WO2013007420A1 - Electrode, procédé destiné à la fabrication d'une électrode et réservoir d'énergie comprenant une électrode - Google Patents

Electrode, procédé destiné à la fabrication d'une électrode et réservoir d'énergie comprenant une électrode Download PDF

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Publication number
WO2013007420A1
WO2013007420A1 PCT/EP2012/058847 EP2012058847W WO2013007420A1 WO 2013007420 A1 WO2013007420 A1 WO 2013007420A1 EP 2012058847 W EP2012058847 W EP 2012058847W WO 2013007420 A1 WO2013007420 A1 WO 2013007420A1
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WO
WIPO (PCT)
Prior art keywords
electrode
lithium
basic structure
electrically insulating
pores
Prior art date
Application number
PCT/EP2012/058847
Other languages
German (de)
English (en)
Inventor
Ulrich Hasenkox
Martin Tenzer
Ralf Liedtke
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
Publication of WO2013007420A1 publication Critical patent/WO2013007420A1/fr

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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
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/134—Electrodes based on metals, Si or alloys
    • 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
    • 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
    • H01M4/139—Processes of manufacture
    • H01M4/1395—Processes of manufacture of electrodes based on metals, Si or alloys
    • 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
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/381—Alkaline or alkaline earth metals elements
    • H01M4/382—Lithium
    • 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
    • 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
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • 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
    • H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
    • 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

