WO2014141547A1 - Dispositif et procédé de production d'une batterie secondaire au lithium-ion - Google Patents

Dispositif et procédé de production d'une batterie secondaire au lithium-ion Download PDF

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Publication number
WO2014141547A1
WO2014141547A1 PCT/JP2013/082324 JP2013082324W WO2014141547A1 WO 2014141547 A1 WO2014141547 A1 WO 2014141547A1 JP 2013082324 W JP2013082324 W JP 2013082324W WO 2014141547 A1 WO2014141547 A1 WO 2014141547A1
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Prior art keywords
ion secondary
secondary battery
lithium ion
current collector
electrode material
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PCT/JP2013/082324
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English (en)
Japanese (ja)
Inventor
千恵美 窪田
昌作 石原
菊池　廣
高原　洋一
正志 西亀
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株式会社日立製作所
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Priority to KR1020157013558A priority Critical patent/KR101697249B1/ko
Priority to CN201380066009.6A priority patent/CN104871360A/zh
Publication of WO2014141547A1 publication Critical patent/WO2014141547A1/fr

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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
    • H01M4/139—Processes of manufacture
    • 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
    • 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 present invention relates to a technique for manufacturing a lithium ion secondary battery, and more particularly to a technique effective when applied to the manufacture of an electrode plate of a lithium ion secondary battery.
  • Patent Document 1 Japanese Patent No. 3539911
  • Patent Document 1 states that “a method for producing a coating sheet coated with at least an active material, a binder and a solvent, wherein the coating film is at a temperature below the boiling point of the solvent contained in the coating. Heating the coating sheet at a temperature lower than the temperature below the boiling point of the solvent so as to maintain a uniform state of the first step of heating the sheet and the distribution of the binder in the coating film. A second step of heating and a third step of heating the coating sheet at a temperature equal to or higher than the temperature lower than the boiling point of the solvent. Through the third step, the coating sheet is the second step. It is described as “a method for producing a coating film sheet in which a state in which the distribution of the binder in the coating film is made uniform by the process is maintained” is described.
  • lithium ion secondary batteries have the advantages of high energy density, long cycle life, low self-discharge characteristics, and high operating voltage, so that they can be used in digital cameras, notebook personal computers, mobile phones, etc. Widely used in portable electronic devices.
  • lithium ion secondary batteries capable of realizing high capacity, high output, and high energy density as electric vehicle batteries and power storage batteries.
  • the development of an electric vehicle that uses a motor as a power source and a hybrid vehicle that uses both an engine (internal combustion engine) and a motor as power sources are being developed. Yes.
  • Lithium ion secondary batteries are also attracting attention as power sources for such electric vehicles and hybrid vehicles.
  • lithium ion secondary batteries are also becoming increasingly important for applications such as solar power generation and power storage for effective use of nighttime power.
  • the positive electrode plate and the negative electrode plate are wound or laminated via a separator that prevents contact between both electrode plates. And after accommodating this winding body or laminated body in a battery exterior container, electrolyte solution is inject
  • an electrode slurry is prepared by kneading an active material capable of releasing and occluding lithium ions by charge / discharge and a conductive additive powder with a binder, a solvent, etc., and this slurry is applied using a coating means such as a die coater. Apply thinly and evenly on the metal foil that is the current collector foil. Thereafter, the solvent contained in the slurry on the metal foil (hereinafter, the coating slurry before drying is referred to as a coating film) is dried to form an electrode film and manufacture an electrode plate.
  • an electrode is manufactured through a series of steps including production of a slurry-like electrode material, application of the electrode material to a current collector foil and drying, or a combination of these steps. It is necessary to manufacture a board. However, since the production of such an electrode plate requires a considerable economic burden, the improvement is desired, and the maintenance and management of the quality of the electrode plate is also desired.
  • Patent Document 1 proposes a method of dividing the drying process into a plurality of processes having different application temperatures.
  • this method includes a drying step at a low temperature, the drying rate of the electrode cannot be increased, and the productivity is lowered. Furthermore, it is not easy to make the binder concentration distribution uniform by drying by evaporation of the solvent from the surface of the coating film.
  • the present invention maintains / improves the quality of an electrode plate by manufacturing an electrode plate in which the binder is almost uniformly distributed in the electrode film at a low cost while improving productivity. It is an object of the present invention to provide a manufacturing method and a manufacturing apparatus capable of performing the above, and a lithium ion secondary battery using the electrode plate.
  • the present application includes a plurality of means for solving the above problems. At least a coating portion for applying a slurry-like electrode material containing a positive or negative active material, a binder, a solidifying agent, and a first solvent to the surface of the current collector foil, and the surface of the current collector foil.
  • a solidification chamber for solidifying the slurry-like electrode material, and a liquid component contained in the electrode material solidified in the solidification chamber are removed, and the electrode material is removed.
