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WO2020126416A1 - Procédé de production d'une cellule électrochimique - Google Patents

Procédé de production d'une cellule électrochimique Download PDF

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Publication number
WO2020126416A1
WO2020126416A1 PCT/EP2019/083147 EP2019083147W WO2020126416A1 WO 2020126416 A1 WO2020126416 A1 WO 2020126416A1 EP 2019083147 W EP2019083147 W EP 2019083147W WO 2020126416 A1 WO2020126416 A1 WO 2020126416A1
Authority
WO
WIPO (PCT)
Prior art keywords
functional layer
ceramic functional
porous substrate
ceramic
substrate
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/EP2019/083147
Other languages
German (de)
English (en)
Inventor
Markus Siebert
Anja Griessl
Nicolas Maier
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Robert Bosch GmbH
Original Assignee
Robert Bosch GmbH
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Robert Bosch GmbH filed Critical Robert Bosch GmbH
Publication of WO2020126416A1 publication Critical patent/WO2020126416A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B18/00—Layered products essentially comprising ceramics, e.g. refractory products
    • 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
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • 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
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H01M4/8828—Coating with slurry or ink
    • H01M4/8835—Screen printing
    • 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
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H01M4/8846—Impregnation
    • 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
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H01M4/8857—Casting, e.g. tape casting, vacuum slip casting
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide 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
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • 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

  • an electrochemical cell in particular a fuel cell, which comprises at least one porous substrate and at least one ceramic functional layer, wherein in at least one method step the ceramic functional layer is applied as a green body on a transfer substrate before being applied to the porous substrate being beaten before.
  • the invention is based on a method for producing an electrochemical cell, in particular a fuel cell, which comprises at least one porous substrate and at least one ceramic functional layer, the ceramic functional layer being formed as a green body in at least one method step before being applied to the porous substrate a transfer substrate is brought up.
  • the porous substrate is pressed into the unsintered ceramic functional layer located on the transfer substrate.
  • An “electrochemical cell” is to be understood in particular to mean at least a part, in particular a subassembly, of a fuel cell and / or an electrolyser.
  • the electrochemical cell can also comprise the entire fuel cell or the entire electrolyzer.
  • the electrochemical cell at least as part of a high-temperature fuel cell, in particular a solid oxide fuel cell, SOFC for short, and / or as part of a high-temperature electrolyzer.
  • the electrochemical cell preferably comprises at least one ceramic functional layer of a fuel cell or an electrolyzer.
  • the ceramic functional layer can be embodied as a fuel electrode, as an air electrode, as an electrolyte, as a gas barrier, as a diffusion barrier, as a reaction barrier layer, as an electron blocker, as an oxidation protection or as a further ceramic functional layer which appears to be useful to the person skilled in the art.
  • the ceramic functional layer can be porous or gas-tight.
  • “ceramic” should be understood to mean a material that consists of at least 25% by volume, preferably at least 50% by volume, of a ceramic.
  • a ceramic material can also be embodied as a composite material comprising a ceramic, such as a cermet.
  • a “porous substrate” should preferably be understood to mean a porous base for the application of the ceramic functional layer. “Porous” should be understood in particular to be gas permeable.
  • a porous object may have pores, holes, recesses, channels, shafts or the like and / or be formed in a lattice-like, braid-like or sponge-like manner in order to enable gas conduction through and / or along the object.
  • the porous substrate has at least one application surface for the ceramic functional layer.
  • at least the application surface of the porous substrate is porous.
  • the porous substrate preferably comprises at least one carrier element for supporting the ceramic functional layer.
  • the carrier element is porous.
  • the Wennele element is designed as a metal carrier, in particular for the production of a metal-based fuel cell and / or a metal-based electrolyser.
  • the carrier element is made of a ceramic material.
  • the porous substrate to comprise further layers, in particular a further ceramic functional layer of a fuel cell and / or an electrolyser, which are applied in particular to the porous substrate on the carrier element before the ceramic functional layer is applied.
  • a surface of the Carrier element or the further ceramic functional layer the application surface for the ceramic functional layer.
  • a “transfer subordinate” is to be understood in particular as a temporary base for an object, which is still removed from the object during a manufacturing process.
  • the transfer substrate is provided for temporary support and / or transport of the ceramic functional layer prior to application to the porous substrate. “To see ahead” should be understood to mean, in particular, specially furnished, specially designed and / or specially equipped.
