WO2016201941A1 - Batterie au lithium-ion à performance de cycle longue - Google Patents

Batterie au lithium-ion à performance de cycle longue Download PDF

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Publication number
WO2016201941A1
WO2016201941A1 PCT/CN2015/098496 CN2015098496W WO2016201941A1 WO 2016201941 A1 WO2016201941 A1 WO 2016201941A1 CN 2015098496 W CN2015098496 W CN 2015098496W WO 2016201941 A1 WO2016201941 A1 WO 2016201941A1
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cycle performance
lithium
lithium ion
ion battery
battery
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Chinese (zh)
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田东
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—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
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/5825—Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • 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 invention relates to a lithium ion battery with long cycle performance, belonging to the field of lithium ion batteries.
  • lithium-ion batteries have developed rapidly.
  • the negative electrode material of the lithium ion battery includes a carbon material, an intermetallic compound, a tin-based compound, and the like.
  • the commercial lithium ion battery anode material is made of graphite-based carbon material, has low lithium insertion/deintercalation potential, suitable reversible capacity, rich resources, and low price, and is an ideal anode material for lithium ion batteries.
  • the graphite material has a low discharge and discharge platform, and has a high lithium insertion capacity.
  • the lithium intercalation capacity of the lithium intercalation compound LiC6 is 372 mAh/g, and the first charge and discharge efficiency is high. It has been found through research that graphite forms a SEI film during the first cycle by reacting with the electrolyte.
  • This film allows lithium ions to pass freely and prevents solvated lithium ions from entering, thus forming this layer of SEI film on the graphite surface. It is possible to prevent the graphite electrode from being further corroded by the electrolyte and maintaining good cycle performance.
  • the positive electrode material of a lithium ion battery is generally an excessive metal oxide such as LiCoO 2 , LiNiO 2 , LiMnO 2 , and LiNi x Co y Mn (1-xy) O 2 , and the like, and a phosphate of an excessive metal.
  • the LiCoO 2 electrode with layered structure has good performance, and is a cathode material widely used in commercial lithium ion batteries on the market, but it also has disadvantages such as high price and large pollution; LiMn 2 O 4 with spinel structure is cheap and pollution-free. It has been regarded as the material of choice for replacing LiCoO 2 and has been extensively studied. However, due to its low capacity and severe capacity degradation at high temperatures, its application range is still limited.
  • LiNiO 2 Compared with LiCoO 2 with similar structure, LiNiO 2 It has the advantages of high capacity, high power and moderate price, but it also has difficulties in synthesis and poor thermal stability, and its practical process has been slow. However, as the performance of doped multi-element oxides (such as LiNi x Co y Mn (1-xy) O 2 , etc.) is improved and improved, the application of lithium ion batteries is extended to electric vehicles (EV, HEV), Industrial large battery fields such as energy storage power stations and military applications are becoming research hotspots.
  • EV electric vehicles
  • HEV electric vehicles
  • conductive agents are indispensable as a lithium battery.
  • the purpose of the component is to form an effective conductive network in the active material.
  • the composite of the active material and the conductive agent hereinafter referred to as "composite electrode"
  • the amount of the conductive agent must be added to and exceeds a certain amount. When the amount exceeds this amount, the conductive agent particles can be filled with full activity.
  • the gap between the particles of the material, and the effective contact between the conductive agents, the conductivity of the composite electrode is fundamentally improved.
  • the former lithium-ion battery conductive agent is mainly Super-P and KS series. Both of these products are imported from abroad.
  • the former is a nano-scale carbon black product, which has a small particle size and a large specific surface area. It also has good electrical conductivity, but because of its small particle size and large specific surface area, it is difficult to disperse, and then it is micron-sized conductive graphite, which is easy to disperse, but its conductivity is worse than Super-P. Therefore, in the actual use process, both are added at the same time, and the complement is insufficient.
  • the graphite thin structure is unique, with good electrical conductivity, thermal conductivity, stability and a large specific surface area. As a conductive agent for lithium ion batteries, it can greatly improve the energy density of the battery, and at the same time increase the rate of charge and discharge of the material to meet the requirements of the power battery.
