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WO2015022858A1 - Solution électrolytique pour batteries lithium-air - Google Patents

Solution électrolytique pour batteries lithium-air Download PDF

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Publication number
WO2015022858A1
WO2015022858A1 PCT/JP2014/069971 JP2014069971W WO2015022858A1 WO 2015022858 A1 WO2015022858 A1 WO 2015022858A1 JP 2014069971 W JP2014069971 W JP 2014069971W WO 2015022858 A1 WO2015022858 A1 WO 2015022858A1
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WO
WIPO (PCT)
Prior art keywords
lithium
electrolytic solution
halide salt
solution according
air battery
Prior art date
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Ceased
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PCT/JP2014/069971
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English (en)
Japanese (ja)
Inventor
橋本　和仁
翔一 松田
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University of Tokyo NUC
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University of Tokyo NUC
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Publication date
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Publication of WO2015022858A1 publication Critical patent/WO2015022858A1/fr
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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
    • H01M12/00—Hybrid cells; Manufacture thereof
    • H01M12/04—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type
    • H01M12/06—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type with one metallic and one gaseous electrode
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M12/00—Hybrid cells; Manufacture thereof
    • H01M12/04—Hybrid cells; Manufacture thereof composed of a half-cell of the fuel-cell type and of a half-cell of the primary-cell type
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M12/00—Hybrid cells; Manufacture thereof
    • H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H01M2300/0028—Organic electrolyte characterised by the solvent
    • 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 an electrolyte for a lithium-air battery and a lithium-air battery containing the electrolyte.
  • Lithium-air batteries that use oxygen in the air as the positive electrode active material and lithium metal or the like as the negative electrode active material do not need to contain oxygen as the positive electrode active material in the battery and have a high energy density. It is expected as a power storage system in next-generation electric vehicles and solar / wind power generation facilities (for example, Patent Document 1).
  • the lithium-air battery has a mechanism that allows oxygen reduction (discharge) and oxygen generation (charge) at the positive electrode, and lithium dissolution (discharge) / deposition (charge) at the negative electrode, thereby enabling charge / discharge. Specifically, the following oxygen reduction reaction proceeds at the positive electrode.
  • the present invention uses a lithium-air battery electrolyte that can maintain a high discharge capacity even when undesirable lithium oxide is deposited on the surface of the positive electrode, and the electrolyte. It is an object of the present invention to provide a lithium-air battery.
  • the present inventors have found that the discharge capacity can be improved by adding a halide salt to the electrolytic solution, and the present invention has been completed.
  • the invention provides: (9) Lithium having a positive electrode containing oxygen as a positive electrode active material, a negative electrode containing a negative electrode active material capable of occluding and releasing lithium ions, and the electrolytic solution described in any one of (1) to (8) above -Air batteries; (10) The lithium-air battery according to (9), wherein the positive electrode includes an oxygen redox catalyst; (11) The lithium-air battery according to (9), wherein the negative electrode active material is metallic lithium, a lithium alloy, or a lithium metal oxide.
  • the present invention by adding a halide salt to the electrolytic solution, it is possible to affect the lithium oxide production process in the positive electrode and improve the conductivity of the lithium oxide. Thereby, the electric potential fall in the discharge reaction of a positive electrode is suppressed, and the improvement of the energy capacity of a battery is achieved. Therefore, the improvement in the energy density of the lithium air battery is beneficial in applications in secondary batteries such as automobile batteries and storage batteries.