  • the solidification chamber has a contact width of the solidified liquid along a direction orthogonal to a conveying direction of the current collector foil, which is equal to or greater than a width of the slurry-like electrode material applied to the surface of the current collector foil. It is a manufacturing apparatus of a lithium ion secondary battery provided with the solidification liquid contact mechanism prescribed
  • High quality lithium ion secondary batteries can be manufactured at low cost while improving productivity.
  • FIG. 1 is a schematic cross-sectional view showing a solidification chamber of an electrode plate manufacturing apparatus in Example 1.
  • FIG. FIG. 3 is a plan view of a main part of a current collector foil showing a spray pattern of a solidified liquid in Example 1.
  • 3 is a graph showing a flow rate distribution of a solidified liquid in Example 1.
  • A is a top view of the spray mask provided in the solidification chamber of the electrode plate manufacturing apparatus in Example 2
  • (b) is a sectional view of the spray mask.
  • (A) is a top view of the spray mask provided in the solidification chamber of the electrode plate manufacturing apparatus in Example 3,
  • (b) is a sectional view of the spray mask.
  • It is a whole block diagram which shows the conventional single-side coating type electrode plate manufacturing apparatus.
  • It is a whole block diagram which shows the conventional sequential double coated electrode plate manufacturing apparatus.
  • the electrode material used to form the electrode film constituting the positive electrode or negative electrode of a lithium ion secondary battery is composed of an active material capable of releasing and occluding lithium ions by charging and discharging, and a conductive auxiliary powder. It is a high-viscosity slurry liquid that is kneaded and dispersed with a binder, a solvent, and the like.
  • the slurry-like electrode described above is applied to the surface of the current collector foil 55 supplied from the current collector foil roll 53 using a coating means 52 such as a die coater installed in the coating unit 51. Apply the material thinly and evenly.
  • the current collector foil 55 coated with the slurry-like electrode material (coating film) is dried by a roller transport system 54 for transporting the current collector foil 55 at a constant speed while being in contact with the back surface of the current collector foil 55.
  • the solvent component contained in the coating film is heated and evaporated to dry the electrode material, and the electrode film is formed on the surface of the current collector foil 55.
  • the current collector foil 55 is wound around the electrode roll 57 and conveyed to the next step.
  • a normal electrode plate manufacturing process such a process is separately performed on the front surface and the back surface of the current collector foil 55 to manufacture an electrode plate having electrode films formed on both surfaces of the current collector foil 55.
  • the conveying speed of the current collector foil in the drying process of the manufacturing apparatus is about 1 to 100 m / min, and the observation speed is about 1 to 100 minutes.
  • the transport speed in the drying chamber is slow, so that drying at a relatively low temperature with a reduced evaporation rate of the solvent becomes possible. Therefore, it is possible to cope with even a small drying room, and the quality of the electrode plate to be manufactured is easily stabilized.
  • a method of abruptly drying the solvent at a high temperature may be considered in order to increase the productivity of the electrode plate and reduce the equipment cost and running cost by reducing the size of the drying chamber.
  • the surface of the coating film is dried first, and the composition of the electrode material varies between the inside and the surface of the coating film, or cracks occur on the surface of the coating film. .
  • the electrode plate manufacturing process and equipment are generally constructed by adjusting the two in the middle of both extremes and empirically obtaining the optimum value. Therefore, it has been required to realize an electrode plate manufacturing method that can be applied and dried at high speed and can stabilize the quality of the electrode plate.
  • FIG. 10 shows a conventional sequential double-side coated electrode plate manufacturing apparatus.
  • the coating means 52A such as a die coater installed in the coating section 51A
  • the above-described slurry-like electrode material is thinly and uniformly applied to the surface of the current collector foil 55 supplied from the current collector foil roll 53.
  • a hot-air drying furnace showing a current collecting foil 55 coated with a slurry-like electrode material as a drying chamber 56A by a roller conveying system 54A that conveys the current collecting foil 55 at a constant speed while being in contact with the back surface of the current collecting foil 55.
  • a roller conveying system 54A that conveys the current collecting foil 55 at a constant speed while being in contact with the back surface of the current collecting foil 55.
  • the solvent component contained in the coating film is heated and evaporated to dry and solidify the electrode material, and the electrode film is formed on the surface of the current collector foil 55.
  • a series of steps so far are the same as the example of FIG.
  • the current collector foil 55 on which the electrode film is formed is conveyed to the next coating unit 51 ⁇ / b> B without being wound around the electrode roll 57,
  • the slurry-like electrode material is thinly and uniformly applied to the back surface of the current collector foil 55 using the coating means 52B.
  • the current collector foil 55 is sent to the next hot air drying furnace shown as the drying chamber 56B by the roller transport system 54B that transports the current collector foil 55 at a constant speed while being in contact with the surface of the current collector foil 55.
