CA2058054C - Method of separating hydrogen isotope - Google Patents
Method of separating hydrogen isotope Download PDFInfo
- Publication number
- CA2058054C CA2058054C CA002058054A CA2058054A CA2058054C CA 2058054 C CA2058054 C CA 2058054C CA 002058054 A CA002058054 A CA 002058054A CA 2058054 A CA2058054 A CA 2058054A CA 2058054 C CA2058054 C CA 2058054C
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- Canada
- Prior art keywords
- hydrogen
- water
- isotope
- tritium
- enriched
- Prior art date
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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- Fuel Cell (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
A method of a hydrogen isotope is disclosed. This method uses an isotope exchange reaction between water and hydrogen, in which oxgen is electrochemically transferred from water to be enriched with a heavy isotope to hydrogen to be enriched with a light isotope, thereby permitting separation of a hydrogen isotope with a largely reduced electric power consumption, not requiring electric power supply, or with a gain of electric power.
Description
METHOD OF SEPARATING HYDROGEN ISOTOPE
[FIELD OF THE INVENTION]
The present invention relates to a method of separating a hydrogen isotope. More particularly, the present invention relates to a method of separating a hydrogen isotope, which is useful for separation, enrichment and removal of tritium in a nuclear fusion reactor, upgrading of heavy water and enrichment and removal of tritium in a heavy water reactor, separation and removal of tritium in nuclear fuel reprocessing, and separation, recovery and removal of tritium used in a usual test or research, and further, separation of the other hydrogen isotope except for tritium in a manufacture of heavy water.
[DESCRIPTION OF THE PRIOR ARTJ
The method of separating a hydrogen isotope based on isotope exchange reaction between water and hydrogen is advantageous in that the separation coefficient is high in the state of equilibrium, permitting an achievement of a very high separatiing performance using a single apparatus because of the possibility of constituting a counter-current-type reaction tower, and because chemically easy-to-handle substances such as water and hydrogen are only used. While this is a hopeful method for the manufacture of heavy water, removal and recovery of tritium from water containing tritium oxides (hereinafter tritium water), it requires a step of repeating to reduce water to be enriched with a heavy isotope (for example, heavy hydrogen ~QS~Q~ 9~
~r tritium relative to light hydrogen) to hydrogen, and the electric power consumption in electrolysis used fox this purpose is one of the serious uroblems.
rr~ia.1 illustrates one of the embodiments of the conventional method of separating tritium water based or_ the combination of a counter-current-type isotope exchange reaction tower and an electrolytic cell. As shown in rig. l, tritium Water as a raw material is supplied through a raw material inlet port (2) into an exchange reaction tower (1), enriched in the reaction tower (1), and sent through an enriched water outlet port (3) to an electrolytic cell (8). In the electrolytic cell (8), tritium water is decomposed into hydrogen and oxygen containing tritium at a high concentration, a part of hydrogen is taken out as a product, and the remaining part is fed through a hydrogen inlet port (4) into the exchange reaction tower (1).
On the other hand, oxygen, which contains tritium water vapor in the original state, is sub,~edted to remove tritium water through a water separator (10), and then sent into a hydrogen recombinator ('1) by way of an oxygen feed line. After hydrogen has tritium transfer into water in the exchange reaction tower (1), hydrogen is sent through a hydrogen outlet port (5) into the hydrogen recombinator ('I) where hydrogen is oxidized. A
part of thus-produced water is dumpted as depleted water or cleaned water, and the remaining part is fed again through a depleted water inlet port (6) into the exchange reaction tower (1).
In such a conventional method, for example, oxidation ~0~~~3'.:~
of hydrogen and decomposition of water shoud be continuously carried out to keep the flows of hydrogen and water to be necessitated for isotope separation. The method is particularly defective in that it reauires a large amount of electric power for the decomposition of water, and this seriously results in preventing the practical application.
The present invention has an object to provide a new method which permits saving electric power consumption in the step of repeating to reduce water to be enriched with a heavy isotope to hydrogen, and does not even reauire electric power for the decomposition of water.
Other objects, features and advantages of the present invention will be apparent from the following description taken in connection with the accompanying drawings.
