WO2020155993A1 - 负极极片、锂离子二次电池及装置 - Google Patents

负极极片、锂离子二次电池及装置 Download PDF

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WO2020155993A1
WO2020155993A1 PCT/CN2019/129372 CN2019129372W WO2020155993A1 WO 2020155993 A1 WO2020155993 A1 WO 2020155993A1 CN 2019129372 W CN2019129372 W CN 2019129372W WO 2020155993 A1 WO2020155993 A1 WO 2020155993A1
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Prior art keywords
active material
ion secondary
lithium ion
pole piece
material layer
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PCT/CN2019/129372
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English (en)
French (fr)
Inventor
黄亚萍
张小文
金海族
林永寿
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Contemporary Amperex Technology Co Ltd
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Contemporary Amperex Technology Co Ltd
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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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • 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
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • This application relates to the field of batteries, and more specifically to a negative pole piece, a lithium ion secondary battery and a device.
  • Lithium-ion secondary batteries are one of the main members of the power battery family.
  • the improvement of energy density and cycle life is critical to battery performance.
  • the power battery completes the charging and discharging process through the insertion and extraction of ions between the positive and negative active materials, and the design of the negative pole piece will directly affect the performance of the battery.
  • How to rationally design the negative pole piece to obtain a battery with both electrochemical performance and kinetic performance is a common problem faced by the industry.
  • the purpose of this application is to provide a negative pole piece, a lithium ion secondary battery and a device, the lithium ion secondary battery has high energy density, long cycle life and good dynamic performance .
  • the present application provides a negative pole piece, including: a negative current collector;
  • a first active material layer provided on the negative current collector which includes a first active material
  • the second active material layer provided on the first active material layer includes a second active material
  • the first active material is flake-shaped, and the second active material is spherical or quasi-spherical.
  • the present application provides a lithium ion secondary battery, which includes a positive pole piece, a negative pole piece, a separator, and an electrolyte, wherein the negative pole piece is according to the first aspect of the present application.
  • the negative pole piece is according to the first aspect of the present application.
  • the application provides a device including the lithium ion secondary battery described in the second aspect of the application.
  • the negative pole piece of the present application adopts double active material layers, and the first active material layer and the second active material layer select active materials of specific shapes, which can make the lithium ion secondary battery have high Energy density, long cycle life and good dynamic performance.
  • the device of the present application includes the lithium ion secondary battery described in the second aspect of the present application, and therefore has at least the same advantages as the lithium ion secondary battery.
  • FIG. 1 is a schematic diagram of an embodiment of a lithium ion secondary battery.
  • Fig. 2 is a schematic diagram of an embodiment of a battery module.
  • Fig. 3 is a schematic diagram of an embodiment of a battery pack.
  • Fig. 4 is an exploded view of Fig. 3.
  • FIG. 5 is a schematic diagram of an embodiment of a device in which a lithium ion secondary battery is used as a power source.
  • the negative electrode piece includes: a negative electrode current collector; a first active material layer provided on the negative electrode current collector, which includes the first active material; and a first active material layer provided on the first active material layer
  • the second active material layer includes a second active material, the first active material is sheet-shaped, and the second active material is spherical or quasi-spherical.
  • the negative pole piece adopts a double active material layer, and the first active material layer and the second active material layer select active materials of a specific shape.
  • the inventor found that when the negative pole piece adopts the double active material layer, not only Increasing the energy density of the battery can also effectively improve the cracking of the active material layer, mainly because the double-layer coating reduces the internal stress of the active material layer during the drying process of the pole piece and solves the cracking problem caused by the increase in coating weight , Thereby improving the cycle performance of the battery can effectively improve the energy density, cycle life and dynamic performance of the battery.
  • the first active material is selected as flake particles. Due to their sharp edges and corners, they are easier to bite and pack together during the compaction process, thereby further improving the energy density and cycle performance of the battery; the second active material is selected as spherical or quasi-spherical Particles, which can enable the second active material layer to maintain a good porosity under a higher compaction density, so that the battery has a higher energy density and excellent dynamic performance.
  • the flatness of the first active material has a certain influence on the performance of the battery.
  • the flatness of the flake particles is characterized by the concept of flatness, where the flatness It is the three-dimensional size of the ratio of the short diameter to the thickness of the first active material, where the smallest size is the thickness, the largest size is the long diameter, and the size in the middle is the short diameter.
  • the flatness of the flake particles is too small or the thickness of the particles is too small, so that the sharpness of the edges and corners of the material is reduced.
  • the degree of mutual engagement decreases to a certain extent, resulting in the energy density of the negative pole piece. Decrease; the flatness of the flake particles is too large or the thickness is too small, so that the material is too dense, which is not conducive to the deintercalation of lithium ions, and the dynamic performance of the negative pole piece decreases.
  • the ratio of the short diameter to the thickness (ie, the flatness) of the first active material is 0.1-2.0, more preferably 0.5-1.8.
  • the average particle size D 50 of the second active material also has a certain influence on the performance of the negative electrode piece.
  • the average particle size of the second active material is 5 ⁇ m-40 ⁇ m; more preferably, it is 8 ⁇ m-35 ⁇ m.
  • the porosity of the active material layer also has a certain influence on the performance of the negative electrode sheet.
