WO2024198566A1 - 电化学装置和电子装置 - Google Patents

电化学装置和电子装置 Download PDF

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Publication number
WO2024198566A1
WO2024198566A1 PCT/CN2023/141698 CN2023141698W WO2024198566A1 WO 2024198566 A1 WO2024198566 A1 WO 2024198566A1 CN 2023141698 W CN2023141698 W CN 2023141698W WO 2024198566 A1 WO2024198566 A1 WO 2024198566A1
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layer
negative electrode
silicon
electrochemical device
active material
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French (fr)
Inventor
扶强
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Ningde Amperex Technology Ltd
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Ningde Amperex Technology 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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/134—Electrodes based on metals, Si or alloys
    • 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
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • 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
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • 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
    • 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

Definitions

  • the present invention relates to the field of electrochemical energy storage, and in particular to electrochemical devices and electronic devices.
  • silicon-based materials as negative electrode active materials can greatly improve the energy density of electrochemical devices, but silicon-based materials are accompanied by more than 300% volume expansion and contraction during lithium ion insertion and extraction, leading to problems such as capacity decay. Therefore, further improvements in this regard are expected.
  • the present application provides an electrochemical device, the electrochemical device includes a negative electrode plate, the negative electrode plate includes a negative electrode current collector, a first layer and a second layer, and the negative electrode current collector is located between the first layer and the second layer.
  • the first layer includes a first negative electrode active material
  • the second layer includes a second negative electrode active material
  • the first negative electrode active material includes graphite
  • the second negative electrode active material includes graphite and a silicon-based material.
  • the ratio of the impedance of the first layer to the impedance of the second layer is 0.7 to 0.9.
  • the ratio of the capacity of the first layer to the capacity of the second layer is 0.6 to 1. In some embodiments, the ratio of the capacity of the first layer to the capacity of the second layer is 0.7 to 1. In some embodiments, the mass percentage of the silicon-based material in the second layer is 6% to 40%. In some embodiments, the mass percentage of the silicon-based material in the second layer is 12% to 20%. In some embodiments, the second layer further includes a binder, and the mass percentage of the binder in the second layer is 1.4% to 5%.
  • the second layer further includes carbon nanotubes, and the mass percentage of the carbon nanotubes in the second layer is In some embodiments, the second layer further comprises sodium carboxymethyl cellulose, and the mass percentage of sodium carboxymethyl cellulose in the second layer is 0.3% to 0.7%.
  • the silicon-based material comprises at least one of silicon, silicon-carbon material or silicon-oxygen material.
  • An embodiment of the present application further provides an electronic device, comprising the above-mentioned electrochemical device.
  • the present application makes the first negative electrode active material in the first layer of the negative electrode plate include graphite, and the second negative electrode active material in the second layer include graphite and a silicon-based material.
  • the ratio of the impedance of the first layer to the impedance of the second layer is 0.7 to 0.9, so that the second negative electrode active layer has a smaller rate during the charge and discharge process, and can improve the capacity retention rate of the electrochemical device without substantially losing the energy density of the electrochemical device.
  • FIG. 1 illustrates a cross-sectional view of a negative electrode sheet along a width direction according to some embodiments.
  • FIG. 1 shows a cross-sectional view of a negative electrode sheet along the width direction according to some embodiments.
  • the negative electrode sheet includes a negative electrode current collector 110, a first layer 111, and a second layer 112, and the negative electrode current collector 110 is located between the first layer 111 and the second layer 112.
  • the first layer 111 includes a first negative electrode active material
  • the first negative electrode active material includes graphite and substantially does not include a silicon-based material.
  • the mass percentage of the silicon-based material in the first negative electrode active material is less than 0.2%, it can be considered that the first negative electrode active material substantially does not include a silicon-based material.
  • the ineffective pores between the graphite in the first layer 111 during the cycle are reduced, thereby reducing the overall expansion of the negative electrode sheet.
  • the second layer 112 includes a second negative electrode active material
  • the second negative electrode active material includes graphite and a silicon-based material. Therefore, the present application concentrates the silicon-based material on one side of the negative electrode current collector 110. Generally, the mass percentage of the silicon-based material of the layers on both sides of the negative electrode current collector is the same. In the present application, it is equivalent to replacing the silicon-based material on one side with an equal volume of graphite, and replacing the graphite on the other side with an equal volume of silicon-based material.
  • the ratio of the impedance of the first layer 111 to the impedance of the second layer 112 is 0.7 to 0.9.
  • the impedance of the first layer 111 and the impedance of the second layer 112 can be adjusted by the Si content, conductive agent content, binder type, coating formula, coating quality, and compaction density of the corresponding coating. Since the impedance of the first layer 111 is less than the impedance of the second layer 112, the first layer 111 can be allowed to have a larger charge and discharge rate, and the second layer 112 can have a smaller charge and discharge rate. In this way, without changing the overall charge and discharge rate of the electrochemical device, reducing the charge and discharge rate of the second layer 112 containing silicon-based materials can slow down the capacity decay rate of the negative electrode plate and improve the capacity retention rate of the electrochemical device.
  • the ratio of the capacity of the first layer 111 to the capacity of the second layer 112 is 0.6 to 1.
  • the capacity of the first layer 111 can be adjusted by the coating quality, and the capacity of the second layer 112 can be adjusted by the coating quality and/or the Si content.
