An apparatus and method for electrolytic enrichment of low-purity heavy water while producing high-purity deuterium gas

Abstract

The application discloses a kind of equipment and method for electrolytic concentration low-purity heavy water while producing high-purity deuterium gas.The equipment of the application includes electrolysis power supply (1), water tank (2), electrolytic cell (3), gas-water separation chamber (4), purification column (6), gas storage tank (7), thermometer (8), synthesis chamber (9), fire barrier (10), fire barrier (11), condensation chamber (14), buffer chamber (15), gas chamber (16), gas mixing chamber (17), water tank (18), cooling device (20), hydrogen gas-water separator (24), oxygen gas-water separator (25);The application utilizes sulfonated tetrafluoroethylene group fluoropolymer-copolymer membrane electrolytic cell to reduce the volume of electrolytic concentration low-purity heavy water, and the low-purity deuterium gas electrolyzed by reducing the volume is re-synthesized in synthesis chamber and condensed into heavy water, which improves the production efficiency of high-purity deuterium gas, and has excellent electrolysis effect and economy.

Description

Technical Field

[0001] This invention relates to the field of deuterium gas preparation and heavy water concentration technology, and in particular to an equipment and method for electrolytically concentrating low-purity heavy water to simultaneously produce high-purity deuterium gas. Background Technology

[0002] High-purity deuterium gas is widely used in semiconductors, optical fiber materials, special lamp sources, medical testing, chemical tracers, and pharmaceuticals. Generally, the preparation of high-purity deuterium gas requires high-purity heavy water. However, low-purity heavy water contains light water (H₂O and HDO). During the preparation process, the light water is mainly converted into H₂ and HDO. Removing H₂ and HDO from deuterium gas is extremely difficult, making it impossible to directly prepare high-purity deuterium gas from low-purity heavy water.

[0003] Currently, the main method used in heavy water electrolysis is alkaline electrolysis. The electrolysis process requires the participation of electrolytes, which places high demands on the reliability of the electrolysis equipment. It also needs to consider the recovery and treatment of alkaline solution. The overall equipment is complex, the process is cumbersome, and the cost is high.

[0004] Existing electrolytic concentration technologies for low-purity heavy water do not take into account that heavy water will solidify when the temperature is below 4°C. Furthermore, different voltages and currents will affect the deuterium-hydrogen separation coefficient, resulting in an excessively low deuterium-hydrogen separation coefficient. The existing process is disconnected from the actual electrolytic concentration process, which significantly increases the consumption of low-purity heavy water.

[0005] The volume reduction electrolytic concentration of low-purity heavy water faces the problem that the low-purity heavy water is continuously consumed during the electrolysis process without being recycled and reused, ultimately resulting in huge consumption and waste of low-purity heavy water. Summary of the Invention

[0006] The purpose of this invention is to provide an apparatus and method for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, in order to solve the problems existing in the prior art.

[0007] To achieve the above objectives, the present invention provides the following solution:

[0008] An apparatus for electrolyzing and concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas is characterized by comprising a power supply, a water tank, a cooling device, an electrolytic cell, a gas-water separation chamber, valves, a purification column, a gas storage tank, a thermometer, a synthesis chamber, a flame arrestor layer, a flame arrester, a condensation chamber, a buffer chamber, a gas chamber, a gas mixing chamber, a tailwater tank, a hydrogen gas-water separator, and an oxygen gas-water separator.

[0009] The water tank is connected to the electrolytic cell to supply heavy water, the power supply is connected to the electrolytic cell to supply power, and the cooling device is connected to the electrolytic cell to regulate the temperature. The gas generated by electrolysis in the electrolytic cell enters the gas-liquid separation chamber through a pipeline. The gas-liquid separation chamber is connected to a purification column and a buffer chamber respectively. The purification column further purifies tritium gas and is connected to a gas storage tank. The buffer chamber is connected to the synthesis chamber and the condensation chamber in pairs through pipelines equipped with valves. Heavy water vapor can be generated in the synthesis chamber through the action of a catalyst. The synthesis chamber is also connected to the condensation chamber through other pipelines without valves. The heavy water vapor enters the condensation chamber from the synthesis chamber through this pipeline and condenses to form heavy water. The condensed heavy water enters the tailwater tank through the pipeline between the condensation chamber and the tailwater tank.

[0010] As a further optimization of the present invention, valves are respectively installed on the connecting pipes of the gas-liquid separation chamber, the purification column, and the buffer chamber, and the valves are opened and closed according to different electrolysis stages.

[0011] As a further optimization of the present invention, the buffer chamber is connected to the synthesis chamber and the condensation chamber in pairs through pipes equipped with valves, and the valves can be opened and closed according to different electrolysis stages;

[0012] As a further optimization of the invention, the synthesis chamber is also connected to the condensation chamber via other pipes without valves.