  • the greater the porosity the easier it is for the electrolyte to fully contact the active material, which is more conducive to the deintercalation of lithium ions.
  • the excessive porosity will reduce the amount of active material coated per unit volume, resulting in a decrease in the energy density of the negative electrode.
  • the smaller the porosity the easier it is to increase the energy density of the negative pole piece, but it may cause the dynamic performance of the negative pole piece to decrease.
  • the porosity of the second active material layer is greater than the porosity of the first active material layer.
  • the porosity of the second active material layer is greater than the porosity of the first active material, it is beneficial for the electrolyte to quickly infiltrate the electrode pole piece, which is beneficial to increase the liquid absorption rate of the negative electrode piece, and at the same time,
  • the lower porosity of the first active material layer helps to improve the liquid storage capacity of the negative electrode piece.
  • the porosity of the first active material layer is 15%-35%, more preferably 20%-30%.
  • the porosity of the second active material layer is 30%-50%, more preferably 35%-45%.
  • the coating weight per unit area of the active material also has a certain effect on the performance of the negative electrode.
  • the coating weight per unit area is an important parameter that affects the energy density of the negative electrode.
  • the unit coating weight of the negative electrode The smaller the battery, the better the dynamic performance of the battery, but at the same time the energy density of the battery will be lower; on the contrary, the dynamic performance will decrease and the energy density will increase.
  • the coating weight per unit area (single side) of the first active material layer and/or the second active material layer is 20 g/m 2 -200 g/m 2 , more preferably 50 g/m 2 -180 g/m 2 .
  • the inventor further researched and found that when the ratio of the coating weight per unit area of the second active material layer to the first active material layer is 0.05-0.5, the energy density and cycle performance of the battery can be further improved.
  • the ratio of the coating weight per unit area of the second active material layer to the coating weight per unit area of the first active material layer is 0.1-0.45.
  • the thickness of the first active material layer is 30 ⁇ m-100 ⁇ m, preferably 50 ⁇ m-80 ⁇ m; the thickness of the second active material layer is 30 ⁇ m-100 ⁇ m, preferably 50 ⁇ m-80 ⁇ m. If the thickness is too small, the energy density of the battery will be affected, and if the thickness is too large, the bonding force between the active material layers will be reduced, and mold release will occur, thereby affecting the cycle performance of the battery.
  • the first active material and the second active material are selected from soft carbon, hard carbon, graphite, silicon, silicon-oxygen compounds, silicon-carbon composites, and metals that can form alloys with lithium. One or more.
  • the first active material and the second active material are both graphite.
  • the lithium ion secondary battery of the second aspect of the present application which includes a positive pole piece, a negative pole piece, a separator and an electrolyte, wherein the negative pole piece is the negative pole piece according to the first aspect of the application .
  • the positive electrode sheet includes a positive electrode current collector and a positive electrode film provided on at least one surface of the positive electrode current collector and including a positive electrode active material, a conductive agent, and a binder.
  • the specific type and composition of the positive pole piece are not subject to specific restrictions, and can be selected according to actual needs.
  • the positive electrode active material is selected from, but not limited to, one or more of the following materials: lithium transition metal composite oxides, including lithium iron phosphide, lithium iron manganese phosphide, lithium cobalt oxide, lithium nickel oxide, and lithium manganese oxide , Lithium nickel manganese oxide, lithium nickel cobalt manganese oxide, lithium nickel cobalt aluminum oxide and these lithium transition metal oxides added other transition metals or non-transition metal compounds.
  • the type of the separator is not specifically limited, and it can be any separator material used in existing batteries, such as polyethylene, polypropylene, and polyvinylidene fluoride. Ethylene and their multilayer composite film, but not limited to these.
  • the specific type and composition of the electrolyte are not subject to specific restrictions, and can be selected according to actual needs.
  • the lithium ion secondary battery may include an outer package for packaging the positive pole piece, the negative pole piece, and the electrolyte.
  • the positive pole piece, the negative pole piece and the separator can be laminated or wound to form a laminated structure electrode assembly or a wound structure electrode assembly, the electrode assembly is packaged in an outer package; the electrolyte can be an electrolyte, which is infiltrated In the electrode assembly.
  • the number of electrode assemblies in the lithium ion secondary battery can be one or several, which can be adjusted according to requirements.
  • the outer packaging of the lithium ion secondary battery may be a soft bag, such as a pouch type soft bag.
  • the material of the soft bag can be plastic, such as one or more of polypropylene (PP), polybutylene terephthalate (PBT), polybutylene succinate (PBS), and the like.
  • the outer packaging of the lithium ion secondary battery may also be a hard case, such as an aluminum case.
  • Fig. 1 shows a lithium ion secondary battery 5 having a square structure as an example.
  • the lithium ion secondary battery can be assembled into a battery module, and the number of lithium ion secondary batteries contained in the battery module can be multiple, and the specific number can be adjusted according to the application and capacity of the battery module.
  • Fig. 2 is a battery module 4 as an example.
  • a plurality of lithium ion secondary batteries 5 may be arranged in sequence along the length direction of the battery module 4. Of course, it can also be arranged in any other manner. Furthermore, the plurality of lithium ion secondary batteries 5 can be fixed by fasteners.
  • the battery module 4 may further include a housing having an accommodation space, and a plurality of lithium ion secondary batteries 5 are accommodated in the accommodation space.
