Device and method for verifying gas-solid reaction kinetic model of polonium trapping material

Abstract

The invention relates to the technical field of radionuclide test equipment, in particular to a verification device and method for a gas-solid reaction kinetic model of a polonium trapping material, and the verification device comprises a gas supply assembly which can output a set flow of test gas; an inner cavity of the first temperature-controllable heating furnace is connected with the output end of the gas supply assembly, the first temperature-controllable heating furnace is provided with a feeding mechanism and a first radiometer in a matched mode, and the feeding mechanism is used for feeding an evaporation crucible filled with polonium into the inner cavity of the first temperature-controllable heating furnace; an inner cavity of the second temperature-controllable heating furnace is communicated with an inner cavity of the first temperature-controllable heating furnace, a trapping material filling bed is arranged in the inner cavity of the second temperature-controllable heating furnace, and a second radiometer and a second pressure meter are arranged at the gas outlet end of the second temperature-controllable heating furnace in a matched mode; the characteristic research requirements of the Po-210 aerosol trapping material are met. The verification method is based on the verification device.

Description

Technical Field

[0001] The invention relates to the technical field of radionuclide test 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] The fourth generation of advanced fast reactors has a high inherent safety and unique advantages in regenerative fuel cycle, radioactive waste reprocessing, reactor system simplification, and shortened refueling cycle, and therefore has received international attention. However, due to the characteristics of the fourth generation of advanced fast reactors, volatile radioactive nuclides Po-210 will be produced under neutron activation conditions.

[0003] Po-210 is an extremely toxic radionuclide that is very easy to form Po-210 radioactive aerosols. Its half-life is 138.4 days. It belongs to the extremely toxic group of nuclides. If it enters the body, it will destroy the cell structure of human tissues and organs, damage DNA and cause cell death. When a radionuclide release accident occurs in the reactor, including a double-layer container rupture accident, a primary circuit cover gas system leakage accident and a heat exchanger secondary side outlet pipe rupture accident, the leaked Po-210 aerosol may have a serious impact on the staff and the environment. Therefore, it is necessary to develop Po-210 aerosol capture materials to capture the escaped aerosols. When studying the characteristics of Po-210 aerosol capture materials, it is necessary to establish a gas-solid reaction kinetic model of polonium capture materials. Summary of the invention

[0004] The present invention provides a device and method for verifying the gas-solid reaction kinetic model of a polonium capture material, which is suitable for laboratory-scale simulation of the gas-solid reaction kinetics of aerosols of polonium capture materials 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 equipped with 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 equipped with 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 comprises 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, is provided with a capture material filling bed, and 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] When in 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 period of time. During the metal heating process, the gas carrying the polonium capture material is monitored in real time by the first radiometer, and at the same 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, 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 reacts with the polonium metal vapor. The radiation equivalent in the captured gas is then detected in real time by the second radiometer. Thus, the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to verify the gas-solid reaction kinetics experiment.

[0009] The temperatures in the first temperature-controllable heating furnace and the second temperature-controllable heating furnace can be controlled, and the temperature of the gas-solid reaction can be controlled, so that the adsorption capture experiment of the capture material at different temperatures can be carried out. 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.

[0010] Therefore, the gas-solid reaction kinetic model verification device of the polonium capture material provided by the present invention can be used for laboratory-scale gas-solid reaction kinetic simulation of the polonium capture material aerosol, 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 storage 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 storage 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, and the vacuum pump is connected in series to the gas outlet end of the suction bottle assembly to force absorption of the participating gases in the pipeline through the vacuum pump to reduce 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 rises to the desired simulation temperature, the evaporation crucible with 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 with a set flow rate is input 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 a gas-solid reaction kinetics experiment.

