CN112973445B - Automatic processing device for separating Ac-225 and operation method thereof - Google Patents

Automatic processing device for separating Ac-225 and operation method thereof Download PDF

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CN112973445B
CN112973445B CN202110168480.2A CN202110168480A CN112973445B CN 112973445 B CN112973445 B CN 112973445B CN 202110168480 A CN202110168480 A CN 202110168480A CN 112973445 B CN112973445 B CN 112973445B
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separation column
module
plug valve
liquid inlet
solution
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CN112973445A (en
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曹石巍
谈存敏
秦芝
田伟
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Institute of Modern Physics of CAS
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D59/00Separation of different isotopes of the same chemical element
    • B01D59/28Separation by chemical exchange
    • B01D59/32Separation by chemical exchange by exchange between fluids
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00Technologies related to metal processing
    • Y02P10/20Recycling

Abstract

The application belongs to the technical field of nuclear medicine, and relates to an automatic processing system for separating Ac-225 and an operation method thereof, wherein the automatic processing system comprises the following steps: the device comprises a leaching liquid inlet module, a material liquid inlet module, a first liquid inlet pump, a second liquid inlet pump, a separation column module, a recovery part, a plug valve module and a control module; the eluent liquid inlet module is connected with the first liquid inlet pump, the liquid inlet module is connected with the second liquid inlet pump, the first liquid inlet pump and the second liquid inlet pump are connected with the separation column module through the plug valve module, the separation column module is connected with the recovery part through the plug valve module, the solution containing Ac-225 is collected in the recovery part, and the control module is connected with the first liquid inlet pump, the second liquid inlet pump and the plug valve module and is used for selecting the solution entering the separation column module and the recovery part. The method is used for separating the isotope Ac-225, has the characteristics of rapidness, high efficiency, small waste liquid amount, high efficiency, low radioactivity risk, simple and convenient operation and the like, and can meet the domestic medical isotope research and application market.

Description

Automatic processing device for separating Ac-225 and operation method thereof
Technical Field
The application relates to an automatic processing system for separating Ac-225 and an operation method thereof, belonging to the technical field of nuclear medicine.
Background
The accelerator is used as an important mode for producing medical isotopes, is mainly used for producing neutron-deficient medical isotopes, and overcomes the defect of single medical isotope types at present to a great extent. Currently, the types of radionuclides that can be produced using accelerators account for over 60% of known medical isotope types, such as Mo-99/Tc-99m, cu-64, at-211, Y-88, F-18, C-11, I-123, ga-68, ac-225, ra-223, lu-177, and the like. The accelerator can directly irradiate to produce medical isotope, has the advantages of low construction cost and high target utilization rate, and is expected to become a new route for producing medical isotope by replacing a reactor. Therefore, the problem to be solved is to separate and purify medical isotopes generated by accelerator irradiation.
Ac-225 has a half-life t as a 100% alpha-decay radionuclide 1/2 The energy of the radiation is 5.8MeV, and the range in soft tissue is only equivalent to the diameter of 5-9 cells. Since the Ac-225 cascade decay process also includes 6 short life childrenThe body can emit 4 alpha particles after each decay, can effectively remove cancer cells for many times, and finally can decay into nontoxic Bi-209. Notably, its daughter Bi-213 (t 1/2 =45.6 min) decays, and also emits characteristic gamma rays of 440keV, so that review imaging can be performed simultaneously during treatment.
Currently, ac-225 is obtained mainly by irradiation of 232Th targets with high energy proton beams, but this approach is accompanied by a number of impurity species in addition to Ac-225 production. Methods for separating Ra and Ac from irradiated thorium targets have been widely used in the prior art, and are mainly classified by ion exchange or extraction chromatography. With further research on coordination chemistry and continuous development of chelating methods, sulfate, citrate or other reagents are used as complexing agents, so that positive tetravalent Th ion matrixes can generate anion complexes, ra and Ac are reserved in a cationic form, and the separation operation process of Th/Ac (Ra) can be simplified, but due to almost consistent chemical properties between lanthanide and product Ac, selective removal of such impurities is more challenging, and particularly if elements such as lanthanum, cerium and the like with high yield are not completely separated, medical application of accelerator irradiation of Ac-225 products is limited.
