WO2013095038A1 - Ensemble électrode et procédé de fabrication de ce dernier - Google Patents

Ensemble électrode et procédé de fabrication de ce dernier Download PDF

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WO2013095038A1
WO2013095038A1 PCT/KR2012/011258 KR2012011258W WO2013095038A1 WO 2013095038 A1 WO2013095038 A1 WO 2013095038A1 KR 2012011258 W KR2012011258 W KR 2012011258W WO 2013095038 A1 WO2013095038 A1 WO 2013095038A1
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electrode
separator
porous polymer
cells
polymer
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PCT/KR2012/011258
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English (en)
Korean (ko)
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임현철
이병선
서인용
최원길
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주식회사 아모그린텍
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Publication of WO2013095038A1 publication Critical patent/WO2013095038A1/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
    • 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
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • 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
    • H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
    • 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
    • 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
    • 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
    • H01M50/426—Fluorocarbon polymers
    • 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
    • H01M50/431—Inorganic material
    • 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
    • H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
    • 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
    • H01M50/463—Separators, membranes or diaphragms characterised by their shape
    • 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
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/491—Porosity
    • 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
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/494—Tensile strength
    • 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
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/497—Ionic conductivity
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • 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
    • H01M50/403—Manufacturing processes of separators, membranes or diaphragms
    • 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
    • H01M50/429—Natural polymers
    • H01M50/4295—Natural cotton, cellulose or wood
    • 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
    • H01M50/44—Fibrous material
    • 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
    • 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 an electrode assembly and a method of manufacturing the same, in particular, by using an electrospinning method to form and separate a separator consisting of a porous polymer web of ultrafine fibers integrally and continuously on one or both sides of the positive electrode or negative electrode, productivity and safety
  • the present invention relates to an electrode assembly and a method of manufacturing the same, which can be improved.
  • Lithium secondary batteries generate electrical energy by oxidation and reduction reactions when lithium ions are intercalated / deintercalated at the positive and negative electrodes.
  • a lithium secondary battery is prepared by using a material capable of reversibly intercalating / deintercalating lithium ions as an active material of a positive electrode and a negative electrode, and filling an organic electrolyte or a polymer electrolyte between the positive electrode and the negative electrode.
  • a lithium secondary battery is composed of an electrode assembly in which a negative electrode plate and a positive electrode plate are wound or stacked in a predetermined form with a separator (separation membrane) interposed therebetween, and a case in which the electrode assembly and the electrolyte solution are stored.
  • the basic function of the separator of the lithium secondary battery is to prevent the short circuit by separating the positive electrode and the negative electrode, and furthermore, it is important to suck the electrolyte required for the battery reaction and maintain high ion conductivity.
  • an additional function is required to prevent the movement of substances that inhibit battery reaction or to secure safety when an abnormality occurs.
  • Lithium ion secondary batteries with high energy density and large capacity, secondary batteries including lithium ion polymer batteries should have a relatively high operating temperature range, and the temperature increases when they are continuously used in high rate charge / discharge states. Separators are required to have higher heat resistance and thermal stability than those required by ordinary separators. In addition, it should have excellent battery characteristics such as high ion conductivity that can cope with rapid charging and discharging and low temperature.
  • the separator is located between the anode and the cathode of the battery to insulate it, maintains the electrolyte to provide a path for ion conduction, and when the temperature of the battery becomes too high, a part of the separator melts to block pores in order to block the current.
  • the separator should have a low shutdown temperature and a higher short circuit temperature.
  • the electrode part may be contracted at 150 ° C. or more, resulting in a short circuit. Therefore, it is very important to have both the closing function and the heat resistance for high energy density and large sized secondary battery. That is, a separator having excellent heat resistance, low thermal shrinkage, and excellent cycle performance according to high ion conductivity is required.
  • polyolefin-based microporous polymer membranes such as polypropylene and polyethylene or multiple membranes thereof are usually used.
  • the porous membrane layer is in the form of a sheet or a film, there is a drawback that the sheet-like separator shrinks together with the pore blocking of the porous membrane due to heat generation due to internal short circuit or overcharge. Therefore, when the sheet-like separator collapses due to the internal heat generation of the battery, the separator is reduced and the missing part is directly in contact with the positive electrode and the negative electrode, which leads to ignition, rupture, and explosion.
  • the polyolefin separator is immersed in a heat-resistant resin in order to secure sufficient safety at high energy density and size, but the charge and discharge characteristics are reduced because the pore of the polyolefin separator is blocked to limit the movement of lithium ions. Even if the heat resistance is secured, it is far less than the demand for large-capacity batteries such as automobiles.
  • the porosity of the commonly used polyolefin separator is about 40% and the pore size is several tens of nm in size, so there is a limit in ion conductivity for a large capacity battery. .
  • Korean Patent Laid-Open Publication No. 2004-108525 proposes a film-type separator consisting of a composite membrane in which a polymer nanoweb is laminated by electrospinning on a polyolefin-based porous membrane as a strength support.
  • Korean Patent Laid-Open No. 2011-35847 proposes a separator in which inorganic particles are coated on a polyolefin-based porous membrane using a binder.
  • lithium dendrite In the film-like separator, full charge lithium dendrite is formed during overcharging. This is because the film is formed in the excitation space between the negative electrode and the film, and lithium ions that cannot enter the inside of the negative electrode accumulate on the surface of the negative electrode, that is, the excitable space between the negative electrode and the film, and precipitate as a lithium metal phase. When lithium is deposited on the entire surface, the deposited lithium dendrites may penetrate through the separator on the film to contact the positive electrode and the negative electrode, and at the same time, side reaction between lithium metal and the electrolyte proceeds, and the battery ignites due to heat generation and gas generation. There is a problem, exploding.
  • the film-like separator is a polyolefin-based film separator, in addition to the portion damaged by the initial heat generation during internal short circuit, the peripheral film is continuously contracted or melted, and the portion where the film separator burns out becomes wider. Can be generated. That is, when the temperature of the battery suddenly rises due to external heat transfer or the like, there is a problem that the temperature rise of the battery continues for a certain time and the breakage of the separator occurs even though the micropores of the separator are closed.
  • International Publication No. WO 2001/89022 relates to a lithium secondary battery comprising a superfine fibrous porous polymer separator and a method for manufacturing the same, wherein the porous polymer separator melts one or more polymers or dissolves one or more polymers in an organic solvent.
  • a method of forming a porous separator by injecting a molten polymer or a polymer solution obtained by the method into a barrel of an electrospinning machine, and then injecting the molten polymer or a polymer solution through a nozzle onto a substrate to form a porous separator It is.
  • the porous polymer membrane is prepared by the electrospinning of a polymer solution in which at least one polymer is dissolved in an organic solvent to a thickness of 50 ⁇ m, to form a porous polymer membrane between the negative electrode and the positive electrode to produce a lithium secondary battery It is inserted and integrated into lamination.
  • Korean Patent Laid-Open Publication No. 2008-13208 discloses a heat-resistant ultra-fine fibrous separator and a manufacturing method thereof, and a secondary battery using the same.
  • the heat-resistant ultra-fine fibrous separator is manufactured by an electrospinning method and has a melting point of 180 ° C. It consists of ultrafine fibers of a heat resistant polymer resin having no abnormalities or melting points, or ultrafine fibers of a polymer resin capable of swelling in an electrolyte solution together with ultrafine fibers of a heat resistant polymer resin.
  • Patent Publication No. 2008-13208 proposes to contain 1-95% by weight of an inorganic additive such as TiO 2 in order to improve mechanical properties, ion conductivity, and electrochemical properties in the separator.
