WO2024251327A1 - Procédé de production d'un parafoudre poreux et batterie au lithium-ion - Google Patents

Procédé de production d'un parafoudre poreux et batterie au lithium-ion Download PDF

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Publication number
WO2024251327A1
WO2024251327A1 PCT/DE2024/100485 DE2024100485W WO2024251327A1 WO 2024251327 A1 WO2024251327 A1 WO 2024251327A1 DE 2024100485 W DE2024100485 W DE 2024100485W WO 2024251327 A1 WO2024251327 A1 WO 2024251327A1
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WO
WIPO (PCT)
Prior art keywords
lithium
porous
ion battery
precursor
arrester
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/DE2024/100485
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German (de)
English (en)
Inventor
Bjoern-Ingo Hieronymus HOGG
Thomas Woehrle
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Bayerische Motoren Werke AG
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Bayerische Motoren Werke AG
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.)
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Publication date
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Priority to CN202480037378.0A priority Critical patent/CN121263876A/zh
Publication of WO2024251327A1 publication Critical patent/WO2024251327A1/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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • 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 invention relates to a method for producing a porous conductor for an electrode of a lithium-ion battery and to a lithium-ion battery comprising an electrode with a porous conductor.
  • lithium ion battery is used synonymously for all terms commonly used in the prior art for galvanic elements and cells containing lithium, such as lithium battery, lithium cell, lithium ion cell, lithium ion battery, lithium polymer cell and lithium ion accumulator.
  • rechargeable batteries secondary batteries
  • battery battery
  • cell battery
  • electrochemical cell electrochemical cell
  • the lithium ion battery can also be a solid-state battery, for example a ceramic or polymer-based solid-state battery.
  • Lithium-ion batteries have at least two different electrodes, a positive one (cathode) and a negative one (anode). Each of these electrodes has at least one active material, each of which is applied to a conductor for electrical contact.
  • the cathode and the anode are arranged one above the other to form an electrode arrangement, for example in stacks, with a separator being used for electrical insulation between the cathode and anode.
  • Lithium-ion batteries that use metallic lithium (hereinafter also referred to as "lithium metal”) as the anode active material are of particular interest, as they have a particularly high specific capacity. This results in a high energy density or specific energy of the lithium-ion battery, which in this case can also be referred to as a lithium metal cell.
  • lithium metal metallic lithium
  • lithium metal anodes One challenge when using such lithium metal anodes is to achieve the most homogeneous possible deposition of metallic lithium during charging and at the same time to use the highest possible current density in order to shorten the charging time.
  • the shortest possible charging time is of crucial importance. Inhomogeneous deposition of lithium promotes the formation of so-called “lithium dendrites" starting from the lithium metal anode, which can damage the separator and thus lead to internal short circuits. Lithium dendrites can also react kinetically quickly with the electrolyte system of the lithium-ion battery, causing the cell capacity to decrease irreversibly.
  • lithium metal anodes Another problem with the use of lithium metal anodes is the volume changes that occur due to the lithium metal depositing and dissolving, which can cause the cell volume to increase or decrease by around 10 to 20%.
  • This "breathing" of the lithium-ion battery's electrodes during each charge/discharge cycle requires complex structural designs to reduce the resulting mechanical stress. Otherwise, at the cell level, there can be a different pressure distribution on the ensemble of electrodes and separators, mechanical damage such as pulverization, cracking, reduction in porosity, in particular the porosity of the separator, pore closure, pore smearing or decoupling of the electrode film from the conductor, which can have a detrimental effect on the service life, performance and reliability of the lithium-ion battery.
  • the object of the invention is achieved by a method for producing a porous conductor for an electrode of a lithium-ion battery, comprising the following steps: a) a porous conductor precursor is provided, wherein the conductor precursor comprises polytetrafluoroethylene, and b) the polytetrafluoroethylene present in the porous conductor precursor is at least partially reacted with metallic lithium to form amorphous carbon to form the porous conductor.
  • PTFE polytetrafluoroethylene
  • LiF lithium fluoride
  • the invention is based on the basic idea of producing a porous conductor with a defined three-dimensional structure by chemically reacting a conductor precursor that contains PTFE and has a predetermined porous structure through contact with metallic lithium.
