WO2011079735A1 - 大容量动力锂离子电池及其制备方法 - Google Patents

大容量动力锂离子电池及其制备方法 Download PDF

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WO2011079735A1
WO2011079735A1 PCT/CN2010/080001 CN2010080001W WO2011079735A1 WO 2011079735 A1 WO2011079735 A1 WO 2011079735A1 CN 2010080001 W CN2010080001 W CN 2010080001W WO 2011079735 A1 WO2011079735 A1 WO 2011079735A1
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ion battery
solvent
polymer electrolyte
positive electrode
lithium ion
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French (fr)
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刘志远
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Wuhu Power Technology Research Co Ltd
Chery Automobile Co Ltd
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Wuhu Power Technology Research Co Ltd
Chery Automobile 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H01M50/417—Polyolefins
    • 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
    • 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
    • H01M10/058—Construction or manufacture
    • H01M10/0583—Construction or manufacture of accumulators with folded construction elements except wound ones, i.e. folded positive or negative electrodes or separators, e.g. with "Z"-shaped electrodes or separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0085—Immobilising or gelification of electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0088—Composites
    • H01M2300/0094—Composites in the form of layered products, e.g. coatings
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the invention belongs to the technical field of lithium ion battery energy, and particularly relates to a large-capacity power lithium ion battery and a preparation method thereof. Background technique
  • Ni-Cd, Ni-MH batteries, lithium-ion batteries are environmentally friendly, high specific energy (140Wh/kg), high voltage platform, long cycle life, small self-discharge, no memory
  • High specific energy 140Wh/kg
  • high voltage platform long cycle life
  • small self-discharge no memory
  • features such as effects have been widely used in military and civilian applications, including 3C electronic products, various power tools, etc., and have potential as power sources for hybrid vehicles and electric vehicles.
  • a lithium ion battery disclosed in Chinese Patent Application No. 200810066054.2 has a negative electrode using a lithium titanate active material in a mass ratio of 90% to 93%, and a positive electrode using a phosphoric acid in an amount of 88% to 90% by mass.
  • the vanadium lithium active material, the electrolyte uses organic solvents such as ethylene carbonate (EC), propylene carbonate (DMC), ethyl methyl carbonate (EMC), and the lithium ion monomer power battery capacity is only 335 ⁇ 345 mAh;
  • organic solvents such as ethylene carbonate (EC), propylene carbonate (DMC), ethyl methyl carbonate (EMC), and the lithium ion monomer power battery capacity is only 335 ⁇ 345 mAh;
  • EC ethylene carbonate
  • DMC propylene carbonate
  • EMC ethyl methyl carbonate
  • the positive electrode active material of which is lithium manganate (LiMn 2 0 4 ), lithium iron phosphate (LiFeP0 4 ), lithium nickel cobaltate (LiNi x ) Co y M z 0 2 ) and one or more of a ternary material (LiNi x Mn x Cow x 0 2 ), or a mixture of lithium cobaltate (LiCo0 2 ) and one of them;
  • a negative electrode active material is a sub Micron-sized lithium titanate; electrolyte is lithium hexafluorophosphate (LiPF 6 ), solvent is a mixture of ethylene carbonate (EC), dimethyl carbonate (DMC) and ethyl methyl carbonate (EMC), this lithium ion single Body battery capacity is only 400 mAh.
  • the above two types of lithium ion batteries use less safe organic electrolytes, and the monomer capacity is small, and they cannot be used as power sources in the fields of hybrid vehicles and electric vehicles
  • the technical problem to be solved by the present invention is to provide a large-capacity power lithium ion battery which can be used as a power source in the automotive field in view of the deficiencies of the prior art.
  • the present invention provides a large-capacity power lithium ion battery, which is composed of a positive electrode,
  • the gel state polymer electrolyte film, the polyethylene porous film, the gel polymer electrolyte film and the negative electrode are sequentially stacked and packaged, wherein the negative electrode and the positive electrode are separated by a polyethylene porous film, and the positive electrode or the negative electrode respectively Separated from the polyethylene porous film by the gel state polymer electrolyte film, the key is that the active material of the negative electrode is modified lithium titanate; the active material of the positive electrode is ternary material, lithium manganate and phosphoric acid One or more of iron lithium; the gel state polymer electrolyte is mixed with an electrolyte solution containing a lithium salt and an organic solvent and a polymer electrolyte dissolved in a solvent, and then coated on both sides of the polyethylene porous film or respectively It is coated on both sides of the positive and negative electrodes to dry.
