WO2021141074A1 - Élément de stockage d'énergie à électrolyte non aqueux et son procédé de fabrication - Google Patents

Élément de stockage d'énergie à électrolyte non aqueux et son procédé de fabrication Download PDF

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WO2021141074A1
WO2021141074A1 PCT/JP2021/000276 JP2021000276W WO2021141074A1 WO 2021141074 A1 WO2021141074 A1 WO 2021141074A1 JP 2021000276 W JP2021000276 W JP 2021000276W WO 2021141074 A1 WO2021141074 A1 WO 2021141074A1
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aqueous electrolyte
negative electrode
power storage
active material
lithium
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PCT/JP2021/000276
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English (en)
Japanese (ja)
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宇史 岡島
崇司 奥坊
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株式会社Ｇｓユアサ
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Publication of WO2021141074A1 publication Critical patent/WO2021141074A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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]
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H01G11/32—Carbon-based
    • H01G11/38—Carbon pastes or blends; Binders or additives therein
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/22—Electrodes
    • H01G11/30—Electrodes characterised by their material
    • H01G11/32—Carbon-based
    • H01G11/42—Powders or particles, e.g. composition thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-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
    • H01G11/58—Liquid electrolytes
    • H01G11/62—Liquid electrolytes characterised by the solute, e.g. salts, anions or cations therein
    • 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
    • H01M10/056—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
    • 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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • 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
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • 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
    • 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

  • the present invention relates to a non-aqueous electrolyte power storage device and a method for manufacturing the same.
  • Non-aqueous electrolyte secondary batteries represented by lithium-ion non-aqueous electrolyte secondary batteries are widely used in electronic devices such as personal computers and communication terminals, automobiles, etc. due to their high energy density.
  • the non-aqueous electrolyte secondary battery generally includes an electrode body having a pair of electrodes electrically separated by a separator, and a non-aqueous electrolyte interposed between the electrodes, and transfers ions between the two electrodes. It is configured to charge and discharge by doing so.
  • capacitors such as lithium ion capacitors and electric double layer capacitors are also widely used as power storage elements other than non-aqueous electrolyte secondary batteries.
  • a lithium ion non-aqueous electrolyte secondary battery having a quick charging performance As an energy source for the above-mentioned automobiles and the like, a lithium ion non-aqueous electrolyte secondary battery having a quick charging performance is required.
  • a manganese-containing oxide having a specific composition and a spinel structure and a nickel-containing oxide having a specific composition and a layered structure are used as the positive electrode active material.
  • a technology that enables quick charging has been proposed.
  • the present invention has been made based on the above circumstances, and an object of the present invention is to provide a non-aqueous electrolyte power storage element having excellent quick charging characteristics and a method for manufacturing the same.
  • the non-aqueous electrolyte power storage element includes a negative electrode, a positive electrode, and a non-aqueous electrolyte solution, and the negative electrode has a negative electrode active material layer containing graphite and an acrylic resin, and the non-aqueous electrolysis
  • the solution contains at least one of lithium difluorooxalatoborate and lithium difluorophosphate.
  • the method for manufacturing a non-aqueous electrolyte power storage element includes accommodating a negative electrode, a positive electrode, and a non-aqueous electrolyte solution in a case, and the negative electrode includes a negative electrode active material layer containing graphite and an acrylic resin.
  • the non-aqueous electrolyte solution contains at least one of lithium difluorooxalatoborate and lithium difluorophosphate.
  • the non-aqueous electrolyte power storage element according to one aspect of the present invention is excellent in quick charging characteristics.
  • the method for manufacturing a non-aqueous electrolyte power storage element according to one aspect of the present invention can manufacture a non-aqueous electrolyte power storage element having excellent quick charging characteristics.
  • FIG. 1 is an external perspective view showing a non-aqueous electrolyte power storage element according to an embodiment of the present invention.
  • FIG. 2 is a schematic view showing a power storage device configured by assembling a plurality of non-aqueous electrolyte power storage elements according to an embodiment of the present invention.
  • the non-aqueous electrolyte power storage element includes a negative electrode, a positive electrode, and a non-aqueous electrolyte solution, and the negative electrode has a negative electrode active material layer containing graphite and an acrylic resin, and the non-aqueous electrolysis
  • the solution contains at least one of lithium difluorooxalatoborate and lithium difluorophosphate.
  • the negative electrode active material layer of the non-aqueous electrolyte storage element contains graphite as the negative electrode active material and the acrylic resin as the binder, and the non-aqueous electrolyte solution is lithium difluorooxalatoborate and lithium difluoro.
