CN112011074A - Organic silicon modified polyimide film and preparation method thereof - Google Patents
Organic silicon modified polyimide film and preparation method thereof Download PDFInfo
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- 229920001721 polyimide Polymers 0.000 title claims abstract description 57
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title claims abstract description 28
- 229910052710 silicon Inorganic materials 0.000 title claims abstract description 28
- 239000010703 silicon Substances 0.000 title claims abstract description 28
- 238000002360 preparation method Methods 0.000 title claims abstract description 10
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 42
- 239000002904 solvent Substances 0.000 claims abstract description 14
- 239000000377 silicon dioxide Substances 0.000 claims abstract description 12
- 235000012239 silicon dioxide Nutrition 0.000 claims abstract description 8
- 239000000178 monomer Substances 0.000 claims description 30
- GTDPSWPPOUPBNX-UHFFFAOYSA-N ac1mqpva Chemical compound CC12C(=O)OC(=O)C1(C)C1(C)C2(C)C(=O)OC1=O GTDPSWPPOUPBNX-UHFFFAOYSA-N 0.000 claims description 17
- 150000004985 diamines Chemical class 0.000 claims description 16
- 229920005575 poly(amic acid) Polymers 0.000 claims description 15
- 125000006158 tetracarboxylic acid group Chemical group 0.000 claims description 13
- YDYSEBSNAKCEQU-UHFFFAOYSA-N 2,3-diamino-n-phenylbenzamide Chemical group NC1=CC=CC(C(=O)NC=2C=CC=CC=2)=C1N YDYSEBSNAKCEQU-UHFFFAOYSA-N 0.000 claims description 12
- 125000003368 amide group Chemical group 0.000 claims description 10
- 238000010438 heat treatment Methods 0.000 claims description 10
- 239000004593 Epoxy Substances 0.000 claims description 8
- 239000006087 Silane Coupling Agent Substances 0.000 claims description 8
- 239000000203 mixture Substances 0.000 claims description 8
- 239000002245 particle Substances 0.000 claims description 7
- 239000011248 coating agent Substances 0.000 claims description 6
- 238000000576 coating method Methods 0.000 claims description 6
- 238000004519 manufacturing process Methods 0.000 claims description 6
- 238000000034 method Methods 0.000 claims description 6
- 239000002105 nanoparticle Substances 0.000 claims description 6
- 125000003118 aryl group Chemical group 0.000 claims description 5
- 150000008064 anhydrides Chemical class 0.000 claims description 4
- YGYCECQIOXZODZ-UHFFFAOYSA-N 4415-87-6 Chemical compound O=C1OC(=O)C2C1C1C(=O)OC(=O)C12 YGYCECQIOXZODZ-UHFFFAOYSA-N 0.000 claims description 3
- QQGYZOYWNCKGEK-UHFFFAOYSA-N 5-[(1,3-dioxo-2-benzofuran-5-yl)oxy]-2-benzofuran-1,3-dione Chemical compound C1=C2C(=O)OC(=O)C2=CC(OC=2C=C3C(=O)OC(C3=CC=2)=O)=C1 QQGYZOYWNCKGEK-UHFFFAOYSA-N 0.000 claims description 3
- OTARVPUIYXHRRB-UHFFFAOYSA-N diethoxy-methyl-[3-(oxiran-2-ylmethoxy)propyl]silane Chemical compound CCO[Si](C)(OCC)CCCOCC1CO1 OTARVPUIYXHRRB-UHFFFAOYSA-N 0.000 claims description 3
- 238000006068 polycondensation reaction Methods 0.000 claims description 3
- DQZNLOXENNXVAD-UHFFFAOYSA-N trimethoxy-[2-(7-oxabicyclo[4.1.0]heptan-4-yl)ethyl]silane Chemical compound C1C(CC[Si](OC)(OC)OC)CCC2OC21 DQZNLOXENNXVAD-UHFFFAOYSA-N 0.000 claims description 3
- BPSIOYPQMFLKFR-UHFFFAOYSA-N trimethoxy-[3-(oxiran-2-ylmethoxy)propyl]silane Chemical compound CO[Si](OC)(OC)CCCOCC1CO1 BPSIOYPQMFLKFR-UHFFFAOYSA-N 0.000 claims description 3
- LJMPOXUWPWEILS-UHFFFAOYSA-N 3a,4,4a,7a,8,8a-hexahydrofuro[3,4-f][2]benzofuran-1,3,5,7-tetrone Chemical compound C1C2C(=O)OC(=O)C2CC2C(=O)OC(=O)C21 LJMPOXUWPWEILS-UHFFFAOYSA-N 0.000 claims description 2
