid solution on a copper foil with the wet film thickness of 30-35 microns, drying the solvent at 80-150 ℃, transferring the copper-clad plate into a vacuum oven, imidizing at 180-300 ℃, and cooling to obtain the copper-clad plate.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine is synthesized by the following method: under the protection of nitrogen, adding 4-bromo-N, N-bis (trimethylsilyl) aniline and magnesium into a dry reactor filled with fresh diethyl ether, reacting at 30 ℃ for 1h, and then refluxing and stirring for reacting for 3 h; after the system is cooled to room temperature, trifluoropropylmethyldichlorosilane with the same amount as 4-bromo-N, N-bis (trimethylsilyl) aniline is added into a reactor, the reaction mixture reacts for 2 hours at the reflux temperature, and N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silanamine is obtained by distillation; adding the obtained N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silane amine into a drying reactor filled with triethylamine under the protection of nitrogen, dropwise adding deionized water with the mole number of 1/2 of the N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silane amine at 80 ℃, reacting for 5h, cooling the reaction mixture to room temperature, filtering to remove solids to obtain a viscous liquid crude product, adding ethanol into the crude product, stirring for 3h at room temperature, spin-drying to remove the ethanol, washing with the deionized water to obtain 4,4' - (1), 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the content of the silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine accounts for 5-20% of the total mole number of the silicon-containing diamine monomer and other diamine monomers.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the polar aprotic solvent is one of N-methylpyrrolidone, N-dimethylacetamide and N, N-dimethylformamide.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the other diamine monomers further comprise one or more of 2,2' -bis (trifluoromethyl) -4,4' -diaminobiphenyl, 2' -bis (trifluoromethyl) -4,4' -diaminophenyl ether, 4- (hexafluoroisopropyl) bis (p-phenoxy) diphenylamine, 4' -diaminophenyl ether and p-phenylenediamine.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the other dianhydride monomers comprise one or more of 3,3',4,4' -benzophenone tetracarboxylic dianhydride, 2,3,3', 4-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride and 3,3',4,4' -biphenyl tetracarboxylic dianhydride.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the ratio of the total mole number of the silicon-containing diamine monomer and other diamine monomers to the total mole number of the 4,4' -hexafluoroisopropyl phthalic anhydride and other dianhydride monomers is 1.02: 1.
in the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, in the precursor polyamic acid solution, the solid content of the silicon-containing diamine monomer, the other diamine monomer, the 4,4' -hexafluoroisopropyl phthalic anhydride and the other dianhydride monomer accounts for 20% of the total mass of the precursor polyamic acid.
In the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the molar ratio of the 4-bromo-N, N-bis (trimethylsilyl) aniline to the magnesium is 1: 1.008.
in the preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant, the molar ratio of the N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silanamine to triethylamine is 1: 4.
has the advantages that:
the novel siloxane chain segment is introduced, so that on one hand, the contact area of the polyimide material and other matrixes is remarkably increased, the adhesion is remarkably enhanced, the peeling strength between the polyimide film and the copper foil is improved, the preparation of the adhesive-free flexible printed circuit board is realized, on the other hand, the siloxane chain segment also contains fluorine, and the siloxane chain segment can be synergistically acted with other fluorine-containing monomers in a system, so that the dielectric constant and the dielectric loss of the obtained material are further reduced, the preparation of the adhesive-free high-frequency high-speed flexible printed circuit board is finally realized, and the peeling strength is very high.
Drawings
FIG. 1 is a structural formula and nuclear magnetic hydrogen spectrum of 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine;
FIG. 2 is a structural formula and a carbon spectrum of 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine.
Detailed Description
In order to make the technical means, the characteristics, the objectives and the functions of the present invention easy to understand, the present invention will be further described with reference to the following embodiments.
