Gaseous hydrogen isotope separation device, gaseous hydrogen isotope separation system and gaseous hydrogen isotope separation method

Abstract

The invention relates to a gaseous hydrogen isotope separation device and system and a gaseous hydrogen isotope separation method, and belongs to the technical field of hydrogen isotope separation. The gaseous hydrogen isotope separation device comprises an anode gas diffusion layer, an anode catalyst layer, a proton exchange membrane, a cathode catalyst layer and a cathode gas diffusion layer which are sequentially stacked; the anode gas diffusion layer and the anode catalyst layer are positioned in an anode region of the gaseous hydrogen isotope separation device, and the cathode catalyst layer and the cathode gas diffusion layer are positioned in a cathode region of the gaseous hydrogen isotope separation device; the gas inlet and the first gas outlet are formed in the anode region; the second gas outlet is formed in the cathode region; the gas inlet is used for being communicated with hydrogen isotope mixed gas; the anode region is connected with the anode of a power supply, and the cathode region is connected with the cathode of the power supply. According to the device, the hydrogen isotope mixed gas can be rapidly separated, the separation factor of the gaseous hydrogen isotope is high, and the separation effect is good.

Description

Technical Field

[0001] This application relates to the field of hydrogen isotope separation technology, and particularly to a gaseous hydrogen isotope separation device, system and method for separating gaseous hydrogen isotopes. Background Technology

[0002] Hydrogen isotopes play a crucial role in various industrial applications and scientific research. In fusion reactors, tritium (D2) and tritium (T2) are commonly used as fuels for fusion reactions. However, unreacted deuterium and tritium must be rapidly recovered, separated, purified, and recycled to ensure the stable operation of the fusion reactor. Therefore, the development and improvement of hydrogen isotope gas separation technologies are of great significance for fusion reactors and other applications involving deuterium and tritium.

[0003] Currently, the main methods for separating hydrogen isotopes include cryogenic distillation and cryogenic chromatography. Cryogenic distillation requires an ultra-low temperature environment (20–25 K), which consumes a lot of energy and has high construction costs. Cryogenic chromatography has a small throughput and requires intermittent liquid nitrogen supply and removal operations, making the equipment system complex and unable to be scaled up for the separation of gaseous hydrogen isotopes. Summary of the Invention

[0004] The purpose of this application is to provide a gaseous hydrogen isotope separation device, system, and method, which can rapidly separate gaseous hydrogen isotopes with good separation effect.

[0005] In a first aspect, this application provides a gaseous hydrogen isotope separation device, comprising an anode gas diffusion layer, an anode catalyst layer, a proton exchange membrane, a cathode catalyst layer, and a cathode gas diffusion layer stacked sequentially; the anode gas diffusion layer and the anode catalyst layer are located in the anode region of the gaseous hydrogen isotope separation device, and the cathode catalyst layer and the cathode gas diffusion layer are located in the cathode region of the gaseous hydrogen isotope separation device; the gaseous hydrogen isotope separation device further includes: a gas inlet and a first gas outlet disposed in the anode region, and a second gas outlet disposed in the cathode region; the gas inlet is used to communicate with a hydrogen isotope mixture; the anode region is used to connect to the positive terminal of a power source, and the cathode region is used to connect to the negative terminal of a power source.

[0006] The gaseous hydrogen isotope separation device provided in this application is used to separate hydrogen isotope mixtures. The hydrogen reduction reaction occurring at the cathode catalyst layer and the hydrogen oxidation reaction occurring at the anode catalyst layer can both rapidly generate significant electrocatalytic gaseous hydrogen isotope separation effects. This causes high-mass gases in the hydrogen isotope mixture to accumulate in the anode region, while low-mass gases accumulate in the cathode region, thereby achieving rapid separation of the hydrogen isotope mixture. Furthermore, the separation factor of gaseous hydrogen isotopes is high, and the separation effect is good.

[0007] In conjunction with the first aspect, in an optional embodiment of this application, the gaseous hydrogen isotope separation device is further provided with a temperature controller.

[0008] In the above technical solution, by controlling the temperature inside the gaseous hydrogen isotope separation device to 25-45℃, the separation factor of gaseous hydrogen isotopes can be further improved, thereby enhancing the separation effect of gaseous hydrogen isotopes.

[0009] In conjunction with the first aspect, in an optional embodiment of this application, the gaseous hydrogen isotope separation device is further provided with a gas humidifier, which is used to humidify the hydrogen isotope mixture.

[0010] In the above technical solution, the separation rate of gaseous hydrogen isotopes can be further improved by humidifying the hydrogen isotope mixture.

[0011] In conjunction with the first aspect, in the optional embodiments of this application, the anode catalyst layer, the proton exchange membrane, and the cathode catalyst layer do not contain carbon materials with a single-layer carbon atom structure.

[0012] In the above technical solution, the protons generated during the separation of gaseous hydrogen isotopes are not affected by the difference in migration rate of carbon atoms in the monolayer, so that the cathode catalyst layer and the anode catalyst layer can fully generate an electrocatalytic separation effect of gaseous hydrogen isotopes, significantly improving the separation rate of gaseous hydrogen isotopes.

[0013] Alternatively, the anode catalyst layer, proton exchange membrane, and cathode catalyst layer may not contain graphene.

[0014] In conjunction with the first aspect, in an optional embodiment of this application, the cathode catalyst in the cathode catalyst layer is selected from at least one of Ir, Ru, Au, Pd and Ni.

[0015] Optionally, the cathode catalyst is selected from at least one of Ru and Ni.

[0016] In the above technical solution, compared with other materials used for the cathode catalyst in the cathode catalyst layer, using Ru or Ni as the cathode catalyst can significantly improve the separation factor of gaseous hydrogen isotopes and improve the separation effect of gaseous hydrogen isotopes.

