WO2012093616A1 - 蓄電デバイス - Google Patents
蓄電デバイス Download PDFInfo
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- WO2012093616A1 WO2012093616A1 PCT/JP2011/080150 JP2011080150W WO2012093616A1 WO 2012093616 A1 WO2012093616 A1 WO 2012093616A1 JP 2011080150 W JP2011080150 W JP 2011080150W WO 2012093616 A1 WO2012093616 A1 WO 2012093616A1
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- current collector
- positive electrode
- active material
- negative electrode
- corrosion
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/04—Hybrid capacitors
- H01G11/06—Hybrid capacitors with one of the electrodes allowing ions to be reversibly doped thereinto, e.g. lithium ion capacitors [LIC]
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/66—Current collectors
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/74—Terminals, e.g. extensions of current collectors
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/04—Construction or manufacture in general
- H01M10/0436—Small-sized flat cells or batteries for portable equipment
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
- H01M10/0566—Liquid materials
- H01M10/0568—Liquid materials characterised by the solutes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
- H01M50/102—Primary casings, jackets or wrappings of a single cell or a single battery characterised by their shape or physical structure
- H01M50/109—Primary casings, jackets or wrappings of a single cell or a single battery characterised by their shape or physical structure of button or coin shape
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- 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
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- 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
- Y02E60/13—Energy storage using capacitors
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- 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
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- 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
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/60—Other road transportation technologies with climate change mitigation effect
- Y02T10/70—Energy storage systems for electromobility, e.g. batteries
Definitions
- the present invention relates to a highly safe power storage device that suppresses a decrease in power storage capacity and a manufacturing method thereof, and more particularly to a power storage device of a secondary battery such as a lithium ion secondary battery and a manufacturing method thereof.
- electrochemical capacitors such as secondary batteries, electric double layer capacitors and hybrid capacitors mounted on them
- a high energy density is required for an electricity storage device such as the above, and further reliability such as high safety is required.
- This type of electricity storage device includes a positive electrode and a negative electrode, a separator interposed between these electrodes, and a cell tank that contains the electrodes and separator and is filled with an electrolyte so as to immerse them.
- the energy stored by the electric double layer and / or the oxidation-reduction reaction is repeatedly discharged, and charging / discharging is repeatedly performed.
- Each of the positive electrode and the negative electrode of such an electricity storage device is provided with an active material layer containing an active material and a current collector in contact with the layer surface of the active material layer in order to extract electric energy from the active material.
- the active material layer is prepared by preparing a coating solution containing the active material and applying it to a metal foil or the like as a current collector, or by pressing and rolling the active material together with a binder as an electrode.
- the current collector is made of a material that suppresses the reaction with the electrolyte.
- the current collector has an electrolyte containing lithium fluorophosphate (LiPF 6 ) or the like as an electrolyte.
- LiPF 6 lithium fluorophosphate
- aluminum or the like is used that suppresses the reaction even when the positive electrode potential becomes 4.0 V or more during charging.
- LiTFSI lithium bistrifluoromethanesulfonylimide
- LiTFS lithium trifluoromethanesulfonate
- these electrolytes are fluorinated phosphoric acid.
- it has the advantages of high solubility in organic solvents, excellent thermal stability, and the suppression of hydrogen fluoride generation during repeated charge and discharge, but when the positive electrode potential becomes 4.0 V or higher during charging. It has been reported that it reacts with aluminum as a current collector (Non-Patent Document 1), and there has been a problem in putting these substances into practical use as electrolytes.
- Patent Document 1 A non-aqueous electrolyte secondary battery (Patent Document 1) that suppresses the above has been reported.
- Patent Document 2 a secondary battery that has an electrolyte containing 1.5 mol / L or more of LiTFS, makes the electrolyte nonflammable, and is excellent in safety.
- this secondary battery is highly safe, it contains a high concentration of LiTFS, and even when an electrolyte solution with a low electrolyte concentration is used, corrosion of the current collector can be suppressed, and the current collector and electrolyte There is a demand for an electricity storage device that can expand the selection range.
- the problem of the present invention is to suppress the reaction between the electrolyte and the current collector contained in the electrolytic solution, to suppress the corrosion of the current collector and the deterioration of the electrolytic solution, to suppress the reduction of the energy capacity,
- An object of the present invention is to provide a power storage device that is excellent in stability, durability, and reliability at a potential, and a method for manufacturing the same.
- the present invention is an electricity storage device having a positive electrode having a positive electrode active material layer on a positive electrode current collector, a negative electrode having a negative electrode active material layer on a negative electrode current collector, a separator, and an electrolyte solution, the positive electrode current collector or The negative electrode current collector, or both of them has a corrosion-inhibiting film on the surface, and the thickness of the corrosion-inhibiting film is 50 nm or more.