  • the quick charging performance of the non-aqueous electrolyte power storage element is excellent by containing at least one of the phosphates.
  • the reason for this is not clear, but it can be considered as follows.
  • styrene-butadiene rubber is contained as the binder for the negative electrode, it is relatively abundantly distributed on the edge surface of graphite, which is the negative electrode active material.
  • an acrylic resin is contained as the binder for the negative electrode, it is uniformly distributed around the graphite.
  • the content ratio of lithium difluorooxalatoborate or lithium difluorophosphate in the non-aqueous electrolytic solution is preferably 0.2% by mass or more and 2.0% by mass or less.
  • the content ratio of lithium difluorooxalatoborate or lithium difluorophosphate is in the above range, the quick charging performance of the non-aqueous electrolyte power storage element can be further improved.
  • the positive electrode contains a positive electrode active material containing nickel, cobalt and manganese.
  • the positive electrode contains a positive electrode active material containing nickel, cobalt and manganese, the energy density of the non-aqueous electrolyte power storage element can be improved.
  • the non-aqueous electrolyte power storage element includes a negative electrode, a positive electrode, and a non-aqueous electrolyte solution.
  • a non-aqueous electrolyte secondary battery will be described as an example of the non-aqueous electrolyte power storage element.
  • the positive electrode and the negative electrode usually form electrode bodies that are alternately superposed by stacking or winding through a separator.
  • the electrode body is housed in a case, and the case is filled with a non-aqueous electrolyte.
  • the non-aqueous electrolyte is interposed between the positive electrode and the negative electrode. Further, as the above case, a known metal case, resin case or the like which is usually used as a case of a non-aqueous electrolyte secondary battery can be used.
  • the negative electrode has a negative electrode base material and a negative electrode active material layer.
  • the negative electrode active material layer contains a negative electrode active material.
  • the negative electrode active material layer is laminated directly or via an intermediate layer along at least one surface of the negative electrode base material.
  • the negative electrode base material is a base material having conductivity.
  • metals such as copper, nickel, stainless steel and nickel-plated steel or alloys thereof are used, and copper or a copper alloy is preferable.
  • examples of the form of the negative electrode base material include foils and thin-film deposition films, and foils are preferable from the viewpoint of cost. That is, a copper foil is preferable as the negative electrode base material. Examples of the copper foil include rolled copper foil and electrolytic copper foil.
  • conductive means that the volume resistivity is measured according to JIS-H-0505 (1975 years) is not more than 1 ⁇ 10 7 ⁇ ⁇ cm, "non-conductive "means that the volume resistivity is 1 ⁇ 10 7 ⁇ ⁇ cm greater.
  • the negative electrode active material layer is laminated directly along at least one surface of the negative electrode base material or via an intermediate layer.
  • the negative electrode active material layer is formed from a so-called negative electrode mixture containing a negative electrode active material.
  • the negative electrode active material layer contains graphite and an acrylic resin.
  • the non-aqueous electrolyte power storage element contains graphite as a negative electrode active material.
  • graphite include natural graphite and artificial graphite.
  • the negative electrode active material layer may include other negative electrode active materials such as other carbon materials such as non-graphitizable carbon (hard carbon) and easily graphitizable carbon (soft carbon), semi-metals such as Si, Sn and the like.
  • the metal, these semi-metals or oxides of the metal, or a composite of these semi-metals or metals and a carbon material may be contained. These materials may be used alone or in combination of two or more. Among these, it is preferable to contain non-graphitizable carbon. By containing non-graphitizable carbon, the expansion of the negative electrode during charging can be suppressed to a small value. In addition, the shape of the negative electrode active material layer can be better and more stably maintained for a long period of time.
  • Graphite refers to a carbon material having an average lattice spacing (d 002 ) of (002) planes determined by X-ray diffraction before charging / discharging or in a discharged state of 0.33 nm or more and less than 0.34 nm.
  • Examples of graphite include natural graphite and artificial graphite. Artificial graphite is preferable from the viewpoint that a material having stable physical properties can be obtained.
  • Non-graphitic carbon refers to a carbon material having an average lattice spacing (d 002 ) of (002) planes determined by X-ray diffractometry before charging / discharging or in a discharged state of 0.34 nm or more and 0.42 nm or less.
  • Examples of non-graphitizable carbon include non-graphitizable carbon and easily graphitizable carbon.
  • the non-graphitic carbon include a resin-derived material, a petroleum pitch or a petroleum pitch-derived material, a petroleum coke or a petroleum coke-derived material, a plant-derived material, an alcohol-derived material, and the like.
