CN118712453A - Secondary batteries and devices - Google Patents

Secondary batteries and devices Download PDF

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Publication number
CN118712453A
CN118712453A CN202311717222.0A CN202311717222A CN118712453A CN 118712453 A CN118712453 A CN 118712453A CN 202311717222 A CN202311717222 A CN 202311717222A CN 118712453 A CN118712453 A CN 118712453A
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negative electrode
active material
lithium
secondary battery
equal
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李思远
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Weilai Battery Technology Anhui Co ltd
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Weilai Battery Technology Anhui Co ltd
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Priority to CN202311717222.0A priority Critical patent/CN118712453A/en
Publication of CN118712453A publication Critical patent/CN118712453A/en
Priority to PCT/CN2024/128007 priority patent/WO2025123962A1/en
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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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • 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
    • H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/362—Composites
    • 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
    • H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)

Abstract

本申请提供了二次电池及装置，该二次电池包括正极极片、负极极片和电解液，负极极片包括负极活性材料层以及位于负极活性材料层表面的负极固体电解质界面膜；采用X射线光电子能谱仪测试，负极固体电解质界面膜中硫元素的质量百分含量为Z％；负极活性材料层包括负极活性材料，负极活性材料表面有碳包覆层；每100g负极活性材料对应Y g的碳包覆层；电解液包含碳酸亚乙烯酯和含硫添加剂；每100g负极活性材料对应在电解液中添加T g碳酸亚乙烯酯；该二次电池满足：0.5≤Y/T+Z/50≤2.6。本申请通过调控单位负极活性材料对应的碳酸亚乙烯酯含量、负极活性材料表面的碳包覆量以及负极固体电解质界面膜中硫含量，以提高负极极片成膜稳定性，降低二次电池的阻抗，提高其循环寿命和低温性能。The present application provides a secondary battery and a device, the secondary battery comprises a positive electrode plate, a negative electrode plate and an electrolyte, the negative electrode plate comprises a negative electrode active material layer and a negative electrode solid electrolyte interface film located on the surface of the negative electrode active material layer; the mass percentage of sulfur element in the negative electrode solid electrolyte interface film is Z% as tested by an X-ray photoelectron spectrometer; the negative electrode active material layer comprises a negative electrode active material, and a carbon coating layer is provided on the surface of the negative electrode active material; a carbon coating layer of Y g corresponds to each 100g of the negative electrode active material; the electrolyte comprises vinylene carbonate and a sulfur-containing additive; T g of vinylene carbonate is added to the electrolyte for each 100g of the negative electrode active material; the secondary battery satisfies: 0.5≤Y/T+Z/50≤2.6. The present application improves the film formation stability of the negative electrode plate, reduces the impedance of the secondary battery, and improves its cycle life and low temperature performance by regulating the vinylene carbonate content corresponding to the unit negative electrode active material, the carbon coating amount on the surface of the negative electrode active material, and the sulfur content in the negative electrode solid electrolyte interface film.

Description

Secondary battery and device
Technical Field
The application relates to the field of energy storage, in particular to a secondary battery and a device.
Background
The lithium ion battery has wide application in the aspects of smart phones, unmanned aerial vehicles, hybrid electric vehicles and the like, but with the development of society, the lithium ion battery with low energy density is difficult to meet the demand, and the development of a battery system with high capacity/high safety becomes the development direction of the lithium ion battery with high energy density.
The excellent thermal stability of the lithium iron phosphate battery is widely applied to the fields of power and energy storage batteries, and although the thermal stability is high, under a high-energy scene, the dynamic performance of the battery core is obviously reduced due to the high pole piece compaction density, so that the risk of lithium precipitation in the charge and discharge process is increased, and the problem limits the application of the lithium iron phosphate battery under the high-energy scene. In addition, the degree of matching of the electrolyte and the negative electrode material also affects the transmission of lithium ions at the negative electrode tab/electrolyte interface. If they are not well matched, the conductivity of lithium ions is reduced, the risk of lithium precipitation of the battery core is increased, and the cycle life of the lithium ion battery is shortened.
Therefore, in order to meet the social demand for high energy density batteries and solve the problems of lithium iron phosphate batteries in high energy scenarios, it is necessary to develop a novel battery system in which matching of electrolyte and anode materials and their interactions with anode materials all require intensive research.
Disclosure of Invention
In view of the above problems in the prior art, the present application provides a secondary battery and an apparatus. According to the application, the film forming stability of the negative electrode is improved, the lithium precipitation condition of the negative electrode is reduced, the overall impedance of the secondary battery is further reduced, and the cycle life and low-temperature performance of the secondary battery are improved by regulating and controlling the relationship among the ethylene carbonate content corresponding to the unit negative electrode active material, the carbon coating amount on the surface of the negative electrode active material and the sulfur content in the negative electrode solid electrolyte interface film.