- the electricity storage device of the present invention suppresses the reaction between the electrolyte and the current collector contained in the electrolytic solution, can suppress the corrosion of the current collector and the deterioration of the electrolytic solution, suppress the reduction of energy capacity, High potential, excellent stability and durability, and high reliability.
- An electricity storage device of the present invention is an electricity storage device having a positive electrode having a positive electrode active material layer on a positive electrode current collector, a negative electrode having a negative electrode active material layer on a negative electrode current collector, a separator, and an electrolyte solution.
- the electric current collector, the negative electrode current collector, or both of them have a corrosion-inhibiting film on the surface, and the thickness of the corrosion-inhibiting film is 50 nm or more.
- a secondary battery As an embodiment to which the electricity storage device of the present invention is applied, a secondary battery will be described as an example.
- the positive electrode has a positive electrode active material layer and a positive electrode current collector on which the positive electrode active material layer is stacked.
- the positive electrode active material layer only needs to contain a positive electrode active material, and the positive electrode active material is preferably bound by a positive electrode binder.
- lithium manganate having a layered crystal structure such as LiMnO 2 , Li x Mn 2 O 4 (0 ⁇ x ⁇ 2), Li x Mn 1.5 Ni 0.5 O 4 (0 ⁇ x ⁇ 2) , Lithium manganate having a spinel crystal structure; LiCoO 2 , LiNiO 2 or a part of these transition metals may be Al, Fe, P, Ti, Si, Pb, Sn, In, Bi, Ag, Ba, Ca, Hg, Pd, Pt, Te, Zn, La substituted with at least two kinds; LiNi 1/3 Co 1/3 Mn 1/3 O 2 and other lithium transition metals whose specific transition metal does not exceed half Oxides; those lithium transition metal oxides that contain Li in excess of the stoichiometric composition.
- a positive electrode active material can be used individually by 1 type or in combination of 2 or more types.
- the binder for the positive electrode is preferably one that can bind the positive electrode active material in a small amount, has stability with respect to the electrolytic solution, and can integrally hold the positive electrode active material in the battery.
- the following can be mentioned.
- polyvinylidene fluoride, vinylidene fluoride-hexafluoropropylene copolymer, vinylidene fluoride-tetrafluoroethylene copolymer, styrene-butadiene copolymer rubber, polytetrafluoroethylene, polypropylene, polyethylene, polyimide, polyamideimide, poly Acrylic acid etc. can be mentioned.
- polyvinylidene fluoride is preferable from the viewpoint of versatility and low cost.
- the amount of the positive electrode binder to be used is preferably 2 to 15 parts by mass with respect to 100 parts by mass of the positive electrode active material from the viewpoints of “sufficient binding force” and “high energy” which are in a trade-off relationship. .
- the positive electrode active material layer may contain a conductive auxiliary material that can lower the impedance in order to increase the conductivity of the current collector and the positive electrode active material.
- a conductive auxiliary material carbonaceous fine particles such as graphite, carbon black, and acetylene black can be used.
- the thickness of the positive electrode active material layer containing the positive electrode active material is preferably 140 to 180 ⁇ m. If the thickness of the positive electrode active material layer is in the above range, it is possible to obtain a battery having a high energy density while suppressing the occupied volume in the battery from becoming excessive.
- the thickness of the positive electrode active material layer As the thickness of the positive electrode active material layer, a value measured by a stylus thickness meter can be adopted. Or when forming by vapor deposition, the value calculated
- the positive electrode current collector for fixing the positive electrode active material layer is selected from materials having excellent electronic conductivity, stable presence in the battery, high adhesion to the positive electrode active material, small volume, and high density. It is preferable. As such a material, one or more selected from aluminum, nickel, chromium, stainless steel, copper, silver, and alloys containing any of these metals are preferable. Examples of the shape include foil, flat plate, and mesh.
- the thickness of the positive electrode current collector can be 10 to 30 ⁇ m as a guide. If the thickness of the positive electrode current collector is within the above range, it is possible to suppress an excessive occupation volume in the battery.
- Such a positive electrode current collector preferably has a corrosion-inhibiting film having a thickness of 50 nm or more.
- the corrosion-inhibiting film is provided on the positive electrode current collector, the negative electrode current collector described later, or both, but is preferably provided on the positive electrode current collector.
- the corrosion-inhibiting film is formed in advance, and does not include an oxide film formed on the surface when left in the air or a so-called passive film formed with charge / discharge in the battery. That is, it is a film formed on the current collector surface by physical or electrochemical techniques such as vapor deposition, coating, and sputtering.
