CN111446488A - Secondary battery and device thereof - Google Patents
Secondary battery and device thereof Download PDFInfo
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- CN111446488A CN111446488A CN202010365063.2A CN202010365063A CN111446488A CN 111446488 A CN111446488 A CN 111446488A CN 202010365063 A CN202010365063 A CN 202010365063A CN 111446488 A CN111446488 A CN 111446488A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/028—Positive electrodes
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Abstract
The present application relates to a secondary battery and a device thereof. The secondary battery comprises a positive pole piece, wherein the positive pole piece comprises a positive current collector and a positive active material layer, and the positive active material layer is positioned on the surface of the positive current collector and comprises a first positive active material and a second positive active material which have different working voltage platforms; and the lithium ion solid phase diffusion coefficient of the positive pole piece is 10‑17cm2·s‑1～10‑5cm2·s‑1And the resistance of the positive pole piece is 0.05-2 omega. The power performance of the secondary battery provided by the application is obviously improved under the conditions of low temperature, particularly low temperature and low SOC.
Description
Technical Field
The present invention relates to the field of batteries, and in particular, to a secondary battery and a device thereof.
Background
Lithium ion batteries are widely used in electric vehicles and consumer electronics because of their advantages of high energy density, high output power, long cycle life, and low environmental pollution. During the driving process of the electric vehicle, the power requirement on the driving power supply is high, and therefore, the lithium ion battery is also required to have better power characteristics.
Temperature is one of the most significant environmental factors affecting the charge and discharge performance of a battery, and the power performance of a lithium ion battery is reduced in a low temperature environment. In addition, the state of charge (SOC) of the battery reflects the ratio of the remaining capacity of the battery to the battery capacity, and the power performance of the lithium ion battery is often affected in the low SOC state. Therefore, the conventional lithium ion battery has poor performance in the aspects of low-temperature and low-SOC power, working condition energy efficiency, low-temperature capacity, energy conservation rate and other key performances.
The application is provided for overcoming the defects of the prior art.
Disclosure of Invention
In view of this, embodiments of the present application provide a secondary battery and a device thereof.
In a first aspect, the present application provides a secondary battery, including a positive electrode plate, where the positive electrode plate includes a positive electrode current collector and a positive electrode active material layer, where the positive electrode active material layer is located on a surface of the positive electrode current collector, where the positive electrode active material layer includes a first positive electrode active material and a second positive electrode active material having different working voltage platforms; the lithium ion solid phase diffusion coefficient of the positive pole piece is 10-17cm2·s-1～10-5cm2·s-1Preferably 10-13cm2·s-1～10-9cm2·s-1(ii) a The resistance of the positive pole piece is 0.05-2 omega, preferably 0.1-1.5 omega.
In a second aspect, the present application provides a device comprising a secondary battery as in the first aspect of the present application, which can be used as a power source for the device and also as an energy storage unit for the device.
Compared with the prior art, the technical scheme of the application has at least the following beneficial effects.
The secondary battery provided by the application comprises a first positive active material and a second positive active material which have different working voltage platforms in a positive active material layer of a positive pole piece, the charging and discharging platforms of the two positive active materials are complementary and generate a synergistic effect, and better matching is realized through ion conduction performance and electron conduction performance of the pole piece, so that the lithium ion solid phase diffusion coefficient and the resistance of the positive pole piece are in a better range. Therefore, the secondary battery comprising the positive pole piece has the key performances of power, working condition energy efficiency, low-temperature capacity, energy conservation rate and the like under low temperature, particularly low temperature and low SOC.
The device of the present application includes the secondary battery provided by the present application, and thus has at least the same advantages as the secondary battery.
Drawings
The secondary battery and the device according to the present invention will be described in detail below with reference to the accompanying drawings and embodiments.
Fig. 1 is a perspective view of a secondary battery according to an embodiment of the present application as a lithium ion secondary battery;
fig. 2 is an exploded view of the lithium ion secondary battery shown in fig. 1;
FIG. 3 is a perspective view of a battery module according to an embodiment of the present application;
fig. 4 is a perspective view of a battery pack according to an embodiment of the present application;
fig. 5 is an exploded view of the battery pack of fig. 4;
FIG. 6 is a schematic view of an apparatus according to an embodiment of the present application;
wherein the reference numerals are as follows:
1, a battery pack;
2, putting the box body on the box body;
3, discharging the box body;
4 a battery module;
5 a secondary battery;
51, outer packaging;
52 an electrode assembly;
53 a cap assembly.
Detailed Description
The present application is further described below in conjunction with the detailed description. It should be understood that these specific embodiments are merely illustrative of the present application and are not intended to limit the scope of the present application.
Secondary battery
The application provides a secondary battery, positive pole piece includes anodal mass flow body and anodal active material layer, anodal active material layer is located anodal mass flow body surface, wherein, anodal active material layer is including the anodal active material of first positive pole active material and the anodal active material of second that have different operating voltage platforms, the lithium ion solid phase diffusion coefficient of positive pole piece is 10-17cm2·s-1～10-5cm2·s-1Preferably 10-13cm2·s-1～10-9cm2·s-1(ii) a The resistance of the positive electrode plate is 0.05-2 omega, preferably 0.1-1.5 omega, and more preferably 0.2-1 omega.