  • non-graphitizable carbon refers to a carbon material having d 002 of 0.36 nm or more and 0.42 nm or less.
  • graphitizable carbon refers to a carbon material having d 002 of 0.34 nm or more and less than 0.36 nm.
  • the "discharged state” means a state in which the open circuit voltage is 0.7 V or more in a unipolar battery using a negative electrode containing a carbon material as a negative electrode active material as a working electrode and metal Li as a counter electrode. Since the potential of the metal Li counter electrode in the open circuit state is substantially equal to the oxidation-reduction potential of Li, the open circuit voltage in the single-pole battery is substantially equal to the potential of the negative electrode containing the carbon material with respect to the oxidation-reduction potential of Li. .. That is, the fact that the open circuit voltage in the single-pole battery is 0.7 V or more means that lithium ions that can be occluded and discharged are sufficiently released from the carbon material that is the negative electrode active material during charging and discharging. ..
  • the lower limit of the graphite content in the negative electrode active material is preferably 60% by mass, more preferably 70% by mass, and even more preferably 80% by mass.
  • the upper limit of this content 99% by mass is preferable, and 95% by mass is more preferable.
  • the content of the negative electrode active material in the negative electrode active material layer is not particularly limited, but the lower limit thereof is preferably 50% by mass, more preferably 80% by mass, and even more preferably 90% by mass. On the other hand, as the upper limit of this content, 99% by mass is preferable, and 98% by mass is more preferable.
  • the negative electrode mixture of the non-aqueous electrolyte power storage element contains an acrylic resin as a binder.
  • the "acrylic resin” refers to a resin formed from a monomer containing acrylic acid or methacrylic acid, or a derivative thereof as a main component.
  • Main component means that the content ratio of the structural unit derived from acrylic acid or methacrylic acid or a derivative thereof in the acrylic resin is 50% by mass or more.
  • the lower limit of the content ratio of the structural unit derived from acrylic acid or methacrylic acid or a derivative thereof in the acrylic resin is 50% by mass, preferably 60% by mass, more preferably 70% by mass, still more preferably 75% by mass.
  • acrylic resin examples include polyacrylic acid, methyl polyacrylate, polyacrylamide, a copolymer containing acrylic acid, and an alkali metal salt of polyacrylic acid, and examples thereof include polyacrylic acid, methyl polyacrylate, and polyacrylamide.
  • the alkali metal salt of polyacrylic acid is preferable, and polyacrylic acid is more preferable.
  • the copolymer containing polyacrylonitrile and acrylonitrile shall not be contained in the acrylic resin.
  • the negative electrode mixture can be used as another binder, for example, a fluororesin (polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), etc.), a thermoplastic resin such as polyethylene, polypropylene, polyacrylic acid, or polyimide; Elastomers such as propylene-diene rubber (EPDM), sulfonated EPDM, styrene-butadiene rubber (SBR), and fluororubber; and thermoplastic polymers may be contained.
  • a fluororesin polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), etc.
  • a thermoplastic resin such as polyethylene, polypropylene, polyacrylic acid, or polyimide
  • Elastomers such as propylene-diene rubber (EPDM), sulfonated EPDM, styrene-butadiene rubber (SBR), and fluororubber
  • thermoplastic polymers may
  • the binder preferably has a low content of a resin having a structural unit derived from butadiene, such as styrene-butadiene rubber (SBR), and substantially a resin having a structural unit derived from butadiene. It is more preferable not to include it.
  • SBR styrene-butadiene rubber
  • the upper limit of the mass ratio of the styrene-butadiene rubber (SBR) to the acrylic resin 2.3 is preferable, 1.5 is more preferable, 1.0 is further preferable, and 0.5 is particularly preferable. preferable.
  • the content ratio of the structural unit derived from butadiene is small.
  • the upper limit of the content ratio of the structural unit derived from butadiene in the copolymer containing the structural unit derived from acrylic acid and the structural unit derived from butadiene is preferably, for example, 50% by mass, more preferably 40% by mass. 30% by mass is even more preferable, and 25% by mass is even more preferable.
  • the acrylic resin does not have to contain a structural unit derived from butadiene from the viewpoint of improving output performance, and may contain a structural unit derived from butadiene from the viewpoint of adhesion of the negative electrode active material layer.
  • the lower limit of the content ratio of the structural unit derived from butadiene in the copolymer containing the structural unit derived from acrylic acid and the structural unit derived from butadiene may be, for example, 1% by mass, 2% by mass, 5% by mass, or In some cases, 10% by mass is preferable.
