WO2016068200A1 - セル、セルスタック装置、モジュールおよびモジュール収容装置 - Google Patents
セル、セルスタック装置、モジュールおよびモジュール収容装置 Download PDFInfo
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- WO2016068200A1 WO2016068200A1 PCT/JP2015/080421 JP2015080421W WO2016068200A1 WO 2016068200 A1 WO2016068200 A1 WO 2016068200A1 JP 2015080421 W JP2015080421 W JP 2015080421W WO 2016068200 A1 WO2016068200 A1 WO 2016068200A1
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- support
- electrode layer
- cell
- solid electrolyte
- gas passage
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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
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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
- H01M8/1213—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material
- H01M8/1226—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the electrode/electrolyte combination or the supporting material characterised by the supporting layer
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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
- H01M8/023—Porous and characterised by the material
- H01M8/0236—Glass; Ceramics; Cermets
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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
- H01M8/0265—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant the reactant or coolant channels having varying cross sections
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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
- H01M8/0297—Arrangements for joining electrodes, reservoir layers, heat exchange units or bipolar separators to each other
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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
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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
- H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported 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
- H01M8/2428—Grouping by arranging unit cells on a surface of any form, e.g. planar or tubular
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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
- H01M8/2465—Details of groupings 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
- H01M8/10—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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- 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
Definitions
- the present invention relates to a cell, a cell stack device, a module, and a module housing device.
- the fuel cell device accommodates a cell stack device in which a plurality of solid oxide fuel cell cells (hereinafter sometimes abbreviated as fuel cell cells) are electrically connected in series as cells, and the cell stack device. And a storage container.
- fuel cell cells solid oxide fuel cell cells
- the fuel cell of such a fuel cell device extends in the longitudinal direction and has a support containing nickel (Patent Document 1).
- the support is provided with a gas passage penetrating in the longitudinal direction inside, and the fuel gas flows through the gas passage.
- An object of the present invention is to provide a cell, a cell stack device, a module, and a module housing device that can suppress damage.
- the cell of the present invention is columnar, contains nickel, has a gas passage penetrating in the longitudinal direction inside, and has one end provided with an outlet of the gas passage and an inlet of the gas passage.
- a support having the other end provided, a first electrode layer located on the support, a solid electrolyte layer located on the first electrode layer, and a second electrode located on the solid electrolyte layer
- the one end portion of the support has a smaller amount of metallic nickel than the central portion in the longitudinal direction.
- a plurality of cell stack devices of the present invention are arranged and have the above-described cells electrically connected to each other.
- the module of the present invention includes a storage container and the above-described cell stack device stored in the storage container.
- a module housing apparatus of the present invention includes an exterior case, the above-described module housed in the exterior case, and an auxiliary device housed in the exterior case and operating the module. It is characterized by that.
- one end portion in the longitudinal direction has a smaller amount of metallic nickel than the central portion in the longitudinal direction, so even if oxygen-containing gas flows into the support from the outlet of the gas passage, It can be set as the cell which can suppress the damage by expansion
- FIG. 1 shows an example of a cell stack apparatus using the cell shown in FIG. 1, wherein (a) is a side view schematically showing the cell stack apparatus, and (b) is one part of the cell stack apparatus surrounded by a broken line in (a). It is sectional drawing which expands and shows a part. It is an external appearance perspective view which shows an example of a module. It is a perspective view which abbreviate
- FIG. 1 shows an example of an embodiment of a cell, where (a) is a cross-sectional view and (b) is a side view. In both drawings, a part of each component of the cell 10 is shown enlarged. Similarly, other drawings are partially enlarged. In the following description, a solid oxide fuel cell is used as the cell 10 and may be simply referred to as a cell.
- the cell 10 includes a support 1.
- the support 1 is columnar.
- the support body 1 is flat plate shape.
- the support body 1 is a hollow flat plate type, and is an elongate plate shape.
- a plurality of gas passages 2 pass through the support 1 at appropriate intervals in the longitudinal direction L of the support 1, and the cell 10 is provided with various members on the support 1. Have a structure.
- the support 1 has a longitudinal direction L as shown in FIG. As can be understood from the shape shown in FIG. 1, a pair of main surfaces (first main surface n1, second main surface n2) facing each other and a pair of main surfaces n1, n2 are connected to each other. It is made into the plate shape comprised by the arc-shaped surface (side surface) m. In addition, as in the example shown in FIGS. 1A and 1B, the plate-like support 1 also has a short direction w.
- a fuel electrode layer 3 as a first electrode layer is disposed so as to cover the first main surface n1 (one main surface: lower surface) and the arcuate surfaces m on both sides.
- a solid electrolyte layer 4 made of ceramics having gas barrier properties is disposed so as to cover the surface.
- the thickness of the solid electrolyte layer 4 is preferably 40 ⁇ m or less, 20 ⁇ m or less, and more preferably 15 ⁇ m or less from the viewpoint of improving power generation performance.
