WO2004097971A1 - Batterie au lithium secondaire empilee et sa fabrication - Google Patents

Batterie au lithium secondaire empilee et sa fabrication Download PDF

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Publication number
WO2004097971A1
WO2004097971A1 PCT/KR2004/000961 KR2004000961W WO2004097971A1 WO 2004097971 A1 WO2004097971 A1 WO 2004097971A1 KR 2004000961 W KR2004000961 W KR 2004000961W WO 2004097971 A1 WO2004097971 A1 WO 2004097971A1
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WO
WIPO (PCT)
Prior art keywords
separator
plates
anode
cathode
folding
Prior art date
Application number
PCT/KR2004/000961
Other languages
English (en)
Inventor
Whanjin Roh
Original Assignee
Enerland Co. Ltd.
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 claimed from KR10-2003-0026290A external-priority patent/KR100514215B1/ko
Priority claimed from KR10-2003-0026289A external-priority patent/KR100514214B1/ko
Priority claimed from KR1020030026294A external-priority patent/KR100555848B1/ko
Application filed by Enerland Co. Ltd. filed Critical Enerland Co. Ltd.
Publication of WO2004097971A1 publication Critical patent/WO2004097971A1/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
    • H01M10/04—Construction or manufacture in general
    • H01M10/0413—Large-sized flat cells or batteries for motive or stationary systems with plate-like electrodes
    • 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
    • H01M10/04—Construction or manufacture in general
    • H01M10/045—Cells or batteries with folded plate-like electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0583—Construction or manufacture of accumulators with folded construction elements except wound ones, i.e. folded positive or negative electrodes or separators, e.g. with "Z"-shaped electrodes or separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0082—Organic polymers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0085—Immobilising or gelification of electrolyte
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a lithium secondary battery and its fabrication, more specifically to a stacked lithium secondary battery in which a plurality of cathode plates and a plurality of anode plates, each of which are separated by a separator, are alternatively facing each other and its fabrication.
  • a battery is a device to convert chemical energy of chemicals into electrical energy through electrochemical reaction, and is classified into two categories: a primary battery and a secondary battery.
  • a primary battery a battery that converts chemical energy of chemicals into electrical energy through electrochemical reaction
  • a secondary battery a battery that stores electrical energy.
  • lithium secondary battery is the most important one, because it has the highest voltage and the largest energy density among existing batteries.
  • the lithium secondary battery according to the method is fabricated by successively depositing a grid-type anode current collector (11), a matrix-film type anode (12), a matrix-film type separator (13), a matrix-film type cathode (14) and a grid-type cathode current collector (15), followed by laminating the members to integrate them, and folding the laminated members in a zig-zag fashion. More detailed explanation can be obtained from US 5,460,904.
  • the lithium secondary battery fabricated by the method (“integrated lithium secondary battery”) comprises both the anode and the cathode in an integral form, and it suffers from the disadvantage that damage to the electrodes sometimes occurs in the folding process.
  • KR 309,604 and 336,396 disclose examples in which a plurality of anode plates and a plurality of cathode plates are used.
  • Fig. 9 is a cross sectional view showing an arrangement of a plurality of anode plates and cathode plates on a separator, in accordance with the KR 309,604.
  • the method disclosed in KR 309,604 and 336,396 comprises adhering a plurality of anode plates (22) to one surface of the separator (21) with a predetermined interval (a distance inside which at least one electrode plate can be inserted), adhering a plurality of cathode plates (23) to the other surface of the separator (21) with a predetermined interval (a gap inside which at least one electrode plate can be inserted), and folding the separator in a zig-zag fashion to obtain a lithium secondary battery having a stacked structure in which each of the anode plates (22) and each of the cathode plates (23) are alternatively stacked.
  • Unexplained reference numeral (24) is an adhesive layer.
  • the stacked lithium secondary battery avoids the disadvantage of the above mentioned integrated lithium secondary battery; this method can prevent the damage to the electrode caused by a folding process.
  • the folding process is complicated, and that it is difficult to tightly fasten the separator because folding of the separator is performed in zig-zag fashion.