  • the content of the acrylic resin in the binder is preferably 50% by mass or more, more preferably 70% by mass or more, further preferably 80% by mass or more, further preferably 90% by mass or more, and particularly preferably 99% by mass or more. Preferably, it may be 100% by mass.
  • the lower limit of the content of the binder in the negative electrode active material layer 0.2% by mass is preferable, 0.5% by mass is more preferable, and 1% by mass is further preferable.
  • the upper limit of this content is preferably 10% by mass, more preferably 5% by mass.
  • the content of the binder in the negative electrode active material layer is preferably 0.2% by mass or more and 10% by mass or less, and more preferably 0.5% by mass or more and 5% by mass or less.
  • the negative electrode mixture contains optional components such as a conductive agent, a thickener, and a filler, if necessary.
  • the conductive agent is not particularly limited as long as it is a conductive material.
  • a conductive agent include carbonaceous materials, metals, conductive ceramics and the like.
  • the carbonaceous material include graphitized carbon, non-graphitized carbon, graphene-based carbon and the like.
  • non-graphitized carbon include carbon nanofibers, pitch-based carbon fibers, and carbon black.
  • carbon black include furnace black, acetylene black, and ketjen black.
  • Examples of graphene-based carbon include graphene, carbon nanotubes (CNT), and fullerenes.
  • the shape of the conductive agent include powder and fibrous.
  • the conductive agent one of these materials may be used alone, or two or more of these materials may be mixed and used. Further, these materials may be used in combination.
  • a material in which carbon black and CNT are composited may be used.
  • carbon black is preferable from the viewpoint of electron conductivity and coatability
  • acetylene black is particularly preferable.
  • the thickener examples include polysaccharide polymers such as carboxymethyl cellulose (CMC) and methyl cellulose.
  • CMC carboxymethyl cellulose
  • methyl cellulose examples include polysaccharide polymers such as carboxymethyl cellulose (CMC) and methyl cellulose.
  • the filler is not particularly limited.
  • the main component of the filler include polyolefins such as polypropylene and polyethylene, silica, alumina, zeolite, and glass.
  • the intermediate layer is a coating layer on the surface of the negative electrode base material, and contains conductive particles such as carbon particles to reduce the contact resistance between the negative electrode base material and the negative electrode active material layer.
  • the structure of the intermediate layer is not particularly limited and can be formed by, for example, a composition containing a resin binder and conductive particles.
  • the positive electrode has a positive electrode base material and a positive electrode active material layer.
  • the positive electrode active material layer contains a positive electrode active material.
  • the positive electrode active material layer is laminated directly or via an intermediate layer along at least one surface of the positive electrode base material.
  • the positive electrode base material is a base material having conductivity.
  • metals such as aluminum, titanium, tantalum, and stainless steel or alloys thereof are used.
  • aluminum and aluminum alloys are preferable from the viewpoint of balance of potential resistance, high conductivity and cost.
  • examples of the form of the positive electrode base material include foil, a vapor-deposited film, and the like, and foil is preferable from the viewpoint of cost. That is, aluminum foil is preferable as the positive electrode base material.
  • Examples of aluminum or aluminum alloy include A1085 and A3003 specified in JIS-H4000 (2014).
  • the positive electrode active material layer is formed from a so-called positive electrode mixture containing a positive electrode active material.
  • a positive electrode active material for example, a known positive electrode active material can be appropriately selected.
  • a material capable of occluding and releasing lithium ions is usually used.
  • the positive electrode active material include a lithium transition metal composite oxide having an ⁇ -NaFeO type 2 crystal structure, a lithium transition metal oxide having a spinel type crystal structure, a polyanion compound, a chalcogen compound, sulfur and the like.
  • lithium transition metal composite oxide having an ⁇ -NaFeO type 2 crystal structure examples include Li [Li x Ni 1-x ] O 2 (0 ⁇ x ⁇ 0.5) and Li [Li x Ni ⁇ Co (1-). x- ⁇ ) ] O 2 (0 ⁇ x ⁇ 0.5, 0 ⁇ ⁇ 1), Li [Li x Co (1-x) ] O 2 (0 ⁇ x ⁇ 0.5), Li [Li x Ni ⁇ Mn (1-x- ⁇ ) ] O 2 (0 ⁇ x ⁇ 0.5, 0 ⁇ ⁇ 1), Li [Li x Ni ⁇ Mn ⁇ Co (1-x- ⁇ - ⁇ ) O 2 ( 0 ⁇ x ⁇ 0.5, 0 ⁇ , 0 ⁇ , 0.5 ⁇ + ⁇ ⁇ 1), Li [Li x Ni ⁇ Co ⁇ Al (1-x- ⁇ - ⁇ ) ] O 2 (0 ⁇ x Examples thereof include ⁇ 0.5, 0 ⁇ , 0 ⁇ , 0.5 ⁇ +
  • Examples of the lithium transition metal oxide having a spinel-type crystal structure include Li x Mn 2 O 4 and Li x Ni ⁇ Mn (2- ⁇ ) O 4 .