  • the ratio of the capacity of the first layer 111 to the capacity of the second layer 112 is 0.7 to 1.
  • the capacity retention rate of the electrochemical device is more significantly improved.
  • the mass percentage of the silicon-based material in the second layer 112 is 6% to 40%, or the mass percentage of silicon in the second layer 112 is 4% to 20%. In some embodiments, since only silicon in the silicon-based material plays a role in capacity, when the mass percentage of the silicon-based material in the second layer 112 is less than 6%, the mass percentage of silicon is very small, and the energy density gain of the electrochemical device decreases significantly; when the mass percentage of the silicon-based material in the second layer 112 is greater than 40%, the mass percentage of silicon is large, and the cyclic expansion of the second layer 112 will increase. In some embodiments, the mass percentage of the silicon-based material in the second layer 112 is 12% to 20%. When the mass percentage of the silicon-based material in the second layer 112 is 12% to 20%, or the mass percentage of silicon in the second layer 112 is 4% to 10%, the effect of improving the capacity retention rate of the electrochemical device is more significant.
  • the silicon-based material includes at least one of silicon, silicon-oxygen material, silicon-carbon material, or silicon-oxygen-carbon material.
  • the negative electrode current collector 110 may be at least one of copper foil, nickel foil, or a carbon-based current collector.
  • the first layer 111 and the second layer 112 may each include a conductive agent, a binder, and a thickener (e.g., sodium carboxymethyl cellulose).
  • the conductive agent in the first layer 111 and the second layer 112 may include conductive carbon black, Ketjen black, flake graphite, graphene, carbon At least one of nanotubes or carbon fibers.
  • the binder in the first layer 111 and the second layer 112 may include at least one of carboxymethyl cellulose (CMC), polyacrylic acid, polyvinyl pyrrolidone, polyaniline, polyimide, polyamide-imide, polysiloxane, styrene-butadiene rubber, epoxy resin, polyester resin, polyurethane resin or polyfluorene.
  • CMC carboxymethyl cellulose
  • the mass percentage of the first negative electrode active material in the first layer is 97% to 98%.
  • the mass percentage of the second negative electrode active material in the second layer is 93.6% to 98%.
  • the mass ratio of the first negative electrode active material, thickener and binder in the first layer 111 may be (97 to 98): (0.2 to 0.6): (1.8 to 2.4). In some embodiments, the mass ratio of the second negative electrode active material, conductive agent, binder and thickener in the second layer 112 may be (93.6 to 98): (0.3 to 0.7): (1.4 to 5): (0.3 to 0.7). In some embodiments, the second layer 112 further includes a binder, and the mass percentage of the binder in the second layer 112 is 1.4% to 5%. In some embodiments, the second layer 112 further includes carbon nanotubes, and the mass percentage of the carbon nanotubes in the second layer 112 is 0.3% to 0.7%. In some embodiments, the second layer 112 further includes sodium carboxymethyl cellulose, and the mass percentage of the sodium carboxymethyl cellulose in the second layer 112 is 0.3% to 0.7%.
  • the electrochemical device further includes a positive electrode sheet and a separator, wherein the positive electrode sheet and the negative electrode sheet are separated by the separator disposed therebetween.
  • the positive electrode sheet includes a positive electrode current collector and a positive electrode active material layer, and the positive electrode active material layer is located on one side or both sides of the positive electrode current collector.
  • the positive electrode current collector can be made of aluminum foil, and of course, other positive electrode current collectors commonly used in the art can also be used.
  • the thickness of the positive electrode current collector can be 1 ⁇ m to 50 ⁇ m.
  • the positive electrode active material layer may include a positive electrode active material, a conductive agent, and a binder.
  • the positive electrode active material may include at least one of lithium cobaltate, lithium iron phosphate, lithium aluminum oxide, lithium manganate, or nickel cobalt manganate.
  • the conductive agent in the positive electrode active material layer may include at least one of conductive carbon black, lamellar graphite, graphene, or carbon nanotubes.
  • the binder in the positive electrode active material layer may include at least one of polyvinylidene fluoride, a copolymer of vinylidene fluoride-hexafluoropropylene, a styrene-acrylate copolymer, a styrene-butadiene copolymer, a polyamide, a polyacrylonitrile, a polyacrylate, a polyacrylic acid, a polyacrylate, sodium carboxymethyl cellulose, polyvinyl acetate, polyvinylpyrrolidone, polyvinyl ether, polymethyl methacrylate, polytetrafluoroethylene, or polyhexafluoropropylene.
  • the mass ratio of the positive electrode active material, the conductive agent, and the binder in the positive electrode active material layer is (80-99): (0.1-10): (0.1-10), but this is merely an example, and any other suitable mass ratio may be used.
  • the separator includes at least one of polyethylene, polypropylene, polyvinylidene fluoride, polyethylene terephthalate, polyimide or aramid.
  • polyethylene includes at least one selected from high-density polyethylene, low-density polyethylene or ultra-high molecular weight polyethylene.
  • polyethylene and polypropylene have a good effect on preventing short circuits and can improve the stability of the battery through the shutdown effect.
  • the thickness of the separator is in the range of about 3 ⁇ m to 20 ⁇ m.
