WO2023134340A1 - Matériau actif d'électrode négative, plaque d'électrode négative, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique associé - Google Patents

Matériau actif d'électrode négative, plaque d'électrode négative, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique associé Download PDF

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WO2023134340A1
WO2023134340A1 PCT/CN2022/137551 CN2022137551W WO2023134340A1 WO 2023134340 A1 WO2023134340 A1 WO 2023134340A1 CN 2022137551 W CN2022137551 W CN 2022137551W WO 2023134340 A1 WO2023134340 A1 WO 2023134340A1
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negative electrode
graphite
hard carbon
active material
electrode active
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PCT/CN2022/137551
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English (en)
Chinese (zh)
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范国凌
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宁德时代新能源科技股份有限公司
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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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/139—Processes of manufacture
    • H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • 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
    • 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

Definitions

  • the present application relates to the technical field of batteries, in particular to a negative electrode active material, a negative electrode sheet, a secondary battery, a battery module, a battery pack and an electrical device thereof.
  • the present application is made in view of the above problems, and its purpose is to provide a negative electrode active material, a negative electrode sheet, a secondary battery, a battery module, a battery pack and an electrical device thereof with good fast charging performance.
  • the first aspect of the present application provides a negative electrode active material
  • the negative electrode active material includes graphite and hard carbon
  • the average sphericity of the graphite is 0.1 ⁇ A ⁇ 0.7
  • the average sphericity of the hard carbon is 0.7 ⁇ B ⁇ 1 , and 0.1 ⁇ B-A ⁇ 0.8.
  • hard carbon is selected as a component of the negative electrode active material.
  • hard carbon compared with traditional artificial graphite and natural graphite, hard carbon also has a large number of microporous structures, which can provide a large number of lithium ion channels and additional lithium storage space, making it have a faster lithium storage speed and Higher lithium storage capacity; on the other hand, hard carbon is hard to be compressed, which can also make it play the role of a skeleton in the pole piece, uniformly disperse the stress generated by graphite, and can better reduce the volume expansion of the pole piece .
  • the special structure of hard carbon also makes it difficult to be compressed, and the negative electrode sheet made of it alone has a low compaction density, which cannot meet the energy density requirements of secondary batteries. Therefore, the present invention mixes graphite and hard carbon together as the negative electrode active material, which can increase the charging speed of the secondary battery while meeting the energy density requirement of the secondary battery.
  • the combination of hard carbon with high average sphericity and graphite with low average sphericity can be equivalently considered as a circle of graphite around each hard carbon particle.
  • the peripheral graphite particles and the central hard carbon particles intercalate lithium together.
  • the characteristics of fast lithium intercalation and high capacity of hard carbon enable it to buffer and shunt lithium ions for the surrounding graphite particles.
  • the high sphericity of hard carbon particles can make the diffusion paths of lithium ions in all directions similar, thereby ensuring The uniformity of lithium intercalation prevents some areas of hard carbon particles from high lithium intercalation, rapid saturation and loss of buffering capacity, resulting in electrochemical polarization of graphite particles and even lithium precipitation. Therefore, the present application further improves the fast charging performance of the secondary battery by selecting hard carbon with a high average sphericity and graphite with a low average sphericity to match.
  • the average sphericity difference between hard carbon particles and graphite particles should not be too small.
  • it can prevent graphite and hard carbon from being independent when they are mixed, and the particle spacing is large.
  • graphite can be formed to surround hard carbon. structure, thereby ensuring the fast charging performance of the secondary battery.
  • the peak intensity I D1 of the D peak and the peak intensity I G1 of the G peak satisfy 0.4 ⁇ I D1 /I G1 ⁇ 2; and/or, the hardness In the Raman spectrum of carbon, the relationship between the peak intensity I D2 of the D peak and the peak intensity I G2 of the G peak satisfies 1 ⁇ I D2 /I G2 ⁇ 2.
  • the present application can ensure that graphite and hard carbon have relatively large defects by selecting graphite and hard carbon within the appropriate range of D peak and G peak intensity ratios. These defects can provide ion channels and make the material conduct ions faster, thereby Guarantee the fast charging performance of the secondary battery.
  • the peak intensities ID1 and ID2 of the D peak and the peak intensities I G1 and I G2 of the G peak satisfy ID1 /I G1 ⁇ I D2 /I G2 .
  • the ratio of the graphite D peak and G peak intensity of the selected graphite in the present application is larger than that of hard carbon, that is, compared with the selected graphite, the selected hard carbon has larger surface defects, which can ensure that the hard carbon has a faster Lithium intercalation speed and higher lithium storage capacity, and then during the charging process, it can buffer and shunt the surrounding graphite particles to store lithium ions, so as to further improve the fast charging performance of the secondary battery.