  • the fact that an object is provided for a specific function should in particular be understood to mean that the object fulfills and / or executes this specific function in at least one application and / or operating state.
  • the transfer substrate is designed as paper with a water-soluble coating or as a polymer film, for example as siliconized or unsiliconized polyester.
  • the ceramic functional layer is applied to the transfer substrate in at least one process step.
  • the ceramic functional layer with the transfer substrate is preferably arranged on the porous substrate.
  • the ceramic functional layer is preferably fixed to the porous substrate, in particular in a state of the ceramic functional layer arranged on the transfer substrate.
  • the transfer substrate is preferably detached from the ceramic functional layer in at least one method step, in particular after the ceramic functional layer has been fixed to the porous substrate.
  • the ceramic functional layer is preferably applied to the transfer substrate in a pasty state.
  • a green body of the ceramic functional layer is preferably produced on the transfer substrate in at least one method step.
  • the green compact comprises at least one ceramic powder, for example based on yttrium-stabilized zirconium dioxide (YSZ), gadolinium-doped cerium dioxide (CGO), with a perovskite structure such as lanthanum-strontium-cobalt-ferrite (LSCF) or another which is useful to the person skilled in the art appearing ceramic material for the production of the ceramic functional layer.
  • YSZ yttrium-stabilized zirconium dioxide
  • CGO gadolinium-doped cerium dioxide
  • LSCF lanthanum-strontium-cobalt-ferrite
  • the green compact especially additional lent, a metal powder or a metal oxide powder such as nickel or nickel oxide.
  • the green compact preferably comprises a binder, a solvent and / or further additives.
  • the ceramic powder is processed with the metal powder, the metal oxide powder, the binder, the solvent and / or the further additives into a paste.
  • the paste is preferably applied to the transfer substrate to form the green body in a screen printing process, a stencil printing process, a slip casting process, a film drawing process or the like. The paste is preferably applied as a thin layer to the transfer substrate.
  • a “thin layer” is understood to mean, in particular, a layer with a layer thickness that extends in particular in a direction perpendicular to a surface of the transfer substrate of less than 200 pm, preferably less than 100 pm, particularly preferably less than 50 pm become.
  • the layer thickness of a thin layer, which extends in particular in a direction perpendicular to the upper surface of the transfer substrate is greater than 1 pm, preferably greater than 5 pm.
  • the porous substrate is preferably pressed into the unsintered ceramic functional layer.
  • the ceramic functional layer with the transfer substrate is preferably arranged on a flat surface, the ceramic functional layer facing away from the flat surface.
  • the porous substrate is preferably arranged on the ceramic functional layer, in particular the application surface of the porous substrate facing the ceramic functional layer.
  • a pressure is preferably applied to the ceramic functional layer and / or the porous substrate in order to press the porous substrate into the ceramic functional layer and / or to press the ceramic functional layer into the porous substrate.
  • the porous substrate is preferably moved in the direction of the ceramic functional layer during the pressing process. Alternatively or additionally, the ceramic functional layer is moved on the transfer substrate in the direction of the porous substrate.
  • a depth of penetration of the porous substrate into the ceramic functional layer is preferably controlled or regulated during the pressing process.
  • the porous substrate preferably remains from the trans- spaced apart.
  • a temperature is preferably applied to the ceramic functional layer and / or the porous substrate during a pressing process.
  • the ceramic functional layer is preferably connected as green to the porous substrate.
  • the green compact with the porous substrate is bonded to the porous substrate in a moist, semi-dry or dry state.
  • a “moist state” is to be understood in particular to mean that the solvent in the green compact still comprises at least 85%, preferably at least 90%, particularly preferably at least 95% of its original added mass.
  • a “dry state” should be understood in particular to mean that the solvent has been expelled from the green body.
  • a “semi-dry state” is to be understood in particular to mean that at least 10%, preferably at least 15%, particularly preferably at least 20% of the original mass of the solvent has been expelled from the green compact.
  • a green compact in a semi-dry state still comprises at least 10%, preferably at least 20%, particularly preferably at least 30% of the original mass of the solvent.
  • a porous surface of the porous substrate can advantageously be laminated reliably with a continuous layer made of a ceramic material.
  • sagging of the ceramic material into a cavity of the porous substrate can advantageously be avoided.
  • an advantageously flat ceramic functional layer can be provided on a porous substrate.
