CN111864179B - Positive pole piece and preparation method thereof, lithium ion battery containing positive pole piece and application of lithium ion battery - Google Patents

Positive pole piece and preparation method thereof, lithium ion battery containing positive pole piece and application of lithium ion battery Download PDF

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CN111864179B
CN111864179B CN202010917785.4A CN202010917785A CN111864179B CN 111864179 B CN111864179 B CN 111864179B CN 202010917785 A CN202010917785 A CN 202010917785A CN 111864179 B CN111864179 B CN 111864179B
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active material
material layer
ion battery
lithium ion
lithium cobaltate
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CN111864179A (en
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梁晓静
楚英
夏小勇
陶德瑜
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Dongguan Weike Battery Co ltd
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Dongguan Weike Battery 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
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • 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
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • 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
    • H01M2004/028—Positive 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 invention provides a positive pole piece, a preparation method thereof, a lithium ion battery containing the positive pole piece and an application thereof, wherein the positive pole piece comprises a current collector, a first active substance layer and a second active substance layer which are sequentially stacked, and lithium cobaltate particles in the second active substance layer comprise first-particle-size lithium cobaltate particles and second-particle-size lithium cobaltate particles; d50 of the lithium cobaltate particles with the first particle size is 5-8 mu m; d50 of the lithium cobaltate particles with the second particle size is 12-16 mu m; by adopting the structure, the positive pole piece greatly improves the high-temperature storage performance of the battery and the power performance after high-temperature storage while the power performance of the battery is not lost, and well considers the power performance and the high-temperature storage performance of the unmanned aerial vehicle battery.

Description

Positive pole piece and preparation method thereof, lithium ion battery containing positive pole piece and application of lithium ion battery
Technical Field
The invention belongs to the field of lithium ion batteries, and relates to a positive pole piece, a preparation method thereof, a lithium ion battery containing the positive pole piece and application thereof.
Background
As a new energy industry, the application field of lithium ion batteries is continuously developing and expanding, such as the fields of mobile phones, digital cameras, notebook computers, unmanned aerial vehicles, starting power supplies, electric vehicles, energy storage power stations and the like. In recent years, unmanned aerial vehicle technology is continuously innovated, and lithium ion batteries are also rapidly developed in the field. Compared with the common battery, the battery for the unmanned aerial vehicle is more complex in use working conditions and environment, most of the battery is in a severe environment with larger temperature difference in an unmanned area, and higher requirements are provided for the environmental adaptability of the unmanned aerial vehicle battery.
At present, the normal discharge temperature of the existing lithium ion battery is-20 ℃ to 45 ℃, once the normal discharge temperature exceeds the use temperature of 45 ℃, the electrolyte and the electrode material of the lithium ion battery generate oxidation-reduction reaction, so that the internal resistance of the lithium ion battery is increased, the capacity is quickly attenuated, the cycle life is shortened, and the user experience is seriously influenced. Aiming at the improvement of the performance, the current method in the industry is to optimize the anode material and the electrolyte, but due to the limitation of the material, the improvement of the performance is not breakthrough progress at present, the high-temperature storage performance of the battery cell is deteriorated to a certain extent while the battery cell meets the requirement of the power performance of the unmanned aerial vehicle, and the power performance of the battery cell after being stored at the high temperature of 60 ℃ under full power becomes worse, so that in order to expand the application range of the lithium ion battery in the field of the unmanned aerial vehicle, a lithium ion battery product with constant battery discharge performance under the high-temperature condition, which can be applied to the unmanned aerial vehicle, needs to be designed.
CN103579615A discloses a lithium battery positive electrode material and a lithium battery using the same, which are characterized in that through a great deal of research on the particle size and specific surface area of lithium cobaltate, the particle size D50 of the lithium cobaltate is 2-16 mu m, and the specific surface area is 0.2-1.0 m2When the voltage per gram is higher than the voltage per gram, the lithium ion intercalation path is short, the resistance is small, the impedance of the battery is low, and the low-temperature discharge requirement of the lithium battery is met. In addition, the lithium battery containing the positive electrode material is disclosed, and the lithium battery effectively improves the discharge capacity retention rate at low temperature due to the adoption of the positive electrode material containing the small-particle-size lithium cobalt oxide with small ionic resistance. Although the method solves the problem of discharging of the lithium battery at low temperature, the storage performance of the lithium battery cannot be ensured under the high-temperature condition of more than 60 ℃.
CN106784855A discloses a manufacturing method of a high-temperature lithium ion battery for an unmanned aerial vehicle, wherein an aluminum foil/copper foil with a porous structure is adopted as a lithium ion battery current collector obtained by the manufacturing method, so that the internal resistance of the battery can be reduced, and the rate discharge performance of the battery can be improved. Meanwhile, the battery adopts high-temperature electrolyte, the additive in the electrolyte is a mixed additive consisting of 3, 3-sulfonyl dipropionitrile, vinylene carbonate and propylene sulfite, a compact and stable protective film is formed on the surfaces of a positive electrode and a negative electrode, the side reaction between the electrolyte and the electrodes at high temperature is inhibited, the battery is prevented from bulging, and the high-temperature characteristic of the battery is improved. However, the battery has a complex structure and a plurality of preparation processes, the power performance of the battery cannot be ensured under the condition of 60 ℃, and the application range is small.