  • the smaller the OI value the smaller the direction selectivity of graphite in the lithium intercalation process, which is conducive to the diffusion of lithium intercalation expansion, so that the expansion generated by the lithium intercalation process is dispersed in all directions. Therefore, the present application can reduce the cyclic expansion of the negative electrode sheet by selecting graphite within a suitable OI value range.
  • the graphite has a volume average particle diameter Dv50 of 3 ⁇ m to 30 ⁇ m; and/or, the hard carbon has a volume average particle diameter Dv50 of 3 ⁇ m to 9 ⁇ m.
  • the present application can shorten the short diffusion path of graphite particles and hard carbon particles from the core to the surface by controlling the average volume particle diameter Dv50 of the graphite and the hard carbon within an appropriate range, thereby ensuring that lithium ions pass from the outside to the inside.
  • the short transmission time can increase the lithium intercalation speed of the negative electrode active material and improve the fast charging performance of the secondary battery.
  • the mass percentage of the hard carbon is 1% to 99%, optionally 10% to 70%, and further optionally, the hard carbon The mass percentage is 10% to 50%.
  • the mass percentage of the hard carbon is not higher than the mass percentage of the graphite.
  • the mass percentage of the hard carbon and the graphite in an appropriate range in the present application, it is possible to prevent the poor rate performance caused by too low a hard carbon ratio, and to improve the fast charging performance of the secondary battery.
  • the second aspect of the present application provides a negative electrode sheet, the negative electrode sheet contains the negative electrode active material according to the first aspect of the present application. Compared with other negative pole pieces, the negative pole piece of the present application has excellent fast charging performance.
  • the negative electrode sheet has a compacted density of 1.00 g/cm 3 to 1.80 g/cm 3 . Therefore, the present application can meet the capacity requirement of the secondary battery by controlling the compacted density of the negative electrode sheet within an appropriate range.
  • a third aspect of the present application provides a secondary battery, which includes the negative electrode sheet of the second aspect of the present application.
  • the secondary battery has excellent fast charging performance.
  • a fourth aspect of the present application provides a battery module including the secondary battery of the third aspect of the present application.
  • the battery module has excellent fast charging performance.
  • a fifth aspect of the present application provides a battery pack, which includes the battery module of the fourth aspect of the present application.
  • the battery pack has excellent fast charging performance.
  • an electric device comprising at least one of the secondary battery of the third aspect of the present application, the battery module of the fourth aspect of the present application, or the battery pack of the fifth aspect of the present application.
  • the electric device has excellent fast charging performance.
  • the present application provides a negative electrode active material.
  • the negative electrode active material selects hard carbon with a high average sphericity and graphite with a low average sphericity, which can be equivalently regarded as a ring of graphite around each hard carbon particle.
  • the peripheral graphite particles and the central hard carbon particles intercalate lithium together.
  • the characteristics of fast lithium intercalation and high capacity of hard carbon enable it to buffer and shunt lithium ions for the surrounding graphite particles.
  • the negative electrode sheet comprising the above-mentioned negative electrode active material of the present application has excellent fast charging performance.
  • the present application provides a secondary battery, a battery module, a battery pack, and an electrical device including the negative electrode sheet.
  • the secondary battery, battery module, battery pack and electrical device also have excellent fast charging performance.
  • FIG. 1 is a schematic diagram of a lithium intercalation process according to an embodiment of the present application.
  • FIG. 2 is a scanning electron microscope (SEM) image of an anode active material according to an embodiment of the present application.
  • FIG. 3 is a schematic diagram of a secondary battery according to an embodiment of the present application.
  • FIG. 4 is an exploded view of the secondary battery according to one embodiment of the present application shown in FIG. 3 .
  • FIG. 5 is a schematic diagram of a battery module according to an embodiment of the present application.
  • FIG. 6 is a schematic diagram of a battery pack according to an embodiment of the present application.
  • Fig. 7 is an exploded view of the battery pack according to one embodiment of the present application shown in Fig. 6 .
  • FIG. 8 is a schematic diagram of an electrical device in which a secondary battery is used as a power source according to an embodiment of the present application.
  • ranges disclosed herein are defined in terms of lower and upper limits, and a given range is defined by selecting a lower limit and an upper limit that define the boundaries of the particular range. Ranges defined in this manner may be inclusive or exclusive and may be combined arbitrarily, ie any lower limit may be combined with any upper limit to form a range. For example, if ranges of 60-120 and 80-110 are listed for a particular parameter, it is understood that ranges of 60-110 and 80-120 are contemplated. Additionally, if the minimum range values 1 and 2 are listed, and if the maximum range values 3, 4, and 5 are listed, the following ranges are all expected: 1-3, 1-4, 1-5, 2- 3, 2-4 and 2-5.
  • the numerical range "a-b” represents an abbreviated representation of any combination of real numbers between a and b, where a and b are both real numbers.