[0017] Optionally, the loading of the cathode catalyst in the cathode catalyst layer is 0.1 mg / cm³. 2 ~1mg / cm 2 .

[0018] In conjunction with the first aspect, in an optional embodiment of this application, the anolyte catalyst in the anolyte catalyst layer contains Pt, and the cathode catalyst in the cathode catalyst layer does not contain Pt.

[0019] In the above technical solution, when the anode catalyst contains Pt, the cathode catalyst does not contain highly active Pt, which enables the cathode catalyst layer and the anode catalyst layer to fully generate an electrocatalytic separation effect of gaseous hydrogen isotopes, significantly improving the separation rate and separation effect of gaseous hydrogen isotopes.

[0020] Optionally, the loading of the anode catalyst in the anode catalyst layer is 0.1 mg / cm³. 2 ~1mg / cm 2 .

[0021] In conjunction with the first aspect, in an optional embodiment of this application, the proton exchange membrane is a Nafion membrane.

[0022] In a second aspect, this application provides a gaseous hydrogen isotope separation system, comprising: at least two gaseous hydrogen isotope separation devices arranged along a preset direction as provided in any of the first aspects above; wherein, the second gas outlet of each gaseous hydrogen isotope separation device is connected to the gas inlet of a gaseous hydrogen isotope separation device adjacent to it and located downstream in the preset direction; and the first gas outlet of each gaseous hydrogen isotope separation device is connected to the gas inlet of a gaseous hydrogen isotope separation device adjacent to it and located upstream in the preset direction.

[0023] The gaseous hydrogen isotope separation system provided in this application is equipped with at least two gaseous hydrogen isotope separation devices connected in series, and the gas path is designed to improve the separation effect of gaseous hydrogen isotopes.

[0024] In conjunction with the second aspect, in an optional embodiment of this application, the gaseous hydrogen isotope separation system includes a plurality of gaseous hydrogen isotope separation devices arranged along a preset direction, and the hydrogen isotope mixture is used to communicate with the gas inlet of the gaseous hydrogen isotope separation device located in the middle of the preset direction.

[0025] In the above technical solution, the hydrogen isotope mixture is connected to the gas inlet of the gaseous hydrogen isotope separator located in the middle of the preset direction. After the hydrogen isotope mixture is separated by the gaseous hydrogen isotope separator located in the middle of the preset direction, the high mass number gas in the hydrogen isotope mixture is enriched upstream step by step, and the low mass number gas in the hydrogen isotope mixture is enriched downstream step by step, which can greatly improve the separation effect of gaseous hydrogen isotopes.

[0026] Thirdly, this application provides a method for separating gaseous hydrogen isotopes, wherein the method employs a gaseous hydrogen isotope separation device as provided in any of the first aspects above; or, the method employs a gaseous hydrogen isotope separation system as provided in any of the second aspects above; the method includes: connecting the gaseous hydrogen isotope separation device to a power source, introducing a hydrogen isotope mixture into a gas inlet, and collecting the outflowing gases from a first gas outlet and a second gas outlet respectively.

[0027] The method for separating gaseous hydrogen isotopes provided in this application can rapidly separate hydrogen isotope mixtures, and the separation factor of gaseous hydrogen isotopes is high, resulting in good separation effect.

[0028] Optionally, the temperature inside the gaseous hydrogen isotope separation device is controlled at 25℃~45℃. Attached Figure Description

[0029] To more clearly illustrate the technical solutions of the embodiments of this application, the accompanying drawings used in the embodiments will be briefly introduced below. It should be understood that the following drawings only show some embodiments of this application and should not be regarded as a limitation of the scope. For those skilled in the art, other related drawings can be obtained based on these drawings without creative effort.

[0030] Figure 1 This is a schematic diagram of the structure of the gaseous hydrogen isotope separation device provided in the embodiments of this application.

[0031] Figure 2 A diagram illustrating the separation mechanism of the gaseous hydrogen isotope separation device provided in the embodiments of this application.

[0032] Figure 3 This is a schematic diagram of the structure of the gaseous hydrogen isotope separation system provided in an embodiment of this application.

[0033] Figure 4 The figure shows the separation effect of the gaseous hydrogen isotope separation device in Example 1 on gaseous hydrogen isotopes.

[0034] Figure 5 This is a comparison chart of the separation factors of gaseous hydrogen isotopes at different temperatures using the gaseous hydrogen isotope separation device of Example 1.

[0035] Figure 6 The graph shows a comparison of the separation effects of the gaseous hydrogen isotope separation devices in Examples 1-5 on gaseous hydrogen isotopes.

[0036] Icons: 100-Gaseous hydrogen isotope separation device; 101-Gas inlet; 102-First gas outlet; 103-Second gas outlet; 110-Anode gas diffusion layer; 120-Anode catalyst layer; 130-Proton exchange membrane; 140-Cathode catalyst layer; 150-Cathode gas diffusion layer; 160-Electrode plate; 170-Power supply; 180-First pipeline; 181-First gas mass flow controller; 182-Gas humidifier; 183-First valve.

[0037] 200 - Gaseous hydrogen isotope separation system; 201 - Preset direction; 210 - First collection device; 220 - Second collection device; 230 - Second pipeline; 231 - Second gas mass flow controller; 232 - Second valve; 233 - First gas detection device; 240 - Third pipeline; 241 - Third gas mass flow controller; 242 - Third valve; 243 - Second gas detection device. Detailed Implementation

[0038] The embodiments of the technical solution of this application will now be described in detail with reference to the accompanying drawings. These embodiments are only used to more clearly illustrate the technical solution of this application and are therefore merely examples, and should not be used to limit the scope of protection of this application.