- An oxygen electrode layer 6 as a second electrode layer is disposed on the surface of the solid electrolyte layer 4 on the first main surface n1 so as to face the fuel electrode layer 3 through the intermediate layer 9. .
- the intermediate layer 9 is provided between the oxygen electrode layer 6 and the solid electrolyte layer 4.
- the second main surface n2 (the other main surface: upper surface) on which the solid electrolyte layer 4 is not laminated is made of lanthanum chromite (LaCrO 3 system) oxide having gas barrier properties through an adhesion layer (not shown).
- a dense interconnector layer 8 is disposed.
- the fuel electrode layer 3 and the solid electrolyte layer 4 are provided from the first main surface n1 to the second main surface n2 via the arcuate surfaces m at both ends, and at both ends of the solid electrolyte layer 4 Both ends of the interconnector layer 8 are laminated and joined.
- the solid electrolyte layer 4 and the interconnector layer 8 surround the support 1 so that fuel gas flowing through the inside does not leak to the outside.
- the solid electrolyte layer 4 and the interconnector layer 8 form a cylindrical body having a gas barrier property.
- the inside of the cylindrical body is a fuel gas flow path, and the fuel gas supplied to the fuel electrode layer 3
- the oxygen-containing gas supplied to the oxygen electrode layer 6 is blocked by the cylindrical body.
- the oxygen electrode layer 6 having a rectangular planar shape is provided except for the upper and lower ends of the support 1, while the interconnector layer 8 is Although not shown, the support 1 is provided from the upper end to the lower end in the longitudinal direction L, and both ends of the support 1 in the short direction W are joined to the surfaces of both ends of the solid electrolyte layer 4.
- the portion where the fuel electrode layer 3 and the oxygen electrode layer 6 face each other through the solid electrolyte layer 4 functions as a fuel cell to generate electric power. That is, electricity is generated by flowing an oxygen-containing gas such as air outside the oxygen electrode layer 6 and flowing a fuel gas (hydrogen-containing gas) through the gas passage 2 in the support 1 and heating it to a predetermined operating temperature. And the electric current produced
- the fuel electrode layer 3 as the first electrode layer, a generally known one can be used, and porous conductive ceramics such as ZrO 2 (stabilized zirconia and And also includes partial stabilization) and Ni and / or NiO.
- porous conductive ceramics such as ZrO 2 (stabilized zirconia and And also includes partial stabilization) and Ni and / or NiO.
- the solid electrolyte layer 4 has a function as an electrolyte that bridges ions between electrodes, and at the same time needs to have a gas barrier property in order to prevent leakage between the fuel gas and the oxygen-containing gas. It is formed from ZrO 2 in which 3 to 15 mol% of a rare earth element is dissolved. In addition, as long as it has the said characteristic, you may form using another material etc.
- the oxygen electrode layer 6 as the second electrode layer is not particularly limited as long as it is generally used.
- the oxygen electrode layer 6 can be formed from a conductive ceramic made of a so-called ABO 3 type perovskite oxide.
- the oxygen electrode layer 6 is required to have gas permeability, and preferably has an open porosity of 20% or more, particularly 30 to 50%.
- the interconnector layer 8 can be formed from conductive ceramics, but is required to have reduction resistance and oxidation resistance because it is in contact with a fuel gas (hydrogen-containing gas) and an oxygen-containing gas (air, etc.). Therefore, a lanthanum chromite perovskite oxide (LaCrO 3 oxide) is preferably used.
- the interconnector layer 8 must be dense in order to prevent leakage of fuel gas flowing through the plurality of gas passages 2 formed in the support 1 and oxygen-containing gas flowing outside the support 1, It is preferable to have a relative density of 93% or more, particularly 95% or more.
- the support 1 is required to be gas permeable so as to allow the fuel gas to permeate to the fuel electrode layer 3, and further to be conductive in order to collect current via the interconnector layer 8. Therefore, as the support 1, it is necessary to adopt a material satisfying such a requirement as a material, and for example, conductive ceramics, cermet, or the like can be used.
- nickel and a specific rare earth oxide Y 2 O 3 , Yb 2 O 3 etc.
- the support 1 is formed from the above.
- nickel includes both non-oxidized metallic nickel (Ni) and nickel oxide (NiO, Ni 2 O 3 and the like).
- nickel including metallic nickel and nickel oxide: rare earth oxide in terms of maintaining good conductivity of the support 1 and approximating the thermal expansion coefficient to that of the solid electrolyte layer 4. It is preferably present in a volume ratio of 35:65 to 65:35.
- the support 1 may contain other metal components and oxide components as long as required characteristics are not impaired.
- the support 1 preferably has an open porosity of 30% or more, particularly 35 to 50% in order to have the required gas permeability, and its conductivity is 300 S / cm or more, particularly It is preferable that it is 440 S / cm or more.
- the solid electrolyte layer 4 and the oxygen electrode layer 6 are strongly bonded to each other between the solid electrolyte layer 4 and the oxygen electrode layer 6, and the components of the solid electrolyte layer 4 and the oxygen electrode layer 6 react with each other.
