CN108479393B - Method for removing protium in gas containing tritium hydrogen isotope - Google Patents
Method for removing protium in gas containing tritium hydrogen isotope Download PDFInfo
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- CN108479393B CN108479393B CN201810348846.2A CN201810348846A CN108479393B CN 108479393 B CN108479393 B CN 108479393B CN 201810348846 A CN201810348846 A CN 201810348846A CN 108479393 B CN108479393 B CN 108479393B
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D59/00—Separation of different isotopes of the same chemical element
- B01D59/22—Separation by extracting
- B01D59/26—Separation by extracting by sorption, i.e. absorption, adsorption, persorption
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Abstract
The invention discloses a method for removing protium in tritium-hydrogen isotope-containing gas, which comprises the following steps: cooling the palladium diatomite chromatographic column to below zero centigrade, introducing tritium-hydrogen isotope-containing raw material gas from the front end of the palladium diatomite chromatographic column until the content of the tritium-hydrogen isotope-containing raw material gas is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column, and stopping the operation; heating the palladium diatomite chromatographic column to a temperature of less than or equal to 150 ℃, collecting tritium-hydrogen-isotope-containing product gas released from the rear end of the palladium diatomite chromatographic column, and simultaneously collecting tritium-hydrogen-isotope-containing backflow gas released from the front end of the palladium diatomite chromatographic column until the residual tritium-hydrogen-isotope-containing raw material gas reaches 30% of the capacity of the palladium diatomite chromatographic column; the method utilizes a palladium diatomite chromatographic column to realize the high-efficiency removal of a small amount of protium in tritium at negative pressure and normal temperature, so as to obtain the deuterium-tritium product gas with the protium content lower than 0.3 percent, and the extraction rate of deuterium and tritium is higher than 90 percent.
Description
Technical Field
The invention belongs to the technical field of hydrogen isotope treatment, and particularly relates to a method for removing protium in gas containing tritium hydrogen isotopes.
Background
Because protium is unfavorable for the fusion reaction of deuterium and tritium, the protium content in the deuterium and tritium fuel gas for target production is strictly controlled in the ICF inertial confinement fusion target preparation process. With the intensive ICF related research in China, the demand of purifying the deuterium-tritium fuel for removing protium is continuously increased. In order to meet the above requirements, it is necessary to conduct a research on the purification of a small amount of deuterium tritium and related engineering work.
In contrast to the tendency of low temperature molecular sieves to enrich heavy hydrogen isotopes, metallic hydrogen storage materials such as uranium, titanium, palladium, tend to enrich light hydrogen isotopes and thus can be used for enrichment and filtration of protium.
The TCAP separation process generally requires that a steady gradient distribution of hydrogen isotope concentration in a separation column is realized through a total reflux mode, a sample is injected from the midpoint of the separation column, after one cold and hot cycle, light hydrogen isotopes are obtained from the tail end of the separation column, and heavy isotopes are obtained from the front end of the separation column. The traditional TCAP technology is realized by a large-capacity separation column and large-scale heating and cooling accessory equipment. The large capacity of the separation column means that the deuterium-tritium retention amount is large, and for the purification of a small amount of deuterium-tritium, the improvement of the product extraction rate of the deuterium-tritium is not facilitated. The use of large heating and cooling equipment increases the early investment and operating costs. In order to realize the rapid and efficient purification of a small amount of deuterium tritium gas with low protium concentration, an inventor team performs the miniaturization design and the cold experimental check of the separation performance of a TCAP separation system, and explores the protium purification and filtration process of the small amount of deuterium tritium. Because the affinity of protium and palladium is stronger, the protium moves in the palladium column and slows down to cause the retention in the column; the affinity of deuterium tritium and palladium is weaker, and partial deuterium tritium flows out of the chromatographic column before protium; as long as protium does not penetrate the chromatographic column, the purification and filtration of the deuterium-tritium gas can be realized. As protium is accumulated in the column, the concentration of hydrogen isotopes in the column is slowly changed, namely the hydrogen isotopes are in a metastable state of concentration, the content of deuterium and tritium is continuously reduced, the tritium retention in the column can be further reduced, and the product extraction rate is improved.