  • Examples of the polyanion compound include LiFePO 4 , LiMnPO 4 , LiNiPO 4 , LiCoPO 4 , Li 3 V 2 (PO 4 ) 3 , Li 2 MnSiO 4 , Li 2 CoPO 4 F and the like.
  • the chalcogen compound include titanium disulfide, molybdenum disulfide, molybdenum dioxide and the like. The atoms or polyanions in these materials may be partially substituted with atoms or anion species consisting of other elements.
  • the lithium transition metal composite oxide is preferable as the positive electrode active material from the viewpoint of increasing energy density, and a nickel cobalt manganese-containing lithium transition metal composite containing nickel, cobalt and manganese as constituent elements in addition to Li is preferable. Oxides are more preferred.
  • the surface of the material listed as the positive electrode active material may be coated with another material.
  • one of these materials may be used alone, or two or more of these materials may be mixed and used.
  • the content of the positive electrode active material in the positive electrode active material layer is not particularly limited, but the lower limit thereof is preferably 50% by mass, more preferably 80% by mass, and even more preferably 90% by mass. On the other hand, as the upper limit of this content, 99% by mass is preferable, and 98% by mass is more preferable.
  • the positive electrode mixture contains optional components such as a binder, a conductive agent, a thickener, and a filler, if necessary.
  • binder examples include fluororesins (polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), etc.), thermoplastic resins such as polyethylene, polypropylene, polyacrylic acid, and polyimide; ethylene-propylene-diene rubber (EPDM), Elastomers such as sulfonated EPDM, styrene-butadiene rubber (SBR), fluororubber; and thermoplastic polymers can be mentioned.
  • fluororesins polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), etc.
  • thermoplastic resins such as polyethylene, polypropylene, polyacrylic acid, and polyimide
  • EPDM ethylene-propylene-diene rubber
  • SBR styrene-butadiene rubber
  • fluororubber examples of the binder can be mentioned.
  • Optional components such as conductive agent, thickener, filler, etc. can be selected from the materials exemplified in the above negative electrode.
  • the intermediate layer is a coating layer on the surface of the positive electrode base material, and contains conductive particles such as carbon particles to reduce the contact resistance between the positive electrode base material and the positive electrode active material layer.
  • the composition of the intermediate layer is not particularly limited, and can be formed by, for example, a composition containing a resin binder and conductive particles.
  • Non-aqueous electrolyte usually contains a non-aqueous solvent and an electrolyte salt dissolved in the non-aqueous solvent.
  • the non-aqueous electrolyte solution contains at least one of lithium difluorooxalatoborate and lithium difluorophosphate as additives.
  • Non-aqueous solvent can be appropriately selected from known non-aqueous solvents.
  • the non-aqueous solvent include cyclic carbonate, chain carbonate, carboxylic acid ester, phosphoric acid ester, sulfonic acid ester, ether, amide, nitrile and the like.
  • the non-aqueous solvent those in which some of the hydrogen atoms contained in these compounds are replaced with halogen may be used.
  • Cyclic carbonates include ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), vinyl ethylene carbonate (VEC), chloroethylene carbonate, fluoroethylene carbonate (FEC), difluoroethylene carbonate (DFEC), and styrene carbonate. , 1-Phenylvinylene carbonate, 1,2-diphenylvinylene carbonate and the like. Of these, EC is preferable.
  • chain carbonate examples include diethyl carbonate (DEC), dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), diphenyl carbonate, trifluoroethyl methyl carbonate, and bis (trifluoroethyl) carbonate.
  • DEC diethyl carbonate
  • DMC dimethyl carbonate
  • EMC ethyl methyl carbonate
  • diphenyl carbonate trifluoroethyl methyl carbonate
  • bis (trifluoroethyl) carbonate bis (trifluoroethyl) carbonate.
  • EMC is preferable.
  • the non-aqueous solvent it is preferable to use cyclic carbonate or chain carbonate, and it is more preferable to use cyclic carbonate and chain carbonate in combination.
  • the cyclic carbonate By using the cyclic carbonate, the dissociation of the electrolyte salt can be promoted and the ionic conductivity of the non-aqueous electrolyte solution can be improved.
  • the chain carbonate By using the chain carbonate, the viscosity of the non-aqueous electrolytic solution can be kept low.