  • the above-mentioned battery modules can also be assembled into a battery pack, and the number of battery modules contained in the battery pack can be adjusted according to the application and capacity of the battery pack.
  • Figures 3 and 4 show the battery pack 1 as an example.
  • the battery pack 1 may include a battery box and a plurality of battery modules 4 provided in the battery box.
  • the battery box includes an upper box body 2 and a lower box body 3, and the upper box body 2 can be installed on the lower box body 3 to form a closed space for accommodating the battery module 4.
  • a plurality of battery modules 4 may be arranged in the battery box in any manner.
  • a device in the third aspect of the present application, includes the lithium ion secondary battery of the second aspect of the present application.
  • the lithium ion secondary battery can be used as a power source for the device or as the The energy storage unit of the device.
  • the device can be, but is not limited to, mobile devices (such as mobile phones, laptop computers, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf Vehicles, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc.
  • the device can select a lithium ion secondary battery, battery module or battery pack according to its usage requirements.
  • Figure 5 is a device as an example.
  • the device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle.
  • battery packs or battery modules can be used.
  • the device may be a mobile phone, a tablet computer, a notebook computer, etc.
  • the device is generally required to be light and thin, and a lithium ion secondary battery can be used as a power source.
  • the lithium ion secondary batteries of Examples 1-13 and Comparative Examples 1-5 were prepared according to the following methods.
  • the positive electrode active material LiNi 1/3 Co 1/3 Mn 1/3 O 2 , the conductive agent Super-P, and the binder PVDF are mixed in a mass ratio of 94:3:3, and the solvent NMP is added and stirred under the action of a vacuum mixer Until the system is uniform, the positive electrode slurry is obtained; the positive electrode slurry is evenly coated on the two surfaces of the positive electrode current collector aluminum foil, dried at room temperature and then transferred to the oven to continue drying, and then cold pressed and slit to obtain positive electrode pieces .
  • Ethylene carbonate (EC) and ethyl methyl carbonate (EMC) are mixed in a volume ratio of 3:7 to obtain an organic solvent, and then fully dried LiPF 6 is dissolved in the mixed organic solvent to prepare a concentration of 1mol/L Of electrolyte.
  • Liquid absorption rate p*( ⁇ *R 2 )*H/t
  • R Capillary diameter
  • H The height of the inhaled electrolyte in the capillary
  • the produced lithium ion secondary battery is charged and discharged for the first time with a current of 0.5C (that is, the current value of completely discharging the theoretical capacity within 2h).
  • the charging is constant current and constant voltage charging, and the termination voltage is 4.2V ,
  • the cut-off current is 0.05C, the final discharge voltage is 2.8V, and the discharge energy of 0.5C is recorded as W0; the energy is divided by the volume of the lithium ion secondary battery to obtain the volumetric energy density of the lithium ion secondary battery.
  • the produced lithium ion secondary battery is charged and discharged for the first time with a current of 1C (that is, the current value of completely discharging the theoretical capacity within 1h).
  • the charging is constant current and constant voltage charging, and the termination voltage is 4.2V.
  • the current is 0.05C
  • the end-of-discharge voltage is 2.8V
  • its theoretical capacity is recorded as C0
  • the lithium-ion secondary battery is left for 24 hours and then charged to 4.2V with 1C constant current and constant voltage, and 4.2V constant voltage to 0.05C
  • Discharge the fully charged lithium ion secondary battery for 30 minutes with a current of 1C0 adjust the capacity of the lithium ion secondary battery to 50% SOC state, stand for 60 minutes, discharge at 4C0 pulse for 30 seconds, and record the pulse discharge and discharge of the lithium ion secondary battery At the end of the voltage, the power performance of the lithium ion secondary battery is obtained.
  • the resistance of the lithium ion secondary battery before cycling At room temperature, the produced lithium ion secondary battery is charged and discharged for the first time with a current of 1C (that is, the current value of completely discharging the theoretical capacity within 1h).
  • the charging is constant current and constant voltage charging, and the termination voltage is 4.2V.
  • the current is 0.05C
  • the discharge termination voltage is 2.8V
  • the BOL (Before of life) of the lithium ion secondary battery is recorded, which is the discharge capacity Cb at the first cycle.
  • the test condition is 1C/1C cycle under normal temperature conditions, and the discharge capacity Ce of lithium ion secondary battery is recorded at any time.
  • the ratio of Ce to Cb is the capacity retention rate during the cycle. When the capacity retention rate is lower than
  • the test is stopped when it reaches 80% or equal to EOL (End of life), and the number of cycles of the lithium-ion secondary battery when EOL is reached is recorded to determine the cycle life.
  • Example 1 450 2200 2657
  • Example 2 455 2300 2754
  • Example 3 460 2366 3066
  • Example 4 485 2658 3565
  • Example 5 487 2467 3347
  • Example 6 478 2243 2744
  • Example 7 480 2145 2621
  • Example 8 480 2655 3480
  • Example 9 475 2455 3219
  • Example 10 461 2554 3455
  • Example 11 466 2538 3480
  • Example 12 477 2547 3490
  • Example 13 453 2523 3324 Comparative example 1
  • 440 1800 2000 Comparative example 2 430 1850 2200 Comparative example 3 445 1600 1720 Comparative example 4 440 1860 2300 Comparative example 5 440 1950 2150
  • the negative electrode provided in Examples 1-13 adopts double active material layers, and when the first active material is flaky particles and the second active material is spherical particles, the lithium ion secondary battery can take care of both High energy density, long cycle life and excellent dynamic performance.
