WO2015197597A2 - Batterie couche mince à faible teneur en fluide et à durée de vie accrue - Google Patents

Batterie couche mince à faible teneur en fluide et à durée de vie accrue Download PDF

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Publication number
WO2015197597A2
WO2015197597A2 PCT/EP2015/064069 EP2015064069W WO2015197597A2 WO 2015197597 A2 WO2015197597 A2 WO 2015197597A2 EP 2015064069 W EP2015064069 W EP 2015064069W WO 2015197597 A2 WO2015197597 A2 WO 2015197597A2
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WIPO (PCT)
Prior art keywords
film battery
thin
inorganic
silicon
fluid
Prior art date
Application number
PCT/EP2015/064069
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German (de)
English (en)
Other versions
WO2015197597A3 (fr
Inventor
Miriam Kunze
Ulrich Peuchert
Original Assignee
Schott 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.)
Filing date
Publication date
Priority claimed from DE102015103857.9A external-priority patent/DE102015103857A1/de
Application filed by Schott Ag filed Critical Schott Ag
Priority to CN201580033610.4A priority Critical patent/CN106663748A/zh
Priority to JP2016575011A priority patent/JP2017521827A/ja
Publication of WO2015197597A2 publication Critical patent/WO2015197597A2/fr
Publication of WO2015197597A3 publication Critical patent/WO2015197597A3/fr
Priority to US15/386,060 priority patent/US20170104188A1/en

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    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/083—Glass compositions containing silica with 40% to 90% silica, by weight containing aluminium oxide or an iron compound
    • C03C3/085—Glass compositions containing silica with 40% to 90% silica, by weight containing aluminium oxide or an iron compound containing an oxide of a divalent metal
    • C03C3/087—Glass compositions containing silica with 40% to 90% silica, by weight containing aluminium oxide or an iron compound containing an oxide of a divalent metal containing calcium oxide, e.g. common sheet or container glass
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/11—Primary casings; Jackets or wrappings characterised by their shape or physical structure having a chip structure, e.g. micro-sized batteries integrated on chips
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/078—Glass compositions containing silica with 40% to 90% silica, by weight containing an oxide of a divalent metal, e.g. an oxide of zinc
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/089—Glass compositions containing silica with 40% to 90% silica, by weight containing boron
    • C03C3/091—Glass compositions containing silica with 40% to 90% silica, by weight containing boron containing aluminium
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/089—Glass compositions containing silica with 40% to 90% silica, by weight containing boron
    • C03C3/091—Glass compositions containing silica with 40% to 90% silica, by weight containing boron containing aluminium
    • C03C3/093—Glass compositions containing silica with 40% to 90% silica, by weight containing boron containing aluminium containing zinc or zirconium
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/095—Glass compositions containing silica with 40% to 90% silica, by weight containing rare earths
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C3/00—Glass compositions
    • C03C3/04—Glass compositions containing silica
    • C03C3/076—Glass compositions containing silica with 40% to 90% silica, by weight
    • C03C3/097—Glass compositions containing silica with 40% to 90% silica, by weight containing phosphorus, niobium or tantalum
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C8/00—Enamels; Glazes; Fusion seal compositions being frit compositions having non-frit additions
    • C03C8/24—Fusion seal compositions being frit compositions having non-frit additions, i.e. for use as seals between dissimilar materials, e.g. glass and metal; Glass solders
    • 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
    • H01M10/04—Construction or manufacture in general
    • H01M10/0436—Small-sized flat cells or batteries for portable equipment
    • 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
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/117—Inorganic 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/117—Inorganic material
    • H01M50/119—Metals
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/121—Organic 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/183—Sealing members
    • H01M50/186—Sealing members characterised by the disposition of the sealing members
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/183—Sealing members
    • H01M50/19—Sealing members characterised by the material
    • H01M50/191—Inorganic 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/183—Sealing members
    • H01M50/19—Sealing members characterised by the material
    • H01M50/193—Organic material
    • 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
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/131—Primary casings; Jackets or wrappings characterised by physical properties, e.g. gas permeability, size or heat resistance
    • 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
    • H01M6/40—Printed batteries, e.g. thin film batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the invention relates to thin-film batteries, in particular lithium-based thin-film batteries, which have a low fluid content and a resulting increased
  • miniaturized storage elements for electrical energy are becoming increasingly important, for example for so-called smart cards.