  • FIG. 1 is a graph showing anion dependence of a discharge curve (chronopotentiometry) in a halide salt / LiTFSA / DME electrolyte.
  • FIG. 2 is a graph showing the cation dependence of a discharge curve (chronopotentiometry) in a halide salt / LiTFSA / DME electrolyte solution.
  • FIG. 3 is a graph showing the salt concentration dependence of the discharge curve (chronopotentiometry) in the halide salt / LiTFSA / DME electrolyte.
  • FIG. 4 is a graph showing a charge / discharge curve in the LiPF 6 / TEGDME electrolytic solution.
  • FIG. 5 is a graph showing a discharge curve (chronopotentiometry) in a LiPF 6 / TEGDME electrolyte and a Nyquist plot by impedance measurement.
  • the halide salt used in the electrolytic solution of the present invention can be a fluoride salt, a chloride salt, or a bromide salt, but is preferably a chloride salt.
  • the cation constituting the halide salt is preferably tetraalkylammonium, N-alkylpyridinium, or N, N-dialkylpyrrolidinium.
  • the alkyl can be a C 1 -C 10 alkyl, preferably C 1 -C 4 .
  • the cation is more preferably tetraethylammonium, N-butylpyridinium, or N-methyl-N-butylpyrrolidinium, and most preferably tetraethylammonium.
  • the halide salt is preferably tetraethylammonium chloride, N-butylpyridinium chloride, N-methyl-N-butylpyrrolidinium chloride, and most preferably tetraethylammonium chloride.
  • the concentration of the halide salt in the electrolytic solution of the present invention can be any concentration up to the saturation concentration as long as the effect of the present invention is obtained. Although it depends on the solvent to be used later, it is preferably 0.5 to 5 mM, more preferably 1 to 3 mM.
  • the non-aqueous solvent can be used for the solvent used in the electrolyte solution of this invention, Preferably it is an aprotic organic solvent.
  • the non-aqueous solvent include ethylene carbonate (EC), propylene carbonate (PC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), ethyl carbonate, butylene carbonate, ⁇ -butyrolactone, sulfolane.
  • 1,2-dimethoxymethane, 1,2-dimethoxyethane (DME), tetraethyl glycol dimethyl ether (TEGDME), 1,3-dimethoxypropane, diethyl ether, tetrahydrofuran, 2-methyltetrahydrofuran, dimethyl sulfoxide (DMSO) Can be mentioned. Among these, one type may be used alone, or two or more types may be used in combination. However, it is not limited to these. In particular, 1,2-dimethoxyethane (DME) or tetraethyl glycol dimethyl ether (TEGDME) is preferred.
  • the non-aqueous solvent is preferably a solvent having high oxygen solubility from the viewpoint that dissolved oxygen can be efficiently used for the reaction.
  • a low-volatile liquid such as an ionic liquid such as N-methyl N-butylpyrrolidinium bis (trifluoromethanesulfonyl) imide, tetraethylammonium bistrifluoromethanesulfonylimide, or the like can be used.
  • It can also be used in the form of a non-aqueous gel electrolyte in which a polymer is added to the non-aqueous electrolyte and gelled. This can be obtained by adding a polymer such as polyethylene oxide (PEO), polyacrylonitrile (PAN), or polymethyl methacrylate (PMMA) to the electrolytic solution of the present invention and gelling.
  • PEO polyethylene oxide
  • PAN polyacrylonitrile
  • PMMA polymethyl methacrylate
  • the electrolytic solution of the present invention can contain a supporting electrolyte salt generally used in lithium-air batteries. Specifically, lithium that dissociates in the electrolytic solution and supplies lithium ions.
  • Salt The lithium salt.
  • the lithium salt is not particularly limited, and examples thereof include LiPF 6 , LiN (CF 3 SO 2 ) 2 (“LiTFSA”), LiN (C 2 F 5 SO 2 ) 2 (“LiBETI”), LiCF 3 SO 3 , LiC 4 F 9 SO 3 , LiC (CF 3 SO 2 ) 3 , LiN (CF 3 SO 2 ) (C 2 F 5 SO 2 ), LiN (CF 3 SO 2 ) (C 3 F 7 SO 2 ), LiN (CF 3 SO 2 ) (C 4 F 9 SO 2 ), LiN (SO 2 F) 2 , LiBF 4 , LiClO 4 , and any combination thereof.
  • the concentration range of the lithium salt in the electrolytic solution can be generally used, and can be appropriately adjusted by those skilled in the art.
  • the said electrolyte solution can also contain another component as needed for the purpose of the improvement of the function.
  • the other components include conventionally known overcharge inhibitors, dehydrating agents, deoxidizing agents, and property improving aids.
  • overcharge inhibitor examples include aromatic compounds such as biphenyl, alkylbiphenyl, terphenyl, partially hydrogenated terphenyl, cyclohexylbenzene, t-butylbenzene, t-amylbenzene, diphenyl ether, and dibenzofuran; 2-fluoro Partially fluorinated products of the above aromatic compounds such as biphenyl, o-cyclohexylfluorobenzene, p-cyclohexylfluorobenzene; fluorinated anisole such as 2,4-difluoroanisole, 2,5-difluoroanisole and 2,6-difluoroaniol Compounds.
