WO2015067474A2 - Cellule électrochimique et procédé de fabrication de celle-ci - Google Patents

Cellule électrochimique et procédé de fabrication de celle-ci Download PDF

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Publication number
WO2015067474A2
WO2015067474A2 PCT/EP2014/072701 EP2014072701W WO2015067474A2 WO 2015067474 A2 WO2015067474 A2 WO 2015067474A2 EP 2014072701 W EP2014072701 W EP 2014072701W WO 2015067474 A2 WO2015067474 A2 WO 2015067474A2
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WO
WIPO (PCT)
Prior art keywords
lithium
fibers
protective layer
electrochemical cell
ion
Prior art date
Application number
PCT/EP2014/072701
Other languages
German (de)
English (en)
Other versions
WO2015067474A3 (fr
Inventor
Thomas Wöhrle
Felix Eberle
Bernd Schumann
Calin Iulius WURM
Vikram Anil GODBOLE
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 CN201480061234.5A priority Critical patent/CN105765759B/zh
Publication of WO2015067474A2 publication Critical patent/WO2015067474A2/fr
Publication of WO2015067474A3 publication Critical patent/WO2015067474A3/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
    • 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
    • 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
    • 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
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M12/00—Hybrid cells; Manufacture thereof
    • H01M12/08—Hybrid cells; Manufacture thereof composed of a half-cell of a fuel-cell type and a half-cell of the secondary-cell type
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • 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
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/431—Inorganic material
    • H01M50/434—Ceramics
    • 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
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0088—Composites
    • 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
    • H01M4/40—Alloys based on alkali metals
    • H01M4/405—Alloys based on lithium
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/18—Cells with non-aqueous electrolyte with solid electrolyte
    • H01M6/185—Cells with non-aqueous electrolyte with solid electrolyte with oxides, hydroxides or oxysalts as solid electrolytes
    • 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 an electrochemical cell and a method for their production and their use according to the preamble of the independent claims.
  • lithium-ion batteries will be used in stationary applications (such as in wind turbines), in mobile applications (such as in hybrid and electric vehicles) and in the consumer sector (for example, in laptops and mobile phones)
  • Battery systems are used whose operating principle is not based on an intercalation of metallic substances in the electrode material, but on the use of metallic anodes such.
  • Lithium anodes wherein as the counter electrode, for example, an oxygen electrode is provided.
  • the operation of this type of battery systems is based on a chemical transformation of the anode material and shows very high energy densities or high specific energies at the cellular level.
  • oxygen electrode when the lithium anode is connected to a discharging process of the battery cell, the reduction of molecular oxygen and the formation of lithium peroxides occur.
  • lithium-air cells thus comprise at least one oxygen-based positive electrode and at least one metallic lithium-based or lithium-silicon alloy negative electrode in which lithium is incorporated into a silicon lattice Processes associated with a crystalline structural change of the electrode.
  • Such Lithium-air cell can be found, for example, in US 5,510,209 A or in the publication by Jake Christensen et al., Journal of The Electrochemical Society, 159 (2) R1-R30 (2012).
  • this type of battery cells for example, also have an anode of a lithium alloy, for example in the form of an indium or aluminum alloy.
  • the abovementioned oxygen cathode may, for example, have a porous structure of carbon or gold with pores in the nanometer range, which may be the substances produced during a discharge of the battery cell, for example
  • a gas distributor flow field
  • a lithium-ion-conducting separator which acts electrically insulating.
  • This separator is designed to be free of pores to prevent gases and liquid media, which could damage metallic lithium, for example, from the anode.
  • Separator material is, inter alia, sintered gas-tight ceramic layers, u. a. for example in the form of grenades.
  • sintered gas-tight ceramic layers u. a. for example in the form of grenades.
  • Such systems can be found, for example, in DE 10 2004 010 892 B3 or DE 10 2007 030 604 A1.
  • a dense, thin-laid ceramic lithium ion conductive layer protects the metallic lithium lithium anode from harmful gases such as nitrogen, carbon dioxide or water vapor, as well as liquid solvents that may be part of an electrolyte in the battery cell. These can be irreversible with metallic lithium of the anode which may undesirably cause lithium dendrites to possibly cause internal short circuits.
  • volume surges of the metallic lithium anode occur and greatly burden the mechanical integrity of the thin ceramic layer.
  • the resulting mechanical stress leads to enormous pressure on the ceramic protective layer, which can lead to embrittlement or mechanical breakage.
  • there may be a replacement of the layered ceramic by unequal pressurization and their lack of elasticity.
  • DE 10 2010 054 610 A1 discloses an electrochemical cell whose negative electrode is coated with a protective layer, which in turn has fibers made of a lithium-ion-conducting material.
  • the present invention relates to an electrochemical cell, a process for their preparation and their use with the characterizing features of the independent claims.
  • an electrochemical cell which has a lithium-containing anode and a cathode, wherein the lithium-containing anode is provided with a protective layer.
  • This protective layer comprises fibers of a non-lithium-ion-conducting material, wherein the fibers are in contact with a lithium-ion-conducting material of the protective layer.
  • the protective layer contains in addition to fibers of a non-lithium-ion conducting material, a lithium-ion conductive material.
  • SiBNC fibers carbon fibers, glass fibers, fibers made of a non-lithium ion-conducting ceramic material or as plastic fibers, for example, made of a polyimide or paramid.
  • the advantage of using these fibers is that they are chemically inert and mechanically stable, and even with the addition of smaller amounts of fibers, there are above-average effects with regard to the mechanical strength and elasticity of the protective layer.
