# US 10,122,023 B2 · Fuel cell with separator, method for manufacturing same, and fuel cell stack

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- Number: US 10,122,023 B2
- Document ID: US10122023B2
- Status: Granted
- Kind: B2
- Application number: 14/423,610
- Filed: 2013-08-26
- Published: 2015-11-05
- Granted: 2018-11-06
- Earliest claimed: 2012-08-31
- Assignees: Ngk Spark Plug Co., Ltd.
- Applicants: Ngk Spark Plug Co., Ltd.
- Inventors: Makoto Kuribayashi; Etsuya Ikeda; Wataru Matsutani; Yosuke Yatsuya; Masaaki Murase
- Web page: https://patentgrep.com/patent/US10122023B2

## CPC

- H01M 8/0206: Metals or alloys
- H01M 8/0247: characterised by the form (characterised by a channel configuration H01M8/0258)
- H01M 8/0273: with sealing or supporting means in the form of a frame
- H01M 8/0282: Inorganic material
- H01M 8/1004: characterised by membrane-electrode assemblies [MEA] (H01M8/12 takes precedence)
- H01M 8/1246: the electrolyte consisting of oxides
- H01M 2008/1293: {Fuel cells with solid oxide electrolytes}
- H01M 2300/0074: Ion conductive at high temperature
- Y02E 60/50: Fuel cells
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A fuel cell with separator includes a fuel cell body having a cathode, an anode, and a solid electrolyte layer disposed between the cathode and the anode; a plate-like metal separator having first and second main surfaces and an opening which opens at the first and second main surfaces; a joint formed of an Ag-containing brazing filler metal and adapted to join the fuel cell body and the first main surface of the metal separator; and a seal formed of a glass-containing sealing material and disposed closer to the opening than is the joint, the seal being located between the first main surface and the fuel cell body and extending along the entire perimeter of the opening.

## Claims

### Claim 1

A fuel cell with separator comprising
a fuel cell body having a cathode, an anode, and a solid electrolyte layer disposed between the cathode and the anode;
a plate-like metal separator having first and second main surfaces and an opening which opens at the first and second main surfaces;
a joint formed of an Ag-containing brazing filler metal and adapted to join the fuel cell body and the first main surface of the metal separator; and
a seal formed of a glass-containing sealing material and disposed closer to the opening than is the joint, the seal being located between the first main surface and the fuel cell body and extending along the entire perimeter of the opening and having a sealing part,
wherein the sealing part is in contact with the first main surface of the metal separator,
and wherein the seal is disposed closer to the opening than all joints so as to hinder the flow of oxidizer gas to the metal of all joints.

### Claim 2 (depends on 1)

A fuel cell with separator according to claim 1, wherein
the joint has a first joint portion and a second joint portion located closer to the opening than is the first joint portion, and
the second joint portion is lower in oxygen diffusion coefficient than the first joint portion.

### Claim 3 (depends on 1)

A fuel cell with separator according to claim 1, wherein the metal separator contains Al in an amount of 0.1% by mass to 10% by mass.

### Claim 4 (depends on 1)

A fuel cell with separator according to claim 1, wherein the metal separator has a thickness of 0.5 mm or less.

### Claim 5 (depends on 1)

A fuel cell with separator according to claim 1, wherein a gap exists between the joint and the seal.

### Claim 6 (depends on 1)

A fuel cell with separator according to claim 1, wherein the brazing filler metal is higher in melting temperature than the sealing material.

### Claim 7 (depends on 1)

A fuel cell with separator according to claim 1, wherein a portion of the seal located toward the joint has an Ag-containing mixed layer.

### Claim 8 (depends on 7)

A fuel cell with separator according to claim 7, wherein in the mixed layer, Ag content is highest at a portion located toward the joint.

### Claim 9 (depends on 7)

A fuel cell with separator according to claim 7, wherein the joint and the mixed layer are disposed along the entire perimeter of the opening.

### Claim 10 (depends on 7)

A fuel cell with separator according to claim 7, wherein the seal has a thermal expansion coefficient of 8 ppm/K to 12 ppm/K within a temperature range of room temperature to 300° C., and the mixed layer has a width of 50 μm or more.

### Claim 11 (depends on 7)

A fuel cell with separator according to claim 7, wherein the joint contains an oxide whose oxygen dissociation pressure is lower than 1×10−13 Pa at 800° C.

### Claim 12 (depends on 11)

A fuel cell with separator according to claim 11, wherein the oxide contained in the joint is of Al or In.

