CN116364848A - Negative electrode sheet and secondary battery - Google Patents

Negative electrode sheet and secondary battery Download PDF

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Publication number
CN116364848A
CN116364848A CN202111617568.4A CN202111617568A CN116364848A CN 116364848 A CN116364848 A CN 116364848A CN 202111617568 A CN202111617568 A CN 202111617568A CN 116364848 A CN116364848 A CN 116364848A
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negative electrode
active material
electrode active
range
secondary battery
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CN202111617568.4A
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慈祥云
郝嵘
彭宇东
齐成紫
张笑莉
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BYD Co Ltd
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BYD Co Ltd
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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
    • 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
    • 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
    • H01M10/054—Accumulators with insertion or intercalation of metals other than lithium, e.g. with magnesium or aluminium
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • 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

Abstract

The application provides a negative electrode plate, including negative electrode current collector and set up the negative electrode active material layer on the surface of negative electrode current collector at least one side, contain negative electrode active material in the negative electrode active material layer, define following parameter k:
Figure DDA0003436996770000011
and k is in the range of 10.00-20.00; wherein Dv10, dv50, dv90 respectively represent particle diameter values corresponding to the cumulative volume distribution percentages of the anode active material reaching 10%, 50%, 90%, in μm; x represents the average aspect ratio of the particles of the anode active material. The cathode plate has proper tortuosity and can ensure the circulation of the battery made by the cathode plateThe ring performance and the safety performance are better, and the energy density is higher. The application also provides a secondary battery.

