Automatic separation method and device for fission molybdenum-99

Abstract

The embodiment of the invention provides an automatic fission molybdenum-99 separation method and device which are applied to a fission molybdenum-99 separation device, and the fission molybdenum-99 separation device comprises a separation system, a liquid supply system and a control system. The separation system comprises a first separation device, a second separation device and a third separation device which are sequentially connected. The liquid supply system is connected with the separation system, and the control system is used for controlling the liquid supply system to convey the stored media to the separation system according to a set sequence. The automatic separation method of the fission molybdenum-99 comprises the steps that the first separation device is filled with aluminum oxide, the second separation device is filled with anion exchange resin, and the third separation device is filled with activated carbon. The first separation device is used for carrying out primary separation on the target dissolving liquid to obtain primary purified liquid; the separation system comprising the first separation device, the second separation device and the third separation device is arranged, the liquid supply system and the control system are arranged, and the control system controls medium injection of the liquid supply system, so that the whole separation process can be completely automatic.

Description

Technical Field

[0001] The present application relates to the technical field of radionuclide separation, and in particular to an automatic separation method and device for fission molybdenum-99. Background Art

[0002] Molybdenum-99 is an important medical radioactive isotope. Molybdenum-99 / technetium-99m generators made from molybdenum-99 are widely used in the clinical field of nuclear medicine. Molybdenum-99 is often extracted from the fission products of uranium-235. After obtaining the molybdenum-99 solution, it is prepared into a fission molybdenum-99 / technetium-99m generator for users. In the related technology, during the separation and purification of molybdenum-99, due to the very high dose in the operating area, manual operation is likely to cause radiation damage to the operator. At the same time, since the separation process is lengthy and time-consuming, it requires long-term monitoring and operation by dedicated personnel, which consumes manpower. Summary of the invention

[0003] The present application provides an automatic separation method and device for fission molybdenum-99, which is used to solve the problem of radiation damage to operators and labor consumption during the separation and purification of molybdenum-99. The specific method is as follows:

[0004] The first aspect of the present application provides an automatic separation method of fission molybdenum-99, which is applied to a fission molybdenum-99 separation device, wherein the fission molybdenum-99 separation device comprises a separation system, a liquid supply system and a control system; the separation system comprises a first separation device, a second separation device and a third separation device connected in sequence; the liquid supply system is connected to the separation system; the control system is used to control the liquid supply system to transport the stored medium to the separation system in a set sequence; the automatic separation method of fission molybdenum-99 comprises:

[0005] Filling the first separation device with alumina, filling the second separation device with the anion exchange resin, and filling the third separation device with activated carbon;

[0006] The control system controls the target solution to be separated in the liquid supply system to be added to the first separation device, and the first separation device performs primary separation on the target solution to obtain a primary purified solution;

[0007] The control system controls the first-level purified liquid to be separated in the liquid supply system to be added to the second separation device, and the second separation device performs secondary separation on the first-level purified liquid to obtain a secondary purified liquid;

[0008] The control system controls the secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the third separation device performs three-stage separation on the secondary purified liquid to obtain a tertiary purified liquid.

[0009] In one embodiment, the control system controls the target solution to be separated in the liquid supply system to be added to the first separation device, and the first separation device performs a primary separation on the target solution to obtain a primary purified solution, which includes:

[0010] The control system controls the 0.1mol / L-1.0mol / L nitric acid solution in the liquid supply system to elute the aluminum oxide, so as to pretreat the aluminum oxide;

[0011] The control system controls the target solution to be separated in the liquid supply system to be added into the first separation device, and the target solution is adsorbed by the alumina;

[0012] The control system controls the first eluent in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution;

[0013] The control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to desorb from the alumina to obtain the primary purified liquid.

[0014] In one embodiment, the control system controls the first eluent in the liquid supply system to elute the aluminum oxide, and removing impurities in the target solution includes:

[0015] The control system controls the 0.1mol / L-1.0mol / L nitric acid solution in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution;

[0016] The control system controls the deionized water in the liquid supply system to elute the aluminum oxide until the pH value of the deionized water flowing out of the eluent is neutral;

[0017] The control system controls the physiological saline in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution;

[0018] The control system controls the 0.01 mol / L-0.1 mol / L ammonia solution in the liquid supply system to elute the aluminum oxide to change its surface environment.

[0019] In one embodiment, the control system controls the primary purified liquid to be separated in the liquid supply system to be added to the second separation device, and the second separation device performs secondary separation on the primary purified liquid to obtain the secondary purified liquid, which includes:

[0020] The control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to elute the anion exchange resin, so as to pretreat the anion exchange resin;

[0021] The control system controls the primary purified liquid to be separated in the liquid supply system to be added into the second separation device, and the anion exchange resin is used to adsorb the primary purified liquid;

[0022] The control system controls the second eluent in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid;

[0023] The control system controls the 1.0 mol / L-2.0 mol / L ammonium carbonate solution in the liquid supply system to desorb from the anion exchange resin to obtain the secondary purified liquid.

[0024] In one embodiment, the control system controls the second eluent in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid, including:

[0025] The control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid;

[0026] The control system controls the deionized water in the liquid supply system to elute the anion exchange resin until the pH value of the deionized water flowing out of the eluent is neutral;

[0027] The control system controls the 0.01mol / L-0.015mol / L malonic acid solution in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid;

[0028] The control system controls the deionized water in the liquid supply system to elute the anion exchange resin until the pH value of the deionized water flowing out of the eluent is neutral.

[0029] In one embodiment, the control system controls the secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the third separation device performs three-stage separation on the secondary purified liquid to obtain the three-stage purified liquid, which includes:

[0030] The control system controls the pH value in the liquid supply system to be 2.0-2.5, and the nitric acid solution is used to elute the activated carbon for pre-treating the activated carbon;

[0031] The control system controls the concentrated nitric acid solution in the liquid supply system to adjust the pH value of the secondary purification liquid to 2.0-2.5;

[0032] The control system controls the acid-adjusted secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the activated carbon is used to adsorb the secondary purified liquid;

[0033] The control system controls the third eluent in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid;

[0034] The control system controls the 0.2 mol / L-1.0 mol / L sodium hydroxide solution in the liquid supply system to desorb from the activated carbon to obtain the tertiary purified liquid.

[0035] In one embodiment, the control system controls the third eluent in the liquid supply system to elute the activated carbon, and removing impurities in the secondary purification liquid includes:

[0036] The control system controls the pH value of the nitric acid solution in the liquid supply system to be 2.0-2.5 to elute the activated carbon to remove impurities in the secondary purification liquid;

[0037] The control system controls the 1.5%-3.0% bromine aqueous solution in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid.

[0038] In one embodiment, after the first separation device is filled with alumina, the second separation device is filled with anion exchange resin, and the third separation device is filled with activated carbon, the method further comprises:

[0039] The control system controls the deionized water in the liquid supply system to wash the fine particles in the aluminum oxide;

[0040] The control system controls the deionized water in the liquid supply system to wash the fine particles on the anion exchange resin;

[0041] The control system controls the deionized water in the liquid supply system to rinse the fine particles in the activated carbon.

[0042] The second aspect of the present application provides an automatic separation device for fissionable molybdenum-99, which is used to separate and purify molybdenum-99 from a target solution containing molybdenum-99, comprising:

[0043] frame;

[0044] A separation system, the separation system is arranged on the frame, the separation system comprises a first separation device, a second separation device and a third separation device connected in sequence; the first separation device is used to perform a primary separation on the target solution to obtain a primary purified solution; the second separation device is used to perform a secondary separation on the primary purified solution to obtain a secondary purified solution; the third separation device is used to perform a tertiary separation on the secondary purified solution to obtain a tertiary purified solution;

[0045] A liquid supply system, the liquid supply system is arranged on the frame, the liquid supply system is connected to the separation system, the liquid supply system includes a liquid storage device, and the liquid storage device can be used to store at least the target solution, the eluent, the desorption liquid, the primary purification liquid, the secondary purification liquid and the tertiary purification liquid;

[0046] A control system, wherein the control system automatically controls the medium stored in the liquid supply system to be injected into the separation system according to a set sequence.

