# US 10,480,082 B2 · High-temperature, low-temperature—gradient methods for (CO-)electrolysis of water (SOEC) or for producing electricity within a reactor or fuel-cell stack (SOFC) respectively

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- Number: US 10,480,082 B2
- Document ID: US10480082B2
- Status: Granted
- Kind: B2
- Application number: 15/751,319
- Filed: 2016-08-12
- Published: 2018-08-23
- Granted: 2019-11-19
- Earliest claimed: 2015-08-12
- Assignees: Commissariat A L'energie Atomique Et Aux Energies Alternatives
- Applicants: Commissariat A L'energie Atomique Et Aux Energies Alternatives
- Inventors: Magali Reytier; Nicolas Bardi
- Web page: https://patentgrep.com/patent/US10480082B2

## CPC

- C25B 1/04: by electrolysis of water
- C25B 1/00: Electrolytic production of inorganic compounds or non-metals
- C25B 1/042: by electrolysis of steam
- C25B 1/23: Carbon monoxide or syngas
- C25B 9/65: Means for supplying current; Electrode connections; Electric inter-cell connections
- C25B 9/70: Assemblies comprising two or more cells
- C25B 9/73: of the filter-press type
- C25B 15/08: Supplying or removing reactants or electrolytes; Regeneration of electrolytes
- C25B 15/083: {Separating products}
- H01M 8/04298: Processes for controlling fuel cells or fuel cell systems
- H01M 8/12: operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M 8/249: comprising two or more groupings of fuel cells, e.g. modular assemblies
- H01M 2008/1293: {Fuel cells with solid oxide electrolytes}
- Y02E 60/36: Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
- Y02E 60/50: Fuel cells
- Y02P 20/129: Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- C25B: ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR (anodic or cathodic protection C23F13/00; single-crystal growth C30B)
- 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

The invention essentially consists in supplying fuel (either steam or a mixture of steam with CO2 or H2 or CH4) to distinct zones of a cell or a group of stacked cells and of an adjacent cell or group of adjacent stacked cells within a given (co-)electrolysis reactor or a SOFC fuel-cell stack.

## Claims

### Claim 1

A method for high-temperature electrolysis of steam, or for co-electrolysis of steam and of carbon dioxide, implemented in a reactor comprising:
a stack of individual electrolysis cells of a solid oxide type, each comprising a cathode, an anode and an electrolyte inserted between the cathode and the anode, and
a plurality of electrical and fluid interconnectors, each arranged between two adjacent individual electrolysis cells with one face thereof in electrical contact with the anode of one of the two adjacent individual electrolysis cells and the other face thereof in electrical contact with the cathode of the other of the two adjacent individual electrolysis cells, the method comprising:
supplying a first zone of each electrical and fluid interconnector of a first group with steam or with a mixture of steam and of carbon dioxide, and distributing it to a cathode of each individual electrolysis cell of the first group, then recovering hydrogen produced or a synthesis gas, which is a mixture of carbon monoxide and of hydrogen in a second zone of the each electrical and fluid interconnector of the first group, and
supplying a first zone of each electrical and fluid interconnector of a second group, at least one of which is adjacent to the electrical and fluid interconnector of the first group, with steam or with a mixture of steam and of carbon dioxide, and distributing it to a cathode of each individual electrolysis cell of the second group, at least one of which is adjacent to the electrolysis cell of the first group, then recovering hydrogen produced or a synthesis gas, which is a mixture of carbon monoxide and of hydrogen in a second zone of the each electrical and fluid interconnector of the second group, the first and second zones of the electrical and fluid interconnectors of the second group not being located vertically in line respectively with the first and second zones of the electrical and fluid interconnectors of the first, group,
wherein, within the stack, the supplying and a circulation respectively to the electrical and fluid interconnectors and to the electrolysis cells of the first group are carried out independently relative to the supplying and a circulation respectively to the electrical and fluid interconnectors and to the electrolysis cells of the second group.

### Claim 2 (depends on 1)

The method of claim 1, wherein the first and second zones of the electrical and fluid interconnectors of the first and second groups are arranged such that the distributing the steam or of the mixture of steam and of carbon dioxide to the cathode of the electrolysis cells of the first group is carried out in co-current to the to the electrolysis cells of the second group.