  • the improvement of the performance of lithium-ion batteries is mainly due to the improvement of the performance of each material and the cooperation of various components. Therefore, by selecting a suitable material system, lithium-ion batteries with different performance characteristics can be prepared for different needs.
  • the invention provides a lithium ion battery with long cycle performance
  • the material system is lithium iron phosphate with stable cycle performance as positive electrode, lithium titanate with excellent cycle performance as negative electrode, and high conductivity.
  • Graphene is a conductive additive.
  • the lithium iron phosphate positive electrode material has a specific capacity of 145 to 160 mAh/g, a first efficiency of 92.5 to 94.5%, a double-sided surface density of 15 to 30 mg/cm 2 , and a positive electrode compaction density of 1.9 to 2.3 g/cm 3 .
  • the lithium titanate negative electrode material has a gram specific capacity of 150 to 165 mAh/g, a first efficiency of 93 to 95.5%, a negative electrode compaction density of 1.3 to 1.6 g/cm 3 , and a negative electrode sheet surface density corresponding to a positive electrode active material excess ratio. It is 3% to 10%.
  • the positive electrode tab is prepared by first preparing 2 to 5 wt% of a binder-polyvinylidene fluoride (PVDF) and 80 to 120 wt% of a solvent-methylpyrrolidone (NMP), and then adding 1 to 3 wt%.
  • PVDF binder-polyvinylidene fluoride
  • NMP solvent-methylpyrrolidone
  • the graphene conductive agent is well dispersed, and finally 80 to 95.5 wt% of active material lithium iron phosphate is added, mixed into a slurry, the viscosity is adjusted, and a pole piece is coated on an aluminum foil of 0.010 to 0.016 mm, and a positive electrode piece is obtained by rolling and slitting.
  • the double-sided density of the positive electrode is 20 to 30 mg/cm 2
  • the compact density is 2.0 to 2.3 g/cm 3 .
  • the negative electrode tab is prepared by disposing 1 to 2 wt% thickener sodium carboxymethylcellulose (CMC) and deionized water into a glue solution, and dispersing 0.5 to 2 wt% of graphene conductive agent, and then dispersing. Add 93.8 to 98% by weight of active material lithium titanate, and finally add 2 to 4.4% by weight of binder-styrene-butadiene rubber (SBR), mix into slurry, adjust viscosity, and coat the electrode on 0.08-0.010mm copper foil.
  • the sheet has a negative compaction density of 1.4 to 1.6 g/cm 3 .
  • the separator is separated between the positive electrode and the negative electrode, and the separator is 0.012 to 0.025 mm.
  • a solid electrolyte membrane (SEI film) is formed on the surface during the first charge and discharge process.
  • the solid electrolyte membrane is formed by reacting an electrolyte, a negative electrode material and lithium ions, and irreversibly consuming lithium ions, which is a major factor in forming irreversible capacity.
  • the electrolyte is easily co-incorporated with it.
  • the electrolyte is reduced, and the generated gas product causes the graphite sheet to peel off.
  • the graphite sheet peeling off will form a new interface, resulting in further SEI formation, thereby causing a decrease in battery cycle performance.
  • lithium titanate Compared with graphite carbon materials, lithium titanate has many advantages. Among them, the deintercalation of lithium ions in lithium titanate is reversible, and the crystal form of lithium ions does not occur during the process of inserting or extracting lithium titanate. Change, volume change is less than 1%, so it is called "zero strain material", which can avoid the structure damage caused by the back and forth expansion of the electrode material in the charge and discharge cycle, thereby improving the cycle performance and service life of the electrode, reducing the cycle The number of times increases to a large attenuation of the specific capacity, and has better cycle performance than the carbon negative electrode; according to the above, a high energy density lithium ion battery designed by the present invention, after the battery is assembled, is placed and formed. , aging, and can be divided.
  • the beneficial effects and progress of the present invention are as follows:
  • a lithium ion battery having long cycle performance described in this embodiment uses lithium iron phosphate as a positive electrode active material, a lithium iron phosphate having a specific capacity of 149 mAh/g, a first efficiency of 93.2%, and a lithium titanate as a negative electrode material.
  • the gram ratio is 160 mAh/g, and the first efficiency is 93.5%.