The lithium ion batteries described in the above documents have problems of small battery adaptive temperature range, poor power performance, and the like, and cannot solve the problem of power performance reduction of the lithium battery at a high temperature of 60 ℃. The lithium ion battery which can still ensure the power performance under the high temperature condition is always paid attention to and expected by technical personnel in the industry by adopting a simpler method, and the problem to be solved at present is how to prepare a battery pole piece which meets the requirement. Therefore, it is necessary to develop a positive electrode plate which can be applied to an unmanned aerial vehicle and can still maintain high power performance at a high temperature of 60 ℃.
Disclosure of Invention
The invention aims to provide a positive pole piece, a preparation method thereof, a lithium ion battery containing the positive pole piece and application thereof, in particular to the positive pole piece which can be applied to an unmanned aerial vehicle and can still ensure the power performance under the high-temperature condition of 60 ℃ and the lithium ion battery containing the positive pole piece.
In order to achieve the purpose, the invention adopts the following technical scheme:
in a first aspect, the invention provides a positive electrode plate, which includes a current collector, a first active material layer and a second active material layer, which are sequentially stacked, wherein lithium cobaltate particles in the second active material layer include lithium cobaltate particles with a first particle size and lithium cobaltate particles with a second particle size; the first-particle-diameter lithium cobaltate particles have a D50 of 5 to 9 μm, for example: 5 μm, 5.5 μm, 6 μm, 6.5 μm, 7 μm, 7.5 μm, 8 μm or the like; the D50 of the lithium cobaltate particles with the second particle size is 12 μm to 16 μm, for example: 12 μm, 12.5 μm, 13 μm, 13.5 μm, 14 μm, 14.5 μm, 15 μm, 15.5 μm, 16 μm, or the like.
The second active material layer adopts the two lithium cobaltate particles with the specific particle size ranges, wherein the lithium cobaltate particles with small particle size can reduce battery impedance and improve battery efficiency, the lithium cobaltate particles with large particle size can improve battery stability, and the technical effect of improving the high-temperature stability of the battery while ensuring battery power is realized after the lithium cobaltate particles with large particle size are mixed.
According to the positive pole piece, lithium cobaltate with high stability is used as a positive active material, and the second active material layer uses the two lithium cobaltate particles with specific particle size ranges, so that the problems of poor multiplying power and low-temperature discharge performance caused by the use of the lithium cobaltate with high stability in the prior art are effectively solved.
Preferably, the mass ratio of the first-particle-diameter lithium cobaltate particles to the total amount of lithium cobaltate particles in the second active material layer is 0 to 50 wt.% and does not contain 0, for example: 2 wt.%, 5 wt.%, 10 wt.%, 20 wt.%, 30 wt.%, 40 wt.% or 50 wt.%, etc., preferably 5 to 50 wt.%.
The mass ratio of the first-particle-size lithium cobaltate particles in the second active material layer is in the range, so that the high-temperature and low-temperature performance of the electric core system is favorably considered, and if the mass ratio is more than 50%, the high-temperature performance of the electric core is not remarkably improved, and the performance requirement under the high-temperature condition cannot be met.
Preferably, the D90 of the lithium cobaltate particles with the first particle size is 9-12 μm, and the D10 is 2-4 μm;
preferably, the lithium cobaltate particles with the second particle size have D90 of 23-27 μm and D10 of 4-8 μm.
Preferably, the total mass percentage of the lithium cobaltate particles in the second active material layer is 95 to 98 wt.% based on 100 wt.% of the mass of the second active material layer, for example: 95 wt.%, 95.5 wt.%, 96 wt.%, 96.5 wt.%, 97 wt.%, 97.5 wt.%, or 98 wt.%, etc.
Preferably, the mass of the second active material layer is less than 50 wt.%, based on 100% of the sum of the masses of the first active material layer and the second active material layer; for example: 5 wt.%, 10 wt.%, 15 wt.%, 20 wt.%, 25 wt.%, 30 wt.%, 35 wt.%, 40 wt.% or 45 wt.%, etc., preferably 5 to 15 wt.%.
The mass ratio of the first active material layer to the second active material layer in the active material layer is controlled within the range, so that the rate performance and the low-temperature discharge performance of the battery are improved, and the degradation of the high-temperature performance of full-charge storage is reduced; when the mass ratio of the second active material layer is 50% or more, the battery power performance becomes poor and the required power cannot be achieved.
Preferably, the first active material layer contains therein lithium cobaltate particles having a D50 of 5 to 9 μm, for example: 5 μm, 6 μm, 7 μm, 8 μm, or 9 μm.
Preferably, the D90 of the lithium cobaltate particles in the first active material layer is 9 to 12 μm, and D10 is 2 to 4 μm.
The first active material layer uses the lithium cobaltate particles with smaller particle sizes, so that the ionic impedance of the battery is reduced, the lithium ions are embedded, meanwhile, the second active material layer uses the lithium cobaltate particles with two different particle size ranges, and the battery core is subjected to power degradation and larger expansion under the high-temperature condition, and is mainly caused by side reactions of a positive electrode material, particularly a surface positive electrode material, and an electrolyte under the high temperature condition. Therefore, the alleviation of the side reaction of the surface layer cathode material and the electrolyte is the key to the improvement of the high-temperature performance of the system, and the improvement of the surface layer cathode material is only carried out, so that the low-temperature performance and the power performance of the whole system are not obviously deteriorated.
