WO2019015892A1 - Procédé de fabrication d'un séparateur solide pour un élément de batterie - Google Patents

Procédé de fabrication d'un séparateur solide pour un élément de batterie Download PDF

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Publication number
WO2019015892A1
WO2019015892A1 PCT/EP2018/065850 EP2018065850W WO2019015892A1 WO 2019015892 A1 WO2019015892 A1 WO 2019015892A1 EP 2018065850 W EP2018065850 W EP 2018065850W WO 2019015892 A1 WO2019015892 A1 WO 2019015892A1
Authority
WO
WIPO (PCT)
Prior art keywords
separator
separator material
battery cell
optionally
takes place
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.)
Ceased
Application number
PCT/EP2018/065850
Other languages
German (de)
English (en)
Inventor
Silvan Hippchen
Anne BUCHKREMER
Danijel NIKOLIC
Guido Klamt
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.)
Robert Bosch GmbH
Original Assignee
Robert Bosch 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 Robert Bosch GmbH filed Critical Robert Bosch GmbH
Priority to EP18732313.4A priority Critical patent/EP3656005A1/fr
Publication of WO2019015892A1 publication Critical patent/WO2019015892A1/fr
Anticipated expiration legal-status Critical
Ceased 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
    • 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
    • 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
    • H01M50/417—Polyolefins
    • 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
    • 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
    • H01M50/403—Manufacturing processes of separators, membranes or diaphragms
    • 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 method for producing a
  • Solid state separator for a battery cell The present invention further relates to a method for manufacturing a battery cell with an improved solid state separator.
  • Electrochemical energy storage devices such as lithium-ion batteries, are widely used in many daily applications. They are used, for example, in computers such as laptops, mobile phones, smart phones, and other applications. Even with the currently strongly driven
  • lithium-based batteries such as lithium-ion batteries or lithium batteries are used as energy sources in electric vehicles because of their high specific energy.
  • lithium-ion batteries for example, are often used for lithium-ion batteries.
  • lithium-ion batteries for example, are often used for lithium-ion batteries.
  • Solid electrolytes or solid state separators used. These are often made of a polymer or a ceramic and are produced in particular in a wet chemical synthesis.
  • the present invention relates to a method for producing a
  • Solid state separator for a battery cell comprising the method steps: a) providing separator material;
  • step c) optionally drying the separator material provided in step a) and optionally comminuted;
  • Separator material was not mixed with a conductive salt.
  • the above method steps can proceed in the order described above, in a different order, or at least partially simultaneously.
  • a method described above allows in a surprising manner to produce a solid state separator with a particularly small amount of
  • a solid state separator can be displayed in a particularly defined way.
  • the method may include manufacturing a solid-state separator for a lithium-ion battery or a lithium battery having a lithium-metal anode, but is not limited to these examples.
  • the present invention relates to a process forming part of a process for producing a
  • Battery cell or a battery is.
  • the method comprises the following method steps.
  • the method comprises the provision of
  • Separator material As such, basically any separator material may be provided which may be preferred for the desired application.
  • the separator material can be selected according to the desired properties, for example if the solid-state separator to be produced is to serve equally well as a solid-state electrolyte. Since the solid-state separator to be generated has a particularly low content
  • the separator material may already be provided in dry form, in particular in a non-solvent form.
  • the separator material can be provided with a moisture content or solvent content of less than or equal to 0.1 ppm, based on the mass of the solids of the separator material and the mass of the solvent.
  • the separator material having a particle size for example a particle size dgo, is provided which is less than or equal to 15 ⁇ m, for example less than or equal to 10 ⁇ m.
  • the separator material may be present or provided in a particle size, such as a particle size dgo, in a range of greater than or equal to 1 ⁇ to less than or equal to 15 ⁇ .
  • the particle size can be determined, for example, by laser diffractometry.
  • a particle size D90 may in particular mean that 90% of the particles are smaller than the stated value.
  • Process step b) can connect a comminution of the separator material provided in process step a). This may be particularly advantageous if the separator material provided in process step a) has too large a particle size. Insofar as the particles provided in method step a) have a larger particle size than desired, for example if the particle size is above the range defined above, then, according to method step b), the separator material can be comminuted. However, insofar as the particles provided in process step a) have a sufficiently small size, for example if they are already in the above-described range of particle size, can be applied to the
  • Step b) are omitted.
  • Process step c) comprise drying the separator material. This can be particularly advantageous if the separator material a
  • Drying of the separator material can be carried out, for example, by a temperature treatment at about elevated temperature, ie at about room temperature (22 ° C) elevated temperature, and further optionally under reduced to the ambient pressure of about lbar pressure.
  • the exact adjustment of the temperature or the pressure can be dependent on the selected separator material.
