CN116504990A - Composite current collector and preparation method and application thereof - Google Patents

Composite current collector and preparation method and application thereof Download PDF

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Publication number
CN116504990A
CN116504990A CN202211665330.3A CN202211665330A CN116504990A CN 116504990 A CN116504990 A CN 116504990A CN 202211665330 A CN202211665330 A CN 202211665330A CN 116504990 A CN116504990 A CN 116504990A
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China
Prior art keywords
layer
conductive layer
protective layer
current collector
conductive
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Pending
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CN202211665330.3A
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Chinese (zh)
Inventor
公秀凤
孙欣森
刘钢
李东亮
姜艳茹
李其其格
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Amrit Technology Beijing Co ltd
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Amrit Technology Beijing Co ltd
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Application filed by Amrit Technology Beijing Co ltd filed Critical Amrit Technology Beijing Co ltd
Priority to CN202211665330.3A priority Critical patent/CN116504990A/en
Publication of CN116504990A publication Critical patent/CN116504990A/en
Priority to CN202311091465.8A priority patent/CN117154102A/en
Pending legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/043—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/20—Layered products comprising a layer of metal comprising aluminium or copper
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B9/041—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material of metal
    • 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
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • C08J7/04—Coating
    • C08J7/042—Coating with two or more layers, where at least one layer of a composition contains a polymer binder
    • C08J7/0423—Coating with two or more layers, where at least one layer of a composition contains a polymer binder with at least one layer of inorganic material and at least one layer of a composition containing a polymer binder
    • 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
    • C08J7/00—Chemical treatment or coating of shaped articles made of macromolecular substances
    • C08J7/04—Coating
    • C08J7/06—Coating with compositions not containing macromolecular substances
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
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    • C23C14/20—Metallic material, boron or silicon on organic substrates
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    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/06—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the coating material
    • C23C14/14—Metallic material, boron or silicon
    • C23C14/20—Metallic material, boron or silicon on organic substrates
    • C23C14/205—Metallic material, boron or silicon on organic substrates by cathodic sputtering
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/24—Vacuum evaporation
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/24—Vacuum evaporation
    • C23C14/26—Vacuum evaporation by resistance or inductive heating of the source
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/24—Vacuum evaporation
    • C23C14/28—Vacuum evaporation by wave energy or particle radiation
    • C23C14/30—Vacuum evaporation by wave energy or particle radiation by electron bombardment
    • C—CHEMISTRY; METALLURGY
    • C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
    • C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
    • C23C14/00—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material
    • C23C14/22—Coating by vacuum evaporation, by sputtering or by ion implantation of the coating forming material characterised by the process of coating
    • C23C14/34—Sputtering
    • C23C14/35—Sputtering by application of a magnetic field, e.g. magnetron sputtering
    • 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
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0404—Methods of deposition of the material by coating on electrode collectors
    • 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
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0421—Methods of deposition of the material involving vapour deposition
    • H01M4/0423—Physical vapour deposition
    • 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
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0421—Methods of deposition of the material involving vapour deposition
    • H01M4/0423—Physical vapour deposition
    • H01M4/0426—Sputtering
    • 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
    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2307/00—Properties of the layers or laminate
    • B32B2307/20—Properties of the layers or laminate having particular electrical or magnetic properties, e.g. piezoelectric
    • B32B2307/202—Conductive
    • 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
    • C08J2367/00—Characterised by the use of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Derivatives of such polymers
    • C08J2367/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
    • 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
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Abstract

The invention relates to the technical field of current collectors, and discloses a composite current collector, a preparation method and application thereof. The composite current collector sequentially comprises: protective layer I, conducting layer I, tie coat I, substrate, tie coat II, conducting layer II and protective layer II. The method comprises the following steps: preparing a bonding layer I on the upper surface of a substrate, preparing a bonding layer II on the upper surface and the lower surface of the substrate, preparing a conductive layer I on the bonding layer I, preparing a conductive layer II on the bonding layer II, preparing a protective layer I on the conductive layer I, and preparing a protective layer II on the conductive layer II to obtain the composite current collector. The lithium ion battery prepared by the composite current collector has high stability, high safety and longer service life.