[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 device for verifying the gas-solid reaction kinetic model of 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 circle 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, 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 kinetic experiment is performed to verify the gas-solid reaction kinetics, thereby meeting the requirements for studying the characteristics 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 penetration adsorption amount and saturation adsorption amount of the capture material according to the test data; the calculation model of the penetration 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, 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 is the outlet heavy element vapor concentration after t minutes, in mg / m 3 ; W is the adsorbent loading, unit: g; q E is the saturated adsorption capacity, in mg / g; T E Depletion time, in 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 50% penetration time, unit is min; C is the outlet heavy element concentration, unit is mg / m 3 ; C0 is the imported heavy element concentration, unit: 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 of the polonium capture material provided by the present invention comprises 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, is provided with a capture material filling bed, and 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, the first temperature-controllable heating furnace can be used to provide the temperature required for the polonium evaporation simulation, 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 corresponding flow rate can be output through the gas supply component, and the gas pressure of the output test gas is monitored and 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 reacts with the polonium metal vapor, and then the radiation equivalent in the captured gas is 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 can control the temperatures inside the first temperature-controllable heating furnace and the second temperature-controllable heating furnace, and can control the temperature of the gas-solid reaction, so that adsorption and capture experiments of the capture materials at different temperatures can be carried out; 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 device for verifying the gas-solid reaction kinetic model of 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 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 circle 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, 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] In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the following briefly introduces 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 regarded as limiting the scope. For ordinary technicians in this field, other related drawings can also be obtained based on these drawings without creative work.

[0030] In the attached picture:

[0031] Figure 1 This is a schematic diagram of the gas path principle of the device for verifying the gas-solid reaction kinetic model of the 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 variation of 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] In order to make the purpose, technical solution and advantages of the embodiments of the present application clearer, the technical solution in the embodiments of the present application will be clearly and completely described below in conjunction with the drawings in the embodiments of the present application. Obviously, the described embodiments are part of the embodiments of the present application, rather than all the embodiments. The components of the embodiments of the present application described and shown in the drawings here 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 which protection is sought, but merely represents selected embodiments of the present application. Based on the embodiments in the present application, all other embodiments obtained by ordinary technicians in the field 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 drawings, so once an item is defined in one drawing, it does not need to be further defined and explained in subsequent drawings. 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 orientation or position relationship is based on the orientation or position relationship shown in the accompanying drawings, or is the orientation or position relationship in which the product of the application is conventionally placed when in use, or is the orientation or position relationship conventionally understood by those skilled in the art. It is only for the convenience of describing the present application and simplifying the description, and does not indicate or imply that the device or element referred to must have a specific orientation, be constructed and operated in a specific orientation, and therefore cannot be understood as a limitation on the present application.

[0040] In the description of this application, unless otherwise clearly specified and limited, the terms "set", "install", "connect", and "connect" should be understood in a broad sense, for example, it can be a fixed connection, a detachable connection, or an integral connection; it can be a mechanical connection or an electrical connection; it can be a direct connection or an indirect connection through an intermediate medium, or it can be the internal communication of two elements. For ordinary technicians in this field, the specific meanings of the above terms in this application can be understood according to specific circumstances.

[0041] Example 1

[0042] Combination Figure 1 The present embodiment provides a gas-solid reaction kinetic model verification device for polonium capture materials, comprising: a gas supply component 10, the gas supply component 10 being capable of outputting test gas of a set flow rate and corresponding pressure; a first temperature-controllable heating furnace 20, the inner cavity of the first temperature-controllable heating furnace 20 being connected to the output end of the gas supply component 10, the first temperature-controllable heating furnace 20 being adapted with a feeding mechanism 21 and a first radiometer 22, the feeding mechanism 21 being 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, the inner cavity of the second temperature-controllable heating furnace 30 being connected to the inner cavity of the first temperature-controllable heating furnace 20, the inner cavity of the second temperature-controllable heating furnace 30 being provided with a capture material filling bed 31, and the gas outlet end of the second temperature-controllable heating furnace 30 being adapted with a second radiometer 32 and a second pressure gauge 33.