From prior art studies, it has been found that there is currently no universal device or system for separating Ra and Ac from irradiated thorium targets. Therefore, the experimenters mostly adopt a manual separation method, the dependency on the manual capability of operators is great, the operation is discontinuous, the steps are complicated, the product loss is more, the recovery rate and the separation efficiency are low, the treatment speed is low, the treatment capacity is small, and particularly, the method has great limitation on the separation and purification of medical isotopes with shorter service life and cannot meet the requirements of the accelerator on large-scale production and application to the nuclear medicine field. In addition, the existing separation method can generate larger radiation dose for operators and bring potential harm to personal safety.
Disclosure of Invention
Aiming at the problems, the application aims to provide an automatic processing system for separating Ac-225 and an operation method thereof, which are used for separating isotope Ac-225, have the characteristics of rapidness, high efficiency, small waste liquid amount, high efficiency, universality, low radioactivity risk, simple and convenient operation and the like, and can meet the domestic medical isotope research and application market.
In order to achieve the above purpose, the present application adopts the following technical scheme: an automated processing system for separating Ac-225, comprising: the device comprises a leaching liquid inlet module, a material liquid inlet module, a first liquid inlet pump, a second liquid inlet pump, a separation column module, a recovery part, a plug valve module and a control module; the eluent liquid inlet module is connected with the first liquid inlet pump, the liquid inlet module is connected with the second liquid inlet pump, the first liquid inlet pump and the second liquid inlet pump are connected with the separation column module through the plug valve module, the separation column module is connected with the recovery part through the plug valve module, the solution containing Ac-225 is collected in the recovery part, and the control module is connected with the first liquid inlet pump, the second liquid inlet pump and the plug valve module and is used for selecting the solution entering the separation column module and the recovery part.
Further, the leacheate liquid inlet module comprises a deionized water pipeline, a first leacheate pipeline, a second leacheate pipeline, a third leacheate pipeline and a fourth leacheate pipeline, each leacheate pipeline is connected with the first liquid inlet pump through a first plug valve component in the plug valve module, and the first plug valve component comprises a plurality of T-shaped three-way plug valves.
Further, a plurality of three-way plug valves are all arranged on a main pipeline, interfaces, perpendicular to the main pipeline, of the three-way plug valves are connected with corresponding pipelines in the eluent liquid inlet module, when the three-way plug valves are opened, the corresponding pipelines in the eluent liquid inlet module are communicated, and when the three-way plug valves are closed, the three-way plug valves are connected with the main pipeline.
Further, the first eluent is an ammonium sulfate solution with a concentration of 0.3-0.6 mol/L, the second eluent is a nitric acid solution with a concentration of 0.01-0.1 mol/L, the third eluent is a nitric acid solution with a concentration of 4-6 mol/L, and the fourth eluent is a nitric acid solution with a concentration of 9-13 mol/L.
Further, the feed liquid is a solution of a Th target subjected to proton irradiation, comprising: th with concentration of 0.01-0.1 mol/L 4+ Ammonium sulfate solution with concentration of 0.4-0.6 mol/L and solution of nuclear reaction product of the Th target irradiated by proton beam.
Further, the separation column module comprises two separation columns connected in parallel, and the two separation columns are connected together through a second plug valve assembly in the plug valve module, wherein the first separation column is a cation column, and the second separation column is a DGA resin column.
Further, the automated processing system further comprises a waste liquid module, the waste liquid module is connected with the recovery part through a third plug valve assembly in the plug valve module, and the waste liquid module can separate waste liquid with high radioactivity, low radioactivity and non-radioactivity.
Further, the waste module includes a line for receiving Ra-223 byproducts, a line for receiving la+ce components, a line for receiving high radioactivity waste, a line for receiving low radioactivity waste, and a line for receiving non-radioactive waste.
The application also discloses an operation method of the automatic processing system for separating Ac-225, which adopts any one of the automatic processing systems for separating Ac-225 and comprises the following steps: s1, introducing deionized water to remove pipeline air; s2, introducing the feed liquid into a pretreated first separation column, and introducing the solution flowing out of the first separation column into a pipeline for receiving high-radioactivity waste liquid for collection; s3, eluting the first separation column by adopting a first eluting solution, and introducing the solution flowing out of the first separation column into a pipeline for receiving the high-radioactivity waste liquid for collection; s4, leaching the first separation column by using a second leaching solution, and introducing the solution flowing out of the first separation column into a pipeline for receiving the low-radioactivity waste liquid for collection; s5, sequentially and continuously eluting the first separation column and the pretreated second separation column by adopting a third eluent, and introducing the solution flowing out of the second separation column into a pipeline for receiving Ra-223 byproducts for collection; s6, leaching the second separation column by using a fourth leaching solution, and introducing the solution flowing out of the second separation column into a recovery part for recovery; s7, eluting the second separation column by deionized water, and introducing the solution flowing out of the second separation column into a pipeline for receiving the La+Ce component.