Description

Composite current collector and preparation method and application thereof
Technical Field
The invention relates to the technical field of current collectors, in particular to a composite current collector, a preparation method and application thereof.
Background
Unlike conventional pure copper/aluminum, the composite current collector is a composite of a base film and copper/aluminum. Taking PET copper foil as an example, the structure is 4.5 mu m PET base film and two 1 mu m copper layers on two sides, and the PET base film has the advantages that: 1) The PET layer and the magnetron sputtering form a flame-retardant structure, so that the possibility of burning, ignition and explosion of the battery is reduced; 2) The PET material has light weight, and reduces the overall quality of the battery, thereby improving the energy density; 3) The use amount of copper foil/aluminum foil is reduced, and the cost is low.
Unlike conventional foil manufacturing processes, conventional aluminum and copper foils are mainly produced using rolling or electrolytic processes. The composite aluminum/copper foil is a metal layer which is prepared on the surface of a plastic film through magnetron sputtering and vacuum evaporation, and then the metal layer is thickened through water electroplating to prepare the composite metal foil so as to replace the traditional current collector. The water electroplating method has the following defects: 1) The electroplating material is single, and the surface of the non-conductive base material needs conductive treatment; 2) The coating is easy to generate chromatic aberration, and the color of the vacuum coating is not stable; 3) The density of the electroplated layer is poor; 4) The environmental protection problems of waste water, waste gas and the like exist, and the method is not friendly to the environment.
However, in the existing composite current collector, metal is generally deposited on a flexible polymer substrate in vacuum to obtain a sandwich structure of a conductive layer, a polymer layer and a conductive layer, and the substrate is subjected to vacuum deposition, so that the flexible substrate is required to be repeatedly film-formed for more than 20 times due to the problem of thermal damage, the composite current collector obtained by the method has the advantages of over-high rigidity, large film brittleness of the composite current collector, very low elongation at break, and insufficient connection strength between the substrate and the conductive layer, so that the conductive layer is easy to fall off from the substrate, and no protection measure is taken above the conductive layer.
Accordingly, there is a need to provide a composite current collector product having high binding force, high mechanical strength and high conductivity that is efficiently formed into a film without the occurrence of product problems such as "thermal damage".
Disclosure of Invention
The invention aims to solve the problems of low mechanical strength, low conductivity, thermal damage to a base material and low connection strength between the base material and a conductive layer of a composite current collector in the prior art, and provides a composite current collector, a preparation method and application thereof.
In order to achieve the above object, a first aspect of the present invention provides a composite current collector, comprising, in order: the protective layer I, the conductive layer I, the bonding layer I, the substrate, the bonding layer II, the conductive layer II and the protective layer II;
when the conductive layer I and the conductive layer II are aluminum, the materials of the protective layer I and the protective layer II are respectively and independently selected from one or more of nickel, chromium, conductive polypyrrole and conductive polyaniline; when the conductive layer I and the conductive layer II are copper, the materials of the protective layer I and the protective layer II are respectively and independently selected from one or more of nickel, chromium and modified benzotriazole;
the materials of the bonding layer I and the bonding layer II are respectively and independently selected from one or more of nickel, copper, chromium, nichrome, nickel-copper alloy, cobalt oxide, chromium oxide, nickel oxide and aluminum oxide.
The second aspect of the present invention provides a method for preparing a composite current collector, the method comprising the steps of:
(1) Preparing a bonding layer I on the upper surface of a substrate, and preparing a bonding layer II on the lower surface of the substrate to obtain a first intermediate;
(2) Preparing a conductive layer I on the bonding layer I, and preparing a conductive layer II on the bonding layer II to obtain a second intermediate;
(3) And preparing a protective layer I on the conductive layer I, and preparing a protective layer II on the conductive layer II to obtain the composite current collector.