The lithium ion solid phase diffusion coefficient of the positive pole piece represents the diffusion mass transfer speed of lithium ions in the pole piece, and particularly refers to the quantity of lithium ion substances vertically passing through the pole piece in unit area in unit time in a porous electrode under the unit concentration gradient condition. The resistance of the positive pole piece reflects the electron conductivity of the pole piece, and the resistance value of the pole piece is small, so that the electron conductivity of the pole piece is good, the ohmic polarization is small, and the discharge platform is high at low temperature. In the embodiment of the application, the first positive active material and the second positive active material with different working voltage platforms are used in the positive pole piece of the secondary battery, and the first positive active material and the second positive active material are complementary through the charging and discharging platforms of the two positive active materials to generate a synergistic effect, so that the lithium ion solid phase diffusion coefficient and the resistance of the positive pole piece are in a better range, namely the ion conducting performance and the electron conducting performance of the pole piece are better matched. Therefore, the secondary battery comprising the pole piece has the key performances of power, working condition energy efficiency, low-temperature capacity, energy conservation rate and the like under low temperature, particularly low temperature and low SOC.
The first positive active material described herein may be selected from layered lithium nickel transition metal oxides.
In some embodiments of the present application, the layered lithium nickel transition metal oxide as the first positive electrode active material is selected from the group consisting of L ix1Ni(1-y1-z1-a1)Coy1Mnz1M1a1O2、Lix2Ni(1-y2-z2-a2)Coy2Alz2M2a2O2And one or more of composite materials obtained by coating and modifying the materials; wherein x1 is more than or equal to 0.90 and less than or equal to 1.05, y1 is more than 0 and less than or equal to 0.2, z1 is more than 0 and less than or equal to 0.2, a1 is more than or equal to 0 and less than or equal to 0.05, and M1 is selected from one or more of Ti, Al, Zr, Mg, Zn, Ba, Mo and B; x2 is more than or equal to 0.90 and less than or equal to 1.05, y2 is more than 0 and less than or equal to 0.1, z2 is more than 0 and less than or equal to 0.1, a2 is more than or equal to 0 and less than or equal to 0.05, and M2 is selected from one or more of Ti, Mn, Zr, Mg, Zn, Ba, Mo and B.
In some embodiments of the present application, the layered lithium nickel transition metal oxide as the first positive electrode active material is preferably selected from L ix1Ni(1-y1-z1-a1)Coy1Mnz1M1a1O2、Lix2Ni(1-y2-z2-a2)Coy2Alz2M2a2O2And one or more of composite materials obtained by coating and modifying the materials; wherein y1+ z1+ a1 is more than 0 and less than or equal to 0.4; y2+ z2+ a2 is more than 0 and less than or equal to 0.4.
Specifically, the layered lithium nickel transition metal oxides described herein include, but are not limited to, L iNi0.5Co0.2Mn0.3O2、LiNi0.5Co0.25Mn0.25O2、LiNi0.55Co0.15Mn0.3O2、LiNi0.55Co0.1Mn0.35O2、LiNi0.55Co0.05Mn0.4O2、LiNi0.6Co0.2Mn0.2O2、LiNi0.65Co0.15Mn0.2O2、LiNi0.65Co0.12Mn0.23O2、LiNi0.65Co0.1Mn0.25O2、LiNi0.65Co0.05Mn0.3O2、LiNi0.7Co0.1Mn0.2O2、LiNi0.75Co0.1Mn0.15O2、LiNi0.8Co0.1Mn0.1O2、LiNi0.85Co0.05Mn0.1O2、LiNi0.88Co0.05Mn0.07O2、LiNi0.9Co0.05Mn0.05O2、LiNi0.92Co0.03Mn0.05O2、LiNi0.95Co0.02Mn0.03O2And the like, the material can also be a material obtained by partially substituting and modifying the material by doping elements M1 or M2, wherein M1 is selected from one or more of Ti, Al, Zr, Mg, Zn, Ba, Mo and B, and M2 is selected from one or more of Ti, Mn, Zr, Mg, Zn, Ba, Mo and B.
The second positive electrode active material described in the present application is selected from olivine-type lithium-containing phosphates.
In some embodiments of the present application, the olivine-type lithium-containing phosphate as the second positive electrode active material is L iFe1-x3-y3Mnx3M’y3PO4Wherein x3 is more than or equal to 0 and less than or equal to 1, y3 is more than or equal to 0 and less than or equal to 0.1, x3+ y3 is more than or equal to 0 and less than or equal to 1, and M' is selected from one or more of transition metal elements except Fe and Mn and non-transition metal elements.
In other embodiments of the present application, the olivine-type lithium-containing phosphate as the second positive electrode active material is preferably a doping-modified L iFePO4、LiMnPO4、LiMn1-x4Fex4PO4Wherein 0 < x4 < 1.
Furthermore, the matching of the lithium ion solid-phase diffusion coefficient and the powder resistivity range of the first positive active material and the second positive active material and the proportion of the relative content of the first positive active material and the second positive active material enable the complementary effect of the charging and discharging platform of the two positive active materials to be more prominent, enable the matching degree of the ion conductivity and the conductivity of the positive pole piece to be better, and further remarkably improve the power performance of the battery cell under low temperature and low SOC. Based on this, some alternative embodiments provided by the present application are as follows:
in some embodiments of the present application, the first positive electrode active material has a lithium ion solid phase diffusion coefficient of 10- 13cm2·s-1～10-7cm2·s-1(ii) a In other embodiments of the present application, the first positive electrode active material preferably has a lithium ion solid phase diffusion coefficient of 10-11cm2·s-1～10-9cm2·s-1。
In some embodiments of the present application, the first positive electrode active material has a powder resistivity of 1000 Ω · cm to 20000 Ω · cm at 20 MPa; in some embodiments of the present application, the powder resistivity of the first positive electrode active material at 20MPa is preferably 2000 Ω · cm to 10000 Ω · cm; in another embodiment of the present application, the powder resistivity of the first positive electrode active material at 20MPa is more preferably 3000 Ω · cm to 6000 Ω · cm.