  • the solvent component contained in the coating film applied to the back surface of the current collector foil 55 is heated and evaporated to dry and solidify the electrode material, and an electrode film is formed on the back surface of the current collector foil 55. Thereby, an electrode plate having electrode films formed on both surfaces of the current collector foil 55 is manufactured. Thereafter, the current collector foil 55 is wound around the electrode roll 57 and conveyed to the next step.
  • FIG. 11 shows a double-sided coating batch drying type manufacturing apparatus proposed for solving the above-mentioned problems.
  • a first coating means 52A for applying a slurry-like electrode material to the surface of the current collector foil 55 and a second electrode for applying a slurry-like electrode material to the back surface of the current collector foil 55 are applied to the coating unit 51 of this manufacturing apparatus.
  • Coating means 52B In this manufacturing apparatus, the electrode material is thinly and uniformly applied to the front surface and the back surface of the current collector foil 55 supplied from the current collector foil roll 53 using the two coating means 52A and 52B.
  • the solvent component in the coating film is heated and evaporated in a hot-air drying furnace shown as the drying chamber 56 to dry and solidify the electrode material, thereby forming an electrode film.
  • a hot-air drying furnace shown as the drying chamber 56 to dry and solidify the electrode material, thereby forming an electrode film.
  • the slurry-like electrode material coated on the current collector foil is directly introduced into the drying chamber and dried.
  • the manufacturing method according to the present embodiment includes a solidification step of solidifying the slurry-like electrode material before conveying it to the drying step.
  • a solidification step of solidifying the slurry-like electrode material By providing this solidification step, various problems caused by drying the slurry-like electrode material as it is in the drying step can be solved simultaneously.
  • FIG. 1 is an overall configuration diagram showing a single-side coating type electrode plate manufacturing apparatus according to the present embodiment.
  • an electrode material for forming the positive electrode or the negative electrode of the lithium ion secondary battery is prepared, and this electrode material is used in the electrode plate manufacturing apparatus shown in FIG.
  • the coating means 12 such as a die coater installed in the coating unit 11 is filled.
  • the electrode material in the present embodiment includes at least a positive electrode or negative electrode active material powder capable of releasing and occluding lithium ions by charging and discharging, and optionally a conductive agent powder, and further between the powder components or powder after drying.
  • the above-described high-viscosity slurry-like electrode material is thinly and uniformly applied to the surface of the current collector foil 15 supplied from the current collector foil roll 13 using the coating means 12 installed in the coating unit 11. To do. This process is referred to as a coating process.
  • the current collector foil 15 is introduced into the solidification chamber 18 by the roller transport system 14 that transports the current collector foil 15 at a constant speed while being in contact with the back surface of the current collector foil 15 coated with the electrode material.
  • the coating film is solidified by bringing the solidified liquid that is the second solvent in the form of the above into contact with the surface of the coating film.
  • the solidified liquid that is the second solvent of the present embodiment has the property that the solidifying agent contained in the electrode material is insoluble, and the first solvent It is necessary to have the property of mutual dissolution.
  • the second solvent When the second solvent comes into contact with the surface of the coating film, the second solvent penetrates into the coating film while being mutually dissolved with the first solvent in the coating film.
  • the solubility of the solidifying agent decreases, so that the solidifying agent precipitates in the coating film, and the precipitated solidifying agent and active material particles contained in the coating film, etc. And the whole coating film is solidified.
  • This process is referred to as a solidification process. Normally, this solidification process is much shorter than the time required for drying, etc., so various components in the coating film are instantaneously fixed, and their concentration distribution and composition fluctuations may occur. Absent.
  • a solidification step is performed in which the solidified liquid as the second solvent is brought into contact with the surface of the coating film, and the coating film is solidified.
  • the components in the electrode material may flow out to the non-coated portion of the surface 15.
  • a current collecting tab for charging and outputting electricity from the electrode plate is attached to the electrode plate of a normal lithium ion secondary battery, so an electrode film is not formed on the entire surface of the current collecting foil, and both ends in the width direction. The part is exposed. Therefore, also in the present embodiment, in the coating process, the electrode material is not applied to the entire surface of the current collector foil, and both ends in the width direction are left uncoated. If the electrode material adheres to this non-coated part, more specifically, the current collector tab mounting position, the current collector tab attachment failure and the resistance between the current collector foil and current collector tab will increase. There is a risk that the characteristics of
  • a spray nozzle (not shown in FIG. 1) for spraying the solidified liquid onto the surface of the coating film is provided in the solidification chamber 18. It is provided inside.
  • the position and amount of spraying can be controlled by the form of the spray nozzle, so the solidified liquid is contacted to the coating film without exceeding the mounting position of the current collecting tab. Can be made.
  • the current collector foil 15 holding the solidified coating film is carried into the drying chamber 16 by the roller conveyance system 14.
  • the electrode component of the lithium ion secondary battery is formed by heating and evaporating the solvent component in the coating film to dry the electrode material and forming an electrode film on the surface of the current collector foil 15 by a known method such as hot air drying. Manufacture a board. This process is referred to as a drying process.