The third aspect of the invention provides an application of the composite current collector disclosed in the first aspect of the invention or the composite current collector manufactured by the manufacturing method disclosed in the second aspect of the invention in a lithium ion battery.
Through the technical scheme, the beneficial technical effects obtained by the invention are as follows:
according to the invention, the bonding layer is arranged in the composite current collector, so that the connection strength between the conductive layer and the base material can be obviously improved, and the conductive layer is prevented from falling off in the use process. The composite current collector has the advantages of high mechanical strength, high conductivity and no thermal damage to the base material. The lithium ion battery prepared by the composite current collector has high stability, high safety and longer service life.
Drawings
Fig. 1 is a schematic structural view of a composite current collector according to the present invention.
Description of the reference numerals
1-a substrate; 2-tie layer I; 3-tie layer II; 4-conductive layer I; 5-conductive layer II; 6-a protective layer I; 7-protective layer II.
Detailed Description
The endpoints and any values of the ranges disclosed herein are not limited to the precise range or value, and are understood to encompass values approaching those ranges or values. For numerical ranges, one or more new numerical ranges may be found between the endpoints of each range, between the endpoint of each range and the individual point value, and between the individual point value, in combination with each other, and are to be considered as specifically disclosed herein.
A first aspect of the present invention provides a composite current collector, as shown in fig. 1, comprising, in order: protective layer I6, conductive layer I4, adhesive layer I2, substrate 1, adhesive layer II 3, conductive layer II 5 and protective layer II 7; when the conductive layer I4 and the conductive layer II 5 are aluminum, the materials of the protective layer I6 and the protective layer II 7 are respectively and independently selected from one or more of nickel, chromium, conductive polypyrrole and conductive polyaniline; when the conductive layer I4 and the conductive layer II 5 are copper, the materials of the protective layer I6 and the protective layer II 7 are respectively and independently selected from one or more of nickel, chromium and modified benzotriazole;
the materials of the bonding layers I2 and II 3 are respectively and independently selected from one or more of nickel, copper, chromium, nichrome, nickel-copper alloy, cobalt oxide, chromium oxide, nickel oxide and aluminum oxide.
The adhesive layer is used for enhancing the bonding force between the substrate and the conductive layer.
The structure of the composite current collector is sequentially a protective layer I-conductive layer I-bonding layer I-base material-bonding layer II-conductive layer II-protective layer II from top to bottom.
In a preferred embodiment, the substrate 1 is selected from one or more of Polyethylene (PE), polystyrene (PS), polyvinylchloride (PVC), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polypropylene (PP), biaxially oriented polypropylene (BOPP), polypropylene (PPE), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyethylene terephthalate (PEN), poly-p-phenylene terephthalamide (PPA), polyamide (PA), polyimide (PI), poly-p-phenylene ether (PPO), poly-p-Phenylene Sulfide (PPs), polycarbonate (PC), polyetheretherketone (PEEK), polyoxymethylene (POM), epoxy, phenolic, acrylonitrile-butadiene-styrene copolymer (ABS), preferably one or more of polypropylene (PP), polyethylene terephthalate (PET) and Polyimide (PI).
The biaxially oriented polypropylene film (BOPP) is prepared by co-extruding polypropylene particles to form a sheet and then stretching in the longitudinal and transverse directions (bidirectionally). Biaxially oriented polypropylene films known in the art may be used in the present invention.
In a preferred embodiment, the mass fraction of nickel in the nichrome in the materials of the binding layer I2 and the binding layer II 3 is 70-90%, such as 70%, 75%, 80%, 85%, 90%, and any value in the range of any two values mentioned above; the mass fraction of chromium is 10-30%, e.g. 10%, 15%, 20%, 25%, 30%, and any value in the range of any two values mentioned above.
