US20150218713A1 - Component Constituting an HTE Electrolyser Interconnector or SOFC Fuel Cell Interconnector and Associated Production Processes - Google Patents
Component Constituting an HTE Electrolyser Interconnector or SOFC Fuel Cell Interconnector and Associated Production Processes Download PDFInfo
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- US20150218713A1 US20150218713A1 US14/429,610 US201314429610A US2015218713A1 US 20150218713 A1 US20150218713 A1 US 20150218713A1 US 201314429610 A US201314429610 A US 201314429610A US 2015218713 A1 US2015218713 A1 US 2015218713A1
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B1/00—Electrolytic production of inorganic compounds or non-metals
- C25B1/01—Products
- C25B1/02—Hydrogen or oxygen
- C25B1/04—Hydrogen or oxygen by electrolysis of water
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
- C25B11/036—Bipolar electrodes
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- C25B9/18—
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/60—Constructional parts of cells
- C25B9/65—Means for supplying current; Electrode connections; Electric inter-cell connections
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
- C25B9/70—Assemblies comprising two or more cells
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- H01M2/202—
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- 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
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0206—Metals or alloys
- H01M8/0208—Alloys
- H01M8/021—Alloys based on iron
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- 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
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0215—Glass; Ceramic materials
- H01M8/0217—Complex oxides, optionally doped, of the type AMO3, A being an alkaline earth metal or rare earth metal and M being a metal, e.g. perovskites
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- 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
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0223—Composites
- H01M8/0228—Composites in the form of layered or coated products
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- 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
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
- H01M8/026—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant characterised by grooves, e.g. their pitch or depth
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- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04201—Reactant storage and supply, e.g. means for feeding, pipes
- H01M8/04216—Reactant storage and supply, e.g. means for feeding, pipes characterised by the choice for a specific material, e.g. carbon, hydride, absorbent
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- 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
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- 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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
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- 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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
- H01M8/2425—High-temperature cells with solid electrolytes
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- 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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
- H01M8/2425—High-temperature cells with solid electrolytes
- H01M8/2432—Grouping of unit cells of planar configuration
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- 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
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- 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
- H01M50/50—Current conducting connections for cells or batteries
- H01M50/502—Interconnectors for connecting terminals of adjacent batteries; Interconnectors for connecting cells outside a battery casing
- H01M50/521—Interconnectors for connecting terminals of adjacent batteries; Interconnectors for connecting cells outside a battery casing characterised by the material
- H01M50/522—Inorganic material
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- 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
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- 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
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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- 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 present invention relates to the field of solid oxide fuel cells (SOFC) and to that of high-temperature electrolysis (HTE) or high-temperature steam electrolysis (HTSE).
- SOFC solid oxide fuel cells
- HTE high-temperature electrolysis
- HTSE high-temperature steam electrolysis
- the present invention relates to components made of metal alloy constituting interconnection devices that are subjected to high temperatures and, on the one hand, to a reductive atmosphere that is either rich in steam H 2 O/H 2 (wet hydrogen or hydrogen rich in steam) in the HTE reactors or rich in H 2 in the SOFC cells, and, on the other hand, to an oxidizing atmosphere that is either rich in O 2 in the HTE reactors, or rich in air in the SOFC cells, one of the functions of which is to ensure the passage of the electrical current in the HTE reactors.
- H 2 O/H 2 wet hydrogen or hydrogen rich in steam
- interconnectors also known as interconnectors or interconnection plates
- interconnectors are devices that connect in series each electrochemical cell (electrolysis cell) in the stack of HTE reactors and cells, thus combining the production of each.
- the interconnectors thus ensure the functions of conveying and collecting current and delimit the circulation compartments (distribution and/or collection) of the gases.
- the interconnectors must be able to withstand corrosion in atmospheres that may be very oxidizing in very high temperature ranges, typically between 600 and 900° C., such as atmospheres rich in steam H 2 O/H 2 on the cathode side of HTE electrolyzers, which corrosion may be harmful to the durability of these electrolyzers.
- the interconnectors must have in these atmospheres a thermomechanical behavior close to that of electrochemical cells so as to conserve good leaktightness between compartments with cathodes, known as the cathode compartments, and compartments with anodes, known as the anode compartments.
- the present invention is more particularly directed toward simplifying the production of interconnectors, of interdigital or channel plate type, and of reducing the manufacturing cost thereof, so as to reduce the manufacturing cost of an HTE electrolyzer or of an SOCF fuel cell equipped therewith.
