CN110620238A - Current collector and preparation method thereof, negative electrode and secondary battery - Google Patents
Current collector and preparation method thereof, negative electrode and secondary battery Download PDFInfo
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- CN110620238A CN110620238A CN201910915966.0A CN201910915966A CN110620238A CN 110620238 A CN110620238 A CN 110620238A CN 201910915966 A CN201910915966 A CN 201910915966A CN 110620238 A CN110620238 A CN 110620238A
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- 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
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- 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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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- 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
- H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
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- 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
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- 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
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Composite Materials (AREA)
- Cell Electrode Carriers And Collectors (AREA)
Abstract
The invention discloses a current collector and a preparation method thereof, wherein the current collector comprises a copper sheet body and a PI film layer formed on the copper sheet body, the PI film layer is divided into a plurality of PI units which are spaced from each other through laser scanning irradiation, and the peripheral side wall of each PI unit is provided with laser-induced graphene. The invention also discloses a negative electrode comprising the current collector and a corresponding secondary battery. The current collector provided by the invention is applied to the secondary battery, so that the secondary battery has higher and more stable coulombic efficiency and longer cycle life.
Description
Technical Field
The invention belongs to the technical field of secondary batteries, and particularly relates to a current collector and a preparation method thereof, and also relates to a negative electrode containing the current collector and a corresponding secondary battery.
Background
The lithium battery has the advantages of wide working temperature range, stable discharge voltage, low self-discharge rate, long service life and the like, and is widely applied to various fields, in particular to the fields of aerospace, military, long-life instruments and meters, logistics tracking, automotive electronics, mobile digital products and the like.
The lithium battery works on the principle of an electrochemical device for converting chemical energy into electric energy, and in the process, a medium is needed for transferring the electric energy converted from the chemical energy, and a conductive material is used as a current collector. Among the common materials, the metallic material is the most conductive material, among which copper is inexpensive and has good conductivity.
The preparation of the current electrode using copper foil as the current collector is mainly as follows: and directly coating the active material slurry on the surface of the copper foil, and fixing the active material on the surface of the current collector through a binder after drying. In the electrode structure, expansion and separation between the active material and the current collector are easy to occur in the continuous charging and discharging process, the internal resistance is increased, and the lithium metal battery still has the problems of low coulombic efficiency, rapid capacity degradation and the like.
Disclosure of Invention
In view of the defects in the prior art, the invention provides a current collector and a preparation method thereof, wherein the current collector can enable secondary batteries such as lithium batteries and the like to have higher and more stable coulombic efficiency and longer cycle life.
In order to achieve the purpose, the invention adopts the following technical scheme:
a current collector comprises a copper sheet body and a PI film layer formed on the copper sheet body, wherein the PI film layer is divided into a plurality of PI units which are spaced from each other through laser scanning irradiation, and laser-induced graphene is formed on the peripheral side wall of each PI unit.
Specifically, the PI units spaced from each other are arranged on the copper sheet body in a matrix array.
Specifically, the copper sheet body is a copper foil, and the thickness of the copper sheet body is 10-20 microns.
Specifically, the thickness of the PI film layer is 50-70 μm.
The invention also provides a preparation method of the current collector, which comprises the following steps: providing a copper sheet body and preparing and forming a PI film layer on the copper sheet body; and carrying out laser scanning irradiation on the PI film layer, dividing the PI film layer into a plurality of PI units which are spaced from each other, and forming laser-induced graphene on the peripheral side wall of each PI unit.
Specifically, the process conditions for performing laser scanning irradiation are as follows: the laser power density is 60W/cm2～95W/cm2The scanning speed is 2 cm/s-4 cm/s, and the scanning interval is 400 mu m-800 mu m.
Specifically, laser scanning irradiation is respectively carried out on the PI film layer along a first direction and a second direction which are perpendicular to each other, so that a plurality of PI units which are formed and spaced from each other are arranged on the copper sheet body in a matrix array mode.
Specifically, the laser scanning irradiation times of the PI film layer along the first direction and/or the second direction are 3-8 times.
The invention also provides an electrode pole piece, which comprises the current collector.
It is another aspect of the present invention to provide a secondary battery including the electrode tab as described above.
According to the current collector and the preparation method thereof provided by the embodiment of the invention, a copper sheet (copper foil) is used as a body, a PI film layer is divided into a plurality of mutually spaced PI units by Laser scanning irradiation, and Laser Induced Graphene (LIG) is formed around each PI unit, so that the prepared current collector is applied to secondary batteries such as lithium batteries, and the secondary batteries can have higher and more stable coulombic efficiency and longer cycle life.