In some embodiments of the present application, the second positive electrode active material has a lithium ion solid phase diffusion coefficient of 10- 17cm2·s-1～10-11cm2·s-1(ii) a In some embodiments of the present application, the second positive electrode active material preferably has a lithium ion solid phase diffusion coefficient of 10-16cm2·s-1～10-13cm2·s-1(ii) a In other embodiments of the present application, the second positive electrode active material more preferably has a lithium ion solid phase diffusion coefficient of 10-15cm2·s-1～10-14cm2·s-1。
In some embodiments of the present application, the second positive electrode active material has a powder resistivity of 10 Ω · cm to 4000 Ω · cm at 20 MPa; in some embodiments of the present application, the powder resistivity of the second positive electrode active material at 20MPa is preferably 20 Ω · cm to 800 Ω · cm; in another embodiment of the present application, the powder resistivity of the second positive electrode active material at 20MPa is more preferably 200 Ω · cm to 550 Ω · cm.
In some embodiments of the present application, the second positive electrode active material is present in an amount of 0.5 to 50% by mole of the positive electrode active material; in some embodiments of the present application, the second positive electrode active material is preferably contained in an amount of 0.6 to 30% by mole of the positive electrode active material; in other embodiments of the present application, the second positive electrode active material is more preferably contained in an amount of 0.7 to 20% by mole of the positive electrode active material.
Further, the present application proposes a preferable form of the first positive electrode active material particle. In some embodiments of the present application, the particle morphology of the first positive electrode active material is single crystal particles, polycrystalline particles, or a mixture of single crystal particles and a small amount of polycrystalline particles; single crystal particles are preferred. The single crystal grains mean that the entirety of the crystal is composed of the same spatial lattice in the three-dimensional direction. Compared with polycrystalline particles, the single crystal particles have the characteristics of few interfaces, low specific surface area and high mechanical strength, are not easy to break in the processing and using processes, and particularly have fewer side reactions and higher chemical stability when used under high voltage.
Further, the present application also proposes a preferable mode of the average particle diameter of the second positive electrode active material. In some embodiments of the present application, the average particle diameter Dv50 of the second positive electrode active material is 1 μm to 15 μm; in some embodiments of the present application, the average particle diameter Dv50 of the second positive electrode active material is preferably 4.5 μm to 10 μm; in other embodiments of the present application, the average particle diameter Dv50 of the second positive electrode active material is more preferably 5 μm to 9 μm.
In the preferred embodiment of the present application, a first positive active material (ternary positive material single crystal particle) with a small average particle size and a second positive active material (lithium iron phosphate secondary particle) with a large average particle size are mixed to serve as the positive active material of the electrode plate of the present application, which is beneficial to improving the compaction density of the electrode plate, thereby improving the energy density of the battery cell.
Further, in some embodiments of the present application, the first positive electrode active material has an X-ray diffraction pattern in which I003/I110 is 2 to 20; in some embodiments of the present application, I003/I110 in an X-ray diffraction pattern of the first positive electrode active material is preferably 4 to 15; in other embodiments of the present application, I003/I110 in the X-ray diffraction pattern of the first positive electrode active material is more preferably 6 to 10.
In some embodiments of the present application, the first positive electrode active material has a lattice parameter c/a in an X-ray diffraction pattern of 2 to 7; in some embodiments of the present application, the first positive electrode active material preferably has a lattice parameter c/a in an X-ray diffraction pattern of 3 to 6.
As described above, the present application proposes the preferred embodiment of I003/I110 and lattice parameter c/a in the X-ray diffraction pattern of the first positive electrode active material. Wherein I003/I110 in the X-ray diffraction pattern of the first positive electrode active material is a diffraction peak intensity ratio of (003) planes to (110) planes on the XRD diffraction pattern of the first positive electrode active material, reflects the number and length of diffusion paths of lithium ions and the diffusion rate of lithium ions, and is an ion transport kinetic characteristic. In general, the smaller I003/I110, the better the kinetics of lithium ion transport. And the lattice parameter c/a in the X-ray diffraction pattern of the first positive electrode active material is the ratio of the c axis of the lattice parameter of the minimum composition unit (i.e. in an independent lattice) in the crystal structure to the a axis on the X-ray diffraction pattern of the first positive electrode active material, the c axis reflects the size of a lithium ion diffusion channel, and the a axis reflects the length of a lithium ion diffusion path. The larger the c/a is, the larger the diffusion channel is, the shorter the diffusion path is, and the faster the lithium ion diffusion transport is. By optimizing I003/I110 and lattice parameter c/a in an X-ray diffraction pattern of the first positive electrode active material, the ion conduction performance of the first positive electrode active material is in a better range, so that the matching of the ion conduction performance and the conductive performance of the pole piece is promoted.