  • lithium-based thin-film batteries have a number of particularly preferred properties, for example, a low weight and a high
  • Cycle stability i. the number of loading and unloading
  • Lithium-based batteries or accumulators has an extremely low reduction potential. Also, other of the active battery materials of a lithium-based battery or a lithium-based Accumulators are extremely vulnerable to
  • Anode material in a lithium-based electrical energy storage unit does not use elemental or metallic lithium, but rather a material that is improved in its durability, such as graphite, is incorporated into the lithium as an elemental material, i. with the
  • Oxidation level 1 can be intercalated. But even this material has a high reactivity.
  • Other lithium-based battery materials also have high hygroscopicity, i. have an attractive effect on water.
  • Lithium carbonate Li 2 CC> 3, lithium hydroxide, LiOH or
  • US 2004/0018424 A1 describes a rechargeable lithium-based thin film cell comprising a polyimide substrate.
  • the polyimide substrate is specially dried by first placing the polyimide in acetone, replacing it
  • the thin-film cell still has a
  • Parylene topcoat which acts as a permeation barrier to protect cell materials from degradation.
  • the substrate material thus obtained is still not completely freed of water, but it has only come to a reduction of the water content. Furthermore have polymeric
  • Encapsulating materials usually have insufficient barrier to fluids, especially for particularly sensitive applications.
  • the electrochemical storage unit in which a Multilayer laminate is pressed onto the functional layers of the electrochemical storage unit.
  • the multilayer laminate may contain a metallic layer. Furthermore, in contact with the
  • Organic adhesive material itself corrosively acts on the functional materials of the cell.
  • Functional layers are applied to a substrate.
  • the thin-film battery comprises a cover, which at a distance from the surface of the thin-film battery
  • Functional layer creates a gap. Furthermore, the battery is protected by a seal or encapsulation based on an organic polymer between the substrate and the cover from environmental influences.
  • the gap serves to compensate for thickness variations or thermal expansion of the functional layers of the battery, which can result in the respective charging and discharging cycles of the battery.
  • the disadvantage here is that such a gap is naturally fluid-filled and thus
  • Encapsulation materials usually have a permeation rate for fluids, such as water, which is d m 2 at about 1 g / cc. Although this is sufficient for most applications of such sealing polymers, but you come in applications in the high performance area, ie
  • Devices such as a thin-film-based lithium-ion battery or a lithium-ion battery to the limits of performance.
  • hermetic encapsulation for a lithium-ion battery This can consist both of an encapsulation, that between the substrate and that on the substrate
  • the heating of the substrate material can be carried out both before the coating thereof with a first layer and during the
  • US 2010/0190051 A1 describes a barrier layer for a thin-film battery. This can both off
  • Tin compounds such as tin oxide, phosphate or - fluorophosphate exist, as well as be formed of glass, for example, a chalcogenide glass, a tellurite glass or a borate glass.
  • the layer encapsulates the layers of the thin-film battery and even completely prevents or prevents the layers from being exposed to air or moisture.
  • these layers have a good barrier effect, in particular the glass materials themselves are extremely susceptible to environmental influences.
  • the chalcogenide glasses are not stable in air and decompose.
  • the layer materials are not suitable for use in batteries which are to be stored under normal environmental conditions.
  • Lithium electrode This consists of a protective layer, which may be formed amorphous or glassy, but at the same time ion conducting for the active battery material, that is lithium in this case, the layer always being produced by a coating process and being thinner than 5 ym.