A first aspect of the present application provides a secondary battery including a positive electrode tab, a negative electrode tab, and an electrolyte, the negative electrode tab including a negative electrode active material layer and a negative electrode solid electrolyte interface film on a surface of the negative electrode active material layer; the method comprises the steps of testing by adopting an X-ray photoelectron spectrometer, wherein the mass percentage of sulfur element in the anode solid electrolyte interface film is Z%; the negative electrode active material layer comprises a negative electrode active material, and a carbon coating layer is arranged on the surface of the negative electrode active material; a carbon coating layer corresponding to Y g per 100g of anode active material; the electrolyte comprises vinylene carbonate and a sulfur-containing additive; each 100g of negative electrode active material is correspondingly added with T g ethylene carbonate into the electrolyte; the secondary battery satisfies the following conditions: Y/T+Z/50 is more than or equal to 0.5 and less than or equal to 2.6.
A second aspect of the present application provides an apparatus comprising the aforementioned secondary battery.
The technical scheme of the application can realize the following beneficial effects:
According to the application, the relationship among the content of vinylene carbonate corresponding to the unit anode active material, the carbon coating amount on the surface of the anode active material and the sulfur content in the anode solid electrolyte interface film is regulated so as to meet specific limiting conditions, thereby improving the anode film forming stability, reducing the anode lithium precipitation condition, further reducing the overall impedance of the secondary battery and improving the cycle life and low-temperature performance of the secondary battery. The reason is that the lithium precipitation condition of the battery cell is strongly related to the cycle performance, and in a limited range, the interface impedance of the solid electrolyte interface film (SEI) of the negative electrode can be effectively reduced by increasing the sulfur content in the SEI film, so that the lithium precipitation condition of the battery cell is reduced; the carbon coating content on the surface of the negative electrode is increased, so that the ion/electron transmission rate of an electrode/electrolyte interface can be increased, and the diffusion resistance of lithium ions is reduced, thereby reducing the high-rate lithium precipitation condition; by reducing the content of ethylene carbonate in the electrolyte, the thickness and the polymer content of the SEI film can be effectively reduced, so that the energy barrier of lithium ions crossing SEI is reduced, and the high-rate lithium precipitation condition is lightened.
Detailed Description
For the purpose of making the objects, technical solutions and advantages of the present application more apparent, the technical solutions of the present application will be clearly and completely described below with reference to the embodiments, and it is apparent that the described embodiments are some embodiments of the present application, but not all embodiments. The related embodiments described herein are of illustrative nature and are intended to provide a basic understanding of the application. The embodiments of the present application should not be construed as limiting the application.
For simplicity, only a few numerical ranges are specifically disclosed herein. However, any lower limit may be combined with any upper limit to form a range not explicitly recited; and any lower limit may be combined with any other lower limit to form a range not explicitly recited, and any upper limit may be combined with any other upper limit to form a range not explicitly recited. Furthermore, each separately disclosed point or individual value may itself be combined as a lower limit or upper limit with any other point or individual value or with other lower limit or upper limit to form a range not explicitly recited.
In the description herein, unless otherwise indicated, "above", "below" includes this number.
Unless otherwise indicated, terms used in the present application have well-known meanings commonly understood by those skilled in the art. Unless otherwise indicated, the numerical values of the parameters set forth in the present application may be measured by various measurement methods commonly used in the art (e.g., may be tested according to the methods set forth in the examples of the present application).
The list of items to which the term "at least one of," "at least one of," or other similar terms are connected may mean any combination of the listed items. For example, if items a and B are listed, the phrase "at least one of a and B" means only a; only B; or A and B. In another example, if items A, B and C are listed, the phrase "at least one of A, B and C" means only a; or only B; only C; a and B (excluding C); a and C (excluding B); b and C (excluding A); or A, B and C. Item a may comprise a single component or multiple components. Item B may comprise a single component or multiple components. Item C may comprise a single component or multiple components.
1. Secondary battery
One or more embodiments of the present application provide a secondary battery including a positive electrode tab, a negative electrode tab, and an electrolyte, the negative electrode tab including a negative electrode active material layer and a negative electrode solid electrolyte interface film on a surface of the negative electrode active material layer; the method comprises the steps of testing by adopting an x-ray photoelectron spectrometer, wherein the mass percentage of sulfur element in a cathode solid electrolyte interface film is Z%; the negative electrode active material layer comprises a negative electrode active material, and a carbon coating layer is arranged on the surface of the negative electrode active material; a carbon coating layer corresponding to Y g per 100g of anode active material; the electrolyte comprises vinylene carbonate and a sulfur-containing additive; adding Tg vinylene carbonate into the electrolyte for every 100g of negative electrode active material; the secondary battery satisfies the following conditions: Y/T+Z/50 is more than or equal to 0.5 and less than or equal to 2.6.
According to the application, the relationship among the ethylene carbonate content corresponding to the unit negative electrode active material, the carbon coating amount on the surface of the negative electrode active material and the sulfur content in the negative electrode solid electrolyte interface film is regulated, so that the conditions are met, the film forming stability of the negative electrode plate is improved, the lithium precipitation condition of the negative electrode plate is reduced, the overall impedance of the secondary battery is further reduced, and the cycle life and the low-temperature performance of the secondary battery are improved.
In some embodiments, Y/t+z/50 is 0.5, 0.6, 0.7, 0.8, 0.9, 1.0, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, 2.0, 2.1, 2.2, 2.3, 2.4, 2.5, 2.6, or a range of any two of the foregoing values.