  • the surface of the isolation membrane may further include a porous layer, the porous layer being disposed on at least one surface of the isolation membrane, the porous layer including inorganic particles and a binder, the inorganic particles being selected from at least one of aluminum oxide ( Al2O3 ), silicon oxide ( SiO2 ), magnesium oxide (MgO), titanium oxide ( TiO2 ), hafnium dioxide ( HfO2 ), tin oxide ( SnO2 ), cerium dioxide ( CeO2 ), nickel oxide (NiO) , zinc oxide (ZnO), calcium oxide (CaO), zirconium oxide ( ZrO2 ), yttrium oxide ( Y2O3 ), silicon carbide (SiC), boehmite, aluminum hydroxide, magnesium hydroxide, calcium hydroxide, or barium sulfate.
  • Al2O3 aluminum oxide
  • SiO2 silicon oxide
  • MgO magnesium oxide
  • TiO2 titanium oxide
  • HfO2 hafnium dioxide
  • the pores of the isolation membrane have a diameter in the range of about 0.01 ⁇ m to 1 ⁇ m.
  • the binder of the porous layer is selected from at least one of polyvinylidene fluoride, copolymer of vinylidene fluoride and hexafluoropropylene, polyamide, polyacrylonitrile, polyacrylate, polyacrylic acid, polyacrylate, sodium carboxymethyl cellulose, polyvinylpyrrolidone, polyvinyl ether, polymethyl methacrylate, polytetrafluoroethylene or polyhexafluoropropylene.
  • the porous layer on the surface of the separator can improve the heat resistance, oxidation resistance and electrolyte wetting performance of the separator, and enhance the adhesion between the separator and the pole piece.
  • the electrochemical device includes a lithium ion battery, but the present application is not limited thereto.
  • the electrochemical device also includes an electrolyte, and the electrolyte includes at least one of a fluoroether, a fluoroethylene carbonate, or an ether nitrile.
  • the electrolyte also includes a lithium salt, and the lithium salt includes lithium bis(fluorosulfonyl)imide and lithium hexafluorophosphate, and the concentration of the lithium salt is 1 mol/L to 2 mol/L, and the mass ratio of lithium bis(fluorosulfonyl)imide and lithium hexafluorophosphate is 0.06 to 5.
  • the electrolyte may also include a non-aqueous solvent.
  • the non-aqueous solvent may be a carbonate compound, a carboxylate compound, an ether compound, other organic solvents, or a combination thereof.
  • the carbonate compound may be a linear carbonate compound, a cyclic carbonate compound, a fluorinated carbonate compound or a combination thereof.
  • chain carbonate compound examples include diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), Ethyl methyl carbonate (MEC) and combinations thereof.
  • chain carbonate compound examples include diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), methylpropyl carbonate (MPC), ethylpropyl carbonate (EPC), Ethyl methyl carbonate (MEC) and combinations thereof.
  • cyclic carbonate compounds examples include ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), vinyl ethylene carbonate (VEC) or combinations thereof.
  • fluorinated carbonate compounds are fluoroethylene carbonate (FEC), 1,2-difluoroethylene carbonate, 1,1-difluoroethylene carbonate, 1,1,2-trifluoroethylene carbonate, 1,1,2,2-tetrafluoroethylene carbonate, 1-fluoro-2-methylethylene carbonate, 1-fluoro-1-methylethylene carbonate, 1,2-difluoro-1-methylethylene carbonate, 1,1,2-trifluoro-2-methylethylene carbonate, trifluoromethylethylene carbonate or combinations thereof.
  • FEC fluoroethylene carbonate
  • 1,2-difluoroethylene carbonate 1,1-difluoroethylene carbonate
  • 1,1,2-trifluoroethylene carbonate 1,1,2,2-tetrafluoroethylene carbonate
  • 1-fluoro-2-methylethylene carbonate 1-fluoro-1-methylethylene carbonate
  • 1,2-difluoro-1-methylethylene carbonate 1,1,2-trifluoro-2-methylethylene carbonate
  • trifluoromethylethylene carbonate trifluoromethylethylene carbonate
  • carboxylic acid ester compound examples include methyl acetate, ethyl acetate, n-propyl acetate, tert-butyl acetate, methyl propionate, ethyl propionate, propyl propionate, ⁇ -butyrolactone, decanolide, valerolactone, mevalonolactone, caprolactone, methyl formate, or a combination thereof.
  • ether compound examples include dibutyl ether, tetraglyme, diglyme, 1,2-dimethoxyethane, 1,2-diethoxyethane, ethoxymethoxyethane, 2-methyltetrahydrofuran, tetrahydrofuran, or a combination thereof.
  • organic solvents examples include dimethyl sulfoxide, 1,2-dioxolane, sulfolane, methyl sulfolane, 1,3-dimethyl-2-imidazolidinone, N-methyl-2-pyrrolidone, formamide, dimethylformamide, acetonitrile, trimethyl phosphate, triethyl phosphate, trioctyl phosphate, and phosphoric acid esters or combinations thereof.
  • Embodiments of the present application also provide electronic devices including the above-mentioned electrochemical devices.
  • the electronic devices of the embodiments of the present application are not particularly limited, and they can be any electronic devices known in the prior art.
