CN116864178A - Carrier-free lutetium-177 solution preparation system and method - Google Patents
Carrier-free lutetium-177 solution preparation system and method Download PDFInfo
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- CN116864178A CN116864178A CN202310890778.3A CN202310890778A CN116864178A CN 116864178 A CN116864178 A CN 116864178A CN 202310890778 A CN202310890778 A CN 202310890778A CN 116864178 A CN116864178 A CN 116864178A
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- OHSVLFRHMCKCQY-NJFSPNSNSA-N lutetium-177 Chemical compound [177Lu] OHSVLFRHMCKCQY-NJFSPNSNSA-N 0.000 title claims abstract description 94
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- 229920005989 resin Polymers 0.000 claims abstract description 20
- NAWDYIZEMPQZHO-AKLPVKDBSA-N ytterbium-176 Chemical compound [176Yb] NAWDYIZEMPQZHO-AKLPVKDBSA-N 0.000 claims abstract description 12
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- 229910052765 Lutetium Inorganic materials 0.000 claims description 19
- 229910052769 Ytterbium Inorganic materials 0.000 claims description 19
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- NAWDYIZEMPQZHO-NJFSPNSNSA-N ytterbium-175 Chemical compound [175Yb] NAWDYIZEMPQZHO-NJFSPNSNSA-N 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
- G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
- G21G1/001—Recovery of specific isotopes from irradiated targets
Abstract
The application discloses a system and a method for preparing a solution of lutetium-177 without a carrier, belonging to the technical field of radionuclide separation. The preparation system comprises: the device comprises a radioactive shielding box body, a target material processing device, a ytterbium lutetium separation device and a radioactivity detection device; the ytterbium lutetium separation device comprises a multi-stage continuous separation unit, wherein a first-stage separation column is filled with phosphate extraction resin, and a second-stage separation column is filled with DGA resin; the liquid inlet of each stage of separation column is connected with an inorganic acid leaching solution storage tank, and the liquid outlet of each stage of separation column is respectively connected with a waste liquid tank and a lutetium-177 solution collecting bottle. The preparation system of the carrier-free lutetium-177 solution provided by the application has the advantages of reasonable structure, simplicity in operation, convenience in use, stable performance, low cost and higher degree of automation, and can be used for efficiently and safely completing the discharge treatment of the ytterbium-176 target after irradiation to obtain the carrier-free lutetium-177 solution. The preparation method has strong operability and good separation effect.
Description
Technical Field
The application relates to the technical field of radionuclide separation, in particular to a system and a method for preparing a solution of unsupported lutetium-177.
Background
The carrier-free lutetium-177 is a medical radionuclide which is of great interest and can be used for diagnosing and treating partial cancers, such as prostate cancer, neuroendocrine tumor and the like. Existing technology 177 Lu-DOTATATE、 177 Two radiopharmaceuticals of Lu-PSMA-617 are used commercially in europe and the united states. The excellent use effect of the carrier-free lutetium-177 nuclide makes the carrier-free lutetium-177 nuclide become a therapeutic nuclide which is most concerned in recent years and has been rapidly increased in clinical application.
The carrier-free lutetium-177 is an important raw material of lutetium-177 radiopharmaceuticals, and is generated by enriching ytterbium-176 through reactor irradiation, but the target material enriched ytterbium-176 and the product lutetium-177 are subjected to radiochemical separation after generation to obtain the carrier-free lutetium-177 meeting the use requirements.
Currently, the production of unsupported lutetium-177 has mainly the following problems: 1. the large-scale production needs to process lutetium-177 above dozens of curies at a time, and the device needs to be operated by a manipulator or an automatic device, and comprises target material treatment, material transfer, release separation and the like; 2. the ytterbium lutetium separation process needs to carry out multistage separation and purification, and the common method is that a radioactive detector is arranged on each separation column to monitor the radioactivity intensity, so that the device has complex composition and high probability of failure due to the large number of the detectors; 3. the effluent liquid of each column is collected in a liquid storage tank system in the separation process and then is sampled to the next separation column through a pump, and the process is complex and long in time consumption. Therefore, there is a need for a carrier-free lutetium-177 production system and method that is simple to operate, can be continuously sampled, and can detect all separation processes with a single detector.
Disclosure of Invention
The application aims to provide a system and a method for preparing a solution of unsupported lutetium-177, which are used for solving the problems of complex separation operation and long time consumption of the existing unsupported lutetium-177.
The technical scheme for solving the technical problems is as follows:
the application provides a carrier-free lutetium-177 solution preparation system, which comprises:
a radiation shielding housing;
the target material treatment device is arranged in the radioactive shielding box body and is used for disassembling a quartz tube filled with target materials, heating and dissolving the target materials and separating lutetium-177 feed liquid;
the ytterbium and lutetium separation device is arranged in the radioactive shielding box body and is used for separating ytterbium and lutetium from lutetium-177 feed liquid to obtain carrier-free lutetium-177 solution;
the ytterbium lutetium separating device comprises a multi-stage continuous separating unit, the separating unit comprises: the first-stage separation column and the second-stage separation column are sequentially connected end to end; the first-stage separation column is filled with phosphate extraction resin, and the second-stage separation column is filled with DGA resin;
the liquid inlet of each stage of separation column is connected with an inorganic acid leaching solution storage tank, and the liquid outlet of each stage of separation column is respectively connected with a waste liquid tank and a lutetium-177 solution collecting bottle; and
the radioactivity detection device is connected with the liquid outlet pipeline of each stage of separation column and is used for detecting the radioactivity intensity of the liquid outlet of each stage of separation column.