  • the numerical range "0-5" indicates that all real numbers between "0-5" have been listed in this article, and "0-5" is only an abbreviated representation of the combination of these values.
  • a certain parameter is an integer ⁇ 2
  • the method includes steps (a) and (b), which means that the method may include steps (a) and (b) performed in sequence, and may also include steps (b) and (a) performed in sequence.
  • steps (c) means that step (c) may be added to the method in any order, for example, the method may include steps (a), (b) and (c) , may also include steps (a), (c) and (b), may also include steps (c), (a) and (b) and so on.
  • the “comprising” and “comprising” mentioned in this application mean open or closed.
  • the “comprising” and “comprising” may mean that other components not listed may be included or included, or only listed components may be included or included.
  • the term "or” is inclusive unless otherwise stated.
  • the phrase "A or B” means “A, B, or both A and B.” More specifically, the condition "A or B” is satisfied by either of the following: A is true (or exists) and B is false (or does not exist); A is false (or does not exist) and B is true (or exists) ; or both A and B are true (or exist).
  • the inventors of the present application can make the secondary battery containing the material have good fast charging performance.
  • the negative electrode active material of the present application and the negative electrode sheet, secondary battery, battery module, battery pack and electrical device containing the same will be described in detail below.
  • the first embodiment of the present application can provide a negative electrode active material, characterized in that the negative electrode active material includes graphite and hard carbon, the average sphericity of the graphite is 0.1 ⁇ A ⁇ 0.7, and the average sphericity of the hard carbon is Degree 0.7 ⁇ B ⁇ 1, and 0.1 ⁇ B-A ⁇ 0.8.
  • 0.1 ⁇ B-A ⁇ 0.4 0.1 ⁇ B-A ⁇ 0.5, 0.1 ⁇ B-A ⁇ 0.6, 0.4 ⁇ B-A ⁇ 0.5, 0.4 ⁇ B-A ⁇ 0.6, 0.4 ⁇ B-A ⁇ 0.8, 0.5 ⁇ B-A ⁇ 0.6, 0.5 ⁇ B-A ⁇ 0.8 or 0.6 ⁇ B-A ⁇ 0.8.
  • sphericity refers to the ratio of the smallest diameter to the largest diameter of a particle. The closer to a spherical particle in shape, the closer its sphericity is to 1.
  • the average sphericity refers to the average sphericity of graphite or hard carbon in the negative electrode active material.
  • the average sphericity of graphite and hard carbon can be tested by methods known in the art.
  • Malvern's Morphologi G3-ID instrument and its supporting graphics software and Raman accessories can be used for characterization.
  • Morphologi G3-ID can be used to capture and process images of a certain number of dispersed particles, accurately analyze the microstructure and shape of particles, obtain the longest diameter and shortest diameter of all particles, and calculate each The ratio of the shortest diameter to the longest diameter of the particle, so as to obtain the sphericity of each particle, and take the average value of the sphericity of all particles, that is, to obtain the average sphericity of graphite and hard carbon.
  • Malvern Morphologi G3-ID can be used to capture and process images of a certain number of dispersed particles to obtain the longest and shortest diameters of all particles, and calculate the shortest and longest diameters of each particle The ratio of the sphericity of each particle is obtained, and the composition of each particle is confirmed by Raman spectroscopy, the graphite and hard carbon particles are classified, and the sphericity of the two is calculated separately, that is, the average sphericity of graphite and hard carbon is obtained.
  • both hard carbon and graphite have a certain rigidity, and the sphericity will not change during the mixing process of the present application, and the sphericity can be kept consistent before and after mixing.
  • hard carbon is selected as a component of the negative electrode active material.
  • hard carbon compared with traditional artificial graphite and natural graphite, hard carbon also has a large number of microporous structures, which can provide a large number of lithium ion channels and additional lithium storage space, so that it has a faster storage capacity. Lithium speed and higher lithium storage capacity.
  • the volume of hard carbon basically remains unchanged after storing lithium, and its characteristics of being difficult to be compressed can also make it play the role of a skeleton in the pole piece, uniformly disperse the stress generated by graphite, and can better reduce the stress of the pole piece. Volume expansion.
  • the special structure of hard carbon also makes it difficult to be compressed, and the negative electrode sheet made of it alone has a low compaction density, which cannot meet the energy density requirements of secondary batteries. Therefore, the present invention mixes graphite and hard carbon together as the negative electrode active material, which can increase the charging speed of the secondary battery while meeting the energy density requirement of the secondary battery.
  • the combination of hard carbon with high average sphericity and graphite with low average sphericity can be equivalently regarded as a circle of graphite around each hard carbon particle.
  • the peripheral graphite particles and the central hard carbon particles intercalate lithium together.
  • the characteristics of fast lithium intercalation and high capacity of hard carbon enable it to buffer and shunt lithium ions for the surrounding graphite particles.