  • the lithium-ion conducting material contained in the protective layer comprises a ceramic garnet having the composition LiLaZr0 2 , a perovskite having the composition Li 0 , 57 La 0 , 3 TiO 3 or a sulfide-based ceramic lithium-ion conductor, in particular based on Lii 0 GeP 2 Si2 contains.
  • the advantage of these lithium-ion conducting materials is that they are long-term stable and chemically inert, so that together with the fibers contained in the protective layer, a significant improvement in the life of the electrochemical cell and a significantly improved cycle stability is achieved.
  • the surface of the lithium-containing anode of the electrochemical cell is first provided with fibers such that a porous matrix is formed. Subsequently, a lithium-ion conducting material is introduced into this porous matrix.
  • the protective layer for the lithium-containing anode of the electrochemical cell is first generated separately. For this purpose, in a first step, a porous matrix of fibers of a non-lithium-ion-conducting material on the surface of
  • Ion-conducting material equipped. This loading can be done for example by sputtering, laser evaporation of the lithium-ion conducting material or by an aerosol coating.
  • the electrochemical cell of the invention can be advantageously in
  • lithium-ion or lithium-air batteries for example in mobile or stationary applications.
  • Figure 1 shows the schematic cross section of an inventive
  • FIG. 1 shows a battery cell 10 according to one embodiment of the
  • the battery cell 10 includes a housing 12 in which the electrochemical components of the battery cells 10 are housed. These include in particular a preferably lithium-containing battery cells 10 are housed. These include in particular a preferably lithium-containing battery cells 10 are housed. These include in particular a preferably lithium-containing battery cells 10 are housed. These include in particular a preferably lithium-containing battery cells 10 are housed. These include in particular a preferably lithium-containing battery cells 10 are housed. These include in particular a preferably lithium-containing
  • Anode 14 and a cathode 16 If the battery cell 10, for example, designed as a lithium-air cell, then the anode 14 comprises metallic lithium, for example in the form of elemental lithium or in the form of a lithium alloy.
  • the cathode 16 may in this case, for example, as air or
  • Oxygen electrode performs his.
  • the anode 14 for example, a protective layer 18 on.
  • the anode 14 is preferably covered with the protective layer 18 substantially over its full area, at least on its large area facing the cathode 16.
  • the protective layer 18 comprises fibers 20 which increase the mechanical stability of the protective layer 18 with respect to its elasticity and mechanical properties
  • fibers 20 preferably fibers of a non-lithium-ion conducting material are provided, such as SiBNC fibers or fibers of another, non-lithium-ion-conducting ceramic material.
  • carbon fibers are also suitable as well as plastic fibers, for example of polyimide or an aramid.
  • the fibers 20 preferably form a porous matrix within the protective layer 18;
  • the fibers 20 can be present, for example, in woven form or else in a three-dimensionally disordered form.
  • at least one lithium-ion conductive material 22 is introduced, which influences the overall conductivity of the protective layer 18 with regard to the conduction of lithium ions. So the conductivity is the
  • Protective layer for lithium ions preferably at least 10 "6 S / cm.
  • the layer thickness of the protective layer 18 is, for example, 0.1 to 1000 ⁇ .
  • the protective layer 18 itself comprises fibers with a total weight fraction of 0.1 to 50 percent by weight based on the total weight of the protective layer 18.
  • Protective layer 18 is introduced from fibers 20, ceramic lithium-ion conductors such as corresponding perovskites, for example Li 0) 57 La 0 , 3 are suitable Ti0 3 and ceramic lithium-ion conductors of the sulfide class such as.
  • LiioGeP 2 Si 2 LiioGeP 2 Si 2 .
  • a ceramic garnet of the composition LiLaZr0 2 is suitable as a ceramic lithium-ion conductor, for example.
  • the lithium-ion conductive material 22 ensures sufficient conductivity of the protective layer 18 for lithium ions.
  • the lithium-ion conductive material 22 can be introduced, for example, by sputtering, or by an aerosol coating into the porous matrix of the fibers 20.
  • the porous matrix of fibers 20 on the surface of the anode 14 can first be produced in a first step.
  • the generated porous matrix of fibers 20 is equipped with the lithium-ion-conducting material 22.
  • porous matrix of fibers 20 it is also possible first separately to produce the porous matrix of fibers 20, to equip them with the lithium-ion conducting material 22 and to apply this pre-fabricated protective layer 18 in a final step on a large area of the anode 14.
  • the electrochemical cell 10 may additionally include a non-illustrated
  • the protective layer 18 additionally assumes the function of a separator within the electrochemical cell 10.
  • the electrochemical cell A is a
  • the electrochemical cell B is an electrochemical cell with a protective layer according to the prior art, as listed, for example, in US Pat. No. 6,402,795 or US Pat. No. 6,723,140.
  • the electrochemical cell C is an electrochemical cell 10 according to the invention containing a protective layer 18 in contact with its anode 14.
  • the number of cycles is here the number of cycles comprising a charge and a discharge process, which can be completed until the electrochemical cell has only a residual electrical capacity of 80% of the nominal capacity. It is a C / 20 cyclization, i. H. one cycle of discharge lasts 20 hours, with the discharge current selected accordingly.
  • the electrochemical cell according to the invention can be advantageously, for example, as a battery cell in mobile applications such as e-bikes, in electric vehicles or in hybrid vehicles and in stationary applications, for example, energy storage for regenerative
  • the above-described electrochemical cell is not limited to the embodiment as a lithium-air cell but may, for example, be designed as a lithium-ion cell of today's generation.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Ceramic Engineering (AREA)
  • General Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Physics & Mathematics (AREA)
  • Hybrid Cells (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)