According to the invention, the bonding layer is arranged in the composite current collector, so that the connection strength between the conductive layer I and the base material and between the base material and the conductive layer II can be obviously improved, the conductive layer I and the conductive layer II are prevented from falling off in the use process, and the stability and the safety of the lithium ion battery prepared by using the composite current collector are obviously improved.
In a preferred embodiment, the conductive layer I4 and the conductive layer II 5 are the same material and are selected from aluminum or copper. In the invention, when the materials of the conductive layer I4 and the conductive layer II 5 are aluminum, the composite current collector is a positive current collector; when the materials of the conductive layer I4 and the conductive layer II 5 are copper, the composite current collector is a negative current collector.
In a preferred embodiment, the conductive layers I4 and II 5 are aluminum, and the materials of the protective layers I6 and II 7 are independently selected from one or more of nickel, chromium, conductive polypyrrole, and conductive polyaniline, respectively.
In the present invention, nickel or chromium generates nickel oxide or chromium oxide under air conditions, and may be used as a protective layer.
In the present invention, the conductive polypyrrole and the conductive polyaniline can be obtained by doping. The polyaniline may be doped with a protonic acid. The doping of polypyrrole is generally classified into chemical doping (the oxidant is ferric iron, ammonium persulfate or metal-organic coupling) and electrochemical doping (electric field).
In the invention, the protective layer is prepared on the conductive layer, and has the effects of conductivity and corrosion resistance, and metallic nickel and chromium have conductivity and can generate a compact corrosion-resistant oxide film in a natural state, so that the protective layer has the corrosion-resistant effect; the doped polypyrrole/polyaniline has high conductivity, light weight, low monomer cost and easy processing into films.
In a preferred embodiment, the conductive layers I4 and II 5 are copper, and the materials of the protective layers I6 and II 7 are independently selected from nickel and/or modified benzotriazole (modified BTA), respectively.
In the invention, metallic nickel can generate nickel oxide under natural conditions to prevent the copper layer from oxidative discoloration.
In a preferred embodiment, the modified benzotriazole is Benzotriazole (BTA) and 2-mercaptoMixtures of Benzothiazoles (MBT). When preparing the protective layer, the conductive layer is treated with BTA to form a layer of complex (Cu) formed by BTA and monovalent copper ions on the copper surface 2 BTA) protective film can prevent further corrosion of copper. The hydrogen atom on the mercapto group of the 2-Mercaptobenzothiazole (MBT) molecule can be dissociated in water, and the chemical adsorption between the sulfur atom and copper forms a very firm complex (Cu-MBT) protective film to inhibit the corrosion of copper.
The preparation method of the modified benzotriazole can be selected from the following steps: preparing a compound solution of 0.5mmol/L BTA and 0.5mmol/L MBT, magnetically stirring until the compound solution is completely dissolved, coating a copper current collector base film by a coating machine, drying for 30min in a drying box at 50-80 ℃, and taking out.
In the invention, the protective layer I and the protective layer II prepared by nickel and/or modified BTA can prevent copper from being oxidized and prevent electrolyte from corroding the conductive layer.
That is, in the invention, the interface resistance between the current collector and the active material can be reduced by arranging the protective layer I and the protective layer II in the composite current collector, so that the internal resistance of the lithium ion battery prepared by using the composite current collector is reduced, and the multiplying power performance and the cycle performance of the lithium ion battery are improved.
In a preferred embodiment, the thickness of the substrate 1 is in the range of 2-12 μm, e.g. 2 μm, 3 μm, 5 μm, 8 μm, 10 μm, 12 μm, and any value in the range of any two values mentioned above. The thickness of the adhesive layers I2 and II 3 is independently selected from any value in the range of 0.01-0.1 μm, e.g. 0.01 μm, 0.03 μm, 0.05 μm, 0.08 μm, 0.1 μm, and any two values mentioned above, respectively. The thickness of the conductive layer I4 and the conductive layer II 5 are independently selected from any value in the range of 0.1-1.5 μm, for example 0.1 μm, 0.3 μm, 0.5 μm, 1 μm, 1.2 μm, 1.5 μm, and any two values mentioned above, respectively. The thickness of the protective layers I6 and II 7 is independently selected from any value within the range of 0.01-1 μm, for example 0.01 μm, 0.05 μm, 0.1 μm, 0.3 μm, 0.5 μm, 0.8 μm, 1 μm, and any two values of the above, respectively.