- the corrosion inhibiting film may be provided over the entire surface of the positive electrode current collector, but may be provided in a portion excluding a portion where the positive electrode active material layer is laminated. That is, the positive electrode active material layer may be laminated on a positive electrode current collector that does not have a corrosion inhibiting film, or may be laminated on the positive electrode current collector via a corrosion inhibiting film. Further, the corrosion inhibiting film may be provided on the positive electrode active material layer, but it is preferable that the lithium ion occlusion and release in the positive electrode active material layer is not inhibited by an increase in the interface resistance with the electrolytic solution.
- the thickness of the corrosion inhibiting film is 50 nm or more, preferably 80 nm or more, and more preferably 100 nm or more.
- membrane can also be made to be equivalent to the thickness of a positive electrode active material layer, it is preferable that it is 5 micrometers or less, More preferably, it is 1 micrometer or less.
- the oxide film formed by being left in the air and the passive film formed on the current collector as the battery is charged and discharged often have a thickness of 10 nm or less, but 10 nm or less. When the thickness is too large, it is difficult to sufficiently suppress the reaction between the electrolyte and the current collector. Moreover, when providing a corrosion inhibitor film
- the corrosion-inhibiting film is formed of a lithium compound such as lithium fluoride or lithium carbonate because the effect of suppressing the reaction with an electrolyte contained in the electrolytic solution is high.
- the formation method of the corrosion inhibiting film can be formed by vapor deposition, sputtering, spin coating, or the like. Among these, vapor deposition with a simple operation procedure is preferable.
- the corrosion inhibiting film is formed on the current collector surface before or after the positive electrode active material layer is formed on the current collector.
- the positive electrode active material layer may be formed after forming the corrosion suppression film over the entire surface of the current collector surface, but after the positive electrode active material layer is laminated on the current collector surface, the corrosion suppression film is formed.
- a film may be formed.
- the corrosion inhibiting film is provided on the positive electrode current collector on which the positive electrode active material layer is not laminated, after forming the positive electrode active material layer on the positive electrode current collector, the positive electrode active material layer is masked, It is preferable to form a corrosion-inhibiting film by the method. Alternatively, the portion where the positive electrode active material layer on the positive electrode current collector is laminated may be masked to form a corrosion inhibiting film, and then the portion where the corrosion inhibiting film is formed may be masked to form the positive electrode active material layer. .
- the positive electrode includes a positive electrode active material and a binder, if necessary, a conductive auxiliary material, a solvent, etc., and a mixture obtained by mixing the mixture as a coating solution, using a doctor blade method on the positive electrode current collector It can be formed by coating by a die coater method or the like, or press-bonding and rolling the mixture, punching it into the shape of the positive electrode active material layer, and press-bonding it to the positive electrode current collector.
- the negative electrode includes a negative electrode active material layer and a negative electrode current collector on which the negative electrode active material layer is stacked.
- the negative electrode active material layer only needs to contain a negative electrode active material, and the negative electrode active material is preferably bound to the negative electrode current collector by a negative electrode binder.
- the negative electrode active material a material capable of inserting and extracting lithium ions can be used. Specifically, the following can be mentioned.
- carbon materials such as carbon and graphite, metals such as Al, Fe, P, Ti, Si, Pb, Sn, In, Bi, Ag, Ba, Ca, Hg, Pd, Pt, Te, Zn, La, etc.
- An alloy or a compound such as an oxide containing any of the above metals can be used. These may be used alone or in combination of two or more, and may further contain one or more other metals or non-metals. Specific examples include tin or silicon oxides and carbides.
- the negative electrode binder is preferably one that can bind the negative electrode active material in a small amount, has stability to the electrolytic solution, and can hold the negative electrode active material integrally in the battery.
- examples thereof include those exemplified as the binder for the positive electrode, and it is also preferable to use polyvinylidene fluoride.
- the amount of the negative electrode binder to be used is preferably 5 to 25 parts by mass with respect to 100 parts by mass of the negative electrode active material, from the viewpoint of sufficient binding force and high energy in a trade-off relationship.
- the negative electrode active material layer can contain a conductive auxiliary material in order to increase the conductivity of the current collector and the negative electrode active material.
- a conductive auxiliary material used as the conductive auxiliary material used, the conductive auxiliary material used for the positive electrode active material layer and Similar ones can be used.
- the thickness of the negative electrode active material layer containing the negative electrode active material is preferably 100 to 140 ⁇ m. If the thickness of the negative electrode active material layer is in the above range, it is possible to obtain a battery with a high energy density while suppressing the occupied volume in the battery from becoming excessive.
