A device and method for verifying gas-solid reaction kinetic model of polonium capture material
By designing a verification device for the gas-solid reaction kinetics model of polonium capture materials, the difficult problem of studying the characteristics of Po-210 aerosol capture materials was solved, the characteristics research and verification of Po-210 aerosol capture materials were realized on a laboratory scale, and accurate experimental data and model verification were provided.
Patent Information
- Application Number
- CN202411613942.7
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2024-11-13
- Publication Date
- 2025-09-30
- Estimated Expiration
- 2044-11-13
AI Technical Summary
Existing technologies make it difficult to effectively study and verify the characteristics of Po-210 aerosol capture materials, especially the capture effect of Po-210 aerosols in reactor accidents, due to the lack of suitable experimental equipment and methods.
A gas-solid reaction kinetics model verification device for polonium capture materials was designed, including a gas supply assembly, a temperature-controllable heating furnace, and a capture material packed bed. By simulating polonium evaporation and gas-solid reaction, the gas radiation equivalent was monitored in real time, and gas-solid reaction kinetics experiments were performed.
The characteristics of Po-210 aerosol capture materials have been studied on a laboratory scale. Adsorption and capture experiments can be performed at different temperatures, meeting the needs of characteristic research on Po-210 aerosol capture materials and providing accurate experimental data and model verification.
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Figure CN119510684B_ABST
Abstract
Description
Technical Field
[0001] The present invention relates to the technical field of radionuclide testing equipment, and in particular to a device and method for verifying a gas-solid reaction kinetic model of a polonium capture material. Background Art
[0002] Fourth-generation advanced fast reactors (G4FRs) have attracted significant international attention due to their high inherent safety profile and unique advantages in regenerative fuel cycles, radioactive waste reprocessing, simplified reactor systems, and shortened refueling cycles. However, due to the inherent characteristics of G4FRs, neutron activation can produce the volatile radioactive nuclide Po-210.
[0003] Po-210 is an extremely toxic radionuclide that readily forms radioactive aerosols. Its half-life is 138.4 days, placing it in the extremely toxic group. Once introduced into living organisms, it can damage the cellular structure of tissues and organs, damage DNA, and lead to cell death. When a reactor releases radioactive nuclides, such as a double-walled containment breach, a leak in the primary cover gas system, or a rupture in the secondary outlet piping of a heat exchanger, the released Po-210 aerosols can have serious consequences for workers and the environment. Therefore, the development of Po-210 aerosol capture materials is necessary to capture these escaping aerosols. To investigate the properties of Po-210 aerosol capture materials, a gas-solid reaction kinetic model for these materials is necessary. Summary of the Invention
[0004] The present invention provides a device and method for verifying the gas-solid reaction kinetic model of polonium capture materials, which is suitable for laboratory-scale gas-solid reaction kinetic simulation of polonium capture material aerosols and meets the requirements for characteristic research of Po-210 aerosol capture materials.
[0005] The present invention is achieved through the following technical solutions:
[0006] In the first aspect, the present invention provides a device for verifying the gas-solid reaction kinetic model of polonium capture material, comprising: a gas supply component, which can output test gas with a set flow rate and corresponding pressure; a first temperature-controlled heating furnace, the inner cavity of the first temperature-controlled heating furnace is connected to the output end of the gas supply component, the first temperature-controlled heating furnace is adapted to have a feeding mechanism and a first radiometer, the feeding mechanism is used to feed an evaporation crucible filled with polonium into the inner cavity of the first temperature-controlled heating furnace; a second temperature-controlled heating furnace, the inner cavity of the second temperature-controlled heating furnace is connected to the inner cavity of the first temperature-controlled heating furnace, the inner cavity of the second temperature-controlled heating furnace is provided with a capture material filling bed, and the gas outlet end of the second temperature-controlled heating furnace is adapted to have a second radiometer and a second pressure gauge.
[0007] The gas-solid reaction kinetic model verification device of polonium capture material provided by the present invention includes a gas supply component, a first temperature-controllable heating furnace and a second temperature-controllable heating furnace. The inner cavity of the first temperature-controllable heating furnace is connected to the output end of the gas supply component and is adapted to be equipped with a feeding mechanism and a first radiometer. The second temperature-controllable heating furnace is connected to the inner cavity of the first temperature-controllable heating furnace and is provided with a capture material packed bed. The gas outlet end of the second temperature-controllable heating furnace is adapted to be equipped with a second radiometer and a second pressure gauge.
[0008] During use, the inner cavity temperature of the first controllable temperature heating furnace is raised to the temperature required for polonium evaporation simulation, and then the polonium metal powder is placed in the first controllable temperature heating furnace through the feeding mechanism and reacted for a certain time. During the metal heating process, the gas containing the polonium capture material is monitored in real time by the first radiometer. At the same time, the corresponding flow rate of test gas can be output through the gas supply component, and the gas pressure of the output test gas is monitored, so that the polonium metal vapor is purged to the second controllable temperature heating furnace through the test gas, and the polonium capture material in the capture material filling bed undergoes a gas-solid reaction with the polonium metal vapor. The radiation equivalent in the captured gas is then detected in real time by the second radiometer. Therefore, the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to conduct gas-solid reaction kinetics experimental verification.
