CN110970598A - Composite negative electrode of lithium battery, preparation method thereof and lithium battery comprising negative electrode - Google Patents
Composite negative electrode of lithium battery, preparation method thereof and lithium battery comprising negative electrode Download PDFInfo
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- CN110970598A CN110970598A CN201911340636.XA CN201911340636A CN110970598A CN 110970598 A CN110970598 A CN 110970598A CN 201911340636 A CN201911340636 A CN 201911340636A CN 110970598 A CN110970598 A CN 110970598A
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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
- H01M4/134—Electrodes based on metals, Si or alloys
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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
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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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
- H01M4/139—Processes of manufacture
- H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
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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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/381—Alkaline or alkaline earth metals elements
- H01M4/382—Lithium
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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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/628—Inhibitors, e.g. gassing inhibitors, corrosion inhibitors
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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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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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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Abstract
The invention provides a lithium battery composite negative electrode, a preparation method thereof and a lithium battery comprising the lithium battery composite negative electrode. The lithium battery composite negative electrode provided by the embodiment of the invention can avoid lithium dendrite, is safer in charge and discharge processes, and is beneficial to capacity exertion and circulation.
Description
Technical Field
The invention relates to a lithium battery, in particular to a lithium battery composite negative electrode capable of avoiding lithium dendrites and a preparation method thereof.
Background
The prior lithium-sulfur battery negative electrode prelithiation generally comprises coating a negative electrode material on a copper foil and embedding lithium by lithium powder, a lithium belt or an electrochemical method. Lithium is supplemented by lithium powder, so that the requirement on the operating environment is strict, and the lithium powder has greater potential safety hazard; in the contact chemical lithium intercalation or lithium foil composite negative electrode, the lithium absorbed by the negative plate is far less than the lithium provided by the metal lithium plate, so that the lithium intercalation is uneven, the deformation of the plate is caused, and the lithium metal is still exposed in the electrolyte and is in direct contact with the diaphragm, so that potential safety hazards exist.
Disclosure of Invention
One of the primary objects of the present invention is to provide a lithium battery composite negative electrode, comprising a current collector layer, a lithium layer and a carbon-based material layer, wherein the lithium layer is disposed on the current collector layer; the carbon-based material layer is arranged on one surface of the lithium layer far away from the current collector layer.
According to an embodiment of the invention, the current collector layer is a copper layer.
According to an embodiment of the invention, the material in the carbon-based material layer comprises one or more of graphite, hard carbon, silicon carbon.
According to an embodiment of the present invention, the material in the carbon-based material layer includes a conductive agent and a binder.
An embodiment of the present invention further provides a method for preparing a lithium battery composite negative electrode, including:
providing a lithium/current collector composite layer formed by compounding a lithium layer and a current collector layer;
coating the negative electrode slurry on the lithium surface of the lithium/current collector composite layer, and drying to obtain a composite negative electrode;
the anode paste includes a carbon-based material.
According to an embodiment of the present invention, the anode paste includes a conductive agent and a binder.
According to an embodiment of the present invention, the lithium/current collector composite layer is a copper-lithium composite tape.
According to an embodiment of the present invention, the copper-lithium composite tape includes a copper layer, and a lithium layer disposed on the copper layer, or two lithium layers disposed on opposite surfaces of the copper layer, respectively.
According to an embodiment of the invention, the carbon-based material is selected from one or more of graphite, hard carbon, silicon carbon.
The invention further provides a lithium battery, which comprises the lithium battery composite negative electrode.
The lithium battery composite negative electrode provided by the embodiment of the invention can avoid lithium dendrite, is safer in charge and discharge processes, and is beneficial to capacity exertion and circulation.
Drawings
Fig. 1 is a schematic structural view of a lithium battery composite negative electrode according to an embodiment of the present invention.
