High-pressure hydrogen isotope gas source preparation method and device based on hydrogen absorption material

Abstract

The invention provides a preparation method of a high-pressure hydrogen isotope gas source based on a hydrogen absorption material, which has the advantages of high safety, simple and reliable high-pressure obtaining mode, controllable and repeatable pressure, high gas utilization rate and less waste. The reversible hydrogen absorption material is placed in a closed container, the volume of an inner cavity of the closed container is larger than that of the reversible hydrogen absorption material, then the reversible hydrogen absorption material placed in the closed container adsorbs hydrogen isotope gas, and when the hydrogen isotope gas is needed, the reversible hydrogen absorption material is desorbed; and the released hydrogen isotope gas generates positive pressure in the fixed volume of the closed container, so that a high-pressure hydrogen isotope gas source is formed.

Description

Technical Field

[0001] This invention relates to the technical field of isotope gas processing, specifically to a method for preparing a high-pressure hydrogen isotope gas source based on hydrogen-absorbing materials. This invention also provides a device for preparing a high-pressure hydrogen isotope gas source based on hydrogen-absorbing materials. Background Technology

[0002] Hydrogen isotopes (especially tritium) have important applications in nuclear energy, controlled nuclear fusion, isotope tracing, and analytical chemistry. In these studies, small amounts of hydrogen isotope gases with controllable pressure are often required, such as carrier gases or sample gases for gas chromatography (GC) analysis, and feed gases for pressure swing adsorption (PSA) studies.

[0003] Currently, the main conventional methods for obtaining small amounts of high-pressure hydrogen isotope gas in the laboratory are: (1) Direct gas supply from high-pressure cylinders: Hydrogen isotope gas is pre-filled into high-pressure steel cylinders. This method has significant drawbacks: A. Significant safety risks: High-pressure storage of radioactive tritium gas implies a huge risk of leakage and radioactive contamination.

[0004] b. Significant gas waste: Each experiment requires only a small amount of gas, but the high-pressure gas remaining in the cylinder is difficult to fully utilize, resulting in the waste of expensive and radioactive isotopic gases. c. Pressure cannot be flexibly adjusted: The output pressure is affected by the pressure decay inside the bottle, making it difficult to obtain a stable and precisely set initial pressure.

[0005] (2) Mechanical compressor boosting: Using a miniature compressor to compress low-pressure gas has the following drawbacks: The system is complex and prone to contamination: the compressor has a large dead volume and complex piping, which can easily cause adsorption residues and cross-contamination of high-purity and high-value hydrogen isotope gases, especially tritium. There is a risk of leakage and hydrogen permeation: dynamic sealing points may become gas leakage points, which is unacceptable for tritium. f Not suitable for extremely small amounts of gas: Compressors typically have minimum requirements for gas flow rate and are not suitable for laboratory micro-analysis that requires only a few milliliters to hundreds of milliliters of standard state gas.

[0006] Therefore, existing technologies lack a safe, efficient, partless method for preparing trace high-pressure hydrogen isotope gas sources that is particularly suitable for processing radioactive tritium. Summary of the Invention

[0007] To address the aforementioned problems, this invention provides a method for preparing a high-pressure hydrogen isotope gas source based on hydrogen-absorbing materials. This method is highly safe, the high-pressure acquisition is simple and reliable, the pressure is controllable and repeatable, and it also has high gas utilization and low waste.

[0008] A method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material is characterized by: placing a reversible hydrogen-absorbing material in a sealed container, wherein the inner volume of the sealed container is larger than the volume of the reversible hydrogen-absorbing material; then, the reversible hydrogen-absorbing material in the sealed container adsorbs hydrogen isotope gas; when hydrogen isotope gas is needed, the reversible hydrogen-absorbing material is desorbed, so that the released hydrogen isotope gas generates positive pressure within the fixed volume of the sealed container, thereby forming a high-pressure hydrogen isotope gas source.