- the invention is also directed toward improving the electrical contact between an interconnector and an electrochemical cell against which it bears.
- An SOFC fuel cell or an HTE electrolyzer consists of a stack of elementary units each comprising a solid oxide electrochemical cell, consisting of three anode/electrolytic/cathode layers superposed one on the other and of interconnection plates made of metal alloys also known as bipolar plates, or interconnectors.
- the function of the interconnectors is to ensure both the passage of the electrical current and the circulation of the gases in the region of each cell (steam injected, hydrogen and oxygen extracted in an HTE electrolyzer; air and hydrogen injected and water extracted in an SOFC cell) and of separating the anode and cathode compartments which are the compartments for circulation of the gases on the anode and cathode side, respectively, of the cells.
- H 2 O steam is injected into the cathode compartment.
- this dissociation produces dihydrogen gas H 2 and oxygen ions.
- the dihydrogen is collected and evacuated at the outlet of the hydrogen compartment.
- the oxygen ions O 2 ⁇ migrate toward the electrolyte and recombine as dioxygen at the interface between the electrolyte and the oxygen electrode (anode).
- air oxygen
- hydrogen is injected into the cathode compartment and hydrogen is injected into the anode compartment.
- the hydrogen H 2 becomes converted into H + ions and releases electrons that are captured by the anode.
- the H + ions arrive at the cathode, where they combine with the O 2 ⁇ ions constituted from the oxygen of the air, to form water.
- the transfer of the H + ions and of the electrons to the cathode produces a continuous electrical current from the hydrogen.
- Chromia-forming ferritic stainless steels are among the interconnector alloys that are the most promising for HTE electrolyzers, given that they have already been successfully used as alloys in SOFC high-temperature fuel cells [1-3].
- these interconnector alloys those already commercialized under the names Crofer 22 APU and Crofer 22 H based on Fe-22%Cr, by the company ThyssenKrupp VDM, or the product having the name Sanergy HT based on Fe-22%Cr, by the company Sandvik, or alternatively the product under the name K41X by the company APERAM for operating temperatures of between 600 and 900° C.
- Alloys of this type may have a coefficient of thermal expansion in the region of that of cell materials and relatively good corrosion resistance when compared with other metal materials. Nevertheless, it requires a certain number of coatings intended, firstly, to protect it against oxidation and to prevent the evaporation of the Cr under the operating conditions, which, on the oxidizing side, pollute the electrode with air and considerably degrade its function, and, secondly, a coating that makes it possible to minimize the electrical resistance between the interconnector and the cell.
- the literature thus describes coatings, on the one hand, for SOFC cell interconnectors, and, on the other hand, for the face of the interconnectors facing the oxygen electrode [6]. These coatings have the sole function of limiting the evaporation of chromium, of ensuring electron conduction and good resistance to oxidation of the alloy in air, i.e. in the atmosphere in cathode compartments of SOCF cells.
- FIGS. 1 , 1 A and 1 B show a channel plate 1 commonly used both in HTE electrolyzers and in SOFC fuel cells.
- the conveyance or collection of the current at the electrode is performed by the teeth or ribs 10 which are in direct mechanical contact with the electrode concerned.
- the introduction of steam at the cathode or of draining gas at the anode in an HTE electrolyzer, the introduction of air (O 2 ) at the cathode or of hydrogen at the anode in an SOCF cell is symbolized by the arrows in FIG. 1 .
- the collection of the hydrogen produced at the cathode or of the oxygen produced at the anode in an HTE electrolyzer, the collection of the water produced at the cathode or of the excess hydrogen at the anode in an SOCF cell is performed by the channels 11 which emerge in a fluidic connection, commonly known as a manifold, which is common to the stack of cells.
- a fluidic connection commonly known as a manifold
- Another interconnecting plate 1 has already been proposed [7]. It is represented in FIG. 2 with the circulation of the fluid represented by the arrows: its structure is of interdigital type.
- this channel plate or plate of interdigital structure require a large thickness of material, typically from 5 to 10 mm, for the zone of collection of the gases produced and forming by machining in the bulk, of the gas distribution channels.
- a photographic representation of such a machined plate is given in FIG. 3 .
- the material and machining costs are high and directly linked to the fineness of pitch of the channels to be machined: more particularly inter-channel distances of less than 1 mm.
- the use of thin sheet metals, typically from 0.5 to 2 mm, drawn and then assembled together by laser welding has already been tested.
- a photographic representation of such a plate obtained by assembling drawn sheet metals is given in FIG. 4 .