  • the volume ratio of the cyclic carbonate to the chain carbonate is preferably in the range of, for example, 5:95 to 50:50.
  • electrolyte salt As the electrolyte salt, a known electrolyte salt usually used as an electrolyte salt of a general non-aqueous electrolyte for a power storage element can be used. Examples of the electrolyte salt include lithium salt, sodium salt, potassium salt, magnesium salt, onium salt and the like, but lithium salt is preferable.
  • lithium salt examples include inorganic lithium salts such as LiPF 6 , LiPO 2 F 2 , LiBF 4 , LiClO 4 , LiSO 3 CF 3 , LiC (SO 2 CF 3 ) 3 , LiC (SO 2 C 2 F 5 ) 3, etc.
  • inorganic lithium salts such as LiPF 6 , LiPO 2 F 2 , LiBF 4 , LiClO 4 , LiSO 3 CF 3 , LiC (SO 2 CF 3 ) 3 , LiC (SO 2 C 2 F 5 ) 3, etc.
  • examples thereof include a lithium salt having a hydrocarbon group in which hydrogen is substituted with fluorine.
  • an inorganic lithium salt is preferable, and LiPF 6 is more preferable.
  • the lower limit of the content of the electrolyte salt in the non-aqueous solution 0.1 mol / dm 3 is preferable, 0.3 mol / dm 3 is more preferable, 0.5 mol / dm 3 is further preferable, and 0.7 mol / dm 3 is preferable.
  • the upper limit is not particularly limited, but is preferably 2.5 mol / dm 3, more preferably 2 mol / dm 3, more preferably 1.5 mol / dm 3.
  • the non-aqueous solution means a state in which an electrolyte salt is dissolved in a non-aqueous solvent, and means a state before an additive such as a boron-containing oxalate complex salt is dissolved.
  • the non-aqueous electrolyte contains at least one of lithium difluorooxalatoborate and lithium difluorophosphate.
  • the non-aqueous electrolyte power storage element is excellent in quick charging characteristics.
  • the lower limit of the content of lithium difluorooxalatoborate or lithium difluorophosphate in the non-aqueous electrolyte is preferably 0.05% by mass, more preferably 0.2% by mass, further preferably 0.3% by mass, and 0. 5% by mass is even more preferable.
  • the upper limit of this content is preferably 2.0% by mass, more preferably 1.5% by mass.
  • the content of lithium difluorooxalatoborate or lithium difluorophosphate is in the above range, the effect of suppressing the increase in internal resistance after the charge / discharge cycle can be further improved.
  • the content of lithium difluorooxalatoborate or lithium difluorophosphate means the mass of lithium difluorooxalatoborate or lithium difluorophosphate with respect to the mass of the non-aqueous solution.
  • the non-aqueous electrolyte may contain both lithium difluorooxalatoborate and lithium difluorophosphate.
  • the lower limit of the sum of the contents of lithium difluorooxalatoborate and lithium difluorophosphate is preferably 0.05% by mass, preferably 0. .2% by mass is more preferable, 0.3% by mass is further preferable, and 0.4% by mass is further preferable.
  • the upper limit of this content 4.0% by mass is preferable, 3.0% by mass is more preferable, 2.0% by mass is more preferable, and 1.5% by mass is preferable in some cases.
  • the sum of the contents of lithium difluorooxalatoborate and lithium difluorophosphate is in the above range, the effect of suppressing the increase in internal resistance after the charge / discharge cycle can be further improved.
  • the sum of the contents of lithium difluorooxalatoborate and lithium difluorophosphate means the sum of the masses of lithium difluorooxalatoborate and lithium difluorophosphate with respect to the mass of the non-aqueous solution.
  • lithium difluorooxalatoborate and lithium difluorophosphate may be added to the non-aqueous electrolyte.
  • the other additives include lithium bis (fluorosulfonyl) imide (LiFSI), lithium fluorosulfonate, lithium tetrafluorooxalatrate, and the like.
  • the non-aqueous electrolyte can be obtained by dissolving at least one of the electrolyte salt, lithium difluorooxalatoborate and lithium difluorophosphate in the non-aqueous solvent.
  • separator for example, a woven fabric, a non-woven fabric, a porous resin film, or the like is used. Among these, a porous resin film is preferable from the viewpoint of strength, and a non-woven fabric is preferable from the viewpoint of liquid retention of a non-aqueous electrolyte.
  • polyolefins such as polyethylene and polypropylene are preferable from the viewpoint of strength, and polyimide and aramid are preferable from the viewpoint of oxidative decomposition resistance. Moreover, you may combine these resins.
