CN112892212A - Fusion reactor low tritium retained hydrogen isotope separation device - Google Patents
Fusion reactor low tritium retained hydrogen isotope separation device Download PDFInfo
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- CN112892212A CN112892212A CN202110101922.1A CN202110101922A CN112892212A CN 112892212 A CN112892212 A CN 112892212A CN 202110101922 A CN202110101922 A CN 202110101922A CN 112892212 A CN112892212 A CN 112892212A
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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
- B01D59/50—Separation involving two or more processes covered by different groups selected from groups B01D59/02, B01D59/10, B01D59/20, B01D59/22, B01D59/28, B01D59/34, B01D59/36, B01D59/38, B01D59/44
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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
- B01D59/02—Separation by phase transition
- B01D59/04—Separation by phase transition by distillation
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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
- B01D59/10—Separation by diffusion
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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
Abstract
The invention discloses a fusion reactor low tritium retention hydrogen isotope separation device, which comprises: the system comprises a cryogenic rectification system, a cryogenic chromatographic separation system, a membrane separation system and a tritium storage system, wherein the cryogenic rectification system, the cryogenic chromatographic separation system and the membrane separation system are sequentially connected according to the flowing direction of gas, the tritium storage system is connected with a gas outlet of the cryogenic chromatographic separation system and is used for storing tritium after separation, the cryogenic rectification system and the cryogenic chromatographic separation system are used for completing two-stage separation and concentration of hydrogen-tritium mixed gas, and the membrane separation system is used for separating He gas in the mixed gas. The fusion reactor low-tritium retention hydrogen isotope separation device disclosed by the invention solves the problem that a large amount of tritium is retained in a separation system and cannot be used, and improves the utilization rate of tritium and the inherent safety of the device; the hydrogen isotope separation device disclosed by the invention has the advantages that the economy, the reliability and the resource utilization rate are greatly improved, and the production cost is saved.
Description
Technical Field
The invention belongs to the field of nuclear fuel, and particularly relates to a hydrogen isotope separation device.
Background
The fusion reactor needs to generate tritium through the reaction of neutrons and lithium in a breeding envelope while burning tritium so as to realize the self-sustaining of the fuel of the fusion reactor. Tritium generated in the breeding blanket is swept out by carrier gas containing hydrogen, but because the abundance of the tritium in the carrier gas is usually 0.01-0.1%, the requirement of fusion fuel on the abundance of the tritium (the abundance of the tritium is 50-90%) cannot be met, the carrier gas needs to be sent into a hydrogen isotope separation system for tritium separation and concentration.
The current tritium separation and concentration processes mainly involve: thermal diffusion method, low temperature distillation method, low temperature chromatography, palladium chromatography and laser separation, etc., wherein the low temperature distillation method is the most common tritium separation and concentration method.
At present, a device for carrying out tritium concentration and extraction by using a cryogenic rectification method is shown in figure 1, the device is a double-column cascade cryogenic rectification device, and the operation of carrying out tritium separation and concentration by using the device is as follows: the method comprises the steps of firstly feeding raw materials (T: H is 1: 1000) coming out of a proliferation cladding into a rectification column A for separating tritium and hydrogen, concentrating tritium in a reboiler A, concentrating hydrogen in a condenser A at the top of the rectification column, heating by the reboiler A, repeatedly separating hydrogen and tritium for multiple times through the rectification column A until the tritium-hydrogen ratio in the condenser A is concentrated to be 1: 50, then carrying out secondary concentration through a rectification column B, condensing the tritium-hydrogen ratio after the secondary concentration to be more than 1: 1, finally collecting and storing the tritium through a tritium storage system, condensing liquid hydrogen to 20K through the condenser A and the condenser B, and returning the liquid hydrogen to the proliferation cladding from the top end of the rectification column A for recycling.
Although the double-rectifying-column cascaded hydrogen isotope separation device or more rectifying-column cascaded devices can be continuously operated and can realize the concentration of low-grade tritium of a breeding blanket, when the reboiler is heated, in order to prevent the reboiler from being dried, a certain amount of liquid hydrogen tritium must be reserved in the reboiler, however, the concentration of tritium in the last stage of reboiler is very high, which causes a large amount of tritium to be detained in the system and cannot be stored and utilized, which not only brings great challenges to radiation protection and safety of the system, but also causes the loss of tritium detained in the system due to decay, and finally causes the fuel of the fusion reactor to be unable to realize self-sustaining. In addition, equipment in the low-temperature rectification device works in a liquid hydrogen temperature zone, equipment such as a pump, a flowmeter and the like required by liquid hydrogen conveying is expensive in manufacturing cost and high in precision requirement, and a mature and reliable product is not available at home at present.