  • the large-capacity power lithium ion battery provided by the invention adopts modified lithium titanate (Li 4 Ti 5 0 12 /C ) as an active material of a negative electrode, and uses a ternary material (LiNi x Mn y C 0l y 0 2 or One or more of lithium manganate (LiMn 2 0 4 ) and lithium iron phosphate (LiFeP0 4 ) are used as positive electrode active materials, which have better thermal stability and structural stability, and the capacity of single cells is 10A1! ⁇ 50Ah or so, with high safety performance, good high rate performance, good cycle performance and long cycle life.
  • the modified lithium titanate has a particle size smaller than ⁇ and a specific surface of more than 2.0 m 2 /g.
  • the polymer electrolyte is polyvinylidene fluoride, a vinylidene fluoride-hexafluoropropylene copolymer, a homopolymer or copolymer of ethylene oxide-epoxy propylene, polymethyl methacrylate, polyacrylonitrile, polyamino One or more mixtures of formic acid esters, and a solvent for dissolving the polymer electrolyte is one or a mixture of one of a ketone solvent, a lipid solvent and a heterocyclic solvent.
  • the ketone solvent is one or a mixed solvent of acetone and methyl ethyl ketone
  • the lipid solvent is diethyl carbonate, dipropyl carbonate, ethyl acetate, methyl acetate, ethylene sulfite, and sub
  • the heterocyclic solvent is one or a mixed solvent of r-butyrolactone or tetrahydrofuran.
  • the lithium salt is a mixture of one or more of LiPF 6 , LiC 10 4 , LiBOB, LiBF 4 , LiBF 6 , LiAsF 6 , LiCF 3 S0 3 and LiN (S0 2 C 2 F 5 ) 2 .
  • the organic solvent may be a ketone or a lipid organic solvent, and is not particularly required.
  • a second object of the present invention is to provide a method for preparing the above-described large-capacity power lithium ion battery, which comprises the following steps:
  • Step A preparing a negative electrode slurry by dissolving 75 wt% to 98 wt% of modified lithium titanate, 1 wt% to 15 wt% of a conductive agent, and 1 wt% to 10 wt% of a binder in a solvent.
  • Step ⁇ containing 80% by weight to 98% by weight of the positive electrode active material, 1% by weight to 10% by weight of the guide
  • the electric agent and 1% by weight to 10% by weight of the binder are dissolved in a solvent to prepare a positive electrode slurry, and the aluminum foil having a thickness of 15 ⁇ m to 20 ⁇ m is used as a current collector, and the positive electrode slurry is coated on the front and back surfaces of the aluminum foil. Drying, forming a pole piece, then rolling and shearing the pole piece to form a positive electrode;
  • Step C dissolving an electrolyte solution prepared by dissolving a lithium salt in an organic solvent, mixing with a polymer solution obtained by dissolving a polymer in a solvent, and applying it on both surfaces of a polyethylene porous film or positive and negative electrodes, and drying to obtain a gel state polymer electrolyte film;
  • Step D The above positive electrode, gel polymer electrolyte membrane, polyethylene porous membrane, gel polymer electrolyte membrane and negative electrode are sequentially passed through a stack, a coating, a welding electrode, and a packaging process to obtain a power lithium ion. a semi-finished battery, wherein the negative electrode and the positive electrode are separated by a gel polymer electrolyte membrane and a polyethylene porous film;
  • Step ⁇ The power lithium ion battery semi-finished product obtained in step D is formed, divided and tested to obtain a finished lithium ion battery.
  • the coating amount of the negative electrode slurry on the negative electrode is less than 40 mg/cm 2 .
  • the coating amount of the positive electrode slurry on the positive electrode is less than 40 mg/cm 2 .
  • the conductive agent described in the above steps A, B is a mixture of one or more of superconducting carbon black, conductive graphite or conductive carbon nanotubes; the binder is polytetrafluoroethylene, polyvinylidene fluoride Or a mixture of one or more of the polymeric resins; the solvent in the positive electrode slurry and the negative electrode slurry is N-methylpyrrolidone or dimethylamide or dimethylacetamide.
  • the power lithium ion battery of the invention has the characteristics of environmental friendliness, good high rate performance, good heat dissipation performance, simple preparation, no environmental pollution, no leakage, long storage life, easy enlargement, wide temperature range, and wide temperature range. It is used as a power source in the fields of hybrid electric vehicles and electric vehicles.