In order to verify the concept of the purification process, the inventor team designed a small purification heat experimental device based on the metastable heat cycle adsorption method, from the initial results, the protium content can be reduced from 50% to about 3%, but the protium content processing requirement of less than 1% is not met, in the patent with the patent number Z L201410354818.3 disclosed in the Chinese patent document library, a protium removing method under positive pressure is mentioned, but before the operation, the leakage detection operation is required, the risk of tritium leakage is higher, in addition, the protium content after the processing is higher (0.75%), the protium content does not reach the requirement that the protium content limited by the physical experiment is less than 0.3%, in addition, the extraction rate of the product of the tritium is not high (65%), in order to improve the protium removing effect, the protium removing method in the tritium-containing hydrogen isotope gas needs to be further developed.
Disclosure of Invention
The technical problem to be solved by the invention is to provide a method for removing protium in a tritium-hydrogen isotope-containing gas.
The method for removing protium in the gas containing tritium hydrogen isotopes sequentially comprises the following steps:
a. cooling the palladium diatomite chromatographic column to below zero centigrade, introducing tritium-hydrogen isotope-containing raw material gas from the front end of the palladium diatomite chromatographic column until the content of the tritium-hydrogen isotope-containing raw material gas is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column, and stopping the operation;
b. heating the palladium diatomite chromatographic column to a temperature of less than or equal to 150 ℃, collecting tritium-hydrogen-isotope-containing product gas released from the rear end of the palladium diatomite chromatographic column, and simultaneously collecting tritium-hydrogen-isotope-containing backflow gas released from the front end of the palladium diatomite chromatographic column until the residual tritium-hydrogen-isotope-containing raw material gas reaches 30% of the capacity of the palladium diatomite chromatographic column;
c. cooling the palladium diatomite chromatographic column to below zero centigrade, introducing collected backflow gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column, and introducing raw material gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column until the total amount of the backflow gas containing tritium hydrogen isotopes and the raw material gas containing tritium hydrogen isotopes is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column;
d. and c, repeating the steps b and c, and ending the circulation after the repetition times reach the set times.
The pressure of the tritium-hydrogen isotope-containing raw material gas introduced from the front end of the palladium diatomite chromatographic column in the step a is lower than one atmospheric pressure.
And c, the pressure of the product gas containing tritium hydrogen isotopes released from the rear end of the palladium diatomite chromatographic column and the pressure of the backflow gas containing tritium hydrogen isotopes released from the front end of the palladium diatomite chromatographic column in the step b are lower than one atmospheric pressure.
The method for removing protium in the tritium-hydrogen isotope-containing gas obviously reduces the tritium operation pressure, the pressure of the tritium-hydrogen isotope-containing raw material gas in the step a, and the pressure of the tritium-hydrogen isotope-containing product gas and the tritium-hydrogen isotope-containing reflux gas in the step b to be lower than one atmospheric pressure. The safety of tritium use is greatly improved by negative pressure operation. The temperature is less than or equal to 150 ℃, the high-temperature permeation and the environmental release of tritium are reduced, and the physical health of operators is better guaranteed. The protium removing process of the present invention operates automatically and has raised reliability. The protium content in the tritium hydrogen isotope-containing gas after the treatment of the method for removing protium meets the requirement that the protium content defined by a physical experiment is less than 0.3 percent. Moreover, the extraction rate of tritium products is improved to more than 90%, tritium resources are effectively utilized, and the pressure of waste treatment is reduced.
The method for removing protium in the gas containing tritium hydrogen isotopes is used for automatically removing protium in the gas with protium content higher than 1% deuterium and tritium under negative pressure and normal temperature to obtain deuterium and tritium product gas with protium content lower than 0.3%, and the extraction rate of deuterium and tritium is higher than 90%.
