WO1999048164A1 - Accumulateur et son procede de fabrication - Google Patents

Accumulateur et son procede de fabrication Download PDF

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Publication number
WO1999048164A1
WO1999048164A1 PCT/JP1998/001108 JP9801108W WO9948164A1 WO 1999048164 A1 WO1999048164 A1 WO 1999048164A1 JP 9801108 W JP9801108 W JP 9801108W WO 9948164 A1 WO9948164 A1 WO 9948164A1
Authority
WO
WIPO (PCT)
Prior art keywords
secondary battery
adhesive
resin
negative electrode
positive electrode
Prior art date
Application number
PCT/JP1998/001108
Other languages
English (en)
Japanese (ja)
Inventor
Yasuhiro Yoshida
Michio Murai
Takayuki Inuzuka
Kouji Hamano
Hisashi Shiota
Shigeru Aihara
Daigo Takemura
Jun Aragane
Hiroaki Urushibata
Original Assignee
Mitsubishi Denki Kabushiki Kaisha
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority to CH694766A priority Critical patent/CH483049A/fr
Priority to CH694766D priority patent/CH694766A4/xx
Application filed by Mitsubishi Denki Kabushiki Kaisha filed Critical Mitsubishi Denki Kabushiki Kaisha
Priority to PCT/JP1998/001108 priority patent/WO1999048164A1/fr
Publication of WO1999048164A1 publication Critical patent/WO1999048164A1/fr

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Classifications

    • 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
    • G—PHYSICS
    • G04—HOROLOGY
    • G04D—APPARATUS OR TOOLS SPECIALLY DESIGNED FOR MAKING OR MAINTAINING CLOCKS OR WATCHES
    • G04D3/00—Watchmakers' or watch-repairers' machines or tools for working materials
    • G—PHYSICS
    • G04—HOROLOGY
    • G04D—APPARATUS OR TOOLS SPECIALLY DESIGNED FOR MAKING OR MAINTAINING CLOCKS OR WATCHES
    • G04D3/00—Watchmakers' or watch-repairers' machines or tools for working materials
    • G04D3/0002—Watchmakers' or watch-repairers' machines or tools for working materials for mechanical working other than with a lathe
    • G04D3/0053—Watchmakers' or watch-repairers' machines or tools for working materials for mechanical working other than with a lathe for framework components
    • 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
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • 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
    • 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
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • H01M50/461—Separators, membranes or diaphragms characterised by their combination with electrodes with adhesive layers between electrodes and separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/04—Cells with aqueous electrolyte
    • H01M6/06—Dry cells, i.e. cells wherein the electrolyte is rendered non-fluid
    • H01M6/10—Dry cells, i.e. cells wherein the electrolyte is rendered non-fluid with wound or folded electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/40—Printed batteries, e.g. thin film 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
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to a secondary battery, particularly to a lithium ion battery. More specifically, the present invention relates to a high-performance secondary battery that can take any form such as a thin type, and a method for forming the secondary battery.
  • Background art
  • Lithium-ion batteries are secondary batteries that are expected to achieve the highest voltage and the highest energy density among batteries to date, and improvements are being actively made today.
  • the positive electrode is a plate-like electrode formed by applying an active material made of powder such as lithium cobalt oxide to a current collector, and the negative electrode is similarly made of a carbon-based material.
  • a plate-like electrode is used in which an active material made of powder is applied to a current collector.
  • lithium ions can move between the two electrodes and that an ion conductive layer having no electron conductivity exists.
  • a separator which is a porous film such as polyethylene, is filled with a nonaqueous electrolyte is used for the ion conductive layer.
  • a rigid housing made of metal or the like 1 It is used for holding a negative electrode 5 and a separator 4 containing an electrolytic solution and the like. Without the housing 1, it is difficult to maintain the bonding between the electrodes 3, 5 and the separator 4, and the bonding part peels off, deteriorating the battery characteristics. Due to the housing 1, the weight of the battery is increased, and it is difficult to form an arbitrary shape. Currently, research into batteries that do not require a housing 1 is being conducted to reduce the weight and thickness. One of the challenges in developing a battery that does not require a housing 1 is how to join the positive electrode 3, the negative electrode 5, and the separator 4 sandwiched between these electrodes, and maintain the state without applying external force. Can be maintained.
  • the long electrode, the separator When bonding the electrode to the separator, the long electrode, the separator may be wound or folded, or the cut electrode or the separator may be laminated. It is necessary to fix with a jig until the agent dries. Fixing with a jig is a cause of poor workability. If there is no need to fix the jig before and during drying, the productivity of the battery becomes extremely efficient. Therefore, a method of forming a battery that does not require a jig before and during drying is desired. Disclosure of the invention
  • the method for forming the first secondary battery according to the present invention comprises: a positive electrode, a negative electrode, and a separator.
  • a method for forming a secondary battery in which the electrolyte is impregnated with an electrolyte the adhesive resin and the adhesive plastic resin between the positive electrode and the separator and between the anode and the separator are used.
  • the method includes a step of partially overlapping and overlapping, and a step of deforming the plastic resin.
  • the positive electrode, the negative electrode and the separator are dried each time they are laminated, or the holding treatment is performed to maintain the state of the laminated state by partially laminating an adhesive plastic resin.
  • the method for forming a second secondary battery according to the present invention is the method for forming the first secondary battery, wherein the plastic resin is deformed by applying a pressure higher than the plastic resin can be plastically deformed. It is.
  • the plastic resin is plastically deformed by pressurization, so that the depth of the void formed between the positive electrode and the negative electrode and the separator, that is, the depth of the gap between the positive electrode and the negative electrode and the separator is increased.
  • the distance between the electrodes can be reduced, and the ionic conduction resistance between the positive and negative electrodes and the separator when the electrolyte is held in these gaps is sufficiently small, enabling use at high load rates.