  • the inorganic additive when the inorganic additive is contained in a large amount of spinning solution, there is a problem in that the spinning is impossible due to the dispersibility, and when it is spun together with the polymer material, the strength of the inorganic additive is lowered because it acts as an impurity in the spun fiber.
  • film separators made of polyolefin-based film separators such as those disclosed in Japanese Patent Application Laid-Open Nos. 2005-209570 and 2004-108525, or nanofiber webs disclosed in Korean Patent Application No. 2008-13208, are separated from electrodes.
  • the assembly productivity is low as the manufacture is made in a state inserted between the positive electrode and the negative electrode after being manufactured in a state.
  • Korean Patent Laid-Open No. 2007-114412 discloses a plurality of penetrations to facilitate the access of the electrolyte to the corresponding portion of the separation film surrounding the side of the electrode assembly. The technique which formed the sphere is proposed.
  • such a stack type or stack-fold type electrode assembly has a low adhesion between the electrode and the separator, resulting in a high interface resistance between the electrode and the separator, and a problem of precipitation of lithium dendrite in the excited space between the cathode and the film separator. Can be.
  • Korean Patent Laid-Open No. 2010-72532 proposes a technique for forming a heat shrink suppressing polymer layer by electrospinning a shutdown polymer layer and a polyethylene terephthalate (PET) layer on an electrode plate.
  • the Patent Publication No. 2010-72532 proposes to integrally form two or more kinds of separators by electrospinning two or more polymers having different characteristics on one side of the electrode plate, thereby forming the separator on the electrode plate.
  • No technique has been proposed for the continuous mass production of integrally formed electrode assemblies.
  • Korean Patent Laid-Open Publication No. 2000-53776 fixes a plurality of electrodes on a surface of a rotating rotor plate, and arranges at least one nozzle for injecting a polymer solution from the top, and applies the voltage to the nozzles.
  • a technique for forming a polymer film on the substrate has been proposed, a technique for inexpensively producing a plurality of continuous electrodes has not been presented.
  • the present invention has been made in view of the problems of the prior art, the object of which is to punch-molded the electrode strip coated with the negative electrode or the positive electrode active material on one side or both sides of the strip-type electrode current collector in a step-by-step manner In-line forming a plurality of unit electrode cells, and subsequently forming a separator consisting of a porous nanofiber web on one side or both sides of the plurality of unit electrode cells, and then sequentially separating the unit electrode cells
  • the present invention provides an electrode assembly capable of continuously producing a plurality of unit electrode cells and a method of manufacturing the same.
  • Another object of the present invention is to continuously mold a plurality of unit electrode cells by punch-molding an electrode strip coated with a negative electrode or a positive electrode active material on one or both surfaces of a strip-type electrode current collector in a step-by-step manner using progressive equipment. It is to provide an electrode assembly that can be produced and a method of manufacturing the same.
  • Yet another object of the present invention is to form a cell assembly by simply stacking a cathode and an anode formed integrally with the separator by forming a cathode or an anode or both sides of the cathode and the anode by an electrospinning method to form a cell, so as to assemble and mass production It is to provide this excellent electrode assembly.
  • Another object of the present invention is to provide an electrode assembly capable of suppressing dendrite formation by electrospinning a polymer film of an inorganic pore directly on the surface of the negative electrode to be in close contact with the negative electrode surface, thereby improving stability.
  • the electrode assembly according to the first aspect of the present invention includes a positive electrode, a negative electrode, and a separator separating the positive electrode and the negative electrode.
  • the separator comprises a first non-porous polymer film layer made of a polymer material swelling in the electrolyte and capable of conducting electrolyte ions; And a porous polymer web layer made of ultra-fine fibrous form of a mixture of heat resistant polymer or heat resistant polymer and swellable polymer and inorganic particles, wherein the first non-porous polymer film layer and the porous polymer web layer are formed on both sides of the cathode and the anode, respectively. It is formed by being separated or laminated on either side of either the positive electrode and the negative electrode.
  • the polymer film of the inorganic pores is directly electrospun onto the surface of the negative electrode to form a close contact with the negative electrode surface, thereby maintaining the conductivity of the lithium ions while eliminating the formation of space between the negative electrode and the film to accumulate lithium ions to accumulate lithium metal.
  • dendrite formation can be suppressed and stability can be improved.
  • the electrode assembly may alternately stack a plurality of anodes sealed by the porous polymer web layer and a plurality of cathodes sealed by the first non-porous polymer film layer.
  • assembling can be performed by simply stacking the negative electrode and the positive electrode in which the separator is integrally formed, the assembly and mass production are excellent, and as a result, in order to form a large-capacity battery used in electric vehicles, etc. Fabrication can be made easily.
  • the positive electrode and the negative electrode may each have a bicell structure in which an electrode active material is formed on both surfaces of an electrode current collector.
  • the present invention is also applicable to the full cell structure in which the electrode active material is formed on one surface of the electrode current collector, respectively.
  • the positive electrode and the negative electrode may each have a separator formed on a plurality of unit electrode cells obtained by continuously blanking the electrode strips formed on both surfaces of the strip type electrode current collector.
  • the plurality of unit electrode cells include at least two connection bridges interconnecting adjacent unit electrode cells to block the flow of the unit electrode cells when forming the separator, and the connection bridge includes a separator after the separator is formed. It is preferable to cut together.
  • the content of the inorganic particles is contained in the range of 10 to 25% by weight based on the polymer in the mixture, the size of the inorganic particles is preferably set to 10 to 100nm, preferably 15 to 25nm range.
  • the film does not maintain the film form, shrinkage occurs, the desired heat resistance characteristics are not obtained, and if it exceeds 25% by weight, the radiation troubles that contaminate the spinning nozzle tip Phenomenon occurs and the solvent volatilization is fast and the film strength decreases.
  • the inorganic particles when the size of the inorganic particles is less than 10nm, the volume is too large and difficult to handle, and when it exceeds 100nm, the phenomenon that the inorganic particles are agglomerated occurs a lot of exposed outside the fiber causes the strength of the fiber is lowered.
  • the inorganic particles preferably have a size smaller than the fiber diameter so as to be included in the nanofibers, and when using a small amount of inorganic particles having a size larger than the fiber diameter, the ion conductivity in a range that does not interfere with the strength and radioactivity of the fiber Can improve.
  • the thickness of the inorganic porous polymer film layer is set in the range of 5 to 14um, respectively, and the thickness of the porous polymer web layer is set in the range of 5 to 50um, preferably 10 to 25um.
  • the inorganic particles are TiO 2 , BaTiO 3 , Li 2 O, LiF, LiOH, Li 3 N, BaO, Na 2 O, Li 2 CO 3 , CaCO 3 , LiAlO 2 , SiO 2 , Al 2 O 3 , SiO, SnO , SnO 2 , PbO 2 , ZnO, P 2 O 5 , CuO, MoO, V 2 O 5 , B 2 O 3 , Si 3 N 4 , CeO 2 , Mn 3 O 4 , Sn 2 P 2 O 7 , Sn 2 At least one selected from B 2 O 5 , Sn 2 BPO 6, and mixtures thereof may be used, and the first non-porous polymer film layer may use any one of PVDF, PEO, PMMA, and TPU.
  • the mixture is composed of a heat-resistant polymer, swelling polymer and inorganic particles, it is preferable that the heat-resistant polymer and swelling polymer is mixed in a weight ratio of 5: 5 to 7: 3 range.