- the intermediate layer 9 can also be provided for the purpose of suppressing the formation of a reaction layer having a high electrical resistance.
- the intermediate layer 9 can be formed with a composition containing Ce (cerium) and other rare earth elements, for example, (1): (CeO 2 ) 1-x (REO 1.5 ) x
- RE is at least one of Sm, Y, Yb, and Gd
- x is a number that satisfies 0 ⁇ x ⁇ 0.3. It is preferable to have the composition represented by these. Further, from the viewpoint of reducing electric resistance, it is preferable to use Sm or Gd as RE, and for example, it is preferably made of CeO 2 in which 10 to 20 mol% of SmO 1.5 or GdO 1.5 is dissolved. .
- the solid electrolyte layer 4 and the oxygen electrode layer 6 are firmly bonded, and the component of the solid electrolyte layer 4 and the component of the oxygen electrode layer 6 react to form a reaction layer having a high electric resistance.
- the intermediate layer 9 can also be formed of two layers.
- an adhesion layer is provided between the interconnector layer 8 and the support 1 to reduce a difference in thermal expansion coefficient between the interconnector layer 8 and the support 1. You can also.
- the adhesion layer can have a composition similar to that of the fuel electrode layer 3, and is formed of, for example, ZrO 2 (referred to as stabilized zirconia) in which a rare earth element such as YSZ is dissolved and Ni and / or NiO. can do.
- ZrO 2 referred to as stabilized zirconia
- the volume ratio of ZrO 2 in which the rare earth element is dissolved and Ni and / or NiO is preferably in the range of 40:60 to 60:40.
- the support 1 has one end provided with the outlet of the gas passage 2 and the other end provided with the inlet of the gas passage 2. Moreover, in the support body 1, the one end part in a longitudinal direction has metal nickel content less than the center part in a longitudinal direction.
- the central portion refers to the middle portion when the support 1 is divided into five in the longitudinal direction.
- an one end part means the part of the one end side at the time of dividing into five.
- the oxygen-containing gas supplied to the fuel cell 10 is introduced into the support 1 from the outlet of the gas passage 2.
- the metal nickel contained in the support 1 is oxidized to become nickel oxide, which causes volume expansion.
- the metal nickel content at one end portion in the longitudinal direction is smaller than the metal nickel content at the central portion in the longitudinal direction, so that even if the metal nickel is oxidized and expanded, it is supported. Since the amount of expansion at one end of the body 1 can be suppressed, damage due to volume expansion can be suppressed.
- the ratio of metallic nickel in the one end part is lower than that in the central part.
- the metal nickel ratio is determined by (peak value of metallic nickel by X-ray diffraction) / (sum of peak value of metallic nickel and peak value of nickel oxide by X-ray diffraction) ⁇ 100 (%). The sum of the peak value of NiO and the peak value of Ni 2 O 3 is used as the peak value of nickel oxide.
- the metal nickel content at the center of the support 1 is 1, the metal nickel content at one end of the support 1 is preferably in the range of 0.4 to 0.95.
- the metallic nickel content is small at one end, the expansion amount at the one end can be effectively suppressed.
- the fall of the electrical conductivity of the support body 1 can be suppressed in one end part.
- the content of metallic nickel may gradually decrease from the central portion in the longitudinal direction of the support 1 toward one end portion, or may decrease rapidly with a certain point as a boundary.
- the one end part in a longitudinal direction has a porosity lower than the center part in a longitudinal direction.
- the oxygen-containing gas supplied to the fuel cell 10 may flow into the support 1 from the outlet of the gas passage 2, but the longitudinal direction of the support 1 Since the porosity of one end of the lower portion is lower than that of the central portion, the amount of oxygen-containing gas flowing into the support at one end can be suppressed.
- the porosity of the central portion in the longitudinal direction of the support 1 is 1, the porosity of one end in the longitudinal direction of the support 1 is preferably in the range of 0.8 to 0.95. .
- the porosity may be gradually decreased from the central portion in the longitudinal direction of the support 1 toward one end portion, or may be rapidly decreased at a certain point as a boundary.
- FIG. 2 shows another example of the embodiment of the cell, and shows a part of the longitudinal sectional view of the cell.
- the gas passage 2 preferably has a diameter at one end smaller than that at the center.
- the oxygen-containing gas supplied to the fuel cell 10 may flow into the support 1 from the outlet of the gas passage 2, but one end of the gas passage 2 is in the center portion. Since it is smaller than the diameter, the backflow of the oxygen-containing gas into the gas passage 2 can be suppressed. Therefore, since the inflow of the oxygen-containing gas can be suppressed at one end where the amount of metallic nickel is small, damage due to volume expansion can be further suppressed.
- the diameter of one end in the longitudinal direction of the support 1 is 1, the diameter of the central portion in the longitudinal direction of the support 1 is preferably in the range of 1.003 to 1.03.
- the diameter of the gas passage 2 may be gradually decreased from the central portion in the longitudinal direction of the support 1 toward the other end, or may be rapidly decreased with a certain point as a boundary.
