CN115312786A - Method for producing modified polymer film, and use thereof - Google Patents
Method for producing modified polymer film, and use thereof Download PDFInfo
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- CN115312786A CN115312786A CN202211084772.9A CN202211084772A CN115312786A CN 115312786 A CN115312786 A CN 115312786A CN 202211084772 A CN202211084772 A CN 202211084772A CN 115312786 A CN115312786 A CN 115312786A
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- polymer film
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- modified polymer
- plasma polymerization
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- 229920006254 polymer film Polymers 0.000 title claims abstract description 114
- 238000004519 manufacturing process Methods 0.000 title claims description 7
- 230000004048 modification Effects 0.000 claims abstract description 63
- 238000012986 modification Methods 0.000 claims abstract description 63
- 238000006116 polymerization reaction Methods 0.000 claims abstract description 60
- 229920000642 polymer Polymers 0.000 claims abstract description 54
- 229910052751 metal Inorganic materials 0.000 claims abstract description 49
- 239000002184 metal Substances 0.000 claims abstract description 49
- 238000006243 chemical reaction Methods 0.000 claims abstract description 28
- 238000000034 method Methods 0.000 claims abstract description 26
- 239000002994 raw material Substances 0.000 claims abstract description 22
- VVJKKWFAADXIJK-UHFFFAOYSA-N Allylamine Chemical compound NCC=C VVJKKWFAADXIJK-UHFFFAOYSA-N 0.000 claims abstract description 14
- 238000002360 preparation method Methods 0.000 claims abstract description 14
- WGYKZJWCGVVSQN-UHFFFAOYSA-N propylamine Chemical compound CCCN WGYKZJWCGVVSQN-UHFFFAOYSA-N 0.000 claims abstract description 14
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 claims abstract description 11
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 claims abstract description 11
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 claims abstract description 7
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 claims abstract description 7
- CERQOIWHTDAKMF-UHFFFAOYSA-N Methacrylic acid Chemical compound CC(=C)C(O)=O CERQOIWHTDAKMF-UHFFFAOYSA-N 0.000 claims abstract description 7
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical compound COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229920001577 copolymer Polymers 0.000 claims abstract description 6
- 239000010410 layer Substances 0.000 claims description 82
- -1 polypropylene Polymers 0.000 claims description 34
- 239000002131 composite material Substances 0.000 claims description 29
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 27
- 239000000463 material Substances 0.000 claims description 23
- 239000004743 Polypropylene Substances 0.000 claims description 22
- 229920001155 polypropylene Polymers 0.000 claims description 22
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 20
- 239000007789 gas Substances 0.000 claims description 19
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 18
- 239000011241 protective layer Substances 0.000 claims description 18
- 230000035484 reaction time Effects 0.000 claims description 16
- 239000004642 Polyimide Substances 0.000 claims description 14
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- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 11
- 229910052802 copper Inorganic materials 0.000 claims description 11
- 239000010949 copper Substances 0.000 claims description 11
- 229910052759 nickel Inorganic materials 0.000 claims description 10
- 239000002033 PVDF binder Substances 0.000 claims description 9
- 239000004721 Polyphenylene oxide Substances 0.000 claims description 9
- 239000004734 Polyphenylene sulfide Substances 0.000 claims description 9
- 229910052786 argon Inorganic materials 0.000 claims description 9
- 229920001707 polybutylene terephthalate Polymers 0.000 claims description 9
- 229920000139 polyethylene terephthalate Polymers 0.000 claims description 9
- 239000005020 polyethylene terephthalate Substances 0.000 claims description 9
- 229920006380 polyphenylene oxide Polymers 0.000 claims description 9
- 229920000069 polyphenylene sulfide Polymers 0.000 claims description 9
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 9
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 9
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 9
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 8
- 239000001301 oxygen Substances 0.000 claims description 8
- 229910052760 oxygen Inorganic materials 0.000 claims description 8
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 6
- 239000002041 carbon nanotube Substances 0.000 claims description 6
- 229910021389 graphene Inorganic materials 0.000 claims description 6
- 229910000838 Al alloy Inorganic materials 0.000 claims description 5
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims description 5
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 claims description 5
- 239000005751 Copper oxide Substances 0.000 claims description 5
- 229910000881 Cu alloy Inorganic materials 0.000 claims description 5
- 239000004952 Polyamide Substances 0.000 claims description 5
- 239000004793 Polystyrene Substances 0.000 claims description 5
- WGLPBDUCMAPZCE-UHFFFAOYSA-N Trioxochromium Chemical compound O=[Cr](=O)=O WGLPBDUCMAPZCE-UHFFFAOYSA-N 0.000 claims description 5
- 239000006230 acetylene black Substances 0.000 claims description 5
- 229910045601 alloy Inorganic materials 0.000 claims description 5
- 239000000956 alloy Substances 0.000 claims description 5
- 229910052799 carbon Inorganic materials 0.000 claims description 5
- 239000002134 carbon nanofiber Substances 0.000 claims description 5
- 229910052804 chromium Inorganic materials 0.000 claims description 5
- 239000011651 chromium Substances 0.000 claims description 5
- 229910000423 chromium oxide Inorganic materials 0.000 claims description 5
- 229910000428 cobalt oxide Inorganic materials 0.000 claims description 5
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 claims description 5
- 229910000431 copper oxide Inorganic materials 0.000 claims description 5
- 229910002804 graphite Inorganic materials 0.000 claims description 5
- 239000010439 graphite Substances 0.000 claims description 5
- 239000003273 ketjen black Substances 0.000 claims description 5
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical class C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 5
- 229910000480 nickel oxide Inorganic materials 0.000 claims description 5