- This technique has the advantage of limiting the cost of starting material, but does not make it possible to achieve a channel fineness as high as that by machining Specifically, the possibilities of production for the depth of the channels, the unit tooth width and the pitch between teeth are limited. Furthermore, the cost of the drawing tooling necessitates large-scale production.
- Patent U.S. Pat. No. 6,106,967 thus proposes a flat, thin (1-10 mm) interconnector made of metal (superalloy) and an electrochemical cell with electrodes bearing internal channels ensuring the distribution of the fluids.
- this solution has the advantage of allowing good distribution of the fluids, it does not at all improve the quality of the electrical contact between the metal and the electrodes. Furthermore, such cells are complex and consequently expensive to produce.
- Patent application US 2004/0 200 187 proposes to place between the electrodes and the flat metal separator (superalloy), a corrugated preformed structure made of metal (alloy based on chromium or alloy based on noble metals). This structure ensures the electrical contact between the electrodes and the separator.
- This solution has the drawback of being applied to the cathode compartment (SOCF) and thus of subjecting the corrugated preformed structure to substantial oxidation.
- Patent application WO 2010/085 248 proposes the addition of a porous metal layer welded to the machined interconnector.
- This layer is preferentially a nickel plate, which is placed on either side of the cell, i.e. in contact with the anode and the cathode.
- this plate becomes deformed on increasing in temperature via the bimetal effect. The consequence of this bimetal effect is either the loss of the electrical contact or the degradation of the cell.
- SOCF cathode compartment
- Patent application US 2002/0 048 700 proposes the use of a metal grate which may be placed between the electrodes and the flat interconnector.
- the purpose of this grate is to improve the distribution of the gases toward the electrodes. It is also placed on either side of the cell, i.e. in the oxidizing (cathode) and reducing (anode) compartments.
- the metals preferentially selected are nickel or copper.
- the nickel or copper or alloys thereof gives rise to the formation of a highly resistive oxide layer. This solution is therefore unviable.
- Patent application CA 2 567 673 proposes the deposition of layers onto a flat interconnector.
- the layers are deposited from a suspension composed of a solvent, polymers and a primary phase and a secondary phase intended to adjust the thermomechanical behavior (coefficient of thermal expansion) to that of the electrochemical cell.
- the primary phase is preferably made of Ni, Ag, Au, Pt, Pd, Rh, Cu, Co or oxides thereof or doped cerium oxide or of other conductive oxides.
- the secondary phase may be oxides such as Al 2 O 3 , MgO, TiO 2 , manganese oxides or ZrO 2 .
- the primary phase is composed of manganite, or more broadly of conductive perovskite.
- the secondary phase is composed of noble metals or of oxides such as CuO, La 2 O 3 , SrO, or of manganese or cobalt oxides.
- the suspension may be applied via various processes such as dipping, spraying or screen printing.
- a heat treatment 600-1000° C. makes it possible to remove the organic materials.
- this solution has the advantage of providing materials that are specifically suited to the anode and cathode compartments, it does not afford fluid management of the gases between the flat interconnector and the electrodes. Furthermore, on account of the high compactness of the residual layer after heat treatment, the loss of pressure generated by the layers is detrimental to good functioning of the cells.
- One aim of the invention is to at least partly satisfy this need.
- Another aim of the invention is to propose an interconnector that makes it possible to achieve the proceeding aim and that is inexpensive to produce.
- the invention relates, in one of its aspects, to a component comprising a substrate made of metal alloy, of chromia-forming type, the base element of which is iron (Fe) or nickel (Ni), the substrate having two main flat faces, one of the main flat faces being coated with a coating comprising a thick ceramic layer, said thick ceramic layer being grooved, delimiting channels that are suitable for distributing and/or collecting gases, such as H 2 O steam, H 2 ; air.
- gases such as H 2 O steam, H 2 ; air.
- the invention also relates to a component comprising a substrate made of metal alloy, of chromia-forming type, the base element of which is iron (Fe) or nickel (Ni), the substrate having two main flat faces, one of the main flat faces being coated with a thick metallic layer, said thick metallic layer being grooved, delimiting channels that are suitable for distributing and/or collecting gases, such as H 2 O steam, H 2 ; O 2 , draining gas.
- gases such as H 2 O steam, H 2 ; O 2 , draining gas.
- one of the main flat faces is coated with a coating comprising a thick ceramic layer and the other of the main flat faces is coated with a thick metallic layer, each of the thick layers being grooved, delimiting channels that are suitable for distributing and/or collecting gases, such as H 2 O steam, draining gas, air, O 2 , H 2 .