Therefore, a fusion reactor low-tritium retention hydrogen isotope separation device is urgently needed, low retention of liquid tritium in a system is realized, self-sustaining of fuel of a fusion reactor can be guaranteed, and economical efficiency and reliability are greatly improved.
Disclosure of Invention
In view of the above, the invention provides a fusion reactor low tritium hydrogen retention isotope separation device.
In order to achieve the purpose, the invention adopts the following technical scheme: a fusion reactor low tritium hydrogen retention isotope separation apparatus, the apparatus comprising:
a cryogenic rectification system comprising: the system comprises a reboiler, a rectification column, a condenser and a heat regenerator, wherein the reboiler is arranged at the bottom of the rectification column, the condenser is positioned at the top of the rectification column, and the heat regenerator is arranged on a gas inlet pipeline and a gas outlet pipeline of a low-temperature rectification system; the cryogenic rectification system is provided with a plurality of gas inlets and a plurality of gas outlets and is placed in the vacuum cold box;
a cryogenic chromatographic separation system, the cryogenic chromatographic separation system comprising: the liquid nitrogen Dewar flask and the chromatographic column are arranged in the liquid nitrogen Dewar flask; the low-temperature chromatographic separation system comprises a gas inlet and two gas outlets, and the gas inlet of the low-temperature chromatographic separation system is connected with one gas outlet of the low-temperature rectification system;
the membrane separation system is characterized in that a separation membrane in the membrane separation system is made of palladium-based alloy materials, the membrane separation system comprises a gas inlet and two gas outlets, and the gas inlet of the membrane separation system is connected with one gas outlet of the low-temperature chromatographic separation system; one of two gas outlets of the membrane separation system is connected with the cryogenic rectification system, and the other gas outlet of the membrane separation system is connected with a connecting pipeline of the cryogenic rectification system and the cryogenic chromatographic separation system;
and the tritium storage system is connected with the other gas outlet of the low-temperature chromatographic separation system.
Preferably, the working temperature of the rectification column is 15-25K, the working pressure is 100-1000 kPa, and a plurality of low-temperature sensors with the accuracy of +/-20 mK are uniformly arranged on the rectification column in the length direction.
Preferably, a porous filler and a liquid hydrogen distributor are arranged in the rectification column.
Preferably, the porous filler is stainless steel.
Preferably, a temperature regulating valve and an auxiliary heater are arranged in the condenser, and a cold source of the condenser is helium with the temperature of 14K-15K.
Preferably, the chromatographic column is in a spiral pipe shape, and porous molecular sieve materials are filled in the chromatographic column.
Preferably, the particle size of the molecular sieve material is 1-4 mm; the heating activation temperature of the molecular sieve material is 473K-573K.
Preferably, the vacuum degree of the vacuum cold box is 10-5Pa～10-2pa, arranging a cold screen on the inner wall of the cold box, and mounting a temperature sensor and a liquid level sensor on the cold screen.
Preferably, the cold shield is liquid nitrogen.
Preferably, the cryogenic rectification system is scalable to multiple stages as required.
The invention has the beneficial effects that: 1. the fusion reactor low tritium retention hydrogen isotope separation device disclosed by the invention utilizes a low-temperature rectification system to carry out primary separation and concentration, then utilizes a low-temperature chromatographic separation system to carry out secondary separation and concentration of tritium, hydrogen tritium is separated in a gaseous state in the low-temperature chromatographic separation system, and the condition that high-concentration tritium is retained in the system does not exist, so that the fusion reactor low tritium retention hydrogen isotope separation device solves the problem that a large amount of tritium is retained in the separation system and cannot be stored and used, thereby improving the utilization rate of tritium, ensuring the self-holding of tritium fuel in a reactor, simultaneously improving the inherent safety of the device and reducing the tritium radiation protection difficulty; 2. the fusion reactor low-tritium retention hydrogen isotope separation device disclosed by the invention works in a liquid nitrogen temperature region, and compared with a device with a liquid hydrogen temperature, the device disclosed by the invention does not need expensive devices such as a pump and a flowmeter required by liquid hydrogen conveying, so that the economical efficiency and the reliability are greatly improved; 3. the hydrogen isotope separation device disclosed by the invention has the advantages that the helium gas is used for sweeping the hydrogen tritium gas into the low-temperature chromatographic column, the membrane separation system is arranged for separating the helium gas from the hydrogen tritium gas, the separated helium gas is recycled, and the hydrogen tritium gas is returned to the low-temperature rectification system for re-separation, so that the utilization rate of resources is improved, and the production cost is saved; 4. the invention is provided with a liquid level sensor, a temperature sensor and the like, monitors the device in real time, can automatically adjust according to the monitoring result and realizes the automatic operation of the device.