[0009] The temperatures within the first and second temperature-controlled heating furnaces can be controlled to control the temperature of the gas-solid reaction, enabling adsorption capture experiments of the capture material at different temperatures. Furthermore, based on the test gas pressure and the value of the second pressure gauge, the change in gas flow rate before and after the reaction can be calculated.
[0010] Therefore, the gas-solid reaction kinetics model verification device of the polonium capture material provided by the present invention can be used for laboratory-scale gas-solid reaction kinetics simulation of polonium capture material aerosols, meeting the requirements for characteristic research of Po-210 aerosol capture materials.
[0011] In an optional embodiment of the present application, the gas supply assembly includes: a gas cylinder, which is used to store test gas; a test gas flow controller, which is connected in series to the gas outlet end of the gas cylinder; a first pressure gauge, which is arranged at the output end of the test gas flow controller to ensure that the gas supply assembly can output the test gas at a set flow rate and detect the input pressure of the test gas in real time.
[0012] In an optional embodiment of the present application, it also includes a tail gas absorption bottle assembly, which contains a soluble acidic solution. The tail gas absorption bottle assembly is connected in series to the gas outlet end of the second temperature-controllable heating furnace to absorb the captured tail gas during the reaction process through the soluble acidic solution in the tail gas absorption bottle assembly.
[0013] In an optional embodiment of the present application, a vacuum pump is further included, which is connected in series to the gas outlet end of the suction bottle assembly to force the gas in the pipeline to be absorbed by the vacuum pump, thereby reducing the deposition and diffusion of the gas in the pipeline.
[0014] In an optional embodiment of the present application, the gas outlet of the vacuum pump is equipped with a third radiometer to detect the radiation equivalent of the gas exhausted by the vacuum pump in real time, so as to ensure that the exhaust gas is completely captured.
[0015] In a second aspect, the present invention provides a method for verifying a gas-solid reaction kinetic model of a polonium capture material, based on the aforementioned gas-solid reaction kinetic model verification device of a polonium capture material, comprising the following steps:
[0016] Raising the temperature in the first temperature-controllable heating furnace to a temperature required for polonium evaporation simulation;
[0017] After the temperature in the first temperature-controllable heating furnace reaches the desired simulation temperature, the evaporation crucible containing the polonium metal powder is introduced into the inner cavity of the first temperature-controllable heating furnace, and the radiation equivalent of the gas in the first temperature-controllable heating furnace is monitored in real time;
[0018] At the same time, a test gas at a set flow rate is fed into the inner ring of the first temperature-controllable heating furnace to purge the polonium metal vapor to the polonium capture material installed in the capture material packed bed;
[0019] The radiation equivalent of the gas captured by the capture material packed bed is used as the outlet concentration of the polonium capture material to conduct gas-solid reaction kinetics experiments.
[0020] The method for verifying the gas-solid reaction kinetic model of a polonium capture material provided by the present invention is based on the aforementioned gas-solid reaction kinetic model verification device for a polonium capture material. After the temperature in a first temperature-controllable heating furnace is raised to the temperature required for polonium evaporation simulation, an evaporation crucible with polonium metal powder is introduced into the inner cavity of the first temperature-controllable heating furnace, and the radiation equivalent of the gas in the first temperature-controllable heating furnace is monitored in real time. At the same time, a test gas with a set flow rate is input into the inner ring of the first temperature-controllable heating furnace to blow the polonium metal vapor to the polonium capture material installed in the capture material packed bed, and the radiation equivalent of the gas after capture by the capture material packed bed is used as the outlet concentration of the polonium capture material, and a gas-solid reaction kinetics experiment is performed to verify the gas-solid reaction kinetics, thereby meeting the requirements for characteristic research of Po-210 aerosol capture materials.
[0021] In an optional embodiment of the present application, the step of introducing the gas captured by the capture material packed bed into a tail gas absorption bottle assembly containing a soluble acidic solution, so that the captured tail gas of the reaction process is absorbed by the soluble acidic solution in the tail gas absorption bottle assembly.
[0022] In an optional embodiment of the present application, the method further includes the step of calculating the breakthrough adsorption capacity and saturation adsorption capacity of the capture material based on the test data; the calculation model of the breakthrough adsorption capacity is: The calculation model of the saturated adsorption capacity is: Where: q B is the penetration adsorption amount, q E is the saturated adsorption capacity, in mg / g; F is the gas volume flow rate, in mL / min; t B is the penetration time, in min; C0 is the inlet heavy element vapor concentration, C i The concentration of heavy element vapor at the outlet after t minutes, in mg / m 3 ; W is the adsorbent loading amount, unit g; q E is the saturated adsorption capacity, unit is mg / g; T E Depletion time, unit: mL / min.