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims description 5
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 5
- 229920002647 polyamide Polymers 0.000 claims description 5
- 239000011112 polyethylene naphthalate Substances 0.000 claims description 5
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- 239000002096 quantum dot Substances 0.000 claims description 5
- 229910000990 Ni alloy Inorganic materials 0.000 claims description 3
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 3
- 229910001000 nickel titanium Inorganic materials 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 239000004332 silver Substances 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- 229920003207 poly(ethylene-2,6-naphthalate) Polymers 0.000 claims 1
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- 229920000915 polyvinyl chloride Polymers 0.000 claims 1
- 230000007774 longterm Effects 0.000 abstract 1
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- 238000012360 testing method Methods 0.000 description 9
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical group [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 5
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- 238000007738 vacuum evaporation Methods 0.000 description 5
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 238000005240 physical vapour deposition Methods 0.000 description 4
- 239000000853 adhesive Substances 0.000 description 3
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- 238000011065 in-situ storage Methods 0.000 description 2
- 229920002521 macromolecule Polymers 0.000 description 2
- 238000001755 magnetron sputter deposition Methods 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
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- 238000007639 printing Methods 0.000 description 2
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- 238000001132 ultrasonic dispersion Methods 0.000 description 2
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
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- 238000005520 cutting process Methods 0.000 description 1
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- 229910001882 dioxygen Inorganic materials 0.000 description 1
- 238000007772 electroless plating Methods 0.000 description 1
- 238000010894 electron beam technology Methods 0.000 description 1
- 238000009713 electroplating Methods 0.000 description 1
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/02—Details
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
- H01M4/662—Alloys
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Composite Materials (AREA)
- Manufacturing & Machinery (AREA)
- Treatments Of Macromolecular Shaped Articles (AREA)
Abstract
The application relates to a preparation method of a modified polymer film, the modified polymer film and application thereof, belonging to the technical field of batteries. The application discloses a modified polymer film, which comprises a high molecular polymer base film and a surface modification layer, wherein the surface modification layer is formed on at least one surface of the high molecular polymer base film through a plasma polymerization method. The reaction raw material of the surface modification layer comprises one or more of acrylic acid, acrylonitrile, allylamine, ethylenediamine, n-propylamine, methacrylic acid, methyl methacrylate and derivatives and copolymers thereof. The modified polymer film provided by the application has the advantages of large surface polarity, high surface tension and long-term stability, and can be firmly combined with a metal layer.
Description
Technical Field
The invention relates to the technical field of batteries, in particular to a preparation method of a modified polymer film, the modified polymer film and application thereof.
Background
Metallized polymer films are widely used in the fields of electronics, packaging, printing, and the like due to their excellent properties of conductivity, barrier, flexibility, and light weight. The current common metallized polymer film products in the market comprise a composite current collector, a film electrode, a packaging aluminum-plated film, a printing film and the like. In the conventional technology, a metal is deposited directly on the surface of a polymer film such as polypropylene, polyethylene, polyester and the like by using a physical vapor deposition technology to prepare a metallized polymer film. However, there is a problem in that the polymer film is not firmly bonded to the surface metal layer during the actual production of the metallized polymer film.
Disclosure of Invention
An object of the present invention is to provide a method for preparing a modified polymer film, a modified polymer film and a use thereof, which can improve the surface polarity of the modified polymer film, make the surface tension thereof high and stable for a long time, and can be firmly bonded to a metal layer.
In order to achieve the purpose, the following technical scheme is adopted in the application:
in one aspect of the present application, there is provided a modified polymer film comprising a high molecular polymer base film and a surface modification layer formed on at least one surface of the high molecular polymer base film by a plasma polymerization method.
In some embodiments, the reaction raw material of the surface modification layer includes one or more of acrylic acid, acrylonitrile, allylamine, ethylenediamine, n-propylamine, methacrylic acid, methyl methacrylate, and derivatives and copolymers thereof.
In some embodiments, the material of the high polymer based film includes one or more of polypropylene (PP), polyethylene (PE), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polyimide (PI), polypropylene, polyvinyl chloride (PVC), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyphenylene Sulfide (PPs), polyphenylene oxide (PPO), polystyrene (PS), polyamide, polyimide, and derivatives thereof.
In some embodiments, the thickness of the high molecular polymer-based film is 1 μm or more; preferably 2 to 20 μm.
In some embodiments, the surface modification layer has a thickness of 5 to 200nm; preferably 10 to 100nm.
In another aspect of the present application, there is provided a method for preparing the above-described modified polymer film, the method comprising the steps of: and carrying out plasma polymerization modification on the surface of the high-molecular polymer base film so as to form the surface modification layer on at least one surface of the high-molecular polymer base film.