[0039] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this application belongs; the terminology used herein is for the purpose of describing particular embodiments only and is not intended to limit this application; the terms “comprising” and “having”, and any variations thereof, in the specification and the foregoing description of the drawings are intended to cover non-exclusive inclusion.

[0040] In the description of the embodiments of this application, technical terms such as "first" and "second" are used only to distinguish different objects and should not be construed as indicating or implying relative importance or implicitly specifying the number, specific order, or primary and secondary relationship of the indicated technical features. In the description of the embodiments of this application, "multiple" means two or more, unless otherwise explicitly defined.

[0041] In this document, the term "embodiment" means that a particular feature, structure, or characteristic described in connection with an embodiment may be included in at least one embodiment of this application. The appearance of this phrase in various places throughout the specification does not necessarily refer to the same embodiment, nor is it a separate or alternative embodiment mutually exclusive with other embodiments. It will be explicitly and implicitly understood by those skilled in the art that the embodiments described herein can be combined with other embodiments.

[0042] In the description of the embodiments of this application, the term "multiple" refers to two or more (including two).

[0043] In the description of the embodiments of this application, the technical terms "middle", "upper", "lower", "inner" etc. indicate the orientation or positional relationship based on the orientation or positional relationship shown in the drawings. They are only for the convenience of describing the embodiments of this application and simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation. Therefore, they should not be construed as limitations on the embodiments of this application.

[0044] In the description of the embodiments of this application, unless otherwise expressly specified and limited, the technical term "connection" and other such terms should be interpreted broadly. For example, it can refer to a fixed connection, a detachable connection, or an integral connection; it can refer to a mechanical connection or an electrical connection; it can refer to a direct connection or an indirect connection through an intermediate medium; it can refer to the internal communication of two components or the interaction between two components. Those skilled in the art can understand the specific meaning of the above terms in the embodiments of this application according to the specific circumstances.

[0045] This application provides a gaseous hydrogen isotope separation device. Figure 1 Please refer to the schematic diagram of the gaseous hydrogen isotope separation device provided in the embodiments of this application. Figure 1 The gaseous hydrogen isotope separation device 100 provided in this application includes an anode gas diffusion layer 110, an anode catalyst layer 120, a proton exchange membrane 130, a cathode catalyst layer 140, and a cathode gas diffusion layer 150 stacked sequentially.

[0046] The side of the proton exchange membrane 130 facing away from the cathode catalyst layer 140 is defined as the anode region, and the side of the proton exchange membrane 130 facing away from the anode catalyst layer 120 is defined as the cathode region.

[0047] The anode gas diffusion layer 110 and the anode catalyst layer 120 are located in the anode region of the gaseous hydrogen isotope separator 100, and the cathode catalyst layer 140 and the cathode gas diffusion layer 150 are located in the cathode region of the gaseous hydrogen isotope separator 100. The anode region is used to connect to the positive terminal of the power supply 170, and the cathode region is used to connect to the negative terminal of the power supply 170.

[0048] The gaseous hydrogen isotope separation device 100 further includes: a gas inlet 101 and a first gas outlet 102 disposed in the anode region, and a second gas outlet 103 disposed in the cathode region. The gas inlet 101 is used to communicate with the hydrogen isotope mixture; the first gas outlet 102 is used to discharge the high-mass gas from the hydrogen isotope mixture, and the second gas outlet 103 is used to discharge the low-mass gas from the hydrogen isotope mixture.

[0049] In this application, a hydrogen isotope mixture refers to a mixture containing at least two of the following gases: H2, D2, and T2.

[0050] When using the gaseous hydrogen isotope separation device 100 provided in this application to separate hydrogen isotope mixtures, the anode region is first connected to the positive terminal of the DC power supply 170, and the cathode region is connected to the negative terminal of the DC power supply 170; then the hydrogen isotope mixture is introduced into the gas inlet 101.

[0051] In this application, the first gas outlet 102 is configured such that the separated high-mass hydrogen isotope gas passes through the anode gas diffusion layer 110 and then flows out of the first gas outlet 102; the second gas outlet 103 is configured such that the separated low-mass hydrogen isotope gas passes through the cathode gas diffusion layer 150 and then flows out of the second gas outlet 103.

[0052] Figure 2 This is a separation mechanism diagram of the gaseous hydrogen isotope separation device provided in the embodiments of this application. Please refer to it. Figure 1 and Figure 2 Taking a hydrogen isotope mixture containing only H2 and D2 as an example, when the gaseous hydrogen isotope separation device 100 provided in this application is used to separate the hydrogen isotope mixture, the hydrogen isotope mixture first reacts in the anode catalyst layer 120 under the action of the positive electrode of the power supply 170 to produce protons. The produced protons pass through the proton exchange membrane 130 and enter the cathode catalyst layer 140. The hydrogen reduction reaction (HER) occurring in the cathode catalyst layer 140 and the hydrogen oxidation reaction (HOR) occurring in the anode catalyst layer 120 can both quickly produce obvious electrocatalytic gaseous hydrogen isotope separation effects, causing the high mass number gas (i.e., D2) in the hydrogen isotope mixture to be enriched in the anode region and flow out through the first gas outlet 102, while the low mass number gas (i.e., H2) in the hydrogen isotope mixture is enriched in the cathode region and flow out through the second gas outlet 103. By collecting the outflowing gases from the first gas outlet 102 and the second gas outlet 103 respectively, the separated H2 and D2 can be obtained.

[0053] Therefore, the gaseous hydrogen isotope separation device 100 provided in this application uses the electrocatalytic reaction process on both sides of the proton exchange membrane 130 as the rate-controlling step, which can realize the rapid separation of hydrogen isotope mixtures, and the gaseous hydrogen isotope separation factor is high and the separation effect is good.