  • the high sphericity of hard carbon particles can make the diffusion paths of lithium ions in all directions similar, thereby ensuring The uniformity of lithium intercalation prevents some areas of hard carbon particles from high lithium intercalation, rapid saturation and loss of buffering capacity, resulting in electrochemical polarization of graphite particles and even lithium precipitation.
  • the present application further improves the fast charging performance of the secondary battery by selecting the hard carbon with high average sphericity and the graphite with low average sphericity to match.
  • the average sphericity difference between hard carbon particles and graphite particles should not be too small.
  • it can prevent graphite and hard carbon from being independent when they are mixed, and the particle spacing is large.
  • graphite can be formed to surround hard carbon. structure, thereby ensuring the fast charging performance of the secondary battery.
  • the peak intensity I D1 of the D peak and the peak intensity I G1 of the G peak satisfy 0.4 ⁇ I D1 /I G1 ⁇ 2; and/or, the hardness In the Raman spectrum of carbon, the peak intensity I D2 of the D peak and the peak intensity I G2 of the G peak satisfy 0.01 ⁇ I D2 /I G2 ⁇ 0.7, optionally, 0.4 ⁇ I D1 /I G ⁇ 1.3 , 0.4 ⁇ I D1 /I G1 ⁇ 1.6, 1.3 ⁇ I D1 /I G1 ⁇ 1.6, 1.3 ⁇ I D1 /I G1 ⁇ 2, or 1.6 ⁇ I D1 /I G1 ⁇ 2; alternatively, 0.01 ⁇ I D2 /I G2 ⁇ 0.05, 0.01 ⁇ I D2 /I G2 ⁇ 0.1, 0.05 ⁇ I D2 /I G2 ⁇ 0.1, 0.05 ⁇ I D2 /I G2 ⁇ 0.1, 0.05 ⁇ I D2 /I G
  • the peak intensities ID1 and ID2 of the D peak and the peak intensities I G1 and I G2 of the G peak satisfy ID1 /I G1 ⁇ I D2 /I G2 .
  • Peak D and peak G are common Raman characteristic peaks in Raman spectroscopy detection. These two peaks will appear in the test near a specific wave number.
  • the D peak is located at 1300cm -1 ⁇ 1400cm -1 , representing defects in the carbon atom lattice;
  • the G peak is located at 1500cm -1 ⁇ 1600cm -1 , representing the in-plane stretching vibration degree of sp 2 hybridization of carbon atoms.
  • the ratio of the intensity of the D peak to the G peak represents the degree of defect in the carbon layer, and the higher the ratio, the greater the degree of defect.
  • the intensities of peak D and peak G of graphite and hard carbon can be tested by methods known in the art. As an example, it can be characterized by a Finder one model laser Raman spectrometer from Zolix.
  • graphite and hard carbon can be guaranteed to have relatively large defects, and these defects can provide ion channels, allowing the material to conduct ions faster, thereby Guarantee the fast charging performance of the secondary battery.
  • the ratio of the intensity of the D peak to the G peak of the selected graphite is larger than that of hard carbon, that is, compared with the selected graphite, the selected hard carbon has larger surface defects. Therefore, it can ensure that the hard carbon has a faster lithium insertion speed and a higher lithium storage capacity, and in the charging process, it can buffer and shunt lithium ions for the surrounding graphite particles to further improve the fast charging performance of the secondary battery. .
  • the OI value is the degree of orientation, which is the ratio of the XRD diffraction intensity of the plane perpendicular to the Z-axis of the graphite crystal plane to the XRD diffraction intensity of the plane parallel to the Z-axis of the graphite crystal plane.
  • the OI value of graphite can be tested by methods known in the art.
  • characterization may be performed by a Bruker model D8-Discover X-ray diffractometer.
  • the present application can reduce the cyclic expansion of the negative electrode sheet by selecting graphite within a suitable OI value range.
  • the graphite has a volume average particle diameter Dv50 of 3 ⁇ m to 30 ⁇ m; and/or, the hard carbon has a volume average particle diameter Dv50 of 3 ⁇ m to 9 ⁇ m.
  • the volume average particle diameter Dv50 of the graphite is optionally 3 ⁇ m ⁇ 12 ⁇ m or 12 ⁇ m ⁇ 30 ⁇ m.
  • the volume average particle diameter Dv50 of the hard carbon is optionally 3 ⁇ m ⁇ 6 ⁇ m, 6 ⁇ m ⁇ 9 ⁇ m.
  • the present application can shorten the short diffusion path of graphite particles and hard carbon particles from the core to the surface by controlling the average volume particle diameter Dv50 of the graphite and the hard carbon within an appropriate range, thereby ensuring that lithium ions pass from the outside to the inside.
  • the short transmission time can increase the lithium intercalation speed of the negative electrode active material and improve the fast charging performance of the secondary battery.
