Electrochemical element, electrochemical module, electrochemical device, and energy system

Abstract

The electrochemical element (Q) has a metal substrate (1) and a plurality of electrochemical reaction sections. The metal substrate (1) has a gas flow-allowing region that allows gas flow between the surface side (4) and the back side (5) of the metal substrate (1). The electrochemical reaction section has at least an electrode layer (A), an electrolyte layer (B), and a counter electrode layer (C), and is disposed on the surface side (4) of the metal substrate (1). The electrolyte layer (B) is disposed between the electrode layer (A) and the counter electrode layer (C), and gas that has flowed through the gas flow-allowing region is supplied to the electrode layer (A).

Description

Technology Field

[0001] The present invention relates to an electrochemical element, an electrochemical module, an electrochemical device, and an energy system. Background Technology

[0002] Conventional solid oxide fuel cells (hereinafter referred to as "SOFCs") are being developed primarily with structures using ceramic materials as support substrates. Additionally, to improve the performance of SOFCs, the development of SOFCs in which multiple generators are arranged side-by-side on a single support substrate is underway.

[0003] Patent Document 1 discloses an SOFC called a "horizontal stripe type" in which, for example, a flat sintered body made of a porous material such as CSZ (calcia-stabilized zirconia), which is a ceramic, is used as a support substrate, and a plurality of laminates (generators) consisting of a fuel electrode, a solid electrolyte membrane, a reaction barrier, and an air electrode are arranged on one of the support substrates. Prior art literature

[0004] Japanese Patent Publication No. 2012-38696 The problem to be solved

[0005] When using expensive and brittle ceramics as a support substrate, it is necessary to significantly increase the thickness of the substrate to achieve a certain level of strength, which leads to high costs and challenges in terms of size and weight. Furthermore, when using a ceramic support substrate, it is difficult to perform fine processing to arrange multiple generators side-by-side on a single substrate, which also presents the challenge of high processing costs.

[0006] The present invention has been made in consideration of the aforementioned problems, and its purpose is to provide an electrochemical device that is compact, high-performance, and has excellent strength and reliability while suppressing material and processing costs. means of solving the problem

[0007] The characteristic configuration of an electrochemical device according to the present invention for achieving the above objective comprises a metal substrate and a plurality of electrochemical reaction units,

[0008] The metal substrate has a gas flow-allowing region that allows gas flow between the surface side and the back side of the metal substrate.

[0009] The above electrochemical reaction unit has at least an electrode layer, an electrolyte layer, and a counter electrode layer, and is disposed on the surface side of the metal substrate, and the electrolyte layer is disposed at least between the electrode layer and the counter electrode layer, and gas that has passed through the gas flow allowance region is supplied to the electrode layer.

[0010] According to the above-described characteristic configuration, since a plurality of electrochemical reaction units are arranged on a metal substrate that has sufficient strength even when thin, it is possible to obtain a compact, high-performance electrochemical device with excellent strength and reliability while suppressing material and processing costs.

[0011] Another characteristic feature of the electrochemical element according to the present invention is that the metal substrate has a plurality of gas flow-allowing regions spaced apart from each other, and the electrolyte layer of the electrochemical reaction part is disposed to cover at least a portion of each of the gas flow-allowing regions or the electrode layer installed in the gas flow-allowing regions.

[0012] According to the characteristic configuration described above, even when a plurality of electrochemical elements are arranged side by side on a metal substrate, gas sealing can be performed by a gastight electrolyte layer, thereby obtaining a compact, high-performance electrochemical element with excellent strength and reliability. That is, since the electrolyte layer is arranged to cover at least each gas flow-allowing area or the electrode layer installed in the gas flow-allowing area, it is possible to suppress the leakage of gas supplied to the electrode layer by passing through the gas flow-allowing area from the back side of the metal substrate to the surface side of the metal substrate, which is desirable as it can improve the performance and reliability of the electrochemical element.

[0013] Another characteristic feature of the electrochemical device according to the present invention is that a metal oxide film is formed on the surface side of the metal substrate, at least in the region where the metal substrate and the electrode layer are in contact.

[0014] According to the above-described characteristic configuration, since the diffusion of components such as Cr from the metal substrate into the electrode layer can be suppressed by the metal oxide film, the degradation of the performance of the electrochemical reaction unit can be suppressed, thereby improving the performance of the electrochemical reaction unit.

[0015] Another characteristic feature of the electrochemical device according to the present invention is that a metal oxide film is formed on the surface side of the metal substrate in an area not covered by at least the electrode layer, the electrolyte layer, or the counter electrode layer.

[0016] According to the above-described characteristic configuration, since the generation of high-resistance components by the evaporation of components such as Cr oxide from the metal substrate and reaction with the counter electrode layer, etc., can be suppressed by the metal oxide film, the degradation of the performance of the electrochemical reaction unit can be suppressed, thereby increasing the performance of the electrochemical reaction unit.

[0017] Another characteristic feature of the electrochemical device according to the present invention is that the metal oxide film is an oxide containing a metal element included in at least the metal substrate.

[0018] According to the above-described characteristic configuration, in the process of forming an electrochemical reaction part such as an electrode layer on a metal substrate, the surface of the metal substrate is oxidized to form a metal oxide film together, so the process of forming a metal oxide film separately can be omitted, and material costs and processing costs can be reduced.

[0019] Another characteristic feature of the electrochemical device according to the present invention is that the metal oxide film is an insulating film.

[0020] According to the characteristic configuration described above, since the metal substrate and the electrode layer are insulated by a film having electrical insulating properties, conduction through the metal substrate between multiple electrochemical reaction units can be suppressed. In particular, when multiple electrochemical reaction units formed on a metal substrate are connected in series, leakage current from the electrochemical reaction units to the metal substrate can be suppressed, thereby improving the performance of the electrochemical reaction units. Furthermore, when multiple electrochemical reaction units formed on a metal substrate are connected in parallel, a conduction path may be separately installed between the metal substrate and the electrode layer.

[0021] Another characteristic feature of the electrochemical device according to the present invention is that the metal substrate contains at least one of Si, Al, and a group 2 to group 7 element.

[0022] According to the characteristic configuration described above, an insulating film containing silica, alumina, or oxides of Group 2 to Group 12 elements can be formed on the surface of a metal substrate by a simple treatment such as heating in air, for example, thereby enabling the production of a low-cost electrochemical device with reduced material and manufacturing costs. Furthermore, for example, if a metal material containing at least one of Si and Al in an amount of about 1% to 5% by weight is used as the material of the metal substrate, it is preferable because an insulating film can be easily formed on its surface by a sintering treatment. Additionally, if a metal material containing at least one of Si and Al in an amount of about 3% to 5% by weight is used, it is even more preferable because an insulating film can be formed on its surface even more easily by a sintering treatment.

[0023] Another characteristic feature of the electrochemical element according to the present invention is that a plurality of the electrochemical reaction units are electrically connected in series.

[0024] According to the above-described characteristic configuration, since a plurality of electrochemical reaction units are electrically connected in series, the structure for electrical connection from the electrochemical element to the outside can be simplified. Furthermore, when the electrochemical reaction units operate as a fuel cell, since they are electrically connected in series, the voltages generated by the electrochemical reaction units can be combined and output from the electrochemical element, which is desirable as it allows the output voltage of a single electrochemical element to be increased.

[0025] In addition, by electrically connecting the electrode layer of one electrochemical reaction unit and the counter electrode layer of another electrochemical reaction unit, a plurality of electrochemical reaction units can be electrically connected in series.

[0026] Another characteristic feature of the electrochemical element according to the present invention is that a plurality of the electrochemical reaction units are electrically connected in parallel.

[0027] According to the above-described characteristic configuration, since a plurality of electrochemical reaction units are electrically connected in parallel, the structure for electrical connection from the electrochemical element to the outside can be simplified. Furthermore, when the electrochemical reaction units operate as a fuel cell, since they are electrically connected in parallel, the currents generated from the electrochemical reaction units can be combined and output from the electrochemical element, which is desirable as it allows the output current of a single electrochemical element to be increased.

[0028] In addition, by electrically connecting the electrode layer of one electrochemical reaction unit and the electrode layer of another electrochemical reaction unit, a plurality of electrochemical reaction units can be electrically connected in parallel.

[0029] The characteristic configuration of the electrochemical module according to the present invention for achieving the above objective is that the aforementioned electrochemical elements are arranged in a plurality of sets.

[0030] According to the above-described characteristic configuration, since the aforementioned electrochemical elements are arranged in a multiple assembly state, it is possible to obtain a compact, high-performance electrochemical module with excellent strength and reliability while suppressing material and processing costs.

[0031] A characteristic configuration of the electrochemical device according to the present invention for achieving the above objective is that it has at least the aforementioned electrochemical module and reformer, and has a fuel supply unit that supplies a fuel gas containing a reducing component to the electrochemical module.

[0032] According to the characteristic configuration described above, since the device has an electrochemical module and a reformer and a fuel supply unit that supplies fuel gas containing reducing components to the electrochemical module, it is possible to utilize existing raw fuel supply infrastructure, such as city gas, and extract power from an electrochemical module with excellent durability, reliability, and performance, thereby realizing an electrochemical device with excellent durability, reliability, and performance. Furthermore, since it is easy to construct a system for recycling unused fuel gas emitted from the electrochemical module, a high-efficiency electrochemical device can be realized.

[0033] Another characteristic feature of the electrochemical device according to the present invention for achieving the above objective is that it has an inverter that extracts power from the electrochemical module.

[0034] According to the above-described characteristic configuration, a high-efficiency electrochemical device for extracting power from an electrochemical module can be realized.

[0035] The characteristic configuration of the energy system according to the present invention for achieving the above objective is that it comprises the aforementioned electrochemical device and a heat exhaust utilization unit that reuses heat discharged from the electrochemical device.

[0036] According to the above-described characteristic configuration, since it comprises an electrochemical device and a heat utilization unit that reuses heat discharged from the electrochemical device, it is possible to realize an energy system with excellent durability, reliability, and performance, as well as excellent energy efficiency. Furthermore, by combining it with a power generation system that generates power using the combustion heat of unused fuel gas discharged from the electrochemical device, it is also possible to realize a hybrid system with excellent energy efficiency. Brief explanation of the drawing

[0037] FIG. 1 is a front view, a cross-sectional view, and a top view showing the stacked structure of an electrochemical device. FIG. 2 is a front view, a cross-sectional view, and a top view showing the stacked structure of an electrochemical device. FIG. 3 is a front view, a cross-sectional view, and a top view showing the stacked structure of an electrochemical device. FIG. 4 is a front view, a cross-sectional view, and a top view showing the stacked structure of an electrochemical device. Figure 5 is a perspective view showing the structure of an electrochemical device. Figure 6 is a perspective view showing the structure of an electrochemical device. Figure 7 is a schematic diagram showing the configuration of the electrochemical module. Figure 8 is a schematic diagram showing the configuration of the electrochemical module. Figure 9 is a schematic diagram showing the configuration of the electrochemical module. Figure 10 is a schematic diagram showing the configuration of an electrochemical device and an energy system. Figure 11 is a cross-sectional view showing the structure of an electrochemical device. Figure 12 is a cross-sectional view showing the structure of an electrochemical device. Figure 13 is a cross-sectional view showing the structure of an electrochemical device. Figure 14 is a cross-sectional view showing the structure of an electrochemical device. Figure 15 is a cross-sectional view showing the structure of an electrochemical device. Figure 16 is a cross-sectional view showing the structure of an electrochemical device. Figure 17 is a cross-sectional view showing the structure of an electrochemical device. Figure 18 is a cross-sectional view showing the structure of an electrochemical device. Figure 19 is a cross-sectional view showing the structure of an electrochemical device. Figure 20 is a cross-sectional view showing the structure of an electrochemical device. Figure 21 is a cross-sectional view showing the structure of an electrochemical device. Figure 22 is a cross-sectional view showing the structure of an electrochemical device. Figure 23 is a cross-sectional view showing the structure of an electrochemical device. Figure 24 is a cross-sectional view showing the structure of an electrochemical device. Figure 25 is a cross-sectional view showing the structure of an electrochemical device. Figure 26 is a cross-sectional view showing the structure of an electrochemical module. FIG. 27 is a front view and a cross-sectional view showing the structure of an electrochemical device. FIG. 28 is a top view showing the structure of an electrochemical device. Figure 29 is a cross-sectional view showing the structure of a metal substrate. Figure 30 is a cross-sectional view showing the structure of an electrochemical device. Specific details for implementing the invention

[0038] <First Embodiment>

[0039] Hereinafter, an electrochemical element according to the first embodiment will be described based on FIG. 1. The electrochemical element (Q) has a metal substrate (1) and a plurality of electrochemical reaction parts (R). The metal substrate (1) has a gas flow allowance region (P) that allows gas flow between the surface side (4) and the back side (5) of the metal substrate (1). The electrochemical reaction part (R) has at least an electrode layer (A), an electrolyte layer (B), and a counter electrode layer (C), and is disposed on the surface side (4) of the metal substrate (1). The electrolyte layer (B) is disposed in a portion between the electrode layer (A) and the counter electrode layer (C), and gas that has flowed through the gas flow allowance region (P) is supplied to the electrode layer (A).

[0040] In this embodiment, five electrochemical reaction sections (R) (first electrochemical reaction section (R1), second electrochemical reaction section (R2), third electrochemical reaction section (R3), fourth electrochemical reaction section (R4) and fifth electrochemical reaction section (R5)) are arranged along the long side of the metal substrate (1) on the surface of a rectangular metal substrate (1).

[0041] In addition, in this embodiment, the electrochemical reaction unit (R) is configured by forming 31 layers on the surface of the metal substrate (1). The first layer in contact with the metal substrate (1) includes an electrode layer (A), an electrolyte layer (B), and an insulating layer (D). The second layer above the first layer includes an electrolyte layer (B), an insulating layer (D), and a conductive layer (E). And, the third layer above the second layer, that is, the uppermost layer, includes a counter electrode layer (C).

[0042] Below, the configuration of the metal substrate (1) and the electrochemical reaction unit (R) is described, and then the arrangement and detailed structure of a plurality of the electrochemical reaction units (R) and the case in which the electrochemical element (Q) operates as a fuel cell are described.

[0043] The top of FIG. 1 is a front view of the electrochemical element (Q) seen from a direction perpendicular to its length direction. The middle of FIG. 1 is a cross-sectional view of the electrochemical element (Q) seen from the same direction as the top. The bottom of FIG. 1 is a top view of the electrochemical element (Q) seen from the surface side (4) of the metal substrate (1). Also, below, the length direction of the rectangular metal substrate (1) may be simply referred to as the "length direction," and the width direction of the rectangular metal substrate (1) may be simply referred to as the "width direction."

[0044] In the bottom top view of FIG. 1, the first layer, the second layer, and a portion of the third layer are removed to explain the layered structure of the electrochemical element (Q). The lines (thick lines) indicating the removal locations of each layer in the bottom top view of FIG. 1 are shown in the top front view of FIG. 1. In detail, from the center of the second electrochemical reaction section (R2) to the center of the third electrochemical reaction section (R3), the upper third layer (charge electrode layer (C)) is removed. From the center of the third electrochemical reaction section (R3) to the center of the fourth electrochemical reaction section (R4), the third layer and the second layer (electrolyte layer (B), insulating layer (D), and conductive layer (E)) are removed. From the center of the fourth electrochemical reaction section (R4) to the center of the fifth electrochemical reaction section (R5), the third layer, the second layer, and the first layer (electrode layer (A), electrolyte layer (B), and insulating layer (D)) are shown in a state where they have been removed.