Preferably, the mass percentage of the lithium cobaltate particles in the first active material layer is 95-98 wt.%, for example: 95 wt.%, 95.5 wt.%, 96 wt.%, 96.5 wt.%, 97 wt.%, 97.5 wt.%, or 98 wt.%, etc.
Preferably, the total surface density of the first active material layer and the second active material layer is 12.50 to 14.00mg/cm2For example: 12.50mg/cm2、12.60mg/cm2、12.80mg/cm2、12.90mg/cm2、13.00mg/cm2、13.20mg/cm2、13.40mg/cm2、13.60mg/cm2、13.80mg/cm2Or 14.00mg/cm2And the like.
Preferably, the average compacted density of the first active material layer and the second active material layer after rolling is within the range of 3.65-3.85 mg/cm3For example: 3.65mg/cm3、3.70mg/cm3、3.75mg/cm3、3.80mg/cm3Or 3.85mg/cm3And the like.
The surface density and the average compacted density are controlled within the ranges, and the obtained lithium ion battery has excellent high-temperature storage performance and power performance.
In a second aspect, the invention provides a preparation method of the positive electrode plate according to the first aspect, wherein the preparation method is a double-layer coating method.
Illustratively, the preparation method of the positive pole piece comprises the following steps:
(1) stirring to obtain first active material layer slurry and second active material layer slurry, wherein the first active material layer slurry is used as bottom layer slurry, the viscosity is 6000-10000, and preferably 7000-9000; the second active material layer slurry is used as surface layer slurry, and the viscosity is 1500-5000, preferably 2000-4000.
(2) Coating two layers of slurry simultaneously by using a double-die head device, and regulating and controlling the pressure of each die head to regulate and control the coating weight of each layer; and drying the pole piece in the coating process.
(3) And rolling the pole piece to reach the required integral compaction density to obtain the positive pole piece.
According to the invention, the double-layer pole piece can be prepared by adopting a double-layer coating method, and the lithium cobaltate particles with the two specific particle sizes are used in the second active material layer, so that the high stability of the lithium cobaltate is ensured, and the rate capability and the high-low temperature discharge performance of the battery are considered at the same time.
In a third aspect, the present invention further provides a lithium ion battery, where the lithium ion battery includes the positive electrode tab according to the first aspect.
The lithium ion battery adopts the positive pole piece in the first aspect, and can simultaneously give consideration to the rate capability and the high-temperature and low-temperature discharge performance of the battery.
Preferably, the lithium ion battery further comprises a negative electrode plate.
Preferably, the negative electrode plate comprises a negative electrode current collector and a negative electrode active material layer located on the surface of the negative electrode current collector.
Preferably, the negative electrode current collector comprises a carbon-coated copper foil.
Preferably, the negative electrode active material in the negative electrode active material layer includes artificial graphite, preferably quick-charging graphite.
Preferably, the particle diameter D50 of the negative electrode active material is 12 to 15 μm, for example: 12 μm, 12.5 μm, 13 μm, 13.5 μm, 14 μm, 14.5 μm, 15 μm, or the like.
Preferably, the negative electrode active material mass content in the negative electrode active material layer is 97 wt.% or more, for example: 97 wt.%, 97.5 wt.%, etc.
Preferably, the compacted density of the negative electrode active material layer is 1.70-1.78 mg/cm3For example: 1.70mg/cm3、1.71mg/cm、1.72mg/cm3、1.73mg/cm3、1.74mg/cm3、1.75mg/cm3、1.76mg/cm3、1.77mg/cm3Or 1.78mg/cm3And the like.
Preferably, the N/P of the lithium ion battery is set to be 1.06-1.08, such as 1.07.
The theoretical capacity/actual Positive capacity (N/P) of the Negative pole piece is the ratio of the capacity of the reversible surface of the Negative pole to the capacity of the reversible surface of the Positive pole in the same stage under the same operation condition.
Preferably, the lithium ion battery includes a separator.
Preferably, the membrane comprises a ceramic coated membrane.
Preferably, the lithium ion battery includes a positive electrode tab and a negative electrode tab.
Preferably, the positive and negative electrode tabs comprise aluminum tabs and/or copper nickel-plated tabs.
Preferably, the lithium ion battery comprises an aluminum plastic packaging film.
Preferably, the lithium ion battery comprises an electrolyte.
The electrolyte of the lithium ion battery adopts high-temperature and low-temperature electrolyte.
Preferably, the solvent of the electrolyte includes any one or a combination of at least two of ethylene carbonate, propylene carbonate, diethyl carbonate, propylene propyl ester and propylene ethyl ester, preferably a combination of ethylene carbonate, propylene carbonate, diethyl carbonate, propylene propyl ester and propylene ethyl ester.
Preferably, the volume ratio of ethylene carbonate, propylene carbonate, diethyl carbonate, propylene propyl ester and propylene ethyl ester is 10 (10-20): 5-15): 30-50: (5-20), for example: 10:20:5:45:20, 10:10:15:35:20, 10:20:5:50:15, 10:10:10:50:20, 10:20:10:30:20, 10:20:15:50:10, 10:10:15:50:5, 10:20:15:50:5, or 10:10:15:50:15, etc.
In a fourth aspect, the invention provides a use of the lithium ion battery according to the third aspect for a drone.