  • FIG. 1 is a flow chart of a method for preparing a large-capacity power lithium ion battery of the present invention
  • Fig. 2 is a view showing a stacking manner of a positive electrode, a negative electrode, and a polyethylene porous film coated with a gel polymer electrolyte of the high-capacity lithium ion battery of the present invention.
  • Example 1 The large-capacity power lithium ion battery of the embodiment is designed according to the rated capacity of the single cell of 10 Ah, and is composed of a positive electrode, a gel state polymer electrolyte film, a polyethylene porous film, a gel state polymer electrolyte film, and a negative electrode.
  • the polyethylene porous film coated with the gel polymer electrolyte and the negative electrode are stacked and packaged, wherein the negative electrode and the positive electrode are separated by the gel polymer electrolyte film and the polyethylene porous film, the key lies in the negative
  • the active material of the electrode is a modified lithium titanate having a particle diameter of 0.165 ⁇ and a specific surface area of 9.2 m 2 /g; the active material of the positive electrode is a ternary material; and the film of the gel state polymer electrolyte is included
  • the electrolyte of the lithium salt or the organic solvent is mixed with the polymer electrolyte dissolved in the solvent, and then coated on the polyethylene porous film or dried on both sides of the positive and negative electrodes.
  • the specific preparation method is as follows:
  • Step A 84% by weight of modified lithium titanate, 7% by weight of conductive carbon black and 9% by weight of polyvinylidene fluoride are used as solute, and N-methylpyrrolidone is used as a solvent to adjust a paste-like negative electrode slurry.
  • the negative electrode slurry is applied to the front and back sides of the copper foil and dried at 120 ° C for 6 hours to form a pole piece, and then the pole piece is crushed and sheared. , a negative electrode is formed, and the density of the negative electrode is 4.6 g/cm 3 ;
  • Step B using 95% by weight of ternary material, 1.5% by weight of black block black, 1.5% by weight of conductive carbon black, and 4% by weight of polyvinylidene fluoride as a solute, and adjusting with N-methylpyrrolidone as a solvent
  • Paste positive electrode slurry using 15 ⁇ thick aluminum foil as current collector, apply positive electrode slurry to the front and back sides of aluminum foil and dry at 120 °C for 8 hours to make pole piece, then pole The sheet is rolled and sheared to form a positive electrode, and the density of the positive electrode is 3.8 g/cm 3 ;
  • Step C The lithium salt LiPF 6 is dissolved in an organic solvent to prepare an electrolyte, and mixed with a polymer electrolyte dissolved in a solvent.
  • a film of a gel state polymer electrolyte is obtained, wherein the solute of the polymer solution is a vinylidene fluoride-hexafluoropropylene copolymer, and the solvent is diethyl carbonate. a mixture of dipropylene carbonate;
  • Step D sequentially depositing the above positive electrode, gel polymer electrolyte membrane, polyethylene porous membrane, gel polymer electrolyte membrane and negative electrode through stacking, coating, welding of lugs, packaging with aluminum-plastic composite film, etc. After the process, a power lithium ion battery semi-finished product is obtained. As shown in FIG. 2, the negative electrode 1 and the positive electrode 2 are separated by a film 3 of a gel state polymer electrolyte during stacking;
  • Step E The power lithium ion battery semi-finished product obtained in step D is formed, divided, and tested to obtain a finished lithium ion battery product.
  • the internal resistance of the power lithium ion battery of this embodiment is 2.4m Q
  • the capacity is 21.93Ah
  • the open circuit voltage is 2.436V
  • the battery has a voltage platform of 2.212V
  • the battery capacity retention rate after 500 cycles is 96.86%. .
  • Example 2 The large-capacity power lithium ion battery of the present embodiment is designed according to the rated capacity of the single cell of 40 Ah, and is sequentially stacked by a positive electrode, a gel state polymer electrolyte film, a polyethylene porous film, a gel state polymer electrolyte film, and a negative electrode. And encapsulated, wherein the negative electrode and the positive electrode are separated by a gel polymer electrolyte membrane and a polyethylene porous membrane, the key is that the active material of the negative electrode has a particle diameter of 0.165 ⁇ and a specific surface area of 9.2 m 2 /g.
  • the active material of the positive electrode is a ternary material
  • the film of the gelled polymer electrolyte is mixed with an electrolyte solution containing a lithium salt and an organic solvent and a polymer electrolyte dissolved in a solvent, and then coated It is coated on the polyethylene porous film or both sides of the positive and negative electrodes.