[0045] Metal substrate

[0046] The metal substrate (1) is a rectangular flat plate made of metal. A plurality of through holes (2) are formed in the metal substrate (1) through the surface side (4) and the back side (5). Through these through holes (2), gas flow is made possible between the surface side (4) and the back side (5) of the metal substrate (1). In this embodiment, the plurality of through holes (2) are formed at the intersection points of a grid parallel to the long side and the short side of the metal substrate (1). Furthermore, the metal substrate (1) must have sufficient strength to form an electrochemical element as a support, and for example, a thickness of about 0.1 mm to 2 mm, preferably about 0.1 mm to 1 mm, and more preferably about 0.1 mm to 0.5 mm can be used. In addition, sintered metal or foamed metal may be used for the metal substrate (1).

[0047] And at positions corresponding to the five electrochemical reaction sections (R), five gas flow allowance areas (P), which are regions where multiple through holes (2) are gathered (first gas flow allowance area (P1), second gas flow allowance area (P2), third gas flow allowance area (P3), fourth gas flow allowance area (P4), fifth gas flow allowance area (P5)), are formed. That is, in this embodiment, the gas flow allowance areas (P) are formed by through holes (2). The five gas flow allowance areas (P) are formed spaced apart from each other in the longitudinal direction. The space between the gas flow allowance areas (P) is a region (gas flow prohibition area) where gas flow is prohibited between the surface side (4) and the back side (5) of the metal substrate (1).

[0048] An insulating film (3) (metal oxide film) is formed on the surface of the metal substrate (1). The insulating film (3) insulates the electrode layer (A) of the electrochemical reaction unit (R) from the metal substrate (1), thereby realizing insulation between adjacent electrode layers (A) of the electrochemical reaction unit (R). Therefore, the insulating film (3) only needs to be formed on at least the surface side of the metal substrate (1), and at least in the area where the metal substrate (1) and the electrode layer (A) come into contact. In this embodiment, the insulating film (3) is formed over the entire surface of the metal substrate (1). In addition, in this embodiment, as described later, a conductive layer (E) is formed adjacent to the first electrochemical reaction unit (R1) for electrical connection between the electrochemical element (Q) and the outside. It is preferable that the insulating film (3) is also formed in the area where the conductive layer (E) and the metal substrate (1) come into contact.

[0049] The resistance value of the insulating film (3) is 1 kΩ·cm 2 It just needs to be at least that level, and 10kΩ·cm 2 If it is above a certain level, it is desirable to be able to secure sufficient electromotive force and current even when the electrochemical element (Q) is operated as a fuel cell.

[0050] The insulating film (3) can be formed by various methods, but a method of oxidizing the surface of the metal substrate (1) to form a metal oxide is preferably used. In addition, when an alloy containing Cr is used as a cell-to-cell connection member of the SOFC, an oxide film is formed on the surface of the cell-to-cell connection member to act as a diffusion barrier to suppress the scattering of Cr. In this case, to reduce the voltage drop in the diffusion barrier, the diffusion barrier is formed as thinly as possible to lower the resistance value. Unlike the diffusion barrier, the insulating film (3) of this embodiment insulates the space between the metal substrate (1) and the electrode layer (A) as described above, and is formed to have a high resistance value in order to insulate the space between the electrode layers (A) of the electrochemical reaction unit (R). Furthermore, since the insulating film (3) is a metal oxide film, it can also have the function of a diffusion barrier (e.g., suppression of Cr scattering).

[0051] In addition, the insulating film (3) may be formed on the surface of the metal substrate (1) by an oxide film containing silica or alumina, oxides of group 2 to group 12 elements, etc., which has high insulating properties, by a sputtering method, a PVD method such as a PLD method, a CVD method, a spray coating method, etc., or by plating and oxidation treatment.

[0052] As the material for the metal substrate (1), a metal material with excellent heat resistance, oxidation resistance, and corrosion resistance is used. For example, ferritic stainless steel, austenitic stainless steel, nickel-based alloys, etc. are used. In particular, an alloy containing chromium is preferably used. For example, in the case of an Fe-Cr alloy material containing about 15% to 25% by weight of Cr, the coefficient of thermal expansion becomes similar to that of the electrode layer (A) or electrolyte layer (B) formed thereon, so an electrochemical device with excellent reliability and durability can be obtained, so it is preferred. In addition, a Cr-rich Cr-Fe alloy containing 70% or more by weight of Cr may be used. In addition, Ni-Cr-Al alloys or Fe-Cr-Al alloys may also be used. In this embodiment, a material containing at least one of Si and Al is preferably used. In this case, by heat-treating the metal substrate (1) under an atmosphere with controlled oxygen partial pressure, an insulating film (3) having an appropriate resistance value can be preferably formed on the surface of the metal substrate (1). For example, if a metal material containing at least one of Si and Al in an amount of about 1% to 5% by weight is used as the material of the metal substrate (1), it is preferable because an insulating film (3) can be easily formed on its surface by sintering treatment. Furthermore, if a metal material containing at least one of Si, Al, and Group 2 to Group 12 elements in an amount of about 3% to 5% by weight is used, it is more preferable because an insulating film (3) can be formed on its surface even more easily by sintering treatment.

[0053] <Tubular Gas Distribution Division>

[0054] In this embodiment, a U-shaped member (11) and a cover portion (12) are joined to a metal substrate (1) to form a tubular gas flow portion (10). The U-shaped member (11) is a member having a U-shaped cross-section perpendicular to the longitudinal direction. The long side of the metal substrate (1) and the long side of the U-shaped member (11) (the side corresponding to the two top points of the U) are joined, and one end of the formed tub is blocked by the cover portion (12). Thus, a tubular gas flow portion (10) in the shape of a flat plate or a flat bar is formed as a whole, having an internal space (22) inside. The metal substrate (1) is arranged parallel to the central axis of the tubular gas flow portion (10).

[0055] A plurality of holes (gas outlets (13)) are formed in the cover portion (12). The end opposite to the cover portion (12) of the tubular gas flow portion (10) is open, thereby forming a gas inlet (21). Thus, when the electrochemical element (Q) is in operation, the gas introduced from the open end of the tubular gas flow portion (10) flows through the internal space (22) of the tubular gas flow portion (10), flows through the gas flow allowance area (P) of the metal substrate (1), reaches the surface side (4), and is supplied to the electrode layer (A). The remaining gas flows out from the gas outlet (13) of the cover portion (12).

[0056] As for the materials of the U-shaped member (11) and the cover part (12), it is preferable to use the same material as the metal substrate (1) so that physical properties such as the coefficient of thermal expansion are uniform throughout the entire cylindrical gas flow section (10). In addition, if ferritic stainless steel is used for the materials of the cylindrical gas flow section (10), including the metal substrate (1), the coefficient of thermal expansion becomes similar to that of YSZ (yttrium stabilized zirconia) or GDC (gadolinium dope ceria, also called CGO) used as materials in the electrochemical reaction section (R). Therefore, even when low and high temperature cycles are repeated, the electrochemical element (Q) is less likely to be damaged. Thus, it is preferable to realize an electrochemical element (Q) with excellent long-term durability.

[0057] And as for the material of the cylindrical gas circulation section (10), a thermal conductivity of 3 Wm -1 K -1 It is desirable to use materials exceeding 10Wm -1 K -1 It is even more desirable if the material exceeds [value]. For example, stainless steel has a thermal conductivity of 15 to 30 Wm -1 K -1 Since it is of that degree, a tubular gas distribution section (10) is preferred as a material.

[0058] In addition, as the material for the cylindrical gas flow section (10), it is more preferable to use a high-toughness material that does not cause brittle fracture. Compared to ceramic materials, metal materials have high toughness, and are preferred as the material for the cylindrical gas flow section (10).

[0059] Furthermore, in the cylindrical gas flow section (10), it is preferable to configure the portion of the metal substrate (1) excluding the gas flow allowance area (P) so that gas cannot flow from the internal space (22) of the cylindrical gas flow section (10) to the outside. For this reason, it is preferable to form the portion of the cylindrical gas flow section (10) excluding the gas flow allowance area (P) with a material that does not allow gas to pass through, such as a crystalline metal. Meanwhile, the gas flow allowance area (P) of the metal substrate (1) may be formed by a porous metal plate, etc., instead of the aforementioned through hole (2).

[0060] Electrochemical reaction unit

[0061] The electrochemical reaction unit (R) according to the present embodiment has an electrode layer (A), an electrolyte layer (B), a counter electrode layer (C), and an intermediate layer.

[0062] Electrode layer

[0063] The electrode layer (A) is formed in the form of a film on the surface of the surface side (4) of the metal substrate (1), that is, on the insulating film (3). The thickness of the film can be, for example, about 1 μm to 100 μm, preferably about 5 μm to 50 μm. By making the film thickness such, it is possible to reduce the amount of expensive electrode layer material used and achieve cost reduction while ensuring sufficient electrode performance.

[0064] As the material for the electrode layer (A), composite materials such as those with NiO-cerium oxide (ceria) as the main component, Ni-cerium oxide (ceria) as the main component, NiO-zirconia as the main component, Ni-zirconia as the main component, CuO-cerium oxide (ceria) as the main component, or Cu-cerium oxide (ceria) as the main component may be used. Furthermore, solid solutions of cerium oxide (ceria), zirconia, etc., or these doped with heterogeneous elements, are referred to as aggregates of the composite material. The electrode layer (A) is formed to have gas permeability. For example, it is configured to have a plurality of fine pores on the surface and inside the electrode layer (A).

[0065] It is preferable that the electrode layer (A) be formed by a low-temperature firing method (for example, a wet method that does not perform firing treatment in a high-temperature region such as 1400°C, but uses firing treatment in a low-temperature region such as 1100°C or lower), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using these processes available in the low-temperature region, a good electrode layer (A) is obtained by processing in a low-temperature region such as 1100°C or lower, without using firing in a high-temperature region such as 1400°C. Because of this, damage to the metal substrate (1) caused by high-temperature heating can be suppressed, and also, elemental interdiffusion caused by high-temperature heating between the metal substrate (1) and the electrode layer (A) can be suppressed, so it is desirable to realize an electrochemical device (Q) with excellent durability.

[0066] Electrolyte layer

[0067] The electrolyte layer (B) is installed in the form of a film between the electrode layer (A) and the counter electrode layer (C). The thickness of the film can be, for example, about 1 μm to 50 μm, preferably about 1 μm to 20 μm, and more preferably about 2 μm to 10 μm. By having such a film thickness, it is possible to reduce the amount of expensive electrolyte layer material used, thereby reducing costs while ensuring sufficient electrolyte performance.

[0068] As the material for the electrolyte layer (B), solid electrolyte materials capable of conducting oxide ions or hydrogen ions, such as various zirconia-based materials, cerium oxide-based materials, and various perovskite-based composite oxides, can be used. In particular, zirconia-based ceramics are preferably used. If the electrolyte layer (B) is made of zirconia-based ceramics, the operating temperature of the electrochemical device (Q) can be made higher than that of ceria-based ceramics, thereby enabling the construction of a highly efficient electrochemical device (Q).

[0069] It is preferable that the electrolyte layer (B) be formed by a low-temperature sintering method (a wet method that does not perform sintering treatment in a high-temperature region such as 1400°C, for example, but uses sintering treatment in a low-temperature region such as 1100°C or lower), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using a film deposition process that is usable in these low-temperature regions, a dense electrolyte layer (B) with high airtightness is obtained by processing in a low-temperature region such as 1100°C or lower, for example, without using sintering in a high-temperature region such as 1400°C. Because of this, damage to the metal substrate (1) caused by high-temperature heating can be suppressed, and elemental interdiffusion caused by high-temperature heating between the metal substrate (1) and the electrode layer (A) can be suppressed, so it is desirable to realize an electrochemical device (Q) with excellent durability.

[0070] The electrolyte layer (B) is densely constructed to maintain airtightness. Furthermore, it is desirable for the electrolyte layer (B) to include a layer with a relative density of 90% or more. It is more desirable to include a layer with a relative density of 95% or more, and even more desirable to include a layer with a relative density of 98% or more. In this way, the electrolyte layer (B) can be made dense by increasing the relative density. Here, relative density refers to the ratio of the density of the actually formed electrolyte layer (B) to the theoretical density of the electrolyte material.

[0071] Daejeon Extreme Layer

[0072] The counter electrode layer (C) is installed in a film form on the electrolyte layer (B). The film thickness can be, for example, about 1 μm to 100 μm, preferably about 5 μm to 50 μm. By making the film thickness such, it is possible to reduce the amount of expensive counter electrode layer material used, thereby reducing costs while ensuring sufficient counter electrode performance.

[0073] As a material for the counter electrode layer (C), composite oxides such as LSCF (La-Sr-Co-Fe-based oxide), LSC (La-Sr-Co-based oxide), LSM (La-Sr-Mn-based oxide), SSC (Sm-Sr-Co-based oxide), and SDC (Ce-Sm-based oxide) may be used. Furthermore, it is preferable to form the counter electrode layer (C) by a low-temperature sintering method (a wet method that does not perform sintering treatment in a high-temperature region such as 1400°C, for example, but uses sintering treatment in a low-temperature region such as 1100°C or lower), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using these processes that are usable in a low-temperature region, a good counter electrode layer (C) is obtained by processing in a low-temperature region such as 1100°C or lower, for example, without using sintering in a high-temperature region such as 1400°C. For this reason, damage caused by high-temperature heating to the metal substrate (1) can be suppressed, and also, the interdiffusion of elements caused by high-temperature heating between the metal substrate (1) and the electrode layer (A) can be suppressed, so it is desirable to realize an electrochemical device (Q) with excellent durability.

[0074] Middle layer

[0075] Additionally, an intermediate layer may be formed in the form of a film between the electrode layer (A) and the electrolyte layer (B). The thickness of the film may be, for example, about 1 μm to 100 μm, preferably about 2 μm to 50 μm, and more preferably about 5 μm to 20 μm. By having such a film thickness, it becomes possible to reduce the amount of expensive intermediate layer material used, thereby reducing costs while ensuring sufficient intermediate layer performance.

[0076] As the material for the intermediate layer, for example, cerium oxide-based materials or zirconia-based materials can be used. By introducing the intermediate layer between the electrode layer (A) and the electrolyte layer (B), the performance, reliability, and durability of the electrochemical reaction part (R) can be improved. Furthermore, it is preferable to form the intermediate layer by a low-temperature sintering method (for example, a wet method that uses sintering treatment in a low-temperature region of, for example, 1100°C or lower, without performing sintering treatment in a high-temperature region such as 1400°C), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using these processes that are usable in the low-temperature region, a good intermediate layer is obtained by processing in a low-temperature region of, for example, 1100°C or lower, without using sintering in a high-temperature region such as 1400°C. For this reason, damage caused by high-temperature heating to the metal substrate (1) can be suppressed, and also, the interdiffusion of elements caused by high-temperature heating between the metal substrate (1) and the electrode layer (A) can be suppressed, so it is desirable to realize an electrochemical device (Q) with excellent durability.

[0077] In addition, an intermediate layer may be formed in the form of a film between the electrolyte layer (B) and the counter electrode layer (C). The thickness of the film can be, for example, about 1 μm to 100 μm, preferably about 2 μm to 50 μm, and more preferably about 5 μm to 20 μm. By having such a film thickness, it is possible to reduce the amount of expensive intermediate layer material used, thereby reducing costs while ensuring sufficient intermediate layer performance.

[0078] For the intermediate layer material, for example, cerium oxide-based materials or zirconia-based materials can be used. By introducing the intermediate layer between the electrolyte layer (B) and the counter electrode layer (C), the reaction between the constituent material of the counter electrode layer (C) and the constituent material of the electrolyte layer (B) is effectively suppressed, thereby improving the long-term stability of the performance of the electrochemical reaction part (R). Furthermore, it is preferable to form the intermediate layer by a low-temperature sintering method (for example, a wet method that uses sintering treatment in a low-temperature region of about 1100°C or lower, for example, without performing sintering treatment in a high-temperature region such as 1400°C), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using these processes that are usable in the low-temperature region, a good intermediate layer is obtained by processing in a low-temperature region of about 1100°C or lower, for example, without using sintering in a high-temperature region such as 1400°C. For this reason, damage caused by high-temperature heating to the metal substrate (1) can be suppressed, and also, the interdiffusion of elements caused by high-temperature heating between the metal substrate (1) and the electrode layer (A) can be suppressed, so it is desirable to realize an electrochemical device (Q) with excellent durability.