Further, the pretreatment process of the first separation column and the second separation column is as follows: and eluting the first separation column by using a first eluent, and eluting the second separation column by using a third eluent, wherein the flow rates of the first eluent and the third eluent are 1-5 mL/min, and the volumes of the first eluent and the third eluent are more than 5 times of the volumes of the first separation column and the second separation column respectively.
Due to the adoption of the technical scheme, the application has the following advantages:
1. according to the scheme, the medical isotope Ac-225 can be rapidly, efficiently, repeatedly, automatically and massively separated and purified from the Th target irradiated by the accelerator, and the complicated manual operation and the potential risks caused by high-dose radioactive isotopes are avoided.
2. The application selects strong acid resistant medium as the touch material, the dead volume of the liquid pipeline is small, the waste liquid amount is small, and the product purity is high.
3. The system has closed-loop control and jamming detection capability, adopts the design of separating the pneumatic executive component from the electronic circuit, and has higher reliability and fault tolerance capability.
4. The application separates the high-radioactivity, low-radioactivity and non-radioactivity waste liquid, is convenient for subsequent treatment, and avoids the pollution possibly caused by the high-radioactivity waste liquid.
Drawings
FIG. 1 is a block diagram of an automated processing system for separating Ac-225 in accordance with one embodiment of the present application;
FIG. 2 is a block diagram of a T-shaped three-way plug valve in accordance with one embodiment of the present application;
FIG. 3 is a schematic diagram of an automated processing system incorporating a control module according to one embodiment of the present application;
fig. 4 is a structural view of a coaxial coupling according to an embodiment of the present application, fig. 4 (a) is a front view of the coaxial coupling, and fig. 4 (b) is a top view of the coaxial coupling;
FIG. 5 is a schematic diagram showing the connection relationship between a cylinder and a plug valve according to an embodiment of the present application;
FIG. 6 is a schematic view of a valve island structure in an embodiment of the application;
FIG. 7 is a schematic illustration of a method of operation of an automated processing system for separating Ac-225 in one embodiment of the present application;
FIG. 8 is a graph of gamma spectroscopy of a solution containing Ac-225 as a product in an embodiment of the application.
Detailed Description
The present application will be described in detail with reference to specific examples thereof in order to better understand the technical direction of the present application by those skilled in the art. It should be understood, however, that the detailed description is presented only to provide a better understanding of the application, and should not be taken to limit the application. In the description of the present application, it is to be understood that the terminology used is for the purpose of description only and is not to be interpreted as indicating or implying relative importance.
Example 1
The embodiment discloses an automated processing system for separating Ac-225, as shown in FIG. 1, comprising: the device comprises eluent liquid inlet modules A0-A5, a liquid inlet module A6, a first liquid inlet pump P1, a second liquid inlet pump P2, separation column modules C1-C2, a recovery part A11, plug valve modules A12-A16, a control module and a waste liquid module.
The eluent liquid inlet module is connected with the first liquid inlet pump, the liquid inlet module is connected with the second liquid inlet pump, the first liquid inlet pump and the second liquid inlet pump are connected with the separation column module through the plug valve module, the separation column module is connected with the recovery part through the plug valve module, the solution containing Ac-225 is collected in the recovery part, and the control module is connected with the first liquid inlet pump, the second liquid inlet pump and the plug valve module and is used for selecting the solution entering the separation column module and the recovery part.
The eluent liquid inlet module comprises a deionized water pipeline A0, a first eluent pipeline A1, a second eluent pipeline A2, a third eluent pipeline A3 and a fourth eluent pipeline A4, and each eluent pipeline is connected with a first liquid inlet pump through a first plug valve component in the plug valve module.
The first eluent is ammonium sulfate solution with the concentration of 0.3-0.6 mol/L, the second eluent is nitric acid solution with the concentration of 0.01-0.1 mol/L, the third eluent is nitric acid solution with the concentration of 4-6 mol/L, and the fourth eluent is nitric acid solution with the concentration of 9-13 mol/L.
