WO2024036472A1 - Matériau actif d'électrode positive et son procédé de préparation, plaque d'électrode positive, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique - Google Patents

Matériau actif d'électrode positive et son procédé de préparation, plaque d'électrode positive, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique Download PDF

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WO2024036472A1
WO2024036472A1 PCT/CN2022/112738 CN2022112738W WO2024036472A1 WO 2024036472 A1 WO2024036472 A1 WO 2024036472A1 CN 2022112738 W CN2022112738 W CN 2022112738W WO 2024036472 A1 WO2024036472 A1 WO 2024036472A1
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active material
lithium
cathode active
positive electrode
optionally
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PCT/CN2022/112738
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English (en)
Chinese (zh)
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魏冠杰
古力
孟阵
张宇
李星
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宁德时代新能源科技股份有限公司
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Priority to CN202280087729.XA priority Critical patent/CN118613932A/zh
Priority to PCT/CN2022/112738 priority patent/WO2024036472A1/fr
Publication of WO2024036472A1 publication Critical patent/WO2024036472A1/fr

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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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • 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 lithium batteries, and in particular to a positive active material and a preparation method thereof, as well as a positive electrode sheet, a secondary battery, a battery module, a battery pack and an electrical device including the positive active material.
  • lithium-ion batteries are widely used in energy storage power systems such as hydraulic, thermal, wind and solar power stations, as well as power tools, electric bicycles, electric motorcycles, electric vehicles, Military equipment, aerospace and other fields. Due to the great development of lithium-ion batteries, higher requirements have been put forward for their energy density, cycle performance and safety performance.
  • cathode materials include layered structure materials (such as lithium cobalt oxide, lithium manganate, lithium nickel oxide, etc.), spinel structure materials, polyanionic materials, ternary materials, and lithium-rich materials that are currently attracting much attention. wait.
  • lithium-ion battery systems prepared from these cathode materials still have problems such as low energy density, high cost, and poor safety. They cannot meet people's growing needs for battery fast charging, cycle stability, safety, etc. Therefore, it is necessary to adopt Certain strategies are used to optimize cathode materials to improve secondary battery cycle performance, rate performance and safety performance.
  • This application was conducted in view of the above-mentioned issues, and its purpose is to provide a cathode active material with improved cycle performance and rate performance, and to provide a preparation method of the cathode active material and a cathode active material containing the cathode active material of the application.
  • a first aspect of the present application provides a cathode active material.
  • the cathode active material is a secondary particle formed by stacking primary particles, wherein the primary particles include a lithium-rich manganese-based matrix material and a
  • the coating layer on the surface of the lithium-rich manganese base material includes a fast ion conductor and a metal compound conductive agent.
  • the cathode active material of the present application has improved cycle performance and rate performance.
  • the fast ion conductor is selected from one or more of lithium silicate, lithium phosphate, lithium borate, lithium niobate, lithium aluminate, lithium zirconate and lithium pyrophosphate, optionally,
  • the fast ion conductor is selected from one or more of lithium silicate, lithium phosphate and lithium borate; optionally, the amount of the fast ion conductor is 0.5-20% by weight, optionally 2-12% by weight , based on the weight of the cathode active material.
  • the metal compound conductive agent is selected from one or more of titanium carbide, titanium nitride and titanium boride; optionally, the amount of the metal compound conductive agent is 0.5-10% by weight. , optionally 1-6% by weight, based on the weight of the cathode active material.
  • the weight ratio of the fast ion conductor to the metal compound conductive agent in the cathode active material is 1.3-3:1, optionally 1.7-2.7:1.
  • the chemical formula of the lithium-rich manganese-based matrix material is xLi 2 MnO 3 ⁇ (1-x)LiMO 2 , wherein M is selected from Fe, Al, Co, Mn, Ni, Cr, Ti , Mo, Nb, Zr, Sn, V, Mg, Cu, Zn, B, Na, Ca and Ru in one or more combinations, optionally, the M is selected from Co, Ni, Cr, One or a combination of one or more of V, Mo, Mn, Al, Nb and Ti, and 0 ⁇ x ⁇ 1.
  • the Dv50 of the positive active material is 5-20 ⁇ m, optionally 7-13 ⁇ m, and the Dv50 of the primary particles is 0.05-1 ⁇ m, optionally 0.1-0.4 ⁇ m.
  • the particle size of the positive active material is within the above range, the compacted density of the positive active material can be optimized, thereby further improving the performance of the positive active material.
  • the compacted density of the positive active material under 5 tons of force is 2.4-3.4g/cm 3 , optionally 2.7-3.2g/cm 3 .
  • the filling degree between the particles of the cathode active material is high, which is beneficial to further improving the processing performance of the cathode active material.
  • the thickness of the coating layer is 0.005-0.2 ⁇ m, optionally 0.01-0.1 ⁇ m, and more optionally 0.04-0.08 ⁇ m.
  • the thickness of the coating layer meets the above range, it is conducive to further improving the cycle performance and rate performance of the cathode active material.