  • the system of lithium metal and deposited protective layer is referred to as an encapsulated electrode and has the consequence that the lithium electrode in contact with fluids, for example
  • No. 6,387,563 B1 describes a protective layer for a thin-film battery, the protective layer consisting of an epoxy-based system and a glass layer.
  • the epoxide layer acts as an adhesive layer for the
  • the epoxy layer can be cured through the glass layer.
  • Epoxy resin can thereby the formation of "gas pockets" in the battery and thus their reactions with the
  • Encapsulation consists of an organic compound onto which a "cap” or a superstrate is applied, leaving a gap in the battery, or that
  • Organic encapsulant material may also be applied so as to completely encase the layered structure of the thin film battery.
  • the US 2013/0260230 AI describes a method for
  • WO 2014/062676 Al describes the use of a glass substrate which has a thermal
  • US 2012/040211 A describes a glass film which can serve as a substrate for a lithium-ion battery.
  • This glass film has a water permeation rate of less than 1 g / m 2 -d and an oxygen permeation rate of less than 1 cc / m 2 -d. However, such a value is still extremely high and is more in the
  • Lifespan can be used.
  • the object of the invention is to provide a thin-film battery with an increased service life and a low content of fluids, in particular of corrosive and / or degradative fluids.
  • Another aspect of the invention relates to the provision of a
  • the invention is achieved by a thin-film battery according to claim 1, an inorganic, silicon-containing,
  • silicate substantially fluid-free material according to claim 22 and a method for
  • the thin film battery of the present invention is a rechargeable battery.
  • the thin film battery of the present invention is a thin film battery of the present invention.
  • Such thin film batteries typically include a substrate on which different ones in a particular sequence
  • Functional layers such as Abieiter for cathode and anode, a cathode layer, an electrolyte and optionally an anode are applied as well as other layers, for example, for encapsulation of the battery to protect against degradation due to environmental influences.
  • a construction of a battery is described by way of example in US 2004/0018424 Al, wherein the exact design of the battery may differ depending on the type and manufacturer.
  • the thin-film battery, particularly the lithium-based thin film battery, of the present invention has a long life, and the life of such a battery can be specified in a variety of ways.
  • a failure of the battery consists in the fact that the battery can no longer be supplied or removed energy or that the
  • One cycle includes one charge and one charge each
  • Atmosphere i.e. uncontrolled temperature
  • Thin-film battery is also the so-called
  • the thin film battery of the present invention has an increased life such that at least one of the following features is satisfied:
  • cycle stability is at least 5000 cycles, preferably at least 10,000 cycles and more preferably at least 15,000 cycles,
  • it can not be stored for at least 1 year, preferably for at least 2 years and more preferably for at least 5 years, in particular not in a controlled environment with respect to temperature and / or humidity, or it has a continuous operating stability of at least
  • fluids are liquids and / or gaseous substances and also their chemical or physical adsorbates and / or their derivatives.
  • a derivative in the present invention is understood to be a compound of a fluid which is present in solid form but can easily be converted back into a fluid form, for example by the addition of heat and the resulting decomposition of the fluid
  • fluid here means water in liquid form or as water vapor, or else its presence as chemically or physically bound surface water in Form of an adsorbate or its occurrence as, for example, water of crystallization in solid form in one
  • CO 2 can be present in gaseous or adsorbed form
  • the total content of the thin film battery of the present invention is 2000 ppm or less, preferably 500 ppm or less, and more preferably 200 ppm or less, and more preferably 50 ppm or less, based on the weight of the thin film battery.
  • a thin-film battery or a material having such a low fluid content is referred to in the present invention as substantially fluid-free.
