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CN104945903A - Fold-resistant composite material - Google Patents

Fold-resistant composite material Download PDF

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Publication number
CN104945903A
CN104945903A CN201510409701.5A CN201510409701A CN104945903A CN 104945903 A CN104945903 A CN 104945903A CN 201510409701 A CN201510409701 A CN 201510409701A CN 104945903 A CN104945903 A CN 104945903A
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Prior art keywords
folding
matrix material
hour
molecular weight
hours
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CN201510409701.5A
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Chinese (zh)
Inventor
党斌
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Suzhou Kemiao New Material Co Ltd
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Suzhou Kemiao New Material Co Ltd
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Priority to CN201510409701.5A priority Critical patent/CN104945903A/en
Publication of CN104945903A publication Critical patent/CN104945903A/en
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    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L79/00Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing nitrogen with or without oxygen or carbon only, not provided for in groups C08L61/00 - C08L77/00
    • C08L79/04Polycondensates having nitrogen-containing heterocyclic rings in the main chain; Polyhydrazides; Polyamide acids or similar polyimide precursors
    • C08L79/08Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2201/00Properties
    • C08L2201/08Stabilised against heat, light or radiation or oxydation
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/02Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/03Polymer mixtures characterised by other features containing three or more polymers in a blend
    • C08L2205/035Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00Polymer mixtures characterised by other features
    • C08L2205/08Polymer mixtures characterised by other features containing additives to improve the compatibility between two polymers

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Macromolecular Compounds Obtained By Forming Nitrogen-Containing Linkages In General (AREA)

Abstract

The invention relates to a fold-resistant composite material. Cobalt phthalocyanine, stearic acid and polyether diol are evenly mixed to be reacted at the temperature of 85 DEG C for two hours to obtain a mixture; 1,3-bis(isocyanatomethyl)-cyclohexan, thioacetamide, bisphenol A dianhydride and polyoxyethylene rosin ester are sequentially added into the mixture to be stirred at the temperature of 110 DEG C for four hours, then phenylcyclohexane and hydroxylamine potassium are added to be stirred at the temperature of 120 DEG C for one hour; at last, polyimide resin, phenoxy resin and tetrazole are added to be stirred at the temperature of 120 DEG C for half an hour, and accordingly a fold-resistant prefabricated object is obtained; then the fold-resistant prefabricated object is placed in a mold, and the fold-resistant composite material is obtained through hot pressing. The fold-resistant composite material has excellent mechanical property and heat resistance, and the application and development requirements of the fold-resistant composite material can be met.