  • An inorganic layer may be arranged between the separator and the electrode (usually the positive electrode).
  • This inorganic layer is a porous layer also called a heat-resistant layer or the like.
  • a separator having an inorganic layer formed on one surface of the porous resin film can also be used.
  • the inorganic layer is usually composed of inorganic particles and a binder, and may contain other components.
  • FIG. 1 shows a schematic view of a rectangular non-aqueous electrolyte storage element 1 (non-aqueous electrolyte secondary battery) which is an embodiment of the non-aqueous electrolyte storage element according to the present invention.
  • the figure is a perspective view of the inside of the case.
  • the electrode body 2 is housed in the case 3.
  • the electrode body 2 is formed by winding a positive electrode having a positive electrode active material layer and a negative electrode having a negative electrode active material layer around the separator.
  • the positive electrode is electrically connected to the positive electrode terminal 4 via the positive electrode current collector 4', and the negative electrode is electrically connected to the negative electrode terminal 5 via the negative electrode current collector 5'. Further, a non-aqueous electrolyte is injected into the case 3.
  • the configuration of the non-aqueous electrolyte power storage element according to the present invention is not particularly limited, and examples thereof include a cylindrical battery, a square battery (rectangular battery), and a flat battery.
  • the negative electrode, the positive electrode, and the non-aqueous electrolyte containing at least one of the above-mentioned lithium difluorooxalatoborate and lithium difluorophosphate are contained in a case.
  • the positive electrode can be obtained by laminating the positive electrode active material layer directly on the positive electrode base material or via an intermediate layer.
  • the positive electrode active material layer is laminated by applying a positive electrode mixture paste to the positive electrode base material.
  • the negative electrode can be obtained by laminating the negative electrode active material layer directly on the negative electrode base material or via an intermediate layer, similarly to the positive electrode.
  • the negative electrode active material layer is laminated by applying a negative electrode mixture paste containing graphite and an acrylic resin to the negative electrode base material.
  • the positive electrode mixture paste and the negative electrode mixture paste may contain a dispersion medium.
  • the dispersion medium for example, an aqueous solvent such as water or a mixed solvent mainly composed of water; or an organic solvent such as N-methylpyrrolidone or toluene can be used.
  • the method for manufacturing the non-aqueous electrolyte power storage element includes, for example, laminating the negative electrode and the positive electrode via a separator as another step.
  • An electrode body is formed by laminating the negative electrode and the positive electrode via a separator.
  • the method of accommodating the negative electrode, the positive electrode, the non-aqueous electrolyte, etc. in the case can be performed by a known method. After accommodating, a non-aqueous electrolyte power storage element can be obtained by sealing the accommodating port. Details of each element constituting the non-aqueous electrolyte power storage element obtained by the above manufacturing method are as described above.
  • the non-aqueous electrolyte power storage device of the present invention is not limited to the above embodiment.
  • non-aqueous electrolyte power storage element is a non-aqueous electrolyte secondary battery
  • other non-aqueous electrolyte power storage elements include capacitors (electric double layer capacitors, lithium ion capacitors) and the like.
  • non-aqueous electrolyte secondary battery include a lithium ion non-aqueous electrolyte secondary battery.
  • a laminated electrode body formed from a laminated body obtained by stacking a plurality of sheet bodies including a positive electrode, a negative electrode and a separator may be provided.
  • the present invention can also be realized as a power storage device including the plurality of non-aqueous electrolyte power storage elements.
  • the technique of the present invention may be applied to at least one non-aqueous electrolyte power storage element included in the power storage device.
  • an assembled battery can be constructed by using one or a plurality of non-aqueous electrolyte power storage elements (cells) of the present invention, and a power storage device can be further configured by using the assembled battery.
  • the power storage device can be used as a power source for automobiles such as electric vehicles (EV), hybrid electric vehicles (HEV), and plug-in hybrid vehicles (PHEV). Further, the power storage device can be used for various power supply devices such as an engine starting power supply device, an auxiliary power supply device, and an uninterruptible power supply (UPS).
  • UPS uninterruptible power supply
  • FIG. 2 shows an example of a power storage device 30 in which a power storage unit 20 in which two or more electrically connected non-aqueous electrolyte power storage elements 1 are assembled is further assembled. Even if the power storage device 30 includes a bus bar (not shown) that electrically connects two or more non-aqueous electrolyte power storage elements 1 and a bus bar (not shown) that electrically connects two or more power storage units 20. Good.
  • the power storage unit 20 or the power storage device 30 may include a condition monitoring device (not shown) that monitors the state of one or more power storage elements.