Detailed Description
Exemplary embodiments that embody features and advantages of the invention are described in detail below in the specification. It is to be understood that the invention is capable of other embodiments and that various changes in form and details may be made therein without departing from the scope of the invention and the description and drawings are to be regarded as illustrative in nature and not as restrictive.
As shown in fig. 1, an embodiment of the present invention provides a lithium battery composite negative electrode, including a current collector layer, a lithium layer and a carbon-based material layer, wherein the lithium layer is disposed on the current collector layer, the lithium layer includes a first surface and a second surface disposed opposite to the first surface, the lithium layer is disposed on the current collector layer through the first surface, the carbon-based material layer is disposed on the second surface of the lithium layer far from the current collector layer, and the current collector layer may be a copper layer.
According to the composite negative electrode of the lithium battery, the carbon-based material layer is formed on the surface of lithium, and the carbon-based material layer can be used as a protective layer of lithium metal and is a site for lithium ion insertion and extraction. Meanwhile, because the reaction sites are transferred to the carbon-based negative electrode from the metallic lithium, the growth of lithium dendrite caused by the uneven deposition of the metallic lithium in the charging and discharging process is also avoided.
According to the composite negative electrode of the lithium battery, disclosed by the embodiment of the invention, a part of lithium ions can be stored in the negative electrode in advance, so that the lithium ions consumed by forming or repairing an SEI (solid electrolyte interphase) film in the first charge-discharge or circulation process are compensated.
The lithium battery composite negative electrode provided by the embodiment of the invention can be used for a sulfur lithium battery to avoid the reaction of lithium polysulfide and metal lithium, so that the process is safer, and the cycle and rate performance can be improved.
In one embodiment, the carbon-based material layer includes one or more of graphite, hard carbon, and silicon carbon.
In one embodiment, the thickness of the lithium layer is 10 to 50 μm, such as 15 μm, 20 μm, 25 μm, 30 μm, 40 μm, 45 μm, and the like.
An embodiment of the present invention provides a method for preparing a lithium battery composite negative electrode, including: providing a lithium/current collector composite layer; coating the cathode slurry on the surface of the lithium layer, and drying to obtain the composite cathode; wherein the negative electrode slurry includes a carbon-based material, and the lithium/current collector composite layer is formed by compositing lithium and a current collector.
In one embodiment, the lithium/current collector composite layer is a copper-lithium composite tape.
In one embodiment, the copper-lithium composite strip may be formed by rolling or electrodepositing metallic lithium on the surface of a copper current collector.
In one embodiment, the copper-lithium composite tape includes a copper layer and a lithium layer disposed on a surface of the copper layer.
In one embodiment, the copper-lithium composite tape includes a copper layer and two lithium layers disposed on opposite surfaces of the copper layer, respectively.
In one embodiment, the anode paste may include a carbon-based material, a conductive agent, and a binder.
In one embodiment, the negative electrode slurry includes 90 to 95 wt% of a carbon-based material, 2 to 4 wt% of a conductive agent, and 3 to 6 wt% of a binder.
In one embodiment, the carbon-based material may be graphite, hard carbon, silicon carbon; the conductive agent may be Super P (SP); the binder may be polyvinylidene fluoride (PVDF) (oily system).
In one embodiment, the carbon-based material, the conductive agent and the binder are mixed in proportion to prepare a slurry, the slurry is uniformly coated on one or two surfaces of the copper-lithium composite tape in an inert protective atmosphere after being dispersed, and then the copper-lithium composite tape is dried in a vacuum oven to prepare the composite negative electrode.
The invention provides a lithium battery, which comprises the lithium battery composite negative electrode.
An embodiment of the present invention provides a method for preparing a lithium battery, including preparing a negative electrode according to the above method.
In one embodiment, the positive electrode for the lithium battery may be manufactured by uniformly coating the positive electrode slurry on both sides of the aluminum current collector, followed by drying in a vacuum oven.