- CQMIJLIXKMKFQW-UHFFFAOYSA-N 4-phenylbenzene-1,2,3,5-tetracarboxylic acid Chemical compound OC(=O)C1=C(C(O)=O)C(C(=O)O)=CC(C(O)=O)=C1C1=CC=CC=C1 CQMIJLIXKMKFQW-UHFFFAOYSA-N 0.000 claims description 2
- WOSVXXBNNCUXMT-UHFFFAOYSA-N cyclopentane-1,2,3,4-tetracarboxylic acid Chemical compound OC(=O)C1CC(C(O)=O)C(C(O)=O)C1C(O)=O WOSVXXBNNCUXMT-UHFFFAOYSA-N 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- 239000003960 organic solvent Substances 0.000 claims description 2
- JXUKBNICSRJFAP-UHFFFAOYSA-N triethoxy-[3-(oxiran-2-ylmethoxy)propyl]silane Chemical compound CCO[Si](OCC)(OCC)CCCOCC1CO1 JXUKBNICSRJFAP-UHFFFAOYSA-N 0.000 claims description 2
- 239000007822 coupling agent Substances 0.000 claims 1
- 239000004642 Polyimide Substances 0.000 abstract description 10
- 238000001035 drying Methods 0.000 description 20
- 239000011521 glass Substances 0.000 description 13
- 239000002994 raw material Substances 0.000 description 12
- 238000003756 stirring Methods 0.000 description 9
- 238000011056 performance test Methods 0.000 description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 6
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 4
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 238000007865 diluting Methods 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 238000002834 transmittance Methods 0.000 description 3
- 239000004952 Polyamide Substances 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229920002647 polyamide Polymers 0.000 description 2
- 230000008961 swelling Effects 0.000 description 2
- QHHKLPCQTTWFSS-UHFFFAOYSA-N 5-[2-(1,3-dioxo-2-benzofuran-5-yl)-1,1,1,3,3,3-hexafluoropropan-2-yl]-2-benzofuran-1,3-dione Chemical compound C1=C2C(=O)OC(=O)C2=CC(C(C=2C=C3C(=O)OC(=O)C3=CC=2)(C(F)(F)F)C(F)(F)F)=C1 QHHKLPCQTTWFSS-UHFFFAOYSA-N 0.000 description 1
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 1
- 230000005540 biological transmission Effects 0.000 description 1
- WKDNYTOXBCRNPV-UHFFFAOYSA-N bpda Chemical compound C1=C2C(=O)OC(=O)C2=CC(C=2C=C3C(=O)OC(C3=CC=2)=O)=C1 WKDNYTOXBCRNPV-UHFFFAOYSA-N 0.000 description 1
- 238000004140 cleaning Methods 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 230000003014 reinforcing effect Effects 0.000 description 1
- 238000002791 soaking Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 238000000870 ultraviolet spectroscopy Methods 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 230000037303 wrinkles Effects 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
- C08J5/18—Manufacture of films or sheets
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G83/00—Macromolecular compounds not provided for in groups C08G2/00 - C08G81/00
- C08G83/001—Macromolecular compounds containing organic and inorganic sequences, e.g. organic polymers grafted onto silica
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J2387/00—Characterised by the use of unspecified macromolecular compounds, obtained otherwise than by polymerisation reactions only involving unsaturated carbon-to-carbon bonds
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Health & Medical Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Materials Engineering (AREA)
- Inorganic Chemistry (AREA)
- Macromolecular Compounds Obtained By Forming Nitrogen-Containing Linkages In General (AREA)
Abstract
The invention provides an organic silicon modified polyimide film and a preparation method thereof, wherein polyimide and silicon dioxide are effectively bonded, so that the organic silicon modified polyimide has excellent solvent resistance and heat resistance, and unique comprehensive performance is endowed to the organic silicon modified polyimide.