- the metal nickel content on the surface side of the support 1 is preferably less than the metal nickel content on the inner side of the support 1.
- the metal nickel content on the inner side of the support 1 is 1, the metal nickel content on the surface side of the support 1 is preferably in the range of 0.85 to 0.98.
- the metal nickel content on the surface side of the support 1 is smaller than the metal nickel content on the inner side of the support 1 at one end in the longitudinal direction of the support 1. Since one end in the longitudinal direction of the support 1 provided with the outlet of the gas passage 2 flows in a large amount of oxygen-containing gas, the support 1 and the fuel electrode layer 3 provided on the surface of the support 1 in particular, Separation from the solid electrolyte layer 4 is likely to occur. Therefore, particularly at one end in the longitudinal direction of the support 1, damage such as separation from the solid electrolyte layer 4 is effectively suppressed by relatively reducing the metal nickel content on the surface side of the support 1. be able to.
- the end portion side in the short direction W has a smaller amount of metallic nickel than the central portion in the short direction W.
- the central portion refers to a middle portion when the support 1 is divided into five in the short direction.
- an one end part means the part of the one end side at the time of dividing into five.
- both end portions of the solid electrolyte layer 4 are disposed on the end portion side of the second main surface n2 of the support 1.
- FIG. 3 is a cross-sectional view of another embodiment showing a fuel cell having a fuel electrode layer as a support. Even in this case, the same effect as that of FIG. 1 can be obtained. That is, in the embodiment of FIG. 1, the fuel electrode layer 3, the solid electrolyte layer 4, and the oxygen electrode layer 6 are laminated on the support 1. However, as in the embodiment of FIG. The support 1 may be provided with the solid electrolyte layer 4 and the oxygen electrode layer 6.
- the support 2 is provided with a plurality of gas passages 2.
- the gas passage 2 may be singular.
- a method for measuring the metallic nickel content at one end in the longitudinal direction of the support 1 and the metallic nickel content at the central portion in the longitudinal direction is shown below.
- the support 1 is trimmed until the inner walls of these gas passages 2 are exposed.
- an intermediate point located on the inner wall of the gas passage 2 and in the middle in the longitudinal direction is determined.
- the ratio of metallic nickel at the five intermediate points is calculated, and the average value is calculated.
- the average value of the metallic nickel ratios at the five intermediate points is also calculated at the center in the longitudinal direction.
- a method for measuring the diameter of the gas passage 2 at one end in the longitudinal direction of the support 1 and the diameter of the gas passage 2 at the center in the longitudinal direction will be described below.
- the support 1 is cut away to expose the inner wall of the gas passage 2 as shown in FIG.
- an intermediate point is determined on the inner wall of the gas passage 2 at one end in the same manner as described above.
- the diameter of the gas passage 2 at this intermediate point is obtained by a method such as calipers. This is performed in five arbitrarily selected gas passages 2, and an average value is calculated.
- a similar method may be performed for the central portion. These average values may be the diameter of the gas passage 2 at one end in the longitudinal direction and the diameter of the gas passage 2 at the central portion in the longitudinal direction.
- the method for measuring the porosity of one end portion in the longitudinal direction of the support 1 and the porosity of the central portion in the longitudinal direction is shown below. First, the one end part and center part of the support body 1 are each cut out. Next, it polishes and grinds until members other than the support bodies 1 such as the oxygen electrode layer 6 and the interconnector layer 8 are removed. Next, what is necessary is just to obtain
- the measuring method of the metallic nickel content on the surface side of the support 1 and the metallic nickel content on the inner side is shown below.
- a first point adjacent to the gas passage 2 is determined on the end face.
- a line extending in the thickness direction of the support 1 is drawn on the end face. The line passes through the first point.
- a second point that is on the line and is adjacent to the first main surface n1 of the support 1 is determined.
- the metal nickel ratio is calculated at the first point and the second point.
- the operation of calculating the ratio of the metallic nickel at the first point and the second point has been performed in one arbitrarily selected gas passage 2, but the same operation is performed in the other four arbitrary gas passages 2. Also do in. Next, the average value of the metallic nickel ratios at the five first points is obtained and used as the metallic nickel content on the inner side. Next, the average value of the metallic nickel ratios at the five second points is determined and used as the metallic nickel content on the surface side.
- a method for measuring the content of metallic nickel at one end in the lateral direction on the second main surface n2 side of the support 1 and the content of metallic nickel at the center in the lateral direction will be described below.
- the end surface on the one end side of the support 1 is observed.
- a point adjacent to the gas passage 2 at one end is determined on the end face.
- the metal nickel ratio is obtained and set as the metal nickel content at one end.
- a point adjacent to the central gas passage 2 is determined on the end face. At this point, the metal nickel ratio is obtained and set as the metal nickel content in the center.
- Ni and / or NiO powder powder of an inorganic oxide such as Y 2 O 3 , an organic binder, and a solvent are mixed to prepare a clay.
- the organic binder is mixed and adjusted to such an amount that the clay can obtain fluidity.