  • the separator material provided in process step a) has a sufficiently high dry content or a sufficiently low liquid content, which may be, for example, in the range defined above, the process step c) can be dispensed with.
  • the separator material has at least one of a moisture content in a range of less than or equal to 0.1 ppm and a particle size in a range of less than or equal to 15 ⁇ prior to at least one of process steps d) and e).
  • the method described above may further comprise mixing the separator material with at least one of a conductive salt and a binder material.
  • a conductive salt may be particularly advantageous if the separator material is to form a solid state separator and at the same time performs the function of a solid electrolyte.
  • a conductive salt can be understood in a conventional manner a
  • a suitable conducting salt for example when the separator is used in a lithium-ion battery, include, for example, LiTFSi, LiP F6, LiClO, Li BF, UCF 3 SO 3 or LiN (SO 2 CF 3) 2.
  • the proportion of conductive salt incorporated in the separator material may in particular depend on the specific application and be chosen without difficulty by the person skilled in the art. Especially in this
  • the separator to be generated equally serve as electrolyte without having to resort to solvents.
  • a binder material may be added, such as to obtain improved mechanical properties. This may be advantageous, for example, with a ceramic separator material.
  • Binder materials include, for example, polymers generally known in the art, such as polyvinylidene fluoride (PVDF) or polyethylene glycol (PEG).
  • PVDF polyvinylidene fluoride
  • PEG polyethylene glycol
  • the separator can be produced porous and then a
  • Solid state separator are added or filled in the pores.
  • corresponding liquid electrolytes include, for example, a mixture of ethylene carbonate, dimethyl carbonate and LIP F6.
  • the porosity of the separator can also be adjusted via the pressing duration and the pressing pressure, or over the duration of the homogenization, as described below.
  • the method described above comprises as process step e) the hot pressing of the separator material to form a separator.
  • the separator may be substantially completed.
  • the final thickness of the separator can be provided in this process step, which can be adjustable according to the desired specifications in a manner understandable to the person skilled in the art.
  • the homogeneity of the separator can be improved, which can enhance the effect of the separator.
  • the separator can be produced in a particularly defined and controllable manner. For example, by adjusting the pressing conditions, the porosity of the separator can be influenced, which can be advantageous in terms of application and can enable high adaptability.
  • hot pressing may, in particular, be understood as treating the separator with conditions increased to room temperature of 22 ° C. and atmospheric pressure of 1 bar, wherein, in particular, pressing between two pressing elements, such as two press plates, can be realized ,
  • hot pressing may be performed only once, or several times in succession.
  • the separator thus produced may be formed by folding
  • the layer thickness can be adjustable, and this is basically possible before or after an optional addition of the electrolyte.
  • a method as described above may have significant advantages over the prior art solutions, as described below.
  • Lithium-ion batteries usually comprise a negative electrode or anode and a positive electrode or cathode, which electrodes are separated by a liquid or solid electrolyte layer.
  • lithium ions Li + ions
  • the lithium ions in the corresponding electrode material, such as graphite, or at the deposition on the anode can precipitate under unfavorable conditions metallic lithium disorderly.
  • the thus deposited lithium can form dendritic structures, which can grow through the electrolyte up to the positive electrode, which can ultimately lead to a short circuit of the battery cell.
  • a separator can be produced by the hot pressing in a defined and adaptive manner.
  • a homogenization of the separator material for example, the mixture produced in process step c) takes place.
  • a homogenization of the separator material such as by particularly effective mixing of separator material and conductive salt, it may be possible for the separator produced to have a defined composition at each position. This makes possible for a separator produced with such a separator
  • Battery cell a particularly defined and powerful work.
  • a homogenization is carried out by the action of a particular to room temperature (22 ° C) increased
  • an effective homogenization of the separator material and about an effective mixing of the substances contained in the mixture comprising the separator material and the conductive salt can be made possible.
  • homogenization may be carried out for a time ranging from greater than or equal to 1 hour to less than or equal to 24 hours, such as in a range greater than or equal to 5 hours to less than or equal to 18 hours, for example in a range of greater than or equal to 8 hours to less than or equal to 12 hours.
  • Suitable temperatures for homogenization can
  • the separator material comprises at least one of a copolymer and a composite material.
  • a copolymer containing at least one polymer component selected from the group consisting of polyethylene, polypropylene, polystyrene and derivatives thereof may be used.
  • the separator material for example, a composite material of a
  • inorganic material such as a ceramic material or a sulfidic glass, and a polymer or copolymer, for example, as described above.
  • a ceramic material or a sulfidic glass and a polymer or copolymer, for example, as described above.
  • These materials pull water out of the system, which can improve cell longevity in the long term.
  • the proposed method minimizes the amount of water present in the cell and ensures a defined composition of the materials.