The lithium ion battery can still maintain high power performance at 60 ℃, the power performance and the high-temperature storage performance of the lithium ion battery are well considered, the high-temperature storage performance of the lithium ion battery is greatly improved while the power performance of the lithium ion battery is not lost, and the lithium ion battery is suitable for being used as a battery of an unmanned aerial vehicle.
Preferably, the working temperature of the lithium ion battery is-20 to 60 ℃, for example: -20 ℃, 10 ℃, 0 ℃, 10 ℃, 20 ℃, 30 ℃, 40 ℃, 50 ℃ or 60 ℃ and the like.
Compared with the prior art, the invention has the following beneficial effects:
(1) the second active material layer in the positive pole piece uses the two lithium cobaltate particles with specific particle sizes, wherein the lithium cobaltate particles with small particle sizes can reduce battery impedance, improve battery efficiency and improve the discharge capacity retention rate of a lithium battery, the lithium cobaltate particles with large particle sizes are beneficial to improving the stability of the battery, the proportion of the lithium cobaltate on the surface layer is low, the side reaction of the lithium cobaltate on the surface layer is reduced, the high-temperature performance degradation of full-charge storage is reduced, and the stability of the battery at the high temperature of 60 ℃ can be improved while the rate performance of the battery is ensured by mixing the two lithium cobaltate particles.
(2) According to the invention, the two lithium cobaltate particles with specific particle diameters are mixed in the second active material layer in the positive pole piece, so that the power performance and the high-temperature storage performance of the unmanned aerial vehicle battery are well considered.
Drawings
FIG. 1 is an electron micrograph of an active material layer of a positive electrode sheet in example 1 of the present invention;
FIG. 2 is a graph comparing the thermal expansion of cells after 30 days storage at 60 ℃ for the cells of example 1 of the present invention and comparative examples 1-2;
FIG. 3 is a graph comparing cell swell after 12h storage at 85 ℃ for cells of example 1 of the present invention and comparative examples 1-2;
FIG. 4 is a graph comparing the 4C discharge curves at room temperature/-10 ℃ for cells from example 1 of the present invention and comparative examples 1-2;
FIG. 5 is a graph of constant voltage discharge at-5 ℃ of 60% SOC 3.0V for cells in example 1 of the present invention and comparative examples 1-2;
FIG. 6 is a graph showing constant voltage discharge at 60% SOC 3.0V at 15 ℃ after 30 days of storage at 60 ℃ in the battery cells of example 1 and comparative examples 1-2 according to the present invention.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
In the embodiments of the present invention, the types of the active material, the conductive agent, and the binder in the first active material layer may be the same or different, and the following examples are only illustrative and not intended to limit the present invention.
Example 1
The embodiment provides a positive electrode plate, which comprises a current collector, a first active substance layer and a second active substance layer, wherein the first active substance layer is located between the current collector and the second active substance layer, the first active substance layer and the second active substance layer both comprise a positive active substance, a conductive agent and a binder, the current collector adopts an aluminum foil, the positive active substance is lithium cobaltate, the binder is polyvinylidene fluoride (PVDF), the conductive agent is a carbon black and carbon nanotube compound conductive agent, and the compound ratio of the carbon black and the carbon nanotube is 1: 1;
wherein, in the first active material layer, the particle diameter D50 of the lithium cobaltate particles is 5.5 μm, D90 is 10 μm, and D10 is 3 μm; 97.3 wt.% of the lithium cobaltate active material in the first active material layer;
in the second active material layer, the lithium cobaltate particles comprise first particle size lithium cobaltate particles and second particle size lithium cobaltate, wherein the first particle size lithium cobaltate D50 is 5.5 μm, the D90 is 10 μm, the D10 is 3 μm, the second particle size lithium cobaltate D50 is 15 μm, the D90 is 25 μm, and the D10 is 7 μm;
the first active material layer accounts for 95 wt.%, and the second active material layer accounts for 5 wt.%, based on 100% of the mass of the positive electrode active material layer;
50 wt.% of the second-particle-diameter lithium cobaltate particles in the second active material layer based on the total mass of the lithium cobaltate particles; the total amount of the lithium cobaltate active material in the second active material layer was 98 wt.%;
the total surface density of the first active material layer and the second active material layer was 12.95mg/cm3Average compacted density of 3.75mg/cm3。
Fig. 1 is an electron microscope image of the active material layer of the positive electrode sheet in this example, and it can be seen from this image that the mass ratio of the second active material layer is smaller than that of the first active material layer, and the proportion of the lithium cobaltate particles having the first particle diameter to the total amount of lithium cobaltate particles in the second active material layer is smaller than that of the lithium cobaltate particles having the second particle diameter.
The embodiment also provides a battery cell, which comprises the positive pole piece, the negative pole piece and a diaphragm, wherein the negative active material in the negative pole piece is quick-charging graphite, the current collector uses carbon-coated copper foil, and the compaction design of the carbon-coated copper foil is 1.75mg/cm2Mass percent of negative active material 97 wt.%;
the diaphragm is coated by ceramic.
The embodiment also provides a lithium ion battery, which comprises the battery cell and the electrolyte;
the solvent of the electrolyte is ethylene carbonate, propylene carbonate, diethyl carbonate, propylene propyl ester and propylene ethyl ester which are 10:20:5:50:15, and the lithium salt is LiPF6The additive is vinylene carbonate: fluoroethylene carbonate: 1, 3-propanesultone: succinonitrile adiponitrile 0.3:1.8:4:0.5: 1.