- a thermoplastic resin from a viewpoint of performing the injection molding mentioned later.
- a support body molded object is produced by injection molding using this clay, and this is dried.
- a calcined body obtained by calcining the support molded body at 900 to 1000 ° C. for 2 to 6 hours may be used.
- a resin molded body having a predetermined shape is fixed in advance with a jig such as a pin inside a mold used for injection molding.
- a resin that evaporates and burns at the temperature at the time of calcining or firing the support molded body is used.
- the shape of the resin molded body is set to a desired shape of the gas passage 2. For example, when forming the gas passage 2 having a diameter at one end smaller than that at the center as shown in FIG. 2, a resin molded body having the same shape as the gas passage 2 may be prepared.
- a support molded body having a resin molded body inside is obtained by injecting the above-mentioned clay into a mold provided with such a resin molded body and performing injection molding. Thereafter, the support molded body is calcined or fired, and the resin molded body is burned down by raising the temperature to a predetermined temperature. Therefore, the area occupied by the resin molded body in the support is a space. Therefore, it is possible to obtain the support 1 having the gas passage 2 whose diameter at the one end is smaller than the diameter at the center.
- raw materials of NiO and ZrO 2 (YSZ) in which Y 2 O 3 is dissolved are weighed and mixed. Thereafter, an organic binder and a solvent are mixed with the mixed powder to prepare a slurry for the fuel electrode layer.
- a ZrO 2 powder in which a rare earth element is solid-dissolved and a slurry obtained by adding toluene, a binder powder, a commercially available dispersant, etc., are formed by a method such as a doctor blade to form a sheet-like solid electrolyte layer molded body. Make it.
- the fuel electrode layer slurry is applied onto the obtained sheet-shaped solid electrolyte layer molded body and dried to form a fuel electrode layer molded body, thereby forming a sheet-shaped laminated molded body.
- the surface on the fuel electrode layer molded body side of the sheet-shaped laminated molded body in which the fuel electrode layer molded body and the solid electrolyte layer molded body are laminated is laminated on the support molded body to form a molded body.
- the laminated molded body is calcined at 800 to 1200 ° C. for 2 to 6 hours.
- an interconnector layer material for example, LaCrMgO 3 -based oxide powder
- an organic binder for example, LiCrMgO 3 -based oxide powder
- a solvent for example, a solvent
- a method for producing a fuel cell having an adhesion layer will be described.
- an adhesion layer molded body positioned between the support 1 and the interconnector layer 8 is formed.
- An adhesion layer molded body is formed by coating on a support molded body between both ends of the layer molded body.
- an intermediate layer 9 disposed between the solid electrolyte layer 4 and the oxygen electrode layer 6 is formed.
- CeO 2 powder in which GdO 1.5 is dissolved is heat-treated at 800 to 900 ° C. for 2 to 6 hours to prepare a raw material powder for the intermediate layer molded body.
- Toluene is added to the raw material powder as a solvent to prepare an intermediate layer slurry, and this slurry is applied onto the solid electrolyte layer formed body to prepare an intermediate layer formed body.
- the interconnector layer slurry is applied to the upper surface of the adhesion layer molded body so that both ends of the interconnector layer molded body are laminated on both ends of the solid electrolyte molded body (calcined body), and laminated.
- a molded body is produced.
- the interconnector layer slurry is prepared, the interconnector layer sheet is prepared, and the both ends of the interconnector layer sheet are laminated on both ends of the solid electrolyte molded body.
- An interconnector layer sheet can be laminated to produce a laminated molded body.
- the above-mentioned laminated molded body is subjected to binder removal treatment, and simultaneously sintered (co-fired) in an oxygen-containing atmosphere at 1400 to 1500 ° C., particularly 1425 to 1475 ° C. for 2 to 6 hours.
- a slurry containing an oxygen electrode layer material for example, LaCoO 3 oxide powder
- a solvent and a pore increasing agent is applied onto the intermediate layer by dipping or the like, and baked at 1000 to 1300 ° C. for 2 to 6 hours.
- an oxygen electrode layer material for example, LaCoO 3 oxide powder
- a solvent and a pore increasing agent is applied onto the intermediate layer by dipping or the like, and baked at 1000 to 1300 ° C. for 2 to 6 hours.
- the configuration in which the metal nickel content is reduced at one end of the support 1 is realized by a method in which the diameter of the inlet of the gas passage 2 at one end of the support 1 is smaller than that at the center.
- a method in which the porosity of one end portion of the support 1 is lower than that of the central portion may be employed.
- hydrogen gas is less likely to diffuse at the one end of the support 1 than at the center and the reduction is less likely to proceed, and the metal nickel content can be less than at the center.
- extrusion molding can be used as a method of making the porosity of one end of the support 1 lower than that of the central portion.
- resin beads may be added simultaneously when preparing clay by mixing Ni and / or NiO powder, powder of inorganic oxide such as Y 2 O 3 , organic binder, and solvent.
- a resin that evaporates and burns at the temperature at the time of calcining or firing the support molded body is used.