[0054] It is understandable that if the hydrogen isotope mixture contains H2, D2, and T2 simultaneously, when the gaseous hydrogen isotope separation device 100 provided in this application is used to separate the hydrogen isotope mixture, the high mass number gases (i.e., T2 and D2) in the hydrogen isotope mixture are enriched in the anode region and flow out through the first gas outlet 102, while the low mass number gases (i.e., D2 and H2) in the hydrogen isotope mixture are enriched in the cathode region and flow out through the second gas outlet 103. In this case, it is only necessary to pass the gases collected from the first gas outlet 102 and the second gas outlet 103 back into the gaseous hydrogen isotope separation device 100 for further separation.

[0055] Please see Figure 1 The gaseous hydrogen isotope separation device 100 provided in this application further includes two electrode plates 160; one electrode plate 160 is located in the anode region and is attached to the side of the anode gas diffusion layer 110 away from the proton exchange membrane 130; the other electrode plate 160 is located in the cathode region and is attached to the side of the cathode gas diffusion layer 150 away from the proton exchange membrane 130. The electrode plate 160 located in the anode region is used for electrical connection to the positive electrode of the power supply 170, and the electrode plate 160 located in the cathode region is used for electrical connection to the negative electrode of the power supply 170.

[0056] In this embodiment, the electrode plate 160 is a graphite plate.

[0057] In the embodiments of this application, the first gas outlet 102 is disposed at the electrode plate 160 in the anode region, and the second gas outlet 103 is disposed at the electrode plate 160 in the cathode region.

[0058] It should be noted that, for example, the first gas outlet 102 and the second gas outlet 103 can also be located in other areas; for example, the first gas outlet 102 can be located in the anode gas diffusion layer 110, as long as the separated high-mass hydrogen isotope gas can pass through the anode gas diffusion layer 110 and then flow out from the first gas outlet 102; the second gas outlet 103 can be located in the cathode gas diffusion layer 150, as long as the separated low-mass hydrogen isotope gas can pass through the cathode gas diffusion layer 150 and then flow out from the second gas outlet 103.

[0059] In the embodiments of this application, the gas inlet 101 is disposed at the electrode plate 160 in the anode region. It should be noted that, for example, the gas inlet 101 can also be disposed in other regions; for example, the gas inlet 101 can be disposed in the anode gas diffusion layer 110, as long as it can enable the hydrogen isotope mixture to enter the gaseous hydrogen isotope separator 100 through the gas inlet 101 and then enter the anode gas diffusion layer 110.

[0060] In some optional embodiments of this application, the proton exchange membrane 130 is a Nafion membrane. It should be noted that in other feasible embodiments, the proton exchange membrane 130 can also be other membrane structures, as long as they can conduct protons.

[0061] Both the anode catalyst layer 120 and the cathode catalyst layer 140 contain a carbon support and a catalytic material supported on the carbon support. The anode catalyst in the anode catalyst layer 120 needs to have electrocatalytic hydrogen oxidation reaction performance; the cathode catalyst in the cathode catalyst layer 140 needs to have electrocatalytic hydrogen reduction reaction performance.

[0062] In some optional embodiments of this application, the anode catalyst layer 120, proton exchange membrane 130, and cathode catalyst layer 140 do not contain carbon materials with a single-layer carbon atom structure. This allows the protons generated during the separation of gaseous hydrogen isotopes to be unaffected by differences in the migration rates of single-layer carbon atoms, enabling the cathode catalyst layer 140 and anode catalyst layer 120 to fully exert an electrocatalytic separation effect on gaseous hydrogen isotopes, significantly improving the separation rate of gaseous hydrogen isotopes.

[0063] Furthermore, in this embodiment, the anode catalyst layer 120, the proton exchange membrane 130, and the cathode catalyst layer 140 do not contain graphene.

[0064] In some optional embodiments of this application, the carbon support in the anode catalyst layer 120 and the cathode catalyst layer 140 is carbon powder; in other feasible embodiments, the carbon support in the anode catalyst layer 120 and the cathode catalyst layer 140 may also be other carbon materials, etc.

[0065] In some optional embodiments of this application, the anode catalyst in the anode catalyst layer 120 contains Pt; as an example, the anode catalyst can be Pt or a Pt-based alloy, etc.

[0066] Furthermore, when the anode catalyst in the anode catalyst layer 120 contains Pt, the cathode catalyst in the cathode catalyst layer 140 does not contain Pt.

[0067] When the anode catalyst contains Pt, and the cathode catalyst does not contain highly active Pt, the cathode catalyst layer 140 and the anode catalyst layer 120 can fully generate an electrocatalytic separation effect of gaseous hydrogen isotopes, significantly improving the separation rate and separation effect of gaseous hydrogen isotopes.

[0068] Furthermore, in this embodiment, the anode catalyst is Pt.

[0069] In some optional embodiments of this application, the loading of the anode catalyst in the anode catalyst layer 120 is 0.1 mg / cm³. 2 ~1mg / cm2 As an example, the loading of the anode catalyst in the anode catalyst layer 120 can be 0.1 mg / cm³. 2 0.2 mg / cm 2 0.3 mg / cm 2 0.4 mg / cm 2 0.5 mg / cm 2 0.6 mg / cm 2 0.7 mg / cm 2 0.8 mg / cm 2 0.9 mg / cm 2 and 1mg / cm 2 The value of any one of the points or the range between any two.

[0070] In some optional embodiments of this application, the cathode catalyst in the cathode catalyst layer 140 is selected from at least one of Ir, Ru, Au, Pd and Ni.