### Claim 3 (depends on 1)

The method of claim 1, wherein the first and second zones of the first and second groups of the electrical and fluid interconnectors are arranged such that the distributing the steam or of the mixture of steam and of carbon dioxide to the cathode of the electrolysis cells of the first group is carried out in counter-current to the distributing to the electrolysis cells of the second group.

### Claim 4 (depends on 1)

The method of claim 1, the method further comprising:
supplying a third zone of the each electrical and fluid interconnector of the first group with a draining gas, and distributing it to the anode of the each electrolysis cell of the first group, then recovering oxygen produced and, where appropriate, the draining gas in a fourth zone of the each electrical and fluid interconnector of the first group, and
supplying a third zone of the each electrical and fluid interconnector of the second group with a draining gas, and distributing it to the anode of the each electrolysis cell of the second group, then recovering oxygen produced and, where appropriate, the draining gas in a fourth zone of the each electrical and fluid interconnector of the second group, the third and fourth zones of the electrical and fluid interconnectors of the second group being located vertically in line respectively with the third and fourth zones of the electrical and fluid interconnectors of the first group, so as to have a supply of draining gas and a recovery of oxygen produced which are common to the first and second groups.

### Claim 5 (depends on 1)

The method of claim 1, the method further comprising:
supplying a third zone of the each electrical and fluid interconnector of the first group with a draining gas, and distributing it to the anode of the each electrolysis cell f the first group, then recovering oxygen produced and, where appropriate, the draining gas in a fourth zone of the each electrical and fluid interconnector of the first group, and
supplying a third zone of the each electrical and fluid interconnector of the second group with a draining gas, and distributing it to the anode of the each electrolysis cell of the second group, then recovering oxygen produced and, where appropriate, the draining gas in a fourth zone of the each electrical and fluid interconnector of the second group, the third and fourth zones of the electrical and fluid interconnectors of the second group not being located vertically in line respectively with the third and fourth zones of the electrical and fluid interconnectors of the first group, so as to have a supply of draining gas and a recovery of oxygen produced which are separate between the first group and the second group.

### Claim 6 (depends on 5)

The method of claim 5, wherein the third and fourth zones of the electrical and fluid interconnectors of the first and second groups are arranged such that the distributing the draining gas and of the oxygen produced by electrolysis at the anode of the electrolysis cells of the first group is carried out in counter-current to the distributing the electrolysis cells of the second group.

### Claim 7

A method for producing electricity a high temperature, implemented in a solid oxide fuel cell comprising:
a stack of individual electrochemical cells of an SOFC type, each comprising a cathode, an anode and an electrolyte inserted between the cathode and the anode, and
a plurality of electrical and fluid interconnectors, each arranged between two adjacent individual electrochemical cells with one face thereof in electrical contact with the anode of one of the two adjacent individual electrochemical cells and the other face thereof in electrical contact with the cathode of the other of the two adjacent individual electrochemical cells, the method comprising:
supplying a first zone of each electrical and fluid interconnector of a first group with fuel, and distributing it to an anode of each individual electrochemical cell of the first group, then recovering surplus fuel and water produced in a second zone of the each electrical and fluid interconnector of the first group, and
supplying a first zone of each electrical and fluid interconnector of a second group, at least one of which is adjacent to the each electrical and fluid interconnector of the first group, with fuel, and distributing it to an anode of each individual electrochemical cell of the second group, at least one of which is adjacent to the electrochemical cell of the first group, then recovering surplus fuel and ater produced in a second zone of the each electrical and fluid interconnector of the second group, the first and second zones of the electrical and fluid interconnectors of the second group not being located vertically in line respectively with the first and second zones of the electrical and fluid interconnectors of the first group,
wherein, within the stack, the supplying and a circulation respectively to the electrical and fluid interconnectors and to the electrochemical cells of the first group are carried out independently relative to the supplying and circulation respectively to the electrical and fluid interconnectors and to the electrochemical cells of the second group.

### Claim 8 (depends on 7)

The method of claim 7, wherein the first and second zones of the electrical and fluid interconnectors of the first and second groups are arranged such that the distributing the fuel to the anode of the electrochemical cells of the first group is carried out in co-current to the distributing to the electrochemical cells of the second group.