- the resin beads are composed of a large amount of granular materials.
- a support molded body having a large number of resin beads at one end and a small number of resin beads at the center is produced by extrusion molding, and dried.
- a calcined body obtained by calcining the support molded body at 900 to 1000 ° C. for 2 to 6 hours may be used.
- the resin beads are burned out.
- the above-described method is used.
- the resin beads to be mixed into the corresponding portion of the support molded body may be less than other portions.
- FIG. 4 shows an example of a cell stack apparatus configured by electrically connecting a plurality of the cells 10 shown in FIG. 1 in series via the current collecting member 13, and FIG.
- stuck apparatus 11 roughly, (b) is a partial expanded sectional view of the cell stack apparatus 11 of (a), and has extracted and shown the part enclosed with the broken line shown in (a). .
- the part corresponding to the part surrounded by the broken line shown in (a) is indicated by an arrow, and in the cell 10 shown in (b), the above-described intermediate layer or the like is shown. Some members are omitted.
- each cell 10 is arranged via a current collecting member 13 to constitute a cell stack 12, and the lower end portion (the other end portion) of each fuel cell 10 is a fuel.
- the gas tank 16 for supplying the fuel gas to the battery cell 10 is fixed with an adhesive such as a glass sealing material.
- the cell stack 12 is sandwiched from both ends of the fuel cell 10 in the arrangement direction by the elastically deformable conductive member 14 whose lower end is fixed to the gas tank 16.
- the conductive member 14 has a current drawing portion 15 for drawing current generated by power generation of the cell stack 12 (fuel cell 10) in a shape extending outward along the arrangement direction of the fuel cells 10. Is provided.
- two cells 10 are electrically connected by a current collecting member 13, and the current collecting member 13 is short, for example, on a rectangular heat-resistant alloy plate at a predetermined interval in the longitudinal direction.
- a slit extending in the hand direction is formed, and strips between the slits are alternately projected in the thickness direction of the heat-resistant alloy plate, and the strips protruding in the opposite direction are electrically connected to the cells 10 respectively.
- the cell stack 12 is configured by bonding with the adhesive.
- FIG. 5 is an external perspective view showing an example of a module 18 in which the cell stack device 11 is stored in the storage container 19.
- the cell stack device 11 shown in FIG. 4 is installed inside the rectangular parallelepiped storage container 19. It is housed and configured.
- a reformer 20 for reforming raw fuel such as natural gas or kerosene to generate fuel gas is disposed above the cell stack 12. ing.
- the fuel gas generated by the reformer 20 is supplied to the gas tank 16 via the gas flow pipe 21 and supplied to the gas passage 2 provided inside the fuel cell 10 via the gas tank 16.
- FIG. 5 shows a state in which a part (front and rear surfaces) of the storage container 19 is removed and the cell stack device 11 and the reformer 20 housed inside are taken out rearward.
- the cell stack device 11 can be slid and stored in the storage container 19.
- the cell stack device 11 may include the reformer 20.
- the oxygen-containing gas introduction member 22 provided inside the storage container 19 is disposed between a pair of cell stacks 12 juxtaposed to the gas tank 16, and the oxygen-containing gas flows into the flow of the fuel gas.
- an oxygen-containing gas is supplied to the lower end of the fuel cell 10 so that the side of the fuel cell 10 flows from the lower end toward the upper end.
- the temperature of the fuel cell 10 can be increased by reacting the fuel gas discharged from the gas passage 2 of the fuel cell 10 with the oxygen-containing gas and burning it on the upper end side of the fuel cell 10. The activation of the cell stack device 11 can be accelerated.
- the fuel cell 10 is placed above the fuel battery cell 10 (cell stack 12).
- the arranged reformer 20 can be warmed. Thereby, the reforming reaction can be efficiently performed in the reformer 20.
- the cell stack device 11 using the above-described fuel cell 10 is housed in the housing container 19, so that the module 18 with improved reliability can be obtained.
- FIG. 6 is a perspective view showing an example of a module housing device in which the module 18 shown in FIG. 5 and an auxiliary machine for operating the cell stack device 11 are housed in the outer case. In FIG. 6, a part of the configuration is omitted.
- the module housing device 23 shown in FIG. 6 divides the inside of the exterior case composed of the columns 24 and the exterior plate 25 into upper and lower portions by the partition plate 26, and the upper side serves as a module storage chamber 27 that houses the module 18 described above.
- the lower side is configured as an auxiliary equipment storage chamber 28 for storing auxiliary equipment for operating the module 18.
- auxiliary machines stored in the auxiliary machine storage chamber 28 are not shown.
- the partition plate 26 is provided with an air circulation port 29 for flowing the air in the auxiliary machine storage chamber 28 to the module storage chamber 27 side, and a part of the exterior plate 25 constituting the module storage chamber 27 An exhaust port 30 for exhausting the air in the module storage chamber 27 is provided.
- the module housing device 23 with improved reliability is configured by housing the module 18 with improved reliability in the module housing chamber 27. it can.
- the hollow plate type solid oxide fuel cell has been described.