[0023] In an optional embodiment of the present application, the method further includes the steps of fitting the experimental data to establish an adsorption kinetics model, and verifying the adsorption kinetics model of similar materials through an adsorption kinetics empirical model.
[0024] Specifically, the adsorption kinetics empirical model is Where: K' is the rate parameter, unit min -1 ; τ is the 50% penetration time, in min; C is the outlet heavy element concentration, in mg / m 3 ; C0 is the concentration of imported heavy elements, unit is mg / m 3 ; t is time, unit is min.
[0025] Compared with the prior art, the present invention has the following advantages and beneficial effects:
[0026] 1. The gas-solid reaction kinetic model verification device for polonium capture materials provided by the present invention includes a gas supply component, a first temperature-controlled heating furnace and a second temperature-controlled heating furnace. The inner cavity of the first temperature-controlled heating furnace is connected to the output end of the gas supply component and is adapted to be equipped with a feeding mechanism and a first radiometer. The second temperature-controlled heating furnace is connected to the inner cavity of the first temperature-controlled heating furnace and is provided with a capture material packed bed. The gas outlet end of the second temperature-controlled heating furnace is adapted to be equipped with a second radiometer and a second pressure gauge. The first temperature-controlled heating furnace can provide the temperature required for polonium evaporation simulation, and the first radiometer can be used to measure the polonium capture material. The gas of the material is monitored in real time, the test gas of the corresponding flow rate can be output through the gas supply component, and the gas pressure of the output test gas is monitored. The polonium metal vapor is purged to the second controllable temperature heating furnace through the test gas, and the polonium capture material in the capture material packed bed undergoes a gas-solid reaction with the polonium metal vapor. The radiation equivalent in the captured gas is then detected in real time by the second radiometer. Therefore, the radiation equivalent of the captured gas can be used as the outlet concentration of the polonium capture material to conduct gas-solid reaction kinetics experimental verification, thereby meeting the characteristics research needs of Po-210 aerosol capture materials.
[0027] 2. The device for verifying the gas-solid reaction kinetic model of polonium capture materials provided by the present invention has controllable temperatures in the first and second temperature-controlled heating furnaces, and can control the temperature of the gas-solid reaction, thereby enabling adsorption and capture experiments of the capture material at different temperatures; at the same time, based on the gas pressure of the test gas and the value of the second pressure gauge, the change in gas flow rate before and after the reaction can be calculated; therefore, it can be used for laboratory-scale simulation of the gas-solid reaction kinetics of polonium capture material aerosols.
[0028] 3. The present invention provides a method for verifying the gas-solid reaction kinetic model of polonium capture materials. Based on the aforementioned gas-solid reaction kinetic model verification device for polonium capture materials, after the temperature in the first temperature-controllable heating furnace is raised to the temperature required for polonium evaporation simulation, the evaporation crucible with polonium metal powder is sent into the inner cavity of the first temperature-controllable heating furnace, and the radiation equivalent of the gas in the first temperature-controllable heating furnace is monitored in real time. At the same time, a set flow rate of test gas is input into the inner ring of the first temperature-controllable heating furnace to blow the polonium metal vapor to the polonium capture material installed in the capture material packed bed, and the radiation equivalent of the gas after capture by the capture material packed bed is used as the outlet concentration of the polonium capture material, and the gas-solid reaction kinetics experiment is verified to meet the characteristics research needs of Po-210 aerosol capture materials. BRIEF DESCRIPTION OF THE DRAWINGS
[0029] To more clearly illustrate the technical solutions of the embodiments of the present invention, the following briefly describes the drawings required for use in the embodiments. It should be understood that the following drawings only illustrate certain embodiments of the present invention and should not be considered as limiting the scope of the present invention. Those skilled in the art can also derive other relevant drawings based on these drawings without inventive effort.
[0030] In the attached figure:
[0031] Figure 1 Schematic diagram of the gas path principle of the device for verifying the gas-solid reaction kinetic model of polonium capture material according to an embodiment of the present invention;
[0032] Figure 2 This is a graph showing the variation of the adsorption amount of metal vapor by the polonium capture material according to an embodiment of the present invention over time;
[0033] Figure 3 This is a graph showing the change in the adsorption amount of metal vapor by the polonium capture material according to an embodiment of the present invention at different temperatures.
[0034] Reference numerals:
[0035] 10-gas supply assembly, 11-gas storage bottle, 12-test gas flow controller, 13-first pressure gauge, 20-first temperature-controllable heating furnace, 21-feeding mechanism, 22-first radiometer, 23-evaporation crucible, 30-second temperature-controllable heating furnace, 31-capture material packed bed, 32-second radiometer, 33-second pressure gauge, 40-tail gas absorption bottle assembly, 50-vacuum pump, 51-third radiometer. DETAILED DESCRIPTION
[0036] To make the objectives, technical solutions, and advantages of the embodiments of the present application more clear, the technical solutions in the embodiments of the present application will be clearly and completely described below in conjunction with the accompanying drawings of the embodiments of the present application. Obviously, the described embodiments are only part of the embodiments of the present application, not all of the embodiments. Generally, the components of the embodiments of the present application described and shown in the drawings herein can be arranged and designed in various different configurations.