  • a method of manufacturing an electrode assembly comprising: a first step of forming an electrode strip by coating an electrode active material layer on at least one surface of a strip type electrode current collector; A second step of partially separating and forming a plurality of unit electrode cells from the electrode strip by performing sequential first blanking while transferring the electrode strip in a step-by-step manner; A third step of forming a separator on both surfaces while continuously transferring the plurality of unit electrode cells; And a fourth step of completely separating the plurality of unit electrode cells from the electrode strip by performing sequential second blanking while transferring the plurality of unit electrode cells in which the separator is formed in a step-by-step manner. It features.
  • a plurality of unit electrode cells are formed by punch-molding an electrode strip coated with a negative electrode or a positive electrode active material on one or both surfaces of a strip type electrode current collector in a step-by-step manner, and then forming an inorganic porous polymer film layer. After forming a separator consisting of a porous nanofiber web layer on one side or both sides of the plurality of unit electrode cells in succession, the plurality of unit electrode cells in a series in-line (in-line) method to sequentially separate the unit electrode cells Can produce.
  • a plurality of unit electrode cells may be continuously produced by punch-molding an electrode strip coated with a negative electrode or a positive electrode active material on one or both surfaces of a strip type electrode current collector in a step-by-step manner.
  • the plurality of unit electrode cells obtained in accordance with the second step may be formed through at least two horizontal connection bridges of adjacent unit electrode cells to block flow of the unit electrode cells when forming a separator. Punching can be done to interconnect.
  • the plurality of unit electrode cells obtained according to the second step may include a cross bridge disposed between adjacent unit electrode cells and a cross between the cross bridge and adjacent unit electrode cells, respectively, to block flow of the unit electrode cells when forming a separator.
  • the punching molding is performed to interconnect each other through at least two horizontal connection bridges having different connection positions, or the plurality of unit electrode cells obtained according to the second step may block the flow of the unit electrode cells when forming a separator.
  • the cross bridges disposed between the adjacent unit electrode cells and the cross between the cross unit and the adjacent unit electrode cells are connected to each other by at least two horizontal connection bridges having different connection positions and having the same connection position on one side and the other side. Punch molding can be made.
  • a portion where the electrode terminal is to be formed is preferably connected to the electrode strip.
  • the electrode strip may include first and second uncoated regions, each of which is not coated with an electrode active material layer, on both sides, and may be formed in advance to prevent the formation of a separator in the first and second non-coated regions before the third step.
  • the method may further include attaching the masking tape.
  • the electrode strip may include first and second uncoated regions, each of which is not coated with the electrode active material layer, on both sides, and in the fourth step, when the plurality of unit electrode cells are separately separated,
  • the method may further include sequentially forming a plurality of piercing holes at regular intervals in the first and second uncoated regions of the electrode strip prior to the second step to be used to determine the position.
  • the separator is formed of a first inorganic porous polymer film layer made of a polymer material capable of swelling in an electrolyte and conducting electrolyte ions, and the first inorganic porous polymer.
  • the porous polymer web layer may further include a superfine fibrous form of a mixture of a heat resistant polymer or a heat resistant polymer and a swellable polymer and an inorganic particle to cover the film layer.
  • the third step may be performed by electrospinning a first spinning solution in which a heat resistant polymer or a heat resistant polymer and a swellable polymer and inorganic particles are mixed to form a first porous polymer web layer made of ultra-fine fibrous fibers. Forming on the surface of the substrate; And a second porous polymer web layer formed of ultra-fine fibers by electrospinning a second spinning solution comprising a polymer material capable of swelling in an electrolyte solution and conducting electrolyte ions on the first porous polymer web layer, and then forming a second porous polymer web layer. And heat treating the web layer to form a first inorganic porous polymer film layer.
  • a first non-porous polymer film layer made of a polymer material capable of conducting electrolyte ions and swelling in the electrolyte is formed in the unit electrode cell to form a negative electrode, and a heat resistant polymer or a heat resistant polymer and a swellable polymer;
  • a positive electrode may be formed by forming a porous polymer web layer formed of ultra-fine fibrous fibers of a mixture of inorganic particles in the unit electrode cell.
  • a plurality of unit electrode cells are formed by punch-molding an electrode strip coated with a negative electrode or a positive electrode active material on one or both surfaces of the strip-shaped electrode current collector in a step-by-step manner, followed by porous nano After forming a separator consisting of a fibrous web continuously on one side or both sides of the plurality of unit electrode cells, it is possible to continuously produce a plurality of unit electrode cells in an in-line manner to sequentially separate the unit electrode cells. .
  • a plurality of unit electrode cells may be continuously produced by punch-molding an electrode strip coated with a negative electrode or a positive electrode active material on one or both surfaces of a strip type electrode current collector in a step-by-step manner.
  • the assembly can be made by simply stacking the negative electrode and the positive electrode in which the separator is integrally assembled. This is excellent, and as a result it can be easily manufactured in a stack type in a large size in order to configure a large capacity battery used in electric vehicles and the like.
  • the negative electrode is maintained while conduction of lithium ions by swelling the electrolyte and forming a polymer film of inorganic pores made of a polymer material capable of conducting electrolyte ions directly on the surface of the negative electrode to form a close contact with the negative electrode surface.
  • the interfacial resistance between the electrode and the separator is low by forming the polymer web layer or the inorganic porous polymer film layer of the heat-resistant ultra-fine fibers containing the inorganic material in the positive electrode or the negative electrode by the electrospinning method. Can be prevented.
  • a single or multi-layered laminate of the polymer web layer and the inorganic porous polymer film layer is easily manufactured by sequentially forming an anode or a cathode by an electrospinning method.
  • the thermal shrinkage is small, the heat resistance is excellent, the mechanical strength is high, the safety is high, the cycle characteristics are high, and the energy density is high. With high capacity.
  • FIG. 1 is a cross-sectional view showing an electrode assembly according to a first embodiment of the present invention
  • FIG. 2 is a cross-sectional view showing an electrode assembly according to a second embodiment of the present invention.
  • FIG. 3 is a plan view illustrating electrode assemblies according to first and second embodiments of the present invention.
  • FIG. 4 is a plan view showing a cathode in an electrode assembly according to a first embodiment of the present invention
  • 5 and 6 are cross-sectional views taken along line X-X of FIG. 4 and line Y-Y of FIG. 4, respectively.
  • FIG. 7 is a plan view showing a modification of the electrode assembly according to the present invention.
  • FIG. 8 is a process flowchart showing a method of manufacturing a secondary battery according to the present invention.
  • FIG. 9 is a process plan view illustrating a manufacturing process of a unit electrode cell for a negative electrode using a continuous blanking method according to the present invention.
  • FIG. 10 is a cross-sectional view illustrating a unit electrode cell blanking process of FIG. 9; FIG.
  • 11 and 12 are each a plan view illustrating a manufacturing process of a unit electrode cell in which a bridge shape is deformed by a continuous blanking method according to the present invention
  • FIG. 13 is a process plan view for explaining a manufacturing process of a unit electrode cell for a positive electrode used in the first embodiment using a continuous blanking method according to the present invention
  • FIG. 14 is a process plan view for explaining a process for manufacturing a unit electrode cell for a positive electrode used in a second embodiment using a continuous blanking method according to the present invention
  • Example 15 is a photograph showing a sample of Example 1 in which a separator having a two-layer structure is formed on both surfaces of an anode.
  • the structure of the electrode assembly of the secondary battery according to the present invention will be described, and then the unit electrode cell used in the electrode assembly and the manufacturing method of the secondary battery are described.
  • FIG. 1 is a cross-sectional view showing an electrode assembly according to a first embodiment of the present invention
  • FIG. 2 is a cross-sectional view showing an electrode assembly according to a second embodiment of the present invention
  • FIG. 3 is a first and second embodiment of the present invention.
