EP2583335A1 - Batterie aux ions lithium comprenant des matières d'électrode amorphes - Google Patents

Batterie aux ions lithium comprenant des matières d'électrode amorphes

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Publication number
EP2583335A1
EP2583335A1 EP11721717.4A EP11721717A EP2583335A1 EP 2583335 A1 EP2583335 A1 EP 2583335A1 EP 11721717 A EP11721717 A EP 11721717A EP 2583335 A1 EP2583335 A1 EP 2583335A1
Authority
EP
European Patent Office
Prior art keywords
lithium
ion battery
separator
battery according
oxide
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP11721717.4A
Other languages
German (de)
English (en)
Inventor
Tim Schaefer
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Li Tec Battery GmbH
Original Assignee
Li Tec Battery GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Li Tec Battery GmbH filed Critical Li Tec Battery GmbH
Publication of EP2583335A1 publication Critical patent/EP2583335A1/fr
Withdrawn legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—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
    • 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
    • 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
    • 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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/5805—Phosphides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/581—Chalcogenides or intercalation compounds thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/581—Chalcogenides or intercalation compounds thereof
    • H01M4/5815—Sulfides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/44—Fibrous material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/491—Porosity
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • H01M50/494—Tensile strength
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
    • 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 rechargeable lithium-ion battery having a positive electrode, which comprises at least one amorphous chalcogenide, in particular an oxide, which comprises lithium ions or which can conduct lithium ions.
  • Secondary batteries can be used as energy storage for mobile information devices because of their high energy density and high capacity. They are also used for tools, electric cars and hybrid cars.
  • the batteries are subject to high demands in terms of electrical capacity and energy density. They should remain stable, especially in the charge and discharge cycle, i. to suffer the least possible loss of electrical capacity. In addition, they should be rechargeable quickly. Rapid chargeability is particularly desirable for use in electrically powered automobiles to improve the usability of these cars.
  • WO 99/59218 discloses a secondary battery having two electrodes which are interconnected by an electrolyte, wherein the active material in at least one of the electrodes comprises an oxide or chalcogenide or a lithium-containing oxide or chalcogenide of the transition metals.
  • the negative electrode may include, for example, amorphous or crystalline lithium manganate.
  • separator insulating ceramic glass or polypropylene are called. It is also known to use an anode of lithium metal and a cathode of a glassy (amorphous) lithium iron phosphate to increase the charging speed of a battery (Kang, B. and Ceder, G., "Batten / materials for ultrafast charging and discharging", Nature, Vol. 458, pages 190-193 (March 12, 2009)).
  • the object of the present invention is to provide a rechargeable lithium-ion battery with improved charging characteristics.
  • the charging speed should be increased compared to conventional lithium-ion batteries.
  • a rechargeable lithium-ion battery comprising:
  • a positive electrode comprising at least one amorphous chalcogenide which comprises lithium ions or which can conduct lithium ions;
  • the amorphous chalcogenide is one
  • Lithium-containing compound of one or more of the chalcogen elements oxygen, sulfur, selenium and tellurium; or
  • a lithium-containing compound of one or more of the chalcogen elements oxygen, sulfur, selenium and tellurium with one or more metals, transition metals, arsenic, germanium, phosphorus, antimony, boron, in particular lead, aluminum, gallium, indium, titanium; or
  • a compound of one or more of the chalcogen elements oxygen, sulfur, selenium and tellurium with one or more metals, transition metals, arsenic, germanium, phosphorus, antimony, Boron, in particular lead, aluminum, gallium, indium, titanium, which can conduct lithium ions.
  • the elements contained in the amorphous chalcogenide are not present in a stoichiometric ratio.
  • the amorphous chalcogenide is selected from a lithium phosphate; a lithium phosphate containing a transition metal; a mixed oxide of lithium oxide and one or more transition metal oxides; a transition metal oxide which can conduct lithium ions; or a mixture of two or more thereof.
  • the amorphous chalcogenide is present as a coating on the positive electrode (a).
  • the positive electrode (a) comprises, in addition to the amorphous chalcogenide, a crystalline oxide which comprises lithium ions or which can conduct lithium ions.
  • the crystalline chalcogenide is selected from: lithium manganate, lithium nickelate, lithium cobaltate, or a mixed oxide of two or more of these oxides; Lithium iron phosphate.