  • the flatness affects the occluding ability between the first active material and further affects the energy density of the lithium ion secondary battery.
  • the flatness of the first active material By reasonably controlling the flatness of the first active material, the Between 0.1-2, the energy density of the pole piece can be increased to a certain extent, and the problem of poor liquid absorption performance caused by too dense pole piece can be avoided.
  • the electrochemical performance of the pole piece is effectively improved by controlling the unit coating weight of the pole piece, and the unit coating weight of the first active material layer of the pole piece is controlled to be 20 g/m 2 -200g/m 2 and controlling the ratio of the unit coating weight of the second active material layer to the unit coating weight of the first active material layer to be between 0.05-0.5, which can further increase the energy of the lithium ion secondary battery density.
  • Examples 1-13 the energy density, power performance, and cycle performance of lithium ion secondary batteries have also been significantly improved (Examples 1-13); when controlling spherical graphite in the first active material layer or mixed use, although the energy density is improved, the power And the cycle performance is basically not improved (Comparative Example 5); in addition, the power and cycle performance of the lithium ion secondary battery under a thick unit coating weight are also significantly improved (such as Example 9 and Comparative Example 3).
  • Comparative Examples 1-3 and Comparative Example 5 when a single active material layer is used, the above-mentioned distinguishing effect may be due to the fact that the surface area of the pole piece is subjected to greater force during single-layer coating, which is likely to cause overpressure.
  • the porosity of the surface area of the pole piece is low, which is not conducive to the diffusion of lithium ions.
  • the negative electrode adopts double-layer or multi-layer coating.
  • the high dynamic performance and high porosity of the second active material layer of the negative electrode piece can ensure the smooth conduction of lithium ions in the pores. Reduce the lithium ion transmission impedance and increase the lithium ion diffusion rate, thereby improving the rate and cycle performance of the lithium ion secondary battery.