  • the current collector foil 15 is wound around the electrode roll 17 and conveyed to the next step.
  • the current collection foil 15 is conveyed using the contact-type roller conveyance system 14 which contacts the current collection foil 15. be able to. That is, in this embodiment, since it is not necessary to use a complicated and expensive non-contact type conveyance system, an inexpensive drying chamber 16 using a contact type roller conveyance system 14 is employed. This advantage is particularly high when the electrode materials applied on both surfaces of the current collector foil 15 are dried together, but of course does not exclude the use of a non-contact type transport system.
  • the liquid coating film is not dried, but the coating film solidified in the solidification chamber 18 may be dried. Rapid drying is possible in a short time while preventing fluctuations and fluctuations in the thickness of the coating film.
  • the drying equipment can be downsized without reducing the quality of the electrode film.
  • the drying chamber 16 of the present embodiment shown in FIG. 1 has a structure such as a hot-air drying furnace similar to the conventional drying chamber shown in FIGS. 9 to 11, but has a structure in the drying chamber as compared with the conventional drying chamber.
  • the conveyance path can be shortened.
  • a spinel-structured lithium-containing composite oxide containing manganese is excellent in thermal stability, and thus a highly safe battery can be manufactured.
  • the positive electrode active material only the above-mentioned spinel-structured lithium-containing composite oxide containing manganese may be used, but it may be used in combination with other positive electrode active materials.
  • a positive electrode active material for example, olivine type represented by Li 1 + x MO 2 ( ⁇ 0.1 ⁇ x ⁇ 0.1, M: Co, Ni, Mn, Al, Mg, Zr, Ti, etc.) Compounds and the like.
  • the lithium-containing transition metal oxide having a layered structure LiCoO 2 and LiNi 1-x Co xy Al y O 2 (0.1 ⁇ x ⁇ 0.3, 0.01 ⁇ y ⁇ 0. 2) and other oxides containing at least Co, Ni and Mn (LiMn 1/3 Ni 1/3 Co 1/3 O 2 , LiMn 5/12 Ni 5/12 Co 1/6 O 2 , LiNi 3 / 5 Mn 1/5 Co 1/5 O 2 etc.).
  • Examples of the active material for the negative electrode used in the present embodiment include graphite materials such as natural graphite (flaky graphite), artificial graphite, and expanded graphite, graphitizable carbonaceous materials such as coke obtained by firing pitch, Examples thereof include carbon materials such as non-graphitizable carbonaceous materials such as amorphous carbon obtained by low-temperature firing of furyl alcohol resin (PFA), polyparaphenylene (PPP), and phenol resin.
  • PFA furyl alcohol resin
  • PPP polyparaphenylene
  • lithium or a lithium-containing compound can also be used as the negative electrode active material.
  • Examples of the lithium-containing compound include lithium alloys such as Li—Al, and alloys containing elements that can be alloyed with lithium, such as Si and Sn.
  • an oxide-based material such as Sn oxide or Si oxide can be used.
  • the conduction aid used in the present embodiment is usually used as an electron conduction aid to be contained in the positive electrode film, for example, carbon black, acetylene black, ketjen black, graphite, carbon fiber, carbon nanotube, etc.
  • the carbon material is preferable.
  • acetylene black or ketjen black is particularly preferable from the viewpoint of the amount of addition and conductivity, and the productivity of the coating electrode material slurry.
  • Such a conductive additive may be contained in the negative electrode film, or may be preferably contained in the negative electrode film.
  • the binder used in this embodiment preferably contains a binder for binding the active material and the conductive additive.
  • a binder for example, a polyvinylidene fluoride polymer (a polymer of a fluorine-containing monomer group containing 80% by mass or more of vinylidene fluoride as a main component monomer), a rubber polymer, or the like is preferably used. Two or more of these polymers may be used in combination.
  • the binder used in the present embodiment is preferably provided in the form of a solution dissolved in a solvent.
  • Examples of the fluorine-containing monomer group for synthesizing the polyvinylidene fluoride-based polymer include vinylidene fluoride, a mixture of vinylidene fluoride and other monomers, and a monomer mixture containing 80% by mass or more of vinylidene fluoride. It is done.
  • Examples of the other monomer include vinyl fluoride, trifluoroethylene, trifluorochloroethylene, tetrafluoroethylene, hexafluoropropylene, and fluoroalkyl vinyl ether.
  • Examples of the rubber polymer include styrene butadiene rubber (SBR), ethylene propylene diene rubber, and fluorine rubber.
  • the binder used in the present embodiment may be added separately from the component having the performance as a solidifying agent, or the binder itself may have a function as a solidifying agent.
