Classifications

• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/05—Accumulators with non-aqueous electrolyte
  • H01M10/052—Li-accumulators
  • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/05—Accumulators with non-aqueous electrolyte
  • H01M10/058—Construction or manufacture
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M10/00—Secondary cells; Manufacture thereof
  • H01M10/05—Accumulators with non-aqueous electrolyte
  • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
  • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
  • H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/04—Processes of manufacture in general
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M4/00—Electrodes
  • H01M4/02—Electrodes composed of, or comprising, active material
  • H01M4/36—Selection of substances as active materials, active masses, active liquids
  • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
  • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
  • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
  • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
  • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
• • H—ELECTRICITY
  • H01—ELECTRIC ELEMENTS
  • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
  • H01M6/00—Primary cells; Manufacture thereof
  • H01M6/14—Cells with non-aqueous electrolyte
  • H01M6/18—Cells with non-aqueous electrolyte with solid electrolyte
  • H01M6/188—Processes of manufacture
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
  • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
  • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
  • Y02E60/10—Energy storage using batteries
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
  • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
  • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
  • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

• the present invention relates to a method for producing a lithium secondary battery using an ion conductive polymer, and more specifically, to a negative electrode using a carbon material capable of electrochemically removing / desorbing lithium as an active material,
• a lithium ion battery comprising a positive electrode using a chalcogenide containing lithium as an active material, and a polymer electrolyte layer in which a non-aqueous electrolyte is held by an ion conductive polymer matrix disposed between the positive electrode and the negative electrode.
• the present invention relates to a method for manufacturing a secondary battery. Background art
• Lithium secondary batteries have a much higher theoretical energy density than other batteries and can be made smaller and lighter, and are being actively researched and developed as power sources for portable electronic devices.
• power consumption is increasing rapidly along with the rapid performance improvement, and accordingly, the power supply is required to have good discharge characteristics even at higher loads.
• non-aqueous electrolytes and conventional polymer separators have been used in the form of batteries following conventional batteries using non-aqueous electrolytes (called lithium-ion batteries).
• lithium-ion batteries non-aqueous electrolytes
• Studies are being made on batteries using polymer electrolytes that also have the functions described above. Lithium secondary batteries using polymer electrolytes have received great attention because of their great advantages, such as being small, lightweight, and thin, and having no electrolyte leakage.
• non-aqueous electrolyte batteries such as lithium secondary batteries are commercially available.
• the electrolyte a solution in which an electrolyte salt is dissolved in an organic solvent is generally used.However, this non-aqueous electrolyte is liable to leak out of parts, elute and volatilize electrode materials, etc. Problems such as reliability and the scattering of electrolyte during the sealing process were problems.
• a lithium secondary battery that uses a macroscopic solid polymer electrolyte is being developed to solve this problem.
• a non-aqueous electrolyte generally a solution in which a lithium salt is dissolved in a non-protonic polar solvent
• a liquid porous ion-conducting polymer matrix
• ion conductive polymer It was difficult to completely control the leakage of non-aqueous electrolyte in various environments using this material.
• graphite material can theoretically incorporate lithium into its crystal lattice at a ratio of one lithium atom to six carbon atoms, and therefore has a high capacity per unit weight and unit volume. Carbon material.
• the potential for lithium insertion and desorption is flat, chemically stable, and greatly contributes to battery cycle stability.
• Graphite-based carbon materials as described above can achieve a discharge capacity close to the theoretical capacity in a non-aqueous electrolyte mainly composed of ethylene carbonate (EC), but because of their high crystallinity, decomposition of the non-aqueous electrolyte is There is still the problem of causing the problem.
• EC ethylene carbonate
• PC propylene carbonate
• a solvent for non-aqueous electrolytes has a wide potential window, a low freezing point (–70 ° C), or a high chemical stability.
• a graphite-based carbon material is used as the negative electrode active material, the decomposition reaction of PC occurs remarkably, and only 10% of PC is present in the electrolytic solution.
• the fact that a negative electrode made of a material cannot be charged or discharged means that J. Electrochem. Soc., Vol. 144, 174 (1
• the viscosity of the ion-conductive polymer precursor before polymerization is somewhat higher than that of the non-aqueous electrolyte. Uniform permeation into the interior.Permeation is considered to be insufficient, and when prototypes of batteries using several types of ion-conducting polymers are actually manufactured, the original positive and negative electrode active materials are possessed. A phenomenon in which the charge / discharge capacity could not be sufficiently exhibited was observed. Therefore, it was concluded that uniform penetration and permeation of the ion-conductive polymer into the inside of the electrode was indispensable for improving various battery characteristics.