  • the gap formed between the electrodes and the separator and caused by loose fastening of the separator deteriorates cycle life of an electrochemical cell and charge/discharge characteristics.
  • the probability of the gap formation is higher, which makes it difficult to fabricate a cell having uniform electrical property.
  • KR published Patent No. 2002-93781 by our present inventor disclose a method for fabricating a lithium secondary battery, comprising arranging both of the anode plates and the cathode plates onto one surface of the separator in a predetermined order, and then folding the separator in a fixed one direction rather than in a zig-zag fashion.
  • the method avoids the disadvantages caused by the zig-zag folding, and provides an additional advantage that adhesion of the electrode plates are performed in one direction to facilitate the adhesion of the electrode plates.
  • the method suffers from a possible electrical short by neighboring arrangement of the cathode plate and the anode plate.
  • the method suffers from a requirement of a larger facility and a larger working space caused by larger length of the separator to which the electrode plates are adhered.
  • An object of the present invention is to provide a method for fabricating a stacked lithium secondary battery in which folding is performed in a fixed one-direction rather than in a zig-zag fashion to enhance the charge/discharge characteristics of the cell and a possible electrical short is prevented.
  • Another object of the present invention is to provide a method for fabricating a stacked lithium secondary battery in which the length occupied by electrode plates is minimized such that only small-scaled facility is required for adhesion of the electrode plates.
  • object of the present invention is to provide a method for fabricating a stacked lithium secondary battery in which an adhesion process of electrode plates can be simplified.
  • Fig. 1 is a drawing showing a pre-stacked body in accordance with the present invention, in which Fig. 1(A) and Fig. 1(B) are a cross-sectional view and a top view thereof, respectively.
  • Fig. 2 is a drawing showing a preferred embodiment of the present invention to obtain the pre-stacked body, in which Fig. 2(A) and Fig. 2(B) are a cross-sectional view and a top view thereof, respectively.
  • Fig. 3 is a drawing illustrating the process for fabricating the pre-stacked body using the arrangement of Fig. 2, in which Fig. 3(A) and Fig. 3(B) are respectively a cross-sectional view and a top view showing the arrangement of the electrode plates after folding the portion to which no anode plate is attached, and Fig. 3(C) and Fig. 3(D) are respectively a cross-sectional view and a top view showing the arrangement of the electrode plates after an accompanying attachment of the cathode plates has been carried out.
  • Fig. 4 is a drawing showing another preferred embodiment of the present invention to obtain the pre-stacked body.
  • Fig. 5 is a perspective view of an electrode plate having a tap obtained by coating both surfaces of a current collector with a solution containing an electrode active material, and cutting the coated current collector in a suitable size.
  • Fig. 6A and 6B show the stacked bodies obtained from the successive folding of the pre-stacked bodies in a fixed one-direction.
  • Fig. 7 is a characteristic graph showing cycle life of the battery of Example 2.
  • Fig. 8 is a drawing showing a conventional method for fabricating an integrated lithium secondary battery.
  • Fig. 9 is a cross-sectional view showing an arrangement of a plurality of anode plates and cathode plates onto a separator, in accordance with a prior art of KR 309,604.
  • the method according to the present invention comprises: a) providing a pre-stacked body comprised of a first separator, a plurality of first electrode plates adhered onto upper surface of the first separator in a neighboring manner, a second separator located on the first electrode plates, and a plurality of second electrode plates adhered onto upper surface of the second separator in a neighboring manner; b) successively folding the pre-stacked body in a fixed one direction along folding lines formed between the electrode plates to obtain a stacked body; and c) housing the obtained stacked body within a pouch, followed by injection of an electrolyte solution and packaging.
  • Fig. 1 is a drawing showing a pre-stacked body in accordance with the present invention, in which Fig. 1(A) and Fig. 1(B) are a cross-sectional view and a top view thereof, respectively.
  • a plurality of first electrode plates (100a) and second electrode plates (100b) (hereinafter, totally “100") are adhered onto a first separator (200') and a second separator (200") (hereinafter, totally “200"), respectively.
  • the electrode plates (100) adhered onto the separator (200) are arranged in a neighboring manner.