[0037] Therefore, the following detailed description of the embodiments of the present application provided in the accompanying drawings is not intended to limit the scope of the present application for protection, but merely represents selected embodiments of the present application. All other embodiments obtained by persons of ordinary skill in the art based on the embodiments in the present application without creative work are within the scope of protection of the present application.
[0038] It should be noted that similar reference numerals and letters represent similar items in the following figures. Therefore, once an item is defined in one figure, it does not need to be further defined or explained in subsequent figures. In the absence of conflict, the embodiments and features in the embodiments of this application can be combined with each other.
[0039] In the description of the embodiments of the present application, the indicated orientations or positional relationships are based on the orientations or positional relationships shown in the accompanying drawings, or are the orientations or positional relationships in which the product of the application is conventionally placed when in use, or are the orientations or positional relationships conventionally understood by those skilled in the art. These are merely for the convenience of describing the present application and simplifying the description, and do not indicate or imply that the device or component referred to must have a specific orientation, be constructed and operated in a specific orientation. Therefore, they should not be understood as limitations on the present application.
[0040] In the description of this application, unless otherwise expressly specified or limited, the terms "disposed," "installed," "connected," and "connected" should be understood in a broad sense. For example, they can refer to fixed, detachable, or integral connections; mechanical or electrical connections; direct or indirect connections through an intermediate medium; and internal communication between two components. Those skilled in the art will understand the specific meanings of the above terms in this application based on the specific circumstances.
[0041] Example 1
[0042] Combine Figure 1 This embodiment provides a device for verifying the gas-solid reaction kinetic model of a polonium capture material, comprising: a gas supply component 10, wherein the gas supply component 10 is capable of outputting a test gas with a set flow rate and corresponding pressure; a first temperature-controlled heating furnace 20, wherein the inner cavity of the first temperature-controlled heating furnace 20 is connected to the output end of the gas supply component 10, and the first temperature-controlled heating furnace 20 is adapted to be equipped with a feeding mechanism 21 and a first radiometer 22, wherein the feeding mechanism 21 is used to feed an evaporation crucible 23 filled with polonium into the inner cavity of the first temperature-controlled heating furnace 20; a second temperature-controlled heating furnace 30, wherein the inner cavity of the second temperature-controlled heating furnace 30 is connected to the inner cavity of the first temperature-controlled heating furnace 20, and the inner cavity of the second temperature-controlled heating furnace 30 is provided with a capture material filled bed 31, and the gas outlet end of the second temperature-controlled heating furnace 30 is adapted to be equipped with a second radiometer 32 and a second pressure gauge 33.
[0043] Specifically, the gas supply assembly 10 includes: a gas cylinder 11 for storing test gas; a test gas flow controller 12 connected in series to the gas outlet of the gas cylinder 11; and a first pressure gauge 13, disposed at the output of the test gas flow controller 12 to ensure that the gas supply assembly 10 can output the test gas at a set flow rate and to monitor the input pressure of the test gas in real time. The gas cylinder 11 is typically a steel cylinder, and the test gas is generally an inert gas, such as argon or helium; nitrogen cannot be used.
[0044] It is understood that the first temperature-controlled heating furnace 20 and the second temperature-controlled heating furnace 30 can be two-stage programmable temperature-controlled high-temperature reactors or split programmable temperature-controlled high-temperature reactors that are stacked or placed separately, with the two-stage programmable temperature-controlled high-temperature reactor being preferred. The feeding mechanism 21 is typically an automated stepper motor feeding mechanism 21, such as a screw-slider mechanism driven by a stepper motor. A crucible is provided at the lower end of the feeding mechanism 21 to serve as a metal powder evaporation simulation crucible.
[0045] On this basis, this embodiment also includes a tail gas absorption bottle assembly 40, which contains a soluble acidic solution. The tail gas absorption bottle assembly 40 is connected in series to the gas outlet end of the second temperature-controlled heating furnace 30 to absorb the captured tail gas during the reaction process through the soluble acidic solution in the tail gas absorption bottle assembly 40.
[0046] It should be understood that the tail gas absorption bottle assembly 40 generally includes a plurality of absorption bottles connected in series, each of which contains a soluble acid solution, such as inorganic acid solutions such as hydrochloric acid solution, nitric acid solution and sulfuric acid solution.
[0047] Furthermore, this embodiment also includes a vacuum pump 50, which is connected in series to the gas outlet end of the suction bottle assembly to forcefully absorb the gas in the pipeline through the vacuum pump 50, thereby reducing the deposition and diffusion of the gas in the pipeline.