  • An overcharge inhibitor may be used individually by 1 type, and may use 2 or more types together.
  • the content of the overcharge inhibitor in the electrolytic solution is preferably 0.01 to 5% by mass.
  • the overcharge inhibitor in the electrolytic solution it becomes easier to suppress the rupture / ignition of the secondary battery due to overcharge, and the secondary battery can be used more stably.
  • the dehydrating agent examples include molecular sieves, sodium sulfate, magnesium sulfate, calcium hydride, sodium hydride, potassium hydride, lithium aluminum hydride and the like.
  • a solvent obtained by performing rectification after dehydrating with the dehydrating agent can be used. Moreover, you may use the solvent which performed only the dehydration by the said dehydrating agent, without performing rectification.
  • the property improving aid examples include succinic anhydride, glutaric anhydride, maleic anhydride, citraconic anhydride, glutaconic anhydride, itaconic anhydride, diglycolic anhydride, cyclohexanedicarboxylic anhydride, cyclopentanetetracarboxylic acid Carboxylic anhydrides such as anhydrides and phenylsuccinic anhydrides; ethylene sulfite, 1,3-propane sultone, 1,4-butane sultone, methyl methanesulfonate, busulfan, sulfolane, sulfolene, dimethyl sulfone, diphenyl sulfone, methyl Sulfur-containing compounds such as phenylsulfone, dibutyl disulfide, dicyclohexyl disulfide, tetramethylthiuram monosulfide, N, N-dimethylmethanesul
  • Hydrocarbon compounds such as fluorobenzene, difluorobenzene, hexafluorobenzene, benzotrifluoride and the like can be mentioned.
  • These characteristic improvement aids may be used alone or in combination of two or more.
  • the content of the characteristic improving auxiliary in the electrolytic solution is preferably 0.01 to 5% by mass.
  • the positive electrode can be one that is normally used as a positive electrode of an air battery, includes a conductive material having a gap through which oxygen and lithium ions can move, and may contain a binder. Moreover, you may contain the catalyst which accelerates
  • conductive material for example, carbon materials, conductive fibers such as metal fibers, metal powders such as copper, silver, nickel, and aluminum, and organic conductive materials such as polyphenylene derivatives can be used.
  • carbon material graphite, soft carbon, hard carbon, carbon black, ketjen black, acetylene black, graphite, activated carbon, carbon nanotube, carbon fiber and the like can be used.
  • mesoporous carbon obtained by firing a synthetic resin containing an aromatic ring, petroleum pitch or the like can be used.
  • fluorine resins such as polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), ethylenetetrafluoroethylene (ETFE), polyethylene, polypropylene, or the like can be preferably used.
  • the negative electrode current collector is not particularly limited as long as it has conductivity, but a rod-like body, a plate-like body, a foil-like body, a net-like body mainly composed of copper, nickel, aluminum, stainless steel or the like. Etc. can be used.
  • MnO 2 , Fe 2 O 3 , NiO, CuO, Pt, Co, or the like can be used as a catalyst for performing an oxygen redox reaction with high efficiency.
  • a porous body such as a mesh (grid) metal, a sponge (foamed) metal, a punched metal, or an expanded metal is used in order to increase the diffusion of oxygen.
  • the metal include copper, nickel, aluminum, and stainless steel.
  • the negative electrode in the lithium-air battery of the present invention is an electrode containing a negative electrode active material capable of electrochemically inserting and extracting lithium ions.
  • Examples of such a negative electrode active material include lithium metal or an alloy containing a lithium element, a metal oxide, and a metal nitride.
  • examples of the alloy having a lithium element include a lithium aluminum alloy, a lithium tin alloy, a lithium lead alloy, and a lithium silicon alloy.
  • the metal oxide having a lithium element can be, for example, lithium titanium oxide (Li 4 Ti 6 O 12, etc.) and the like.
  • examples of the metal nitride containing a lithium element include lithium cobalt nitride, lithium iron nitride, and lithium manganese nitride.
  • Carbonaceous materials such as natural graphite (graphite), highly oriented graphite (HOPG), and amorphous carbon can also be used. These negative electrode active materials may be used individually by 1 type, and may use 2 or more types together.