- a cylindrical or flat plate type solid oxide fuel cell may be used.
- a so-called horizontal stripe fuel cell may be used.
- various intermediate layers may be formed between the members in accordance with the function.
- a fuel battery cell in which an oxygen electrode layer, a solid electrolyte layer, and a fuel electrode layer are disposed on a conductive support may be used.
- NiO powder having an average particle size of 0.5 ⁇ m and Y 2 O 3 powder having an average particle size of 0.9 ⁇ m were calcined and reduced to a volume ratio of 48% by volume for NiO and 52% by volume for Y 2 O 3.
- the kneaded material prepared with an organic binder and a solvent was molded by injection molding, dried and degreased to prepare a support molded body.
- a resin molded body having the same shape as that of the gas passage is included in order to form the gas passage 2 having a diameter at one end smaller than that at the central portion.
- a support molded body was produced.
- a sheet for a solid electrolyte layer having a thickness of 30 ⁇ m was prepared by a doctor blade method.
- the slurry for forming the intermediate layer formed body is composed of a complex oxide containing 90 mol% of CeO 2 and 10 mol% of rare earth element oxide (GdO 1.5 , SmO 1.5 ), or 92 mol of CeO 2. %, And a composite oxide containing 8 mol% of GdO 1.5 was pulverized with a vibration mill or a ball mill using isopropyl alcohol (IPA) as a solvent, and calcined at 900 ° C. for 4 hours. The powder was crushed to adjust the degree of aggregation of the ceramic particles, and an acrylic binder and toluene were added to the powder and mixed.
- IPA isopropyl alcohol
- a slurry for the fuel electrode layer is prepared by mixing the NiO powder having an average particle size of 0.5 ⁇ m, the ZrO 2 powder in which Y 2 O 3 is dissolved, an organic binder, and a solvent, and screen-printed on the solid electrolyte layer sheet. It was applied by the method and dried to form a fuel electrode layer molded body. Subsequently, a slurry for forming the intermediate layer molded body is applied by screen printing on the solid electrolyte layer sheet on the surface opposite to the surface on which the fuel electrode layer molded body is formed, and dried. An intermediate layer molded body was formed.
- a sheet-like laminated molded body in which an intermediate layer molded body and a fuel electrode layer molded body are formed on both surfaces of the solid electrolyte layer sheet is laminated at a predetermined position of the support molded body with the fuel electrode layer molded body side facing inward.
- the laminated molded body in which the molded bodies were laminated as described above was calcined at 1000 ° C. for 3 hours.
- the above-described resin molded body was burned out, and a support molded body having a gas passage 2 having a diameter at one end smaller than that at the center was obtained.
- a raw material composed of Ni and YSZ was mixed and dried, and an organic binder and a solvent were mixed to prepare an adhesion layer slurry.
- the adjusted slurry for the adhesion layer is applied to the portion of the support where the fuel electrode layer (and the solid electrolyte layer) is not formed (the portion where the support is exposed), and the adhesion layer formed body is laminated, and the intermediate layer formed body And the slurry for interconnector layers was apply
- the above-mentioned laminated molded body was debindered and co-fired at 1450 ° C. for 2 hours in an oxygen-containing atmosphere.
- a mixed liquid composed of La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3 powder having an average particle diameter of 2 ⁇ m and isopropyl alcohol was prepared, and the surface of the intermediate layer of the laminated sintered body was formed.
- the air electrode layer formed body was formed by spray coating, and baked at 1100 ° C. for 4 hours to form the air electrode layer. 1 to 6 fuel cells were produced.
- the size of the produced fuel cell is 25 mm ⁇ 200 mm, the thickness of the support (the thickness between the first main surface n1 and the second main surface n2) is 2 mm, the open porosity is 35%, and the thickness of the fuel electrode layer The thickness was 10 ⁇ m, the open porosity was 24%, the thickness of the air electrode layer was 50 ⁇ m, the open porosity was 40%, and the relative density of the solid electrolyte layer was 97%.