In some embodiments, when the surface of the high molecular polymer base film is subjected to plasma polymerization modification, introducing a mixed gas consisting of oxygen and argon and a reaction raw material;
the mixed gas bombards the surface of the high molecular polymer base film to provide reactive sites, and the reaction raw material is grafted to the surface of the high molecular polymer base film through the reactive sites, so that the surface modification layer is formed.
In some embodiments, the surface of the high molecular polymer-based film is modified by plasma polymerization by using a plasma polymerization device;
the plasma polymerization device comprises a radio frequency power supply, and the frequency of the radio frequency power supply is 3-30 MHz; preferably 10 to 20MHz; the power of the plasma polymerization device is 10-50W; preferably 20 to 40W.
In some embodiments, the reaction time for the plasma polymerization modification is 1 to 60min.
In a further aspect of the present application, there is provided a metallized polymer film comprising a metal layer and the modified polymer film described above or the modified polymer film prepared by the above preparation method, wherein the metal layer is located on at least one surface modification layer of the modified polymer film;
optionally, the material of the metal layer comprises one or more of copper, copper alloy, aluminum alloy, nickel alloy, titanium and silver.
Yet another aspect of the present application provides a composite current collector comprising the metallized polymer film described above.
In some embodiments, the composite current collector further comprises a protective layer disposed on a surface of the metal layer;
optionally, the material of the protective layer comprises one or more of nickel, chromium, nickel-based alloy, copper oxide, aluminum oxide, nickel oxide, chromium oxide, cobalt oxide, graphite, carbon black, acetylene black, ketjen black, carbon nano quantum dots, carbon nanotubes, carbon nanofibers, and graphene;
optionally, the thickness of the protective layer is 10 to 200nm; preferably 50 to 100nm;
optionally, the thickness of the metal layer is 300 to 2000nm; preferably 500 to 1000nm.
Further, the present application provides an electrode plate, the pole piece includes above-mentioned compound mass flow body.
Further, the application provides a battery, the battery includes above-mentioned electrode sheet.
Still further, the present application provides an electronic device including the above battery.
Compared with the prior art, the modified polymer film and the preparation method thereof have the following advantages:
(1) The modified polymer film forms a surface modified layer on the surface of the high-molecular polymer base film through a plasma polymerization method, has larger surface polarity and higher surface tension, is stable for a long time, and can be firmly combined with a metal layer.
(2) In the preparation method of the modified polymer film, the reaction raw material is grafted on the surface of the high molecular polymer base film through the reactive sites, so that the surface modified layer is formed, the surface polarity of the modified polymer film prepared by the preparation method is obviously improved, the corresponding surface tension is also obviously improved, the surface tension of the modified polymer film is stable for a long time, and the firm combination of the high molecular polymer base film and the metal layer can be effectively promoted.
Detailed Description
In order that the invention may be more fully understood, reference will now be made to the accompanying examples. This invention may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. The terminology used in the description of the invention herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. Further, the term "plurality" means at least two, e.g., two, three, etc., unless explicitly specified otherwise.
In the present invention, the technical features described in the open type include a closed technical solution composed of the listed features, and also include an open technical solution including the listed features.
In the present invention, the numerical intervals are regarded as continuous, and include the minimum and maximum values of the range and each value between the minimum and maximum values, unless otherwise specified. Further, when a range refers to an integer, each integer between the minimum and maximum values of the range is included. Further, when multiple range-describing features or characteristics are provided, the ranges may be combined. In other words, unless otherwise indicated, all ranges disclosed herein are to be understood to encompass any and all subranges subsumed therein.
In one embodiment of the present disclosure, a modified polymer film is provided, which includes a high molecular polymer base film and a surface modification layer formed on at least one surface of the high molecular polymer base film by a plasma polymerization method.
The traditional metallized polymer film has the problem that the polymer film is not firmly combined with the metal layer on the surface, because the polarity of the polymer film such as polypropylene, polyethylene, polyester and the like is weaker, the surface tension is lower, the affinity between the polymer film with low surface tension and the metal layer with high surface tension is poorer, and the adhesion between the two interfaces is lower and the combination is not firm. In order to solve this problem, a corona method is generally used to increase the surface tension of the polymer film, so as to improve the bonding strength between the polymer film and the metal layer. However, this method has the following disadvantages: (1) On the premise of ensuring that the mechanical property of the polymer film is not changed obviously, the surface tension of the polymer film after corona treatment is generally 35-50 mN/m, compared with the surface tension (25-35 mN/m) of the polymer film before treatment, the lifting amplitude is limited, and a larger difference still exists between the surface tension and the surface tension (more than 100 mN/m) of the metal layer, so that the combination effect between the two is not ideal; (2) The polymer film after corona treatment has unstable surface tension, and after being stored for a period of time, the surface tension is reduced and finally approaches the surface tension of the polymer film before treatment, namely the polymer film has the problem of unstable storage.