  • the bonding area between the positive electrode and the negative electrode and the separation can be increased, and the strength of the battery can be increased.
  • the step of deforming the plastic resin by applying the pressure includes impregnating with an electrolytic solution. It will be done later.
  • the resin is impregnated with the electrolyte and the resin is plastically deformed while the electrolyte is present in the micropores of the positive electrode and the negative electrode, thereby preventing resin from entering the micropores and improving the battery performance. Drop can be prevented.
  • a fourth method for forming a secondary battery according to the present invention is the same as the first method for forming a secondary battery, wherein the deformation of the plastic resin is heated.
  • a thermoplastic resin can be used. By heating and flowing the thermoplastic resin to deform it, the length of the gap formed between the positive electrode and the negative electrode and the separation, that is, the distance between the positive electrode and the negative electrode and the separation, Can be reduced, and the ion conduction resistance between the positive electrode and the negative electrode and the separator when the electrolytic solution is held in the gap becomes sufficiently small, so that it can be used at a high load factor.
  • the adhesive strength is generated by the flow of the thermoplastic resin, not only the contact area between the resin and the separator or between the positive electrode and the negative electrode surface increases, but also the anchor formed by the resin penetrating into the fine pores on the surface. The effect is also obtained, and a practical secondary battery with high adhesive strength can be obtained.
  • the adhesive resin is an adhesive whose adhesive strength is increased by heating.
  • a sixth method of forming a secondary battery according to the present invention is the method of forming the fifth secondary battery, wherein the adhesive whose adhesive strength is increased by heating is a thermo-crosslinkable resin. is there.
  • the method for forming a seventh secondary battery according to the present invention is the method for forming a secondary battery according to the fifth aspect, wherein the adhesive whose adhesive strength is increased by the heating is an adhesive dissolved in a solvent. Things.
  • the adhesive force is improved by heat, the adhesive force is increased, and the heat resistance of the battery can be increased. As a result, the strength of the completed battery can be made large enough to withstand practical use.
  • An eighth method for forming a secondary battery according to the present invention includes a method for forming a secondary battery in which a positive electrode and a negative electrode are included in a constituent element, and the constituent element is impregnated with an electrolytic solution. And a step of partially overlapping a plastic resin having adhesiveness and an adhesive resin, and a step of deforming the plastic resin. According to this method, it is necessary to provide a holding jig for drying each superposition of the positive electrode and the negative electrode or for maintaining a superimposed state by partially laminating an adhesive plastic resin and laminating. Since the subsequent steps do not need to be performed sequentially, they can be performed collectively, and productivity is greatly improved due to simplification of manufacturing equipment.
  • the plastic resin is deformed by applying a pressure higher than the plastic resin can be plastically deformed. It is what you do. According to this method, the depth of the void formed between the positive electrode and the negative electrode, that is, the distance between the positive electrode and the negative electrode can be reduced by plastically deforming the plastic resin by applying pressure. However, when the electrolyte is held in the gap, the ionic conduction resistance between the positive electrode and the negative electrode becomes sufficiently small, enabling use at a high load factor and reducing the bonding area between the positive electrode and the negative electrode. By increasing the size, the strength of the battery can be increased.
  • the step of deforming the plastic resin by applying the pressure may include impregnating an electrolyte. It will be done later. According to this method, by impregnating the electrolyte and plastically deforming the resin while the electrolyte is present in the fine pores of the positive electrode and the negative electrode, the resin is prevented from penetrating into the fine pores, and the battery performance is reduced. Can be prevented.
  • the eleventh method for forming a secondary battery according to the present invention is the same as the eighth method for forming a secondary battery, except that the deformation of the plastic resin is heated. According to this method, a thermoplastic resin can be used.
  • the depth of the gap formed between the positive electrode and the negative electrode that is, the distance between the positive electrode and the negative electrode can be reduced.
  • the ionic conduction resistance between the positive electrode and the negative electrode when the electrolytic solution is held is sufficiently small, and it can be used at a high load factor.
  • the adhesive strength is exhibited by the flow of the thermoplastic resin, not only the contact area between the resin and the surface of the positive electrode and the negative electrode becomes large, but also the anchor effect caused by the resin penetrating into the fine pores on the surface. Thus, a practical secondary battery having high adhesive strength can be obtained.
  • the adhesive resin is an adhesive whose adhesive strength is increased by heating.
  • the adhesive whose adhesive strength is increased by heating is a thermo-crosslinkable resin. is there.
  • the method for forming a second rechargeable battery according to the first or second method is such that the adhesive whose adhesive strength increases by heating is an adhesive dissolved in a solvent. It is.
  • the adhesive strength is improved by heat, the adhesive strength is enhanced, and the heat resistance of the battery can be increased. It can be large enough to withstand the heat.
  • a first secondary battery according to the present invention includes a positive electrode formed by bonding a positive electrode active material layer to a positive electrode current collector; a negative electrode formed by bonding a negative electrode active material layer to a negative electrode current collector;
  • the above-mentioned active material layers and the above-mentioned respective active material layers are formed so as to form a gap communicating between the respective positive electrode active material layers and the above-mentioned negative electrode active material layer and between the above-mentioned respective active material layers and the above-mentioned separate layer.
  • It is provided with an electrode laminate having a plastic resin which is solid at room temperature, has a sticky surface, and is deformed by heating or pressing, and an adhesive resin, which are arranged between the separators. According to this, since it has a plastic resin which is solid at room temperature and has a sticky surface and is deformed by heating or pressing, and an adhesive resin, a high-performance secondary battery can be produced with high productivity. can get.
  • the area of the void is 30% to 90% of the total area of each facing surface where each active material layer faces the separator. %. According to this, the ionic conduction resistance between the positive electrode, the negative electrode, and the separator when the electrolyte is held in the gap formed between the positive electrode, the negative electrode, and the separator becomes sufficiently small, It can be used at a high load rate and has practically sufficient adhesive strength.