[0047] In one embodiment, the liquid supply system includes a pipeline assembly, which includes a first pipeline assembly, a second pipeline assembly, a third pipeline assembly and a fourth pipeline assembly; the liquid injection ports of the first separation device, the second separation device and the third separation device are connected to the liquid storage device through the first pipeline assembly; the liquid outlet of the first separation device is connected to the liquid injection port of the second separation device through the second pipeline assembly; the liquid outlet of the second separation device is connected to the liquid injection port of the third separation device through the third pipeline assembly; and the fourth pipeline assembly is connected to the liquid outlet of the third separation device.

[0048] In one embodiment, the control system includes a first reversing valve, the first reversing valve is arranged in the first pipeline assembly, and the first reversing valve is used to selectively open or close the first pipeline assembly; and / or,

[0049] The control system comprises a second reversing valve, the second reversing valve is arranged on the second pipeline assembly, and the second reversing valve is used to selectively open or close the second pipeline assembly; and / or,

[0050] The control system comprises a third reversing valve, the third reversing valve is arranged on the third pipeline assembly, and the third reversing valve is used to selectively open or close the third pipeline assembly; and / or,

[0051] The control system includes a fourth reversing valve, which is disposed on the fourth pipeline assembly and is used to selectively open or close the fourth pipeline assembly.

[0052] In one embodiment, the automatic separation device of fission molybdenum-99 includes a detection system, and the detection system includes an acid-base detector and a radioactivity detector, and the radioactivity detector is used to detect radioactivity data in the first separation device, the second separation device and the third separation device.

[0053] The automatic separation method of fission molybdenum-99 provided in the present application realizes the three-stage separation and purification of molybdenum-99 by setting a separation system including a first separation device, a second separation device and a third separation device, which is beneficial to improving the effect of separation and purification of molybdenum-99. By setting a liquid supply system and a control system, the control system controls the medium injection of the liquid supply system, and the entire separation process can be fully automated. The separation process does not require human operation, which is beneficial to reducing the impact of radiation on the operator and solving the problem of requiring personnel to monitor the operation during the long separation process. At the same time, automated control can also accurately control various parameters in the separation process, which is beneficial to improving the separation and purification effect. BRIEF DESCRIPTION OF THE DRAWINGS

[0054] Figure 1 A schematic diagram of the structure of an automatic separation device for fissionable molybdenum-99 provided in one embodiment of the present application;

[0055] Figure 2 A flow chart of an automatic separation method of fissionable molybdenum-99 provided in one embodiment of the present application.

[0056] Description of Reference Numerals

[0057] 10. Separation device; 1. Separation system; 11. First separation device; 12. Second separation device; 13. Third separation device; 2. Liquid supply system; 21. Liquid storage device; 211. Target solution bottle; 212. Desorption liquid bottle; 213. First eluent bottle; 214. Second eluent bottle; 215. Third eluent bottle; 216. Waste liquid bottle; 217. Primary purification liquid bottle; 218. Secondary purification liquid bottle; 219. Third purification liquid bottle; 22. Pipeline assembly; 221. First pipeline component; 222. Second pipeline component; 223. Third pipeline component; 224. Fourth pipeline component; 3. Control system; 31. First reversing valve; 32. Second reversing valve; 33. Third reversing valve; 34. Fourth reversing valve; 35. Infusion pump; 4. Detection system; 41. Radioactive detector. DETAILED DESCRIPTION

[0058] It should be noted that, in the absence of conflict, the embodiments and technical features in the embodiments of the present application can be combined with each other, and the detailed description in the specific implementation method should be understood as an explanation of the purpose of the present application and should not be regarded as an improper limitation on the present application.

[0059] Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by technicians in the technical field to which this application belongs; the terms used herein are only for the purpose of describing specific embodiments and are not intended to limit this application; the terms "including" and "having" and any variations thereof in this application are intended to cover non-exclusive inclusions.

[0060] In the description of the embodiments of the present application, the technical terms "first", "second", "third", etc. are only used to distinguish different objects, and cannot be understood as indicating or implying relative importance or implicitly indicating the number, specific order or primary and secondary relationship of the indicated technical features. In the description of the embodiments of the present application, the meaning of "multiple" is more than two, unless otherwise clearly and specifically defined.

[0061] Reference to "embodiments" herein means that a particular feature, structure, or characteristic described in conjunction with the embodiments may be included in at least one embodiment of the present application. The appearance of the phrase in various locations in the specification does not necessarily refer to the same embodiment, nor is it an independent or alternative embodiment that is mutually exclusive with other embodiments. It is explicitly and implicitly understood by those skilled in the art that the embodiments described herein may be combined with other embodiments.

[0062] In the description of the embodiments of the present application, the term "and / or" is only a description of the association relationship of associated objects, indicating that three relationships may exist. For example, A and / or B can represent: A exists alone, A and B exist at the same time, and B exists alone. In addition, the character " / " in this article generally indicates that the associated objects before and after are in an "or" relationship.

[0063] In the description of the embodiments of the present application, the orientation or position relationship indicated by technical terms such as "length", "width", "thickness", "up", "down", "front", "back", "left", "right", "vertical", "horizontal", "top", "bottom", "inside", "outside", "circumferential", "height direction", "first direction", and "second direction" are based on the orientation or position relationship shown in the accompanying drawings. They are only for the convenience of describing the embodiments of the present application and simplifying the description, and do not indicate or imply that the referred device or element must have a specific orientation, be constructed, operated or used in a specific orientation. Therefore, they should not be understood as limitations on the embodiments of the present application.

[0064] In the description of the embodiments of the present application, unless otherwise clearly specified and limited, technical terms such as "installed", "connected", "connected", "fixed" and the like 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, and it can be a connection between two elements or an interaction relationship between two elements. For those of ordinary skill in the art, the specific meanings of the above terms in the embodiments of the present application can be understood according to the specific circumstances.

[0065] In the description of the embodiments of the present application, unless otherwise clearly specified and limited, the technical term "contact" should be understood in a broad sense, and may be direct contact or contact through an intermediate medium layer. It may be contact with essentially no interaction force between the two contacting parties, or it may be contact with interaction force between the two contacting parties.

[0066] The present application provides an automatic separation device 10 for fissionable molybdenum-99, which is used to separate and purify molybdenum-99 from a target solution containing molybdenum-99. Figure 1 , the separation device 10 includes a frame, a separation system 1, a liquid supply system 2 and a control system 3. The separation system 1 is arranged on the frame. The separation system 1 includes a first separation device 11, a second separation device 12 and a third separation device 13 connected in sequence. The first separation device 11 is used to perform a primary separation on the target solution to obtain a primary purified liquid. The second separation device 12 is used to perform a secondary separation on the primary purified liquid to obtain a secondary purified liquid. The third separation device 13 is used to perform a tertiary separation on the secondary purified liquid to obtain a tertiary purified liquid. The liquid supply system 2 is arranged on the frame, and the liquid supply system 2 is connected to the separation system 1. The liquid supply system 2 includes a liquid storage device 21, and the liquid storage device 21 can at least be used to store a target solution, a washing liquid, a desorption liquid, a primary purified liquid, a secondary purified liquid and a tertiary purified liquid. The control system 3 automatically controls the medium stored in the liquid supply system 2 to be injected into the separation system 1 according to a set order.

[0067] The frame is the supporting structure of the separation device 10. Other structures in the separation device 10, such as the liquid supply system 2 and the control system 3, are fixedly installed through the frame, so that the separation device 10 forms a whole, which is convenient for the arrangement and transportation of the separation device 10. At the same time, the frame can also provide protection for other structures in the separation device 10, preventing external objects from contacting other structures in the separation device 10 and causing damage to the separation device 10.