  • the binder is added separately from the component having the performance as a solidifying agent, the above-mentioned polymer material having the property of binding the active material and the conductive assistant is preferably used as the binder, but it is not necessarily in the form of a solution dissolved in a solvent. However, it may be in the form of an emulsion in which a polymer material is dispersed in a solvent.
  • the content of the binder in the electrode material is 0.1% by mass or more, more preferably 0.3% by mass or more and 10% by mass or less, more preferably 5%, based on the dried electrode film. It is desirable that it is less than mass%. If the binder content is too low, not only will the coating film solidify in the solidification process, but the mechanical strength of the electrode film obtained after drying will be insufficient, causing the electrode film to peel from the current collector foil. There is. On the other hand, if the binder content is too large, the amount of the active material in the electrode film decreases, and the battery capacity may be lowered.
  • the current collector foil used in the present embodiment is not limited to a sheet-like foil, and a pure metal or alloy conductive material such as aluminum, copper, stainless steel, titanium, etc. is used as its base, and a net, punch Metal foil, foam metal, foil processed into a plate shape, or the like can also be used.
  • the thickness of the substrate is, for example, 5 ⁇ m to 30 ⁇ m, more preferably 8 ⁇ m to 16 ⁇ m.
  • Examples of the method for applying the slurry-like electrode material of the present embodiment to the surface of the current collector foil include various application methods such as an extrusion coater, a reverse roller, a doctor blade, and an applicator.
  • first solvent and second solvent used in the present embodiment are appropriately selected and used.
  • a solvent should be selected on the basis of the solubility of the solidifying agent of the present embodiment, or the components of the binder that also serves as the solidifying agent, and the mutual solubility of the solvent.
  • Examples of the first solvent include aprotic polar solvents represented by N-methylpyrrolidone, dimethyl sulfoxide, propylene carbonate, dimethylformamide, ⁇ -butyrolactone, and the like, or a mixed solution containing two or more of these.
  • Examples of the second solvent include protic solvents represented by water, ethanol, isopropyl alcohol, acetic acid, and the like, or a mixed solution containing two or more of these, but are limited to the examples given here. Is not to be done. In some cases, it is possible to select aliphatic saturated hydrocarbons, aliphatic amines, esters, ethers, various halogen-based solvents, and the like as the second solvent. Further, in some cases, it is possible to select to exchange the first solvent and the second solvent. The selection of the solvent depends on the selection of the solidifying component used for the electrode film and the combination of the two types of solvents.
  • the solidification chamber of the present embodiment includes a solidification liquid supply device for bringing the solidification liquid made of the second solvent into contact with the coating film on the current collector foil containing the first solvent. Further, the solidification chamber has a solidification liquid in which the contact area of the solidification liquid is not less than the end of the application width in the direction perpendicular to the conveyance direction of the current collector foil and within the current collection tab attachment position of the non-application part of the current collector foil A contact mechanism is provided. Specifically, it is a method in which the solidified liquid is brought into contact with the coating film surface using a spray nozzle provided in the solidified liquid supply device, and only in the above-described spray region by adjusting the type and arrangement of the spray nozzle. Contact the solidified solution.
  • the solidification step includes a method of controlling the contact area of the solidified liquid by attaching a spray mask between the spray nozzle and the coating film.
  • the method of controlling the contact region of the solidified liquid ejected from the spray nozzle with the spray mask can control the spray region more easily than the method of controlling the spray region by the type and arrangement of the spray nozzle. A more specific configuration of the solidification device will be clarified in Examples described later.
  • the method for drying the solidified coating film is not limited to general hot air drying. That is, a heating method of irradiating electromagnetic waves such as infrared rays, far infrared rays or visible light may be used, or a dielectric heating method using a high frequency electric field may be used. Furthermore, an induction heating method using a change in magnetic flux can be used, or a contact heating method using a heating roll or a hot plate incorporating a heater can be used.
  • the lithium ion secondary battery that can be provided by the present embodiment can be manufactured in the same manner as a conventional lithium ion secondary battery except that it includes positive and negative electrode plates manufactured by the above-described method. . That is, there is no particular limitation on the structure and size of the battery outer container that houses these electrode plates, or the structure of the wound body or laminate including the positive and negative electrode plates as main components.
  • the manufacture of the present embodiment that can maintain / improve the quality of the electrode plate by manufacturing the electrode plate in which the binder is almost uniformly distributed in the electrode film at a low cost while improving the productivity.
  • the method and the manufacturing apparatus have been described, preferred examples for realizing the present embodiment will be described below.
  • Example 1 In the first embodiment, the spray nozzle is placed in the solidification chamber so that the contact width of the solidified liquid along the direction orthogonal to the conveying direction of the current collector foil is equal to or larger than the width of the coating film and within the current collecting tab attachment position.
  • An electrode plate manufacturing apparatus in which is disposed will be described.
  • the solidification chamber 18 of the first embodiment is surrounded by an outer wall 21 made of metal or synthetic resin, and a space isolated from the outside is provided on the conveyance path of the current collector foil 15. It has been.