Example 2
This example differs from example 1 only in that the lithium cobaltate particles used in the first active material layer of the positive electrode sheet had a D50 of 5.0 μm, a D90 of 11 μm and a D10 of 3.5 μm, and the lithium cobaltate particles used in the second active material layer had a D50 of 5 μm, a D90 of 11 μm, a D10 of 3.5 μm, a D50 of 14 μm, a D90 of 24 μm and a D10 of 8 μm, and other parameters and conditions were exactly the same as in example 1.
Example 3
This example differs from example 1 only in that the mass of the first active material layer accounts for 85 wt.%, and the mass of the second active material layer accounts for 15 wt.%, based on 100% of the sum of the masses of the first active material layer and the second active material layer. Other parameters and conditions were exactly the same as in example 1.
Example 4
This example differs from example 1 only in that the mass of the first active material layer accounts for 80 wt.%, and the mass of the second active material layer accounts for 20 wt.%, based on 100% of the sum of the masses of the first active material layer and the second active material layer. Other parameters and conditions were exactly the same as in example 1.
Example 5
This example differs from example 1 only in that the mass of the first active material layer accounts for 97 wt.%, and the mass of the second active material layer accounts for 3 wt.%, based on 100% of the sum of the masses of the first active material layer and the second active material layer. Other parameters and conditions were exactly the same as in example 1.
Example 6
This example differs from example 1 only in that the first particle diameter lithium cobaltate particles account for 5 wt.% and the second particle diameter lithium cobaltate particles account for 95 wt.% based on 100% by mass of the total lithium cobaltate particles in the second active material layer, and other parameters and conditions are exactly the same as in example 1.
Example 7
This example is different from example 1 only in that the mass of the lithium cobaltate particles of the first particle diameter accounts for 3 wt.%, the mass of the lithium cobaltate particles of the second particle diameter accounts for 97 wt.%, and other parameters and conditions are exactly the same as those in example 1, based on 100% of the total mass of the lithium cobaltate particles in the second active material layer.
Example 8
This example is different from example 1 only in that the mass ratio of the lithium cobaltate particles of the first particle diameter is 60 wt.%, and the mass ratio of the lithium cobaltate particles of the second particle diameter is 40 wt.%, based on 100% by mass of the total lithium cobaltate particles in the second active material layer, and other parameters and conditions are exactly the same as those in example 1.
Example 9
The positive electrode plate provided by the embodiment comprises a current collector, a first active substance layer and a second active substance layer, wherein the first active substance layer is positioned between the current collector and the second active substance layer, the first active substance layer and the second active substance layer both comprise a positive active substance, a conductive agent and a binder, the current collector adopts an aluminum foil, the positive active substance is lithium cobaltate, the binder is PVDF, the conductive agent is a carbon black and carbon nanotube compound conductive agent, and the compounding ratio of the carbon black and the carbon nanotube is 1: 1;
wherein the particle diameter D50 of the lithium cobaltate particles of the first active material layer is 7 μm, D90 is 13 μm, and D10 is 3 μm; 96 wt.% of the lithium cobaltate active material in the first active material layer;
in the second active material layer, the lithium cobaltate particles include first particle size lithium cobaltate particles and second particle size lithium cobaltate, wherein the first particle size lithium cobaltate is 7 μm, the D90 is 13 μm, the D10 is 3 μm, the second particle size lithium cobaltate is D50 is 16 μm, the D90 is 26 μm, and the D10 is 6 μm;
the first active material layer accounts for 10 wt.%, and the second active material layer accounts for 90 wt.%, based on 100% of the mass of the positive electrode active material layer;
30 wt.% of the second-particle-diameter lithium cobaltate particles in the second active material layer based on the total mass of the lithium cobaltate particles; the total amount of the lithium cobaltate active material in the second active material layer was 97 wt.%;
the total surface density of the first active material layer and the second active material layer is 13mg/cm3Average compacted density of 3.7mg/cm3。
The embodiment also provides a battery cell, which comprises the positive pole piece, the negative pole piece and the diaphragm, wherein the negative active material in the negative pole piece is quick-charging graphite, the current collector uses copper foil and aluminum foil, and the compaction design is 1.76mg/cm2Mass percent of negative active material 97.6 wt.%;
the diaphragm is coated by ceramic.
The embodiment also provides a lithium ion battery, which comprises the battery cell and the electrolyte;
the solvent of the electrolyte is ethylene carbonate, propylene carbonate, diethyl carbonate, propylene ethyl ester and propylene propyl ester, the ratio of ethylene carbonate to propylene ethyl ester is 10:10:10:50:20, and LiPF is used as lithium salt6The additive is vinylene carbonate: fluoroethylene carbonate: 1, 3-propanesultone: succinonitrile adiponitrile 0.3:1.8:4:0.5: 1.