[0079] The intermediate layer described above can be installed on only one side or on both sides. That is, a configuration in which the electrode layer (A), electrolyte layer (B), intermediate layer, and counter electrode layer (C) are stacked in this order is also possible. A configuration in which the electrode layer (A), intermediate layer, electrolyte layer (B), and counter electrode layer (C) are stacked in this order is also possible. A configuration in which the electrode layer (A), intermediate layer, electrolyte layer (B), intermediate layer, and counter electrode layer (C) are stacked in this order is also possible.

[0080] <Electrochemical reaction in the electrochemical reaction section (R)>

[0081] The electrochemical reaction unit (R) configured as described above receives a supply of gas and generates an electrochemical reaction.

[0082] In the case where the electrochemical reaction unit (R) operates as a fuel cell and an oxide ion conductor is used as the electrolyte, for example, a fuel containing hydrogen gas is supplied to the electrode layer (A), and a gas containing oxygen is supplied to the counter electrode layer (C). In this case, oxygen molecules (O2) in the counter electrode layer (C) electrons (e - Reacts with ) to produce oxygen ions (oxide ions) (O 2- ) is generated. This oxygen ion (O 2- ) moves to the electrode layer (A) through the electrolyte layer (B). In the electrode layer (A), hydrogen molecules (H2) and oxygen ions (O 2- Reacts with ), water (H2O) and electrons (e - ) is generated. When a hydrogen ion conductor is used as the electrolyte, in the electrode layer (A), hydrogen molecules (H2) electrons (e - ) emits protons (hydrogen ions) (H + ) is generated. That hydrogen ion (H + ) moves to the counter electrode layer (C) through the electrolyte layer (B). In the counter electrode layer (C), oxygen molecules (O2) become hydrogen ions (H + Reacting with ), electrons (e - Water (H2O) is produced by consuming ).

[0083] Due to the above reaction, an electromotive force is generated between the electrode layer (A) and the charged electrode layer (C), and power generation is performed.

[0084] In the case where the electrochemical reaction unit (R) operates as an electrolytic cell, and an oxide ion conductor is used as the electrolyte, when a voltage is applied between the electrode layer (A) and the counter electrode layer (C), water molecules (H2O) in the electrode layer (A) electrons (e - ) receives hydrogen molecules (H2) and oxygen ions (oxide ions) (O 2- Generates ) oxygen ions (O 2- ) moves to the charged electrode layer (C) through the electrolyte layer (B). In the charged electrode layer (C), oxygen ions (O 2-) emits electrons to become oxygen molecules (O2). When a hydrogen ion conductor is used as an electrolyte, oxygen molecules (O2) and hydrogen ions (H) are formed from water (H2O) in the counter electrode layer (C). + ) generates and electrons (e - Releases hydrogen ions (H + ) moves to the electrode layer (A) through the electrolyte layer (B), and in the electrode layer (A), hydrogen ions (H + ) electron(e - It reacts with ) to produce hydrogen molecules (H2).

[0085] Through the above reaction, water molecules (H2O) are electrolyzed into hydrogen (H2) and oxygen (O2).

[0086] Electrical connections of the electrochemical reaction section

[0087] In the following description, the electrode layer (A), electrolyte layer (B), and counter electrode layer (C) of the first electrochemical reaction unit (R1) are referred to as the first electrode layer (A1), the first electrolyte layer (B1), and the first counter electrode layer (C1). The electrode layer (A), electrolyte layer (B), and counter electrode layer (C) of the second electrochemical reaction unit (R2) are referred to as the second electrode layer (A2), the second electrolyte layer (B2), and the second counter electrode layer (C2). The same applies to the third and subsequent electrochemical reaction units (R).

[0088] In this embodiment, a plurality of electrochemical reaction units (R) are electrically connected in series. Additionally, the electrode layer (A) of one electrochemical reaction unit (R) and the counter electrode layer (C) of another electrochemical reaction unit (R) are electrically connected.

[0089] Based on the cross-sectional view of the middle section of FIG. 1, the connection between the first electrochemical reaction unit (R1) and the second electrochemical reaction unit (R2) is described. In the first and second layers, an insulating layer (D) and a conductive layer (E) are formed between the first electrochemical reaction unit (R1) and the second electrochemical reaction unit (R2). Through these insulating layer (D) and conductive layer (E), a series connection between the first electrochemical reaction unit (R1) and the second electrochemical reaction unit (R2) is realized.

[0090] The insulating layer (D) can be composed of, for example, an insulating metal oxide such as alumina. In this embodiment, the insulating layer (D) is formed densely and in a gastight state that suppresses gas permeability.

[0091] The conductive layer (E), also called an interconnect, can be composed of a conductive metal oxide such as, for example, LaCrO3 (lanthanum chromite) or SrTiO3 (strontium titanate). In this embodiment, the conductive layer (E) is formed densely and in a gastight state that suppresses gas permeability.

[0092] In the first layer, an insulating layer (D) is formed between the first electrode layer (A1) and the second electrode layer (A2). In the second layer, an insulating layer (D) and a conductive layer (E) are formed between the first electrolyte layer (B1) and the second electrolyte layer (B2). The insulating layer (D) of the second layer is formed across both the insulating layer of the first layer and the first electrode layer (A1). The conductive layer (E) is formed across both the insulating layer of the first layer and the second electrode layer (A2). In the third layer, the first counter electrode layer (C1) is formed extending from above the first electrolyte layer (B1), beyond the insulating layer (D) of the second layer, to the conductive layer (E). That is, the conductive layer (E) of the second layer is in contact with both the first counter electrode layer (C1) and the second electrode layer (A2) and is electrically connected.

[0093] With the above configuration, the first electrode layer (A1) and the second electrode layer (A2) are insulated from each other by the presence of an insulating layer (D). And the first counter electrode layer (C1) and the second electrode layer (A2) are electrically connected by the presence of a conductive layer (E).

[0094] When the electrochemical reaction unit (R) operates as a fuel cell, an electromotive force is generated between the electrode layer (A) and the counter electrode layer (C), as described above. In this case, because the first counter electrode layer (C1) and the second electrode layer (A2) are electrically connected, an electromotive force is generated between the first electrode layer (A1) and the second counter electrode layer (C2) by combining the electromotive force of the first electrochemical reaction unit (R1) and the electromotive force of the second electrochemical reaction unit (R2). That is, in this case, it can be said that the first electrochemical reaction unit (R1) and the second electrochemical reaction unit (R2) are electrically connected in series.

[0095] As shown in the cross-sectional view of FIG. 1, the second counter electrode layer (C2) and the third electrode layer (A3) are also connected by a conductive layer (E). The third counter electrode layer (C3) and the fourth electrode layer (A4) are also connected by a conductive layer (E). The fourth counter electrode layer (C4) and the fifth electrode layer (A5) are also connected by a conductive layer (E). That is, each electrochemical reaction section (R) from the second electrochemical reaction section (R2) to the fifth electrochemical reaction section (R5) is also electrically connected in series in the same way.

[0096] At both ends of the electrochemical reaction unit (R) electrically connected in series, a configuration for electrically connecting to the outside of the electrochemical element (Q) is arranged. In this embodiment, a current collecting member (26) is connected to the fifth electrode layer (C5) of the fifth electrochemical reaction unit (R5). Then, a conductive layer (E) is connected to the first electrode layer (A1) of the first electrochemical reaction unit (R1), and a current collecting member (26) is connected on the conductive layer (E).

[0097] For the current collector (26), a material having conductivity and gas permeability is used. For example, an expanded metal or metal mesh made of a metal foil with an oxidation-resistant coating, or a felt-like material is used.

[0098] When the electrochemical element (Q) configured as described above is operated as a fuel cell, an electromotive force is generated between the current collecting members (26) at both ends. Then, when the current collecting members (26) are connected to an external load, as shown in the cross-sectional view of FIG. 1, current flows from the current collecting member (26) on the side of the first electrochemical reaction unit (R1) toward the current collecting member (26) of the fifth electrochemical reaction unit (R5), as indicated by arrow I. That is, five fuel cells (electrochemical reaction units (R)) connected in series supply power to the outside.

[0099] And when the electrochemical element (Q) according to the present embodiment is operated as the electrolytic cell described above, a voltage is applied between a pair of current collecting members (26). In this case, since the electrode layer (A) and the counter electrode layer (C) of each electrochemical reaction unit (R) are connected as described above, a voltage is applied to each electrochemical reaction unit (R), and an electrolytic reaction proceeds. That is, in this case as well, it can be seen that five electrolytic cells are connected in series and operated, so the electrochemical reaction units (R) can be said to be electrically connected in series.

[0100] Third Electrolyte of Gas in Electrochemical Devices

[0101] In the electrochemical element (Q), gas that has flowed through the gas flow allowance region (P) of the metal substrate (1) is supplied to the electrode layer (A), but it is necessary to prevent the gas from leaking to the counter electrode layer (C). To this end, the electrochemical element (Q) according to the present embodiment has the following structure for making the gas into a third electrolyte.

[0102] In this embodiment, the first electrode layer (A1) is formed to cover the first gas flow allowance area (P1). Likewise, the other second electrode layer (A2) to the fifth electrode layer (A5) are each formed to cover the second gas flow allowance area (P2) to the fifth gas flow allowance area (P5). That is, the electrode layer (A) is installed to cover the gas flow allowance area (P) in an area larger than the gas flow allowance area (P). In this case, if the electrode layer (A) is covered with a gastight layer, gas leakage can be suppressed.

[0103] The following description focuses on the third electrochemical reaction section (R3). The third electrode layer (A3) is covered by the third electrolyte layer (B3), the insulating layer (D), and the conductive layer (E). The third electrolyte layer (B3) is positioned to cover the third electrode layer (A3) installed in at least the third gas flow allowance area (P3).

[0104] In detail, the third electrolyte layer (B3) is formed over a wider width than the third electrode layer (A3) in the width direction. The third electrode layer (A3) is placed above the third electrode layer (A3), i.e., in the second layer, in the region where the third electrode layer (A3) exists. In the region where the third electrode layer (A3) does not exist (regions on both sides in the width direction of the third electrode layer (A3)), the third electrolyte layer (B3) is placed above the metal substrate (1), i.e., in the first layer. The third electrolyte layer (B3) of the first layer and the third electrolyte layer (B3) of the second layer are formed as a continuous layer, and gas leakage from the connection portion between the two is suppressed.

[0105] Both ends in the longitudinal direction of the third electrode layer (A3) are covered by an insulating layer (D) and a conductive layer (E). The insulating layer (D) and the conductive layer (E) of the second layer are extended in a long, narrow manner in the width direction, and in the area where the third electrode layer (A3) does not exist (areas on both sides in the width direction of the third electrode layer (A3)), they are respectively connected to the insulating layer (D) and the conductive layer (E) of the first layer. The insulating layer (D) of the first layer and the insulating layer (D) of the second layer, and the conductive layer (E) of the first layer and the conductive layer (E) of the second layer are formed as continuous layers, and gas leakage from the connection portion between the two is suppressed.

[0106] As explained above, the third electrode layer (A3) is covered by the third electrolyte layer (B3), the insulating layer (D), and the conductive layer (E). Since the electrolyte layer (B), the insulating layer (D), and the conductive layer (E) are all gastight layers with low gas permeability, the leakage of gas supplied to the third electrode layer (A3) to the counter electrode layer (C) side is suppressed by the above configuration.

[0107] Although the above explanation focused on the third electrochemical reaction section (R3), the same applies to the second electrochemical reaction section (R2), the fourth electrochemical reaction section (R4), and the fifth electrochemical reaction section (R5). Furthermore, regarding the first electrochemical reaction section (R1), one side in the longitudinal direction is covered only by a conductive layer (E), but gas leakage is similarly suppressed.

[0108] The structure of the electrochemical reaction unit (R) according to the above-described embodiment can be formed as follows. First, the first electrode layer (A), insulating layer (D), and conductive layer (E) are formed on the metal substrate (1) in a planar shape as shown in the top view at the bottom of FIG. 1. Next, the second electrolyte layer (B), insulating layer (D), and conductive layer (E) are formed on the metal substrate (1) and the first layer in a planar shape as shown in the top view at the bottom of FIG. 1, that is, with a width wider in the width direction than the first layer. Thus, the electrode layer (A) is covered by the electrolyte layer (B), insulating layer (D), and conductive layer (E). Then, the third electrode layer (C) is formed on the second layer.

[0109] <Second Embodiment>

[0110] An electrochemical element (Q) according to a second embodiment is shown in FIG. 2. In the following second to tenth embodiments and other embodiments, the same reference numerals are used for components identical to those in the first embodiment, and descriptions may be omitted.

[0111] In this electrochemical element (Q), through holes (2) are formed continuously along the longitudinal direction of the metal substrate (1). That is, the gas flow-allowing region (P) is formed as a single continuous region. Also, in this embodiment, the electrode layer (A) installed in the gas flow-allowing region (P) is covered by an electrolyte layer (B), an insulating layer (D), and a conductive layer (E). Therefore, the leakage of gas supplied to the electrode layer (A) toward the charged electrode layer (C) is suppressed.

[0112] <Third Embodiment>

[0113] An electrochemical element (Q) according to a third embodiment is shown in FIG. 3. In this embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0114] At least in the portion of the surface of the metal substrate (1) that is in contact with the electrode layer (A), a diffusion barrier film (6) (metal oxide film) is formed instead of an insulating film. The diffusion barrier film (6) is installed to suppress scattering of Cr from the metal substrate (1). Unlike the insulating film, the diffusion barrier film (6) has conductivity and is configured to have a low resistance value so as not to suppress the conduction between the electrode layer (A) of the electrochemical reaction unit (R) and the metal substrate (1).

[0115] And, the metal oxide film covering the region of the surface of the metal substrate (1) that is not covered by the electrode layer, the electrolyte layer, or the counter electrode layer may have the function of suppressing the evaporation of components such as Cr oxide from the metal substrate (1), and may be an insulating film or a conductive diffusion barrier film.

[0116] The resistance value of the diffusion barrier (6) is 0.1Ω·cm 2 It should be approximately 0.05Ω·cm or less. 2 If the amount is less than that, it is desirable because sufficient electromotive force and current can be secured even when the electrochemical element (Q) is operated as a fuel cell.

[0117] As the material for the metal substrate (1), a metal material with excellent heat resistance, oxidation resistance, and corrosion resistance is used. For example, ferritic stainless steel, austenitic stainless steel, nickel-based alloys, etc. are used. In particular, an alloy containing chromium is preferably used. For example, in the case of an Fe-Cr alloy material containing about 15% to 25% by weight of Cr, the coefficient of thermal expansion becomes similar to that of the electrode layer (A) or electrolyte layer (B) formed thereon, and an electrochemical device with excellent reliability and durability can be obtained, so it is preferred. In addition, a Cr-rich Cr-Fe alloy containing 70% or more by weight of Cr may be used. In addition, Ni-Cr-Al alloys or Fe-Cr-Al alloys may also be used. The diffusion barrier film (6) can be formed by various methods, but a method of oxidizing the surface of the metal substrate (1) to form a metal oxide is preferably used. In that case, a diffusion barrier film (6) having an appropriate thickness and resistance value can be preferably formed on the surface of the metal substrate (1) by heat-treating the metal substrate (1) under an atmosphere in which the oxygen partial pressure is controlled to be low, or under an inert gas or hydrogen atmosphere. In particular, if an Fe-Cr alloy material containing about 15% to 25% by weight of Cr is used on the metal substrate (1), it is preferable to form a diffusion barrier film mainly composed of chromium oxide on its surface by sintering treatment. In addition, the diffusion barrier film (6) may be formed on the surface of the metal substrate (1) by a PVD method such as sputtering or PLD, a CVD method, a spray coating method, etc., or may be formed by plating and oxidation treatment. In addition, the diffusion barrier film (6) may include a spinel phase with high conductivity.