  • the current collector foil 15 coated with the electrode material coating film 22 is solidified by a roller transport system 14 in a solidification chamber having a spray nozzle 23, a solidified liquid tank 25 in which a solidified liquid 24 is stored, a supply pump 26, and a waste liquid tank 27. 18 is introduced. Then, the coating film 22 is solidified by coming into contact with the solidified liquid 24 supplied from the spray nozzle 23 and is carried out to the next drying apparatus.
  • the spray pattern 33 of the solidified liquid 24 sprayed on the surface of the coating film 22 is a current collecting tab in which the spray region end in the coating film width direction is installed at a non-coating portion of the current collecting foil 15. It is inside the attachment position 28. Therefore, the electrode material component in the coating film 22 does not flow out to the current collecting tab attachment position 28.
  • the shape of the spray pattern 33 is not limited to the elliptical shape shown in FIG. 3 as long as the end of the spray region in the application width direction is inside the current collecting tab attachment position 28. It may be a combined pattern or the like. Furthermore, the flow rate distribution in the spray region has a uniform flow rate distribution as shown in FIG. 4, and the position where the flow rate is 50% of the flow rate at the center of the spray nozzle 23 is equal to or greater than the end of the coating film width.
  • the spray region having such a uniform flow distribution may be realized by a single nozzle or by combining a plurality of nozzles. By using the spray nozzle 23 having such a spray pattern and flow rate distribution, the solidified liquid can be brought into contact with the coating film surface evenly, and the in-plane uniformity of the electrode film can be improved.
  • a one-fluid nozzle that ejects only a liquid and a two-fluid nozzle that ejects a mixture of liquid and gas can be used. From the viewpoint of reducing the impact when water contacts the coating film solidified by spraying, a two-fluid nozzle capable of spraying finer droplets is desirable. Further, by setting the average particle diameter D50 of the spray particles sprayed from the spray nozzle 23 to 20 ⁇ m or less, more preferably 10 ⁇ m or less, damage such as coating film defects can be prevented.
  • the injection pattern of a single nozzle a flat pattern, a straight pattern, a full cone pattern, or the like can be used depending on the shape of the nozzle orifice.
  • the flow rate distribution it is sufficient that the uniform flow rate distribution shown in FIG. 4 is formed when the nozzles are combined, and the nozzle alone has a spray nozzle having various flow rate distributions such as a mountain-shaped flow rate distribution and an equal flow rate distribution. Can be used.
  • the spray hitting force per unit area is preferably adjusted to 5 g / cm or less, more preferably 1 g / cm from the viewpoint of damage to the coating film.
  • lithium nickel cobalt manganate as a lithium transition metal composite oxide
  • Graphite powder and acetylene black which are conductive assistants
  • PVdF polyvinylidene fluoride
  • NMP first N-methyl-2-pyrrolidone
  • the viscosity of the positive electrode slurry measured with a rotational viscometer was about 10 Pa ⁇ s.
  • the kneaded positive electrode slurry was applied to an aluminum foil (positive electrode current collector foil) having a thickness of 20 ⁇ m and a width of 200 mm with an applicator so as to have a thickness of 100 ⁇ m and a width of 150 mm.
  • the current collecting tab attachment position in the non-application part was 15 mm from the coating film terminal.
  • the above process is a coating process for applying a slurry-like electrode material on the surface of the current collector foil.
  • the aluminum foil coated with the electrode material was carried into the solidification chamber 18 shown in FIG. 2, and the electrode material was solidified by spraying the solidified liquid onto the coating film surface.
  • Pure water was used as the solidified liquid
  • an internal mixing type two-fluid nozzle was used as the spray nozzle.
  • the average particle diameter D50 of the spray particles ejected from the two-fluid nozzle was 10 ⁇ m.
  • the distance from the spray nozzle to the coating film was 100 mm, the spray pressure was 0.1 MPa, and the spray hitting force was adjusted to 1 g / cm.
  • the spray pattern was a full cone circular shape, the spray area was 80 mm in diameter, and the 50% flow area was 70 mm.
  • Two spray nozzles were arranged in the width direction of the coating film and sprayed onto the coating film surface.
  • the above process is a solidification process in which the electrode material is solidified by bringing the solidified liquid composed of the second solvent different from the first solvent contained in the electrode material into contact with the electrode material.
  • the above solidification phenomenon is a phenomenon in which water adhering by spraying penetrates while mutually dissolving with NMP in the coating film, and the solubility of the binder contained in the coating film decreases due to an increase in the moisture concentration in the coating film. It is.
  • the deposited binder bonds the positive electrode particles and the like, and solidifies the coating film. Since the electrode material solidified in this way loses fluidity and adhesiveness and is held on the aluminum foil, it can sufficiently withstand a contact-type conveying method in which a roller is brought into contact.