Further, in the carrier-free lutetium-177 solution preparation system, the number of the radioactive shielding boxes is at least 2, the target material processing device and the ytterbium lutetium separating device are respectively arranged in different radioactive shielding boxes, and the target material processing device and the ytterbium lutetium separating device are communicated through a pump pipe.
Further, in the unsupported lutetium-177 solution preparation system, the target processing device comprises: the quartz tube cleaning tank is used for cleaning a quartz tube filled with target materials; the target material treatment tank is used for smashing and disintegrating a quartz tube filled with target materials, heating and dissolving the target materials, and obtaining lutetium-177 feed liquid;
preferably, the target processing device further comprises a steam condensing sleeve connected to the target processing device for collecting and heating to dissolve to generate acid steam.
Further, in the carrier-free lutetium-177 solution preparation system, the carrier-free lutetium-177 solution preparation system further comprises a transportation trolley, and the transportation trolley is arranged at the back of the radioactive shielding box body.
Further, in the unsupported lutetium-177 solution preparation system, the number of inorganic acid leaching solution storage tanks is at least 4;
preferably, the number of the inorganic acid leaching solution storage tanks is 4, and the inorganic acid leaching solution storage tanks respectively store 0.05 to 0.1mol/L HCl and 0.05 to 0.1mol/L HNO 3 、1.0～2.0mol/L HNO 3 、3.0～5.0mol/L HNO 3 ；
Preferably, 1.0 to 2.0mol/L HNO is stored 3 The temperature of the leaching solution is between room temperature and 80 ℃;
further, in the unsupported lutetium-177 solution preparation system, the size of the second stage separation column in the separation unit is smaller than the size of the first stage separation column;
preferably, the size of the separation column is determined by the required mass of the ytterbium-176 target material to be separated, and the mass of the resin filled in the separation column is not less than 200% of the required adsorption capacity for ytterbium-176 separation;
preferably, the ytterbium lutetium separation device at least comprises three separation units, and the sizes of the separation columns in the separation units are sequentially reduced;
preferably, the ytterbium lutetium separation device comprises three separation units, and the sizes of the separation columns in the ytterbium lutetium separation device are as follows: phi 30 multiplied by 1000mm and phi 30 multiplied by 150mm; phi 30 x 500mm and phi 20 x 100mm; phi 10 multiplied by 500mm and phi 10 multiplied by 40mm;
preferably, each stage of separation column is respectively connected with a plunger pump for conveying liquid, and the flow rate of the plunger pump is 0-200 mL/min;
preferably, the ytterbium lutetium separating device is made of PP or PEEK nonmetallic materials.
The application also provides a method of a carrier-free lutetium-177 solution preparation system, comprising:
conveying the irradiated quartz tube filled with the target material into a radioactive shielding box, cleaning, decomposing, heating and dissolving the target material to obtain lutetium-177 feed liquid;
adopts HNO of 0.05 to 0.1mol/L 3 Eluting a first-stage separation column in the separation unit by 3.0-5.0 mol/L HNO 3 Eluting a second separation column in the separation unit to complete pretreatment of the separation column;
loading lutetium-177 feed liquid into a first-stage separation column in a separation unit, and adopting 1.0-2.0 mol/L HNO with the temperature of 40-50 DEG C 3 Eluting, conveying effluent liquid to a waste liquid tank for collection, and monitoring the change of the radioactivity intensity in the eluting process;
when the radioactivity intensity is 'low to high to low to high', 3.0-5.0 mol/L HNO is used instead 3 Eluting the first-stage separation column, conveying effluent to a second-stage separation column in a separation unit, and monitoring the change of the radioactivity intensity in the eluting process;
the radioactive intensity is rapidly increased and rapidly reduced, and 3.0-5.0 mol/L HNO of the first-stage separation column is stopped when the decrease is slow 3 Leaching, adopting HNO with the concentration of 0.05-0.1 mol/L 3 Eluting the second-stage separation column by 1-3 times of column volume, then delivering the effluent to a waste liquid tank for collection, eluting the second-stage separation column in the separation unit by adopting 0.05-0.1 mol/L HCl, delivering the effluent to the first-stage separation column in the next separation unit, and simultaneously monitoring the change of the radioactivity intensity in the eluting process;
the radioactive intensity is rapidly increased and rapidly reduced, and when the reduction is slow, the radioactive intensity stops 0.05 to 0.1mol/L HNO of the second-stage separation column in the separation unit 3 Leaching;
and the next separation unit is sequentially leached according to the previous steps, and the separation process is repeated for a plurality of times, so as to finish ytterbium lutetium separation.
Further, in the preparation method of the carrier-free lutetium-177 solution, the step of heating and dissolving the target material is as follows: adding 1-4 mol/L hydrochloric acid or nitric acid solution, heating to 80-100 ℃ to dissolve target material.
Further, in the preparation method of the unsupported lutetium-177 solutionAfter the ytterbium and lutetium are separated, 0.05 to 0.1mol/L HNO is adopted 3 Eluting a first-stage separation column in the separation unit by adopting 3.0-5.0 mol/LHNO 3 The second stage separation column in the separation unit is rinsed.
Further, in the preparation method of the carrier-free lutetium-177 solution, the separation process of the next separation unit is sequentially carried out twice repeated leaching.
The application has the following beneficial effects:
1. the preparation system of the carrier-free lutetium-177 solution provided by the application has the advantages of reasonable structure, simplicity in operation, convenience in use, stable performance, low cost and higher degree of automation, and can be used for efficiently and safely completing the discharge treatment of the ytterbium-176 target after irradiation to obtain the carrier-free lutetium-177 solution. The preparation method has strong operability and good separation effect.