Description
Technical Field
The invention relates to the technical field of optical materials, in particular to an organic silicon modified polyimide film and a preparation method thereof.
Background
In the industries of photoelectric display and the like, the novel polyimide film is used for replacing a glass material, so that the characteristics of lightness, thinness, folding and the like of a screen can be realized. To meet these characteristics, the novel polyimide must have sufficient chemical resistance, heat resistance, and light transmittance to protect the components of the display. In addition, such a novel substrate must be durable against solvents used in cleaning, peeling, etching, and the like performed in the process of manufacturing a display, and also needs to be resistant to high temperatures.
Disclosure of Invention
Based on the technical problems in the background art, the invention provides an organic silicon modified polyimide film and a preparation method thereof, wherein polyimide and silicon dioxide are effectively bonded, so that the organic silicon modified polyimide has excellent solvent resistance and heat resistance, and unique comprehensive performance is endowed to the organic silicon modified polyimide.
The invention provides a preparation method of an organic silicon modified polyimide film, which comprises the following steps:
s1, modifying the silicon dioxide nano particles by using an epoxy silane coupling agent to obtain surface modified silicon dioxide;
s2, uniformly mixing the amido group-containing diamine monomer and the surface modified silicon dioxide obtained in the step S1, and then adding the aromatic tetracarboxylic dianhydride monomer to perform polycondensation reaction to obtain organic silicon modified polyamic acid;
and S3, coating the organic silicon modified polyamic acid obtained in the step S2 with a film, and heating and curing to obtain the organic silicon modified polyimide film.
Preferably, the silica nanoparticles have a particle size of 20 to 150 nm.
Preferably, the epoxy silane coupling agent is one or more of 2- (3, 4-epoxycyclohexyl) ethyltrimethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane and 3-glycidoxypropyltriethoxysilane.
Preferably, the amido-containing diamine monomer is diaminobenzanilide.
Preferably, the tetracarboxylic dianhydride monomer is one or more of 4, 4'- (hexafluoroisopropylidene) diphthalic anhydride, 4, 4' -oxydiphthalic anhydride, 3', 4, 4' -biphenyltetracarboxylic dianhydride, 1, 2, 3, 4-cyclobutane tetracarboxylic dianhydride, 1, 2, 4, 5-cyclopentane tetracarboxylic dianhydride, and 1, 2, 4, 5-cyclohexane tetracarboxylic dianhydride.
Preferably, in step S1, the epoxy silane coupling agent is added into the solvent and heated until completely dissolved, then the silica nanoparticles are added, stirred and mixed thoroughly, and dried to obtain the surface-modified silica.
Preferably, the surface-modified silica is present in an amount of 1 to 10 wt% based on the amount of amido-containing diamine monomer.
Preferably, in step S2, the amido group-containing diamine monomer and the surface-modified silica obtained in step S1 are added to an organic solvent, stirred at 20-30 ℃ for 2-4h, and then the aromatic tetracarboxylic dianhydride monomer is added to react at 30-40 ℃ for 4-6h to obtain the organosilicon-modified polyamic acid.
Preferably, in step S3, the organosilicon modified polyimide film is obtained by coating the organosilicon modified polyamic acid obtained in step S2 with a film and reacting at 100-400 ℃ for 3-10 h.
The invention also provides an organic silicon modified polyimide film which is prepared by the preparation method.