The application creatively provides a modified polymer film from the aspect of surface modification treatment, a surface modification layer is formed on one side or two sides of a high molecular polymer base film through a plasma polymerization method, the surface polarity of the obtained modified polymer film is obviously improved, the corresponding surface tension is also obviously improved, the surface tension of the modified polymer film is stable for a long time, and the firm combination of the high molecular polymer base film and a metal layer can be effectively promoted. Therefore, the metallized polymer film prepared by using the modified polymer film as the base material film can effectively solve the problem that the modified polymer film is not firmly combined with the metal layer.
In some embodiments, the reaction raw material of the surface modification layer includes one or more of acrylic acid, acrylonitrile, allylamine, ethylenediamine, n-propylamine, methacrylic acid, methyl methacrylate, and derivatives and copolymers thereof.
It is understood that the reaction material of the surface modification layer includes, but is not limited to, any one of acrylic acid, acrylonitrile, allylamine, ethylenediamine, n-propylamine, methacrylic acid, methyl methacrylate, and their derivatives and copolymers, or the reaction material of the surface modification layer includes, but is not limited to, a mixture of any several of acrylic acid, acrylonitrile, allylamine, ethylenediamine, n-propylamine, methacrylic acid, methyl methacrylate, and their derivatives and copolymers in any ratio.
In some embodiments, the material of the high polymer based film includes one or more of polypropylene (PP), polyethylene (PE), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polyimide (PI), polypropylene, polyvinyl chloride (PVC), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyphenylene Sulfide (PPs), polyphenylene oxide (PPO), polystyrene (PS), polyamide, polyimide, and derivatives thereof.
It is understood that the material of the high polymer base film includes, but is not limited to, any one of polypropylene (PP), polyethylene (PE), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polyimide (PI), polypropylene, polyvinyl chloride (PVC), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyphenylene Sulfide (PPs), polyphenylene oxide (PPO), polystyrene (PS), polyamide, polyimide and their derivatives, or a mixture of a Plurality of Polypropylene (PP), polyethylene (PE), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polyimide (PI), polypropylene, polyvinyl chloride (PVC), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyphenylene Sulfide (PPs), polyphenylene oxide (PPO), polystyrene (PS), polyamide, polyimide and their derivatives in any ratio.
In some embodiments, the thickness of the high molecular polymer-based film is 1 μm or more; preferably 2 to 20 μm.
It is understood that the thickness of the polymer based film is 1 μm or more than 1 μm, including but not limited to any value between 1 μm and 20 μm, for example, the thickness of the polymer based film may be 1 μm, 2 μm, 3 μm, 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm, 15 μm, 16 μm, 17 μm, 18 μm, 19 μm, 20 μm. The thickness of the high molecular polymer-based film is preferably 2 to 20 μm in consideration of the use, production cost and stability.
In some embodiments, the surface modification layer has a thickness of 5 to 200nm; preferably 10 to 100nm.
It is understood that the thickness of the surface modification layer may be any value between 5 and 200nm, for example, the thickness of the surface modification layer may be 5nm, 7nm, 10nm, 20nm, 30nm, 40nm, 50nm, 60nm, 70nm, 80nm, 90nm, 100nm, 110nm, 120nm, 130nm, 140nm, 150nm, 160nm, 170nm, 180nm, 190nm, 200nm. The effect of the surface modification layer of this application is that the surface property (surface tension) of improving the high molecular polymer base film increases surface modification layer thickness and can not further promote the surface property under the even prerequisite of modification, still can increase the raw materials cost simultaneously. In addition, the thickness of the surface modification layer is preferably 10 to 100nm in consideration of easy production operation.
In another aspect of the present application, there is provided a method for preparing the above-described modified polymer film, comprising the steps of: the surface of the high molecular polymer base film is subjected to plasma polymerization modification so as to form a surface modification layer on at least one surface of the high molecular polymer base film.
In some embodiments, when the surface of the high molecular polymer base film is subjected to plasma polymerization modification, a mixed gas composed of oxygen and argon and a reaction raw material are introduced;
the mixed gas bombards the surface of the macromolecule polymer basement membrane to provide reactive sites, and the reaction raw material is grafted on the surface of the macromolecule polymer basement membrane through the reactive sites, so that the surface modification layer is formed.
It should be explained that the oxygen of the present application is used to bombard the high molecular polymer base membrane during the generation of the oxygen plasma, so as to provide the grafting modification reactive site, the argon gas is used to generate the argon plasma, bombard the high molecular polymer base membrane and coarsen the surface of the high molecular polymer base membrane, and the reaction raw material is grafted on the surface of the high molecular polymer base membrane through the reactive site, so as to form the surface modification layer. The surface polarity of the modified polymer film prepared by the preparation method is obviously improved, the corresponding surface tension is also obviously improved, and the surface tension of the modified polymer film is stable for a long time, so that the firm combination of the high molecular polymer base film and the metal layer can be effectively promoted.
In some embodiments, the plasma polymerization apparatus comprises two copper electrodes, optionally at a distance of 5 to 20cm, preferably 8 to 15cm, depending on the effect.
In some embodiments, the surface of the high molecular polymer-based film is modified by plasma polymerization by using a plasma polymerization device;
the plasma polymerization device comprises a radio frequency power supply, and the frequency of the radio frequency power supply is 3-30 MHz; preferably 10-20 MHz; the power of the plasma polymerization device is 10-50W; preferably 20 to 40W.