  • the negative electrode layer in the present invention may contain only the negative electrode active material, or may contain at least one of a conductive material and a binder in addition to the negative electrode active material.
  • a negative electrode active material has a foil shape
  • a negative electrode containing only the negative electrode active material can be obtained.
  • the negative electrode active material is in a powder form, a negative electrode having a negative electrode active material and a binder (binder) can be obtained.
  • a doctor blade method, a molding method using a pressure press, or the like can be used as a method for forming a negative electrode using a powdered negative electrode active material.
  • the same materials as the positive electrode can be used.
  • the separator used in the lithium-air battery of the present invention is not particularly limited as long as it has a function of electrically separating the positive electrode layer and the negative electrode layer.
  • PE polyethylene
  • a porous sheet made of a resin such as polypropylene (PP), polyester, cellulose, or polyamide, or a porous insulating material such as a nonwoven fabric such as a nonwoven fabric or a glass fiber nonwoven fabric.
  • the shape of the lithium-air battery of the present invention is not particularly limited as long as it can accommodate a positive electrode, a negative electrode, and an electrolyte solution.
  • a cylindrical shape, a coin shape, a flat plate shape, a laminate Examples include molds.
  • the battery housing case may be an open-air battery case or a sealed battery case.
  • the battery case In the case of a battery case that is open to the atmosphere, the battery case has a vent hole through which the atmosphere can enter and exit, and the atmosphere can contact the air electrode.
  • the battery case is a sealed battery case, it is preferable to provide a gas (air) supply pipe and a discharge pipe in the sealed battery case.
  • the gas to be supplied / exhausted is preferably a dry gas, in particular, preferably has a high oxygen concentration, and more preferably pure oxygen (99.99%).
  • the electrolyte solution and lithium-air battery of the present invention are suitable for use as a secondary battery, but use of a primary battery is not excluded.
  • FIG. 1 shows a comparison of discharge curves obtained when the cation component of a halide salt is fixed to tetraethylammonium (TEA) and different anion components are used.
  • the halide salts used here are tetraethylammonium chloride (TEA-Cl), tetraethylammonium bromide (TEA-Br), and tetraethylammonium sulfonate (TEA-sulfo) as a comparative example, each having a concentration of 1 mM. is there.
  • the solvent is 1,2-dimethoxyethane (DME), and the lithium salt is LiTFSA. From the results of FIG. 1, it was found that the discharge capacity was most improved in the case of TEACl, which was about 330 mC.
  • FIG. 2 shows a comparison of discharge curves obtained when the anion component of the halide salt is fixed to chloride (Cl ⁇ ) and different cation components are used.
  • the halide salts used here are tetraethylammonium chloride (TEA-Cl), tetramethylammonium chloride (TMA-Cl), tetraamylammonium chloride (TAA-Cl), N-butylpyridinium chloride (BP-Cl), chloride N-methyl-N-butylpyrrolidinium (MBP-Cl), each having a concentration of 1 mM.
  • the solvent is 1,2-dimethoxyethane (DME), and the lithium salt is LiTFSA.
  • FIG. 3 shows the result of measuring the concentration dependence of TEA-Cl in which the most remarkable improvement in discharge capacity was observed.
  • the solvent is 1,2-dimethoxyethane (DME), and the lithium salt is LiTFSA. From FIG. 3, it was found that the discharge capacity was improved at 0.5 mM, and the greatest improvement was obtained at 1.0 mM.
  • FIG. 4 shows charging / discharging curves with and without addition of TEA-Cl.
  • the solvent tetraethyl glycol dimethyl ether (TEGDME), the lithium salt is LiPF 6.
  • TEGDME solvent tetraethyl glycol dimethyl ether
  • the TEA-Cl reduced the overvoltage in both charging and discharging. This is thought to be because the Li—O bond present on the positive electrode surface is weakened by the TEA cation during charging, while the Cl ⁇ anion acts on the desolvation of Li + ions during discharge. It is thought that this is because.
  • Impedance comparison As shown in FIG. 5, when TEA-Cl was added and when it was not added, impedance was compared when TEA-Cl was added and when TEA-Cl was added using Nyquist plot. The decrease in ion impedance at the time of addition indicates that the improvement in the discharge capacity is due to the fact that the electronic conductivity of Li 2 O 2 deposited on the positive electrode surface is increased by TEA-Cl.