Detailed Description
The present invention will be described in detail with reference to examples.
Example 1
In the embodiment, the content of He-3 in the gas to be treated is less than 1%, the content of protium in the feed gas is equal to 2%, and the content of tritium is more than 97%.
a. Cooling the palladium diatomite chromatographic column to below zero centigrade, introducing tritium-hydrogen isotope-containing raw material gas from the front end of the palladium diatomite chromatographic column until the content of the tritium-hydrogen isotope-containing raw material gas is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column, and stopping the operation;
b. heating the palladium diatomite chromatographic column to a temperature of less than or equal to 150 ℃, collecting tritium-hydrogen-isotope-containing product gas released from the rear end of the palladium diatomite chromatographic column, and simultaneously collecting tritium-hydrogen-isotope-containing backflow gas released from the front end of the palladium diatomite chromatographic column until the residual tritium-hydrogen-isotope-containing raw material gas reaches 30% of the capacity of the palladium diatomite chromatographic column;
c. cooling the palladium diatomite chromatographic column to below zero centigrade, introducing collected backflow gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column, and introducing raw material gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column until the total amount of the backflow gas containing tritium hydrogen isotopes and the raw material gas containing tritium hydrogen isotopes is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column;
d. and c, repeating the steps b and c, and ending the circulation after the repetition times reach the set times.
The processing raw material gas of the single step of b-c is 100m L/h, when the protium content in the column is enriched from 2% to 50%, the protium content in the product gas is still kept to be less than 0.3%, at this time, the extraction rate of tritium is 98%, and the retention amount of tritium in the column is 2% of the total processing tritium amount.
Example 2
In the embodiment, the content of He-3 in the gas to be treated is less than 1%, the content of protium in the feed gas is equal to 5%, and the content of tritium is more than 94%.
a. Cooling the palladium diatomite chromatographic column to below zero centigrade, introducing tritium-hydrogen isotope-containing raw material gas from the front end of the palladium diatomite chromatographic column until the content of the tritium-hydrogen isotope-containing raw material gas is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column, and stopping the operation;
b. heating the palladium diatomite chromatographic column to a temperature of less than or equal to 150 ℃, collecting tritium-hydrogen-isotope-containing product gas released from the rear end of the palladium diatomite chromatographic column, and simultaneously collecting tritium-hydrogen-isotope-containing backflow gas released from the front end of the palladium diatomite chromatographic column until the residual tritium-hydrogen-isotope-containing raw material gas reaches 30% of the capacity of the palladium diatomite chromatographic column;
c. cooling the palladium diatomite chromatographic column to below zero centigrade, introducing collected backflow gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column, and introducing raw material gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column until the total amount of the backflow gas containing tritium hydrogen isotopes and the raw material gas containing tritium hydrogen isotopes is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column;
d. and c, repeating the steps b and c, and ending the circulation after the repetition times reach the set times.
The processing raw material gas of the single step of b-c is 100m L/h, when the protium content in the column is enriched from 5% to 50%, the protium content in the product gas is still kept to be less than 0.3%, at this time, the extraction rate of tritium is 95%, and the retention amount of tritium in the column is 5% of the total processing tritium amount.
The present invention is not limited to the above-described embodiments, and those skilled in the art will be able to make various modifications without creative efforts from the above-described conception, and fall within the scope of the present invention.