  • the second active material layer can transmit more pressure during cold pressing to the first active material layer, increasing the pressure of the first active material layer. The actual density can increase the energy density of the lithium ion secondary battery without losing power performance.
  • the technical solution greatly improves the rate and cycle performance of the lithium ion secondary battery under a thick unit coating weight.

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Abstract

一种锂离子二次电池（5）的负极极片、锂离子二次电池及装置，含有双层活性物质层，能够改善锂离子二次电池倍率、循环性能、提高锂离子二次电池能量密度。该负极极片包括常规集流体、片状的第一活性物质层和球形或类球形的第二活性物质层，使得锂离子二次电池兼具高动力学性能和高能量密度的优点。

Description

负极极片、锂离子二次电池及装置 技术领域
本申请涉及电池领域，更具体地涉及一种负极极片、锂离子二次电池及装置。
背景技术
近来动力电池市场的需求逐渐扩大，对动力电池的电化学性能和动力学性能的需求也越来越高。锂离子二次电池是动力电池家族的主要成员之一，对于锂离子二次电池来说，能量密度和循环寿命的提升对于电池性能至关重要。
从技术原理来说，动力电池是通过离子在正负极活性物质之间嵌入和脱出完成充电和放电过程，其中负极极片设计将直接影响电池的性能。如何通过合理设计负极极片，从而得到兼顾电化学性能和动力学性能的电池是目前行业内普遍面临的问题。
发明内容
鉴于背景技术中存在的问题，本申请的目的在于提供一种负极极片、锂离子二次电池及装置，所述锂离子二次电池兼具高能量密度、长循环寿命以及良好的动力学性能。
为达到上述目的，在本申请的第一方面，本申请提供了一种负极极片，包括：负极集流体；
设置在所述负极集流体上的第一活性物质层，其包括第一活性物质；和
设置在所述第一活性物质层上的第二活性物质层，其包括第二活性物质，
所述第一活性物质为片状，所述第二活性物质为球形或类球形。
在本申请的第二方面，本申请提供了一种锂离子二次电池，其包括正极 极片、负极极片、隔离膜以及电解液，其中，所述负极极片为根据本申请第一方面所述的负极极片。
在本申请的第三方面，本申请提供了一种装置，其包括本申请第二方面所述的锂离子二次电池。
相比于现有技术，本申请至少包括如下所述的有益效果：
本申请的所述的负极极片采用双活性物质层，且所述第一活性物质层和所述第二活性物质层选择特定形状的活性物质，可以使所述锂离子二次电池兼具高能量密度、长循环寿命及良好的动力学性能。本申请的装置包括本申请第二方面所述的锂离子二次电池，因而至少具有与所述锂离子二次电池相同的优势。
附图说明
图1是锂离子二次电池的一实施方式的示意图。
图2是电池模块的一实施方式的示意图。
图3是电池包的一实施方式的示意图。
图4是图3的分解图。
图5是锂离子二次电池用作电源的装置的一实施方式的示意图。
其中，附图标记说明如下：
1电池包
2上箱体
3下箱体
4电池模块
5锂离子二次电池
具体实施方式
下面详细说明本申请的负极极片、锂离子二次电池及装置。
首先说明本申请第一方面的负极极片，负极极片包括：负极集流体；设 置在负极集流体上的第一活性物质层，其包括第一活性物质；和设置在第一活性物质层上的第二活性物质层，其包括第二活性物质，所述第一活性物质为片状，所述第二活性物质为球形或类球形。
所述负极极片采用双活性物质层，且第一活性物质层和第二活性物质层选择特定形状的活性物质，发明人经过大量研究发现，当负极极片采用双活性物质层时，不仅可以提高电池的能量密度，还可以有效改善活性物质层开裂问题，主要是因为通过双层涂布，降低了极片烘干过程中活性物质层的内应力，解决了涂布重量增加导致的开裂问题，从而改善电池的循环性能可以有效地提升电池的能量密度、循环寿命以及动力学性能。
所述第一活性物质选择片状颗粒，由于其棱角尖锐，在压实过程中更容易相互咬合而紧密堆积在一起，进一步提升电池的能量密度和循环性能；第二活性物质选择球形或类球形颗粒，其可以使第二活性物质层在较高的压实密度下仍能保持良好的孔隙率，从而使电池具有更高的能量密度及优异的动力学性能。
进一步地，所述第一活性物质的扁平程度对于电池的性能有一定影响，为了更加清楚的表征片状颗粒的扁平程度，规定片状颗粒的扁平程度采用扁平度的概念表征，其中，扁平度为第一活性物质的短径与厚度的比值的三维尺寸，其中尺寸最小的为厚度，尺寸最大的为长径，尺寸位于中间的为短径。扁平度偏低的片状颗粒由于颗粒短径过小或厚度较大，使得材料自身棱角尖锐程度下降，在压实过程中，其相互咬合的程度有一定的下降，造成负极极片能量密度的下降；扁平度偏高的片状颗粒由于其短径过大或厚度过小使得材料咬合太过致密，从而不利于锂离子脱嵌，负极极片的动力学性能反而下降。
优选地，所述第一活性物质的短径与厚度的比值(即扁平度)为0.1-2.0，进一步优选为0.5-1.8。
进一步地，所述第二活性物质的平均粒径D 50对负极极片的性能也有一定 的影响。第二活性物质的平均粒径越小，其与电解液的接触越充分，越有利于活性离子与电子的电荷交换，从而更有利于电池的快速充电，但是第二活性物质的平均粒径过小，负极浆料的制备越困难，负极极片的一致性可能受到影响。
