WO2004049475A1 - Composition d'agregation pour electrode d'une batterie electrolytique non aqueuse, melange electrolytique, electrode et batterie utilisant cette composition - Google Patents

Composition d'agregation pour electrode d'une batterie electrolytique non aqueuse, melange electrolytique, electrode et batterie utilisant cette composition Download PDF

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Publication number
WO2004049475A1
WO2004049475A1 PCT/JP2003/014903 JP0314903W WO2004049475A1 WO 2004049475 A1 WO2004049475 A1 WO 2004049475A1 JP 0314903 W JP0314903 W JP 0314903W WO 2004049475 A1 WO2004049475 A1 WO 2004049475A1
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WO
WIPO (PCT)
Prior art keywords
electrode
polymer
battery
negative electrode
vinylidene fluoride
Prior art date
Application number
PCT/JP2003/014903
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English (en)
Japanese (ja)
Inventor
Mitsuyasu Sakuma
Nobuo Ahiko
Tomoaki Kawakami
Takumi Katsurao
Original Assignee
Kureha Chemical Industry Company, Limited
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.)
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Publication date
Application filed by Kureha Chemical Industry Company, Limited filed Critical Kureha Chemical Industry Company, Limited
Priority to JP2004555003A priority Critical patent/JP4851092B2/ja
Priority to AU2003284631A priority patent/AU2003284631A1/en
Publication of WO2004049475A1 publication Critical patent/WO2004049475A1/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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • H01M4/622—Binders being polymers
    • H01M4/623—Binders being polymers fluorinated polymers
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/621—Binders
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • Non-aqueous electrolyte battery electrode binder composition and electrode mixture using the same are non-aqueous electrolyte battery electrode binder composition and electrode mixture using the same,
  • the present invention relates to an electrode binder used in the production of a nonaqueous electrolyte battery, particularly a lithium ion battery, an electrode mixture using the same, an electrode, and a nonaqueous electrolyte battery using the same.
  • Non-aqueous rechargeable batteries using lithium as batteries that can obtain more energy with a small volume and weight are used as power sources for small electronic devices mainly used in homes such as mobile phones, personal computers, and video camcorders. Has been used.
  • the electrode structure for a lithium-ion battery is used in a state where an active material and a conductive agent are held on a current collector by a binder.
  • a lithium composite oxide is used as a positive electrode active material
  • a carbon-based material is used as a negative electrode active material
  • a carbon-based material is used as a negative electrode active material.
  • a vinylidene fluoride polymer is mainly used as a binder for binding the active materials.
  • Japanese Patent Application Laid-Open No. 11-329443 exemplifies a mixture of a vinylidene fluoride-based polymer and a cellulose-based polymer having no functional group. It was not considered at all.
  • the main problem of the present invention is to maintain the required high capacity of a non-aqueous electrolyte battery while improving its performance stability and safety in the event of an internal short circuit.
  • An object of the present invention is to provide a binder composition for an electrode, and an electrode and a non-aqueous electrolyte battery using the same.
  • a positive electrode and / or a negative electrode of a nonaqueous electrolyte battery including a positive electrode capable of inserting and extracting lithium and a negative electrode.
  • a binder composition used as a binder of the above comprising at least a functional group-containing vinylidene fluoride polymer and a polar polymer having a hydroxyl group and / or a carbonyl group in the molecule. It is intended to provide a binder composition for a non-aqueous electrolyte battery electrode characterized by the following.
  • the present invention provides an electrode mixture containing the binder composition and an electrode active material, an electrode having a layer of the electrode mixture on a current collector, and at least one of a positive electrode and a negative electrode.
  • the present invention provides a non-aqueous electrolyte battery including:
  • the carboxyl group ⁇ glycidyl group in the vinylidene fluoride polymer and the hydroxyl group and carbonyl group of the polar polymer form a hydrogen bond with the hydroxyl group on the surface of the current collector and the surface of the electrode active material, and the adhesiveness as a binder