[BRLEF DESCRIPTION OF THE DRAWINGS
Fig.l illustrates one of the embodiments of the conventional method of separating tritium water based on the combination of a counter-current-type isotope exchange reaction tower and an electrolytic cell;
Fig.2 illustrates one of the embodiments of the present invention in which an apparatus for transferring oxygen from water to hydrogen is used;
Fig.3 depicts another embodiment of the present invention in which a fuel cell as a recombinator is used; and Fig.4 depicts further another embodiment of the present invention in which an oxidizing/reducing agent is used as a parameter for the reduction of water and oxidation of hydrogen. ' (DETAILED DESCRIPTION OF ThB EMBODIMENTS]
According to the present invention, it is possible to separate a hydrogen isotope With almost no consumption of electric power for the water decomposition step, or in some cases, even with a gain of power.
The present invention is described below further in detail with a separation of tritium from tritium water as an example.
Fig.2 illustrates one of the embodiments in which an apparatus simultaneously carrying out to convert water to hydrogen and from hyarogen to water through transferrig oxygen from watex to be enriched with a heavy isotope to hydrogen to be enriched with a light isotope is combined with a Water-hydrogen isotope exchange tower. More specifically, Fig.2 indicates a concrete case where tritium water is enriched using an oxygen ion conductive solid electrolytic cell as a water-hydrogen converter. Tritium water as a raw material is supplied through a raw material Water inlet port (12) to a water-hydrogen isotope exchange reaction tower (11), enriched in this reaction tower (11), and sent through an enriched water outlet port (13) to a water-hydrogen exchanger (1'1). A part of the produced hydrogen is taken out as a product, and the remaining part is sent back through a hydrogen inlet port (14) to the exchange reaction tower (11). Hydrogen has tritium transfer to water in the exchange reaction tower (11), and is sent through a hydrogen - a -2~a~~~~
cutlet port (15) to the water-hydrogen converter (1Z), converted into deleted water. The resultant depleted water is rejected or supplied again through a depleted water inlet port (16) to the exchange reaction tower (11). The hydrogen isotope in tritium water is continuously separated during the process as described above. The water-hydrogen converter (1?) supplies water enriched with a heavy isotope on one side of an oxygen ion conductive solid electrolytic barrier membrane (18), and hydrogen enriched with a light isotope on the other side of that. When a barrier membrane having a nature of permitting permeation or' oxygen comes in contact with water on one side thereof, and with hydrogen on the other side, the difference in oxygen potential causes oxygen transfer from water to hydrogen.
This results in simultaneous conversions of oxygen from water to hydrogen and from hydrogen to water. These conversions are never mixed up each other because hydrogen isotopes are seperated through the barrier membrance. Since these conversions take place spontaneously to some extent, it is usually unecessary to supply electric power, but oxygen may forcedly be transferred to the hydrogen side by applying voltage onto the both sides of the barrier membrance.
The electric power reauired for this transfer of oxygen is far smaller than that reauired for conventional electrolysis.
It is thus possible to separate a hydrogen isotope and to consume almost no electric power by the combination of the isotope exchange reaction and a solid electrolytic cell.
The above-mentioned embodiment is involved in a method In which electrolysis and recombination reaction are carried out in a single apparatus. It is also possible to achieve those with separate apparatuses.
Fig.3 shows a process of electrolyzing water with the use of electric power produced when the recombination reaction is utilized in generation or a fuel cell. In Fig.3, while an isotope exchange reaction tower (11) is the same as shown in Fig.2, hydrogen enriched with a light isotope is sent through the hydrogen outlet port (15) to a hydrogen oxygen fuel cell (19), and water enriched with a heavy isotope is sent through an enriched water outlet port (13) to an electrolytic cell (20), respectively. In the case where an oxygen ion conductive solid electrolytic cell as shown in Fig.2 is used as that electrolytic cell (20), the generating oxygen is so highly pure that water and hydrogen are not contaminated by tritium even when supplying the oxygen to the fuel cell (19). Oxidation of hydrogen in the fuel cell (19) spontaneously ocurrs and proceeds, enabling to take out electric power. The electric cell (20) is operated with this electric power. Because the amount of water supplied to the electrolytic cell (20) is almost eaual to that of hydrogen supplied to the fuel cell (19), the amount of electric generation of the fuel cell (19) serves the electric power necessary for electrolysis, if electric loss is disregarded.
Furthermore, while decomposition of water in the electrolytic cell (20) operated at a high temperature of about 900°C reauires a voltage of about 0.9 V, the electro motive force or' the hydrogen oxygen fuel cell (19) operated at the room temperature ~fl5~~~~
is about 1.2 V. It is therefore theoretically possible to achieve a gain of electric power by appropriately setting these operating temperatures.
Fig.4 depicts one of the embodiments in which energy is tran3ferred through an aapropriate oxidation/reduction agent from an oxidation step of rydrogen to a reduction step of water.