  • the thin-film battery of the present invention has at least one element made of an inorganic, silicon-containing, in particular
  • silicate, substantially fluid-free material a fluid content, in particular an H 2 ⁇ 0 content, of less than 2 wt .-%, preferably less than 0.5 wt .-% and
  • the fluid content of the inorganic, silicon-containing, in particular silicate, substantially fluid-free material is determined by thermal analysis, for example by a differential thermal analysis or a thermogravimetry or a dynamic
  • the thin-film battery furthermore has at least one encapsulation, wherein the encapsulation at least partially seals at least one interface of at least one functional layer of the thin-film battery. It is under a
  • Functional layer of the battery understood a layer which is active in the loading and unloading for
  • anode or in the form of an electron or ion-conducting function.
  • the at least one encapsulation is preferably at least partially in the form of the inorganic,
  • Substantially fluid-free material is formed.
  • the encapsulation may also be at least partially in the form of an organic and / or semi-organic Material, for example, be formed as a hybrid material of a SiC> 2 gel with functional organic groups.
  • the inorganic, silicon-containing, in particular silicate, essentially fluid-free material of the present invention has a permeation rate for fluids, especially for water, of ⁇ 10 -3 g / (m 2 -d), preferably of ⁇ 10 -5 g / (m 2 -d) and more preferably of ⁇ 10 ⁇ 6 g / (m 2 -d).
  • the inorganic, silicon-containing, in particular silicate, substantially fluid-free material of the present invention is a further embodiment of the invention.
  • Invention further has a specific electrical resistance at a temperature of 350 ° C and a
  • Siliceous, substantially fluid-free material of the present invention is preferably characterized by a maximum load temperature 9 Max of at least
  • the maximum load temperature is the temperature at which the
  • Decomposition of the material for example by decomposition into several, including gaseous, components, or its melting or softening temperature. Unless it is a
  • Glass transition temperature T g is determined by the intersection of the tangents to the two branches of
  • the inorganic, silicon-containing, in particular silicate, substantially fluid-free material of the present invention is a further embodiment of the invention.
  • Expansion coefficient in the range of 2.0 x 10 -6 / ⁇ to 10 x 10 "6 / ⁇ , preferably of 2.5 10" 6 / K to 9.5 10 "6 / K and particularly preferably from 3.0 x 10 -6 / ⁇ to 9.5 x 10 -6 / ⁇ on.
  • the linear thermal expansion coefficient is meant in the range of 20-300 ° C. the terms and 0 (20-300 are within the scope of this The value given is the nominal mean thermal
  • Silicate-like, substantially fluid-free material of the present invention preferably contains network formers and separation site formers, the molar ratio of separation site formers to network formers is less than or equal to 0.25, preferably less than or equal to 0.2 and particularly preferably between 0.015 and 0.16.
  • network elements are elements which form coordination polyhedra with oxygen, these being
  • alkali and / or alkaline earth metals as network formers are exemplified aluminum and / or boron and / or silicon into consideration.
  • Silicate, substantially fluid-free material of the present invention preferably has in its structure a network of corner-sharing structural
  • Fluids are suitable.
  • mica or phyllosilicates generally in their crystalline Structure on the one layers, in which the coordination polyhedron, in this case of oxygen tetrahedral coordinated silicon, in the form of
  • Hexagonal rings are arranged in the middle fluids can be stored. Furthermore, between the layers of the layered silicates further compounds
  • Phyllosilicates are also referred to as swellability and often exploited technically, for example, by targeted organic groups are added, but then represents a disadvantage when freedom from fluid is required.
  • Composition - for example, ions can migrate. This is in the case of so-called "LLZO" materials
  • zirconium are constructed (wherein a part of the zirconium may also be replaced by niobium or tantalum or similar elements) and have a particularly high lithium-ion conductivity.
  • Embodiment of the invention isotropic.
  • a material is then called, if its
  • silicate substantially fluid-free
  • Material formed amorphous. It is preferably a glass.
  • inorganic, silicon-containing, in particular silicate, essentially fluid-free material can be present as substrate and / or as superstrate in the thin-film battery according to the invention.