  • the volume average particle diameter Dv50 of graphite and hard carbon can be tested by methods known in the art.
  • a Malvern laser particle size analyzer may be used to perform a characterization test, for example, a Malvern Mastersizer-3000 and other instruments may be used for testing.
  • the mass percentage of the hard carbon is 1% to 99%, optionally 10% to 70%, and further optionally, the hard carbon The mass percentage is 10% to 50%.
  • the mass percentage of the hard carbon is not higher than the mass percentage of the graphite.
  • the mass percentage of the hard carbon and the graphite within an appropriate range, it is possible to prevent the poor rate performance caused by too low a hard carbon ratio, and to improve the fast charging performance of the secondary battery.
  • the second embodiment of the present application may provide a negative electrode sheet, which includes the negative electrode active material of the above-mentioned first embodiment.
  • the negative electrode sheet has excellent fast charging performance.
  • the negative electrode sheet has a compacted density of 1.00 g/cm 3 to 1.80 g/cm 3 .
  • the compacted density of the negative electrode sheet is 1.00g/cm 3 -1.30g/cm 3 , 1.00g/cm 3 -1.35g/cm 3 , 1.00g/cm 3 -1.40g/cm 3 , 1.00g /cm 3 ⁇ 1.49g/cm 3 , 1.00g/cm 3 ⁇ 1.63g/cm 3 , 1.30g/cm 3 ⁇ 1.35g/cm 3 , 1.30g/cm 3 ⁇ 1.40g/cm 3 , 1.30g/cm 3 ⁇ 1.49g/cm 3 , 1.30g/cm 3 ⁇ 1.63g/cm 3 , 1.30g/cm 3 ⁇ 1.80g/cm 3 , 1.35g/cm 3 ⁇ 1.40g/cm 3 , 1.35g/cmm
  • the third embodiment of the present application may provide a secondary battery, which includes the negative electrode sheet of the above-mentioned second embodiment. Secondary batteries have excellent fast charging performance.
  • a fourth embodiment of the present application may provide a battery module including the secondary battery of the above-mentioned third embodiment.
  • the battery module has excellent fast charging performance.
  • a fifth embodiment of the present application may provide a battery pack, which includes the battery module of the above-mentioned fourth embodiment.
  • the battery pack has excellent fast charging performance.
  • the sixth embodiment of the present application may provide an electric device including at least one of the secondary battery of the third embodiment, the battery module of the fourth embodiment, or the battery pack of the fifth embodiment.
  • the electric device has excellent fast charging performance.
  • a secondary battery in one embodiment, includes a positive pole piece, a negative pole piece, an electrolyte, and a separator.
  • the electrolyte plays the role of conducting lithium ions between the positive pole piece and the negative pole piece.
  • the separator is arranged between the positive pole piece and the negative pole piece, which mainly plays a role in preventing the short circuit of the positive and negative poles, and at the same time allows ions to pass through.
  • the separator in this application includes a composite flame retardant material as a coating component.
  • the positive electrode sheet includes a positive electrode current collector and a positive electrode film layer disposed on at least one surface of the positive electrode collector, and the positive electrode film layer includes the positive electrode active material according to the first aspect of the present application.
  • the positive electrode current collector has two opposing surfaces in its own thickness direction, and the positive electrode film layer is disposed on any one or both of the two opposing surfaces of the positive electrode current collector.
  • the positive electrode current collector can be a metal foil or a composite current collector.
  • aluminum foil can be used as the metal foil.
  • the composite current collector may include a polymer material base and a metal layer formed on at least one surface of the polymer material base.
  • the composite current collector can be formed by forming metal materials (aluminum, aluminum alloy, nickel, nickel alloy, titanium, titanium alloy, silver and silver alloy, etc.) on a polymer material substrate (such as polypropylene (PP), polyethylene terephthalic acid It is formed on substrates such as ethylene glycol ester (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
  • PP polypropylene
  • PET polyethylene glycol ester
  • PBT polybutylene terephthalate
  • PS polystyrene
  • PE polyethylene
  • the positive electrode active material may be a positive electrode active material known in the art for batteries.
  • the positive active material may include at least one of the following materials: olivine-structured lithium-containing phosphate, lithium transition metal oxide, and their respective modified compounds.
  • the present application is not limited to these materials, and other conventional materials that can be used as positive electrode active materials of batteries can also be used. These positive electrode active materials may be used alone or in combination of two or more.