[0009] Its further features are: The hydrogen isotope gas contains tritium; The reversible hydrogen absorption material is pre-activated and then placed in a pressure-resistant, sealed container with a precisely known internal volume. At room temperature, under a relatively low pressure that is adapted to the equilibrium plateau pressure of the selected reversible hydrogen absorption material, hydrogen isotope gas is fully absorbed by the reversible hydrogen absorption material to form stable hydrides. At this time, the sealed container is in a low-pressure or near-normal-pressure state related to the reversible hydrogen absorption material. The desorption of the reversible hydrogen-absorbing material is achieved by heating; The final pressure inside the sealed container can be precisely controlled by controlling the desorption amount or desorption rate of the reversible hydrogen-absorbing material.

[0010] A high-pressure hydrogen isotope gas source preparation device based on hydrogen absorption materials is characterized in that it includes: a sealed container having pressure resistance. Hydrogen absorption material bed; Gas filling and releasing valve; And heating components.

[0011] The hydrogen-absorbing material bed is disposed inside the sealed container, and the sealed container is provided with the gas filling and releasing valve. The heating component is used to heat the hydrogen-absorbing material bed.

[0012] Its further features are: It also includes a pressure sensor; the pressure sensor is used to monitor the pressure inside the container; It also includes a temperature controller, which is used to control the heating and desorption operation of the heating element; The hydrogen-absorbing material of the hydrogen-absorbing material bed is at least one of uranium, zirconium-cobalt alloy, titanium-iron-manganese alloy or vanadium-based alloy or at least two mixed materials. The gas charging / discharging valve includes a vacuum / charging valve, an output valve, and a tail gas collection valve.

[0013] One application involves using a high-pressure hydrogen isotope gas source prepared by a high-pressure hydrogen isotope gas source preparation method based on hydrogen-absorbing materials, or a high-pressure hydrogen isotope gas source preparation device based on hydrogen-absorbing materials, for gas chromatography analysis or pressure swing adsorption research.

[0014] The present invention has the following beneficial effects: (1) High safety, especially suitable for tritium: Under normal conditions, radioactive tritium is fixed in the form of solid hydride, which greatly reduces the risk of leakage and diffusion, and there is no need to store tritium gas in high-pressure steel cylinders for a long time; (2) The high pressure is simple and reliable: no mechanical compressor is required. High pressure can be generated in a fixed volume simply by heating and desorption. The system has no dynamic seals, which completely eliminates mechanical leakage. (3) High gas utilization rate and little waste: The reversible hydrogen absorption material can almost completely absorb and desorb the gas with almost no residue. High pressure gas can be produced as needed according to experimental requirements, avoiding waste of residual gas in the cylinder. (4) Pressure is controllable and repeatable: By precisely controlling the heating temperature, time and desorption amount, the same pressure of gas can be repeatedly generated, which is beneficial to the repeatability and comparability of the experiment; (5) Compact system with less pollution: The entire system is small in size and has simple pipelines, which reduces the adsorption loss and cross-contamination of gas during transmission and ensures the purity of hydrogen isotope gas. (6) Multifunctionality: The same device can generate gas sources with different pressures by controlling the desorption conditions, which is suitable for various application scenarios such as gas chromatography injection, pressure swing adsorption cycle, and permeation experiment. Attached Figure Description

[0015] Figure 1 This is a simplified schematic diagram of a specific embodiment of the high-pressure hydrogen isotope gas source preparation device based on hydrogen-absorbing materials of the present invention; The names corresponding to the serial numbers in the diagram are as follows: Storage / desorption chamber 1, heating jacket 2, pressure sensor 3, vacuum / gas filling valve 4, output valve 5, tail gas recovery port valve 6, control and display unit 7, hydrogen absorption material bed 8. Detailed Implementation

[0016] A method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material: A reversible hydrogen-absorbing material is placed in a sealed container, wherein the inner volume of the sealed container is larger than the volume of the reversible hydrogen-absorbing material. The reversible hydrogen-absorbing material in the sealed container then adsorbs hydrogen isotope gas. When hydrogen isotope gas is needed, the reversible hydrogen-absorbing material is desorbed, so that the released hydrogen isotope gas generates positive pressure in the fixed volume of the sealed container, thereby forming a high-pressure hydrogen isotope gas source.