- gases such as H 2 O steam, draining gas, air, O 2 , H 2 .
- the term “thick layer” means a layer whose thickness is greater than that of a layer obtained via a “thin-layer” technique, typically the thickness is between 2 and 15 ⁇ m.
- the term “chromia-forming” has here, and in the context of the invention, the usual meaning, i.e. a substrate made of metal alloy containing chromium. Reference may be made to paragraph 1.4 on page 30 of publication [9] to see the usual meaning of this definition.
- the material of the thick metallic layer is chosen from nickel (Ni) and alloys thereof, and also all the chromia-forming alloys whose base element is iron (Fe).
- the thickness of the ceramic layer is between 60 and 500 ⁇ m.
- the thickness of the metallic layer is between 60 and 500 ⁇ m.
- the chromia-forming metal alloy of the substrate may be chosen from ferritic (Fe—Cr), austenitic (Ni—Fe—Cr) stainless-steel alloys or superalloys based on nickel forming at the surface a layer of chromium oxide Cr 2 O 3 , known as the chromia layer.
- the substrate consists of at least one thin sheet, in which the thickness of a thin sheet is preferably between 0.1 and 1 mm.
- the substrate consists of a single plate with flat main faces, the thickness of which is preferably between 1 and 10 mm.
- the component according to the invention constitutes a constituent an interconnector of a high-temperature electrolysis (HTE) reactor comprising a stack of elementary electrolysis cells each formed from a cathode, an anode and an electrolyte intercalated between the cathode and the anode, the thick grooved ceramic layer being in contact with the anode of one of two adjacent elementary cells, the thick grooved metallic layer being in contact with the cathode of the other of the two adjacent elementary cells.
- HTE high-temperature electrolysis
- the component constitutes an interconnector of a fuel cell (SOFC) comprising a stack of elementary cells each formed from a cathode, an anode and an electrolyte intercalated between the cathode and the anode, the thick grooved ceramic layer being in contact with the cathode of one of two adjacent elementary cells, the thick grooved metallic layer being in contact with the anode of the other of the two adjacent elementary cells.
- SOFC fuel cell
- An interconnector according to the present invention is more advantageous than an interconnector according to the prior art, since the coating with a thick ceramic layer on a main face and with, where appropriate, a thick metallic layer on the other main face has a flexible nature.
- the thick ceramic and metallic layers according to the invention are in raw form in the interconnector, i.e. not dense. They therefore have mechanical adaptability. This is a fundamental advantage in the case of an HTE electrolyzer or an SOFC fuel cell in each of which it is necessary to apply a compression force (load) to ensure leaktightness between the various cells constituting the stack.
- a compression force load
- the adjustment imperfections between the various components of the stack may thus be compensated for by these adaptations (deformations) of the thick layers.
- the channels produced in the context of the invention the width of the channels is thus advantageously between 0.15 and 5 mm, where as the depth of the channels is advantageously between 0.1 and 0.5 mm.
- a subject of the invention is also a process for preparing a component, intended to constitute an interconnector for a fuel cell (SOFC) or a high-temperature electrolyzer (HTE), comprising the following steps:
- a subject of the invention is also a process for preparing a component, intended to constitute an interconnector for a fuel cell (SOFC) or a high-temperature electrolyzer (HTE), comprising the following steps:
- steps b1/ and c1/ performed on one flat face of the substrate
- steps b2/ and c2/ are performed on the other flat face of the substrate.
- the thick ceramic or metallic layer is obtained by pouring in a strip, step b1/and/or b2/ consisting of hot-bonding or hot-pressing or chemical bonding of the strip onto one or the other of the faces of the substrate.
- the suspension containing the ceramic powder, the solvents, dispersants, binders and plasticizers is poured onto a non-stick support. After evaporating off the solvents, said crude strips are obtained.
- step b1/ consists of hot-pressing or hot-bonding of the crude ceramic strip at a temperature of between 60 and 130° C. This temperature range is advantageous since these temperatures are high enough to obtain softening of the polymeric binders contained in a ceramic strip but not too high so as not to thermally degrade them.
- step b1/ and/or b2/ consists of screen printing in thick layers of a ceramic or metallic paste onto one or other of the faces of the substrate.
- step c1/ may be performed by calendaring the crude ceramic strip obtained by pouring between two rolls heated to the softening point of the polymers of the ceramic strip, at least one of the two rolls comprising ribs corresponding to the channels to be delimited, step b1/ being performed after step c1/.