  • the negative electrode (b) comprises carbon and / or lithium titanate.
  • the positive electrode comprises, in addition to the amorphous chalcogenide, sulfur and / or a lithium sulfide and the negative electrode lithium metal or a lithium alloy.
  • the fibers of the nonwoven fabric are formed as polymer fibers.
  • the polymer fibers are selected from the group of polymers consisting of polyester, polyolefin, polyamide, polyacrylonitrile, polyimide, polyetherimide, polysulfone, polyamideimide, polyether, polyphenylene sulfide, aramid, or mixtures of two or more of these polymers.
  • the polymer fibers comprise a polyethylene terephthalate.
  • the separator (c) consists of an at least partially permeable carrier, which is not or only poorly electron-conducting, wherein the carrier is coated on at least one side with an inorganic material, using as an at least partially permeable carrier an organic material is configured as a non-woven fabric, wherein the organic material is configured in the form of polymer fibers, preferably polymer fibers of polyethylene terephthalate (PET), wherein the web is coated with an inorganic ion-conductive material, which preferably in a temperature range of 40 ° C.
  • PET polyethylene terephthalate
  • the inorganic ion-conductive material preferably comprises at least one compound from the group of oxides, phosphates, sulfates, titanates, silicates, aluminosilicates with at least one of the elements zirconium, aluminum, lithium, particularly preferably zirconium oxide, wherein preferably the inorganic ion-conducting material has particles with a maximum diameter below 100 nm.
  • the battery is located between the separator (c) and the positive electrode (a) and / or between the separator (c) and the negative electrode (b) a polymer layer which is formed as a film or as a non-woven.
  • the polymer layer comprises a polyolefin.
  • the electrolyte comprises an organic solvent and a conducting salt.
  • the organic solvent is selected from ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, methyl propyl carbonate, butyl methyl carbonate, ethyl propyl carbonate, dipropyl carbonate, cyclopentanones, sulfolanes, dimethyl sulfoxide, 3-methyl-1,3-oxazolidine-2-one , ⁇ -butyrolactone, 1,2-diethoxymethane, tetrahydrofuran, 2-methyltetrahydrofuran, 1,3-dioxolane, methyl acetate, ethyl acetate, nitromethane, 1,3-propanesultone, and mixtures of two or more of these solvents.
  • the conducting salt is selected from LiPF 6 , LiBF 4 , LiClO 4 , LiAsF 6 , LiCF 3 S0 3 , LiN (CF 3 S0 2 ) 2 , LiC (CF 3 S0 2 ) 3 , LiS0 3 C x F 2x + i, LiN (S0 2 C x F 2x + i) 2 or LiC (S0 2 C x F 2x + i) 3 with 0 ⁇ x ⁇ 8, Li [(C 2 O 4 ) 2 B], and mixtures of two or more of these salts.
  • means for cooling in or on the battery are provided.
  • the invention also relates to a lithium-ion battery comprising:
  • a positive electrode comprising sulfur and / or a lithium sulfide and at least one amorphous chalcogenide which comprises lithium ions or which can conduct lithium ions;
  • Lithium alloy (c) a separator between the positive and negative electrodes; wherein the separator comprises a porous membrane, a ceramic electrolyte separator, a glass electrolyte separator, or a polymeric electrolyte;
  • the invention also relates to the use of the lithium-ion battery for powering mobile information devices, tools, electrically powered automobiles, and hybrid-powered automobiles.
  • lithium ion battery includes terms such as “lithium ion secondary battery” “lithium ion secondary battery”, “lithium ion cell”, “lithium sulfur battery”, “lithium sulfide” “Battery”, “Lithium Sulfur Battery”, “Lithium Sulfur Cell” and the like, which means that the term “lithium ion battery” is used as a generic term for the terms commonly used in the art for this battery type becomes.
  • chalcogenide means an oxide, sulfide, selenide or telluride.
  • the term also includes chemical compounds of one or more of the chalcogen elements oxygen, sulfur, selenium and tellurium with one or more metals, transition metals, arsenic, germanium, phosphorus, Antimony, boron, especially lead, aluminum, gallium, indium, titanium.