  • the adhesive resin is an adhesive whose adhesive strength is increased by heating.
  • a fourth secondary battery according to the present invention is the above-mentioned third secondary battery, wherein the adhesive whose adhesive strength is increased by heating is a thermo-crosslinkable resin.
  • the adhesive whose adhesive strength is increased by heating is an adhesive dissolved in a solvent.
  • the adhesive strength can be increased, the heat resistance of the battery can be increased, and the battery strength can be increased. It can be large enough to be practical.
  • a sixth secondary battery according to the present invention is the first secondary battery according to the first aspect, Of the present invention. According to this, a compact, stable secondary battery having a large battery capacity can be obtained.
  • a seventh secondary battery provides a positive electrode in which a positive electrode active material layer is joined to a positive electrode current collector; a negative electrode in which a negative electrode active material layer is joined to a negative electrode current collector; A plastic resin, which is solid at room temperature, has a sticky surface, and is deformed by heating or pressing, and an adhesive resin, which is disposed between the active material layers so as to form voids communicating between the layers.
  • An electrode laminate having the following. According to this, in a secondary battery having no separation, the same effect as the first secondary battery can be obtained.
  • An eighth secondary battery according to the present invention is the above-described seventh secondary battery, comprising a plurality of electrode laminates. According to this, a compact, stable secondary battery having a large battery capacity can be obtained.
  • FIG. 1 is a schematic cross-sectional view showing a battery structure of a lithium ion battery according to an embodiment of the present invention
  • FIG. 2 is a sectional view showing an adhesive resin according to an embodiment of the present invention
  • FIG. 3 is a schematic view showing a coating method of the present invention.
  • FIG. 3 is a schematic sectional view showing a lithium ion battery according to an embodiment of the present invention.
  • FIGS. 4, 5 and 6 show the present invention.
  • FIG. 7 is a schematic sectional view showing a battery structure of a lithium ion secondary battery according to another embodiment
  • FIG. 7 is a schematic sectional view showing a conventional lithium ion secondary battery.
  • the present invention is applied to a battery having a structure in which an ion conductive layer is disposed between a positive electrode and a negative electrode and between the positive electrode and the negative electrode.
  • the following embodiment mainly includes a single electrode stack including a positive electrode, an ion conductive layer, and a negative electrode.
  • a layer electrode type battery will be described, the present invention is also applicable to a layered electrode type battery in which a single electrode laminate is stacked.
  • FIG. 1 is a schematic cross-sectional view showing a battery structure of a lithium-ion battery according to an embodiment of the present invention, that is, a structure of an electrode stack.
  • reference numeral 3 denotes a positive electrode active material layer 32
  • the positive electrode joined to the body 3 1, the negative electrode 5 joined to the negative electrode active material layer 5 2 on the negative electrode current collector 51, and the separator 4 arranged between the positive electrode 3 and the negative electrode 5.
  • Numeral 8 is partially arranged like a point, a line, or a lattice between opposing surfaces of the positive electrode active material layer 32 and the negative electrode active material layer 52 and the separator 4, and is solid and viscous at room temperature. It is a resin that has adhesive properties and deforms when heated or pressed. Numerals 6 are partially arranged in a point-like, linear, or lattice-like manner between the facing surfaces of the positive electrode active material layer 32 and the negative electrode active material layer 52 and the separator 4, and each active material layer 3 It is an adhesive resin that joins 2, 5, and 2 to Separee.
  • Reference numeral 7 denotes a void portion that communicates between the positive electrode active material layer 32 and the negative electrode active material layer 52 and the separator 4. The void 7, the separator 4, and the active material layers 32, 52 hold a non-aqueous electrolyte containing lithium ions.
  • a liquid in which the adhesive resin is dissolved in a solvent may be applied to the interface between the separator 4 and the active material layers 32, 52 to evaporate the solvent.
  • the solvent is evaporated and becomes porous due to volume shrinkage or crystallization of the resin.
  • the resin 8 and the adhesive resin 6 having at least a part of the surface having adhesiveness are interposed between the positive electrode 3 and the separator 4 and between the negative electrode 5 and the separator 4 and are superposed.
  • the positive electrode 3 and the separator 4 and the negative electrode 5 and the separator 4 are temporarily fixed with the adhesive force of the resin 8, and then the resin 8 and the resin 8 are applied as necessary by applying pressure, heating, or the like as described below.
  • the gap between the electrodes 3 and 5 and the separation 4 is reduced, and the depth of the gap 7 is set to a predetermined value.
  • the resin 8 and the adhesive resin 6 used in the present invention can be used as long as they do not dissolve in the electrolytic solution.
  • the area of the void 7 formed by the adhesive resin 6 is desirably 30% to 90% of the total area of each opposing surface where the active material layers 32, 52 and the separator 4 oppose each other, Most preferably, it is about 60%. If it is less than 30%, the electrical connection between the electrode active material layers 32 and 52 and the separator 4 becomes insufficient, and the ionic conduction resistance between the electrodes 3 and 5 increases. However, it becomes difficult to obtain sufficient battery characteristics. On the other hand, if it exceeds 90%, the adhesion between the electrodes 3, 5 and the separator 4 becomes insufficient, and peeling occurs.
  • the depth of the void 7 formed between the active material layers 32, 52 and the separator 41 is determined by the amount of the electrolyte.
  • the ionic conductivity in the case of about 10 _ 2 S / cm, which is usually used, if it is 30 ⁇ m or less, the distance between the active material layers 32 and 52 and the separator 4 Since the ionic conduction resistance of the battery becomes sufficiently small, and the battery can be used at a high load factor that is not inferior to a battery using a conventional outer can, it is preferable that the ion conductivity be 30 m or less.