• the viscosity of the ion-conductive polymer precursor before polymerization is somewhat higher than that of the non-aqueous electrolyte, so that if it permeates into the separator base material and is poorly penetrated, the ion conductivity becomes higher. This leads to bias, resulting in a decrease in the ionic conductivity of the ion-conductive polymer itself, which has a significant effect on battery characteristics.
• An object of the present invention is to solve the above problems.
• the present invention provides a negative electrode having an active material layer of a carbon material capable of electrochemically inserting / desorbing lithium; a positive electrode having an active material layer of a chalcogenide compound containing lithium; and
• the present invention relates to a method for manufacturing a lithium secondary battery including a polymer electrolyte in which a non-aqueous electrolyte is held in a prepared ion-conductive polymer matrix.
• the present invention provides an ion-conductive polymer precursor / non-aqueous electrolyte mixed solution for impregnating the inside of an electrode with a polymer-electrolyte layer formed on an electrode.
• the ion-conducting polymer precursor / non-aqueous electrolyte mixture has a concentration lower than that of the ion-conducting polymer precursor, so that the ion-conducting polymer seeps and penetrates into the electrode. It is based on the finding that it is significantly improved.
• the first method according to the present invention comprises the following steps.
• the active material is a carbon material capable of electrochemically introducing and desorbing lithium. Preparing a negative electrode and a positive electrode using a chalcogenide containing lithium as an active material;
• step B only the non-aqueous electrolyte solution containing no precursor of the ion-conductive polymer is allowed to penetrate into the interior of each electrode. It was found that some of the conductive polymer precursors migrated into the electrode by diffusion and could achieve the same purpose. Therefore, the second method according to the present invention is the same as the first method except that a non-aqueous electrolyte containing no ion-conductive polymer precursor is used in Step B.
• a subsequent non-aqueous electrolyte containing no or a low percentage of the precursor of the ion-conducting polymer matrix is penetrated into the electrode and, if present, into the separator substrate.
• the penetration of the non-aqueous electrolyte containing the on-conducting polymer matrix precursor into the electrode and the separator substrate is improved, and as a result, the matrix is formed by polymerization of the precursor.
• the interfacial resistance between the electrode and the polymer electrolyte layer is reduced, and the discharge characteristics under high load and the charge / discharge cycle characteristics can be improved.
• a uniform A conductive polymer gel is formed, and it is possible to obtain stable battery performance without bias in ionic conductivity and current distribution.
• FIG. 1 is a graph showing the discharge capacities at different current values of the batteries of Examples 1 and 2 as compared with the battery of Comparative Example 1.
• FIG. 2 shows a discharge capacity carp at a constant current discharge of 10 mA of the batteries of the present invention according to Examples 1 and 2 compared to the battery of Comparative Example 1;
• FIG. 3 is a graph showing the results of a charge / discharge cycle test of the batteries of the present invention according to Examples 1 and 2, as compared with the battery of Comparative Example 1.
• the battery of the present invention can be manufactured by forming an ion-conductive polymer layer on each of a previously prepared negative electrode and positive electrode and superposing both layers, but is not limited thereto.
• the positive electrode and the negative electrode are basically formed by forming respective active material layers in which the positive and negative electrode active materials are fixed with a binder, on a metal foil serving as a current collector.
• a metal foil serving as a current collector examples include aluminum, stainless steel, titanium, copper, nickel, and the like. Considering electrochemical stability, extensibility, and economy, aluminum foil is used for the positive electrode. Copper foil is mainly used for the negative electrode.
• the form of the positive and negative electrode current collectors is mainly a metal foil.
• the form of the current collector may be a mesh, an expanded metal, a lath body, a porous body in addition to the metal foil.
• a resin film coated with an electron conductive material may be used, but the present invention is not limited to this.
• the material include graphite particles having amorphous carbon adhered to the surface.
• graphite particles are immersed in coal-based heavy oil such as tar or pitch, or petroleum-based heavy oil such as heavy oil, pulled up, and heated to a temperature higher than the carbonization temperature to decompose the heavy oil. It can be obtained by grinding the carbon material as needed.