[0043] Specifically, the gas supply assembly 10 includes: a gas cylinder 11, which is used to store test gas; a test gas flow controller 12, which is connected in series to the gas outlet of the gas cylinder 11; and a first pressure gauge 13, which is arranged at the output end of the test gas flow controller 12 to ensure that the gas supply assembly 10 can output the test gas of the set flow rate and detect the input pressure of the test gas in real time. Among them, the gas cylinder 11 is usually a steel cylinder group, and the test gas is generally an inert gas, such as argon and helium, and nitrogen cannot be used.

[0044] It is understandable that the first temperature-controlled heating furnace 20 and the second temperature-controlled heating furnace 30 can be two-stage program-controlled high-temperature reaction furnaces, or split program-controlled high-temperature reaction furnaces stacked or placed separately, preferably two-stage program-controlled high-temperature reaction furnaces. The feeding mechanism 21 usually adopts an automated stepper motor feeding mechanism 21, such as a screw slider mechanism driven by a stepper motor. At the same time, 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, the present 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 of 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, the present embodiment further comprises a vacuum pump 50, which is connected in series to the gas outlet end of the air suction bottle assembly so as to forcefully absorb the participating gases 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 exhausted by 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 by 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 equipped with 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 and is provided with a capture material filling bed 31. The gas outlet end of the second temperature-controlled heating furnace 30 is equipped with a second radiometer 32 and a second pressure gauge 33. The tail gas absorption bottle component 40 and the vacuum pump 50 are connected in series at the gas outlet end of the second temperature-controlled heating furnace 30 in sequence.

[0051] When in use, the inner cavity temperature of the first controllable temperature heating furnace 20 is increased 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 with 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 of the capture material filling bed 31 reacts with the polonium metal vapor in a gas-solid reaction, and then the radiation equivalent in the captured gas is detected in real time by the second radiometer 32. 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.

[0052] During the gas-solid reaction, the captured tail gas enters the tail gas absorption bottle assembly 40 under the suction of the vacuum pump 50, so that the tail gas captured during the reaction process is completely absorbed by the soluble acid solution, and the vacuum pump 50 can forcefully absorb the participating gas in the pipeline, which can reduce the deposition and diffusion of the gas in the pipeline. In addition, the third radiometer 51 can detect the radiation equivalent of the gas discharged by the vacuum pump 50, and the volume of the required soluble acid solution can be adjusted in combination with the value of the third radiometer 51 until the tail gas can be completely captured and absorbed.

[0053] The temperatures in the first temperature-controllable heating furnace 20 and the second temperature-controllable heating furnace 30 can be controlled, and the temperature of the gas-solid reaction can be controlled, so that the adsorption capture experiment of the capture material at different temperatures can be carried out. At the same time, based on the gas pressure of the test gas and the value of the second pressure gauge 33, the change of the gas flow rate before and after the reaction can be calculated.

[0054] Therefore, the gas-solid reaction kinetic model verification device of the polonium capture material provided in this embodiment has the characteristics of precise temperature control of polonium evaporation simulation, less diffusion deposition, precise reactor control and easy exhaust gas treatment. It can be used for laboratory-scale gas-solid reaction kinetic simulation of polonium capture material aerosols and meet the characteristics research needs 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 Embodiment 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] That is, the temperature in the evaporation simulation unit (the first temperature-controllable heating furnace 20 is stable) is raised to the temperature required for polonium evaporation simulation by program temperature control. Before reaching the temperature, the feeding mechanism 21 is retracted so that the crucible containing the metal powder is away from the high temperature zone. In this embodiment, the temperature required for polonium evaporation simulation is 500°C-700°C.

[0059] S20, after the temperature in the first temperature-controllable heating furnace 20 rises to the desired simulation temperature, the evaporation crucible 23 with the polonium metal powder is sent 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 circle 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 the first temperature-controllable heating furnace 20 rises to the desired simulation temperature, the crucible with the metal powder is sent to the high-temperature reaction zone of the first temperature-controllable heating furnace 20 through the program-controlled feeding mechanism 21 to react for a certain period of time. During the metal heating process, the gas with the polonium capture material is monitored in real time through the second radiometer 32, and the appropriate gas flow rate is set through the test gas flow controller 12 to purge the polonium metal vapor to the capture material packed bed 31, and the polonium capture material and the polonium metal vapor undergo a gas-solid reaction.