- the negative electrode current collector for fixing the negative electrode active material layer is selected from materials having excellent electron conductivity, stable presence in the battery, high adhesion to the negative electrode active material, small volume, and high density. It is preferable. Examples of such a material include the same material as that of the positive electrode current collector, and the shape thereof can also be the same shape as that of the positive electrode current collector.
- the thickness of the negative electrode current collector can be 8 to 10 ⁇ m. If the thickness of the negative electrode current collector is within the above range, it is possible to suppress the occupied volume in the battery from becoming excessive.
- Such a negative electrode current collector can have a corrosion-inhibiting film having a thickness of 50 nm or more, like the positive electrode current collector.
- the corrosion-inhibiting film formed on the negative electrode current collector is also formed in advance, and includes oxide films formed on the surface when left in the air and passive films formed upon charging / discharging of batteries. Absent.
- the corrosion inhibiting film formed on the negative electrode current collector may be provided over the entire surface of the negative electrode current collector, or may be provided on a portion other than the portion where the negative electrode active material layer is laminated. That is, the negative electrode active material layer may be laminated on a negative electrode current collector that does not have a corrosion inhibiting film, or may be laminated on the negative electrode current collector via a corrosion inhibiting film.
- the corrosion inhibiting film may be provided on the negative electrode active material layer, it is preferable not to inhibit the insertion and release of lithium ions in the negative electrode active material layer due to an increase in the interface resistance with the electrolytic solution.
- the corrosion inhibiting film provided on the negative electrode current collector is also the same thickness as the corrosion inhibiting film provided on the positive electrode current collector, that is, 50 nm or more, preferably 80 nm or more, and more preferably 100 nm or more. Further, the thickness of the corrosion-inhibiting film may be up to about the same as the thickness of the negative electrode active material layer, but is preferably 5 ⁇ m or less, more preferably 1 ⁇ m or less, and is provided on the positive electrode current collector.
- membrane can be mentioned, and it can form by the same method.
- the negative electrode manufacturing method is similar to the positive electrode manufacturing method described above, in which a coating liquid containing a negative electrode active material is applied onto a negative electrode current collector, and a negative electrode active material containing a negative electrode active material is formed in the shape of a negative electrode active material layer.
- the negative electrode current collector may be formed by pressure bonding, the negative electrode active material layer may be formed on the negative electrode current collector, or the negative electrode current collector may be formed on a previously formed negative electrode active material layer.
- the electrolytic solution is disposed by immersing the positive electrode and the negative electrode, enables movement of a charged body between the positive electrode and the negative electrode, and uses an electrolyte dissolved in an organic solvent.
- organic solvent include ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), vinylene carbonate (VC), vinyl ethylene carbonate (VEC), ethylene sulfite (ES), Propane sultone (PS), butane sultone (BS), dioxathiolane-2,2-dioxide (DD), sulfolene, 3-methylsulfolene, sulfolane (SL), succinic anhydride (SUCAH), propionic anhydride, acetic anhydride, Maleic anhydride, diallyl carbonate (DAC), diphenyl disulfide (DPS), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), chloroethylene carbonate, dieth
- R v1 and R v2 are alkyl groups, respectively.
- a fluorinated ether having a fluorinated alkyl group structure, an ionic liquid, phosphazene, or the like may be mixed. These organic solvents may be used alone or in combination of two or more.
- ethylene carbonate, diethyl carbonate, propylene carbonate, dimethyl carbonate, ethyl methyl carbonate, ⁇ -butyrolactone, ⁇ -valerolactone, trimethyl phosphate, triethyl phosphate and the like are particularly preferable.
- the supporting salt of the electrolyte contained in the electrolytic solution include LiPF 6 , LiI, LiBr, LiCl, LiAsF 6 , LiAlCl 4 , LiClO 4 , LiBF 4 , LiSbF 6 , LiCF 3 SO 3 (abbreviation: LiTFS), LiC 4 F 9 SO 3 , LiN (FSO 2 ) 2 , LiN (C 2 F 5 SO 2 ) 2 (abbreviation: LiTFSI), LiN (C 2 F 5 SO 2 ) 2 (abbreviation: LiBETI), LiN (CF 3 SO 2 ) (C 2 F 5 SO 2 ), LiN (CF 3 SO 2 ) (C 4 F 9 SO 2 ), LiN (CF 2 SO 2 ) 2 (CF 2 ) having a 5-membered ring or a 6-membered ring, LiN (CF 2 SO 2) 2 (CF 2) 2, LiPF 5 (CF 3) to at least one fluorine atom substituted with the fluoroal
- a sulfonyl compound represented by the chemical formula (1) can be used as the electrolyte.