[0071] To further improve the separation effect of gaseous hydrogen isotopes, in this embodiment, the cathode catalyst is selected from at least one of Ru and Ni. Compared with the cathode catalyst in the cathode catalyst layer 140, using Ru or Ni as the cathode catalyst can significantly improve the separation factor of gaseous hydrogen isotopes and enhance the separation effect of gaseous hydrogen isotopes.

[0072] It should be noted that in other feasible embodiments of this application, the cathode catalyst may also be an alloy, such as Ir-based alloy, Ru-based alloy, Au-based alloy, Pd-based alloy, or Ni-based alloy.

[0073] In some optional embodiments of this application, the loading of the cathode catalyst in the cathode catalyst layer 140 is 0.1 mg / cm³. 2 ~1mg / cm 2 As an example, the loading of the cathode catalyst in the cathode catalyst layer 140 can be 0.1 mg / cm³. 2 0.2 mg / cm 2 0.3 mg / cm 2 0.4 mg / cm 2 0.5 mg / cm 2 0.6 mg / cm 2 0.7 mg / cm 2 0.8 mg / cm 2 0.9 mg / cm 2 and 1mg / cm 2 The value of any one of the points or the range between any two.

[0074] In some optional embodiments of this application, the corresponding catalyst solution can be sprayed onto both sides of the proton exchange membrane 130 using the CCM method, and then hot-pressed to form the anodic catalyst layer 120 and the cathode catalyst layer 140 located on both sides of the proton exchange membrane 130.

[0075] In some optional embodiments of this application, both the anode gas diffusion layer 110 and the cathode gas diffusion layer 150 are carbon paper containing microporous layers, such as Toray YLS series carbon paper.

[0076] In some optional embodiments of this application, after the anode catalyst layer 120 and the cathode catalyst layer 140 are formed on both sides of the proton exchange membrane 130, the anode gas diffusion layer 110, the cathode gas diffusion layer 150, and the electrode plate 160 are assembled into a whole.

[0077] In some optional embodiments of this application, the gaseous hydrogen isotope separation device 100 is further provided with a temperature controller (not shown in the figure). By controlling the temperature inside the gaseous hydrogen isotope separation device 100 to 25-45°C, the separation factor of gaseous hydrogen isotopes can be further improved, thereby enhancing the separation effect of gaseous hydrogen isotopes.

[0078] Furthermore, the gaseous hydrogen isotope separation device 100 is also provided with a first pipeline 180, which is connected to the gas inlet 101 to introduce hydrogen isotope mixed gas into the gas inlet 101.

[0079] Furthermore, a first gas mass flow controller 181 is also installed on the first pipeline 180 to monitor the gas flow rate in real time.

[0080] In some optional embodiments of this application, a gas humidifier 182 is also provided on the first pipeline 180 to humidify the hydrogen isotope mixture; by humidifying the hydrogen isotope mixture, the separation rate of gaseous hydrogen isotopes can be further improved.

[0081] Furthermore, the humidifying component is selected according to the composition of the gaseous hydrogen isotope mixture; for example, if the gaseous hydrogen isotope mixture contains H2 and D2, the corresponding humidifying component is at least one of H2O and D2O.

[0082] In some optional embodiments of this application, a first valve 183 is also provided on the first pipeline 180 to control the opening and closing of the first pipeline 180. As an example, the first valve 183 can be a three-way valve or the like.

[0083] This application also provides a gaseous hydrogen isotope separation system 200. Figure 3 For a schematic diagram of the gaseous hydrogen isotope separation system 200 provided in this embodiment, please refer to [link / reference]. Figure 3 The gaseous hydrogen isotope separation system 200 includes at least two gaseous hydrogen isotope separation devices 100 arranged along a preset direction 201.

[0084] The structure and connection relationships of the gaseous hydrogen isotope separation device 100 are described above and will not be repeated here.

[0085] The second gas outlet 103 of each gaseous hydrogen isotope separator 100 is connected to the gas inlet 101 of the adjacent gaseous hydrogen isotope separator 100 located downstream of the preset direction 201; the first gas outlet 102 of each gaseous hydrogen isotope separator 100 is connected to the gas inlet 101 of the adjacent gaseous hydrogen isotope separator 100 located upstream of the preset direction 201.

[0086] The gaseous hydrogen isotope separation system 200 provided in this application is provided with at least two gaseous hydrogen isotope separation devices 100 connected in series, and the gas path is designed accordingly; if the separation factor of a single gaseous hydrogen isotope separation device 100 is α, then the separation factor of the gaseous hydrogen isotope separation system 200 formed by n gaseous hydrogen isotope separation devices 100 is α. n Therefore, the separation effect of gaseous hydrogen isotopes can be improved.

[0087] In some optional embodiments of this application, the gaseous hydrogen isotope separation system 200 includes a plurality of gaseous hydrogen isotope separation devices 100 arranged along a preset direction 201. As an example, the number of gaseous hydrogen isotope separation devices 100 in the gaseous hydrogen isotope separation system 200 can be three, four, five, six, seven, or even more. It should be noted that this application does not limit the specific number of gaseous hydrogen isotope separation devices 100 in the gaseous hydrogen isotope separation system 200, and the number can be set according to specific circumstances.

[0088] In the gaseous hydrogen isotope separation system 200, the gaseous hydrogen isotope separation device 100 located in the middle of the preset direction 201 is used as the boundary, and its upstream region is defined as the anode enrichment region and its downstream region is defined as the cathode enrichment region.

[0089] In some optional embodiments of this application, when the gaseous hydrogen isotope separation system 200 includes a plurality of gaseous hydrogen isotope separation devices 100 arranged along a preset direction 201, the hydrogen isotope mixture is used to communicate with the gas inlet 101 of the gaseous hydrogen isotope separation device 100 located in the middle of the preset direction 201.