  • amorphous means that an X-ray diffractogram preferably has a broad scattering band peaking at 2 ⁇ in the range of 20 to 70 ° using CuKa radiation, but the X-ray diffractogram may have one or more diffraction lines attributed to crystalline structures. Then, the maximum intensity of the crystalline diffraction line observed at 2 ⁇ in the range of 20 to 70 ° is preferably not more than 500 times, more preferably not more than 100 times, especially not more than 5 times that Intensity of the peak of the broad scattering range observed at 2 ⁇ in the range of 20 to 70 ° becomes. Most preferably, no diffraction line is observed which can be assigned to a crystalline region.
  • the amorphous character of the chalcogenide can also be confirmed by transmission electron microscopy, differential calorimetry or FTIR absorption spectra.
  • the methods are known to the person skilled in the art.
  • Condition for the amorphous state is that in the preparation of the chalcogenide, the elements contained therein can not regularly order, that is, it must not come to crystallization. Therefore, sintering processes for the production of the amorphous chalcogenides are particularly well suited.
  • chalcogenides can also be amorphous if the elements contained therein are present in a non-stoichiometric ratio. Instead of the term “amorphous” can synonymously also the term “glassy” (English: “vitreous", “glassy”) are used.
  • chalcogenide ... which can guide lithium ions means that the chalcogenide conducts lithium ions under the electrochemical processes taking place in the battery.
  • transition metal means the elements including their cations with atomic numbers 21 to 30, 39 to 48, 57 to 80 of the Periodic Table of the Chemical Elements.
  • crystalline means that the maximum intensity of the crystalline diffraction line observed at 2 ⁇ in the range of 20 to 70 ° is preferably more than 500 times the intensity of a broad scattering peak at 2 ⁇ in the range of 20 to 70 ° is.
  • nonwoven means a sheet of fibers, especially of polymer fibers, by definition the fibers are unwoven, so that the nonwoven is unwoven and the term “non-woven” is used instead of the term “nonwoven.”
  • nonwoven fabrics or “non-woven material”.
  • nonwoven is used synonymously with the term “nonwoven fabric”.
  • nonwoven is also synonymous with "w / 'r / ce” with terms such or "felt” is used.
  • positive electrode defines the electrode of the Battery that absorbs electrons when discharged, ie when connected to a consumer. It is the cathode under these conditions.
  • negative electrode defines the electrode of the battery, which emits electrons when discharged, ie when connected to a consumer, and is the anode under these conditions.
  • a first aspect of the invention relates to a lithium-ion battery comprising:
  • a positive electrode comprising at least one amorphous chalcogenide, preferably an oxide which comprises lithium ions or which can conduct lithium ions;
  • the lithium-ion battery is characterized in that the amorphous oxide is selected from a lithium phosphate; a lithium phosphate containing a transition metal; a mixed oxide of lithium oxide and one or more transition metal oxides; a transition metal oxide which can conduct lithium ions; or a mixture of two or more thereof.
  • the preparation of the amorphous oxide is known or can be carried out by known methods, for example by sintering methods in which suitable Starting compounds, which lead to the amorphous oxide, are reacted together.
  • suitable Starting compounds which lead to the amorphous oxide, are reacted together.
  • the presence of an amorphous phase can be checked as described above, for example by X-ray diffractometry or by differential scanning calorimetry (DSC) in a known manner.
  • DSC differential scanning calorimetry
  • Mixed oxides are preferably prepared by reacting the individual oxides with each other, preferably by sintering.
  • the individual components are preferably used in proportions that do not lead to a stoichiometric presence of the individual oxides in the mixed oxide.
  • the amorphous oxide is a lithium iron phosphate.
  • Processes for the production of amorphous lithium iron phosphates are known, for example, from the document cited in the prior art and from "Material Science-Poland, Vol. 1, 2009 (The thermal stability, local structure and electrical properties of lithium-iron phosphate glasses) "known.
  • the amorphous chalcogenide preferably an oxide
  • amorphous oxide is present as a coating on the positive electrode (a).
  • the electrode includes, in addition to the amorphous oxide, other components that can assist in the electrochemical processes occurring in the battery.
  • the lithium-ion battery is characterized in that the positive electrode (a) comprises, in addition to the amorphous oxide: a crystalline oxide which comprises lithium ions or which can conduct lithium ions.