  • the specific preparation method is as follows:
  • Step A 84% by weight of modified lithium titanate, 7% by weight of conductive carbon black and 9% by weight of polyvinylidene fluoride are used as solute, and N-methylpyrrolidone is used as a solvent to adjust a paste-like negative electrode slurry.
  • the negative electrode slurry is applied to the front and back sides of the copper foil and dried at 120 ° C for 6 hours to form a pole piece, and then the pole piece is crushed and sheared. , a negative electrode is formed, and the density of the negative electrode is 4.6 g/cm 3 ;
  • Step B containing 93% by weight of lithium manganate, 1.5% by weight of ethyl black, 2% by weight of conductive carbon black, 3.5% by weight of polyvinylidene fluoride as a solute, and N-methylpyrrolidone as a solvent
  • Paste positive electrode slurry using 15 ⁇ thick aluminum foil as current collector, apply positive electrode slurry to the front and back sides of aluminum foil and dry at 120 °C for 8 hours to make pole piece, then pole The sheet is rolled and sheared to form a positive electrode, and the density of the positive electrode is 3.8 g/cm 3 ;
  • Step C The lithium salt 1 ⁇ ?? 6 is dissolved in an organic solvent to prepare an electrolyte, and is polymerized in a solvent.
  • the electrolyte After the electrolyte is mixed, it is coated on the two surfaces of the polyethylene porous film or the positive and negative electrodes, and dried to obtain a film of a gel state polymer electrolyte, wherein the solute of the conductive polymer solution is a vinylidene fluoride-hexafluoropropylene copolymer.
  • the solvent is a mixture of diethyl carbonate and dipropyl carbonate;
  • Step D sequentially depositing the above positive electrode, gel polymer electrolyte membrane, polyethylene porous membrane, gel polymer electrolyte membrane and negative electrode through stacking, coating, welding of lugs, packaging with aluminum-plastic composite film, etc. After the process, a power lithium ion battery semi-finished product is obtained. As shown in FIG. 2, the negative electrode 1 and the positive electrode 2 are separated by a film 3 of a gel state polymer electrolyte during stacking;