  • the term "neighboring" should not be understood that there is physical contact between two adjoining plates, but it means that the two adjoining plates can be overlapped each other when one of the two plates is fold along a folding line (300) formed between the two adjoining plates.
  • the electrode plates (100) should be arranged onto the separator (200) to satisfy the requirements that taps (103a) of the first electrode plates (100a) should overlap one another and taps (103b) of the second electrode plates (103b) should be overlap one another, when successively folded along the folding lines (300).
  • the overlapped taps (103a, 103b) are each independently connected to suitable lead lines (for example, nickel and aluminum lead lines, respectively) by an ultrasonic welding.
  • the first electrode plates (100a) are anode plates
  • the second electrode plates (100b) are cathode plates.
  • the first separator (200') and the second separator (200") can exist in a separate form.
  • the separate form of the first separator (200') and the second separator (200") can be obtained from independent attachment of a plurality of the anode plates (100a) and a plurality of the cathode plates (100b) to separated separators (200' and 200").
  • Such a form can simplify the adhesion process of the electrode plates (100).
  • the electrode plate's arrangement of KR 309,604 which is shown in Fig.
  • the first separator (200') and the second separator (200") can exist in a connected form.
  • the first separator (200') and the second separator (200") exist as one sheet.
  • Such a form can be obtained by adhering a plurality of anode plates (100a) to a portion of one surface of a separator (200) in a neighboring manner as shown in Fig. 2(A) or Fig. 2(B), covering the anode plates (100a) with the separator (200) by folding along a folding line (300) the portion to which no electrode plate is adhered (please refer to Fig. 3(A) and Fig.
  • FIG. 3(B) which respectively shows a cross-sectional view and a top view of the folded structure along a folding line (300)), and then adhering a plurality of cathode plates (100b) onto the separator (200) in a neighboring manner and in the same direction with the adhesion direction of the anode plates (100a) (please refer to Fig. 3(C) and 3(D) ).
  • FIG. 4 Another embodiment in which the first separator (200') and the second separator (200") exist in a connected form is shown in Fig. 4. As shown in Fig.
  • a plurality of anode plates (100a) are attached to an upper side of a first row (200') of a separator (200) in a neighboring manner and a plurality of cathode plates (100b) are attached to a lower side of a second row (200') of a separator (200) in a neighboring manner.
  • the first row (200') and the second row (200") of the separator (200) are folded along a central line A- A' to give the pre-stacked body of Fig. 1.
  • the stacked body according to the present invention can exist in a form in which unit members (10a and 10b, totally “10") are successively deposited, which is shown in Fig. 1(C).
  • Adhesion of the electrode plates (100) to the separator (200) is performed by a well known method of the art.
  • a binder can be coated onto the separator (200) to which the electrode plates (100) will be fixed, or it can be coated onto the electrode plates (100) which will be adhered to the separator (200).
  • an ion conductive polymer material selected from the group consisting of polypropylene oxide, polyurethane, polymethylmethacrylate, polybutylmethacrylate, polycyanoacrylate, polyethylene acrylic acid, polyacrylonitrile, polyvinylidene fluoride, polyhexapropylene fluoride, polyethylene oxide, or mixture thereof can be mentioned.
  • the ion conductive polymer material is dissolved into a suitable solvent, and then coated on the separator (200) or the electrode plates (100).
  • a suitable solvent for a solvent to be used, dimethyl carbonate, acetonitrile, tetrahydrofurane, acetone and methyl ethyl ketone can be mentioned.
  • Fig. 5 is a perspective view showing a preferred embodiment of the electrode plate (100) in accordance with the present invention.
  • the electrode plate (100) is prepared by coating both surfaces of a current collector (101) with a solution containing an electrode active material to form a coating layer (102) of the electrode active material, followed by cutting the coated current collector (101) in a suitable size.
  • the electrode plate (100) can be cut into, for example, a rectangular or circular shape.
  • the shape of the electrode plate (100) can be changed depending on the desired form of the final electrochemical cell.
  • the electrode plate (100) having a desired shape can be mass-manufactured by adjusting the template of a cutter or a puncher in a suitable shape.
  • the electrode active material (a cathode active material and an anode active material) coated on the surface of the current collector (101) is not particularly limited.