In some embodiments, 1.0.ltoreq.Y/T+Z/50.ltoreq.2.2. In the limit range, the sulfur-containing component in the SEI film replaces a polymer component generated by Vinylene Carbonate (VC), the SEI film impedance is reduced, meanwhile, the improvement of the carbon content on the surface of the anode active material can effectively accelerate the migration rate of lithium ions, lighten the lithium precipitation of a battery core, and further improve the cycle life and the low-temperature energy retention rate of the secondary battery.
In some embodiments, 1.5.ltoreq.T.ltoreq.2.5. By defining the content of Vinylene Carbonate (VC) corresponding to a unit negative electrode active material, a stable and low-impedance negative electrode solid electrolyte interface film (SEI) is formed on a negative electrode tab, and the reduced content of vinylene carbonate can improve the low-temperature performance of a secondary battery, but can affect the cycle life of the secondary battery; the content of Vinylene Carbonate (VC) corresponding to the unit cathode active material is limited in the reasonable range so as to ensure the cycle life and the low-temperature performance of the secondary battery. In some embodiments, T is 1.5, 1.6, 1.7, 1.8, 1.9, 2.0, 2.1, 2.2, 2.3, 2.4, 2.5, or a range of any two of the foregoing values. In some embodiments, 1.5.ltoreq.T.ltoreq.2.4.
In some embodiments, 1.5.ltoreq.Y.ltoreq.4.0. The excessive thickness of the carbon coating layer can cause larger loss of active lithium during the charge and discharge of the first ring of the battery; the carbon coating layer is too thin, so that the interface dynamics of the negative electrode plate is insufficient, and lithium precipitation is generated under the high-rate condition of the battery cell; the carbon coating amount on the surface of the anode active material is controlled within the range, so that the transmission process of lithium ions among anode particles can be accelerated, the lithium ion conductivity is maximized in the battery cell, the occurrence of lithium precipitation is reduced, and the cycle life and low-temperature performance of the battery cell are improved. In some embodiments, Y is 1.5、1.6、1.7、1.8、1.9、2.0、2.1、2.2、2.3、2.4、2.5、2.6、2.7、2.8、2.9、3.0、3.1、3.2、3.3、3.4、3.5、3.6、3.7、3.8、3.9、4.0 or a range of any two of the values described above. In some embodiments, 2.ltoreq.Y.ltoreq.3.5.
In some embodiments, 0.01.ltoreq.Z.ltoreq.15. In the SEI film, too high sulfur content Z can lead to the reduction of corresponding polymer components, the reduction of SEI mechanical properties and the influence on long-cycle performance; the low sulfur content Z can cause the increase of the impedance of the SEI film, and the energy barrier of lithium ions crossing SEI is improved, so that the lithium precipitation risk of the battery cell is improved; the sulfur content Z is controlled in the range, so that the excellent mechanical property of the SEI film and the moderate lithium ion crossing energy barrier are both facilitated, and the high-multiplying power long-cycle of the battery cell is realized. In some embodiments, Z is 0.01, 0.05, 0.1, 0.5, 1, 1.5, 2,4, 6, 8, 10, 12, 14, 15, or a range of any two of the foregoing values. In some embodiments, 5.ltoreq.Z.ltoreq.10.
In some embodiments, the sulfur-containing additive includes at least one of a sulfonate, a sulfate, and a sulfite. The sulfur-containing additive can improve the composition and structure of the SEI film, so that the SEI film is lower and stable in resistance, side reactions can be effectively inhibited from continuously occurring due to contact of electrolyte and anode active materials, the electrolyte is consumed, lithium ion crossing energy barriers are reduced, and the cycle life of the secondary battery is prolonged.
In some embodiments, the sulfonate ester includes at least one of 1, 3-propane sultone (1, 3-PS), 1-propylene-1, 3-sultone (PST), and 1, 4-butane sultone (1, 4-BS).
In some embodiments, the sulfate comprises at least one of vinyl sulfate (DTD), 4-methyl ethylene sulfate (PCS), 4-ethyl ethylene sulfate (PES), 4-propyl ethylene sulfate (PEGLST), and propylene sulfate (TS).
In some embodiments, the sulfite comprises at least one of ethylene sulfite (DTO), dimethyl sulfite (DMS), and diethyl sulfite (DES).
In some embodiments, the sulfur-containing additive is present in an amount of 0.05% to 5% by mass. In some embodiments, the sulfur-containing additive is present in an amount of 0.05%, 0.1%, 0.2%, 0.3%, 0.4%, 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1.0%, 1.5%, 2.0%, 2.5%, 3.0%, 3.5%, 4.0%, 4.5%, 5.0% by mass, or any value therebetween. In some embodiments, the sulfur-containing additive is present in an amount of 0.1% to 3% by mass.
In some embodiments, the electrolyte further comprises other additives including at least one of a fluorine-containing cyclic carbonate, a fluorine-containing lithium salt. In some embodiments, the other additives include at least one of fluoroethylene carbonate, lithium difluorophosphate, and lithium difluorooxalato borate. Other additives can synergistically optimize the components and mechanical properties of the SEI film, and improve the long-cycle stability of the SEI film.