In a preferred embodiment, the bonding force between the conductive layer I4 and the substrate 1 and between the conductive layer II 5 and the substrate 1 is independently in the range of 0.5 to 20N/15mm, for example 0.5N/15mm, 1N/15mm, 2N/15mm, 4N/15mm, 5N/15mm, 7N/15mm, 8N/15mm, 10N/15mm, 11N/15mm, 13N/15mm, 15N/15mm, 18N/15mm, 20N/15mm, and any value in the range of any two values mentioned above, respectively, preferably 2 to 15N/15mm.
In a preferred embodiment, the sheet resistance of the composite current collector is 3 to 5000mΩ/≡, preferably 10 to 500mΩ/≡.
In a preferred embodiment, the composite current collector has an electrical resistivity of 1×10 -8 -8×10 -8 Omega.m, preferably 1.5X10 -8 -5×10 -8 Ω·m。
In a preferred embodiment, the grain size of the conductive layer I4 and the conductive layer II 5 is in the range of 10nm to 2000nm, for example 10nm, 100nm, 300nm, 500nm, 1000nm, 1500nm, 2000nm, and any value in the range of any two values mentioned above. In the present invention, the grain size refers to the size of the metal particles in the conductive layer I4 and the conductive layer II 5.
In a preferred embodiment, the thickness of the composite current collector is 0.1-13 μm, for example 0.1 μm, 1 μm, 3 μm, 5 μm, 8 μm, 10 μm, 13 μm, and any value in the range of any two values mentioned above, preferably 2-12 μm.
In a preferred embodiment, the composite current collector is capable of achieving excellent tensile strength, elongation at break, elastic modulus, sheet resistance, electrical resistivity.
In a preferred embodiment, the composite current collector may achieve the following properties:
the tensile strength is 100-400MPa, the elongation at break is more than or equal to 20%, the binding force is more than or equal to 0.5N/15mm, the sheet resistance is 3-5000mΩ/≡s, and the resistivity is 1 multiplied by 10 -8 -8×10 -8 Ω·m。
The composite current collector provided by the invention has the advantages that the protective layers (the protective layer I and the protective layer II), the conductive layers (the conductive layers I and the conductive layers II) and the bonding layers (the bonding layers I and the bonding layers II) interact with the base material, so that the dosage of aluminum copper can be reduced, the thickness of the current collector is reduced, the weight of the current collector is lightened, the mechanical property of the current collector is increased, the production cost of the current collector can be reduced, and the energy density and the service life of the lithium ion battery are improved.
According to the invention, the bonding layer is arranged in the composite current collector, so that the connection strength between the conductive layer and the base material can be obviously improved, and the conductive layer is prevented from falling off in the use process. The composite current collector has the advantages of high mechanical strength, high conductivity and no thermal damage to the base material. The lithium ion battery prepared by the composite current collector has high stability, high safety and longer service life.
A second aspect of the present invention provides a method for preparing the composite current collector according to the first aspect of the present invention, the method comprising the steps of:
(1) Preparing a bonding layer I on the upper surface of a substrate, and preparing a bonding layer II on the lower surface of the substrate to obtain a first intermediate;
(2) Preparing a conductive layer I on the bonding layer I, and preparing a conductive layer II on the bonding layer II to obtain a second intermediate;
(3) And preparing a protective layer I on the conductive layer I, and preparing a protective layer II on the conductive layer II to obtain the composite current collector.
In a preferred embodiment, the materials of the bonding layer I and the bonding layer II are independently selected from nickel and/or nichrome, and the bonding layer I and the bonding layer II are prepared by sputtering or vapor deposition.