Description

Negative electrode sheet and secondary battery
Technical Field
The application relates to the technical field of batteries, in particular to a negative electrode plate and a secondary battery.
Background
The fast charge performance and life of the battery are related to the migration path of active ions in the anode active material layer, and the tortuosity of the anode active material layer can directly reflect the length of the migration path. If the tortuosity is too high, active ions can not be timely embedded into the negative electrode or directly reduced and separated out on the surface of the negative electrode, so that the safety performance and the cycle life of the battery are affected, and if the tortuosity is too low, the compaction density of the pole piece is small, the internal resistance of the battery is large, and the energy exertion is affected. Therefore, it is necessary to regulate the tortuosity of the negative electrode sheet to improve the quick charge performance and the service life of the battery.
Disclosure of Invention
In view of the above, the application provides a negative electrode plate and a secondary battery, so as to solve the problems of poor quick charge performance and short cycle life caused by over-high tortuosity of the current negative electrode plate.
In a first aspect, the present application provides a negative electrode tab comprising a negative electrode current collector and a negative electrode active material layer disposed on at least one side surface of the negative electrode current collector, defining the following parameter k:
Figure BDA0003436996750000011
and k is in the range of 10.00-20.00;
wherein Dv10, dv50, dv90 represent particle diameter values corresponding to the cumulative volume distribution percentages of the anode active material contained in the anode active material layer reaching 10%, 50%, 90%, respectively, in μm; x represents the average aspect ratio of particles of the anode active material.
In the negative electrode plate provided by the first aspect of the application, the negative electrode active material layer of the negative electrode plate is controlled to meet the defined parameter k within the range of 10.00-20.00, so that the tortuosity of the negative electrode plate is suitable, active ions can be smoothly embedded into/separated from the negative electrode active material layer, the migration path is shorter, the lithium precipitation phenomenon is difficult to occur on the surface of the negative electrode plate, the quick charge performance, the circulation performance and the safety performance of a battery containing the negative electrode plate are better, and meanwhile, the tortuosity of the negative electrode plate cannot be too low to cause too low compaction density of the electrode plate, large internal resistance of the battery, low energy density and the like.
In a second aspect, the present application provides a secondary battery comprising a negative electrode tab as described above. The secondary battery can maintain high capacity and has better cycle stability when cycled under high multiplying power.
Drawings
Fig. 1A is a schematic structural diagram of a negative electrode tab according to an embodiment of the present application.
Fig. 1B is a schematic structural diagram of a negative electrode tab according to an embodiment of the present application.
Detailed Description
Embodiments of the present application will be described below with reference to the accompanying drawings in the embodiments of the present application.
Referring to fig. 1A and fig. 1B together, the embodiment of the present application provides a negative electrode tab 10, where the negative electrode tab 10 includes a current collector 11 and a negative electrode active material layer 12 sequentially disposed on at least one side surface of the negative electrode current collector 11, and the negative electrode active material layer 12 contains a negative electrode active material, and the following parameter k is defined:
Figure BDA0003436996750000021
and k is in the range of 10.00-20.00;
wherein Dv10, dv50, dv90 represent particle diameter values corresponding to the cumulative volume distribution percentages of the anode active material contained in the anode active material layer 12 reaching 10%, 50%, 90%, respectively, in μm; x represents the average aspect ratio of particles of the anode active material.
By controlling the negative electrode active material layer 12 of the negative electrode sheet 10 to meet the defined parameter k within the range of 10.00-20.00, the tortuosity of the negative electrode sheet 10 can be suitable, active ions can be smoothly embedded into/separated from the negative electrode active material layer 12, the migration path is shorter, and the lithium precipitation phenomenon is not easy to occur on the surface of the negative electrode sheet 10, so that the battery containing the negative electrode sheet has better quick charge performance, cycle performance and safety performance, and meanwhile, the phenomena of larger internal resistance, lower energy density and the like of the battery caused by insufficient contact compaction among active material particles in the electrode sheet due to excessively low tortuosity of the negative electrode sheet are avoided.
The Dv10, dv50, dv90 may be obtained by performing a particle size distribution test on the negative electrode active material, and the specific test method may be referred to as GB/T19077-2016/ISO 13320:2009 particle size distribution laser diffraction method, and the test instrument may be a laser particle sizer (e.g., malvern 3000). Values of Dv10, dv50, dv90 were found from the obtained laser particle size distribution map of the negative electrode active material.
The above x can be obtained by averaging the ratio of the longest side to the shortest side of the plurality of particles on a scanning electron microscope (scanning electron microscope, SEM) photograph of the anode active material. x is dimensionless. Specifically, for SEM photographs of the anode active material (particles containing a certain number (generally more than 1000) of anode active materials), the longest side and the shortest side of each particle were measured using Image J software, the ratio of the longest side to the shortest side of each particle was calculated, and the ratio of the plurality of particles in the picture was averaged to obtain x. In some embodiments, the average aspect ratio x of the particles of the anode active material is in the range of 1 to 6.
In this application, the negative electrode current collector may have the negative electrode active material layer 12 on one side (as shown in fig. 1A), or may have the negative electrode active material layer 12 on both opposite side surfaces (as shown in fig. 1B, these two negative electrode active material layers may be respectively designated as 12, 12'). When the anode current collector has anode active material layers on both opposite side surfaces, the anode active material layer on any one surface may satisfy the parameter k within the range of 10.00 to 20.00, and of course, both anode active material layers may respectively have the parameter k within the range of 10.00 to 20.00.
In addition, the anode active material contained in the anode active material layer 12 may be one material or a plurality of materials. Specifically, the negative active material includes one or more of lithium titanate, a carbon material, a silicon-based material, a tin-based material, and the like, but is not limited thereto. Where the anode active material includes a plurality of materials (e.g., includes graphite and elemental silicon), dv10, dv50, dv90 refer to the relevant particle size values of the mixed anode active material, and x is also calculated from SEM photographs of the mixed anode active material.
The carbon material may be one or more of graphite, carbon fiber, soft carbon, hard carbon, mesophase carbon microsphere, graphene, etc., but is not limited thereto, and graphite is preferred. The silicon-based material may include elemental silicon, silicon alloys, silicon oxides, silicon-carbon composites, and the like. The tin-based material may include elemental tin, tin oxides, tin-based alloys, and the like. In some embodiments of the present application, the negative electrode active material includes a plurality of materials having different materials, and includes graphite, wherein the mass ratio of graphite in the negative electrode active material is 40-95%. This helps to improve the rate performance of the overall anode active material.
In embodiments of the present application, the Dv50 may be in the range of 7-18 μm. In some embodiments, dv50 may be in the range of 8-18 μm. Preferably, the Dv50 is in the range of 9-16 μm. The Dv50 of the particles can represent the distribution condition of the whole particles of the anode active material, the Dv50 can influence the lithium ion removal/intercalation speed, the circulation stability and the like in the circulation process, and the proper Dv50 can enable the battery prepared by the anode piece to have more excellent performance.
In embodiments of the present application, the Dv10 may be in the range of 2-15 μm. In some embodiments, dv10 may be in the range of 2-10 μm. Preferably, dv10 is in the range of 3-9 μm.
In embodiments of the present application, the Dv90 is in the range of 12-30 μm. In some embodiments, dv90 may be in the range of 18-30 μm. Preferably, dv90 is in the range of 18-28 μm.
Controlling Dv10, dv90 in the above-described range helps to ensure that the anode active material has an appropriate number of large and small particles, facilitates the formation of close packing between anode active material particles, and has an appropriate porosity. Among them, the above Dv 50/(Dv 90-Dv 10) reflects the concentration of the particle size distribution of the anode active material particles, and when this value is large, it means that the concentration of the particle size distribution of the anode active material particles is high.