  • lithium transition metal oxides may include, but are not limited to, lithium cobalt oxides (such as LiCoO 2 ), lithium nickel oxides (such as LiNiO 2 ), lithium manganese oxides (such as LiMnO 2 , LiMn 2 O 4 ), lithium Nickel cobalt oxide, lithium manganese cobalt oxide, lithium nickel manganese oxide, lithium nickel cobalt manganese oxide (such as LiNi 1/3 Co 1/3 Mn 1/3 O 2 (also referred to as NCM 333 ), LiNi 0.5 Co 0.2 Mn 0.3 O 2 (also abbreviated as NCM 523 ), LiNi 0.5 Co 0.25 Mn 0.25 O 2 (also abbreviated as NCM 211 ), LiNi 0.6 Co 0.2 Mn 0.2 O 2 (also abbreviated as NCM 622 ), LiNi At least one of 0.8 Co 0.1 Mn 0.1 O 2 (also referred to as NCM 811 ), lithium nickel cobalt aluminum oxide (such as LiNi
  • the olivine structure contains Examples of lithium phosphates may include, but are not limited to, lithium iron phosphate (such as LiFePO 4 (also may be abbreviated as LFP)), composite materials of lithium iron phosphate and carbon, lithium manganese phosphate (such as LiMnPO 4 ), lithium manganese phosphate and carbon At least one of a composite material, lithium manganese iron phosphate, and a composite material of lithium manganese iron phosphate and carbon.
  • lithium iron phosphate such as LiFePO 4 (also may be abbreviated as LFP)
  • composite materials of lithium iron phosphate and carbon such as LiMnPO 4
  • LiMnPO 4 lithium manganese phosphate and carbon
  • the positive electrode film layer may further optionally include a binder.
  • the binder may include polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene At least one of ethylene terpolymer, tetrafluoroethylene-hexafluoropropylene copolymer and fluorine-containing acrylate resin.
  • the positive electrode film layer may also optionally include a conductive agent.
  • the conductive agent may include at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
  • the positive electrode sheet can be prepared in the following manner: the above-mentioned components used to prepare the positive electrode sheet, such as positive electrode active material, conductive agent, binder and any other components, are dispersed in a solvent (such as N -methylpyrrolidone) to form a positive electrode slurry; the positive electrode slurry is coated on the positive electrode current collector, and after drying, cold pressing and other processes, the positive electrode sheet can be obtained.
  • a solvent such as N -methylpyrrolidone
  • the negative electrode sheet includes a negative electrode current collector and a negative electrode film layer arranged on at least one surface of the negative electrode current collector, and the negative electrode film layer includes a negative electrode active material.
  • the negative electrode current collector has two opposing surfaces in its own thickness direction, and the negative electrode film layer is disposed on any one or both of the two opposing surfaces of the negative electrode current collector.
  • the negative electrode current collector can use a metal foil or a composite current collector.
  • copper foil can be used as the metal foil.
  • the composite current collector may include a base layer of polymer material and a metal layer formed on at least one surface of the base material of polymer material.
  • Composite current collectors can be formed by metal materials (copper, copper alloys, nickel, nickel alloys, titanium, titanium alloys, silver and silver alloys, etc.) on polymer material substrates (such as polypropylene (PP), polyethylene terephthalic acid It is formed on substrates such as ethylene glycol ester (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
  • the negative electrode active material includes graphite and hard carbon, and the graphite may include at least one of artificial graphite and natural graphite.
  • negative electrode active materials known in the art for batteries can also be added, as an example, at least one of the following materials can be added: soft carbon, silicon-based materials, tin-based materials and lithium titanate, etc. .
  • the silicon-based material may be selected from at least one of elemental silicon, silicon-oxygen compounds, silicon-carbon composites, silicon-nitrogen composites, and silicon alloys.
  • the tin-based material may be selected from at least one of simple tin, tin oxide compounds and tin alloys.
  • the present application is not limited to these materials, and other conventional materials that can be used as the active material of the negative electrode of the battery can also be added.
  • the negative electrode film layer may further optionally include a binder.
  • the binder can be selected from styrene-butadiene rubber (SBR), polyacrylic acid (PAA), sodium polyacrylate (PAAS), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium alginate (SA), poly At least one of methacrylic acid (PMAA) and carboxymethyl chitosan (CMCS).
  • the negative electrode film layer may also optionally include a conductive agent.
  • the conductive agent can be selected from at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene and carbon nanofibers.
  • the negative electrode film layer may optionally include other additives, such as thickeners (such as sodium carboxymethylcellulose (CMC-Na)) and the like.
  • thickeners such as sodium carboxymethylcellulose (CMC-Na)
  • CMC-Na sodium carboxymethylcellulose
  • the negative electrode sheet can be prepared in the following manner: the above-mentioned components used to prepare the negative electrode sheet, such as negative electrode active material, conductive agent, binder and any other components, are dispersed in a solvent (such as deionized water) to form a negative electrode slurry; the negative electrode slurry is coated on the negative electrode current collector, and after drying, cold pressing and other processes, the negative electrode sheet can be obtained.
  • a solvent such as deionized water
  • the electrolyte plays the role of conducting ions between the positive pole piece and the negative pole piece.