  • the cathode (a) of the battery according to the invention preferably comprises a crystalline compound having the formula LiMP0 4 , wherein M is at least one transition metal cation of the elements of atomic numbers 21 to 30 of the Periodic Table of the Elements, this transition metal cation preferably from the group consisting of Mn , Fe, Ni and Ti or a combination of these elements, and wherein the compound preferably has an olivine structure, preferably higher olivine, with Fe being particularly preferred.
  • a lithium iron phosphate with olivine structure of the empirical formula LiFeP0 4 can be used.
  • the positive electrode contains the crystalline lithium phosphate or lithium iron phosphate as defined above, preferably in the form of nanocrystalline particles.
  • the nanoparticles can take any shape, that is, they can be coarse-spherical or elongated.
  • the lithium phosphate or lithium iron phosphate has a particle size measured as D 95 value of less than 15 pm.
  • the particle size is less than 10 ⁇ .
  • the lithium phosphate or lithium iron phosphate has a particle size measured as D 95 value between 0.005 pm to 10 pm.
  • the lithium phosphate or lithium iron phosphate has a particle size measured as D 95 value of less than 10 pm, wherein the D 50 value is 4 pm ⁇ 2 pm and the D 0 value is less than 1, 5 pm.
  • the cathode may also comprise a lithium manganate, preferably spinel-type LiMn 2 O 4 , a lithium cobaltate, preferably LiCoO 2 , or a lithium nickelate, preferably LiNiO 2 , or a mixture of two or three of these oxides, or a lithium mixed oxide, which contains nickel, manganese and cobalt (NMC) include.
  • a lithium manganate preferably spinel-type LiMn 2 O 4
  • a lithium cobaltate preferably LiCoO 2
  • a lithium nickelate preferably LiNiO 2
  • a lithium mixed oxide which contains nickel, manganese and cobalt (NMC) include.
  • the cathode comprises in a preferred embodiment at least one active material of a lithium-nickel-manganese-cobalt mixed oxide (NMC), which is not in a spinel structure, in a mixture with a lithium manganese oxide (LMO) in spinel structure.
  • NMC lithium-nickel-manganese-cobalt mixed oxide
  • LMO lithium manganese oxide
  • the active material comprises at least 30 mol%, preferably at least 50 mol% NMC and at least 10 mol%, preferably at least 30 mol% LMO, in each case based on the total moles of the active material of the cathodic electrode (ie not based on the cathodic electrode as a whole, which in addition to the active material may also comprise conductivity additives, binders, stabilizers, etc.).
  • NMC and LMO together account for at least 60 mole% of the active material, more preferably at least 70 mole%, more preferably at least 80 mole%, even more preferably at least 90 mole%, each based on the total moles of active material of the cathodic electrode (ie not based on the total cathodic electrode, which in addition to the active material may also comprise conductivity additives, binders, stabilizers, etc.).
  • the composition of the lithium-nickel-manganese-cobalt mixed oxide there are no restrictions with respect to the composition of the lithium-nickel-manganese-cobalt mixed oxide, except that this oxide in addition to lithium at least 5 mol%, preferably in each case at least 15 mol%, more preferably in each case at least 30 mol% of nickel, manganese and cobalt must contain, in each case based on the total number of moles of transition metals in the lithium-nickel-manganese-cobalt mixed oxide.
  • the lithium-nickel-manganese-cobalt mixed oxide can be doped with any other metals, in particular transition metals, as long as it is ensured that the abovementioned molar minimum amounts of Ni, Mn and Co are present.
  • a lithium-nickel-manganese-cobalt mixed oxide of the following stoichiometry is particularly preferred: Li [Co 1/3 Mn 1 3 Ni 3] O 2, the proportion of Li, Co, Mn, Ni and O in each case being + / - 5 mol% may vary.
  • the lithium phosphate or lithium iron phosphate or lithium oxide (s) used and the materials used for the negative electrode (a) are generally held together by a binder holding these materials on the electrode , For example, polymeric binders can be used.
  • polyvinylidene fluoride polyethylene oxide, polyethylene, polypropylene, polytetrafluoroethylene, polyacrylate, ethylene (propylene-diene monomer) copolymer (EPDM), and mixtures and copolymers thereof may preferably be used.