  • Thin-film battery form and as a Superstrat a cover, which, for example, on the finished coatings of the thin-film battery
  • inorganic, silicon-containing, in particular silicate, substantially fluid-free material then, if it is not used as a substrate, so as a base for the application of other finishes or structures, but as Auflagerndes element,
  • cover or as a cover glass is used.
  • the Superstrat can also do that before his own Use as a superstrate, for example, as a cover glass, have been subjected to separate processes, during which it has the function of a substrate for these separate
  • Processes has taken, and wear, for example, structures or structures, such as optical coatings for selectively adjusting the optical transmission.
  • the superstrate can be formed from the same material, that is to say with the same chemical composition, as the latter
  • the superstrate is merely used as a diffusion barrier with respect to the passage of fluids, ie, for example, optical or
  • Expansion coefficients of substrate and superstrate are different, can be a thermal
  • Expansion coefficient of the glass solder are chosen so that it assumes an average value. Furthermore, the
  • the material is preferably formed as a band or disc, for example as a glass band or glass pane, and wherein the shaping is inline as a hot forming process,
  • the inorganic, silicon-containing, in particular silicate, substantially fluid-free material of the thin-film battery according to the invention is also possible for the inorganic, silicon-containing, in particular silicate, substantially fluid-free material of the thin-film battery according to the invention to be present as an alternative or additionally as a layer.
  • the material if it is present as a layer, by a vapor deposition, preferably by a
  • the thin-film battery according to the invention further comprises at least one fluid getter.
  • a getter is a material that can bind fluid.
  • this getter is designed as
  • this getter comprises a metal, for example a non-noble metal, preferably an alkali metal or alkaline earth metal or a mixture or alloy of metals, for example
  • Both fonts have in common that they turn off on lithium-based systems that have a liquid electrolyte, i. one which consists of a solvent and a conductive salt. If water or hydrogen in the
  • Battery cover associated with the escape of hazardous substances, may result. Furthermore, non-soluble lithium compounds, such as LiF, may continue to form, depriving the system of the element essential to electrical energy storage.
  • non-soluble lithium compounds such as LiF
  • the getter materials of the present invention are rather formed such that other fluids, for example, in addition to water, also oxygen and / or nitrogen,
  • Getter materials effective mechanisms can still be effective in a pure solid-state battery, which is an object of the present invention. Rather, here are missing important components, which for the course of the necessary in the prior art reactions are necessary.
  • fluorine is in such
  • Solid state battery is not available, so that an RF gettering is not displayed.
  • the inorganic, silicon-containing in particular
  • siliceous, substantially fluid-free material of the present invention has a thickness less than 2 mm
  • preferably less than 1 mm particularly preferably less than 500 ⁇ m, very particularly preferably less than or equal to 200 ⁇ m and most preferably not more than 100 ⁇ m.
  • Invention comprises the inorganic, silicon-containing,
  • silicate essentially fluid-free
  • Material has a certain content of lithium. This is particularly advantageous when it comes to the
  • thin-film battery according to the invention is a lithium-based thin-film battery. If one of the measures for generating the fluid freedom of the material is carried out, i. For example, an annealing, and this only after the application of functional layers takes place, for example, during the annealing of a
  • the Li 2 O content is 7.0% by weight or less, preferably 5.2% by weight or less, and especially
  • the thin film battery of the invention can be prepared by a process comprising at least the
  • Fluid content in particular a H 2 0 content, of less than 2 wt .-%, preferably less than 0.5
  • Wt .-% and particularly preferably less than 0.2 wt .-% and most preferably less than 0.05 wt .-%, wherein the fluid content and within the chemical structure of the material bound fluid substances, for example in the form from
  • Boundary surface of at least one functional layer of the thin-film battery seals.
  • the substrate and / or at least one encapsulation of the thin-film battery is at least partially in the form of an inorganic, silicon-containing, in particular silicate, im
  • Substantially fluid-free material is formed.