  • a second aspect of the application provides a method for preparing a cathode active material, which method includes the following steps:
  • step S2 Add the fast ion conductor precursor, metal compound conductive agent and dispersant polyvinylpyrrolidone into water and mix evenly, then add the primary particles of the lithium-rich manganese-based cathode active material precursor of step S1) into the water and mix evenly to obtain Suspensions of solid mixtures;
  • step S3 spray-dry the suspension of the solid mixture in step S2) for secondary granulation to obtain positive electrode active material precursor powder;
  • step S4 Mix the cathode active material precursor powder and the lithium source in step S3) evenly, and sinter them to obtain the cathode active material
  • the positive active material is a secondary particle formed by stacking primary particles, wherein the primary particle includes a lithium-rich manganese-based matrix material and a coating layer located on the surface of the lithium-rich manganese-based matrix material, and the coating layer includes Fast ion conductor and metal compound conductive agent.
  • the Dv50 of the primary particles of the lithium-rich manganese-based cathode active material precursor is 0.05-1.1 ⁇ m, optionally 0.1-0.4 ⁇ m.
  • the particle size of the primary particles of the precursor it is beneficial to obtain a cathode active material with improved rate performance and cycle performance.
  • the solid mixture includes primary particles of a fast ion conductor precursor, a metal compound conductive agent, and a lithium-rich manganese-based cathode active material precursor, wherein the fast ion conductor
  • the precursor is selected from one or more of silicon dioxide, lithium phosphate, lithium borate, niobium pentoxide, alumina, zirconium dioxide and lithium dihydrogen phosphate.
  • the fast ion conductor precursor is selected from One or more of silica, lithium phosphate, and lithium borate; optionally, the amount of the fast ion conductor is 0.4-16% by weight, optionally 1.5-9.5% by weight, based on the solid mixture by weight, and the metal compound conductive agent is selected from one or more of titanium carbide, titanium nitride and titanium boride; optionally, the amount of the metal compound conductive agent is 0.4-8% by weight, Optional is 0.8-5% by weight, based on the weight of the solid mixture.
  • the sintering atmosphere is oxygen, air or compressed air
  • the sintering temperature is 700-1000°C
  • the sintering time is 5-10 h.
  • a third aspect of the present application provides a positive electrode sheet.
  • 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 current collector.
  • the positive electrode film layer includes the positive electrode activity of the first aspect of the application. material or a cathode active material prepared by the method of the second aspect of the present application, and the content of the cathode active material in the cathode film layer is more than 10% by weight, based on the total weight of the cathode film layer.
  • a fourth aspect of the application provides a secondary battery, which includes the cathode active material of the first aspect of the application or the cathode active material prepared according to the method of the second aspect of the application.
  • a fifth aspect of the present application provides a battery module including the secondary battery of the fourth aspect of the present application.
  • a sixth aspect of the present application provides a battery pack, which includes the battery module of the fifth aspect of the present application.
  • a seventh aspect of the present application provides an electrical device, which includes at least one selected from the group consisting of the secondary battery of the fourth aspect of the present application, the battery module of the fifth aspect of the present application, or the battery pack of the sixth aspect of the present application. A sort of.
  • the battery modules, battery packs and electrical devices of the present application include the secondary battery provided by the present application, and therefore have at least the same advantages as the secondary battery.
  • FIG. 1 is a schematic diagram of a secondary battery according to an embodiment of the present application.
  • FIG. 2 is an exploded view of the secondary battery according to the embodiment of the present application shown in FIG. 1 .
  • FIG. 3 is a schematic diagram of a battery module according to an embodiment of the present application.
  • Figure 4 is a schematic diagram of a battery pack according to an embodiment of the present application.
  • FIG. 5 is an exploded view of the battery pack according to an embodiment of the present application shown in FIG. 4 .
  • FIG. 6 is a schematic diagram of a power consumption device using a secondary battery as a power source according to an embodiment of the present application.
  • Ranges disclosed herein are defined in terms of lower and upper limits. 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 of the endpoints, and may be arbitrarily combined, that is, 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, understand that ranges of 60-110 and 80-120 are also expected. Furthermore, if the minimum range values 1 and 2 are listed, and if the maximum range values 3, 4, and 5 are listed, then 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" means that all real numbers between "0-5" have been listed in this article, and "0-5" is just an abbreviation of these numerical combinations.
  • a certain parameter is an integer ⁇ 2
  • condition "A or B” is satisfied by any of the following conditions: 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).
  • Lithium-rich manganese-based cathode materials are considered to be the preferred cathode materials for the next generation of high-specific-energy batteries due to their high specific capacity (>250mAh/g), low cost, and good thermal stability.
  • Lithium-rich manganese-based cathode materials mainly use environmentally friendly manganese elements, which have low nickel and cobalt content and may even be cobalt-free, effectively avoiding the problem of nickel and cobalt resources. At the same time, compared with cobalt and nickel, manganese is not only cheap And the reserves are abundant. However, the lithium ion diffusion coefficient of lithium-rich materials is low, resulting in poor rate performance.
  • a suitable surface coating layer can not only provide a fast transmission channel for lithium ions/electrons, but also isolate electrolysis Direct contact between the liquid and the cathode material to prevent the reaction between the two from deteriorating battery performance.
  • a single coating layer only has one property, that is, while improving ion conductivity, it may hinder the transmission of electrons and affect conductivity, and vice versa.
  • the carbon layer has good conductivity, but its lithium ion transport capacity is relatively low. Poor.
  • multi-layer coating means that the preparation process is more complicated, and the bonding strength between the coating layers is difficult to guarantee. As the cycle process proceeds, the coating layer and the base material may be separated, thus degrading the performance.