- R 1 , R 2 and R 3 independently represent a halogen atom or a fluorinated alkyl group.
- Specific examples of the sulfonyl compound represented by the formula (1) include LiC (CF 3 SO 2 ) 3 and LiC (C 2 F 5 SO 2 ) 3 .
- the lithium salts and sulfonyl compounds can be used alone or in combination of two or more.
- an electrolytic solution to which lithium trifluoromethanesulfonate (LiTFS) or lithium bistrifluoromethanesulfonylimide (LiTFSI) is used, even at a high potential such as 4.5 V (vsLi / Li + ) A high corrosion inhibitory effect on the current collector can be obtained.
- the electrolyte concentration in the organic solvent is preferably 0.01 mol / L or more and 3 mol / L or less, more preferably 0.5 mol / L or more and 1.5 mol / L or less.
- the electrolyte concentration is within this range, safety can be improved, and a battery having high reliability and contributing to reduction of environmental load can be obtained.
- any separator may be used as long as it suppresses the contact between the positive electrode and the negative electrode, does not inhibit the permeation of the charged body, and has durability against the electrolytic solution.
- the material that can be used include polyolefin microporous membranes such as polypropylene and polyethylene, cellulose, polyethylene terephthalate, polyimide, polyamideimide, polyfucvinylidene, and polytetrafluoroethylene. These can be used as porous films, woven fabrics, non-woven fabrics and the like.
- the thickness of the separator can be set to 20 to 30 ⁇ m, for example, so that the occupied volume in the battery can be prevented from becoming excessive.
- outer package those having a strength capable of stably holding the positive electrode, the negative electrode, the separator, and the electrolytic solution, electrochemically stable and watertight with respect to these substances are preferable.
- a laminated laminate type secondary battery a laminate film such as polypropylene or polyethylene coated with aluminum or silica can be used as the outer package.
- the shape of the secondary battery may be any of a cylindrical type, a flat wound square type, a laminated square type, a coin type, a flat wound laminated type, and a laminated laminate type.
- a coin-type secondary battery 10 shown in the exploded configuration diagram of FIG. 1 includes a negative electrode in which a negative electrode active material layer 4 is laminated on a negative electrode current collector 3, and a positive electrode in which a positive electrode active material layer 6 is laminated on a positive electrode current collector 7.
- the separator 5 is disposed so as to avoid the contact, and is accommodated in the exterior body 1 filled with an electrolyte solution (not shown) via the insulating packing 2.
- the corrosion of the current collector on which the corrosion-inhibiting film is formed is suppressed, and the decrease in energy capacity is suppressed even when used in a battery having a high energy capacity.
- a lithium metal as a working electrode, a reference electrode, and a counter electrode obtained by forming a LiF film having a film thickness of 200 nm on a positive electrode current collector made of aluminum in a portion where the positive electrode active material is not laminated, 1 mol / L
- a triode cell using an electrolytic solution in which LiTFSI or LiTFS was dissolved in an organic solvent containing EC: DEC at 3: 7 was swept from 3.0 to 4.3 V (vsLi / Li +), respectively, FIG. As shown in FIG.
- an electric double layer capacitor can be mentioned.
- a separator 14 is interposed between the electrodes 12 and 13, and is housed together with an electrolyte solution (not shown) in an outer package made up of a can 15 and a cap 16.
- the can 15 and the cap 16 function as current collectors for the electrodes 12 and 13, respectively.
- the inner wall surfaces of the can 15 and the cap 16 have a corrosion inhibiting film (not shown) that suppresses the reaction to the solvent and electrolyte contained in the electrode solution.
- Examples of the electrodes 12 and 13 include those formed by mixing activated carbon mixed with a lithium compound such as lithium oxide, a conductive agent such as carbon black, polytetrafluoroethylene, polyvinylidene fluoride, carboxymethyl cellulose, or the like as a binder.
- the separator can be formed of the same material as the separator used for the secondary battery, and cellulose or the like can be preferably used.
- the can 15 and the cap 16 constituting the current collector can be the same as the secondary battery, but it is preferable to use stainless steel or the like.
- a lithium fluoride film or the like can be applied, and an oxide film formed by being left in the air or an electrochemical reaction in the capacitor is not used. It is not formed by vapor deposition or coating.
- the thickness is 50 nm or more, more preferably 100 nm or more, and is 5 ⁇ m or less, more preferably 1 ⁇ m or less.
- the electrolyte solution can use the same organic solvent and electrolyte as the above secondary battery, and specifically, a solution obtained by dissolving LiTFSI, LiTFS, LiPF6, etc. in propylene carbonate at a concentration of 1 mol / L. Can be used.