Example 10
The positive electrode plate provided by the embodiment comprises a current collector, a first active substance layer and a second active substance layer, wherein the first active substance layer is positioned between the current collector and the second active substance layer, the first active substance layer and the second active substance layer both comprise a positive active substance, a conductive agent and a binder, the current collector adopts an aluminum foil, the positive active substance is lithium cobaltate, the binder is PVDF, the conductive agent is a carbon black and carbon nanotube compound conductive agent, and the compounding ratio of the carbon black and the carbon nanotube is 1: 1;
the particle diameter D50 of the lithium cobaltate particles of the first active material layer was 6 μm, D90 was 12 μm, and D10 was 4 μm; 96.4 wt.% of the lithium cobaltate active material in the first active material layer;
in the second active material layer, the lithium cobaltate particles include first particle size lithium cobaltate particles and second particle size lithium cobaltate, wherein the first particle size lithium cobaltate D50 is 6 μm, the D90 is 12 μm, the D10 is 4 μm, the second particle size lithium cobaltate D50 is 14 μm, the D90 is 25 μm, and the D10 is 8 μm;
the first active material layer accounts for 80 wt.%, and the second active material layer accounts for 20 wt.%, based on 100% of the mass of the positive electrode active material layer;
75 wt.% of the second-particle-diameter lithium cobaltate particles in the second active material layer based on the total mass of the lithium cobaltate particles; 98 wt.% of the lithium cobaltate active material in the second active material layer;
the total surface density of the first active material layer and the second active material layer is designed to be 13mg/cm3Average compacted density of 3.72mg/cm3。
The embodiment provides a battery cell, which comprises the positive pole piece, the negative pole piece and a diaphragm, wherein the negative active material in the negative pole piece is quick-charging graphite, copper foil and aluminum foil are used as current collectors, and the compaction design is 1.74mg/cm2Mass percent of negative active material 97.8 wt.%;
the diaphragm is coated by ceramic.
The embodiment also provides a lithium ion battery, which comprises the battery cell and the electrolyte;
the solvent of the electrolyte is ethylene carbonate, propylene carbonate, diethyl carbonate, propylene ethyl ester and propylene propyl ester, the ratio of ethylene carbonate to propylene ethyl ester is 10:10:15:50:5, and LiPF is used as lithium salt6The additive is vinylene carbonate: fluoroethylene carbonate: 1, 3-propanesultone: succinonitrile adiponitrile 0.3:1.8:4:0.5: 1.
Comparative example 1
The comparative example is different from example 1 only in that the particle diameters of lithium cobaltate particles used in the first active material layer and the second active material layer in the positive electrode sheet are both 8 μm in D50, 15 μm in D90 and 3 μm in D10, and other parameters and conditions are exactly the same as those in example 1.
Comparative example 2
The comparative example is different from example 1 only in that the particle diameters of lithium cobaltate particles used in the first active material layer and the second active material layer in the positive electrode sheet are both 15 μm in D50, 27 μm in D90 and 5 μm in D10, and other parameters and conditions are exactly the same as those in example 1.
Comparative example 3
The comparative example differs from example 1 only in that the particle diameters of the lithium cobaltate particles used in the second active material layer in the positive electrode sheet were each 15 μm in D50, 27 μm in D90, and 5 μm in D10, and other parameters and conditions were exactly the same as in example 1.
Comparative example 4
This comparative example differs from example 1 only in that the first-particle-diameter lithium cobaltate particles in the second active material layer had a D50 of 3 μm, a D90 of 15 μm, a D10 of 10 μm, second-particle-diameter lithium cobaltate particles having a D50 of 20 μm, a D90 of 30 μm, and a D10 of 12 μm, and other parameters and conditions were exactly the same as in example 1.
Comparative example 5
This comparative example differs from example 1 only in that the second active material layer used lithium cobaltate particles of the first particle diameter having a D50 of 4 μm, a D90 of 8 μm and a D10 of 1 μm, and used lithium cobaltate particles of the second particle diameter having a D50 of 6 μm, a D90 of 10 μm and a D10 of 3 μm, and other parameters and conditions were exactly the same as in example 1.
And (3) performance testing:
the cells in examples 1-10 and comparative examples 1-5 were subjected to a thermal expansion test, a low-temperature discharge performance test, a high-temperature rate performance test, and a cycle performance test; the test method is as follows:
the method for testing the thermal expansion of the battery cell comprises the following steps:
recording initial voltage, internal resistance and thickness at 25 + -2 deg.C, charging to 4.40V at 1.8C, cutting off at constant voltage of 0.05C, measuring thickness A1 with fully charged battery, storing in oven at 85 deg.C for 12 hr, measuring thickness A2 with thermal expansion rate (A2-A1)/A1
Recording initial voltage, internal resistance and thickness at 25 + -2 deg.C, charging to 4.40V at 1.8C, cutting off at constant voltage of 0.05C, measuring thickness A1 with fully charged battery, storing in high temperature oven at 60 deg.C for 30 days, measuring thickness A2 with thermal expansion rate (A2-A1)/A1
The low-temperature discharge performance test method comprises the following steps:
charging to 4.40V at 1.8C at 25 + -2 deg.C, cutting off at constant voltage of 0.05C, and discharging to 3.0V at 4.0C after standing at-10 deg.C for 2 hr.
Charging to 4.40V at 1.8C at 25 + -2 deg.C, cutting off at constant voltage of 0.05C, and discharging to 2.75V at 7.0C after standing at-10 deg.C for 2 hr.
The high-temperature rate performance test method comprises the following steps:
charging to 4.40V at 1.8C at 25 + -2 deg.C, cutting off at constant voltage of 0.05C, standing for 30 min, and discharging to 2.75V at 7.0C.
The cycle performance test method comprises the following steps:
1. charging to 4.40V at 25 + -2 deg.C with 1.8C, stopping at constant voltage of 0.05C, standing for 10min, discharging at 4.0C under constant current to 3.0V, standing for 10min, and circulating for 500 cycles.