• Such treatment significantly suppresses the decomposition reaction of the nonaqueous electrolyte and lithium salt that occurs at the negative electrode during charging, thereby improving the charge / discharge cycle life and preventing the generation of gas due to the decomposition reaction. It becomes possible.
• pores related to the specific surface area measured by the BET method are closed by the adhesion of carbon derived from heavy oil or the like, and the specific surface area is 5 m 2.
• Z g or less preferably in the range of 1 to 5 m 2 Zg. If the specific surface area is too large, the contact area with the polymer-electrolyte becomes large, which is not preferable because side reactions easily occur.
• Lia (A) b (B) c 02 (where A is one of the transition metal elements) Species or two or more elements, where B is a non-metallic or semi-metallic element from Groups IIIB, IVB and VB of the periodic table, an alkaline earth metal, or a metallic element such as Zn, Cu, or Ti A, b, and c are 0 ⁇ a ⁇ l.15, 0.85 ⁇ b + c ⁇ 1.30, 0 and c, respectively. It is desirable to select from at least one of the composite oxide having a layered structure or the composite oxide having a spinel structure represented by.
• a typical composite oxide is L i C o 0 2, L i N i 0 2, L i C ox N i! -x 02 (0 ⁇ ⁇ 1)
• a carbonaceous material is used as the negative electrode active material, even if a voltage change (approximately 1 VV s. Li / Li +) occurs due to charging and discharging of the carbonaceous material itself, a sufficiently practical operating voltage is obtained.
• the Li ion required for the battery charge / discharge reaction can be reduced before assembling the battery, for example, Li Co 0 2 , Li Ni 0 2 It has the benefits already included in the form.
• the binder is selected from thermoplastic resins that are chemically stable and soluble in suitable solvents but not affected by non-aqueous electrolytes.
• thermoplastic resins are known, but for example, polyvinylidene fluoride (PVDF), which is selectively soluble in N-methyl-2-pyrrolidone (NMP), is preferably used.
• PVDF polyvinylidene fluoride
• NMP N-methyl-2-pyrrolidone
• thermoplastic resins examples include acrylonitrile, methacrylonitrile, vinyl fluoride, chloroprene, vinylpyridine and its derivatives, vinylidene chloride, ethylene, propylene, cyclic gen (for example, polymers and copolymers such as cyclopentadiene and 1,3-cyclohexadiene are included. A binder-resin dispersion may be used instead of the solution.
• the electrode is made by kneading the active material and, if necessary, the conductive material with a binder resin solution to make a paste, applying this to a uniform thickness on a metal foil using a suitable coater, and drying. It is produced by post-pressing.
• the binder ratio in the active material layer should be kept to the minimum necessary. Generally, 1 to 15% by weight is sufficient. When used, the amount of the conductive material is generally 2 to 15% by weight of the active material layer.
• Each polymer monoelectrolyte layer is formed integrally with the active material layer of each electrode thus manufactured.
• These layers are obtained by impregnating or holding a non-aqueous electrolyte containing a lithium salt in an ion-conductive polymer matrix.
• Such layers are macroscopically solid, but microscopically, the salt solution forms a continuous phase and has a higher ionic conductivity than the solid polymer electrolyte without solvent.
• This layer is formed by polymerizing a monomer of a matrix polymer with a lithium salt-containing nonaqueous electrolyte by thermal polymerization, photopolymerization, or the like.
• One monomer component that can be used for this purpose must include polyether segments and be polyfunctional with respect to the polymerization site so that the polymer forms a three-dimensional crosslinked gel structure.
• a typical such monomer is a polyether polyol in which the terminal hydroxy groups are esterified with acrylic acid or methacrylic acid (collectively referred to as "(meth) acrylic acid”).
• polyether polyols are based on polyhydric alcohols such as ethylene glycol, glycerin, trimethylolpropane, etc., with ethylene oxide (EO) alone or with EO and propylene oxide. It is obtained by addition polymerization of oxide (P 0).
• the polyfunctional polyetherpoly (meth) acrylate can be copolymerized alone or in combination with the monofunctional polyetherpoly (meth) acrylate.
• Typical polyfunctional and monofunctional polymers can be represented by the following general formula: CH 2
• R 2 and R a are a hydrogen atom or a methyl group
• R 4 0-A. CC CH 2 (R 4 is a lower alkyl group, R 5 is a hydrogen atom or a methyl group, A 5 has at least three ethylene oxide units (E ⁇ ), and optionally has a propylene oxide unit (P ⁇ ).