  • a lithium ion selective permeable film is formed on the surface of the electrode active material to block the permeation of the non-aqueous electrolyte, and is synthesized by the reaction between the electrolyte and lithium ions during charging and discharging on the surface of the electrode active material.
  • Examples of the functional group-containing vinylidene fluoride-based polymer of the present invention include vinylidene fluoride monomer alone or other monomers copolymerizable with a vinylidene fluoride monomer, for example, carbonization of ethylene or propylene.
  • Copolymers are preferably used.
  • Monomers having a functional group include those having a carboxyl group and those having a glycidyl group.
  • carboxyl group-containing monomer examples include unsaturated monobasic acids such as acrylic acid and crotonic acid, unsaturated dibasic acids such as maleic acid and citraconic acid, and monomethyl maleate which is a monoalkyl ester thereof. Esters, monoethyl maleate, monomethyl citraconic acid, monoethyl citraconic ester and the like.
  • the glycidyl group-containing monomer examples include acrylidicidyl ether, methacrylic glycidyl ether, glycidinole crotonate, and dalicidyl acetyl acetate.
  • a functional group-containing vinylidene fluoride polymer obtained by copolymerizing at least one or more of these is preferably used.
  • These functional group-containing vinylidene fluoride polymers can be obtained by known methods such as suspension polymerization, emulsion polymerization, and solution polymerization.
  • a vinylidene fluoride-based polymer may be dehydrofluorinated with a heated base or the like, and then treated with an organic acid or an oxidizing agent to obtain a polymer containing a functional group.
  • the molecular weight of a functional group-containing vinylidene fluoride polymer is determined by measuring the intrinsic viscosity (4 g of resin in 1 liter of N, N —The logarithmic viscosity at 30 ° C. of a solution dissolved in dimethylformamide) is 0.8 to 20 dl / g, preferably 1.0 to 20 dl Zg, and more preferably 1.0 to 1 dl / g. 5 dl / g, more preferably 1.2 to 15 dl Zg is suitably used. If the intrinsic viscosity of the vinylidene fluoride polymer is less than the above range, the viscosity of the electrode mixture becomes low and coating becomes difficult, and if it exceeds the above range, dissolution in an organic solvent becomes difficult and Absent.
  • the polar polymer used in the present invention includes a polymer having a hydroxyl group and a polymer having a carboxy group.
  • the polymer having a hydroxyl group include an ethylene vinylinoleanol copolymer, a senorelose polymer, and a vinylol phenol polymer.
  • the polymer having a carboxy group include a polyacrylic acid-based polymer, more specifically, polyacrylic acid, a polyacrylic acid cross-linked polymer, and metal salts thereof.
  • the polar polymer include polybutylpyrrolidone Is also preferably used.
  • a polar polymer having a hydroxyl group or a hydroxyl group, a homopolymer of vinylidene fluoride, vinylidene fluoride and fusidani vinyl a copolymer of vinylidene fluoride and a monomer copolymerizable with vinylidene fluoride such as trifluoroethylene, chlorofluoroethylene, tetrafluoroethylene, and hexafluoropropylene can be added.
  • the mixing ratio between the functional group-containing vinylidene fluoride copolymer and the polar polymer is 10 to 99% by weight, preferably, the functional group-containing vinylidene fluoride copolymer. 20-95 weight. / 0 , the polar polymer is 1 to 90% by weight, preferably 5 to 80% by weight. If the mixing ratio of the polar polymer is less than the above range, the state of coating on the surface of the active material is insufficient and the contact area between the surface of the active material and the electrolytic solution is increased, resulting in poor battery safety. Further, the adhesiveness between the polymer electrode and the current collector and the binding property between the electrode active materials are reduced, and there is a concern that the discharge capacity during repeated charge and discharge is reduced.
  • the mixing ratio of the polar polymer is larger than the above range, the film formed on the electrode surface becomes too thick, the lithium ion permeability at the interface between the active material and the electrolyte is inferior, and the internal resistance increases. There is a concern that the charge / discharge capacity may decrease.
  • the binder composition of the present invention is usually prepared by dissolving a functional group-containing vinylidene fluoride polymer and a polar polymer constituting the binder composition in a solvent, and further dissolving the positive electrode or negative electrode active material and, if necessary, An auxiliary agent such as a conductive auxiliary agent to be added is dispersed to form a slurry-like electrode mixture, which is used for manufacturing an electrode.