  • Step E The power lithium ion battery semi-finished product obtained in step D is formed, divided, and tested to obtain a finished lithium ion battery product.
  • the internal resistance of the power lithium ion battery of this embodiment is 2.35m Q
  • the capacity is 43.74Ah
  • the open circuit voltage is 2.537V
  • the battery has a voltage platform of 2.364V
  • the battery capacity retention rate after 8 cycles is 87.68%. .

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Description

大容量动力锂离子电池及其制备方法 技术领域
本发明属于锂离子电池能源技术领域， 特别涉及到一种大容量动力锂离子电池及 其制备方法。 背景技术
随着社会发展和科技进步， 人们对能源的需求越来越大。相比传统的铅酸蓄电池、 Ni-Cd、 Ni-MH电池来说， 锂离子蓄电池具有对环境友好、 比能量高 （140Wh/kg)、 电 压平台高、 循环寿命长、 自放电小、 无记忆效应等特点， 已广泛应用于军用、 民用领 域， 包括 3C 电子产品、 各种电动工具等， 并有希望作为动力源应用于混合动力车、 电动汽车领域。
目前锂离子电池技术还不够成熟， 存在安全性、 循环寿命、 比能量等一些问题， 特别是安全性和循环寿命的缺点， 大大限制了锂离子电池在汽车领域的应用。 例如申 请号为 200810066054.2 的中国专利申请中公开的一种锂离子电池， 其负电极采用占 90%〜93%质量比的钛酸锂活性物质，正电极采用占 88%〜90%质量比的磷酸钒锂活性 物质， 电解液采用碳酸乙烯脂 （EC )、 碳酸丙烯脂 （DMC )、 碳酸甲乙酯 （EMC ) 等 有机溶剂， 其锂离子单体动力电池容量只有 335〜345mAh ; 又例如申请号为 200810052728.3 的中国专利申请中公开的一种可快速充电的锂离子电池， 其正电极活 性物质为锰酸锂 （LiMn204)、 磷酸铁锂 （LiFeP04)、 镍钴酸锂 （ LiNixCoyMz02) 和三 元材料 （LiNixMnxCowx02) 中的一种或多种， 或钴酸锂 （LiCo02) 与其中的一种混合 物； 负电极活性材料为亚微米级钛酸锂； 电解质为六氟磷酸锂 （LiPF6 )， 溶剂为乙烯 碳酸脂 （EC )、 二甲基碳酸脂 （DMC ) 和乙基甲基碳酸脂 （EMC) 的多元混合物， 这 种锂离子单体电池容量只有 400多 mAh。 上述两种锂离子电池使用不太安全的有机电 解液， 单体容量很小， 都无法作为动力源应用于混合动力车、 电动汽车领域。 发明内容
本发明所要解决的技术问题在于， 针对现有技术的不足， 提供一种可作为动力源 应用于汽车领域的大容量动力锂离子电池。
为了解决上述的技术问题， 本发明提供了一种大容量动力锂离子电池， 由正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚合物电解质薄膜和负电极依次通 过堆叠、 封装而成， 其中负电极和正电极通过聚乙烯多孔薄膜隔离， 且正电极或负电 极分别与聚乙烯多孔薄膜之间通过凝胶态聚合物电解质薄膜隔离， 关键在于所述负电 极的活性材料为改性钛酸锂； 所述正电极的活性材料为三元材料、 锰酸锂和磷酸铁锂 中的一种或多种； 所述凝胶态聚合物电解质由包含锂盐、 有机溶剂的电解液与溶于溶 剂的聚合物电解质混合后， 涂覆于聚乙烯多孔薄膜两面上或分别涂覆于正负电极两面 上干燥而成。
