CN116799326A - Lithium ion battery and preparation method thereof - Google Patents

Lithium ion battery and preparation method thereof Download PDF

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Publication number
CN116799326A
CN116799326A CN202310882857.XA CN202310882857A CN116799326A CN 116799326 A CN116799326 A CN 116799326A CN 202310882857 A CN202310882857 A CN 202310882857A CN 116799326 A CN116799326 A CN 116799326A
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CN
China
Prior art keywords
anode
lithium ion
ion battery
graphite
anode material
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Pending
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CN202310882857.XA
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Chinese (zh)
Inventor
彭成龙
朱伯礼
高云雷
于子龙
陈杰
郑明清
项海标
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Zhejiang Liwei Energy Technology Co ltd
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Zhejiang Liwei Energy Technology Co ltd
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Priority to CN202310882857.XA priority Critical patent/CN116799326A/en
Publication of CN116799326A publication Critical patent/CN116799326A/en
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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
    • H01M10/058—Construction or manufacture
    • H01M10/0587—Construction or manufacture of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
    • 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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • 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
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/61—Types of temperature control
    • H01M10/613—Cooling or keeping cold
    • 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
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/653—Means for temperature control structurally associated with the cells characterised by electrically insulating or thermally conductive materials
    • 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
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/654—Means for temperature control structurally associated with the cells located inside the innermost case of the cells, e.g. mandrels, electrodes or electrolytes
    • 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
    • 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
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • H01M4/139—Processes of manufacture
    • 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
    • H01M4/139—Processes of manufacture
    • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes

Abstract

The invention discloses a lithium ion battery and a preparation method thereof, wherein the lithium ion battery comprises a battery core formed by winding a cathode pole piece, an anode pole piece and an isolating film arranged between the cathode pole piece and the anode pole piece, the anode pole piece is coated with anode materials formed by a plurality of layers of hexahedral structures at corners of the battery core, and six surfaces of the hexahedral structures are formed by anode materials A; the interior of the hexahedral structure is composed of an anode material B1; the anode material a comprises a graphite alkyne. According to the invention, by utilizing the heat conduction property of the graphite alkyne, the three-dimensional network structure formed by the graphite alkyne is arranged at the corner, so that the stability of the electrode and uniform heat dissipation are better kept, and the problem of corner lithium precipitation and the problem of corner temperature rise can be greatly improved. On the other hand, the graphite alkyne has excellent lithium storage performance, the theoretical capacity of the graphite alkyne is more than 2 times of that of graphite, the CB value at the corner can be greatly increased, and the risk of corner lithium precipitation is reduced.