In a preferred embodiment, the materials of the bonding layer I and the bonding layer II are aluminum oxides, and the preparation method of the bonding layer I and the bonding layer II is in-situ reaction.
In a preferred embodiment, the method for preparing the conductive layer I and the conductive layer II is evaporation, preferably evaporation-resistant or electron gun evaporation.
In the present invention, the evaporation-blocking means a resistance heating evaporation method.
In the invention, the conductive layer I and the conductive layer II are prepared by adopting the vapor-blocking or electron gun vapor deposition, so that the conductive layer with high density can be obtained, the defects are fewer, the resistivity is relatively low, and the obtained composite current collector meets the requirements of a battery.
In a preferred embodiment, the material of the protective layer I and the protective layer II is nickel, and the preparation method of the protective layer I and the protective layer II is sputtering.
In a preferred embodiment, the conductive layer I and the conductive layer II are aluminum, the material of the protective layer I and the protective layer II is conductive polypyrrole, and the preparation method of the protective layer I and the protective layer II includes: firstly, sequentially coating a silane coupling agent, pyrrole monomer solution and FeCl on the surfaces of the conductive layer I and the conductive layer II 3 The solution is polymerized, then washed and dried.
In a preferred embodiment, the silane coupling agent is KH550.
In a preferred embodiment, the pyrrole monomer solution is an ethanol solution of pyrrole monomer. For example, the purified pyrrole monomer is formulated with absolute ethanol to give a pyrrole monomer solution of a certain concentration.
In a preferred embodiment, the FeCl 3 The solution is FeCl 3 Is a solution of (a) and (b).
Wherein, in the invention, the surfaces of the conductive layer I and the conductive layer II are coated with a silane coupling agent, then with pyrrole monomer solution, and then with FeCl 3 Solution, silane coupling agent, pyrrole monomer and FeCl 3 The polymerization reaction can occur when the polymer is contacted at room temperature, and the conductive polypyrrole is generated. After the polymerization reaction is finished, the mixture can be respectively washed by clean water and ethanol to remove redundant FeCl 3 The solution is dried to obtain the polypyrrole film.
In a preferred embodiment, the conductive layer I and the conductive layer II are aluminum, the material of the protective layer I and the protective layer II is conductive polyaniline, and the preparation method of the protective layer I and the protective layer II includes: firstly, mixing aniline, p-toluenesulfonic acid solution (serving as protonic acid) and potassium dichromate uniformly to obtain a mixed coating; and then the mixed paint is coated on the surfaces of the conductive layer I and the conductive layer II, and the mixed paint reacts for 20-30 hours under the vacuum and the temperature of 80-90 ℃.
In a preferred embodiment, the vacuum condition has a vacuum degree of 100 to 150Pa, preferably 133Pa.
In the invention, when the conductive layer I and the conductive layer II are aluminum, aniline, p-toluenesulfonic acid and potassium dichromate are subjected to polymerization reaction on the surfaces of the conductive layer I and the conductive layer II, so that conductive polyaniline can be generated, and a polyaniline film is obtained.
In a preferred embodiment, the conductive layer I and the conductive layer II are copper, and the material of the protective layer I and the protective layer II is modified benzotriazole.
In a preferred embodiment, the sputtering is magnetron sputtering. Preferably, the operating conditions of the magnetron sputtering include: vacuum degree higher than 10 -3 Pa; the main roll temperature is-25 ℃ to +35 ℃, such as-25 ℃, -15 ℃, -5 ℃, 0 ℃, 10 ℃, 20 ℃, 25 ℃, 30 ℃, 35 ℃, or any value in between the foregoing; the main roller running speed is below 20m/min, such as 5m/min, 10m/min, 15m/min, 20m/min, or any value between the foregoing values; the sputtering power is 20kW or less, for example 5kW, 15kW, 20kW, or any value in between the foregoing values.
The description about the degree of vacuum is as follows: the smaller the value of the rarefaction degree of the gas in the vacuum state, the rarefaction degree of the gas is indicated, and the higher the vacuum degree is.