  • the inorganic, silicon-containing, in particular silicate, substantially fluid-free material as a substrate in the form of a disc-shaped molding, wherein the substrate for generating the fluid freedom during or after the molding of a heat treatment, in particular a heat treatment at below 500 ° C, and / or flame treatment is subjected, wherein the Annealing preferably during the thermal treatment of at least one of
  • a getter material for fluids for example a getter material in the form of a metal, preferably a base metal, for example an alkali or
  • Alkaline earth metal and / or mixtures and alloys of metals is formed, or a getter material in the form of an adsorbent, applied to the substrate.
  • the getter is doing before the implementation of the
  • silicate essentially fluid-free materials.
  • Embodiment 1 A composition of an inorganic, silicon-containing, in particular silicate, essentially fluid-free material is furthermore given by way of example by the following composition in% by weight:
  • Embodiment 9 Yet another composition of an inorganic, silicon-containing, in particular silicate, im
  • Embodiment 13 Yet another composition of an inorganic, silicon-containing, in particular silicate, im
  • the glass may be contained at 0 to 1 wt .-%: P 2 0 5 , SrO, BaO; and a refining agent 0 to 1 wt .-% Sn0 2, Ce0 2 or As 2 C> 3 or other refining agents.
  • Substantially fluid-free material is still exemplified by the following composition in wt. -%:
  • Substantially fluid-free material is still exemplified by the following composition in
  • Embodiment 21 Yet another composition of an inorganic, silicon-containing, in particular silicate, im
  • Embodiment 23 Another composition of an inorganic,
  • R 2 O means the sum of the alkali ions present in the material and further preferably comprises Na 2 ⁇ 0, Li 2 ⁇ 0 and K 2 O.
  • R 2 O may be included if not already listed, optionally refining agents to 0 to 1 wt .-%, such as Sn0 2, Ce0 2, As 2 0 3, Cl ⁇ , F ⁇ , sulfates.
  • Bias in particular a chemical bias.
  • the chemical bias of a glass is obtained by an ion exchange in a transfer bath. If a toughened glass is used, this is prior to the application of functional layers of an electrical Storage system characterized in that it has a chemical bias, which is characterized by a thickness of the ion-exchanged layer L DO L of at least 10 ym, preferably at least 15 ym and on
  • Compressive stress at the surface (Oes) of the glass of preferably at least 100 MPa, preferably at least 200 MPa, more preferably at least 300 MPa and most preferably 480 MPa or more.
  • Functional layers of an electrical storage system may, depending on the process, result in a change in the state of stress of the glass used as the substrate. It has surprisingly been found that the bias of
  • Glass is not set to zero, but rather a residual stress is maintained in the glass, so that
  • Glass is increased compared to a conventional, non-tempered glass.
  • the present in the final energy storage glass as a substrate may be characterized in that it is present as at least partially chemically tempered glass, wherein the at least partially chemical
  • Preload is obtained by an ion exchange in a transfer bath and a subsequent thermal
  • L DO L thickness of the ion-exchanged layer
  • Oes surface of the glass
  • thermal load is greater than the compressive stress on the glass surface after thermal stress.
  • Pretension of the glass obtained in a barter in which lithium ions are contained Pretension of the glass obtained in a barter in which lithium ions are contained.
  • a swap bath containing various alkali ions, e.g. Potassium and low to lowest levels of lithium.
  • a step-shaped process e.g. Exchange with potassium and a quick further exchange with lithium-containing bath.
  • disc-shaped discrete element can be such that any existing other alkali metal oxides are proportionally reduced in the composition of the disc-shaped discrete element, so that the content of the other components relative to the alkali metal oxides remains the same, or else the Li 2 0 is added additively to the other components, so that their proportion is reduced accordingly.
  • L1 2 O is contained in a disk-shaped discrete element, is its content at least 0.1 wt .-%, and is still smaller than 7.0 wt .-%, preferably less than 5.2 wt .-%, more preferably less as 2.5 wt .-%, most preferably less than 0.5 wt .-%, and most preferably less than 0.2 wt .-%, particularly preferably ⁇ 0.1% by weight.