• the non-aqueous electrolyte is a solution in which a lithium salt is dissolved in a non-protonic polar organic solvent.
• a lithium salt as a solute, L i C 1 0 4, L i BF 4, L i A s F 6, L i ⁇ F 6, L i I, L i B r, L i CF a S 03, Li CF 3 C 0 2 , Li NC (S 0 2 CF 3 ) 2 , Li N (COCF 3 ) 2 , Li C (S 0 2 CF 3 ) 3 , Li SCN and combinations thereof including.
• Non-limiting examples of the organic solvent include cyclic carbonates such as ethylene carbonate and propylene carbonate, and chain carbonates such as dimethyl carbonate, getyl carbonate, and methyl ethyl carbonate.
• Lactones such as arbutyrolactone; esters such as methyl propionate and ethyl ethyl propionate; ethers such as tetrahydrofuran and its derivatives, 1,3-dioxane, 1,2-dimethoxetane and methyldiglyme; Nitritols such as acetonitrile and benzonitrile; dioxolane and its derivatives; sulfolane and its derivatives; and mixtures thereof.
• an optimal system can be selected for the organic solvent of the non-aqueous electrolyte used in the step B and the step C according to each purpose and property.
• the non-aqueous electrolyte in the process B seeps into the electrode and the inside.
• Z To facilitate penetration, the viscosity of propylene carbonate (PC), 7- Petrolactone (GBL), ethyl methyl carbonate (EMC), dimethyl carbonate (DMC), getyl carbonate (DEC), or a mixture thereof is preferred.
• PC and GBL are preferred to suppress the volatilization of these organic solvents during battery fabrication.
• the non-aqueous electrolyte used in step C is mainly composed of EC and mixed with other solvents selected from PC, GBL, EMC, DEC and DMC in order to suppress side reactions with the graphite-based carbon material.
• the system is preferred.
• a non-aqueous electrolyte obtained by dissolving 3 to 35% by weight of a lithium salt in the above mixed solvent having EC of 2 to 50% by weight, preferably 2 to 35% by weight has a high ion conductivity even at a low temperature. It is preferable because it can be obtained.
• other systems may be preferred depending on the properties of the graphite-based carbon material.
• the mixing ratio of the monomer and the lithium salt-containing non-aqueous electrolyte is sufficient for the non-aqueous electrolyte to form a continuous phase in the formed gel polymer electrolyte, but the electrolyte is separated over time. It must not be too much to seep out. This can generally be achieved by setting the weight ratio of the monomer Z electrolyte in the range of 30/70 to 2/98, preferably in the range of 20/80 to 2Z98.
• the separator substrate is a microporous membrane of a polymer which is chemically stable in a non-aqueous electrolyte such as polypropylene, polyethylene or polyester, or a sheet (paper, nonwoven fabric, etc.) of these polymer fibers. And that these substrates air permeability is l ⁇ 5 0 0 sec / cm 3 , a polymer electrolyte substrate: 9 in a weight ratio of polymer one electrolyte 1: 9-5 0: it can be maintained at 5 0 The ratio of But mechanical strength and ionic conduction It is preferred to get the right balance with the degree.
• step C When forming a polymer electrolyte layer integrated with an electrode without using a separator base material, permeate a non-aqueous electrolyte containing no monomer in the B step in each of the positive and negative electrodes. Then, in step C, a nonaqueous electrolyte containing a monomer is applied thereon, and after polymerization, the positive electrode and the negative electrode may be bonded together with the polymer electrolyte inside.
• the base material is overlaid on one of the electrodes, the non-aqueous electrolyte is penetrated into the inside of the electrode and the base material simultaneously in step B, and then the non-aqueous electrolyte
• the solution is applied and polymerized to form a polymer-electrolyte layer integrated with the substrate and the electrode.
• the battery can be completed by bonding this to the other electrode on which the polymer electrolyte layer integrated by the same method as above is formed. This method is preferable because it is simple and can surely form a polymer electrolyte integrated with the electrode and the separator base material when used.
• the ratio of the monomer is lower than that of the mixture of the monomer and the non-aqueous electrolyte used in the step C
• Monomer Use non-aqueous electrolyte. Even in this case, as in the case of using a non-aqueous electrolytic solution containing no monomer in step B, the penetration and penetration of the ion-conducting polymer into the separator can be improved when used inside the electrode and when used. .