Drawings
FIG. 1 is a schematic structural diagram of a fusion reactor low tritium retention hydrogen isotope separation device of the invention;
FIG. 2 is a schematic diagram of the cryogenic rectification system of the present invention;
FIG. 3 is a schematic diagram showing the sequence of hydrogen and tritium precipitation in a chromatographic column;
in the figure: 1. the reboiler 2, the rectifying column 3, the condenser 4, the membrane separation system 5, the low-temperature chromatographic separation system 6, the tritium storage system 7, the vacuum cold box 8, the cold screen 9 and the heat regenerator.
Detailed Description
It will be appreciated by those of ordinary skill in the art that the embodiments described herein are intended to assist the reader in understanding the principles of the invention and are to be construed as being without limitation to such specifically recited embodiments and examples. Those skilled in the art can make various other specific changes and combinations based on the teachings of the present invention without departing from the spirit of the invention, and these changes and combinations are within the scope of the invention.
The invention is described in detail below with reference to the figures and specific embodiments.
A fusion reactor low tritium hydrogen retention isotope separation apparatus as shown in fig. 1, the apparatus comprising: a cryogenic rectification system, a cryogenic chromatographic separation system 5, a membrane separation system 4, and a tritium storage system 6.
As shown in FIG. 2, the cryogenic rectification system further comprising: reboiler 1, rectifying column 2, condenser 3 and regenerator 9, reboiler 1 is installed in rectifying column 2 bottom, condenser 3 is located rectifying column 2 top, regenerator 9 is installed and is used for retrieving the cold volume in the tail gas and the heat of the gas that gets into the system on the air inlet pipeline of cryogenic rectification system and gas outlet pipeline, realizes the heat exchange between the hydrogen that gets into the system and the tail gas of output. The cryogenic rectification system is provided with a plurality of gas inlets and a plurality of gas outlets.
The material of the rectifying column 2 is 316L stainless steel, the working temperature is 15-25K, and the working pressure is 100-1000 kPa. And (4) carrying out leakage rate test on all welding lines on the rectifying column after liquid nitrogen quenching, wherein the test frequency is not less than 3 times. Porous stainless steel filler and a liquid hydrogen distributor are placed in the rectification column, the porous filler is added into the rectification column 2 for the purpose of increasing the reaction time of hydrogen and tritium mixed gas or liquid in the rectification column and increasing the separation degree of hydrogen and tritium, and a plurality of low-temperature sensors, such as T1-T3 in figure 2 and pressure gauges P1 and P2, are arranged in the length direction of the rectification column and used for monitoring the temperatures of different heights of the rectification column, the temperature measurement range of the temperature sensors is 15K-77K, and the precision of the low-temperature sensors is +/-20 mK.
The stainless steel packing in the rectification column has a large specific surface area, and once solid impurities such as dust or liquid impurities such as oil dirt exist on the packing, the contact and balance efficiency of gas/liquid on the packing is greatly influenced, so that the cleaning treatment of the rectification packing is very important. The cleaning of the rectification packing follows the following steps:
s1: and (3) soaking the filler in an alcohol tank, taking out the filler from the alcohol tank, putting the filler into an ultrasonic cleaner with alcohol, and opening the cleaner for ultrasonic cleaning for 30 min. The ultrasonic cleaning can cause the temperature of the filler to rise and accelerate the evaporation, and the time is required to be grasped;
s2: after ultrasonic cleaning, washing the filler with clear water, wherein each filler needs to be washed for 5-10 minutes continuously;
s3: the filler is placed in order and then is blown by dry nitrogen, dust in gaps of the filler is blown out, evaporation of moisture on the filler is accelerated, and water stains are prevented from being formed.
S4: wrapping the filler with absorbent paper, and drying in a vacuum drying oven at 100 deg.C.