According to the invention, the silicon dioxide is modified by the epoxy silane coupling agent, the silicon dioxide modified by the epoxy silane coupling agent is bonded with the amido group-containing diamine monomer, and then the amido group-containing diamine monomer and the aromatic tetracarboxylic dianhydride monomer are subjected to polycondensation, so that in the obtained organic silicon modified polyimide, the epoxy silane coupling agent is used as a connecting bridge of the polyimide and the silicon dioxide, so that the silicon dioxide is uniformly dispersed in a polyimide matrix as a reinforcing particle, and the organic silicon modified polyimide film has excellent comprehensive performance.
Detailed Description
Hereinafter, the technical solution of the present invention will be described in detail by specific examples, but these examples should be explicitly proposed for illustration, but should not be construed as limiting the scope of the present invention.
Example 1
An organic silicon modified polyimide film is prepared by the following steps:
s1, dissolving 0.5mmol of 2- (3, 4-epoxycyclohexyl) ethyltrimethoxysilane in absolute ethyl alcohol, heating to 50 ℃, stirring for 10min, adding 5mmol of silica particles (the average particle size is 50nm), heating to 100 ℃, stirring for 5h, drying at 140 ℃, washing with absolute ethyl alcohol, drying in vacuum, and grinding to obtain surface modified silica;
s2, under the protection of nitrogen, dissolving 30mmol of diaminobenzanilide as a diamine monomer raw material in 150mL of N, N-dimethylacetamide solvent, stirring until the diaminobenzanilide is completely dissolved, adding the surface modified silicon dioxide, stirring at room temperature for 3 hours, adding 30mmol of 4, 4' - (hexafluoroisopropylene) diphthalic anhydride as a tetracarboxylic dianhydride monomer raw material, continuing stirring until the diaminobenzanilide is completely dissolved, and reacting at 30 ℃ for 5 hours to obtain an organic silicon modified polyamic acid solution;
s2, diluting the organic silicon modified polyamide acid solution until the solid content is 10 wt%, coating the diluted organic silicon modified polyamide acid solution on a glass plate, placing the glass plate in a drying oven at 100 ℃, drying for 1h, heating to 200 ℃, drying for 1h, heating to 350 ℃, drying for 2h, taking out the glass plate after the temperature is reduced to 25 ℃, placing the glass plate in water for demoulding, then placing the film in the drying oven at 100 ℃ for drying and removing water to obtain the organic silicon modified polyimide film, and controlling the thickness of the polyimide film to be 50 mu m;
the results of the performance test on the polyimide film are shown in table 1.
Example 2
An organosilicon modified polyimide film was prepared in the same manner as in example 1, except that in step S2, 30mmol of diaminobenzanilide as a diamine monomer raw material and 30mmol of 4, 4' -oxydiphthalic anhydride as a tetracarboxylic dianhydride monomer raw material were used, and the results of the performance test on the polyimide film thus obtained were also shown in table 1.
Example 3
An organosilicon modified polyimide film was prepared in the same manner as in example 1, except that in step S2, 30mmol of diaminobenzanilide as a diamine monomer raw material and 30mmol of 3, 3', 4, 4' -biphenyltetracarboxylic dianhydride as a tetracarboxylic dianhydride monomer raw material were used, and the results of the performance-related tests of the polyimide film thus obtained were also shown in table 1.
Example 4
An organosilicon modified polyimide film was prepared in the same manner as in example 1, except that in step S2, 30mmol of diaminobenzanilide as a diamine monomer raw material and 30mmol of 1, 2, 3, 4-cyclobutanetetracarboxylic dianhydride as a tetracarboxylic dianhydride monomer raw material were used, and the results of the performance-related tests of the polyimide film thus obtained were also shown in table 1.
Example 5
An organosilicon modified polyimide film was prepared in the same manner as in example 1, except that in step S1, 0.5mmol of 3-glycidoxypropyltrimethoxysilane was dissolved in absolute ethanol, the temperature was raised to 50 ℃ and the mixture was stirred for 10 minutes, 5mmol of silica particles (average particle diameter 50nm) were added, the mixture was heated to 100 ℃ and stirred for 5 hours, the mixture was dried at 140 ℃, washed with absolute ethanol and then vacuum-dried, and ground to obtain surface-modified silica, and the results of the performance test on the polyimide film thus obtained are also shown in Table 1.