- step c1/ and/or c2/ may be performed by laser ablation once step b1/and/or b2/, respectively, has been completed.
- step c1/ and/or c2/ is preferably performed using a CO 2 laser and more preferably completed after several passes of the laser over the thick layer.
- FIG. 1 is a schematic front view of an interconnecting plate of an HTE electrolyzer according to the prior art
- FIG. 1A is a detailed view in cross section of an interconnecting plate according to FIG. 1 ,
- FIG. 1B is a view similar to that of FIG. 1A showing the current lines passing through the plate
- FIG. 2 is a schematic front view of another interconnecting plate of an electrolyzer according to the prior art
- FIG. 3 is a photographic reproduction of a plate according to FIG. 1 , obtained by mechanical machining,
- FIG. 4 is a photographic reproduction of a plate according to FIG. 1 , obtained by drawing,
- FIG. 5 is an exploded schematic view of part of a high-temperature electrolyzer comprising interconnectors according to the prior art
- FIG. 6 is an exploded schematic view of part of an SOFC fuel cell comprising interconnectors according to the prior art
- FIG. 7 is a schematic view in cross section of an interconnector coated according to the invention.
- FIG. 8 is a photographic reproduction of an example of a thick grooved ceramic layer hot-bonded onto a substrate made of ferritic alloy in accordance with the invention.
- FIG. 8A is a schematic view in cross section of FIG. 8 showing the considered dimensions of the channels of the thick ceramic layer
- FIG. 9 shows the representative curves of the geometry of the grooves (furrows) obtained by CO 2 laser ablation on a thick ceramic layer
- FIG. 10 shows the variation in profile of the grooves shown in FIG. 9 before and after testing under a compression load and at a temperature of 800° C.
- FIGS. 11A and 11B are photographic reproductions of a thick ceramic layer before and after testing under a compression load and at a temperature of 800 ° C.
- FIG. 12 illustrates the curves of serial resistance measurement of various thick ceramic layers according to the invention and, for comparative purposes, of gold grates, the gold grate and layers being in contact with a substrate made of metal alloy.
- FIGS. 1 to 4 have already been commented on in the preamble. They are therefore not described in detail hereinbelow.
- FIG. 5 represents an exploded view of elementary units of a high-temperature steam electrolyzer according to the prior art.
- This HTE electrolyzer comprises a plurality of elementary electrolysis cells C 1 , C 2 , . . . stacked alternatively with interconnectors 8 ,
- Each cell C 1 , C 2 , . . . consists of a cathode 2 . 1 , 2 . 2 , . . . and of an anode 4 . 1 , 4 . 2 , between which is placed an electrolyte 6 . 1 , 6 . 2 , . . .
- the symbols and arrows indicating the path of steam, of dihydrogen and of oxygen, of the current are shown in this FIG. 5 for reasons of clarity.
- an interconnector 8 is a component made of metal alloy which provides the separation between the anode 7 and cathode 9 compartments, defined by the volumes between the interconnector 8 and the adjacent anode 4 . 2 and between the interconnector 8 and the adjacent cathode 2 . 1 , respectively. They also ensure the distribution of the gases to the cells.
- the injection of steam in each elementary unit takes place in the cathode compartment 9 .
- the collection of the hydrogen produced and of the residual steam at the cathode 2 . 1 , 2 . 2 is performed in the cathode compartment 9 downstream of the cell C 1 , C 2 after dissociation of the steam therefrom.
- the collection of the oxygen produced at the anode 4 . 2 is performed in the anode compartment 7 downstream of the cell C 1 , C 2 after dissociation of the steam therefrom.
- the interconnector 8 ensures the passage of the current between the cells C 1 and C 2 by direct contact with the adjacent electrodes, i.e. between the anode 4 . 2 and the cathode 2 . 1 ( FIG. 1 ).
- FIG. 6 represents the same elementary units as those of FIG. 5 , but for an SOFC fuel cell with elementary cells C 1 , C 2 and the interconnectors 8 .
- the symbols and arrows indicating the path of air, of dihydrogen and of oxygen, of the current are shown in this FIG. 6 for reasons of clarity.
- the injection of air containing oxygen into each elementary unit takes place in the cathode compartment 9 .
- the collection of the water produced at the cathode 2 . 1 , 2 . 2 is performed in the cathode compartment 9 downstream of the cell C 1 , C 2 after recombination of the water by the latter with the hydrogen H 2 injected at the anode 4 . 2 is performed in the anode compartment 7 upstream of the cell C 1 , C 2 .