It is understood that the frequency of the rf power source may be any value between 3 and 30MHz, for example, the frequency of the rf power source may be 3MHz, 5MHz, 8MHz, 10MHz, 14MHz, 18MHz, 20MHz, 23MHz, 26MHz, 30MHz. The frequency of the radio frequency power source is preferably 10 to 20MHz, depending on the effect. The power of the plasma polymerizing apparatus may be any value between 10 and 50W, for example, the power of the plasma polymerizing apparatus may be 10W, 15W, 20W, 25W, 30W, 35W, 40W, 45W, 50W. In view of the effect, the power of the plasma polymerization apparatus is preferably 20 to 40W. When the power of the plasma polymerization device is too low, the reaction rate is too low, and when the power is too high, the reaction is too fast, so that the formed surface modification layer is not uniform.
In some embodiments, the flow ratio of oxygen to argon is (40% to 80%): (60% to 20%).
The vacuum pump of the plasma polymerization device of the present application can adjust the reaction pressure by adjusting the gas flow rate under the condition of normal operation, specifically: first, oxygen gas and argon gas are introduced, and the pressure in the plasma polymerization apparatus is maintained at a value of 10 to 30mTorr by controlling the flow rate of both gases, and then the reaction raw material is introduced, and the pressure in the plasma polymerization apparatus is maintained at a value of 30 to 50mTorr by controlling the flow rate of the reaction raw material. The reactivity is lowered by excessively low or high pressure in the plasma polymerizing apparatus.
In some embodiments, the reaction time for plasma polymerization modification is 1 to 60min.
The reaction time of the plasma polymerization modification may be any value between 1 and 60min, and for example, the reaction time of the plasma polymerization modification may be 1min, 5min, 10min, 15min, 20min, 25min, 30min, 35min, 40min, 45min, 50min, 55min, or 60min.
According to the preparation method of the modified polymer film, parameters such as the reaction time of plasma polymerization modification, the power of a radio frequency power supply of a plasma polymerization device, reaction raw materials and the material of a high polymer base film can be adjusted, so that the surface tension of the modified polymer film and the adhesive force between the modified polymer film and a metal layer are effectively improved.
In a further aspect of the present application, there is provided a metallized polymer film comprising a metal layer and the modified polymer film described above or the modified polymer film prepared by the above preparation method, the metal layer being located on at least one surface modification layer of the modified polymer film;
optionally, the material of the metal layer comprises one or more of copper, copper alloy, aluminum alloy, nickel alloy, titanium and silver.
In some embodiments, the metal layer is prepared by a method comprising one or more of physical vapor deposition, electroplating, and electroless plating, wherein the physical vapor deposition method includes, but is not limited to, resistance heating vacuum evaporation, electron beam heating vacuum evaporation, laser heating vacuum evaporation, and magnetron sputtering.
Yet another aspect of the present application provides a composite current collector comprising the metallized polymer film described above.
In consideration of the conductivity of the material and the cost, the material of the metal layer of the positive composite current collector is preferably aluminum or an aluminum alloy, the content of aluminum in the aluminum alloy is greater than or equal to 80wt%, and more preferably, the content of copper is greater than 90wt%, the material of the metal layer of the negative composite current collector is preferably copper or a copper alloy, the content of copper in the copper alloy is greater than or equal to 80wt%, and more preferably, the content of copper is greater than 90wt%.
In some embodiments, the composite current collector further comprises a protective layer disposed on a surface of the metal layer;
optionally, the material of the protective layer comprises one or more of nickel, chromium, nickel-based alloy, copper oxide, aluminum oxide, nickel oxide, chromium oxide, cobalt oxide, graphite, carbon black, acetylene black, ketjen black, carbon nano quantum dots, carbon nanotubes, carbon nanofibers, and graphene;
optionally, the thickness of the protective layer is 10-200 nm; preferably 50 to 100nm;
optionally, the thickness of the metal layer is 300-2000 nm; preferably 500 to 1000nm.
It is understood that the protective layer provided in the present application is used to prevent the metal layer from being chemically corroded or mechanically damaged, and the material of the protective layer includes, but is not limited to, any one of nickel, chromium, nickel-based alloy, copper oxide, aluminum oxide, nickel oxide, chromium oxide, cobalt oxide, graphite, carbon black, acetylene black, ketjen black, carbon nano quantum dots, carbon nano tubes, carbon nano fibers, and graphene, or the material of the protective layer includes, but is not limited to, any mixture of any several of nickel, chromium, nickel-based alloy, copper oxide, aluminum oxide, nickel oxide, chromium oxide, cobalt oxide, graphite, carbon black, acetylene black, ketjen black, carbon nano quantum dots, carbon nano tubes, carbon nano fibers, and graphene mixed in any proportion. The thickness of the protective layer may be any value between 10 and 200nm, for example, the thickness of the protective layer may be 10nm, 20nm, 30nm, 40nm, 50nm, 60nm, 70nm, 80nm, 90nm, 100nm, 110nm, 120nm, 130nm, 140nm, 150nm, 160nm, 170nm, 180nm, 190nm, 200nm. The thickness of the metal layer is any value between 300 and 2000nm, for example, the thickness of the metal layer may be 300nm, 350nm, 400nm, 450nm, 500nm, 550nm, 600nm, 650nm, 700nm, 750nm, 800nm, 850nm, 900nm, 950nm, 1000nm, 1050nm, 1100nm, 1200nm, 1250nm, 1300nm, 1350nm, 1400nm, 1450nm, 1500nm, 1550nm, 1600nm, 1650nm, 1700nm, 1750nm, 1800nm, 1850nm, 1900nm, 1950nm or 2000nm.