Description

Lithium ion battery and preparation method thereof
Technical Field
The invention relates to the technical field of secondary batteries, in particular to a lithium ion battery and a preparation method thereof.
Background
With the high demands of consumer electronics and electric car markets, the production and application of soft-pack batteries are rapidly increasing, and the safety performance of batteries is also becoming more important. The problem of CB value mismatch caused by overlarge stress and anode pole piece cladding of the cathode pole piece exists at the corner of the winding type soft package battery, so that corner lithium precipitation is easy to cause, and the formed lithium crystal branch not only can cause the increase of the thickness of the battery core, but also can cause the safety risk of internal short circuit caused by diaphragm puncture. The problem of corner lithium separation is a common problem point in the industry and is also a difficult problem of high-rate charging of a winding structure, so that the development of a high-energy high-rate winding type battery cell is greatly limited.
In the current art, there are mainly the following methods: 1. the method of increasing the CB value by increasing the overall coating weight of the anode sheet improves corner lithium precipitation, but is not suitable for practical application because the method greatly reduces the energy density of the battery cell and causes other performance degradation such as hot box. 2. Corner lithium precipitation is mitigated by corner rubberizing or ceramic coating to prevent lithium ions of the cathode from shuttling to the graphite anode, but this reduces the energy density of the system. 3. Lithium evolution from the anode is avoided by removing active material at the cathode corners, but this greatly reduces the capacity of the cell.
Therefore, there is a need to develop new lithium ion batteries to solve the problem of lithium precipitation at the anode corners.
Disclosure of Invention
The present invention aims to solve at least one of the technical problems existing in the prior art. Therefore, the first aspect of the invention provides a lithium ion battery, which can effectively prevent lithium from being separated from an anode plate.
The second aspect of the invention also provides a preparation method of the lithium ion battery.
According to the lithium ion battery provided by the embodiment of the first aspect of the invention, the lithium ion battery comprises a battery core formed by winding a cathode pole piece, an anode pole piece and a separation film arranged between the cathode pole piece and the anode pole piece, wherein anode materials formed by a plurality of layers of hexahedral structures are coated on corners of the battery core, and six surfaces of the hexahedral structures are formed by anode materials A; the interior of the hexahedral structure is composed of an anode material B1; the anode material a comprises a graphite alkyne.
The lithium ion battery provided by the embodiment of the invention has at least the following beneficial effects:
the invention coats anode materials formed by a plurality of layers of hexahedral structures at the corners of the battery core, and six surfaces of the hexahedral structures are formed by anode materials A; the interior of the hexahedral structure is composed of an anode material B1; the anode material a comprises a graphite alkyne. According to the invention, by utilizing the heat conduction property of the graphite alkyne, the three-dimensional network structure formed by the graphite alkyne is arranged at the corner, so that the stability of the electrode and uniform heat dissipation are better kept, and the problem of corner lithium precipitation and the problem of corner temperature rise can be greatly improved. On the other hand, the graphite alkyne has excellent lithium storage performance, the theoretical capacity of the graphite alkyne is more than 2 times of that of graphite, the CB value at the corner can be greatly increased, and the risk of corner lithium precipitation is reduced.
According to some embodiments of the invention, the mass percentage of the anode material a is 1% -50% calculated on the total mass of the anode material a and the anode material B1.
According to some embodiments of the invention, the anode material B1 comprises at least one of natural graphite, artificial graphite, soft carbon, hard carbon, mesocarbon microbeads, tin-based oxide, tin-based composite oxide, silicon-carbon alloy, and lithium titanate.
According to some embodiments of the invention, each layer of the number of layers of hexahedral structures has a thickness not exceeding 1/6 of the thickness of the anode electrode sheet.
According to some embodiments of the invention, the anode sheet has a thickness of 30-200 μm.
According to some embodiments of the invention, the gram capacity of the anode material A is 600-800 mAh/g.
According to some embodiments of the invention, the gram capacity of the anode material B1 is 300 to 400mAh/g.
According to some embodiments of the invention, the graphite alkyne includes at least one of graphite monoalkyne, graphite diyne, or graphite tetrayne.
According to some embodiments of the invention, the hexahedral structure has 2 to 4 layers.
According to some embodiments of the invention, the cell is coated with anode material B2 at a large face.
According to some embodiments of the invention, the anode material B2 comprises at least one of natural graphite, artificial graphite, soft carbon, hard carbon, mesocarbon microbeads, tin-based oxide, tin-based composite oxide, silicon-carbon alloy, and lithium titanate.
According to some embodiments of the invention, the cathode sheet comprises a cathode current collector and a cathode material.
According to some embodiments of the invention, the cathode materials are each independently selected from LiCoO 2 、LiNiO 2 、LiMnO 2 、LiFePO 4 、Li x Ni y Co z MnO 2 At least one of (0)<x<1，0<y<1，0<z<1。
According to some embodiments of the present invention, the separator may be a conventional separator for lithium ion batteries, without limitation.
According to the preparation method of the lithium ion battery provided by the embodiment of the second aspect of the invention, the steps of coating, drying, cold pressing, welding the tab, packaging, liquid injection and the like are carried out after the tab and the isolating film are wound, and the coating of the anode tab in the preparation method is selected from the following modes:
the anode electrode plate comprises an anode electrode plate, a current collector and a cathode electrode plate, wherein the anode electrode plate is formed by a plurality of layers of hexahedral structures, and the six surfaces of the hexahedral structures are formed by anode materials A; the interior of the hexahedral structure is composed of an anode material B1; and coating anode material B2 on the area corresponding to the plane layer of the current collector of the anode plate.
Additional features and advantages of the invention will be set forth in the description which follows, and in part will be obvious from the description, or may be learned by practice of the invention.
Drawings
The foregoing and/or additional aspects and advantages of the invention will become apparent and may be better understood from the following description of embodiments taken in conjunction with the accompanying drawings in which:
FIG. 1 is a schematic view of the structure of an anode sheet of example 1 at the corners and large faces of a cell;
FIG. 2 is a diagram showing lithium separation interfaces of example 1, example 2, comparative example 1 and comparative example 2;
fig. 3 is a schematic view of the structure of the anode material coated at the corners of the cell for the anode electrode sheet of example 1.
Detailed Description