2. The carrier-free lutetium-177 solution preparation system provided by the application has the advantages that the structural design is simple, the operation is easy, the pretreatment operation of high-radioactivity targets such as target tube transportation, cleaning and dissolution is realized, the pretreatment can be completed without complex electrical equipment, and the equipment failure rate is obviously reduced. The ytterbium lutetium separation process adopts a multi-stage separation process, the process of multi-stage separation is judged by intensively monitoring the radioactive change condition of a plurality of pipelines, and the process flow of a separation device system is switched back by the result of radioactive detection, so that the aim of obtaining a high-purity carrier-free lutetium-177 solution product by the process treatment of a sample to be separated through the device is fulfilled, the seamless switching between the separation processes at all stages greatly shortens the time required by the process, and the production efficiency is improved.
3. The ytterbium lutetium separating device provided by the application adopts a simplified pump and valve design, so that the purpose of continuous sample loading and separation is achieved. The operation of a plurality of separation column flows is completed by one pump through different valve combinations, the types and the specifications of the valves are consistent, and the difficulty for maintenance and replacement of the later-stage valves, pipelines and the like is reduced. According to the application, phosphate extraction resin is adopted to separate ytterbium and lutetium, and DGA resin is adopted to convert high acidity solution into low acidity solution, so that the purposes of high-efficiency separation of ytterbium and lutetium and continuous separation of a plurality of columns are realized, and the degree of automation of the device is improved.
4. The radioactivity detection device provided by the application adopts the centralized collection of multiple pipelines, achieves the effect of detecting the change condition of the radioactivity intensity of the multiple pipelines by using only 1 detector, and performs radioactivity detection on all column liquid outlet pipelines by using a radioactivity detection system, so that operators can know the ytterbium-lutetium separation process in real time, and perform operations such as separation flow selection, switching and the like according to the result.
5. The device and the method for preparing the carrier-free lutetium-177 solution have the advantages of simple structural design and easy operation, realize pretreatment operation of high-radioactivity targets such as target tube transportation, cleaning and dissolution, can be completed without complex electrical equipment, and remarkably reduce equipment failure rate. The ytterbium lutetium separation process adopts a multi-stage separation process, the process of multi-stage separation is judged by intensively monitoring the radioactive change condition of a plurality of pipelines, and the process flow of a separation device system is switched back by the result of radioactive detection, so that the aim of obtaining a high-purity carrier-free lutetium-177 solution product by the process treatment of a sample to be separated through the device is fulfilled, the seamless switching between the separation processes at all stages greatly shortens the time required by the process, and the production efficiency is improved.
6. By adopting the device and the method for preparing the solution of the unsupported lutetium-177, the process time required by preparing the unsupported lutetium-177 is obviously shortened. The specific shortening time is mainly expressed in that: 1) Column 1, 4mol/L HNO 3 And in the leaching process, the solution is leached out and collected, the collected solution is treated by evaporation concentration, dilution or a solid phase extraction column to obtain a solution which can be separated for the second time, and the solution is loaded on a second-stage separation column (a No. 3 column described in an example). In practice, the evaporative concentration and dilution methods are not preferable because the evaporative concentration is time consuming, and the dilution method will produce about 40 times of waste liquid, which is not suitable for efficient production. The solid phase extraction column is transformed to obtain solution, and then the solution is put on the column to No. 3, so that the process time is obviously doubled; 2) The design for concentrated detection of radioactivity change by using the multi-flow path of the application can eliminate the need of adjusting the radioactivity detector, and the conventional technology is to align the radioactivity detector with a single oneOnly the bottom of the separation column is detected, and only the position of the detector can be moved or a radioactive detector is arranged in each flow path of different column flows when the detection is carried out. Clearly, moving the detector position is a difficult way to operate and tends to require a significant amount of time to achieve. The arrangement of one detector in each flow path has the defects of too large investment, extremely limited space in the box body and difficult maintenance and repair caused by further compressing the space for use by too many detectors.
Drawings
The accompanying drawings, which are included to provide a further understanding of embodiments of the application and are incorporated in and constitute a part of this specification, illustrate embodiments of the application and together with the description serve to explain the principles of the application. In the drawings:
FIG. 1 is a schematic diagram of the structure of a carrier-free lutetium-177 solution preparation system of the present application.
In the drawings, the reference numerals and corresponding part names:
in the figure: 11-1, 12-2, 2-target processing device, 21-quartz tube cleaning tank, 22-target processing tank, 3-ytterbium lutetium separating device, 31-separating unit, 311-1, 312-2, 313-3, 314-4, 315-5, 316-6, 32-inorganic acid leaching solution storage tank, 33-waste liquid tank, 34-lutetium-177 solution collecting bottle, 4-radioactivity detecting device and 5-transportation trolley.
Detailed Description
For the purpose of making the objects, technical solutions and advantages of the embodiments of the present application more apparent, the technical solutions of the embodiments of the present application will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present application, and it is apparent that the described embodiments are some embodiments of the present application, but not all embodiments of the present application. The components of the embodiments of the present application generally described and illustrated in the figures herein may be arranged and designed in a wide variety of different configurations.
Thus, the following detailed description of the embodiments of the application, as presented in the figures, is not intended to limit the scope of the application, as claimed, but is merely representative of selected embodiments of the application. All other embodiments, which can be made by those skilled in the art based on the embodiments of the application without making any inventive effort, are intended to be within the scope of the application.