In some embodiments, the other additives are present in an amount of 0.05% to 10% by mass based on the mass of the electrolyte. In some embodiments, the other additive is present in an amount of 0.05%, 0.1%, 0.2%, 0.3%, 0.4%, 0.5%, 0.6%, 0.7%, 0.8%, 0.9%, 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10% by mass or a range of any two values recited above. In some embodiments, the other additives are present in an amount of 0.1% to 8% by mass.
In some embodiments, the electrolyte further includes a lithium salt including at least one of lithium hexafluorophosphate (LiPF 6), lithium tetrafluoroborate (LiBF 4), lithium difluorooxalato borate (lipfob), lithium bisoxalato borate (LiBOB), lithium bisfluorosulfonyl imide (LiFSI), and lithium bis (trifluoromethylsulfonyl) imide (LiTFSI).
In some embodiments, the electrolyte further comprises a nonaqueous solvent comprising at least one of a chain carbonate compound, a cyclic carbonate compound, and a carboxylate compound.
In some embodiments, the chain carbonate compound includes, but is not limited to, one or more of dimethyl carbonate (DMC), diethyl carbonate (DEC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), or ethylmethyl carbonate (MEC).
In some embodiments, the cyclic carbonate compound includes, but is not limited to, one or more of Ethylene Carbonate (EC), propylene Carbonate (PC), butylene Carbonate (BC), or Vinyl Ethylene Carbonate (VEC).
In some embodiments, the carboxylate compound includes, but is not limited to, one or more of methyl formate, methyl acetate, ethyl acetate, n-propyl acetate, t-butyl acetate, methyl propionate, ethyl propionate, propyl propionate, gamma-butyrolactone, decalactone, valerolactone, or caprolactone.
In some embodiments, the negative active material includes at least one of graphite, soft carbon, hard carbon, carbon nanotubes, graphene, silicon alloys, silicon oxygen compounds, silicon carbon compounds, metallic lithium, and lithium titanate.
In some embodiments, the anode active material layer further includes a binder and a conductive agent. Binders include, but are not limited to: at least one of polyvinyl alcohol, hydroxypropyl cellulose, diacetyl cellulose, polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, an ethyleneoxy-containing polymer, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, styrene-butadiene rubber, acrylated styrene-butadiene rubber, epoxy resin, nylon, or the like. Conductive agents include, but are not limited to: at least one of carbon-based materials, metal-based materials, conductive polymers, and mixtures thereof. In some embodiments, the carbon-based material comprises natural graphite, synthetic graphite, carbon black, acetylene black, ketjen black, carbon fiber, or any combination thereof. In some embodiments, the metal-based material comprises metal powder, metal fibers, copper, nickel, aluminum, or silver. In some embodiments, the conductive polymer includes a polyphenylene derivative.
In some embodiments, the negative electrode tab further comprises a negative electrode current collector comprising: at least one of copper foil, nickel foil, stainless steel foil, titanium foil, nickel foam, copper foam, a polymer substrate coated with a conductive metal, or any combination thereof.
In some embodiments, the positive electrode sheet includes a positive electrode active material layer including a positive electrode active material. The positive electrode active material includes at least one of a lithium iron phosphate-based material, a lithium cobalt oxide-based material, and a nickel cobalt-based material. In some embodiments, the lithium iron phosphate-based material includes at least one of a Li xFeyR(1-y)PO4 material, where R includes at least one of Mn, co, ti, mg, ca, cr, cu, ni, V, mo, zn, al, B and Nb, 0.05.ltoreq.x.ltoreq.1.2, 0 < y.ltoreq.1. In some embodiments, the lithium cobaltate-based material comprises at least one of a Li 1+zCo1-j-kMajMbkO2 material, wherein Ma is at least one of Al, ga, hf, mg, sn, zn and Zr; mb is at least one of Ni, mn, V, mo, nb, cu, fe, in, W and Cr, j is more than or equal to 0 and less than or equal to 0.01,0, k is more than or equal to 0.01, and z is more than or equal to 0.05 and less than or equal to 0.08. In some embodiments, the nickel cobalt-based material includes at least one of a Li aNimConA(1-m-n)O2 material, where A includes at least one of Mn, al, mg, cr, ca, zr, mo, ag or Nb, 0.9.ltoreq.a.ltoreq. 1.2,0.5.ltoreq.m.ltoreq.1, 0.ltoreq.n.ltoreq.0.5, and m+n.ltoreq.1.
In some embodiments, the positive electrode active material is preferably a lithium iron phosphate-based material, such as LiFePO 4. When the positive electrode active material is a lithium iron phosphate material, the relationship among the content of vinylene carbonate corresponding to the unit negative electrode active material in the system electrolyte, the carbon coating amount of the surface of the negative electrode active material and the sulfur content in the negative electrode solid electrolyte interface film is adapted, so that better film forming characteristics of the negative electrode plate can be obtained.
In some embodiments, the positive electrode active material layer further includes a binder, and optionally includes a conductive material. The binder enhances the bonding of the positive electrode active material particles to each other and also enhances the bonding of the positive electrode active material to the current collector.