The following are specific embodiments of the present invention, and the technical solutions of the present invention will be further described with reference to the embodiments, but the present invention is not limited to these embodiments.
The reagents, methods and apparatus employed in the present invention, unless otherwise specified, are all conventional in the art.
Preparation example
Isolation film: the separator was a 5 μm PE-based film, and the surface was a PVDF oil-based separator coated with 1 μm.
Preparing a cathode plate: (1) 97.6% of lithium cobaltate, 0.5% of conductive agent, 0.6% of carbon black and 1.3% of binder PVDF and NMP solvent are uniformly mixed and stirred to form uniform slurry; (2) coating cathode slurry on aluminum foil; (3) the aluminum foil with the slurry is sent into a drying box to form a dry pole piece.
Preparing an anode plate: (1) first, preparing graphite slurry: uniformly stirring 97.7% of graphite, 2.02% of thickener and 2.21% of binder to form uniform slurry; (2) and preparing graphite alkyne slurry: uniformly stirring 95.1% of graphite alkyne, 2.2% of thickener and 2.7% of binder to form uniform slurry; (3) and coating graphite and graphite alkyne slurry on the surface of the copper foil current collector. The graphite slurry is coated on the large surface of the battery cell, and when the graphite slurry meets the corner region of the pole piece, the graphite slurry and the graphite alkyne slurry are sequentially sprayed according to the designed structure, so that a preset structure is formed. For example, forming a 3D network structure: and spraying the graphite alkyne slurry in sequence according to small areas to form a 3D network, wherein the interior of the 3D network is filled with the graphite slurry. (namely, spraying according to three layers of hexahedrons) (4) drying the prepared large anode pole piece in an oven.
Electrolyte solution: the electrolyte comprises an organic solvent, electrolyte salt, an anode and a cathode film forming additive; specifically, 20% EC+20% DEC+20% PC+40% PP+15% LiPF6+3% FEC+1% LiOFB;
preparation of the battery cell: and rolling, slitting, welding tabs, winding, packaging, baking, injecting liquid, forming, degassing and the like to prepare a battery finished product.
Example 1
Example 1 provides a lithium ion battery comprising a separator, a cathode sheet and an anode sheet, wherein the battery core is prepared according to the preparation method of the preparation example. A schematic structural view of the anode plate at the corners and large faces of the cell is shown in fig. 1.
FIG. 3 is a schematic view of an anode sheet, wherein the anode sheet is coated with anode material consisting of 3 layers of hexahedral structures at corners of a cell, six faces of the hexahedral structures being composed of anode material A graphite monoacetylene; the interior of the hexahedral structure is composed of an anode material B1; anode material B1 is composed of graphite, CMC, and SBR. Wherein the graphite monoacetylene content accounts for 3% of the sum of the mass of the anode material A and the anode material B1.
The anode pole piece is provided with an anode material B1 in the large area of the cell: consists of graphite, CMC and SBR.
The cathode material is the same in the areas of the corners and the large faces; are all LiCoO 2 +carbon black+pvdf+conductive agent carbon nanotubes CNT.
Example 2
Example 2 also provides a lithium ion battery having substantially the same composition, amount and preparation method as example 1, except that the graphite alkyne content accounts for 10% of the sum of the mass of the anode material a and the anode material B1.
Example 3
Example 3 also provides a lithium ion battery having substantially the same composition, amount and preparation method as example 1, except that the graphite alkyne content accounts for 30% of the sum of the mass of the anode material a and the anode material B1.
Example 4
Example 4 also provides a lithium ion battery having substantially the same composition, amount and preparation method as example 1, except that the graphite alkyne content accounts for 50% of the sum of the mass of the anode material a and the anode material B1.
Comparative example 1
Comparative example 1 also provides a lithium ion battery having substantially the same composition, amount and preparation method as in example 1, except that the anode electrode sheet does not contain an anode material a-graphite alkyne at the corner of the cell.
Comparative example 2
Comparative example 1 also provides a lithium ion battery having substantially the same composition, amount and preparation method as in example 1, except that the anode sheet was coated with an anode material at the corner of the cell, the anode material being a mixture of an anode material a graphite alkyne and an anode material B1, wherein the graphite alkyne content is 3%.
Comparative example 3
Comparative example 2 also provides a lithium ion battery having substantially the same composition, amount and preparation method as in example 1, except that the anode electrode sheet was coated with 2 layers of anode material at the corners of the cell, wherein the first layer was the anode material a-graphite alkyne; the second layer is an anode material B1, wherein the content of graphite alkyne accounts for 3 percent.
Performance testing
(1) Lithium precipitation phenomenon
The cell testing method comprises the following steps: the 3C stage charge mode charges to 4.50V and then discharges to 3.0V at 0.5C for 1000 weeks. The circulated battery cell is disassembled, and the lithium precipitation condition of the electrode plate interface is observed, and the result is shown in table 1.
Table 1 test results
Lithium-eluting interfaces of example 1, example 2, comparative example 1 and comparative example 2 are shown in fig. 2. From the analysis of comparative example 1 and examples 1 to 4, it is evident that the corner lithium precipitation is significantly improved by adding the hexahedral structure graphite alkyne material to the corner, and the more significant the lithium precipitation improvement effect thereof is as the graphite alkyne content increases. As is clear from comparative examples 2 to 3 and example 1, the graphite alkyne material exhibiting hexahedral structure distribution characteristics is more remarkable in improvement degree of corner lithium precipitation. This is because the structure is more advantageous for corner heat dissipation.
(2) Phenomenon of temperature rise
And the temperature of different areas is monitored by placing different temperature sensors in different areas of the surface of the test battery cell by adopting a multi-path thermometer to test the temperature, so that the temperature change of different areas of the battery cell is obtained. The results are shown in Table 2.
Table 2 cell temperature profile
From an analysis of comparative example 1 and examples 1-4, it can be seen that the addition of a graphite alkyne material at the corners facilitates a reduction in the corner temperature, thereby reducing the lithium precipitation potential and thus reducing the corner lithium precipitation. And as can be seen with examples 1-4, the corner temperature gradually decreases as the corner graphite alkyne content increases. As is clear from comparative examples 2 to 3 and example 1, when the graphite alkyne is in a disordered structure or a double-layer distribution, the corner temperature is higher than that of example 1, which indicates that when the graphite alkyne structure is distributed in a hexahedral structure, heat dissipation is more favored and the lithium precipitation degree is more slight.
The present invention has been described in detail with reference to the above embodiments, but the present invention is not limited to the above embodiments, and various changes can be made within the knowledge of those skilled in the art without departing from the spirit of the present invention.