The feed liquid is a solution of Th target subjected to proton irradiation, comprising: th with concentration of 0.01-0.1 mol/L 4+ Sulfur with concentration of 0.4-0.6 mol/LAmmonium acid solution and solution of nuclear reaction product of Th target irradiated by proton beam. The feed liquid inlet module A6 adopts a sharp bottom bottle so that the liquid can be completely extracted.
The separation column module comprises two separation columns connected in parallel, and the two separation columns are connected together through a second plug valve component in the plug valve module, wherein the first separation column C1 is a cation column, the model is AG50W multiplied by 8, and the column volume is 5-10mL; the second separation column C2 is a DGA resin column, the loaded resin is TEHDGA, and the column volume is 2-5mL.
The automatic treatment system further comprises a waste liquid module, wherein the waste liquid module is connected with the recovery part through a third plug valve assembly in the plug valve module, and the waste liquid module can separate waste liquid with high radioactivity, low radioactivity and non-radioactivity. The waste liquid module includes a line a12 for receiving Ra-223 byproducts, a line a13 for receiving la+ce components, a line a14 for receiving highly radioactive waste liquid, a line a15 for receiving low radioactive waste liquid, and a line a16 for receiving non-radioactive waste liquid.
The plug valve module comprises first plug valve assemblies V1-V5, second plug valve assemblies V6-V10 and third plug valve assemblies V11-V15, and each plug valve assembly has the same structure and comprises a plurality of T-shaped three-way plug valves. As shown in fig. 2, the plurality of T-shaped three-way stopcocks are all arranged on a main pipeline, the interfaces of the three-way stopcocks, which are vertical to the main pipeline, are connected with the corresponding pipelines in the eluent liquid inlet module, when the three-way stopcock is opened, the corresponding pipelines in the eluent liquid inlet module are communicated, and when the three-way stopcock is closed, the three-way stopcock is connected with the main pipeline. In this embodiment, each plug valve assembly integrates 5T-shaped three-way plug valves, which can freely rotate 360 °. The inner diameter of the main pipeline is 1mm. The vertical joint of the T-shaped three-way plug valve and the main pipeline adopts an international standard internal thread joint 1/4-28UNF. The internal thread joint is connected with a PTFE hard tube, and the other end of the hard tube is connected with a eluent liquid inlet module A0-A5, a separation column module C1-C2, a recovery part A11 and a waste liquid module.
As shown in fig. 1, a main pipeline liquid inlet end of the first plug valve assembly is connected with a deionized water pipeline A0, a liquid outlet end of the first plug valve assembly is connected with a first liquid inlet pump P1, a plug valve V1 is connected with a first leaching liquid pipeline A1, a plug valve V2 is connected with a second leaching liquid pipeline A2, a plug valve V3 is connected with a third leaching liquid pipeline A3, a plug valve V4 is connected with a fourth leaching liquid pipeline A4, and a plug valve V5 is connected with a standby pipeline A5. The main pipeline liquid inlet end in the first plug valve component is connected with a deionized water pipeline A0, the liquid outlet end is connected with a first liquid inlet pump P1, a plug valve V1 is connected with the first eluent pipeline A1, a plug valve V2 is connected with a second eluent pipeline A2, a plug valve V3 is connected with a third eluent pipeline A3, a plug valve V4 is connected with a fourth eluent pipeline A4, and a plug valve V5 is connected with a standby pipeline A5.
The main pipeline liquid inlet end in the second plug valve assembly is connected with a first liquid inlet pump P1, the liquid outlet end is connected with a third plug valve assembly, a plug valve V6 is connected with the liquid outlet end of a second liquid inlet pump P2, a plug valve V7 is connected with the liquid inlet end of a first separation column C1, a plug valve V8 is connected with the liquid outlet end of the first separation column C1, a plug valve V9 is connected with the liquid inlet end of a second separation column C2, and a plug valve V10 is connected with the liquid outlet end of the second separation column C2.
The main pipeline liquid inlet end in the third plug valve assembly is connected with the second plug valve assembly, the liquid outlet end is connected with a pipeline A16 for receiving non-radioactive waste liquid, the plug valve V11 is connected with the recovery part A11, the plug valve V12 is connected with a pipeline A12 for receiving Ra-223 byproducts, the plug valve V13 is connected with a pipeline A13 for receiving La+Ce components, the plug valve V14 is connected with a pipeline A14 for receiving high-radioactive waste liquid, and the plug valve V15 is connected with a pipeline A15 for receiving low-radioactive waste liquid.