[0068] The specific structure of the frame is not limited here, for example, it can be a frame structure made of metal profiles or steel plates welded together, with high stability and load-bearing capacity, which can be suitable for large or medium-sized separation devices 10. It can also be a closed or semi-closed box structure composed of plates, so that the separation device 10 can be provided with additional protection and isolation, reducing the interference of external dust, water and other media on the separation device 10.

[0069] In some embodiments, the rack is a mobile or portable structure. For example, wheels or handles may be provided at the bottom of the rack to facilitate movement and transportation, and is suitable for occasions where the position needs to be changed frequently.

[0070] In some embodiments, the frame adopts a modular design, and a universal quick-release mounting structure is provided on the frame, and the quick-release mounting structure can adjust the position relative to the frame, and the liquid supply system 2 and the control system 3 are installed on the frame through the quick-release mounting structure, so that the installation, adjustment and upgrading of the separation device 10 can be facilitated. The modular design is also conducive to the maintenance of the separation device 10.

[0071] The separation system 1 is a structure that performs separation in the separation device 10. The separation system 1 includes a first separation device 11, a second separation device 12 and a third separation device 13 that are connected to each other, and is responsible for separating and purifying molybdenum-99 in the target solution step by step.

[0072] The first separation device 11, the second separation device 12 and the third separation device 13 provide reaction sites for separating and purifying molybdenum-99. The raw materials required for separating molybdenum-99, such as a target solution, an eluent, a desorption solution, etc., react in these reaction sites to separate and purify molybdenum-99 from the target solution. Usually, the first separation device 11, the second separation device 12 and the third separation device 13 each include a chromatographic column, each chromatographic column is filled with a stationary phase required for each level of separation, and the stationary phase adsorbs molybdenum-99 from the target solution, the eluent washes the impurities on the stationary phase, and the desorption solution desorbs molybdenum-99 from the stationary phase, thereby achieving separation and purification of molybdenum-99.

[0073] The manufacturing material of each chromatographic column needs to be made of a material with good radiation resistance to increase the service life of the chromatographic column. The specific material is not limited here, for example, it can be stainless steel, polytetrafluoroethylene, quartz glass, ceramics, etc.

[0074] It should be noted that the first separation device 11 is responsible for preliminary separation of the original target solution to obtain a primary purified solution. Since there are many impurities in the original target solution and the content of molybdenum-99 in the target solution is low, in order to improve the separation and purification efficiency, the volume of the chromatographic column of the first separation device 11 is generally larger than that of the chromatographic columns of the second separation device 12 and the third separation device 13, and the efficiency of separating and purifying molybdenum-99 is achieved by increasing the amount of the target solution separated and purified per unit time.

[0075] Exemplarily, since the radiation intensity of the target solution is relatively high, the chromatographic column of the first separation device 11 is made of quartz glass with good radiation resistance. The outer diameter of the chromatographic column of the first separation device 11 is 55 mm, and the effective column height of the chromatographic column is 350 mm. The larger volume can provide a larger reaction site for the target solution to improve the separation and purification efficiency.

[0076] Since the content of molybdenum-99 in the primary purified liquid and the secondary purified liquid obtained by the second separation device 12 and the third separation device 13 after the separation in the previous stage is increased, the reaction efficiency in the chromatographic column is also correspondingly improved. Therefore, the volume of the chromatographic column of the second separation device 12 and the third separation device 13 can be smaller than the chromatographic column of the first separation device 11.

[0077] For example, since the primary purified liquid obtained after the primary purification still has a certain radiation, the chromatographic column of the second separation device 12 is made of quartz glass with good radiation resistance, the outer diameter of the chromatographic column of the second separation device 12 is 25 mm, and the effective column height of the chromatographic column of the second separation device 12 is 200 mm.

[0078] Illustratively, since the radiation intensity of the secondary purified liquid obtained after secondary purification is reduced, the chromatographic column of the third separation device 13 is made of glass, the outer diameter of the chromatographic column of the third separation device 13 is 15 mm, and the effective column height of the chromatographic column of the third separation device 13 is 200 mm.

[0079] The effective column height here refers to the height of the chromatographic column that can be filled with the stationary phase. The height of the stationary phase determines the separation and purification effect of the chromatographic column.

[0080] The liquid supply system 2 is connected to the separation system 1, and is responsible for providing the separation system 1 with various liquid media required in the separation and purification process, such as target solution, eluent, desorption liquid, primary purification liquid, secondary purification liquid and tertiary purification liquid, etc. The liquid storage device 21 is a structure for storing the above-mentioned solution media in the liquid supply system 2, and the specific structure is not limited here. Exemplarily, the liquid storage device 21 includes solution bottles for storing various solution media, including a target solution bottle 211, a desorption liquid bottle 212, a first eluent bottle 213, a second eluent bottle 214 and a third eluent bottle 215, etc. The liquid storage device 21 includes a liquid storage bracket, and the solution bottles are placed on the liquid storage bracket.

[0081] In some embodiments, the liquid storage device 21 further includes a waste liquid bottle 216 for storing various acidic solutions, alkaline solutions, water solutions, etc., which flow out after the eluent is eluted during the separation and purification process, so as to facilitate the collection and subsequent treatment of various acidic solutions, alkaline solutions, water solutions, etc. In other embodiments, a waste liquid bottle 216 is provided for each of the first separation device 11, the second separation device 12, and the third separation device 13, so that solutions with different radioactive strengths can be distinguished, which is beneficial to the subsequent treatment and utilization of the solutions.

[0082] In some embodiments, the waste liquid bottle 216 includes a high-level radioactive waste liquid storage area and a medium-level radioactive waste liquid storage area. Among them, the various waste liquids flowing out of the first separation device 11 are stored in the high-level radioactive waste liquid storage area due to their high radioactivity; the various waste liquids flowing out of the second separation device 12 and the third separation device 13 are stored in the medium-level radioactive waste liquid storage area after their radioactivity is reduced during the separation and purification process. In this way, by classifying and storing high-level radioactive waste liquid and medium-level radioactive waste liquid, waste liquids with different radioactivity are classified and processed, which is conducive to reducing the difficulty and cost of waste liquid processing.

[0083] Target solution refers to a solution containing molybdenum-99 obtained from low-enriched uranium or high-enriched uranium targets after irradiation in a reactor.

[0084] The eluent refers to the solution used to elute the stationary phase. The eluent should not react with the stationary phase and the molybdenum-99 products on the stationary phase. The specific type of the eluent is determined according to the stationary phase and the type of impurities to be washed.

[0085] The desorption liquid is a solution that can adsorb and separate molybdenum-99 from the stationary phase, and the molybdenum-99 flows out of the stationary phase along with the desorption liquid. The specific type of the eluent is determined by the type of the stationary phase.

[0086] The control system 3 is a device for controlling the separation and purification in the separation device 10. The control system 3 can be used to control the injection sequence and amount of the medium of the liquid supply system 2 to improve the accuracy of the separation process.

[0087] In some embodiments, the control system is a fully integrated automated process control system, which includes operating software, computers, central controllers, I / O modules and other types of control components.

[0088] The operator can use the operating software on the computer to perform various operations on the device, mainly including the start and stop control of the infusion pump 35, the speed control of the infusion pump 35, and the switch control of various reversing valves.

[0089] The interface of the operating software of the control system 3 can also display in real time the main parameters of the device when it is working, such as flow rate (converted from the rotation speed of the infusion pump 35), target liquid activity (measured by the sensor of the detection system 4), liquid filling status (filling of each solution bottle in the liquid storage device 21), and other necessary data.

[0090] The operating software can be pre-programmed to control the liquid supply system 2 and various reversing valves (such as the first reversing valve 31, the second reversing valve 32, the third reversing valve 33 and the fourth reversing valve 34) to comply with the separation and purification sequence. It can add solutions required for various separation processes (such as controlling the solutions in the first eluent bottle 213, the second eluent bottle 214 and the third eluent bottle 215 to be added in a pre-programmed sequence), control the collection and injection of various intermediate products (such as primary purification liquid, secondary purification liquid and tertiary purification liquid), and control the collection of waste liquid in separation and purification.