  • the depth L of the void portion 7 is set to 10 / m or less, diffusion of the reactive species can be more easily promoted, and the ion conduction resistance can be further reduced. It is more desirable to adjust to. Furthermore, it is said that a diffusion layer of several meters exists on the surface of the active material 32, 52 where an electrode reaction occurs.By adjusting the depth L of the void 7 to less than this, lithium ions can be removed. It is most preferable that the depth L of the void 7 is set to several meters or less, since diffusion is considered to proceed most easily.
  • the adhesive resin 6 is arranged between the electrodes 3 and 5 and the separator 4 in a dotted, linear, or grid-like manner and closely adhered, so that the liquid electrolyte is provided between the electrodes 3 and 5 and the separator 4. Gap 7 that can hold Wear.
  • the ionic conduction resistance between the electrodes 3 and 5 can be reduced to the same level as a battery using a conventional outer can, and furthermore, the electrodes 3 and 5 and the separator 4 Since the gap between them is adhered, the electrodes 3, 5 and the separator 4 can be brought into close contact with each other without an outer can.
  • the adhesive resin 6 When the adhesive resin 6 is a liquid in which the adhesive resin is dissolved in a solvent, the adhesive resin 6 becomes porous due to volumetric shrinkage due to solvent evaporation or crystallization of the resin due to heating and drying. By holding the liquid electrolyte in the portion, the ionic conduction resistance between the electrodes 3 and 5 can be reduced.
  • the secondary battery configured as described above is formed, for example, by the following method.
  • the formation method of the present invention includes a step of applying the positive electrode active material layer 32 and the negative electrode active material layer 52 to the current collectors 31 and 51, respectively, and opposing the positive electrode active material layer 32 and the separator 4.
  • a step of deforming the resin 8 and the adhesive resin 6 to reduce the depth L of the gap 7 is provided.
  • the positive and negative electrode active material powders each of which is mixed with a binder resin to form a paste, and this paste is used to form the positive and negative electrode final bodies 31, 5, 1 Apply to it and dry.
  • any resin that does not dissolve in the electrolyte and does not cause an electrochemical reaction inside the battery can be used.
  • homopolymers or copolymers such as vinylidene fluoride, fluorinated ethylene, atalylonitrile, and ethylene oxide; Lenpropylene diamine rubber or the like can be used.
  • the active material in the positive electrode 3, for example, a composite oxide of lithium and a transition metal such as cobalt, nickel, manganese, a chalcogen compound containing lithium or a composite oxide thereof, and the above-described composite oxide, lithium Chalcogen compounds containing these or complex oxides thereof to which various elements are added in trace amounts are used, and those obtained by adding graphite as an electron conductor to these substances are used.
  • a composite oxide of lithium and a transition metal such as cobalt, nickel, manganese, a chalcogen compound containing lithium or a composite oxide thereof, and the above-described composite oxide
  • lithium Chalcogen compounds containing these or complex oxides thereof to which various elements are added in trace amounts are used, and those obtained by adding graphite as an electron conductor to these substances are used.
  • the present invention is not limited to this, and any other substance that can occlude and release lithium ions necessary for battery operation can be used.
  • these substances are used in the form of particles, and those having a particle size of 0.3 m to 20 m can be used, and particularly preferably 0.3 // m to 5 m belongs to.
  • Carbon fibers can also be used as the negative electrode active material 52. If the particle size is too small, the coverage area of the active material surface with the adhesive during bonding becomes too large, so that lithium ions are not efficiently doped or removed during charging and discharging, and the battery is not used. The characteristics are degraded. If the particle size is too large, it is not preferable because it is not easy to form a thin film and the packing density is reduced.
  • the current collectors 31 and 51 can be used as long as the metal is stable inside the battery, but aluminum is preferably used for the positive electrode 3 and copper is preferably used for the negative electrode 5. As the shape of the current collectors 31 and 51, foil, net, and expansive metal can be used, and foil is preferably used to obtain electrode smoothness.
  • a co-casting method is used, which is shown in FIG. 2 in a perspective view (a) and a side view (b).
  • a coating method of removing the molten resin 6 with a rotating roll 21 having dot-like depressions 21a and transferring the same to a sheet (eg, sheet-like separator 6) is applied.
  • a spray method, a roll method in which a molten resin is poured out from fine holes of a roll and applied, and the like are applicable, and are not particularly limited.
  • the resin 8 and the adhesive resin 6 may be applied by different application methods.
  • Separee 4 can be used as long as it has sufficient strength with an insulating porous membrane, mesh, non-woven cloth, etc., and is not particularly limited, but a porous material made of polypropylene, polyethylene, etc.
  • the use of a film is preferred from the viewpoint of ensuring adhesiveness and safety.
  • it is necessary to have a through-hole but the ratio of the through-hole to the entire area is preferably at least 10%, and more preferably at least 30%.
  • a process of applying a pressure to the superposed positive electrode 3, the separator 4, and the negative electrode 5 that is higher than the plastic deformation of the resin 8 and the adhesive resin 6 is performed. .
  • This pressure can be applied at any time after all overlays have been completed.
  • This process increases the contact area between the resin 8 and the adhesive resin 6 and the electrodes (positive electrode 3 and negative electrode 5) and the electrode 4, increases the adhesive strength, and ensures that the completed battery strength can withstand practical use. The effect is to make it sufficiently large.
  • This step is also necessary for controlling the thickness of the resin 8 and the adhesive resin 6 interposed between the electrodes 3 and 5.
  • Adhesion in this way eliminates the need for holding jigs to dry electrodes 3 and 5 and Separation 4 at the time of superposition, or to maintain the state of superposition, and plastic deformation of the resin.
  • the step of applying more pressure than can be performed can be performed collectively without the necessity of performing it sequentially, and the productivity is greatly improved by simplifying the manufacturing equipment.
  • a non-aqueous liquid electrolyte containing lithium ions used in conventional batteries can be used.