  • a porous conductor is produced whose porosity is derived from the porosity of the conductor precursor used.
  • the resulting porous structure of the The porous arrester ensures that when the porous arrester is used in a lithium-ion battery, metallic lithium can be deposited in a defined and uniform manner on the porous arrester, so that the formation of lithium dendrites during charging and discharging processes is effectively suppressed or at least reduced.
  • volume changes that occur are minimized because the metallic lithium that forms can at least partially collect within the pore structure of the porous arrester.
  • amorphous carbons obtained from PTFE by reacting with metallic lithium have sufficient mechanical stability to be used as conductors in an electrode for lithium-ion batteries.
  • amorphous carbons have sufficiently high electrical conductivity to be able to handle the currents expected in lithium-ion batteries.
  • a further advantage of the produced porous conductor based on amorphous carbon is that electrodes with such a porous conductor have a high flexibility and a low weight, especially compared to conventional conductors based on rolled metal foils, for example rolled aluminum foils.
  • the porous conductor precursor is a fabric, a fleece, a stretched film, a punched film or a membrane.
  • fabrics, fleeces and membranes consisting of PTFE or comprising PTFE are commercially available worldwide.
  • fabrics, fleeces and membranes provide a defined porous three-dimensional structure that is at least partially retained, preferably essentially completely retained, even after the PTFE has been reacted with metallic lithium.
  • the porosity and shape of the porous arrester can be determined by choosing a suitable arrester precursor.
  • any configuration of the porous arrester can be realized.
  • the porous arrester precursor can be made of polytetrafluoroethylene.
  • a porous arrester can be produced that consists only of amorphous carbon and optionally the carbon particles formed during the conversion of PTFE with metallic Lithium-derived further reaction products, in particular lithium fluoride and/or unreacted PTFE.
  • the porous conductor precursor may comprise an electrically conductive matrix coated with polytetrafluoroethylene.
  • amorphous carbon is generated on the surface of the electrically conductive matrix, which contributes to the electrical conductivity of the porous conductor formed.
  • the porosity of the arrester precursor can be provided by the applied coating with PTFE and/or by the electrically conductive matrix, so that the porosity of the produced porous arrester is also provided by the amorphous carbon and/or by the electrically conductive matrix.
  • the matrix may comprise a metal or a metal alloy.
  • the matrix is made of copper, nickel and/or steel.
  • step b at least 90 mole percent of the polytetrafluoroethylene contained in the porous conductor precursor can be reacted in step b), preferably at least 95 mole percent.
  • the polytetrafluoroethylene contained in the porous conductor precursor is particularly preferably reacted completely.
  • the term “fully converted” means that the PTFE contained is completely chemically converted, apart from unavoidable losses.
  • step b) the metallic lithium is applied to the porous arrester precursor.
  • the porous arrester precursor is coated with metallic lithium using a gas-phase process such as chemical vapor deposition (CVD) or physical vapor deposition (PVD).
  • CVD chemical vapor deposition
  • PVD physical vapor deposition
  • the arrester precursor prefferably coated with liquefied lithium.
  • Non-liquefied lithium can also be mechanically pressed into the arrester precursor.
  • the arrester precursor Before contacting with metallic lithium, the arrester precursor can be moistened with an electrolyte, in particular with the same electrolyte that is to be used in the subsequent application of the produced porous arrester in a lithium-ion battery.
  • the electrolyte comprises an electrolyte solvent, which preferably contains an organic solvent selected from the group consisting of ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate, dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), fluoroethylene carbonate (FEC), sulfolane, 2-methyltetrahydrofuran, acetonitrile, 1,3-dioxolane, ⁇ -butyrolactone (GBL), and combinations thereof.
  • an organic solvent selected from the group consisting of ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate, dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), fluoroethylene carbonate (FEC), sulfolane, 2-methyltetrahydrofuran, acetonitrile, 1,3-dioxolane, ⁇ -butyrolact
  • the porous arrester precursor is installed before step b) with a lithium-containing counter electrode and a separator arranged between the porous arrester precursor and the counter electrode to form a lithium-ion battery, with step b) taking place during a charging and discharging process of the lithium-ion battery.
  • step b) taking place during a charging and discharging process of the lithium-ion battery.