In this application, the anode active material layer may include a binder in addition to the anode active material. In some cases, a conductive agent may also be included. Optionally, the mass of the anode active material is 80% -98%, preferably 90% -98% of the mass of the anode active material layer. This allows the negative electrode tab 10 to have a higher negative active material loading to increase the energy density of the battery. Among them, binders and conductive agents are conventional choices in the field of batteries. By way of example, the binder includes, but is not limited to, the binder may include one or more of styrene-butadiene rubber (SBR), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyvinyl alcohol (PVA), polyacrylonitrile (PAN), polyimide (PI), polyacrylic acid (PAA), polyacrylate (e.g., polymethyl methacrylate, polymethyl acrylate, polyethyl acrylate, etc.), polyolefin (e.g., polypropylene, polyethylene, etc.), carboxymethyl cellulose (CMC), sodium alginate, etc. Exemplary conductive agents include, but are not limited to, one or more of carbon nanotubes, graphene, carbon fibers, carbon black (e.g., acetylene black, ketjen black), and the like. In addition, the negative electrode current collector carrying the negative electrode active material layer may include, but is not limited to, copper foil, stainless steel foil, copper alloy foil, carbon-coated copper foil, copper-plated film, or the like.
The embodiment of the application also provides a secondary battery, which comprises the negative electrode plate.
The secondary battery also comprises a positive electrode plate, and a diaphragm and electrolyte which are arranged between the positive electrode plate and the negative electrode plate.
The secondary battery contains the negative electrode plate with proper tortuosity, so that the secondary battery can be ensured to have good cycle performance, high safety performance and higher energy density. Specifically, the secondary battery may be a lithium secondary battery, a sodium secondary battery, a potassium secondary battery, a magnesium secondary battery, an aluminum secondary battery, a zinc secondary battery, or the like.
The positive electrode sheet includes a positive electrode current collector and a positive electrode active material layer disposed on the positive electrode current collector, the positive electrode active material layer including a positive electrode active material, a binder, and optionally a conductive agent. The positive electrode active material may be selected according to the active ions on which the specific secondary battery depends for energy storage. The active ions may include lithium ion, sodium ion, potassium ion, magnesium ion, aluminum ion, zinc ion, and the like. Among them, for a lithium ion battery, the positive electrode active material thereof may include, but is not limited to, one or more of lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt aluminum oxide, and olivine structured lithium-containing phosphate. For sodium ion batteries, positive electrode active materials include, but are not limited to: transition metal oxide, polyanion compound, organic polymer, prussian blue material.
Among them, the separator may be various separator films suitable for secondary batteries in the art, and specifically may be a polymer separator, a non-woven fabric, etc., wherein the polymer separator includes, but is not limited to, a separator of single-layer PP (polypropylene), single-layer PE (polyethylene), double-layer PP/PE, double-layer PP/PP, and triple-layer PP/PE/PP, etc. The electrolyte comprises electrolyte salt and organic solvent, wherein the specific types and compositions of the electrolyte salt and the organic solvent are conventional choices in the field of batteries, and the electrolyte salt and the organic solvent can be selected according to actual requirements.
The technical solution of the present application will be further described with reference to a plurality of specific embodiments.
Example 1
A method of making a negative electrode sheet comprising:
the negative electrode active material (specifically, graphite, the particle size and the dimensional parameters of which are shown in table 1) and the conductive agent (specifically, ketjen black, the binder (CMC and PVDF, the mass ratio is 1:2) are mixed according to the mass ratio of 96:1:3, the mixed powder is placed in a vacuum mixer, deionized water is added for stirring to obtain negative electrode slurry, and the negative electrode slurry is uniformly coated on coated foils.
A method of manufacturing a lithium secondary battery, comprising:
1) Preparing a positive electrode plate:
lithium iron phosphate (LiFePO) as positive electrode active material 4 ) Conductive agent (specifically ketjen black), binder (specifically PVDF) according to 96:1.5:2.5, mixing the powder materials in a mass ratio, placing the mixed powder materials in a vacuum stirrer, adding solvent N-methyl pyrrolidone (NMP), and uniformly stirring to obtain anode slurry; and coating the positive electrode slurry on a positive electrode current collector aluminum foil, and drying, rolling and cutting to obtain the positive electrode plate.
2) Assembling a battery:
the negative electrode plate is taken as a negative electrode, the positive electrode plate is taken as a positive electrode, the diaphragm is taken as a polypropylene diaphragm, and the electrolyte adopts LiPF containing 1mol/L 6 1:1:1 mixed solution of Ethylene Carbonate (EC), ethylmethyl carbonate (EMC) and diethyl carbonate (DEC); the assembly was carried out in a glove box filled with argon, resulting in a laminated lithium battery with a rated capacity of 1.5 Ah.
The following electrochemical properties of the lithium secondary battery in example 1 were tested, and the results are summarized in table 2 below.
The testing method for the charging efficiency and the lithium precipitation condition of the negative electrode comprises the following steps: 1) At 25deg.C, the battery is charged to full state at 1/3C rate, then discharged at 1/3C rate, the above charge and discharge processes are repeated for 3 times, and the third charge capacity is recorded as C 0 The method comprises the steps of carrying out a first treatment on the surface of the 2) The battery is charged to a full state at 4C multiplying power, then is fully discharged at 1C multiplying power, the charging and discharging processes are repeated for 15 times, and the 15 th charging capacity is recorded as C 15 Calculate C 15 /C 0 As the charging efficiency. 3) And then charging the battery to a full state at 4C multiplying power, disassembling the battery, and checking the lithium precipitation condition of the negative electrode.
The method for testing the cycle performance comprises the following steps: at 25 ℃, the battery is charged to a full state at a 1C multiplying power, then is fully discharged at the 1C multiplying power, the charging and discharging processes are repeated, and the capacity retention rate after 1000 circles of circulation is recorded.
The impedance testing method comprises the following steps: 1) Charging the battery to full state at 1/3C ratio, discharging at 1/3C, repeating the charging and discharging process for 3 times, and recording the third charge capacity as C 0 The method comprises the steps of carrying out a first treatment on the surface of the And charging with 1/3C rate to adjust the charge state (state)of charge, SOC) to 50% SOC; 2) The test was carried out at-10℃for 12 hours and the direct current resistance (DCIR) charged at a rate of 1.5C for 30s was measured.
Other embodiments
The negative electrode tabs and batteries of the remaining examples were prepared according to the parameters listed in table 1, and the related properties were tested, and the test results are also summarized in table 2 below.
In addition, in order to highlight the beneficial effects of the technical scheme of the application, comparative examples 1-6 shown in the following table 1 are also provided, and the related results are summarized in table 2. When the cycle life of the battery was not 1000 cycles while testing the cycle performance of the battery, the test was stopped when the discharge capacity of the battery was reduced to 80% of the initial discharge capacity (i.e., the cycle life was reached), and the capacity retention rate at the time of reaching the cycle life was recorded.
Table 1 parameters of the negative electrode sheet composition of each example
Figure BDA0003436996750000071
Table 2 summary of electrochemical properties of cells made from the negative electrode tabs of each example
Figure BDA0003436996750000072
With reference to table 1, it can be known from table 2 that when the configuration of the negative electrode plate makes the custom parameter k within the range of 10.00-20.00, the safety performance of the battery containing the negative electrode plate is better, the negative electrode is not easy to separate out lithium, the quick charge performance of the battery is good, the charging efficiency is higher, the cycle performance is better, and in addition, the impedance of the battery is lower.
The above examples merely represent a few exemplary embodiments of the present application, which are described in more detail and are not to be construed as limiting the scope of the present application. It should be noted that it would be apparent to those skilled in the art that various modifications and improvements could be made without departing from the spirit of the present application, which would be within the scope of the present application. Accordingly, the scope of protection of the present application is to be determined by the claims appended hereto.