[0091] In addition, the operating software can also control various reversing valves according to the feedback data of the detection system 4 to adjust various parameters in the separation and purification to meet the requirements of the separation and purification.

[0092] The equipment operating parameters (such as equipment switch / motor speed / valve switch, etc.) are input by the operator through the software and enter the central controller (PLC). The control program in the PLC is started, and after calculation, the control parameters are output to the corresponding data processing module (I / O module, servo controller, etc.), and finally cause the action control of the motor / valve, etc. through the control hardware.

[0093] In some embodiments, the control system 3 can adjust and maintain the temperature of the chromatographic column so that the chromatographic column operates at a specific temperature to obtain the best separation effect.

[0094] In some embodiments, the control system 3 can monitor and adjust the pressure and flow rate of the mobile phase through the chromatography column.

[0095] The type of control system 3 is not limited here, and can be a manual control system 3, where the operator manually sets and adjusts all parameters. It can be a semi-automatic control system 3, where part of the process is automated, such as automatic injection, but other parameters need to be manually adjusted. It can also be a fully automatic control system 3, where the entire separation process is fully automated, including injection, elution, detection and data processing.

[0096] The fission molybdenum-99 separation device 10 provided in the present application realizes the three-stage separation and purification of molybdenum-99 by setting a separation system 1 including a first separation device 11, a second separation device 12 and a third separation device 13, which is beneficial to improving the effect of separation and purification of molybdenum-99. By setting a liquid supply system 2 and a control system 3, the control system 3 controls the medium injection of the liquid supply system 2, and the entire separation process can be fully automated. The separation process does not require human operation, which is beneficial to reducing the impact of radiation on the operator and solving the problem of requiring personnel to monitor the operation during the long separation process. At the same time, automated control can also accurately control various parameters in the separation process, which is beneficial to improving the separation and purification effect.

[0097] In some embodiments, see Figure 1 The liquid supply system 2 includes a pipeline assembly 22, and the pipeline assembly 22 includes a first pipeline component 221, a second pipeline component 222, a third pipeline component 223 and a fourth pipeline component 224. The liquid injection ports of the first separation device 11, the second separation device 12 and the third separation device 13 are connected to the liquid storage device 21 through the first pipeline component 221. The liquid outlet of the first separation device 11 is connected to the liquid injection port of the second separation device 12 through the second pipeline component 222. The liquid outlet of the second separation device 12 is connected to the liquid injection port of the third separation device 13 through the third pipeline component 223. The fourth pipeline component 224 is connected to the liquid outlet of the third separation device 13.

[0098] The first pipeline assembly 221 is a device responsible for transporting the medium in the liquid storage device 21 to the injection ports of the first separation device 11, the second separation device 12 and the third separation device 13. The medium transported by the first pipeline assembly 221 includes but is not limited to target solution, eluent and desorption solution, etc.

[0099] The second pipeline assembly 222 is a device that connects the liquid outlet of the first separation device 11 and the liquid injection port of the second separation device 12, and is used to transport the primary purified liquid processed by the first separation device 11 to the next separation stage.

[0100] In some embodiments, the second pipeline assembly 222 is further provided with a primary purified liquid bottle 217 for temporarily storing the primary purified liquid obtained by desorption of the desorption liquid in preparation for the next separation stage.

[0101] In some embodiments, the second pipeline assembly 222 is also provided with a waste liquid discharge pipeline connected to the liquid outlet of the first separation device 11, which is used to discharge various acid solutions, alkali solutions, water and the like discharged after elution with the eluent.

[0102] The third pipeline assembly 223 is a device for connecting the liquid outlet of the second separation device 12 and the liquid injection port of the third separation device 13, and is used to transport the secondary purified liquid processed by the second separation device 12 to the next separation stage.

[0103] In some embodiments, the third pipeline assembly 223 is further provided with a secondary purification liquid bottle 218 for temporarily storing the secondary purification liquid obtained by desorption of the desorption liquid in preparation for the next separation stage.

[0104] In some embodiments, the third pipeline assembly 223 is also provided with a waste liquid discharge pipeline connected to the liquid outlet of the second separation device 12, which is used to discharge various acid solutions, alkali solutions, water and the like discharged after eluting with the eluent.

[0105] The fourth pipeline assembly 224 is a liquid outlet device connected to the third separation device 13, and is used to collect the tertiary purified liquid obtained by the final separation and transport it to subsequent processing or storage links.

[0106] In some embodiments, the fourth pipeline assembly 224 is further provided with a tertiary purified liquid bottle 219 for temporarily storing the tertiary purified liquid obtained by desorption of the desorption liquid in preparation for the next stage.

[0107] In some embodiments, the fourth pipeline assembly 224 is also provided with a waste liquid discharge pipeline connected to the liquid outlet of the third separation device 13, for discharging various acid solutions, alkali solutions, water and the like discharged after eluting with the eluent.

[0108] In some embodiments, an infusion pump 35 is also provided in the first pipeline assembly 221 and / or the second pipeline assembly 222 and / or the third pipeline assembly 223 and / or the fourth pipeline assembly 224. The infusion pump 35 is connected to the control system 3 and is used to control the flow of the medium in the pipeline assembly 22 to achieve the functions of adding and draining liquid.

[0109] The specific structure of the infusion pump 35 is not limited here, for example, it can be a peristaltic pump, so that the medium is squeezed into the pipeline assembly 22 through a dedicated hose, avoiding contact between the pump core and the liquid, and improving the service life of the infusion pump 35. Of course, it can also be an air pump, which drives the flow of the medium through the flow of air.

[0110] The fixing method of the infusion pump 35 is not limited here. For example, the infusion pump 35 can be fixed to the frame by pressing or screw locking.

[0111] The special hose here is made of radiation-resistant, acid-resistant and alkali-resistant materials, such as fluororubber, high polymer materials and the like.

[0112] The type of pipeline of the pipeline assembly 22 is not limited here. For example, a sterilized disposable tube can be used to reduce the amount of impurities entering the system.

[0113] The pipelines of the pipeline assembly 22 can be made of transparent Teflon material, which has good radiation resistance and acid and alkali resistance and can also facilitate external observation of the liquid flow.

[0114] The pipeline interface can adopt Luer series connector to achieve quick sealing. The pipeline interface can be made of polyetheretherketone, which has good mechanical strength and sealing performance, and is resistant to radiation, acid and alkali.

[0115] By setting the first pipeline assembly 221, the second pipeline assembly 222, the third pipeline assembly 223 and the fourth pipeline assembly 224, the liquid storage device 21 is connected, the first separation device 11, the second separation device 12 and the third separation device 13 are connected, so that the flow of the solution required for separation in the separation device 10 is achieved. By controlling the inflow and outflow of the solution in the pipeline system, the separation process can be achieved, and the principle is simple.

[0116] In some embodiments, see Figure 1 The control system 3 includes a first reversing valve 31 , which is disposed on the first pipeline assembly 221 , and is used to selectively open or close the first pipeline assembly 221 .

[0117] The first reversing valve 31 is installed on the first pipeline assembly 221 and is responsible for controlling the flow of fluid from the liquid storage device 21 to the first separation device 11. It can be selectively opened or closed by the control system 3 to allow or prevent the fluid from flowing to the first separation device 11.

[0118] More specifically, the first reversing valve 31 connects the target solution bottle 211, the desorption solution bottle 212, the first eluent bottle 213, the second eluent bottle 214 and the third eluent bottle 215 to the first pipeline. The first reversing valve 31 can control each solution to flow to the first separation device 11, the second separation device 12 and the third separation device 13 by controlling each pipeline connected to different solution bottles.

[0119] In some embodiments, two first reversing valves 31 may be provided to enable a specific solution to flow to a specific separation device 10 during a specific separation process, thereby promoting the separation process.

[0120] In some embodiments, see Figure 1 The control system 3 includes a second reversing valve 32 , which is disposed in the second pipeline assembly 222 , and is used to selectively open or close the second pipeline assembly 222 .