[0048] Correspondingly, the gas outlet end of the vacuum pump 50 is equipped with a third radiometer 51 to detect the radiation equivalent of the gas discharged from the vacuum pump 50 in real time, so as to ensure that the exhaust gas is completely captured.
[0049] It should be noted that, during the test, each component was connected with a 6mm or 10mm stainless steel reaction tube, the accuracy of the gas supplied by the test gas flow controller 12 was ±0.1mL / min, and the accuracy of the two pressure gauge valves was 1.5%.
[0050] In summary, the gas-solid reaction kinetic model verification device of polonium capture material provided in this embodiment includes a gas supply component 10, a first temperature-controlled heating furnace 20, a second temperature-controlled heating furnace 30, a tail gas absorption bottle component 40 and a vacuum pump 50. The inner cavity of the first temperature-controlled heating furnace 20 is connected to the output end of the gas supply component 10, and is adapted to have a feeding mechanism 21 and a first radiometer 22. The second temperature-controlled heating furnace 30 is connected to the inner cavity of the first temperature-controlled heating furnace 20, is provided with a capture material filling bed 31, and the gas outlet end of the second temperature-controlled heating furnace 30 is adapted to have a second radiometer 32 and a second pressure gauge 33. The tail gas absorption bottle component 40 and the vacuum pump 50 are sequentially connected in series to the gas outlet end of the second temperature-controlled heating furnace 30.
[0051] During use, the inner cavity temperature of the first controllable temperature heating furnace 20 is raised to the temperature required for polonium evaporation simulation, and then the polonium metal powder is placed in the first controllable temperature heating furnace 20 through the feeding mechanism 21 and reacted for a certain period of time. During the metal heating process, the gas containing the polonium capture material is monitored in real time by the first radiometer 22. At the same time, the test gas of the corresponding flow rate can be output through the gas supply component 10, and the gas pressure of the output test gas is monitored, so that the polonium metal vapor is purged to the second controllable temperature heating furnace 30 through the test gas, and the polonium capture material in the capture material filled bed 31 reacts with the polonium metal vapor in a gas-solid reaction. The radiation equivalent in the captured gas is then detected in real time by the second radiometer 32. Thus, the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to conduct gas-solid reaction kinetics experimental verification.
[0052] During the gas-solid reaction, the captured exhaust gas is drawn into the exhaust gas absorption bottle assembly 40 by the vacuum pump 50, where it is thoroughly absorbed by the soluble acidic solution. The vacuum pump 50 also forcibly absorbs the participating gases in the pipeline, reducing gas deposition and diffusion within the pipeline. Furthermore, the third radiometer 51 can detect the radiation equivalent of the exhaust gas from the vacuum pump 50. The value of the third radiometer 51 can be used to adjust the volume of the soluble acidic solution required to completely capture and absorb the exhaust gas.
[0053] The temperatures within the first and second temperature-controlled heating furnaces 20 and 30 can be controlled to control the temperature of the gas-solid reaction, enabling adsorption and capture experiments of the capture material at different temperatures. Furthermore, based on the test gas pressure and the value of the second pressure gauge 33, the change in gas flow rate before and after the reaction can be calculated.
[0054] Therefore, the gas-solid reaction kinetics model verification device for polonium capture materials provided in this embodiment has the characteristics of precise temperature control of polonium evaporation simulation, less diffusion and deposition, precise reactor control, and easy exhaust gas treatment. It can be used for laboratory-scale gas-solid reaction kinetics simulation of polonium capture material aerosols, meeting the requirements of characteristic research of Po-210 aerosol capture materials.
[0055] Example 2
[0056] This embodiment provides a method for verifying a gas-solid reaction kinetic model of a polonium capture material, based on the gas-solid reaction kinetic model verification device of a polonium capture material described in Example 1, comprising the following steps:
[0057] S10, raising the temperature in the first temperature-controllable heating furnace 20 to a temperature required for polonium evaporation simulation.
[0058] Specifically, the temperature in the evaporation simulation unit (the first temperature-controlled heating furnace 20 is kept stable) is raised to the desired polonium evaporation temperature through programmable temperature control. Before reaching this temperature, the feeding mechanism 21 retracts, moving the crucible containing the metal powder away from the high-temperature zone. In this embodiment, the desired polonium evaporation temperature is between 500°C and 700°C.
[0059] S20, after the temperature in the first temperature-controllable heating furnace 20 reaches the desired simulation temperature, the evaporation crucible 23 containing the polonium metal powder is introduced into the inner cavity of the first temperature-controllable heating furnace 20, and the radiation equivalent of the gas in the first temperature-controllable heating furnace 20 is monitored in real time;
[0060] At the same time, a test gas with a set flow rate is input into the inner ring of the first temperature-controllable heating furnace 20 to purge the polonium metal vapor to the polonium capture material installed in the capture material packed bed 31 .