[0118] In this embodiment, similar to the first embodiment, five gas flow allowance regions (P) (first gas flow allowance region (P1) to fifth gas flow allowance region (P5)) are formed spaced apart from each other on a metal substrate (1). Additionally, five electrochemical reaction sections (R) (first electrochemical reaction section (R1) to fifth electrochemical reaction section (R5)) are formed spaced apart from each other.

[0119] In detail, first, five electrode layers (A) (first electrode layer (A1) to fifth electrode layer (A5)) are formed to cover each gas flow allowance area (P) in an area larger than each gas flow allowance area (P). The five electrode layers (A) are formed spaced apart from each other. Then, five electrolyte layers (B) (first electrolyte layer (B1) to fifth electrolyte layer (B5)) are formed to cover each electrode layer (A) in an area larger than each electrode layer (A). The five electrolyte layers (B) are formed spaced apart from each other. Five counter electrode layers (C) (first counter electrode layer (C1) to fifth counter electrode layer (C5)) are formed on each electrolyte layer (B).

[0120] Each gas flow-allowing region (P) is covered by an electrode layer (A), and each electrode layer (A) is covered by an electrolyte layer (B), thereby preventing the gas supplied from the gas flow-allowing region (P) to the electrode layer (A) from leaking to the counter electrode layer (C). That is, in this embodiment, the metal substrate (1) has a plurality of gas flow-allowing regions (P) spaced apart from each other, and the electrolyte layer (B) of the electrochemical reaction unit (R) is arranged to cover the electrode layer (A) installed in each gas flow-allowing region (P).

[0121] In this embodiment, as described above, a conductive diffusion barrier film (6) is formed on the surface of the metal substrate (1). Accordingly, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through the metal substrate (1). In the first and second embodiments, the electrode layer (A) and the counter electrode layer (C) of adjacent electrochemical reaction units (R) are electrically connected, so that the electrochemical reaction units (R) are connected in series. In this embodiment, the electrode layer (A) of adjacent electrochemical reaction units (R) is electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R).

[0122] When the electrochemical element (Q) according to the present embodiment is operated as a fuel cell, hydrogen that has flowed through the gas flow allowance region (P) is supplied to the electrode layer (A), oxygen is supplied to the counter electrode layer (C), and an electromotive force is generated between the electrode layer (A) and the counter electrode layer (C). Since the first electrode layer (A1) to the fifth electrode layer (A5) are electrically connected by the metal substrate (1), they have the same potential. Then, a current collection member (not shown) mounted on the first counter electrode layer (C1) to the fifth counter electrode layer (C5) and the metal substrate (1) (or tubular gas flow section (10)) are connected to the outside, and electromotive force and current are extracted to the outside. That is, five fuel cells (electrochemical reaction section (R)) connected in parallel supply power to the outside.

[0123] When the electrochemical element (Q) according to the present embodiment is operated as an electrolytic cell, water (water vapor) that has flowed through the gas flow allowance region (P) is supplied to the electrode layer (A), and a voltage is applied between the current collection member (not shown) mounted on the first electrode layer (C1) to the fifth electrode layer (C5) and the metal substrate (1) (or tubular gas flow section (10)). In this way, since the first electrode layer (A1) to the fifth electrode layer (A5) are electrically connected by the metal substrate (1), a voltage is applied to each electrochemical reaction section (R), and an electrolytic reaction proceeds. That is, in this case as well, it can be seen that five electrolytic cells are connected in parallel and operated, so the electrochemical reaction section (R) can be said to be electrically connected in parallel.

[0124] <Fourth Embodiment>

[0125] An electrochemical element (Q) according to a fourth embodiment is shown in FIG. 4. In this electrochemical element (Q), as in the second embodiment, through holes (2) are formed continuously along the longitudinal direction of the metal substrate (1). That is, the gas flow-allowing region (P) is formed as a single continuous region. A diffusion barrier film (6) is formed on the surface of the metal substrate (1).

[0126] Five electrode layers (A) (first electrode layer (A1) to fifth electrode layer (A5)) are formed on the surface side (4) of the metal substrate (1). The five electrode layers (A) are formed spaced apart from each other. On top of this, an electrolyte layer (B) is formed over an area larger than the gas flow allowance area (P), covering the gas flow allowance area (P). In this embodiment, the electrolyte layer (B) is formed as a single continuous layer, extending across the first and second layers and covering almost the entire surface side (4) of the metal substrate (1). The five electrode layers (A) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed. And, five counter electrode layers (C) (first counter electrode layer (C1) to fifth counter electrode layer (C5)) are formed in the region corresponding to the electrode layer (A) on the electrolyte layer (B).

[0127] Since five electrode layers (A) and five counter electrode layers (C) are formed spaced apart from each other, an electrochemical reaction can occur between the opposing electrode layers (A) and counter electrode layers (C) and the electrolyte layer (B) that is clamped by them. That is, a first electrochemical reaction section (R1) is formed by the first electrode layer (A1), the first counter electrode layer (C1), and the first electrolyte layer (B1) that is clamped by them. Similarly, a second electrochemical reaction section (R2) to a fifth electrochemical reaction section (R5) is formed by the second electrode layer (A2) to the fifth electrode layer (A5), the second counter electrode layer (C2) to the fifth counter electrode layer (C5), and the second electrolyte layer (B2) to the fifth electrolyte layer (B5) that is clamped by them. That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0128] And, similar to the third embodiment, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through a metal substrate (1). Therefore, it can be said that a plurality of electrochemical reaction units (R) are electrically connected in parallel.

[0129] <Fifth Embodiment>

[0130] In the above-described embodiment, a plurality of electrochemical reaction units (R) were installed in a single row along the length direction of a rectangular metal substrate (1). It is also possible to modify this to form a plurality of electrochemical reaction units (R) arranged in a plurality of rows.

[0131] An electrochemical element (Q) according to the fifth embodiment is shown in FIG. 5. In this embodiment, an example is shown in which five electrochemical reaction units (R) are arranged side by side in two rows on a metal substrate (1). For details, in the row immediately in front of FIG. 5, a current collector (26), a conductive layer (E), a first electrochemical reaction unit (R1), and a second electrochemical reaction unit (R2) are arranged in this order, and in the inner row of FIG. 5, a fifth electrochemical reaction unit (R5), a fourth electrochemical reaction unit (R4), and a third electrochemical reaction unit (R3) are arranged in this order.

[0132] An insulating film (3) (metal oxide film) is formed on the surface of the metal substrate (1). Although not shown in the illustration, a plurality of through holes (2) are formed in the metal substrate (1) that penetrate the surface side (4) and the back side (5), and five gas flow allowance regions (P), which are areas where the plurality of through holes (2) are gathered, are formed at positions corresponding to five electrochemical reaction parts (R). Also, as in the second embodiment, it is possible to form gas flow allowance regions (P) over the entire metal substrate (1). However, in such a case, the gas flow allowance regions (P) are formed to be received inside the area where the conductive layer (E) and the electrolyte layer (B) are formed, and it is necessary to suppress the leakage of gas from the back side (5) of the metal substrate (1) to the side of the counter electrode layer (C) (the surface side (4) of the metal substrate (1)).

[0133] Also, while FIG. 5 shows a metal substrate (1) and an electrochemical reaction section (R), it is also possible to form a tubular gas flow section (10) by mounting a U-shaped member (11) and a cover section (12) on the metal substrate (1), just like in the first embodiment.

[0134] In this embodiment, similar to the first and second embodiments, the first electrochemical reaction unit (R1) to the fifth electrochemical reaction unit (R5) are electrically connected in series and connected to a pair of current collectors (26). That is, the electrode layer (A) of one electrochemical reaction unit (R) and the counter electrode layer (C) of another electrochemical reaction unit (R) are electrically connected. The structure of each electrochemical reaction unit (R), that is, the arrangement and positional relationship of the electrode layer (A), electrolyte layer (B), counter electrode layer (C), insulating layer (D), and conductive layer (E), is formed in the same way as in the first embodiment.

[0135] <6th Embodiment>

[0136] An electrochemical element (Q) according to the sixth embodiment is shown in FIG. 6. In this embodiment, an example is shown in which four electrochemical reaction units (R) are arranged side by side in two rows on a metal substrate (1). For details, the first electrochemical reaction unit (R1) and the second electrochemical reaction unit (R2) are arranged in this order in the front row of FIG. 6, and the fourth electrochemical reaction unit (R4) and the third electrochemical reaction unit (R3) are arranged in this order in the inner row of FIG. 6.

[0137] A diffusion barrier film (6) (metal oxide film) is formed on the surface of the metal substrate (1). Although not shown in the illustration, a plurality of through holes (2) are formed in the metal substrate (1) through the surface side (4) and the back side (5), and four gas flow allowance regions (P), which are areas where the plurality of through holes (2) are gathered, are formed at positions corresponding to four electrochemical reaction parts (R). Also, as in the fourth embodiment, it is possible to form gas flow allowance regions (P) over the entire metal substrate (1). However, in such a case, the gas flow allowance regions (P) are formed to be received inside the area formed by the conductive layer (E) and the electrolyte layer (B), and it is necessary to suppress the leakage of gas from the back side (5) of the metal substrate (1) to the side of the counter electrode layer (C) (the surface side (4) of the metal substrate (1)).

[0138] In this embodiment, the first electrochemical reaction unit (R1) to the fourth electrochemical reaction unit (R4) are electrically connected in parallel, just as in the third or fourth embodiment. That is, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected. The structure of each electrochemical reaction unit (R), that is, the arrangement and positional relationship of the electrode layer (A), electrolyte layer (B), and counter electrode layer (C), is formed in the same way as in the fourth embodiment.

[0139] Also, while FIG. 6 shows a metal substrate (1) and an electrochemical reaction section (R), it is also possible to form a tubular gas flow section (10) by mounting a U-shaped member (11) and a cover section (12) on the metal substrate (1), just like in the first embodiment.

[0140] <Seventh Embodiment>

[0141] FIG. 7 shows the configuration of an electrochemical module (M). The electrochemical module (M) is a module in which the aforementioned electrochemical elements (Q) are arranged in a stacked state. In the electrochemical module (M) according to the seventh embodiment, an electrochemical element (Q) in which a plurality of electrochemical reaction parts (R) are electrically connected in series, that is, an electrochemical element (Q) according to the first, second, and fifth embodiments is used.

[0142] The electrochemical module (M) has a gas manifold (17) and five electrochemical elements (Q). The electrochemical elements (Q) are connected to the gas manifold (17) such that the gas inlet (21) of the tubular gas flow section (10) of the electrochemical elements (Q) communicates with the internal space of the gas manifold (17). In this embodiment, five electrochemical elements (Q) are stacked with the electrochemical reaction section (R) facing one side (right side of FIG. 7) and mounted on the gas manifold (17).

[0143] In this embodiment, an electrochemical element (Q) is used in which a plurality of electrochemical reaction units (R) are electrically connected in series, and the electrochemical reaction units (R) and the metal substrate (1), that is, the tubular gas flow unit (10), are insulated from each other. Therefore, when mounting the tubular gas flow unit (10) to the gas manifold (17), there is no need to perform insulation, so mounting can be performed by a simple and robust method such as welding.

[0144] The electrochemical elements (Q) of the electrochemical module (M) are electrically connected to each other. In this embodiment, the current collector (26) connected to the first electrochemical reaction unit (R1) of each electrochemical element (Q) is electrically connected to each other and connected to the outside. Then, the current collector (26) connected to the fifth electrochemical reaction unit (R5) of each electrochemical element (Q) is electrically connected to each other and connected to the outside. By being connected as described above, five electrochemical reaction units (R) connected in series are connected in parallel in five sets.

[0145] When operating the electrochemical module (M) as a fuel cell, hydrogen is supplied to the inside of the gas manifold (17) and oxygen is supplied around the electrochemical element (Q). In this way, a reaction as a fuel cell proceeds in each electrochemical reaction section (R), and an electromotive force and current are generated. The generated power is extracted to the outside of the electrochemical module (M) from the current collector (26).

[0146] <8th Embodiment>

[0147] FIG. 8 shows another embodiment of the electrochemical module (M). In the electrochemical module (M) according to the eighth embodiment, an electrochemical element (Q) is used in which a plurality of electrochemical reaction units (R) are electrically connected in parallel, i.e., the electrochemical element (Q) according to the third, fourth, and sixth embodiments.

[0148] Similar to the seventh embodiment, the electrochemical element (Q) is connected to the gas manifold (17) so that the gas inlet (21) of the tubular gas flow section (10) of the electrochemical element (Q) communicates with the internal space of the gas manifold (17). In this embodiment, five electrochemical elements (Q) are stacked with the electrochemical reaction section (R) facing one side (right side of FIG. 7) and mounted on the gas manifold (17). Then, a current collector (26) is placed between the electrochemical elements (Q) and electrically connects the electrochemical reaction section (R) to the back side (14) of the tubular gas flow section (10) of the electrochemical element (Q). Thus, five sets of electrochemical reaction sections (R) connected in parallel are connected in series.

[0149] When operating the electrochemical module (M) as a fuel cell, hydrogen is supplied to the inside of the gas manifold (17) and oxygen is supplied around the electrochemical element (Q). In this way, a reaction as a fuel cell proceeds in each electrochemical reaction section (R), and an electromotive force and current are generated. The generated power is extracted from both ends of the stacked electrochemical element (Q). That is, the generated power is drawn out to the outside of the electrochemical module (M) from the back surface (14) of the tubular gas flow section (10) of the first electrochemical reaction section (R1) and the current collection member (26) of the fifth electrochemical reaction section (R5).

[0150] In addition, in this embodiment, an electrochemical element (Q) is used in which a plurality of electrochemical reaction units (R) are electrically connected in parallel, so the electrochemical reaction unit (R) and the metal substrate (1), i.e., the tubular gas flow unit (10), are not insulated and are in a conductive state. Therefore, when mounting the tubular gas flow unit (10) to the gas manifold (17), it is necessary to insulate the tubular gas flow unit (10) and the gas manifold (17). For example, the tubular gas flow unit (10) and the gas manifold (17) are joined by a glass sealing material.

[0151] <Ninth Embodiment>

[0152] FIG. 9 illustrates another embodiment of an electrochemical module (M). In the electrochemical module (M) according to the ninth embodiment, an electrochemical element (Q) according to the sixth embodiment shown in FIG. 6, that is, an electrochemical element (Q) in which a plurality of electrochemical reaction units (R) are electrically connected in parallel, may preferably be used. The electrochemical module (M) is constructed by stacking the electrochemical element (Q) with a cell-to-cell connection member (71) in between.

[0153] The inter-cell connecting member (71) is a plate-shaped member that is conductive and at the same time non-gas permeable, and has grooves (72) formed on the surface and the back surface that are orthogonal to each other. The inter-cell connecting member (71) can be made of a metal such as stainless steel or a metal oxide.

[0154] As shown in FIG. 9, when an electrochemical element (Q) is stacked with the cell-to-cell connecting member (71) in between, gas can be supplied to the electrochemical element (Q) through the groove (72). In detail, one groove (72) becomes the first gas flow path (72a) and supplies gas to the surface side of the electrochemical element (Q), that is, the charged electrode layer (C). The other groove (72) becomes the second gas flow path (72b) and supplies gas to the back side of the electrochemical element (Q), that is, the gas flow allowance area (P) of the metal substrate (1).