[0121] The second reversing valve 32 is installed on the second pipeline assembly 222 to control the fluid flow between the liquid outlet of the first separation device 11 and the liquid injection port of the second separation device 12. By opening or closing this valve, it is possible to control whether the fluid enters the second separation device 12 for further separation.

[0122] More specifically, the second reversing valve 32 controls the various acid solutions, alkali solutions, water solutions and the like discharged after elution of the elution liquid to flow into the waste liquid bottle 216 , and controls the primary purified liquid obtained after desorption to flow into the primary purified liquid bottle 217 .

[0123] In some embodiments, see Figure 1 The control system 3 includes a third reversing valve 33 , which is disposed in the third pipeline assembly 223 , and is used to selectively open or close the third pipeline assembly 223 .

[0124] The third reversing valve 33 is installed on the third pipeline assembly 223 to control the fluid flow between the liquid outlet of the second separation device 12 and the liquid injection port of the third separation device 13. By opening or closing this valve, it is possible to control whether the fluid enters the third separation device 13 for further separation.

[0125] More specifically, the third reversing valve 33 controls the various acid solutions, alkali solutions, water solutions and the like discharged after elution of the elution liquid to the waste liquid bottle 216 , and controls the secondary purification liquid obtained after desorption to the secondary purification liquid bottle 218 .

[0126] In some embodiments, see Figure 1 The control system 3 includes a fourth reversing valve 34 , which is disposed on the fourth pipeline assembly 224 , and is used to selectively open or close the fourth pipeline assembly 224 .

[0127] The fourth reversing valve 34 is installed on the fourth pipeline assembly 224 to control the fluid flow of the liquid outlet of the third separation device 13. It can be used to close the final output of the fluid, or guide it to a desired subsequent processing or storage location.

[0128] More specifically, the fourth reversing valve 34 controls the various acid solutions, alkali solutions, water solutions and the like discharged after elution of the elution liquid to the waste liquid bottle 216 , and controls the tertiary purified liquid obtained after desorption to the tertiary purified liquid bottle 219 .

[0129] The types of the reversing valves are not limited here, for example, they may be electromagnetic reversing valves, hydraulic reversing valves, electro-hydraulic reversing valves, etc. It should be noted that these reversing valves and the control system 3 are controlled by the control system 3 .

[0130] It is understandable that the control system 3 automatically controls the medium stored in the liquid supply system 2 to be injected into the separation system 1 in a set order, that is, controls the opening and closing of the above-mentioned reversing valves to realize the separation and purification process. The specific control method is not limited here, and it only needs to comply with the separation and purification process, control the solution required for separation and purification to be injected into the set amount at the set time, and meet the reaction requirements.

[0131] By setting the first reversing valve 31, it is possible to realize that various solutions in the liquid storage device 21 flow to the specific separation device 10 in a specific separation process, thereby controlling the progress of the separation process, and the control principle is simple. By setting the second reversing valve 32, the third reversing valve 33 and the fourth reversing valve 34, the opening and circulation of the liquid storage ports and the liquid injection ports of the first separation device 11, the second separation device 12 and the third separation device 13 are controlled to realize the injection and discharge of the process solution, which is conducive to improving the continuity of the separation and purification process. The entire separation process can realize the automatic control of the separation and purification process by controlling the coordinated opening and closing of each reversing valve.

[0132] In some embodiments, see Figure 1 The automatic separation device 10 of fission molybdenum-99 includes a detection system 4, which includes an acid-base detector and a radioactive detector 41. The radioactive detector 41 is used to detect radioactive data in the first separation device 11, the second separation device 12 and the third separation device 13.

[0133] The acid-base detector is an instrument used to detect the acidity and alkalinity of a substance. In the automatic separation device 10 of fission molybdenum-99, the acid-base detector plays an important role. It can monitor the acidity and alkalinity of each part of the separation device 10 in real time and provide key parameter information for the separation process.

[0134] pH has an important influence on the separation and chemical reaction of substances. In the separation process of fission molybdenum-99, different pH conditions may affect the separation effect of molybdenum-99 and other impurities and the progress of chemical reactions. Through the monitoring of the acid-base detector, the pH in the separation process can be adjusted in time to achieve the best separation effect.

[0135] The type of acid-base detector is not limited here. For example, the acid-base detector is a long-arm pH meter with a long measuring probe or electrode arm, which enables it to penetrate into some deeper containers, pipes or difficult-to-reach locations to measure the pH value. In this way, the operator can remotely measure the pH of each part of the automatic separation device 10 of fission molybdenum-99, reducing the impact of radiation on the operator.

[0136] Radioactive detector 41 refers to a material or device that can indicate, record and measure nuclear radiation. It is an indispensable tool and means in nuclear physics, particle physics research and radiation application.

[0137] Here, the radioactive detector 41 includes a lead chamber and a sodium iodide crystal gamma detector. When each level of purified liquid passes through, these pipelines are placed in the lead chamber to detect the radioactive peak time of the gamma energy and measure the radioactive activity of each level of purified liquid.

[0138] In some embodiments, the sensor assembly includes an electrochemical sensor disposed in each chromatographic column for detecting changes in chemical reactions under radiation and feeding back to a central controller, which determines the progress of the reaction and controls each reversing valve to cooperate and perform corresponding steps.

[0139] In some embodiments, the sensor assembly includes a time sensor for calculating the reaction time after the solution is injected to assist in determining the progress of the reaction.

[0140] In some embodiments, the sensor assembly includes a pH sensor disposed at the liquid outlet of each chromatographic column, which is used to detect the pH value of the discharged solution to assist in determining the progress of the reaction.

[0141] It should be noted that the various sensor elements in the detection system 4 need to be in direct contact with radioactive substances and therefore must be radiation-resistant, have a long life, and a wide range to meet the high radiation environment requirements of the separation device 10 .

[0142] The detection system 4 can be connected to the control system 3. The detection system 4 transmits the detection data to the central processing unit of the control system 3. After the central processing unit processes the data, it brings it into the pre-programmed program for judgment to output various corresponding commands and control the operation of other execution components of the control system 3 to ensure the orderly progress of the separation process.

[0143] By setting up a detection system 4, it is used to detect and monitor the radiation data in the first separation device 11, the second separation device 12 and the third separation device 13, so as to realize real-time monitoring of the separation and purification process. In addition, the detection system 4 can be connected to the control system 3 to transmit the detection data to the central controller to realize automatic control of the separation and purification process.

[0144] The present application provides an automatic separation method of fission molybdenum-99, which is applied to a fission molybdenum-99 separation device 10. Figure 1 The fission molybdenum-99 separation device 10 includes a separation system 1, a liquid supply system 2 and a control system 3. The separation system 1 includes a first separation device 11, a second separation device 12 and a third separation device 13 connected in sequence. The liquid supply system 2 is connected to the separation system 1, and the control system 3 is used to control the liquid supply system 2 to transport the stored medium to the separation system 1 according to a set sequence.

[0145] like Figure 2 As shown, the automatic separation method of fissionable molybdenum-99 includes the following steps S110 to S140:

[0146] Step S110, filling alumina into the first separation device, filling anion exchange resin into the second separation device, and filling activated carbon into the third separation device.

[0147] Alumina, anion exchange resin and activated carbon are all stationary phases for adsorbing molybdenum-99, and have good adsorption effect on molybdenum-99. It should be noted that alumina is an inorganic ion exchanger, which has good selectivity for molybdenum-99 and strong radiation resistance. Anion exchange resin has high selectivity for molybdenum-99, but as an organic matter, it will decompose under strong radiation environment, affecting the separation and purification effect. Therefore, alumina is used as a stationary phase in the first separation device 11 to perform a primary separation on the target solution with the largest radioactivity. The radioactivity of the primary purified solution obtained by the primary separation is significantly reduced, which meets the radiation environment of the anion exchange resin. Finally, activated carbon is used to further purify impurities (especially iodine-131) in fission molybdenum-99, and the organic matter introduced in the separation process is removed by strong adsorption.