[0013] As a further optimization of the present invention, the buffer chamber consists of a gas chamber and a gas mixing chamber, wherein the gas chamber is connected to the gas mixing chamber through a pipe equipped with a valve;

[0014] As a further optimization of the present invention, the gas mixing chamber is connected to the gas-water separation chamber, the synthesis chamber, and the condensation chamber, respectively.

[0015] As a further optimization of the present invention, the synthesis chamber includes a thermometer and a fire-resistant layer, the fire-resistant layer is filled with quartz sand, and a flame arrester is installed on the pipe at the lower entrance of the synthesis chamber.

[0016] As a further optimization of this invention, the gas-liquid separation chamber includes a hydrogen gas-liquid separator and an oxygen gas-liquid separator, each with independent pipelines. The condensate in the hydrogen and oxygen gas-liquid separators forms a liquid seal. When the water level is too high, the condensate level in both separators is controlled between one-third and one-half of the separator volume. When the water level exceeds one-half of the separator volume, the valve opens, and water flows back to the water tank through the pipeline. When the water level is below one-third of the separator volume, the valve closes. The hydrogen gas-liquid separator is connected to the purification column and the gas synthesis chamber via a valve-controlled pipeline, and the oxygen gas-liquid separator is connected to the gas synthesis chamber via a valve-controlled pipeline.

[0017] As a further optimization of the present invention, the electrolytic cell contains, from the inside out, a sulfonated tetrafluoroethylene vinyl fluoropolymer-polymer membrane, an anode and cathode catalyst layer, an anode and cathode gas diffusion layer, and an anode and cathode end plates. The cathode of the electrolytic cell generates deuterium, hydrogen, and other gases and gas mixtures, which enter a hydrogen gas-water separator through pipes. The anode of the electrolytic cell generates oxygen, which enters an oxygen gas-water separator through pipes.

[0018] As a further optimization of the present invention, the lower purity heavy water collected in the tailwater tank can be recycled back to the water tank for electrolytic concentration;

[0019] This invention also provides a method for concentrating low-purity heavy water using an electrolytic concentration device to simultaneously produce high-purity deuterium gas, the steps of which are as follows:

[0020] Step 1: Adjust valves 5, 13, 12 and 21 to the closed state, and adjust valves 19 and 27 to the open state. Inject the low-purity heavy water in the water tank into the electrolytic cell and carry out electrolysis under the conditions of voltage 3V, current 50-100A and temperature 5-20℃.

[0021] Step Two: The gas generated by electrolysis in Step One enters the gas-water separation chamber through a pipeline. Then, the condensed water in the gas-water separation chamber flows back to the water tank through a pipeline after the valve is opened. The dry gas separated in the gas-water separation chamber enters the gas mixing chamber. After the dry gas enters the gas mixing chamber, helium gas enters the gas mixing chamber through valve 21 and mixes evenly with the dry gas. Then, valve 13 is opened, and the evenly mixed gas enters the synthesis chamber from the gas mixing chamber. Under the action of the catalyst, heavy water vapor is generated. The heavy water vapor in the synthesis chamber enters the condensation chamber through a pipeline to form lower purity heavy water, which finally flows to the tailwater tank.

[0022] Step 3: Repeat steps 1 and 2.

[0023] Step 4: When the purity of heavy water in the tank is ≥99.5%, the electrolysis conditions of the electrolytic cell in Step 1 are changed to voltage 1.5~2.5V, current 2~10A, and temperature 5~10℃. Then, Step 1 to Step 2 are repeated. When the purity of heavy water in the tank is ≥99.95%, electrolysis is stopped, and high-purity heavy water is obtained.

[0024] As a further optimization of the present invention, the condensate water level in the hydrogen gas-water separator and the oxygen gas-water separator is controlled at one-third to one-half of the separator volume. When the water level exceeds one-half of the separator volume, the valve opens and the water flows back to the water tank through the pipe. When the water level is lower than one-third of the separator volume, the valve closes.

[0025] As a further optimization of the present invention, the lower purity heavy water collected in the tailwater tank can be recycled back to the water tank for electrolytic concentration.

[0026] As a further optimization of the present invention, the temperature of the synthesis chamber in step two is controlled at 350-400°C, and the catalyst is palladium powder.

[0027] As a further optimization of the present invention, the residual gas in the condensation chamber that has not formed steam in step two can enter the synthesis chamber by opening valve 12 to participate in the next synthesis of heavy water steam.