  • the lithium-ion battery is also characterized in that the crystalline oxide is selected from: a lithium manganate, a lithium nickelate, a lithium cobaltate, or a mixed oxide of two or more of these oxides; a lithium iron phosphate.
  • the anode (b) of the battery of the invention may be made of a variety of materials suitable for use with a lithium ion electrolyte battery.
  • the negative electrode may contain lithium metal or lithium in the form of an alloy, either in the form of a foil, a grid, or in the form of particles held together by a suitable binder.
  • the use of lithium metal oxides such as lithium titanium oxide is also possible. In principle, all materials which are capable of forming lithium intercalation compounds can be used.
  • Suitable materials for the negative electrode then include, for example: graphite, synthetic graphite, carbon black, mesocarbon, doped carbon, fullerenes, niobium pentoxide, tin alloys, titanium dioxide, tin dioxide, and mixtures of these substances.
  • the separator (c) used for the battery must be permeable to lithium ions to ensure ion transport for lithium ions between the positive and negative electrodes. On the other hand, the separator must be insulating for electrons.
  • the separator of the battery according to the invention comprises a web of unwoven fibers, preferably nonwoven polymer fibers. Preferably, the nonwoven is flexible and has a thickness of less than 30 pm. Methods for producing such nonwovens are known in the art.
  • the polymer fibers are selected from the group of polymers consisting of polyacrylonitrile, polyolefin, polyester, polyimide, polyether imide, polysulfone, polyamide, polyether.
  • Suitable polyolefins are, for example, polyethylene, polypropylene, polytetrafluoroethylene, polyvinylidene fluoride.
  • Preferred polyesters are preferably polyethylene terephthalates.
  • the separator comprises a nonwoven, which is coated on one or both sides with an inorganic material.
  • coating also includes that the ionic conductive inorganic material may be located not only on one side or both sides of the web, but also within the web.
  • the material used for the coating is preferably at least one compound from the group of oxides, phosphates, sulfates, titanates, silicates, aluminosilicates at least one of zirconium, aluminum or lithium.
  • the ion-conductive inorganic material is preferably ion-conducting in a temperature range of -40 ° C to 200 ° C, i. ion-conducting for the lithium ions.
  • the ion-conducting material comprises or consists of zirconium oxide.
  • a separator may be used, which consists of an at least partially permeable carrier, which is not or only poorly electron-conducting.
  • This support is coated on at least one side with an inorganic material.
  • an organic material is used, which is designed as non-woven web.
  • the organic material is in the form of polymer fibers, preferably polymer fibers of polyethylene terephthalate (PET).
  • PET polyethylene terephthalate
  • the nonwoven fabric is coated with an inorganic ion-conducting material which is preferably ion-conducting in a temperature range of -40 ° C to 200 ° C.
  • the inorganic ion-conducting material preferably comprises at least one compound from the group of oxides, phosphates, sulfates, titanates, silicates, aluminosilicates with at least one of the elements zirconium, aluminum, lithium, particularly preferably zirconium oxide.
  • the inorganic ion-conducting material preferably has particles with a largest diameter of less than 100 nm.
  • Such a separator is marketed in Germany, for example, under the trade name "Separion ®" by the company Evonik AG.
  • Methods for producing such separators are known from the prior art, for example from EP 1 017 476 B1, WO 2004/021477 and WO 2004/021499.
  • the separator used in the battery according to the invention comprising a nonwoven made of nonwoven polymer fibers and the inorganic coating, it can only come to shutdown (shutdown), when melted by the high temperature, the polymer structure of the support material and penetrates into the pores of the inorganic material and this thereby closing.
  • the separator does not break down (collapse) since the inorganic particles ensure that complete melting of the separator can not occur. This ensures that there are no operating states in which a large-area short-circuit can occur.
  • separators Due to the type of nonwoven used, which has a particularly suitable combination of thickness and porosity, separators can be produced which can meet the requirements for separators in high-performance batteries, in particular lithium high-performance batteries.
  • the simultaneous use of oxide particles that are precisely matched in their particle size to produce the porous (ceramic) coating will result in a particularly high porosity of the final separator is achieved, the pores are still small enough to prevent unwanted growth of "lithium whiskers" through the separator. Due to the high porosity of the separator, however, care must be taken to ensure that no dead space is created in the pores.