  • a first aspect of the present application provides a cathode active material.
  • the cathode active material is a secondary particle formed by stacking primary particles, wherein the primary particles include a lithium-rich manganese-based matrix material and a lithium-rich manganese-based base material located on the rich lithium-rich manganese base material.
  • a coating layer on the surface of the lithium manganese base material, the coating layer includes a fast ion conductor and a metal compound conductive agent.
  • the cathode active material of the present application is a secondary particle formed by stacking primary particles, and a homogeneous composite is constructed on the outer surface of the matrix material of the primary particles.
  • the coating layer includes a fast ion conductor and a metal compound conductive agent.
  • the fast ion conductor can effectively improve the ion transmission capability of the cathode active material
  • the metal compound conductive agent can effectively improve the electron transmission capability of the cathode active material. It forms a continuous ion and electron channel in the coating layer.
  • the cathode active material of the present application can be modified through surface coating to prevent direct contact between the cathode active material and the electrolyte, inhibit the occurrence of side reactions, and improve the cycle performance of the cathode active material.
  • the surface of each primary particle has The completed coating layer, even if the secondary particles are broken, will not seriously affect the cycle stability of the material.
  • the secondary particles are composed of multiple primary particles gathered together to form spherical or spherical-like particles; the primary particles are single particles with a Dv50 of about 0.05-1 ⁇ m and there is no obvious agglomeration between particles.
  • the fast ion conductor is selected from one or more of lithium silicate, lithium phosphate, lithium borate, lithium niobate, lithium aluminate, lithium zirconate and lithium pyrophosphate.
  • the fast ion conductor is selected from one or more of lithium silicate, lithium phosphate and lithium borate; optionally, the amount of the fast ion conductor is 0.5-20% by weight, optionally 2-12% by weight , based on the weight of the cathode active material.
  • the coating layer will be too thick, which is not conducive to the transmission efficiency of ions in the cathode active material; if the content of the fast ion conductor is too low, lithium ions cannot be effectively transported.
  • the metal compound conductive agent is selected from one or more of titanium carbide, titanium nitride and titanium boride; optionally, the amount of the metal compound conductive agent is 0.5-10% by weight. , optionally 1-6% by weight, based on the weight of the cathode active material.
  • the rate performance and cycle performance of the cathode active material can be further improved. If the content of the metal compound conductive agent is too high, the coating layer will be too thick, which is detrimental to the transmission efficiency of ions in the cathode active material; if the content of the metal compound conductive agent is too low, electrons cannot be effectively transported.
  • the weight ratio of the fast ion conductor to the metal compound conductive agent in the cathode active material is 1.3-3:1, optionally 1.7-2.7:1.
  • the cathode active material can have both high ionic conductivity and electronic conductivity, thereby further improving the cycle performance and performance of the cathode active material. magnification performance.
  • the chemical formula of the lithium-rich manganese-based matrix material is xLi 2 MnO 3 ⁇ (1-x)LiMO 2 , wherein M is selected from Fe, Al, Co, Mn, Ni, Cr, Ti , Mo, Nb, Zr, Sn, V, Mg, Cu, Zn, B, Na, Ca and Ru in one or more combinations, optionally, the M is selected from Co, Ni, Cr, One or a combination of one or more of V, Mo, Mn, Al, Nb and Ti, and 0 ⁇ x ⁇ 1.
  • the Dv50 of the positive active material is 5-20 ⁇ m, optionally 7-13 ⁇ m, and the Dv50 of the primary particles is 0.05-1 ⁇ m, optionally 0.1-0.4 ⁇ m.
  • the particle size of the positive active material is within the above range, the compacted density of the positive active material can be optimized, thereby further improving the performance of the positive active material.
  • the compacted density of the cathode active material under 5 tons of force is 2.4-3.4g/cm 3 , optionally 2.7-3.2g/cm 3 .
  • the higher the compaction density the greater the weight of the active material per unit volume. Therefore, increasing the compaction density is beneficial to increasing the volumetric energy density of the battery core.
  • the positive active material has a high compaction density and a high filling degree between particles, which is not only conducive to further improving the processing performance of the positive active material.
  • the compacted density can be measured according to GB/T 24533-2009.
  • the thickness of the coating layer is 0.005-0.2 ⁇ m, optionally 0.01-0.1 ⁇ m, and more optionally 0.04-0.08 ⁇ m.
  • the cathode active material can have improved cycle performance and rate performance. If the thickness of the coating layer is too thick, it will be detrimental to the transmission efficiency of electrons and ions; if the thickness of the coating layer is too thin, it will not be able to effectively transmit electrons and ions.
  • the weight a of the fast ion conductor in the positive active material and the weight b of the metal compound conductive agent satisfy the following: 2 ⁇ a*b/(a+b) ⁇ 4, optional Ground, 2.5 ⁇ a*b/(a+b) ⁇ 3.