- the current produced during the recombination of the water is collected by the interconnectors 8 .
- these interconnectors 8 are usually prepared by mechanical machining of thick plates or by using thin metal sheets, typically from 0.5 to 2 mm, drawn and then assembled by laser welding.
- the material and machining costs are high.
- the production technique has the advantage of limiting the cost of starting material, but does not make it possible to achieve a channel fineness as high as that by machining
- the production possibilities for the depth of the channels, the unit tooth width and the pitch between teeth are limited. Furthermore, the cost of the drawing tooling necessitates large-scale production. In addition, the electrical contact between the electrodes and the interconnector is not entirely satisfactory in particular due to the lack of planarity of the electrodes.
- the component 8 constituting the novel interconnector according to the invention comprises a substrate 82 made of metal alloy, the base element of which is iron (Fe) or nickel (Ni), the substrate having two main flat faces, one of the main flat faces being coated with a coating comprising a thick ceramic layer 80 and the other of the main flat faces being coated with a thick metallic layer 81 , each of the thick layers being grooved, delimiting channels 800 , 810 suitable for the distribution and/or collection of gases, such as H 2 O steam, draining gas, air, O 2 , H 2 .
- gases such as H 2 O steam, draining gas, air, O 2 , H 2 .
- a thin protective ceramic layer 83 may be intercalated between the thick ceramic layer 80 and the substrate 82 .
- the working conditions are the same as those conventionally used: the circulation of a reducing gaseous mixture is performed in the channels 810 of the thick metallic layer 81 and that of an oxidizing gaseous mixture takes place in the channels 800 of the thick ceramic layer 80 .
- the various steps in the production of an example of a thick ceramic layer 80 with its channels 800 and various tests proving the possibility of its use in the targeted applications, i.e. SOFC fuel cells and HTE electrolyzers, are described below.
- the example below is performed starting with a substrate 82 consisting of a single thin metal sheet made of commercial ferritic alloy of the CROFER 22 APU type.
- Step 1/ Manufacture of a Crude LSM Strip
- a mixture is prepared between a compound with a weight of 60 g of lanthanum manganite of formula La 0.8 Sr 0.2 MnO 3 with 0.8% by weight of oleic acid as dispersant, 15.7% of 2-butanone and 15.7% of ethanol as solvents.
- the mixture is milled in a planetary mill.
- the operating cycle of the planetary mill is as follows:
- a weight of 3.2 g of polyvinyl butyral (PVB 90) and 5.5 g of polyethylene glycol (PEG 400) as solvent are then added to the milled mixture, and the whole is then mixed using a planetary mill.
- the operating cycle of the planetary mill is as follows:
- the mixture is then deaerated using a mixer of roll type.
- the operating cycle of the roll mixer is as follows:
- the suspension obtained after deaeration is then poured in a strip using a doctor blade.
- the active height of the blade is equal to 1000 ⁇ m.
- the pouring speed is equal to 1.5 m/min.
- the pouring is performed onto a sheet of silicone-treated polymer (polyester) so as to promote the detachment of the strip once dried.
- the dried crude strip of LSM is finally chopped to the sizes corresponding to an air electrode in an SOFC cell, against which the strip is intended to bear.
- the cutting may be performed, for example, using a laser cutting table.
- Step 2/ hot-pressing
- the crude strip of LSM is then placed on a thin sheet of ferritic steel 1.5 mm thick and is then welded thereto by hot-pressing using a press.
- the thickness of the crude strip of LSM is 325 ⁇ m.
- the process is performed in an identical manner.
- the operating cycle of the press is as follows:
- Step 3/ production of the grooves
- Grooving is performed by laser ablation of the crude strip of LSM.
- the ablation is performed using a flatbed plotter equipped with a CO 2 laser of variable power up to a maximum power of 50 watts.
- the speed of movement of the laser is also variable, up to a maximum speed of 2 cm/s.
- the use of such a machine is particularly advantageous since it makes it possible by means of its variable operating characteristics to burn, i.e. to perform abrasion, more or less deeply the polymers constituting the crude strip, which thus releases the associated charge, the LSM. More or less deep grooves (furrows) may thus be dug. Where appropriate, several passes of the CO 2 laser over the crude strip may be performed to increase the depth and/or width of the grooves to a greater or lesser extent.
- FIG. 8 is a photographic reproduction of a thick layer of LSM grooved and hot-bonded onto a substrate consisting of a single sheet of CROFER 22 APU according to the invention.
- the photographed layer has, for example, a surface area of 100 cm 2 .