  • Electrode method for producing an electrode and energy storage comprising an electrode
  • the present invention relates to an electrode, a method for producing an electrode and an energy storage device comprising an electrode. More particularly, the present invention relates to an anode for a lithium-sulfur battery and a lithium-sulfur battery having improved stability.
  • Batteries are widely used and used in a variety of applications.
  • lithium-sulfur batteries may be mentioned here which, for example, can have a higher energy density than conventional lithium cells.
  • a lithium-sulfur battery usually consists of a cathode, a separator, an electrolyte and an anode.
  • the cathode may comprise a current collector, such as a metal foil, on which a sulfur-containing mixture is applied as the active material of a cathode coating. Since sulfur is electrically insulating, the cathode coating usually contains a conductive additive, such as carbon black.
  • a binder such as a polymer is usually provided in the cathode coating.
  • the separator is in particular a material which is ionically conductive and the anode space of the
  • Cathode compartment separates.
  • the electrolyte is also ionically conductive.
  • the anode usually comprises a current conductor, such as copper, and a metallic lithium foil.
  • a porous anode active material comprises a salt or an oxide of a Group 14 element and a non-active material that has no reactivity with respect to lithium, such as silica.
  • an electrically conductive substance is added to this material and a binder is added for suitable stability.
  • the present invention relates to an electrode, in particular for a lithium-sulfur battery, comprising a basic structure, which is at least partially constructed of a porous, electrically conductive, carbon-based material, wherein the electrode further comprises metallic lithium which at least partially in the Pores of the basic structure is arranged.
  • a basic structure may in particular be a structure, such as a substrate, which in itself is a stable and
  • the basic structure may already have a suitable mechanical stability or dimensional stability, so that a further carrier substrate need not be required.
  • a carbon-based material may also be used within the meaning of the present invention
  • Invention be a substance or a mixture of substances, which or which
  • the carbon-based material according to the present invention is still porous.
  • a porous material can be understood to mean, in particular, a material which in particular has open pores.
  • the carbonaceous material or the basic structure is configured in particular with an open porosity and is therefore gas-permeable or at least partially open to the outside.
  • the basic structure also has closed pores which may be located inside the basic structure.
  • the carbon-based material is electrically conductive. In particular, electrical conductivities can be provided, which are sufficient for use as an electrode.
  • An advantage of a carbon-based basic structure can be seen in the fact that it may have a low weight, which significantly improves the use of an electrode according to the invention, for example in mobile applications.
  • carbon-based materials are often very inexpensive, which makes the production of the electrode and thus the electrode as such inexpensive.
  • the electrode further comprises metallic lithium which is at least partially disposed in the pores of the basic structure.
  • the lithium may provide the electrode with its function, in particular as an anode in a lithium-sulfur battery.
  • the lithium can be present in particular in the form of a powder or as particles, which in the basic structure
  • the lithium can furthermore be provided in the basic structure or in the electrode such that it is arranged exclusively in the pores, but not on the surface of the basic structure or of the electrode.
  • the particles may have a particle size of ⁇ 1 mm, for example> 5 ⁇ to ⁇
  • the pores may still have a suitable size even after the dissolution of the lithium. Furthermore, the lithium can thus have a particularly good reactivity.
  • the electrode In order to give the basic structure or the electrode with the lithium improved mechanical stability, the electrode
  • the active material of the electrode in an embodiment of the invention further comprise a suitable binder.
  • the binder may in particular comprise or consist of an organic material, such as a polymer.
  • Suitable binders include, for example, polyolefins, polyacrylates, polyesters, polycarbonates. According to the invention, an electrode is provided which has an improved
  • the stability may in particular relate to the stability of the capacity in a plurality of
  • the electrode furthermore has an improved service life, which likewise increases the service life of an energy store equipped with the electrode according to the invention.
  • the electrode by using a porous and conductive basic structure, during charging or discharging, for example, deposition and degradation of lithium on the surface of the electrode can be significantly reduced or even avoided.
  • the electrode is dimensionally stable, in particular with respect to a charge and / or discharge cycle, so that its dimensions do not change, for example, during a degradation and separation of lithium during use. There is thus no or no significant change in volume. This can be a mechanical
  • Damage to the cell components or the cell structure can be reduced or completely prevented, which further reduces the formation of poorly conductive intermediate layers at least.
  • the longevity of the electrode and thus an energy storage device equipped with the electrode can be improved.
  • the high surface area caused by the porous basic structure can be used to realize a high flow rate during a discharge, without, for example, a drop in the cell voltage during discharge due to diffusion voltages.
  • a dendrite formation on the electrode used, for example, as an anode can be avoided by depositing lithium, for example when charging, for example, a lithium-sulfur battery, inside or substantially only in the interior of the pore structure. This can be further avoided that lithium depending on different
  • the basic structure can be constructed from carbon black or graphite.
  • a desired porous structure can be easily produced by easily applicable and easy to control methods.
  • basic structures with a high reproducibility can be produced.
  • such a basic structure offers the advantage that it already has a sufficient electrical conductivity for use as an electrode, whereby the insertion of another conductive substance or a Stromableiters is not necessary.
  • the production can be simplified and material saved, which can save costs and weight.
  • Basic structure in this embodiment further sufficient mechanical stability, so that the electrode itself in a variety of
  • the electrode may comprise a carrier substrate, on which the basic structure is arranged.
  • the mechanical stability of the electrode can be further improved.
  • This embodiment may be particularly advantageous if a particularly high mechanical stability of the electrode is desired.
  • the electrode can be produced without generating a particularly stable basic structure.
  • the carrier substrate can serve, for example, as an additional current conductor, if this is desired in certain fields of application.
  • an electrically insulating material in particular in the form of a porous layer, may be arranged on at least part of the surface of the electrode.
  • the electrically insulating material may be arranged on the surface of the basic structure.
  • the material can completely cover a free surface of the basic structure, such as the surface facing a cathode for use in an energy store, but not close the open porosity of the basic structure, in order to further ensure accessibility
  • Suitable pore sizes may be in a range of ⁇ ⁇ .
  • Electrode-facing surface of the electrode or the basic structure are completely avoided. As a result, the flow rate can be increased more effectively and, for example, a dendrite formation or a reduction of the capacity can be further avoided.
  • electrically non-conductive substances can be used as the insulating material or as the insulating layer.
  • polymers, ceramics or fibers can be used. In detail, these may be polymers consisting of a
  • Solution are applied to the matrix structure of the anode and dried, or melt systems or porous films, which are laminated to the surface. Also conceivable are coating compositions which consist of a polymer and one or more electrically insulating materials in the form of particles or fibers. Also are laminated or glued on