2. Charging to 4.40V at 45 + -2 deg.C with 1.8C, stopping at constant voltage of 0.05C, standing for 10min, discharging at 4.0C under constant current to 3.0V, standing for 10min, and circulating for 500 cycles.
The performance test results are shown in table 1 and fig. 2-6:
TABLE 1
Figure BDA0002665640540000151
Figure BDA0002665640540000161
As can be seen from table 1, the cell provided by the invention improves the high-temperature stability of the cell while improving the energy density, power performance and cycle performance of the cell, and gives good consideration to both the power performance and high-temperature storage performance of the unmanned aerial vehicle cell.
And comparing the examples 3 to 4 with the examples 1 and 5, wherein the mass ratio of the second active material layer is preferably 5 to 15 wt.%, and the mass ratio of the second active material layer is maintained at the above ratio, which is favorable for ensuring the rate capability and the high-temperature stability of the battery cell, when the mass ratio of the second active material layer is less than 5%, the mixed-particle-size lithium cobalt oxide particles are less, the high-temperature stability of the battery cell is poor, and when the mass ratio of the second active material layer is more than 15%, the small-particle-size lithium cobalt oxide particles are less, and the battery cell efficiency is low.
As can be seen from comparison of examples 7 to 8 and examples 1 and 6, the proportion of the first-particle-size lithium cobaltate particles is preferably 5 to 50% based on 100% of the total mass of the lithium cobaltate particles in the second active material layer, and maintaining the proportion of the first-particle-size lithium cobaltate particles is advantageous for ensuring rate capability and high-temperature stability of the cell, when the proportion of the first-particle-size lithium cobaltate particles is less than 5%, the rate capability of the cell is poor, and when the proportion of the first-particle-size lithium cobaltate particles is more than 50%, the stability of the cell is poor.
As can be seen from comparison of example 1 and comparative examples 1 to 5, the use of the lithium cobaltate particles having the above two specific particle diameters for the second active material layer can improve the stability of the cell at a high temperature of 60 ℃ while ensuring the rate capability of the cell.
Fig. 2 and 3 show the comparative thermal expansion of the cells after 30 days storage at 60 c and 12 hours storage at 85 c for the cells of example 1 and comparative examples 1-2, respectively.
As can be seen from fig. 2 and 3, after a lapse of time under the high temperature conditions of 60 c and 85 c, the cell swelling degree of the positive electrode active material of comparative example 1, which selected small-sized lithium cobaltate (5.5 μm for D50, 10 μm for D90, and 3 μm for D10) as a positive electrode active material, was the greatest, the cell swelling degree of the positive electrode active material in comparative example 2 using large-sized lithium cobaltate particles (15 μm for D50, 27 μm for D90, and 5 μm for D10) was minimized, in example 1, the second active material layer used mixed particles (in which the first particle size lithium cobaltate D50 was 5.5 μm, D90 was 10 μm, D10 was 3 μm, the second particle size lithium cobaltate D50 was 15 μm, D90 was 27 μm, and D10 was 5 μm) as the positive electrode active material exhibited a slightly larger degree of cell expansion than the cell using the large particle lithium cobaltate system, but much smaller than the cell using the small particle lithium cobaltate system.
As can also be seen from fig. 2 and 3, the degree of swelling of the cell selected in comparative example 1 using the small-sized lithium cobaltate as the positive electrode active material was large both at 85 ℃ for 12 hours and at 60 ℃ for 30 days; in contrast, the cell in comparative example 2 using large-sized lithium cobaltate particles as a positive electrode active material did not change much in the degree of cell expansion from the cell in example 1 using the mixed particles as a positive electrode active material; further, it is demonstrated that the high-temperature storage stability of the cell is ensured by using two lithium cobaltate particles having specific particle size ranges in the second active material layer in the present invention.
The comparative graph of the 4C discharge curve at room temperature/-10 ℃ of the cells and the 60% SOC constant voltage discharge curve at-5 ℃ of the cells in example 1 and comparative examples 1-2 are shown in fig. 4 and 5, and it can be seen from fig. 4 and 5 that the discharge efficiency of the cell using the small-sized lithium cobaltate particles as the positive electrode active material in comparative example 1 and the cell using the mixed particles as the positive electrode active material in example 1 are relatively close to each other at-10 ℃ or-5 ℃, and the discharge effect of the cell using the large-sized lithium cobaltate particles as the positive electrode active material in comparative example 2 is significantly poor.
From the above, it can be seen that the battery cell formed by using the mixed particles with two specific particle sizes as the positive active material in the invention can ensure the discharge efficiency of the battery cell and simultaneously give good consideration to the stability under high temperature conditions, thereby improving the comprehensive performance of the battery cell.
The applicant declares that the above description is only a specific embodiment of the present invention, but the scope of the present invention is not limited thereto, and it should be understood by those skilled in the art that any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are within the scope and disclosure of the present invention.

Claims (34)

1. The positive pole piece is characterized by comprising a current collector, a first active material layer and a second active material layer which are sequentially stacked, wherein lithium cobaltate particles in the second active material layer comprise first-particle-size lithium cobaltate particles and second-particle-size lithium cobaltate particles; d50 of the lithium cobaltate particles with the first particle size is 5-9 mu m; the second-particle-diameter lithium cobaltate particles have a D50 value of 12 to 16 [ mu ] m, and the mass ratio of the second active material layer is 5 to 15 wt.% based on 100% of the sum of the masses of the first active material layer and the second active material layer.