[0090] In the above configuration, the hydrogen isotope mixture is connected to the gas inlet 101 of the gaseous hydrogen isotope separator 100 located in the middle of the preset direction 201. After the hydrogen isotope mixture is separated by the gaseous hydrogen isotope separator 100 located in the middle of the preset direction 201, the high mass number gas in the hydrogen isotope mixture is gradually enriched upstream, and the low mass number gas in the hydrogen isotope mixture is gradually enriched downstream, which can greatly improve the separation effect of gaseous hydrogen isotopes.

[0091] Furthermore, in the gaseous hydrogen isotope separation system 200, only the gaseous hydrogen isotope separation device 100 used to connect with the hydrogen isotope mixing gas source needs to be equipped with a first pipeline 180, and other gaseous hydrogen isotope separation devices 100 do not need to be equipped with a first pipeline 180.

[0092] Please see Figure 3 In the embodiments provided in this application, the positive terminal of the external DC power supply 170 is simultaneously connected to the anode region of all gaseous hydrogen isotope separation devices 100, and the negative terminal of the external DC power supply 170 is simultaneously connected to the cathode region of all gaseous hydrogen isotope separation devices 100; thus realizing the control of the entire gaseous hydrogen isotope separation system 200 through one external DC power supply 170.

[0093] It should be noted that, in other optional embodiments of this application, each gaseous hydrogen isotope separation device 100 may be provided with an external DC power supply 170 to achieve individual control of each gaseous hydrogen isotope separation device 100.

[0094] In some optional embodiments of this application, the gaseous hydrogen isotope separation system 200 is further provided with a first collection device 210 and a second collection device 220.

[0095] The first collection device 210 is located upstream of all gaseous hydrogen isotope separators 100 and is connected to the first gas outlet 102 of the gaseous hydrogen isotope separator 100 located upstream of the preset direction 201, so as to collect the high mass number gas from the hydrogen isotope mixture enriched in the entire gaseous hydrogen isotope separation system 200. As an example, the first collection device 210 is a gas storage tank.

[0096] The second collection device 220 is located downstream of all gaseous hydrogen isotope separators 100 and is connected to the second gas outlet 103 of the gaseous hydrogen isotope separator 100 located downstream of the preset direction 201, so as to collect the low mass number gas in the hydrogen isotope mixture enriched by the entire gaseous hydrogen isotope separation system 200. As an example, the second collection device 220 is a gas storage tank.

[0097] In this application, the gaseous hydrogen isotope separation system 200 is further provided with a second pipeline 230, which is used to connect the first collection device 210 and the first gas outlet 102 of the gaseous hydrogen isotope separation device 100 located upstream of the preset direction 201.

[0098] The second pipeline 230 is also equipped with a second gas mass flow controller 231, a second valve 232, and a first gas detection device 233; wherein, the second mass flow controller 231 is used to monitor the gas flow rate in real time; the second valve 232 is used to control the opening and closing of the second pipeline 230; and the first gas detection device 233 is used to detect gas components, for example, the first gas detection device 233 can be a gas chromatograph, etc.

[0099] In this application, along the passage of the second pipeline 230, the first collecting device 210, the second gas mass flow controller 231, the second valve 232 and the first gas outlet 102 are connected in sequence; the second valve 232 is a three-way valve, and the three passages of the three-way valve are respectively connected to the first gas outlet 102, the first collecting device 210 and the first gas detection device 233.

[0100] In this application, the gaseous hydrogen isotope separation system 200 is further provided with a third pipeline 240, which is used to connect the second collection device 220 and the second gas outlet 103 of the gaseous hydrogen isotope separation device 100 located downstream of the preset direction 201.

[0101] The third pipeline 240 is also equipped with a third gas mass flow controller 241, a third valve 242, and a second gas detection device 243; wherein, the third mass flow controller 241 is used to monitor the gas flow rate in real time; the third valve 242 is used to control the opening and closing of the third pipeline 240; and the second gas detection device 243 is used to detect gas components, for example, the second gas detection device 243 can be a gas chromatograph, etc.

[0102] In this application, along the passage of the third pipeline 240, the second collecting device 220, the third gas mass flow controller 241, the third valve 242 and the second gas outlet 103 are connected in sequence; the third valve 242 is a three-way valve, and the three passages of the three-way valve are respectively connected to the second gas outlet 103, the second collecting device 220 and the second gas detection device 243.

[0103] In some optional embodiments of this application, all gaseous hydrogen isotope separation devices 100 can be connected and then packaged and assembled into a whole with end plates (not shown in the figure), tooling (not shown in the figure), etc.

[0104] This application also provides a method for separating gaseous hydrogen isotopes, wherein the method for separating gaseous hydrogen isotopes employs the gaseous hydrogen isotope separation device provided above; or, the method for separating gaseous hydrogen isotopes employs the gaseous hydrogen isotope separation system provided above; the method for separating gaseous hydrogen isotopes includes: connecting the gaseous hydrogen isotope separation device to a power source, introducing a hydrogen isotope mixture into a gas inlet, and collecting the outflowing gases from a first gas outlet and a second gas outlet respectively.

[0105] The method for separating gaseous hydrogen isotopes provided in this application can rapidly separate hydrogen isotope mixtures, and the separation factor of gaseous hydrogen isotopes is high, resulting in good separation effect.

[0106] In some optional embodiments of this application, the temperature inside the gaseous hydrogen isotope separation device is controlled at 25°C to 45°C.

[0107] As an example, the temperature of the gaseous hydrogen isotope separation device can be controlled to any one of 25°C, 30°C, 35°C, 40°C and 45°C or a range between any two.

[0108] In some optional embodiments of this application, the hydrogen isotope mixture is humidified before being introduced into the gas inlet; this can further improve the separation rate of gaseous hydrogen isotopes.