[0028] In the above concentration process of low-purity heavy water, the low-purity heavy water in the tank is continuously improved in purity through volume reduction electrolysis to obtain high-purity heavy water. The electrolysis concentration process conditions are: electrolytic cell temperature 5-20℃, electrolysis voltage 3V, and current 50-100A. When the purity of heavy water in the tank is ≥99.5%, electrolysis is stopped, and the cooling device and power supply are adjusted. Electrolysis is carried out for a long time under the conditions of electrolytic cell temperature 5-10℃, electrolysis voltage 1.5-2.5V, and current 2-10A. During the entire process, the gas produced by electrolysis is converted into low-purity heavy water through the synthesis chamber and condensation chamber and collected in the tank.

[0029] This invention also provides a method for producing high-purity deuterium gas using an equipment for electrolytically concentrating low-purity heavy water, characterized by the following steps:

[0030] Adjust valves 5, 13, 27, and 21 to the open position, and adjust valves 19 and 12 to the closed position. High-purity heavy water in the water tank is injected into the electrolytic cell for electrolysis. The gas generated by electrolysis in the electrolytic cell enters the gas-liquid separation chamber through a pipeline. Then, the high-purity heavy water condensed in the gas-liquid separation chamber flows back to the water tank through the pipeline after the valve is opened. The deuterium gas separated in the gas-liquid separation chamber flows to the purification column through a pipeline. The deuterium gas is further purified by the purification column and finally collected in the gas storage tank.

[0031] The oxygen separated in the gas-liquid separation chamber flows through pipelines to the gas mixing chamber, synthesis chamber, and condensation chamber in sequence, purging the entire system, and finally being discharged at the outlet of the tailwater tank.

[0032] The condensate water level in the hydrogen gas-water separator and the oxygen gas-water separator is controlled between one-third and one-half of the separator volume. When the water level exceeds one-half of the separator volume, the valve opens and the water flows back to the water tank through the pipe. When the water level is lower than one-third of the separator volume, the valve closes.

[0033] As a further optimization of the present invention, the electrolysis conditions are: electrolytic cell temperature 10–50°C, electrolysis voltage 40V, and electrolysis current 50–100A.

[0034] The present invention discloses the following technical effects:

[0035] This invention discloses an apparatus for electrolyzing and concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, as well as a method for concentrating low-purity heavy water and producing tritium gas. This invention utilizes a sulfonated tetrafluoroethylene vinyl fluoropolymer-polymer membrane electrolyzer to electrolyze and concentrate low-purity heavy water using a reduced-capacity electrolysis method, and then produces high-purity deuterium gas. The entire process requires no electrolyte and generates no residue or waste liquid. The low-purity deuterium gas removed during reduced-capacity electrolysis is resynthesized and condensed back into heavy water in the synthesis chamber, significantly improving the recovery rate of heavy water in the production of high-purity deuterium gas. Furthermore, the process is optimized in both the reduced-capacity electrolysis and concentration of low-purity heavy water and the production of high-purity deuterium gas, enhancing the separation coefficient of hydrogen and deuterium in the reduced-capacity electrolysis and concentration of low-purity heavy water, and improving the production efficiency of high-purity deuterium gas. This invention exhibits excellent electrolysis performance and economic efficiency. Attached Figure Description

[0036] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the embodiments will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0037] Figure 1 This is a schematic diagram of an apparatus for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, as described in this invention.

[0038] Figure 2 This is a schematic diagram of the structure of the buffer chamber;

[0039] Figure 3 This is a schematic diagram of the structure of the gas-water separation chamber;

[0040] The components include: 1. Power supply; 2. Water tank; 3. Electrolytic cell; 4. Gas-water separation chamber; 5. Valve; 6. Purification column; 7. Gas storage tank; 8. Thermometer; 9. Synthesis chamber; 10. Flame arrestor layer; 11. Flame arrester; 12. Valve; 13. Valve; 14. Condensation chamber; 15. Buffer chamber; 16. Gas chamber; 17. Gas mixing chamber; 18. Tailwater tank; 19. Valve; 20. Cooling device; 21. Valve; 22. Pipeline; 23. Pipeline; 24. Hydrogen gas-water separator; 25. Oxygen gas-water separator; 26. Valve; 27. Valve. Detailed Implementation

[0041] Various exemplary embodiments of the present invention will now be described in detail. This detailed description should not be considered as a limitation of the present invention, but rather as a more detailed description of certain aspects, features, and embodiments of the present invention.

[0042] It should be understood that the terminology used in this invention is merely for describing particular embodiments and is not intended to limit the invention. Furthermore, with respect to numerical ranges in this invention, it should be understood that each intermediate value between the upper and lower limits of the range is also specifically disclosed. Every smaller range between any stated value or intermediate value within a stated range, and any other stated value or intermediate value within said range, is also included in this invention. The upper and lower limits of these smaller ranges may be independently included or excluded from the range.

[0043] Unless otherwise stated, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art. While only preferred methods and materials have been described herein, any methods and materials similar or equivalent to those described herein may be used in the implementation or testing of this invention. All references to this specification are incorporated by way of citation to disclose and describe methods and / or materials associated with those references. In the event of any conflict with any incorporated reference, the content of this specification shall prevail.