  • the separators used for the invention also have the advantage that partially adhere to the inorganic surfaces of the separator material, the anions of the conducting salt, which leads to an improvement of the dissociation and thus to a better ion conductivity in the high current range.
  • the separator used for the battery according to the invention comprising a flexible nonwoven fabric with a porous inorganic coating on and in this nonwoven, wherein the material of the nonwoven fabric is selected from unwoven, non-electrically conductive polymer fibers, is also characterized in that the nonwoven fabric has a thickness of less than 30 ⁇ m, a porosity of more than 50%, preferably of 50 to 97%, and a pore radius distribution in which at least 50% of the pores have a pore radius of 75 to 150 ⁇ m.
  • the separator particularly preferably comprises a nonwoven which has a thickness of 5 to 30 ⁇ m, preferably a thickness of 10 to 20 ⁇ m. Also particularly important is a homogeneous distribution of pore radii in the web as indicated above. An even more homogeneous pore radius distribution in the nonwoven, in combination with optimally matched oxide particles of a certain size, leads to an optimized porosity of the separator.
  • the thickness of the substrate has a great influence on the properties of the separator, since on the one hand the flexibility but also the sheet resistance of the electrolyte-impregnated separator depends on the thickness of the substrate.
  • the small thickness is a particularly low electrical resistance achieved the separator in the application with an electrolyte.
  • the separator itself has a very high electrical resistance, since it itself must have insulating properties.
  • thinner separators allow increased packing density in a battery pack so that one can store a larger amount of energy in the same volume.
  • the web has a porosity of 60 to 90%, more preferably from 70 to 90%.
  • the porosity is defined as the volume of the web (100%) minus the volume of the fibers of the web, ie the proportion of the volume of the web that is not filled by material.
  • the volume of the fleece can be calculated from the dimensions of the fleece.
  • the volume of the fibers results from the measured weight of the fleece considered and the density of the polymer fibers.
  • the large porosity of the substrate also allows a higher porosity of the separator, which is why a higher uptake of electrolytes with the separator can be achieved.
  • non-electrically conductive fibers of polymers as defined above which are preferably selected from polyacrylonitrile (PAN), polyesters such.
  • PAN polyacrylonitrile
  • PET polyethylene terephthalate
  • PO polyolefin
  • PP polypropylene
  • PE polyethylene
  • the polymer fibers of the nonwovens preferably have a diameter of from 0.1 to 10 ⁇ m, more preferably from 1 to 4 ⁇ m.
  • Particularly preferred flexible nonwovens have a basis weight of less than 20 g / m 2 , preferably from 5 to 10 g / m 2 .
  • the separator has a porous, electrically insulating, ceramic coating on and in the fleece.
  • the porous inorganic coating on and in the nonwoven comprises oxide particles of the elements Li, Al, Si and / or Zr with an average particle size of 0.5 to 7 ⁇ , preferably from 1 to 5 ⁇ and most preferably from 1, 5 to 3 pm.
  • the separator particularly preferably has a porous inorganic coating on and in the nonwoven, the aluminum oxide particles having an average particle size of from 0.5 to 7 ⁇ m, preferably from 1 to 5 ⁇ m and very particularly preferably from 1.5 to 3 ⁇ which are bonded to an oxide of the elements Zr or Si.
  • the maximum particle size is preferably 1/3 to 1/5 and particularly preferably less than or equal to 1/10 of the thickness of the nonwoven used.
  • the separator preferably has a porosity of from 30 to 80%, preferably from 40 to 75% and particularly preferably from 45 to 70%.
  • the porosity refers to the achievable, ie open pores.
  • the porosity can be determined by the known method of mercury porosimetry or can be calculated from the volume and density of the starting materials used, if it is assumed that only open pores are present.
  • the separators used for the battery according to the invention are also distinguished by the fact that they can have a tensile strength of at least 1 N / cm, preferably of at least 3 N / cm and very particularly preferably of 3 to 10 N / cm.
  • the separators can preferably be bent without damage to any radius down to 100 mm, preferably down to 50 mm and most preferably down to 1 mm.