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

Abstract

Le problème à résoudre dans le cadre de la présente invention consiste à fournir : une solution électrolytique pour batteries lithium-air qui peut conserver une capacité de décharge élevée même dans des cas où un oxyde de lithium indésirable est déposé sur une surface d'électrode positive; et une batterie lithium-air qui utilise la solution électrolytique. La solution proposée consiste en une solution électrolytique pour batteries lithium-air qui contient un solvant non aqueux et un sel d'halogénure; et une batterie lithium-air qui comprend la solution électrolytique.
PCT/JP2014/069971 2013-08-15 2014-07-29 Solution électrolytique pour batteries lithium-air Ceased WO2015022858A1 (fr)

Applications Claiming Priority (2)

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JP2013-168765 2013-08-15
JP2013168765A JP2016181325A (ja) 2013-08-15 2013-08-15 リチウム−空気電池用電解液

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WO2015022858A1 true WO2015022858A1 (fr) 2015-02-19

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH05258782A (ja) * 1992-03-13 1993-10-08 Hitachi Ltd 空気電池
JPH06310182A (ja) * 1993-04-27 1994-11-04 Shigeyuki Yasuda 電気化学的発電装置
JP2011108388A (ja) * 2009-11-13 2011-06-02 Nippon Telegr & Teleph Corp <Ntt> リチウム空気電池
WO2011074325A1 (fr) * 2009-12-16 2011-06-23 トヨタ自動車株式会社 Sel fondu à température normale, électrode, cellule, agent permettant d'empêcher la recharge, et procédé d'observation d'un échantillon
JP2013527567A (ja) * 2010-04-23 2013-06-27 リオクス パワー インコーポレイテッド 充電式金属空気電池のための可溶性酸素発生触媒

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH05258782A (ja) * 1992-03-13 1993-10-08 Hitachi Ltd 空気電池
JPH06310182A (ja) * 1993-04-27 1994-11-04 Shigeyuki Yasuda 電気化学的発電装置
JP2011108388A (ja) * 2009-11-13 2011-06-02 Nippon Telegr & Teleph Corp <Ntt> リチウム空気電池
WO2011074325A1 (fr) * 2009-12-16 2011-06-23 トヨタ自動車株式会社 Sel fondu à température normale, électrode, cellule, agent permettant d'empêcher la recharge, et procédé d'observation d'un échantillon
JP2013527567A (ja) * 2010-04-23 2013-06-27 リオクス パワー インコーポレイテッド 充電式金属空気電池のための可溶性酸素発生触媒

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