The technical scheme of the application is as follows:
a carrier-free lutetium-177 solution preparation system comprising:
the radioactive shielding box body 1 is used for installing a placing device and providing shielding capacity with the lead equivalent thickness being more than or equal to 20mm, and reduces the irradiation of radioactive ray dose to operators. The tank has a waste liquid tank for discharging radioactive waste liquid to a waste liquid pipe.
The target material treatment device 2 is arranged in the radioactive shielding box body and used for smashing and disintegrating a quartz tube filled with target materials, heating and dissolving the target materials and separating lutetium-177 feed liquid; the target material treatment device aims to realize the functions of cleaning, disassembling and target material dissolving of the quartz tube.
The ytterbium and lutetium separation device 3 is arranged in the radioactive shielding box body 1 and is used for separating ytterbium and lutetium from lutetium-177 feed liquid to obtain carrier-free lutetium-177 solution;
ytterbium lutetium separating device 3 includes a multi-stage continuous separating unit 31, separating unit 31 includes: the first-stage separation column and the second-stage separation column are sequentially connected end to end; the first-stage separation column is filled with phosphate extraction resin, and the second-stage separation column is filled with DGA resin;
the liquid inlet of each stage of separation column is connected with an inorganic acid leaching solution storage tank 32, and the liquid outlet of each stage of separation column is respectively connected with a waste liquid tank 33 and a lutetium-177 solution collecting bottle 34; and
and the radioactivity detection device 4 is connected with the liquid outlet pipeline of each stage of separation column and is used for detecting the radioactivity intensity of the liquid outlet of each stage of separation column.
According to the carrier-free lutetium-177 solution preparation system provided by the application, a quartz tube filled with target materials is cleaned, disintegrated and heated and dissolved through a target material treatment device to obtain lutetium-177 feed liquid for ytterbium-lutetium separation, and the ytterbium-lutetium separation device completes the ytterbium-lutetium separation through a multistage column separation process to obtain the carrier-free lutetium-177 solution. In the ytterbium and lutetium separation process, all separation column liquid outlet pipelines are subjected to radioactivity detection through a radioactivity detection device, so that operators can know the ytterbium and lutetium separation process in real time, and operations such as separation flow selection, switching and the like can be performed according to the result.
The carrier-free lutetium-177 solution preparation system provided by the application has the advantages that the structural design is simple, the operation is easy, the pretreatment operation of high-radioactivity targets such as target tube transportation, cleaning and dissolution is realized, the pretreatment can be completed without complex electrical equipment, and the equipment failure rate is obviously reduced. The ytterbium lutetium separation process adopts a multi-stage separation process, the process of multi-stage separation is judged by intensively monitoring the radioactive change condition of a plurality of pipelines, and the process flow of a separation device system is switched back by the result of radioactive detection, so that the aim of obtaining a high-purity carrier-free lutetium-177 solution product by the process treatment of a sample to be separated through the device is fulfilled, the seamless switching between the separation processes at all stages greatly shortens the time required by the process, and the production efficiency is improved.
The whole preparation system has reasonable structure, simple operation, convenient use, stable performance, low cost and higher degree of automation. The whole preparation method has strong operability and good separation effect.
Further, the number of the radioactive shielding boxes is at least 2, and the target material processing device and the ytterbium-lutetium separating device are respectively arranged in different radioactive shielding boxes and are communicated through a pump pipe. Further, the number of the radioactive shielding boxes is preferably 2, namely, a 1-radioactive shielding box 11 and a 2-radioactive shielding box 12, and through holes are arranged between the adjacent boxes for installing solution pipelines, signal or power wires and the like. The target material processing device is arranged in a No. 1 radioactive shielding box, the radioactive shielding box and the radioactive detection device are arranged in a No. 2 radioactive shielding box, lutetium-177 feed liquid is conveyed from the No. 1 radioactive shielding box to a ytterbium-lutetium separation device in the No. 2 radioactive shielding box through a pump pipe by utilizing a through hole between the No. 1 and No. 2 boxes, and loading is completed.
Further, the target material processing apparatus 2 includes: a quartz tube cleaning tank 21 for cleaning a quartz tube containing a target material; and a target material treatment tank 22 for crushing and disintegrating the quartz tube containing the target material, heating and dissolving the target material, and separating lutetium-177 feed liquid. The quartz tube is cleaned, the inner target barrel used for quartz tube transfer is combined, the purpose of sharing the transfer target barrel with the inner cleaning barrel is achieved, the cleaning process is simple, the cleaning tank is simple in design, and the operation steps are reduced. The dissolution tank is shared by disintegration and dissolution, and the process is simple and practical.
Still further preferably, the target processing apparatus further comprises a steam condensing assembly coupled to the target processing apparatus for collecting heated dissolved acid vapors. The steam condensation collection suite is additionally arranged in the dissolution process, so that corrosion and pollution of acid liquor and radioactive aerosol to the box body and other equipment are avoided, and the safety and cleanness of the use environment of the device are ensured.
Further, the carrier-free lutetium-177 solution preparation system further comprises a transportation trolley, wherein the transportation trolley is arranged at the back of the radioactive shielding box body. A trolley conveying track is arranged on the back surface of the radioactive shielding box body, and material transmission between the box bodies can be realized through the conveying trolley.