Further, in some embodiments of the present application, the carbon coating content of the second positive electrode active material is 0.1% to 5% by mass, preferably 0.5% to 3% by mass, and more preferably 1% to 2% by mass. Within the above range, the second positive electrode active material has low powder resistivity, good conductivity, and good interface stability.
In some implementations of the present applicationIn a mode, the provided positive pole piece meets the following requirements: 0.41 < (R)d+Rct)/Rcat< 0.99, and 0.2 < Rct/RdLess than 2; wherein R iscatIs the total impedance, R, of the positive electrode sheetdIs the lithium ion diffusion resistance, R, of the positive electrode sheetctAnd transferring impedance to the charge of the positive pole piece. Under the conditions, the ionic conductivity and the electronic conductivity of the positive pole piece are optimally matched.
As described above, in the present application, two positive active materials having different working voltage platforms are mixed according to a certain ratio, and the material type, lithium ion solid phase diffusion coefficient, powder resistivity, particle morphology, particle size, carbon coating amount, and specific parameters in an X-ray diffraction pattern of the two positive active materials are optimized, so that the ionic conductivity and the electronic conductivity of a positive electrode sheet using the mixed positive active material are well matched, and thus, the critical performances of a secondary battery including the positive electrode sheet, such as power, working condition energy efficiency, low temperature capacity, energy retention rate, and the like at low temperature, especially at low temperature and low SOC, are significantly improved.
In addition, the positive pole piece of the application can also comprise a conductive agent and a binder, wherein the types and the contents of the conductive agent and the binder are not particularly limited and can be selected according to actual requirements. The binder typically includes a fluorinated polyolefin-based binder, and water is typically a good solvent relative to the fluorinated polyolefin-based binder, i.e., the fluorinated polyolefin-based binder typically has good solubility in water, for example, the fluorinated polyolefin-based binder may include, but is not limited to, polyvinylidene fluoride (PVDF), vinylidene fluoride copolymers, or modified (e.g., carboxylic acid, acrylic acid, acrylonitrile, etc.) derivatives thereof, and the like. In the positive electrode material layer, the mass percentage content of the binder may be that the binder itself has poor conductivity, and thus the amount of the binder used cannot be excessively high. Preferably, the mass percentage content of the binder in the positive active material layer is less than or equal to 2 wt%, so as to obtain lower pole piece impedance. The conductive agent of the positive electrode tab may be various conductive agents suitable for a lithium ion (secondary) battery in the art, and for example, may be one or a combination of more of acetylene black, conductive carbon black, carbon fiber (VGCF), Carbon Nanotube (CNT), ketjen black, and the like.
In the positive pole piece of this application, the kind of anodal mass flow body does not also not receive specific restriction, can select according to actual demand. The positive electrode current collector may be generally a layer body, and is generally a structure or a part that can collect current, and the positive electrode current collector may be various materials suitable for being used as a positive electrode current collector of an electrochemical energy storage device in the art, for example, the positive electrode current collector may include, but is not limited to, a metal foil, and more specifically, may include, but is not limited to, a nickel foil, an aluminum foil.
The preparation method of the positive pole piece comprises the following steps:
mixing the first positive electrode active substance and the second positive electrode active substance in a solvent according to a molar percentage, adding a conductive agent, a binder and the like to obtain a mixed slurry with the viscosity of 3000mPa & s-20000 mPa & s, and standing the mixed slurry for 24-48 hours to obtain the positive electrode active material slurry which is not gelled, delaminated or settled. The slurry is coated on an electrode current collector (or is coated on a primer layer of the electrode current collector in advance), then is dried, and finally is subjected to post-treatment and welding of an electric connection component to prepare the required positive pole piece. In some embodiments, the positive electrode active material layer may be formed after forming the electrical connection member on the current collector.
The solvent used for mixing the first positive electrode active material and the second positive electrode active material may be one or more selected from water, N-dimethylpyrrolidone (NMP), N-Dimethylformamide (DMF), dimethyl sulfoxide (DMSO), ethanol, glycerol, and the like, and the viscosity of the resulting mixed slurry is 3000mPa · s to 20000mPa · s.
The viscosity of the mixed slurry can be measured by adopting a viscometer, the model of the equipment is Brookfield DV2T L V, reference standard GB/T10247-.
Fig. 1 is a perspective view illustrating a secondary battery according to an embodiment of the present invention as a lithium ion secondary battery, and fig. 2 is an exploded view of the lithium ion secondary battery shown in fig. 1. Referring to fig. 1 and 2, a lithium ion secondary battery 5 (hereinafter referred to simply as a battery cell 5) according to the present application includes an exterior package 51, an electrode assembly 52, a cap assembly 53, and an electrolyte (not shown). The number of the electrode assemblies 52 is not limited, and may be one or more, wherein the electrode assemblies 52 are accommodated in the outer package 51.
It should be noted that the battery cell 5 shown in fig. 1 is a can-type battery, but the present application is not limited thereto, and the battery cell 5 may be a pouch-type battery, that is, the housing 51 is replaced by a metal plastic film and the top cover assembly 53 is eliminated.
The configuration and production method of the secondary battery of the present application are known per se, except for using the above-described positive electrode sheet containing the first positive electrode active material and the second positive electrode active material.