For example, a water gas equilibrium (H20 + CO = H2 + C02) is now explained as follows: Hydrogen enriched with a light isotope from the isotope exchange reaction tower (11) is sent through the hydrogen outlet port (15) to a hydrogen oxidation reactor (21), and water enriched with a heavy isotope is sent through the enriched water outlet port (13) to a water reduction reactor (22), respectively. As a water gas eauilibrium(H20 + CO
- H2 + C02) reaction is a reversible equilibrium reaction, hydrogen and carbon dioxide are produced until the ea_uilibrium is reached when water and carbon monoxide are supplied to the water reduction reactor (22). On the other hand, water and carbon monoxide are produced when hydrogen and carbon dioxide are supplied to the hydrogen oxidation reactor (21).
By separating carbon dioxide anti carbon monoxide from those reactors and circulating the same, it is possible to supply water and hydrogen to the water-hydrogen isotope exchange reaction tower (11) through oxidation of hydrogen and reduction of water almost without energy consumption. In the practical application of this embodiment, the steps of separating carbon monoxide and carbon dioxide from water and hydrogen may be omitted by using an oxygen ion conductive solid electrolytic .:ell as shown in Fig.2 for the reactors (21) and (22).
It is needless to mention that various embodiments of the present invention are possible in details of the constitution thereof.
_ g _
[FIELD OF THE INVENTION]
The present invention relates to a method of separating a hydrogen isotope. More particularly, the present invention relates to a method of separating a hydrogen isotope, which is useful for separation, enrichment and removal of tritium in a nuclear fusion reactor, upgrading of heavy water and enrichment and removal of tritium in a heavy water reactor, separation and removal of tritium in nuclear fuel reprocessing, and separation, recovery and removal of tritium used in a usual test or research, and further, separation of the other hydrogen isotope except for tritium in a manufacture of heavy water.
[DESCRIPTION OF THE PRIOR ARTJ
The method of separating a hydrogen isotope based on isotope exchange reaction between water and hydrogen is advantageous in that the separation coefficient is high in the state of equilibrium, permitting an achievement of a very high separatiing performance using a single apparatus because of the possibility of constituting a counter-current-type reaction tower, and because chemically easy-to-handle substances such as water and hydrogen are only used. While this is a hopeful method for the manufacture of heavy water, removal and recovery of tritium from water containing tritium oxides (hereinafter tritium water), it requires a step of repeating to reduce water to be enriched with a heavy isotope (for example, heavy hydrogen ~QS~Q~ 9~
~r tritium relative to light hydrogen) to hydrogen, and the electric power consumption in electrolysis used fox this purpose is one of the serious uroblems.
rr~ia.1 illustrates one of the embodiments of the conventional method of separating tritium water based or_ the combination of a counter-current-type isotope exchange reaction tower and an electrolytic cell. As shown in rig. l, tritium Water as a raw material is supplied through a raw material inlet port (2) into an exchange reaction tower (1), enriched in the reaction tower (1), and sent through an enriched water outlet port (3) to an electrolytic cell (8). In the electrolytic cell (8), tritium water is decomposed into hydrogen and oxygen containing tritium at a high concentration, a part of hydrogen is taken out as a product, and the remaining part is fed through a hydrogen inlet port (4) into the exchange reaction tower (1).
On the other hand, oxygen, which contains tritium water vapor in the original state, is sub,~edted to remove tritium water through a water separator (10), and then sent into a hydrogen recombinator ('1) by way of an oxygen feed line. After hydrogen has tritium transfer into water in the exchange reaction tower (1), hydrogen is sent through a hydrogen outlet port (5) into the hydrogen recombinator ('I) where hydrogen is oxidized. A
part of thus-produced water is dumpted as depleted water or cleaned water, and the remaining part is fed again through a depleted water inlet port (6) into the exchange reaction tower (1).
In such a conventional method, for example, oxidation ~0~~~3'.:~
of hydrogen and decomposition of water shoud be continuously carried out to keep the flows of hydrogen and water to be necessitated for isotope separation. The method is particularly defective in that it reauires a large amount of electric power for the decomposition of water, and this seriously results in preventing the practical application.
The present invention has an object to provide a new method which permits saving electric power consumption in the step of repeating to reduce water to be enriched with a heavy isotope to hydrogen, and does not even reauire electric power for the decomposition of water.
Other objects, features and advantages of the present invention will be apparent from the following description taken in connection with the accompanying drawings.