In some embodiments, the binder includes, but is not limited to: polyvinyl alcohol, hydroxypropyl cellulose, diacetyl cellulose, polyvinyl chloride, carboxylated polyvinyl chloride, polyvinyl fluoride, an ethyleneoxy-containing polymer, polyvinylpyrrolidone, polyurethane, polytetrafluoroethylene, polyvinylidene fluoride, polyethylene, polypropylene, styrene-butadiene rubber, acrylated styrene-butadiene rubber, epoxy resin, nylon, or the like.
In some embodiments, the conductive material includes, but is not limited to: carbon-based materials, metal-based materials, conductive polymers, and mixtures thereof. In some embodiments, the carbon-based material is selected from natural graphite, synthetic graphite, carbon black, acetylene black, ketjen black, carbon fiber, or any combination thereof. In some embodiments, the metal-based material is selected from metal powder, metal fiber, copper, nickel, aluminum, or silver. In some embodiments, the conductive polymer is a polyphenylene derivative.
In some embodiments, the positive electrode tab further includes a positive electrode current collector, which may be a metal foil or a composite current collector. For example, aluminum foil may be used. The composite current collector may be formed by forming a metal material (copper, copper alloy, nickel alloy, titanium alloy, silver alloy, or the like) on a polymer substrate.
In some embodiments, a separator is provided between the positive and negative electrode sheets to prevent shorting. The materials and shape of the separator that can be used in the embodiments of the present application are not particularly limited, and may be any of the techniques disclosed in the prior art. In some embodiments, the separator comprises a polymer or inorganic, etc., formed from a material that is stable to the electrolyte of the present application.
In some embodiments, the barrier film comprises a base film comprising at least one of a polyethylene film, a polypropylene film, a PP/PE/PP composite film, a polyimide film, an aramid film, a polyethylene terephthalate film, or a nonwoven fabric, and a coating layer disposed on the base film. In some embodiments, the coating includes at least one of a polymer layer, an inorganic ceramic layer, or a hybrid layer of a polymer and an inorganic ceramic layer.
In some embodiments, the inorganic ceramic layer includes inorganic particles including at least one of aluminum oxide, silicon oxide, magnesium oxide, titanium oxide, hafnium oxide, tin oxide, cerium oxide, nickel oxide, zinc oxide, calcium oxide, zirconium oxide, yttrium oxide, silicon carbide, boehmite, aluminum hydroxide, magnesium hydroxide, calcium hydroxide, or barium sulfate, and a binder. The binder comprises at least one of polyvinylidene fluoride, copolymer of vinylidene fluoride-hexafluoropropylene, polyamide, polyacrylonitrile, polyacrylate, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, polymethyl methacrylate, polytetrafluoroethylene or polyhexafluoropropylene.
The polymer layer contains a polymer, and the material of the polymer comprises at least one of polyamide, polyacrylonitrile, acrylic polymer, polyacrylic acid, polyacrylate, polyvinylpyrrolidone, polyvinyl ether, polyvinylidene fluoride or poly (vinylidene fluoride-hexafluoropropylene).
In some embodiments, a method of manufacturing a secondary battery includes providing an electrode assembly, injecting a liquid, packaging, and forming. In some embodiments, the temperature of the formation is from 40 ℃ to 50 ℃, e.g., 40 ℃, 41 ℃, 42 ℃, 43 ℃, 44 ℃, 45 ℃, 46 ℃, 47 ℃, 48 ℃, 49 ℃, 50 ℃, or a range consisting of any two of the foregoing values.
In some embodiments, the forming comprises: the constant current charge is carried out for 120 minutes at 0.05C under the conditions of a temperature of 40-50 ℃, for example 45 ℃, a pressure of 130-300 kgf, for example 210kgf, the constant current and constant voltage charge is carried out at 0.1C to 3.8V, and the discharge is carried out at 0.2C to 2.3V.
In some embodiments, the secondary battery is a lithium secondary battery or a sodium secondary battery. In some embodiments, lithium secondary batteries include, but are not limited to: lithium metal secondary batteries, lithium ion secondary batteries, lithium polymer secondary batteries, or lithium ion polymer secondary batteries.
In some embodiments, the secondary battery may include an outer package, which may be a hard shell, such as a hard plastic shell, an aluminum shell, a steel shell, or the like. The exterior package of the secondary battery may also be a pouch type pouch, for example. The soft bag can be made of one or more of polypropylene (PP), polybutylene terephthalate (PBT), polybutylene succinate (PBS), etc.
In some embodiments, the shape of the secondary battery is not particularly limited, and may be cylindrical, square, or any other shape.
In some embodiments, the application also provides a battery module. The battery module includes the secondary battery described above. The battery module of the present application employs the above-described secondary battery, and thus has at least the same advantages as the secondary battery. The number of secondary batteries included in the battery module of the present application may be plural, and the specific number may be adjusted according to the application and capacity of the battery module.
In some embodiments, the application also provides a battery pack, which comprises the battery module. The number of battery modules included in the battery pack may be adjusted according to the application and capacity of the battery pack.
2. Device and method for controlling the same
The application also provides a device comprising at least one of the secondary battery, the battery module or the battery pack.
In some embodiments, the apparatus includes, but is not limited to: electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric storage systems, and the like. In order to meet the high power and high energy density requirements of the device for the secondary battery, a battery pack or a battery module may be employed.