Drawings
Fig. 1 is an SEM image of a current collector provided by an embodiment of the present invention;
fig. 2 is a schematic structural diagram of a single PI cell in a current collector provided by an embodiment of the present invention;
fig. 3 is an SEM image of a single PI cell in a current collector provided by an embodiment of the present invention;
FIG. 4 is an enlarged SEM image of the edge portion of a single PI unit in an embodiment of the present invention;
fig. 5 is a process flow diagram of a method of making a current collector of an embodiment of the present invention;
FIG. 6 shows the cell samples of example 4 at 1mA/cm2A coulombic efficiency map at current density of (a);
FIG. 7 shows a sample of the cell of example 4 at 2mA/cm2A coulombic efficiency map at current density of (a);
FIG. 8 shows the cell sample of example 4 at 5mA/cm2Coulombic efficiency at current density of (a).
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, embodiments of the present invention are described in detail below with reference to the accompanying drawings. Examples of these preferred embodiments are illustrated in the accompanying drawings. The embodiments of the invention shown in the drawings and described in accordance with the drawings are exemplary only, and the invention is not limited to these embodiments.
It should be noted that, in order to avoid obscuring the present invention with unnecessary details, only the structures and/or processing steps closely related to the scheme according to the present invention are shown in the drawings, and other details not so relevant to the present invention are omitted.
The embodiment of the invention provides a current collector, and referring to fig. 1 to 4, the current collector comprises a copper sheet body 1 and a PI (polyimide) film layer 2 formed on the copper sheet body 1. The PI film layer 2 is divided into a plurality of PI units 21 spaced from each other by laser scanning irradiation, and laser-induced graphene 22 is formed on the peripheral side wall of each PI unit 21.
Referring to fig. 5, the method for preparing the current collector includes the steps of:
s10, providing a copper sheet body and preparing and forming a PI film layer on the copper sheet body.
The copper sheet body is preferably a copper foil, and the thickness of the copper sheet body can be set to be 10-20 micrometers. The PI film layer can be formed by selecting a commercially available PI adhesive tape and adhering the commercially available PI adhesive tape to the copper sheet body, and the thickness of the PI film layer is preferably 50-70 μm.
S20, carrying out laser scanning irradiation on the PI film layer, dividing the PI film layer into a plurality of PI units which are spaced from each other, and forming laser-induced graphene on the peripheral side wall of each PI unit.
At the position heated by laser irradiation, the PI film layer is divided into a plurality of PI units which are spaced from each other, and the PI film is heated and induced to form laser-induced graphene, so that the PI units which are formed by surrounding PI materials by the laser-induced graphene and have a 3D structure are obtained on the copper sheet body.
Specifically, the process conditions for performing laser scanning irradiation are as follows: the laser power density is 60W/cm2～95W/cm2The scanning speed is 2 cm/s-4 cm/s, and the scanning interval is 400 mu m-800 mu m.
In a preferred embodiment, the PI film layer is respectively irradiated by laser scanning along a first direction and a second direction perpendicular to each other (e.g., an X direction and a Y direction in a coordinate system), so that a plurality of PI units spaced from each other are arranged on the copper sheet body in a matrix array, as shown in the arrangement structure shown in fig. 1.
And the laser scanning irradiation is carried out on the PI film layer along the first direction and/or the second direction for 3-8 times.
According to the current collector and the preparation method thereof, the copper sheet (copper foil) is used as the body, the PI film layer is divided into a plurality of PI units which are spaced from each other through laser scanning irradiation, and Laser Induced Graphene (LIG) is formed around each PI unit, so that the prepared current collector is applied to secondary batteries such as lithium batteries, and the secondary batteries can have higher and more stable coulombic efficiency and longer cycle life. Specifically, because the LIG is surrounded around the PI unit, the LIG has high defect, multi-doping property and high porous structural characteristic, so that rapid lithium nucleation dynamics are generated in the electrodeposition process, the nucleation overpotential of the Li in the LIG is obviously lower than that on a bare copper foil, the cohesive force of a current collector and a negative active material (metal lithium) is improved, the negative active material is prevented from falling off from the current collector, and meanwhile, the 3D structure of the LIG reduces the current density, so that the battery has higher and more stable coulomb efficiency and longer cycle life.
Example 1
Firstly, a commercial copper foil with the thickness of 12 μm is taken, and a layer of polyimide adhesive tape is adhered on the copper foil, wherein the thickness of the polyimide adhesive tape is 50 μm.
And secondly, performing laser scanning irradiation on the polyimide adhesive tape to obtain a current collector sample A1.
Wherein, the parameters of laser scanning are as follows: the laser power density is 86W/cm2The scanning speed is 3cm/s, and the scanning distance is 400 mu m; scanning was performed 4 times in the X direction and Y direction, respectively.