  • the aluminum foil holding the solidified coating film is transported to a drying chamber and dried in a hot air drying oven at 120 ° C. for 10 minutes to evaporate and remove pure water and NMP contained in the solidified coating film.
  • the positive electrode plate for lithium ion secondary batteries was manufactured.
  • the above process is a drying process in which the solvent component is removed from the electrode material and dried.
  • the amount of the binder on the aluminum foil side was 5.2%, the surface side was 4.4%, and the aluminum foil side The amount of the binder was 16% more. Moreover, as a result of observing the tab attachment position surface of aluminum foil, adhesion of electrode material was not confirmed.
  • Example 2 In the second embodiment, the spray nozzle is placed in the solidification chamber so that the contact width of the solidified liquid along the direction orthogonal to the conveying direction of the current collector foil is equal to or greater than the width of the coating film and within the current collector tab attachment position.
  • An electrode plate manufacturing apparatus in which a spray mask is disposed will be described.
  • the solidification chamber 18 of the second embodiment is surrounded by an outer wall 21 made of metal or synthetic resin, as in the first embodiment.
  • An isolated space is provided.
  • the current collector foil 15 coated with the electrode material coating film 22 is solidified by a roller transport system 14 in a solidification chamber having a spray nozzle 23, a solidified liquid tank 25 in which a solidified liquid 24 is stored, a supply pump 26, and a waste liquid tank 27. 18 is introduced. Then, the coating film 22 is solidified by coming into contact with the solidified liquid 24 supplied from the spray nozzle 23 and is carried out to the next drying apparatus.
  • the spray nozzle 23 of the second embodiment the same type of spray nozzle as that described in the first embodiment can be used. However, unlike the first embodiment, the spray nozzle 23 is disposed between the spray nozzle 23 and the roller conveyance system 14. Since the spray area is determined by the spray mask 29 arranged in the above, the shape of the spray pattern is not limited.
  • Fig. 6 shows an example of a spray mask.
  • the spray mask 29 provided with an opening in the center has an inclined portion 30 that is high on the center side and low on the outer peripheral side so that excessive solidified liquid does not flow to the coating film side.
  • an example of the linear inclined portion 30 has been described.
  • the spray mask 29 in which the inclined portion 30 has a round (R) may be used.
  • a discharge groove 31 for discharging the excessive solidified liquid to the outside is provided on the outer periphery of the spray mask 29.
  • the positive electrode slurry prepared in Example 1 was applied to an aluminum foil (positive electrode current collector foil) having a thickness of 20 ⁇ m and a width of 200 mm with an applicator so as to have a thickness of 100 ⁇ m and a width of 150 mm.
  • the current collecting tab attachment position in the non-application part was 15 mm from the coating film terminal.
  • the aluminum foil coated with the electrode material was carried into the solidification chamber 18 shown in FIG. 2, and the electrode material was solidified by spraying the solidified liquid onto the coating film surface.
  • Pure water was used as the solidified liquid
  • an internal mixing type two-fluid nozzle was used as the spray nozzle.
  • the average particle diameter D50 of the spray particles ejected from the two-fluid nozzle was 10 ⁇ m.
  • the distance from the spray nozzle to the coating film was 100 mm, the spray pressure was 0.1 MPa, and the spray hitting force was adjusted to 1 g / cm.
  • the spray pattern was a full cone circular shape, the spray area was 100 mm in diameter, and the 50% flow area was 80 mm.
  • Two spray nozzles were arranged in the width direction of the coating film, a spray mask was attached between the spray nozzle and the coating film, and the surface of the coating film was sprayed.
  • the opening diameter of the spray mask was 100 mm in the coating width direction and 50 mm in the transport direction.
  • the aluminum foil holding the solidified coating film is transported to a drying chamber and dried in a hot air drying oven at 120 ° C. for 10 minutes to evaporate and remove pure water and NMP contained in the solidified coating film.
  • the positive electrode plate for lithium ion secondary batteries was manufactured.
  • the amount of the binder on the aluminum foil side was 5.0%, the surface side was 4.3%, and the aluminum foil side The amount of the binder was 14% more. Moreover, as a result of observing the tab attachment position surface of aluminum foil, adhesion of electrode material was not confirmed.
  • Example 3 an electrode plate manufacturing apparatus in which a heater is attached to the spray mask used in the second embodiment will be described.
  • the solidification chamber 18 of the second embodiment is surrounded by a metal or synthetic resin outer wall 21 as in the second embodiment, and a space isolated from the outside is provided on the conveyance path of the current collector foil 15. ing.
  • the current collector foil 15 coated with the electrode material coating film 22 is solidified by a roller transport system 14 in a solidification chamber having a spray nozzle 23, a solidified liquid tank 25 in which a solidified liquid 24 is stored, a supply pump 26, and a waste liquid tank 27. 18 is introduced. Then, the coating film 22 is solidified by coming into contact with the solidified liquid 24 supplied from the spray nozzle 23 and is carried out to the next drying apparatus.