In other embodiments, the device may be a cell phone, tablet, notebook, or the like. The device is generally required to be light and thin, and a secondary battery can be used as a power source.
Hereinafter, the secondary battery of the present application will be further described with reference to specific examples and comparative examples.
Examples and comparative examples
The present application will be described in further detail with reference to examples and comparative examples, but the present application is not limited to these examples unless departing from the gist thereof.
The materials, solvents, etc. used in the examples below were all commercially available.
Example 1
Preparing a positive electrode plate: the positive electrode active material LiFePO 4, conductive carbon black (superP) as a conductive agent and polyvinylidene fluoride (PVDF) as a binder are fully homogenized in an N-methylpyrrolidone NMP solvent system according to the weight ratio of LiFePO 4: superP:PVDF=97:1.5:1.5, and then uniformly coated on two surfaces of a positive electrode current collector aluminum foil with the thickness of 12 mu m, and the positive electrode plate is obtained by drying and rolling.
Preparing a negative electrode plate: artificial graphite as a cathode active material and a conductive agent superP, CMC, PAA are prepared by the following steps of: superP:CMC: PAA=96:2:1:1 in deionized water, and then coating the mixture on two surfaces of a negative current collector copper foil with the thickness of 8 mu m, and drying, rolling and stripping the mixture to obtain a negative electrode plate.
Preparation of electrolyte: in a glove box protected by nitrogen (moisture <1ppm, oxygen content <1 ppm), mixing Ethylene Carbonate (EC), dimethyl carbonate (DMC) and methyl ethyl carbonate (EMC) according to the mass ratio of EC to DMC to EMC=20 to 15 to 49.5, adding lithium hexafluorophosphate (LiPF 6) to the molar concentration of 1mol/L (12.5% by mass) based on the total mass of the electrolyte, adding 1.5% of ethylene carbonate (VC), 0.5% of ethylene sulfate (DTD) and 1% of fluoroethylene carbonate (FEC), and stirring uniformly to obtain the electrolyte.
Isolation film: a PE porous polymer film having a thickness of 11 μm was used as a separator.
Preparation of a lithium ion battery: sequentially stacking the prepared positive pole piece, the isolating film and the negative pole piece, enabling the isolating film to be positioned between the positive pole piece and the negative pole piece, and winding to obtain a bare cell; and placing the bare cell in an aluminum plastic film outer package, baking for 48 hours at 75 ℃ in vacuum, fully drying, injecting prepared lithium ion battery electrolyte, vacuum packaging, standing for 12 hours at normal temperature and 12 hours at 45 ℃, and then carrying out a formation and partial volume step to obtain the lithium ion battery. Wherein the step of forming the component comprises the following steps: charging at 45deg.C under 147kgf and 0.05C for 120min, charging at 0.1C for 60min, charging at 0.33C for 54min, standing at 45deg.C for 24 hr, 0.5C constant current constant voltage charge to 3.8V,0.33C constant current discharge to 2.3V,0.5C constant current constant voltage charge to 3.8V,0.33C discharge to 2.3V, and (5) circulating for two circles to finish the separation.
Examples 2 to 10
Examples 2 to 10 were carried out by adjusting the kind of the positive electrode active material, the kind and content of the sulfur-containing additive in the electrolyte, the content of vinylene carbonate, the kind and content of other additives, the carbon coating amount of the negative electrode active material, the sulfur content in the SEI solid electrolyte film, etc. on the basis of example 1, and specific adjustment measures and detailed data are shown in table 1. Other preparation methods were the same as in example 1.
Comparative example 1
Comparative example 1 differs from example 1 in the preparation of the electrolyte: in a glove box protected by nitrogen (moisture <1ppm, oxygen content <1 ppm), mixing Ethylene Carbonate (EC), dimethyl carbonate (DMC) and methyl ethyl carbonate (EMC) according to the mass ratio EC: DMC: emc=20:15:46.25, adding lithium hexafluorophosphate (LiPF 6) to a molar concentration of 1mol/L (mass percentage content of 12.5%), adding 5% of Vinylene Carbonate (VC), 0.25% of vinyl sulfate (DTD) and 1% of fluoroethylene carbonate (FEC), and stirring uniformly to obtain an electrolyte. Other preparation methods were the same as in example 1.
Comparative examples 2 to 7
Comparative examples 2 to 7 were achieved by adjusting the kind of the positive electrode active material, the kind and content of the sulfur-containing additive in the electrolyte, the content of vinylene carbonate, the kind and content of other additives, the carbon coating amount of the negative electrode active material, the sulfur content in the SEI solid electrolyte film, etc., based on comparative example 1, and specific adjustment measures and detailed data are shown in table 1. Other preparation methods were the same as in example 1.
Test method
1. X-ray photoelectron spectrometer (XPS) test
Discharging the lithium ion battery to 2.3V at the current of 0.1C, and dismantling the lithium ion battery in a glove box filled with argon to obtain the electrode plate. Cutting the obtained electrode plate into a test sample with the size of 8mm multiplied by 8mm, soaking and cleaning for half an hour by using a low-boiling point dimethyl carbonate DMC solvent, after the test sample is completely dried, pasting the test sample on a sample table of XPS, enabling the surface of the negative electrode active material layer, which is far away from a current collector, to face upwards, and measuring under the condition of not being exposed to the atmosphere.