  • 4 is a plan view showing a cathode of the electrode assembly according to the first exemplary embodiment of the present invention.
  • FIGS. 5 and 6 are cross-sectional views taken along line XX of FIG. 4 and line YY of FIG. 4, respectively. .
  • the electrode assembly 10 largely includes a cathode 1 and an anode 2.
  • the negative electrode 1 is disposed to face the positive electrode 2 and includes a pair of negative electrode active material layers 13a and 13b formed on both sides of the negative electrode current collector 11 to form a bicell.
  • the negative electrode 1 may include negative electrode active material layers 13a and 13b formed on one surface of the negative electrode current collector 11 to form a full cell.
  • the positive electrode 2 includes positive electrode active material layers 23a and 23b formed on both surfaces of the positive electrode current collector 21 to form a bicell.
  • the positive electrode 2 may include positive electrode active material layers 23a and 23b formed on one surface of the positive electrode current collector 21 to form a full cell.
  • the cathode active material layers 23a and 23b include a cathode active material capable of reversibly intercalating and deintercalating lithium ions.
  • Representative examples of the cathode active material include LiCoO 2 , LiNiO 2 , LiNiCoO 2 , and LiMnO 2. , LiMn 2 O 4 , V 2 O 5 , V 6 O 13 or LiNi 1-xy Co x M y O 2 (0 ⁇ x ⁇ 1, 0 ⁇ y ⁇ 1, 0 ⁇ x + y ⁇ 1, M is Al Lithium-transition metal oxides such as metals such as Sr, Mg, and La).
  • the negative electrode active material layers 13 and 13a include a negative electrode active material capable of intercalating and deintercalating lithium ions, and the negative electrode active material may be crystalline or amorphous carbon, carbon fiber, or carbon based carbon composite. It may be selected from the group consisting of a negative electrode active material, tin oxide, lithiated thereof, lithium, lithium alloys and mixtures thereof. However, the present invention is not limited to the type of the negative electrode active material.
  • the negative electrode 1 and the positive electrode 2 are prepared by mixing an appropriate amount of an active material, a conductive agent, a binder, and an organic solvent to prepare a slurry, and then, as the negative electrode and the positive electrode current collectors 11 and 21, on both sides of a copper or aluminum sheet or the like. It can be obtained by casting the prepared slurry, drying and rolling.
  • the positive electrode is used by casting a slurry composed of LiCoO 2 , super-P carbon, PVdF as an active material, a conductive agent, a binder on an aluminum foil, and the negative electrode as MCMB (mesocarbon microbeads), super-P carbon, PVdF
  • MCMB mesocarbon microbeads
  • the positive electrode and the negative electrode after the slurry is cast, it is preferable to perform roll pressing in order to increase the adhesion between the particles and the metal foil.
  • Separation membranes 3a and 3b having a multi-layer structure on the surface of the negative electrode 1 are formed of a polymer that swells in an electrolyte solution to cover the negative electrode active material layers 13a and 13b, respectively, and is made of a polymer capable of conducting electrolyte ions.
  • the separators 3a and 3b may be porous polymer webs obtained by electrospinning swellable polymers instead of the first inorganic porous polymer film layers 31a and 31b.
  • the porous polymer web may be formed by dissolving a swellable polymer in a solvent to form a spinning solution, and then electrospinning the spinning solution on a negative electrode active material layer to form a porous polymer web made of ultra-fine fibers.
  • PVDF is obtained by calendering the porous polymer web at a temperature lower than the melting point of PVDF).
  • the first inorganic porous polymer film layers 31a and 31b formed to cover the negative electrode active material layers 13a and 13b in the negative electrode 1 are swelled in the electrolyte and polymers capable of conducting electrolyte ions, for example, Polyvinylidene fluoride (PVDF), Poly-Ethylen Oxide (PEO), polymethyl methacrylate (PMMA), or Thermoplastic Poly Urethane (TPU) can be used.
  • the first inorganic porous polymer film layers 31a and 31b form a spinning solution by dissolving the polymer in a solvent, and then electrospinning the spinning solution on the anode active material layer to form a porous polymer web made of ultra-fine fibrous fibers. By heat-treating or calendering the porous polymer web at a temperature lower than the melting point of the polymer, the polymer film layers 31a and 31b of the inorganic pores are obtained.
  • the heat treatment temperature can be performed at a temperature slightly lower than the melting point of the polymer because the solvent remains in the polymer web, and also to form the inorganic porous film while preventing the polymer web from completely melting by the heat treatment. to be.
  • the inorganic porous polymer film layers 31a and 31b made of a material capable of conducting electrolyte swelling and swelling in the electrolyte are directly electrospun onto the surfaces of the negative electrode active material layers 13a and 13b, respectively.
  • swelling is performed by the electrolyte solution while maintaining conduction of lithium ions while blocking the formation of space between the negative electrode active material layers 13a and 13b and the film to prevent lithium ions from accumulating and depositing into lithium metal. can do.
  • dendrite formation can be suppressed on the surface of the cathode 1 and safety can be improved.
  • the inorganic-containing porous polymer web layers 33a and 33b formed on the first inorganic porous film layers 31a and 31b dissolve a mixture of a heat resistant polymer or a heat resistant polymer and a swellable polymer and inorganic particles in a solvent to form a spinning solution. Thereafter, the spinning solution is electrospun on the first non-porous polymer film layers 31a and 31b to form a porous polymer web made of ultra-fine fibrous, and the obtained porous polymer web is formed by calendering at a temperature below the melting point of the polymer. .
  • the inorganic particles are Al 2 O 3 , TiO 2 , BaTiO 3 , Li 2 O, LiF, LiOH, Li 3 N, BaO, Na 2 O, Li 2 CO 3 , CaCO 3 , LiAlO 2 , SiO 2 , SiO, SnO , SnO 2 , PbO 2 , ZnO, P 2 O 5 , CuO, MoO, V 2 O 5 , B 2 O 3 , Si 3 N 4 , CeO 2 , Mn 3 O 4 , Sn 2 P 2 O 7 , Sn 2 B 2 O 5, Sn 2 BPO 6 and can be used at least one member selected from among those of the respective mixtures.
  • the content of the inorganic particles is preferably contained in the range of 10 to 25% by weight based on the total mixture when the size of the inorganic particles is between 10 and 100 nm. . More preferably, the inorganic particles are contained in the range of 10 to 20% by weight, and the size is in the range of 15 to 25 nm.
  • the heat resistant polymer and the swellable polymer are preferably mixed in a weight ratio of 5: 5 to 7: 3, and more preferably 6: 4.
  • the swellable polymer is added as a binder to help bond between the fibers.
  • the mixing ratio of the heat resistant polymer and the swellable polymer is less than 5: 5 by weight, the heat resistance is poor, and thus the high temperature characteristics are not obtained.
  • the mixing ratio is greater than 7: 3 by weight, the strength is decreased and radiation trouble occurs.
  • the heat resistant polymer resin usable in the present invention is a resin that can be dissolved in an organic solvent for electrospinning and has a melting point of 180 ° C. or higher, for example, polyacrylonitrile (PAN), polyamide, polyimide, polyamideimide, Aromatic polyesters such as poly (meth-phenylene isophthalamide), polysulfones, polyetherketones, polyethylene terephthalates, polytrimethylene terephthalates, polyethylene naphthalates, and the like, polytetrafluoroethylene, polydiphenoxyphosphazenes Polyphosphazenes such as poly ⁇ bis [2- (2-methoxyethoxy) phosphazene], polyurethane copolymers including polyurethanes and polyetherurethanes, cellulose acetates, cellulose acetate butyrates, cellulose acetate pros Cypionate and the like can be used.