  • the solvent is preferably a polar organic solvent, such as N-methyl-2-pyrrolidone, N, N-dimethylformamide, N, N-dimethylacetamide, N, N-dimethylsulfoxide, Hexamethylphosphamide, triethyl phosphate, acetone and the like. These organic solvents can be used alone or in combination of two or more.
  • the active material of the lithium ion secondary battery for other in the case of the positive electrode, the general formula L i MY 2 (M is C o, N i, F e , Mn, C r, transition metals V, etc. At least one of the following: Y is a chalcogen element such as 0 or S); in the case of a negative electrode, natural graphite, artificial graphite, coke, activated carbon, phenolic resin, pitch, etc.
  • powdery carbonaceous material a metal oxide-based G e 0, G e 0 2 , SO, S n0 2, P b O, P b 0 2 or the like or a mixed metal oxide thereof, S i, S i S
  • a key compound such as n and a silicon compound are used.
  • the binder composition is used in an amount of 0.1 to 30 parts by weight, and especially 0 to 30 parts by weight, based on 100 parts by weight of the electrode (positive electrode or negative electrode) active material and the conductive additive (these are collectively referred to as “powder electrode material”). It is preferable to use 5 to 20 parts by weight.
  • the solvent may be used alone or as a mixture of two or more, and the binder composition may be used in an amount of 0.1 to 30 parts by weight, particularly 100 parts by weight of the solvent. It is preferable to use it at a ratio of 1 to 20 parts by weight.
  • a homogenizer As a device used for mixing the mixture comprising the binder composition, the powdered electrode material, and the organic solvent, a homogenizer, a multiaxial planetary dispersion / mixing / kneading machine or an emulsifier can be used, but is not limited thereto. It is not done.
  • the mixture slurry prepared by the above method is uniformly dispersed and mixed with the powdered electrode material and the binder composition, and is applied to the current collector with good applicability.
  • the coating method may be a known method, and among them, the doctor blade method is preferably used.
  • the mixture on the current collector is solvent-dried at, for example, 50 to 170 ° C., and if necessary, subjected to a pressing step to form an electrode structure for a non-aqueous secondary battery or the like.
  • the binder composition and the electrode mixture of the present invention are used for forming at least one of a positive electrode and a negative electrode, and if any one of them is preferably used for forming a negative electrode. This is because the powdered electrode material constituting the negative electrode requires a binder having higher adhesiveness, and the binder composition of the present invention is particularly suitable.
  • the polymer slurry is dehydrated, washed with water, dehydrated, and then dried at 80 ° C for 20 hours.
  • the functional group-containing hydrofluoric acid of the present invention having a yield of 89% and an inherent viscosity of 1.1 d 1 A vinylidene fluoride polymer A was obtained.
  • the polymer slurry is dehydrated, washed with water, dehydrated, and dried at 80 ° C for 20 hours.
  • a vinylidene fluoride polymer having a yield of 91% and an inherent viscosity of 1.1 d 1 / g is obtained.
  • C polyvinylidene fluoride
  • N-methyl-2-pyrrolidone was added to 94 parts by weight of lithium cobaltate ("Cellseed C-5", manufactured by Nippon Chemical Industry), 3 parts by weight of vinylidene fluoride polymer C, and 3 parts by weight of carbon black. 43 parts by weight were added and mixed to prepare a positive electrode mixture. The obtained mixture was uniformly applied on a 10 / m-thick aluminum foil so that the film thickness after drying was about 100 ⁇ , and dried at 130 ° C for 25 minutes. A positive electrode structure (active material amount: 29 1 g / m 2 ) was obtained.
  • a negative electrode mixture composition A of the present invention was prepared by mixing 88 parts by weight of spherical natural graphite powder (produced in China) with an average particle diameter of 30 ⁇ m and 67 parts by weight of NMP. The resulting mixture was applied evenly on a copper foil with a thickness of 8 / zm to a thickness of about 100 / xm after drying, and dried at 130 ° C for 25 minutes. A negative electrode structure A (the amount of the active material: 163 g / m 2 ) was obtained.