  • the ceramic functional layer can compensate for a porosity and / or unevenness of the porous substrate with advantageously little material.
  • the green part of the ceramic functional layer is at least substantially completely dried in a state connected to the porous substrate.
  • “Essentially completely dried” is to be understood in particular to mean that more than 80%, preferably more than 90%, particularly preferably more than 95% of the solvent has been driven off.
  • the green compact is preferably subjected to a temperature of at least 25 ° C., preferably at least 50 ° C.
  • the green compact with a temperature of less than 200 ° C, preferably applied at less than 100 ° C.
  • the green compact is preferably dried before the transfer substrate is removed.
  • the green body is preferably dried in a moist or semi-dry state.
  • drying takes place after the porous substrate has been pressed into the ceramic functional layer or after the ceramic functional layer has been pressed into the porous substrate.
  • the ceramic functional layer is fixed to the porous substrate by drying, in particular in a form-fitting and / or integral manner with the porous substrate.
  • the inventive configuration allows the ceramic functional layer to be connected to the porous substrate with advantageously little pressure and / or at an advantageously low temperature.
  • an advantageously tight fit of the ceramic functional layer to the outer and / or inner contours of the porous substrate can be achieved during pressing of the porous substrate into the not yet dried ceramic functional layer or during pressing of the not yet dried ceramic functional layer into the porous substrate .
  • an advantageously stable connection of the ceramic functional layer to the porous substrate can be achieved.
  • the green of the ceramic functional layer is at least partially predried in at least one process step before it is applied to the porous substrate.
  • the green compact is placed in a semi-dry or at least substantially completely dry state before being applied to the porous substrate. Drying is preferably carried out for predrying the green compact, in particular using a lower temperature and / or time period than for at least substantially complete drying.
  • a strength and plastic deformability of the green compact of the ceramic functional layer can advantageously be set by the design according to the invention.
  • the porous substrate can be pressed in under advantageously controlled conditions. In particular, an undesired, for example lateral, deformation of the ceramic functional layer can advantageously be avoided.
  • the green of the ceramic functional layer is at most partially pre-dried before being applied to the porous substrate.
  • the green compact of the ceramic functional layer is pressed into the porous substrate in a moist state or a semi-dry state.
  • the porous substrate is pressed into the green compact of the ceramic functional layer in a moist state or a semi-dry state of the green compact.
  • the ceramic functional layer be applied to a smooth application surface of the transfer substrate in at least one method step.
  • “Smooth” is to be understood in particular to mean that an average roughness depth (R z ) is less than 10 pm, preferably is less than 5 pm, particularly preferably is less than 3 pm and / or that an average roughness value (R a ) is less than 3 pm, preferably less than 2 pm, especially before is less than 1 pm.
  • the smooth application surface of the transfer substrate is provided so that a surface of the ceramic functional layer, which is applied to the transfer substrate, is formed smoothly.
  • the smooth surface of the ceramic functional layer is arranged facing away from the porous substrate when the ceramic functional layer is connected to the porous substrate.
  • the transfer substrate is removed from the smooth surface after the ceramic functional layer has dried.
  • the smooth surface of the ceramic functional layer is provided for the application of at least one additional ceramic functional layer.
  • the additional ceramic functional layer with an ink or paste-based method, for example by means of stencil printing, by means of ink jet printing, by means of dip coating, by means of liquid spraying or the like, by lamination of cast or extruded foils, by gas phase processes such as physical or chemical vapor deposition (PVD, CVD) or atomic layer separation (ALD) or another method that appears to the person skilled in the art to be applied to the smooth surface.
  • PVD physical or chemical vapor deposition
  • CVD atomic layer separation
  • ALD atomic layer separation
  • the additional ceramic functional layer is analogous to the ceramic one Functional layer is applied to the ceramic functional layer with a transfer printing substrate. It is also conceivable that the additional ceramic functional layer is applied to the transfer substrate before the ceramic functional layer. In particular, the ceramic functional layer is applied to the additional ceramic functional layer on the transfer substrate. In particular, it is conceivable that in at least one process step at least the two ceramic functional layers located on the transfer substrate are applied to the porous substrate in a single process step. Due to the configuration according to the invention, a surface of the ceramic functional layer can advantageously be made smooth. In particular, a smooth surface can be provided for building up additional ceramic functional layers, in particular despite a high porosity and / or high roughness of the porous substrate. In particular, additional ceramic functional layers that are applied to the ceramic functional layer can advantageously be applied thinly. In particular, perforation of an additional ceramic functional layer due to structural elements of a non-smooth surface of the ceramic functional layer can be avoided.