Still more preferably, the inorganic acid leaching solution is stored in inorganic acid leaching solution storage tanks, and the number of the inorganic acid leaching solution storage tanks is at least 4;
still more preferably, the number of inorganic acid leaching solution storage tanks is 4, and the inorganic acid leaching solution storage tanks respectively store 0.05 to 0.1mol/L HCl and 0.05 to 0.1mol/L HNO 3 、1.0～2.0mol/L HNO 3 、3.0～5.0mol/L HNO 3 ；
Still more preferably, 1.0 to 2.0mol/L HNO is stored 3 The temperature of the leaching solution is between room temperature and 80 ℃;
further, the size of the second stage separation column in the separation unit is smaller than the size of the first stage separation column;
still more preferably, the size of the separation column is determined by the required mass of ytterbium-176 target material to be separated, and the mass of resin filled in the separation column is not less than 200% of the required adsorption capacity for ytterbium-176 separation;
still more preferably, the ytterbium lutetium separation device comprises at least three separation units, and the sizes of the separation columns in the separation units are sequentially reduced;
still further preferably, the ytterbium lutetium separation device comprises three separation units, and the size of the separation column in the ytterbium lutetium separation device is in turn: phi 30 multiplied by 1000mm and phi 30 multiplied by 150mm; phi 30 x 500mm and phi 20 x 100mm; phi 10 multiplied by 500mm and phi 10 multiplied by 40mm;
still more preferably, each stage of separation column is respectively connected with a plunger pump for conveying liquid, and the flow rate of the plunger pump is 0-200 mL/min;
still more preferably, the ytterbium lutetium separation device is made of PP or PEEK nonmetallic material. The plunger pump, the multi-way valve, the separation column, the solution storage tank, the corresponding pipelines and the like in the ytterbium lutetium separation device are all made of non-metal materials such as PP or PEEK and the like.
In addition, the carrier-free lutetium-177 solution preparation system also comprises a control system, and a pump and a valve in the preparation system can be manually or automatically controlled by a PLC control system of an upper computer to remotely control the ytterbium-lutetium separation process in the box body.
A method for preparing a solution of unsupported lutetium-177 comprising:
conveying the irradiated quartz tube filled with the target material into a radioactive shielding box, cleaning, crushing, disintegrating, heating and dissolving the target material, and separating lutetium-177 feed liquid;
adopts HNO of 0.05 to 0.1mol/L 3 Eluting a first-stage separation column in the separation unit by 3.0-5.0 mol/L HNO 3 Eluting a second separation column in the separation unit to complete pretreatment of the separation column;
loading lutetium-177 feed liquid into a first-stage separation column in a separation unit, and adopting 1.0-2.0 mol/L HNO with the temperature of 40-50 DEG C 3 Eluting, conveying effluent liquid to a waste liquid tank for collection, and monitoring the change of the radioactivity intensity in the eluting process;
when the radioactivity intensity is 'low to high to low to high', 3.0-5.0 mol/L HNO is used instead 3 Eluting the first-stage separation column, conveying effluent to the second-stage separation column, and monitoring the change of the radioactivity intensity in the eluting process;
the radioactive intensity is rapidly increased and rapidly reduced, and 3.0-5.0 mol/L HNO of the first-stage separation column is stopped when the decrease is slow 3 Leaching with 0.05-0.1 mol/L HNO 3 Eluting the second-stage separation column by 1-3 times of column volume, then delivering the effluent to a waste liquid tank for collection, eluting the second-stage separation column by adopting 0.05-0.1 mol/L HCl, delivering the effluent to a first-stage separation column in a next separation unit, and simultaneously monitoring the change of radioactivity intensity in the eluting process;
the radioactive intensity is rapidly increased and rapidly reduced, and when the reduction is slow, the operation of the second-stage separation column is stopped at 0.05-0.1 mol/L HNO 3 The leaching is carried out,
and the next separation unit is sequentially leached according to the previous steps, and the separation process is repeated for a plurality of times, so as to finish ytterbium lutetium separation.
Further, the step of heating and dissolving the target material is as follows: adding 1-4 mol/L hydrochloric acid or nitric acid solution, heating to 80-100 ℃ to dissolve target material.
Further, after the separation of ytterbium and lutetium is completed, 0.05 to 0.1mol/L HNO is adopted 3 Eluting a first-stage separation column in the separation unit by 3.0-5.0 mol/L HNO 3 The second stage separation column in the separation unit is rinsed.
Further, the next separation unit separation process is sequentially carried out twice repeated leaching.
For further explanation of the present application, the carrier-free lutetium-177 solution preparation system and method provided by the present application are described below with reference to examples, but it should be understood that these examples are implemented on the premise of the technical solution of the present application, and detailed implementation and specific operation procedures are given only for further explanation of the features and advantages of the present application, and not limitation of the claims of the present application, and the scope of protection of the present application is not limited to the examples described below.
Example 1
Referring to fig. 1, a carrier-free lutetium-177 solution preparation system provided in an embodiment of the application includes: a radioactive shielding box body 1, a target material processing device 2, a ytterbium lutetium separating device 3 and a radioactive detection device 4.
The number of the radioactive shielding boxes 1 is two, namely a number 1 radioactive shielding box 11 and a number 2 radioactive shielding box 12. The thickness of the box body is more than or equal to 20mm lead equivalent, and a plurality of through holes for pipeline arrangement are arranged between two adjacent box bodies. The size of the shielding box is as follows: two lead glass peeping windows with the size of 500X 600mm are prepared on the front face, wherein the width is 2500X 1500X 1800mm, the depth is 1500X 1800mm, the clamping force is more than or equal to 7kg, and 2 joints are matched with the mechanical arm. 1 waste disposal duct and floor drain are provided, the dimension phi is 150mm. The trolley conveying track is arranged on the back of the radioactive shielding box, and the conveying trolley 5 and the track are parallel to the back of the box body and can stay at the position of the trolley door of the box body, so that the purpose of conveying materials between the box bodies is realized.