优选地，所述第二活性物质的平均粒径为5μm-40μm；进一步优选为8μm-35μm。
进一步地，所述活性物质层的孔隙率对负极极片的性能也有一定的影响。孔隙率越大，电解液越容易与活性物质充分接触，越利于锂离子的脱嵌，但孔隙率过大会造成单位体积内涂布的活性物质的量减少，造成负极极片能量密度的减少，孔隙率越小，越容易提升负极极片的能量密度，但可能造成负极极片动力学性能下降。
优选地，所述第二活性物质层的孔隙率大于第一活性物质层的孔隙率。
当所述第二活性物质层的孔隙率大于所述第一活性物质的孔隙率时，有利于电解液快速的浸润电极极片，有利于提高所述负极极片的吸液速率，同时，所述第一活性物质层较低的孔隙率有助于提高所述负极极片的储液能力。
优选地，所述第一活性物质层的孔隙率为15％-35％，更优选为20％-30％。
优选地，所述第二活性物质层的孔隙率为30％-50％，更优选为35％-45％。
进一步地，活性物质的单位面积涂布重量对于负极极片的性能也有一定的影响，单位面积涂布重量是影响负极极片能量密度的重要参数，一般情况下，负极极片的单位涂布重量越小，电池的动力学性能越好，但同时电池的能量密度也会越低；反之，则动力学性能下降，而能量密度有所提升。
优选地，所述第一活性物质层和/或第二活性物质层的单位面积涂布重量(单面)为20g/m 2-200g/m 2，更优选为50g/m 2-180g/m 2。
发明人进一步研究发现，当所述第二活性物质层与所述第一活性物质层的单位面积涂布重量的比值为0.05-0.5时，可进一步提升电池的能量密度和循环性能。优选地，所述第二活性物质层的单位面积涂布重量与第一活性物质 层的单位面积涂布重量的比值为0.1-0.45。
进一步地，所述第一活性物质层的厚度为30μm-100μm，优选为50μm-80μm；所述第二活性物质层的厚度为30μm-100μm，优选为50μm-80μm。厚度过小会影响电池的能量密度，厚度过大将导致活性物质层之间的粘结力降低，出现脱模现象，从而影响电池的循环性能。
在本申请的负极极片中，所述第一活性物质和第二活性物质选自软碳、硬碳、石墨、硅、硅氧化合物、硅碳复合物以及能与锂形成合金的金属中的一种或几种。
优选地，所述第一活性物质和第二活性物质均为石墨。
其次说明本申请第二方面的锂离子二次电池，其包括正极极片、负极极片、隔离膜以及电解液，其中，所述负极极片为根据本申请第一方面所述的负极极片。
在本申请第二方面的锂离子二次电池中，正极极片包括正极集流体以及设置在正极集流体至少一个表面上且包括正极活性材料、导电剂以及粘结剂的正极膜片。正极极片的具体种类及组成均不受到具体的限制，可根据实际需求进行选择。
正极活性材料选自但不限于以下物质的一种或几种：锂过渡金属复合氧化物，包含锂铁磷化物、锂铁锰磷化物、锂钴氧化物、锂镍氧化物、锂锰氧化物、锂镍锰氧化物、锂镍钴锰氧化物、锂镍钴铝氧化物以及这些锂过渡金属氧化物添加其他过渡金属或非过渡金属得到的化合物。
在本申请第二方面的锂离子二次电池中，所述隔离膜的种类并不受到具体的限制，可以是现有电池中使用的任何隔离膜材料，例如聚乙烯、聚丙烯、聚偏氟乙烯以及它们的多层复合膜，但不仅限于这些。
在本申请第二方面的锂离子二次电池中，所述电解液的具体种类及组成均不受到具体的限制，可根据实际需求进行选择。
在一些实施例中，锂离子二次电池可以包括外包装，用于封装正极极片、负极极片和电解质。作为一个示例，正极极片、负极极片和隔离膜可经叠片或卷绕形成叠片结构电极组件或卷绕结构电极组件，电极组件封装在外包装内；电解质可采用电解液，电解液浸润于电极组件中。锂离子二次电池中电极组件的数量可以为一个或几个，可以根据需求来调节。
在一些实施例中，锂离子二次电池的外包装可以是软包，例如袋式软包。软包的材质可以是塑料，如可包括聚丙烯(PP)、聚对苯二甲酸丁二醇酯(PBT)、聚丁二酸丁二醇酯(PBS)等中的一种或几种。锂离子二次电池的外包装也可以是硬壳，例如铝壳等。
本申请对锂离子二次电池的形状没有特别的限制，其可以是圆柱形、方形或其他任意的形状。如图1是作为一个示例的方形结构的锂离子二次电池5。
在一些实施例中，锂离子二次电池可以组装成电池模块，电池模块所含锂离子二次电池的数量可以为多个，具体数量可根据电池模块的应用和容量来调节。
图2是作为一个示例的电池模块4。参照图2，在电池模块4中，多个锂离子二次电池5可以是沿电池模块4的长度方向依次排列设置。当然，也可以按照其他任意的方式进行排布。进一步可以通过紧固件将该多个锂离子二次电池5进行固定。
可选地，电池模块4还可以包括具有容纳空间的壳体，多个锂离子二次电池5容纳于该容纳空间。
在一些实施例中，上述电池模块还可以组装成电池包，电池包所含电池模块的数量可以根据电池包的应用和容量进行调节。
图3和图4是作为一个示例的电池包1。参照图3和图4，在电池包1中可以包括电池箱和设置于电池箱中的多个电池模块4。电池箱包括上箱体2和下箱体3，上箱体2能够盖设于下箱体3，并形成用于容纳电池模块4的封闭 空间。多个电池模块4可以按照任意的方式排布于电池箱中。
接下来说明本申请第三方面的装置。
在本申请的第三方面提供一种装置，所述装置包括本申请第二方面的锂离子二次电池，所述锂离子二次电池可以用作所述装置的电源，也可以用作所述装置的能量储存单元。所述装置可以但不限于是移动设备(例如手机、笔记本电脑等)、电动车辆(例如纯电动车、混合动力电动车、插电式混合动力电动车、电动自行车、电动踏板车、电动高尔夫球车、电动卡车等)、电气列车、船舶及卫星、储能系统等。
所述装置可以根据其使用需求来选择锂离子二次电池、电池模块或电池包。