- FIG. 9 shows the representative curves of the geometry of grooves (furrows), i.e. their height and their width, derived from a number, respectively, of two and four passes of the CO 2 laser.
- the widths L1 of the teeth 801 obtained may be reduced to 150 ⁇ m and those L2 of the channels 800 may be reduced to 150 ⁇ m. It goes without saying that the widths L1, L2 may be greater than 150 ⁇ m.
- the height zero corresponds to the interface with the thin sheet of ferritic steel and that each of the geometries was obtained by adjusting the speed of movement of the laser to a value equal to 40% of the maximum speed indicated above and the power to a value equal to 50% of the maximum power indicated above (50 W).
- the metal component coated with the thick layer of LSM obtained in the example described above is placed under a compression load in the stack so as to ensure the electrical contact with the other elements of the stack and in particular the cathode of an SOFC cell.
- HTE high-temperature electrolysis
- it may be subjected to high temperatures of between 600° C. and 900° C.
- thermomechanical behavior under a compression force a test was performed according to which the LSM layer was subjected to a temperature of 800° C. and to a load of 0.2 MPa.
- FIG. 10 shows the representative curves of the geometry of grooves (furrows) before and after the 0.2 MPa load. From this figure, it emerges that the crude layer of LSM is crushed by only about 15 ⁇ m. This proves that the crude layer of LSM can be perfectly adapted mechanically to an electrochemical cell of an HTE reactor or SOFC fuel cell, under the high working temperature conditions. In other words, the crude nature of the LSM layer makes it possible to have a good thermomechanical behavior which implies a good mechanical contact with an electrochemical cell despite the possible surface imperfections of the latter.
- FIGS. 11A and 11B are three-dimensional representations of the LSM layer before and after, respectively, the test at 800° C. under a 0.2 MPa load. It is clearly seen that the crude layer of LSM remains integral after use due to its sufficiently high mechanical strength.
- measurements of the serial resistance with the component made of metal alloy were performed to characterize the electrical conductivity of the LSM layer obtained under representative operating conditions simulating the entry of cathode compartments 9 of an SOFC cell.
- the measuring method used is the “four-point” method as explained in publication [8].
- the LSM layer lacks channels, whereas in samples Nos. 2 to 4, the LSM layer is grooved defining identical channels with a unit width L1 equal to 1 mm, two adjacent channels being spaced by a tooth or rib of unit width L2 equal to 0.25 mm.
- FIG. 12 shows the results of measurement of the serial resistance of the various samples as a function of time. It is pointed out here that the measuring points between about 7 hours and 10 hours have not been reported in FIG. 12 .
- the thickness of the LSM layers in samples Nos. 1 to 4 is 325 ⁇ m, whereas the thickness of the grates in samples Nos. 5 and 6 is 500 ⁇ m.
- an LSM layer according to the invention has a negligible electrical contact resistance, of less than 10 m ⁇ .cm 2 .
- a thick metallic layer according to the invention on the face of a metal substrate opposite that comprising the thick ceramic layer may be performed in a similar manner to that which has been described, i.e. with pouring in a strip, followed by hot-pressing and production of grooves by ablation using a CO 2 laser.