In a preferred embodiment, the evaporation is vacuum evaporation. Preferably, the operating conditions of the vacuum evaporation include: vacuum degree higher than 10 -3 Pa; the chill roll temperature is from-25 ℃ to +35 ℃, such as-25 ℃, -15 ℃, -5 ℃, 0 ℃, 10 ℃, 20 ℃, 25 ℃, 30 ℃, 35 ℃, or any value in between the foregoing; ES distance. Gtoreq.50 mm, e.g., 50mm, 55mm, 60mm, 70mm, 80mm, 100mm, 120mm, or any value therebetween; the evaporating temperature is 800 ℃, such as 800 ℃, 850 ℃, 900 ℃, 1000 ℃, 1100 ℃, 1200 ℃, 1500 ℃, or any value between the foregoing values.
In the present invention, the ES distance refers to the distance between the evaporation source and the substrate.
The evaporation source is a conductive metal material that is vaporized by heating in a vacuum deposition chamber. The substrate is a pre-evaporated film.
The third aspect of the invention provides an application of the composite current collector disclosed by the first aspect of the invention or the composite current collector prepared by the preparation method disclosed by the second aspect of the invention in a lithium ion battery.
In the invention, the method for testing the relevant parameters is as follows:
thickness/roughness: national standard of the people's republic of China GB/T11378-2005 (metal coating thickness measuring profilometer method).
Areal density: national standard GB/T22638.10-2016 of the people's republic of China (part 10 of aluminium foil test method: determination of coating surface Density).
Sheet resistance/resistivity: ASTM F390 in the united states (standard test method for measuring sheet resistance of metal films using the collinear four-probe method).
Binding force: national standard of the people's republic of China GB/T2792-2014 (test method of adhesive tape peel strength).
Mechanical properties: china HG/T2580-2008 (determination of tensile Strength and elongation at break of rubber or Plastic coated fabrics).
Wetting tension: national standard GB/T22638.4-2016 (aluminium foil test method part 4: determination of surface wetting tension) of the people's republic of China.
The preferred embodiments of the present invention have been described in detail above, but the present invention is not limited thereto. Within the scope of the technical idea of the invention, a number of simple variants of the technical solution of the invention are possible, including combinations of the individual technical features in any other suitable way, which simple variants and combinations should likewise be regarded as being disclosed by the invention, all falling within the scope of protection of the invention.

Claims (10)

1. A composite current collector, comprising, in order: the protective layer I, the conductive layer I, the bonding layer I, the substrate, the bonding layer II, the conductive layer II and the protective layer II;
when the conductive layer I and the conductive layer II are aluminum, the materials of the protective layer I and the protective layer II are respectively and independently selected from one or more of nickel, chromium, conductive polypyrrole and conductive polyaniline; when the conductive layer I and the conductive layer II are copper, the materials of the protective layer I and the protective layer II are respectively and independently selected from one or more of nickel, chromium and modified benzotriazole;
the materials of the bonding layer I and the bonding layer II are respectively and independently selected from one or more of nickel, copper, chromium, nichrome, nickel-copper alloy, cobalt oxide, chromium oxide, nickel oxide and aluminum oxide.
2. The composite current collector of claim 1 wherein the substrate is selected from one or more of polyethylene, polystyrene, polyvinyl chloride, polyvinylidene fluoride, polytetrafluoroethylene, polypropylene, biaxially oriented polypropylene, polyethylene terephthalate, polybutylene terephthalate, polyethylene terephthalate, poly-p-phenylene terephthalamide, polyamide, polyimide, poly-p-phenylene ether, poly-p-phenylene sulfide, polycarbonate, polyetheretherketone, polyoxymethylene, epoxy, phenolic, and acrylonitrile-butadiene-styrene copolymer.
3. A composite current collector according to claim 1 or 2, wherein the mass fraction of nickel in the nichrome is 70-90% and the mass fraction of chromium in the materials of the tie layers I and II is 10-30%.