The specific test conditions and steps are as follows: single crystal spectral alkα radiation was used, as for the X-ray spot, 1000X 1750 μm ellipse form output of 10KV and 22mA was used, 284.8eV was used for neutral carbon C1s, and as for data processing such as peak differentiation, 3-point smoothing, peak area measurement, background subtraction and peak synthesis were used to calculate atoms of each component.
2. -20 ℃ Energy retention test
And (3) charging the lithium ion battery to 3.8V under the constant current and constant pressure of 0.1C under the condition of normal temperature (25 ℃), discharging to 2.3V under the constant current and constant pressure of 0.1C, circulating for three times, and recording the averaged discharge energy data as normal temperature discharge energy S1. And then placing the battery cell at the temperature of minus 20 ℃, charging to 3.8V under the constant current and constant voltage of 0.1C, discharging to 2.3V under the constant current and constant voltage of 0.1C, recording low-temperature discharge energy S2, and calculating the energy retention rate as S2/S1.
3. Normal temperature cycle life test
Under the condition of normal temperature (25 ℃), the lithium ion battery is charged to 3.8V under the condition of constant current and constant voltage of 1C, and then discharged to 2.3V under the condition of constant current of 1C. When the capacity is less than 80% of the initial capacity, the cycle is stopped and the number of cycles is recorded.
4. DC impedance DCR test of battery cell
The lithium ion battery with the cycle capacity retention rate of 100 circles in the test is adjusted to the target SOC by using 0.33C current, the battery is kept still for 30 minutes, the voltage V 0 at the moment is recorded as the OCV of the corresponding SOC, the discharge current I 1 is used for discharging for t seconds, and the voltage V 1 of the t seconds is recorded; and calculating DCR by using a calculation formula of the discharge direct current internal resistance, wherein the formula is DCR= (V 0-V1)/I1).
5. Lithium precipitation test for negative electrode plate
After 300 circles of circulation, the lithium ion battery is flushed to 3.8V under constant current and constant pressure of 1C, then the fully charged core is disassembled, and the lithium precipitation condition at the negative pole piece is observed.
The test data are shown in Table 1 below.
TABLE 1
As can be seen from the data comparison results of examples 1 to 10 and comparative examples 1 to 7 in Table 1, the application makes the relationship among the ethylene carbonate content (T) corresponding to the unit negative electrode active material, the carbon coating amount (Y) on the surface of the negative electrode active material and the sulfur content (Z%) in the negative electrode solid electrolyte interface film satisfied 0.5 < Y/T+Z/50 < 2.6, and in the limit range, the negative electrode sheet does not or slightly precipitates lithium, the overall impedance of the secondary battery is remarkably reduced, the cycle number is more than 1700 circles, and the energy retention rate at low temperature is remarkably improved. The reason is that the lithium precipitation condition of the battery cell is strongly related to the cycle performance, and in a limited range, the interface impedance of the SEI film can be effectively reduced and the lithium precipitation condition of the battery cell can be reduced by increasing the sulfur content (Z%) in the Solid Electrolyte Interface (SEI) of the negative electrode; the carbon coating content (Y) on the surface of the negative electrode plate is increased, so that the ion/electron transmission rate of an electrode/electrolyte interface can be increased, and the diffusion resistance of lithium ions is reduced, thereby reducing the high-rate lithium precipitation condition; by reducing the ethylene carbonate content (T) in the electrolyte, the thickness and the polymer content of the SEI film can be effectively reduced, so that the energy barrier of lithium ions crossing SEI is reduced, and the high-rate lithium precipitation condition is lightened.
As can be seen from examples 1 to 5 and examples 6 to 10, the present application satisfies 1.0.ltoreq.Y/T+Z/50.ltoreq.2.2 by controlling the relationship among the vinylene carbonate content (T) corresponding to the unit anode active material, the carbon coating amount (Y) on the surface of the anode active material, and the sulfur content (Z%) in the anode solid electrolyte interface film, in which the anode electrode sheet does not precipitate lithium, the overall resistance of the secondary battery is further reduced, the number of cycles is 2100 or more, and the energy retention at low temperature is further improved. The reason is that in the limit range, the sulfur-containing component in the SEI film replaces the polymer component generated by Vinylene Carbonate (VC), the resistance of the SEI film is reduced, meanwhile, the improvement of the carbon content on the surface of the anode active material can effectively accelerate the migration rate of lithium ions, lighten the lithium precipitation of a battery core and further improve the cycle life and the low-temperature energy retention rate of the secondary battery.
While certain exemplary embodiments of the application have been illustrated and described, the application is not limited to the disclosed embodiments. Rather, one of ordinary skill in the art will recognize that certain modifications and changes may be made to the described embodiments without departing from the spirit and scope of the present application as described in the appended claims.