  • the present invention further relates to an energy store, in particular a lithium-sulfur battery, comprising at least one electrode according to the invention.
  • the electrode according to the invention may in particular be an anode of the above-described energy store.
  • the energy store according to the invention can have an improved service life and an improved current density.
  • the present invention further relates to a method for producing an electrode, in particular for a lithium-sulfur battery, comprising the method steps:
  • step b) dispersing the mixture of step a) in a solvent; c) drying the dispersion obtained in step b), in particular by a heat treatment.
  • Energy storage such as a lithium-sulfur battery, can be produced, which has an improved life, and increased capacity even after a plurality of charge and discharge cycles.
  • the electrode is particularly dimensionally stable.
  • a mixture may first be produced which comprises an electrically conductive carbon-based material and metallic lithium.
  • the carbon-based material may be, for example, carbon black or graphite or another compound that is electrically conductive and on
  • Carbon based. This material may also be in the form of small particles are present, for example with a particle size of ⁇ ⁇ , preferably from> 30nm to ⁇ 45 microns.
  • Lithium may also be present in the mixture, for example in the form of a powder.
  • the mixture may further contain a suitable binder such as an inert polymer. The mixture thus prepared may then be in a suitable binder.
  • Solvents such as methyl-2-pyrrolidinone, dialkyl-ethylene glycol or -propylenglykolether with any number of ethylene glycol or propylene glycol, at least one organic carbonate, at least one aliphatic or aromatic cyclic hydrocarbon dispersed.
  • the binder can dissolve, for example, in the solvent and impart suitable stability only in the finished state of the electrode.
  • the proportions can contain between> 1 to ⁇ 50% by weight of binder,> 5 to ⁇ 50% by weight of conductive additive and> 10 to ⁇ 70% by weight of lithium. It may also be possible to introduce the individual components individually into the solvent and thus to prepare and disperse the mixture.
  • the dispersion is dried, whereby a mechanically stable anode is obtained.
  • This can be done for example by a heat treatment, the temperature in particular below the
  • Melting point of lithium of 180 ° C can lie.
  • binders are conceivable which are not soluble in the solvent used, but co-sinter in the drying step. According to the invention, however, a production method without a binder is conceivable, wherein the electrode can consist only of the carbon-based material and lithium.
  • the aforementioned materials may, for example
  • the porosity can be generated in particular by the evaporation of the solvent, wherein the pore sizes are adjustable by the choice of the reaction conditions and the particle sizes used.
  • the structure can be compacted after drying by a pressing operation to adjust the pore size.
  • the pore size may be due to the materials and process parameters used, while being good is reproducible.
  • the electrode can be brought into a suitable form, for example before the drying step.
  • the method comprises the further method step:
  • an improved stability of the electrode can be achieved in this embodiment, which further increases the scope of application of the electrode produced by the inventive method.
  • the step of application can in this case take place in particular before the drying step, since in this production stage a material which is easy to process is present in particular as a dispersion.
  • the dispersion can be doctored onto the carrier substrate.
  • a carrier substrate for example, a metal foil or a metal mesh are suitable. It is also possible
  • Umlaminier polish in which the dispersion is brought from a carrier film on an electrically conductive electrode carrier.
  • the method comprises the further
  • an electrically insulating material in particular as an electrically insulating layer, on at least a part of the surface of the electrode.
  • this further method step it is possible in a suitable manner to completely prevent the deposition of lithium, in particular, on the outer surface of the electrode facing the cathode.
  • An application of the electrically insulating material in this embodiment for example, by applying polymers from a solution followed by a drying step.
  • the lamination, doctoring or sticking of an electrically insulating material, in particular as a film are possible.
  • the electrically insulating material may be, for example, in addition to a polymer, a porous ceramic or a fiber.
  • Fig. 1 is a schematic representation of an embodiment of a
  • FIG. 2 is a schematic representation of the embodiment of FIG. 1 after a discharge process
  • Fig. 3 is a schematic representation of the embodiment of Figure 1 after a charging process.
  • FIG. 1 shows a schematic embodiment of an electrode 1 according to the invention.
  • the electrode 1 can be used, for example, in an energy store such as a lithium-ion battery or a lithium-sulfur battery. Such energy storage are about usable in at least partially electrically powered vehicles. Further are
  • Energy storage according to the invention can be used in all kinds of mobile and stationary applications.
  • Other examples include, for example, mobile phones, computers or household appliances.
  • the electrode 1 comprises a basic structure 2, which is constructed at least partially from a porous, electrically conductive, carbon-based material.
  • the basic structure 2 consists of this material.
  • the carbon-based material may be carbon black or graphite.
  • the basic structure 2 is furthermore porous, ie has pores 3.
  • the pores 3 are preferably open pores, which are open to the outside, ie have accessibility from outside the electrode 1.
  • Exemplary suitable pore sizes of the basic structure 2 may be in a range of ⁇ 1 mm, in particular> 1 ⁇ m to ⁇ 2 ⁇ m.
  • the electrode 1 according to the invention further comprises metallic lithium 4, which is arranged at least partially in the pores 3 of the basic structure 2.
  • the electrode 1 further comprises a binder which is not shown in detail in FIG. If an enhancement of the mechanical stability of the electrode 1 is desired, this is further feasible in that the electrode 1 comprises a carrier substrate 5 on which the basic structure 2 is arranged.
  • the carrier substrate 5 can be any suitable carrier substrate 5 on which the basic structure 2 is arranged.
  • an electrically insulating material 6, in particular in the form of a porous layer, may be arranged on at least part of the surface of the electrode 1 or the basic structure 2. This makes it possible to prevent lithium from precipitating on the surface of the electrode 1 in particular, which can further improve the properties of the electrode 1, as will be explained with reference to FIGS. 2 and 3. The growth of dendrites which can grow through the separator is thereby prevented.
  • the electrically insulating material 6 may in particular a
  • Polymer a ceramic or a fiber.
  • Mixture comprising an electrically conductive carbon-based material and metallic lithium are produced.
  • the mixture may further include, as far as this is desired with respect to the mechanical stability of the electrode 1, a binder. This mixture can then be dispersed in a solvent.
  • a carrier substrate 5 is desired, the
  • Dispersion are applied to the carrier substrate 5. Thereafter, the dispersion alone or the dispersion applied on the support substrate 5 may be dried and further shaped by, for example, a heat treatment.
  • an electrically insulating material 6, in particular as an electrically insulating layer, can be applied to at least part of the surface of the electrode 1 or of the surface of the basic structure 2.
  • Figure 2 is one, for example in a lithium-sulfur battery
  • electrode 1 shown after a discharge.
  • the electrode 1 corresponds to that shown in FIG. 1, with identical or corresponding ones
  • FIG. 3 An electrode 1 according to the invention after a charging process is shown in FIG. 3, the electrode corresponding to that shown in FIG. 1, for which reason identical or corresponding components are provided with the same reference numerals.
  • FIG. 3 it can be seen that, in turn, the charging process takes place, for example, when charging a lithium-sulfur battery
  • the lithium 4 has thereby deposited completely or at least predominantly in the pores 3.
  • the lithium can be