  • the porous arrester precursor must already have sufficient electrical conductivity to serve as an arrester during the charging and discharging process of the lithium-ion battery, in which the porous arrester precursor is converted into the porous arrester.
  • the porous arrester precursor can be combined with other components known for applications in lithium-ion batteries, such as a binding agent or electrode binder, to form an electrode, which is then combined with the counter electrode and the separator to form the lithium-ion battery.
  • a binding agent or electrode binder such as a binding agent or electrode binder
  • the electrode consists of the porous conductor precursor.
  • the lithium-containing counter electrode is in particular a cathode which comprises any pre- or overlithiated cathode active material which can provide the desired amount of lithium for converting the PTFE.
  • the overlithiated cathode active material may contain a lithium-containing additive which is released during the first charging process of the lithium-ion battery under release of lithium ions.
  • the lithium-containing additive includes or is lithium peroxide (U2O2).
  • the cathode active material can be pre- or overlithiated in such a way that even after the PTFE has been converted in the porous conductor precursor, an amount of lithium that can be cycled within the lithium-ion battery is provided, which enables the lithium-ion battery to have the capacity desired for the intended application of the lithium-ion battery.
  • the cathode active material can be a so-called "overlithiated oxide” (OLO).
  • the cathode active material is selected in such a way that it releases more lithium ions in the first charging process of the lithium-ion battery than are incorporated into the structure of the cathode active material in the immediately following discharge process (also referred to as “irreversible loss” or “first cycle efficiency”). In this way, the loss of lithium ions available for cyclization that occurs anyway can be used to convert the arrester precursor into a porous arrester. Examples of such cathode active materials are described in Hu et al: “Revisiting the initial irreversible capacity loss of LiNi0.6Co0.2Mn0.2O2 cathode material batteries” (Energy Storage Materials, Vol. 50, 2022, pp.
  • the porous conductor is accordingly particularly intended and configured to be used in an anode of a lithium-ion battery, preferably a lithium metal anode.
  • porous conductor especially if it is not first generated in an already assembled lithium-ion battery, to be used as a conductor in a cathode of a lithium-ion battery.
  • the object of the invention is further achieved by a lithium-ion battery comprising an electrode with a porous conductor, wherein the porous conductor was obtained by a method as described above.
  • the features and properties of the method according to the invention apply accordingly to a lithium-ion battery according to the invention and vice versa.
  • the lithium-ion battery according to the invention is characterized by the porous conductor produced according to the method according to the invention through only small volume changes during charging and discharging processes, for example volume changes of less than 5%, preferably less than 1%, in each case based on the total volume of the lithium-ion battery. In this way, the lithium-ion battery has a long service life and dimensional stability.
  • the lithium-ion battery has a higher specific energy density with the same content of active materials compared to lithium-ion batteries that use purely metal-based arresters, for example arresters made of rolled foil.
  • the porous conductor preferably has a three-dimensional pore structure.
  • the three-dimensional pore structure ensures a uniform three-dimensional deposition of metallic lithium during the charging process of the lithium-ion battery.
  • the three-dimensional pore structure is predetermined by the arrangement and type of structural elements present in the porous arrester.
  • the three-dimensional pore structure is defined by the webs of the porous arrester, in particular by the web width, web thickness, web length and the crossing points of the webs.
  • the three-dimensional pore structure is determined by the porous conductor precursor used in the manufacture of the lithium-ion battery.
  • the porous conductor is preferably an anode of the lithium ion battery, particularly preferably a lithium metal anode.
  • - Fig. 1 shows schematically a conductor precursor as it can be used in a method according to the invention for producing a porous conductor
  • - Fig. 2 schematically shows an arrester obtained by reacting the arrester precursor with metallic lithium
  • - Fig. 3 is a schematic sectional view through a lithium-ion battery in which the arrester precursor from Fig. 1 is installed, and
  • - Fig. 4 shows a lithium-ion battery according to the invention.
  • FIG. 1 schematically shows a porous arrester precursor 10 which is used in a method according to the invention for producing a porous arrester 12 (cf. Fig. 2).