The target material treatment device 2 is arranged on a No. 1 radioactive shielding box 11, and a quartz tube filled with target material in the No. 1 box body is cleaned, disintegrated and heated by the target material treatment device to be dissolved, so that lutetium-177 feed liquid for ytterbium and lutetium separation is obtained.
The target material processing apparatus 2 includes: a quartz tube cleaning tank 21 for cleaning a quartz tube containing a target material; and a target material treatment tank 22 for crushing and disintegrating the quartz tube containing the target material, heating and dissolving the target material, and separating lutetium-177 feed liquid.
The quartz tube cleaning tank 21 comprises an outer tank and an inner tank which are made of polytetrafluoroethylene, wherein the outer tank is provided with a liquid inlet, and cleaning solution is added by a peristaltic pump, and is generally deionized water or dilute nitric acid; the bottom of the outer barrel is provided with a liquid outlet which is connected with the waste liquid tank through a liquid discharge pipe and is discharged into a waste liquid sewer pipe. The bottom of the inner barrel is provided with a plurality of round holes or slits for discharging liquid, the size of the inner barrel is matched with a transfer device for containing quartz tubes, and the quartz tubes are contained by the container after the reactor is piled out, the target is cut and the quartz tubes are taken out to be used as the quartz tube transfer inner barrel. The structural design can reduce the operation procedure of the quartz tube and simplify the pretreatment flow.
The target material treatment tank 22 consists of a polytetrafluoroethylene barrel, a polytetrafluoroethylene hammer and a heater, the barrel wall is provided with a liquid adding port which is connected with a liquid adding pipe and can be used for adding dissolving liquid into the barrel, and the dissolving liquid is generally 1-4 mol/L HNO 3 Or HCl; the polytetrafluoroethylene hammer is a solid cylinder, and a hook is arranged at the top of the polytetrafluoroethylene hammer for controlling the lifting of the hammer, so that the aim of disassembling the quartz tube is fulfilled. The heater is a platform heating plate, the heating temperature is adjustable within the range of room temperature to 300 ℃, and the heating table is welded with oneAnd the stainless steel or aluminum barrel rack is used for fixing the polytetrafluoroethylene barrel and preventing the polytetrafluoroethylene barrel from toppling.
The target processing device 2 further comprises a steam condensing sleeve connected to the target processing device for collecting and heating to dissolve to generate acid steam. The steam condensing external member mainly comprises a round cover with an air suction hole, a polytetrafluoroethylene air suction pipe, a glass condensing pipe, a Monte gas washing bottle and the like, so that the collection of acid steam generated by heating and dissolving is realized, and the acid steam is prevented from greatly drifting in a box body to corrode the box body and other articles. The steam condensation collection suite is additionally arranged in the dissolution process, so that corrosion and pollution of acid liquor and radioactive aerosol to the box body and other equipment are avoided, and the safety and cleanness of the use environment of the device are ensured.
And taking down the transferring inner barrel provided with the quartz target tube from the transportation trolley by using a mechanical arm, putting the inner barrel into a quartz tube cleaning tank, adding cleaning solution into the quartz tube cleaning tank, and discharging the cleaning solution after the quartz tube is soaked. And lifting the inner barrel provided with the quartz target tube from the quartz tube cleaning tank, and clamping and transferring the quartz tube into the target material processing tank by a mechanical arm. After the quartz tube is transferred, the hammer is operated by a manipulator to smash and disintegrate the quartz target tube in the barrel, and the hammer is removed after repeated smashing for 5-10 times. The dissolution is then carried out by heating and the vapors are collected by condensing means. After dissolution is completed, a liquid suction pipeline with a filter is inserted into the bottom of the target material treatment tank. And finishing the pretreatment of the target material and the target material treatment flow.
The ytterbium lutetium separating device 3 is arranged in the No. 2 radioactive shielding box 12, and lutetium-177 feed liquid is conveyed from the No. 1 box to the ytterbium lutetium separating device in the No. 2 box through a pump pipe by utilizing a through hole between the No. 1 box and the No. 2 box, so that sample loading is completed. And (3) pressurizing a solution obtained by dissolving the target material in a target material treatment tank in the No. 1 radioactive shielding box by a pump, entering the No. 2 box from the No. 1 box, loading the solution into a ytterbium and lutetium separating device 3, and separating ytterbium and lutetium from lutetium-177 feed liquid to obtain a carrier-free lutetium-177 solution.
The ytterbium lutetium separating device comprises a multi-stage continuous separating unit, and the separating unit 31 comprises: the first-stage separation column and the second-stage separation column are sequentially connected end to end; the first-stage separation column is filled with phosphate extraction resin, and the second-stage separation column is filled with DGA resin; the liquid inlet of each stage of separation column is connected with an inorganic acid leaching solution storage tank 32, and the liquid outlet of each stage of separation column is respectively connected with a waste liquid tank 33 and a lutetium-177 solution collecting bottle 34.