图5是作为一个示例的装置。该装置为纯电动车、混合动力电动车、或插电式混合动力电动车等。为了满足该装置对锂离子二次电池的高功率和高能量密度的需求，可以采用电池包或电池模块。
作为另一个示例的装置可以是手机、平板电脑、笔记本电脑等。该装置通常要求轻薄化，可以采用锂离子二次电池作为电源。
为详细说明技术方案的技术内容、构造特征、所实现目的及效果，以下结合具体实施例详予说明。应理解，这些实施例仅用于说明本申请而不用于限制本申请的范围。
实施例1-13和对比例1-5的锂离子二次电池均按照下述方法进行制备。
(1)正极极片的制备
将正极活性材料LiNi 1/3Co 1/3Mn 1/3O 2、导电剂Super-P、粘结剂PVDF按质量比94:3:3进行混合，加入溶剂NMP，在真空搅拌机作用下搅拌至体系呈均一状，获得正极浆料；将正极浆料均匀涂覆在正极集流体铝箔的两个表面上，室温晾干后转移至烘箱继续干燥，然后经过冷压、分切得到正极极片。
(2)负极极片的制备
i、单层活性物质层负极极片的制备(对比例1-3和对比例5负极极片按照单层活性物质负极极片的制备方法制备)
将表1中对比例1-3和对比例5所示的负极活性材料、导电剂Super-P、粘结剂SBR、增稠剂CMC、按质量比96:1:2:1进行混合，在去离子水溶剂体系中充分搅拌混合均匀后，得到浆料；将负极浆料均匀涂覆在负极集流体铜箔的两个表面上，室温晾干后转移至烘箱继续干燥，然后经过冷压、分切得到负极极片。
ii、双层活性物质层负极极片的制备(实施例1-13和对比例4负极极片按照双层活性物质层负极极片的制备方法制备)
将表1中实施例1-13和对比例4所示的第一活性物质层的第一活性物质，导电剂Super-P、粘结剂SBR、增稠剂CMC、按质量比96:1:2:1进行混合，在去离子水溶剂体系中充分搅拌混合均匀后，得到浆料A；
将表1中实施例1-13和对比例4所示的第二活性物质层的第二活性物质，导电剂Super-P、粘结剂SBR、增稠剂CMC、按质量比96:1:2:1进行混合，在去离子水溶剂体系中充分搅拌混合均匀后，得到浆料B；
先将浆料A涂覆于Cu箔上，烘干，得到涂覆了第一活性物质层的极片A；接着在极片A表面涂浆料B，烘干，然后经过冷压、分切得到具有双层活性物质层的负极极片。
(3)电解液的制备
将碳酸乙烯酯(EC)、碳酸甲乙酯(EMC)按照按体积比3:7进行混合得到有机溶剂，接着将充分干燥的LiPF 6溶解于混合后的有机溶剂中，配制成浓度1mol/L的电解液。
(4)隔离膜的制备
选PE/PP/PE三层多孔聚合薄膜作为隔离膜。
(5)锂离子二次电池的制备
将上述正极极片、隔离膜、负极极片按顺序叠好，使隔离膜处于正、负极极片之间起到隔离的作用，然后卷绕得到电极组件；将电极组件置于外包装壳中，干燥后注入电解液，经过真空封装、静置、化成、整形等工序，获得锂离子二次电池。
接下来说明活性物质扁平度的测试方法和锂离子二次电池的性能测试方法。
(1)扁平度的测试采用以下方法：
i、通过扫描电子显微镜，统计出20个颗粒的长径L1、短径L2、厚度T1；
ii、通过颗粒的短径和厚度比(L2/T1)计算出颗粒的扁平度，求出平均值，作为材料的扁平度。
(2)极片吸液速率的测试采用以下方法：
取辊压后的负极极片，在毛细管中吸入一定高度的电解液后置于极片表面，采用秒表记录电解液全部被极片吸收所需时间t；
吸液速率＝p*(π*R 2)*H/t
P：电解液密度；
R：毛细管直径；
H：毛细管中吸入电解液的高度；
t：时间。
(3)体积能量密度测试采用以下方法：
常温下，所制作锂离子二次电池以0.5C(即2h内完全放掉理论容量的电流值)的电流进行第一次充电和放电，充电时为恒流恒压充电，终止电压为4.2V，截至电流为0.05C，放电终止电压为2.8V，记录其0.5C的放电能量为W0；能量除以锂离子二次电池的体积，得到锂离子二次电池的体积能量密度。
(4)功率性能测试采用以下方法：
常温下，所制作锂离子二次电池以1C(即1h内完全放掉理论容量的电流值)的电流进行第一次充电和放电，充电为恒流恒压充电，终止电压为4.2V， 截至电流为0.05C，放电终止电压为2.8V，记录其理论容量为C0；然后锂离子二次电池搁置24H后以1C恒流恒压充电至4.2V，4.2V恒压充电至0.05C；然后采用1C0的电流对满充锂离子二次电池进行放电30min，调节锂离子二次电池的容量为50％SOC状态，静置60min，以4C0脉冲放电30s，记录锂离子二次电池脉冲放电前和放电末的电压，得到锂离子二次电池的功率性能。
(5)循环性能测试采用以下方法：
循环前先测试锂离子二次电池的电阻。常温下，所制作锂离子二次电池以1C(即1h内完全放掉理论容量的电流值)的电流进行第一次充电和放电，充电为恒流恒压充电，终止电压为4.2V，截至电流为0.05C，放电终止电压为2.8V，记录锂离子二次电池BOL(Before of life)即首次循环时放电容量Cb。然后进行循环寿命检测，测试条件为常温条件下，进行1C/1C循环，随时记录锂离子二次电池时放电容量Ce，Ce与Cb的比值即为循环过程容量保持率，在容量保持率低于或等于80％时停止测试，认为达到EOL(End of life)，记录达到EOL时锂离子二次电池循环圈数，用于判断循环寿命。
实施例1-13和对比例1-5提供的负极极片的相关参数见表1，实施例1-13和对比例1-5制备的锂离子二次电池的测试结果见表2。
表1实施例1-13和对比例1-5提供的负极极片的相关参数
Figure PCTCN2019129372-appb-000001
Figure PCTCN2019129372-appb-000002
表2实施例1-13和对比例1-5制备的锂离子二次电池的测试结果
  能量密度(Wh/L) 功率(W) 寿命(圈)