Example 1
The embodiment provides a preparation method of a polyimide printed circuit board with high peel strength and low dielectric constant, which comprises the following steps:
1. preparation of silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine: under the protection of nitrogen, 1.58g,5.00mmol of 4-bromo-N, N-bis (trimethylsilyl) aniline and 121mg,5.04mmol of magnesium are added into a dry reactor filled with fresh ether, and the mixture is reacted for 1 hour at 30 ℃ and then stirred under reflux for 3 hours; after cooling the system to room temperature, 1.06g,5.00mol of trifluoropropylmethyldichlorosilane was added to the reactor and the reaction mixture was reacted at reflux temperature for 2h, followed by distillation to give 118.0mg,3.25mmol of N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silanamine in a yield of 65.1%. The resulting N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silanamine was added to a dry reactor containing 1.21g,12.00mmol of triethylamine under nitrogen protection, 27mg,1.50mmol of deionized water was added dropwise at 80 ℃ for 5h of reaction, the reaction mixture was cooled to room temperature and the solid was removed by filtration to give a crude viscous liquid. The crude product was added with ethanol, stirred at room temperature for 3h, spin dried to remove the ethanol, and washed 3 times with deionized water to give 1.04g,2.16mmol of 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine.
Referring to fig. 1 and 2, the structural formula of 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine, and the nuclear magnetic hydrogen spectrum and the carbon spectrum are shown as follows:1H NMR (500 MHz, DMSO-d6) δ 0.26 (s, 6H), 1.21 (t, J = 9.5 Hz, 4H), 2.16-2.22 (m, 4H), 4.04 (s, 4H), 6.70 (d, J = 9.1 Hz, 4H), 7.35 (d, J = 9.1 Hz, 4H)； 13C NMR (125 MHz, DMSO-d6) δ 149.11, 135.40, 128.80, 128.46, 126.66, 114.66, 33.21, 33.13, 33.05, 32.97, 31.50, 31.28, 31.07, 30.85。
2. adding a silicon-containing diamine monomer composition into a reaction kettle, wherein the silicon-containing diamine monomer composition comprises 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine and 2,2' -bis (trifluoromethyl) -4,4' -diaminobiphenyl, and the molar ratio of the silicon-containing diamine monomer composition to the 2: 8. n, N-dimethylacetamide was added and dissolved at room temperature with stirring for about 0.5 h. After complete dissolution, a dianhydride monomer composition comprising 4,4 '-hexafluoroisopropyl phthalic anhydride and 2,3,3', 4-biphenyl tetracarboxylic dianhydride in a molar ratio of 2: 1. the ratio of the total moles of dianhydride monomer composition to the total moles of silicon-containing diamine monomer composition is 1.02: 1. regulating the temperature in ice-water bath to 5-10 ℃. And (3) continuing stirring for 12 hours after the last dosing is finished, adjusting the solid content of the solution to be 20%, and polymerizing for 12 hours at low temperature to obtain the precursor polyamide acid solution containing siloxane and fluorine with certain viscosity. The precursor polyamic acid solution is vacuumed for 0.5 hour, then coated on a copper foil, the thickness of a wet film is 30 microns, the solvent is dried under the conditions of 80 ℃,1 hour, 120 ℃, 150 ℃ and 1 hour, then the copper-clad plate is transferred into a vacuum oven, and imidization is carried out for 30min at 180 ℃, 210 ℃, 240 ℃, 270 ℃ and 300 ℃. After cooling, the non-glue type polyimide printed circuit board with high peel strength and low dielectric constant of the embodiment can be obtained.