[0017] Among them, hydrogen isotope gas includes tritium; The reversible hydrogen absorption material is pre-activated and then placed in a pressure-resistant, sealed container with a precisely known internal volume. Desorption of reversible hydrogen-absorbing materials is achieved by heating; The final pressure inside a sealed container can be precisely controlled by adjusting the amount or rate of desorption of the reversible hydrogen-absorbing material.

[0018] The specific implementation steps are as follows: S1 places a specific reversible hydrogen-absorbing material (such as uranium, zirconium cobalt, titanium iron manganese, vanadium-based alloys or certain coordination hydrides) that has been activated into a sealed container with a precisely known pressure and volume, which serves as a storage / desorption chamber; S2 allows hydrogen isotope gas to be fully absorbed by hydrogen-absorbing materials at a low pressure of less than 0.5 MPa and at room temperature, forming stable hydrides. At this time, the closed container system that has absorbed hydrogen isotope gas is in a low-pressure or normal-pressure state, which ensures high safety. When a high-pressure gas source is required, the S3 seals and isolates the storage / desorption chamber. Hydrogen isotope gas is desorbed from the reversible hydrogen absorption material by controlling the heating of the reversible hydrogen absorption material. Since the desorption process of S4 takes place in a closed container with a fixed volume, the released gas cannot expand, causing the pressure inside the closed container to rise rapidly. The target pressure value can be accurately obtained through theoretical calculation or pressure sensor monitoring. The theoretical calculation is based on the hydrogen absorption capacity of the material, the desorption rate, and the volume of the cavity. The target pressure value ranges from 1 to 10 MPa or even higher. The high-pressure gas generated by S5 can be directly guided through valves to the gas chromatograph inlet, pressure swing adsorption unit, or other analytical instruments.

[0019] In step S2, the specific value of the lower pressure depends on the selected reversible hydrogen absorption material. When the reversible hydrogen absorption material is uranium, the lower pressure is <0.01 MPa. When the reversible hydrogen absorption material is zirconium-cobalt alloy, the lower pressure is between 0.01 MPa and 0.5 MPa.

[0020] Reversible hydrogen absorption materials need to have good reversible absorption and desorption properties for hydrogen isotopes (especially tritium), a suitable equilibrium pressure plateau, fast kinetic performance, and resistance to disproportionation and pulverization. The volume of the sealed container (storage / desorption chamber) needs to be precisely designed and matched with the hydrogen absorption capacity of the reversible hydrogen absorption material to achieve the target pressure; the entire sealed container needs to meet the requirements of high vacuum and high pressure sealing. The entire method integrates controllable desorption and pressure management strategies: heating method (such as electric heat tracing), heating rate and temperature feedback control, to achieve a smooth and controllable pressure rise process; It possesses special tritium processing technology, material compatibility (reducing tritium retention), and requires the design of an exhaust gas recovery interface.

[0021] A high-pressure hydrogen isotope gas source preparation device based on hydrogen absorption material includes a sealed container, a hydrogen absorption material bed, a gas filling and releasing valve, a heating component, a pressure sensor, and a temperature controller. The sealed container has pressure resistance; the hydrogen absorption material bed is set inside the sealed container, and the sealed container is equipped with a gas filling and releasing valve; the heating unit is used to heat the hydrogen absorption material bed. Pressure sensors are used to monitor the pressure inside a container; The temperature controller is used to control the heating and desorption operations of the heating element; The hydrogen-absorbing material in the hydrogen-absorbing material bed is at least one of uranium, zirconium-cobalt alloy, titanium-iron-manganese alloy or vanadium-based alloy, or at least two mixed materials. In a specific embodiment, the preparation of a high-pressure gas source for tritium gas chromatography analysis is described in [reference needed]. Figure 1 It comprises a storage / desorption chamber 1, a heating jacket 2, a pressure sensor 3, a vacuum / filling valve 4, an output valve 5, a tail gas recovery port valve 6, and a control and display unit 7. The storage / desorption chamber 1 is a sealed container, the heating jacket 2 is a heating device, and the vacuum / filling valve 4, the output valve 5, and the tail gas recovery port valve 6 are combined to form a gas filling and releasing valve; the control and display unit 7 acts as a temperature controller, used by the heating jacket 2 to heat and desorb the hydrogen-absorbing material bed 8. The hydrogen absorption material bed 8 inside the storage / desorption chamber 1 is specifically 100g of zirconium cobalt (ZrCo) alloy particles (already activated).