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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)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

La présente invention concerne une électrode (1), notamment pour une batterie lithium-soufre. Afin d'améliorer la stabilité dimensionnelle ainsi que les propriétés de capacité, l'électrode (1) comprend une structure de base (2) constituée au moins partiellement d'un matériau poreux conducteur d'électricité à base de carbone, l'électrode (1) comportant en outre du lithium métallique (4) lequel est au moins partiellement disposé dans les pores (3) de la structure de base (2). En outre, la présente invention concerne un procédé destiné à la fabrication d'une électrode (1) ainsi qu'un réservoir d'énergie comprenant l'électrode (1).
PCT/EP2012/058847 2011-07-12 2012-05-14 Electrode, procédé destiné à la fabrication d'une électrode et réservoir d'énergie comprenant une électrode WO2013007420A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102011079026.8 2011-07-12
DE102011079026A DE102011079026A1 (de) 2011-07-12 2011-07-12 Elektrode, Verfahren zum Herstellen einer Elektrode und Energiespeicher umfassend eine Elektrode

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WO2013007420A1 true WO2013007420A1 (fr) 2013-01-17

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WO (1) WO2013007420A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CZ307429B6 (cs) * 2016-10-14 2018-08-15 Contipro A.S. Způsob výroby kompozitního materiálu aktivní katody Li-S baterií
US10468665B2 (en) 2015-01-29 2019-11-05 Sigma Lithium Limited Composite materials

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102014207999A1 (de) * 2014-04-29 2015-10-29 Robert Bosch Gmbh Dreidimensional strukturierte Lithium-Anode
EP3293801A1 (fr) 2016-09-12 2018-03-14 Lithium Energy and Power GmbH & Co. KG Électrode ayant un comportement de sécurité amélioré et cellule de batterie la comprenant

Citations (3)

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Publication number Priority date Publication date Assignee Title
US5814420A (en) * 1994-11-23 1998-09-29 Polyplus Battery Company, Inc. Rechargeable positive electrodes
US20070190422A1 (en) * 2006-02-15 2007-08-16 Fmc Corporation Carbon nanotube lithium metal powder battery
US20100051856A1 (en) 2008-08-26 2010-03-04 Samsung Sdi Co., Ltd. Porous anode active material, method of manufacturing the same, anode comprising the same, and lithium battery comprising the anode

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5814420A (en) * 1994-11-23 1998-09-29 Polyplus Battery Company, Inc. Rechargeable positive electrodes
US20070190422A1 (en) * 2006-02-15 2007-08-16 Fmc Corporation Carbon nanotube lithium metal powder battery
US20100051856A1 (en) 2008-08-26 2010-03-04 Samsung Sdi Co., Ltd. Porous anode active material, method of manufacturing the same, anode comprising the same, and lithium battery comprising the anode

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US10468665B2 (en) 2015-01-29 2019-11-05 Sigma Lithium Limited Composite materials
CZ307429B6 (cs) * 2016-10-14 2018-08-15 Contipro A.S. Způsob výroby kompozitního materiálu aktivní katody Li-S baterií

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