  • PAN polyacrylonitrile
  • Polyamide polyimide
  • the swellable polymer resin usable in the present invention is a resin that swells in an electrolyte and can be formed into ultrafine fibers by electrospinning.
  • PVDF polyvinylidene fluoride
  • poly (vinylidene fluoride-co-hexa) Fluoropropylene) perfuluropolymer
  • poly (oxymethylene-oligo- Oxyethylene) polyoxides including polyethylene oxide and polypropylene oxide
  • polyvinylacetate poly (vinylpyrrolidone-vinylacetate)
  • polystyrene and polystyrene acrylonitrile copolymers polyacrylonitrile methyl methacrylate copolymers
  • Polyacrylic containing Casting reel can be given to the copolymer, polymethyl me
  • the separators 3a and 3b having a multi-layer structure are formed on the surface of the cathode 1.
  • the separators 3a and 3b may be formed on the surface of the anode 2 instead of the cathode 1.
  • the inorganic-containing porous polymer web layers 33: 33a and 33b are first formed on the surface of the anode 2, and the first inorganic porous polymer film layers 31: 31a and 31b are formed of the porous polymer web layer 33. It is formed on the surfaces of 33a and 33b to be in close contact with the cathode 1 during assembly.
  • the two-layer structure separation membranes 3a and 3b are formed on either the negative electrode 1 or the positive electrode 2, but the separation membrane 3 is the first as shown in the second embodiment shown in FIG. It is composed of the inorganic porous polymer film layers 31: 31a and 31b and the inorganic-containing porous polymer web layers 33: 33a and 33b, and may be formed separately from the cathode 1 and the anode 2.
  • the first non-porous polymer film layers 31: 31a and 31b are formed on the negative electrode 1 to cover the negative electrode active material layers 13a and 13b, and the inorganic material to cover the positive electrode active material layers 23a and 23b. It is also possible that the porous polymeric web layers 33: 33a and 33b are formed on the anode 2.
  • the second inorganic porous polymer film layer on the surfaces of the inorganic material-containing porous polymeric web layers 33a and 33b of the anode 2 in the same manner as the first inorganic porous polymer film layers 31a and 31b.
  • the first inorganic porous polymer film layers 31a and 31b and the second inorganic porous polymer film layer are bonded to each other.
  • the first inorganic porous polymer film layers 31a and 31b and the inorganic material-containing porous polymer web layers 33a and 33b may be integrally formed on the negative electrode 2 or may be formed separately from the negative electrode 1 and the positive electrode 2.
  • the thickness of the inorganic-containing porous polymer web layer (33a, 33b) is set in the range of 5 to 50um
  • the thickness of the first inorganic porous polymer film layer (31a, 31b) is preferably set in the range of 5 to 14um.
  • the function of the separator is that the inorganic-containing porous polymer web layers 33a and 33b have a higher porosity than the first inorganic-porous polymer film layers 31a and 31b, and thus the first inorganic rather than the inorganic-containing porous polymer web layers 33a and 33b.
  • the thickness of the first inorganic porous polymer film layers 31a and 31b is preferably adjusted in consideration of the ion conductivity and energy density of the film layer.
  • the first inorganic porous polymer film layers 31a and 31b and the inorganic porous polymer web layers 33a and 33b serving as separators may be formed of the cathode 1 or the anode 2 as shown in FIG. 1. It encloses with a sealing structure, or surrounds the cathode 1 and the anode 2 simultaneously with the sealing structure like FIG.
  • the electrode assemblies 10 and 10a of the present invention may form a unit cell by simply stacking the cathode 1 and the anode 2, for example, a large capacity for an electric vehicle.
  • the present invention has a high assembly productivity compared to the prior art that goes through the process of folding a plurality of bi-cell with a separate membrane film.
  • the negative electrode 1 and the positive electrode 2 are provided with the negative electrode and positive electrode terminals 11a and 21a which protrude a part of the negative electrode and the positive electrode current collectors 11 and 21.
  • the electrode assemblies 10 and 10a of the present invention are laminated and assembled with a plurality of negative electrodes 1 and positive electrodes 2, the negative electrode terminal 11a of the negative electrode 1 and the positive electrode terminal 21a of the positive electrode 2 as shown in FIG. 3.
  • the protruding negative electrode terminal 11a and positive electrode terminal 21a are welded and integrated together.
  • the protruding negative terminal 11a and the positive terminal 21a form terminals so as to have a space therebetween. It is preferable in terms of safety.
  • porous polymer web layers 33a and 33b contain an inorganic material and thus retain their shape without shrinking or melting even when heat-treated at 500 ° C.
  • the electrode of the present invention maintains a constant voltage between 5V and 6V and a battery temperature of less than 100 ° C by continuously consuming overcharge current by causing a very small short-circuit rather than a hard short during overcharge. Overcharge stability can also be improved.
  • the secondary battery of the present invention includes an electrolyte in an electrode assembly including a separator.
  • the electrolyte according to the present invention includes a non-aqueous organic solvent, and the non-aqueous organic solvent may be carbonate, ester, ether or ketone.
  • the present invention is not limited to the type of nonaqueous organic solvent.
  • the electrolyte according to the present invention includes a lithium salt
  • the lithium salt acts as a source of lithium ions in the battery to enable the operation of the basic lithium battery, for example LiPF 6 , LiBF 4 , LiSbF 6 , LiAsF 6 , LiClO 4 , LiCF 3 SO 3 , LiN (CF 3 SO 2 ) 2 , LiN (C 2 F 5 SO 2 ) 2 , LiAlO 4 , LiAlCl 4 , LiN (C x F 2x + 1 SO 2 ) (C y F 2x + 1 SO 2 ), wherein x and y are natural water and LiSO 3 CF 3 and include one or more or mixtures thereof.
  • the positive electrode 2 and the negative electrode 1 are combined to form the electrode assemblies 10, 10a, and then placed in an aluminum or aluminum alloy can or similar container, and then the opening is closed with a cap assembly. An electrolyte is injected to prepare a lithium secondary battery.
  • both surfaces of the slurry including the negative electrode active materials 13a and 13b are cast and roll pressed so as to form a bicell on the negative electrode current collector 11 in the form of a strip to form a negative electrode strip 12 (S11). Winding to reel.
  • the negative electrode active materials 13a and 13b formed in the negative electrode current collector 11 are formed with piercing holes 12a and 12b in a subsequent step, and also the negative electrode terminal 11a as shown in FIG. 9. It is desirable to exclude the constant width of both sides.
  • the pierce mold 16 is used to transfer the cathode strip 12 wound on the reel by step-by-step or continuously by using a pair of feed rollers 14a and 14b driven by a step motor or a servo motor.
  • a plurality of piercing holes (12a, 12b) are formed on both sides at regular intervals.
  • the plurality of piercing holes 12a and 12b may be used to determine the position of each electrode cell when the plurality of unit electrode cells continuously connected are separately separated in the secondary process.
  • the piercing holes 12a and 12b are generally holes used to transfer materials, the battery electrode material is thin and cannot be transferred using the piercing holes 12a and 12b, but is a strip material used as a current collector. It may be applied depending on the type or thickness of the.
  • masking tapes 15a and 15b are attached to the portion where the negative electrode terminal 11a is formed so as to omit the uncoated portion forming process, thereby forming a separator.
  • the pierce holes 12a and 12b may be used for the use of the negative electrode strip 12 as both sides of the negative electrode current collector 11 increase in tensile strength.