In this embodiment, the separation unit has 3 sets of 6 separation columns, which are sequentially designated column 1, column 2, column 312, column 3, column 4, column 314, column 5, column 315, and column 6, 316. The size of the No. 1 column is phi 30 multiplied by 1000mm, the size of the No. 2 column is phi 30 multiplied by 150mm, the size of the No. 3 column is phi 30 multiplied by 500mm, the size of the No. 4 column is phi 20 multiplied by 100mm, the size of the No. 5 column is phi 10 multiplied by 500mm, and the size of the No. 6 column is phi 10 multiplied by 40mm. The separating column is made of non-metal materials such as PP or PEEK, wherein 3 separating columns 1, 3 and 5 are filled with phosphate extraction resin such as LN and LN2, and 3 separating columns 2, 4 and 6 are filled with DGA resin. The size of the separation column is determined according to the required quality of the ytterbium-176 target material to be separated, and the quality of the resin is not less than 200% of the required adsorption capacity for ytterbium-176 separation.
The ytterbium lutetium separating device comprises components such as a plunger pump, a multi-way valve, a connecting pipeline and the like besides a separating column, wherein the plunger pump is a PEEK pump head, the flow is 0-200 mL/min, and the pressure resistance is 15Mpa. The multi-way valve and the pipeline are made of PEEK, and the pipe diameter is 1/8 inch.
The number of the inorganic acid leaching solution storage tanks is 4, and the inorganic acid leaching solution storage tanks respectively store 0.05 to 0.1mol/L HCl and 0.05 to 0.1mol/L HNO 3 、1.0～2.0mol/L HNO 3 、3.0～5.0mol/L HNO 3 The method comprises the steps of carrying out a first treatment on the surface of the Wherein 1.0 to 2.0mol/L HNO 3 The storage tank is designed with a water bath heating jacket structure, the water bath temperature is adjustable at room temperature to 80 ℃, a mechanical stirrer is designed in the storage tank to improve the uniformity of the solution temperature, and the solution temperature in the storage tank is detected by a polytetrafluoroethylene temperature probe. The liquid storage amount of the eluent storage tank is detected by a magnetic flap PEEK liquid level meter, and the volume is not less than 20 times of the sum of the volumes of 6 separation columns.
The ytterbium lutetium separating device adopts a simplified pump and valve design to achieve the purpose of continuous sample loading and separation. The operation of 6 separation column flows is completed by one pump through different valve combinations, the types and the specifications of the valves are consistent, and the difficulty for maintenance and replacement of later-stage valves, pipelines and the like is reduced. According to the application, phosphate extraction resin is adopted to separate ytterbium and lutetium, and DGA resin is adopted to convert high acidity solution into low acidity solution, so that the purposes of high-efficiency separation of ytterbium and lutetium and continuous separation of 6 columns are realized, and the automation degree of the device is improved.
The radioactivity detection device 4 is arranged in the No. 2 radioactivity shielding box 12, and all column liquid outlet pipelines are subjected to radioactivity detection through the radioactivity detection device, so that operators can know the ytterbium lutetium separation process in real time, and operations such as separation flow selection, switching and the like can be performed according to the result.
The radioactivity detecting device 4 is composed of a radioactivity detector and a shielding lead chamber, wherein the detector is a geiger tube, sodium iodide or other type. The thickness of the shielding lead chamber is not less than 20mm. The ytterbium-175 and lutetium-177 separation condition (the radioactive intensity change passing through the detection area in the detection pipeline) of 6 separation columns can be detected by only one detector, and the space occupation rate and the device cost in the box body are greatly reduced.
The radioactivity detection device adopts multiple pipelines to collect intensively, and achieves the effect of detecting the change condition of the radioactivity intensity of 6 pipelines by using only 1 detector.
Example 2
Based on the unsupported lutetium-177 solution preparation system provided in example 1, the unsupported lutetium-177 solution preparation method of the embodiment of the application comprises:
s1: and (3) placing the irradiated quartz tube into a transferring inner barrel, placing the inner barrel into a transferring trolley, transferring the inner barrel to a No. 1 shielding box body through a trolley track, taking down the inner barrel from the transferring trolley by using a joint type manipulator, and transferring the inner barrel into a cleaning circular groove. And then, a liquid adding pump power supply is started to fill the cleaning solution (generally deionized water or dilute nitric acid) into the cleaning tank through a liquid adding port, the liquid adding pump power supply is closed after the filling of the solution is completed, the quartz tube is soaked for a certain time (5-10 minutes), a liquid outlet valve of the cleaning tank is opened, and the cleaning waste liquid is drained. Then lifting the inner barrel, obliquely pouring out the quartz tube in the barrel into the dissolution barrel, putting the polytetrafluoroethylene hammer into the dissolution barrel, and repeatedly crushing the quartz tube in the barrel for a plurality of times (the crushing condition of the quartz tube is observed through a camera arranged at the top of the box body).
S2: after the steps are completed, taking out the hammer and beatingDissolving solution (1-4 mol/L HNO) is added into the dissolving barrel through a liquid adding opening by starting a dissolving solution adding pump power supply 3 Or HCl), covering the air extraction cover on the dissolution barrel by using a mechanical arm, opening a condensed water switch, opening an air extraction pump for extraction, and then opening a heating plate heating switch, wherein the heating temperature is 80-100 ℃. And 5-10 mL of dissolving solution is added every 10-15 minutes in the heating process, the heating is stopped after 3-5 times of repetition, and the air exhaust cover is opened to check the treatment condition of the target material in the barrel through the camera after the temperature is reduced. After the target material is completely dissolved, adding a certain amount of deionized water into the barrel for redissolving, and inserting a liquid suction pipe with a filter head into the bottom of the barrel for transferring lutetium-177 feed liquid to the ytterbium-lutetium separation device.