Example 6
An organosilicon modified polyimide film was prepared in the same manner as in example 1, except that in step S1, 0.5mmol of 3-glycidoxypropylmethyldiethoxysilane was dissolved in absolute ethanol, the temperature was raised to 50 ℃ and the mixture was stirred for 10 minutes, 5mmol of silica particles (average particle diameter 50nm) were added, the mixture was heated to 100 ℃ and the mixture was stirred for 5 hours, the mixture was dried at 140 ℃, washed with absolute ethanol and then vacuum-dried, and ground to obtain surface-modified silica, and the results of the performance tests on the polyimide film thus obtained were as shown in table 1.
Comparative example 1
A polyimide film, the preparation method of which comprises:
s1, under the protection of nitrogen, dissolving 30mmol of diaminobenzanilide as a diamine monomer raw material in 150mL of N, N-dimethylacetamide solvent, adding 30mmol of 4, 4' - (hexafluoroisopropylene) diphthalic anhydride as a tetracarboxylic dianhydride monomer raw material, continuously stirring until the monomers are completely dissolved, and reacting at 30 ℃ for 5 hours to obtain a polyamic acid solution;
s2, diluting the polyamic acid solution to a solid content of 10 wt%, coating the polyamic acid solution on a glass plate, placing the glass plate in a drying oven at 100 ℃, drying for 1h, heating to 200 ℃, drying for 1h, heating to 350 ℃, drying for 2h, taking out the glass plate after the temperature is reduced to 25 ℃, placing the glass plate in water for demoulding, then placing the film in the drying oven at 100 ℃ for drying and removing water to obtain the polyimide film, and controlling the thickness of the polyimide film to be 50 microns;
the results of the performance test on the polyimide film are shown in table 1.
Comparative example 2
A polyimide film, the preparation method of which comprises:
s1, under the protection of nitrogen, dissolving 30mmol of diaminobenzanilide as a diamine monomer raw material in 150mL of N, N-dimethylacetamide solvent, stirring until the diaminobenzanilide is completely dissolved, adding 5mmol of silica particles (the average particle size is 50nm), stirring at room temperature for 3 hours, adding 30mmol of 4, 4' - (hexafluoroisopropylene) diphthalic anhydride as a tetracarboxylic dianhydride monomer raw material, continuing stirring until the diaminobenzanilide is completely dissolved, and reacting at 30 ℃ for 5 hours to obtain an organosilicon modified polyamic acid solution;
s2, diluting the polyamic acid solution to a solid content of 10 wt%, coating the polyamic acid solution on a glass plate, placing the glass plate in a drying oven at 100 ℃, drying for 1h, heating to 200 ℃, drying for 1h, heating to 350 ℃, drying for 2h, taking out the glass plate after the temperature is reduced to 25 ℃, placing the glass plate in water for demoulding, and then placing the film in the drying oven at 100 ℃ for drying and removing water to obtain the polyimide film, wherein the thickness is controlled to be 50 microns;
the results of the performance test on the polyimide film are shown in table 1.
The polyimide films obtained in examples 1 to 6 and comparative examples 1 to 2 were subjected to the performance tests shown in the following methods, and the results are shown in Table 1.
Coefficient of linear thermal expansion: a thermal mechanical analyzer was used to apply a 50mN load under a nitrogen atmosphere, and the temperature was measured at a temperature rise rate of 10 ℃/min to obtain an average value.
Solvent resistance: the polyimide film was immersed in the selected solvent (N-methylpyrrolidone) for 30 minutes at room temperature for the measurement. If after soaking it is substantially free of surface wrinkles, swelling or any other visible damage, the film is considered solvent resistant, rated: insoluble in a solvent and not swellable (A); insoluble in a solvent, swelling (B); dissolving (C) in a solvent.
Total light transmittance: the total light transmittance was measured by uv-vis spectroscopy.