  • a second aspect of the application provides a method for preparing a cathode active material, which method includes the following steps:
  • step S2 Add the fast ion conductor precursor, metal compound conductive agent and dispersant polyvinylpyrrolidone into water and mix evenly, then add the primary particles of the lithium-rich manganese-based cathode active material precursor of step S1) into the water and mix evenly to obtain Suspensions of solid mixtures;
  • step S3 spray-dry the suspension of the solid mixture in step S2) for secondary granulation to obtain positive electrode active material precursor powder;
  • step S4 Mix the cathode active material precursor powder and the lithium source in step S3) evenly, and sinter them to obtain the cathode active material
  • the positive active material is a secondary particle formed by stacking primary particles, wherein the primary particle includes a lithium-rich manganese-based matrix material and a coating layer located on the surface of the lithium-rich manganese-based matrix material, and the coating layer includes Fast ion conductor and metal compound conductive agent.
  • a homogeneous composite coating layer is constructed on the outer surface of the matrix material of the primary particles, which effectively improves the ion transmission capacity and electron transmission capacity of the positive electrode active material, thereby obtaining a positive electrode active material with improved rate performance. material; on the other hand, it can significantly improve the bonding strength between the coating layer and the base material, avoid the degradation of battery performance caused by the shedding of the coating layer caused by uneven stress during the cycle, and effectively improve the cycle performance of the cathode active material.
  • the Dv50 of the primary particles of the lithium-rich manganese-based cathode active material precursor is 0.05-1.1 ⁇ m, optionally 0.1-0.4 ⁇ m.
  • the particle size of the primary particles of the precursor it is beneficial to obtain a cathode active material with improved rate performance and cycle performance.
  • the crushing method includes one or more of grinding, jet crushing, mechanical mill crushing and high-energy ball milling.
  • the crushing method is high-energy ball milling.
  • the solid mixture in step S2), includes primary particles of a fast ion conductor precursor, a metal compound conductive agent, and a lithium-rich manganese-based cathode active material precursor, wherein the fast ion conductor
  • the precursor is selected from one or more of silicon dioxide, lithium phosphate, lithium borate, niobium pentoxide, alumina, zirconium dioxide and lithium dihydrogen phosphate.
  • the fast ion conductor precursor is selected from One or more of silica, lithium phosphate, and lithium borate; optionally, the amount of the fast ion conductor is 0.4-16% by weight, optionally 1.5-9.5% by weight, based on the solid mixture by weight, and the metal compound conductive agent is selected from one or more of titanium carbide, titanium nitride and titanium boride; optionally, the amount of the metal compound conductive agent is 0.4-8% by weight, Optional is 0.8-5% by weight, based on the weight of the solid mixture.
  • the sintering atmosphere is oxygen, air or compressed air
  • the sintering temperature is 700-1000°C, for example, it can be 700°C, 800°C, 900°C or 1000°C, etc. , but are not limited to the listed point values.
  • the sintering time is 5-10h. For example, it can be 5h, 6h, 7h, 8h, 9h or 10h, but is not limited to the listed point values. The same applies as long as the values are within the above range.
  • a third aspect of the present application provides a positive electrode sheet.
  • 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 current collector.
  • the positive electrode film layer includes the positive electrode activity of the first aspect of the application. material or a cathode active material prepared by the method of the second aspect of the present application, and the content of the cathode active material in the cathode film layer is more than 10% by weight, based on the total weight of the cathode film layer.
  • a fourth aspect of the application provides a secondary battery, which includes the cathode active material of the first aspect of the application or the cathode active material prepared according to the method of the second aspect of the application.
  • a fifth aspect of the present application provides a battery module including the secondary battery of the fourth aspect of the present application.
  • a sixth aspect of the present application provides a battery pack, which includes the battery module of the fifth aspect of the present application.
  • a seventh aspect of the present application provides an electrical device, which includes at least one selected from the group consisting of the secondary battery of the fourth aspect of the present application, the battery module of the fifth aspect of the present application, or the battery pack of the sixth aspect of the present application. A sort of.
  • a secondary battery is provided.
  • a secondary battery typically includes a positive electrode plate, a negative electrode plate, an electrolyte and a separator.
  • active ions are inserted and detached back and forth between the positive and negative electrodes.
  • the electrolyte plays a role in conducting ions between the positive and negative electrodes.
  • the isolation film is placed between the positive electrode piece and the negative electrode piece. It mainly prevents the positive and negative electrodes from short-circuiting and allows ions to pass through.
  • 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 current collector.
  • the positive electrode film layer includes the positive electrode active material of the first aspect of the present application.
  • the positive electrode current collector has two surfaces facing each other in its own thickness direction, and the positive electrode film layer is disposed on any one or both of the two opposite surfaces of the positive electrode current collector.
  • the positive electrode current collector may be a metal foil or a composite current collector.
  • the metal foil aluminum foil can be used.
  • the composite current collector may include a polymer material base layer and a metal layer formed on at least one surface of the polymer material base layer.
  • the composite current collector can be formed by forming metal materials (aluminum, aluminum alloys, nickel, nickel alloys, titanium, titanium alloys, silver and silver alloys, etc.) on polymer material substrates (such as polypropylene (PP), polyterephthalate It is formed on substrates such as ethylene glycol ester (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
  • PP polypropylene
  • PBT polybutylene terephthalate
  • PS polystyrene
  • PE polyethylene
  • the cathode active material may also be a cathode active material known in the art for use in batteries.
  • the cathode active material may include at least one of the following materials: an olivine-structured lithium-containing phosphate, a lithium transition metal oxide, and their respective modified compounds.