Claims (8)

1. The negative electrode plate is characterized by comprising a negative electrode current collector and a negative electrode active material layer arranged on at least one side surface of the negative electrode current collector, wherein the negative electrode active material layer contains a negative electrode active material and the following parameter k is defined:
Figure FDA0003436996740000011
and k is in the range of 10.00-20.00;
wherein Dv10, dv50, dv90 respectively represent particle diameter values corresponding to the cumulative volume distribution percentages of the negative electrode active material reaching 10%, 50%, 90%, in μm; x represents the average aspect ratio of particles of the anode active material.
2. The negative electrode tab of claim 1 wherein x is in the range of 1-6.
3. The negative electrode sheet of claim 1, wherein Dv50 is in the range of 7-18 μm.
4. The negative electrode sheet of claim 1, wherein Dv10 is in the range of 2-15 μm.
5. The negative electrode sheet of claim 1, wherein Dv90 is in the range of 12-30 μm.
6. The negative electrode sheet of any one of claims 1-5, wherein the negative electrode active material comprises one or more of lithium titanate, a carbon material, a silicon-based material, and a tin-based material.
7. The negative electrode sheet of claim 6, wherein the negative electrode active material comprises a carbon material comprising graphite, the graphite being present in the negative electrode active material in a mass ratio of 40-95%.
8. A secondary battery comprising the negative electrode tab of any one of claims 1-7.
CN202111617568.4A 2021-12-27 2021-12-27 Negative electrode sheet and secondary battery Pending CN116364848A (en)

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