  • the material that has been used as an electrode active material in the filed of a lithium secondary battery can be widely used.
  • Preferred cathode and anode active materials are exemplified in US Patent Nos. 5,837,015, 5,635,151 and 5,501,548.
  • a lithium transition metal oxide capable of intercalation/deintercalation of lithium ion such as LiCoO 2 , LiMn 2 O 4 , LiNiO 2 or LiMnO 2
  • a cathode active material a material capable of intercalation/deintercalation of lithium ion, such as lithium metal, lithium alloy, carbon and graphite, can be mentioned.
  • the anode active material is carbon or graphite.
  • the cathode active material has a high electrochemical potential during intercalation/deintercalation reaction, while the anode active material has a low electrochemical potential.
  • the cathode or anode material is dispersed into a suitable solvent, coated onto the surface of the current collector (101), and cut into a desired size to form a cathode or anode plate, respectively.
  • the electrode active material may be coated on one surface of the current collector. Preferably, it is coated on both surfaces of the current collector (101), as shown in Fig. 5. Double-sided coating provides an increased discharge capacity per unit volume.
  • preferred examples of the current collector (101) please refer to US Patent Nos. 5,837,015, 5,635,151 and 5,501,548, which are incorporated herein by reference. According to the specific embodiment of the present invention, an aluminum thin plate and a copper thin plate were used as a cathode and anode current collector (101), respectively.
  • the electrode active material is, in general, coated on the surface of the current collector (101) in combination with a current conductive material that increases conductivity of the electrochemical cell and a binder that adheres both the electrode active material and the current conductive material to the current collector (101).
  • a current conductive material that increases conductivity of the electrochemical cell
  • a binder that adheres both the electrode active material and the current conductive material to the current collector (101).
  • the choice of the current conductive material and the binder would be readily accomplished in reference to the electrode active material that is well known to a person of ordinary skill in the art to which the present invention pertains.
  • other additives for example, an antioxidant, a flame retardant, and so on can be optionally used.
  • the number of the anode plates (100a) or the cathode plates (100b) can be suitably selected, regarding the anode active material to be used, the cathode active material to be used, the electrolyte to be used, and the desired discharge capacity of the battery.
  • the number of the anode plates (100a) used is more than that of the cathode plates (100b) by 1.
  • the folding process may be complicated. Therefore, the anode plates are used in a range of 2-100.
  • 3-50, more preferably, 3-20, most preferably 4-15 anode plates are used.
  • Fig. 6 is a cross-sectional view showing stacked bodies obtained from successive folding of the pre-stacked body shown in Fig. 1(A) or 1(B) in a fixed one-direction.
  • the staked bodies comprises a plurality of the anode plates (100a) and the cathode plates (100b) which are facing each other and separated by the separator (200).
  • the anode plates (100a) and the cathode plates (100b) are completely separated by the separator (200) so that the danger of an electrical short is completely removed.
  • the separator (200) is successively folded in a fixed one direction along the folding lines (300), yielding a configuration in which separated double-layered films are successively folded in a fixed one- direction from an inner side to an outer side.
  • the separator (200) does not have a configuration in which a single-layered film is successively folded in a fixed one-direction from an inner side to an outer side (so called "spiral shape") which was generally shown in the conventional stacked battery, but has the configuration in which separated double-layered films are successively folded in a fixed one-direction from an inner side to an outer side, and into spaces formed between the double-layered films, the anode plates (100a) and the cathode plates (100b) are alternatively positioned.
  • present invention has because the double-layered films are successively folded in a
  • the separator (200) is successively folded along folding lines (300) after the portion to which no electrode plate is attached has been folded such that it has a configuration in which a connected double-layered film is successively folded from an inner side to an outer side.
  • the separator (200) has a configuration of because a connected double-layered film is successively folded from an inner side to an outer side. In this configuration, the separator (200) prevents a direct electrical contact of the anode plates (100a) with the cathode plates (100b) and provides pores for ion passage.
  • Preferred examples are porous polyolefin films such as a polyethylene film or a polypropylene film, porous polyvinylidene fluoride films, porous hexapropylene fluoride films and porous polyethylene oxide films, but are not limited thereto.