  • the high tensile strength and the good bendability of the separator have the advantage that changes in the geometries of the electrodes occurring during the charging and discharging of a battery can be through the separator without being damaged.
  • the bendability also has the advantage that commercially standardized wound cells are produced with this separator. you can. In these cells, the electrode / separator layers are spirally wound together in a standardized size and contacted.
  • Preferred electrolytes (d) for the lithium-ion batteries are non-aqueous and include an organic solvent and a lithium salt.
  • Preferred lithium salts have inert anions and are non-toxic.
  • Suitable lithium salts are preferably lithium hexafluorophosphate, lithium hexafluoroarsenate, lithium bis (trifluoromethylsulfonyl imide), lithium trifluoromethanesulfonate, lithium tris (trifluoromethylsulfonyl) methide, lithium tetrafluoroborate, lithium perchlorate, lithium tetrachloroaluminate, lithium chloride, lithium bisoxalatoborate, and mixtures thereof.
  • the lithium salt is selected from LiPF 6) LiBF 4, LiCI0 4, LiAsF 6, LiCF 3 S0 3, LiN (CF 3 S0 2) 2, LiC (CF 3 S0 2) 3, LiS0 3 C x F 2x + i , LiN (S0 2 C x F 2x + i) 2 or LiC (S0 2 C x F 2x + 1 ) 3 with 0 ⁇ x ⁇ 8, Li [(C 2 O 4 ) 2 B], and mixtures of two or several of these salts.
  • the electrolyte is present as an electrolyte solution.
  • Suitable solvents are preferably inert. Suitable solvents include, for example, ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethylmethyl carbonate, methylpropycarbonate, butylmethyl carbonate, ethylpropyl carbonate, dipropyl carbonate, cyclopentanones, sulfolanes, dimethyl sulphoxide, 3-methyl-1,3-oxazolidine-2-one, ⁇ - Butyrolactone, 1, 2-Diethoxy- methane, tetrahydrofuran, 2-methyltetrahydrofuran, 1, 3-dioxolane, methyl acetate, ethyl acetate, nitromethane, 1, 3-propanesultone, and mixtures of two or more of these solvents.
  • the electrolyte may include other adjuvants commonly used in electrolytes for lithium ion batteries.
  • these are radical scavengers such as biphenyl, flame retardant additives such as organic phosphoric acid esters or hexamethylphosphoramide, or acid scavengers such as Amines.
  • So-called Kochladeadditive such as cyclohexylbenzene may also be included in the electrolyte.
  • Adjuvants which can influence the formation of the "solid electrolyte interface” layer (SEI) on the electrodes, preferably carbon-containing electrodes, can likewise be used in the electrolyte.
  • SEI solid electrolyte interface layer
  • Such an adjuvant is preferably vinylene carbonate.
  • coolant is provided in the battery. Coolants are preferably tubes that can be charged with a liquid for dissipating heat that arises, for example, when charging the battery.
  • a second aspect of the invention relates to a lithium ion battery comprising:
  • a positive electrode comprising sulfur and / or a lithium sulfide and at least one amorphous chalcogenide which comprises lithium ions or which can conduct lithium ions;
  • the positive electrode (cathode (a)) comprises a matrix of carbon in which the sulfur and / or lithium sulfide are embedded.
  • the positive electrode (cathode (a)) comprising a matrix of carbon in which the sulfur and / or lithium sulfide are embedded is coated with the amorphous chalcogenide, preferably an oxide.
  • the negative electrode comprises a lithium alloy.
  • Suitable lithium alloys are preferably alloys of lithium with aluminum or tin or antimony, for example LiAl or Li 22 Sn 5 or LiSb 3 .
  • the lithium alloy is preferably embedded in a matrix of carbon.
  • the positive electrode also comprises a matrix of carbon.
  • the negative electrode comprises an alloy of lithium and tin together with carbon.
  • electrodes comprising metallic lithium or a lithium alloy can have the property of expanding during charging and contracting during the discharging process. This can lead to power loss of the battery.
  • a lithium alloy in a matrix of carbon it is possible to compensate for volume changes of the battery advantageous.
  • the negative electrode comprises silicon wires whose dimensions are in the nanoscale.
  • the use of silicon as a nanowire can also counteract the undesirable change in volume of the anode during charging or discharging become.