In one embodiment, the positive electrode slurry includes a sulfur positive electrode material, a conductive agent, and a binder; the sulfur anode material can be a sulfur-carbon composite material, such as a composite of sulfur and polypyrrole, polyacrylonitrile, and the like; the conductive agent may be SP, SP/CNT (carbon nanotube), etc.; the binder may be polyvinylidene fluoride PVDF (organic systems) and CMC plus SBR or LA133 etc. (aqueous systems).
In one embodiment, the positive electrode slurry includes 88 to 95 wt% of a sulfur positive electrode material, 2 to 5 wt% of a conductive agent, and 3 to 10 wt% of a binder.
In one embodiment, a lithium composite negative electrode sheet and a sulfur positive electrode are cut into a certain size, the single-sheet soft package battery is assembled through the procedures of lamination, ultrasonic welding, liquid injection, sealing and the like, a single-side polyethylene PE base film is adopted to be coated with a 2-micron sulfur-cut lithium-conductive coating to serve as a diaphragm, 1.0 mol/L1, 3-Dioxolane (DOL) solution of bis (trifluoromethyl) sulfimide Lithium (LiTFSI) and ethylene glycol dimethyl ether (DME) are mixed according to the volume ratio of 1:1, and 4 wt% of lithium nitrate LiNO is added3The mass ratio of liquid sulfur as the electrolyte (mass ratio of the electrolyte to sulfur) is 3:1 to 20: 1.
In one embodiment, the liquid sulfur mass ratio may be 5:1, 8:1, 10:1, 15:1, 18:1, and the like.
According to the lithium battery composite negative electrode provided by the embodiment of the invention, the lithium source is provided by the metal lithium, the metal lithium is not in direct contact with the diaphragm, and the electrolyte is not in direct contact with the lithium due to the addition of the carbon-based negative electrode on the surface, so that the loss of the metal lithium and the electrolyte is avoided.
Hereinafter, a lithium battery according to an embodiment of the present invention will be further described with reference to specific examples. Wherein, the raw materials are all obtained from the market.
Example 1
The sulfur-polypyrrole compound is used as a positive electrode material, is mixed with a conductive agent SP and a binder LA133 according to a mass ratio of 95:2:3, is mixed into slurry by taking deionized water as a solvent, is uniformly coated on an Al current collector, and the S loading capacity is 4mg/cm2Then drying the anode plate in a vacuum oven at 60 ℃ for 24 hours to obtain an anode plate;
taking hard carbon as a negative electrode material, mixing the hard carbon with a conductive agent SP and polyvinylidene fluoride (PVDF) according to a mass ratio of 95:2:3, taking N-methyl pyrrolidone (NMP) as a solvent, mixing the mixture into slurry, uniformly coating the slurry on the lithium surface of a copper/lithium composite belt in an inert protective atmosphere, and uniformly coating the slurry on the lithium surface of the copper/lithium composite belt with a single-side surface density of 14.4mg/cm2Then drying the anode plate in a vacuum oven at 80 ℃ for 24 hours to obtain a hard carbon-lithium-copper composite anode plate;
the hard carbon-lithium-copper composite negative plate and the positive plate are assembled into a single-piece soft package battery, a 2-micron sulfur-cut lithium-conductive coating is coated on one side of a polyethylene PE base film to serve as a diaphragm, and the volume ratio of 1.0mol/L lithium bistrifluoromethylsulfonyl imide (LiTFSI)/1, 3-Dioxolane (DOL) + ethylene glycol dimethyl ether (DME) is 1: 1/4 wt% lithium nitrate LiNO is added3Constant current charge and discharge tests are carried out on the electrolyte, the multiplying power is 0.5C, the cut-off voltage is 1.75-2.5V, the charge and discharge capacity of the previous 30 charge and discharge cycles is recorded, and related results are shown in table 1.
