WO2021217586A1 - 二次电池及其制备方法、含有该二次电池的装置 - Google Patents
二次电池及其制备方法、含有该二次电池的装置 Download PDFInfo
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- WO2021217586A1 WO2021217586A1 PCT/CN2020/088300 CN2020088300W WO2021217586A1 WO 2021217586 A1 WO2021217586 A1 WO 2021217586A1 CN 2020088300 W CN2020088300 W CN 2020088300W WO 2021217586 A1 WO2021217586 A1 WO 2021217586A1
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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
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
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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
- H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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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
- H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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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
- H01M4/362—Composites
- H01M4/364—Composites as mixtures
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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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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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
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Definitions
- This application belongs to the field of electrochemical technology, and more specifically, relates to a secondary battery, a preparation method thereof, and a device containing the secondary battery.
- secondary batteries As a new type of high-voltage, high-energy-density rechargeable battery, secondary batteries have outstanding characteristics such as light weight, high energy density, no pollution, no memory effect, and long service life, so they are widely used in the new energy industry.
- this application provides a secondary battery, a preparation method thereof, and a device containing the secondary battery. Good fast charging performance and cycle performance.
- a first aspect of the present application provides a secondary battery, including a negative electrode piece, the negative electrode piece comprising a negative electrode current collector and a negative electrode film layer, the negative electrode film layer includes a first negative electrode film layer and A second negative electrode film layer, the first negative electrode film layer is disposed on at least one surface of the negative electrode current collector and includes a first negative electrode active material, and the second negative electrode film layer is disposed on the first negative electrode film layer and includes a second negative electrode Active material; both the first negative active material and the second negative active material include artificial graphite; the first negative active material includes primary particles, and the primary particles are in the first negative active material The quantity accounted for A satisfies: A ⁇ 50%.
- the second aspect of the present application provides a method for preparing a secondary battery, which includes preparing a negative electrode piece of the secondary battery by the following steps: 1) forming a first negative electrode active material on at least one surface of a negative electrode current collector A negative electrode film layer; 2) forming a second negative electrode film layer including a second negative electrode active material on the first negative electrode film layer; wherein both the first negative electrode active material and the second negative electrode active material include artificial graphite
- the first negative active material includes primary particles, and the number of primary particles in the first negative active material accounts for A ⁇ 50%.
- a third aspect of the present application provides a device including the secondary battery described in the first aspect of the present application or a secondary battery manufactured according to the method described in the second aspect of the present application.
- the negative pole piece of the secondary battery of the present application includes a double-coated structure, and the different composition of the active material of each coating is controlled during the design, so that the secondary battery can have a higher energy density while taking into account better speed. Charging performance and long cycle life.
- the device of the present application includes the secondary battery provided by the present application, and thus has at least the same advantages as the secondary battery.
- FIG. 1 is a schematic diagram of an embodiment of the secondary battery of the present application.
- FIG. 2 is a schematic diagram of an embodiment of the negative pole piece in the secondary battery of the present application.
- FIG. 3 is a schematic diagram of another embodiment of the negative pole piece in the secondary battery of the present application.
- Fig. 4 is an exploded schematic view of an embodiment of the secondary battery of the present application.
- Fig. 5 is a schematic diagram of an embodiment of a battery module.
- Fig. 6 is a schematic diagram of an embodiment of a battery pack.
- Fig. 7 is an exploded view of Fig. 6.
- FIG. 8 is a schematic diagram of an embodiment of a device in which the secondary battery of the present application is used as a power source.
- FIG. 9 is an SEM image of primary particles in an embodiment of the first negative electrode active material.
- FIG. 10 is an SEM image of secondary particles in an embodiment of the second negative electrode active material.
- any lower limit can be combined with any upper limit to form an unspecified range; and any lower limit can be combined with other lower limits to form an unspecified range, and any upper limit can be combined with any other upper limit to form an unspecified range.
- each individually disclosed point or single value can be used as a lower limit or upper limit in combination with any other point or single value or with other lower or upper limits to form an unspecified range.
- the first aspect of the application provides a secondary battery.
- the secondary battery includes a positive pole piece, a negative pole piece and an electrolyte.
- active ions are inserted and extracted back and forth between the positive pole piece and the negative pole piece.
- the electrolyte conducts ions between the positive pole piece and the negative pole piece.
- the thickness of the negative electrode film layer is often increased, but the increase in thickness will affect both the fast charging performance and the cycle performance of the battery. This is because the negative active material swells during the cycle, which leads to a decrease in the bonding force between the active material and the substrate, and even film release. This phenomenon becomes more serious when the thickness increases; at the same time, the thickness increases. The diffusion path of active ions is increased, so that the fast charging performance of the battery will also be affected. Therefore, how to make the battery have better fast charging performance and cycle performance under the premise of higher energy density is still a huge technical challenge.
- the negative pole piece in the secondary battery of the present application includes a negative electrode current collector and a negative electrode film layer.
- the negative electrode film layer includes a first negative electrode film layer and a second negative electrode film layer.
- the negative electrode current collector is on at least one surface and includes a first negative electrode active material, and the second negative electrode film layer is disposed on the first negative electrode film layer and includes a second negative electrode active material; the first negative electrode active material and the second negative electrode active material
- the negative electrode active materials all include artificial graphite; the first negative electrode active material includes primary particles, and the number of the primary particles in the first negative electrode active material accounts for the ratio A: A ⁇ 50%.
- the secondary battery can have both better fast charging performance and cycle performance under the premise of higher energy density.