Claims (10)

1. The lithium ion battery comprises a battery cell formed by winding a cathode pole piece, an anode pole piece and an isolating film arranged between the cathode pole piece and the anode pole piece, and is characterized in that the anode pole piece is coated with anode materials formed by a plurality of layers of hexahedral structures at corners of the battery cell, and six surfaces of the hexahedral structures are formed by anode materials A; the interior of the hexahedral structure is composed of an anode material B1; the anode material a comprises a graphite alkyne.
2. The lithium ion battery according to claim 1, wherein the mass percentage of the anode material a is 1% to 50% based on the total mass of the anode material a and the anode material B1.
3. The lithium ion battery of claim 1, wherein the anode material B1 comprises at least one of natural graphite, artificial graphite, soft carbon, hard carbon, mesocarbon microbeads, tin-based oxides, tin-based composite oxides, silicon-carbon alloys, and lithium titanate.
4. The lithium ion battery of claim 1, wherein each layer of the plurality of layers of hexahedral structures has a thickness of no more than 1/6 of a thickness of the anode electrode sheet.
5. The lithium ion battery of claim 1, wherein the gram capacity of the anode material a is 600-800 mAh/g.
6. The lithium ion battery according to claim 1, wherein the gram capacity of the anode material B1 is 300 to 400mAh/g.
7. The lithium ion battery of claim 1, wherein the graphite alkyne comprises at least one of graphite monoacetylene, graphite diacetylene, or graphite tetracetylene.
8. The lithium ion battery of claim 1, wherein the number of layers of the hexahedral structure is 2 to 4.
9. The lithium ion battery according to claim 1, characterized in that anode material B2 is coated at a large face of the cell.
10. The method for preparing a lithium ion battery according to any one of claims 1 to 9, wherein the coating of the anode sheet in the preparation method is selected from the following modes:
the anode electrode plate comprises an anode electrode plate, a current collector and a cathode electrode plate, wherein the anode electrode plate is formed by a plurality of layers of hexahedral structures, and the six surfaces of the hexahedral structures are formed by anode materials A; the interior of the hexahedral structure is composed of an anode material B1; and coating anode material B2 on the area corresponding to the plane layer of the current collector of the anode plate.
CN202310882857.XA 2023-07-18 2023-07-18 Lithium ion battery and preparation method thereof Pending CN116799326A (en)

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Application Number Priority Date Filing Date Title
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Publications (1)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN117577960A (en) * 2024-01-11 2024-02-20 江苏正力新能电池技术有限公司 Electrode assembly, battery and electric equipment

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN117577960A (en) * 2024-01-11 2024-02-20 江苏正力新能电池技术有限公司 Electrode assembly, battery and electric equipment
CN117577960B (en) * 2024-01-11 2024-04-09 江苏正力新能电池技术有限公司 Electrode assembly, battery and electric equipment

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