[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. (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 in the reaction process.

[0064] The radiation equivalent of the exhaust gas of the vacuum pump 50 is detected by the third radiometer 51 , and the volume of the required soluble acid solution is adjusted in combination with the value of the third radiometer 51 until the exhaust gas can be completely captured and absorbed.

[0065] Generally, the soluble acid solution is a nitric acid solution with a mass fraction of 1%-8%. After the gas-solid reaction is completed, the feeding mechanism 21 is returned to the initial position through program control to cut off the metal evaporation of the polonium capture material.

[0066] S40, taking the radiation equivalent of the gas captured by the capture material packed bed 31 as the outlet concentration of the polonium capture material, and conducting a gas-solid reaction kinetics experiment verification. The specific steps are:

[0067] S41, calculating the penetration adsorption amount and saturation adsorption amount of the capture material according to the test data; the calculation model of the penetration 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, 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 is the outlet heavy element vapor concentration after t minutes, in mg / m 3 ; W is the adsorbent loading, unit: g; q E is the saturated adsorption capacity, in mg / g; T E Depletion time, in 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 kinetic 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: Where: K' is the rate parameter, unit min -1 ; τ is 50% penetration time, unit is min; C is the outlet heavy element concentration, unit is mg / m 3 ; C0 is the imported heavy element concentration, unit: mg / m 3 ; t is time, unit is min.

[0072] Based on the steps described in this embodiment, the following four verification tests were performed:

[0073] Verification test 1

[0074] The following steps are involved:

[0075] 1) The inner cavity temperature of the first temperature-controllable heating furnace is raised to 500° C., a 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.

[0076] 2) When the temperature reaches the required simulation temperature of 500° C., the crucible with the metal powder is extended into the high-temperature reaction zone of the first temperature-controllable heating furnace through the feeding mechanism, and the reaction is carried out for 30 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time by the first radiometer;

[0077] 3) Setting a suitable gas flow rate of 100 mL / min through a test gas flow controller to blow the metal vapor in the first temperature-controllable heating furnace to the capture material packed bed;

[0078] 4) The metal vapor entering the capture material packed bed reacts with the polonium capture material in a gas-solid reaction at a reaction temperature of 30°C. The radiation equivalent in the captured gas is detected in real time using a second radiometer, and the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to verify the gas-solid reaction kinetics experiment.

[0079] 5) After the reaction is completed, the gas is completely absorbed by using a soluble acid solution (5% nitric acid, hydrochloric acid, sulfuric acid) to capture the tail gas during the reaction.

[0080] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position to cut off the metal evaporation of the polonium capture material.

[0081] Verification test 2

[0082] The following steps are involved:

[0083] 1) The inner cavity temperature of the first temperature-controllable heating furnace is raised to 550° C., a 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.

[0084] 2) When the temperature rises to the required simulation temperature of 550° C., the crucible with the metal powder is extended into the high-temperature reaction zone of the first temperature-controllable heating furnace through the feeding mechanism, and the reaction is carried out for 60 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time by the first radiometer;

[0085] 3) Setting a suitable gas flow rate of 120 mL / min through a test gas flow controller to blow the metal vapor in the first temperature-controllable heating furnace to the capture material packed bed;

[0086] 4) The metal vapor entering the capture material packed bed reacts with the polonium capture material in a gas-solid reaction at a reaction temperature of 60°C. The radiation equivalent in the captured gas is detected in real time using a second radiometer, and the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to verify the gas-solid reaction kinetics experiment.

[0087] 5) After the reaction is completed, the gas is completely absorbed by a soluble acid solution (5% nitric acid) to capture the tail gas during the reaction.

[0088] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position to cut off the metal evaporation of the polonium capture material.