Description

A kind of folding matrix material
Technical field
The invention belongs to advanced composite material technical field, be specifically related to a kind of folding matrix material.
Background technology
Material is the pillar of modern science and technology and social development, and the competition of modern high technology depends on the development of Materials science to a great extent.So-called polymer is often referred to the macromolecular cpd connect with chemical bond by ten million micromolecular compound.Commodity polymer material is divided into the 5 large classes such as plastics, rubber, fiber, tackiness agent, coating.Matrix material is the heterogeneous material prepared through recombining process by two or more the material such as metallic substance, stupalith or macromolecular material, various material makes up for each other's deficiencies and learn from each other in performance, produce synergistic effect, make the over-all properties of matrix material be better than former composition material and meet various different requirement.The development of modern high technology be unable to do without matrix material, and matrix material, to the development of modern science and technology, has very important effect.The depth of investigation and speed and the scale of applying range and production development thereof of matrix material, become one of important symbol of a measurement national science advanced technology level.Matrix material mainly can be divided into structural composite material and the large class of functional composite material two.Functional composite material is generally made up of functive constituent element and matrix constituent element, and matrix not only plays integrant effect, and can produce collaborative or add powerful effect.Functional composite material refers to the matrix material providing other physicalies except mechanical property.As: conduction, superconduction, partly lead, magnetic, piezoelectricity, damping, suction ripple, wave transparent, friction, shielding, fire-retardant, folding, sound absorption, heat insulation etc. highlight a certain function, be referred to as functional composite material.Functional composite material is primarily of functive and reinforcement and matrix composition, and functive can be made up of one or more functional materialss.The matrix material of pluralistic function body can have several functions, meanwhile, also likely produces new function due to complex effect.Multifunctional composite is the developing direction of functional composite material.
The exploitation of novel material is the guide that Materials science develops with research, is the foundation stone of 21st century six large high-tech area.Matrix material is type material, because of diversified function and outstanding performances such as its folding, antifatigue, high temperature resistant, vibration dampings, be used widely in fields such as the Aeronautics and Astronautics over nearly 30 years, the energy, traffic, machinery, building, chemical industry, biomedicine and physical culture, 21 century Material Field opened one's arms and met the arrival in matrix material epoch.Along with matrix material development and application, matrix material has been formed in the middle of network penetration to industry-by-industry field.
Folding resistance (folding endurance) refers under certain stress, and paper, cardboard, plastics sheet or film bear weather resistance when reacting bending or folding at a certain temperature.It is the ability that experimental material resists local structural variation and subsurface defect development under repeated stress and effects of strain, has very large practicality.At present, strongthener mainly S high-strength glass fibre, carbon fiber and the aramid fiber of advanced composite material, aramid fiber is the common name of aromatic polyamide fibrid.It is that a kind of intensity is high, the high and low density of modulus, folding, synthetic that wear resistance is good organic fibre, but thermal characteristics is always barely satisfactory.
Summary of the invention
The object of this invention is to provide a kind of folding matrix material, it has excellent folding quality.
To achieve the above object of the invention, the technical solution used in the present invention is: a kind of folding matrix material, makes by after the hot pressing of folding preformed objects; Described folding preformed objects is (53 ~ 62) by mass ratio: (1 ~ 3): (18 ~ 20): (14 ~ 18): (11 ~ 13): (15 ~ 16): (6 ~ 8): (5 ~ 8): (18 ~ 25): (2 ~ 5): (12 ~ 15): the polyimide resin of (7 ~ 12), azanol potassium, 1,3-two (isocyanatomethyl)-hexanaphthene, polyether glycol, phenoxy resin, rosin polyoxyethylene ester, thioacetamide, phenylcyclohexane, bisphenol A dianhydride, tetrazolium, stearic acid, Cobalt Phthalocyanine are that raw material obtains;