Claims (10)

1. A secondary battery, characterized in that the secondary battery comprises a positive electrode plate, a negative electrode plate and electrolyte, wherein the negative electrode plate comprises a negative electrode active material layer and a negative electrode solid electrolyte interface film positioned on the surface of the negative electrode active material layer; testing by adopting an X-ray photoelectron spectrometer, wherein the mass percentage of sulfur element in the anode solid electrolyte interface film is Z%;
The negative electrode active material layer comprises a negative electrode active material, and a carbon coating layer is arranged on the surface of the negative electrode active material; y g of the carbon coating layer for every 100g of the anode active material;
The electrolyte comprises vinylene carbonate and a sulfur-containing additive; each 100g of negative electrode active material is correspondingly added with T g ethylene carbonate into the electrolyte;
The secondary battery satisfies: Y/T+Z/50 is more than or equal to 0.5 and less than or equal to 2.6.
2. The secondary battery according to claim 1, wherein the secondary battery further satisfies at least one of the following conditions:
(1)1.0≤Y/T+Z/50≤2.2；
(2)1.5≤T≤2.5；
(3)1.5≤Y≤4.0；
(4)0.01≤Z≤15。
3. the secondary battery according to any one of claims 1 or 2, wherein the secondary battery further satisfies at least one of the following conditions:
(1)1.5≤T≤2.4；
(2)2≤Y≤3.5；
(3)5≤Z≤10。
4. The secondary battery according to any one of claims 1 or 2, wherein the sulfur-containing additive includes at least one of a sulfonate, a sulfate, and a sulfite; the sulfur-containing additive is contained in an amount of 0.05 to 5% by mass based on the mass of the electrolyte.
5. The secondary battery according to claim 4, wherein the sulfonate comprises at least one of methane disulfonic acid methylene ester, 1, 3-propane sultone, 1-propylene-1, 3-sultone, and 1, 4-butane sultone; and/or the number of the groups of groups,
The sulfate comprises at least one of vinyl sulfate, 4-methyl ethylene sulfate, 4-ethyl ethylene sulfate, 4-propyl ethylene sulfate and propylene sulfate; and/or the number of the groups of groups,
The sulfite includes at least one of ethylene sulfite, dimethyl sulfite and diethyl sulfite.
6. The secondary battery according to any one of claims 1 or 2, wherein the electrolyte further comprises other additives including at least one of a fluorine-containing cyclic carbonate and a fluorine-containing lithium salt; the mass content of the other additive is 0.05% to 10% based on the mass of the electrolyte.
7. The secondary battery according to claim 6, wherein the other additive includes at least one of fluoroethylene carbonate, lithium difluorophosphate and lithium difluorooxalato borate.
8. The secondary battery according to any one of claims 1 or 2, wherein the positive electrode sheet includes a positive electrode active material including at least one of a lithium iron phosphate-based material, a lithium cobalt oxide-based material, and a nickel cobalt-based material;
The lithium iron phosphate material comprises at least one of Li xFeyR(1-y)PO4 materials, wherein R comprises at least one of Mn, co, ti, mg, ca, cr, cu, ni, V, mo, zn, al, B and Nb, x is more than or equal to 0.05 and less than or equal to 1.2, and y is more than 0 and less than or equal to 1; and/or the number of the groups of groups,
The lithium cobaltate material comprises at least one of Li 1+zCo1-j-kMajMbkO2 materials, wherein Ma is at least one of Al, ga, hf, mg, sn, zn and Zr; mb is at least one of Ni, mn, V, mo, nb, cu, fe, in, W and Cr, j is more than or equal to 0 and less than or equal to 0.01,0, k is more than or equal to 0.01, and z is more than or equal to 0.05 and less than or equal to 0.08; and/or the number of the groups of groups,
The nickel-cobalt material comprises at least one of Li aNimConA(1-m-n)O2 materials, wherein A comprises at least one of Mn, al, mg, cr, ca, zr, mo, ag or Nb, a is more than or equal to 0.9 and less than or equal to 1.2,0.5 and less than or equal to m and less than or equal to 1, n is more than or equal to 0 and less than or equal to 0.5, and m+n is more than or equal to 1.
9. The secondary battery according to any one of claims 1 or 2, wherein the anode active material includes at least one of graphite, soft carbon, hard carbon, carbon nanotubes, graphene, silicon, a silicon alloy, a silicon oxygen compound, a silicon carbon compound, metallic lithium, and lithium titanate; and/or the number of the groups of groups,
The electrolyte further comprises a nonaqueous solvent and a lithium salt, wherein the nonaqueous solvent comprises at least one of a chain carbonate compound, a cyclic carbonate compound and a carboxylate compound; the lithium salt includes at least one of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium difluorooxalato borate, lithium bisoxalato borate, lithium bisfluorosulfonyl imide, and lithium bis (trifluoromethanesulfonyl) imide.
10. An apparatus, characterized in that the apparatus comprises the secondary battery according to any one of claims 1 to 9.
CN202311717222.0A 2023-12-13 2023-12-13 Secondary batteries and devices Pending CN118712453A (en)

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CN110391409A (en) * 2019-07-25 2019-10-29 昆山宝创新能源科技有限公司 Lithium cell cathode material and preparation method thereof and lithium battery
JP7322684B2 (en) * 2019-12-06 2023-08-08 Tdk株式会社 lithium ion secondary battery
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CN118712453A (en) * 2023-12-13 2024-09-27 蔚来电池科技(安徽)有限公司 Secondary batteries and devices

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