  • the positive electrode tab is prepared by first disposing the binder PVDF (3 wt%) and the solvent NMP (80 wt%) into a glue solution, dispersing 2 wt% of the graphene, and finally adding the active material lithium iron phosphate 95 wt%, mixing. The slurry was slurried, and the viscosity was adjusted. Then, a pole piece was coated on an aluminum foil of 0.016 mm, and the double-sided surface density was 30 mg/cm 2 , and the positive electrode piece was obtained by rolling and cutting, and the compacted density was 2.0 g/cm 3 ;
  • the negative pole piece is prepared by disposing CMC 1.2wt% and deionized water into a glue solution, adding graphene 0.5% by weight to disperse, then adding active material lithium titanate 96.3wt%, and finally adding binder 2.0wt%. The mixture was mixed into a slurry to adjust the viscosity.
  • the pole piece was coated on a copper foil of 0.010 mm, and the density of the negative electrode surface was calculated to correspond to the excess of the positive electrode active material capacity ratio of 5%, and the compactness of the negative electrode piece was 1.5 g/ Cm 3 ;
  • the battery prepared by the present invention was subjected to a 3800-week cycle test, and the capacity retention rate was 81.91%, showing excellent cycle performance.
  • a lithium ion battery having long cycle performance described in this embodiment uses lithium iron phosphate as a positive electrode active material, a lithium iron phosphate having a specific capacity of 155 mAh/g, a first efficiency of 94.5%, and a lithium titanate as a negative electrode material.
  • the gram ratio is 162 mAh/g, and the first efficiency is 95.2%.
  • the positive electrode tab is prepared by first disposing the binder PVDF (2.5 wt%) and the solvent NMP (80 wt%) into a glue solution, dispersing 1.5 wt% of the graphene, and finally adding the active material lithium iron phosphate 96 wt%. , mixing into a slurry, adjusting the viscosity, and then coating a pole piece on a 0.016 mm aluminum foil, a double-sided surface density of 25 mg / cm 2 , and rolling and slitting to obtain a positive electrode piece, compaction density of 2.2 g / cm 3 ;
  • the negative pole piece was prepared by disposing CMC 1.5wt% and deionized water into a glue solution, adding graphene 0.5% by weight to disperse, then adding active material lithium titanate 96.7wt%, and finally adding binder 1.8wt%. The mixture was mixed into a slurry to adjust the viscosity.
  • the pole piece was coated on a copper foil of 0.010 mm, and the density of the negative electrode surface was calculated to correspond to the excess of the positive electrode active material capacity ratio of 6%, and the compact density of the negative electrode piece was 1.55 g/ Cm 3 ;
  • the battery prepared by the present invention was subjected to a 1000-week cycle test, and the capacity retention rate was 97.70%, showing excellent cycle performance.
  • a lithium ion battery having long cycle performance described in this embodiment uses lithium iron phosphate as a positive electrode active material, a lithium iron phosphate having a specific capacity of 160 mAh/g, a first efficiency of 94.3%, and a lithium titanate as a negative electrode material.
  • the gram ratio is 165mAh/g, and the first efficiency is 95.5%.
  • the positive electrode tab is prepared by first disposing the binder PVDF (2.0 wt%) and the solvent NMP (80 wt%) into a glue solution, dispersing 1.0 wt% of the graphene, and finally adding the active material lithium iron phosphate 97 wt%. , mixing into a slurry, adjusting the viscosity, and then coating a pole piece on a 0.016 mm aluminum foil, the double-sided surface density of 20 mg / cm 2 , and rolling and slitting to obtain a positive electrode piece, compaction density of 2.3 g / cm 3 ;
  • the negative electrode pole piece is prepared by disposing CMC 1.5wt% and deionized water into a glue solution, adding graphene 0.5% by weight to disperse, then adding active material lithium titanate 97wt%, and finally adding binder 1.5wt%, mixing. The slurry was formed into a slurry, and the viscosity was adjusted. The pole piece was coated on a copper foil of 0.010 mm, and the density of the negative electrode surface was calculated to correspond to the excess ratio of the positive electrode active material to 6%, and the compact density of the negative electrode piece was 1.60 g/cm.
  • the battery prepared by the present invention was subjected to a 1000-week cycle test, and the capacity retention rate was 98.20%, showing excellent cycle performance.
  • the present invention illustrates the detailed process parameters and process flow of the present invention by the above embodiments, but the present invention is not limited to the above detailed process parameters and process flow, that is, does not mean that the present invention must rely on the above detailed process parameters and The process can only be implemented. It should be apparent to those skilled in the art that any modifications of the present invention, equivalent substitution of the various materials of the products of the present invention, addition of auxiliary components, selection of specific means, and the like, are all within the scope of the present invention.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)