- the first negative electrode active material and the second negative electrode active material both include artificial graphite, and the number of primary particles in the first negative electrode active material accounts for A ⁇ 50%, the ratio of the first negative electrode active material and the second negative electrode active material can be effectively increased.
- the contact surface between the current collectors, this multi-surface contact can ensure the bonding reliability of long-term multiple charging and discharging, and at the same time improve the electron conduction efficiency, thereby effectively improving the cycle performance and fast charging performance of the battery.
- the quantity ratio A of the primary particles in the first negative electrode active material satisfies: A ⁇ 70%, more preferably, 80% ⁇ A ⁇ 100%.
- the range of A may be: 75% ⁇ A ⁇ 98%, 80% ⁇ A ⁇ 95%, 85% ⁇ A ⁇ 100%, 90% ⁇ A ⁇ 100%, and so on.
- the inventors have found through in-depth research that when the anode active material and anode film layer of the present application meet the above design conditions, if one or more of the following parameters are optionally satisfied, the secondary can be further improved.
- the performance of the battery if one or more of the following parameters are optionally satisfied, the secondary can be further improved.
- the second negative electrode active material includes secondary particles, and the quantity of the secondary particles in the second negative electrode active material accounts for a ratio B that satisfies: B ⁇ 30%.
- B the quantity of the secondary particles in the second negative electrode active material.
- the inventor found through research that the second negative electrode film layer is closer to the side of the separator, and the active ion concentration in the area where it is located is higher. If the active material in the second negative electrode film layer contains a certain content of secondary particles, it can provide desorption. The number of intercalated active ion channels is exactly matched with the actual distribution of active ions in this area, which can further improve the fast charging performance and cycle performance of the battery. More preferably, the amount of the secondary particles in the second negative electrode active material satisfies B ⁇ 50%.
- the range of B can be: 30% ⁇ B ⁇ 100%, 40% ⁇ B ⁇ 85%, 45% ⁇ B ⁇ 98%, 50% ⁇ B ⁇ 100%, 55% ⁇ B ⁇ 95%, 60% ⁇ B ⁇ 98%, 80% ⁇ B ⁇ 99%, 70% ⁇ B ⁇ 95%, etc.
- the mass ratio of artificial graphite in the first negative electrode active material is ⁇ 50%, more preferably 60%-100%.
- the mass ratio of artificial graphite in the second negative electrode active material is ⁇ 80%, more preferably 90%-100%.
- Volume particle size distribution D V 10 may reflect the proportion of smaller particles in the active material, when the volume of the first negative electrode active material particle size distribution D V 10 smaller than the volume of the second negative electrode active material a particle size distribution of 10 D V, can Further improve the volumetric energy density and fast charging performance of the battery.
- the volume distribution particle diameter D V 10 of the first negative electrode active material may be 3 ⁇ m to 8 ⁇ m, more preferably 4 ⁇ m to 7 ⁇ m.
- the volume distribution particle diameter D V 10 of the second negative electrode active material may be 5 ⁇ m to 11 ⁇ m, more preferably 6 ⁇ m to 10 ⁇ m.
- the tap density of the first negative electrode active material is greater than the tap density of the second negative electrode active material.
- the battery can have both a higher volume energy density and better fast charging performance.
- the tap density of the first negative electrode active material may be 0.8 g/cm 3 to 1.3 g/cm 3 , more preferably 0.95 g/cm 3 to 1.15 g/cm 3 .
- the tap density of the second negative electrode active material may be 0.7 g/cm 3 to 1.2 g/cm 3 , more preferably 0.85 g/cm 3 to 1.05 g/cm 3 .
- the first volume of the negative electrode active material particle size distribution D V 50 is greater than the volume of the second negative electrode active material particle size distribution D V 50.
- the degree of matching with the battery during the concentration gradient of the active ions is preferably, may Effectively improve the fast charging performance of the battery.
- the first negative electrode active material has a larger particle size, which has more vacancies for receiving active ions, that is, a larger gram capacity, which is beneficial to the improvement of battery quality and energy density; at the same time, the second negative electrode active material has a larger particle size.
- the adhesive has more attachment sites on the surface, and the particles are less broken during cold pressing, and the probability of the material to produce a new surface is reduced. Therefore, it has a strong electrical conductivity during the charging and discharging process of the battery, and It can effectively suppress the "broken bridge" phenomenon of the electrolyte and further improve the cycle life of the battery.
- the volume distribution particle diameter D V 50 of the first negative electrode active material may be 13 ⁇ m to 21 ⁇ m, more preferably 15 ⁇ m to 19 ⁇ m.
- the volume distribution particle diameter D V 50 of the second negative electrode active material may be 11 ⁇ m to 19 ⁇ m, more preferably 13 ⁇ m to 17 ⁇ m.
- the graphitization degree of the first negative electrode active material is greater than the graphitization degree of the second negative electrode active material.
- the energy density and cycle performance of the battery can be further improved.
- the graphitization degree of the first negative electrode active material may be 92%-97%, more preferably 93%-96%.
- the graphitization degree of the second negative electrode active material may be 90%-95%, and more preferably 92%-94%.
- the specific surface area (SSA) of the first negative active material is greater than the specific surface area (SSA) of the second negative active material.
- the specific surface area (SSA) of the first negative active material is greater than the specific surface area (SSA) of the second negative active material, the energy density and fast charging performance of the battery can be further improved.
- the first negative electrode active material the specific surface area (SSA) of 1.6m 2 /g ⁇ 2.6m 2 / g, more preferably 1.8m 2 /g ⁇ 2.3m 2 / g.