  • the feeding of the negative electrode strip 12 may be carried by motor rotation through the rollers 14a and 14b, and the protrusions are formed on the rotating rollers by using the piercing holes 12a and 12b. Is fixed to the piercing holes (12a, 12b) as a gear can be transferred according to the rotation of the rotary roller.
  • the piercing hole 12a is formed together with the negative electrode terminal 11a or the positive electrode terminal 21a after a separator is formed for the unit electrode cells 20a-20c and the unit electrode cells 30a-30d in a subsequent process.
  • the negative electrode At least two piercing holes 12a located outside the terminal 11a or the positive terminal 21a can be used when the negative electrode 1 and the positive electrode 2 are stacked.
  • blanking i.e., punching
  • the blanking equipment 18 is performed using the blanking equipment 18 in a subsequent process so that the plurality of unit electrode cells 20a-20c are removed from the negative electrode strip 12. Partially separated leaving the part to be formed (S12).
  • the step-by-step method transfer of the negative electrode strip 12 it transfers by 1 unit process length, and performs blanking for each unit process 1ST, 2ST, and between adjacent unit electrode cells 20a-20c.
  • a space S between the unit electrode cells 20a-20c and the masking tapes 15a, 15b, respectively a rectangle having a constant area, such as a rectangle or a square, of each unit electrode cell 20a-20c. Punch to have shape.
  • the setting between the start part and the end part of the unit processes 1ST and 2ST can be modified differently.
  • the corners of the quadrangle are rounded so as to easily form a sealing structure when the separators are formed on both sides of the unit electrode cells 20a-20c in a subsequent process.
  • the unit electrode cells 20a-20c form a separator using, for example, an air electrospinning (AES) method in a subsequent process
  • the polymer spinning solution is applied at a high pressure through a plurality of spinning nozzles.
  • each spinning nozzle is placed in an environment in which air is injected.
  • the unit electrode cells 20a-20c need to block the flow of the unit electrode cells 20a-20c in order to maintain the position in a high air pressure environment while the electrospinning of the polymer spinning solution for forming the membrane is performed at a desired portion. have.
  • the separate electrode unit cells 20a-20c are also transported along the collector of the electrospinning equipment and are continuously transported to be wound on the winder for subsequent processing. It is highly desirable in terms of productivity that they are interconnected together.
  • connection bridges 24a-24c are interconnected between the upper, middle and lower sides of the unit electrode cells 20a-20c in consideration of these points.
  • punching molding is performed such that a portion forming the negative electrode terminal 11a is connected to the negative electrode strip 12.
  • the negative electrode active materials 13a and 13b coated on the bridges 24a to 24c may be exposed to the cut surface when the unit electrode cells 20a to 20c are separately separated, even though both surfaces are coated with a separator in a subsequent process. Fine pieces of the negative electrode active materials 13a and 13b coated from the portions of the bridges 24a to 24c may be separated and exposed. If necessary, the negative electrode active materials 13a and 13b coated on the connection bridges 24a to 24c may be removed.
  • the bridges 24a-24c of the unit electrode cells 20a-20c shown in FIG. 9 have a left / right symmetrical structure, but may be modified into an asymmetrical structure as shown in FIGS. 11 and 12.
  • the positions of the horizontal bridges 25a-25d disposed on one side and the other side of the unit electrode cells 20a and 20b are set at different levels, and the unit electrodes are also disposed on the lower side as necessary.
  • a pair of vertical bridges 25e and 25f may be further formed to prevent the flow of the cells 20a and 20b.
  • the crossing bridge 12c disposed between the unit electrode cells 20a and 20b serves to hold the horizontal bridges 25a to 25d.
  • horizontal bridges 26a-26d and 27a-27d disposed on one side and the other side of unit electrode cells 20a and 20b adjacent to each other are set at different levels.
  • the crossing bridge 12c disposed between the unit electrode cells 20a and 20b serves to hold four adjacent horizontal bridges 26c, 26d, 27a, and 27b.
  • the positions of the horizontal bridges 25a-25d are set to different levels, or the positions of the horizontal bridges 26a-26d; 27a-27d of adjacent unit electrode cells 20a, 20b are mutually different.
  • safety can be achieved by preventing short-circuit between bridges from occurring when stacked in a multilayer structure.
  • the separator 3 is formed on both sides of the unit electrode cells 20a and 20b, and the separator 3 is formed on both sides of the unit electrode cell for the anode in the same manner, so that the cathode 1 and the anode ( In the case of alternately stacking 2), it is preferable from the viewpoint of long-term reliability that the bridge portions exposed when separating the unit electrode cells 20a-20c are laminated in the same position.
  • the bridge structure for interconnecting the unit electrode cells 20a-20c may be any type that minimizes the bridge exposed portion when the individual electrodes are separated while holding the flow of the unit electrode cells 20a-20c during the separator formation process. Modifications may also be made to the structure.
  • the unit electrode cells 20a-20c punched out from the negative electrode strip 12 are then wined together with the paper 26a supplied from a paper roll 26 for easy transport to the spinning chamber for forming the separator. It is wound in a roll form by a further 28.
  • the paper 26a wound together with the unit electrode cells 20a-20c prevents damage from occurring by contacting the bipolar anode active materials 13a and 13b with each other, and also serves to maintain a wound state. .
  • anode unit electrode cells 30a-30d in the same or similar manner as the method and structure of the cathode unit electrode cells 20a-20c.
  • a cathode current collector having a strip shape
  • the positive electrode active materials 23a and 23b are double-sided formed (coated) on 21 to form a positive electrode strip 22, and blanking (ie, punching molding) while transferring in a step-by-step manner as shown in FIG.
  • the positive electrode unit electrodes 30a-30d are completely separated from the positive electrode strip 22.
  • each of the unit electrode cells 30a-30d exposes the positive electrode current collector 21, in which the positive electrode active materials 23a and 23b are not coated, to form the positive electrode terminal 21a.
  • the positive electrode unit electrodes 30a-30d may be prepared.
  • the cathode strips 22 are formed by forming (coating) the cathode active materials 23a and 23b on both sides of the cathode current collector 21 having a strip shape, and as shown in FIG. 14, a one-step process in a step-by-step manner. After the length transfer, blanking (ie, punching) is performed for each unit process 1ST and 2ST to partially separate the unit electrode cells 30a-30c for the anode from the cathode strip 22. .
  • connection bridges 24a-24c between the unit electrode cells 30a-30c to block the flow of the unit electrode cells 30a-30c in a subsequent process for forming the separator.
  • the upper side, the middle side, and the lower side are interconnected, and the upper part or the lower side of the unit electrode cells (30a-30c) is formed so that the part forming the positive terminal (21a) is connected to the positive electrode strip (22).
  • the first non-porous polymer film layer 31a is formed to cover the negative electrode active material layer 13a.
  • the first non-porous polymer film layer 31a swells in an electrolyte and forms a spinning solution by dissolving a polymer capable of conducting electrolyte ions, for example, PVDF in a solvent, and forming the spinning solution in the negative electrode active material layer.
  • the electrospinning (13a) to form a porous polymer web made of ultra-fine fibrous the first non-porous polymer film layer 31a by heat-treating or calendering the porous polymer web at a temperature slightly lower than the melting point of the polymer To form.
  • the heat treatment temperature may be performed at a temperature slightly lower than the melting point of the polymer because the solvent remains in the polymer web, and the inorganic web film is formed while preventing the polymer web from completely melting by the heat treatment. For sake.
  • the radiation method applied to the present invention is a general electrospinning, air electrospinning (AES: Air-Electrospinning), electrospray (electrospray), electrobrown spinning (centrifugal electrospinning), flash Any one of flash-electrospinning can be used.