- Such an electric double layer capacitor is excellent in safety because the reaction between the current collector and the electrolyte contained in the electrolyte is suppressed, the decrease in energy capacity is suppressed.
- Example 1 [Production of positive electrode]
- lithium manganese composite oxide (LiMn 2 O 4 ) -based material is mixed with VGCF (manufactured by Showa Denko KK) as a conductive agent, and dispersed in N-methylpyrrolidone (NMP) as a slurry. It was. The slurry was applied to an aluminum foil as a positive electrode current collector and dried to prepare an electrode having a diameter of 12 mm.
- VGCF manufactured by Showa Denko KK
- NMP N-methylpyrrolidone
- the aluminum current collector on which the positive electrode active material layer was formed was set in a vapor deposition device using a vapor deposition device, and a metal foil was placed on the positive electrode active material layer and masked.
- the crucible filled with lithium fluoride was heated while keeping the inside of the apparatus in a vacuum, and a film of lithium fluoride was formed on the surface where the current collector was not masked.
- the film formation was completed from the change in the weight of the crystal resonator disposed inside the vapor deposition apparatus, and a lithium fluoride film having a thickness of 100 nm was obtained.
- a positive electrode having a current collector in which a portion where the positive electrode active material layer was not laminated was coated with a corrosion prevention film of lithium fluoride was obtained.
- a negative electrode active material As a negative electrode active material, a graphite-based material was dispersed in N-methylpyrrolidone (NMP) to form a slurry. Slurry was apply
- NMP N-methylpyrrolidone
- the produced coin-type lithium secondary battery was first discharged at a current of 0.073 mA, an upper limit potential of 4.2 V, and a lower limit potential of 3.0 V.
- the initial discharge capacity was obtained by converting the measured value of the discharge amount per unit mass of the positive electrode active material.
- Example 2 A coin-type lithium secondary battery was produced in the same manner as in Example 1 except that the thickness of the lithium fluoride film formed on the positive electrode aluminum current collector was changed to 200 nm, and the initial discharge capacity was determined. The results are shown in Table 1.
- Example 3 A coin-type lithium secondary battery was prepared in the same manner as in Example 1 except that the thickness of the lithium fluoride film formed on the positive electrode aluminum current collector was changed to 500 nm, and the initial discharge capacity was determined. The results are shown in Table 1.
- Example 4 A coin-type lithium secondary battery was prepared in the same manner as in Example 1 except that an electrolytic solution in which LiPF 6 was dissolved was used instead of LiTFSI, and the initial discharge capacity was obtained. The results are shown in Table 1.
- Example 1 A coin-type lithium secondary battery was prepared in the same manner as in Example 1 except that no lithium fluoride film was formed on the positive electrode aluminum current collector, and the initial discharge capacity was determined. The results are shown in Table 1.
- Example 2 A coin-type lithium secondary battery was produced in the same manner as in Example 1 except that the lithium fluoride film was not formed on the aluminum current collector of the positive electrode, and an electrolytic solution in which LiPF 6 was dissolved instead of LiTFSI was used. The discharge capacity was determined. The results are shown in Table 1.
- the initial discharge capacity was 0 mAh / g (Comparative Example 1), and the battery did not operate. This is thought to be impossible to charge because LiTFSI and aluminum have undergone an oxidation reaction.
- the initial discharge capacity can be obtained even when LiTFSI is used as the supporting salt. This is presumably because the lithium fluoride film functioned as a corrosion-inhibiting film and suppressed the reaction between the current collector and the supporting salt.
- the initial discharge capacity is improved by using an aluminum current collector having a lithium fluoride film (Example 4, Comparative Example 2). It is considered that this is because the lithium fluoride film suppresses the reaction between LiPF 6 and the aluminum current collector, as in the case of using LiTFSI.
- the corrosion inhibiting film formed on the current collector suppresses the reaction between the current collector and the electrolyte contained in the electrolytic solution when a voltage is applied, so the selection of the electrolytic solution containing the electrolyte and the current collector
- the design conditions of the electricity storage device can be relaxed.
- the present invention can be used in all industrial fields that require a power source and industrial fields related to the transport, storage and supply of electrical energy.
- power supplies for mobile devices such as mobile phones and laptop computers; electric vehicles such as electric cars, hybrid cars, electric bikes, and electric assist bicycles; power supplies for moving and transport media such as trains, satellites, and submarines; UPS It can be used for backup power sources such as power storage facilities for storing power generated by solar power generation, wind power generation, and the like.