本发明提供的大容量动力锂离子电池， 采用了改性钛酸锂 （Li4Ti5012/C ) 作为负 电极的活性材料， 以三元材料 （ LiNixMnyC0l y02 或
Figure imgf000004_0001
)、 锰酸锂 ( LiMn204) 和磷酸铁锂 （LiFeP04) 中的一种或多种作为正电极活性材料， 其热稳定 性与结构稳定性更好， 单体电池容量在 10A1！〜 50Ah左右， 具有较高的安全性能， 良 好的高倍率性能， 良好的循环性能和长循环寿命。
所述改性钛酸锂的粒度小于 Ιμηι, 比表面大于 2.0m2/g。
所述聚合物电解质为聚偏二氟乙烯、 偏氟乙烯 -六氟丙烯共聚物、 环氧乙烯 -环氧 丙烯的均聚物或共聚物、 聚甲基丙烯酸甲酯、 聚丙烯腈、 聚氨基甲酸脂中的一种或多 种混合物， 溶解聚合物电解质的溶剂为酮类溶剂、 脂类溶剂和杂环化溶剂中的一种或 几种混合溶剂。
所述酮类溶剂为丙酮、 甲乙酮中的一种或两种混合溶剂， 所述脂类溶剂为碳酸二 乙脂、 碳酸二丙脂、 乙酸乙酯、 乙酸甲酯、 亚硫酸亚乙酯、 亚硫酸亚丙酯中的一种或 多种混合溶剂， 所述杂环化溶剂为 r-丁内酯、 四氢呋喃中的一种或两种混合溶剂。
所述锂盐为 LiPF6、 LiC104、 LiBOB、 LiBF4、 LiBF6、 LiAsF6、 LiCF3S03和 LiN ( S02C2F5 ) 2中的一种或多种混合物。
所述有机溶剂可以采用酮类或者脂类有机溶剂， 没有特别要求。
本发明的第二个目的是提出上述大容量动力锂离子电池的制备方法， 该制备方法 包括以下步骤：
步骤 A: 将含 75重量％〜98重量％的改性钛酸锂、 1重量％〜15重量％的导电剂 和 1重量％〜10重量％的粘结剂溶于溶剂中制成负电极浆料，以 9μηι〜13μηι厚的铜箔 为集流体， 将负电极浆料涂在铜箔正、 反面上并干燥， 制成极片， 然后将极片碾压、 剪切， 制成负电极；
步骤 Β: 将含 80重量％〜98重量％的正电极活性材料、 1重量％〜10重量％的导 电剂和 1重量％〜10重量％的粘结剂溶于溶剂中制成正电极浆料， 以 15μηι〜20μηι厚 的铝箔为集流体， 将正电极浆料涂覆在铝箔正、 反面上并干燥， 制成极片， 然后将极 片碾压、 剪切， 制成正电极；
步骤 C : 将锂盐溶于有机溶剂中制成的电解液， 与聚合物溶于溶剂中得到的聚合 物溶液混合后涂于聚乙烯多孔薄膜或正、 负电极的两表面上， 干燥后得到凝胶态聚合 物电解质薄膜；
步骤 D: 将上述的正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚 合物电解质薄膜和负电极依次通过堆叠、 包膜、 焊接极耳、 封装工序后得到动力锂离 子电池半成品， 其中负电极和正电极通过凝胶态聚合物电解质膜和聚乙烯多孔薄膜隔 离；
步骤 Ε : 将步骤 D中得到的动力锂离子电池半成品进行化成、 分容、 检测， 得到 动力锂离子电池成品。
上述步骤 Α中， 负电极浆料在负电极上的涂覆量小于 40mg/cm2。
上述步骤 B中， 正电极浆料在正电极上的涂覆量小于 40mg/cm2。
上述步骤 A、 B 中所述的导电剂为超级导电炭黑、 导电石墨或导电纳米碳管中的 一种或几种的混合物； 所述的粘结剂为聚四氟乙烯、 聚偏氟乙烯或聚合类树脂中的一 种或几种的混合物； 正电极浆料和负电极浆料中的溶剂为 N-甲基吡咯烷酮或二甲基酰 胺或二甲基乙酰胺。
本发明的动力锂离子电池具有对环境友好、 良好的高倍率性能、 良好的散热性能 等特点， 并且制备简单， 没有环境污染， 无泄漏， 存储寿命长， 易于大型化， 使用温 度范围宽， 可作为动力源应用在混合电动汽车、 电动汽车等领域。 附图说明
图 1是本发明的大容量动力锂离子电池的制备方法流程图；
图 2是本发明的大容量动力锂离子电池的正电极、 负电极和涂覆有凝胶态聚合物 电解质的聚乙烯多孔薄膜的堆叠方式图。 具体实施方式
下面结合具体实施例和附图来详细说明本发明。
实施例 1 : 本实施例的大容量动力锂离子电池， 按单体电池额定容量 10Ah设计， 由正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚合物电解质薄膜和负电极依次正 电极、 涂覆有凝胶态聚合物电解质的聚乙烯多孔薄膜和负电极通过堆叠、 封装而成， 其中负电极和正电极通过凝胶态聚合物电解质薄膜和聚乙烯多孔薄膜隔离， 关键在于 所述负电极的活性材料为粒径为 0.165μηι， 比表面积为 9.2m2/g的改性钛酸锂； 所述正 电极的活性材料为三元材料； 所述凝胶态聚合物电解质的薄膜由包含锂盐、 有机溶剂 的电解液与溶于溶剂的聚合物电解质混合后， 涂覆于聚乙烯多孔薄膜上或正负电极两 面上干燥而成。 如图 1所示， 其具体的制备方法如下：