2. The positive electrode sheet according to claim 1, wherein the mass ratio of the first-particle-diameter lithium cobaltate particles to the total amount of the lithium cobaltate particles in the second active material layer is 0 to 50 wt.% and does not contain 0.
3. The positive electrode sheet according to claim 2, wherein the mass ratio of the first-particle-diameter lithium cobaltate particles to the total amount of the lithium cobaltate particles in the second active material layer is 5 to 50 wt.%.
4. The positive electrode sheet according to claim 1, wherein the first-particle-size lithium cobaltate particles have a D90 of 9 to 12 μm and a D10 of 2 to 4 μm.
5. The positive electrode sheet according to claim 1, wherein the lithium cobaltate particles having the second particle size have a D90 of 23 to 27 μm and a D10 of 4 to 8 μm.
6. The positive electrode sheet according to claim 1, wherein the total mass percentage of the lithium cobaltate particles in the second active material layer is 95 to 98 wt.% based on 100 wt.% of the mass of the second active material layer.
7. The positive electrode sheet according to claim 1, wherein the first active material layer contains lithium cobaltate particles having a D50 of 5 to 9 μm.
8. The positive electrode sheet according to claim 7, wherein the lithium cobaltate particles in the first active material layer have a D90 of 9 to 12 μm and a D10 of 2 to 4 μm.
9. The positive electrode sheet according to claim 7, wherein the mass percentage of the lithium cobaltate particles in the first active material layer is 95 to 98 wt.%.
10. The positive electrode sheet according to claim 1, wherein the first active material layer and the second active material layer have a total coating surface density of 12.50 to 14.00mg/cm2。
11. The positive electrode sheet according to claim 1, wherein the average compacted density of the first active material layer and the second active material layer after rolling is in a range of 3.65 to 3.85g/cm3。
12. The method for preparing a positive electrode plate according to any one of claims 1 to 11, wherein the preparation method is a double-layer coating method.
13. The method of claim 12, comprising the steps of:
(1) stirring to obtain first active material layer slurry and second active material layer slurry, wherein the first active material layer slurry is used as bottom layer slurry, and the viscosity is 7000-9000; the second active material layer slurry is used as surface layer slurry, and the viscosity is 2000-4000;
(2) coating two layers of slurry simultaneously by using a double-die head device, and regulating and controlling the pressure of each die head to regulate and control the coating weight of each layer; drying the pole piece in the coating process;
(3) and rolling the pole piece to reach the required integral compaction density to obtain the positive pole piece.
14. A lithium ion battery, characterized in that the lithium ion battery comprises the positive electrode sheet according to any one of claims 1 to 11.
15. The lithium ion battery of claim 14, further comprising a negative electrode tab.
16. The lithium ion battery of claim 15, wherein the negative electrode tab comprises a negative electrode current collector and a negative electrode active material layer on a surface thereof.
17. The lithium ion battery of claim 16, wherein the negative current collector comprises a carbon coated copper foil.
18. The lithium ion battery according to claim 16, wherein the negative electrode active material in the negative electrode active material layer comprises artificial graphite.
19. The lithium ion battery according to claim 18, wherein the negative electrode active material in the negative electrode active material layer is quick-charging graphite.
20. The lithium ion battery according to claim 18, wherein the negative electrode active material in the negative electrode active material layer has a particle diameter D50 of 12 to 15 μm.
21. The lithium ion battery according to claim 20, wherein the negative electrode active material in the negative electrode active material layer is contained in an amount of 97 wt.% or more.
22. The lithium ion battery according to claim 16, wherein the negative electrode active material in the negative electrode active material layer has a compacted density of 1.70 to 1.78mg/cm3。
23. The lithium ion battery according to claim 14, wherein the N/P of the lithium ion battery is set to 1.06 to 1.08.
24. The lithium ion battery of claim 14, wherein the lithium ion battery comprises a separator.
25. The lithium ion battery of claim 24, wherein the separator comprises a ceramic coated separator.
26. The lithium ion battery of claim 14, wherein the lithium ion battery comprises positive and negative tabs.
27. The lithium ion battery of claim 26, wherein the positive and negative electrode tabs comprise aluminum tabs and/or copper nickel plated tabs.
28. The lithium ion battery of claim 14, wherein the lithium ion battery comprises an aluminum plastic packaging film.
29. The lithium ion battery of claim 14, wherein the lithium ion battery comprises an electrolyte.
30. The lithium ion battery of claim 29, wherein the solvent of the electrolyte comprises any one of ethylene carbonate, propylene carbonate, diethyl carbonate, propyl propionate, or ethyl propionate, or a combination of at least two thereof.
31. The lithium ion battery of claim 30, wherein the solvent of the electrolyte is a combination of ethylene carbonate, propylene carbonate, diethyl carbonate, propyl propionate, and ethyl propionate.
32. The lithium ion battery of claim 31, wherein the solvent of the electrolyte, the ethylene carbonate, the propylene carbonate, the diethyl carbonate, the propylene propyl ester and the propylene ethyl ester are in a mass ratio of 10 (10-20): 5-15): 30-50: 5-20.
33. Use of a lithium ion battery according to any of claims 14-32 for a drone.
34. The use according to claim 33, wherein the lithium ion battery has an operating temperature of-20 to 60 ℃.
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