- the second negative electrode active material the specific surface area (SSA) of 0.7m 2 /g ⁇ 1.5m 2 / g, more preferably 0.8m 2 /g ⁇ 1.3m 2 / g.
- the thickness of the negative electrode film layer is greater than or equal to 60 ⁇ m, more preferably 65 ⁇ m to 80 ⁇ m. It should be noted that the thickness of the negative electrode film layer is the sum of the thicknesses of the first negative electrode film layer and the second negative electrode film layer.
- the thickness ratio of the second negative electrode film layer to the first negative electrode film layer is 1:1 to 3:2.
- the thickness ratio of the first and second negative electrode membrane layers is in the given range, it is beneficial to form a gradient pore distribution in the upper and lower layers, so that the liquid phase conduction resistance of active ions from the positive electrode on the surface of the negative electrode membrane layer is reduced, and it will not cause ions on the surface layer. Accumulation causes the problem of lithium evolution.
- the uniform diffusion of active ions in the film is beneficial to reduce polarization, which can further improve the fast charging performance and cycle performance of the battery.
- the areal density of the negative electrode film layer is 8 mg/cm 2 -13 mg/cm 2 , preferably 9 mg/cm 2 -12.5 mg/cm 2 . It should be noted that the areal density of the negative electrode film layer refers to the areal density of the entire negative electrode film layer (that is, the sum of the areal densities of the first negative electrode film layer and the second negative electrode film layer).
- the compacted density of the negative electrode film layer is 1.4 g/cm 3 to 1.7 g/cm 3 , preferably 1.5 g/cm 3 to 1.65 g/cm 3 .
- the compaction density of the negative electrode film layer refers to the compaction density of the entire negative electrode film layer (that is, the ratio of the areal density of the negative electrode film layer to the thickness).
- the compaction density of the negative electrode film layer is within the given range, which enables the negative electrode pole piece to have high reversible capacity, but also has good low cycle expansion performance and dynamic performance, so as to further improve the energy density of the battery and fast Charging capacity and cycle performance.
- the primary particles and the secondary particles have the meanings known in the art.
- Primary particles refer to particles that have not formed an agglomerated state.
- the secondary particles refer to the agglomerated particles formed by the aggregation of two or more primary particles.
- Primary particles and secondary particles can be easily distinguished by taking a SEM image using a scanning electron microscope. For example, FIG. 9 shows an SEM image of primary particles in a typical first negative electrode active material, and FIG. 10 shows an SEM image of secondary particles in a typical second negative electrode active material.
- the proportion of primary particles or secondary particles in the negative electrode active material can be tested by methods known in the art, for example, can be determined by scanning electron microscopy.
- the test can refer to JY/T010-1996.
- multiple (for example, 20) different areas can be randomly selected in the sample to be tested for scanning test, and at a certain magnification (for example, 1000 times), the number of primary particles in each test area can be calculated.
- the percentage of the total number of particles is the percentage of the number of primary particles in the region, and the average of the calculation results of multiple test regions is taken as the percentage of the number of primary particles in the negative electrode active material. Similarly, the test of the proportion of the secondary particles in the negative electrode active material can also be performed.
- the tap density of the negative active material has a well-known meaning in the art, and can be tested using methods known in the art.
- both Dv10 and Dv50 of the negative electrode active material have meanings known in the art, and can be tested by methods known in the art.
- Dv10 and Dv50 are as follows:
- Dv10 the particle size when the cumulative volume distribution percentage of the negative active material reaches 10%
- Dv50 The particle size corresponding to the cumulative volume distribution percentage of the negative active material reaches 50%.
- the graphitization degree of the negative electrode active material has a well-known meaning in the art, and can be tested by a method known in the art.
- an X-ray diffractometer such as Bruker D8 Discover
- CuK ⁇ rays are usually used as the radiation source, and the wavelength of the rays is The scanning 2 ⁇ angle range is 20° ⁇ 80°, and the scanning rate can be 4°/min.
- the specific surface area (SSA) of the negative electrode active material has a well-known meaning in the art, and can be tested using methods known in the art.
- BET Brunauer Emmett Teller
- the thickness of the negative electrode film layer can be measured by a micrometer, for example, it can be measured by a micrometer with a model of Mitutoyo293-100 and an accuracy of 0.1 ⁇ m.
- the thickness of each of the first negative electrode film layer and the second negative electrode film layer can be tested by using a scanning electron microscope (such as ZEISS Sigma300).
- the test method may be as follows: firstly, the negative pole piece is cut into a sample to be tested of a certain size (for example, 2 cm ⁇ 2 cm), and the negative pole piece is fixed on the sample table by paraffin wax.
- sample stage into the sample rack, lock and fix it, turn on the power of the argon ion cross-section polisher (such as IB-19500CP) and vacuum (such as 10 -4 Pa), set the argon flow (such as 0.15 MPa) and voltage (such as 8KV) and polishing time (for example, 2 hours), adjust the sample stage to swing mode to start polishing.
- the power of the argon ion cross-section polisher such as IB-19500CP
- vacuum such as 10 -4 Pa
- argon flow such as 0.15 MPa
- voltage such as 8KV
- polishing time for example, 2 hours
- the average value of the test results of a plurality of test areas is taken as the average value of the thickness of the first negative electrode film layer and the second negative electrode film layer.
- the areal density of the negative electrode film layer has a well-known meaning in the art, and can be tested by a method known in the art.