[0044] Various modifications and variations can be made to the specific embodiments described in this specification without departing from the scope or spirit of the invention, as will be apparent to those skilled in the art. Other embodiments derived from this specification will also be readily apparent to those skilled in the art. This specification and embodiments are merely exemplary.

[0045] The terms “include,” “including,” “have,” “contain,” etc., used in this article are all open-ended terms, meaning that they include but are not limited to.

[0046] An apparatus for electrolyzing and concentrating low-purity heavy water to simultaneously produce high-purity deuterium gas includes a power supply, an electrolysis power supply 1, a water tank 2, an electrolytic cell 3, a gas-water separation chamber 4, a valve 5, a purification column 6, a gas storage tank 7, a thermometer 8, a synthesis chamber 9, a flame arrestor layer 10, a flame arrester 11, a valve 12, a valve 13, a condensation chamber 14, a buffer chamber 15, a gas chamber 16, a gas mixing chamber 17, a tailwater tank 18, a valve 19, a cooling device 20, a valve 21, pipes 22 and 23, a hydrogen gas-water separator 24, an oxygen gas-water separator 25, a valve 26, and a valve 27.

[0047] Water tank 2 is connected to electrolytic cell 3 to supply low-purity heavy water; power supply 1 is connected to electrolytic cell 3 to supply power; cooling device 20 is connected to electrolytic cell 3 to regulate the temperature of electrolytic cell 3; the gas generated by electrolysis in electrolytic cell 3 enters gas-water separation chamber 4 through a pipe; a mixture of deuterium and hydrogen generated at the cathode of electrolytic cell 3 enters hydrogen gas-water separator 24 through pipe 21; oxygen generated at the anode of electrolytic cell enters oxygen gas-water separator 25 through pipe 22; gas-water separation chamber 4 is connected to purification column 6 and buffer chamber 15 respectively; purification column 6 is connected to gas storage tank 7; buffer chamber 15 is connected to synthesis chamber 9 and condensation chamber 14 respectively; synthesis chamber 9 is connected to condensation chamber 14, and condensation chamber 14 is connected to tailwater tank 18.

[0048] The hydrogen gas-water separator 24 and the oxygen gas-water separator 25 are connected to the water tank 2 via pipes equipped with valves 26.

[0049] A valve 5 is installed on the connecting pipe between the gas-liquid separation chamber 4 and the purification column 6, and a valve 19 is installed on the connecting pipe between the gas-liquid separation chamber 4 and the buffer chamber 15. Valves 5 and 19 are switched on and off according to different electrolysis stages.

[0050] The buffer chamber 15 is connected to the synthesis chamber 9 and the condensation chamber 14 respectively through T-shaped pipes equipped with valves 13 and 12. Valves 12 and 13 are switched on and off according to different electrolysis stages.

[0051] The buffer chamber 15 consists of a gas chamber 16 and a gas mixing chamber 17. The gas chamber 16 is connected to the gas mixing chamber 17 through a pipe equipped with a valve 21.

[0052] The gas mixing chamber 17 is connected to the gas-liquid separation chamber 4, the synthesis chamber 9, and the condensation chamber 14, respectively.

[0053] The synthesis chamber 9 includes a thermometer 8 and a fire-resistant layer 10, which is filled with quartz sand. A flame arrester 11 is installed on the pipe connecting the lower entrance of the synthesis chamber 9 to the buffer chamber 15.

[0054] Low-purity heavy water electrolytic concentration:

[0055] like Figure 1 , Figure 2 , Figure 3 As shown, an electrolytic concentration and recovery preparation device for low-purity heavy water includes: an electrolytic power supply 1, a water tank 2, an electrolytic cell 3, a gas-water separation chamber 4, a valve 5, a thermometer 8, a synthesis chamber 9, a valve 12, a valve 13, a condensation chamber 14, a buffer chamber 15 consisting of a gas chamber 16 and a gas mixing chamber 17, a tailwater tank 18, a valve 19, a cooling device 20, a valve 21, a pipe 22, a pipe 23, a hydrogen gas-water separator 24, an oxygen gas-water separator 25, a valve 26, and a valve 27.

[0056] The method for concentrating low-purity heavy water to obtain high-purity heavy water using the above apparatus is as follows:

[0057] Step 1: Adjust valves 5, 12, 13, 26, and 21 to the closed position, and adjust valves 19 and 27 to the open position. Inject the low-purity heavy water from water tank 2 into electrolytic cell 3 for volume reduction electrolysis. The electrolysis conditions are: temperature 5–20℃, electrolysis voltage 3V, and current 50–100A. High current allows for efficient electrolysis of low-purity heavy water.