Abstract

L'invention concerne une cellule électrochimique (10) qui comporte une anode contenant du lithium (14) et une cathode (16). L'anode contenant du lithium (14) comporte une couche protectrice (18), et la couche protectrice (18) comprend des fibres (20), en matériau non conducteur d'ions lithium, qui sont en contact avec un matériau (22) conducteur d'ions lithium de la couche protectrice (18).
PCT/EP2014/072701 2013-11-08 2014-10-23 Cellule électrochimique et procédé de fabrication de celle-ci WO2015067474A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN201480061234.5A CN105765759B (zh) 2013-11-08 2014-10-23 电化学电池及其制造方法

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102013222784.1 2013-11-08
DE201310222784 DE102013222784A1 (de) 2013-11-08 2013-11-08 Elektrochemische Zelle und Verfahren zu deren Herstellung

Publications (2)

Publication Number Publication Date
WO2015067474A2 true WO2015067474A2 (fr) 2015-05-14
WO2015067474A3 WO2015067474A3 (fr) 2015-07-02

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Country Link
CN (1) CN105765759B (fr)
DE (1) DE102013222784A1 (fr)
WO (1) WO2015067474A2 (fr)

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KR101926917B1 (ko) 2016-08-17 2018-12-07 현대자동차주식회사 리튬 공기 전지용 음극 및 이의 제조방법
KR102328253B1 (ko) * 2016-09-30 2021-11-18 주식회사 엘지에너지솔루션 전도성 직물로 형성된 보호층을 포함하는 리튬 이차전지용 음극 및 이를 포함하는 리튬 이차전지
US10177427B2 (en) * 2017-02-10 2019-01-08 General Electric Company Electrochemical cell for use in high temperature metal-air battery
US10826145B2 (en) 2017-02-10 2020-11-03 General Electric Company Electrochemical cell for use in high temperature metal-air battery
CN107293690B (zh) * 2017-06-12 2019-12-13 中航锂电（洛阳）有限公司 一种锂离子电池正极复合极片及其制备方法、锂离子电池
CN111788718A (zh) * 2018-03-05 2020-10-16 罗伯特·博世有限公司 抑制金属离子电池组电池中的枝晶形成和生长的离子沉积偏置
CN110911685B (zh) * 2019-11-28 2021-09-14 宁德新能源科技有限公司 用于负极的组合物和包含该组合物的保护膜、负极和装置

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US5723140A (en) 1996-01-30 1998-03-03 Pearsall; Charles W. Method for treating pressure ulcers
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DE102004010892B3 (de) 2004-03-06 2005-11-24 Christian-Albrechts-Universität Zu Kiel Chemisch stabiler fester Lithiumionenleiter
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DE102010054610A1 (de) 2010-12-15 2012-06-21 Li-Tec Battery Gmbh Elektrochemische Zelle

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US5723140A (en) 1996-01-30 1998-03-03 Pearsall; Charles W. Method for treating pressure ulcers
US6402795B1 (en) 1998-02-18 2002-06-11 Polyplus Battery Company, Inc. Plating metal negative electrodes under protective coatings
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DE102004010892B3 (de) 2004-03-06 2005-11-24 Christian-Albrechts-Universität Zu Kiel Chemisch stabiler fester Lithiumionenleiter
DE102007030604A1 (de) 2007-07-02 2009-01-08 Weppner, Werner, Prof. Dr. Ionenleiter mit Granatstruktur
DE102010054610A1 (de) 2010-12-15 2012-06-21 Li-Tec Battery Gmbh Elektrochemische Zelle

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Publication number Publication date
CN105765759A (zh) 2016-07-13
DE102013222784A1 (de) 2015-05-13
WO2015067474A3 (fr) 2015-07-02
CN105765759B (zh) 2019-04-19

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