[0109] Furthermore, humidifying the hydrogen isotope mixture to a relative humidity of 30%–100% can accelerate the separation rate of gaseous hydrogen isotopes.

[0110] As an example, the relative humidity can be any one of 30%, 40%, 50%, 60%, 70%, 80%, 90%, and 100%, or a range between any two.

[0111] In some optional embodiments of this application, the current density of the power supply regulation is 0.025 A / cm². 2 ~0.3A / cm 2 It can achieve both a high separation rate and a high separation factor.

[0112] As an example, the current density can be 0.025 A / cm². 2 0.05A / cm 2 0.075A / cm 2 0.1A / cm 2 0.125A / cm 2 0.15A / cm 2 0.175A / cm 2 0.2A / cm 2 0.225A / cm 20.25A / cm 2 0.275A / cm 2 and 0.3A / cm 2 The value of any one of the points or the range between any two.

[0113] To make the objectives, technical solutions, and advantages of the embodiments of this application clearer, the technical solutions in the embodiments of this application will be clearly and completely described below. Where specific conditions are not specified in the embodiments, conventional conditions or conditions recommended by the manufacturer shall apply. Reagents or instruments whose manufacturers are not specified are all conventional products that can be purchased commercially.

[0114] Example 1

[0115] This embodiment provides a gaseous hydrogen isotope separation device, which is prepared by the following steps:

[0116] (1) Cut the Nafion N211 membrane material to 2cm. 2 After being treated in H2O2 at 80℃ for 1 hour, the membrane was rinsed three times with deionized water. Then, it was placed in a 5wt% H2SO4 aqueous solution and treated at 80℃ for 1 hour, rinsed three times with deionized water, and stored in a dry environment for later use to obtain the Nafion proton exchange membrane.

[0117] (2) A Pt / C catalyst and Nafion resin solution with a mass ratio of 2:1 were added to isopropanol and ultrasonically dispersed in an ice-water bath for 20 min to obtain an anode catalyst ink. A Ni / C catalyst and Nafion resin solution with a mass ratio of 2:1 were added to isopropanol and ultrasonically dispersed in an ice-water bath for 20 min to obtain a cathode catalyst ink.

[0118] The Nafion proton exchange membrane was placed on a heating stage at 60°C. Then, using an airbrush, cathode catalyst ink and anode catalyst ink were coated onto both sides of the Nafion proton exchange membrane, forming an anode catalyst layer and a cathode catalyst layer on both sides of the proton exchange membrane. The cathode catalyst loading in the cathode catalyst layer was 0.5 mg / cm³. 2 The loading of the anolyte catalyst in the anolyte catalyst layer is 0.5 mg / cm³. 2 .

[0119] (3) Toray YLS series carbon paper is selected as the anode gas diffusion layer and the cathode gas diffusion layer. The anode gas diffusion layer is placed on the surface of the anode catalyst layer and the cathode gas diffusion layer is placed on the surface of the cathode catalyst layer. After hot pressing, a sandwich structure is formed. Then, graphite plates are placed on the surfaces of the anode gas diffusion layer and the cathode gas diffusion layer respectively and packaged into a whole. The graphite plate in the anode area is connected to the positive terminal of the DC power supply, and the graphite plate in the cathode area is connected to the negative terminal of the DC power supply to obtain a gaseous hydrogen isotope separation device.

[0120] The graphite plate in the anode region is provided with a gas inlet and a first gas outlet, while the graphite plate in the cathode region is provided with a second gas outlet.

[0121] Example 2

[0122] This embodiment provides a gaseous hydrogen isotope separation device. The only difference between this embodiment and Embodiment 1 is that the cathode catalyst in Embodiment 1 is replaced with Ru instead of Ni.

[0123] Example 3

[0124] This embodiment provides a gaseous hydrogen isotope separation device. The only difference between this embodiment and Embodiment 1 is that the cathode catalyst in Embodiment 1 is replaced with Ir instead of Ni.

[0125] Example 4

[0126] This embodiment provides a gaseous hydrogen isotope separation device. The only difference between this embodiment and Embodiment 1 is that the cathode catalyst in Embodiment 1 is replaced with Au instead of Ni.

[0127] Example 5

[0128] This embodiment provides a gaseous hydrogen isotope separation device. The only difference between this embodiment and Embodiment 1 is that the cathode catalyst in Embodiment 1 is replaced with Cu instead of Ni.

[0129] Experimental Example 1

[0130] The separation factor of the gaseous hydrogen isotope separation device obtained in Example 1 for gaseous hydrogen isotopes was tested, and the results are as follows: Figure 4 As shown.

[0131] The detection method is as follows: A mixture of H2 / D2 (molar ratio 1:1) is humidified and introduced into a gaseous hydrogen isotope separator via an H2O / D2O (molar ratio 1:1) flow rate controlled at 20 mL / min. The gases exiting from the first and second gas outlets are dried, and then passed into a gas chromatograph for analysis of the gas components. The separation factor is calculated. The temperature of the gaseous hydrogen isotope separator is controlled at 25℃, and the current density is 0.2 A / cm³. 2 .

[0132] In Experiment 1, 1.4 mL / cm³ could be achieved within 1 minute. 2 Separation of hydrogen isotope gases.

[0133] from Figure 4 It can be seen that the separation factor of the gaseous hydrogen isotope separation device in Example 1 is 1.95, which shows a good separation effect on gaseous hydrogen isotopes.

[0134] Experiment Example 2

[0135] A comparison of the separation factors of gaseous hydrogen isotopes at different temperatures using the gaseous hydrogen isotope separation device obtained in Example 1 is shown in the following figures. Figure 5 As shown.