The molecular weight of described polyimide resin is 3000 ~ 5000;
Described phenoxy resin molecular weight is 10800 ~ 14500;
The molecular weight of described rosin polyoxyethylene ester is 800 ~ 1500;
The molecular weight of described polyether glycol is 3800 ~ 5500.
In the present invention, described polyimide resin by 3,3 ', 4,4 '-benzophenone tetracarboxylic dianhydride and 12 methylenediamine condensation reactions obtain.
In the present invention, by polyether glycol, phenoxy resin and bisphenol A dianhydride being combinationally used, excellent heat resistance can be obtained and the more tough and polymkeric substance of excellent solvent resistance.By adding rosin polyoxyethylene ester, thioacetamide, phenylcyclohexane, the even density of the filler in system, can obtain good mix, becomes the paste-like being easily prepared into and having mobility; Be conducive to polymer polymerization.
In the present invention, azanol potassium can form small molecules hapto when resin solidification, is conducive to resin system evenly crosslinked, generally exists with the methanol solution of azanol potassium; Rosin polyoxyethylene ester, also known as polyoxylethylene abietate, take rosin as raw material, obtains under base catalysis with ethylene oxide polymerization.
In the present invention, organic object is the primary bond composition of solid gums, and the bonding force that molecular weight (state of cure) shows for organic constituent has material impact, reactive when in particular concerning the consistency of each component and solidify; Low material rate of drying is comparatively slow, and high resin system is not good to the wettability of inorganic filler.Organic-compound system of the present invention is not only uniformly dispersed being uniformly mixed in process, and overflow is moderate in bonding processes, evenly crosslinked.
In the present invention, preferably, polyimide resin, azanol potassium, 1,3-two (isocyanatomethyl)-hexanaphthene, polyether glycol, phenoxy resin, rosin polyoxyethylene ester, thioacetamide, phenylcyclohexane, bisphenol A dianhydride, tetrazolium, stearic acid, Cobalt Phthalocyanine that described folding preformed objects is 60: 2: 18: 15: 11: 16: 7: 7: 20: 5: 15: 10 by mass ratio are that raw material obtains.
In the present invention, Cobalt Phthalocyanine, stearic acid, polyether glycol are mixed, within 2 hours, obtain mixture in 85 DEG C of reactions; Successively two for 1,3-(isocyanatomethyl)-hexanaphthene, thioacetamide, bisphenol A dianhydride, rosin polyoxyethylene ester are added in mixture, stir 4 hours in 110 DEG C, then add phenylcyclohexane, azanol potassium, stir 1 hour in 120 DEG C; Finally add polyimide resin, phenoxy resin, tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.Heat pressing process is: 0.3MPa/130 DEG C/0.5 hour+0.3MPa/150 DEG C/1 hour+0.5MPa/170 DEG C/2 hours.
Because technique scheme is used, the present invention compared with prior art has following advantages:
1. the folding preformed objects that the present invention utilizes forms rationally, between each component, consistency is good, has prepared folding matrix material thus, has good good solubility-resistence, resistance toheat, there is excellent folding quality especially, meet the development and application of folding matrix material.
2. in preparation folding matrix material raw material disclosed by the invention, raw material is simple and easy to get, without the need to the complex reaction of prior art, the matrix material of preparation has excellent folding quality, solidification effect is good, crosslinking structure is even, micromolecular compound can as the compatilizer of macromolecule organic, increase the consistency of each component of system on the one hand, avoid on the other hand forming fragility large cross-linking set during hot-press solidifying, ensure that resin system forms stable structure, folding resistance is strong, achieves beyond thought effect; And avoid the problem of the heat-resisting difference of high-ductility composite material in prior art.
embodiment:
Below in conjunction with embodiment, the invention will be further described:
In the present embodiment, polyimide resin by 3,3 ', 4,4 '-benzophenone tetracarboxylic dianhydride and 12 methylenediamine condensation reactions obtain; Heat pressing process is: 0.3MPa/130 DEG C/0.5 hour+0.3MPa/150 DEG C/1 hour+0.5MPa/170 DEG C/2 hours.
Embodiment one
10g Cobalt Phthalocyanine, 15g stearic acid, 15g polyether glycol (molecular weight is 4500) are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively by 18g1, two (the isocyanatomethyl)-hexanaphthene of 3-, 7g thioacetamide, 20g bisphenol A dianhydride, 16g rosin polyoxyethylene ester (molecular weight is 1000) add in mixture, stir 4 hours in 110 DEG C, then add 7g phenylcyclohexane, 2g azanol potassium, stir 1 hour in 120 DEG C; Finally add 60g polyimide resin (molecular weight is 4000), 11g phenoxy resin (molecular weight is 12000), 5g tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Embodiment two