[0155] When operating this electrochemical module (M) as a fuel cell, oxygen is supplied to the first gas flow path (72a) and hydrogen is supplied to the second gas flow path (72b). In this way, a reaction as a fuel cell proceeds in each electrochemical reaction section (R) of the electrochemical element (Q), and an electromotive force and current are generated. The generated power is drawn out to the outside of the electrochemical module (M) from the cell-to-cell connection member (71) at both ends of the stacked electrochemical element (Q).

[0156] In addition, in the ninth embodiment, mutually orthogonal grooves (72) are formed on the surface and back surface of the inter-cell connecting member (71), but mutually parallel grooves (72) may also be formed on the surface and back surface of the inter-cell connecting member (71).

[0157] <10th Embodiment>

[0158] Using the electrochemical element (Q) and electrochemical module (M) described above, an electrochemical device (Y) and an energy system (Z) can be constructed.

[0159] Energy Systems, Electrochemical Devices

[0160] Figure 10 shows an overview of the energy system (Z) and the electrochemical device (Y).

[0161] The energy system (Z) has an electrochemical device (Y) and a heat exchanger (53) as a heat utilization unit that reuses heat discharged from the electrochemical device (Y).

[0162] The electrochemical device (Y) has an electrochemical module (M), a fuel supply unit that supplies fuel gas containing a reducing component to the electrochemical module (M) having a desulfurizer (31) and a reformer (34), and an inverter (38) that extracts power from the electrochemical module (M).

[0163] In detail, the electrochemical device (Y) has a desulfurizer (31), a reforming water tank (32), a vaporizer (33), a reformer (34), a blower (35), a combustion unit (36), an inverter (38), a control unit (39), a storage container (40), and an electrochemical module (M).

[0164] The desulfurization unit (31) removes (desulfurizes) sulfur compound components contained in hydrocarbon-based raw fuels such as city gas. When sulfur compounds are contained in the raw fuel, providing the desulfurization unit (31) can suppress adverse effects on the reformer (34) or electrochemical element (Q) caused by sulfur compounds. The vaporizer (33) generates steam from the reforming water supplied from the reforming water tank (32). The reformer (34) uses the steam generated in the vaporizer (33) to steam reform the raw fuel desulfurized in the desulfurization unit (31) to produce a reformed gas containing hydrogen.

[0165] The electrochemical module (M) generates electricity by electrochemically reacting the reformed gas supplied from the reformer (34) and the air supplied from the blower (35). The combustion unit (36) mixes the reaction exhaust gas discharged from the electrochemical module (M) with air to burn the combustible components in the reaction exhaust gas.

[0166] The electrochemical module (M) has a plurality of electrochemical elements (Q) and a gas manifold (17). The plurality of electrochemical elements (Q) are arranged in parallel while electrically connected to each other, and one end (bottom) of an electrochemical element (Q) is fixed to the gas manifold (17). The electrochemical element (Q) generates power by electrochemically reacting the reforming gas supplied through the gas manifold (17) with the air supplied from the blower (35).

[0167] The inverter (38) adjusts the output power of the electrochemical module (M) to have the same voltage and frequency as the power received from the commercial power grid (not shown). The control unit (39) controls the operation of the electrochemical device (Y) and the energy system (Z).

[0168] The vaporizer (33), reformer (34), electrochemical module (M), and combustion unit (36) are housed in a storage container (40). The reformer (34) performs a reforming treatment of the raw fuel using the combustion heat generated by the combustion of the reaction exhaust gas in the combustion unit (36).

[0169] The raw fuel is supplied to the desulfurizer (31) through the raw fuel supply path (42) by the operation of the booster pump (41). The modified water in the modified water tank (32) is supplied to the vaporizer (33) through the modified water supply path (44) by the operation of the modified water pump (43). Then, the raw fuel supply path (42) joins the modified water supply path (44) at a point downstream of the desulfurizer (31), and the modified water and raw fuel joined outside the storage container (40) are supplied to the vaporizer (33) equipped inside the storage container (40).

[0170] The reforming water is vaporized in the vaporizer (33) to become steam. The raw fuel containing the steam generated in the vaporizer (33) is supplied to the reformer (34) through the steam-containing raw fuel supply line (45). In the reformer (34), the raw fuel is steam-reformed to produce a reformed gas (a first gas having a reducing component) with hydrogen gas as the main component. The reformed gas produced in the reformer (34) is supplied to the gas manifold (17) of the electrochemical module (M) through the reformed gas supply line (46).

[0171] The reforming gas supplied to the gas manifold (17) is distributed to a plurality of electrochemical elements (Q) and supplied to the electrochemical elements (Q) from the bottom, which is the connection part between the electrochemical elements (Q) and the gas manifold (17). Mainly hydrogen (reducing component) in the reforming gas is used in the electrochemical reaction in the electrochemical elements (Q). The reaction exhaust gas containing residual hydrogen gas that was not used in the reaction is discharged to the combustion section (36) from the top of the electrochemical elements (Q).

[0172] The reaction exhaust gas is combusted in the combustion section (36) to become combustion exhaust gas, which is then discharged to the outside of the storage container (40) through the combustion exhaust gas outlet (50). A combustion catalyst section (51) (e.g., a platinum-based catalyst) is placed in the combustion exhaust gas outlet (50) to combust and remove reducing components such as carbon monoxide or hydrogen contained in the combustion exhaust gas. The combustion exhaust gas discharged from the combustion exhaust gas outlet (50) is sent to a heat exchanger (53) via the combustion exhaust gas discharge path (52).

[0173] The heat exchanger (53) generates hot water by exchanging heat between the combustion exhaust gas produced by combustion in the combustion section (36) and the supplied cold water. That is, the heat exchanger (53) operates as a heat utilization section that reuses the heat discharged from the electrochemical device (Y).

[0174] In addition, instead of the array utilization unit, a reaction exhaust gas utilization unit may be installed that utilizes the reaction exhaust gas discharged (without combustion) from the electrochemical module (M). The reaction exhaust gas contains residual hydrogen gas that was not used in the reaction in the electrochemical element (Q). In the reaction exhaust gas utilization unit, heat utilization by combustion or power generation by a fuel cell, etc., is performed using the residual hydrogen gas, thereby enabling effective energy utilization.

[0175] <11th Embodiment>

[0176] An electrochemical element (Q) according to the present embodiment is shown in FIG. 11. In the present embodiment, as in the fourth embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0177] The electrochemical element (Q) according to the present embodiment is configured to have a metal substrate (1) and four electrochemical reaction sections (R) (first electrochemical reaction section (R1) to fourth electrochemical reaction section (R4)). The electrochemical reaction section (R) of the present embodiment is configured to have an electrode layer (A), an intermediate layer (F), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C).

[0178] The configuration of the metal substrate (1) of this embodiment is the same as that of the third embodiment. That is, the material of the metal substrate (1) is the same as that of the metal substrate (1) according to the third embodiment. A diffusion barrier film (6) is formed on the surface of the metal substrate (1). Four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) are formed on the metal substrate (1) at spaced apart from each other.

[0179] Four electrochemical reaction sections (R) (first electrochemical reaction section (R1) to fourth electrochemical reaction section (R4)) are formed on the surface side (4) of the metal substrate (1).

[0180] In detail, first, four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) are formed to cover each gas flow allowance area (P) in an area larger than each gas flow allowance area (P). The four electrode layers (A) are formed spaced apart from each other.

[0181] Four intermediate layers (F) (first intermediate layer (F1) to fourth intermediate layer (F4)) are formed by covering each electrode layer (A) in an area larger than each electrode layer (A). The four intermediate layers (F) are formed spaced apart from each other.

[0182] Four electrolyte layers (B) (first electrolyte layer (B1) to fourth electrolyte layer (B4)) are formed by covering each electrode layer (A) and intermediate layer (F) in an area larger than each electrode layer (A) and intermediate layer (F). The four electrolyte layers (B) are formed spaced apart from each other.

[0183] Four reaction prevention layers (G) (first reaction prevention layer (G1) to fourth reaction prevention layer (G4)) are formed on each electrolyte layer (B).

[0184] Four counter electrode layers (C) (first counter electrode layer (C1) to fourth counter electrode layer (C4)) are formed on each reaction prevention layer (G).

[0185] In this embodiment, an intermediate layer (F) is formed in the form of a film between the electrode layer (A) and the electrolyte layer (B). The thickness of the film can be, for example, about 1 μm to 100 μm, preferably about 2 μm to 50 μm, and more preferably about 5 μm to 20 μm. By having such a film thickness, it is possible to reduce the amount of expensive materials used and thereby reduce costs while ensuring sufficient performance.

[0186] For the material of the intermediate layer (F), for example, cerium oxide-based materials or zirconia-based materials can be used. By introducing the intermediate layer (F) between the electrode layer (A) and the electrolyte layer (B), the performance, reliability, and durability of the electrochemical reaction part (R) can be improved. Furthermore, it is preferable to form the intermediate layer (F) by a low-temperature sintering method (for example, a wet method that uses sintering treatment in a low-temperature region of about 1100°C or lower, for example, without sintering treatment in a high-temperature region such as 1400°C), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using these processes that are usable in a low-temperature region, a good intermediate layer (F) is obtained by processing in a low-temperature region of about 1100°C or lower, for example, without using sintering in a high-temperature region such as 1400°C. For this reason, it is desirable to be able to suppress damage to the metal substrate (1) caused by high-temperature heating, and also to suppress the interdiffusion of elements caused by high-temperature heating between the metal substrate (1) and the electrode layer (A), thereby realizing an electrochemical device (Q) with excellent durability.

[0187] In this embodiment, a reaction prevention layer (G) is formed in the form of a film between the electrolyte layer (B) and the counter electrode layer (C). The thickness of the film can be, for example, about 1 μm to 100 μm, preferably about 2 μm to 50 μm, and more preferably about 5 μm to 20 μm. By having such a film thickness, it is possible to reduce the amount of expensive materials used and thereby reduce costs while ensuring sufficient performance.

[0188] For the material of the reaction prevention layer (G), for example, cerium oxide-based materials or zirconia-based materials can be used. By introducing the reaction prevention layer (G) between the electrolyte layer (B) and the counter electrode layer (C), the reaction between the constituent material of the counter electrode layer (C) and the constituent material of the electrolyte layer (B) is effectively suppressed, thereby improving the long-term stability of the performance of the electrochemical reaction part (R). Furthermore, it is preferable to form the reaction prevention layer (G) by a low-temperature sintering method (for example, a wet method that uses sintering treatment in a low-temperature region of about 1100°C or lower, for example, without performing sintering treatment in a high-temperature region such as 1400°C), a PVD method such as sputtering or pulsed laser deposition, a CVD method, or a spray coating method. By using these processes that are usable in a low-temperature region, a good reaction prevention layer (G) is obtained by processing in a low-temperature region of about 1100°C or lower, for example, without using sintering in a high-temperature region such as 1400°C. For this reason, it is desirable to be able to suppress damage to the metal substrate (1) caused by high-temperature heating, and also to suppress the interdiffusion of elements caused by high-temperature heating between the metal substrate (1) and the electrode layer (A), thereby realizing an electrochemical device (Q) with excellent durability.

[0189] Each gas flow-allowing region (P) is covered by an electrode layer (A), and each electrode layer (A) (and intermediate layer (F)) is covered by an electrolyte layer (B), thereby preventing the gas supplied from the gas flow-allowing region (P) to the electrode layer (A) from leaking to the counter electrode layer (C). That is, in this embodiment, the metal substrate (1) has a plurality of gas flow-allowing regions (P) spaced apart from each other, and the electrolyte layer (B) of the electrochemical reaction unit (R) is arranged to cover the entirety of each gas flow-allowing region (P).

[0190] In this embodiment, as described above, a conductive diffusion barrier film (6) is formed on the surface of the metal substrate (1). Accordingly, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through the metal substrate (1). That is, in this embodiment, the electrode layers (A) of adjacent electrochemical reaction units (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R).

[0191] <12th Embodiment>

[0192] An electrochemical element (Q) according to the present embodiment is shown in FIG. 12. In the present embodiment, as in the 11th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0193] Unlike the 11th embodiment, the electrochemical reaction section (R) according to the present embodiment does not have an intermediate layer (F). That is, the electrochemical reaction section (R) is composed of an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The configuration excluding the intermediate layer (F) is similar to the 11th embodiment.

[0194] Each gas flow-allowing region (P) is covered by an electrode layer (A), and each electrode layer (A) is covered by an electrolyte layer (B), thereby preventing the gas supplied from the gas flow-allowing region (P) to the electrode layer (A) from leaking to the charged electrode layer (C). That is, in this embodiment, the metal substrate (1) has a plurality of gas flow-allowing regions (P) spaced apart from each other, and the electrolyte layer (B) of the electrochemical reaction unit (R) is arranged to cover the entirety of each gas flow-allowing region (P).

[0195] In this embodiment, as described above, a conductive diffusion barrier film (6) is formed on the surface of the metal substrate (1). Accordingly, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through the metal substrate (1). That is, in this embodiment, the electrode layers (A) of adjacent electrochemical reaction units (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R).

[0196] <13th Embodiment>

[0197] An electrochemical element (Q) according to the present embodiment is shown in FIG. 13. In the present embodiment, as in the 11th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0198] Unlike the 11th embodiment, in the electrochemical reaction section (R) according to the present embodiment, an electrolyte layer (B) is installed across a plurality of electrochemical reaction sections (R). The configuration excluding the electrolyte layer (B) is similar to the 11th embodiment.

[0199] In detail, the electrolyte layer (B) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) and four intermediate layers (F) (first intermediate layer (F1) to fourth intermediate layer (F4)). The four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) and the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed. And, in the region corresponding to the electrode layer (A) on the electrolyte layer (B), four reaction prevention layers (G) (first reaction prevention layer (G1) to fourth reaction prevention layer (G4)), and four counter electrode layers (C) (first counter electrode layer (C1) to fourth counter electrode layer (C4)) are formed.

[0200] Since four electrode layers (A) and four counter electrode layers (C) are formed spaced apart from each other, an electrochemical reaction can occur between the opposing electrode layers (A) and counter electrode layers (C) and the electrolyte layer (B) that is clamped between them. That is, a first electrochemical reaction section (R1) is formed by the first electrode layer (A1) and the first counter electrode layer (C1) and the portion clamped between them (first intermediate layer (F1), electrolyte layer (B), and first reaction prevention layer (G1)). Likewise, the second electrochemical reaction section (R2) to the fourth electrochemical reaction section (R4) is formed by the second electrode layer (A2) to the fourth electrode layer (A4), the second counter electrode layer (C2) to the fourth counter electrode layer (C4), and the portions clamped thereto (the second intermediate layer (F2) to the fourth intermediate layer (F4), the electrolyte layer (B), and the second reaction prevention layer (G2) to the fourth reaction prevention layer (G4)). That is, in this embodiment, a plurality of electrochemical reaction sections (R) are arranged on the surface side (4) of the metal substrate (1).

[0201] And, similar to the third embodiment, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through a metal substrate (1). Therefore, it can be said that a plurality of electrochemical reaction units (R) are electrically connected in parallel.

[0202] <14th Embodiment>

[0203] An electrochemical element (Q) according to the present embodiment is shown in FIG. 14. In the present embodiment, as in the 13th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0204] Unlike the 13th embodiment, the electrochemical reaction section (R) according to the present embodiment does not have an intermediate layer (F). That is, the electrochemical reaction section (R) is composed of an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The configuration excluding the intermediate layer (F) is similar to the 13th embodiment.

[0205] Each gas flow-allowing region (P) is covered by an electrode layer (A), and each electrode layer (A) is covered by an electrolyte layer (B), thereby preventing the gas supplied from the gas flow-allowing region (P) to the electrode layer (A) from leaking to the charged electrode layer (C). That is, in this embodiment, the metal substrate (1) has a plurality of gas flow-allowing regions (P) spaced apart from each other, and the electrolyte layer (B) of the electrochemical reaction unit (R) is arranged to cover the entirety of each gas flow-allowing region (P).