[BRLEF DESCRIPTION OF THE DRAWINGS
Fig.l illustrates one of the embodiments of the conventional method of separating tritium water based on the combination of a counter-current-type isotope exchange reaction tower and an electrolytic cell;
Fig.2 illustrates one of the embodiments of the present invention in which an apparatus for transferring oxygen from water to hydrogen is used;
Fig.3 depicts another embodiment of the present invention in which a fuel cell as a recombinator is used; and Fig.4 depicts further another embodiment of the present invention in which an oxidizing/reducing agent is used as a parameter for the reduction of water and oxidation of hydrogen. ' (DETAILED DESCRIPTION OF ThB EMBODIMENTS]
According to the present invention, it is possible to separate a hydrogen isotope With almost no consumption of electric power for the water decomposition step, or in some cases, even with a gain of power.
The present invention is described below further in detail with a separation of tritium from tritium water as an example.
Fig.2 illustrates one of the embodiments in which an apparatus simultaneously carrying out to convert water to hydrogen and from hyarogen to water through transferrig oxygen from watex to be enriched with a heavy isotope to hydrogen to be enriched with a light isotope is combined with a Water-hydrogen isotope exchange tower. More specifically, Fig.2 indicates a concrete case where tritium water is enriched using an oxygen ion conductive solid electrolytic cell as a water-hydrogen converter. Tritium water as a raw material is supplied through a raw material Water inlet port (12) to a water-hydrogen isotope exchange reaction tower (11), enriched in this reaction tower (11), and sent through an enriched water outlet port (13) to a water-hydrogen exchanger (1'1). A part of the produced hydrogen is taken out as a product, and the remaining part is sent back through a hydrogen inlet port (14) to the exchange reaction tower (11). Hydrogen has tritium transfer to water in the exchange reaction tower (11), and is sent through a hydrogen - a -2~a~~~~
cutlet port (15) to the water-hydrogen converter (1Z), converted into deleted water. The resultant depleted water is rejected or supplied again through a depleted water inlet port (16) to the exchange reaction tower (11). The hydrogen isotope in tritium water is continuously separated during the process as described above. The water-hydrogen converter (1?) supplies water enriched with a heavy isotope on one side of an oxygen ion conductive solid electrolytic barrier membrane (18), and hydrogen enriched with a light isotope on the other side of that. When a barrier membrane having a nature of permitting permeation or' oxygen comes in contact with water on one side thereof, and with hydrogen on the other side, the difference in oxygen potential causes oxygen transfer from water to hydrogen.
This results in simultaneous conversions of oxygen from water to hydrogen and from hydrogen to water. These conversions are never mixed up each other because hydrogen isotopes are seperated through the barrier membrance. Since these conversions take place spontaneously to some extent, it is usually unecessary to supply electric power, but oxygen may forcedly be transferred to the hydrogen side by applying voltage onto the both sides of the barrier membrance.
The electric power reauired for this transfer of oxygen is far smaller than that reauired for conventional electrolysis.
It is thus possible to separate a hydrogen isotope and to consume almost no electric power by the combination of the isotope exchange reaction and a solid electrolytic cell.
The above-mentioned embodiment is involved in a method In which electrolysis and recombination reaction are carried out in a single apparatus. It is also possible to achieve those with separate apparatuses.
Fig.3 shows a process of electrolyzing water with the use of electric power produced when the recombination reaction is utilized in generation or a fuel cell. In Fig.3, while an isotope exchange reaction tower (11) is the same as shown in Fig.2, hydrogen enriched with a light isotope is sent through the hydrogen outlet port (15) to a hydrogen oxygen fuel cell (19), and water enriched with a heavy isotope is sent through an enriched water outlet port (13) to an electrolytic cell (20), respectively. In the case where an oxygen ion conductive solid electrolytic cell as shown in Fig.2 is used as that electrolytic cell (20), the generating oxygen is so highly pure that water and hydrogen are not contaminated by tritium even when supplying the oxygen to the fuel cell (19). Oxidation of hydrogen in the fuel cell (19) spontaneously ocurrs and proceeds, enabling to take out electric power. The electric cell (20) is operated with this electric power. Because the amount of water supplied to the electrolytic cell (20) is almost eaual to that of hydrogen supplied to the fuel cell (19), the amount of electric generation of the fuel cell (19) serves the electric power necessary for electrolysis, if electric loss is disregarded.