As shown in fig. 3, the control module in this embodiment includes a switch, a communication sub-module, a CPU and an I/O sub-module, where the communication sub-module is connected with an upper computer, and the I/O sub-module is connected with a cylinder 1, and the cylinder 1 is connected with each T-type three-way plug valve through a coaxial coupling 2. The structure of the coaxial coupling 2 is shown in fig. 4, where fig. 4 (a) is a front view of the coaxial coupling 2, and fig. 4 (b) is a top view of the coaxial coupling 2. Each cylinder 1 is connected with a power supply and a gas source through a valve island 3 comprising a plurality of electromagnetic valves. As shown in fig. 5, in this embodiment, the radial dimension of each cylinder 1 is 20mm, the swing angle is 90 degrees, the magnetic switch feedback is provided, 5 cylinders are arranged on the container bottom plate 4 in a group, the screws are used for fixing the container bottom plate 4 side by side, and the distance between the centers of adjacent cock is equal to the distance between the output shafts of the adjacent swing cylinders 1. The output shaft of the cylinder 1 and the plug valve are connected by a coaxial coupling 2. One end of the coupling piece is provided with a cross-shaped groove for embedding a rotary rod 5, the rotary rod 5 is connected with a cock of the cock valve and used for controlling the cock valve to rotate, and the diameter of the rotary rod 5 is 4mm. The other end of the coaxial coupling piece 2 is a round hole which is used for connecting with the output shaft of the air cylinder 1, and holes are formed in the side wall of the coaxial coupling piece 2 in the direction perpendicular to the output shaft, so that an M3 flat head screw is screwed into a milling plane of the shaft after the output shaft is inserted. The plug valve is fixed on the container bottom plate 4 by a fixing screw, so that the three parts of the cylinder 1, the coaxial coupling piece 2 and the plug valve are ensured to coaxially rotate and cannot fall off. The arrow direction in fig. 5 is the cylinder rotation direction.
The cylinder 1 is pushed to rotate by the external air pressure. The rotation angle of each swing cylinder 1 is 90 degrees, and the rotation moment is not less than 1.5 N.m/MPa. The rotation direction and initial state thereof depend on the connection sequence of the gas input port and the solenoid valve island 3. As shown in fig. 6, 15 2-position 3-way solenoid valves are installed on the valve island 3, and the two output ends of A and B of each solenoid valve are respectively connected with two input ends GA and GB of the cylinder 1 by phi 8 quick-plug hoses. The magnetic switch on the cylinder 1 for position feedback is connected to the I/O interface of the PLC, and the acquisition of the position feedback signal forms a closed loop control. The valve island 3 is connected with a communication submodule of the PLC through a field bus, and the opening and closing states of each electromagnetic valve are controlled through a relay.
In the embodiment, the air source can adopt an air steel cylinder or an air compressor, and the output air pressure is not less than 0.5MPa after the pressure is reduced. The air source outlet is connected with a filtering pressure-reducing valve and a micro-fog separator. The working gas is air, argon or nitrogen.
Example two
Based on the same inventive concept, this embodiment discloses a method for operating an automated processing system for separating Ac-225, the automated processing system employing the automated processing system for separating Ac-225 of any one of the first embodiments, as shown in fig. 7, comprising the steps of:
s1, introducing ionized water to remove air in the pipeline. The specific operation process is as follows: immersing all the pipelines at the lower ends of the plug valves V1-V5 into a liquid storage bottle filled with deionized water, starting a first liquid inlet pump P1, enabling deionized water in a deionized water pipeline A0 to reach a pipeline A16 for receiving non-radioactive waste liquid through the plug valve V1 and the first liquid inlet pump P1, and removing air in a main pipeline; sequentially opening plug valves V1, V2, V3, V4 and V5 to remove air of each pipeline; stopping the first liquid inlet pump P1, starting the plug valve V6, starting the second liquid inlet pump P2, and exhausting air in the liquid inlet module A6; the plug valves V7, V9 are opened, the plug valves V8, V10 are closed, and the air in the first separation column C1 and the second separation column C2 is discharged. Wherein the flow rates of the first liquid inlet pump P1 and the second liquid inlet pump P2 are 2-10 mL/min. After completion, all plug valves are closed.