- the test method can be: take a negative electrode piece coated on one side and cold pressed (if it is a negative electrode piece coated on both sides, wipe off the negative electrode film on one side first), and punch it into an area of Weigh the small disc of S1 and record it as M1. Then wipe off the negative electrode film of the above-mentioned weighed negative electrode sheet, weigh the weight of the negative electrode current collector, and record it as M0.
- the area density of the negative electrode film layer (weight of the negative electrode sheet M1-weight of the negative electrode current collector M0 )/S1.
- multiple groups for example, 10 groups) of samples to be tested can be tested, and the average value thereof can be calculated as the test result.
- the sample can be sampled as follows:
- an optical microscope or a scanning electron microscope can be used to assist in determining the position of the boundary between the first negative electrode film layer and the second negative electrode film layer.
- the negative electrode film layer can be provided on one surface of the negative electrode current collector, or can be provided on both surfaces of the negative electrode current collector at the same time.
- FIG. 2 shows a schematic diagram of an embodiment of the negative pole piece 10 of the present application.
- the negative electrode piece 10 is composed of a negative electrode current collector 101, a first negative electrode film layer 103 respectively disposed on both surfaces of the negative electrode current collector, and a second negative electrode film layer 102 disposed on the first negative electrode film layer 103.
- FIG. 3 shows a schematic diagram of another embodiment of the negative pole piece 10 of the present application.
- the negative electrode piece 10 is composed of a negative electrode current collector 101, a first negative electrode film layer 103 disposed on one surface of the negative electrode current collector, and a second negative electrode film layer 102 disposed on the first negative electrode film layer 103.
- each negative electrode film layer (such as film thickness, areal density, compaction density, etc.) given in this application all refer to the parameter range of a single-sided film layer.
- the film layer parameters on any one of the surfaces meet the requirements of the present application, which is considered to fall within the protection scope of the present application.
- the ranges of film thickness, areal density and the like mentioned in this application all refer to the film parameters after being compacted by cold pressing and used for assembling the battery.
- the negative electrode current collector can be a conventional metal foil or a composite current collector (a metal material can be arranged on a polymer substrate to form a composite current collector).
- a metal material can be arranged on a polymer substrate to form a composite current collector.
- copper foil may be used as the negative electrode current collector.
- the first negative electrode film layer and/or the second negative electrode film layer usually include a negative electrode active material, an optional binder, an optional conductive agent, and other optional auxiliary agents, It is usually formed by coating and drying the negative electrode film slurry.
- the negative electrode film slurry coating is usually formed by dispersing the negative electrode active material and optional conductive agent and binder in a solvent and stirring uniformly.
- the solvent can be N-methylpyrrolidone (NMP) or deionized water, for example.
- Other optional additives can be, for example, thickening and dispersing agents (such as sodium carboxymethyl cellulose CMC-Na), PTC thermistor materials, and the like.
- the conductive agent may include one or more of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
- the binder may include styrene-butadiene rubber (SBR), water-based acrylic resin, polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), ethylene-vinyl acetate copolymer One or more of (EVA), polyvinyl alcohol (PVA) and polyvinyl butyral (PVB).
- SBR styrene-butadiene rubber
- PVDF polyvinylidene fluoride
- PTFE polytetrafluoroethylene
- EVA ethylene-vinyl acetate copolymer
- EVA polyvinyl alcohol
- PVB polyvinyl butyral
- the first negative electrode active material and/or the second negative electrode active material may optionally include a certain amount of other commonly used negative electrode active materials in addition to the aforementioned negative electrode active material of the present application, For example, one or more of soft carbon, hard carbon, silicon-based material, tin-based material, and lithium titanate.
- the silicon-based material can be selected from one or more of elemental silicon, silicon-oxygen compounds, silicon-carbon composites, and silicon alloys.
- the tin-based material can be selected from one or more of elemental tin, tin oxide compounds, and tin alloys. The preparation methods of these materials are well known and can be obtained commercially. Those skilled in the art can make an appropriate choice according to the actual use environment.
- the negative electrode sheet does not exclude other additional functional layers in addition to the above-mentioned negative electrode film layer.
- the negative pole piece of the present application may further include a conductive coating (for example, composed of a conductive agent and a binder) disposed between the negative current collector and the first film layer.
- the negative pole piece of the present application may further include a protective layer provided on the surface of the second film layer.
- the positive electrode sheet includes a positive electrode current collector and a positive electrode film layer provided on at least one surface of the positive electrode current collector and including a positive electrode active material.
- the positive electrode current collector has two opposite surfaces in its thickness direction, and the positive electrode film layer may be laminated on either or both of the two opposite surfaces of the positive electrode current collector.
- the positive electrode current collector can be a conventional metal foil or a composite current collector (a metal material can be arranged on a polymer substrate to form a composite current collector).
- a metal material can be arranged on a polymer substrate to form a composite current collector.
- aluminum foil may be used as the positive electrode current collector.
- the positive active material may be a positive active material for secondary batteries that is well known in the art.
- the positive electrode active material may include one or more of lithium transition metal oxides, lithium-containing phosphates with an olivine structure, and their respective modified compounds.