Furthermore, while decomposition of water in the electrolytic cell (20) operated at a high temperature of about 900°C reauires a voltage of about 0.9 V, the electro motive force or' the hydrogen oxygen fuel cell (19) operated at the room temperature ~fl5~~~~
is about 1.2 V. It is therefore theoretically possible to achieve a gain of electric power by appropriately setting these operating temperatures.
Fig.4 depicts one of the embodiments in which energy is tran3ferred through an aapropriate oxidation/reduction agent from an oxidation step of rydrogen to a reduction step of water.
For example, a water gas equilibrium (H20 + CO = H2 + C02) is now explained as follows: Hydrogen enriched with a light isotope from the isotope exchange reaction tower (11) is sent through the hydrogen outlet port (15) to a hydrogen oxidation reactor (21), and water enriched with a heavy isotope is sent through the enriched water outlet port (13) to a water reduction reactor (22), respectively. As a water gas eauilibrium(H20 + CO
- H2 + C02) reaction is a reversible equilibrium reaction, hydrogen and carbon dioxide are produced until the ea_uilibrium is reached when water and carbon monoxide are supplied to the water reduction reactor (22). On the other hand, water and carbon monoxide are produced when hydrogen and carbon dioxide are supplied to the hydrogen oxidation reactor (21).
By separating carbon dioxide anti carbon monoxide from those reactors and circulating the same, it is possible to supply water and hydrogen to the water-hydrogen isotope exchange reaction tower (11) through oxidation of hydrogen and reduction of water almost without energy consumption. In the practical application of this embodiment, the steps of separating carbon monoxide and carbon dioxide from water and hydrogen may be omitted by using an oxygen ion conductive solid electrolytic .:ell as shown in Fig.2 for the reactors (21) and (22).
It is needless to mention that various embodiments of the present invention are possible in details of the constitution thereof.
_ g _
Claims
1. A method of separating a hydrogen isotope, by isotope exchange between water and hydrogen, which comprises the steps of supplying tritium-enriched water, which is produced in a water-hydrogen isotope exchange reaction tower, to one side of an oxygen ion conductive solid electrolytic barrier membrane, the membrane being oxygen permeable, which is provided with a water-hydrogen exchanger, supplying hydrogen enriched with a light isotope to the other side of the oxygen ion conductive solid electrolytic barrier membrane, and separating tritium by transferring oxygen from the tritium-enriched water to the hydrogen due to a difference of oxygen potential.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP20912/1991 | 1991-02-14 | ||
| JP3020912A JP2584902B2 (en) | 1991-02-14 | 1991-02-14 | Hydrogen isotope separation method |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CA2058054A1 CA2058054A1 (en) | 1992-08-15 |
| CA2058054C true CA2058054C (en) | 2003-02-11 |
Family
ID=12040435
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CA002058054A Expired - Fee Related CA2058054C (en) | 1991-02-14 | 1991-12-19 | Method of separating hydrogen isotope |
Country Status (2)
| Country | Link |
|---|---|
| JP (1) | JP2584902B2 (en) |
| CA (1) | CA2058054C (en) |
Families Citing this family (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP6949749B2 (en) * | 2018-02-07 | 2021-10-13 | 大陽日酸株式会社 | Method for producing stable carbon monoxide isotope and method for producing stable carbon dioxide isotope |
| CN114414650B (en) * | 2022-01-27 | 2023-07-14 | 中国科学院地质与地球物理研究所 | Analysis method of hydrocarbon isotopes in methane |
| JP2024047240A (en) * | 2022-09-26 | 2024-04-05 | 京都フュージョニアリング株式会社 | Hydrogen isotope transport device and hydrogen isotope transport method |
Family Cites Families (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5633323A (en) * | 1979-08-21 | 1981-04-03 | Dainippon Shoji Kk | Load collapse-proof method |
| FR2498157A1 (en) * | 1981-01-19 | 1982-07-23 | Cazas Ets | METHOD AND APPARATUS FOR GROUPING UNIT DOSE CONTAINERS |
| GB2231880A (en) * | 1989-04-03 | 1990-11-28 | Warner Lambert Co | Starch |
-
1991
- 1991-02-14 JP JP3020912A patent/JP2584902B2/en not_active Expired - Fee Related
- 1991-12-19 CA CA002058054A patent/CA2058054C/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| CA2058054A1 (en) | 1992-08-15 |
| JPH05802A (en) | 1993-01-08 |
| JP2584902B2 (en) | 1997-02-26 |
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| Date | Code | Title | Description |
|---|---|---|---|
| EEER | Examination request | ||
| MKLA | Lapsed |