[0089] Verification test 3

[0090] The following steps are involved:

[0091] 1) The inner cavity temperature of the first temperature-controllable heating furnace is raised to 600° C., a 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) When the temperature reaches the required simulation temperature of 600° C., the crucible with the metal powder is extended into the high-temperature reaction zone of the first temperature-controllable heating furnace through the feeding mechanism, and the reaction is carried out for 90 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time by the first radiometer;

[0093] 3) Setting a suitable gas flow rate of 150 mL / min through a 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 reacts with the polonium capture material in a gas-solid reaction, and the reaction temperature is 90°C. How to separate the temperatures of the two furnaces? The second radiometer is used to detect the radiation equivalent in the captured gas in real time, and the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to verify the gas-solid reaction kinetics experiment.

[0095] 5) After the reaction is completed, the gas is completely absorbed by a soluble acid solution (5% nitric acid) to capture the tail gas during the reaction.

[0096] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position to cut off the metal evaporation of the polonium capture material.

[0097] Verification test 4

[0098] The following steps are involved:

[0099] 1) The inner cavity temperature of the first temperature-controllable heating furnace is raised to 650° C., a 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 rises to the required simulation temperature of 650° C., the crucible with the metal powder is extended into the high-temperature reaction zone of the first temperature-controllable heating furnace through the feeding mechanism, and the reaction is carried out for 150 minutes. During the metal heating process, the gas containing the polonium capture material is monitored in real time by the first radiometer;

[0101] 3) Setting a suitable gas flow rate of 180 mL / min through a test gas flow controller to blow the metal vapor in the first temperature-controllable heating furnace to the capture material packed bed;

[0102] 4) The metal vapor entering the capture material packed bed reacts with the polonium capture material in a gas-solid reaction at a reaction temperature of 120°C. The radiation equivalent in the captured gas is detected in real time using a second radiometer, and the radiation equivalent of the captured gas is used as the outlet concentration of the polonium capture material to conduct a gas-solid reaction kinetics experiment verification.

[0103] 5) After the reaction is completed, the gas is completely absorbed by using a soluble acid solution and an inorganic acid (5% nitric acid) to capture the tail gas during the reaction.

[0104] 6) When the gas-solid reaction is completed, the feeding mechanism is controlled to return to the initial position to cut off the metal evaporation of the polonium capture material.

[0105] Based on the process described in verification test 1-4, the test was carried out to verify the calculation of the penetration adsorption amount and saturation adsorption amount of the capture material. The processed data is 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 device for verifying the gas-solid reaction kinetic model of polonium capture materials recorded in Example 1. After the temperature in the first temperature-controllable heating furnace is raised to the temperature required for the polonium evaporation simulation, the 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 circle 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, 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 requirements 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 a test gas of a set flow rate and a 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), and 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 connected to 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 filling 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 of polonium capture material 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 of polonium capture material according to claim 1, characterized in that: It also includes a tail gas absorption bottle assembly (40), which contains a soluble acid solution, and 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 of polonium capture material according to claim 3, characterized in that: It also includes a vacuum pump (50), which is connected in series to the gas outlet end of the suction bottle assembly.

5. The gas-solid reaction kinetic model verification device of polonium capture material according to claim 4, characterized in that: The gas outlet end of the vacuum pump (50) is 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 gas-solid reaction kinetic model verification device 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 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); The radiation equivalent of the gas captured by the capture material packed bed (31) is used as the outlet concentration of the polonium capture material to conduct a 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 also includes 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: It also includes the steps of: calculating the penetration adsorption capacity and saturation adsorption capacity of the capture material according to the test data; The calculation model of the penetration 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: 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 outlet heavy element vapor concentration after t minutes, in mg / m 3 ; W is the adsorbent loading, unit: g; q E is the saturated adsorption capacity, in mg / g; T E Depletion time, in mL / min.

9. The method for verifying the gas-solid reaction kinetic model of polonium capture material according to claim 6, characterized in that: The method also includes the steps of fitting the test 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 material 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.

Images