In this embodiment, the laser used was 532nm wavelength laser, the maximum power laser beam was 3W, and the spot radius was about 200 μm.
Wherein, fig. 1, fig. 3 and fig. 4 are SEM images of the current collector sample prepared in the present example.
Example 2
Firstly, a commercial copper foil with the thickness of 10 μm is taken, and a layer of polyimide adhesive tape is adhered on the copper foil, wherein the thickness of the polyimide adhesive tape is 60 μm.
And secondly, performing laser scanning irradiation on the polyimide adhesive tape to obtain a current collector A2.
Wherein, the parameters of laser scanning are as follows: the laser power density is 95W/cm2The scanning speed is 2cm/s, and the scanning distance is 600 mu m; scanning 5 in the X-and Y-directions, respectivelyNext, the process is carried out.
Example 3
Firstly, a commercial copper foil with the thickness of 20 μm is taken, and a layer of polyimide adhesive tape is adhered on the copper foil, wherein the thickness of the polyimide adhesive tape is 70 μm.
And secondly, performing laser scanning irradiation on the polyimide adhesive tape to obtain a current collector A3.
Wherein, the parameters of laser scanning are as follows: the laser power density is 70W/cm2The scanning speed is 4cm/s, and the scanning distance is 800 μm; the X and Y directions were scanned 6 times, respectively.
Example 4
In this embodiment, the current collector samples a1 to A3 prepared in the above embodiments 1 to 3 are respectively assembled into a lithium battery, and then the lithium battery is subjected to an electrochemical test, specifically as follows:
the specific battery structure can adopt a CR2032 button cell, the current collector samples A1-A3 are respectively used as a negative electrode, an electrode which is the same as the negative electrode is used as a positive electrode, a polypropylene material is used as a diaphragm, 1mol/L1M bis (trifluoromethane) sulfimide Lithium (LiTFSI) is dissolved in 1, 3-dioxolane/1, 2-dimethoxyethane (DOL/DME), and LiNO containing 1 percent3The mixed solution of the additives is used as electrolyte and assembled into button cell samples B1-B3 in a glove box. In addition, by way of comparison, a button cell sample B4 was assembled with reference to the same process above, using commercially pure copper foil as the current collector.
It should be noted that, after the current collector is assembled into a battery, discharging is performed first, so that Li is deposited on the current collector, and the current collector after lithium metal deposition is formed into a negative electrode.
The assembled battery samples B1 to B4 were subjected to comparative tests to obtain the following performance parameter table (table 1), in which the coulombic efficiency of lithium intercalation/deintercalation at room temperature was measured using a Land (blue) battery test system. It should be noted that the number of each battery sample can be assembled according to actual needs, for example, the number of the battery samples B1 and B4 is three respectively, so as to perform the test under different parameter conditions respectively.
TABLE 1
As can be understood from table 1, the lithium secondary battery using the current collector provided by the embodiment of the present invention has higher and more stable coulombic efficiency and longer cycle life than the lithium secondary battery directly using a commercial copper foil as a current collector.
FIG. 6 shows cell sample B1 (LIGHT) at 1mA/cm versus comparative cell sample B4(Bare cu)2Coulombic efficiency at current density of (a). The lithium secondary battery using the current collector provided by the embodiment of the invention has the capacity of generating electricity at 1mAh/cm-2After discharging is performed for 200 times under the current density, the coulombic efficiency can still be kept above 99%, and the coulombic efficiency is stable in the circulating process; and lithium secondary battery using commercial copper foil as current collector at 1mAh/cm-2After 50 discharge cycles at the current density of (a), the coulomb efficiency is reduced to below 90%.
FIG. 7 shows cell sample B1 (LIGHT) at 2mA/cm versus comparative cell sample B4(Bare cu)2Coulombic efficiency at current density of (a). The lithium secondary battery using the current collector provided by the embodiment of the invention has the capacity of generating 2mAh/cm-2The current density of the current can be stably circulated for more than 120 times, and the coulomb efficiency in the circulation process is stable; and lithium secondary battery using commercial copper foil as current collector at 2mAh/cm-2After 80 cycles at current density, the cell failed.
FIG. 8 shows cell sample B1 (LIGHT) at 5mA/cm versus comparative cell sample B4(Bare cu)2Coulombic efficiency at current density of (a). The lithium secondary battery using the current collector provided by the embodiment of the invention has the capacity of 5mAh/cm-2The current density of the current can be stably circulated for more than 100 times, and the coulomb efficiency in the circulation process is stable; and the lithium secondary battery directly using commercial copper foil as the current collector is at 5mAh/cm-2After 40 cycles at current density, the cell failed.