[0058] Step 2: The gas generated in electrolytic cell 3 enters the gas-liquid separation chamber 4 through a pipe. A mixture of deuterium and hydrogen generated at the cathode of electrolytic cell 3 enters the hydrogen gas-liquid separator 24 through pipe 21. Oxygen generated at the anode of electrolytic cell enters the oxygen gas-liquid separator 25 through pipe 22. The dry gas in the gas-liquid separation chamber 4 enters the gas mixing chamber 17 through a pipe. As the pressure in the mixing chamber 17 continuously increases, valves 19 and 27 are closed, and valve 21 is opened, allowing helium from gas chamber 16 to enter the gas mixing chamber 17, resulting in more uniform gas mixing. Then, valve 13 is opened, and the uniformly mixed gas flows out from the mixing chamber. The gas mixture from chamber 17 enters synthesis chamber 9. Using a palladium catalyst, the mixed gas in synthesis chamber 9 produces lower-purity heavy water vapor. It is crucial to maintain the temperature of synthesis chamber 9 between 350 and 420°C, as the hydrogen-deuterium-oxygen mixture poses a certain explosion risk. An explosion will not occur below 460°C. The lower-purity heavy water vapor in synthesis chamber 9 enters condensation chamber 14 through a pipe to form lower-purity heavy water. The collected lower-purity heavy water flows through a pipe to tailwater tank 18. Gas in condensation chamber 14 that has not yet produced steam can enter synthesis chamber 9 to participate in the next synthesis by adjusting valve 12 to the open position. The condensate in gas-water separation chamber 4 can flow back to water tank 2 through a pipe by opening valve 26. The condensate level in hydrogen gas-water separator 24 and oxygen gas-water separator 25 is controlled between one-third and one-half of the separator volume. When the water level exceeds one-half of the separator volume, valve 26 opens, and the water flows back to the water tank through a pipe. When the water level is below one-third of the separator volume, valve 26 closes.

[0059] Step 3: Repeat steps 1 and 2 above multiple times. Taking advantage of the fact that hydrogen is deposited on the cathode at a slower rate than deuterium, as the electrolysis process continues, deuterium gradually accumulates in the heavy water in tank 2, and high-purity heavy water is collected.

[0060] Step 4: When the purity of heavy water in water tank 2 is ≥99.5%, adjust the cooling device 20 and the electrolysis power supply 1 to change the electrolysis conditions of electrolysis cell 3. Under electrolysis conditions of 5-10℃, 1.5-2.5V, and 2-10A, repeat steps 1 and 2 for a longer period of electrolysis to improve the deuterium-hydrogen separation coefficient and further concentrate the heavy water efficiently until the purity of heavy water is ≥99.95%. Then stop the operation of the entire equipment to obtain high-purity heavy water. The gas generated during the entire electrolysis process is converted into low-purity heavy water through the synthesis chamber 9 and the condensation chamber 14 and collected in the tailwater tank 18. The even lower purity heavy water collected in the tailwater tank 18 can be recycled back to water tank 2. Using this invention, a longer electrolysis process is carried out to concentrate and recover the heavy water, and high-purity deuterium gas is generated again. When the purity of the final recovered lower purity heavy water in the tailwater tank is less than 10%, it is not advisable to recycle it back to the water tank for reuse.

[0061] Production of high-purity deuterium gas:

[0062] like Figure 1 , Figure 2 , Figure 3 As shown, the high-purity deuterium gas production device includes: an electrolysis power supply 1, a water tank 2, an electrolytic cell 3, a gas-water separation chamber 4, a valve 5, a purification column 6, a gas storage tank 7, valves 19, 22, 23, a hydrogen gas-water separator 24, an oxygen gas-water separator 25, a valve 26, and a valve 27.

[0063] Adjust valves 5, 13, 27, and 21 to the open state, and adjust valves 19, 26, and 12 to the closed state. High-purity heavy water in water tank 2 is injected into electrolysis cell 3 for electrolysis. The temperature of electrolysis cell 3 is 10-50℃, the voltage is 40V, and the current is 50-100A. The gas generated in electrolysis cell 3 enters gas-water separation chamber 4 through a pipeline. Deuterium gas generated at the cathode of electrolysis cell 3 enters hydrogen gas-water separator 24 through pipeline 21. Oxygen gas generated at the anode of electrolysis cell enters oxygen gas-water separator 25 through pipeline 22. The deuterium gas separated in gas-water separation chamber 4 flows to purification column 6 through a pipeline. The deuterium gas is further purified by purification column 6. The purified tritium gas is finally collected in storage tank 7. The purity of deuterium gas can reach more than 99.9999%. Simultaneously, oxygen in gas-liquid separation chamber 4 flows sequentially through pipelines to gas mixing chamber 17, gas chamber 16, synthesis chamber 9, condensation chamber 14, and tailwater tank 18 to purge the entire system, finally being discharged at the outlet of tailwater tank 18. The high-purity heavy water condensed in gas-liquid separation chamber 4 can flow back to water tank 2 via pipeline by opening valve 26. The condensate water level in hydrogen gas-liquid separator 24 and oxygen gas-liquid separator 25 is controlled between one-third and one-half of the separator volume. When the water level exceeds one-half of the separator volume, valve 26 opens, and water flows back to the water tank through pipelines. When the water level is below one-third of the separator volume, valve 26 closes. Example 1