Example 2
The sulfur-polypyrrole compound is used as a positive electrode material, is mixed with a conductive agent SP and a binder LA133 according to a mass ratio of 95:2:3, is mixed into slurry by taking deionized water as a solvent, is uniformly coated on an Al current collector, and the S loading capacity is 4mg/cm2Then drying the anode plate in a vacuum oven at 60 ℃ for 24 hours to obtain an anode plate;
silicon carbon is used as a negative electrode material, is mixed with a conductive agent SP and a binder PVDF according to the mass ratio of 91:3:6, is mixed with NMP as a solvent to form slurry, and is uniformly coated on the lithium surface of a copper/lithium composite belt under the inert protective atmosphere, wherein the single-side surface density is 9.6mg/cm2Then drying the silicon carbide-lithium-copper composite negative plate in a vacuum oven at 80 ℃ for 24 hours to obtain a silicon carbide-lithium-copper composite negative plate;
the silicon carbon-lithium-copper composite negative plate and the positive plate are assembled into a single soft sheetThe battery pack is characterized in that a 2-micron sulfur-cut lithium-conductive coating is coated on one side of a polyethylene PE base film to serve as a diaphragm, the volume ratio of 1.0mol/L lithium bistrifluoromethylsulfonyl imide (LiTFSI)/1, 3-Dioxolane (DOL) + ethylene glycol dimethyl ether (DME) is 1: 1/4 wt% lithium nitrate LiNO is added3Constant current charge and discharge tests are carried out on the electrolyte, the multiplying power is 0.5C, the cut-off voltage is 1.75-2.5V, the charge and discharge capacity of the previous 30 charge and discharge cycles is recorded, and related results are shown in table 1.
Comparative example 1
The raw materials, process flow and the like used in the example are basically the same as those of the example 1, and the differences are that: the hard carbon-lithium of the composite negative electrode sheet in example 1 is replaced by metallic lithium, i.e., a lithium-copper composite negative electrode sheet is obtained, and the relevant charge and discharge test data of the obtained product are shown in table 1.
Comparative example 2
The raw materials, process flow and the like used in the example are basically the same as those in the example 2, and the differences are that: the silicon carbon-lithium of the composite negative electrode sheet in example 2 is replaced by metal lithium, that is, a lithium-copper composite negative electrode sheet is obtained, and the relevant charge and discharge test data of the obtained product is shown in table 1.
Comparative example 3
The raw materials, process flow and the like used in the example are basically the same as those of the example 1, and the differences are that: firstly, a hard carbon layer is formed on the surface of a copper current collector, then a lithium layer is formed on the surface of the hard carbon layer, so that the lithium-silicon carbon-copper composite negative plate is obtained, and the relevant charge and discharge test data of the obtained product is shown in table 1.
TABLE 1
Unless otherwise defined, all terms used herein have the meanings commonly understood by those skilled in the art.
The described embodiments of the present invention are for illustrative purposes only and are not intended to limit the scope of the present invention, and those skilled in the art may make various other substitutions, alterations, and modifications within the scope of the present invention, and thus, the present invention is not limited to the above-described embodiments but only by the claims.
Claims (10)
1. A lithium battery composite anode, comprising:
a current collector layer;
a lithium layer disposed on the current collector layer; and
and the carbon-based material layer is arranged on one surface of the lithium layer far away from the current collector layer.
2. The lithium battery composite negative electrode as claimed in claim 1, wherein the current collector layer is a copper layer.
3. The lithium battery composite anode of claim 1, wherein the material in the carbon-based material layer comprises one or more of graphite, hard carbon, silicon carbon.
4. The lithium battery composite anode of claim 1, wherein the material in the carbon-based material layer comprises a conductive agent and a binder.
5. A preparation method of a composite negative electrode of a lithium battery comprises the following steps:
providing a lithium/current collector composite layer formed by compounding a lithium layer and a current collector layer;
coating the negative electrode slurry on the lithium surface of the lithium/current collector composite layer, and drying to obtain a composite negative electrode;
the anode paste includes a carbon-based material.