  • the electronic device may include, but is not limited to, a laptop computer, a pen-input computer, a mobile computer, an e-book player, a portable phone, a portable fax machine, a portable copier, a portable printer, a head-mounted stereo headset, a video recorder, an LCD TV, a portable cleaner, a portable CD player, a mini-disc, a transceiver, an electronic notepad, a calculator, a memory card, a portable recorder, a radio, a backup power supply, a motor, a car, a motorcycle, a power bicycle, a bicycle, a drone, a lighting fixture, a toy, a game console, a clock, an electric tool, a flashlight, a camera, a large household battery and a lithium
  • negative electrode sheet artificial graphite, binder polyvinylidene fluoride and sodium carboxymethyl cellulose, which are negative electrode active materials, are dissolved in deionized water in a weight ratio of 97.5:2.1:0.44 to form a first slurry.
  • a 6 ⁇ m thick copper foil is used as the negative electrode current collector, and the first slurry is applied on one side of the negative electrode current collector with a coating weight of 0.086mg/ mm2 to form a first layer.
  • positive electrode sheet The positive electrode active material lithium cobalt oxide, conductive agent, and binder polyvinylidene fluoride (PVDF) are dissolved in N-methylpyrrolidone (NMP) solution at a weight ratio of 97.6:1.1:1.3 to form positive electrode slurry.
  • NMP N-methylpyrrolidone
  • An 8 ⁇ m thick aluminum foil is used as the positive electrode current collector, and the positive electrode slurry is coated on both sides of the positive electrode current collector with a coating thickness of 50 ⁇ m. After drying, cold pressing, and slitting, the positive electrode sheet is obtained.
  • isolation membrane substrate is 8 ⁇ m thick polyethylene (PE), and a 2 ⁇ m alumina ceramic layer is coated on both sides of the isolation membrane substrate. Finally, 2.5 mg of binder polyvinylidene fluoride (PVDF) is coated on both sides of the ceramic layer and dried.
  • PE polyethylene
  • PVDF binder polyvinylidene fluoride
  • Preparation of lithium-ion battery stack the positive electrode sheet, separator, and negative electrode sheet in order, so that the separator is between the positive electrode sheet and the negative electrode sheet to play an isolating role, and wind them to obtain the electrode assembly. Place the electrode assembly in the outer packaging aluminum plastic film, remove moisture at 80°C, inject the above electrolyte and package, and obtain the lithium-ion battery through the process of formation, degassing, shaping, etc.