  • Example 1 to 2 and Comparative Examples 1 to 8 (Negative electrode) A coating liquid (negative electrode mixture paste) containing graphite and non-graphitizable carbon as a negative electrode active material, the binder shown in Table 1, and carboxymethyl cellulose (CMC) as a thickener, and using water as a dispersion medium. ) was prepared.
  • the mass ratio of graphite and non-graphitizable carbon in the negative electrode active material was 85:15.
  • the mixing ratio of the negative electrode active material, the binder, and the thickener was 96: 2: 2 in terms of mass ratio.
  • Non-aqueous electrolyte The content shown in Table 1 is obtained by dissolving 1.4 mol / dm 3 of LiPF 6 in a non-aqueous solvent in which ethylene carbonate (EC) and ethyl methyl carbonate (EMC) are mixed at a volume ratio of 30:70 as a non-aqueous solution.
  • EC ethylene carbonate
  • EMC ethyl methyl carbonate
  • a non-aqueous electrolyte was obtained by dissolving the additive (content ratio when the non-aqueous solution was 100% by mass).
  • lithium difluorooxalatoborate LiFOB
  • lithium difluorophosphate LiDFP
  • vinylene carbonate VC
  • lithium difluorobisoxalate phosphate LiFOP
  • lithium bisoxalatoborate LiBOB
  • the positive electrode contains the above-mentioned positive electrode active material, polyvinylidene fluoride (PVDF) as a binder, and acetylene black as a conductive agent, and uses N-methyl-2-pyrrolidone (NMP) as a dispersion medium.
  • Positive electrode mixture paste was prepared.
  • the mixing ratio of the positive electrode active material, the binder, and the conductive agent was 93: 4: 3 in terms of mass ratio.
  • the coating liquid was applied to both sides of the positive electrode base material, dried, and pressed to form a positive electrode active material layer.
  • An aluminum foil having a thickness of 15 ⁇ m was used as the positive electrode base material.
  • the positive electrode and the negative electrode were laminated via a separator made of a polyethylene base material and an inorganic layer formed on the polyethylene base material to prepare an electrode body.
  • This electrode body was housed in a square electric tank can made of aluminum, and a positive electrode terminal and a negative electrode terminal were attached.
  • the non-aqueous electrolyte was sealed, and the non-aqueous electrolyte power storage elements of Examples and Comparative Examples were obtained.
  • Examples 1 and Example contain an acrylic resin as a binder in the negative electrode active material layer and at least one of lithium difluorooxalatoborate and lithium difluorophosphate as an additive in the non-aqueous electrolyte solution. No. 2 had good quick charging performance.
  • Comparative Example 1 and Comparative Example 2 in which the non-aqueous electrolyte solution did not contain an additive, the quick charging performance was improved as compared with the examples regardless of whether the binder was an acrylic resin or a styrene-butadiene copolymer. It was inferior. Further, even if the non-aqueous electrolytic solution contains at least one of lithium difluorooxalatoborate and lithium difluorophosphate as an additive, Comparative Example 3 and Comparative Example 4 in which the binder is a styrene-butadiene copolymer have quick charging characteristics. The improvement effect of was not obtained.
  • Comparative Examples 5 to 7 in which the non-aqueous electrolyte solution contains any one of vinylene carbonate (VC), lithium difluorobisoxalate phosphate (LiFOP), and lithium bisoxalate borate (LiBOB) as an additive are binders. Although it is an acrylic resin, the effect of improving the quick charging characteristics could not be obtained.
  • the non-aqueous electrolyte power storage element is excellent in quick charging characteristics.
  • the present invention is suitably used as a non-aqueous electrolyte power storage element such as a non-aqueous electrolyte secondary battery used as a power source for personal computers, electronic devices such as communication terminals, automobiles, and the like.
  • Non-aqueous electrolyte power storage element 1
  • Electrode body 3 Case 4 Positive terminal 4'Positive current collector 5 Negative terminal 5'Negative negative current collector 20
  • Power storage unit 30 Power storage device

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Abstract

Un élément de stockage d'énergie à électrolyte non aqueux selon un aspect de la présente invention comprend une électrode négative, une électrode positive, et un électrolyte non aqueux ; l'électrode négative comprenant une couche de matériau actif d'électrode négative qui comprend du graphite et une résine acrylique, et l'électrolyte non aqueux contenant au moins du difluorooxalatoborate de lithium ou du difluorophosphate de lithium.
PCT/JP2021/000276 2020-01-08 2021-01-07 Élément de stockage d'énergie à électrolyte non aqueux et son procédé de fabrication WO2021141074A1 (fr)

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