In some embodiments, the composite current collector includes two protective layers, which may be the same or different in material and may or may not be equal in thickness.
In some embodiments, the protective layer is prepared by a method including, but not limited to, one or more of physical vapor deposition, in-situ formation, and coating. Wherein, the vapor deposition method is preferably one or more of a vacuum evaporation method and a magnetron sputtering method; the in-situ forming method is preferably a method for forming a metal oxide passivation layer on the surface of the metal layer in situ; the coating method is preferably one or more of a die coating method, a blade coating method, and an extrusion coating method.
Further, the present application provides an electrode plate, this electrode plate includes above-mentioned compound mass flow body.
It can be understood that the electrode plate may be a positive electrode plate or a negative electrode plate.
Further, the present application provides a battery, which includes the above electrode plate.
Still further, the present application provides an electronic device, which includes the above battery.
The electronic device is not limited in the present application, and the electronic device may include, but is not limited to, a mobile phone, a desktop computer, a notebook computer, an intelligent appliance, an electric vehicle, an electric bicycle, a digital camera, and the like.
The present invention will be described in further detail with reference to specific examples and comparative examples. Experimental parameters not described in the following specific examples are preferably referred to the guidelines given in the present application, and may be referred to experimental manuals in the art or other experimental methods known in the art, or to experimental conditions recommended by the manufacturer. It is understood that the following examples are more specific to the apparatus and materials used, and in other embodiments, are not limited thereto.
Example 1
Material selection: the selected high molecular polymer base film is a commercial 6 mu m biaxial oriented polypropylene (PP) film; the reaction raw material is acrylic acid, and the purity is analytically pure.
1. Preparation of modified Polymer films
Placing a PP film with the thickness of 6 mu m in a plasma polymerization device, setting the distance between copper electrodes to be 10cm, setting the power of a radio frequency power supply to be 10W, and setting the frequency to be 15MHz;
starting a vacuum pump to perform vacuum pumping treatment, opening a first path of gas source after the internal pressure of the plasma polymerization device reaches 10mTorr, and introducing oxygen and argon, wherein the flow ratio of the oxygen to the argon is 70%:30 percent, the pressure in the plasma polymerization device is maintained at 20mTorr by adjusting the flow of the acrylic acid gas and the acrylic acid gas, the second path of gas source is opened after the pressure is stabilized at 20mTorr, the acrylic acid gas is introduced, and the pressure in the plasma polymerization device is maintained at 40mTorr by adjusting the flow of the acrylic acid gas;
starting a radio frequency power supply, starting timing after power and frequency are stable, namely starting plasma polymerization modification, wherein the reaction time is 5min, after the reaction is finished, closing the radio frequency power supply, the first path of gas source, the second path of gas source and the vacuum pump, and taking out the PP membrane after the internal gas pressure reaches the atmospheric pressure, namely the modified polymer membrane.
2. Preparation of negative composite current collector
2.1 preparing the Metal layer
Placing the modified polymer film in a vacuum evaporation chamber, melting and evaporating high-purity copper wires (the purity is more than 99.99%) in a metal evaporation chamber at the high temperature of 1400-2000 ℃, and depositing evaporated metal atoms on two surfaces of the modified polymer film through a cooling system in the vacuum coating chamber to form a copper metal layer with the thickness of 1 mu m;
2.2 preparation of the protective layer
Uniformly dispersing 1g of graphene into 999g of N-methyl pyrrolidone (NMP) solution by an ultrasonic dispersion method to prepare a coating liquid with the solid content of 0.1wt%, uniformly coating the coating liquid on the surface of a metal layer by a die head coating process, wherein the coating amount is controlled at 80 mu m, and then drying at 100 ℃ to obtain the negative electrode composite current collector.
3. Preparing the composite current collector of the positive electrode
3.1 preparing the Metal layer
Placing the modified polymer film in a vacuum evaporation chamber, melting and evaporating high-purity aluminum wires (the purity is more than 99.99%) in a metal evaporation chamber at the high temperature of 1300-2000 ℃, and depositing evaporated metal atoms on two surfaces of the modified polymer through a cooling system in the vacuum coating chamber to form an aluminum metal layer with the thickness of 1 mu m;
3.2 preparation of protective layer
Uniformly dispersing 1g of carbon nano tube into 999g of N-methyl pyrrolidone (NMP) solution by an ultrasonic dispersion method to prepare a coating liquid with the solid content of 0.1wt%, uniformly coating the coating liquid on the surface of a metal layer by a die head coating process, wherein the coating amount is controlled at 90 mu m, and then drying at 100 ℃ to obtain the anode composite current collector.