  • the porous substrate be coated with a protective layer in at least one process step before the ceramic functional layer is applied.
  • the carrier element is coated with a protective layer.
  • the protective layer is designed as a diffusion barrier and is provided to prevent interdiffusion between the carrier element and the ceramic functional layer. It is also conceivable that the protective layer is provided to prevent oxidation of the carrier element.
  • the protective layer is designed as a further ceramic functional layer. A protective layer designed as a further ceramic functional layer is preferably applied to the carrier element in an analogous manner to the ceramic functional layer.
  • the protective layer is applied to the carrier element by means of a dip coating, a sol-gel process, a gas phase process such as physical gas phase deposition (PVD) or atomic layer deposition (ALD) and / or another process which appears to be useful to the person skilled in the art. Due to the configuration according to the invention, an advantageously reliable Protection of the porous substrate can be achieved, in particular despite the close interlocking of the porous substrate with the ceramic functional layer.
  • PVD physical gas phase deposition
  • ALD atomic layer deposition
  • a highly porous substrate be used in at least one process step.
  • a “highly porous” object is to be understood in particular to mean an object made of a material that has less than 50%, preferably less than 35%, particularly preferably less than 20% of a maximum theoretical density of the material, in particular under the same temperature and pressure conditions. Due to the design according to the invention, an advantageously high gas permeability of the porous substrate can be achieved. In particular, an advantageously large gas distribution can be achieved within the porous substrate. In particular, a pressure drop due to the porous substrate for conveying the gas can advantageously be kept low.
  • the ceramic functional layer and the porous substrate be connected to one another at a pressure of less than 100 MPa in at least one process step.
  • a pressure of less than 50 MPa, particularly preferably less than 25 MPa, is preferably used to bond the ceramic functional layer, in particular in a dry state, and the porous substrate to one another.
  • a pressure of less than 10 MPa, particularly preferably less than 5 MPa is used in order to connect the ceramic functional layer, in particular in a semi-dry or moist state, to the porous substrate.
  • An undesired deformation of the ceramic functional layer can advantageously be avoided by the configuration according to the invention.
  • a penetration depth of the porous substrate into the ceramic functional layer can advantageously be set, in particular depending on a strength and / or a plastic flowability of the ceramic functional layer and / or depending on a porosity and / or pore size of the porous substrate.
  • the ceramic functional layer and the porous substrate be bonded to one another at a temperature of below 200 ° C. in at least one process step.
  • the ceramic functional layer with a temperature of at least 25 ° C., preferably at least 50 ° C.
  • the green compact is subjected to a temperature of less than 200 ° C., preferably less than 100 ° C.
  • the temperature is applied during and / or after the pressure is applied.
  • the green compact is dried after the ceramic functional layer has been pressurized with the porous substrate.
  • the green compact is dried with the porous substrate during the pressurization of the ceramic functional layer.
  • the application of temperature to the ceramic functional layer and / or the porous substrate is carried out for drying for less than 10 min, preferably for less than 5 min, particularly preferably for less than 3 min. It is conceivable that a temperature is applied to the ceramic functional layer and / or the porous substrate during the application of pressure.
  • a temperature admission during a pressurization is less than 200 C, preferably less than 100 C.
  • the temperature admission during the pressurization is greater than 25 ° C, preferably greater than 50 ° C.
  • the temperature application during the pressurization is carried out for more than 1 s, preferably for more than 3 s.
  • a temperature application is carried out during the pressurization for less than 5 minutes, preferably for less than 3 minutes.
  • the temperature for drying is preferably greater than the temperature application during the application of pressure.
  • At least one additional ceramic functional layer of the electrochemical cell which is designed as an electrolyte, is applied to the ceramic functional layer with a layer thickness of less than 15 mhh.
  • the additional functional layer formed as an electrolyte is applied to the smooth surface of the ceramic functional layer.
  • at least one additional ceramic functional layer is applied between the additional ceramic functional layer and the ceramic functional layer.
  • the additional ceramic functional layer designed as an electrolyte is applied analogously to the ceramic functional layer by means of a transfer substrate.
  • the additional ceramic functional layer designed as an electrolyte is preferably applied to the ceramic functional layer using one of the abovementioned methods.