  • the polyethylene film is being widely used as a separator (200) in the art.
  • the separator (200) may be comprised of two or more porous films.
  • a final battery is produced by housing the stacked body into a pouch of the package, followed by injection of the electrolyte solution and heat sealing of the package under vacuum. At this time, iron or aluminum is in general used as a packaging material.
  • an electrolyte liquid electrolyte, gel polymer electrolyte or solid polymer electrolyte can be used.
  • a liquid electrolyte solution prepared by dissolving lithium salts such as LiCF 3 SO 3 , Li(CF 3 SO 2 ) 2 , LiPF 6 , LiBF 4 , LiClO 4 or LiN(SO 2 C 2 F 5 ) 2 into a polar organic solvent such as ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate, was used.
  • lithium salts such as LiCF 3 SO 3 , Li(CF 3 SO 2 ) 2 , LiPF 6 , LiBF 4 , LiClO 4 or LiN(SO 2 C 2 F 5 ) 2 into a polar organic solvent such as ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate and methyl ethyl carbonate
  • the steps of the method according to the present invention can be continuously performed to produce a lithium secondary battery in a large scale.
  • the adhesion process of the electrode plates and the folding process can be continuously performed after a rolled separator has been rolled out in a suitable speed.
  • the electrode plates are neighboring each other, which decrease both the space required for the adhesion of the plates and the scale of the facility required for the adhesion of the plates.
  • the adhesion processes of the electrode plates are performed in the same direction such that a turning-over process of the separator after either the anode plates or the cathode plates has been adhered to the separator can be omitted.
  • the separator onto which the electrode plates are arranged is folded in a fixed one-direction rather than in a zig-zag fashion such that tight fastening of the separator can be accomplished. And, the total number of the folding is reduced as much as 1/2, compared with the conventional methods, which enhances the performance of the process. From the method according to the present invention, a stacked lithium secondary battery comprising a plurality of anode plates and a plurality of cathode plates which are separated by a separator and facing each other is obtained.
  • the stacked lithium secondary battery comprises a plurality of anode plates, a plurality of cathode plates, a separator separating the anode plates and the cathode plates, and an electrolyte
  • the separator has a configuration in which a double-layered film is successively folded in a fixed one-direction from an inner side to an outer side, the anode plates and the cathode plates are facing each other and alternatively arranged into empty spaces formed between the double-layered film, taps of the anode plates and taps of the cathode plates are each independently overlapping one another, and the electrolyte are charged between the anode plates and the separator and between the cathode plates and the separator.
  • the stacked lithium secondary battery avoids the danger of an electrical short caused by an undesired contact of the cathode plate with the anode plate. Further, because the stacked lithium secondary battery is obtained from a fixed one-directional folding, charge/discharge characteristics are enhanced. Specifically, compared to the lithium secondary battery obtained from a zig-zag folding disclosed in KR 309,604 and 336,396, the lithium secondary battery obtained from a fixed one-directional folding enables to tightly fasten the separator, to enhance charge/discharge characteristics, and to extend the cycle life of the battery.
  • a cathode plate sheet was prepared by the conventional process: a mixture of 100 g of LiCoO 2 powder as a cathode active material, 5g of carbon black as a current conductive material and 5g of polyvinylidene fluoride as a binder was homogeneously mixed, and then 100ml of N- methylpyrrolidone was added to the mixture. The obtained solution was coated onto both sides of a aluminum foil having a thickness of 15 ⁇ which serves as a cathode current collector, dried and then pressed with a roll presser. The thickness of the cathode plate sheet was 150 ⁇ m.
  • anode plate sheet was prepared: lOOg of graphite powder and lOg of polyvinylidene fluoride as a binder was homogeneously mixed, and then 100ml of N- methylpyrrolidone was added to the mixture. The obtained solution was coated onto both sides of a copper foil having a thickness of 15 which serves as an anode current collector, dried and then pressed with a roll presser. The thickness of the cathode plate sheet was 150 ⁇ m.
  • the cathode and anode plate sheets were cut with a puncher such that the cathode and anode plates as shown in Fig. 5 in which each of the cathode and anode plates with dimensions of 3 cm x 4 cm has a tap having dimensions of 0.5 cm x 0.5 cm were obtained.