  • Fig. 1 is a schematic representation of a
  • FIG. 2 shows a schematic representation of a further thin film battery according to the invention
  • Fig. 3 is a schematic representation of a
  • silicon-containing, in particular silicate substantially fluid-free material.
  • FIG. 1 schematically shows a thin-film battery 1 according to the present invention. It comprises a substrate 2, which consists of an inorganic,
  • the two drainage layers 3 for the cathode and 4 for the anode are first applied to the substrate 2.
  • Such arrester layers are usually a few microns thick and consist of a metal, such as copper, platinum, aluminum or titanium.
  • the cathode is formed from a lithium transition metal compound, preferably an oxide, for example LiCoC> 2 , from LiMnO 2 or also from LiFePC.
  • the electrolyte 6 is applied, this electrolyte is in the case of the presence of a lithium-based thin-film battery is usually LiPON, a compound as lithium with oxygen,
  • the battery 1 comprises an anode 7, which may for example be lithium titanium oxide or even metallic lithium.
  • the anode layer 7 at least partially overlaps that with the electrolyte layer 6 and the arrester layer 4.
  • the battery 1 comprises an encapsulation layer 8.
  • At least the substrate 2 is in this case inorganic, silicon-containing, in particular silicate,
  • Substantially fluid-free material is formed, wherein as substantially fluid-free in the context of the present invention, a material is understood if it is less than 2 Wt .-%, preferably less than 0.5 wt .-% and especially less than 0.2 wt .-% fluids. Also the
  • Encapsulation layer 8 can be used as an inorganic, silicon-containing, in particular silicate,, im
  • Substantially fluid-free material may be formed.
  • Such encapsulation is characterized by the fact that
  • Fig. 2 is another embodiment of a
  • the structure of the thin-film battery 1 corresponds to
  • Encapsulation layer 8 is formed such that it encloses the entire layer structure of the thin-film battery 1.
  • a superstrate 9 is further arranged, which, for example, also from the inorganic, silicon-containing, in particular
  • substantially fluid-free material of the present invention may be formed. If the encapsulation layer 8 of an organic or
  • Fig. 3 shows the schematic illustration of the inorganic, silicon-containing, in particular silicate, im
  • a shaped body in the context of the present invention is then referred to as a disk-shaped or disk if its extent in a spatial direction is at most half as large as in the other two spatial directions.
  • a tape in the present invention is referred to as tape when the following relationship exists between its length, its width and its thickness: its length is at least ten times greater than its width and this in turn is at least twice as large as its thickness.

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  • Life Sciences & Earth Sciences (AREA)
  • Geochemistry & Mineralogy (AREA)
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  • Inorganic Chemistry (AREA)
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Abstract

L'invention concerne une batterie couche mince à durée de vie accrue et à faible teneur en fluide, sa teneur en fluide étant égale à 2000 ppm maximum, de préférence à 500 ppm maximum, de préférence encore à 200 ppm maximum et mieux encore à 50 ppm maximum. L'invention concerne également un matériau inorganique, contenant du silicium, en particulier silicaté, sensiblement exempt de fluide, ainsi qu'un procédé de fabrication d'une telle batterie couche mince.