Example 2
The present embodiment is different from embodiment 1 in that: adding 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine and 4,4- (hexafluoroisopropyl) bis (p-phenoxy) diphenylamine into a reaction kettle in a molar ratio of 3: 7. n, N-dimethylformamide was added and the mixture was dissolved at room temperature with stirring for about 0.5 h. After complete dissolution, 4,4' -hexafluoroisopropylphthalic anhydride and 3,3',4,4' -benzophenonetetracarboxylic dianhydride were added in five portions by a one-half addition method in a molar ratio of 2: 1, and controlling the temperature to be 5-10 ℃. And (3) continuing stirring for 12 hours after the last dosing is finished, and adjusting the solid content of the solution to 20% to obtain a precursor polyamide acid solution. The polyamic acid solution was defoamed in vacuum for 0.5 hour, then coated on a copper foil with a wet film thickness of 32 μm, the solvent was dried at 80 ℃,1 hour, 120 ℃, 150 ℃,1 hour, and then the copper-clad plate was transferred to a vacuum oven and imidized at 180 ℃, 210 ℃, 240 ℃, 270 ℃, and 300 ℃ for 30min each. After cooling, the non-glue type polyimide printed circuit board with high peel strength and low dielectric constant of the embodiment can be obtained.
Example 3
Adding 4,4'- (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine and 4,4' -diaminophenyl ether in a molar ratio of 4: 6. n-methylpyrrolidone was added and dissolved at room temperature with stirring for about 0.5 h. After complete dissolution, 4' -hexafluoroisopropyl phthalic anhydride and pyromellitic dianhydride were added in five portions by a one-half addition method in a molar ratio of 2: 1, and controlling the temperature to be 5-10 ℃. And after the last dosing is finished, continuously stirring for 12h, adjusting the solid content of the solution to be 20%, obtaining a polyamic acid solution, carrying out vacuum defoaming on the polyamic acid solution for 0.5h, then coating the polyamic acid solution on a copper foil, wherein the thickness of a wet film is 35 microns, drying the solvent at 80 ℃, 1h, 120 ℃, 150 ℃ and 1h, then transferring the copper-clad plate into a vacuum oven, and imidizing the copper-clad plate at 180 ℃, 210 ℃, 240 ℃, 270 ℃ and 300 ℃ for 30min respectively. Cooling to obtain the non-glue polyimide printed circuit board with high peel strength and low dielectric constant.
Comparative example 1
4,4' -diamino phenyl ether is added into a reaction kettle, N-dimethyl acetamide is added, and the mixture is stirred and dissolved for about 0.5h at room temperature. After complete dissolution, adding pyromellitic dianhydride and 2,3,3', 4-biphenyl tetracarboxylic dianhydride in a half-feeding method for five times, wherein the molar ratio is 2: 1, and controlling the temperature to be 5-10 ℃. And (5) after the last dosing is finished, continuously stirring for 12 hours, and adjusting the solid content of the solution to be 20% to obtain the polyamide acid solution. The polyamic acid solution was defoamed in vacuum for 0.5 hour, then coated on a copper foil with a wet film thickness of 32 μm, the solvent was dried at 80 ℃,1 hour, 120 ℃, 150 ℃,1 hour, and then the copper-clad plate was transferred to a vacuum oven and imidized at 180 ℃, 210 ℃, 240 ℃, 270 ℃, and 300 ℃ for 30min each. And cooling to obtain the flexible polyimide printed circuit board.
Comparative example 2
Adding 2,2 '-bis (trifluoromethyl) -4,4' -diaminobiphenyl into a reaction kettle, adding N, N-dimethylacetamide, and stirring and dissolving for about 0.5h at room temperature. After complete dissolution, adding pyromellitic dianhydride and 2,3,3', 4-biphenyl tetracarboxylic dianhydride in a one-half feeding method in a molar ratio of 2: 1, and controlling the temperature to be 5-10 ℃. And (5) after the last dosing is finished, continuously stirring for 12 hours, and adjusting the solid content of the solution to be 20% to obtain the polyamide acid solution. The polyamic acid solution was defoamed in vacuum for 0.5 hour, then coated on a copper foil with a wet film thickness of 32 μm, the solvent was dried at 80 ℃,1 hour, 120 ℃, 150 ℃,1 hour, and then the copper-clad plate was transferred to a vacuum oven and imidized at 180 ℃, 210 ℃, 240 ℃, 270 ℃, and 300 ℃ for 30min each. And cooling to obtain the flexible polyimide printed circuit board.