  • the cathode plates and the anode plates obtained were stored into a cassette.
  • Example 2 Fabrication of a battery from a double-layered pre-stacked body.
  • a polymer solution was prepared by mixing acetonitrile (available from Aldrich) and polyethylene oxide (available from Aldrich, average molecular weight 1,000,000) at a ratio of 100:3 by weight.
  • the rolled porous polyethylene sheet (Tecklon M manufactured by ENTEK, thickness:
  • the projected taps of the cathode plates and the anode plates were led out by nickel and aluminum leads and welded in parallel with an ultrasonic wave, respectively.
  • the stacked body was housed within an aluminum laminating sheet having a pouch to house the stacked body, and an electrolyte solution prepared by dissolving 1.2 mol of LiPF 6 into 3 ml of a mixed solvent of ethylene carbonate and ethylmethyl carbonate (1 : 1 , by volume) was injected into the pouch.
  • Heat-sealing under vacuum produced a stacked lithium secondary battery having a thickness of 38 mm, width of 35 mm and length of 62 mm.
  • Example 3 Fabrication of a battery using the arrangement shown in Fig. 2.
  • the rolled porous polyethylene sheet (TecklonTM manufactured by ENTEK, thickness:
  • the stacked body was housed within an aluminum laminating sheet having a pouch to house the stacked body, and the electrolyte solution prepared by dissolving 1.2 mol of LiPF 6 into 3 ml of a mixed solvent of ethylene carbonate and ethylmethyl carbonate (1 :1, by volume) was injected into the pouch. Heat-sealing under vacuum produced a stacked lithium secondary battery having a thickness of 38 mm, width of 35 mm and length of 62 mm.
  • Example 4 Fabrication of a battery from a double-rowed pre-stacked body.
  • the rolled porous polyethylene sheet (TecklonTM manufactured by ENTEK, thickness: 25 ⁇ m) which has a double-rowed structure and serves as a separator was rolled out and onto upper side of a first row, the polymer solution was coated with a liquid constant delivery apparatus in a thickness of 2 ⁇ m. Thereafter, the anode plates from the cassette were delivered and attached to the upper side of the separator onto which the polymer solution was coated. After the portion to which no anode plate is attached had been folded along the central line(A- A'), the polymer solution was coated onto the folded portion with the liquid constant delivery apparatus and the cathode plates from the cassette were attached in the same direction with that of the anode plates.
  • a stacked body shown in Fig. 6A in which a plurality of the anode plates and the cathode plates separated by a separator are facing each other.
  • the projected taps of the cathode plates and the anode plates were led out by nickel and aluminum leads and welded in parallel with an ultrasonic wave, respectively.
  • the stacked body was housed within an aluminum laminating sheet having a pouch to house the stacked body, and the electrolyte solution prepared by dissolving 1.2 mol of LiPF 6 into 3 ml of a mixed solvent of ethylene carbonate and ethylmethyl carbonate (1 :1 , by volume) was injected into the pouch.
  • Heat-sealing under vacuum produced a stacked lithium secondary battery having a thickness of 38 mm, width of 35 mm and length of 62 mm. Comparative Example 1
  • a plurality of anode plates was adhered onto one side of a separator in which an interval (3.3 cm) was formed between the two anode plates. Thereafter, the separator was turned over and then a plurality of cathode plates was attached onto the opposite side of the separator such that the arrangement shown in Fig. 9 was obtained. Folding was performed in a zig-zag fashion to give a stacked body. The projected taps of the cathode plates and the anode plates were led out by nickel and aluminum leads and welded in parallel with an ultrasonic wave, respectively.
  • the stacked body was housed within an aluminum laminating sheet having a pouch to house the stacked body, and the electrolyte solution prepared by dissolving 1.2 mol of LiPF 6 into 3 ml of a mixed solvent of ethylene carbonate and ethylmethyl carbonate (1 :1, by volume) was injected into the pouch.
  • Heat-sealing under vacuum produced a stacked lithium secondary battery having a thickness of 38 mm, width of 35 mm and length of 62 mm.