As can be seen from table 1 and fig. 6 to 8, the current collector provided in the embodiments of the present invention is applied to a secondary battery such as a lithium battery, so that the secondary battery has higher and more stable coulombic efficiency and longer cycle life.
The foregoing is directed to embodiments of the present application and it is noted that numerous modifications and adaptations may be made by those skilled in the art without departing from the principles of the present application and are intended to be within the scope of the present application.
Claims (10)
1. A current collector comprises a copper sheet body and a PI film layer formed on the copper sheet body, and is characterized in that the PI film layer is divided into a plurality of PI units which are spaced from each other through laser scanning irradiation, and laser-induced graphene is formed on the peripheral side wall of each PI unit.
2. The current collector of claim 1, wherein the plurality of spaced PI cells are arranged in a matrix array on the copper sheet body.
3. The current collector of claim 1, wherein the copper sheet body is a copper foil having a thickness of 10 μ ι η to 20 μ ι η.
4. The current collector of claim 1, wherein the thickness of the PI film layer is 50 μ ι η to 70 μ ι η.
5. A method for preparing the current collector of any one of claims 1 to 4, comprising:
providing a copper sheet body and preparing and forming a PI film layer on the copper sheet body;
and carrying out laser scanning irradiation on the PI film layer, dividing the PI film layer into a plurality of PI units which are spaced from each other, and forming laser-induced graphene on the peripheral side wall of each PI unit.
6. The preparation method of the current collector according to claim 5, wherein the process conditions for performing laser scanning irradiation are as follows: the laser power density is 60W/cm2～95W/cm2The scanning speed is 2 cm/s-4 cm/s, and the scanning interval is 400 mu m-800 mu m.
7. The preparation method of the current collector, according to claim 6, wherein the PI film layer is subjected to laser scanning irradiation along a first direction and a second direction perpendicular to each other, so that the formed PI units spaced from each other are arranged on the copper sheet body in a matrix array.
8. The preparation method of the current collector, according to claim 7, wherein the number of laser scanning irradiation to the PI film layer along the first direction and/or the second direction is 3-8.
9. A negative electrode comprising the current collector of any one of claims 1-4.
10. A secondary battery comprising the negative electrode according to claim 9.
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| CN201910915966.0A CN110620238A (en) | 2019-09-24 | 2019-09-24 | Current collector and preparation method thereof, negative electrode and secondary battery |
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| CN201910915966.0A CN110620238A (en) | 2019-09-24 | 2019-09-24 | Current collector and preparation method thereof, negative electrode and secondary battery |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111556597A (en) * | 2020-05-27 | 2020-08-18 | 安徽宇航派蒙健康科技股份有限公司 | Method for preparing graphene heating film for battery on surface of polyimide insulating substrate |
| CN114220938A (en) * | 2021-11-17 | 2022-03-22 | 喆烯新材(北京)科技有限公司 | Preparation method and preparation equipment of high-adhesion graphene roughened current collector |
| CN114243024A (en) * | 2021-11-17 | 2022-03-25 | 喆烯新材(北京)科技有限公司 | Preparation method and preparation equipment of graphene roughened current collector |
| CN115763823A (en) * | 2022-11-10 | 2023-03-07 | 广东工业大学 | Preparation method and application of laser-induced manganese oxide/graphene array |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111556597A (en) * | 2020-05-27 | 2020-08-18 | 安徽宇航派蒙健康科技股份有限公司 | Method for preparing graphene heating film for battery on surface of polyimide insulating substrate |
| CN114220938A (en) * | 2021-11-17 | 2022-03-22 | 喆烯新材(北京)科技有限公司 | Preparation method and preparation equipment of high-adhesion graphene roughened current collector |
| CN114243024A (en) * | 2021-11-17 | 2022-03-25 | 喆烯新材(北京)科技有限公司 | Preparation method and preparation equipment of graphene roughened current collector |
| CN114220938B (en) * | 2021-11-17 | 2023-09-05 | 荣烯新材(北京)科技有限公司 | Preparation method and preparation equipment of high-adhesion graphene roughened current collector |
| CN114243024B (en) * | 2021-11-17 | 2023-09-05 | 荣烯新材(北京)科技有限公司 | Preparation method and preparation equipment of graphene roughened current collector |
| CN115763823A (en) * | 2022-11-10 | 2023-03-07 | 广东工业大学 | Preparation method and application of laser-induced manganese oxide/graphene array |
| CN115763823B (en) * | 2022-11-10 | 2023-08-04 | 广东工业大学 | Preparation method and application of laser-induced manganese oxide/graphene array |
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