  • Silicon nanowire negative electrodes are also known from lithium ion batteries.
  • the silicon in the form of nanowires replaces the carbon in the anode.
  • the lithium-ion battery is characterized by comprising:
  • a positive electrode comprising sulfur and / or a lithium sulfide and at least one amorphous chalcogenide which comprises lithium ions or which can conduct lithium ions;
  • the fibers are preferably polymer fibers as defined in the first aspect of the invention.
  • separator systems known from the prior art, for example ceramic electrolyte separators or glass electrolyte separators which contain no liquid, or polymeric electrolyte such as polyethers such as polyethylene oxides.
  • Polymeric electrolyte can be used as a gel containing organic liquids in an amount of about 20% by weight.
  • separator membranes ie porous membranes is also possible. They hold a liquid electrolyte in small pores via capillary forces.
  • the membranes preferably include polyolefins such as preferably polyethylene or polypropylene or a laminate of polyethylene and polypropylene.
  • the lithium-ion battery comprises
  • a positive electrode comprising sulfur and / or a lithium sulfide and at least one amorphous chalcogenide, preferably an oxide which comprises lithium ions or which can conduct lithium ions;
  • separator between the positive and negative electrodes; wherein the separator comprises a porous membrane, a ceramic electrolyte separator, a glass electrolyte separator, or a polymeric electrolyte;
  • the usable in the lithium-sulfur battery electrolyte (d) is a non-aqueous electrolyte, preferably an electrolyte as defined above in the first aspect of the invention.
  • Polysulfide anions are preferably added to the electrolyte of the lithium-sulfur battery, for example in the form of Li 2 S 3 , Li 2 S 4 , Li 2 S 6> Li 2 Se.
  • the amount of polysulfide added is such that the electrolyte is saturated with polysulfide.
  • the addition of polysulfide is preferably carried out before the battery is started up.
  • the lithium-ion battery can be constructed from components (a) to (d) by methods known in the art and commonly used for the manufacture of lithium-ion batteries.
  • the preparation is carried out by laminating the electrodes (a) and (b) with the separator (c) which has been impregnated with the electrolyte (d). Fabrication methods for the electrodes are also known from the prior art.
  • the lithium-sulfur battery of the present invention can be used to power mobile information devices, tools, electric cars, and hybrid cars.
  • the combination of the lithium ion-conducting separator with the amorphous chalcogenide, preferably an oxide which comprises lithium ions or which can conduct lithium ions has proven to be favorable for the charging properties of the battery according to the invention. Due to the good conductivity for lithium ions can be achieved with this combination, an advantageous charging speed of the battery. This makes such a battery particularly interesting for electrically powered automobiles.

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  • Electrochemistry (AREA)
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  • Inorganic Chemistry (AREA)
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Abstract

La présente invention concerne une batterie aux ions lithium comprenant : (a) une électrode positive comprenant un chalcogénure amorphe qui comprend des ions lithium ou qui peut diriger des ions lithium; (b) une électrode négative; (c) un séparateur situé entre l'électrode positive et l'électrode négative, le séparateur comprenant un non-tissé de fibres, de préférence de fibres polymères; (d) un électrolyte non aqueux.
EP11721717.4A 2010-06-21 2011-05-17 Batterie aux ions lithium comprenant des matières d'électrode amorphes Withdrawn EP2583335A1 (fr)

Applications Claiming Priority (2)

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DE102010024479A DE102010024479A1 (de) 2010-06-21 2010-06-21 Lithium-Ionen-Batterie mit amorphen Elektrodenmaterialien
PCT/EP2011/002450 WO2011160747A1 (fr) 2010-06-21 2011-05-17 Batterie aux ions lithium comprenant des matières d'électrode amorphes

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US (1) US20130149567A1 (fr)
EP (1) EP2583335A1 (fr)
JP (1) JP2013534027A (fr)
CN (1) CN102947985A (fr)
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WO (1) WO2011160747A1 (fr)

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DE102014213271B4 (de) * 2014-07-09 2023-04-27 Bayerische Motoren Werke Aktiengesellschaft Elektrochemische Zelle
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US20130149567A1 (en) 2013-06-13
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WO2011160747A1 (fr) 2011-12-29
JP2013534027A (ja) 2013-08-29

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