Oxygen permeability: the Oxygen Transmission Rate (OTR) is measured using an oxygen permeameter (e.g., ox-TRAN, MOCON) at 25 ℃ and a relative humidity of 60%.
TABLE 1 test results of polyimide films obtained in examples 1 to 6 and comparative examples 1 to 2
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art should be considered to be within the technical scope of the present invention, and the technical solutions and the inventive concepts thereof according to the present invention should be equivalent or changed within the scope of the present invention.
Claims (10)
1. The preparation method of the organic silicon modified polyimide film is characterized by comprising the following steps:
s1, modifying the silicon dioxide nano particles by using an epoxy silane coupling agent to obtain surface modified silicon dioxide;
s2, uniformly mixing the amido group-containing diamine monomer and the surface modified silicon dioxide obtained in the step S1, and then adding the aromatic tetracarboxylic dianhydride monomer to perform polycondensation reaction to obtain organic silicon modified polyamic acid;
and S3, coating the organic silicon modified polyamic acid obtained in the step S2 with a film, and heating and curing to obtain the organic silicon modified polyimide film.
2. The method for preparing an organosilicon modified polyimide film according to claim 1, wherein the silica nanoparticles have a particle size of 20 to 150 nm.
3. The method for preparing the silicone-modified polyimide film according to claim 1 or 2, wherein the epoxysilane coupling agent is one or more of 2- (3, 4-epoxycyclohexyl) ethyltrimethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, and 3-glycidoxypropyltriethoxysilane.
4. The method for producing an organosilicon modified polyimide film according to any of claims 2 to 3, wherein the amide group-containing diamine monomer is diaminobenzanilide.
5. The method for producing an organosilicon modified polyimide film according to any one of claims 1 to 4, wherein the tetracarboxylic dianhydride monomer is one or more selected from the group consisting of 4, 4'- (hexafluoroisopropylene) diphthalic anhydride, 4, 4' -oxydiphthalic anhydride, 3', 4, 4' -biphenyltetracarboxylic dianhydride, 1, 2, 3, 4-cyclobutanetetracarboxylic dianhydride, 1, 2, 4, 5-cyclopentanetetracarboxylic dianhydride, and 1, 2, 4, 5-cyclohexanetetracarboxylic dianhydride.
6. The method for preparing an organosilicon modified polyimide film according to any one of claims 1 to 5, wherein in step S1, the epoxy silane coupling agent is added into the solvent and heated until completely dissolved, then the silica nanoparticles are added and stirred and mixed thoroughly, and then the mixture is dried to obtain the surface modified silica.
7. The method for producing an organosilicon modified polyimide film according to any of claims 1 to 6, wherein the surface-modified silica is used in an amount of 1 to 10 wt% based on the amount of the amide group-containing diamine monomer.
8. The method for producing an organosilicon modified polyimide film according to any of claims 1 to 7, wherein in step S2, the amido group-containing diamine monomer and the surface-modified silica obtained in step S1 are added to an organic solvent, stirred at 20 to 30 ℃ for 2 to 4 hours, and then the aromatic tetracarboxylic dianhydride monomer is added, and reacted at 30 to 40 ℃ for 4 to 6 hours to obtain an organosilicon modified polyamic acid.
9. The method for preparing the organic silicon modified polyimide film as claimed in any one of claims 1 to 8, wherein in step S3, the organic silicon modified polyamic acid obtained in step S2 is coated and then reacted at 100-400 ℃ for 3-10h to obtain the organic silicon modified polyimide film.
10. An organosilicon-modified polyimide film, which is produced by the production method according to any one of claims 1 to 9.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112831076A (en) * | 2021-02-04 | 2021-05-25 | 浙江中科玖源新材料有限公司 | Preparation method of high-water-resistance transparent polyimide film |
Citations (9)
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|---|---|---|---|---|
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| CN112831076B (en) * | 2021-02-04 | 2022-12-02 | 浙江中科玖源新材料有限公司 | Preparation method of high-water-resistance transparent polyimide film |
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