[0022] The storage / desorption chamber 1 is placed inside the heating jacket 2, with its upper surface exposed. The heating jacket 2 has a control and display unit 7 outside. The upper surface of the storage / desorption chamber 1 is provided with a vacuum / filling valve 4, an output valve 5, and a tail gas recovery port valve 6 through gas passage interfaces. The storage / desorption chamber 1 is also connected to a pressure sensor 3, which is used to monitor the pressure inside the storage / desorption chamber 1 in real time.

[0023] During absorption: The system is evacuated through vacuum / gas filling valve 4 and heated to 300°C for degassing. After cooling to room temperature, a mixture of hydrogen isotopes containing tritium (T2, D2, H2) is introduced at a pressure of 0.1 MPa. The ZrCo alloy absorbs the gas until the pressure is balanced, at which point the gas is safely fixed. Then proceed with the preparation work: close the vacuum / gas filling valve 4 to make the entire storage / desorption chamber 1 sealed, and confirm that the output valve (5) is closed.

[0024] Desorption and pressure generation: Start heating jacket 2 to slowly heat storage / desorption chamber 1 to 200°C. Hydrogen isotope gas in ZrCo alloy begins to desorb, and the pressure in the chamber rises. This is monitored by pressure sensor 3. When the pressure reaches the preset 5.0 MPa, heating is stopped.

[0025] Application: Open output valve 5 to directly introduce high-pressure gas into the quantitative loop or injection system of the gas chromatograph for isotope separation and analysis; after use, the remaining gas can be introduced into a dedicated recovery system through tail gas recovery valve 6.

[0026] It safely obtained a small-volume (approximately 50 mL) high-pressure (5 MPa) tritium mixture, meeting the GC injection requirements and avoiding the use of high-pressure tritium cylinders.

[0027] One application involves using a high-pressure hydrogen isotope gas source prepared by a high-pressure hydrogen isotope gas source preparation method based on hydrogen-absorbing materials, or a high-pressure hydrogen isotope gas source preparation device based on hydrogen-absorbing materials, for gas chromatography analysis or pressure swing adsorption research.

[0028] The present invention has the following beneficial effects: (1) High safety, especially suitable for tritium: Under normal conditions, radioactive tritium is fixed in the form of solid hydride, which greatly reduces the risk of leakage and diffusion, and there is no need to store tritium gas in high-pressure steel cylinders for a long time; (2) The high pressure is simple and reliable: no mechanical compressor is required. High pressure can be generated in a fixed volume simply by heating and desorption. The system has no dynamic seals, which completely eliminates mechanical leakage. (3) High gas utilization rate and little waste: The reversible hydrogen absorption material can almost completely absorb and desorb the gas with almost no residue. High pressure gas can be produced as needed according to experimental requirements, avoiding waste of residual gas in the cylinder. (4) Pressure is controllable and repeatable: By precisely controlling the heating temperature, time and desorption amount, the same pressure of gas can be repeatedly generated, which is beneficial to the repeatability and comparability of the experiment; (5) Compact system with less pollution: The entire system is small in size and has simple pipelines, which reduces the adsorption loss and cross-contamination of gas during transmission and ensures the purity of hydrogen isotope gas. (6) Multifunctionality: The same device can generate gas sources with different pressures by controlling the desorption conditions, which is suitable for various application scenarios such as gas chromatography injection, pressure swing adsorption cycle, and permeation experiment.