Abstract
Description
正極は、正極活物質層と、これを積層する正極集電体とを有する。
負極は、負極活物質層と、これを積層する負極集電体とを有する。
電解液は、正極及び負極を浸漬して配置され、正極及び負極間の荷電体の移動を可能とするものであり、有機溶媒に電解質を溶解したものを用いる。有機溶媒としては、具体的には、例えば、エチレンカーボネート(EC)、プロピレンカーボネート(PC)、ブチレンカーボネート(BC)、ビニレンカーボネート(VC)、ビニルエチレンカーボネート(VEC)、エチレンサルファイト(ES)、プロパンサルトン(PS)、ブタンスルトン(BS)、Dioxathiolane-2,2-dioxide(DD)、スルホレン、3-メチルスルホレン、スルホラン(SL)、無水コハク酸(SUCAH)、無水プロピオン酸、無水酢酸、無水マレイン酸、ジアリルカーボネート(DAC)、ジフェニルジサルファイド(DPS)、ジメチルカーボネート(DMC)、エチルメチルカーボネート(EMC)、クロロエチレンカーボネート、ジエチルカーボネート(DEC)、ジメトキシエタン(DME)、ジメトキシメタン(DMM)、ジエトキシエタン(DEE)、エトキシメトキシエタン、ジメチルエーテル、メチルエチルエーテル、メチルプロピルエーテル、エチルプロピルエーテル、ジプロピルエーテル、メチルブチルエーテル、ジエチルエーテル、フェニルメチルエーテル、テトラヒドロフラン(THF)、テトラヒドロピラン(THP)、1,4-ジオキサン(DIOX)、1,3-ジオキソラン(DOL)、アセトニトリル、プロピオンニトリル、γ-ブチロラクトン、γ-バレロラクトン、ギ酸メチル、酢酸メチル、プロピオン酸エチル等の脂肪族カルボン酸エステル類等を挙げることができる。また、電解液の難燃効果を高めるために、リン酸トリメチル、リン酸トリエチル、リン酸トリプロピル、リン酸トリオクチル、リン酸トリフェニル、Rv1-O-Rv2(Rv1,Rv2はそれぞれアルキル基又はフッ素アルキル基)構造をもつフッ素化エーテル、イオン液体、ホスファゼン等を混合させてもよい。これらの有機溶媒は、単独で使用してもよく、2種以上を併用してもよい。
セパレータは、正極及び負極の接触を抑制し、荷電体の透過を阻害せず、電解液に対して耐久性を有するものであれば、いずれであってもよい。具体的な材質としては、ポリプロピレン、ポリエチレン等のポリオレフィン系微多孔膜、セルロース、ポリエチレンテレフタレート、ポリイミド、ポリアミドイミド、ポリフッカビニリデン、ポリテトラフルオロエチレン等を採用することができる。これらは、多孔質フィルム、織物、不織布等として用いることができる。
外装体としては、上記正極及び負極、セパレータ、電解液を安定して保持可能な強度を有し、これらの物質に対して電気化学的に安定で、水密性を有するものが好ましい。具体的には、例えば、積層ラミネート型の二次電池の場合、外装体としては、アルミニウム、シリカをコーティングしたポリプロピレン、ポリエチレン等のラミネートフィルムを用いることができる。
[実施例1]
[正極の作製]
正極活物質として、リチウムマンガン複合酸化物(LiMn2O4)系材料に、導電剤としてVGCF(昭和電工(株)製)を混合し、これをN-メチルピロリドン(NMP)に分散させてスラリーとした。正極集電体としてのアルミニウム箔に、スラリーを塗布し、乾燥し、直径12mmの電極を調製した。
負極活物質として、黒鉛系材料をN-メチルピロリドン(NMP)に分散させてスラリーとした。負極集電体としての銅箔に、スラリーを塗布し、乾燥し、直径12mmの電極を作製した。
ドライルーム中で、有機溶媒EC:DEC(30:70)に、1mol/LのLiTFSIを溶解した電解液を作製した。
得られた正極を、集電体作用を有するステンレスのコインセル受型上に置き、多孔質のポリエチレンフィルムからなるセパレータ4を挟んで得られた負極と重ね合わせ電極積層体を得た。得られた電極積層体に、上記の方法で得られた電解液を注入し、真空含浸させた。十分に含浸させて電極及びセパレータの空隙を電解液で埋めた後、絶縁パッキンと、集電体作用を有するコインセル受型とを重ね合わせ、専用のかしめ機で外側をステンレス外装で覆って一体化させて、図1に示すコイン型二次電池を作製した。得られたコイン型リチウム二次電池を用いて、以下の方法により初回放電容量を測定した。結果を表1に示す。
作製したコイン型のリチウム二次電池に、0.073mAの電流で、上限電位は4.2V、下限電位は3.0Vで初回放電を行った。放電量の測定値から正極活物質の単位質量当りに換算し、初回放電容量を求めた。
正極のアルミニウム集電体に形成したフッ化リチウム膜の膜厚を、200nmに変更した以外は、実施例1と同様にコイン型リチウム二次電池を作製し、初回放電容量を求めた。結果を表1に示す。
正極のアルミニウム集電体に形成したフッ化リチウム膜の膜厚を、500nmに変更した以外は、実施例1と同様にコイン型リチウム二次電池を作製し、初回放電容量を求めた。結果を表1に示す。