In the lithium ion secondary battery of the present application, the negative electrode tab generally includes a negative electrode current collector and a negative electrode active material layer, which generally includes a negative electrode active material, on a surface of the negative electrode current collector. The negative active material may be any of a variety of materials suitable for use in negative active materials for electrochemical energy storage devices in the art, and may, for example, include, but is not limited to, graphite, soft carbon, hard carbon, carbon fiber, mesocarbon microbeads, silicon-based materials, tin-based materials, lithium titanate, or a combination of one or more of other metals capable of forming an alloy with lithium. Wherein, the graphite can be selected from one or more of artificial graphite, natural graphite and modified graphite; the silicon-based material can be selected from one or more of elemental silicon, silicon-oxygen compound, silicon-carbon compound and silicon alloy; the tin-based material may be selected from elemental tin, tin-oxygen compounds, tin alloys, or combinations of one or more thereof. The negative electrode current collector is generally a structure or part that collects current and may be any of a variety of materials suitable for use as a negative electrode current collector for an electrochemical energy storage device in the art, for example, the negative electrode current collector may include, but is not limited to, a metal foil, and more specifically, may include, but is not limited to, a copper foil. In addition, the negative pole piece can also be a lithium piece.
In the lithium ion secondary battery of the present application, the specific kind and composition of the separator and the electrolyte are not particularly limited and may be selected according to actual needs, and specifically, the separator may be selected from a polyethylene film, a polypropylene film, a polyvinylidene fluoride film, and a multi-layered composite film thereof4、LiPF6、LiBF4、LiAsF6、LiSbF6Etc. inorganic lithium salt, or L iCF3SO3、LiCF3CO2、Li2C2F4(SO3)2、LiN(CF3SO2)2、LiC(CF3SO2)3、LiCnF2n+1SO3(n is more than or equal to 2) and the like. Examples of the organic solvent used in the nonaqueous electrolytic solution include cyclic carbonates such as ethylene carbonate, propylene carbonate, butylene carbonate and vinylene carbonate, linear carbonates such as dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate, linear esters such as methyl propionate, cyclic esters such as γ -butyrolactone, linear ethers such as dimethoxyethane, diethyl ether, diglyme and triglyme, cyclic ethers such as tetrahydrofuran and 2-methyltetrahydrofuran, nitriles such as acetonitrile and propionitrile, and mixtures of these solvents.
In some embodiments, the lithium ion secondary battery may be assembled into a battery module, and the number of the lithium ion secondary batteries contained in the battery module may be plural, and the specific number may be adjusted according to the application and capacity of the battery module. Fig. 3 is a battery module 4 as an example. Referring to fig. 3, in the battery module 4, a plurality of lithium ion secondary batteries 5 may be arranged in series along the longitudinal direction of the battery module 4. Of course, the arrangement may be in any other manner. The plurality of lithium-ion secondary batteries 5 may be further fixed by a fastener. Alternatively, the battery module 4 may further include a case having an accommodation space in which the plurality of lithium ion secondary batteries 5 are accommodated.
In some embodiments, the battery modules may be assembled into a battery pack, and the number of the battery modules contained in the battery pack may be adjusted according to the application and capacity of the battery pack. Fig. 4 and 5 are a battery pack 1 as an example. Referring to fig. 4 and 5, a battery pack 1 may include a battery case and a plurality of battery modules 4 disposed in the battery case. The battery box comprises an upper box body 2 and a lower box body 3, wherein the upper box body 2 can be covered on the lower box body 3 and forms a closed space for accommodating the battery module 4. A plurality of battery modules 4 may be arranged in any manner in the battery box.
Device for measuring the position of a moving object
A second aspect of the present application provides a device comprising the secondary battery of the first aspect of the present application, the secondary battery being used as a power source for the device and also as an energy storage unit for the device. The devices include, but are not limited to, mobile devices (e.g., mobile phones, laptop computers, etc.), electric vehicles (e.g., electric cars, hybrid electric cars, plug-in hybrid electric cars, electric bicycles, electric scooters, electric golf carts, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, and the like.
The device may select a secondary battery, a battery module, or a battery pack according to its use requirements.
Fig. 6 shows a schematic view of an apparatus according to an embodiment of the present application. The device can be a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle, etc. In order to meet the demand of the device for high power and high energy density of the lithium ion secondary battery (i.e., the secondary battery of the present application), a battery pack or a battery module may be employed.
As another example, the device may be a cell phone, a tablet, a laptop, etc. The device is generally required to be thin and light, and a lithium ion secondary battery (i.e., a secondary battery of the present application) may be used as a power source.
Those skilled in the art will understand that: the above-mentioned various limitations or preferred ranges for the component selection, component content and material physical and chemical property parameters of the electrode sheet, electrode active material layer and the like in the different embodiments of the present application can be combined arbitrarily, and the various embodiments obtained by combining the above-mentioned components are still within the scope of the present application and are considered as part of the disclosure of the present specification.
Unless otherwise specified, various parameters referred to in this specification have the common meaning known in the art and can be measured according to methods known in the art. For example, the test can be performed according to the method given in the examples of the present application. In addition, the preferred ranges and options for the various parameters given in the various preferred embodiments can be combined arbitrarily, and the various combinations thus obtained are considered to be within the scope of the disclosure of the present application.
The present application is further illustrated below with reference to specific examples and comparative examples. It should be understood that these examples are for illustrative purposes only and are not intended to limit the scope of the present application.
Examples
The preparation methods of the positive electrode active materials in the respective examples and comparative examples are as follows.