### Claim 9 (depends on 7)

The method of claim 7, wherein the first and second zones of the first and second groups of the electrical and fluid interconnectors are arranged such that the distributing the fuel to the anode of the electrochemical cells of the first group is carried out in counter-current to the distributing to the electrochemical cells of the second group.

### Claim 10 (depends on 7)

The method of claim 7, the method further comprising:
supplying a third zone of the each electrical and fluid interconnector of the first group with an oxidizer, and distributing it to the cathode of the each, electro chemical cell of the first group, then recovering surplus oxidizer in a fourth zone of the each electrical and fluid interconnector of the first group, and
supplying a third zone of the each electrical and fluid interconnector of the second group with an oxidizer such, and distributing it to the cathode of the each electrochemical cell of the second group, then recovering the surplus oxidizer in a fourth zone of the each electrical and fluid interconnector of the second group, the third and fourth zones of electrical and fluid interconnectors of the second group being located vertically in line respectively with the third and fourth zones of electrical and fluid of the first group interconnectors, so as to have a supply of oxidizer and a recovery of surplus oxidizer which are con on to the first and second groups.

### Claim 11 (depends on 7)

The method of claim 7, the method further comprising:
supplying a third zone of the each electrical and fluid interconnector of the first group with an oxidizer, and distributing it to the cathode of the each electrochemical cell of the first group, there recovering surplus oxidizer in a fourth zone of the each electrical and fluid interconnector of the first group, and
supplying a third zone of the each electrical and fluid interconnector of the second group with an oxidizer, and distributing it to the cathode of the each electrochemical cell of the second group, then recovering surplus oxidizer in a fourth zone of the each electrical and fluid interconnector of the second group, the third and fourth zones of electrical and fluid interconnectors of the second group not being located vertically in line respectively with the third and fourth zones of electrical and fluid interconnectors of the first group, so as to have a supply of oxidizer and a recovery of surplus oxidizer which are separate between the first group and the second group.

### Claim 12 (depends on 11)

The method of claim 11, wherein the third and fourth zones of electrical and fluid interconnectors of the first and second group are arranged such that the distributing the oxidizer to the cathode of the electrochemical cells of the first group is carried out in counter-current to the distributing the electrochemical cells of the second group.

### Claim 13 (depends on 7)

The method of claim 7, wherein the fuel is hydrogen, methane or both hydrogen and methane.

### Claim 14 (depends on 1)

The method of claim 1, wherein supplies of gases in the first zone of the electrical and fluid interconnectors of the first group is connected in series to supplies of gases in the first zone of the electrical and fluid interconnectors of the second group.

### Claim 15 (depends on 14)

The method of claim 14, wherein the gases are enriched in a fuel and/or in an oxidizer between an outlet of the first group and an inlet of the second group, or vice-versa.

### Claim 16 (depends on 14)

The method of claim 14, wherein the electrolysis cells of different sizes between the first and the second groups are used, so that all the electrolysis cells are at the same voltage with different fuel compositions.

### Claim 17 (depends on 1)

The method of claim 1, wherein supplies of gases in the first zone of the electrical and fluid interconnector of the first group is in parallel to supplies of gases in the first zone the electrical and fluid interconnector of the second group.

### Claim 18 (depends on 17)

The method of claim 17, wherein the first and second group supplied with same compositions and same flow rates of gas.

### Claim 19 (depends on 17)

The method of claim 17, wherein the first and the second group are supplied with different compositions of methane or hydrogen so as to have different reforming between the first and the second groups.

### Claim 20 (depends on 7)

The method of claim 7, wherein
wherein supplies of gases in the first zone of the electrical and fluid interconnector of the first group is in parallel to supplies of gases in the first zone of the electrical and fluid interconnector of the second group, and
the first and the second group are supplied with a same H2O/CO2/CO ratio.

### Claim 21 (depends on 14)

The method claim 14, wherein, in operation, the supplies in series are changed into supplies in parallel, and
wherein flow rates and compositions are simultaneously made different between the first and the second groups so as to manage a premature degradation of the electrolysis cells of one of the first and the second groups.