  • the additional ceramic functional layer formed as an electrolyte is applied by means of screen printing, in particular with a layer thickness of less than 15 pm.
  • the additional ceramic functional layer formed as an electrolyte is applied by means of physical gas deposition, in particular with a layer thickness of less than 5 pm.
  • the carrier element is designed as a porous metal carrier.
  • the carrier element preferably consists of a chromium-rich ferritic stainless steel.
  • the carrier element is designed as a metal foam, as a wire mesh, as an expanded metal, as a perforated plate or as a porous sintered powder layer.
  • the ceramic functional layer is preferably designed as a diffusion barrier or as a fuel electrode.
  • the ceramic functional layer is designed as an air electrode.
  • the ceramic functional layer in a arranged on the porous substrate stood on a smooth surface, which in particular faces away from the porous substrate.
  • the electrochemical cell has additional ceramic functional layers, which in particular have layers of are built on the smooth surface.
  • the electrochemical cell preferably comprises at least the layer sequence of carrier element, diffusion barrier or the layer sequence of carrier element, fuel electrode.
  • an electrochemical cell according to the invention in particular a fuel cell, the layer sequence carrier element, diffusion barrier, fuel electrode, electrolyte, reaction barrier layer, air electrode.
  • an electrochemical cell according to the invention in particular a fuel cell, comprises the layer sequence of carrier element, fuel electrode, electrolyte, reaction barrier layer, air electrode.
  • an electrochemical cell according to the invention in particular a fuel cell, comprises the layer sequence of carrier element, air electrode, reaction barrier layer, electrolyte, fuel electrode or another layer sequence which appears to be useful to the person skilled in the art.
  • at least one of the layers mentioned is composed of a plurality of partial layers, which in particular comprise different materials.
  • the configuration according to the invention makes it possible to provide an electrochemical cell, in particular a fuel cell, with a porous substrate with an advantageously high porosity.
  • an electrochemical cell with advantageously thin ceramic functional layers, in particular with an advantageously thin, advantageously hole-free, advantageously uniformly thick electrolyte can be provided.
  • the method according to the invention and / or the electrochemical cell according to the invention should / should not be limited to the application and embodiment described above.
  • the method according to the invention and / or the electrochemical cell according to the invention can have a number that differs from a number of individual elements, components and units as well as method steps mentioned in order to fulfill a function described here.
  • values lying within the stated limits are also to be considered disclosed and can be used as desired.
  • Fig. 1 is a schematic representation of a method according to the invention.
  • Fig. 2 is a schematic representation of an extension of the inventive method.
  • FIG. 1 shows a method 10 for producing an electrochemical cell 12, in particular for producing a fuel cell.
  • the electrochemical cell 12 has at least one porous substrate 14.
  • the electrochemical cell 12 has at least one ceramic functional layer 16.
  • the ceramic functional layer 16 is applied as a green body on a transfer substrate 18 before being applied to the porous substrate 14.
  • the porous substrate 14 is pressed into the unsintered ceramic functional layer 16 located on the transfer substrate 18.
  • the transfer substrate 18 is detached from the ceramic functional layer 16 in a detachment step 32.
  • the ceramic functional layer 16 is applied to a smooth application surface 20 of the transfer substrate 18.
  • the ceramic functional layer 16 is provided as a diffusion barrier between the porous substrate 14 and an, in particular nickel-containing, fuel electrode.
  • a paste is preferably produced for applying the ceramic functional layer 16 to the transfer substrate 18.
  • the paste preferably comprises a ceramic powder.
  • the key Ceramic powder designed as gadolinium-doped cerium dioxide.
  • the ceramic powder is preferably mixed with a, in particular organic, binder.
  • the binder is preferably designed as polyvinyl butyral. Alternatively, ethyl or methyl cellulose, acrylate, polyvinyl acetate and / or another soluble polymer is used as the binder.
  • the ceramic powder is preferably mixed with a solvent, in particular with diethylene glycol monobutyl ether.
  • a solvent in particular with diethylene glycol monobutyl ether.
  • water, an alcohol, a carboxylic acid ester, a ketone or the like is used as the solvent.
  • the ceramic powder is mixed with further additives, for example in order to lower a necessary sintering temperature.
  • the paste is applied to the transfer substrate 18 using a screen or stencil printing method, in particular to the smooth application surface 20 of the transfer substrate 18.