4. A composite current collector according to any one of claims 1-3, wherein the binding forces between the conductive layer I and the substrate and between the conductive layer II and the substrate, respectively, are independently 0.5-20N/15mm, preferably 2-15N/15mm;
preferably, the sheet resistance of the composite current collector is 3-5000mΩ/≡, preferably 10-500mΩ/≡; resistivity of 1X 10 -8 -8×10 -8 Omega.m, preferably 1.5X10 -8 -5×10 -8 Ω·m。
5. The composite current collector according to any one of claims 1 to 4, wherein the grain size of the conductive layers I and II is 10nm to 2000nm;
preferably, the thickness of the composite current collector is 0.1 to 13 μm, preferably 2 to 12 μm.
6. A method of preparing a composite current collector, the method comprising the steps of:
(1) Preparing a bonding layer I on the upper surface of a substrate, and preparing a bonding layer II on the lower surface of the substrate to obtain a first intermediate;
(2) Preparing a conductive layer I on the bonding layer I, and preparing a conductive layer II on the bonding layer II to obtain a second intermediate;
(3) And preparing a protective layer I on the conductive layer I, and preparing a protective layer II on the conductive layer II to obtain the composite current collector.
7. The preparation method according to claim 6, wherein in the step (1), the materials of the bonding layer I and the bonding layer II are respectively independently selected from nickel and/or nichrome, and the preparation method of the bonding layer I and the bonding layer II is sputtering or evaporation;
preferably, the materials of the bonding layer I and the bonding layer II are aluminum oxides, and the preparation methods of the bonding layer I and the bonding layer II are in-situ reactions;
preferably, in the step (2), the preparation method of the conductive layer I and the conductive layer II is evaporation, preferably evaporation-resistant or electron gun evaporation.
8. The preparation method according to claim 6 or 7, wherein in the step (3), the material of the protective layer I and the protective layer II is nickel, and the preparation method of the protective layer I and the protective layer II is sputtering;
preferably, the conductive layer I and the conductive layer II are aluminum, the materials of the protective layer I and the protective layer II are conductive polypyrrole, and the preparation method of the protective layer I and the protective layer II includes: firstly, sequentially coating a silane coupling agent, an pyrrole monomer solution and a conductive layer II on the surfaces of the conductive layer I and the conductive layer IIFeCl 3 Polymerizing the solution, and then cleaning and drying;
preferably, the conductive layer I and the conductive layer II are aluminum, the material of the protective layer I and the protective layer II is conductive polyaniline, and the preparation method of the protective layer I and the protective layer II includes: firstly, mixing aniline, p-toluenesulfonic acid solution and potassium dichromate uniformly to obtain a mixed coating; then coating the mixed paint on the surfaces of the conductive layer I and the conductive layer II, and reacting for 20-30 hours at the temperature of 80-90 ℃ under vacuum;
preferably, the conductive layer I and the conductive layer II are copper, and the material of the protective layer I and the protective layer II is modified benzotriazole.
9. The production method according to any one of claims 6 to 8, wherein the sputtering is magnetron sputtering;
preferably, the operating conditions of the magnetron sputtering include: vacuum degree higher than 10 -3 Pa; the temperature of the main roller is between minus 25 ℃ and plus 35 ℃; the running speed of the main roller is below 20 m/min; the sputtering power is below 20 kW;
preferably, the evaporation is vacuum evaporation;
preferably, the operating conditions of the vacuum evaporation include: vacuum degree higher than 10 -3 Pa; the temperature of the cold roller is between minus 25 ℃ and plus 35 ℃; the ES distance is more than or equal to 50mm; the evaporation temperature is more than or equal to 800 ℃.
10. Use of a composite current collector according to any one of claims 1 to 5 or a composite current collector produced by a method according to any one of claims 6 to 9 in a lithium ion battery.
CN202211665330.3A 2022-12-23 2022-12-23 Composite current collector and preparation method and application thereof Pending CN116504990A (en)

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