  • the present application is not limited to these materials, and other traditional materials that can be used as positive electrode active materials of batteries can also be used.
  • These cathode active materials may be used alone or in combination of two or more, wherein the cathode active material of the first aspect of the application accounts for 85-100% and the other cathode active materials account for 0-15%.
  • 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 (can also be abbreviated to NCM 523 ), LiNi 0.5 Co 0.25 Mn 0.25 O 2 (can also be abbreviated to NCM 211 ), LiNi 0.6 Co 0.2 Mn 0.2 O 2 (can also be abbreviated to 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 Li Li
  • the olivine structure contains Examples of lithium phosphates may include, but are not limited to, lithium iron phosphate (such as LiFePO 4 (also referred to as LFP)), composites of lithium iron phosphate and carbon, lithium manganese phosphate (such as LiMnPO 4 ), lithium manganese phosphate and carbon. At least one of composite materials, lithium iron manganese phosphate, and composite materials of lithium iron manganese phosphate and carbon.
  • the weight ratio of the positive electrode active material in the positive electrode film layer is 80-100% by weight, based on the total weight of the positive electrode film layer count.
  • the positive electrode film layer optionally further includes 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 weight ratio of the binder in the positive electrode film layer is 0-20% by weight, based on the total weight of the positive electrode film layer.
  • the positive electrode film layer optionally further includes 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 weight ratio of the conductive agent in the positive electrode film layer is 0-20% by weight, based on the total weight of the positive electrode film layer.
  • the positive electrode sheet can be prepared by dispersing the above-mentioned components for preparing the positive electrode sheet, such as positive active material, conductive agent, binder and any other components in a solvent (such as N -methylpyrrolidone), forming a positive electrode slurry; wherein the solid content of the positive electrode slurry is 40-80wt%, the viscosity at room temperature is adjusted to 5000-25000mPa ⁇ s, and the positive electrode slurry is coated on the positive electrode current collector, After drying, cold pressing and other processes, the positive electrode piece can be obtained.
  • the unit area density of the positive electrode powder coating is 150-350mg/m 2 and the compacted density of the positive electrode piece is 3.0-3.6g/cm 3. The optional 3.3-3.5g/cm 3 .
  • the calculation formula of the compacted density is
  • Compaction density coating surface density / (thickness of electrode piece after extrusion - thickness of current collector).
  • the negative electrode sheet includes a negative electrode current collector and a negative electrode film layer disposed on at least one surface of the negative electrode current collector, where the negative electrode film layer includes a negative electrode active material.
  • the negative electrode current collector has two opposite surfaces in its own thickness direction, and the negative electrode film layer is disposed on any one or both of the two opposite surfaces of the negative electrode current collector.
  • the negative electrode current collector may be a metal foil or a composite current collector.
  • the composite current collector may include a polymer material base layer and a metal layer formed on at least one surface of the polymer material base material.
  • the composite current collector can be formed by forming metal materials (copper, copper alloy, nickel, nickel alloy, titanium, titanium alloy, silver and silver alloy, etc.) on a polymer material substrate (such as polypropylene (PP), polyterephthalate It is formed on substrates such as ethylene glycol ester (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
  • PP polypropylene
  • PBT polybutylene terephthalate
  • PS polystyrene
  • PE polyethylene
  • the negative active material may be a negative active material known in the art for batteries.
  • the negative active material may include at least one of the following materials: artificial graphite, natural graphite, soft carbon, hard carbon, silicon-based materials, tin-based materials, lithium titanate, and the like.
  • the silicon-based material may be selected from at least one of elemental silicon, silicon oxide compounds, silicon carbon composites, silicon nitrogen composites and silicon alloys.
  • the tin-based material may be selected from at least one of elemental tin, tin oxide compounds and tin alloys.
  • the present application is not limited to these materials, and other traditional materials that can be used as battery negative electrode active materials can also be used.
  • the negative active material may have an average particle diameter (D 10 ) of 1 ⁇ m to 15 ⁇ m, preferably 4 ⁇ m to 9 ⁇ m, an average particle diameter (D 50 ) of 12 ⁇ m to 22 ⁇ m, preferably 14 ⁇ m to 17 ⁇ m, and 26 ⁇ m to 40 ⁇ m, preferably Average particle size (D 90 ) of 30 ⁇ m-37 ⁇ m.
  • D 10 is the particle size corresponding to when the cumulative volume distribution percentage of the sample reaches 10%
  • D 50 is the particle size corresponding to when the cumulative volume distribution percentage of the sample reaches 50%
  • D 90 is the corresponding particle size when the cumulative volume distribution percentage of the sample reaches 90%. particle size.
  • the weight ratio of the negative active material in the negative electrode film layer is 70-100% by weight, based on the total weight of the negative electrode film layer.
  • the negative electrode film layer optionally further includes a binder.
  • the binder can be selected from styrene-butadiene rubber (SBR), polyacrylic acid (PAA), polysodium acrylate (PAAS), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium alginate (SA), poly At least one of methacrylic acid (PMAA) and carboxymethyl chitosan (CMCS).
  • SBR styrene-butadiene rubber
  • PAA polyacrylic acid
  • PAAS polysodium acrylate
  • PAM polyacrylamide
  • PVA polyvinyl alcohol
  • SA sodium alginate
  • PMAA methacrylic acid
  • CMCS carboxymethyl chitosan
  • the negative electrode film layer optionally further includes a conductive agent.