  • Table 1 summarizes the results of the Examples and Comparative Example 1.
  • Test 1 Test of Cycle life of batteries Cycle life of the battery of Example 2 was tested and compared with that of Comparative Example 1. The results thereof are shown in Fig 7. As shown in Fig. 7, the lithium secondary battery of the present invention retained 92% or more discharge capacity after more than 150 cycles, while the battery of Comparative Example 1 had a discharge capacity of less than 88% and the tendency of reduction was increasingly high. The batteries of Examples 3 and 4 gave almost the same results with that of Example 2.
  • the method according to the present invention gave the following benefits: firstly, there is no danger of an electrical short caused by an undesired contact of a cathode plate with an anode plate, because the cathode and anode plates are definitively separated by a separator. And, because folding is performed in a fixed one-direction rather than in a zig-zag fashion, the disadvantages caused by a zig-zag folding can be avoid, for example inconvenience of the process, difficulty for tight fastening of a separator which results a gap between the electrode plate and a separator and reduces the cycle life of the battery.
  • the method reduces the scale of an facility required for adhering electrode plates and enables to efficiently utilize a working space, because the anode plates as well as the cathode plates are neighboring one another such that the portion to which the electrode plates are adhered can be reduced as much as 1/2, compared with KR 309,604, KR 336,396 and KR published patent 2002-93781. Further, the number of folding is reduced as much as 1/2, compared with KR 309,604, KR 336,396 and KR published patent 2002-93781, which increases the efficiency of the process.
  • the lithium secondary battery fabricated by the method according to the present invention has highly enhanced charge/discharge characteristics because of stable interface by tight fastening of the separator sandwiched between the anode plate and the cathode plate during successive folding. And, the battery has no danger of an electrical short due to a complete separation between an anode plate and a cathode plate by a separator.

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Secondary Cells (AREA)

Abstract

L'invention concerne un procédé de fabrication d'une batterie au lithium secondaire empilée dans laquelle une pluralité de plaques de cathode et une pluralité de plaques d'anode chacune étant séparée par un séparateur, sont placées face à face par alternance. Ce procédé consiste : a) à prendre un corps pré-empilé comprenant un premier séparateur, une pluralité de premières plaques d'électrode voisines collées sur la surface supérieure du premier séparateur, un deuxième séparateur situé sur les premières plaques d'électrode, et une pluralité de deuxièmes plaques d'électrode voisines collées sur la surface supérieure du deuxième séparateur; b) à plier successivement le corps pré-empilé dans une direction fixe le long de lignes de pliage formées entre les plaques d'électrode afin d'obtenir un corps empilé; et c) à loger le corps empilé obtenu à l'intérieur d'une poche, puis à injecter une solution électrolytique et à conditionner. Ledit procédé simplifie le procédé de pliage par pliage unidirectionnel plutôt que par pliage en zigzag, et réduit l'échelle des installations nécessaires pour le procédé d'adhérence par réduction au minimum de la longueur occupée par les plaques d'électrode. En outre, le séparateur peut être fixé fermement de façon que les caractéristiques de charge/décharge et de cycle de vie de la batterie soient améliorés, en comparaison avec un pliage en zigzag.