[0064] like Figure 1 , Figure 2 , Figure 3 The aforementioned equipment for electrolyzing and concentrating low-purity heavy water to simultaneously produce high-purity deuterium gas includes an electrolysis power source 1, a water tank 2, an electrolytic cell 3, a gas-water separation chamber 4, a valve 5, a purification column 6, a gas storage tank 7, a thermometer 8, a synthesis chamber 9, a flame arrestor layer 10, a flame arrester 11, a valve 12, a valve 13, a condensation chamber 14, a buffer chamber 15, a gas chamber 16, a gas mixing chamber 17, a tailwater tank 18, a valve 19, a cooling device 20, a valve 21, pipes 22 and 23, a hydrogen gas-water separator 24, an oxygen gas-water separator 25, a valve 26, and a valve 27.

[0065] The method for simultaneously producing high-purity deuterium gas by electrolyzing and concentrating low-purity heavy water using the above-mentioned equipment is as follows:

[0066] I. Concentration: Adjust valves 5, 13, 12, 26, and 21 to the closed state, and valves 19 and 27 to the open state. Inject 15L of 40%–70% low-purity heavy water into water tank 2. When the low-purity heavy water in water tank 2 is injected into electrolytic cell 3, control the temperature of electrolytic cell 3 to 5–20℃, the electrolysis voltage to 3V, and the current to 50–100A to perform capacity reduction electrolysis.

[0067] II. Recovery: Electrolytic cell 3 produces a mixture of deuterium and hydrogen at its cathode, which enters the hydrogen gas-water separator 24 via pipe 21. Oxygen produced at the anode enters the oxygen gas-water separator 25 via pipe 22. The dry gas from the hydrogen gas-water separator 24 enters the gas mixing chamber 17 via a pipe equipped with valve 19. The dry gas from the oxygen gas-water separator 25 enters the gas mixing chamber 17 via a pipe equipped with valve 27. As gas is continuously produced, the system pressure gradually increases. When the system pressure exceeds 1.5 MPa, valves 19 and 27 are closed, and valve 21 is opened, allowing helium from gas chamber 16 to enter. The gas mixing chamber 17 mixes with dry gas, further increasing the pressure and making the gas mixture more uniform. Valve 13 is opened, and valve 12 is closed. The uniformly mixed gas enters the synthesis chamber 9 to generate lower-purity heavy water vapor. The temperature in the synthesis chamber is controlled at 350–400°C. Palladium powder catalyst is used. The heavy water vapor in the synthesis chamber 9 enters the condensation chamber 14 through a pipe and condenses to form lower-purity heavy water. The collected lower-purity heavy water flows through a pipe to the tailwater tank 18. Gas that has not yet synthesized into steam in the condensation chamber 14 can enter the synthesis chamber 9 through the condensation chamber 14 by adjusting valve 12 to the open state to participate in the next synthesis. The condensate in the hydrogen gas-water separator 24 and the oxygen gas-water separator 25 can flow back to the water tank 2 through the pipe by opening valve 26. The condensate water level in the hydrogen gas-water separator 24 and the oxygen gas-water separator 25 is controlled between one-third and one-half of the separator volume. When the water level exceeds one-half of the separator volume, valve 26 is opened, and water flows back to the water tank through the pipe. When the water level is lower than one-third of the separator volume, valve 26 is closed.

[0068] III. Re-concentration: Repeat steps I to II above. When the purity of the low-purity heavy water in tank 2 is ≥99.5%, adjust the electrolysis conditions in electrolytic cell 3 using cooling device 20 and power supply 1 to a temperature of 5–10°C, a voltage of 1.5–2.5V, and a current of 2–10A. Continue repeating steps I to II for prolonged electrolysis while keeping other conditions unchanged. Stop electrolysis when the heavy water purity reaches 99.95% or higher. Depending on the initial heavy water purity, approximately 1 / 10 to 1 / 20 of the heavy water volume remains in the electrolytic cell.