The condenser 3 is used for condensing the hydrogen-tritium mixed gas rising to the top of the rectification column, and refluxing the condensed liquid to the rectification column for re-separation. The cold source of the condenser is helium with the temperature of 14K-15K, a temperature regulating valve and an auxiliary heater are arranged in the condenser to regulate and control the cooling capacity, the fluctuation range of the cooling capacity is less than 10W, and a low-temperature sensor is arranged to measure the temperature, namely T5 and T6 in figure 2.
The reboiler 1 at the bottom is heated by a precise thermal resistance, the heating power is controlled with the precision of +/-100 mW, a pressure gauge P3 is arranged in the reboiler for measuring the liquid level in the reboiler and preventing the reboiler from being burnt out, the measuring precision of the pressure gauge is +/-5 Pa, and a temperature sensor T4 is arranged for temperature detection.
The whole cryogenic rectification system is arranged in a vacuum cold box 7, and the vacuum degree of the vacuum cold box is 10-5Pa～10-2Pa, a cold screen 8 is arranged on the inner wall of the cold box, liquid nitrogen can be selected as the cold screen 8, a temperature sensor, such as temperature sensors T7-T12 shown in figure 2, and a liquid level sensor are arranged on the cold screen 8 and used for monitoring the liquid nitrogen cold screenAnd controlling the liquid level of the liquid nitrogen to automatically supplement the liquid nitrogen. A liquid nitrogen cold screen is arranged in the vacuum cold box 7 and is mainly used for shielding environmental heat radiation and maintaining a low-temperature environment required by the work of the low-temperature rectification system. The shell of the vacuum cooling box is integrally cylindrical, and is made of 304 stainless steel materials through internal and external polishing treatment.
The low temperature chromatographic separation system 5 comprises: the device comprises a liquid nitrogen Dewar flask and a chromatographic column, wherein the chromatographic column is placed in the liquid nitrogen Dewar flask and is soaked in liquid nitrogen; the low-temperature chromatographic separation system comprises a gas inlet and two gas outlets, wherein the gas inlet is connected with one gas outlet of the low-temperature rectification system, helium is used as carrier gas, and the hydrogen-tritium mixed gas subjected to first-stage separation and concentration in the low-temperature rectification system is blown into the low-temperature chromatographic separation system 5 for further separation and concentration.
The liquid nitrogen Dewar flask provides the temperature required by the work for the chromatographic column, and is provided with a liquid nitrogen infusion tube, a nitrogen outlet, a pressure gauge, a safety valve, a temperature measuring wire outlet tube, a gas outlet tube, a heating outlet tube and the like; the chromatographic column is wound into a spiral tube, the structure is compact, the occupied area is small, porous molecular sieve materials are filled in the chromatographic column, and the particle size of the molecular sieve materials is 1-4 mm; the heating activation temperature of the molecular sieve material is 473K-573K, and the molecular sieve material can be selected from MS5A and MS 4A.
The membrane separation system 4 adopts palladium-based alloy to manufacture a separation membrane, the membrane separation system comprises an air inlet and two air outlets, the air inlet is connected with one air outlet of the low-temperature chromatographic separation system, tail gas of the low-temperature chromatographic separation system, namely mixed gas of helium and hydrogen tritium gas enters the membrane separation system 4 to separate the helium from the hydrogen tritium gas, meanwhile, the membrane separation system is provided with two air outlets, one of the two air outlets is connected with the low-temperature rectification system, so that the hydrogen tritium mixed gas separated by the membrane separation system enters the low-temperature rectification system to be separated again, and the other outlet is connected to a connecting pipeline of the low-temperature rectification system and the low-temperature chromatographic separation system, so that the separated helium can be recycled.
The working temperature of the membrane separation system 4 is 350-500 DEG C
The tritium storage system 6 is connected with the other gas outlet of the low-temperature chromatographic separation system and is used for collecting, separating and concentrating gaseous tritium.
In fig. 2, P4 and P5 are pressure gauges mounted on the valve box of the vacuum cold box.
The working process of the fusion reactor low tritium retention hydrogen isotope separation device for hydrogen isotope separation is as follows: firstly, raw materials (T: H is 1: 1000) are sent into a cryogenic rectification system for separation, tritium is concentrated by 20 times in a reboiler 1, and the T: H after primary concentration is 1: 50, then under the sweeping of helium carrier gas, the mixed gas of the hydrogen tritium and the helium which is subjected to primary concentration enters a low-temperature chromatographic separation system 5, a chromatographic column is soaked in liquid nitrogen, the temperature is kept at 77K, a porous sieve material filled in the chromatographic column is used for hydrogen tritium separation, the separation time difference caused by the difference of adsorption acting force of hydrogen and tritium on the porous material is mainly utilized, as shown in figure 3, most of hydrogen is separated out from the chromatographic column along with the carrier gas He, the He and the hydrogen tritium gas are separated after entering a membrane separation system 4, the hydrogen tritium gas returns to a rectification column 2, and the He gas is recycled; tritium and a very small amount of hydrogen are subsequently separated out on the chromatographic column and enter the tritium storage system.