7g Cobalt Phthalocyanine, 12g stearic acid, 14g polyether glycol (molecular weight is 4000) are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively by 19g1, two (the isocyanatomethyl)-hexanaphthene of 3-, 7g thioacetamide, 24g bisphenol A dianhydride, 16g rosin polyoxyethylene ester (molecular weight is 800) add in mixture, stir 4 hours in 110 DEG C, then add 5g phenylcyclohexane, 3g azanol potassium, stir 1 hour in 120 DEG C; Finally add 62g polyimide resin (molecular weight is 3000), 12g phenoxy resin (molecular weight is 11000), 4g tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Embodiment three
12g Cobalt Phthalocyanine, 13g stearic acid, 16g polyether glycol (molecular weight is 5000) are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively by 18g1, two (the isocyanatomethyl)-hexanaphthene of 3-, 6g thioacetamide, 18g bisphenol A dianhydride, 15g rosin polyoxyethylene ester (molecular weight is 1500) add in mixture, stir 4 hours in 110 DEG C, then add 6g phenylcyclohexane, 1g azanol potassium, stir 1 hour in 120 DEG C; Finally add 56g polyimide resin (molecular weight is 5000), 12g phenoxy resin (molecular weight is 13000), 5g tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Embodiment four
8g Cobalt Phthalocyanine, 14g stearic acid, 18g polyether glycol (molecular weight is 4800) are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively by 19g1, two (the isocyanatomethyl)-hexanaphthene of 3-, 7g thioacetamide, 19g bisphenol A dianhydride, 16g rosin polyoxyethylene ester (molecular weight is 900) add in mixture, stir 4 hours in 110 DEG C, then add 8g phenylcyclohexane, 2g azanol potassium, stir 1 hour in 120 DEG C; Finally add 53g polyimide resin (molecular weight is 5000), 13g phenoxy resin (molecular weight is 14000), 2g tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Embodiment five
9g Cobalt Phthalocyanine, 15g stearic acid, 16g polyether glycol (molecular weight is 4100) are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively by 20g1, two (the isocyanatomethyl)-hexanaphthene of 3-, 6g thioacetamide, 25g bisphenol A dianhydride, 16g rosin polyoxyethylene ester (molecular weight is 1300) add in mixture, stir 4 hours in 110 DEG C, then add 7g phenylcyclohexane, 2g azanol potassium, stir 1 hour in 120 DEG C; Finally add 55g polyimide resin (molecular weight is 4000), 11g phenoxy resin (molecular weight is 12000), 3g tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Comparative example one
2g Cobalt Phthalocyanine, 15g stearic acid, 15g polyether glycol are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively by 18g1, two (the isocyanatomethyl)-hexanaphthene of 3-, 7g thioacetamide, 20g bisphenol A dianhydride, 16g rosin polyoxyethylene ester add in mixture, stir 4 hours in 110 DEG C, then add 7g phenylcyclohexane, stir 1 hour in 120 DEG C; Finally add 60g polyimide resin, 11g epoxy resin, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Comparative example two
10g Cobalt Phthalocyanine, 15g stearic acid, 15g polyether glycol are mixed, within 2 hours, obtains mixture in 85 DEG C of reactions; Successively two to 18g1,3-(isocyanatomethyl)-hexanaphthene, 20g bisphenol A dianhydride, 16g rosin polyoxyethylene ester are added in mixture, stir 4 hours in 110 DEG C, then add 2g phenylcyclohexane, 2g azanol potassium, stir 1 hour in 120 DEG C; Finally add 60g polyimide resin, 11g phenoxy resin, stir 0.5 hour in 120 DEG C, obtain folding preformed objects; Insert in mould by folding preformed objects again, namely hot pressing obtain folding matrix material.
Performance test
DSC tested glass transition temperature (Tg/ DEG C); Electronic universal tester is utilized to test flexural strength (Rt/MPa); Liquid crystal type balance weight impact testing machine is utilized to test shock strength (α/KJ/m 2); Adopt dynamic mechanical test instrument test storage modulus (E/MPa(35 DEG C)); Folding endurance tester test folding number (T).
The performance test results of above-mentioned folding matrix material is in table 1.
The performance of table 1 folding matrix material
Tg α Rt E T
Embodiment one 154 4.1 78 984 1000
Embodiment two 151 3.8 74 970 1000
Embodiment three 149 3.9 75 964 1000
Embodiment four 150 3.8 76 974 1000
Embodiment five 153 4 74 970 1000
Comparative example one 140 2.7 59 740 303
Comparative example two 138 2.8 60 794 521
To sum up, rationally, between each component, consistency is good for folding matrix material composition disclosed by the invention, prepare folding matrix material thus, there is good thermotolerance, mechanical property, there is excellent folding quality especially, meet the development and application of folding matrix material.