  • the use of copolymers and / or composite materials may advantageously permit the process defined above and may allow a particularly low proportion of solvent in the system.
  • process step b) takes place by grinding.
  • separator material easily obtained a particularly small particle size, as defined for example above.
  • a separator material in the form of particles can be obtained which have a very homogeneous particle size.
  • This can be a mixing or homogenizing of the separator material, such as mixing with a conductive salt, as described above simplify
  • step b) takes place with cooling of the separator material.
  • the separator material may be cooled using liquid nitrogen and / or cooled to a temperature of less than -190 ° C.
  • comminution, such as grinding of the separator material can be made effective or particles with a particularly homogeneous
  • Particle size distribution can be achieved.
  • At least one of the process steps b), c) or d) may take place in at least one of a solvent-free, in particular anhydrous, atmosphere and a protective gas atmosphere, ie in particular an oxygen-free atmosphere.
  • a solvent-free, in particular anhydrous, atmosphere and a protective gas atmosphere ie in particular an oxygen-free atmosphere.
  • at least one, for example all, of process steps b), c) and d) can be carried out under a solvent-free and / or inert gas atmosphere.
  • a particularly defined separator can be produced, which has a particularly low solvent content and
  • a protective gas atmosphere may have an oxygen content of equal to or less than 5%, preferably equal to or less than 3%, more preferably equal to or less than 1%, even more preferably equal to or less than 100 ppm, for example less than or less than 0.1 ppm , based on the mass of the gas.
  • a solvent-free atmosphere may have a solvent content of equal to or less than 5%, preferably equal to or less than 3%, more preferably equal to or less than 1%, even more preferably equal to or less than 100 ppm, for example less or less than 0.1 ppm, based on the mass of the solvent and the gas.
  • process step e) takes place at least one of a temperature of at least 25 ° C, for example of at least 60 ° C, and a pressure of at least 50 bar.
  • a temperature of at least 25 ° C for example of at least 60 ° C
  • a pressure of at least 50 bar may be assisted.
  • the separator can be pressed mechanically in an effective manner and thus adapted to its desired dimensions, such as in particular thickness. The upper limits may be process-related, or the stability or decomposition temperature of the used
  • the separator material has at least two polymer constituents, wherein process step e) takes place at a temperature which is at least one above the melting point
  • Process step e but nevertheless has an advantageous processability.
  • this refinement can contribute to the elimination of residual solvent residues, such as, for example, water residues, and correspondingly, if appropriate, to be able to dispense with further drying steps.
  • the present invention furthermore relates to a method for producing a battery cell, in which a solid state separator is produced and contacted on a first side with an anode and is contacted on a first side opposite the second side with a cathode, wherein the solid state separator is produced, as described in detail above.
  • a solid state separator can be prepared first, as described above. Furthermore, anode and cathode can be provided, as is basically known and to a
  • corresponding layer structure are joined together, for example laminated.
  • a battery cell designed in this way can in particular have the advantages described above for the separator.
  • the danger of dendritic formation can be reduced and thus the long-term stability can be improved.
  • Possible configurations of the battery cell include, but are not limited to, a negative electrode comprising at least one of carbon, silicon, and metallic lithium, and a positive electrode, which may include at least one of UCOO2, LiMn20, or Li FeP0.
  • an electrolyte may be provided, as known from the prior art, for example designed as a liquid electrolyte, for example as a gel electrolyte.
  • a liquid electrolyte may be dispensed with, as far as the separator has the properties of an electrolyte by providing a conducting salt in the separator material, as described in detail above.
  • Fig. 1 is a schematic process diagram of an inventive
  • a method of manufacturing a battery electrode comprising a method of manufacturing a separator material.
  • FIG. 1 shows a process diagram illustrating a method according to the present invention.
  • step 10 according to method step a) shows the provision of
  • the separator material is comminuted at step 12, in accordance with method step c).
  • This step is optional and in particular dependent on the design of the separator material provided in process step a).
  • a drying of the separator material may follow in step 14, for example at step 10 or at step 12.
  • This step is also optional and depends in particular on the configuration of the separator material provided in method step a) or step 10.
  • Step 18, which may be followed by one of the steps 10, 12 or 14 describes according to process step c) the mixing of the optionally comminuted and optionally dried Separator material with a conductive salt, which was provided in accordance with step 16.
  • This step 168 is also optional and depends on whether a mixture of a conductive salt is to be provided with the separator material.
  • step 20 which may be followed by one of the steps 10, 12, 14 or 18, a homogenization of the separator material can take place.
  • step 22 which can be connected to one of the steps 10, 12, 14, 18 or 20 according to method step e), a hot pressing of the separator material. After this step, the separator can be completed. However, at step 24, the addition of a liquid electrolyte, such as a
  • Gel electrolyte connect to the step 22 and may follow the step 26, the formation of a battery cell or a battery with the generated separator to step 22 or 24.