- x in Table 1 indicates a case where one end portion of the support was not damaged
- ⁇ indicates a case where one end portion of the support was damaged
- Support body 2 Gas passage 3: Fuel electrode layer (first electrode layer) 4: Solid electrolyte layer 6: Oxygen electrode layer (second electrode layer) 8: Interconnector layer 10: Fuel cell 11: Cell stack device 18: Module 23: Module housing device
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Abstract
Description
図1は、セルの実施形態の一例を示すもので、(a)は横断面図、(b)は側面図である。なお、両図面において、セル10の各構成の一部を拡大して示している。他の図面についても同様に一部を拡大して示している。なお、以下の説明においてセル10として固体酸化物形の燃料電池セルを用いて説明するものとし、単にセルという場合がある。
(1):(CeO2)1-x(REO1.5)x
式中、REはSm、Y、Yb、Gdの少なくとも1種であり、xは0<x≦0.3を満足する数。
で表される組成を有していることが好ましい。さらには、電気抵抗を低減するという点から、REとしてSmやGdを用いることが好ましく、例えば10~20モル%のSmO1.5またはGdO1.5が固溶したCeO2からなることが好ましい。
支持体1の長手方向における一端部の金属ニッケル含有量、および長手方向における中央部の金属ニッケル含有量の測定方法を以下に示す。まず、ガス通路2を任意に5つ選ぶ。次にこれらのガス通路2の内壁が露出するまで、支持体1を削り込む。次に、5つのガス通路2それぞれにおいて、ガス通路2の内壁上であって長手方向における中間に位置する中間点を決定する。次に、5つの中間点における金属ニッケル比率を算出して、平均値を算出する。また、長手方向における中央部においても同様に5つの中間点における金属ニッケル比率の平均値を算出する。これら平均値をそれぞれ、長手方向における一端部の金属ニッケル含有量、および長手方向における中央部の金属ニッケル含有量とする。
以上説明したセル10の作製方法の一例について説明する。
図4は、図1に示すセル10の複数個を、集電部材13を介して電気的に直列に接続して構成されたセルスタック装置の一例を示したものであり、(a)はセルスタック装置11を概略的に示す側面図、(b)は(a)のセルスタック装置11の一部拡大断面図であり、(a)で示した破線で囲った部分を抜粋して示している。なお、(b)において(a)で示した破線で囲った部分に対応する部分を明確とするために矢印にて示しており、(b)で示すセル10においては、上述した中間層等の一部の部材を省略して示している。
図5は、セルスタック装置11を収納容器19内に収納してなるモジュール18の一例を示す外観斜視図であり、直方体状の収納容器19の内部に、図4に示したセルスタック装置11を収納して構成されている。
図6は、外装ケース内に図5で示したモジュール18と、セルスタック装置11を動作させるための補機とを収納してなるモジュール収容装置の一例を示す斜視図である。なお、図6においては一部構成を省略して示している。
2:ガス通路
3:燃料極層(第1電極層)
4:固体電解質層
6:酸素極層(第2電極層)
8:インターコネクタ層
10:燃料電池セル
11:セルスタック装置
18:モジュール
23:モジュール収容装置
Claims (8)
- 柱状であり、ニッケルを含有しており、内部に長手方向に沿って貫通するガス通路が設けられ、該ガス通路の出口が設けられた一端部および前記ガス通路の入口が設けられた他端部を有する支持体と、
該支持体上に位置する第1電極層と、
該第1電極層上に位置する固体電解質層と、
該固体電解質層上に位置する第2電極層とを有しており、
前記支持体において、前記一端部は、前記長手方向における中央部よりも金属ニッケル含有量が少ない
ことを特徴とするセル。 - 前記支持体において、前記一端部は、前記長手方向における前記中央部よりも気孔率が低い
ことを特徴とする請求項1に記載のセル。 - 前記ガス通路は、前記一端部における径が前記中央部における径よりも小さい
ことを特徴とする請求項1又は請求項2に記載のセル。 - 前記支持体の表面側における金属ニッケル含有量は、
前記支持体の内部側における金属ニッケル含有量よりも少ない
ことを特徴とする請求項1乃至請求項3のいずれかに記載のセル。 - 前記支持体は、一対の主面を有しており、
前記第1電極層は、前記支持体の少なくとも一方主面上に設けられており、
前記固体電解質層は、前記第1電極層を覆って、前記支持体の前記一方主面から他方主面にかけて設けられており、
前記第2電極層は、前記第1電極層と対向するように前記固体電解質層上に設けられており、
前記固体電解質層の端部は、前記他方主面における短手方向の一端部側に位置しており、
前記支持体の他方主面側において、短手方向における一端部の方が短手方向における中央部よりも金属ニッケル含有量が少ない
ことを特徴とする請求項1乃至請求項4のいずれかに記載のセル。 - 複数配列されており、互いに電気的に接続された請求項1乃至5のうちいずれかに記載されたセルを有する
セルスタック装置。 - 収納容器と、
該収納容器に収納された、請求項6に記載のセルスタック装置と、を有する
モジュール。 - 外装ケースと、
該外装ケース内に収納された、請求項7に記載のモジュールと、
前記外装ケース内に収納されており、前記モジュールの運転を行なうための補機と、を有する
モジュール収容装置。
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US15/327,662 US10014542B2 (en) | 2014-10-29 | 2015-10-28 | Cell, cell stack device, module, and module storage device |
JP2016514175A JP5989941B1 (ja) | 2014-10-29 | 2015-10-28 | セル、セルスタック装置、モジュールおよびモジュール収容装置 |
EP15854632.5A EP3214682B1 (en) | 2014-10-29 | 2015-10-28 | Cell, cell stack device, module, and module storage device |
CN201580038570.2A CN106537674B (zh) | 2014-10-29 | 2015-10-28 | 电池单元、电池堆装置、模块以及模块收容装置 |
KR1020177000317A KR101866852B1 (ko) | 2014-10-29 | 2015-10-28 | 셀, 셀 스택 장치, 모듈 및 모듈 수용 장치 |
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