6. The method of claim 5, wherein the negative electrode slurry comprises a conductive agent and a binder.
7. The method of claim 5, wherein the lithium/current collector composite layer is a copper-lithium composite tape.
8. The method of claim 7, wherein the copper-lithium composite tape comprises a copper layer, and one lithium layer disposed on the copper layer, or two lithium layers disposed on opposite surfaces of the copper layer, respectively.
9. The method of claim 5, wherein the carbon-based material is selected from one or more of graphite, hard carbon, silicon carbon.
10. A lithium battery comprising the lithium battery composite negative electrode as recited in any one of claims 1 to 4, or the lithium battery composite negative electrode manufactured by the method as recited in any one of claims 5 to 9.
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| CN201911340636.XA CN110970598A (en) | 2019-12-23 | 2019-12-23 | Composite negative electrode of lithium battery, preparation method thereof and lithium battery comprising negative electrode |
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| CN201911340636.XA CN110970598A (en) | 2019-12-23 | 2019-12-23 | Composite negative electrode of lithium battery, preparation method thereof and lithium battery comprising negative electrode |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111490250A (en) * | 2020-04-26 | 2020-08-04 | 上海汽车集团股份有限公司 | Lithium metal negative electrode, preparation method thereof and lithium metal battery |
| CN111916681A (en) * | 2020-06-23 | 2020-11-10 | 成都新柯力化工科技有限公司 | Method for simply producing silicon-carbon negative electrode plate of power lithium battery by spherical graphite |
| CN114583110A (en) * | 2020-02-28 | 2022-06-03 | 苏州清陶新能源科技有限公司 | Negative pole piece, preparation method thereof and application of negative pole piece in solid-state battery |
| CN114975881A (en) * | 2022-05-31 | 2022-08-30 | 合肥工业大学 | Preparation method of lithium-sulfur battery positive electrode and method for assembling soft package battery by using same |
-
2019
- 2019-12-23 CN CN201911340636.XA patent/CN110970598A/en not_active Withdrawn
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114583110A (en) * | 2020-02-28 | 2022-06-03 | 苏州清陶新能源科技有限公司 | Negative pole piece, preparation method thereof and application of negative pole piece in solid-state battery |
| CN114583110B (en) * | 2020-02-28 | 2023-07-25 | 苏州清陶新能源科技有限公司 | Negative electrode plate, preparation method thereof and application thereof in solid-state battery |
| CN111490250A (en) * | 2020-04-26 | 2020-08-04 | 上海汽车集团股份有限公司 | Lithium metal negative electrode, preparation method thereof and lithium metal battery |
| CN111916681A (en) * | 2020-06-23 | 2020-11-10 | 成都新柯力化工科技有限公司 | Method for simply producing silicon-carbon negative electrode plate of power lithium battery by spherical graphite |
| CN111916681B (en) * | 2020-06-23 | 2021-07-20 | 成都新柯力化工科技有限公司 | Method for simply producing silicon-carbon negative electrode plate of power lithium battery by spherical graphite |
| CN114975881A (en) * | 2022-05-31 | 2022-08-30 | 合肥工业大学 | Preparation method of lithium-sulfur battery positive electrode and method for assembling soft package battery by using same |
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Address after: 166 Kejiao Road, Jintan District, Changzhou City, Jiangsu Province Applicant after: Kaibo Energy Technology Co.,Ltd. Address before: No.1 Jiangdong Avenue, Jintan District, Changzhou City, Jiangsu Province Applicant before: CHINA AVIATION LITHIUM BATTERY RESEARCH INSTITUTE Co.,Ltd. Address after: 166 Kejiao Road, Jintan District, Changzhou City, Jiangsu Province Applicant after: AVIC Innovation Technology Research Institute (Jiangsu) Co.,Ltd. Address before: 166 Kejiao Road, Jintan District, Changzhou City, Jiangsu Province Applicant before: Kaibo Energy Technology Co.,Ltd. |
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Application publication date: 20200407 |