The last stage of separation and concentration of the fusion reactor low tritium retention hydrogen isotope separation device disclosed by the invention adopts a low-temperature chromatographic separation process, all hydrogen isotopes are kept in a gaseous form, and compared with a rectification process, a large amount of tritium in a liquid form is not retained; the carrier gas He gas is recycled, so that the cost and the resource are saved.
Claims (10)
1. A fusion reactor low tritium hydrogen retention isotope separation device, comprising:
a cryogenic rectification system comprising: the system comprises a reboiler (1), a rectifying column (2), a condenser (3) and a heat regenerator (9), wherein the reboiler (1) is installed at the bottom of the rectifying column (2), the condenser (3) is located at the top of the rectifying column (2), and the heat regenerator (9) is installed on a gas inlet pipeline and a gas outlet pipeline of a low-temperature rectifying system; the cryogenic rectification system is provided with a plurality of gas inlets and a plurality of gas outlets and is placed in the vacuum cold box (7);
a cryochromatographic separation system (5), the cryochromatographic separation system (5) comprising: the liquid nitrogen Dewar flask and the chromatographic column are arranged in the liquid nitrogen Dewar flask; the low-temperature chromatographic separation system (5) comprises a gas inlet and two gas outlets, and the gas inlet is connected with one gas outlet of the low-temperature rectification system;
the separation membrane in the membrane separation system (4) is made of palladium-based alloy materials, the membrane separation system (4) comprises a gas inlet and two gas outlets, wherein the gas inlet is connected with one gas outlet of the low-temperature chromatographic separation system (5), one of the two gas outlets is connected with the low-temperature rectification system, and the other gas outlet is connected with a connecting pipeline of the low-temperature rectification system and the low-temperature chromatographic separation system (5);
and the tritium storage system (6) is connected with the other gas outlet of the low-temperature chromatographic separation system (5).
2. A fusion reactor low-tritium retention hydrogen isotope separation device according to claim 1, characterized in that the working temperature of the rectification column (2) is 15-25K, the working pressure is 100-1000 kPa, and a plurality of low-temperature sensors with the precision of +/-20 mK are uniformly arranged on the rectification column (2) in the length direction.
3. A fusion reactor low tritium hydrogen retention isotope separation apparatus as claimed in claim 2, characterized in that porous packing and liquid hydrogen distributor are placed inside the rectification column (2).
4. A fusion reactor low tritium hydrogen retention isotope separation apparatus as claimed in claim 3, wherein the material of the porous filler is stainless steel.
5. A fusion reactor low tritium retention hydrogen isotope separation device as claimed in claim 1, wherein a temperature regulating valve and an auxiliary heater are arranged in the condenser (3), and a cold source of the condenser (3) is helium gas with a temperature of 14K-15K.
6. A fusion reactor low tritium hydrogen retention isotope separation apparatus as claimed in claim l, wherein the chromatographic column is in a spiral tube shape, and porous molecular sieve material is filled in the chromatographic column.
7. A fusion reactor low tritium hydrogen retention isotope separation device as claimed in claim 6, wherein the particle size of the molecular sieve material is 1-4mm, and the heating activation temperature of the molecular sieve material is 473K-573K.
8. A fusion reactor low tritium hydrogen retention isotope separation apparatus as claimed in claim 1, wherein vacuum degree of the vacuum cold box (7) is l0-5Pa～l0-2Pa, a cold screen (8) is arranged on the inner wall of the vacuum cold box (7), and a temperature sensor and a liquid level sensor are installed on the cold screen (8).
9. A fusion reactor low tritium hydrogen retention isotope separation apparatus as claimed in claim 8, wherein the cold shield (8) is liquid nitrogen.
10. A fusion reactor low tritium hydrogen retention isotope separation apparatus as claimed in claim 1, wherein the cryogenic rectification system is scalable to multiple stages as required.
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| CN115180670B (en) * | 2022-06-07 | 2024-01-09 | 中国地质大学（武汉） | Underground water tritium sample multistage evaporation concentration device and pretreatment method |
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