[0148] The type of anion exchange resin is not limited here, and any anion exchange resin that is conducive to adsorbing molybdenum-99 can be used. Exemplarily, the anion exchange resin is AG1-X8 resin.

[0149] Here, it should be noted that the filling of the separation devices 10 at each level can be done automatically by a machine or manually. After the separation devices 10 at each level are filled, the separation system 1 is connected to the liquid supply system 2 and the control system 3, and the operator can stay away from the separation device 10 and remotely operate the control system 3, and the control system 3 automatically controls the separation device 10 to achieve automated separation and purification. Except for this step, which may involve manual operation, the remaining steps do not require manual intervention, which is conducive to protecting the safety of the operator.

[0150] Step S120, the control system controls the target solution to be separated in the liquid supply system to be added to the first separation device, and the first separation device performs primary separation on the target solution to obtain a primary purified solution.

[0151] The primary separation process of the first separation device 11 is not limited here. The first separation device 11 can realize the rough separation of the target solution and reduce the radiation intensity of the target solution, which is beneficial to reduce the influence of radiation on subsequent separation steps.

[0152] Step S130, the control system controls the primary purified liquid to be separated in the liquid supply system to be added to the second separation device, and the second separation device performs secondary separation on the primary purified liquid to obtain secondary purified liquid.

[0153] The secondary separation process of the second separation device 12 is not limited here. The second separation device 12 can realize the secondary separation of the primary purified liquid to prepare for the subsequent fine separation and concentration.

[0154] Step S140, the control system controls the secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the third separation device performs three-stage separation on the secondary purified liquid to obtain a three-stage purified liquid.

[0155] The three-stage separation process of the third separation device 13 is not limited here. The second separation device 12 can realize fine separation of the secondary purified liquid and simultaneously concentrate the secondary purified liquid to obtain a tertiary purified liquid with a higher molybdenum-99 concentration.

[0156] The fission molybdenum-99 separation method provided in the present application realizes the three-stage separation and purification of molybdenum-99 by setting a separation system 1 including a first separation device 11, a second separation device 12 and a third separation device 13, which is beneficial to improving the effect of separation and purification of molybdenum-99. By setting a liquid supply system 2 and a control system 3, the control system 3 controls the medium injection of the liquid supply system 2, so that the entire separation process can be fully automated, and the separation process does not require human operation, which is beneficial to reducing the impact of radiation on the operator and solving the problem of requiring personnel to monitor the operation during the long separation process. At the same time, automated control can also accurately control various parameters in the separation process, which is beneficial to improving the separation and purification effect.

[0157] In some embodiments, the above step S120 includes the following steps S121 to S124:

[0158] Step S121, the control system controls the 0.1mol / L-1.0mol / L nitric acid solution in the liquid supply system to elute the aluminum oxide for pre-treating the aluminum oxide.

[0159] The specific concentration of the nitric acid solution is not limited here, for example, it can be 0.1.0 mol / L, 0.2 mol / L, 0.3 mol / L, 0.4 mol / L, 0.5 mol / L, 0.6 mol / L, 0.7 mol / L, 0.8 mol / L, 0.9 mol / L, 1 mol / L and the like.

[0160] The adsorption of molybdate ions on alumina changes with pH. In an acidic environment, molybdenum-99 is present as -2 molybdate (MoO4 2- ) exists in the form of, and the surface of alumina is positively charged, and the -2 valence molybdate is adsorbed on the surface of alumina by electrostatic adsorption. By controlling the elution of alumina with nitric acid solution, alumina can be placed in an acidic environment, which is beneficial to improving the adsorption effect of alumina on molybdenum-99 in the target solution.

[0161] Step S122, the control system controls the target solution to be separated in the liquid supply system to be added into the first separation device, and the target solution is adsorbed by the aluminum oxide.

[0162] Here, it should be noted that the adsorption of the target solution by alumina is electrostatic adsorption. When the target solution flows through the alumina, the alumina electrostatically adsorbs the molybdenum-99 in the target solution, retains the molybdenum-99 in the solution in the alumina, removes impurities in the target solution that are not adsorbed by the alumina, and realizes the primary separation of molybdenum-99 from the target solution.

[0163] Step S123, the control system controls the first eluting liquid in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution.

[0164] The specific type of the first eluent is not limited here, and is determined specifically according to the type of impurities in the target solution. The impurities in the target solution are removed by eluting with the first eluent to prepare for subsequent desorption.

[0165] Step S124, the control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to desorb from the alumina to obtain a primary purified liquid.

[0166] In an environment with a pH value greater than 6.0, molybdenum-99 still exists in the form of -2 molybdate (MoO4 2- ) form, but the surface of alumina is negatively charged, and the adsorption of alumina to molybdate ions is weakened. By adding 1.0 mol / L-2.0 mol / L ammonia solution, the desorption effect is achieved.

[0167] The addition of the target solution after pre-treating the alumina by eluting the alumina with a nitric acid solution is beneficial to improving the adsorption effect of the alumina on molybdenum-99. The alumina is eluted with the first eluting solution to reduce the impurities entering the primary purification solution. The primary purification solution is obtained by desorbing the alumina with an ammonia solution, and the separation and purification principle is simple.

[0168] In some embodiments, the above step S123 includes the following steps S1231 to S1234:

[0169] Step S1231, the control system controls the 0.1 mol / L-1.0 mol / L nitric acid solution in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution.

[0170] The specific concentration of the nitric acid solution is not limited here, for example, it can be 0.1.0 mol / L, 0.2 mol / L, 0.3 mol / L, 0.4 mol / L, 0.5 mol / L, 0.6 mol / L, 0.7 mol / L, 0.8 mol / L, 0.9 mol / L, 1 mol / L and the like.

[0171] By controlling the elution of alumina with nitric acid solution, on the one hand, it is beneficial to further improve the adsorption of molybdenum-99 in the target solution by alumina, and on the other hand, it is beneficial to remove impurities in the target solution.

[0172] Step S1232, the control system controls the deionized water in the liquid supply system to elute the aluminum oxide until the pH value of the deionized water flowing out of the eluent is neutral.

[0173] Step S1233, the control system controls the physiological saline in the liquid supply system to rinse the impurities on the surface of the aluminum oxide.

[0174] Here, physiological saline is used to elute and remove technetium-99m from the target solution.

[0175] Step S1234, the control system controls the 0.01 mol / L-0.1 mol / L ammonia solution in the liquid supply system to elute the aluminum oxide to change its surface environment.

[0176] By washing with the above-mentioned various eluents, specific impurities in the target solution can be removed, preparing for subsequent desorption and reducing impurities entering the primary purification solution.

[0177] In some embodiments, the above step S130 includes the following steps S131 to S134:

[0178] Step S131, the control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to elute the anion exchange resin for pre-treating the anion exchange resin.

[0179] Here, the anion exchange resin is AG1-X8 resin. The specific concentration of the ammonia solution is not limited here, for example, it can be 1.0mol / L, 1.1mol / L, 1.2mol / L, 1.3mol / L, 1.4mol / L, 1.5mol / L, 1.6mol / L, 1.7mol / L, 1.8mol / L, 1.9mol / L, 2.0mol / L, etc.

[0180] It should be noted that the 1.0 mol / L-2.0 mol / L ammonia solution here is beneficial to improving the adsorption effect of the anion exchange resin on molybdenum-99 in the primary purification liquid when the stationary phase is an anion exchange resin.

[0181] Step S132, the control system controls the primary purified liquid to be separated in the liquid supply system to be added into the second separation device, and the primary purified liquid is adsorbed by the anion exchange resin.

[0182] Here, the anion exchange resin converts the divalent molybdate (MoO4 2-) is adsorbed by the primary purified liquid, while the U matrix and other fission impurities such as strontium (Sr), ruthenium (Ru), zirconium (Zr), etc. in the primary purified liquid exist in the form of cations and do not undergo ion exchange reaction with the anion exchange resin, thereby removing the impurities in the primary purified liquid that are not adsorbed by the anion exchange resin and realizing the secondary separation of molybdenum-99 from the primary purified liquid.