  • the conductive agent may be selected from at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene and carbon nanofibers.
  • the weight ratio of the conductive agent in the negative electrode film layer is 0-20% by weight, based on the total weight of the negative electrode film layer.
  • the negative electrode film layer optionally includes other auxiliaries, such as thickeners (such as sodium carboxymethylcellulose (CMC-Na)) and the like.
  • the weight ratio of the other additives in the negative electrode film layer is 0-15% by weight, based on the total weight of the negative electrode film layer.
  • the negative electrode sheet can be prepared by dispersing the above-mentioned components for preparing the negative electrode sheet, such as negative active materials, conductive agents, binders and any other components in a solvent (such as deionized water) to form a negative electrode slurry, wherein the solid content of the negative electrode slurry is 30-70wt%, and the viscosity at room temperature is adjusted to 2000-10000mPa ⁇ s; the negative electrode slurry is coated on the negative electrode current collector and dried , cold pressing and other processes, the negative electrode piece can be obtained.
  • the negative electrode powder coating unit area density is 75-220mg/m 2
  • the negative electrode plate compacted density is 1.2-2.0g/m 3 .
  • the electrolyte plays a role in conducting ions between the positive and negative electrodes.
  • the type of electrolyte in this application can be selected according to needs.
  • the electrolyte can be liquid, gel, or completely solid.
  • the electrolyte is an electrolyte solution.
  • the electrolyte solution includes electrolyte salts and solvents.
  • the electrolyte salt may be selected from the group consisting of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium hexafluoroarsenate, lithium bisfluorosulfonimide, lithium bistrifluoromethanesulfonimide, trifluoromethane At least one of lithium sulfonate, lithium difluorophosphate, lithium difluoroborate, lithium dioxaloborate, lithium difluorodioxalate phosphate and lithium tetrafluoroxalate phosphate.
  • the concentration of the electrolyte salt is usually 0.5-5mol/L.
  • the solvent may be selected from the group consisting of ethylene carbonate, propylene carbonate, methylethyl carbonate, diethyl carbonate, dimethyl carbonate, dipropyl carbonate, methylpropyl carbonate, ethylpropyl 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 optionally further includes additives.
  • additives may include negative electrode film-forming additives, positive electrode film-forming additives, and may also include additives that can improve certain properties of the battery, such as additives that improve battery overcharge performance, additives that improve battery high-temperature or low-temperature performance, etc.
  • the secondary battery further includes a separator film.
  • a separator film There is no particular restriction on the type of isolation membrane in this application. Any well-known porous structure isolation membrane with good chemical stability and mechanical stability can be used.
  • the material of the isolation membrane can be selected from at least one of glass fiber, non-woven fabric, polyethylene, polypropylene and polyvinylidene fluoride.
  • the isolation film can be a single-layer film or a multi-layer composite film, with no special restrictions. When the isolation film is a multi-layer composite film, the materials of each layer can be the same or different, and there is no particular limitation.
  • the thickness of the isolation film is 6-40 ⁇ m, optionally 12-20 ⁇ m.
  • the positive electrode piece, the negative electrode piece and the separator film can be made into an electrode assembly through a winding process or a lamination process.
  • the secondary battery may include an outer packaging.
  • the outer packaging can be used to package the above-mentioned electrode assembly and electrolyte.
  • the outer packaging of the secondary battery may be a hard shell, such as a hard plastic shell, an aluminum shell, a steel shell, etc.
  • 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 bag may be plastic, and examples of the plastic include polypropylene, polybutylene terephthalate, polybutylene succinate, and the like.
  • FIG. 1 shows a square-structured 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 side plates connected to the bottom plate, and the bottom plate and the side plates enclose a receiving cavity.
  • the housing 51 has an opening communicating with the accommodation cavity, and the cover plate 53 can cover the opening to close the accommodation cavity.
  • the positive electrode piece, the negative electrode piece and the isolation film can be formed into the electrode assembly 52 through a winding process or a lamination process.
  • the electrode assembly 52 is packaged in the containing cavity.
  • the electrolyte soaks into 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 specific actual needs.
  • secondary batteries can be assembled into battery modules, and the number of secondary batteries contained in the battery module can be one or more. Those skilled in the art can select the specific number according to the application and capacity of the battery module.
  • FIG. 3 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 .
  • the plurality of secondary batteries 5 can be fixed by fasteners.
  • the battery module 4 may further include a housing having a receiving space in which a plurality of secondary batteries 5 are received.
  • 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. Those skilled in the art can select the specific number 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 2 and a lower box 3 .
  • the upper box 2 can be covered with the lower box 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 electrical device, which includes at least one of the secondary battery, battery module, or battery pack provided by the present application.
  • the secondary battery, battery module, or battery pack may be used as a power source for the electrical device, or may be used as an energy storage unit for the electrical device.
  • the electric device may include mobile devices (such as mobile phones, laptops, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, and electric golf carts). , electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc., but are not limited to these.
  • a secondary battery, a battery module or a battery pack can be selected according to its usage requirements.
  • FIG. 6 is an electrical device as an example.
  • the electric device is a pure electric vehicle, a hybrid electric vehicle, a plug-in hybrid electric vehicle, etc.
  • a battery pack or battery module can be used.