• a mixture containing a monomer in a ratio of about half the monomer / nonaqueous electrolyte mixture used in the step C can be used.
• a mixture of an ion-conductive polymer precursor (monomer) and a non-aqueous electrolyte containing a lithium salt may be treated with a peroxide or azo-based initiator in the case of thermal polymerization, and photopolymerized (ultraviolet curing In the case of), photopolymerization starts Agents such as 22-dimethoxy-2-phenylacetophenone (DM-II), ⁇ : hydroxyketone, metallocene, bisacylphosphinoxide and the like.
• the amount of the polymerization initiator may be up to several% of the monomer, for example, up to 1%.
• Polymerization can be performed by thermal polymerization or photopolymerization as described above.
• Photopolymerization ultraviolet curing
• UV curing which can cure the monomer / non-aqueous electrolyte mixture in a gel at room temperature in a short time, is preferred.
• Li BF 4 is used as a solvent mixture of propylene carbonate (PC), acetylbutyrolactone (GBL) and ethyl methyl carbonate (EMC) in a volume ratio of 40:20:40. Dissolve to the concentration of O mol Z l o
• the nonwoven fabric and the negative electrode having undergone such a process were irradiated with ultraviolet light having a wavelength of 365 m and an intensity of 30 mWX cm 2 for 3 minutes to form a gel polymer electrolyte integrated with the negative electrode and the nonwoven fabric. Its thickness was 20 m.
• the above non-aqueous electrolyte for process B was permeated into the positive electrode, and then the mixture for CI was poured into the positive electrode.
• the positive electrode having undergone such a process was irradiated with ultraviolet light having a wavelength of 365 nm and an intensity of 30 mW cm 2 for 3 minutes to form a gel-like polymer electrolyte layer integrated with the positive electrode. Its thickness was 10 zm.
• the anode and cathode integrated with the polymer electrolyte layer obtained above The battery was completed by laminating with the lima electrolyte layer inside. Its total thickness was 190 m.
• the battery was replaced by the same operation as in Example 1 except that the nonaqueous electrolyte to be penetrated into each electrode in step B of Example 1 was changed to the following mixed solution of ion conductive polymer Z and nonaqueous electrolyte. Produced. Its total thickness was 190 m.
• the polymerization solution of Example 1 was cast into the negative electrode of Example 1 by casting.
• the wavelength 3 6 5 nm, and the irradiation intensity 3 O m W / cm 3 min 2 UV to form a gel-like polymer one electrolyte layer integrated with the positive electrode. Its thickness was 10 m.
• the battery was completed by laminating with the electrolyte layer inside. Its total thickness was 190 m.
• Example 1 The batteries of Example 1, Example 2 and Comparative Example 1 produced by the above method were charged at a constant current of 2.3 mA until the battery voltage reached 4.IV, and after reaching the IV, the constant voltage was reached. The battery was charged for 12 hours at, and discharged at constant currents of 2.3, 5, 10 mA and 20 mA until the battery voltage reached 2.75 A.
• FIG. 1 shows the results of discharging at each current value under the above conditions.
• FIG. 2 shows the discharge curves when the batteries of Example 1, Example 2 and Comparative Example 1 were each discharged at a constant current of 10 mA.
• the batteries of Example 1 and Example 2 had a smaller voltage drop immediately after discharge and a higher average discharge voltage than the battery of Comparative Example 1. You can see that it is. These results are due to the improved permeation and penetration of the ion conductive polymer into the inside of the positive electrode, the negative electrode and the separator substrate, and as a result, the positive electrode, the negative electrode and the polymer electrolyte This suggests that the interfacial resistance between and has been reduced. Further, the batteries of Example 1, Example 2 and Comparative Example 1 were charged at a constant current of 2.3 mA until the battery voltage reached 4. IV, and after reaching IV, the pre-charge time was 12 at a constant voltage. Figure 3 shows the results of a charge-discharge cycle test in which the battery was charged for 2 hours and discharged at a constant current of 2.3 mA until the battery voltage reached 2.75 V.
• the batteries of Example 1 and Example 2 had better charge / discharge cycle characteristics than the battery of Comparative Example 1. This is because, as described above, the penetration and penetration of the ion conductive polymer into the inside of the positive electrode, the negative electrode, and the separator base material have been improved, and the electrochemical reaction can be uniformly performed over the electrode details. It is considered that stable charge-discharge cycle characteristics have been obtained.

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