  • a solvent for the liquid electrolyte a single solvent of an ester solvent such as ethylene carbonate, propylene carbonate, dimethyl carbonate, and getyl carbonate, and a single solvent of an ether solvent such as dimethoxetane, jetoxetane, getyl ether, and dimethyl ether It is possible to use a mixture of two or more of the above-mentioned solvents of the same system or solvents of different systems.
  • the electrolyte salt used in the liquid electrolyte L i PF 6, L i A s F 6, L i C 10 4, L i BF 4, L i CF 3 S 0 3 ⁇ L i N (CF 3 S 0 2 ) 2 , L i C (CF a S 0 2 ) 3 , L i N (C 2 F 5 S 0 2 ) 2, etc. can be used.
  • the step of applying a pressure higher than the resin can be plastically deformed is performed before impregnation with the electrolytic solution. By doing so, the following effects can be obtained.
  • the plastic deformation of the resin increases the contact area with the electrode active material and the separator and enhances the adhesive strength.
  • the resin separates the porous pores of the electrode and the micropores of the electrode. It also has the undesired effect of degrading the closing battery performance.
  • impregnating the electrolyte and plastically deforming the resin while the electrolyte is present in the micropores of the electrode during separation it is possible to prevent the resin from penetrating into the micropores and prevent the battery performance from deteriorating. The effect is obtained.
  • the bonding may be performed by using a thermoplastic resin and heating the thermoplastic resin to a temperature higher than a temperature at which the thermoplastic resin is easily deformed.
  • the heating method is not limited to a hot plate, an oven, an infrared heater or the like. Since the adhesive force is developed by the flow of the thermoplastic resin, not only does the contact area between the resin and the surface of the separator 4 or the electrodes 3 and 5 increase, but also the anchors formed by the resin penetrating into the micropores on the surface. One effect is also obtained. If the viscosity of the thermoplastic resin is high, it may be desirable to apply pressure during heating, but this is not required.
  • thermoplastic resin has a melting point of 200 ° C. or lower, and any resin can be used as long as it is insoluble in the electrolytic solution. If the fluidity during heating is not suppressed, it can be used even if high melting point components, inorganic substances, etc. are mixed.
  • the heating period can be any time after all the superpositions have been completed. This step has the effect of sufficiently increasing the heat resistance of the completed battery.
  • the bonding may be performed by irradiating ultrasonic waves while applying pressure. Ultrasonic waves efficiently deform the resin and enable bonding even under low pressure or low bonding temperature. Irradiation of ultrasonic waves has an effect of selectively heating a portion where the thermoplastic resin is in contact with the electrode surface. For this reason, bonding is performed very efficiently.
  • the heat resistance of the battery can be increased by using an adhesive whose adhesive strength is increased by heat, such as an adhesive having a thermal crosslinking property, as the adhesive resin 6.
  • an adhesive having a thermal crosslinking property such as an adhesive having a thermal crosslinking property
  • the adhesive resin 6 an adhesive having a thermal crosslinking property
  • this type of adhesive include epoxy resins, thermosetting acrylic resins, phenolic resins, urethane resins, and others, such as amino, furan, and xylene resins, which are resistant to electrolytes. Anything can be used.
  • an adhesive whose adhesive strength is improved by heat, use a solution in which an adhesive resin is dissolved in a solvent, and increase the adhesive strength by evaporating the contained solvent. This makes it possible to bond at a low heating temperature.
  • the combined use of drying under reduced pressure can improve the adhesive strength at room temperature.
  • various types of solvent-soluble polymers can be used in addition to general rubber-based adhesives.
  • the separator 4 is provided between the positive electrode 3 and the negative electrode 5.
  • the secondary battery forming method of the present invention can be applied to a configuration not including the separator.
  • FIG. 4 a structure having a plurality of electrode laminates in which a positive electrode 3 and a negative electrode 5 are alternately arranged between a plurality of separated separators 4 is shown in FIGS. 5 and 6.
  • a positive electrode 3 and a negative electrode 5 are alternately arranged between the rolled strip-shaped separators 4 as shown in the figure, and a structure having a plurality of electrode laminates, and a folded strip-shaped separator 4 (not shown).
  • the method of forming the stacked electrode type battery shown in FIGS. 4 and 5 will be described in detail in the following examples.
  • a method of forming a lithium ion battery has been described.
  • the present invention can be applied to various secondary batteries by changing materials such as an active material and an electrolyte to exhibit an effect. This is a battery forming method.
  • a negative electrode active material paste was prepared by mixing and mixing 95% by weight of Mesophase Microphone Bead Bead Carbon (manufactured by Osaka Gas Co., Ltd.) and 5% by weight of polyvinylidene fluoride as a binder resin.
  • a negative electrode was formed on a current collector made of copper foil having a thickness of about 100 ⁇ m by a dough-blade method. The positive and negative electrodes were cut into 5 cm x 4 cm rectangles, and the cut positive and negative electrodes and the current collecting terminals (tabs) were attached.
  • a polybutene-polypropylene copolymer manufactured by Nitta Gelatin Co., Ltd., product number: H-6285, softening point 84 ° C
  • the copolymer was applied in the form of dots, and the applied amount was about 9 per m 2 .
  • Epoxy adhesive (manufactured by Sribond Co., Ltd., trade name: Slipbond 2071B) is applied to Separe Itesu (Celgard # 2400, manufactured by Hex Celanese) by spraying. did.
  • the separator to which the adhesive was applied was sandwiched between the positive electrode and the negative electrode to which the copolymer had been previously applied, and superposed, and a pressure of 20 g was applied per 1 cm 2 . Due to the adhesiveness of the hot melt adhesive, the positive electrode, the separator, and the negative electrode were bonded together, maintaining the bonded shape without the need for a jig. Thereafter, heating was performed for about 1 hour in an oven heated to 70 ° C. By this heating, the epoxy adhesive was cured.
  • the bonded electrode was inserted into a cylindrical aluminum laminating film, and an electrolyte was injected.