[0206] In this embodiment, as described above, a conductive diffusion barrier film (6) is formed on the surface of the metal substrate (1). Accordingly, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through the metal substrate (1). That is, in this embodiment, the electrode layers (A) of adjacent electrochemical reaction units (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R).

[0207] <15th Embodiment>

[0208] An electrochemical element (Q) according to the present embodiment is shown in FIG. 15. In the present embodiment, similar to the 11th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0209] Unlike the 11th embodiment, in the electrochemical reaction section (R) according to the present embodiment, an electrolyte layer (B) and a reaction prevention layer (G) are installed across a plurality of electrochemical reaction sections (R). The configuration excluding the electrolyte layer (B) and the reaction prevention layer (G) is similar to the 11th embodiment.

[0210] In detail, the electrolyte layer (B) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) and four intermediate layers (F) (first intermediate layer (F1) to fourth intermediate layer (F4)). The four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) and the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0211] The reaction prevention layer (G) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) and four intermediate layers (F) (first intermediate layer (F1) to fourth intermediate layer (F4)) on the electrolyte layer (B). Additionally, four counter electrode layers (C) (first counter electrode layer (C1) to fourth counter electrode layer (C4)) are formed in the region corresponding to the electrode layer (A) on the reaction prevention layer (G).

[0212] Since four electrode layers (A) and four counter electrode layers (C) are formed spaced apart from each other, an electrochemical reaction can occur between the opposing electrode layers (A) and counter electrode layers (C) and the electrolyte layer (B) that is clamped between them. That is, a first electrochemical reaction section (R1) is formed by the first electrode layer (A1) and the first counter electrode layer (C1), and the portion clamped between them (first intermediate layer (F1), electrolyte layer (B), reaction prevention layer (G)). Similarly, a second electrochemical reaction section (R2) to a fourth electrochemical reaction section (R4) is formed by the second electrode layer (A2) to the fourth electrode layer (A4), the second counter electrode layer (C2) to the fourth counter electrode layer (C4), and the portion clamped between them (second intermediate layer (F2) to the fourth intermediate layer (F4), electrolyte layer (B), and reaction prevention layer (G)). That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0213] And, similar to the third embodiment, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through a metal substrate (1). Therefore, it can be said that a plurality of electrochemical reaction units (R) are electrically connected in parallel.

[0214] <16th Embodiment>

[0215] An electrochemical element (Q) according to the present embodiment is shown in FIG. 16. In the present embodiment, as in the 15th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0216] Unlike the 15th embodiment, the electrochemical reaction section (R) according to the present embodiment does not have an intermediate layer (F). That is, the electrochemical reaction section (R) is composed of an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The configuration excluding the intermediate layer (F) is similar to the 15th embodiment.

[0217] Each gas flow-allowing region (P) is covered by an electrode layer (A), and each electrode layer (A) is covered by an electrolyte layer (B), thereby preventing the gas supplied from the gas flow-allowing region (P) to the electrode layer (A) from leaking to the charged electrode layer (C). That is, in this embodiment, the metal substrate (1) has a plurality of gas flow-allowing regions (P) spaced apart from each other, and the electrolyte layer (B) of the electrochemical reaction unit (R) is arranged to cover the entirety of each gas flow-allowing region (P).

[0218] In this embodiment, as described above, a conductive diffusion barrier film (6) is formed on the surface of the metal substrate (1). Accordingly, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through the metal substrate (1). That is, in this embodiment, the electrode layers (A) of adjacent electrochemical reaction units (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R).

[0219] <17th Embodiment>

[0220] An electrochemical element (Q) according to the present embodiment is shown in FIG. 17. In the present embodiment, as in the 11th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0221] Unlike the 11th embodiment, in the electrochemical reaction section (R) according to the present embodiment, an intermediate layer (F), an electrolyte layer (B), and a reaction prevention layer (G) are installed across a plurality of electrochemical reaction sections (R). The configuration excluding the intermediate layer (F), the electrolyte layer (B), and the reaction prevention layer (G) is similar to the 11th embodiment.

[0222] In detail, the intermediate layer (F) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)). The electrolyte layer (B) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) and the intermediate layer (F). The four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) and the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0223] The reaction prevention layer (G) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) and the intermediate layer (F) on the electrolyte layer (B). Additionally, four counter electrode layers (C) (first counter electrode layer (C1) to fourth counter electrode layer (C4)) are formed in the region corresponding to the electrode layer (A) on the reaction prevention layer (G).

[0224] Since four electrode layers (A) and four counter electrode layers (C) are formed spaced apart from each other, an electrochemical reaction can occur between the opposing electrode layers (A) and counter electrode layers (C) and the electrolyte layer (B) that is clamped between them. That is, a first electrochemical reaction section (R1) is formed by the first electrode layer (A1) and the first counter electrode layer (C1), and the portions clamped between them (intermediate layer (F), electrolyte layer (B), and reaction prevention layer (G)). Similarly, a second electrochemical reaction section (R2) to a fourth electrochemical reaction section (R4) is formed by the second electrode layer (A2) to the fourth electrode layer (A4), the second counter electrode layer (C2) to the fourth counter electrode layer (C4), and the portions clamped between them (intermediate layer (F), electrolyte layer (B), and reaction prevention layer (G)). That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0225] And, similar to the third embodiment, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through a metal substrate (1). Therefore, it can be said that a plurality of electrochemical reaction units (R) are electrically connected in parallel.

[0226] <18th Embodiment>

[0227] An electrochemical element (Q) according to the present embodiment is shown in FIG. 18. In the present embodiment, as in the 11th embodiment, the electrode layer (A) of one electrochemical reaction unit (R) and the electrode layer (A) of another electrochemical reaction unit (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R) in parallel.

[0228] Unlike the 11th embodiment, in the electrochemical reaction section (R) according to the present embodiment, an intermediate layer (F) and an electrolyte layer (B) are installed across a plurality of electrochemical reaction sections (R). The configuration excluding the intermediate layer (F) and the electrolyte layer (B) is similar to the 11th embodiment.

[0229] In detail, the intermediate layer (F) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)). The electrolyte layer (B) is formed as a single continuous layer covering the entirety of the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) and the intermediate layer (F). The four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) and the four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0230] And, in the region corresponding to the electrode layer (A) on the electrolyte layer (B), four reaction prevention layers (G) (first reaction prevention layer (G1) to fourth reaction prevention layer (G4)), and four counter electrode layers (C) (first counter electrode layer (C1) to fourth counter electrode layer (C4)) are formed.

[0231] Since four electrode layers (A) and four counter electrode layers (C) are formed spaced apart from each other, an electrochemical reaction can occur between the opposing electrode layers (A) and counter electrode layers (C) and the electrolyte layer (B) that is clamped between them. That is, a first electrochemical reaction section (R1) is formed by the first electrode layer (A1) and the first counter electrode layer (C1), and the portion clamped between them (intermediate layer (F), electrolyte layer (B), and first reaction prevention layer (G1)). Similarly, a second electrochemical reaction section (R2) to a fourth electrochemical reaction section (R4) is formed by the second electrode layer (A2) to the fourth electrode layer (A4), the second counter electrode layer (C2) to the fourth counter electrode layer (C4), and the portion clamped between them (intermediate layer (F), electrolyte layer (B), and the second reaction prevention layer (G2) to the fourth reaction prevention layer (G4)). That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0232] And, similar to the third embodiment, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through a metal substrate (1). Therefore, it can be said that a plurality of electrochemical reaction units (R) are electrically connected in parallel.

[0233] <19th Embodiment>

[0234] An electrochemical element (Q) according to the present embodiment is shown in FIG. 19. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an intermediate layer (F), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The electrode layer (A), the intermediate layer (F), the electrolyte layer (B), the reaction prevention layer (G), and the counter electrode layer (C) constitute an electrochemical reaction section (R).

[0235] The configuration of the metal substrate (1) of this embodiment is the same as that of the third embodiment. That is, the material of the metal substrate (1) is the same as that of the metal substrate (1) according to the third embodiment. A diffusion barrier film (6) is formed on the surface of the metal substrate (1). Four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) are formed on the metal substrate (1) at spaced apart from each other.

[0236] Four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)) are formed to cover each gas flow allowance area (P) in an area larger than each gas flow allowance area (P). The four electrode layers (A) are formed spaced apart from each other.

[0237] Four intermediate layers (F) (first intermediate layer (F1) to fourth intermediate layer (F4)) are formed by covering each electrode layer (A) in an area larger than each electrode layer (A). The four intermediate layers (F) are formed spaced apart from each other.

[0238] The first electrolyte layer (B1) is formed as a single continuous layer covering the entirety of the first electrode layer (A1) and the second electrode layer (A2). Two gas flow-allowing regions (P) (first gas flow-allowing region (P1) and second gas flow-allowing region (P2)) and two electrode layers (A) (first electrode layer (A1) and second electrode layer (A2)) are covered by the first electrolyte layer (B1). As a result, the leakage of gas supplied to the electrode layer (A) toward the counter electrode layer (C) is suppressed.

[0239] The second electrolyte layer (B2) is formed as a single continuous layer covering the entirety of the third electrode layer (A3) and the fourth electrode layer (A4). Two gas flow-allowing regions (P) (third gas flow-allowing region (P3) and fourth gas flow-allowing region (P4)) and two electrode layers (A) (third electrode layer (A3) and fourth electrode layer (A4)) are covered by the second electrolyte layer (B2). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0240] The first reaction prevention layer (G1) is formed as a single continuous layer covering the entirety of the two electrode layers (A) (first electrode layer (A1) and second electrode layer (A2)) and two intermediate layers (F) (first intermediate layer (F1) and second intermediate layer (F2)) on the first electrolyte layer (B1).

[0241] The second reaction prevention layer (G2) is formed as a single continuous layer covering the entirety of the two electrode layers (A) (third electrode layer (A3) and fourth electrode layer (A4)) and the two intermediate layers (F) (third intermediate layer (F4) and fourth intermediate layer (F4)) on the second electrolyte layer (B2).

[0242] The first electrode layer (C1) is formed as a single continuous layer covering the entirety of the two electrode layers (A) (first electrode layer (A1) and second electrode layer (A2)) and two intermediate layers (F) (first intermediate layer (F1) and second intermediate layer (F2)) on the first reaction prevention layer (G1).

[0243] The second electrode layer (C2) is formed as a single continuous layer covering the entirety of the two electrode layers (A) (third electrode layer (A3) and fourth electrode layer (A4)) and the two intermediate layers (F) (third intermediate layer (F4) and fourth intermediate layer (F4)) on the second reaction prevention layer (G2).

[0244] In this embodiment, four electrode layers (A) are formed spaced apart from each other. Electrochemical reactions can occur through these four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)), the electrolyte layer (B), and the counter electrode layer (C) (first counter electrode layer (C1) and second counter electrode layer (C2)). Accordingly, it is interpreted that the first electrochemical reaction section (R1) is formed by the first electrode layer (A1), the left half of the first counter electrode layer (C1), and the portions clamped thereto (first intermediate layer (F1), first electrolyte layer (B1), first reaction prevention layer (G1)).

[0245] It is interpreted that the second electrochemical reaction section (R2) is formed by the second electrode layer (A2), the right half of the first counter electrode layer (C1), and the portions clamped to them (second intermediate layer (F2), first electrolyte layer (B1), first reaction prevention layer (G1)).

[0246] It is interpreted that the third electrochemical reaction section (R3) is formed by the third electrode layer (A3), the left half of the second counter electrode layer (C2), and the parts clamped to them (third intermediate layer (F3), second electrolyte layer (B2), second reaction prevention layer (G2)).

[0247] It is interpreted that the fourth electrochemical reaction section (R4) is formed by the fourth electrode layer (A4), the right half of the second counter electrode layer (C2), and the parts clamped to them (the fourth intermediate layer (F4), the second electrolyte layer (B2), and the second reaction prevention layer (G2)).

[0248] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0249] In addition, in this embodiment, two positive electrode layers (C) are formed spaced apart from each other. Electrochemical reactions can occur through these two positive electrode layers (C) (first positive electrode layer (C1) and second positive electrode layer (C2)), the electrolyte layer (B), and the electrode layer (A) (first electrode layer (A1) to fourth electrode layer (A4)). Accordingly, it is interpreted that the fifth electrochemical reaction section (R5) is formed by the first electrode layer (A1) and the second electrode layer (A2), the first positive electrode layer (C1), and the portions enclosed therein (first intermediate layer (F1) and second intermediate layer (F2), the first electrolyte layer (B1), and the first reaction prevention layer (G1)).

[0250] It is interpreted that the sixth electrochemical reaction part (R6) is composed of the third electrode layer (A3) and the fourth electrode layer (A4), the second counter electrode layer (C2), and the parts clamped thereto (the third intermediate layer (F3) and the fourth intermediate layer (F4), the second electrolyte layer (B2), and the second reaction prevention layer (G2)).

[0251] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0252] In the present embodiment, as in the fifth electrochemical reaction unit (R5) and the sixth electrochemical reaction unit (R6), there are cases where a plurality of gas flow allowance areas (P) correspond to a single electrochemical reaction unit (R). Even in such cases, the electrolyte layer (B) of the electrochemical reaction unit (R) is arranged to cover the entirety of each gas flow allowance area (P). By doing so, the gas supplied to the electrode layer (A) by passing through the gas flow allowance area (P) from the back side of the metal substrate (1) can be suppressed from leaking to the surface side of the metal substrate (1), and the performance and reliability as an electrochemical device can be improved. Specifically, the first electrolyte layer (B1) of the fifth electrochemical reaction unit (R5) is arranged to cover the entirety of the first gas flow allowance area (P1) and the second gas flow allowance area (P2). The second electrolyte layer (B2) of the sixth electrochemical reaction unit (R6) is positioned to cover the entirety of the third gas flow-allowing area (P3) and the fourth gas flow-allowing area (P4).

[0253] <20th Embodiment>

[0254] An electrochemical element (Q) according to the present embodiment is shown in FIG. 20. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). Unlike the 19th embodiment, the electrochemical reaction section (R) according to the present embodiment does not have an intermediate layer (F) installed. That is, the electrochemical reaction section (R) is composed of an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The configuration excluding the intermediate layer (F) is similar to the 19th embodiment.

[0255] The first electrolyte layer (B1) is formed as a single continuous layer covering the entirety of the first electrode layer (A1) and the second electrode layer (A2). Two gas flow-allowing regions (P) (first gas flow-allowing region (P1) and second gas flow-allowing region (P2)) and two electrode layers (A) (first electrode layer (A1) and second electrode layer (A2)) are covered by the first electrolyte layer (B1). As a result, the leakage of gas supplied to the electrode layer (A) toward the counter electrode layer (C) is suppressed.

[0256] The second electrolyte layer (B2) is formed as a single continuous layer covering the entirety of the third electrode layer (A3) and the fourth electrode layer (A4). Two gas flow-allowing regions (P) (third gas flow-allowing region (P3) and fourth gas flow-allowing region (P4)) and two electrode layers (A) (third electrode layer (A3) and fourth electrode layer (A4)) are covered by the second electrolyte layer (B2). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0257] In this embodiment, four electrode layers (A) are formed spaced apart from each other. Electrochemical reactions can occur through these four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)), the electrolyte layer (B), and the counter electrode layer (C) (first counter electrode layer (C1) and second counter electrode layer (C2)). Accordingly, it is interpreted that the first electrochemical reaction section (R1) is formed by the first electrode layer (A1), the left half of the first counter electrode layer (C1), and the portions clamped thereto (first electrolyte layer (B1), first reaction prevention layer (G1)).

[0258] It is interpreted that the second electrochemical reaction section (R2) is formed by the second electrode layer (A2), the right half of the first counter electrode layer (C1), and the portions clamped to them (first electrolyte layer (B1), first reaction prevention layer (G1)).