  • the device may be a mobile phone, a tablet, a laptop, etc.
  • the device is usually required to be thin and light, and a secondary battery can be used as a power source.
  • a transition metal salt solution is prepared according to a molar ratio of Mn and Ni elements of 7:3. The concentration of the solution is 2 mol/L.
  • Salt solution, sodium carbonate solution and ammonia solution are pumped into the reaction kettle at the same time, and the pH of the reaction system is controlled by adjusting the feed flow rate v2 of the sodium carbonate solution to 9.5.
  • the temperature of the reaction system is maintained at 50°C and the stirring speed is 800 rpm/min. React for 20h.
  • the reaction slurry is aged for 10 hours, and then the precipitate is filtered, washed and dried to obtain the lithium-rich manganese-based cathode active material precursor Ni 0.3 Mn 0.7 CO 3 .
  • the lithium-rich manganese-based cathode active material precursor Ni 0.3 Mn 0.7 CO 3 (Dv50 is 8 ⁇ m) prepared above was crushed by high-energy ball milling in a nitrogen atmosphere to obtain primary particles (Dv50) of the lithium-rich manganese-based cathode active material precursor. is 0.3 ⁇ m).
  • Add the fast ion conductor precursor lithium borate, the metal compound conductive agent titanium boride and the dispersant polyvinylpyrrolidone to the water and stir at 800 rpm/min to mix evenly, and then add primary particles of the lithium-rich manganese-based cathode active material precursor to the water. , stir and mix evenly at 500 rpm/min to obtain a suspension of a solid mixture.
  • the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based cathode active material precursor in the solid mixture is 6.1:3.1:90.8.
  • the suspension of the above solid mixture was then spray-dried and granulated twice (manufacturer: Buqi; model: B-290).
  • the air inlet temperature of the spray drying was 250°C and the nozzle diameter was 600 ⁇ m to obtain the positive electrode active material precursor. powder.
  • the above-mentioned positive electrode active material precursor powder and lithium source lithium carbonate were evenly mixed at a weight ratio of 100:50, and then sintered at 800°C for 8 hours in an air atmosphere to obtain the positive electrode active material.
  • [Positive electrode sheet] Mix the above positive active material, conductive agent acetylene black, and binder polyvinylidene fluoride (PVDF) in the N-methylpyrrolidone solvent system in a weight ratio of 92:2.5:5.5, and then coat Put it on aluminum foil, dry it, and cold-press it to obtain the positive electrode piece.
  • the coating amount is 0.4g/cm 2 and the compacted density is 2.4g/cm 3 .
  • [Negative electrode sheet] Mix the negative active material artificial graphite, conductive agent carbon black, and binder styrene-butadiene rubber (SBR) in deionized water at a weight ratio of 92:2:6, then apply it on the copper foil and dry it , cold pressing to obtain the negative electrode piece.
  • the coating amount is 0.2g/cm 2 and the compacted density is 1.7g/cm 3 .
  • isolation film The isolation film is purchased from Cellgard Company, the model is cellgard2400.
  • Electrode Mix ethylene carbonate (EC), ethyl methyl carbonate (EMC), and diethyl carbonate (DEC) in a volume ratio of 1:1:1, and then uniformly dissolve LiPF 6 in the above solution to obtain electrolysis liquid, in which the concentration of LiPF 6 is 1mol/L.
  • the bare battery core is placed in the outer packaging, electrolyte is injected and packaged, and then through chemical formation and volume separation, a lithium-ion secondary full battery (hereinafter also referred to as "full battery”) is obtained.
  • the length ⁇ width ⁇ height of the full battery 148mm ⁇ 28.5mm ⁇ 97.5mm, and the group margin of the battery is 91.0%.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor in the solid mixture is 0.4:3.0: 96.6.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor in the solid mixture is 1.5:3.0: 95.5.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor in the solid mixture is 5.4:3.0: 91.6.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor in the solid mixture is 9.3:3.1: 87.6.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor in the solid mixture is 15.7:3.2: 81.1.
  • the preparation of the secondary battery is the same as in Example 1, except that the Dv50 of the lithium-rich manganese-based cathode active material precursor Ni 0.3 Mn 0.7 CO 3 is 5 ⁇ m.
  • the preparation of the secondary battery is the same as in Example 1, except that the Dv50 of the lithium-rich manganese-based cathode active material precursor Ni 0.3 Mn 0.7 CO 3 is 13 ⁇ m.
  • the preparation of the secondary battery is the same as in Example 1, except that the Dv50 of the lithium-rich manganese-based cathode active material precursor Ni 0.3 Mn 0.7 CO 3 is 20 ⁇ m.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor (Dv50 is 7 ⁇ m) in the solid mixture is 6.0:0.4:93.6.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor (Dv50 is 7 ⁇ m) in the solid mixture is 6.0:0.8:93.2.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor (Dv50 is 8 ⁇ m) in the solid mixture is 6.1:2.3:91.6.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor (Dv50 is 8 ⁇ m) in the solid mixture is 6.2:4.6:89.2.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the weight ratio of lithium borate, titanium boride and lithium-rich manganese-based positive active material precursor (Dv50 is 10 ⁇ m) in the solid mixture is 6.2:7.8:86.0.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the fast ion conductor precursor is silicon dioxide.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the fast ion conductor precursor is lithium phosphate.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the metal compound conductive agent is titanium nitride.