  • Comparative Example 2 The difference between Comparative Example 2 and Examples 1 to 11 lies in the preparation of the negative electrode sheet, specifically, the parameters of the first layer and the second layer are different, see Table 1 and Table 2 for details.
  • the following method is used to measure the corresponding parameters, and the effective area of the single-layer laminated battery used in the present application is 49.5*42 mm 2 .
  • the AC impedance method can be used to test Rs+Rct (Rs refers to ohmic impedance, Rct refers to electrochemical transfer impedance). Due to the influence of other conditions such as the area of the manufactured single-layer laminated battery and the manufacturing process, the absolute value of Rs+Rct may vary, but the ratio of Rs+Rct on both sides of the electrode can be used as the basis for current shunt on both sides of the electrode.
  • Capacity retention rate after 500 cycles capacity after 500 cycles / fresh battery capacity.
  • the capacity test conditions are at 25°C, 0.7C constant current charging to 4.5V, then constant voltage charging to 0.02C, and then 0.2C DC discharge to 3.0V as one cycle, with a total of 500 cycles.
  • Tables 1 and 2 show various parameters and evaluation results of Examples 1 to 11 and Comparative Examples 1 to 4.

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Abstract

本申请的实施例提供了电化学装置和电子装置。电化学装置包括负极极片，负极极片包括负极集流体、第一层和第二层，负极集流体位于第一层和第二层之间。第一层包括第一负极活性材料，第二层包括第二负极活性材料，第一负极活性材料包括石墨，第二负极活性材料包括石墨和硅基材料。第一层的阻抗与第二层的阻抗的比值为0.7至0.9，本申请的负极极片能够在基本不损失电化学装置的能量密度的情况下，提升电化学装置的容量保持率。

Description

电化学装置和电子装置
相关申请的交叉引用
本申请基于申请号为202310303762.8、申请日为2023年03月27日，名称为“电化学装置和电子装置”的中国专利申请提出，并要求该中国专利申请的优先权，该中国专利申请的全部内容在此引入本申请作为参考。
技术领域
本申请涉及电化学储能领域，具体地涉及电化学装置和电子装置。
背景技术
伴随电化学储能技术的发展，对电化学装置(例如，锂离子电池)的能量密度和循环性能提出了越来越高的要求。将硅基材料作为负极活性材料，能够大大地提升电化学装置的能量密度，但是硅基材料在锂离子脱嵌过程中伴随着300％以上的体积膨胀和收缩，导致容量衰减等问题。因此，期望这方面的进一步改进。
发明内容
本申请提供了一种电化学装置，电化学装置包括负极极片，负极极片包括负极集流体、第一层和第二层，负极集流体位于第一层和第二层之间。第一层包括第一负极活性材料，第二层包括第二负极活性材料，第一负极活性材料包括石墨，第二负极活性材料包括石墨和硅基材料。第一层的阻抗与第二层的阻抗的比值为0.7至0.9。
在一些实施例中，第一层的容量与第二层的容量的比值为0.6至1。在一些实施例中，第一层的容量与第二层的容量的比值为0.7至1。在一些实施例中，第二层中的硅基材料的质量百分含量为6％至40％。在一些实施例中，第二层中的硅基材料的质量百分含量为12％至20％。在一些实施例中，第二层还包括粘结剂，第二层中的粘结剂的质量百分含量为1.4％至5％。在一些实施例中，第二层还包括碳纳米管，第二层中的碳纳米管的质量百分含量为 0.3％至0.7％。在一些实施例中，第二层还包括羧甲基纤维素钠，第二层中的羧甲基纤维素钠的质量百分含量为0.3％至0.7％。在一些实施例中，硅基材料包括硅、硅碳材料或硅氧材料中的至少一种。