  • AES Air-Electrospinning
  • electrospray electrospray
  • electrobrown spinning electrobrown spinning
  • flash Any one of flash-electrospinning can be used.
  • the spinning solution is, for example, using a multi-hole spinning pack in which a plurality of spinning nozzles are disposed in the traveling direction and the perpendicular direction of the collector, air electrospinning in which air is sprayed for each spinning nozzle ( AES: It is preferable to use the air-electrospinning (AES) method.
  • AES air-electrospinning
  • the first non-porous polymer film layer 31 b is formed to cover the negative electrode active material layer 13 b by the same method as the method of forming the first non-porous polymer film layer 31 a.
  • an inorganic-containing porous polymer web layer 33a, 33b is formed on the first non-porous polymer film layers 31a and 31b, which is made of a ultrafine fibrous form of a mixture of a heat resistant polymer or a heat resistant polymer and a swellable polymer and inorganic particles.
  • the inorganic-containing porous polymer web layers 33a and 33b first dissolve a heat-resistant polymer or a mixture of a heat-resistant polymer and / or a swellable polymer and an inorganic particle in a solvent to form a spinning solution, and the spinning solution is a first inorganic polymer film.
  • Electrospinning, preferably air electrospinning, on the layer 31a forms a first porous polymeric web made of ultrafine fibrous form.
  • first and second porous polymer webs are calendered to obtain inorganic-containing porous polymer web layers 33a and 33b.
  • the method of forming the separation membranes 3a and 3b of the two-layer structure may be formed in a different order than the above method.
  • the first non-porous polymer film layer 31a and the inorganic-containing porous polymer web layer 33a are sequentially formed to cover the negative electrode active material layer 13a, and then cover the negative electrode active material layer 13b on the opposite side. It is also possible to sequentially form the first non-porous polymer film layer 31b and the inorganic-containing porous polymer web layer 33b.
  • the unit electrode cells 20a-20c are separated from each other with respect to the plurality of cathode unit electrode cells 20a-20c surrounded by two-layer separators 3a and 3b.
  • Cutting lines 40 are set in the separation membranes 3a and 3b extending from the unit electrode cells 20a to 20c while being transferred, and punching is performed to separate the negative electrode terminal 11a (S14).
  • the masking tape 15a attached to the portion of the negative electrode terminal 11a is removed to obtain the negative electrode 1 shown in FIGS. 1 and 7.
  • At least two piercing holes 12a located outside the cathode terminal 11a are punched out when the unit electrode cells 20a-20c are punched out from the cathode strip 12 to the cathode terminal 11a. Cut together and separate.
  • the positive electrode 21 is disposed on the outside of the positive electrode terminal 21a. At least two piercing holes 12a located are cut together and separated.
  • the at least two piercing holes 12a can be used to easily align the plurality of cathodes 1 and 2. .
  • the portions of the piercing holes 12a outside the cathode terminal 11a and the anode terminal 21a are cut off, and the plurality of cathode terminals 11a and the anode
  • the positive electrode terminal 21a of each is welded together and integrated, and is connected with the external terminal of the negative electrode 1 and the positive electrode 2, respectively.
  • the electrode assembly 10 when manufacturing the electrode assembly 10 according to the second embodiment shown in Figure 2, for the negative electrode (1) to cover the first inorganic porous polymer film layer (31a) to cover the negative electrode active material layer (13a) Next, the first non-porous polymer film layer 31 b is formed to cover the negative electrode active material layer 13 b (S13).
  • the positive electrode 2 is formed by dissolving a mixture of a heat resistant polymer or a heat resistant polymer and / or a swellable polymer and an inorganic particle in a solvent so as to cover the cathode active material layer 23a to form a spinning solution, and electrospinning the spinning solution. After forming the first porous polymer web, the same spinning solution is electrospun so as to cover the positive electrode active material layer 23b to form the second porous polymer web. Thereafter, the first and second porous polymer webs are calendered to form inorganic-containing porous polymer web layers 33a and 33b (S13).
  • the first non-porous polymer film layers 31: 31a and 31b are formed on the cathode 1 to cover the anode active material layers 13a and 13b, and then the separator 3 having a single layer structure on both sides thereof is formed.
  • the cutting line 40 is set in the separator 3 region extended from the unit electrode cells 20a-20c while transferring in a step-by-step manner to the plurality of cathode unit electrode cells 20a-20c surrounded by the Further, punching molding for separating the negative electrode terminal 11a is performed (S14). Thereafter, the masking tape 15a attached to the portion of the negative electrode terminal 11a is removed to obtain the negative electrode 1 shown in FIG.
  • the two-layered separator 3 is formed on both sides, respectively.
  • Cutting lines are set in the separator 3 region extending from the unit electrode cells 30a-30c while transferring in a step-by-step manner to a plurality of positive electrode unit electrodes 30a-30c surrounded by Punch molding for separating up to the positive terminal 21a is performed (S14). Thereafter, the masking tape attached to the portion of the positive electrode terminal 21a is removed to obtain the positive electrode 2 shown in FIG.
  • the first inorganic porous polymer film layers 31a and 31b and the inorganic-containing porous polymer web layer 33a and the inorganic portion 11a and the positive electrode terminal 21a are formed in a masking process using masking tape. 33b), it is possible to exclude a separate uncoated region forming process.
  • the case assembly process may be performed (S16).
  • the electrolyte is injected (S17) to manufacture a secondary battery.
  • the negative electrode 1 and / or the positive electrode 2 have a structure sealed by a separator, the negative electrode 1 and the positive electrode 2 are simply opposed to each other and pressed to assemble the electrode assembly 10. 10a), ie, a unit cell can be formed, and thus, it has a high assembly productivity compared to the prior art, which undergoes a process of folding a plurality of bi-cells into separate separator films.
  • the inorganic porous polymer film layers 31a and 31b made of a material capable of conducting electrolyte swelling with swelling in the electrolyte are formed in close contact with the surfaces of the negative electrode active material layers 13a and 13b. While swelling is performed, the formation of spaces between the negative electrode active material layers 13a and 13b and the film can be prevented while the conduction of lithium ions is maintained, thereby preventing lithium ions from accumulating and depositing into lithium metal. As a result, the negative electrode 1 Dendrite formation can be suppressed on the surface), and safety can be improved.
  • a second porous polymer web layer was continuously formed on the first porous polymer web layer. That is, 22 g of polyvinylidene fluoride (PVDF) was added to a solvent in which 62.4 g of dimethylacetamide (DMAc) and 15.6 g of acetone were mixed and stirred at 80 ° C. to prepare a spinning solution, and then the spinning solution was added to a solution tank. Injected and the polymer solution was discharged at 22.5ul / min / hole.
  • PVDF polyvinylidene fluoride
  • the temperature and humidity of the spinning section is the same as the section for making the first porous polymer web layer, by applying a 100KV voltage to the spinning nozzle pack using another high voltage generator and applying an air pressure of 0.2Mpa to the spinning nozzle pack.
  • the second porous polymer web layer was formed on the first porous polymer web layer.
  • the first and second porous polymer web layers having a two-layer structure having different melting points are then subjected to a second porous polymer web layer made of PVDF onto a film of inorganic pores by heat treatment passing through an IR lamp at 120 ° C. Transformed.
  • the opposite side of the positive electrode was continuously formed in the same manner as above to form the first and second porous polymer web layers and the second porous polymer web layer was transformed onto the film of the inorganic pores.
  • the anodes having the first porous polymer web layer and the inorganic porous polymer film layer having a two-layer structure formed on both sides are moved to a calendering device, calendered using a heating / pressing roll, and to remove residual solvent or water.
  • a hot air dryer with a temperature of 100 ° C. was passed.