[0069] IV. Electrolysis to produce deuterium: When the purity of heavy water in water tank 2 is ≥99.95%, adjust valves 5, 13, 27 and 21 to the open state, and valves 19, 26 and 12 to the closed state. Adjust the cooling device 20 and power supply 1 to control the electrolysis conditions of electrolytic cell 3 to a temperature of 10-50℃, an electrolysis voltage of 40V and a current of 50-100A. Inject the heavy water in water tank 2 into electrolytic cell 3 to produce deuterium gas.

[0070] V. Purification: The gas generated by electrolysis in electrolytic cell 3 enters the gas-water separation chamber 4. Deuterium gas generated at the cathode of electrolytic cell 3 enters the hydrogen gas-water separator 24 through pipe 21. Oxygen generated at the anode of electrolytic cell enters the oxygen gas-water separator 25 through pipe 22. The deuterium gas separated by the hydrogen gas-water separator 24 flows to the purification column 6, where it is further purified and finally collected in the gas storage tank 7. Simultaneously, the oxygen separated by the oxygen gas-water separator 25 flows through pipelines sequentially to the gas mixing chamber 17, the synthesis chamber 9, and the condensation chamber 14, purging the entire system and finally being discharged at the outlet of the tailwater tank 18. The high-purity heavy water condensed in the hydrogen gas-water separator 24 and the oxygen gas-water separator 25 can be returned to the water tank 2 through the pipe via the check valve 26. The condensate water level in the hydrogen gas-water separator 24 and the oxygen gas-water separator 25 is controlled between one-third and one-half of the separator volume. When the water level exceeds one-half of the separator volume, valve 26 is opened, and water flows back to the water tank through the pipe. When the water level is lower than one-third of the separator volume, valve 26 is closed.

[0071] Measurements showed that the purity of the deuterium produced by the above process reached 99.999%.

[0072] After testing, the purity of the heavy water collected in tailwater tank 18 reached over 20%, and the heavy water collected in tailwater tank 18 can be recycled and injected into water tank 2 as raw material for the next production.

[0073] In the description of this invention, it should be understood that the terms "longitudinal", "lateral", "up", "down", "front", "rear", "left", "right", "vertical", "horizontal", "top", "bottom", "inner", "outer", etc., indicate the orientation or positional relationship based on the orientation or positional relationship shown in the accompanying drawings, and are only for the convenience of describing this invention, and are not intended to indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation of this invention.

[0074] The embodiments described above are merely preferred embodiments of the present invention and are not intended to limit the scope of the present invention. Various modifications and improvements made by those skilled in the art to the technical solutions of the present invention without departing from the spirit of the present invention should fall within the protection scope defined by the claims of the present invention.

Claims

1. A method for preparing high-purity deuterium gas using an apparatus for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, characterized in that... Includes power supply (1), water tank (2), electrolytic cell (3), gas-water separation chamber (4), purification column (6), gas storage tank (7), synthesis chamber (9), condensation chamber (14), buffer chamber (15), tail water tank (18), and cooling device (20); The water tank (2) is connected to the electrolytic cell (3) to supply low-purity heavy water; the power supply (1) is connected to the electrolytic cell (3) to supply power; the cooling device (20) is connected to the electrolytic cell (3) to regulate the temperature in the electrolytic cell (3); the gas generated by the electrolysis of the electrolytic cell (3) enters the gas-water separation chamber (4) through a pipeline; the gas-water separation chamber (4) is connected to the purification column (6) and the buffer chamber (15) respectively; the purification column (6) is connected to the gas storage tank (7); the buffer chamber (15) is connected to the synthesis chamber (9) and the condensation chamber (14) respectively; the synthesis chamber (9) is connected to the condensation chamber (14), and the condensation chamber (14) is connected to the tailwater tank (18); A valve 1 (5) is provided on the connecting pipe between the gas-liquid separation chamber (4) and the purification column (6). A valve 2 (19) and a valve 3 (27) are provided on the connecting pipe between the gas-liquid separation chamber (4) and the buffer chamber (15). The valve 1 (5), the valve 2 (19) and the valve 3 (27) are switched on and off according to different electrolysis stages. The buffer chamber (15) is connected to the synthesis chamber (9) and the condensation chamber (14) respectively through pipes equipped with valve four (13) and valve five (12). The valve five (12) and the valve four (13) are switched on and off according to different electrolysis stages. The buffer chamber (15) consists of a gas chamber (16) and a gas mixing chamber (17). The gas chamber (16) is connected to the gas mixing chamber (17) through a pipe equipped with valve six (21). The gas mixing chamber (17) is connected to the gas-water separation chamber (4), the synthesis chamber (9) and the condensation chamber (14) respectively. The electrolytic cell (3) consists of, from the inside out, a sulfonated tetrafluoroethylene vinyl fluoropolymer-copolymer membrane, an anode and cathode catalyst layer, an anode and cathode gas diffusion layer, and an anode and cathode end plates; The equipment performs the following steps when concentrating low-purity heavy water: Step 1: Adjust valve 1 (5), valve 4 (13), valve 5 (12) and valve 6 (21) to the closed state, and adjust valve 2 (19) and valve 3 (27) to the open state. The low-purity heavy water in the water tank (2) is injected into the electrolytic cell (3) and electrolyzed under the conditions of voltage 3V, current 50~100A and temperature 5~20℃. Step 2: The gas generated by electrolysis in the electrolytic cell (3) in Step 1 enters the gas-water separation chamber (4) through the pipeline. Then, the condensed water in the gas-water separation chamber (4) flows back to the water tank (2) through the pipeline. The dry gas separated in the gas-water separation chamber (4) enters the gas mixing chamber (17). After the dry gas enters the gas mixing chamber (17), valve six (21) is opened and helium in the gas chamber (16) enters the gas mixing chamber (17) and mixes evenly with the dry gas. Then, valve four (13) is opened and the evenly mixed gas enters the synthesis chamber (9) from the gas mixing chamber (17) and generates heavy water vapor under the action of the catalyst. The heavy water vapor in the synthesis chamber (9) enters the condensation chamber (14) through the pipeline to form lower purity heavy water and finally flows to the tail water tank (18). Step 3: Repeat steps 1 and 2. Step 4: When the purity of heavy water in the water tank (2) is ≥99.5%, the electrolysis conditions of the electrolytic cell (3) in step 1 are changed to voltage 1.5~2.5V, current 2~10A, and temperature 5~10℃. Then, continue to repeat steps 1 to 2. When the purity of heavy water in the water tank (2) is ≥99.95%, stop electrolysis to obtain high-purity heavy water.