  • the paste is applied to the transfer substrate 18 with a flat doctor blade, dispensing, film casting or the like.
  • the paste it is conceivable for the paste to be densified after it has been applied to the transfer substrate 18, in particular in order to maximize a contact area between the paste and the smooth application area 20.
  • the transfer substrate 18 is formed as a siliconized or silicone-free polyester film.
  • the green compact of the ceramic functional layer 16 is at least partially predried before being applied to the porous substrate 14.
  • the green of the ceramic functional layer 16 is at most partially pre-dried before being applied to the porous substrate 14.
  • at least 10% of the solvent is expelled in preparation step 28, for example by storage in a convection oven.
  • the ceramic functional layer 16 is applied to the porous substrate 14 in a moist or at least substantially dry state.
  • the porous substrate 14 comprises a metal element or mesh as a carrier element, of which only two layers with strands running transversely to one another are shown for the sake of clarity.
  • the carrier element is made of Crofer22 or another chromium-rich ferritic stainless steel, for example from one of the alloys 1.4016, 1.4521, 1.4509 or another which is useful to the person skilled in the art appearing metal to support the electrochemical cell 12, in particular a solid oxide fuel cell.
  • the porous substrate 14 is preferably coated with a protective layer 22 before the ceramic functional layer 16 is applied.
  • the porous substrate 14 is coated with a corrosion protection layer.
  • the protective layer 22 is applied to the porous substrate 14 using a gas phase process.
  • transfer substrate 18 is preferably arranged on a flat surface with a surface facing away from ceramic functional layer 16.
  • the porous substrate 14 is preferably placed on the ceramic functional layer 16.
  • the porous substrate 14 is preferably subjected to a pressure, for example with the aid of a hydraulic press, for example, or by applying a weight.
  • the ceramic functional layer 16 and the porous substrate 14 are connected to one another at a pressure of less than 100 MPa, in particular less than 25 MPa.
  • the pressure is preferably less than 10 MPa, particularly preferably less than 5 MPa.
  • the porous substrate 14 is partially pressed into the ceramic functional layer 16 by the pressure.
  • a part of the ceramic functional layer 16 is preferably pressed into hollow spaces of the porous substrate 14.
  • a depth of penetration of the porous substrate 14 into the ceramic functional layer 16 is preferably controlled by means of the pressure and / or by means of a strength and / or a plastic deformability of the ceramic functional layer 16. It is conceivable that the ceramic functional layer 16 is additionally subjected to a temperature, in particular 70 ° C., during an application of the pressure, in particular in order to soften the binder and to increase the plastic deformability.
  • the porous substrate 14 preferably remains spaced from the transfer substrate 18. It is conceivable that temporary spacers are used in order to limit a depth of penetration of the porous substrate 14 into the ceramic functional layer 16.
  • the green compact of the ceramic functional layer 16 is in one with the porous substrate 14 connected state at least substantially completely dig.
  • the ceramic functional layer 16 is thermally treated in a state connected to the porous substrate 14, optionally while maintaining the application of the pressure.
  • the ceramic functional layer 16 and the porous substrate 14 are connected to one another at a temperature of below 200 ° C., in particular below 100 ° C., before being given a temperature of 80 ° C.
  • the ceramic functional layer 16 is fixed to the porous substrate 14 by drying the ceramic functional layer 16 on the porous substrate 14.
  • the transfer substrate 18 is detached from the ceramic functional layer 16.
  • the ceramic functional layer 16 remains fixed on the porous substrate 14.
  • the ceramic functional layer 16 has a smooth surface 34 facing away from the porous substrate 14.
  • the electrochemical cell 12 is sintered after the detachment step 32, in particular at a temperature of more than 800 ° C.
  • FIG. 2 shows a method 10 'as an extension of the method 10.
  • the method 10' follows the detachment step 32 of the method 10.
  • additional ceramic functional layers 26, 36 are built up on the electrochemical cell 12 from the method 10.
  • an electrode application step 38 an additional ceramic functional layer 36 designed as an electrode is applied to the ceramic functional layer 16.
  • a fuel electrode is preferably applied.
  • an air electrode is applied.
  • the additional ceramic functional layer 36 designed as an electrode is applied to the smooth surface 34 of the ceramic functional layer 16.