  • the final product obtained by passing through a hot air dryer is a polymer nanofiber is directly radiated on both sides of the anode electrode, and a separator having a two-layer structure is coated in a sealed form, and the separator on one side is formed of a first porous polymer.
  • the thickness of the web layer was 13um
  • the thickness of the non-porous film layer was formed to 7um
  • one side was made of 20um
  • the total thickness of the membrane on both sides was formed to 40um.
  • Example 1 a large capacity secondary battery can be easily configured by alternately stacking a plurality of positive electrodes sealed in a sealing form on both sides with a plurality of negative electrodes.
  • a second porous polymer web layer was continuously formed on the first porous polymer web layer. That is, 22 g of polyvinylidene fluoride (PVDF) was added to a solvent in which 62.4 g of dimethylacetamide (DMAc) and 15.6 g of acetone were mixed and stirred at 80 ° C. to prepare a spinning solution, and then the spinning solution was added to a solution tank. Injected and the polymer solution was discharged at 22.5ul / min / hole.
  • PVDF polyvinylidene fluoride
  • the temperature and humidity of the spinning section is the same as the section for making the first porous polymer web layer, by applying a 100KV voltage to the spinning nozzle pack using another high voltage generator and applying an air pressure of 0.2Mpa to the spinning nozzle pack. 2 a porous polymeric web layer was formed.
  • the first and second porous polymer web layers having a two-layer structure having different melting points are then subjected to a second porous polymer web layer made of PVDF onto a film of inorganic pores by heat treatment passing through an IR lamp at 120 ° C. Transformed.
  • the first porous polymer web layer and the inorganic porous polymer film layer having a two-layer structure are moved to a calendering device, calendered using a heating / pressing roll, and the temperature is increased at a rate of 20 m / sec to remove residual solvent or water.
  • a separator having a two-layer structure was obtained by passing a hot air dryer at 100 ° C.
  • the thickness of the first porous polymer web layer was 5 ⁇ m
  • the thickness of the inorganic porous film layer was 10 ⁇ m
  • the total thickness was 15 ⁇ m.
  • a charge / discharge test of a 2Ah battery to which the separator of Example 2 was applied was performed.
  • Comparative Examples 1 to 3 the thickness of the first porous polymer web layer was maintained at 5 ⁇ m as in Example 2, and the thickness of the inorganic porous film layer was 4 ⁇ m (Comparative Example 1), 15 um (Comparative Example 2), and 25 um (Comparative Example). Except that set differently to 3) other conditions were applied in the same manner as in Example 2 to prepare a membrane having a two-layer structure.
  • Example 2 When the thickness of the inorganic porous film layer of Example 2 was 10 um, a characteristic graph was obtained in which charge and discharge characteristics were periodically repeated.
  • a separator made of heat-resistant nanofibers by air electrospinning AES
  • 6.6 g of polyacrylonitrile (PAN) and 4.4 g of polyvinylidene fluoride (PVDF) were used as a dimethyl solvent.
  • 89 g of acetamide (DMAc) was added and stirred at 80 ° C. to prepare a mixed spinning solution consisting of a heat resistant polymer and a swellable polymer.
  • 20 wt% of Al 2 O 3 inorganic particles having a thickness of 20 nm are added to the prepared spinning solution.
  • the obtained single-layer porous polymer web layer is moved to a calender equipment, calendered using a heating / pressing roll, and passed through a hot air dryer having a temperature of 100 ° C. at a speed of 20 m / sec to remove residual solvent or water.
  • the separator of Example 3 having a thickness of 20 nm was obtained.
  • Comparative Example 4 Comparative Example 5, Examples 4 to 5 and Comparative Example 6 is 20nm Al 2 O with respect to the whole containing the PAN and PVdF mixed polymer and inorganic particles in the spinning solution in Example 3 as shown in Table 1 below 3
  • the remaining conditions were prepared in the same manner as in Example 3. It was confirmed whether the shrinkage after the heat test of °C °C, and also to investigate the shrinkage rate, tensile strength, the radiation stability of the spinning solution according to the heat resistance test of the separator are listed in Table 1.
  • the separator having the most desirable properties was found to be Example 5 (15 wt%).
  • the heat-resistant separation membrane of the present invention suppresses the heat diffusion phenomenon because the web is made of nanofibers even if the instantaneous temperature rises to 400 ⁇ 500 °C as lithium ions move rapidly through the pinhole, and the heat-resistant polymer and Al in the nanofibers It was shown to have excellent thermal stability by containing 2 O 3 inorganic material.
  • the unit electrode cell constituting the cathode and the anode has been described using a bicell structure as an example, but it is also possible to have a full cell structure.
  • the shape of the unit electrode cell has been described with an example of a square, of course, it is also possible to have a circular or other shape.
  • the separator is formed separately from the cathode and the anode, or illustrated as being formed in a multilayer structure on either side, it is also possible to be formed separately on the cathode and the anode and formed in a multilayer structure on either side. In this case, as the cathode and the anode are pressed and assembled, the separator may form a multilayer structure, thereby easily implementing a shutdown function.
  • the first non-porous polymer film layer and the inorganic-containing porous polymer web layer as a separator may be composed of another polymer web layer.
  • the present invention provides a secondary battery including a lithium ion secondary battery, a lithium ion polymer battery, a supercapacitor that requires high heat resistance and thermal stability such as a hybrid battery, a hybrid electric vehicle, an electric vehicle, and a fuel cell vehicle, as well as secondary batteries of various portable electronic devices. It can be applied to the separator used for this.

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Abstract

La présente invention se rapporte à un ensemble électrode et à un procédé de fabrication de ce dernier, une membrane de séparation qui est composée d'un tissu polymère poreux constitué de fibres ultra fines, étant formée d'un seul tenant et de manière continue avec une surface des deux surfaces d'une électrode positive ou d'une électrode négative par électrofilage afin de séparer les électrodes, ce qui permet d'améliorer la productivité et la sécurité. Le procédé de fabrication d'un ensemble électrode selon la présente invention comprend : une première étape consistant à recouvrir au moins un côté d'un collecteur de courant d'électrode en forme de bande avec une couche de matériau actif d'électrode de sorte à former une bande d'électrode ; une deuxième étape consistant à transférer par étapes la bande d'électrode et à effectuer un premier découpage séquentiel à la presse pour séparer partiellement les multiples cellules d'électrode individuelles de la bande d'électrode ; une troisième étape consistant à former des membranes de séparation au niveau des deux côtés de chaque cellule d'électrode individuelle tout en transférant de manière continue les multiples cellules d'électrode individuelles ; et une quatrième étape consistant à transférer par étapes les multiples cellules d'électrode individuelles qui présentent des membranes de séparation formées sur ces dernières et à effectuer un second découpage séquentiel à la presse de sorte à séparer complètement les multiples cellules d'électrode individuelles de la bande d'électrode.
PCT/KR2012/011258 2011-12-21 2012-12-21 Ensemble électrode et procédé de fabrication de ce dernier WO2013095038A1 (fr)

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CN112615061A (zh) * 2021-01-12 2021-04-06 深圳市格林晟科技有限公司 一种电芯的制备方法及堆叠装置
CN117117086A (zh) * 2023-10-24 2023-11-24 宁德时代新能源科技股份有限公司 一种正极片、电池单体、电池及用电装置

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CN117117086A (zh) * 2023-10-24 2023-11-24 宁德时代新能源科技股份有限公司 一种正极片、电池单体、电池及用电装置
CN117117086B (zh) * 2023-10-24 2024-03-29 宁德时代新能源科技股份有限公司 一种正极片、电池单体、电池及用电装置

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