  • the electrolyte used was ethylene carbonate and 1,2-dimethoxetane as the solvent, and lithium hexafluorophosphate was used as the electrolyte.
  • the aluminum laminate film was sealed to complete the battery.
  • the battery characteristics of the battery thus manufactured were 68 Wh / kg at a current value of 1 C and 50 Wh / kg at a current value of 1.5 C in terms of weight energy density.
  • a 5 cm ⁇ 4 cm rectangular electrode with a current collecting terminal manufactured in the same manner as in Example 1 was used.
  • Polybutene-polypropylene copolymer manufactured by Nitta Gelatin Co., Ltd., product number: H-6825, softening point 84
  • Separe Itesu (Celgard # 2400, manufactured by Hex To Celanese) ° C) with a coater (CP3000, manufactured by MELTEX).
  • the copolymer was applied in the form of dots, and the applied amount was about 9 per m 2 .
  • an acrylic emulsion adhesive (manufactured by Showa Polymer Co., Ltd.) was partially applied by spraying onto the separator coated with the copolymer, and the separator was placed between the positive electrode and the negative electrode. The sandwich was overlapped and a pressure of 20 g / cm 2 was applied. The positive electrode, separator, and negative electrode were adhered by the hot-melt adhesive, and the adhesive shape was maintained without the need for a jig.
  • the aluminum laminate film was sealed to complete the battery.
  • Example 3 A positive electrode and a negative electrode with a current collecting terminal prepared in the same manner as in Example 1 were applied to SIS-Yube hot melt adhesive (AK-1, manufactured by Kanebo NSC Co., Ltd., with a softening point of about 100 ° C). Was applied with Ko overnight (CP3000, manufactured by MELTEX). Hot Tomeruto adhesive is applied in dots, the coating weight was about 1 0 g per lm 2.
  • a 10% N-methylpyrrolidone solution of polyvinylidene fluoride (Kureha Kagaku KF100) was applied by spraying to Separei (Celgard # 240, manufactured by Hex Celanese). This separator was sandwiched between the positive electrode and the negative electrode, and then superposed, and a pressure of 20 g was applied per cm 2 . The positive electrode, the separator, and the negative electrode were adhered to each other due to the adhesiveness of the hot melt adhesive, and the adhesive shape was maintained without the need for a jig.
  • the bonded electrode was inserted into a cylindrically processed aluminum laminate film, and an electrolyte was injected.
  • the electrolyte used was ethylene carbonate and 1,2-dimethoxetane as the solvent, and lithium hexafluorophosphate was used as the electrolyte. After injecting the electrolyte, the aluminum laminate film was sealed to complete the battery.
  • the characteristics of the battery fabricated in this manner were 73 Wh / kg in terms of weight energy density.
  • a 5 cm x 4 cm rectangular electrode with a current collecting terminal manufactured in the same manner as in Example 1 was used.
  • the positive electrode was spray-coated with a SIS-type hot melt adhesive (AK-1, manufactured by Kanebo N.S.C., having a softening point of about 100 ° C).
  • the applied amount was about 15 g per m 2 .
  • the bonded electrode was inserted into a cylindrically processed aluminum laminate film, dried sufficiently, and then an electrolyte was injected.
  • electrolyte ethylene carbonate and 1,2-dimethoxyethane were used as a solvent, and lithium hexafluorophosphate was used as an electrolyte. After injecting the electrolyte, the aluminum laminate film was sealed to complete the battery.
  • the battery characteristics of the battery thus manufactured were 70 Wh / kg at a current value of 1 C and 50 Wh / kg at a current value of 1.5 C in terms of weight energy density.
  • a 5 cm ⁇ 4 cm rectangular electrode with a current collecting terminal manufactured in the same manner as in Example 1 was used.
  • a SIS type hot melt adhesive (AK-1, manufactured by Kanebo NSS Co., Ltd., having a softening point of about 100 ° C) was partially applied to the positive electrode by spraying. The applied amount was about 15 g per m 2 .
  • an epoxy adhesive manufactured by Three Bond Co., Ltd., trade name: Three Bond 207 B
  • Separei Chemicalgard # 240, manufactured by Hex Celanese
  • the electrolyte ethylene carbonate and 1,2-dimethoxyethane were used as solvents, and lithium hexafluorophosphate was used as the electrolyte.
  • the electrolyte solution crushed 2 0 g adhesive layer under pressure per 1 cm 2 at room temperature, to rather small space between the positive electrode and the negative electrode, as a result of Eject and down the excess electrolyte, the space Became about 10 m thick.
  • the battery was completed by sealing the aluminum laminate film.
  • a 5 cm x 4 cm rectangular electrode with a current collecting terminal manufactured in the same manner as in Example 1 was used.
  • Separe Itesu Hybrinese, Celgard # 240
  • a polybutene-polypropylene copolymer manufactured by Nitta Gelatin Co., Ltd., product number: H-6825, softening point 8) 4 ° C
  • CP300 manufactured by MELTEX
  • the copolymer was applied in the form of dots, and the amount applied was about 9 g / m 2 .
  • an acrylic adhesive (part of Showa Polymer Co., Ltd.) was partially applied by spraying to the separator coated with the copolymer, and the separator was sandwiched between the positive and negative electrodes. , 10 ° C Heated on plate for about 2 minutes. As a result, the positive electrode, the separator, and the negative electrode were bonded, and the bonded shape was maintained without the need for a jig.
  • the electrolyte used was ethylene carbonate and 1,2-dimethoxetane as the solvent, and lithium hexafluorophosphate was used as the electrolyte. After injecting the electrolyte, the aluminum film was sealed to complete the battery.
  • the battery characteristics of the battery thus manufactured were 6 ⁇ Wh / kg at a current value of 1 C and 45 Wh / kg at a current value of 1.5 C in terms of weight energy density.
  • This example is a method for forming a lithium ion battery having the flat-plate laminated battery body shown in FIG.