  • the negative electrode structure applied to the current collector and dried was used as a sample, and the peel strength of the electrode mixture layer from the current collector was measured by a 180 ° peel test in accordance with JIS K 6854.
  • Battery A was charged to 4.2 V with a constant current of 0.2 mA, then discharged to 3.0 V with a constant current of 0.2 mA, and then 4.37 V with a constant current of 1 mA. Charged up to.
  • the charge capacity (integral value of the charge current value) of the battery in the second charge was 133 mAh.
  • the above charged battery A was allowed to stand on a wooden plate with the negative electrode facing up, and a nail with a diameter of 1 mm was stabbed and penetrated.
  • the rise in battery surface temperature was measured using an infrared thermograph (“TVS-100” manufactured by Avionics).
  • the maximum temperature rise of battery A after nail penetration was 3 ° C.
  • Example 1 The procedure of Example 1 was repeated except that polyacrylic acid (PAA) (“AQUPEC HV—501”, manufactured by Sumitomo Seika) was used instead of EVOH in the fabrication of the negative electrode. Got B.
  • PAA polyacrylic acid
  • the peel strength of negative electrode structure B was 1. O g f Zmm Battery B had a charge capacity of 135 mAh, and the maximum temperature rise in the nail penetration test was 3.5 ° C.
  • Example 1 The procedure of Example 1 was repeated except that the functional group-containing vinylidene fluoride polymer B was used in place of the functional group-containing vinylidene fluoride polymer A in the preparation of the negative electrode. Got C.
  • the peel strength of negative electrode structure C was 4.3 gf / mm, the charge capacity of battery C was 13 OmAh, and the maximum temperature rise in the nail penetration test was 3 ° C.
  • Example 4 The same procedure as in Example 1 was carried out, except that hydroxethyl cellulose (HEC) (“HEC Daicel EP850”, manufactured by Daicel Chemical Industries) was used instead of EVOH in the preparation of the negative electrode. Battery D was obtained.
  • HEC hydroxethyl cellulose
  • the peel strength of negative electrode structure D was 0.9 gf / mm, the charge capacity of battery D was 133 mAh, and the maximum temperature rise in the nail penetration test was 3 ° C.
  • Example 1 The procedure of Example 1 was repeated, except that polyparabule fuenoren (PPVP) (“Markalinker I-S-2PJ”, Maruzen Petrochemical Co., Ltd.) was used instead of EVOH in the preparation of the negative electrode. Structure H and battery H were obtained.
  • PPVP polyparabule fuenoren
  • the peel strength of the negative electrode structure H was 5.4 g f Zmm, the charging capacity of the battery H was 134 mAh, and the maximum temperature rise in the nail penetration test was 4 ° C.
  • Example 1 The procedure of Example 1 was repeated, except that the amount of the functional group-containing vinylidene fluoride polymer A was increased from 11 g to 12 g in the preparation of the negative electrode, and EV0H was not used. Battery E was obtained.
  • the peel strength of the negative electrode structure E was 0.9 gf / mm, the charge capacity of the battery E was 133 mAh, and the maximum temperature rise in the nail penetration test was 12 ° C.
  • Example 3 The same procedure as in Example 3 was carried out except that the amount of the functional group-containing vinylidene fluoride polymer B was increased from 11 g to 12 g in the preparation of the negative electrode, and EVOH was not used. Battery F was obtained.
  • the peel strength of the negative electrode structure F was 3.1 g f / mm, the charge capacity of the battery F was 124 mAh, and the maximum temperature rise in the nail penetration test was 6.5 ° C.
  • a negative electrode structure G and a battery G were obtained in the same manner as in Example 1, except that a vinylidene fluoride polymer C was used in place of the functional group-containing vinylidene fluoride polymer A in the preparation of the negative electrode.
  • the peel strength of the negative electrode structure G was 0.1 ⁇ g f / mm, the charge capacity of the battery G was 134 mAh, and the maximum temperature rise in the nail penetration test was 6 ° C.
  • a negative electrode structure G and a battery G were obtained in the same manner as in Comparative Example 1, except that the functional group-containing vinylidene fluoride polymer A was used in place of the functional group-containing vinylidene fluoride polymer A in the preparation of the negative electrode.
  • Peel strength of negative electrode structure H is 0.7 f / mm Battery H has a charge capacity of 13 mAh The maximum temperature rise in the nail penetration test was 9 ° C.
  • the binder for the positive electrode Z or the negative electrode was a functional group-containing vinylidene fluoride polymer.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)