[0259] It is interpreted that the third electrochemical reaction section (R3) is formed by the third electrode layer (A3), the left half of the second counter electrode layer (C2), and the portions clamped to them (second electrolyte layer (B2), second reaction prevention layer (G2)).

[0260] It is interpreted that the fourth electrochemical reaction section (R4) is formed by the fourth electrode layer (A4), the right half of the second counter electrode layer (C2), and the portions clamped to them (second electrolyte layer (B2), second reaction prevention layer (G2)).

[0261] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0262] In addition, in this embodiment, two positive electrode layers (C) are formed spaced apart from each other. Electrochemical reactions can occur through these two positive electrode layers (C) (first positive electrode layer (C1) and second positive electrode layer (C2)), the electrolyte layer (B), and the electrode layer (A) (first electrode layer (A1) to fourth electrode layer (A4)). Accordingly, it is interpreted that the fifth electrochemical reaction section (R5) is formed by the first electrode layer (A1) and the second electrode layer (A2), the first positive electrode layer (C1), and the portions enclosed therein (first electrolyte layer (B1), first reaction prevention layer (G1)).

[0263] It is interpreted that the sixth electrochemical reaction part (R6) is composed of the third electrode layer (A3) and the fourth electrode layer (A4), the second counter electrode layer (C2), and the parts clamped thereto (the second electrolyte layer (B2), the second reaction prevention layer (G2)).

[0264] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0265] <21st Embodiment>

[0266] An electrochemical element (Q) according to the present embodiment is shown in FIG. 21. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an intermediate layer (F), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The electrode layer (A), the intermediate layer (F), the electrolyte layer (B), the reaction prevention layer (G), and the counter electrode layer (C) constitute an electrochemical reaction section (R).

[0267] The configuration of the electrochemical element (Q) according to the present embodiment is similar to the 19th embodiment. The difference from the 19th embodiment is that an intermediate layer (F) is installed over a plurality of electrode layers (A). The first intermediate layer (F1) is formed as a single continuous layer covering the entirety of the first electrode layer (A1) and the second electrode layer (A2). The second intermediate layer (F2) is formed as a single continuous layer covering the entirety of the third electrode layer (A3) and the fourth electrode layer (A4).

[0268] The first electrolyte layer (B1) is formed as a single continuous layer covering the entirety of the first electrode layer (A1) and the second electrode layer (A2). Two gas flow-allowing regions (P) (first gas flow-allowing region (P1) and second gas flow-allowing region (P2)) and two electrode layers (A) (first electrode layer (A1) and second electrode layer (A2)) are covered by the first electrolyte layer (B1). As a result, the leakage of gas supplied to the electrode layer (A) toward the counter electrode layer (C) is suppressed.

[0269] The second electrolyte layer (B2) is formed as a single continuous layer covering the entirety of the third electrode layer (A3) and the fourth electrode layer (A4). Two gas flow-allowing regions (P) (third gas flow-allowing region (P3) and fourth gas flow-allowing region (P4)) and two electrode layers (A) (third electrode layer (A3) and fourth electrode layer (A4)) are covered by the second electrolyte layer (B2). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0270] In this embodiment, four electrode layers (A) are formed spaced apart from each other. Electrochemical reactions can occur through these four electrode layers (A) (first electrode layer (A1) to fourth electrode layer (A4)), the electrolyte layer (B), and the counter electrode layer (C) (first counter electrode layer (C1) and second counter electrode layer (C2)). Accordingly, it is interpreted that the first electrochemical reaction section (R1) is formed by the first electrode layer (A1), the left half of the first counter electrode layer (C1), and the portions clamped thereto (first intermediate layer (F1), first electrolyte layer (B1), first reaction prevention layer (G1)).

[0271] It is interpreted that the second electrochemical reaction section (R2) is formed by the second electrode layer (A2), the right half of the first counter electrode layer (C1), and the portions clamped to them (first intermediate layer (F1), first electrolyte layer (B1), first reaction prevention layer (G1)).

[0272] It is interpreted that the third electrochemical reaction section (R3) is formed by the third electrode layer (A3), the left half of the second counter electrode layer (C2), and the parts clamped to them (the second intermediate layer (F2), the second electrolyte layer (B2), and the second reaction prevention layer (G2)).

[0273] It is interpreted that the fourth electrochemical reaction section (R4) is formed by the fourth electrode layer (A4), the right half of the second counter electrode layer (C2), and the parts clamped to them (the second intermediate layer (F2), the second electrolyte layer (B2), and the second reaction prevention layer (G2)).

[0274] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0275] In addition, in this embodiment, two positive electrode layers (C) are formed spaced apart from each other. Electrochemical reactions can occur through these two positive electrode layers (C) (first positive electrode layer (C1) and second positive electrode layer (C2)), the electrolyte layer (B), and the electrode layer (A) (first electrode layer (A1) to fourth electrode layer (A4)). Accordingly, it is interpreted that the fifth electrochemical reaction section (R5) is formed by the first electrode layer (A1) and the second electrode layer (A2), the first positive electrode layer (C1), and the portions enclosed therein (first intermediate layer (F1), first electrolyte layer (B1), and first reaction prevention layer (G1)).

[0276] It is interpreted that the sixth electrochemical reaction part (R6) is composed of the third electrode layer (A3) and the fourth electrode layer (A4), the second counter electrode layer (C2), and the parts clamped thereto (the second intermediate layer (F2), the second electrolyte layer (B2), and the second reaction prevention layer (G2)).

[0277] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0278] <22nd Embodiment>

[0279] An electrochemical element (Q) according to the present embodiment is shown in FIG. 22. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an intermediate layer (F), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The electrode layer (A), the intermediate layer (F), the electrolyte layer (B), the reaction prevention layer (G), and the counter electrode layer (C) constitute an electrochemical reaction section (R).

[0280] The configuration of the metal substrate (1) of this embodiment is the same as that of the third embodiment. That is, the material of the metal substrate (1) is the same as that of the metal substrate (1) according to the third embodiment. A diffusion barrier film (6) is formed on the surface of the metal substrate (1). Four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) are formed on the metal substrate (1) at spaced apart from each other.

[0281] The electrode layer (A) is formed as a single continuous layer covering the entirety of four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)).

[0282] The intermediate layer (F) is formed as a single continuous layer covering the entire electrode layer (A).

[0283] The electrolyte layer (B) is formed as a single continuous layer covering the entire electrode layer (A) and the intermediate layer (F). Four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) and the electrode layer (A) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0284] The reaction prevention layer (G) is formed as a single continuous layer covering the entire electrode layer (A) and intermediate layer (F) on top of the electrolyte layer (B).

[0285] Four counter electrode layers (C) (first counter electrode layer (C1) to fourth counter electrode layer (C4)) are formed in the regions corresponding to the four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) on the reaction prevention layer (G).

[0286] In the electrochemical element (Q) according to the present embodiment, since an electrolyte layer (B) is disposed between the electrode layer (A) and the counter electrode layer (C), an electrochemical reaction can occur between the material supplied to the electrode layer (A) and the material supplied to the counter electrode layer (C) through four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)). Accordingly, it is interpreted that a first electrochemical reaction section (R1) is formed by the first gas flow allowance region (P1) and the first counter electrode layer (C1) in the electrode layer (A), intermediate layer (F), electrolyte layer (B), and reaction prevention layer (G), and by the first counter electrode layer (C1).

[0287] It is interpreted that a second gas flow-allowing region (P2) in the electrode layer (A), intermediate layer (F), electrolyte layer (B), and reaction-preventing layer (G), a portion enclosed by the second counter electrode layer (C2), and a second electrochemical reaction section (R2) are formed by the second counter electrode layer (C2).

[0288] It is interpreted that a third gas flow-allowing region (P3) in the electrode layer (A), intermediate layer (F), electrolyte layer (B), and reaction-preventing layer (G), a portion enclosed by the third counter electrode layer (C3), and a third electrochemical reaction section (R3) are formed by the third counter electrode layer (C3).

[0289] It is interpreted that a fourth gas flow-allowing region (P4) in the electrode layer (A), intermediate layer (F), electrolyte layer (B), and reaction-preventing layer (G), a portion enclosed by the fourth counter electrode layer (C4), and a fourth electrochemical reaction section (R4) are formed by the fourth counter electrode layer (C4).

[0290] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0291] In this embodiment, as described above, a conductive diffusion barrier film (6) is formed on the surface of the metal substrate (1). Accordingly, a plurality of electrode layers (A) formed spaced apart from each other are electrically connected through the metal substrate (1). That is, in this embodiment, the electrode layers (A) of adjacent electrochemical reaction units (R) are electrically connected, thereby electrically connecting a plurality of electrochemical reaction units (R).

[0292] <23rd Embodiment>

[0293] An electrochemical element (Q) according to the present embodiment is shown in FIG. 23. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). Unlike the 22nd embodiment, the electrochemical reaction section (R) according to the present embodiment does not have an intermediate layer (F) installed. That is, the electrochemical reaction section (R) is composed of an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The configuration excluding the intermediate layer (F) is similar to the 22nd embodiment.

[0294] The electrolyte layer (B) is formed as a single continuous layer covering the entire electrode layer (A). Four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)) and the electrode layer (A) are covered by the electrolyte layer (B). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0295] In this embodiment, similar to the 22nd embodiment, four electrochemical reaction units (R) (first electrochemical reaction unit (R1) to fourth electrochemical reaction unit (R4)) are arranged on the surface side (4) of the metal substrate (1). Then, the electrode layer (A) of the adjacent electrochemical reaction unit (R) is electrically connected through the metal substrate (1), so that a plurality of electrochemical reaction units (R) are electrically connected in parallel.

[0296] <24th Embodiment>

[0297] An electrochemical element (Q) according to the present embodiment is shown in FIG. 24. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an intermediate layer (F), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The electrode layer (A), the intermediate layer (F), the electrolyte layer (B), the reaction prevention layer (G), and the counter electrode layer (C) constitute an electrochemical reaction section (R).

[0298] The configuration of the electrochemical element (Q) according to the present embodiment is similar to the 19th embodiment. The difference from the 19th embodiment is that the electrode layer (A) and the intermediate layer (F) are installed over a plurality of gas flow allowance regions (P).

[0299] The first electrode layer (A1) is formed as a single continuous layer covering the entirety of the first gas flow allowance area (P1) and the second gas flow allowance area (P2). The first intermediate layer (F1) is installed covering the entirety of the first electrode layer (A1).

[0300] The second electrode layer (A2) is formed as a single continuous layer covering the entirety of the third gas flow allowance area (P3) and the fourth gas flow allowance area (P4). The second intermediate layer (F2) is installed covering the entirety of the second electrode layer (A2).

[0301] The first electrolyte layer (B1) is formed as a single continuous layer covering the entire first electrode layer (A1). Two gas flow allowance regions (P) (first gas flow allowance region (P1) and second gas flow allowance region (P2)) and the first electrode layer (A1) are covered by the first electrolyte layer (B1). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0302] The second electrolyte layer (B2) is formed as a single continuous layer covering the entire second electrode layer (A2). Two gas flow allowance regions (P) (third gas flow allowance region (P3) and fourth gas flow allowance region (P4)) and the second electrode layer (A2) are covered by the second electrolyte layer (B2). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0303] In the electrochemical element (Q) according to the present embodiment, since an electrolyte layer (B) is disposed between the electrode layer (A) and the counter electrode layer (C), an electrochemical reaction can occur between the material supplied to the electrode layer (A) and the material supplied to the counter electrode layer (C) through four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)). Accordingly, it is interpreted that the first electrochemical reaction section (R1) is formed by the portion of the electrode layer (A) above the first gas flow allowance region (P1), the portion of the intermediate layer (F), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C).

[0304] It is interpreted that the second electrochemical reaction section (R2) is formed by the portion of the electrode layer (A), the portion of the intermediate layer (F), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) on the upper side of the second gas flow allowance area (P2).

[0305] It is interpreted that the third electrochemical reaction section (R3) is formed by the portion of the electrode layer (A), the portion of the intermediate layer (F), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) on the upper side of the third gas flow allowance area (P3).

[0306] It is interpreted that the fourth electrochemical reaction section (R4) is formed by the portion of the electrode layer (A), the portion of the intermediate layer (F), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) on the upper side of the fourth gas flow allowance area (P4).

[0307] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0308] In addition, in this embodiment, two counter electrode layers (C) are formed spaced apart from each other. Electrochemical reactions can occur through these two counter electrode layers (C) (first counter electrode layer (C1) and second counter electrode layer (C2)), the electrolyte layer (B) (first electrolyte layer (B1) and second electrolyte layer (B2)), and the electrode layer (A) (first electrode layer (A1) and second electrode layer (A2)). Accordingly, it is interpreted that the fifth electrochemical reaction section (R5) is formed by the first electrode layer (A1), the first counter electrode layer (C1), and the portions enclosed therein (first intermediate layer (F1), first electrolyte layer (B1), and first reaction prevention layer (G1)).

[0309] It is interpreted that the sixth electrochemical reaction part (R6) is composed of the second electrode layer (A2), the second counter electrode layer (C2), and the parts clamped thereto (the second intermediate layer (F2), the second electrolyte layer (B2), and the second reaction prevention layer (G2)).

[0310] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0311] <25th Embodiment>

[0312] An electrochemical element (Q) according to the present embodiment is shown in FIG. 25. The electrochemical element (Q) according to the present embodiment is composed of a metal substrate (1), an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). Unlike the 19th embodiment, the electrochemical reaction section (R) according to the present embodiment does not have an intermediate layer (F). That is, the electrochemical reaction section (R) is composed of an electrode layer (A), an electrolyte layer (B), a reaction prevention layer (G), and a counter electrode layer (C). The configuration excluding the intermediate layer (F) is similar to the 24th embodiment.

[0313] The first electrolyte layer (B1) is formed as a single continuous layer covering the entire first electrode layer (A1). Two gas flow allowance regions (P) (first gas flow allowance region (P1) and second gas flow allowance region (P2)) and the first electrode layer (A1) are covered by the first electrolyte layer (B1). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0314] The second electrolyte layer (B2) is formed as a single continuous layer covering the entire second electrode layer (A2). Two gas flow allowance regions (P) (third gas flow allowance region (P3) and fourth gas flow allowance region (P4)) and the second electrode layer (A2) are covered by the second electrolyte layer (B2). As a result, the leakage of gas supplied to the electrode layer (A) to the counter electrode layer (C) is suppressed.

[0315] In the electrochemical element (Q) according to the present embodiment, since an electrolyte layer (B) is disposed between the electrode layer (A) and the counter electrode layer (C), an electrochemical reaction can occur between the material supplied to the electrode layer (A) and the material supplied to the counter electrode layer (C) through four gas flow allowance regions (P) (first gas flow allowance region (P1) to fourth gas flow allowance region (P4)). Accordingly, it is interpreted that a first electrochemical reaction section (R1) is formed by the portion of the electrode layer (A), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) above the first gas flow allowance region (P1).

[0316] It is interpreted that the second electrochemical reaction section (R2) is formed by the portion of the electrode layer (A), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) on the upper side of the second gas flow allowance area (P2).

[0317] It is interpreted that the third electrochemical reaction section (R3) is formed by the portion of the electrode layer (A), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) on the upper side of the third gas flow allowance area (P3).

[0318] It is interpreted that the fourth electrochemical reaction section (R4) is formed by the portion of the electrode layer (A), the portion of the electrolyte layer (B), the portion of the reaction prevention layer (G), and the portion of the counter electrode layer (C) above the fourth gas flow allowance area (P4).