  • the present application has no specific limitation on the type of electrolyte, which can be selected according to requirements.
  • electrolytes can be liquid, gel or all solid.
  • the electrolyte is an electrolytic solution.
  • the electrolyte solution includes an electrolyte salt and a solvent.
  • the electrolyte salt may be selected from lithium hexafluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium hexafluoroarsenate, lithium bisfluorosulfonyl imide, lithium bistrifluoromethanesulfonyl imide, trifluoromethane At least one of lithium sulfonate, lithium difluorophosphate, lithium difluorooxalate borate, lithium difluorooxalate borate, lithium difluorodifluorooxalatephosphate and lithium tetrafluorooxalatephosphate.
  • the solvent may be selected from ethylene carbonate, propylene carbonate, ethyl methyl carbonate, diethyl carbonate, dimethyl carbonate, dipropyl carbonate, methyl propyl carbonate, ethyl propyl carbonate, Butylene carbonate, fluoroethylene carbonate, methyl formate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, propyl propionate, methyl butyrate, ethyl butyrate At least one of ester, 1,4-butyrolactone, sulfolane, dimethyl sulfone, methyl ethyl sulfone and diethyl sulfone.
  • the electrolyte may optionally include additives.
  • additives may include negative electrode film-forming additives, positive electrode film-forming additives, and additives that can improve certain performances of the battery, such as additives that improve battery overcharge performance, additives that improve high-temperature or low-temperature performance of batteries, and the like.
  • a separator is further included in the secondary battery.
  • the present application has no particular limitation on the type of the isolation membrane, and any known porous structure isolation membrane with good chemical stability and mechanical stability can be selected.
  • the material of the isolation film can be selected from at least one of glass fiber, non-woven fabric, polyethylene, polypropylene and polyvinylidene fluoride.
  • the separator can be a single-layer film or a multi-layer composite film, without any particular limitation. When the separator is a multilayer composite film, the materials of each layer may be the same or different, and there is no particular limitation.
  • 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 package can be used to package 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, and the like.
  • the outer packaging of the secondary battery may also be a soft bag, such as a bag-type soft bag.
  • the material of the soft case may be plastic, and examples of the plastic include polypropylene, polybutylene terephthalate, polybutylene succinate, and the like.
  • FIG. 3 shows a square-shaped secondary battery 5 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 plates enclose to form an accommodating cavity.
  • the housing 51 has an opening communicating with the accommodating cavity, and the cover plate 53 can cover the opening to close the accommodating cavity.
  • the positive pole piece, the negative pole piece and the separator can be formed into the electrode assembly 52 through a winding process or a lamination process.
  • the electrode assembly 52 is packaged in the accommodating cavity. Electrolyte is infiltrated in the electrode assembly 52 .
  • the number of electrode assemblies 52 contained in the secondary battery 5 can be one or more, and those skilled in the art can select according to actual needs.
  • the secondary battery can be assembled into a battery module, and the number of secondary batteries contained in the battery module can be one or more, and the specific number can be selected by those skilled in the art 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 are arranged in sequence along the length direction of the battery module 4 .
  • multiple secondary batteries 5 may also be arranged in any other manner.
  • the plurality of secondary batteries 5 may be fixed by fasteners.
  • the battery module 4 may also include a case having a housing space in which a plurality of secondary batteries 5 are accommodated.
  • the above-mentioned battery modules can also be assembled into a battery pack.
  • the number of battery modules contained in the battery pack can be one or more, and the specific number can be selected by those skilled in the art 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 disposed in the battery box.
  • the battery box includes an upper box body 2 and a lower box body 3 , the upper box body 2 can cover the lower box body 3 and form a closed space for accommodating the battery module 4 .
  • Multiple battery modules 4 can be arranged in the battery box in any manner.
  • the present application also provides an electric device, which includes at least one of the secondary battery, battery module or battery pack provided in the present application.
  • the secondary battery, battery module or battery pack can be used as a power source of the electric device, and can also be used as an energy storage unit of the electric device.
  • the electric devices may include mobile devices (such as mobile phones, notebook computers, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf carts, etc.) , electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc., but not limited thereto.
  • a secondary battery, a battery module or a battery pack can be selected according to its use requirements.
  • FIG. 8 is an example of an electrical device.
  • the electric device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle.
  • a battery pack or a battery module may be used.
  • a device may be a cell phone, tablet, laptop, or the like.
  • the device is generally required to be light and thin, and a secondary battery can be used as a power source.
  • Example 1 After weighing the selected graphite material and hard carbon material according to the mass ratio, put them into a V-shaped mixer for physical mixing, thereby obtaining the negative electrode active material.
  • the physical parameters of the above-mentioned negative electrode active material are shown in Example 1 in Table 1 below.