Abstract

La présente invention porte sur une batterie au lithium-ion à performance de cycle longue. La présente invention concerne le domaine des batteries. Un système de matière de batterie au lithium-ion a du phosphate de fer et lithium avec une performance de cycle stable en tant que cathode, du titanate de lithium avec une performance de cycle excellente en tant qu'anode et du graphène avec une performances de conductivité élevée en tant qu'un additif conducteur. Un système de matière de cathode et d'anode à performance de cycle excellente est utilisé, la densité surfacique et la densité de compactage d'une pièce de pôle de cathode et d'une pièce de pôle d'anode sont optimisées et commandées, et la performance de cycle de la batterie est considérablement améliorée. Le graphène avec la performance de conductivité élevée est utilisé en tant qu'additif d'agent conducteur, de telle sorte que le défaut de réduction d'une proportion de matière active d'une cathode à une anode en raison du fait qu'un grand nombre d'agents conducteurs classiques ont besoin d'être ajoutés lorsqu'ils sont utilisés est évité, et la densité d'énergie en volume de la batterie est en outre améliorée. Un électrolyte contenant un solvant PC est utilisé, et le point de congélation élevé et la conductivité élevée du solvant PC sont utilisés, de telle sorte que le problème de dissipation de chaleur de batterie sous les conditions de charge-décharge de courant importantes est efficacement tamponné, et la stabilité de cycle de la batterie est en outre garantie. Un procédé de préparation pour la batterie au lithium-ion est simple, et une batterie au lithium fabriquée est d'excellentes performances.
PCT/CN2015/098496 2015-06-13 2015-12-23 Batterie au lithium-ion à performance de cycle longue Ceased WO2016201941A1 (fr)

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CN201510331372.7 2015-06-13
CN201510331372.7A CN104993135A (zh) 2015-06-13 2015-06-13 一种具有长循环性能的锂离子电池

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CN111244371A (zh) * 2020-01-19 2020-06-05 青岛国轩电池有限公司 一种磷酸铁锂电池电芯、高能量密度磷酸铁锂电池及电池的制备方法
CN114430039A (zh) * 2020-10-28 2022-05-03 比亚迪股份有限公司 一种锂离子电池及动力车辆
CN116470010A (zh) * 2023-05-11 2023-07-21 蜂巢能源科技股份有限公司 一种厚电极及其制备方法与应用
CN117105231A (zh) * 2023-08-25 2023-11-24 安徽得壹能源科技有限公司 一种锂电池用的负极材料及其应用
CN117438638A (zh) * 2023-12-18 2024-01-23 汉朔科技股份有限公司 钛酸锂扣式二次电池及电子价签
CN118676360A (zh) * 2023-03-15 2024-09-20 宁德时代新能源科技股份有限公司 一种锂离子电池

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CN104993135A (zh) * 2015-06-13 2015-10-21 田东 一种具有长循环性能的锂离子电池
CN105261747A (zh) * 2015-10-22 2016-01-20 芜湖凯尔电气科技有限公司 锂离子动力电池材料
JP6875522B2 (ja) * 2017-06-15 2021-05-26 株式会社日立製作所 半固体電解質、電極、半固体電解質層付き電極、および二次電池
CN110265648A (zh) * 2019-06-27 2019-09-20 郑州比克电池有限公司 一种软包聚合物锂电池的负极浆料及制备方法
CN115498247B (zh) * 2022-10-27 2023-08-15 欣旺达电动汽车电池有限公司 二次电池及用电设备
CN115472898B (zh) * 2022-10-27 2023-09-15 欣旺达动力科技股份有限公司 一种二次电池及用电设备
CN115954466B (zh) * 2023-03-14 2023-06-06 江苏众钠能源科技有限公司 一种混合活性材料及锂钠混用离子电池

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Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111244371A (zh) * 2020-01-19 2020-06-05 青岛国轩电池有限公司 一种磷酸铁锂电池电芯、高能量密度磷酸铁锂电池及电池的制备方法
CN114430039A (zh) * 2020-10-28 2022-05-03 比亚迪股份有限公司 一种锂离子电池及动力车辆
CN114430039B (zh) * 2020-10-28 2023-08-08 比亚迪股份有限公司 一种锂离子电池及动力车辆
CN118676360A (zh) * 2023-03-15 2024-09-20 宁德时代新能源科技股份有限公司 一种锂离子电池
CN116470010A (zh) * 2023-05-11 2023-07-21 蜂巢能源科技股份有限公司 一种厚电极及其制备方法与应用
CN117105231A (zh) * 2023-08-25 2023-11-24 安徽得壹能源科技有限公司 一种锂电池用的负极材料及其应用
CN117438638A (zh) * 2023-12-18 2024-01-23 汉朔科技股份有限公司 钛酸锂扣式二次电池及电子价签

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