[0319] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0320] In addition, in this embodiment, two counter electrode layers (C) are formed spaced apart from each other. Electrochemical reactions can occur through these two counter electrode layers (C) (first counter electrode layer (C1) and second counter electrode layer (C2)), the electrolyte layer (B) (first electrolyte layer (B1) and second electrolyte layer (B2)), and the electrode layer (A) (first electrode layer (A1) and second electrode layer (A2)). Accordingly, it is interpreted that the fifth electrochemical reaction section (R5) is formed by the first electrode layer (A1), the first counter electrode layer (C1), and the portions enclosed therein (first electrolyte layer (B1) and the first reaction prevention layer (G1)).

[0321] It is interpreted that the sixth electrochemical reaction unit (R6) is formed by the second electrode layer (A2), the second counter electrode layer (C2), and the portions clamped thereto (the second electrolyte layer (B2) and the second reaction prevention layer (G2)).

[0322] That is, in this embodiment, a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1).

[0323] <26th Embodiment>

[0324] An electrochemical module (M) according to the present embodiment is shown in FIG. 26. The electrochemical module (M) according to the present embodiment is a module in which the aforementioned electrochemical elements (Q) are arranged in a stacked state. In the electrochemical module (M) according to the 26th embodiment, electrochemical elements (Q) according to the 11th to 25th embodiments, that is, electrochemical elements (Q) in which a plurality of electrochemical reaction parts (R) are electrically connected in parallel are used.

[0325] The electrochemical module (M) is configured with a plurality of electrochemical elements (Q) (Q1, Q2, etc.) and a plurality of current collector plates (S) (S1, S2, etc.). In this embodiment, the electrochemical elements (Q) are described as having the same configuration as in the eleventh embodiment.

[0326] In this embodiment, a current collecting layer (H) is installed on the charged electrode layer (C) of the electrochemical element (Q). As the current collecting layer (H), a ceramic paste or a metal felt material with excellent conductivity is used.

[0327] The current collector plate (S) is a metal plate formed in a wave shape. As the material for the current collector plate (S), the same material as the aforementioned metal substrate (1) can be used. In addition, it is desirable to form a diffusion barrier film identical to that of the metal substrate (1) on the surface of the current collector plate (S) to suppress Cr scattering. The current collector plate (S) configured as described above can be manufactured at low cost by press molding, etc. Furthermore, the current collector plate (S) is composed of a material that does not allow gas to pass between the surface side and the back side.

[0328] As shown in FIG. 26, an electrochemical element (Q) and a current collector plate (S) are alternately stacked and arranged. The upper peak of the waveform of the current collector plate (S) is joined to the back side (5) of the metal substrate (1) while electrically energized. This joining is performed, for example, by applying a ceramic paste with excellent conductivity and pressing the current collector plate (S) toward the metal substrate (1). Alternatively, it is performed, for example, by welding or brazing.

[0329] The lower normal point of the waveform of the current collector plate (S) is joined to the current collection layer (H) of the electrochemical element (Q) while electrically energized. This joining is performed, for example, by sintering the ceramic paste of the aforementioned current collection layer (H) or by applying pressure to the current collector plate (S) with a metal felt.

[0330] With the above configuration, for example, the current collector plate (S) electrically connects the metal substrate (1) of the electrochemical element (Q1) and the current collection layer (H) of the electrochemical element (Q2). In this way, the electrode layer (A) of the electrochemical element (Q1) and the counter electrode layer (C) of the electrochemical element (Q2) are electrically connected. That is, the electrochemical reaction part (R) of the electrochemical element (Q1) and the electrochemical reaction part (R) of the electrochemical element (Q2) are electrically connected in series.

[0331] When a plurality of electrochemical elements (Q) and a plurality of current collector plates (S) are stacked in the form shown in FIG. 26, the current collector plate (S) is electrically connected to the metal substrate (1) of one electrochemical element (Q) and the current collection layer (H) of the electrochemical element (Q) placed below it. In this way, the electrode layer (A) of one electrochemical element (Q) and the counter electrode layer (C) of the electrochemical element (Q) below it are electrically connected. That is, in the electrochemical module (M) according to the present embodiment, the electrochemical reaction parts (R) of a plurality of electrochemical elements (Q) are electrically connected in series by the current collector plate (S).

[0332] As described above, in the electrochemical element (Q), a plurality of electrochemical reaction units (R) are arranged on the surface side (4) of the metal substrate (1). These plurality of electrochemical reaction units (R) (first electrochemical reaction unit (R1) to fourth electrochemical reaction unit (R4)) are electrically connected in parallel. Thus, in the electrochemical module (M) according to the present embodiment, the electrochemical reaction units (R) are electrically connected in parallel to each electrochemical element (Q), and these electrochemical reaction units (R) are electrically connected in series by a current collector plate (S).

[0333] <Other embodiments>

[0334] (1) In the first and second embodiments described above, an insulating film is formed on the surface of the metal substrate (1). However, when a metal material is used in a component other than the metal substrate (1) in relation to the formation of an electrochemical element (Q) or electrochemical module (M), such as a U-shaped member (11) or a cover part (12) that forms a tubular gas flow section (10), an insulating film or a diffusion barrier film may be formed on the surface of such metal material as needed.

[0335] (2) In the above-described embodiment, an electrode layer (A) is placed between the metal substrate (1) and the electrolyte layer (B), and a counter electrode layer (C) is placed on the opposite side of the metal substrate (1) when viewed from the electrolyte layer (B). A configuration in which the electrode layer (A) and the counter electrode layer (C) are placed in the opposite direction is also possible. That is, a configuration in which a counter electrode layer (C) is placed between the metal substrate (1) and the electrolyte layer (B), and an electrode layer (A) is placed on the opposite side of the metal substrate (1) when viewed from the electrolyte layer (B) is also possible. In this case, it is also necessary to change the supply of gas to the electrochemical element (Q). For example, when operating the electrochemical element (Q) as a fuel cell, oxygen is supplied to the counter electrode layer (C) through the gas flow allowance area (P) of the metal substrate (1), and hydrogen is supplied to the electrode layer (A) from the vicinity of the electrochemical element (Q).

[0336] (3) In the above-described embodiment, five (or four) electrochemical reaction units (R) were installed on the metal substrate (1). The number of electrochemical reaction units (R) is not limited to this, and two or more are sufficient.

[0337] (4) In the above-described embodiment, one or two rows of electrochemical reaction units (R) were installed on the metal substrate (1). The number of rows of electrochemical reaction units (R) is not limited to this, and three or more rows are sufficient.

[0338] (5) In the above-described seventh embodiment, a plurality of electrochemical reaction units (R) connected in series are shown in a form where they are connected in parallel, but a plurality of electrochemical reaction units (R) connected in series may also be configured to be connected in series. In addition, a plurality of electrochemical reaction units (R) connected in series may be configured so that both series connection and parallel connection coexist.

[0339] (6) In the eighth embodiment described above, a plurality of electrochemical reaction units (R) connected in parallel are shown in a series configuration, but a plurality of electrochemical reaction units (R) connected in parallel may also be configured to be connected in parallel. In addition, a plurality of electrochemical reaction units (R) connected in parallel may be configured such that series connection and parallel connection coexist.

[0340] (7) In a single electrochemical element (Q), a series connection and a parallel connection of electrochemical reaction units (R) may coexist. For example, an electrochemical element (Q) may be constructed by forming a 4x4 electrochemical reaction unit (R) on a metal substrate (1), connecting four electrochemical reaction units (R) in series within one row, and connecting the electrochemical reaction units (R) at both ends of the row in parallel. Additionally, a plurality of electrochemical reaction units (R) in which such series connection and parallel connection coexist may be applied to the form of (5) or (6) described above.

[0341] (8) In the above-described embodiments, a flat electrochemical element and an electrochemical module were shown, but the electrochemical element and electrochemical module of the present invention may also be applied in a cylindrical or disc shape.

[0342] (9) In the first and second embodiments described above, a U-shaped member (11) and a cover part (12) are bonded to a metal substrate (1) to form a cylindrical gas flow section (10), but a plurality of metal substrates (1) may be used to form a cylindrical gas flow section (10). FIGS. 27 and 28 show an example in which two side bonding members (15) and a cover part (12) are bonded to two metal substrates (1) to form a cylindrical gas flow section (10). The side bonding members (15) are rectangular members. The long sides of the two metal substrates (1) and the long sides of the two side members (15) are bonded, and one end of the formed tube is blocked by the cover part (12). Thus, a flat or flat-shaped cylindrical gas flow section (10) is formed as a whole, having an internal space (22) inside. The metal substrate (1) is arranged parallel to the central axis of the tubular gas flow section (10), and electrochemical reaction sections are provided on both sides of the electrochemical element.

[0343] By using this electrochemical element (Q), the same electrochemical module (M) as shown in the aforementioned seventh embodiment can be constructed.

[0344] (10) In the above-described embodiment, the through hole (2) formed by penetrating the surface side (4) and the back side (5) of the metal substrate (1) is connected so that gas can flow between the surface side (4) and the back side (5), and its arrangement is not limited to being formed at the intersection of a grid parallel to the long side and the short side as shown in FIGS. 1 to 4, nor is it limited to being a circular hole perpendicular to the plate surface of the metal substrate (1) as shown in FIGS. 1 to 4 and FIGS. 11 to 26. The diameter of the through hole (2) does not have to be constant and may be tapered. Also, the through hole (2) may be curved.

[0345] (11) In the above-described embodiment, the gas flow prohibition area is formed by creating an area that does not form a through hole, but it can also be formed by first forming a through hole and then blocking at least a portion of the through hole. As a method of blocking the through hole, it can be formed by filling the through hole with a sealing material, or by joining or bonding a blocking material (16) that does not form a through hole on one side of a metal substrate as shown in FIG. 29.

[0346] (12) In the above-described embodiments 1, 3, 11 to 26, the gas flow-allowing region (P) is arranged to be covered by the electrode layer (A), but as shown in FIG. 30 (showing only a single electrochemical reaction part), the electrolyte layer (B) is arranged to cover at least the gas flow-allowing region (P) or the electrode layer (A) installed in the gas flow-allowing region (P). By doing so, the gas supplied to the electrode layer by passing through the gas flow-allowing region from the back side of the metal substrate can be suppressed from leaking to the surface side of the metal substrate, and the performance and reliability as an electrochemical device can be improved.

[0347] (13) In the above-described embodiment, an example was described in which the electrochemical elements (Q) in the electrochemical module (M) are arranged in a stacked state, that is, in a multiple assembled state. As for the electrochemical module (M), it is also possible to have the electrochemical elements (Q) assembled in a non-stacked state.

[0348] (14) An electrochemical element may be configured as follows. The electrochemical element has a metal substrate and a plurality of electrochemical reaction units, the metal substrate has a gas flow allowance area that allows gas flow between the surface side and the back side of the metal substrate, the electrochemical reaction unit has at least an electrode layer, an electrolyte layer, and a counter electrode layer, and is disposed on the surface side of the metal substrate, the electrolyte layer is disposed between the electrode layer and the counter electrode layer, and gas that has flowed through the gas flow allowance area is supplied to the electrode layer.

[0349] (15) In addition, the electrochemical element may have the following configuration. The metal substrate has a plurality of gas flow-allowing regions spaced apart from each other, and the electrolyte layer of the electrochemical reaction part is disposed to cover the entirety of each of the gas flow-allowing regions.

[0350] (16) In addition, the electrochemical element may have the following configuration. The metal oxide film is an oxide of a metal element contained in the metal substrate.

[0351] Furthermore, the configuration disclosed in the aforementioned embodiments (including other embodiments; hereinafter the same) may be applied in combination with the configuration disclosed in other embodiments, provided that no contradiction arises. Additionally, the embodiments disclosed in this specification are examples, and the embodiments of the present invention are not limited thereto, and may be appropriately modified within the scope of the purpose of the present invention. Explanation of the symbols

[0352] 1: Metal substrate 3: Insulating film (metal oxide film) 4: Surface side 5: Backside 6: Diffusion barrier (metal oxide film) A: Electrode layer B: Electrolyte layer C: Daejeon polar layer M: Electrochemical Module N: Gas flow prohibited area P: Allowable gas flow area Q: Electrochemical device R: Electrochemical reaction unit Y: Electrochemical device Z: Energy System

Claims

Claim 1 An electrochemical element unit comprising at least one flat metal substrate and a connecting member, wherein the metal substrate has a plurality of electrochemical reaction sections on the surface side thereof, the metal substrate has a gas flow allowance region that allows gas flow between the surface side and the back side thereof, the electrochemical reaction section has at least an electrode layer, a gastight electrolyte layer, and a counter electrode layer, and is disposed on the surface side thereof, and the electrolyte layer is disposed at least between the electrode layer and the counter electrode layer, and the connecting member has a first gas flow path formed on the surface side surface, and is disposed such that the surface side surface and the back side surface of the metal substrate face each other, and the electrode layer is disposed to cover the gas flow allowance region in an area larger than the gas flow allowance region, and also, the electrolyte layer is disposed to cover the top and periphery of the electrode layer in an area larger than the electrode layer, or, the electrode layer is disposed on the gas flow allowance region, and also, the An electrochemical device unit comprising: an electrolyte layer disposed to cover the top and periphery of the electrode layer in an area larger than the gas flow-allowing area, and also to cover the gas flow-allowing area; the electrode layer contacts a gas that passes through the gas flow-allowing area by passing through the first gas flow path of the connecting member; and the counter electrode layer configured to at least contact a gas different from the gas that the electrode layer contacts. Claim 2 In claim 1, the connecting member is an electrochemical element unit that does not have gas permeability. Claim 3 In claim 1 or 2, the connecting member is an electrochemical element unit having conductivity. Claim 4 An electrochemical element unit according to claim 1 or 2, wherein the metal substrate has a plurality of gas flow-allowing regions spaced apart from each other. Claim 5 An electrochemical device unit according to claim 1 or 2, wherein the electrolyte layer separates the gas contacted by the electrode layer from the gas contacted by the counter electrode layer. Claim 6 An electrochemical element unit according to claim 1 or 2, wherein the plurality of electrochemical reaction parts are formed spaced apart from each other. Claim 7 An electrochemical device unit according to claim 1 or 2, wherein a metal oxide film is formed in at least the region where the metal substrate and the electrode layer are in contact on the surface side of the metal substrate. Claim 8 An electrochemical device unit according to claim 1 or 2, wherein a metal oxide film is formed in an area on the surface side of the metal substrate that is not covered by at least the electrode layer, the electrolyte layer, and the counter electrode layer. Claim 9 An electrochemical device unit according to claim 7, wherein the metal oxide film is an oxide containing a metal element included in at least the metal substrate. Claim 10 An electrochemical element unit according to claim 1 or 2, wherein a plurality of the electrochemical reaction units are electrically connected in parallel. Claim 11 An electrochemical module in which a plurality of electrochemical element units described in paragraph 1 are arranged in a assembled state. Claim 12 In claim 11, the above-mentioned connecting member has a second gas flow path formed on its rear side, and the electrochemical module is arranged such that a gas flowing through the second gas flow path of one electrochemical element unit comes into contact with the counter electrode layer of an adjacent other electrochemical element unit. Claim 13 An electrochemical device having an electrochemical element unit described in claim 1 or an electrochemical module described in claim 11, and a fuel supply unit that supplies a fuel gas containing a reducing component to said electrochemical element unit or said electrochemical module. Claim 14 An electrochemical device having an electrochemical element unit described in claim 1 or an electrochemical module described in claim 11, and an inverter that extracts power from said electrochemical element unit or said electrochemical module. Claim 15 An energy system having an electrochemical device described in paragraph 13 and a heat utilization unit that reuses heat discharged from the electrochemical device. Claim 16 A solid oxide type fuel cell unit comprising an electrochemical element unit described in claim 1 or 2, wherein the electrochemical element unit generates a power generation reaction. Claim 17 A solid oxide type electrolytic cell unit comprising an electrochemical element unit described in claim 1 or 2, wherein the electrochemical element unit causes an electrolytic reaction. Claim 18 delete Claim 19 delete Claim 20 delete

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