Claims (3)
1. A method for removing protium in a gas containing tritium hydrogen isotopes, which is characterized by comprising the following steps in sequence:
a. cooling the palladium diatomite chromatographic column to below zero centigrade, introducing tritium-hydrogen isotope-containing raw material gas from the front end of the palladium diatomite chromatographic column until the content of the tritium-hydrogen isotope-containing raw material gas is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column, and stopping the operation;
b. heating the palladium diatomite chromatographic column to a temperature of less than or equal to 150 ℃, collecting tritium-hydrogen-isotope-containing product gas released from the rear end of the palladium diatomite chromatographic column, and simultaneously collecting tritium-hydrogen-isotope-containing backflow gas released from the front end of the palladium diatomite chromatographic column until the residual tritium-hydrogen-isotope-containing raw material gas reaches 30% of the capacity of the palladium diatomite chromatographic column;
c. cooling the palladium diatomite chromatographic column to below zero centigrade, introducing collected backflow gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column, and introducing raw material gas containing tritium hydrogen isotopes from the front end of the palladium diatomite chromatographic column until the total amount of the backflow gas containing tritium hydrogen isotopes and the raw material gas containing tritium hydrogen isotopes is less than or equal to 70% of the capacity of the palladium diatomite chromatographic column;
d. and c, repeating the steps b and c, and ending the circulation after the repetition times reach the set times.
2. A method for protium removal from a tritium-containing gas according to claim 1, characterized in that: the pressure of the tritium-hydrogen isotope-containing raw material gas introduced from the front end of the palladium diatomite chromatographic column in the step a is lower than one atmospheric pressure.
3. A method for protium removal from a tritium-containing gas according to claim 1, characterized in that: and c, the pressure of the product gas containing tritium hydrogen isotopes released from the rear end of the palladium diatomite chromatographic column and the pressure of the backflow gas containing tritium hydrogen isotopes released from the front end of the palladium diatomite chromatographic column in the step b are lower than one atmospheric pressure.
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| CN113318596B (en) * | 2021-06-10 | 2023-05-05 | 中国工程物理研究院核物理与化学研究所 | Separation system and method for deuterium-tritium mixed gas |
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| US5441715A (en) * | 1991-03-26 | 1995-08-15 | Matsushita Electric Industrial Co., Ltd. | Method for the separation of hydrogen isotopes using a hydrogen absorbing alloy |
| WO2012036749A1 (en) * | 2010-09-15 | 2012-03-22 | Savannah River Nuclear Solutions, Llc | Process for separating hydrogen isotopes |
| CN104147928A (en) * | 2014-07-24 | 2014-11-19 | 中国工程物理研究院材料研究所 | Rapid removing method for protium in gas-containing tritium hydrogen isotope |
| CN106474924A (en) * | 2016-11-08 | 2017-03-08 | 中国工程物理研究院材料研究所 | A kind of enrichment method of trace tritium |
| CN107051205A (en) * | 2017-02-15 | 2017-08-18 | 中国工程物理研究院材料研究所 | A kind of low temperature palladium replaces separation method |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101850215B (en) * | 2010-05-24 | 2013-03-13 | 四川材料与工艺研究所 | Low-temperature displacement chromatography hydrogen isotope separation device and method |
| CN105923604B (en) * | 2016-04-20 | 2018-03-30 | 中国工程物理研究院核物理与化学研究所 | Deuterium tritium Rapid recovery device and method in a kind of fusion reactor ash discharge gas |
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Patent Citations (5)
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| US5441715A (en) * | 1991-03-26 | 1995-08-15 | Matsushita Electric Industrial Co., Ltd. | Method for the separation of hydrogen isotopes using a hydrogen absorbing alloy |
| WO2012036749A1 (en) * | 2010-09-15 | 2012-03-22 | Savannah River Nuclear Solutions, Llc | Process for separating hydrogen isotopes |
| CN104147928A (en) * | 2014-07-24 | 2014-11-19 | 中国工程物理研究院材料研究所 | Rapid removing method for protium in gas-containing tritium hydrogen isotope |
| CN106474924A (en) * | 2016-11-08 | 2017-03-08 | 中国工程物理研究院材料研究所 | A kind of enrichment method of trace tritium |
| CN107051205A (en) * | 2017-02-15 | 2017-08-18 | 中国工程物理研究院材料研究所 | A kind of low temperature palladium replaces separation method |
Non-Patent Citations (1)
| Title |
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| 氘氚燃料气体氕纯化系统设计及工艺初探;王伟伟 等;《核技术》;20150531;第38卷(第5期);050603 * |
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