1. Preparation of positive electrode active material
Mixing the first positive electrode active substance and the second positive electrode active substance in a solvent N-dimethyl pyrrolidone (NMP) according to a molar percentage to obtain mixed slurry with the viscosity of 3000mPa & s-20000 mPa & s, and standing the mixed slurry for 24-48 hours to obtain positive electrode active material slurry which is not gelled, delaminated and settled.
2. Preparation of Positive electrode sheet
Fully stirring and mixing a positive electrode active material, conductive carbon and a binder polyvinylidene fluoride (PVDF) in a proper amount of N-methyl pyrrolidone (NMP) solvent according to a weight ratio of 95:3:2 to form uniform positive electrode slurry; coating the slurry on a positive current collector Al foil, drying, and then cold-pressing the pole piece to a designed compact for standby strip division to obtain the positive pole piece.
3. Preparation of the electrolyte
And dissolving an equal volume of ethylene carbonate in propylene carbonate, and uniformly dissolving a proper amount of lithium hexafluorophosphate in the mixed solvent for later use to obtain the electrolyte.
4. Preparation of negative electrode plate
Fully stirring and mixing the negative active material graphite, conductive carbon and a binder polyvinylidene fluoride (PVDF) in a proper amount of aqueous solvent according to the weight ratio of 95:3:2 to form uniform negative slurry; coating the slurry on a Cu foil of a negative current collector, drying, and then cold-pressing the pole piece to a designed compact for standby.
5. Providing a barrier film
A PE film is selected as an isolating film.
6. Preparation of a Battery
The positive pole piece (compacted density: 3.4 g/cm) is processed by the conventional battery manufacturing process3) Separator and negative electrode sheet (compacted density: 1.6g/cm3) And winding the raw materials into a bare cell, then placing the bare cell into a battery shell, injecting electrolyte, sealing, forming and other processes, and finally obtaining the lithium ion secondary battery (hereinafter referred to as the battery).
Test method
1) Method for testing lithium ion diffusion coefficient of positive pole piece and positive active material
The method can be obtained by adopting conventional methods in the field such as a deduction electric CV method, an EIS method, a GITT method, a PITT method and the like and calculating according to Fick first and second laws.
Taking the GITT method as an example, the procedure for testing the lithium ion diffusion coefficient of the first positive electrode active material or the second positive electrode active material is as follows:
grinding the first positive electrode active substance or the second positive electrode active substance into the powder micro-electrode; the powder microelectrode was connected to an electrochemical workstation and coulometric titration was performed. The titration time was 1 hour, and the pause was 4 hours at a pulse current of 20. mu.A. (Note: to compare the influence of pulse current and time, parallel experiment 10 muA, 10min) was performed, after obtaining the GITT curve, the lithium ion diffusion coefficient was calculated using the following formula:
wherein D is the diffusion coefficient of lithium ions; i is0The applied current is 20 muA, Vm is the molar volume of the active material, F is the Faraday constant, A is the electrode surface area, dE/dx is the slope of the coulometric titration curve, i.e. the slope at a certain concentration on the curve of open circuit potential versus L i concentration in the electrode, (dE)/(dt)1/2) Is a pair of polarization voltages t1/2The slope of the curve. Specific references may be found in: xiiet al, Solid State Ionics,2007,178: 1218-; yang et al, Electrochimica Acta,2012,66: 88-93.
2) Method for testing resistance of positive pole piece
Adopt day BT3562 type internal resistance tester to carry out the resistance of positive pole piece, include: and clamping the positive pole piece between two conductive terminals of the internal resistance tester, applying pressure for fixing, and testing the resistance R of the positive pole piece, wherein the diameter of the conductive terminals is 14mm, the applied pressure is 15 MPa-27 MPa, and the sampling point time range is 5 s-17 s. .
3) Powder resistivity testing method under 20MPa of positive electrode active substance
The positive active material powder was dried, and an appropriate amount of the powder was weighed, and then used with a powder resistivity tester, equipment model suzhou lattice ST2722 or mitsunm 7305. And (3) placing the dry powder sample in a mold/sample bin of a resistivity tester, wherein the depth of the sample bin is 20mm, and the sectional area is 1cm2, then slowly applying pressure from small to large, manually collecting data, and recording corresponding powder resistivity test results at different pressure points.
4) Method for testing first positive electrode active material I (003)/I (110) and lattice parameter c/a
The measuring instrument is an X-ray powder diffractometer, the model is Brucker rD 8A-A25 of Brucker Axs company in Germany, a polycrystalline sample is irradiated by monochromatic X-rays, theta is changed by utilizing different orientations of crystals to meet the Bragg equation to generate diffraction peaks, the generated diffraction peaks are utilized to carry out qualitative analysis on the crystal structure and calculate lattice parameters, for example, CuK α rays are used as a radiation source, and the wavelength of the rays is calculated
The angle range of the scanning 2 theta is 10-150 degrees, and the scanning speed is 4 degrees/min. After the diffraction pattern of the powder is obtained, the obtained diffraction pattern is compared with the diffraction pattern in the existing crystal database, such as PDF database, so as to obtain the crystal phase corresponding to the material and the crystal face corresponding to each peak. And then performing simulation according to calculation or by using crystal structure simulation software, for example, calculating the a axis and the c axis of the material according to the hexagonal system formula 1/d2 ═ 4(h2+ hk + k2)/3a2+ l2/c2, and calculating the integrated ratio of the peak intensities of (003) and (110) to obtain I003/I110, wherein the length ratio of the c axis to the a axis is c/a.