Example 2
Essentially the same as in example 1, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 10min.
Example 3
Essentially the same as in example 1, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 20min.
Example 4
Essentially the same as in example 1, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 30min.
Example 5
Essentially the same as in example 1, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 50min.
Example 6
Essentially the same as in example 1, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 1min.
Example 7
Essentially the same as in example 1, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 60min.
Example 8
Essentially the same as example 3, except that: when the modified polymer film was prepared, the power of the radio frequency power source of the plasma polymerization apparatus was 20W.
Example 9
Essentially the same as example 3, except that: when the modified polymer film was prepared, the power of the radio frequency power source of the plasma polymerization apparatus was 30W.
Example 10
Essentially the same as example 3, except that: when the modified polymer film was prepared, the power of the radio frequency power source of the plasma polymerization apparatus was 40W.
Example 11
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the reaction raw material is allylamine.
Example 12
Essentially the same as in example 9, except that: when the modified polymer film is prepared, acrylonitrile is used as a reaction raw material.
Example 13
Essentially the same as in example 9, except that: when preparing the modified polymer film, the reaction raw material is methacrylic acid.
Example 14
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the reaction raw material is n-propylamine.
Example 15
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the reaction raw material is methyl methacrylate.
Example 16
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the reaction raw material is ethylenediamine.
Example 17
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the high molecular polymer base film is a 6 mu m biaxially oriented PET film.
Comparative example 1
Essentially the same as in example 9, except that: the high molecular polymer base film (PP film) was not modified.
Comparative example 2
Essentially the same as in example 9, except that: the surface modification layer is formed by a traditional corona modification method, and the method specifically comprises the following steps: the PP film having a thickness of 6 μm was placed in a roll-to-roll corona treatment apparatus, with a corona power of 10kW and a current of 6A, and the surface of the PP film was subjected to a modification treatment at a line speed of 50 m/min.
Comparative example 3
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 0.5min.
Comparative example 4
Essentially the same as in example 9, except that: when the modified polymer film is prepared, the reaction time of plasma polymerization modification is 62min.
Comparative example 5
Essentially the same as in example 9, except that: when the modified polymer film was prepared, the power of the radio frequency power source of the plasma polymerization apparatus was 5W.
Comparative example 6
Essentially the same as in example 9, except that: when the modified polymer film was prepared, the power of the radio frequency power source of the plasma polymerization apparatus was 60W.
Test example 1 surface tension and adhesion test
The modified polymer films prepared in examples 1 to 15 and comparative examples 1 to 6 were subjected to a surface tension test, and the modified polymer films prepared in examples 1 to 15 and comparative examples 1 to 6 were subjected to a cohesive force test on the positive electrode composite current collector and the negative electrode composite current collector, and the test results are shown in table 1. The test method is as follows:
1. surface tension test
Performing a surface tension test on the modified polymer film according to GB/T14216-2008; the surface tension of the modified polymer film just prepared, i.e., the initial surface tension, was tested, and the prepared modified polymer film was left for three months and then tested for surface tension.
2. Adhesion test
Adhering a layer of Permacel P-94 double-sided adhesive tape on an aluminum foil with the thickness of 1mm, adhering a positive electrode composite current collector/negative electrode composite current collector above the double-sided adhesive tape, and covering a layer of ethylene acrylic acid copolymer film above the positive electrode composite current collector/negative electrode composite current collector(Dupont Nurcel0903, 50 μm thick) and then 1.3X 10 5 N/m 2 Hot pressing at 120 deg.c for 10 sec, cooling to room temperature, cutting into 150mm 15mm strips, fixing the ethylene-acrylic acid copolymer film in the upper fixture of a tensile machine, fixing the rest in the lower fixture, and stripping at 180 deg. angle and 100mm/min speed to obtain the stripping force of the modified polymer film and the metal layer.
Table 1 surface tension and adhesion test results
As can be seen from table 1, compared with comparative examples 1 to 2, the surface tension of the modified polymer film in example 9 is significantly increased, and the surface tension of the modified polymer film is substantially unchanged after being left for three months, so that the stability is significantly improved, and meanwhile, the adhesion between the modified polymer film and the metal layer in the positive electrode composite current collector and the negative electrode composite current collector in example 8 is also significantly increased, which indicates that the surface tension and the stability of the modified polymer film prepared by forming the surface modified layer on the surface of the high polymer base film by the plasma polymerization method provided by the present application are significantly increased, and the adhesion between the modified polymer film and the surface metal layer is also significantly increased;
observing the examples 1 to 7 and the comparative examples 3 to 4, the modified polymer films of the examples 4, 5 and 7 have higher surface tension and higher adhesive force between the modified polymer film and the metal layer in the positive electrode composite current collector and the negative electrode composite current collector, which indicates that the modified polymer film has better modification effect when the reaction time of plasma polymerization modification is 30 min;
observing the examples 3, 8 to 10 and 5 to 6, the modified polymer films of the examples 9 to 10 have relatively high surface tension, and the modified polymer films of the positive electrode composite current collector and the negative electrode composite current collector have relatively high adhesive force with the metal layer, which shows that the modified polymer film has good modification effect when the power of the radio frequency power supply of the plasma polymerization device is 30 to 40W, and the polymerization reaction is too fast when the power of the radio frequency power supply of the plasma polymerization device is too high, thus easily causing uneven reaction;
observation of example 9 and examples 11 to 17 revealed that the surface tension of the modified polymer film of example 17 was significantly high, and the adhesion between the modified polymer film and the metal layer in the positive electrode composite current collector and the negative electrode composite current collector was also significantly high, indicating that the modification effect was good when the high molecular polymer base film was a 6 μm biaxially oriented PET film when the modified polymer film was prepared.