S2, introducing the feed liquid into a pretreated first separation column, and introducing the solution flowing out of the first separation column into a pipeline for receiving the high-radioactivity waste liquid for collection. The specific operation steps are as follows: the plug valve V6 is opened, the second liquid inlet pump P2 is started, the liquid enters the first separation column C1 through the second liquid inlet pump P2, the plug valve V6 and the plug valve V7, the solution is discharged through the plug valve V8 and is collected in the pipeline A14 for receiving the high-radioactivity liquid waste through the plug valve V14. Wherein the Ac and Ra components in the feed solution are retained in the first separation column C1, and the Th component is collected in a pipeline A14 for receiving the high-radioactivity waste liquid. The flow rate of the second liquid inlet pump P2 is 1mL/min, and the volume of the used feed liquid is 110mL. After completion, all plug valves are closed.
S3, eluting the first separation column by using a first eluting solution, and introducing the solution flowing out of the first separation column into a pipeline for receiving the non-radioactive waste liquid for collection. The specific operation steps are as follows: the first liquid inlet pump P1 is started, the plug valve V1 is opened, the first leaching solution passes through the plug valve V1, the first liquid inlet pump P1 and the plug valve V7, enters the first separation column C1, the solution is discharged through the plug valve V8, and is collected in the pipeline A14 for receiving the high-radioactivity waste liquid through the plug valve V14. The solution containing a large amount of Th component in this step is collected in line A14 which receives the high radioactivity waste liquid. The flow rate of the first liquid inlet pump P1 is 1mL/min, and the volume of the used first eluent is 80mL. After completion, all plug valves are closed.
S4, eluting the first separation column by using a second eluting solution, and introducing the solution flowing out of the first separation column into a pipeline for receiving the low-radioactivity waste liquid for collection. The specific operation steps are as follows: the first liquid inlet pump P1 is started, the plug valve V2 is opened, the second leaching solution passes through the plug valve V2, the first liquid inlet pump P1 and the plug valve V7, enters the first separation column C1, the solution is discharged through the plug valve V8, and is collected in the pipeline A15 for receiving the low-radioactivity waste liquid through the plug valve V15. The solution containing the trace Th component in this step was collected in line A15 which received the low radioactivity waste liquid. The flow rate of the first liquid inlet pump P1 is 1mL/min, and the volume of the second eluent is 80mL. After completion, all plug valves are closed.
S5, sequentially and continuously eluting the first separation column and the pretreated second separation column by adopting a third eluting solution, and introducing the solution flowing out of the second separation column into a pipeline for receiving Ra-223 byproducts for collection. The specific operation steps are as follows: the first liquid inlet pump P1 is started, the plug valve V3 is opened, the third leaching solution passes through the plug valve V3, the first liquid inlet pump P1 and the plug valve V7, enters the first separation column C1, discharges the solution through the plug valve V8, passes through the plug valve V9, enters the second separation column C2, discharges the solution through the plug valve V10, passes through the plug valve V12 and is collected in the pipeline A12 for receiving the Ra-223 byproducts. The solution containing the Ra-223 by-product in this step is collected in line a12 which receives the Ra-223 by-product. The flow rate of the first liquid inlet pump P1 is 1mL/min, and the volume of the second eluent is 70mL. After completion, all plug valves are closed.
S6, leaching the second separation column by using a fourth leaching solution, and introducing the solution flowing out of the second separation column into a recovery part for recovery. The specific operation steps are as follows: the first liquid inlet pump P1 is started, the plug valve V4 is opened, the fourth eluent passes through the plug valve V4, the first liquid inlet pump P1 and the plug valve V9, enters the second separation column C2, the solution is discharged through the plug valve V10, and is collected in the recovery part A11 through the plug valve V11. The solution containing the product Ac-225 in this step is collected in the recovery section A11. The flow rate of the first liquid inlet pump P1 is 1mL/min, and the volume of the second eluent is 80mL. After completion, all plug valves are closed.