Comparative example 3
The reaction kettle is added with 2,2 '-bis (trifluoromethyl) -4,4' -diaminophenyl ether, then added with N, N-dimethylacetamide, and stirred and dissolved for about 0.5h at room temperature. After complete dissolution, adding pyromellitic dianhydride and 2,3,3', 4-biphenyl tetracarboxylic dianhydride in a half-feeding method for five times, wherein the molar ratio is 2: 1, and controlling the temperature to be 5-10 ℃. And (5) after the last dosing is finished, continuously stirring for 12 hours, and adjusting the solid content of the solution to be 20% to obtain the polyamide acid solution. The polyamic acid solution was defoamed in vacuum for 0.5 hour, then coated on a copper foil with a wet film thickness of 32 μm, the solvent was dried at 80 ℃,1 hour, 120 ℃, 150 ℃,1 hour, and then the copper-clad plate was transferred to a vacuum oven and imidized at 180 ℃, 210 ℃, 240 ℃, 270 ℃, and 300 ℃ for 30min each. And cooling to obtain the flexible polyimide printed circuit board.
The properties of the materials tested in this example and comparative example are shown in the following table:
as can be seen from the above table, the novel siloxane chain segment is introduced, so that the contact area between the polyimide material and other matrixes is remarkably increased, the adhesion of the polyimide material is remarkably enhanced, the peeling strength between the polyimide film and the copper foil is improved, the preparation of the flexible printed circuit board without glue is realized, on the other hand, the siloxane chain segment also contains fluorine, and the siloxane chain segment can be cooperated with other fluorine-containing monomers in a system to further reduce the dielectric constant and the dielectric loss of the obtained material, and finally, the preparation of the flexible printed circuit board without glue at high frequency and high speed is realized, and the peeling strength is very high.
Further, the content of the silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine accounts for 5-20% of the total molar number of the silicon-containing diamine monomer and other diamine monomers.
Further, the polar aprotic solvent used is one of N-methylpyrrolidone, N-dimethylacetamide, or N, N-dimethylformamide.
Further, the other diamine monomer also comprises one or more of 2,2' -bis (trifluoromethyl) -4,4' -diaminobiphenyl, 2' -bis (trifluoromethyl) -4,4' -diaminophenyl ether, 4- (hexafluoroisopropyl) bis (p-phenoxy) diphenylamine, 4' -diaminophenyl ether and p-phenylenediamine.
Further, the other dianhydride monomer comprises one or more of 3,3',4,4' -benzophenone tetracarboxylic dianhydride, 2,3,3', 4-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride and 3,3',4,4' -biphenyl tetracarboxylic dianhydride.
Further, in the precursor polyamic acid solution, the solid content of the silicon-containing diamine monomer, the other diamine monomer, the 4,4' -hexafluoroisopropyl phthalic anhydride, and the other dianhydride monomer accounts for 20% of the total mass of the precursor polyamic acid.
Finally, it is noted that the above-mentioned preferred embodiments illustrate rather than limit the invention, and that, although the invention has been described in detail with reference to the above-mentioned preferred embodiments, it will be understood by those skilled in the art that various changes in form and detail may be made therein without departing from the scope of the invention as defined by the appended claims.
Claims (10)
1. The preparation method of the polyimide printed circuit board with high peel strength and low dielectric constant is characterized by comprising the following steps: synthesizing a novel silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine by using 4-bromo-N, N-bis (trimethylsilyl) aniline, dissolving the diamine monomer and other diamine monomers in a polar aprotic solvent at normal temperature, and adding 4,4' -hexafluoroisopropyl phthalic anhydride and other dianhydride monomers in a half-feeding method in five times, wherein the molar ratio of the 4,4' -hexafluoroisopropyl phthalic anhydride to the other dianhydride monomers is 2: 1, regulating the temperature to 5-10 ℃ in ice water bath, polymerizing for 12 hours at low temperature to obtain precursor polyamic acid solution containing siloxane and fluorine with certain viscosity, removing bubbles in vacuum for 0.5 hour, coating the polyamic acid solution on a copper foil with the wet film thickness of 30-35 microns, drying the solvent at 80-150 ℃, transferring the copper-clad plate into a vacuum oven, imidizing at 180-300 ℃, and cooling to obtain the copper-clad plate.