2. The method for preparing high-purity deuterium gas using an equipment for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, as described in claim 1, is characterized in that... The synthesis chamber (9) includes a thermometer (8) and a fire-resistant layer (10), the fire-resistant layer (10) being filled with quartz sand, and a flame arrester (11) being installed on the pipe at the lower entrance of the synthesis chamber (9).

3. The method for preparing high-purity deuterium gas using the equipment for electrolytically concentrating low-purity heavy water and simultaneously producing high-purity deuterium gas according to claim 1, characterized in that... The gas-water separation chamber (4) contains a hydrogen gas-water separator (24) and an oxygen gas-water separator (25). The hydrogen gas-water separator (24) and the oxygen gas-water separator (25) are independent pipelines. The condensate in the hydrogen gas-water separator (24) and the oxygen gas-water separator (25) can be returned to the water tank (2) through the pipeline controlled by valve seven (26).

4. The method for preparing high-purity deuterium gas using an equipment for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, as described in claim 3, is characterized in that... The gas generated at the cathode of the electrolytic cell (3) enters the hydrogen gas-water separator (24) through the pipe (23), and the gas generated at the anode of the electrolytic cell (3) enters the oxygen gas-water separator (25) through the pipe (22).

5. The method for preparing high-purity deuterium gas using an equipment for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas, as described in claim 1, is characterized in that: The equipment, when concentrating low-purity heavy water, also includes: The lower purity heavy water collected in the water tank (18) is recycled to the water tank (2) for electrolytic concentration; In step two, the temperature of the synthesis chamber (9) is controlled at 350–400°C, and the catalyst is palladium powder. The residual gas in the condenser (14) of step two enters the synthesis chamber (9) through the opening of valve five (12) to participate in the next synthesis of heavy water vapor.

6. The method for preparing high-purity deuterium gas using the equipment for electrolytically concentrating low-purity heavy water while simultaneously producing high-purity deuterium gas according to any one of claims 1-5, characterized in that... Step five is as follows: Adjust valves 1 (5), 4 (13), 3 (27), and 6 (21) to the open state, and adjust valves 2 (19) and 5 (12) to the closed state. High-purity heavy water in water tank (2) is injected into electrolytic cell (3) for electrolysis. The gas generated by electrolysis in electrolytic cell (3) enters gas-water separation chamber (4) through pipeline. Then, the deuterium gas separated in gas-water separation chamber (4) flows to purification column (6) through pipeline. The high-purity heavy water condensed in gas-water separation chamber (4) flows back to water tank (2) through pipeline. The deuterium gas is further purified by purification column (6) and finally collected in gas storage tank (7). The oxygen separated in the gas-water separation chamber (4) flows through the pipeline to the gas mixing chamber (17), the synthesis chamber (9), and the condensation chamber (14) in sequence, purging the entire system, and finally being discharged at the outlet of the tailwater tank (18).

7. The method for preparing high-purity deuterium gas using the equipment for electrolytic concentration of low-purity heavy water and simultaneous production of high-purity deuterium gas according to claim 6, characterized in that... In step five, the electrolysis conditions are a temperature of 10–50°C, a voltage of 40V, and a current of 50–100A.

Images