5) Method for testing average particle diameter of second positive electrode active material
The measuring instrument: a laser particle size analyzer; the equipment model is as follows: malvern Mastersizer 2000E or Mastersizer 3000. Under the irradiation of laser beam, the angle of scattered light of the positive electrode material particle is in inverse proportion to the particle diameter, the scattered light intensity is logarithmically attenuated along with the increase of the angle, the energy distribution of the scattered light is directly related to the particle diameter distribution, and the particle size distribution characteristic of the particle can be obtained by receiving and measuring the energy distribution of the scattered light. The solvent used for the test can be water or other organic solvent used for preparing the slurry, and the sample is dispersed using ultrasound. The obtained analysis result Dv50I.e. 50% of the total volume has a particle diameter greater than this value and 50% of the total volume has a particle diameter less than this value, expressed as Dv50To indicate the median particle size of the powder.
6) Method for determining mass percentage content of carbon coating of second positive electrode active material
The measuring instrument: C/S content analyzer; the equipment model Dekjex HCS-140. The carbon content in the powder is tested by using a high-frequency induction furnace post-combustion infrared absorption method (conventional method) GBT 20123-2006 according to the determination of the total carbon and sulfur content of the steel. Burning the sample in oxygen to convert carbon and sulfur into CO2、SO2And the signal is converted into a corresponding signal by a detector after entering the absorption cell. The signal is sampled by a computer, and is converted into CO after linear correction2、SO2The concentration is proportional to the value, then the values of the whole analysis process are accumulated, and after the analysis is finished, the accumulation is carried outDividing the value by the weight value in a computer, multiplying by a correction coefficient, and deducting blank to obtain the percentage contents of carbon and sulfur in the sample.
7) Positive pole piece Rd、Rct、RcatTest method
Rcat,、Rd,、RctThe method comprises the steps of obtaining an alternating-current impedance spectrum through the EIS test, deeply analyzing impedance composition by combining an equivalent circuit diagram and an impedance decomposition model to obtain a Nyquist diagram and a bode diagram, then fitting by using Z-view or EC-L ab software, and improving the coincidence degree of a simulation diagram and a practical diagram by adjusting the numerical value of each impedance, wherein the higher the coincidence degree is, the more accurate the impedance result is.
8) Method for testing 273K capacity retention rate of lithium ion battery
Selecting a fresh battery core, using a battery charging and discharging machine and a high-low temperature box, and testing the standard rate discharge capacity of the battery at a specified temperature, wherein the ratio of the discharge capacity to the charge capacity is the capacity retention rate. Relevant terminology and test methods refer to GB/T19596 and GB/T31486.
9) Method for testing 253K power @ 5% SOC of lithium ion battery
Selecting a fresh battery core, and testing the power performance of the battery at a specified temperature and a specified SOC by using a battery charging and discharging machine and a high-low temperature box. Relevant terminology and test methods refer to GB/T19596 and GB/T31486.
Test results and discussion
Specific parameters of electrochemical properties of the positive electrode active material, the positive electrode sheet and the lithium ion secondary battery of examples 1 to 9 and comparative examples 1 to 2 are shown in tables 1 to 4.
Table 1 first positive electrode active material parameters
Table 2 second positive electrode active material parameters
TABLE 3 Positive active Material and Positive Pole piece Performance parameters
TABLE 4 electrochemical Properties of lithium ion batteries
| 273K capacity retention ratio | 253K Power @ 5% SOC [ W ]] | |
| Example 1 | 92％ | 212 |
| Example 2 | 91％ | 207 |
| Example 3 | 90％ | 198 |
| Example 4 | 90％ | 172 |
| Example 5 | 91％ | 159 |
| Example 6 | 92％ | 205 |
| Example 7 | 93％ | 187 |
| Example 8 | 93％ | 167 |
| Example 9 | 93％ | 191 |
| Comparative example 1 | 66％ | 47 |
| Comparative example 2 | 60％ | 39 |
As can be seen from the analysis of the data in tables 1 to 4, compared with comparative examples 1 and 2, in examples 1 to 9, because the first positive electrode active material and the second positive electrode active material having different working voltage platforms are used, the charging and discharging platforms of the two positive electrode active materials are complementary and generate a synergistic effect, so that the ion conductivity and the electron conductivity of the electrode plate are well matched, the lithium ion solid-phase diffusion coefficient and the resistance of the positive electrode plate are in a better range, and the rate capability of the lithium ion secondary battery in a low-temperature low-SOC state is significantly improved. In addition, on the basis of complementing charge and discharge platforms of the two positive electrode active materials, the method further improves the aspects of conductivity, crystallinity, order degree and the like of the positive electrode active materials from the aspects of lithium ion solid phase diffusion coefficient, powder resistivity, particle form, particle size, carbon coating amount, X-ray diffraction spectrum key parameters and the like of the selected first positive electrode active material and the second positive electrode active material, and improves the dynamics and the charge and discharge performance of the battery.
Those skilled in the art will understand that: the application example of the pole piece of the present application is only shown by taking a lithium battery as an example, but the pole piece of the present application can be applied to other types of batteries or secondary batteries, and still can obtain the good technical effects of the present application.
Appropriate changes and modifications to the embodiments described above will become apparent to those skilled in the art from the disclosure and teachings of the foregoing specification. Therefore, the present application is not limited to the specific embodiments disclosed and described above, and some modifications and variations of the present application should fall within the scope of the claims of the present application. In addition, although specific terms are used herein, they are used in a descriptive sense only and not for purposes of limitation.