  • the preparation of the secondary battery is the same as in Example 1, except that in the preparation of the positive active material, the metal compound conductive agent is titanium carbide.
  • the preparation of the secondary battery is the same as in Example 1, except that in (2) the preparation of the positive electrode active material, the lithium-rich manganese-based positive electrode active material precursor Ni 0.3 Mn 0.7 CO 3 obtained in (1) is directly mixed with the lithium source After mixing lithium carbonate evenly with a weight ratio of 100:50, it was sintered at 800°C for 8 hours in an air atmosphere to obtain a lithium-rich manganese-based cathode active material 0.4Li 2 MnO 3 ⁇ 0.6LiNi 0.5 Mn 0.5 O 2 , and use the rich Lithium manganese-based cathode active materials are used to prepare button batteries.
  • the particle size of the cathode active material is measured according to GB/T 19077.1-2016/ISO 13320:2009 (particle size distribution laser diffraction method). Take a clean beaker, add an appropriate amount of the above positive active material, add an appropriate amount of pure water, and ultrasonic at 120W/5min to ensure that the material powder is completely dispersed in the water.
  • the solution is poured into the injection tower of the laser particle size analyzer (Malvern Company, model: Mastersizer3000) and then circulated to the test optical system with the solution.
  • the particles are irradiated by the laser beam and can be obtained by receiving and measuring the energy distribution of the scattered light.
  • Particle size distribution characteristics (opacity: 8-12%), read the corresponding value of Dv50.
  • a line scan (Line Scan Analysis) is performed on the materials in the display screen.
  • the acceleration voltage is 50kV
  • the amplification factor is 100kx
  • the beam current is between 500 and 1000pA.
  • the coating layer and the surface of the lithium-rich manganese-based base material are determined according to the proportion of the corresponding element numbers, so that the thickness of the coating layer can be obtained.
  • the thickness of the coating layer was measured at 5 randomly selected positions on the positive active material particles, and the arithmetic average of the measurement results was taken.
  • the secondary batteries of each example and comparative example were charged to 4.35V at a constant current rate of 0.1C, then charged at a constant voltage until the current was 0.05C, left to stand for 5 minutes, and then discharged at a constant current rate of 0.1C to 2V, record the discharge capacity at this time, which is the 0.1C discharge capacity; let it stand for 30 minutes, then charge the secondary battery with a constant current at a rate of 1C to 4.35V, then charge with a constant voltage until the current is 0.05C, let it stand for 5 minutes, and then Discharge to 2V at a constant current rate of 1C, and record the discharge capacity at this time, which is the 1C discharge capacity;
  • the secondary batteries of each example and comparative example were discharged to 2.5V at 1/3C. Let it stand for 5 minutes, charge to 4.3V at 1/3C, and then charge at a constant voltage of 4.3V until the current is ⁇ 0.05mA. Let it stand for 5 minutes, and record the charging capacity at this time as C0. Discharge to 2.5V according to 1/3C, let it sit for 5 minutes, then charge to 4.3V according to 3C, let it stand for 5 minutes, and record the charging capacity at this time as C1.
  • the 3C charging constant current ratio is C1/C0*100%.
  • the cathode active material of the present application has better cycle performance and rate performance. This is precisely because of the The cathode active material is a secondary particle formed by stacking primary particles. A homogeneous composite coating layer forming a continuous ion and electron channel is constructed on the outer surface of the matrix material of the primary particle, which is conducive to the transmission of ions and electrons.

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Abstract

La présente invention concerne un matériau actif d'électrode positive. Le matériau actif d'électrode positive est constitué de particules secondaires qui sont formées par empilement de particules primaires, les particules primaires comprenant un matériau de matrice à base de manganèse riche en lithium et une couche de revêtement, qui est située sur la surface du matériau de matrice à base de manganèse riche en lithium, la couche de revêtement comprenant un conducteur d'ions rapide et un agent conducteur de composé métallique. Le matériau actif d'électrode positive présente une performance de cyclage et une capacité de débit améliorées. La présente invention concerne en outre un procédé de préparation du matériau actif d'électrode positive, et une plaque d'électrode positive, une batterie secondaire, un module de batterie, un bloc-batterie et un dispositif électrique qui comprennent le matériau actif d'électrode positive de la présente invention.
PCT/CN2022/112738 2022-08-16 2022-08-16 Matériau actif d'électrode positive et son procédé de préparation, plaque d'électrode positive, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique WO2024036472A1 (fr)

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PCT/CN2022/112738 WO2024036472A1 (fr) 2022-08-16 2022-08-16 Matériau actif d'électrode positive et son procédé de préparation, plaque d'électrode positive, batterie secondaire, module de batterie, bloc-batterie et dispositif électrique

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US20220045325A1 (en) * 2020-08-06 2022-02-10 Dongguan Poweramp Technology Limited Positive electrode material, electrochemical device containing same, and electronic device

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CN105428637A (zh) * 2014-09-18 2016-03-23 宁德时代新能源科技有限公司 锂离子电池及其正极材料和正极材料的制备方法
CN105047921A (zh) * 2015-07-14 2015-11-11 宁夏共享新能源材料有限公司 锂离子电池正极材料复合磷酸铁锂及其制备方法和锂离子电池
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