  • the arrester precursor 10 is a porous fabric made of polytetrafluoroethylene (PTFE) which has a large number of webs 16 connected via crossing points 14. Between the crossing points 14 and webs 16 there are pores 17 which determine the porosity of the arrester precursor 10. Corresponding PTFE fabrics as a starting material are commercially available worldwide.
  • PTFE polytetrafluoroethylene
  • the structure of the porous fabric in Fig. 1 is only indicated by way of example.
  • the only decisive factor is that the arrester precursor 10 has a predetermined porosity.
  • the arrester precursor 10 can also be a porous fleece or a porous membrane, for example, instead of a porous fabric.
  • the arrester precursor 10 has a substantially symmetrical pore structure.
  • alternative designs are also possible in which an irregular and three-dimensional pore structure is present in the arrester precursor 10.
  • the PTFE present in the arrester precursor 10 is reacted with metallic lithium to form amorphous carbon, whereby the porous arrester 12 is formed (cf. Fig. 2).
  • the porous arrester 12 also has a porous structure which essentially corresponds to that of the arrester precursor 10, in particular in terms of the web widths and thicknesses, the open geometry and the open areas. In other words, the choice of the porous arrester precursor 10 used also determines the structure and geometry of the porous arrester 12. Accordingly, the porous arrester 12 in the embodiment shown has arrester webs 18 which are connected via arrester crossing points 20 to form a three-dimensional and porous network with arrester pores 21.
  • the porous conductor 12 is mechanically stable and flexible. In addition, the porous conductor 12 is electrically conductive due to the amorphous carbon formed from the PTFE.
  • the conversion of the porous arrester precursor 10 into the porous arrester 12 can be carried out by applying metallic lithium to the arrester precursor 10.
  • the porous arrester precursor is dipped in metallic lithium or metallic lithium is applied to the porous arrester precursor 10 by means of a CVD or PVD process.
  • the reaction between the PTFE of the porous arrester precursor 10 and the applied metallic lithium begins immediately and can be controlled by the amount of applied metallic lithium and/or its exposure time to the porous arrester precursor 10.
  • the porous conductor 12 After the porous conductor 12 is obtained, it can be incorporated into an electrode for a lithium ion battery and the latter can be used in a lithium ion battery. It is also possible for the porous conductor 12 alone to form the electrode of the lithium ion battery.
  • the porous arrester precursor 10 not to consist of PTFE, but to comprise an electrically conductive matrix coated with PTFE.
  • the only decisive factor is that the PTFE of the porous arrester precursor 10 is at least partially accessible to metallic lithium.
  • the porous conductor precursor 10 is provided with a counter electrode 22 and a contact surface 24 connected between the counter electrode 22 and the porous
  • the separator 24 arranged on the arrester precursor 10 is installed to form a lithium-ion battery 26.
  • the counter electrode 22 is a cathode and comprises a cathode current collector 28 onto which a cathode film 30 is applied.
  • the cathode current collector 28 is a non-porous rolled foil made of aluminum, for example a rolled aluminum foil as known from EP 3 714 078 B1
  • the cathode film 30 comprises a particulate cathode active material 32 and an electrode binder 34.
  • the porous conductor precursor 10 forms the anode of the lithium-ion battery 26, so that the lithium-ion battery 26 shown is a so-called “lithium-free” anode, which in the uncharged state of the lithium-ion battery 26 does not contain any cyclable lithium in the anode and thus represents the pure anode current collector.
  • the cathode active material 32 is lithiated and thus capable of reversibly releasing or absorbing lithium ions during a first charging and discharging process of the lithium-ion battery 26.
  • the porous conductor precursor 10 is itself electrically conductive, such that the porous conductor precursor 10 can function as a conductor of the (lithium-free) anode of the lithium-ion battery 26.
  • the conversion of the PTFE contained in the porous conductor precursor 10 takes place during a charging and discharging process of the lithium-ion battery 26.
  • lithium ions migrate from the counter electrode 22, i.e. the cathode, through the separator 24 to the porous conductor precursor 10 and are deposited as metallic lithium at the crossing points 14 and webs 16 within the porous structure of the conductor precursor 10.
  • the PTFE of the porous conductor precursor 10 thus comes into contact with metallic lithium and is converted to lithium fluoride and amorphous carbon to form the porous conductor 12. In this way, the pores of the porous conductor 12 formed in situ are filled with lithium, so that a lithium metal anode is formed (see Fig. 4).
  • the lithium-ion battery 26 with the porous conductor 12 obtained by the method according to the invention is then immediately ready for use.
  • porous conductor 12 or the lithium-containing anode can be removed from the lithium-ion battery 26 and installed in a new lithium-ion battery.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)