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  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • General Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Materials Engineering (AREA)
  • Secondary Cells (AREA)
  • Cell Separators (AREA)

Abstract

La présente invention concerne un procédé de fabrication d'un séparateur solide pour un élément de batterie, ce procédé comprenant les étapes suivantes : a) préparation d'un matériau de séparateur ; b) broyage éventuel du matériau de séparateur préparé à l'étape a) ; c) séchage éventuel du matériau de séparateur préparé à l'étape a) et éventuellement broyé ; d) mélange éventuel du matériau de séparateur avec un sel conducteur et/ou un matériau liant ; e) moulage à chaud du matériau de séparateur pour former un séparateur et f) ajout d'électrolyte liquide au séparateur produit à l'étape e) si le matériau de séparateur n'a pas été mélangé avec un sel conducteur à l'étape d).
PCT/EP2018/065850 2017-07-18 2018-06-14 Procédé de fabrication d'un séparateur solide pour un élément de batterie Ceased WO2019015892A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP18732313.4A EP3656005A1 (fr) 2017-07-18 2018-06-14 Procédé de fabrication d'un séparateur solide pour un élément de batterie

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102017212266.8A DE102017212266A1 (de) 2017-07-18 2017-07-18 Verfahren zum Herstellen eines Festkörperseparators für eine Batteriezelle
DE102017212266.8 2017-07-18

Publications (1)

Publication Number Publication Date
WO2019015892A1 true WO2019015892A1 (fr) 2019-01-24

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PCT/EP2018/065850 Ceased WO2019015892A1 (fr) 2017-07-18 2018-06-14 Procédé de fabrication d'un séparateur solide pour un élément de batterie

Country Status (3)

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EP (1) EP3656005A1 (fr)
DE (1) DE102017212266A1 (fr)
WO (1) WO2019015892A1 (fr)

Citations (3)

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Publication number Priority date Publication date Assignee Title
EP2498320A2 (fr) * 2009-11-03 2012-09-12 Amogreentech Co., Ltd. Couche de séparation fibreuse ultrafine résistante à la chaleur et à solidité élevée, procédé pour la fabrication de celle-ci et cellule secondaire utilisant celle-ci
US20140099556A1 (en) 2012-10-09 2014-04-10 Microsoft Corporation Solid-State Battery Separators and Methods of Fabrication
DE102013219602A1 (de) * 2013-09-27 2015-04-16 Robert Bosch Gmbh Herstellungsverfahren für Lithium-Zellen-Funktionsschicht

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US9306223B2 (en) * 2011-09-22 2016-04-05 Eaglepicher Technologies, Llc Electrolyte materials, thermal battery components, and thermal batteries for intermediate temperature applications
US10333173B2 (en) * 2014-11-14 2019-06-25 Medtronic, Inc. Composite separator and electrolyte for solid state batteries
US10164289B2 (en) * 2014-12-02 2018-12-25 Polyplus Battery Company Vitreous solid electrolyte sheets of Li ion conducting sulfur-based glass and associated structures, cells and methods
DE102015201409A1 (de) * 2015-01-28 2016-07-28 Bayerische Motoren Werke Aktiengesellschaft Komposit-Separator und diesen umfassende Lithiumionenbatterie sowie Verfahren zur Herstellung des Komposit-Separators

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EP2498320A2 (fr) * 2009-11-03 2012-09-12 Amogreentech Co., Ltd. Couche de séparation fibreuse ultrafine résistante à la chaleur et à solidité élevée, procédé pour la fabrication de celle-ci et cellule secondaire utilisant celle-ci
US20140099556A1 (en) 2012-10-09 2014-04-10 Microsoft Corporation Solid-State Battery Separators and Methods of Fabrication
DE102013219602A1 (de) * 2013-09-27 2015-04-16 Robert Bosch Gmbh Herstellungsverfahren für Lithium-Zellen-Funktionsschicht

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Also Published As

Publication number Publication date
DE102017212266A1 (de) 2019-01-24
EP3656005A1 (fr) 2020-05-27

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