The technical features of the embodiments described above may be arbitrarily combined, and for the sake of brevity, all possible combinations of the technical features in the embodiments described above are not described, but should be considered as being within the scope of the present specification as long as there is no contradiction between the combinations of the technical features.
The above-mentioned embodiments only express several embodiments of the present invention, and the description thereof is more specific and detailed, but not construed as limiting the scope of the invention. It should be noted that, for a person skilled in the art, several variations and modifications can be made without departing from the inventive concept, which falls within the scope of the present invention. Therefore, the protection scope of the present patent shall be subject to the appended claims.
Claims (15)
1. A modified polymer film is characterized by comprising a high-molecular polymer base film and a surface modification layer, wherein the surface modification layer is formed on at least one surface of the high-molecular polymer base film through a plasma polymerization method.
2. The modified polymer film of claim 1, wherein the reactive materials of the surface modification layer comprise one or more of acrylic acid, acrylonitrile, allylamine, ethylenediamine, n-propylamine, methacrylic acid, methylmethacrylate, and derivatives and copolymers thereof.
3. The modified polymer film of claim 1, wherein the material of the high molecular polymer base film comprises one or more of polypropylene, polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polyimide, polypropylene, polyvinyl chloride, polyvinylidene fluoride, polytetrafluoroethylene, polyphenylene sulfide, polyphenylene oxide, polystyrene, polyamide, polyimide, and derivatives thereof.
4. The modified polymer film according to claim 1, wherein the thickness of the high molecular polymer base film is 1 μm or more.
5. The modified polymer film of any one of claims 1 to 4, wherein the surface modification layer has a thickness of 5 to 200nm.
6. The method of producing a modified polymer film according to any one of claims 1 to 5, comprising the steps of: and carrying out plasma polymerization modification on the surface of the high-molecular polymer base film so as to form the surface modification layer on at least one surface of the high-molecular polymer base film.
7. The preparation method according to claim 6, wherein when the surface of the high molecular polymer-based film is modified by plasma polymerization, a mixed gas consisting of oxygen and argon and a reaction raw material are introduced;
the mixed gas bombards the surface of the high molecular polymer base film to provide reactive sites, and the reaction raw material is grafted to the surface of the high molecular polymer base film through the reactive sites, so that the surface modification layer is formed.
8. The production method according to claim 6, wherein the surface of the high molecular polymer-based film is subjected to plasma polymerization modification by a plasma polymerization apparatus;
the plasma polymerization device comprises a radio frequency power supply, and the frequency of the radio frequency power supply is 3-30 MHz; the power of the plasma polymerization device is 10-50W.
9. The method according to any one of claims 6 to 8, wherein the reaction time for the plasma polymerization modification is 1 to 60min.
10. A metallized polymer film comprising a metal layer and the modified polymer film according to any one of claims 1 to 5 or the modified polymer film obtained by the production method according to any one of claims 6 to 9, wherein the metal layer is provided on at least one surface modification layer of the modified polymer film;
optionally, the material of the metal layer comprises one or more of copper, copper alloy, aluminum alloy, nickel alloy, titanium and silver.
11. A composite current collector comprising the metallized polymer film of claim 10.
12. The composite current collector of claim 11, further comprising a protective layer disposed on a surface of the metal layer;
optionally, the material of the protective layer comprises one or more of nickel, chromium, nickel-based alloy, copper oxide, aluminum oxide, nickel oxide, chromium oxide, cobalt oxide, graphite, carbon black, acetylene black, ketjen black, carbon nano quantum dots, carbon nanotubes, carbon nanofibers, and graphene;
optionally, the thickness of the protective layer is 10 to 200nm;
optionally, the thickness of the metal layer is 300 to 2000nm.
13. An electrode sheet comprising the composite current collector of claim 11 or 12.
14. A battery comprising the electrode sheet of claim 13.
15. An electronic device comprising the battery according to claim 14.
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| WO2024103525A1 (en) * | 2022-11-15 | 2024-05-23 | 扬州纳力新材料科技有限公司 | Multilayer composite polypropylene material, and preparation method therefor and use thereof |
| WO2024108680A1 (en) * | 2022-11-21 | 2024-05-30 | 扬州纳力新材料科技有限公司 | Polymer composite film, preparation method therefor, composite current collector, electrode sheet, secondary battery and electrical apparatus |
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| WO2024130774A1 (en) * | 2022-12-22 | 2024-06-27 | 扬州纳力新材料科技有限公司 | Polypropylene film and preparation method therefor, composite current collector, and use thereof |
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Application publication date: 20221108 |