Abstract

L'invention concerne un procédé permettant de réaliser un parafoudre poreux (12) pour une électrode d'une batterie lithium-ion (26), ledit procédé comprenant les étapes suivantes : a) un précurseur de parafoudre poreux est fourni, le précurseur de parafoudre comprenant du polytétrafluoroéthylène, et b) le polytétrafluoréthylène présent dans le précurseur de parafoudre poreux est mis à réagir au moins en partie avec du lithium métallique de manière à former du carbone amorphe afin de réaliser le parafoudre poreux (12). En outre, l'invention concerne une batterie lithium-ion (26).
PCT/DE2024/100485 2023-06-05 2024-05-28 Procédé de production d'un parafoudre poreux et batterie au lithium-ion Ceased WO2024251327A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202480037378.0A CN121263876A (zh) 2023-06-05 2024-05-28 用于产生多孔的导出体的方法和锂离子电池

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102023114688.2A DE102023114688A1 (de) 2023-06-05 2023-06-05 Verfahren zum Erzeugen eines porösen Ableiters und Lithiumionenbatterie
DE102023114688.2 2023-06-05

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WO2024251327A1 true WO2024251327A1 (fr) 2024-12-12

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DE (1) DE102023114688A1 (fr)
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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20110165462A1 (en) * 2010-01-07 2011-07-07 Aruna Zhamu Anode compositions for lithium secondary batteries
WO2015043573A2 (fr) * 2013-09-27 2015-04-02 Christian Pszolla Élément de batterie électrochimique rechargeable
WO2020221564A1 (fr) * 2019-04-30 2020-11-05 Innolith Technology AG Élément de batterie rechargeable
EP3740981A1 (fr) 2018-01-16 2020-11-25 elfolion GmbH Matériau fonctionnel en feuille et procédé pour sa fabrication
EP3714078B1 (fr) 2017-11-21 2022-01-05 Speira GmbH Feuille d'électrode de batterie à haute résistance pour la fabrication d'accumulateurs lithium-ion
US20220077494A1 (en) * 2019-07-31 2022-03-10 Innolith Technology AG Rechargeable battery cell

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20110165462A1 (en) * 2010-01-07 2011-07-07 Aruna Zhamu Anode compositions for lithium secondary batteries
WO2015043573A2 (fr) * 2013-09-27 2015-04-02 Christian Pszolla Élément de batterie électrochimique rechargeable
DE102013016560A1 (de) * 2013-09-27 2015-04-02 Heide Biollaz Wiederaufladbare elektrochemische Batteriezelle
EP3714078B1 (fr) 2017-11-21 2022-01-05 Speira GmbH Feuille d'électrode de batterie à haute résistance pour la fabrication d'accumulateurs lithium-ion
EP3740981A1 (fr) 2018-01-16 2020-11-25 elfolion GmbH Matériau fonctionnel en feuille et procédé pour sa fabrication
WO2020221564A1 (fr) * 2019-04-30 2020-11-05 Innolith Technology AG Élément de batterie rechargeable
US20220077494A1 (en) * 2019-07-31 2022-03-10 Innolith Technology AG Rechargeable battery cell

Non-Patent Citations (5)

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Title
GUOBAO LI ET AL.: "The influence of polytetrafluorethylene reduction on the capacity loss of the carbon anode for lithium ion batteries", SOLID STATE IONICS, vol. 90, no. 1-4, 2019, pages 221 - 225, XP004071670, DOI: 10.1016/S0167-2738(96)00367-0
HU ET AL.: "Revisiting the initial irreversible capacity loss of LiNio.sCoo. Mno. O cathode material batteries", ENERGY STORAGE MATERIALS, vol. 50, 2022, pages 373 - 379
JANSTA ET AL.: "„Low temperature electrochemical preparation of carbon with a high surface area from polytetrafluoroethylene''", CARBON, vol. 13, no. 5, pages 377 - 380, XP024031952, DOI: 10.1016/0008-6223(75)90005-6
KANG ET AL.: "Investigating the first-cycle irreversibility of lithium metal oxide cathodes for Li batteries", J MATER SCI, vol. 43, pages 4701 - 4706, XP036668044, DOI: 10.1007/s10853-007-2355-6
ZHANG ET AL.: "Revisiting Polytetrafluorethylene Binder for Solvent-Free Lithium-Ion Battery Anode Fabrication''", BATTERIES, vol. 8, no. 6, 2022, pages 57

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DE102023114688A1 (de) 2024-12-05
CN121263876A (zh) 2026-01-02

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