本申请的实施例还提供了一种电子装置，包括上述的电化学装置。
本申请通过使得负极极片的第一层中的第一负极活性材料包括石墨，第二层中的第二负极活性材料包括石墨和硅基材料，第一层的阻抗与第二层的阻抗的比值为0.7至0.9，使得第二负极活性层在充放电过程中倍率较小，能够在基本不损失电化学装置的能量密度的情况下，提升电化学装置的容量保持率。
附图说明
图1示出了根据一些实施例的负极极片的沿着宽度方向的截面图。
具体实施方式
下面的实施例可以使本领域技术人员更全面地理解本申请，但不以任何方式限制本申请。
本申请的一些实施例提供了一种电化学装置，电化学装置包括负极极片。图1示出了根据一些实施例的负极极片的沿着宽度方向的截面图。在一些实施例中，如图1所示，负极极片包括负极集流体110、第一层111和第二层112，负极集流体110位于第一层111和第二层112之间。在一些实施例中，第一层111包括第一负极活性材料，第一负极活性材料包括石墨而基本上不包括硅基材料。应该理解，第一负极活性材料中的硅基材料的质量百分含量为0.2％以下时可以认为第一负极活性材料基本上不包括硅基材料。通过将硅基材料与第一层111中的石墨完全分离，达到减少循环过程中第一层111中的石墨间的无效孔隙，从而减小负极极片整体的膨胀。
在一些实施例中，第二层112包括第二负极活性材料，第二负极活性材料包括石墨和硅基材料。因此，本申请将硅基材料集中在负极集流体110的其中一侧上。通常地，负极集流体两侧的层的硅基材料的质量百分含量是相同的。在本申请中，相当于是将其中一侧的硅基材料替换为等容量的石墨，另一侧的石墨替换为等容量的硅基材料。
在一些实施例中，第一层111的阻抗与第二层112的阻抗的比值为0.7至0.9。在一些实施例中，可以通过相应涂层的Si含量、导电剂含量、粘结剂类型、涂层配方、涂布质量、压实密度来调节第一层111的阻抗与第二层112的阻抗。由于第一层111的阻抗小于第二层112的阻抗，可以允许第一层111具有更大的充放电倍率，第二层112具有更小的充放电倍率，如此，在不改变电化学装置的整体充放电倍率的情况下，减小含有硅基材料的第二层112的充放电倍率可以减慢负极极片的容量衰减速度，提升电化学装置的容量保持率。
在一些实施例中，第一层111的容量与第二层112的容量的比值为0.6至1。在一些实施例中，可以通过涂布质量来调节第一层111的容量，可以通过涂布质量和/或Si含量来调节第二层112中的容量。通过使得第一层111的容量与第二层112的容量的比值为0.6至1，均可以实现提升电化学装置的容量保持率。
在一些实施例中，第一层111的容量与第二层112的容量的比值为0.7至1。当第一层111的容量与第二层112的容量的比值为0.7至1时，电化学装置的容量保持率的提升效果更为显著。
在一些实施例中，第二层112中的硅基材料的质量百分含量为6％至40％，或第二层112硅的质量百分含量为4％至20％。在一些实施例中，由于硅基材料中只有硅发挥容量，第二层112中的硅基材料的质量百分含量小于6％时，硅的质量百分含量很小，电化学装置的能量密度收益下降显著；第二层112中的硅基材料的质量百分含量大于40％时，硅的质量百分含量较大，第二层112的循环膨胀会增大。在一些实施例中，第二层112中的硅基材料的质量百分含量为12％至20％。当第二层112中的硅基材料的质量百分含量为12％至20％时＝，或第二层112中的硅的质量百分含量为4％至10％，电化学装置的容量保持率的提升效果更为显著。
在一些实施例中，硅基材料包括硅、硅氧材料、硅碳材料或硅氧碳材料中的至少一种。在一些实施例中，负极集流体110可以采用铜箔、镍箔或碳基集流体中的至少一种。第一层111和第二层112均可以包括导电剂、粘结剂和增稠剂(例如，羧甲基纤维素钠)。在一些实施例中，第一层111和第二层112中的导电剂可以包括导电炭黑、科琴黑、片层石墨、石墨烯、碳 纳米管或碳纤维中的至少一种。在一些实施例中，第一层111和第二层112中的粘结剂可以包括羧甲基纤维素(CMC)、聚丙烯酸、聚乙烯基吡咯烷酮、聚苯胺、聚酰亚胺、聚酰胺酰亚胺、聚硅氧烷、丁苯橡胶、环氧树脂、聚酯树脂、聚氨酯树脂或聚芴中的至少一种。在一些实施例中，第一层中的第一负极活性材料的质量百分含量为97％至98％。在一些实施例中，第二层中的第二负极活性材料的质量百分含量为93.6％至98％。在一些实施例中，第一层111中的第一负极活性材料、增稠剂和粘结剂的质量比可以为(97至98)：(0.2至0.6)：(1.8至2.4)。在一些实施例中，第二层112中的第二负极活性材料、导电剂、粘结剂和增稠剂的质量比可以为(93.6至98)：(0.3至0.7)：(1.4至5)：(0.3至0.7)。在一些实施例中，第二层112还包括粘结剂，第二层112中的粘结剂的质量百分含量为1.4％至5％。在一些实施例中，第二层112还包括碳纳米管，第二层112中的碳纳米管的质量百分含量为0.3％至0.7％。在一些实施例中，第二层112还包括羧甲基纤维素钠，第二层112中的羧甲基纤维素钠的质量百分含量为0.3％至0.7％。
在一些实施例中，电化学装置还包括正极极片和隔离膜，正极极片和负极极片由设置在它们之间的隔离膜间隔开。
在一些实施例中，正极极片包括正极集流体和正极活性材料层，正极活性材料层位于正极集流体的一侧或两侧上。在一些实施例中，正极集流体可以采用铝箔，当然，也可以采用本领域常用的其他正极集流体。在一些实施例中，正极集流体的厚度可以为1μm至50μm。