[0061] Specifically, after the temperature in first temperature-controlled heating furnace 20 reaches the desired simulation temperature, a program-controlled feeding mechanism 21 delivers a crucible containing metal powder to the high-temperature reaction zone of first temperature-controlled heating furnace 20 for a predetermined reaction time. During the metal heating process, a second radiometer 32 monitors the gas containing the polonium capture material in real time. A suitable gas flow rate is set using a test gas flow controller 12 to purge the polonium metal vapor into the capture material packed bed 31, where a gas-solid reaction occurs between the polonium capture material and the polonium metal vapor.
[0062] In this embodiment, the gas flow rate output by the test gas flow controller 12 is 100 mL / min-200 mL / min, and the gas-solid reaction temperature is 30° C.-150° C. (the furnace chamber temperature of the second temperature-controllable heating furnace 30 ).
[0063] S30, introducing the gas captured by the capture material packed bed 31 into the tail gas absorption bottle assembly 40 containing a soluble acid solution, so that the soluble acid solution in the tail gas absorption bottle assembly 40 absorbs the captured tail gas during the reaction process.
[0064] The radiation equivalent of the exhaust gas from the vacuum pump 50 is detected by the third radiometer 51 , and the volume of the required soluble acid solution is adjusted according to the value of the third radiometer 51 until the exhaust gas can be completely captured and absorbed.
[0065] Generally, the soluble acidic solution is a nitric acid solution with a mass fraction of 1% to 8%. When the gas-solid reaction is completed, the feeding mechanism 21 is returned to its initial position through program control, and the metal evaporation of the polonium capture material is cut off.
[0066] S40, using the radiation equivalent of the gas captured by the capture material packed bed 31 as the polonium capture material outlet concentration, and conducting a gas-solid reaction kinetics experiment to verify the specific steps are:
[0067] S41. Calculate the penetration adsorption capacity and saturation adsorption capacity of the capture material based on the test data; the calculation model of the penetration adsorption capacity is: The calculation model of the saturated adsorption capacity is: Where: q B is the penetration adsorption amount, q E is the saturated adsorption capacity, in mg / g; F is the gas volume flow rate, in mL / min; t B is the penetration time, in min; C0 is the inlet heavy element vapor concentration, C i The concentration of heavy element vapor at the outlet after t minutes, in mg / m 3 ; W is the adsorbent loading amount, unit g; q E is the saturated adsorption capacity, unit is mg / g; T E Depletion time, unit: mL / min.
[0068] S42. Fit the experimental data to establish an adsorption kinetics model, and verify the adsorption kinetics model of similar materials through the adsorption kinetics empirical model.
[0069] Specifically, based on the experimental data, the Langmuir isotherm equation and the Freundlich adsorption isotherm equation were used to preliminarily fit the experimental data and establish the adsorption kinetics model. Among them, the Langmuir isotherm equation is The Freundlich adsorption isotherm equation is:
[0070] Then, the Yoon-Nelson adsorption kinetics semi-empirical model was introduced to verify the adsorption kinetics model of similar materials. The adsorption kinetics empirical model (Yoon-Nelson model linear equation) is:
[0071] Where: K' is the rate parameter, unit min -1 ; τ is the 50% penetration time, in min; C is the outlet heavy element concentration, in mg / m 3 ; C0 is the concentration of imported heavy elements, unit is mg / m 3 ; t is time, unit is min.
[0072] Based on the steps described in this example, the following four verification tests were performed:
[0073] Verification Test 1
[0074] The following steps are involved:
[0075] 1) The inner chamber temperature of the first temperature-controllable heating furnace is raised to 500° C., the temperature required for polonium evaporation simulation, by programmed temperature control. Before reaching this temperature, the crucible containing the metal powder is kept away from the high temperature zone.
[0076] 2) When the temperature reaches the desired simulated temperature of 500°C, the crucible containing the metal powder is introduced into the high-temperature reaction zone of the first temperature-controlled heating furnace via a feeding mechanism and reacted for 30 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time using a first radiometer;
[0077] 3) Setting an appropriate gas flow rate of 100 mL / min through the test gas flow controller to blow the metal vapor in the first temperature-controlled heating furnace to the capture material packed bed;
[0078] 4) The metal vapor entering the capture material packed bed undergoes a gas-solid reaction with the polonium capture material at a reaction temperature of 30°C. A second radiometer is used to measure the radiation equivalent of the captured gas in real time. This radiation equivalent is used as the polonium capture material outlet concentration for experimental verification of the gas-solid reaction kinetics.
[0079] 5) After the reaction is completed, the gas captured during the reaction is thoroughly absorbed using a soluble acid solution (5% nitric acid, hydrochloric acid, sulfuric acid).
[0080] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position, cutting off the metal evaporation of the polonium capture material.
[0081] Verification Test 2
[0082] The following steps are involved:
[0083] 1) The inner chamber temperature of the first temperature-controllable heating furnace is raised to 550° C., the temperature required for polonium evaporation simulation, by programmed temperature control. Before reaching this temperature, the crucible containing the metal powder is kept away from the high temperature zone.