- lithium transition metal oxides may include, but are not limited to, lithium cobalt oxide, lithium nickel oxide, lithium manganese oxide, lithium nickel cobalt oxide, lithium manganese cobalt oxide, lithium nickel manganese oxide, lithium nickel cobalt manganese oxide
- lithium-containing phosphates with an olivine structure may include, but are not limited to, lithium iron phosphate, lithium iron phosphate and carbon composite material, lithium manganese phosphate, lithium manganese phosphate and carbon composite material, lithium iron manganese phosphate, lithium iron manganese phosphate
- One or more of the composite materials with carbon and its modified compounds may be used. The present application is not limited to these materials, and other conventionally known materials that can be used as positive electrode active materials for secondary batteries can also be used.
- the positive electrode active material may include one or more of the lithium transition metal oxide and its modified compounds shown in Formula 1.
- M is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn 0.5 ⁇ b ⁇ 1, 0 ⁇ c ⁇ 1, 0 ⁇ d ⁇ 1, 1 ⁇ e ⁇ 2, 0 ⁇ f ⁇ 1, M is selected from Mn, Al, Zr
- Zn is selected from Mn, Al, Zr
- Zn is selected from Cu, Cr, Mg, Fe, V, Ti and B
- A is selected from one or more of N, F, S and Cl.
- the modification compound of each of the above-mentioned materials may be doping modification and/or surface coating modification of the material.
- the positive electrode film layer may optionally include a binder and a conductive agent.
- the binder used for the positive electrode film layer may include one or more of polyvinylidene fluoride (PVDF) and polytetrafluoroethylene (PTFE).
- PVDF polyvinylidene fluoride
- PTFE polytetrafluoroethylene
- the conductive agent used for the positive electrode film layer may include one or more of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
- the electrolyte conducts ions between the positive pole piece and the negative pole piece.
- the type of electrolyte in this application can be selected according to requirements.
- the electrolyte may be selected from at least one of solid electrolytes and liquid electrolytes (ie, electrolytes).
- an electrolyte is used as the electrolyte.
- the electrolyte includes electrolyte salt and solvent.
- the electrolyte salt can be selected from LiPF 6 (lithium hexafluorophosphate), LiBF 4 (lithium tetrafluoroborate), LiClO 4 (lithium perchlorate), LiAsF 6 (lithium hexafluoroarsenate), LiFSI (bisfluorosulfonate) Lithium imide), LiTFSI (lithium bistrifluoromethanesulfonimide), LiTFS (lithium trifluoromethanesulfonate), LiDFOB (lithium difluorooxalate), LiBOB (lithium bisoxalate), LiPO 2 F 2 (Lithium difluorophosphate), LiDFOP (lithium difluorodioxalate phosphate) and LiTFOP (lithium tetrafluorooxalate phosphate) one or more.
- LiPF 6 lithium hexafluorophosphate
- LiBF 4 lithium tetrafluoroborate
- the solvent may be selected from ethylene carbonate (EC), propylene carbonate (PC), ethyl methyl carbonate (EMC), diethyl carbonate (DEC), dimethyl carbonate (DMC), Dipropyl carbonate (DPC), methyl propyl carbonate (MPC), ethylene propyl carbonate (EPC), butylene carbonate (BC), fluoroethylene carbonate (FEC), methyl formate (MF), methyl acetate Ester (MA), ethyl acetate (EA), propyl acetate (PA), methyl propionate (MP), ethyl propionate (EP), propyl propionate (PP), methyl butyrate (MB) , Ethyl butyrate (EB), 1,4-butyrolactone (GBL), sulfolane (SF), dimethyl sulfone (MSM), methyl ethyl sulfone (EMS) and diethyl sulfone (ESE) one
- the electrolyte may also optionally include additives.
- the additives can include negative electrode film-forming additives, positive electrode film-forming additives, and additives that can improve certain battery performance, such as additives that improve battery overcharge performance, additives that improve battery high-temperature performance, and battery low-temperature performance. Additives, etc.
- isolation film is arranged between the positive pole piece and the negative pole piece to play a role of isolation.
- isolation membrane there is no particular limitation on the type of isolation membrane in this application, and any well-known porous structure isolation membrane with good chemical stability and mechanical stability can be selected.
- the material of the isolation membrane can be selected from one or more of glass fiber, non-woven fabric, polyethylene, polypropylene, and polyvinylidene fluoride.
- the isolation film can be a single-layer film or a multilayer composite film. When the isolation film is a multilayer composite film, the materials of each layer can be the same or different.
- the positive pole piece, the negative pole piece, and the separator can be made into an electrode assembly through a winding process or a lamination process.
- the secondary battery may include an outer package.
- the outer packaging can be used to encapsulate the above-mentioned electrode assembly and electrolyte.
- the outer packaging of the secondary battery may be a hard case, such as a hard plastic case, aluminum case, steel case, or the like.
- the outer packaging of the secondary battery may also be a soft bag, such as a pouch type soft bag.
- the material of the soft bag can be plastic, such as one or more of polypropylene (PP), polybutylene terephthalate (PBT), polybutylene succinate (PBS), and the like.
- FIG. 1 shows a secondary battery 5 of a square structure as an example.
- the outer package may include a housing 51 and a cover 53.
- the housing 51 may include a bottom plate and a side plate connected to the bottom plate, and the bottom plate and the side plate enclose a receiving cavity.
- the housing 51 has an opening communicating with the containing cavity, and the cover plate 53 is used to cover the opening to close the containing cavity.
- the positive pole piece, the negative pole piece, and the separator may be formed into the electrode assembly 52 through a winding process or a lamination process.
- the electrode assembly 52 is packaged in the receiving cavity.
- the electrolyte is infiltrated in the electrode assembly 52.
- the number of electrode assemblies 52 included in the secondary battery 5 can be one or several, which can be adjusted according to requirements.