PCT/KR2004/000961 2003-04-25 2004-04-26 Batterie au lithium secondaire empilee et sa fabrication WO2004097971A1 (fr)

Applications Claiming Priority (6)

Application Number Priority Date Filing Date Title
KR10-2003-0026290A KR100514215B1 (ko) 2003-04-25 2003-04-25 다열 접착을 이용한 적층형 리튬이차전지의 제조방법
KR10-2003-0026289 2003-04-25
KR10-2003-0026294 2003-04-25
KR10-2003-0026289A KR100514214B1 (ko) 2003-04-25 2003-04-25 분리된 2겹의 격리막을 이용한 적층형 리튬이차전지 및 그제조방법
KR1020030026294A KR100555848B1 (ko) 2003-04-25 2003-04-25 전극판의 한방향 접착이 가능한 적층형 리튬이차전지의제조방법
KR10-2003-0026290 2003-04-25

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EP2808933A4 (fr) * 2012-05-23 2015-07-15 Lg Chemical Ltd Procédé de fabrication d'un ensemble électrode et dispositif électrochimique comprenant l'ensemble électrode
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JP2010278002A (ja) * 2009-05-28 2010-12-09 Samsung Sdi Co Ltd 二次電池用電極組立体及びその製造方法
EP2256853A1 (fr) * 2009-05-28 2010-12-01 Samsung SDI Co., Ltd. Ensemble d'électrode pour batterie et procédé de formation de l'ensemble d'électrode
EP2487747A4 (fr) * 2009-10-07 2015-06-24 Sk Innovation Co Ltd Ensemble d'électrodes pour batterie et procédé de fabrication de celui-ci
JP2013507732A (ja) * 2009-10-07 2013-03-04 エスケー イノベーション カンパニー リミテッド 電池用電極組立体及びその製造方法
CN102576912A (zh) * 2009-10-07 2012-07-11 Sk新技术株式会社 用于电池的电极组件及其制造方法
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US8741469B2 (en) 2009-10-15 2014-06-03 Samsung Sdi Co., Ltd. Electrode assembly with multiple separators wound about a winding center
CN102044657A (zh) * 2009-10-15 2011-05-04 三星Sdi株式会社 电极组件及其制造方法以及具有该电极组件的二次电池
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EP2317594A1 (fr) * 2009-11-02 2011-05-04 Samsung SDI Co., Ltd. Ensemble formant électrode pour batterie secondaire et procédé de fabrication de l'ensemble d'électrode
JP2011096665A (ja) * 2009-11-02 2011-05-12 Samsung Sdi Co Ltd 二次電池用電極組立体及びその製造方法
CN102054955A (zh) * 2009-11-02 2011-05-11 三星Sdi株式会社 二次电池的电极组件及制造该电极组件的方法
FR2976129A1 (fr) * 2011-05-31 2012-12-07 Commissariat Energie Atomique Procede semi-automatique de realisation d'un accumulateur electrochimique li-ion
WO2012163881A1 (fr) * 2011-05-31 2012-12-06 Commissariat à l'énergie atomique et aux énergies alternatives Procede semi-automatique de realisation d'un accumulateur electrochimique li-ion
US9136557B2 (en) 2011-05-31 2015-09-15 Commissariat á l'énergie atomique et aux énergies alternatives Semi-automatic method for manufacturing an electrochemical Li-ion battery
EP2565972A4 (fr) * 2011-06-09 2015-07-22 Lg Chemical Ltd Ensemble électrode et batterie rechargeable au lithium comprenant celui-ci
US9537178B2 (en) 2011-06-09 2017-01-03 Lg Chem, Ltd. Electrode assembly and lithium secondary battery including the same
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US9692027B2 (en) 2011-06-09 2017-06-27 Lg Chem, Ltd. Electrode assembly and lithium secondary battery including the same
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US9893376B2 (en) 2013-09-26 2018-02-13 Lg Chem, Ltd. Methods of preparing electrode assembly and secondary battery
EP2879223A4 (fr) * 2013-09-27 2016-01-06 Lg Chemical Ltd Appareil d'empilement et procédé d'empilement d'unité pour une batterie secondaire
CN105958100A (zh) * 2016-05-29 2016-09-21 合肥国轩高科动力能源有限公司 一种卷绕式叠片电池
US11437651B2 (en) 2016-09-06 2022-09-06 Samsung Sdi Co., Ltd. Stacked electrode assembly and flexible rechargeable battery comprising the same
US12002987B2 (en) 2018-05-18 2024-06-04 Samsung Sdi Co., Ltd. Separator for rechargeable lithium battery and rechargeable lithium battery comprising same
CN110277590A (zh) * 2019-06-28 2019-09-24 蜂巢能源科技有限公司 用于电芯制造的叠片方法和电芯极组制造装备
CN110277590B (zh) * 2019-06-28 2022-04-12 蜂巢能源科技有限公司 用于电芯制造的叠片方法和电芯极组制造装备
WO2023073111A1 (fr) * 2021-10-31 2023-05-04 Körber Technologies Gmbh Procédé et machine de fabrication d'empilement de cellules de l'industrie de production de cellules énergétiques

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