在一些实施例中，正极活性材料层可以包括正极活性材料、导电剂和粘结剂。在一些实施例中，正极活性材料可以包括钴酸锂、磷酸铁锂、铝酸锂、锰酸锂或镍钴锰酸锂中的至少一种。在一些实施例中，正极活性材料层中的导电剂可以包括导电炭黑、片层石墨、石墨烯或碳纳米管中的至少一种。在一些实施例中，正极活性材料层中的粘结剂可以包括聚偏氟乙烯、偏氟乙烯-六氟丙烯的共聚物、苯乙烯-丙烯酸酯共聚物、苯乙烯-丁二烯共聚物、聚酰胺、聚丙烯腈、聚丙烯酸酯、聚丙烯酸、聚丙烯酸盐、羧甲基纤维素纳、聚醋酸乙烯酯、聚乙烯呲咯烷酮、聚乙烯醚、聚甲基丙烯酸甲酯、聚四氟乙烯或聚六氟丙烯中的至少一种。在一些实施例中，正极活性材料层中的正极活性材料、导电剂和粘结剂的质量比为(80-99)：(0.1-10)：(0.1-10)，但是这 仅是示例，可以采用任何其他合适的质量比。
在一些实施例中，隔离膜包括聚乙烯、聚丙烯、聚偏氟乙烯、聚对苯二甲酸乙二醇酯、聚酰亚胺或芳纶中的至少一种。例如，聚乙烯包括选自高密度聚乙烯、低密度聚乙烯或超高分子量聚乙烯中的至少一种。尤其是聚乙烯和聚丙烯，它们对防止短路具有良好的作用，并可以通过关断效应改善电池的稳定性。在一些实施例中，隔离膜的厚度在约3μm至20μm的范围内。
在一些实施例中，隔离膜的表面还可以包括多孔层，多孔层设置在隔离膜的至少一个表面上，多孔层包括无机颗粒和粘结剂，无机颗粒选自氧化铝(Al2O3)、氧化硅(SiO2)、氧化镁(MgO)、氧化钛(TiO2)、二氧化铪(HfO2)、氧化锡(SnO2)、二氧化铈(CeO2)、氧化镍(NiO)、氧化锌(ZnO)、氧化钙(CaO)、氧化锆(ZrO2)、氧化钇(Y2O3)、碳化硅(SiC)、勃姆石、氢氧化铝、氢氧化镁、氢氧化钙或硫酸钡中的至少一种。在一些实施例中，隔离膜的孔具有在约0.01μm至1μm的范围的直径。多孔层的粘结剂选自聚偏氟乙烯、偏氟乙烯-六氟丙烯的共聚物、聚酰胺、聚丙烯腈、聚丙烯酸酯、聚丙烯酸、聚丙烯酸盐、羧甲基纤维素钠、聚乙烯呲咯烷酮、聚乙烯醚、聚甲基丙烯酸甲酯、聚四氟乙烯或聚六氟丙烯中的至少一种。隔离膜表面的多孔层可以提升隔离膜的耐热性能、抗氧化性能和电解质浸润性能，增强隔离膜与极片之间的粘结性。
在一些实施例中，电化学装置包括锂离子电池，但是本申请不限于此。在一些实施例中，电化学装置还包括电解液，电解液包括氟醚、氟代碳酸乙烯酯或醚腈中至少一种。在一些实施例中，电解液还包括锂盐，锂盐包括双(氟磺酰基)酰亚胺锂和六氟磷酸锂，锂盐的浓度为1mol/L至2mol/L，且双(氟磺酰基)酰亚胺锂和六氟磷酸锂的质量比为0.06至5。在一些实施例中，电解液还可以包括非水溶剂。非水溶剂可为碳酸酯化合物、羧酸酯化合物、醚化合物、其它有机溶剂或它们的组合。
碳酸酯化合物可为链状碳酸酯化合物、环状碳酸酯化合物、氟代碳酸酯化合物或其组合。
链状碳酸酯化合物的实例为碳酸二乙酯(DEC)、碳酸二甲酯(DMC)、碳酸二丙酯(DPC)、碳酸甲丙酯(MPC)、碳酸乙丙酯(EPC)、碳酸 甲乙酯(MEC)及其组合。环状碳酸酯化合物的实例为碳酸亚乙酯(EC)、碳酸亚丙酯(PC)、碳酸亚丁酯(BC)、碳酸乙烯基亚乙酯(VEC)或者其组合。所述氟代碳酸酯化合物的实例为碳酸氟代亚乙酯(FEC)、碳酸1,2-二氟亚乙酯、碳酸1,1-二氟亚乙酯、碳酸1,1,2-三氟亚乙酯、碳酸1,1,2,2-四氟亚乙酯、碳酸1-氟-2-甲基亚乙酯、碳酸1-氟-1-甲基亚乙酯、碳酸1,2-二氟-1-甲基亚乙酯、碳酸1,1,2-三氟-2-甲基亚乙酯、碳酸三氟甲基亚乙酯或者其组合。
羧酸酯化合物的实例为乙酸甲酯、乙酸乙酯、乙酸正丙酯、乙酸叔丁酯、丙酸甲酯、丙酸乙酯、丙酸丙酯、γ-丁内酯、癸内酯、戊内酯、甲瓦龙酸内酯、己内酯、甲酸甲酯或者其组合。
醚化合物的实例为二丁醚、四甘醇二甲醚、二甘醇二甲醚、1,2-二甲氧基乙烷、1,2-二乙氧基乙烷、乙氧基甲氧基乙烷、2-甲基四氢呋喃、四氢呋喃或者其组合。
其它有机溶剂的实例为二甲亚砜、1,2-二氧戊环、环丁砜、甲基环丁砜、1,3-二甲基-2-咪唑烷酮、N-甲基-2-吡咯烷酮、甲酰胺、二甲基甲酰胺、乙腈、磷酸三甲酯、磷酸三乙酯、磷酸三辛酯、和磷酸酯或者其组合。
本申请的实施例还提供了包括上述电化学装置的电子装置。本申请实施例的电子装置没有特别限定，其可以是用于现有技术中已知的任何电子装置。在一些实施例中，电子装置可以包括，但不限于，笔记本电脑、笔输入型计算机、移动电脑、电子书播放器、便携式电话、便携式传真机、便携式复印机、便携式打印机、头戴式立体声耳机、录像机、液晶电视、手提式清洁器、便携CD机、迷你光盘、收发机、电子记事本、计算器、存储卡、便携式录音机、收音机、备用电源、电机、汽车、摩托车、助力自行车、自行车、无人机、照明器具、玩具、游戏机、钟表、电动工具、闪光灯、照相机、家庭用大型蓄电池和锂离子电容器等。
下面列举了一些具体实施例和对比例以更好地对本申请进行说明，其中，采用锂离子电池作为示例。
对比例1
负极极片的制备：将负极活性材料人造石墨、粘结剂聚偏氟乙烯和羧甲基纤维素钠按重量比97.5：2.1：0.44的比例溶于去离子水中，形成第一浆料。采用6μm厚的铜箔作为负极集流体，将第一浆料涂布于负极集流体的一侧上，涂布重量为0.086mg/mm2，形成第一层。将负极活性材料人造石墨、Si、粘结剂聚丙烯酸、碳纳米管和羧甲基纤维素钠按重量比59.7：36：3.5：0.4：0.4的比例溶于去离子水中，形成第二浆料。将第二浆料涂布于负极集流体的另一侧上，涂布重量为0.035.5mg/mm2，形成第二层。经过干燥、冷压、分切后得到负极极片。
正极极片制备：将正极活性材料钴酸锂、导电剂、粘结剂聚偏氟乙烯(PVDF)按重量比97.6：1.1：1.3的比例溶于N-甲基吡咯烷酮(NMP)溶液中，形成正极浆料。采用8μm厚的铝箔作为正极集流体，将正极浆料涂覆于正极集流体的两侧上，涂布厚度均为50μm。经过干燥、冷压、分切后得到正极极片。