- the secondary battery can be assembled into a battery module, and the number of secondary batteries contained in the battery module can be multiple, and the specific number can be adjusted according to the application and capacity of the battery module.
- Fig. 5 is a battery module 4 as an example.
- a plurality of secondary batteries 5 may be arranged in sequence along the length direction of the battery module 4. Of course, it can also be arranged in any other manner. Furthermore, the plurality of secondary batteries 5 can be fixed by fasteners.
- the battery module 4 may further include a housing having an accommodating space, and a plurality of secondary batteries 5 are accommodated in the accommodating space.
- the above-mentioned battery modules can also be assembled into a battery pack, and the number of battery modules contained in the battery pack can be adjusted according to the application and capacity of the battery pack.
- the battery pack 1 may include a battery box and a plurality of battery modules 4 provided in the battery box.
- the battery box includes an upper box body 2 and a lower box body 3.
- the upper box body 2 is used to cover the lower box body 3 and form a closed space for accommodating the battery module 4.
- a plurality of battery modules 4 can be arranged in the battery box in any manner.
- the second aspect of the present application provides a method for preparing a secondary battery, which includes preparing the negative pole piece of the secondary battery through the following steps:
- first negative electrode active material and the second negative electrode active material both include artificial graphite; the first negative electrode active material includes primary particles, and the number of the primary particles in the first negative electrode active material accounts for A ⁇ 50%.
- the first negative electrode film layer and the second negative electrode film layer can be coated simultaneously, or they can be applied in two separate steps; preferably, the first negative electrode film layer and the second negative electrode film layer are simultaneously coated. Coating. Coating at the same time can make the adhesion between the upper and lower negative film layers better, which helps to further improve the cycle performance of the battery.
- the positive pole piece of the present application can be prepared as follows: the positive electrode active material, optional conductive agent (such as carbon black and other carbon materials), binder (such as PVDF), etc. are mixed and dispersed in a solvent (such as NMP) In the process, after stirring, it is coated on the positive electrode current collector, and the positive electrode piece is obtained after drying. Materials such as metal foil such as aluminum foil or porous metal plate can be used as the positive electrode current collector.
- the positive electrode tab can be obtained by punching or laser die cutting in the uncoated area of the positive electrode current collector.
- the positive pole piece, the separator film, and the negative pole piece stack the positive pole piece, the separator film, and the negative pole piece in order, so that the separator film is located between the positive and negative pole pieces for isolation, and then use the winding (or lamination) process to form the electrode assembly;
- the electrode assembly is placed in the outer package, and the electrolyte is injected after drying, and the secondary battery is obtained through the processes of vacuum packaging, standing, forming, and shaping.
- the third aspect of the present application provides a device.
- the device includes the secondary battery of the first aspect of the present application or the secondary battery prepared by the method of the second aspect of the present application.
- the secondary battery can be used as a power source of the device, and can also be used as an energy storage unit of the device.
- the device of the present application uses the secondary battery provided by the present application, and therefore has at least the same advantages as the secondary battery.
- the device can be, but is not limited to, mobile devices (such as mobile phones, laptop computers, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf Vehicles, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc.
- mobile devices such as mobile phones, laptop computers, etc.
- electric vehicles such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf Vehicles, electric trucks, etc.
- electric trains ships and satellites, energy storage systems, etc.
- the device can select a secondary battery, a battery module, or a battery pack according to its usage requirements.
- Fig. 8 is a device as an example.
- the device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle, etc.
- a battery pack or a battery module can be used.
- the device may be a mobile phone, a tablet computer, a notebook computer, and the like.
- the device is generally required to be thin and light, and a secondary battery can be used as a power source.
- the positive electrode active material LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811), the conductive carbon black Super-P, and the binder polyvinylidene fluoride (PVDF) in a weight ratio of 96.8:1:2.2 in N-methylpyrrolidone solvent After fully stirring and mixing uniformly, the slurry is coated on the aluminum foil substrate, and the positive pole piece is obtained by drying, cold pressing, slitting, and cutting. Among them, the areal density of the positive electrode film layer is 17.3 mg/cm 2 , and the compaction density is 3.5 g/cm 3 .
- the first step is to prepare negative electrode slurry 1: the first negative electrode active material, binder (SBR), thickener (CMC-Na) and conductive carbon black (Super-P) are adjusted according to 96.2:1.8:1.2:0.8 The weight ratio is fully stirred and mixed in an appropriate amount of deionized water to prepare negative electrode slurry 1. Among them, the number of primary particles in the first negative electrode active material accounts for 50% of A.
- the second step is to prepare the negative electrode slurry 2:
- the second negative electrode active material, the binder SBR, the thickener (CMC-Na) and the conductive carbon black (Super-P) are weighed by 96.2:1.8:1.2:0.8 Stir and mix thoroughly in an appropriate amount of deionized water to prepare negative electrode slurry 2.
- the number of secondary particles in the second negative electrode active material accounts for 95% of the proportion B.
- the negative electrode slurry 1 and the negative electrode slurry 2 are simultaneously extruded through a dual-cavity coating device.
- the negative electrode slurry 1 is coated on the current collector to form a first negative electrode film layer
- the negative electrode slurry 2 is coated on the first negative electrode film layer to form a second negative electrode film layer.
- the areal density of the negative electrode film layer is 11.0 mg/cm 2
- the compacted density is 1.65 g/cm 3 .
- the coated wet film is baked in an oven through different temperature zones to obtain dry pole pieces, and then cold-pressed to obtain the required negative electrode film layer, and then to obtain negative pole pieces through processes such as slitting and cutting.