  • a positive electrode and a negative electrode were prepared using the same materials and method as described in Example 1, the positive electrode, the negative electrode, and an epoxy-based adhesive (manufactured by Sribond Co., Ltd., trade name: Sribond 207) 1 B) was applied by spraying. Two rolls of 12 cm wide and 25 mm thick porous polypropylene sheet (made by Hext Co., Ltd., trade name: Celgard # 2400) were bundled in rolls as separator material. The product was taken out, and one side of each product was coated with an adhesive resin in the form of dots, using a product number: H-6825 (manufactured by Nigeru Gelatin Co., Ltd.) according to the Koiyu method.
  • the positively-fixed positive electrode or negative electrode
  • the adhesive resin is applied in the form of dots and a negative electrode (or positive electrode) is superimposed on this coated surface, and another positive electrode (or negative electrode) is applied.
  • the adhesive resin is temporarily fixed on the uncoated surface of the separator and the adhesive resin is applied in a dot-like manner to the uncoated surface of the separator by a coating method. Is the positive electrode). This step was repeated to form a plurality of electrode laminates in layers.
  • the positive electrode, the separator, and the negative electrode were adhered to each other due to the tackiness of the adhesive resin, and the adhesive shape was maintained without the need for a jig.
  • the battery body in which the plurality of electrode laminates were formed in a layer shape was heated and fused at 70 ° C. by a roll to bond the positive electrode and the negative electrode to the separator. By this heating, the epoxy adhesive was cured.
  • This embodiment relates to a method for forming a lithium ion secondary battery having the flat-plate wound battery structure shown in FIG.
  • the positive electrode and the negative electrode active material were applied to the long positive electrode and negative electrode current collectors in the same manner and in the same manner as described in Example 1 and dried to form the positive electrode 3 and the negative electrode 5.
  • An epoxy-based adhesive (trade name: Slip Bond 207B) manufactured by Sri Bond Co., Ltd. was applied to both surfaces of each negative electrode by spraying.
  • a porous polypropylene sheet with a width of 12 cm and a thickness of 25 m (made by Hext Co., Ltd., trade name: Celgard # 2400), which is bundled in a roll shape as a separator material
  • the product was taken out, and one side and one end of the other side were coated with an adhesive resin in the form of a dot, in the form of an adhesive resin, with the product number: H-62825 (manufactured by Nikko Gelatin Co., Ltd.).
  • the temperature of the adhesive resin is once lowered to room temperature, and one end of the separator is bent by a certain amount.
  • a single positive electrode (or negative electrode) is sandwiched between the two parts, and a negative electrode (or positive electrode) is placed on the application surface of the bent part so as to face this positive electrode (or negative electrode), and this negative electrode (or positive electrode) is separated. I caught in overnight.
  • the positive electrode (or the negative electrode) and the negative electrode (or the positive electrode) are alternately opposed to each other while applying the resin in the form of a dot on the surface opposite to the surface of the separator on which the resin has been previously applied. And rolled up Separete in an oval shape.
  • the battery body on the rolled-up ellipse is heated and fused at 70 ° C by a roll, and the positive electrode, the negative electrode and the separator are adhered to each other. I got a body.
  • the positive and negative electrode current collectors 31 and 51 of this flat laminated battery body were spot-welded to the positive and negative electrodes of the current collector tabs connected to the respective ends of the current collectors 31 and 51 to form the laminated battery body. Electrically connected in parallel.
  • This embodiment is directed to a method of forming a lithium ion secondary battery having the flat-plate wound laminated battery body shown in FIG. 6, which is different from Embodiment 8 above in that each electrode and separator are simultaneously wound. It is.
  • an epoxy-based adhesive manufactured by Three Bond Co., Ltd., trade name: Slip bond 207 1 B
  • a porous polypropylene sheet product name: Celgard # 2400, manufactured by Hext Co., Ltd.
  • a strip-shaped negative electrode (or positive electrode) was arranged so as to protrude by a certain amount from one side of the positive electrode (or negative electrode) with a separator. Bend the protruding negative electrode (or positive electrode) and wrap it around the positive electrode (or negative electrode) with separator, and then bond the positive electrode (or negative electrode) with separate separator, and then fold the negative electrode (or positive electrode). ) Were wrapped around each other, and the positive electrode (or negative electrode) with separator was wound in an elliptical shape so as to wrap the folded negative electrode (or positive electrode). Thereafter, the whole was fused with a heating roll to obtain a wound-type laminated structure battery body as shown in FIG.
  • the positive electrode and the negative electrode current collectors 31 and 51 of the wound laminated battery body are spot-welded to the positive electrode and the negative electrode by connecting current collecting tabs connected to the ends of the current collectors 31 and 51, respectively, so that the laminated battery body is electrically connected. Connected in parallel.
  • the adhesive resin is applied to the separation layer.
  • the active material layers 32 and 52 may be coated. Both may be applied. Industrial applicability

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  • Electrochemistry (AREA)
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  • Engineering & Computer Science (AREA)
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  • General Physics & Mathematics (AREA)
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Abstract

L'invention porte sur une méthode de fabrication d'un accumulateur dont les électrodes négative et positive, qui présentent une densité d'énergie accrue et une taille moindre peuvent prendre une forme quelconque. Ces accumulateurs aux excellentes caractéristiques de charge/décharge permettent d'intercaler un séparateur très proche sans recourir à des bacs solides ni accroître la résistance entre électrodes d'où leur rendement plus élevé. La méthode comprend un procédé consistant à empiler dans l'ordre, une l'électrode négative (5) constituée d'un matériau approprié (52) collé sur un support approprié (51), un séparateur (4), et une électrode positive (3) constituée d'un matériau approprié (32) collé sur un support approprié (31), en interposant partiellement une résine plastique (6) visqueuse et une résine adhésive (8) entre les électrodes (3 et 5) et le séparateur (4), et sur un procédé de déformation de la résine (6). Puisqu'un support n'est pas nécessaire, la productivité de la batterie se trouve améliorée.