步骤 A: 将 84重量％的改性钛酸锂、 7重量％的导电碳黑和 9重量％的聚偏氟乙 烯为溶质， 以 N-甲基吡咯烷酮为溶剂调成膏状的负电极浆料， 以 ΙΟμηι厚的铜箔作集 流体， 将负电极浆料涂到铜箔的正、 反面上并于 120°C条件下干燥 6小时后制成极片， 然后将极片碾压、 剪切， 制成负电极， 负电极的密度为 4.6g/cm3 ;
步骤 B: 将含 95重量％的三元材料、 1.5重量％的乙块黑、 1.5重量％的导电碳黑、 4重量％的聚偏氟乙烯为溶质， 以 N-甲基吡咯烷酮为溶剂调成膏状的正电极浆料， 以 15μηι厚的铝箔作为集流体， 将正电极浆料涂覆到铝箔的正、 反面上并于 120°C条件下 干燥 8小时，制成极片，然后将极片碾压、剪切制成正电极，正电极的密度为 3.8g/cm3; 步骤 C: 将锂盐 LiPF6溶于有机溶剂中制成电解液， 并与溶于溶剂的聚合物电解 质混合后涂于聚乙烯多孔薄膜或正负电极的两面上， 干燥后得到凝胶态聚合物电解质 的薄膜， 其中聚合物溶液的溶质为偏氟乙烯 -六氟丙烯共聚物， 溶剂为碳酸二乙脂、 碳 酸二丙脂的混合物；
步骤 D: 将上述的正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚 合物电解质薄膜和负电极依次通过堆叠、 包膜、 焊接极耳、 用铝塑复合膜封装等工序 后得到动力锂离子电池半成品， 如图 2所示， 堆叠时负电极 1和正电极 2通过凝胶态 聚合物电解质的薄膜 3隔离；
步骤 E: 将 D步骤中得到的动力锂离子电池半成品进行化成、 分容、 检测， 得到 动力锂离子电池成品。
经过测试， 本实施例的动力锂离子电池的内阻为 2.4m Q， 容量为 21.93Ah， 开路 电压为 2.436V, 电池出现 2.212V 的电压平台， 500 次循环后电池容量的保持率为 96.86%。
实施例 2: 本实施例的大容量动力锂离子电池， 按单体电池额定容量 40Ah设计， 由正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚合物电解质薄膜和负电极依次通 过堆叠、 封装而成， 其中负电极和正电极通过凝胶态聚合物电解质膜和聚乙烯多孔薄 膜隔离， 关键在于所述负电极的活性材料为粒径为 0.165μηι， 比表面积为 9.2m2/g的改 性钛酸锂； 所述正电极的活性材料为三元材料； 所述凝胶态聚合物电解质的薄膜由包 含锂盐、 有机溶剂的电解液与溶于溶剂的聚合物电解质混合后， 涂覆于聚乙烯多孔薄 膜或正负电极两面上干燥而成。 如图 1所示， 其具体的制备方法如下：
步骤 A: 将 84重量％的改性钛酸锂、 7重量％的导电碳黑和 9重量％的聚偏氟乙 烯为溶质， 以 N-甲基吡咯烷酮为溶剂调成膏状的负电极浆料， 以 ΙΟμηι厚的铜箔作集 流体， 将负电极浆料涂到铜箔的正、 反面上并于 120°C条件下干燥 6小时后制成极片， 然后将极片碾压、 剪切， 制成负电极， 负电极的密度为 4.6g/cm3 ;
步骤 B: 将含 93重量％的锰酸锂、 1.5重量％的乙块黑、 2重量％的导电碳黑、 3.5 重量％的聚偏氟乙烯为溶质， 以 N-甲基吡咯烷酮为溶剂调成膏状的正电极浆料， 以 15μηι厚的铝箔作为集流体， 将正电极浆料涂覆到铝箔的正、 反面上并于 120°C条件下 干燥 8小时，制成极片，然后将极片碾压、剪切制成正电极，正电极的密度为 3.8g/cm3 ; 步骤 C: 将锂盐 1^??6溶于有机溶剂中制成电解液， 并与溶于溶剂的聚合物电解 质混合后， 涂于聚乙烯多孔薄膜或正负电极的两个表面上， 干燥后得到凝胶态聚合物 电解质的膜， 其中导电聚合物溶液的溶质为偏氟乙烯 -六氟丙烯共聚物， 溶剂为碳酸二 乙脂、 碳酸二丙脂的混合物；
步骤 D: 将上述的正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚 合物电解质薄膜和负电极依次通过堆叠、 包膜、 焊接极耳、 用铝塑复合膜封装等工序 后得到动力锂离子电池半成品， 如图 2所示， 堆叠时负电极 1和正电极 2通过凝胶态 聚合物电解质的薄膜 3隔离；
步骤 E: 将 D步骤中得到的动力锂离子电池半成品进行化成、 分容、 检测， 得到 动力锂离子电池成品。