Claims (11)
1. A secondary battery comprises a positive pole piece, the positive pole piece comprises a positive pole current collector and a positive pole active material layer, the positive pole material layer is positioned on the surface of the positive pole current collector,
the positive electrode active material layer comprises a first positive electrode active material and a second positive electrode active material which have different working voltage platforms;
the lithium ion solid phase diffusion coefficient of the positive pole piece is 10-17cm2·s-1～10-5cm2·s-1Preferably 10-13cm2·s-1～10-9cm2·s-1；
The resistance of the positive pole piece is 0.05-2 omega, preferably 0.1-1.5 omega.
2. The secondary battery according to claim 1,
the first positive electrode active material is selected from layered lithium nickel transition metal oxides;
preferably, the layered lithium nickel transition metal oxide is selected from the group consisting of L ix1Ni(1-y1-z1-a1)Coy1Mnz1M1a1O2、Lix2Ni(1-y2-z2-a2)Coy2Alz2M2a2O2And one or more of composite materials obtained by coating and modifying the materials;
wherein x1 is more than or equal to 0.90 and less than or equal to 1.05, y1 is more than 0 and less than or equal to 0.2, z1 is more than 0 and less than or equal to 0.2, a1 is more than or equal to 0 and less than or equal to 0.05, and M1 is selected from one or more of Ti, Al, Zr, Mg, Zn, Ba, Mo and B; x2 is more than or equal to 0.90 and less than or equal to 1.05, y2 is more than 0 and less than or equal to 0.1, z2 is more than 0 and less than or equal to 0.1, a2 is more than or equal to 0 and less than or equal to 0.05, and M2 is selected from one or more of Ti, Mn, Zr, Mg, Zn, Ba, Mo and B;
more preferably, 0 < y1+ z1+ a1 ≦ 0.4; y2+ z2+ a2 is more than 0 and less than or equal to 0.4.
3. The secondary battery according to claim 1,
the second positive electrode active material is selected from an olivine-type lithium-containing phosphate;
preferably, the olivine lithium-containing phosphate is L iFe1-x3-y3Mnx3M’y3PO4Wherein x3 is more than or equal to 0 and less than or equal to 1, y3 is more than or equal to 0 and less than or equal to 0.1, x3+ y3 is more than or equal to 0 and less than or equal to 1, and M' is selected from one or more of transition metal elements except Fe and Mn and non-transition metal elements;
more preferably, the olivine-type lithium-containing phosphate is selected from the group consisting of doped modified L iFePO4、LiMnPO4、LiMn1- x4Fex4PO4Wherein 0 < x4 < 1.
4. The secondary battery according to claim 1,
the first positive electrode active material has a lithium ion solid phase diffusion coefficient of 10-13cm2·s-1～10-7cm2·s-1More preferably 10-11cm2·s-1～10-9cm2·s-1(ii) a And the number of the first and second electrodes,
the first positive electrode active material has a powder resistivity of 1000 to 20000 Ω · cm, preferably 2000 to 10000 Ω · cm, and more preferably 3000 to 6000 Ω · cm under 20 MPa.
5. The secondary battery according to claim 1,
the second positive electrode active material has a lithium ion solid phase diffusion coefficient of 10-17cm2·s-1～10-11cm2·s-1Preferably 10-16cm2·s-1～10-13cm2·s-1More preferably 10-15cm2·s-1～10-14cm2·s-1(ii) a And the number of the first and second electrodes,
the second positive electrode active material has a powder resistivity of 10 to 4000 Ω · cm, preferably 20 to 800 Ω · cm, and more preferably 200 to 550 Ω · cm, at 20 MPa.
6. The secondary battery according to claim 1, wherein the second positive electrode active material is contained in an amount of 0.5 to 50 mol%, preferably 0.6 to 30 mol%, and more preferably 0.7 to 20 mol% based on the positive electrode active material.
7. The secondary battery according to claim 1, wherein the particle morphology of the first positive electrode active material is selected from single crystal particles, polycrystalline particles, or a mixture thereof, preferably single crystal particles.
8. The secondary battery according to claim 1,
the first positive electrode active material has an X-ray diffraction pattern with an I003/I110 ratio of 2-20, preferably 4-12, and more preferably 6-10; and/or the presence of a gas in the gas,
the lattice parameter c/a in the X-ray diffraction pattern of the first positive electrode active material is 2-7, preferably 3-6.
9. The secondary battery according to claim 1,
the second positive electrode active material has an average particle diameter Dv50 of 1 to 15 μm, preferably 4.5 to 13.5 μm, and more preferably 5 to 9 μm; and/or the presence of a gas in the gas,
the carbon coating of the second positive electrode active material is 0.1 to 5% by mass, preferably 0.5 to 3% by mass, and more preferably 1 to 2% by mass.
10. The secondary battery according to claim 1, wherein the positive electrode sheet satisfies:
0.41＜(Rd+Rct)/Rcat< 0.99, and 0.2 < Rct/Rd＜2；
Wherein R iscatIs the total impedance, R, of the positive electrode sheetdIs the lithium ion diffusion resistance, R, of the positive electrode sheetctAnd transferring impedance to the charge of the positive pole piece.
11. A device comprising the secondary battery according to any one of claims 1 to 10, the secondary battery serving as a power source of the device or an energy storage unit of the device.
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