- EC ethylene carbonate
- EMC ethyl methyl carbonate
- DEC diethyl carbonate
- the secondary batteries of Examples 2 to 35 and Comparative Examples 1 to 3 are similar to the preparation method of the secondary battery of Example 1, but the composition and product parameters of the negative electrode are adjusted. The different product parameters are shown in Table 1 to Table 3. .
- the batteries of the examples and comparative examples were charged and discharged for the first time with a current of 1C (that is, the current value of completely discharging the theoretical capacity within 1h), and the charging was constant current and constant voltage charging, and the termination voltage was 4.2 V, the cut-off current is 0.05C, the discharge end voltage is 2.8V, and its theoretical capacity is recorded as C0; then the battery is constant at 0.5C0, 1C0, 1.5C0, 2C0, 2.5C0, 3C0, 3.5C0, 4C0, 4.5C0 Charge to 4.2V full power cut-off voltage or 0V negative cut-off potential.
- 1C that is, the current value of completely discharging the theoretical capacity within 1h
- the charging window is denoted as C 10% SOC , C 20% SOC , C 30% SOC , C 40% SOC , C 50% SOC , C 60% SOC , C 70% SOC , C 80% SOC , according to the formula (60 /C 20%SOC +60/C 30%SOC +60/C 40%SOC +60/C 50%SOC +60/C 60%SOC +60/C 70%SOC +60/C 80%SOC )*10 % Calculates the charging time T of the battery from 10% to 80% SOC. The shorter the time, the better the fast charging performance of the battery.
- the batteries of the examples and comparative examples were charged and discharged for the first time with a current of 1C.
- the charging was constant current and constant voltage charging with a termination voltage of 4.2V, a cut-off current of 0.05C, and a discharge termination voltage of 2.8 V, record the discharge capacity Cb of the battery cell during the first cycle.
- the test condition is 1C/1C cycle at room temperature (25°C).
- the discharge capacity Ce of the cell is recorded at any time.
- the ratio of Ce to Cb is the cycle capacity retention rate, and the cycle capacity retention rate is equal to 80 Stop the test at% and record the number of cycles.
- the batteries of each embodiment and comparative example were prepared according to the above methods, and various performance parameters were measured. The results are shown in Table 1 to Table 3 below.
- Example 5 and Examples 8-13 also reflect that: both the first negative electrode active material and the second negative electrode active material include artificial graphite, and the ratio of the number of primary particles in the first negative electrode active material A ⁇ 50 %, the number of secondary particles in the second negative electrode active material, B, also has a certain impact on the performance of the battery; especially when B ⁇ 30%, the fast charge performance and cycle performance of the battery can be greatly improved.
- Example 14 the Dv10 of the first negative electrode active material was too small, which would block the pores of the first negative electrode film layer, resulting in deterioration of fast charging performance; in Example 20, the Dv10 of the first negative electrode active material was too large, which would affect Energy density, in order to ensure the same energy density design, can only increase the compaction, reduce the porosity, so that the fast charging performance is reduced, and may further lead to particle breakage and deterioration of cycle performance.
- Example 21 the Dv10 of the second negative electrode active material was too small, which would block the pores of the second negative electrode film layer and be difficult to compact, resulting in deterioration of fast charging performance and cycle performance; while in Example 23, the second negative electrode active material If the Dv10 is too large, it will affect the electronic conductance and charge exchange resistance, and then affect the fast charging performance.
- Example 24 when the Dv10 of the first negative electrode active material is greater than the Dv10 of the second negative electrode active material, the lower negative electrode film layer is more difficult to compress.
- the experimental data of Examples 25 to 35 in Table 3 further reflect the influence of the tap density of the negative electrode active material on the battery performance.
- the lower the tap density of the first negative electrode film the lower the energy density. Therefore, when the tap density of the first negative electrode film is too small (for example, Example 25), in order to ensure the same energy density design, it can only be increased Compaction, which causes a decrease in porosity, a decline in fast charging performance, and may cause particle breakage and deterioration of cycle performance.
- the greater the tap density of the first negative electrode film the denser the filling. Therefore, when the tap density of the first negative electrode film is too large (for example, Example 31), the porosity of the first negative electrode film will be low.
- the tap density of the second negative electrode film layer is too small (such as Example 32), it is difficult to compact. In order to ensure the same energy density design, the compaction can only be increased, which will reduce the porosity and decrease the fast charging performance. It further causes the particles to be broken and the cycle performance deteriorates.
- the tap density of the second negative electrode film layer is too large (such as Example 34), the filling is too dense, and the porosity of the second negative electrode film layer is low, which affects the fast charging performance, and the kinetics of the late cycle performance is insufficient, and the battery decays quickly. .
- Example 35 when the tap density of the second negative electrode film layer is greater than the tap density of the first negative electrode film layer, the second negative electrode film layer is filled more densely, which will affect the fast charging performance and cause particle breakage. Cycle performance.