Abstract

L'invention concerne une composition comprenant au moins un polymère à base de fluorure de vinylidène contenant un groupe fonctionnel, et un polymère polaire présentant un groupe hydroxyle et/ou un groupe carbonyle dans la molécule. Cette composition est utilisée comme matière d'agrégation pour un matériau actif à électrode (une électrode positive ou négative). Une batterie électrolytique non aqueuse peut ainsi obtenir une stabilité du rendement améliorée et une sécurité renforcée au moment d'un court-circuit interne, tout en maintenant une grande capacité nécessaire.
PCT/JP2003/014903 2002-11-22 2003-11-21 Composition d'agregation pour electrode d'une batterie electrolytique non aqueuse, melange electrolytique, electrode et batterie utilisant cette composition WO2004049475A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
JP2004555003A JP4851092B2 (ja) 2002-11-22 2003-11-21 非水電解液電池の電極用バインダー組成物およびその利用
AU2003284631A AU2003284631A1 (en) 2002-11-22 2003-11-21 Binder composition for electrode of nonaqueous electrolyte battery, and electrode mixture, electrode and battery using same

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2002339105 2002-11-22
JP2002-339105 2002-11-22

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WO2004049475A1 true WO2004049475A1 (fr) 2004-06-10

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JP (1) JP4851092B2 (fr)
KR (1) KR20050085095A (fr)
CN (1) CN100365853C (fr)
AU (1) AU2003284631A1 (fr)
TW (1) TW200410439A (fr)
WO (1) WO2004049475A1 (fr)

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JP2010518568A (ja) * 2007-02-09 2010-05-27 コミツサリア タ レネルジー アトミーク 電気化学システムの電極用バインダー、該バインダーを含む電極、及び該電極を含む電気化学システム
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KR20220103940A (ko) 2019-11-19 2022-07-25 스미토모 세이카 가부시키가이샤 이차전지용 결착제
WO2021172383A1 (fr) 2020-02-26 2021-09-02 住友精化株式会社 Agent de liaison pour batterie secondaire
WO2021172385A1 (fr) 2020-02-26 2021-09-02 住友精化株式会社 Procédé de production d'un composé polymère utilisé dans un liant pour batteries secondaires
WO2021172384A1 (fr) 2020-02-26 2021-09-02 住友精化株式会社 Agent de liaison pour batterie secondaire
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US11978906B2 (en) 2020-02-26 2024-05-07 Sumitomo Seika Chemicals Co., Ltd. Binder for secondary battery

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