[0136] The detection method is as follows: A mixture of H2 / D2 (molar ratio 1:1) is humidified and introduced into a gaseous hydrogen isotope separator via an H2O / D2O (molar ratio 1:1) flow rate controlled at 20 mL / min. The gases exiting from the first and second gas outlets are dried, and then passed into a gas chromatograph for analysis of the gas components. The separation factor is calculated. The temperature of the gaseous hydrogen isotope separator is controlled between 5℃ and 45℃, and the current density is 0.1 A / cm³. 2 .

[0137] from Figure 5 It can be seen that when the temperature is between 25℃ and 45℃, the separation factor of the gaseous hydrogen isotope separation device is higher and the separation effect is better.

[0138] Experimental Example 3

[0139] The separation factors of gaseous hydrogen isotopes were compared between the gaseous hydrogen isotope separation devices obtained in Examples 1-5, and the results are as follows: Figure 6 As shown.

[0140] The detection method is as follows: A mixture of H2 / D2 (molar ratio 1:1) is humidified and introduced into a gaseous hydrogen isotope separator via an H2O / D2O (molar ratio 1:1) flow rate controlled at 20 mL / min. The gases exiting the first and second gas outlets are dried, and then passed into a gas chromatograph for analysis of the gas components. The separation factor is calculated. The temperature of the gaseous hydrogen isotope separator is controlled at 25℃, and the current density is 0.025 A / cm². 2 ~0.25A / cm 2 .

[0141] from Figure 6It can be seen that different cathode catalysts have different hydrogen isotope separation effects, among which Ru and Ni have better gaseous hydrogen isotope separation effects.

[0142] The embodiments described above are some, but not all, of the embodiments of this application. The detailed description of the embodiments of this application is not intended to limit the scope of the claimed application, but merely to illustrate selected embodiments. All other embodiments obtained by those skilled in the art based on the embodiments of this application without inventive effort are within the scope of protection of this application.

Claims

1. A gaseous hydrogen isotope separation device, characterized in that, include: The anode gas diffusion layer, anode catalyst layer, proton exchange membrane, cathode catalyst layer and cathode gas diffusion layer are stacked in sequence. The anode gas diffusion layer and the anode catalyst layer are located in the anode region of the gaseous hydrogen isotope separation device, and the cathode catalyst layer and the cathode gas diffusion layer are located in the cathode region of the gaseous hydrogen isotope separation device. The gaseous hydrogen isotope separation device further includes: a gas inlet and a first gas outlet disposed in the anode region, and a second gas outlet disposed in the cathode region; The gas inlet is used to communicate with a hydrogen isotope mixed gas; The anode region is used to connect to the positive terminal of the power supply, and the cathode region is used to connect to the negative terminal of the power supply.

2. The gaseous hydrogen isotope separation device according to claim 1, characterized in that, The gaseous hydrogen isotope separation device is also equipped with a temperature controller.

3. The gaseous hydrogen isotope separation device according to claim 1, characterized in that, The gaseous hydrogen isotope separation device is also equipped with a gas humidifier, which is used to humidify the hydrogen isotope mixture.

4. The gaseous hydrogen isotope separation device according to any one of claims 1-3, characterized in that, The anode catalyst layer, the proton exchange membrane, and the cathode catalyst layer all contain carbon materials without a single-layer carbon atom structure; Optionally, the anode catalyst layer, the proton exchange membrane, and the cathode catalyst layer do not contain graphene.

5. The gaseous hydrogen isotope separation device according to any one of claims 1-3, characterized in that, The cathode catalyst in the cathode catalyst layer is selected from at least one of Ir, Ru, Au, Pd and Ni; Optionally, the cathode catalyst is selected from at least one of Ru and Ni; Optionally, the loading of the cathode catalyst in the cathode catalyst layer is 0.1 mg / cm³. 2 ~1mg / cm 2 .

6. The gaseous hydrogen isotope separation device according to any one of claims 1-3, characterized in that, The anode catalyst in the anode catalyst layer contains Pt, and the cathode catalyst in the cathode catalyst layer does not contain Pt; Optionally, the loading of the anode catalyst in the anode catalyst layer is 0.1 mg / cm³. 2 ~1mg / cm 2 .

7. The gaseous hydrogen isotope separation device according to any one of claims 1-3, characterized in that, The proton exchange membrane is a Nafion membrane.

8. A gaseous hydrogen isotope separation system, characterized in that, include: At least two gaseous hydrogen isotope separation devices as described in any one of claims 1-7, arranged along a predetermined direction; The second gas outlet of each gaseous hydrogen isotope separator is connected to the gas inlet of the adjacent gaseous hydrogen isotope separator located downstream of the preset direction. The first gas outlet of each of the gaseous hydrogen isotope separation devices is connected to the gas inlet of the adjacent gaseous hydrogen isotope separation device located upstream of the preset direction.

9. The gaseous hydrogen isotope separation system according to claim 8, characterized in that, The gaseous hydrogen isotope separation system includes a plurality of gaseous hydrogen isotope separation devices arranged along the preset direction, and the hydrogen isotope mixture is used to communicate with the gas inlet of the gaseous hydrogen isotope separation device located in the middle of the preset direction.

10. A method for separating gaseous hydrogen isotopes, characterized in that, The method for separating gaseous hydrogen isotopes employs a gaseous hydrogen isotope separation device as described in any one of claims 1-7; or, the method for separating gaseous hydrogen isotopes employs a gaseous hydrogen isotope separation system as described in claim 8 or 9. The method for separating gaseous hydrogen isotopes includes: connecting the gaseous hydrogen isotope separation device to a power source, introducing a hydrogen isotope mixture into the gas inlet, and collecting the outflowing gases from the first gas outlet and the second gas outlet, respectively. Optionally, the temperature inside the gaseous hydrogen isotope separation device is controlled at 25°C to 45°C.

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