  • a spray mask 29 with a built-in heater is disposed between the spray nozzle 23 and the roller conveyance system 14.
  • Fig. 7 shows an example of a spray mask.
  • the spray mask 29 has an inclined portion 30 that is high on the center side and low on the outer peripheral side so that excessive solidified liquid does not flow to the coating film side.
  • a heater 32 is built in the inclined portion 30.
  • the spray mask 29 in which the inclined portion 30 is rounded (R) may be used.
  • a discharge groove 31 for discharging the excessive solidified liquid is provided on the outer periphery of the spray mask 29.
  • the amount of the binder on the aluminum foil side was 5.2%, the surface side was 4.5%, and the aluminum foil side The amount of the binder was 15% more. Moreover, as a result of observing the tab attachment position surface of aluminum foil, adhesion of electrode material was not confirmed.
  • Comparative Example 1 the positive electrode slurry of Example 1 was applied to an aluminum foil (positive electrode current collector foil) having a thickness of 20 ⁇ m with an applicator so as to have a thickness of 100 ⁇ m. NMP contained in the film was removed by evaporation to produce a positive electrode plate for a lithium ion secondary battery.
  • the manufacturing method of Comparative Example 1 corresponds to a conventional manufacturing method.
  • the amount of the binder on the aluminum foil side was decreased as compared with the vicinity of the surface. Specifically, the amount of binder on the aluminum foil side was 2.2%, the surface side was 6.5%, and the aluminum foil side was 66% less.
  • Example 2 the positive electrode slurry of Example 1 was applied to an aluminum foil (positive electrode current collector foil) having a thickness of 20 ⁇ m with an applicator so as to have a thickness of 100 ⁇ m, and immersed in pure water for 20 seconds to solidify the electrode material. Then, it dried at 120 degreeC for 10 minute (s) in the hot air drying furnace, the pure water and NMP which were contained in the coating film were removed by evaporation, and the positive electrode plate for lithium ion secondary batteries was manufactured.
  • the manufacturing method of this comparative example 2 is a manufacturing method which does not consider the outflow of the electrode material in the solidification process.
  • the amount of the binder on the aluminum foil side was increased as compared with the vicinity of the surface. Specifically, the amount of binder on the aluminum foil side was 5.3%, the surface side was 4.0%, and the aluminum foil side was 25% more. Moreover, the binder which is an electrode material had adhered from the observation result of the current collection tab attachment position surface.
  • Comparative Example 1 since the coating film is in a liquid state at the start of drying, movement of components such as a binder, that is, convection and diffusion occurs in the film, and it is estimated that the distribution of the electrode material is biased after drying.
  • the coating film was solidified in the solidification step, and at the same time, the components were fixed and the distribution was reduced because the components did not move during drying.
  • concentration on the side of current collection foil becomes relatively high, the adhesiveness of an electrode film and current collection foil became good, and the effect which the durability of a lithium ion secondary battery improved was acquired.
  • the contact roller transport system 14 can be used even in the case of double-sided batch application as shown in FIG. Can be used.
  • the present invention can be used for manufacturing a lithium ion secondary battery.

Abstract

L'invention concerne un dispositif de production d'une batterie secondaire au lithium-ion qui comprend au moins : une unité d'enduction qui applique une suspension épaisse de matériau d'électrode contenant un matériau actif pour une électrode positive ou une électrode négative, un liant, un agent de solidification et un premier solvant sur la surface d'un film collecteur de courant (15) ; une chambre de solidification (18) qui amène un liquide de solidification (24) en contact avec le film d'enduction (22) qui a été appliqué sur la surface du film collecteur de courant (15) et solidifie le film d'enduction (22) ; et une chambre de séchage qui élimine une composante liquide contenue dans le film d'enduction (22) qui s'est solidifié dans la chambre de solidification (18) et sèche le film d'enduction (22). La chambre de solidification (18) est dotée d'une buse de pulvérisation (23) qui règle la largeur de contact du liquide de solidification (24) le long d'une direction qui est orthogonale au sens de convoyage du film collecteur de courant (15) de manière à ce qu'elle soit supérieure à la largeur du film d'enduction (22) qui est appliqué sur la surface du film collecteur de courant (15) et au sein d'une position de fixation de languette de collecteur du film collecteur de courant (15).
PCT/JP2013/082324 2013-03-13 2013-12-02 Dispositif et procédé de production d'une batterie secondaire au lithium-ion WO2014141547A1 (fr)

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CN201380066009.6A CN104871360A (zh) 2013-03-13 2013-12-02 锂离子二次电池的制造装置和制造方法

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WO2020139823A1 (fr) * 2018-12-23 2020-07-02 Worcester Polytechnic Institute Couche intermédiaire adhésive pour électrodes de batterie par fabrication à sec
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JP2014179170A (ja) 2014-09-25

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