隔离膜的制备：隔离膜基材为8μm厚的聚乙烯(PE)，在隔离膜基材的两侧各涂覆2μm氧化铝陶瓷层，最后在涂布了陶瓷层的两侧各涂覆2.5mg的粘结剂聚偏氟乙烯(PVDF)，烘干。
电解液的制备：在含水量小于10ppm的环境下，将六氟磷酸锂与非水有机溶剂(碳酸乙烯酯(EC)：碳酸丙烯酯(PC)：聚丙烯(PP)：二乙基碳酸酯(DEC)＝1：1：1：1，质量百分比)配制成锂盐浓度为1.15mol/L的电解液。
锂离子电池的制备：将正极极片、隔离膜、负极极片按顺序依次叠好，使隔离膜处于正极极片和负极极片中间起到隔离的作用，并卷绕得到电极组件。将电极组件置于外包装铝塑膜中，在80℃下脱去水分后，注入上述电解液并封装，经过化成、脱气、整形等工艺流程得到锂离子电池。
对比例2以及实施例1至11的区别在于负极极片的制备，具体地为第一层和第二层的参数不同，详见表1和表2。
另外，在本申请中，采用如下方法测量相应的参数，且本申请中使用的单层叠片电池有效面积为49.5*42mm2。
1)电池放电到3.0V，拆解得到正极极片和负极极片，泡碳酸二甲酯(DMC)溶液15min后干燥备用；
2)手套箱干燥惰性气体环境，取1)中正极极片和负极极片冲片、正负极匹配加隔离膜制成单层叠片电池，封装注液带压力夹具保持界面接触，0.7C恒流充电至充电截止电压然后恒压充电至电池达到满充状态，截止电流0.02C，0.2C直流放电至3.0V得到单层叠片电池的容量，然后计算得到负极极片单位面积容量(负极极片单位面积容量＝单层叠片电池容量/单层叠片电池有效面积)再根据负极极片的活性涂层面积即可计算得到负极极片单侧的容量，重复上述方法可以得到另一侧的容量；
3)使用2)中单层叠片电池使用交流阻抗法可以测试得到Rs+Rct(Rs指欧姆阻抗，Rct指电化学转移阻抗)，由于制成的单层叠片电池面积、制作工艺等其他条件的影响，Rs+Rct的绝对值可能存在差异，但电极两侧Rs+Rct的比值可作为电极两侧分流的依据。
4)循环500周容量保持率＝循环500周后容量/新鲜电池容量，容量测试条件为在25℃，0.7C恒流充电至4.5V，然后恒压充电至0.02C，然后以0.2C直流放电至3.0V作为一个循环，共循环500圈。
5)将锂离子电池以0.2C的倍率恒流充电至4.45V，然后恒压充电至0.02C，完成锂离子电池满充；接下来使用0.2C的倍率恒流放电，直至电压降低至3.0V，记录放电过程中，放出的总容量为C和电压平台U，测量锂离子电池实际的厚度及长和宽，并计算实际的锂离子电池体积V，能量密度＝C*U/V。
表1和表2示出了实施例1至11和对比例1至4的各项参数和评估结果。
表1

表2
通过比较实施例1至3和对比例1至2可知，在第一层的阻抗与第二层的阻抗的比值为0.7至0.9时，锂离子电池的能量密度损失较小，同时锂离子电池的容量保持率的提升效果较为显著。另外，随着第二层的硅质量含量的减小，锂离子电池的容量保持率呈现先增大后减小的趋势。
通过比较实施例4至6可知，随着第二层中的导电剂含量的增大，第二层的阻抗呈现减小的趋势，锂离子电池的容量保持率呈现减小的趋势。
通过比较实施例7至11可知，随着第一层的容量和第二层的容量的比值的增大，锂离子电池的能量密度呈现减小的趋势，锂离子电池的容量保持率呈现先增大后减小的趋势。
以上描述仅为本申请的较佳实施例以及对所运用技术原理的说明。本领域技术人员应当理解，本申请中所涉及的公开范围，并不限于上述技术特征的特定组合而成的技术方案，同时也应涵盖由上述技术特征或其等同特征进行任意组合而形成的其它技术方案。例如上述特征与本申请中公开的具有类似功能的技术特征进行互相替换而形成的技术方案。

Claims (12)

  1. 一种电化学装置，其包括：
    负极极片，所述负极极片包括负极集流体、第一层和第二层，所述负极集流体位于所述第一层和所述第二层之间；
    其中，所述第一层包括第一负极活性材料，所述第二层包括第二负极活性材料，所述第一负极活性材料包括石墨，所述第二负极活性材料包括石墨和硅基材料，所述第一层的阻抗与所述第二层的阻抗的比值为0.7至0.9。
  2. 根据权利要求1所述的电化学装置，其中，所述第一层的容量与所述第二层的容量的比值为0.6至1。
  3. 根据权利要求1所述的电化学装置，其中，所述第一层的容量与所述第二层的容量的比值为0.7至1。
  4. 根据权利要求1所述的电化学装置，其中，所述第二层中的所述硅基材料的质量百分含量为6％至40％。
  5. 根据权利要求1所述的电化学装置，其中，所述第二层中的所述硅基材料的质量百分含量为12％至20％。
  6. 根据权利要求4所述的电化学装置，其中，所述第二层中的硅的质量百分含量为4％至20％。
  7. 根据权利要求5所述的电化学装置，其中，所述第二层中的硅的质量百分含量为4％至10％。
  8. 根据权利要求4所述的电化学装置，其中，所述第二层还包括粘结剂，所述第二层中的所述粘结剂的质量百分含量为1.4％至5％。
  9. 根据权利要求4所述的电化学装置，其中，所述第二层还包括碳纳米管，所述第二层中的所述碳纳米管的质量百分含量为0.3％至0.7％。
  10. 根据权利要求4所述的电化学装置，其中，所述第二层还包括羧甲基纤维素钠，所述第二层中的所述羧甲基纤维素钠的质量百分含量为0.3％至0.7％。
  11. 根据权利要求1所述的电化学装置，其中，所述硅基材料包括硅、硅碳材料或硅氧材料中的至少一种。
  12. 一种电子装置，包括根据权利要求1至11中任一项所述的电化学装置。
PCT/CN2023/141698 2023-03-27 2023-12-25 电化学装置和电子装置 Ceased WO2024198566A1 (zh)

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