[0183] Step S133, the control system controls the second eluent in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid.

[0184] The specific type of the second eluent is not limited here, and is specifically determined according to the type of impurities in the primary purification liquid. The impurities in the primary purification liquid are removed by eluting with the second eluent to prepare for subsequent desorption.

[0185] Step S134, the control system controls the 1.0 mol / L-2.0 mol / L ammonium carbonate solution in the liquid supply system to desorb from the anion exchange resin to obtain a secondary purified liquid.

[0186] The specific concentration of the ammonium carbonate solution is not limited here, for example, it can be 1.0 mol / L, 1.1 mol / L, 1.2 mol / L, 1.3 mol / L, 1.4 mol / L, 1.5 mol / L, 1.6 mol / L, 1.7 mol / L, 1.8 mol / L, 1.9 mol / L, 2.0 mol / L and the like.

[0187] The anion exchange resin is eluted with an eluent to reduce the impurities entering the secondary purification liquid. The molybdenum-99 on the anion exchange resin is desorbed with an ammonium carbonate solution to obtain the secondary purification liquid. The separation and purification principle is simple.

[0188] In some embodiments, the above step S133 includes the following steps S1331 to S1334:

[0189] Step S1331, the control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid.

[0190] The specific concentration of the ammonia solution is not limited here, for example, it can be 1.0 mol / L, 1.1 mol / L, 1.2 mol / L, 1.3 mol / L, 1.4 mol / L, 1.5 mol / L, 1.6 mol / L, 1.7 mol / L, 1.8 mol / L, 1.9 mol / L, 2.0 mol / L and the like.

[0191] By controlling the elution of the anion exchange resin with an ammonia solution, on the one hand, it is beneficial to further improve the adsorption of molybdenum-99 in the primary purification liquid by the anion exchange resin, and at the same time it is beneficial to remove impurities in the primary purification liquid.

[0192] Step S1332, the control system controls the deionized water in the liquid supply system to elute the anion exchange resin until the pH value of the deionized water flowing out of the eluent is neutral.

[0193] The anion exchange resin is further eluted with deionized water until the pH value of the deionized water discharged from the elution is neutral, so as to prepare for the subsequent elution of the anion exchange resin with an acidic solution such as malonic acid solution, thereby reducing the adverse effect on the elution effect caused by the reaction between the malonic acid solution and the ammonia solution in the previous step.

[0194] Step S1333, the control system controls the 0.01 mol / L-0.015 mol / L malonic acid solution in the liquid supply system to elute impurities on the surface of the anion exchange resin.

[0195] Step S1334, the control system controls the deionized water in the liquid supply system to elute the anion exchange resin until the pH value of the deionized water flowing out of the eluent is neutral.

[0196] Further elution with deionized water is performed to remove impurities in the primary purification solution until the pH value of the deionized water discharged from the elution is neutral, in order to prepare for the subsequent desorption of the anion exchange resin by the ammonium carbonate solution and reduce the weakening of the desorption effect caused by the reaction of the ammonium carbonate solution with the malonic acid solution in the previous step.

[0197] By washing with the above-mentioned various eluents, specific impurities in the primary purification liquid can be removed, preparing for subsequent desorption and reducing impurities entering the secondary purification liquid.

[0198] In some embodiments, the above step S140 includes the following steps S141 to S145:

[0199] Step S141, the control system controls the pH value in the liquid supply system to be 2.0-2.5, and the nitric acid solution is used to wash the activated carbon for pre-treatment of the activated carbon.

[0200] The pH value of the nitric acid solution is not limited here, for example, the pH value can be 2.0, 2.1, 2.2, 2.3, 2.4, 2.5, etc.

[0201] By controlling the elution of activated carbon with nitric acid solution, the activated carbon can be placed in an acidic environment, which is beneficial to improving the adsorption effect of activated carbon on molybdenum-99 in the secondary purification liquid.

[0202] Step S142, the control system controls the concentrated nitric acid solution in the liquid supply system to adjust the pH value of the secondary purification liquid to 2.0-2.5.

[0203] The pH value of the secondary purification liquid is not limited here, for example, the pH value can be 2.0, 2.1, 2.2, 2.3, 2.4, 2.5, etc.

[0204] By controlling the secondary purification liquid to be in a nitric acid environment, it is beneficial to improve the adsorption effect of activated carbon on molybdenum-99 in the secondary purification liquid.

[0205] Step S143, the control system controls the acid-adjusted secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the activated carbon is used to adsorb the secondary purified liquid.

[0206] Here, it should be noted that the adsorption of the secondary purification liquid by the activated carbon is physical adsorption. When the secondary purification liquid flows through the activated carbon, the activated carbon physically adsorbs the molybdenum-99 in the secondary purification liquid, retains the molybdenum-99 in the solution in the activated carbon, removes the impurities in the secondary purification liquid that are not adsorbed by the activated carbon, and realizes the three-stage separation of molybdenum-99 from the target solution.

[0207] Step S144, the control system controls the third eluent in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid.

[0208] The specific type of the third eluent is not limited here, and is determined specifically according to the type of impurities on the surface of the activated carbon. The third eluent is used to remove impurities in the secondary purification liquid, preparing for subsequent desorption.

[0209] Step S145, the control system controls the 0.2 mol / L-1.0 mol / L sodium hydroxide solution in the liquid supply system to desorb from the activated carbon to obtain a tertiary purified liquid.

[0210] The specific concentration of the sodium hydroxide solution is not limited here, for example, it can be 0.2mol / L, 0.3mol / L, 0.4mol / L, 0.5mol / L, 0.6mol / L, 0.7mol / L, 0.8mol / L, 0.9mol / L, 1.0mol / L and the like.

[0211] The activated carbon is pre-treated by eluting it with a nitric acid solution and then added with a secondary purification liquid, which is beneficial to improving the adsorption effect of the activated carbon on molybdenum-99. The activated carbon is eluted with a third eluting liquid to reduce impurities in the secondary purification liquid. The activated carbon is desorbed with a sodium hydroxide solution to obtain a tertiary purification liquid. The separation and purification principle is simple.

[0212] In some embodiments, the above step S144 includes the following steps S1441 to S1442:

[0213] Step S1441, the control system controls the pH value in the liquid supply system to be 2.0-2.5, and the nitric acid solution is used to elute the activated carbon to remove impurities in the secondary purification liquid.

[0214] Step S1442, the control system controls the 1.5%-3.0% bromine aqueous solution in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid.

[0215] The specific concentration of the bromine aqueous solution is not limited here, for example, it can be 1.5%, 1.6%, 1.7%, 1.8%, 1.9%, 2%, 2.1%, 2.2%, 2.3%, 2.4%, 2.5%, 2.6%, 2.7%, 2.8%, 2.9%, 3.0%, etc. The bromine aqueous solution can be used to wash the activated carbon and remove impurities in the secondary purification solution.

[0216] Specific impurities in the secondary purification liquid can be removed by washing with the above-mentioned various eluents.

[0217] In some embodiments, the above step S110 includes the following steps S111 to S113:

[0218] Step S111, the control system controls the deionized water in the liquid supply system to wash the fine particles in the aluminum oxide.

[0219] Step S112, the control system controls the deionized water in the liquid supply system to wash the fine particles on the anion exchange resin.

[0220] Step S113, the control system controls the deionized water in the liquid supply system to wash the fine particles in the activated carbon.

[0221] Fine particles are the finest stationary phases in each stationary phase. These fine stationary phases will flow out with the injection of various solutions during the separation and purification process, becoming impurities in each process solution and the final tertiary purified liquid. Here, the fine particles in each stationary phase are washed out in advance during the separation process by deionized water, reducing their entry into the separation and purification process.

[0222] The above description is only a preferred embodiment of the present application and is not intended to limit the present application. For those skilled in the art, the present application may have various modifications and variations. Any modification, equivalent replacement, improvement, etc. made within the spirit and principle of the present application are included in the protection scope of the present application.