S7, eluting the second separation column by deionized water, and introducing the solution flowing out of the second separation column into a pipeline for receiving the La+Ce component. The specific operation steps are as follows: the first liquid inlet pump P1 is started, deionized water passes through the first liquid inlet pump P1 and a plug valve V9, enters the second separation column C2, and the solution is discharged through the plug valve V10 and is collected in a pipeline A13 for receiving La+Ce components through the plug valve V13. The solution containing the la+ce component in this step is collected in line a13 which receives the la+ce component. The flow rate of the first liquid inlet pump P1 is 1mL/min, and the volume of the second eluent is 60mL. After completion, all plug valves are closed.
The whole experimental process is ended. The recovery part A11 is a solution only containing the Ac-225 product, and the Ac-225 product can be obtained by carrying out subsequent treatment on the solution.
In order to verify the recovery efficiency and the radioactive purity of the solution of the recovery unit A11 according to the present application, the present example performed gamma spectroscopy analysis. The results of the Ac-225 product gamma spectrum analysis are shown in FIG. 8, from which it can be seen that only Ac-225 (represented by the inverted triangle in FIG. 8), its decay daughter Fr-221 (represented by the square in FIG. 8), bi-213 (represented by the diamond in FIG. 8), tl-209 (represented by the circle in FIG. 8) are present in the final product spectrum components. The recovery efficiency of the Ac-225 product obtained by separating from the solution of the Th target after proton beam irradiation by the scheme is not lower than 80%, the recovery efficiency of the byproduct Ra-223 is not lower than 80%, and the radioactive purity of the Ac-225 product is not lower than 95% can be determined by calculating the activities of each component in the solution and the ratio of the activities of each component in the solution before and after separation.
Wherein, the pretreatment process of the first separation column and the second separation column is as follows: the first eluting solution is adopted to leach the first separation column, then the third eluting solution is adopted to leach the second separation column, the flow rates of the first eluting solution and the third eluting solution are 1-5 mL/min, and the specific operation is that the pipelines at the lower ends of the plug valves V1-V5 are respectively connected with the pipelines A1-A5 corresponding to the pipelines, so that all the plug valves return to the initial state, namely the closed state. Then, the plug valve A1 is opened, so that the first eluent enters the first separation column C1 through the plug valve V1, the first liquid inlet pump P1 and the plug valve V7, the solution is discharged through the plug valve V8 and is collected in the pipeline A16 for receiving the non-radioactive waste liquid, and the first liquid inlet pump P1 is kept in an open state until the volume of the first eluent flowing through the first separation column C1 is greater than or equal to five times the volume of the first separation column C1. Then all the plug valves are closed, then the plug valve A3 is opened, the third eluent enters the second separation column C2 through the plug valve V3, the first liquid inlet pump P1 and the plug valve V9, the solution is discharged through the plug valve V10 and is collected in a pipeline A16 for receiving the non-radioactive waste liquid, and the first liquid inlet pump P1 is kept in an open state until the volume of the third eluent flowing through the second separation column C2 is greater than or equal to five times the volume of the second separation column C2. After completion, all plug valves are closed.
It should be noted that, the plug valve V5 and the corresponding pipeline thereof are a standby pipeline, that is, when some other pipeline fails, a corresponding solution can be injected into the pipeline to replace the corresponding pipeline. However, the backup line is not necessary, and whether or not and the number of backup lines are set can be freely set according to the experimental requirements.
Finally, it should be noted that: the above embodiments are only for illustrating the technical aspects of the present application and not for limiting the same, and although the present application has been described in detail with reference to the above embodiments, it should be understood by those of ordinary skill in the art that: modifications and equivalents may be made to the specific embodiments of the application without departing from the spirit and scope of the application, which is intended to be covered by the claims. The foregoing is merely illustrative of the present application, and the present application is not limited thereto, and any person skilled in the art will readily appreciate variations or alternatives within the scope of the present application. Therefore, the protection scope of the application is subject to the protection scope of the claims.