  • the negative electrode active materials of Examples 2-6 were prepared in the same manner as Example 1, except that graphite and hard carbon with different degrees of sphericity were selected as raw materials as shown in Table 1 below.
  • Negative active materials of Examples 7 to 8 were prepared in the same manner as in Example 1, except that the addition amount of raw materials was adjusted as shown in Table 1 below.
  • the negative electrode active materials of Examples 9-10 were prepared in the same manner as Example 1, except that graphite and hard carbon with different ID / IG ratios were selected as raw materials as shown in Table 1 below.
  • the negative electrode active materials of Examples 11-12 were prepared in the same manner as in Example 1, except that graphite with different OI values was selected as shown in Table 1 below.
  • the negative electrode active materials of Examples 13-14 were prepared in the same manner as Example 1, except that graphite and hard carbon with different volume average particle diameters Dv50 were selected as raw materials by screening and other methods as shown in Table 1 below.
  • the negative electrode active materials of Comparative Examples 1-2 were prepared in the same manner as in Example 1, except that the sphericity of graphite and hard carbon was adjusted as shown in Table 1 below.
  • each embodiment and comparative example as negative active material, with conductive agent acetylene black, binding agent styrene-butadiene rubber (SBR) and thickener carbon methyl cellulose sodium (CMC) according to weight ratio 90:5:2:2:1 After fully stirring and mixing in the deionized water solvent system, it is coated on a copper foil, dried, and cold pressed to obtain a negative electrode sheet.
  • the positive electrode material lithium manganese phosphate, conductive agent acetylene black and binder polyvinylidene fluoride (PVDF) are mixed in N-methylpyrrolidone solvent system at a weight ratio of 94:3:3, and then coated on aluminum foil drying and cold pressing to obtain the positive electrode sheet.
  • PVDF polyvinylidene fluoride
  • a porous polymer film made of polyethylene (PE) is used as the separator.
  • the positive electrode sheet, the separator and the negative electrode sheet are stacked in order, so that the separator is placed between the positive and negative electrodes to play the role of isolation, and the bare cell is obtained by winding.
  • the electrolyte is 1mol/L LiPF 6 /(ethylene carbonate (EC)+diethyl carbonate (DEC)+dimethyl carbonate (DMC)) (volume ratio 1:1:1).
  • the bare cell is placed in the outer package, the above-mentioned electrolyte is injected and packaged to obtain a secondary battery.
  • Example 1 92.7%
  • Example 10 90.7%
  • Example 2 90.3%
  • Example 11 90.2%
  • Example 3 89.6%
  • Example 12 93.7%
  • Example 4 91.7%
  • Example 13 93.4%
  • Example 5 89.5%
  • Example 14 92.1%
  • Example 6 90.1%
  • Example 15 93.2%
  • Example 7 88.6% Comparative example 16 91.7%
  • Example 8 85.4% Comparative example 1 83.7%
  • Example 9 93.2% Comparative example 2 83.3%
  • a structure in which graphite surrounds hard carbon can be formed in the negative electrode active material, and hard carbon can buffer and shunt lithium ions for surrounding graphite , to prevent the high degree of lithium intercalation in some areas of hard carbon particles, fast saturation and loss of buffer capacity, the occurrence of electrochemical polarization of graphite particles and even lithium precipitation, to ensure the improvement of the fast charging performance of secondary batteries. Therefore, it is necessary to control the average sphericity of hard carbon and graphite, and the difference between the two average sphericity within an appropriate range.
  • the present application is not limited to the above-mentioned embodiments.
  • the above-mentioned embodiments are merely examples, and within the scope of the technical solution of the present application, embodiments that have substantially the same configuration as the technical idea and exert the same function and effect are included in the technical scope of the present application.
  • various modifications conceivable by those skilled in the art are added to the embodiments, and other forms constructed by combining some components in the embodiments are also included in the scope of the present application. .

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Abstract

La présente demande concerne un matériau actif d'électrode négative, une plaque d'électrode négative, une batterie secondaire, un module de batterie, un bloc-batterie et un dispositif électrique associé. Le matériau actif d'électrode négative comprend du graphite et du carbone dur, la sphéricité moyenne du graphite étant telle que 0,1 ≤ A ≤ 0,7, la sphéricité moyenne du carbone dur étant telle que 0,8 ≤ B < 1, et 0,1 ≤ B - A ≤ 0,8. Selon la présente demande, le carbone dur présentant une sphéricité moyenne relativement élevée est mis en correspondance avec le graphite présentant une sphéricité moyenne relativement faible, et la différence des sphéricités moyennes des deux est régulée dans une certaine plage, de sorte que les performances de charge rapide d'une batterie secondaire peuvent être efficacement améliorées.
PCT/CN2022/137551 2022-01-13 2022-12-08 Matériau actif d'électrode négative, plaque d'électrode négative, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique associé WO2023134340A1 (fr)

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