2. The method for preparing a polyimide printed circuit board with high peel strength and low dielectric constant as claimed in claim 1, wherein the silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine is synthesized by the following method: under the protection of nitrogen, adding 4-bromo-N, N-bis (trimethylsilyl) aniline and magnesium into a dry reactor filled with fresh diethyl ether, reacting at 30 ℃ for 1h, and then refluxing and stirring to react for 3 h; after the system is cooled to room temperature, trifluoropropylmethyldichlorosilane with the same amount as 4-bromo-N, N-bis (trimethylsilyl) aniline is added into a reactor, the reaction mixture reacts for 2 hours at the reflux temperature, and N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silanamine is obtained by distillation; adding the obtained N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silane amine into a drying reactor filled with triethylamine under the protection of nitrogen, dropwise adding deionized water with the mole number of 1/2 of the N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silane amine at 80 ℃, reacting for 5h, cooling the reaction mixture to room temperature, filtering to remove solids to obtain a viscous liquid crude product, adding ethanol into the crude product, stirring for 3h at room temperature, spin-drying to remove the ethanol, washing with the deionized water to obtain 4,4' - (1), 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine.
3. The method as claimed in claim 1, wherein the silicon-containing diamine monomer 4,4' - (1, 3-dimethyl-1, 3-bis (3,3, 3-trifluoropropyl) disiloxane-1, 3-diacyl) diphenylamine is present in an amount of 5-20% based on the total molar amount of the silicon-containing diamine monomer and the other diamine monomers.
4. The method as claimed in claim 1, wherein the polar aprotic solvent is one of N-methylpyrrolidone, N-dimethylacetamide and N, N-dimethylformamide.
5. The method as claimed in claim 1, wherein the other diamine monomers further comprise one or more of 2,2' -bis (trifluoromethyl) -4,4' -diaminobiphenyl, 2' -bis (trifluoromethyl) -4,4' -diaminophenyl ether, 4- (hexafluoroisopropyl) bis (p-phenoxy) diphenylamine, 4' -diaminophenyl ether and p-phenylenediamine.
6. The method as claimed in claim 1, wherein the other dianhydride monomers include one or more of 3,3',4,4' -benzophenone tetracarboxylic dianhydride, 2,3,3', 4-biphenyl tetracarboxylic dianhydride, pyromellitic dianhydride, and 3,3',4,4' -biphenyl tetracarboxylic dianhydride.
7. The method of claim 1, wherein the ratio of the total moles of the silicon-containing diamine monomer and other diamine monomers to the total moles of the 4,4' -hexafluoroisopropylphthalic anhydride and other dianhydride monomers is 1.02: 1.
8. the method for preparing a polyimide printed circuit board with high peel strength and low dielectric constant as claimed in claim 1, wherein the precursor polyamic acid solution contains silicon-containing diamine monomer, other diamine monomer, 4' -hexafluoroisopropyl phthalic anhydride and other dianhydride monomer in an amount of 20% by weight of the total mass of the precursor polyamic acid.
9. The method of claim 2, wherein the molar ratio of 4-bromo-N, N-bis (trimethylsilyl) aniline to magnesium is 1: 1.008.
10. the method as claimed in claim 2, wherein the molar ratio of N- (4- (chloro (methyl) (3,3, 3-trifluoropropyl) silyl) phenyl) -1,1, 1-trimethyl-N- (trimethylsilyl) silanamine to triethylamine is 1: 4.
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