[0084] 2) When the temperature reaches the desired simulated temperature of 550°C, the crucible containing the metal powder is introduced into the high-temperature reaction zone of the first temperature-controlled heating furnace via a feeding mechanism and reacted for 60 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time using a first radiometer;
[0085] 3) Setting an appropriate gas flow rate of 120 mL / min through the test gas flow controller to blow the metal vapor in the first temperature-controlled heating furnace to the capture material packed bed;
[0086] 4) The metal vapor entering the capture material packed bed undergoes a gas-solid reaction with the polonium capture material at a reaction temperature of 60°C. A second radiometer is used to measure the radiation equivalent of the captured gas in real time. This radiation equivalent is used as the polonium capture material outlet concentration for experimental verification of the gas-solid reaction kinetics.
[0087] 5) After the reaction is completed, the gas captured during the reaction is completely absorbed using a soluble acidic solution (5% nitric acid).
[0088] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position, cutting off the metal evaporation of the polonium capture material.
[0089] Verification Test 3
[0090] The following steps are involved:
[0091] 1) The inner chamber temperature of the first temperature-controllable heating furnace is raised to 600° C., the temperature required for polonium evaporation simulation, by program temperature control. Before reaching this temperature, the crucible containing the metal powder is kept away from the high temperature zone.
[0092] 2) After the temperature reaches the desired simulated temperature of 600°C, the crucible containing the metal powder is introduced into the high-temperature reaction zone of the first temperature-controlled heating furnace via a feeding mechanism for 90 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time using a first radiometer;
[0093] 3) Setting an appropriate gas flow rate of 150 mL / min through the test gas flow controller to blow the metal vapor in the first temperature-controllable heating furnace to the capture material packed bed;
[0094] 4) The metal vapor entering the capture material packed bed undergoes a gas-solid reaction with the polonium capture material at a reaction temperature of 90°C. How is the temperature of the two furnaces separated? A second radiometer is used to measure the radiation equivalent of the captured gas in real time. This radiation equivalent is used as the polonium capture material outlet concentration to conduct experimental verification of the gas-solid reaction kinetics.
[0095] 5) After the reaction is completed, the gas captured during the reaction is completely absorbed using a soluble acidic solution (5% nitric acid).
[0096] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position, cutting off the metal evaporation of the polonium capture material.
[0097] Verification Test 4
[0098] The following steps are involved:
[0099] 1) The inner chamber temperature of the first temperature-controllable heating furnace is raised to 650° C., the temperature required for polonium evaporation simulation, by program temperature control. Before reaching this temperature, the crucible containing the metal powder is kept away from the high temperature zone.
[0100] 2) When the temperature reaches the desired simulated temperature of 650°C, the crucible containing the metal powder is introduced into the high-temperature reaction zone of the first temperature-controlled heating furnace via a feeding mechanism and reacts for 150 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time using a first radiometer;
[0101] 3) Setting an appropriate gas flow rate of 180 mL / min through the test gas flow controller to blow the metal vapor in the first temperature-controlled heating furnace to the capture material packed bed;
[0102] 4) The metal vapor entering the capture material packed bed undergoes a gas-solid reaction with the polonium capture material at a reaction temperature of 120°C. A second radiometer measures the radiation equivalent of the captured gas in real time. This radiation equivalent is used as the polonium capture material outlet concentration for experimental verification of the gas-solid reaction kinetics.
[0103] 5) After the reaction is completed, the gas captured during the reaction is thoroughly absorbed using a soluble acid solution and an inorganic acid (5% nitric acid).
[0104] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position, cutting off the metal evaporation of the polonium capture material.
[0105] Based on the process described in verification tests 1-4, the test was carried out to verify the calculation of the penetration adsorption capacity and saturation adsorption capacity of the capture material. The processed data are shown in the attached Figure 2 and Figure 3 shown.
[0106] In general, the method for verifying the gas-solid reaction kinetic model of polonium capture materials provided in this embodiment is based on the gas-solid reaction kinetic model verification device for polonium capture materials recorded in Example 1. After the temperature in the first temperature-controllable heating furnace is raised to the temperature required for polonium evaporation simulation, the evaporation crucible with polonium metal powder is sent into the inner cavity of the first temperature-controllable heating furnace, and the radiation equivalent of the gas in the first temperature-controllable heating furnace is monitored in real time. At the same time, the test gas with a set flow rate is input into the inner ring of the first temperature-controllable heating furnace to blow the polonium metal vapor to the polonium capture material installed in the capture material packed bed, and the radiation equivalent of the gas after capture by the capture material packed bed is used as the outlet concentration of the polonium capture material, and the gas-solid reaction kinetics experiment is verified to meet the characteristics research needs of Po-210 aerosol capture materials.
[0107] The specific implementation methods described above further illustrate the objectives, technical solutions and beneficial effects of the present invention in detail. It should be understood that the above description is only a specific implementation method of the present invention and is not intended to limit the scope of protection of the present invention. Any modifications, equivalent substitutions, improvements, etc. made within the spirit and principles of the present invention should be included in the scope of protection of the present invention.