PCT/EP2015/064069 2014-06-23 2015-06-23 Batterie couche mince à faible teneur en fluide et à durée de vie accrue WO2015197597A2 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
CN201580033610.4A CN106663748A (zh) 2014-06-23 2015-06-23 具有低流体含量和提高的使用寿命的薄膜电池
JP2016575011A JP2017521827A (ja) 2014-06-23 2015-06-23 流体含分が少なく、寿命が向上した薄膜バッテリー
US15/386,060 US20170104188A1 (en) 2014-06-23 2016-12-21 Thin film battery having low fluid content and an increased service life

Applications Claiming Priority (8)

Application Number Priority Date Filing Date Title
DE102014008934.7 2014-06-23
DE102014008934 2014-06-23
DE102014010735.3 2014-07-23
DE102014010735 2014-07-23
DE102015103863.3 2015-03-16
DE102015103857.9 2015-03-16
DE102015103863 2015-03-16
DE102015103857.9A DE102015103857A1 (de) 2014-12-01 2015-03-16 Miniaturisiertes elektronisches Bauelement mit verringerter Bruchgefahr sowie Verfahren zu dessen Herstellung

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US15/386,060 Continuation US20170104188A1 (en) 2014-06-23 2016-12-21 Thin film battery having low fluid content and an increased service life

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2018013854A1 (fr) * 2016-07-13 2018-01-18 Brian Berland Batterie à couches minces dotée d'une couche adhésive
WO2018181545A1 (fr) * 2017-03-29 2018-10-04 Tdk株式会社 Accumulateur lithium-ion totalement solide
US10418658B2 (en) 2014-12-01 2019-09-17 Schott Ag Electrical storage system comprising a disc-shaped discrete element, discrete element, method for the production thereof, and use thereof
WO2020104497A1 (fr) 2018-11-21 2020-05-28 Schott Ag Procédé et dispositif pour la fabrication de verre mince et bande de verre mince

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Publication number Priority date Publication date Assignee Title
US2247331A (en) * 1938-01-22 1941-06-24 Ferguson John Glassmaking batch
JP4245933B2 (ja) * 2003-02-13 2009-04-02 セイコーインスツル株式会社 リフローハンダ付け用非水電解質二次電池
JP2004269347A (ja) * 2003-02-18 2004-09-30 Nippon Electric Glass Co Ltd ガラス組成物
WO2005067645A2 (fr) * 2004-01-06 2005-07-28 Cymbet Corporation Structure barriere en couches possedant une ou plusieurs couches definissables et procede
US7553582B2 (en) * 2005-09-06 2009-06-30 Oak Ridge Micro-Energy, Inc. Getters for thin film battery hermetic package
JP5144845B2 (ja) * 2008-01-31 2013-02-13 株式会社オハラ 固体電池
US20110098171A1 (en) * 2008-03-03 2011-04-28 Saint-Gobain Glass France Method of producing glass
JP5515308B2 (ja) * 2009-02-03 2014-06-11 ソニー株式会社 薄膜固体リチウムイオン二次電池及びその製造方法
WO2010095736A1 (fr) * 2009-02-23 2010-08-26 日本電気硝子株式会社 Film de verre pour batterie lithium-ion
JP5504765B2 (ja) * 2009-09-02 2014-05-28 株式会社豊田中央研究所 全固体型リチウム二次電池
DE102010023176B4 (de) * 2010-06-09 2013-02-21 Schott Ag Verfahren zur Herstellung von Klarglas oder klarem Ziehglas unter Verwendung eines speziellen Läuterverfahrens

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US10418658B2 (en) 2014-12-01 2019-09-17 Schott Ag Electrical storage system comprising a disc-shaped discrete element, discrete element, method for the production thereof, and use thereof
WO2018013854A1 (fr) * 2016-07-13 2018-01-18 Brian Berland Batterie à couches minces dotée d'une couche adhésive
WO2018181545A1 (fr) * 2017-03-29 2018-10-04 Tdk株式会社 Accumulateur lithium-ion totalement solide
JPWO2018181545A1 (ja) * 2017-03-29 2020-05-14 Tdk株式会社 全固体リチウムイオン二次電池
JP7188380B2 (ja) 2017-03-29 2022-12-13 Tdk株式会社 全固体リチウムイオン二次電池
WO2020104497A1 (fr) 2018-11-21 2020-05-28 Schott Ag Procédé et dispositif pour la fabrication de verre mince et bande de verre mince

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