Claims

1. A method for automatically separating fission molybdenum-99, applied to a fission molybdenum-99 separation device, characterized in that: The fission molybdenum-99 separation device comprises a separation system, a liquid supply system and a control system; the separation system comprises a first separation device, a second separation device and a third separation device connected in sequence; the liquid supply system is connected to the separation system; the control system is used to control the liquid supply system to transport the stored medium to the separation system in a set order; The automatic separation method of fissionable molybdenum-99 comprises: The first separation device is filled with alumina, the second separation device is filled with anion exchange resin, and the third separation device is filled with activated carbon; The control system controls the target solution to be separated in the liquid supply system to be added to the first separation device, and the first separation device performs primary separation on the target solution to obtain a primary purified solution; The control system controls the first-level purified liquid to be separated in the liquid supply system to be added to the second separation device, and the second separation device performs secondary separation on the first-level purified liquid to obtain a secondary purified liquid; The control system controls the secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the third separation device performs three-stage separation on the secondary purified liquid to obtain a tertiary purified liquid.

2. The automatic separation method of fissionable molybdenum-99 according to claim 1, characterized in that: The control system controls the target solution to be separated in the liquid supply system to be added to the first separation device, and the first separation device performs primary separation on the target solution to obtain a primary purified solution, which includes: The control system controls the 0.1mol / L-1.0mol / L nitric acid solution in the liquid supply system to elute the aluminum oxide, so as to pretreat the aluminum oxide; The control system controls the target solution to be separated in the liquid supply system to be added into the first separation device, and the target solution is adsorbed by the alumina; The control system controls the first eluent in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution; The control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to desorb from the alumina to obtain the primary purified liquid.

3. The automatic separation method of fissionable molybdenum-99 according to claim 2, characterized in that: The control system controls the first elution liquid in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution, including: The control system controls the 0.1mol / L-1.0mol / L nitric acid solution in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution; The control system controls the deionized water in the liquid supply system to elute the aluminum oxide until the pH value of the deionized water flowing out of the eluent is neutral; The control system controls the physiological saline in the liquid supply system to elute the aluminum oxide to remove impurities in the target solution; The control system controls the 0.01 mol / L-0.1 mol / L ammonia solution in the liquid supply system to elute the aluminum oxide to change its surface environment.

4. The automatic separation method of fissionable molybdenum-99 according to claim 2, characterized in that: The control system controls the first-level purified liquid to be separated in the liquid supply system to be added to the second separation device, and the second separation device performs secondary separation on the first-level purified liquid to obtain the secondary purified liquid, which includes: The control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to elute the anion exchange resin, so as to pretreat the anion exchange resin; The control system controls the primary purified liquid to be separated in the liquid supply system to be added into the second separation device, and the anion exchange resin is used to adsorb the primary purified liquid; The control system controls the second eluent in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid; The control system controls the 1.0 mol / L-2.0 mol / L ammonium carbonate solution in the liquid supply system to desorb from the anion exchange resin to obtain the secondary purified liquid.

5. The automatic separation method of fissionable molybdenum-99 according to claim 4, characterized in that: The control system controls the second eluent in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid, including: The control system controls the 1.0 mol / L-2.0 mol / L ammonia solution in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid; The control system controls the deionized water in the liquid supply system to elute the anion exchange resin until the pH value of the deionized water flowing out of the eluent is neutral; The control system controls the 0.01mol / L-0.015mol / L malonic acid solution in the liquid supply system to elute the anion exchange resin to remove impurities in the primary purification liquid; The control system controls the deionized water in the liquid supply system to elute the anion exchange resin until the pH value of the deionized water flowing out of the eluent is neutral.

6. The automatic separation method of fissionable molybdenum-99 according to claim 4, characterized in that: The control system controls the secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the third separation device performs three-stage separation on the secondary purified liquid to obtain the three-stage purified liquid, which includes: The control system controls the pH value in the liquid supply system to be 2.0-2.5, and the nitric acid solution is used to elute the activated carbon for pre-treating the activated carbon; The control system controls the concentrated nitric acid solution in the liquid supply system to adjust the pH value of the secondary purification liquid to 2.0-2.5; The control system controls the acid-adjusted secondary purified liquid to be separated in the liquid supply system to be added to the third separation device, and the activated carbon is used to adsorb the secondary purified liquid; The control system controls the third eluent in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid; The control system controls the 0.2 mol / L-1.0 mol / L sodium hydroxide solution in the liquid supply system to desorb from the activated carbon to obtain the tertiary purified liquid.

7. The automatic separation method of fissionable molybdenum-99 according to claim 6, characterized in that: The control system controls the third eluent in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid, including: The control system controls the pH value of the nitric acid solution in the liquid supply system to be 2.0-2.5 to elute the activated carbon to remove impurities in the secondary purification liquid; The control system controls the 1.5%-3.0% bromine aqueous solution in the liquid supply system to elute the activated carbon to remove impurities in the secondary purification liquid.

8. The automatic separation method of fissionable molybdenum-99 according to claim 1, characterized in that: After the first separation device is filled with alumina, the second separation device is filled with anion exchange resin, and the third separation device is filled with activated carbon, the method further comprises: The control system controls the deionized water in the liquid supply system to wash the fine particles in the aluminum oxide; The control system controls the deionized water in the liquid supply system to wash the fine particles on the anion exchange resin; The control system controls the deionized water in the liquid supply system to rinse the fine particles in the activated carbon.

9. An automatic separation device for fission molybdenum-99, used for separating and purifying molybdenum-99 from a target solution containing molybdenum-99, characterized in that: include: frame; A separation system, the separation system is arranged on the frame, the separation system comprises a first separation device, a second separation device and a third separation device connected in sequence; The first separation device is used to perform primary separation on the target solution to obtain a primary purified solution; the second separation device is used to perform secondary separation on the primary purified solution to obtain a secondary purified solution; The third separation device is used to perform three-stage separation on the secondary purified liquid to obtain a tertiary purified liquid; A liquid supply system, the liquid supply system is arranged on the frame, the liquid supply system is connected to the separation system, the liquid supply system includes a liquid storage device, and the liquid storage device can be used to store at least the target solution, the eluent, the desorption liquid, the primary purification liquid, the secondary purification liquid and the tertiary purification liquid; A control system, wherein the control system automatically controls the medium stored in the liquid supply system to be injected into the separation system according to a set sequence.

10. The automatic separation device of fissionable molybdenum-99 according to claim 9, characterized in that: The liquid supply system includes a pipeline assembly, and the pipeline assembly includes a first pipeline assembly, a second pipeline assembly, a third pipeline assembly, and a fourth pipeline assembly; The liquid injection ports of the first separation device, the second separation device and the third separation device are connected to the liquid storage device through the first pipeline assembly; the liquid outlet of the first separation device is connected to the liquid injection port of the second separation device through the second pipeline assembly; the liquid outlet of the second separation device is connected to the liquid injection port of the third separation device through the third pipeline assembly; and the fourth pipeline assembly is connected to the liquid outlet of the third separation device.

11. The automatic separation device of fissionable molybdenum-99 according to claim 10, characterized in that: The control system comprises a first reversing valve, which is arranged on the first pipeline assembly, and the first reversing valve is used to selectively open or close the first pipeline assembly; and / or, The control system comprises a second reversing valve, the second reversing valve is arranged on the second pipeline assembly, and the second reversing valve is used to selectively open or close the second pipeline assembly; and / or, The control system comprises a third reversing valve, the third reversing valve is arranged on the third pipeline assembly, and the third reversing valve is used to selectively open or close the third pipeline assembly; and / or, The control system includes a fourth reversing valve, which is disposed on the fourth pipeline assembly and is used to selectively open or close the fourth pipeline assembly.

12. The automatic separation device of fissionable molybdenum-99 according to claim 9, characterized in that: The automatic separation device of fission molybdenum-99 includes a detection system, which includes an acid-base detector and a radioactivity detector. The radioactivity detector is used to detect radioactivity data in the first separation device, the second separation device and the third separation device.

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