PCT/JP1998/001108 1966-05-12 1998-03-17 Accumulateur et son procede de fabrication WO1999048164A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
CH694766A CH483049A (fr) 1966-05-12 1966-05-12 Machine pour la fabrication de platines d'horlogerie
CH694766D CH694766A4 (en) 1966-05-12 1966-05-12 Secondary battery and method for forming the same
PCT/JP1998/001108 WO1999048164A1 (fr) 1966-05-12 1998-03-17 Accumulateur et son procede de fabrication

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CH694766A CH483049A (fr) 1966-05-12 1966-05-12 Machine pour la fabrication de platines d'horlogerie
PCT/JP1998/001108 WO1999048164A1 (fr) 1966-05-12 1998-03-17 Accumulateur et son procede de fabrication

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WO1999048164A1 true WO1999048164A1 (fr) 1999-09-23

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WO (1) WO1999048164A1 (fr)

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008135289A (ja) * 2006-11-28 2008-06-12 Nissan Motor Co Ltd 二次電池およびその製造方法
JP2011129497A (ja) * 2009-12-15 2011-06-30 Samsung Sdi Co Ltd 二次電池
KR101454996B1 (ko) * 2012-03-07 2014-10-30 닛산 지도우샤 가부시키가이샤 이차 전지
JP2015053118A (ja) * 2013-09-05 2015-03-19 日立マクセル株式会社 リチウムイオン二次電池用セパレータおよびその製造方法、並びにリチウムイオン二次電池およびその製造方法
JP2016535923A (ja) * 2013-11-04 2016-11-17 エルジー・ケム・リミテッド 二次電池用接着層の形成方法
JP2018055951A (ja) * 2016-09-28 2018-04-05 日産自動車株式会社 二次電池
JP2018113122A (ja) * 2017-01-10 2018-07-19 日産自動車株式会社 リチウムイオン二次電池の製造方法
EP3244475A4 (fr) * 2015-09-02 2019-08-14 LG Chem, Ltd. Membrane de séparation comprenant des parties de revêtement adhésif ayant différentes forces d'adhérence et ensemble électrode comprenant cette dernière
WO2021161801A1 (fr) * 2020-02-14 2021-08-19 三洋電機株式会社 Batterie secondaire à électrolyte non aqueux

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JPS628471A (ja) * 1985-07-04 1987-01-16 Matsushita Electric Ind Co Ltd 空気ボタン電池
JPS6341864U (fr) * 1986-09-03 1988-03-18
JPS63184560U (fr) * 1987-05-19 1988-11-28
US5437692A (en) * 1994-11-02 1995-08-01 Dasgupta; Sankar Method for forming an electrode-electrolyte assembly
JPH09500485A (ja) * 1993-11-30 1997-01-14 ベル コミュニケーションズ リサーチ，インコーポレイテッド 電解質活性可能なリチウムイオン再充電可能電池セルおよびその製造方法
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JPS628471A (ja) * 1985-07-04 1987-01-16 Matsushita Electric Ind Co Ltd 空気ボタン電池
JPS6341864U (fr) * 1986-09-03 1988-03-18
JPS63184560U (fr) * 1987-05-19 1988-11-28
JPH09500485A (ja) * 1993-11-30 1997-01-14 ベル コミュニケーションズ リサーチ，インコーポレイテッド 電解質活性可能なリチウムイオン再充電可能電池セルおよびその製造方法
US5437692A (en) * 1994-11-02 1995-08-01 Dasgupta; Sankar Method for forming an electrode-electrolyte assembly
JPH09293518A (ja) * 1996-04-26 1997-11-11 Asahi Chem Ind Co Ltd 薄膜状電解質および該電解質を用いた電池

Cited By (13)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008135289A (ja) * 2006-11-28 2008-06-12 Nissan Motor Co Ltd 二次電池およびその製造方法
JP2011129497A (ja) * 2009-12-15 2011-06-30 Samsung Sdi Co Ltd 二次電池
US8999559B2 (en) 2009-12-15 2015-04-07 Samsung Sdi Co., Ltd. Secondary battery
KR101454996B1 (ko) * 2012-03-07 2014-10-30 닛산 지도우샤 가부시키가이샤 이차 전지
JP2015053118A (ja) * 2013-09-05 2015-03-19 日立マクセル株式会社 リチウムイオン二次電池用セパレータおよびその製造方法、並びにリチウムイオン二次電池およびその製造方法
EP2916373B1 (fr) * 2013-11-04 2019-03-13 LG Chem, Ltd. Procédé de formation de couche adhésive pour batterie secondaire
US10193120B2 (en) 2013-11-04 2019-01-29 Lg Chem, Ltd. Method for forming adhesion layer for secondary battery
JP2016535923A (ja) * 2013-11-04 2016-11-17 エルジー・ケム・リミテッド 二次電池用接着層の形成方法
EP3244475A4 (fr) * 2015-09-02 2019-08-14 LG Chem, Ltd. Membrane de séparation comprenant des parties de revêtement adhésif ayant différentes forces d'adhérence et ensemble électrode comprenant cette dernière
US10476064B2 (en) 2015-09-02 2019-11-12 Lg Chem, Ltd. Separator comprising adhesive coating parts having different tack strengths and electrode assembly comprising the same
JP2018055951A (ja) * 2016-09-28 2018-04-05 日産自動車株式会社 二次電池
JP2018113122A (ja) * 2017-01-10 2018-07-19 日産自動車株式会社 リチウムイオン二次電池の製造方法
WO2021161801A1 (fr) * 2020-02-14 2021-08-19 三洋電機株式会社 Batterie secondaire à électrolyte non aqueux

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CH483049A (fr) 1969-08-29
CH694766A4 (en) 1969-08-29

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