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Abstract
Description
Claims (15)
- 一种二次电池,包括负极极片,所述负极极片包括负极集流体及负极膜层,所述负极膜层包括第一负极膜层和第二负极膜层,所述第一负极膜层设置在负极集流体至少一个表面上且包括第一负极活性材料,所述第二负极膜层设置在第一负极膜层上且包括第二负极活性材料;所述第一负极活性材料和所述第二负极活性材料均包括人造石墨;所述第一负极活性材料中包括一次颗粒,且所述一次颗粒在所述第一负极活性材料中的数量占比A满足:A≥50%。
- 根据权利要求1所述的二次电池,其中,A≥70%;优选地,80%≤A≤100%。
- 根据权利要求1~2任一项所述的二次电池,其中,所述第二负极活性材料中包括二次颗粒,且所述二次颗粒在所述第二负极活性材料中的数量占比B满足:B≥30%;优选地,B≥50%。
- 根据权利要求1~3任一项所述的二次电池,其中,所述第一负极活性材料的体积分布粒径D V10小于第二负极活性材料的体积分布粒径D V10。
- 根据权利要求1~4任一项所述的二次电池,其中,所述第一负极活性材料的体积分布粒径D V10为3μm~8μm,优选为4μm~7μm;和/或,所述第二负极活性材料的体积分布粒径D V10为5μm~11μm,优选为6μm~10μm。
- 根据权利要求1~5任一项所述的二次电池,其中,所述第一负极活性材料的振实密度大于所述第二负极活性材料的振实密度。
- 根据权利要求1~6任一项所述的二次电池,其中,所述第一负极活性材料的振实密度为0.8g/cm 3~1.3g/cm 3,优选为0.95g/cm 3~1.15g/cm 3;和/或,所述第二负极活性材料的振实密度为0.7g/cm 3~1.2g/cm 3,优选为0.85g/cm 3~1.05g/cm 3。
- 根据权利要求1~7任一项所述的二次电池,其中,所述第一负极活性材料的体积分布粒径D V50大于第二负极活性材料的体积分布粒径D V50。
- 根据权利要求1~8任一项所述的二次电池,其中,所述第一负极活性材料的体积分布粒径D V50为13μm~21μm,优选为15μm~19μm;和/或,所述第二负极活性材料的体积分布粒径D V50为11μm~19μm,优选为13μm~17μm。
- 根据权利要求1~9任一项所述的二次电池,其中,所述第一负极活性材料的石墨化度大于第二负极活性材料的石墨化度。
- 根据权利要求1~10任一项所述的二次电池,其中,所述第一负极活性材料的石墨化度为92%~97%,优选为93%~96%;和/或,所述第二负极活性材料的石墨化度为90%~95%,优选为92%~94%。
- 根据权利要求1~11任一项所述的二次电池,其中,所述第一负极活性材料的比表面积(SSA)为1.6m 2/g~2.6m 2/g,优选为1.8m 2/g~2.3m 2/g;和/或,所述第二负极活性材料的比表面积(SSA)为0.7m 2/g~1.5m 2/g,优选为0.8m 2/g~1.3m 2/g。
- 根据权利要求1~12任一项所述的二次电池,其中,所述第一负极活性材料中人造石墨的质量占比≥50%,优选为60%~100%;和/或,所述第二负极活性材料中人造石墨的质量占比≥80%,优选为90%~100%。
- 一种二次电池的制备方法,包括通过如下步骤制备所述二次电池的负极极片:1)在负极集流体至少一个表面上形成包括第一负极活性材料的第一负极膜层;2)在所述第一负极膜层上形成包括第二负极活性材料的第二负极膜层;其中,所述第一负极活性材料和所述第二负极活性材料均包括人造石墨;所述第一负极活性材料中包括一次颗粒,且所述一次颗粒在第一负极活性材料中的数量占比A≥50%。
- 一种装置,其特征在于,包括根据权利要求1~13任一项所述的二次电池或根据权利要求14所述方法制备的二次电池。
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JP2022532139A JP7496872B2 (ja) | 2020-04-30 | 2020-04-30 | 二次電池及びその調製方法、当該二次電池を含む装置 |
CN202080006114.0A CN113875047B (zh) | 2020-04-30 | 2020-04-30 | 二次电池及其制备方法、含有该二次电池的装置 |
ES20933636T ES2953953T3 (es) | 2020-04-30 | 2020-04-30 | Batería secundaria, proceso de preparación de la misma y aparato que contiene la batería secundaria |
KR1020227018610A KR102599823B1 (ko) | 2020-04-30 | 2020-04-30 | 이차 전지, 그 제조 방법 및 이차 전지를 포함하는 장치 |
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EP20933636.1A EP3958353B1 (en) | 2020-04-30 | 2020-04-30 | Secondary battery, process for preparing the same and apparatus containing the secondary battery |
PCT/CN2020/088300 WO2021217586A1 (zh) | 2020-04-30 | 2020-04-30 | 二次电池及其制备方法、含有该二次电池的装置 |
HUE20933636A HUE062604T2 (hu) | 2020-04-30 | 2020-04-30 | Másodlagos akkumulátor, eljárás annak elõállítására és másodlagos akkumulátort tartalmazó berendezés |
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CN113875047A (zh) | 2021-12-31 |
US20220102701A1 (en) | 2022-03-31 |
PL3958353T3 (pl) | 2023-10-23 |
CN113875047B (zh) | 2023-11-21 |
EP3958353A4 (en) | 2022-07-13 |
EP3958353A1 (en) | 2022-02-23 |
JP7496872B2 (ja) | 2024-06-07 |
JP2023504473A (ja) | 2023-02-03 |
KR20220097940A (ko) | 2022-07-08 |
US11901546B2 (en) | 2024-02-13 |
KR102599823B1 (ko) | 2023-11-07 |
ES2953953T3 (es) | 2023-11-17 |
EP3958353B1 (en) | 2023-06-28 |
HUE062604T2 (hu) | 2023-11-28 |
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