Applications Claiming Priority (3)
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FR1259040A FR2996065B1 (fr) | 2012-09-26 | 2012-09-26 | Composant constituant un interconnecteur d'electrolyseur eht ou de pile a combustible sofc et procedes de realisation associes |
FR1259040 | 2012-09-26 | ||
PCT/IB2013/058814 WO2014049523A1 (fr) | 2012-09-26 | 2013-09-24 | Composant constituant un interconnecteur d'electrolyseur eht ou de pile a combustible sofc et procedes de realisation associes |
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PCT/IB2013/058814 A-371-Of-International WO2014049523A1 (fr) | 2012-09-26 | 2013-09-24 | Composant constituant un interconnecteur d'electrolyseur eht ou de pile a combustible sofc et procedes de realisation associes |
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US16/799,220 Division US11078579B2 (en) | 2012-09-26 | 2020-02-24 | Component constituting an HTE electrolyser interconnector or SOFC fuel cell interconnector and associated production processes |
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US20150218713A1 true US20150218713A1 (en) | 2015-08-06 |
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US14/429,610 Abandoned US20150218713A1 (en) | 2012-09-26 | 2013-09-24 | Component Constituting an HTE Electrolyser Interconnector or SOFC Fuel Cell Interconnector and Associated Production Processes |
US16/799,220 Active US11078579B2 (en) | 2012-09-26 | 2020-02-24 | Component constituting an HTE electrolyser interconnector or SOFC fuel cell interconnector and associated production processes |
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US16/799,220 Active US11078579B2 (en) | 2012-09-26 | 2020-02-24 | Component constituting an HTE electrolyser interconnector or SOFC fuel cell interconnector and associated production processes |
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US (2) | US20150218713A1 (fr) |
EP (1) | EP2900846B1 (fr) |
JP (1) | JP6476119B2 (fr) |
KR (1) | KR20150064046A (fr) |
AU (1) | AU2013322252B2 (fr) |
CA (1) | CA2885138C (fr) |
DK (1) | DK2900846T3 (fr) |
FR (1) | FR2996065B1 (fr) |
WO (1) | WO2014049523A1 (fr) |
ZA (1) | ZA201502274B (fr) |
Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
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US11557781B2 (en) | 2018-09-05 | 2023-01-17 | Battelle Energy Alliance, Llc | Electrochemical cells for hydrogen gas production and electricity generation, and related systems and methods |
Families Citing this family (10)
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NO343985B1 (en) * | 2017-07-03 | 2019-08-05 | Sintef Tto As | Polymer electrolyte membrane (PEM) water electrolyser cell, stack and system and a method for producing hydrogen in said PEM water electrolyser system |
FR3104324B1 (fr) * | 2019-12-10 | 2021-12-03 | Commissariat A L Energie Atomique Et Aux Energies Alternatives | Procédé de réalisation amélioré d’un composant constituant un interconnecteur d’électrolyseur EHT ou de pile à combustible SOFC. |
FR3113443B1 (fr) | 2020-08-11 | 2022-09-23 | Commissariat Energie Atomique | Réacteur d’électrolyse ou de co-électrolyse (SOEC) ou pile à combustible (SOFC) à empilement de cellules électrochimiques par modules préassemblés, Procédé de réalisation associé. |
JP2022119078A (ja) * | 2021-02-03 | 2022-08-16 | 東芝エネルギーシステムズ株式会社 | 保護層付きインターコネクタ、この保護層付きインターコネクタを具備するセルスタックならびに燃料電池 |
FR3122779B1 (fr) | 2021-05-04 | 2023-11-03 | Commissariat Energie Atomique | Procédé de réalisation d’un empilement à oxydes solides de type SOEC/SOFC et empilement associé |
FR3127639B1 (fr) | 2021-09-29 | 2023-10-27 | Commissariat Energie Atomique | Interconnecteur pour empilement de cellules à oxydes solides de type SOEC/SOFC comportant des éléments en relief différents |
FR3127640B1 (fr) | 2021-09-29 | 2023-10-27 | Commissariat Energie Atomique | Interconnecteur pour empilement de cellules à oxydes solides de type SOEC/SOFC comportant des languettes de géométrie optimisée |
FR3127850A1 (fr) | 2021-10-05 | 2023-04-07 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | Système de conditionnement d’une pluralité d’empilements de cellules à oxydes solides de type SOEC/SOFC à haute température superposés |
FR3129533A1 (fr) | 2021-11-23 | 2023-05-26 | Commissariat A L'energie Atomique Et Aux Energies Alternatives | Système de conditionnement d’une pluralité d’empilements de cellules à oxydes solides de type SOEC/SOFC à haute température |
FR3133947B1 (fr) | 2022-03-22 | 2024-02-09 | Commissariat Energie Atomique | Système de conditionnement d’une pluralité de sous-empilements de cellules à oxydes solides de type SOEC/SOFC à haute température superposés |
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Also Published As
Publication number | Publication date |
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KR20150064046A (ko) | 2015-06-10 |
JP6476119B2 (ja) | 2019-02-27 |
CA2885138A1 (fr) | 2014-04-03 |
FR2996065B1 (fr) | 2017-02-24 |
EP2900846B1 (fr) | 2022-08-17 |
EP2900846A1 (fr) | 2015-08-05 |
JP2015537329A (ja) | 2015-12-24 |
AU2013322252B2 (en) | 2018-02-15 |
FR2996065A1 (fr) | 2014-03-28 |
US11078579B2 (en) | 2021-08-03 |
US20200208275A1 (en) | 2020-07-02 |
DK2900846T3 (da) | 2022-11-07 |
WO2014049523A1 (fr) | 2014-04-03 |
AU2013322252A1 (en) | 2015-04-16 |
CA2885138C (fr) | 2021-09-14 |
ZA201502274B (en) | 2016-07-27 |
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