LiTFSIに変えてLiPF6を溶解した電解液を用いた以外は、実施例1と同様にコイン型リチウム二次電池を作製し、初回放電容量を求めた。結果を表1に示す。
正極のアルミニウム集電体にフッ化リチウム膜を形成しなかった以外は、実施例1と同様にコイン型リチウム二次電池を作製し、初回放電容量を求めた。結果を表1に示す。
正極のアルミニウム集電体にフッ化リチウム膜を形成せず、LiTFSIに変えてLiPF6を溶解した電解液を用いた以外は、実施例1と同様にコイン型リチウム二次電池を作製し、初回放電容量を求めた。結果を表1に示す。
3 負極集電体
4 負極活物質層
5 セパレータ
6 正極活物質層
7 正極集電体
10 コイン型二次電池
Claims (8)
- 正極集電体上に正極活物質層を有する正極、負極集電体上に負極活物質層を有する負極、セパレータ、及び電解液を有する蓄電デバイスであって、正極集電体若しくは負極集電体、又はこれらの両方が、表面に腐食抑制膜を有し、該腐食抑制膜の厚さが50nm以上であることを特徴とする蓄電デバイス。
- 前記腐食抑制膜が蒸着膜であることを特徴とする請求項1に記載の蓄電デバイス。
- 前記腐食抑制膜が、フッ化リチウムを含有することを特徴とする請求項1又は2に記載の蓄電デバイス。
- 正極集電体若しくは負極集電体、又はこれらの両方が、アルミニウム、ニッケル、クロム、ステンレス、銅、銀、及びこれらの金属のいずれかを含む合金から選ばれる1種又は2種以上を含有することを特徴とする請求項1から3のいずれかに記載の蓄電デバイス。
- 前記電解液が、リチウムビストリフルオロメタンスルホニルイミド及びトリフルオロメタンスルホン酸リチウムのリチウム塩から選ばれる一種又は二種を含有することを特徴とする請求項1から4のいずれかに記載の蓄電デバイス。
- 前記電解液が、リチウム塩を0.01mol/L以上、3mol/L以下の範囲で溶解していることを特徴とする請求項1から5のいずれかに記載の蓄電デバイス。
- 集電体上にリチウム塩を蒸着して腐食抑制膜を形成することを特徴とする蓄電デバイスの製造方法。
- 集電体上の活物質層が積層される部分を除いて腐食抑制膜を形成することを特徴とする請求項7記載の蓄電デバイスの製造方法。
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US20140272583A1 (en) * | 2013-03-15 | 2014-09-18 | Ppg Industries Ohio, Inc. | Pretreatment compositions and methods for coating a battery electrode |
JP2015529827A (ja) * | 2012-09-14 | 2015-10-08 | ルノー エス.ア.エス. | リチウム電池用のヘキサフルオロリン酸リチウムLiPF6を含有する電解質内のフッ化水素酸を検出し定量する方法 |
WO2016068680A1 (ko) * | 2014-10-31 | 2016-05-06 | 주식회사 엘지화학 | 전극 조립체 및 이를 포함하는 이차 전지 |
JP2018067532A (ja) * | 2016-10-14 | 2018-04-26 | 三洋化成工業株式会社 | リチウムイオン電池用正極及びリチウムイオン電池 |
JP2018067508A (ja) * | 2016-10-21 | 2018-04-26 | 三洋化成工業株式会社 | リチウムイオン電池の製造方法 |
KR20180083371A (ko) | 2015-12-01 | 2018-07-20 | 닛산 가가쿠 고교 가부시키 가이샤 | 비수계 이차전지 |
US10141575B2 (en) | 2016-09-21 | 2018-11-27 | Kabushiki Kaisha Toshiba | Electrode, nonaqueous electrolyte battery, battery pack, and vehicle |
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WO2017057486A1 (ja) * | 2015-09-28 | 2017-04-06 | Jsr株式会社 | 電極材料、電池、及びキャパシタの製造方法、並びに電極材料の製造装置 |
US11830672B2 (en) | 2016-11-23 | 2023-11-28 | KYOCERA AVX Components Corporation | Ultracapacitor for use in a solder reflow process |
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