实施例1 450 2200 2657
实施例2 455 2300 2754
实施例3 460 2366 3066
实施例4 485 2658 3565
实施例5 487 2467 3347
实施例6 478 2243 2744
实施例7 480 2145 2621
实施例8 480 2655 3480
实施例9 475 2455 3219
实施例10 461 2554 3455
实施例11 466 2538 3480
实施例12 477 2547 3490
实施例13 453 2523 3324
对比例1 440 1800 2000
对比例2 430 1850 2200
对比例3 445 1600 1720
对比例4 440 1860 2300
对比例5 440 1950 2150
从表2可以看出，实施例1-13提供的负极极片采用双活性物质层，且第一活性物质选用片状颗粒，第二活性物质选用球形颗粒时，锂离子二次电池可同时兼顾高能量密度、长循环寿命及优异的动力学性能。
进一步地，从实施例1-8中可以看出，扁平度影响了第一活性物质之间的咬合能力并进一步影响锂离子二次电池的能量密度，通过合理控制第一活性物质的扁平度介于0.1-2之间，即可以一定程度提高极片的能量密度，又可以避免极片太过致密造成吸液性能差的问题。
进一步地，从实施例9-13中可以看出，第二活性物质的粒径介于5μm-40μm之间时，可以一定程度上改善极片第二活性物质层的孔隙率，有效地提高极片的吸液速率，使得电池极片具有优异的浸润性，从而改善锂离子二次电池的动力学性能。
进一步地，实施例8和9中，通过控制极片的单位涂布重量有效地改善了极片的电化学性能，控制极片的第一活性物质层的单位涂布重量介于20g/m 2-200g/m 2之间且控制第二活性物质层的单位涂布重量与第一活性物质层的单位涂布重量的比值为0.05-0.5之间，可以进一步的提高锂离子二次电池的 能量密度。
此外，锂离子二次电池的能量密度、功率性能和循环性能也有明显提升(实施例1-13)；控制球形石墨在第一活性物质层或者混合使用时，虽然能量密度有提升，但是对功率和循环性能基本无改善(对比例5)；此外，厚的单位涂布重量下的锂离子二次电池功率和循环性能也有明显改善(如实施例9和对比例3)。
从对比例1-3和对比例5中可以看出，采用单活性物质层时，产生上述区别效果可能是因为单层涂布时，极片的表层区域受力较大，容易产生过压，造成极片表层区域的孔隙率较低，不利于锂离子的扩散。负极采用双层或多层涂布，控制第二活性物质层的活性物质为球形或类球形时，由于球形颗粒之间的接触较少，可以防止极片表层的颗粒过压，颗粒之间的孔隙不能被完全填充。这样可以获得表层孔隙率较高的负极，提高极片对电解液的吸收速率，这样负极极片第二活性物质层高的动力学性能和高的孔隙率可保证锂离子在孔隙内传导顺畅，降低锂离子传输阻抗，提高锂离子扩散速率，从而改善锂离子二次电池的倍率和循环性能。此外，由于球形或类球形颗粒的抗压性能优于片状颗粒，这样第二活性物质层可以将冷压时的压力更多的传递到第一活性物质层，提高第一活性物质层的压实密度，可在不损失功率性能的基础上提高锂离子二次电池的能量密度。特别地，本技术方案对厚的单位涂布重量下锂离子二次电池的倍率、循环性能有较大提高。
需要说明的是，尽管在本文中已经对上述各实施例进行了描述，但并非因此限制本申请的专利保护范围。因此，基于本申请的创新理念，对本文所述实施例进行的变更和修改，或利用本申请说明书内容所作的等效结构或等效流程变换，直接或间接地将以上技术方案运用在其他相关的技术领域，均包括在本申请的专利保护范围之内。

Claims (11)

  1. 一种负极极片，包括：
    负极集流体；
    设置在所述负极集流体上的第一活性物质层，其包括第一活性物质；和
    设置在所述第一活性物质层上的第二活性物质层，其包括第二活性物质，
    所述第一活性物质为片状，所述第二活性物质为球形或类球形。
  2. 根据权利要求1所述的负极极片，其特征在于，所述第一活性物质扁平度为0.1-2，优选为0.5-1.8。
  3. 根据权利要求1-2中任一项所述的负极极片，其特征在于，所述第二活性物质的平均粒径为5μm-40μm，优选为8μm-35μm。
  4. 根据权利要求1-3中任一项所述的负极极片，其特征在于，所述第二活性物质层的孔隙率大于所述第一活性物质层的孔隙率。
  5. 根据权利要求4所述的负极极片，其特征在于，所述第一活性物质层的孔隙率为15％-35％，优选为20％-30％；和/或，
    所述第二活性物质层的孔隙率为30％-50％，优选为35％-45％。
  6. 根据权利要求1-5中任一项所述的负极极片，其特征在于，所述第一活性物质层和/或所述第二活性物质层的单位涂布重量为20g/m 2-200g/m 2，优选为50g/m 2-180g/m 2。
  7. 根据权利要求6所述的负极极片，其特征在于，所述第二活性物质层的单位涂布重量与所述第一活性物质层的单位涂布重量的比值为0.05-0.5，优选为0.1-0.45。
  8. 根据权利要求1-7中任一项所述的负极极片，其特征在于，所述第一活性物质和所述第二活性物质独立选自软碳、硬碳、石墨、硅、硅氧化合物、硅碳复合物以及能与锂形成合金的金属中的一种或几种。
  9. 根据权利要求8所述的负极极片，其特征在于，所述第一活性物质和所述第二活性物质均为石墨。
  10. 锂离子二次电池，其特征在于，包括根据权利要求1-9中任一项所述 的负极极片。
  11. 一种装置，其特征在于，包括根据权利要求10所述的锂离子二次电池。
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