### Claim 13 (depends on 1)

A fuel cell with separator according to claim 1, wherein
the metal separator contains Al in an amount of 1.5% by mass to 10% by mass;
the joint contains an oxide or compound oxide of Al in an amount of 1% by volume to 25% by volume; and
the seal contains Al in an amount of 1% by mass to 30% by mass as reduced to Al2O3.

### Claim 14 (depends on 13)

A fuel cell with separator according to claim 13, wherein
the metal separator contains Al in an amount of 2% by mass to 10% by mass;
the joint contains an oxide or compound oxide of Al in an amount of 2% by volume to 15% by volume; and
the seal contains Al in an amount of 2% by mass to 20% by mass as reduced to Al2O3.

### Claim 15 (depends on 13)

A fuel cell with separator according to claim 13, wherein at least a portion of the oxide or compound oxide of Al is disposed at the interface between the metal separator and the joint.

### Claim 16 (depends on 13)

A fuel cell with separator according to claim 13, wherein the oxide or compound oxide of Al is Al2O3, an Al-containing spinel-type oxide, or mullite.

### Claim 17 (depends on 13)

A fuel cell with separator according to claim 13, further comprising a restraint formed of the same material as the sealing material and disposed on the second main surface of the metal separator at a position opposite the seal.

### Claim 18 (depends on 17)

A fuel cell with separator according to claim 17, wherein the seal and the restraint are integrated through a connection disposed on a side surface of the opening of the metal separator.

### Claim 19 (depends on 1)

A fuel cell with separator according to claim 1, further comprising a restraint formed of the same material as the sealing material or a material higher in thermal expansion coefficient than the sealing material and disposed on the second main surface of the metal separator at a position opposite the seal.

### Claim 20 (depends on 19)

A fuel cell with separator according to claim 19, wherein the restraint is disposed along the entire perimeter of the opening.

### Claim 21 (depends on 19)

A fuel cell with separator according to claim 19, wherein the seal and the restraint are integrated through a connection disposed on a side surface of the opening of the metal separator.

### Claim 22 (depends on 19)

A fuel cell with separator according to claim 19, wherein a material of the restraint is lower in thermal expansion coefficient than the metal separator.

### Claim 23 (depends on 19)

A fuel cell with separator according to claim 19, wherein a gap exists between the seal and the joint.

### Claim 24 (depends on 19)

A fuel cell with separator according to claim 19, wherein the sealing material has a thermal expansion coefficient of 8 ppm/K to 12 ppm/K within a temperature range of room temperature to 300° C.

### Claim 25 (depends on 1)

A fuel cell stack comprising a fuel cell with separator according to claim 1.

### Claim 26

A method for manufacturing a fuel cell with separator, the fuel cell with separator comprising
a fuel cell body having a cathode, an anode, and a solid electrolyte layer disposed between the cathode and the anode;
a plate-like metal separator having first and second main surfaces and an opening which opens at the first and second main surfaces;
a joint formed of an Ag-containing brazing filler metal and adapted to join the fuel cell body and the first main surface of the metal separator; and
a seal formed of a glass-containing sealing material and disposed closer to the opening than is the joint, the seal being located between the first main surface and the fuel cell body and extending along the entire perimeter of the opening and having a sealing part,
wherein the sealing part is in contact with the first main surface of the metal separator,
and wherein the seal is disposed closer to the opening than all joints so as to hinder the flow of oxidizer gas to the metal of all joints;
the method comprising:
disposing an Ag-containing brazing filler metal on both of the metal separator and the fuel cell body, and
disposing the glass-containing sealing material on at least one of the metal separator on which the brazing filler metal is disposed, and the fuel cell body on which the brazing filler metal is disposed.

### Claim 27 (depends on 26)

A method for manufacturing a fuel cell with separator according to claim 26, further comprising
joining the metal separator and the fuel cell body by melting the brazing filler metal disposed on both of the metal separator and the fuel cell body.

### Claim 28 (depends on 27)

A method for manufacturing a fuel cell with separator according to claim 27, wherein
in the joining, the brazing filler metal is melted in the atmosphere.

### Claim 29 (depends on 28)

A method for manufacturing a fuel cell with separator according to claim 28, further comprising
forming the seal by melting the glass-containing sealing material disposed on at least one of the metal separator and the fuel cell body.

### Claim 30 (depends on 29)

A method for manufacturing a fuel cell with separator according to claim 29, wherein
the joining and the forming are performed simultaneously.

### Claim 31 (depends on 29)

A method for manufacturing a fuel cell with separator according to claim 29, wherein after the joining, the disposing and the forming are performed.