Claims (6)

1. a folding matrix material, is characterized in that, makes by after the hot pressing of folding preformed objects; Described folding preformed objects is (53 ~ 62) by mass ratio: (1 ~ 3): (18 ~ 20): (14 ~ 18): (11 ~ 13): (15 ~ 16): (6 ~ 8): (5 ~ 8): (18 ~ 25): (2 ~ 5): (12 ~ 15): the polyimide resin of (7 ~ 12), azanol potassium, 1,3-two (isocyanatomethyl)-hexanaphthene, polyether glycol, phenoxy resin, rosin polyoxyethylene ester, thioacetamide, phenylcyclohexane, bisphenol A dianhydride, tetrazolium, stearic acid, Cobalt Phthalocyanine are that raw material obtains;
The molecular weight of described polyimide resin is 3000 ~ 5000;
Described phenoxy resin molecular weight is 10800 ~ 14500;
The molecular weight of described rosin polyoxyethylene ester is 800 ~ 1500;
The molecular weight of described polyether glycol is 3800 ~ 5500.
2. folding matrix material according to claim 1, is characterized in that, described polyimide resin by 3,3 ', 4,4 '-benzophenone tetracarboxylic dianhydride and 12 methylenediamine condensation reactions obtain.
3. folding matrix material according to claim 1, it is characterized in that, described rosin polyoxyethylene ester is obtained with ethylene oxide polymerization under base catalysis by rosin.
4. folding matrix material according to claim 1, it is characterized in that, polyimide resin, azanol potassium, 1,3-two (isocyanatomethyl)-hexanaphthene, polyether glycol, phenoxy resin, rosin polyoxyethylene ester, thioacetamide, phenylcyclohexane, bisphenol A dianhydride, tetrazolium, stearic acid, Cobalt Phthalocyanine that described folding preformed objects is 60: 2: 18: 15: 11: 16: 7: 7: 20: 5: 15: 10 by mass ratio are that raw material obtains.
5. folding matrix material according to claim 1, is characterized in that, Cobalt Phthalocyanine, stearic acid, polyether glycol are mixed, within 2 hours, obtain mixture in 85 DEG C of reactions; Successively two for 1,3-(isocyanatomethyl)-hexanaphthene, thioacetamide, bisphenol A dianhydride, rosin polyoxyethylene ester are added in mixture, stir 4 hours in 110 DEG C, then add phenylcyclohexane, azanol potassium, stir 1 hour in 120 DEG C; Finally add polyimide resin, phenoxy resin, tetrazolium, stir 0.5 hour in 120 DEG C, obtain folding preformed objects.
6. folding matrix material according to claim 1, it is characterized in that, described heat pressing process is, 0.3MPa/130 DEG C/0.5 hour+0.3MPa/150 DEG C/1 hour+0.5MPa/170 DEG C/2 hours.
CN201510409701.5A 2015-07-14 2015-07-14 Fold-resistant composite material Pending CN104945903A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111635584A (en) * 2020-06-10 2020-09-08 扬州爱非科鞋业有限公司 Preparation method of folding-resistant upper

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2004269616A (en) * 2003-03-06 2004-09-30 Sumitomo Bakelite Co Ltd Resin composition and cover lay for flexible printed wiring board using the same
JP2004292821A (en) * 2002-06-26 2004-10-21 Hitachi Chem Co Ltd Film adhesive, adhesive sheet, and semiconductor device
CN103509167A (en) * 2013-07-25 2014-01-15 北京理工大学 Anti-droplet and high temperature resistant polyimide type polyurethane and preparation method thereof
CN103665762A (en) * 2012-09-14 2014-03-26 株式会社田村制作所 Thermosetting resin composition, b graded resin film, metal foil, copper-clad board and multi-layer lamination substrate
TW201504037A (en) * 2013-04-16 2015-02-01 Toyo Boseki Metal foil laminate

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2004292821A (en) * 2002-06-26 2004-10-21 Hitachi Chem Co Ltd Film adhesive, adhesive sheet, and semiconductor device
JP2004269616A (en) * 2003-03-06 2004-09-30 Sumitomo Bakelite Co Ltd Resin composition and cover lay for flexible printed wiring board using the same
CN103665762A (en) * 2012-09-14 2014-03-26 株式会社田村制作所 Thermosetting resin composition, b graded resin film, metal foil, copper-clad board and multi-layer lamination substrate
TW201504037A (en) * 2013-04-16 2015-02-01 Toyo Boseki Metal foil laminate
CN103509167A (en) * 2013-07-25 2014-01-15 北京理工大学 Anti-droplet and high temperature resistant polyimide type polyurethane and preparation method thereof

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111635584A (en) * 2020-06-10 2020-09-08 扬州爱非科鞋业有限公司 Preparation method of folding-resistant upper

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Application publication date: 20150930