Claims (7)

1. An automated processing system for separating Ac-225, comprising: the device comprises a leaching liquid inlet module, a material liquid inlet module, a first liquid inlet pump, a second liquid inlet pump, a separation column module, a recovery part, a plug valve module and a control module;
the leaching solution inlet module is connected with the first liquid inlet pump, the liquid inlet module is connected with the second liquid inlet pump, the first liquid inlet pump and the second liquid inlet pump are connected with the separation column module through the plug valve module, the separation column module is connected with the recovery part through the plug valve module, the solution containing Ac-225 is collected in the recovery part, and the control module is connected with the first liquid inlet pump, the second liquid inlet pump and the plug valve module and is used for selecting the solution entering the separation column module and the recovery part;
the automated treatment system further comprises a waste liquid module connected with the recovery part through a third plug valve assembly in the plug valve module, wherein the waste liquid module can separate high-radioactivity, low-radioactivity and non-radioactivity waste liquid;
the waste liquid module comprises a pipeline for receiving Ra-223 byproducts, a pipeline for receiving La+Ce components, a pipeline for receiving high-radioactivity waste liquid, a pipeline for receiving low-radioactivity waste liquid and a pipeline for receiving non-radioactivity waste liquid;
the separation column module comprises two separation columns, the two separation columns are connected together through a second plug valve component in the plug valve module, wherein the first separation column is a cation column, the second separation column is a DGA resin column, the inlet end and the outlet end of the first separation column are connected with a plug valve, the inlet end and the outlet end of the second separation column are connected with a plug valve, if the plug valve of the inlet end of the first separation column or the inlet end of the second separation column is opened, the first separation column or the second separation column is independently started, the first separation column and the second separation column are connected in parallel, and if the plug valves of the inlet end, the outlet end and the inlet end of the second separation column are simultaneously opened, the first separation column and the second separation column are connected in series.
2. The automated Ac-225 separation processing system of claim 1, wherein the rinse liquid feed module comprises a deionized water line, a first rinse liquid line, a second rinse liquid line, a third rinse liquid line, and a fourth rinse liquid line, each rinse liquid line being connected to the first feed pump by a first plug valve assembly in a plug valve module, the first plug valve assembly comprising a plurality of T-shaped three-way plug valves.
3. The automated Ac-225 separation processing system of claim 2, wherein a plurality of said three-way stopcocks are each disposed on a main pipeline, wherein an interface of said three-way stopcock perpendicular to said main pipeline connects a corresponding pipeline of said eluent feed module, wherein said three-way stopcock is configured to communicate with a corresponding pipeline of said eluent feed module when said three-way stopcock is open and to connect said main pipeline when said three-way stopcock is closed.
4. The automated Ac-225 separation treatment system of claim 2, wherein said first leacheate is an ammonium sulfate solution having a concentration of 0.3 to 0.6mol/L, said second leacheate is a nitric acid solution having a concentration of 0.01 to 0.1mol/L, said third leacheate is a nitric acid solution having a concentration of 4 to 6mol/L, and said fourth leacheate is a nitric acid solution having a concentration of 9 to 13 mol/L.
5. The automated Ac-225 separation processing system of any one of claims 1-4, wherein said feed solution is a solution of a Th target subjected to proton irradiation, comprising: th with concentration of 0.01-0.1 mol/L 4+ Ammonium sulfate solution with concentration of 0.4-0.6 mol/L and solution of nuclear reaction product of the Th target irradiated by proton beam.
6. A method of operating an automated processing system for separating Ac-225 employing the automated processing system for separating Ac-225 of any one of claims 1-5, comprising the steps of:
s1, introducing ionized water to remove pipeline air;
s2, introducing the feed liquid into a pretreated first separation column, and introducing the solution flowing out of the first separation column into a pipeline for receiving high-radioactivity waste liquid for collection;
s3, eluting the first separation column by adopting a first eluting solution, and introducing the solution flowing out of the first separation column into a pipeline for receiving the high-radioactivity waste liquid for collection;
s4, leaching the first separation column by using a second leaching solution, and introducing the solution flowing out of the first separation column into a pipeline for receiving the low-radioactivity waste liquid for collection;
s5, sequentially and continuously eluting the first separation column and the pretreated second separation column by adopting a third eluent, and introducing the solution flowing out of the second separation column into a pipeline for receiving Ra-223 byproducts for collection;
s6, leaching the second separation column by using a fourth leaching solution, and introducing the solution flowing out of the second separation column into a recovery part for recovery;
s7, eluting the second separation column by deionized water, and introducing the solution flowing out of the second separation column into a pipeline for receiving the La+Ce component.
7. The method of operating an automated processing system for separating Ac-225 of claim 6, wherein the pretreatment process of the first separation column and the second separation column is: the first separation column is leached by the first leaching solution, the second separation column is leached by the third leaching solution, the flow rates of the first leaching solution and the third leaching solution are 1-5 mL/min, and the volumes of the first leaching solution and the third leaching solution are 5 times or more than 5 times of the volumes of the first separation column and the second separation column respectively.
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