[0029] It will be apparent to those skilled in the art that the present invention is not limited to the details of the exemplary embodiments described above, and that the invention can be implemented in other specific forms without departing from its spirit or essential characteristics. Therefore, the embodiments should be considered in all respects as exemplary and non-limiting, and the scope of the invention is defined by the appended claims rather than the foregoing description. Thus, all variations falling within the meaning and scope of equivalents of the claims are intended to be included within the present invention. No reference numerals in the claims should be construed as limiting the scope of the claims.

[0030] Furthermore, it should be understood that although this specification describes embodiments, not every embodiment contains only one independent technical solution. This narrative style is merely for clarity. Those skilled in the art should consider the specification as a whole, and the technical solutions in each embodiment can also be appropriately combined to form other embodiments that can be understood by those skilled in the art.

Claims

1. A method for preparing a high-pressure hydrogen isotope gas source based on hydrogen-absorbing materials, characterized in that: A reversible hydrogen-absorbing material is placed in a sealed container, with the inner volume of the sealed container being larger than the volume of the reversible hydrogen-absorbing material. The reversible hydrogen-absorbing material in the sealed container then adsorbs hydrogen isotope gas. When hydrogen isotope gas is needed, the reversible hydrogen-absorbing material is desorbed, causing the released hydrogen isotope gas to generate positive pressure within the fixed volume of the sealed container, thereby forming a high-pressure hydrogen isotope gas source.

2. The method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material according to claim 1, characterized in that: The hydrogen isotope gas contains tritium.

3. The method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material according to claim 1, characterized in that: The reversible hydrogen-absorbing material is pre-activated and then placed in a pressure-resistant, sealed container with a precisely known internal volume.

4. The method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material according to claim 1, characterized in that: At room temperature, under a relatively low pressure that is adapted to the equilibrium plateau pressure of the selected reversible hydrogen absorption material, hydrogen isotope gas is fully absorbed by the reversible hydrogen absorption material to form stable hydrides. At this time, the sealed container is in a low-pressure or near-normal-pressure state related to the reversible hydrogen absorption material.

5. The method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material according to claim 1, characterized in that: The desorption of the reversible hydrogen-absorbing material is achieved by heating.

6. The method for preparing a high-pressure hydrogen isotope gas source based on a hydrogen-absorbing material according to claim 5, characterized in that: The final pressure inside the sealed container can be precisely controlled by controlling the desorption amount or desorption rate of the reversible hydrogen-absorbing material.

7. A high-pressure hydrogen isotope gas source preparation apparatus based on hydrogen-absorbing materials, used for performing a high-pressure hydrogen isotope gas source preparation method based on hydrogen-absorbing materials as described in any one of claims 1-6, characterized in that, It includes: sealed A container that is pressure resistant; Hydrogen absorption material bed; Gas filling and releasing valve; And heating components; The hydrogen-absorbing material bed is disposed inside the sealed container, and the sealed container is provided with the gas filling and releasing valve. The heating component is used to heat the hydrogen-absorbing material bed.

8. The high-pressure hydrogen isotope gas source preparation device based on hydrogen-absorbing materials according to claim 7, characterized in that: It also includes a pressure sensor; the pressure sensor is used to monitor the pressure inside the container.

9. The high-pressure hydrogen isotope gas source preparation device based on hydrogen-absorbing materials according to claim 7, characterized in that: It also includes a temperature controller for controlling the heating and desorption operation of the heating element.

10. The high-pressure hydrogen isotope gas source preparation device based on hydrogen-absorbing materials according to claim 7, characterized in that: The hydrogen-absorbing material in the hydrogen-absorbing material bed is at least one of uranium, zirconium-cobalt alloy, titanium-iron-manganese alloy, or vanadium-based alloy, or a mixture of at least two materials.

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