  • the additional ceramic functional layer 36 formed as an electrode is formed by means of an ink or paste-based method, for example by means of stencil printing, by means of ink jet printing, by means of dip coating, by means of liquid spraying or the like, by lamination cast or extruded foils, by gas phase processes such as physical or chemical Gas phase deposition (PVD, CVD) or atomic layer deposition (ALD) or another method that appears useful to the person skilled in the art is applied to the smooth surface 34.
  • PVD, CVD physical or chemical Gas phase deposition
  • ALD atomic layer deposition
  • an electrolyte application step 40 at least one additional ceramic functional layer 26 of the electrochemical cell 12 designed as an electrolyte 24 is applied to the ceramic functional layer 16 with a layer thickness of less than 15 mhh.
  • the electrolyte 24 is applied to the additional functional layer 36 designed as an electrode.
  • the ceramic functional layer 16 forms a smooth surface for the application of the electrolyte 24.
  • the electrolyte 24 is preferably applied using one of the methods mentioned in the previous section. It is conceivable that in method 10 'further additional functional layers, in particular one
  • Reaction barrier layer an air electrode or the like, are applied to the electrochemical cell 12, in particular for the production of a metal-supported solid oxide fuel cell.

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Abstract

L'invention concerne un procédé de production d'une cellule électrochimique, en particulier d'une pile à combustible, qui comprend au moins un substrat poreux (14) et au moins une couche fonctionnelle céramique (16), la couche fonctionnelle céramique (16) étant appliquée, dans au moins une étape de procédé, sur un substrat de transfert (18) en tant que corps vert avant d'être appliquée sur le substrat poreux (14). Selon l'invention, dans au moins une étape de procédé, le substrat poreux (14) est pressé dans la couche fonctionnelle céramique (16) non frittée se trouvant sur le substrat de transfert (18).
PCT/EP2019/083147 2018-12-20 2019-11-29 Procédé de production d'une cellule électrochimique Ceased WO2020126416A1 (fr)

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DE102023211935A1 (de) 2023-11-29 2025-06-05 Robert Bosch Gesellschaft mit beschränkter Haftung Verfahren zur Herstellung einer elektrochemischen Zelle, elektrochemische Zelle, Elektrolysezellenvorrichtung und Brennstoffzellenvorrichtung

Citations (5)

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DE10238938A1 (de) * 2002-08-24 2004-03-04 Robert Bosch Gmbh Keramisches Schichtsystem
KR20130075266A (ko) * 2011-12-27 2013-07-05 한국세라믹기술원 고체산화물 연료전지의 제조방법 및 이에 의해 제조되는 고체 산화물 연료전지
DE112012003921T5 (de) * 2011-09-21 2014-07-03 Korea Electric Power Corp. Verfahren zur Herstellung einer Trägertyp-Überzugsmembran unter Anwendung des Foliengießverfahrens
DE102015217944A1 (de) * 2015-09-18 2017-03-23 Robert Bosch Gmbh Elektrochemische Zelle sowie Verfahren zur Herstellung einer elektrochemischen Zelle
DE102016225970A1 (de) * 2016-12-22 2018-06-28 Robert Bosch Gmbh Verfahren zur Herstellung einer Brennstoff- und/oder Elektrolysezelle sowie eine Brennstoff- und/oder Elektrolysezelle

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Publication number Priority date Publication date Assignee Title
US10115973B2 (en) * 2015-10-28 2018-10-30 Lg Fuel Cell Systems Inc. Composition of a nickelate composite cathode for a fuel cell

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10238938A1 (de) * 2002-08-24 2004-03-04 Robert Bosch Gmbh Keramisches Schichtsystem
DE112012003921T5 (de) * 2011-09-21 2014-07-03 Korea Electric Power Corp. Verfahren zur Herstellung einer Trägertyp-Überzugsmembran unter Anwendung des Foliengießverfahrens
KR20130075266A (ko) * 2011-12-27 2013-07-05 한국세라믹기술원 고체산화물 연료전지의 제조방법 및 이에 의해 제조되는 고체 산화물 연료전지
DE102015217944A1 (de) * 2015-09-18 2017-03-23 Robert Bosch Gmbh Elektrochemische Zelle sowie Verfahren zur Herstellung einer elektrochemischen Zelle
DE102016225970A1 (de) * 2016-12-22 2018-06-28 Robert Bosch Gmbh Verfahren zur Herstellung einer Brennstoff- und/oder Elektrolysezelle sowie eine Brennstoff- und/oder Elektrolysezelle

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