Claims
1. A device for verifying the gas-solid reaction kinetic model of polonium capture materials, characterized in that: include: A gas supply assembly (10), wherein the gas supply assembly (10) is capable of outputting test gas at a set flow rate and corresponding pressure; a first temperature-controllable heating furnace (20), wherein the inner cavity of the first temperature-controllable heating furnace (20) is connected to the output end of the gas supply assembly (10), and the first temperature-controllable heating furnace (20) is equipped with a feeding mechanism (21) and a first radiometer (22), wherein the feeding mechanism (21) is used to feed an evaporation crucible (23) filled with polonium into the inner cavity of the first temperature-controllable heating furnace (20); A second temperature-controllable heating furnace (30), wherein the inner cavity of the second temperature-controllable heating furnace (30) is communicated with the inner cavity of the first temperature-controllable heating furnace (20), the inner cavity of the second temperature-controllable heating furnace (30) is provided with a capture material filled bed (31), and the gas outlet end of the second temperature-controllable heating furnace (30) is adapted to be equipped with a second radiometer (32) and a second pressure gauge (33).
2. The gas-solid reaction kinetic model verification device for polonium capture materials according to claim 1, characterized in that: The air supply assembly (10) comprises: A gas storage cylinder (11), wherein the gas storage cylinder (11) is used to store test gas; A test gas flow controller (12), the test gas flow controller being connected in series to the gas outlet end of the gas storage bottle (11); A first pressure gauge (13), wherein the first pressure gauge (13) is arranged at the output end of the test gas flow controller (12).
3. The gas-solid reaction kinetic model verification device for polonium capture materials according to claim 1, characterized in that: It also includes a tail gas absorption bottle assembly (40), which contains a soluble acid solution. The tail gas absorption bottle assembly (40) is connected in series to the gas outlet end of the second temperature-controllable heating furnace (30).
4. The gas-solid reaction kinetic model verification device for polonium capture materials according to claim 3, characterized in that: It also includes a vacuum pump (50), which is connected in series to the air outlet end of the absorption bottle assembly.
5. The gas-solid reaction kinetic model verification device for polonium capture materials according to claim 4, characterized in that: The air outlet end of the vacuum pump (50) is adapted to be equipped with a third radiometer (51).
6. A method for verifying the gas-solid reaction kinetic model of polonium capture materials, characterized in that: The device for verifying the gas-solid reaction kinetic model of the polonium capture material according to any one of claims 1 to 5 comprises the following steps: Raising the temperature in the first temperature-controllable heating furnace (20) to a temperature required for polonium evaporation simulation; After the temperature in the first temperature-controllable heating furnace (20) rises to a desired simulation temperature, an evaporation crucible (23) containing polonium metal powder is introduced into the inner cavity of the first temperature-controllable heating furnace (20), and the radiation equivalent of the gas in the first temperature-controllable heating furnace (20) is monitored in real time; At the same time, a test gas of a set flow rate is input into the inner ring of the first temperature-controllable heating furnace (20) to purge the polonium metal vapor to the polonium capture material installed in the capture material packed bed (31); The radiation equivalent of the gas captured by the capture material packed bed (31) is used as the polonium capture material outlet concentration to conduct gas-solid reaction kinetics experimental verification.
7. The method for verifying the gas-solid reaction kinetic model of polonium capture material according to claim 6, characterized in that: The method further comprises the step of introducing the gas captured by the capture material packed bed (31) into a tail gas absorption bottle assembly (40) containing a soluble acid solution.
8. The method for verifying the gas-solid reaction kinetic model of polonium capture material according to claim 6, characterized in that: The method further includes the steps of: calculating the penetration adsorption capacity and saturation adsorption capacity of the capture material based on the test data; The calculation model of the breakthrough adsorption amount is: The calculation model of the saturated adsorption capacity is: Where: q B is the penetration adsorption amount, q E is the saturated adsorption capacity, unit is mg / g; F is the gas volume flow rate, unit is mL / min; t B is the penetration time, in min; C0 is the inlet heavy element vapor concentration, C i The concentration of heavy element vapor at the outlet after t minutes, in mg / m 3 ; W is the adsorbent loading amount, unit g; q E is the saturated adsorption capacity, unit is mg / g; T E Depletion time, unit: mL / min.
9. The method for verifying the gas-solid reaction kinetic model of polonium capture materials according to claim 6, characterized in that: The method also includes the steps of fitting the experimental data to establish an adsorption kinetics model, and verifying the adsorption kinetics model of similar materials through an adsorption kinetics empirical model.
10. The method for verifying the gas-solid reaction kinetic model of polonium capture materials according to claim 9, characterized in that: The adsorption kinetics empirical model is: Where: K' is the rate parameter, unit min-1; τ is the 50% penetration time, unit min; C is the outlet heavy element concentration, unit mg / m3; C0 is the inlet heavy element concentration, unit mg / m3; t is the time, unit min.