经过测试， 本实施例的动力锂离子电池的内阻为 2.35m Q， 容量为 43.74Ah， 开路 电压为 2.537V, 电池出现 2.364V 的电压平台， 500 次循环后电池容量的保持率为 87.68%。
最后所应说明的是： 以上实施例仅用以说明本发明而非限制， 尽管参照较佳实施 例对本发明进行了详细说明， 本领域的普通技术人员应当理解， 可以对本发明进行修 改或者等同替换， 而不脱离本发明的精神和范围， 其均应涵盖在本发明的权利要求范 围当中。

Claims

权利要求书
1、 一种大容量动力锂离子电池， 由正电极、 涂覆凝胶态聚合物电解质膜、 聚乙烯 多孔薄膜、 凝胶态聚合物电解质膜和负电极依次通过堆叠、 封装而成， 其中负电极和 正电极通过凝胶态聚合物电解质膜和聚乙烯多孔薄膜隔离， 凝胶态聚合物电解质膜分 别隔于两电极与聚乙烯多孔薄膜之间； 其特征在于， 所述负电极的活性材料为改性钛 酸锂； 所述正电极的活性材料为三元材料、 锰酸锂和磷酸铁锂中的一种或多种； 所述 凝胶态聚合物电解质的薄膜由包含锂盐、 有机溶剂的电解液与溶于溶剂的聚合物电解 质混合后， 涂覆于聚乙烯多孔薄膜或正负电极两面上干燥而成。
2、 根据权利要求 1所述的大容量动力锂离子电池， 其特征在于， 所述改性钛酸锂 的粒度小于 Ιμηι, 比表面大于 2.0m2/g。
3、 根据权利要求 1所述的大容量动力锂离子电池， 其特征在于， 所述聚合物溶液 的溶质为聚偏二氟乙烯、 偏氟乙烯 -六氟丙烯共聚物、 环氧乙烯-环氧丙烯的均聚物或 共聚物、 聚甲基丙烯酸甲酯、 聚丙烯腈、 聚氨基甲酸脂中的一种或多种混合物， 聚合 物溶液中的溶剂为酮类溶剂、 脂类溶剂和杂环化溶剂中的一种或几种混合溶剂。
4、 根据权利要求 3所述的大容量动力锂离子电池， 其特征在于， 所述酮类溶剂为 丙酮、 甲乙酮中的一种或两种混合溶剂， 所述脂类溶剂为碳酸二乙脂、 碳酸二丙脂、 乙酸乙酯、 乙酸甲酯、 亚硫酸亚乙酯、 亚硫酸亚丙酯中的一种或多种混合溶剂， 所述 杂环化溶剂为 r-丁内酯、 四氢呋喃中的一种或两种混合溶剂。
5、 根据权利要求 1或 2或 3或 4所述的大容量动力锂离子电池， 其特征在于， 所 述锂盐为 LiPF6、 LiC104、 LiBOB、 LiBF4、 LiBF6、 LiAsF6、 LiCF3S03和 LiN ( S02C2F5) 2 中的一种或多种混合物。
6、 一种大容量动力锂离子电池的制备方法， 其特征在于， 包括以下步骤： 步骤 A: 将含 75重量％〜98重量％的改性钛酸锂、 1重量％〜15重量％的导电剂 和 1重量％〜10重量％的粘结剂溶于溶剂中制成负电极浆料，以 9μηι〜13μηι厚的铜箔 为集流体， 将负电极浆料涂在铜箔正、 反面上并干燥， 制成极片， 然后将极片碾压、 剪切， 制成负电极；
步骤 B: 将含 80重量％〜98重量％的正电极活性材料、 1重量％〜10重量％的导 电剂和 1重量％〜10重量％的粘结剂溶于溶剂中制成正电极浆料， 以 15μηι〜20μηι厚 的铝箔为集流体， 将正电极浆料涂覆在铝箔正、 反面上并干燥， 制成极片， 然后将极 片碾压、 剪切， 制成正电极；
步骤 C: 将锂盐 LiPF6溶于有机溶剂中制成电解液， 并与溶于溶剂的聚合物电解 质混合后， 涂于聚乙烯多孔薄膜或正负电极两面上， 干燥后得到凝胶态聚合物电解质 的薄膜；
步骤 D: 将上述的正电极、 凝胶态聚合物电解质薄膜、 聚乙烯多孔膜、 凝胶态聚 合物电解质薄膜和负电极依次通过堆叠、 包膜、 焊接极耳、 封装工序后得到动力锂离 子电池半成品， 其中负电极和正电极通过涂覆有凝胶态聚合物电解质的聚乙烯多孔薄 膜隔离；
步骤 E: 将 D步骤中得到的动力锂离子电池半成品进行化成、 分容、 检测， 得到 动力锂离子电池成品。
7、 根据权利要求 6所述的大容量动力锂离子电池的制备方法， 其特征在于， 在步 骤 A中， 负电极浆料在负电极上的涂覆量小于 40mg/cm2。
8、 根据权利要求 6所述的大容量动力锂离子电池的制备方法， 其特征在于， 在步 骤 B中， 正电极浆料在正电极上的涂覆量小于 40mg/cm2。
9、 根据权利要求 6所述的大容量动力锂离子电池的制备方法， 其特征在于， 在步 骤 A、 B 中所述的导电剂为超级导电炭黑、 导电石墨或导电纳米碳管中的一种或几种 的混合物； 所述的粘结剂为聚四氟乙烯、 聚偏氟乙烯或聚合类树脂中的一种或几种的 混合物； 正电极浆料和负电极浆料中的溶剂为 N-甲基吡咯烷酮或二甲基酰胺或二甲基 乙酰胺。
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