S3: inorganic acid leaching solution is adopted to store 0.05 to 0.1mol/L HNO in a tank 3 Eluting column 1 column 311, column 3 column 313, column 5 column 315; 3.0 to 5.0mol/L HNO is adopted 3 Column No. 2 312, column No. 4 314, column No. 6 316. Then, the lutetium-177 feed liquid in S2 is sampled to a No. 1 column 311 through a solution pipeline, and is sequentially eluted by inorganic acid, wherein the temperature in a storage tank of the inorganic acid is 1.0 to 2.0mol/L HNO with the temperature of 40 to 50 DEG C 3 The No. 1 column 311 is rinsed, and the effluent is collected to a waste liquid tank.
While the above process is running, the change of the radioactivity intensity of the radioactivity detector is monitored by the radioactivity detecting device 4 when the radioactivity intensity is 1.0-2.0 mol/L HNO 3 After that, when 'from low to high to low to high', 3.0-5.0 mol/L HNO is used instead 3 The column No. 1 311 is rinsed and the effluent flows to column No. 2 312.
Continuously monitoring the change condition of the radioactivity intensity of the radioactivity detector, stopping 3.0-5.0 mol/L HNO when 'rapid rising, rapid decreasing and slower decreasing' occur 3 And (5) leaching. Beginning column No. 2, flow 312: 0.05 to 0.1mol/L HNO is used 3 After leaching 1-3 times of column volume, the effluent is collected to a waste liquid tank, the No. 2 column 312 is leached by 0.05-0.1 mol/L HCl, and the effluent is led to the No. 3 column 313.
The radioactivity detector is monitored for radioactivity intensity change, and when 'rapid rise, rapid decrease and slow decrease' occur, the leaching of the No. 2 column 312 by 0.05-0.1 mol/L HCl is stopped. Start column No. 3, procedure 313: medium temperature in tank for leaching liquid by inorganic acid1.0 to 2.0mol/L HNO with the temperature of 40 to 50 DEG C 3 The column No. 3, 313, was rinsed and the effluent was collected to a waste tank.
While the process is running, the change of the radioactivity intensity of the radioactivity detector is monitored when the radioactivity intensity is 1.0-2.0 mol/L HNO 3 After that, when 'from low to high to low to high', 3.0-5.0 mol/L HNO is used instead 3 The column 3 (D-3) was rinsed and the effluent was passed to column 4 (D-4).
Continuously monitoring the change condition of the radioactivity intensity of the radioactivity detector, stopping 3.0-5.0 mol/L HNO when 'rapid rising, rapid decreasing and slower decreasing' occur 3 And (5) leaching. Beginning column No. 4 314 flow: 0.05 to 0.1mol/L HNO is used 3 Eluting the No. 4 column 314 with 0.05-0.1 mol/L HCl, and collecting the effluent to the No. 5 column 315 after eluting 1-3 times of column volume;
the radioactivity intensity change of the radioactivity detector is monitored, and when 'rapid rising, rapid falling and slower falling' occur, the leaching of the No. 4 column 314 by 0.05-0.1 mol/L HCl is stopped. Beginning column No. 5 315 flow: 1.0 to 2.0mol/L HNO with the temperature of 40 to 50 ℃ in an inorganic acid leaching solution storage tank 3 The column No. 5, 315, was rinsed and the effluent was collected to a waste tank.
While the process is running, the change of the radioactivity intensity of the radioactivity detector is monitored when the radioactivity intensity is 1.0-2.0 mol/L HNO 3 After that, when 'from low to high to low to high', 3.0-5.0 mol/L HNO is used instead 3 The column No. 5 315 is rinsed and the effluent is passed to column No. 6 316.
Continuously monitoring the change condition of the radioactivity intensity of the radioactivity detector, stopping 3.0-5.0 mol/L HNO when 'rapid rising, rapid decreasing and slower decreasing' occur 3 And (5) leaching. Start column No. 6 316 flow: 0.05 to 0.1mol/L HNO is used 3 Eluting the No. 6 column 316 by 0.05-0.1 mol/L HCl after 1-3 times of column volume, and collecting the effluent to a carrier-free lutetium-177 solution collecting bottle.
The change of the radioactivity intensity of the radioactivity detector is monitored, and when 'rapid rising, rapid falling and slower falling' occur, the leaching of the No. 6 column 316 by 0.05-0.1 mol/L HCl is stopped. And finishing the ytterbium lutetium separation process.
After the above steps are completed, the separation column is washed by deionized water with 3 to 5 times of column volume, and then 0.05 to 0.1mol/L HNO is used 3 Eluting the No. 1 column 311, the No. 3 column 313 and the No. 5 column 315,3.0 to 5.0mol/L HNO 3 Column No. 2 312, column No. 4 314, column No. 6 316 are rinsed for the next ytterbium lutetium separation.
The foregoing detailed description of the application has been presented for purposes of illustration and description, and it should be understood that the application is not limited to the particular embodiments disclosed, but is intended to cover all modifications, equivalents, alternatives, and improvements within the spirit and principles of the application.
Claims (10)
1. A carrier-free lutetium-177 solution preparation system, comprising:
a radiation shielding housing;
the target material treatment device is arranged in the radioactive shielding box body and is used for disassembling a quartz tube filled with target materials, heating and dissolving the target materials and separating lutetium-177 feed liquid;
the ytterbium and lutetium separation device is arranged in the radioactive shielding box body and is used for separating ytterbium and lutetium from lutetium-177 feed liquid to obtain carrier-free lutetium-177 solution;
the ytterbium lutetium separating device comprises a multi-stage continuous separating unit, the separating unit comprises: the first-stage separation column and the second-stage separation column are sequentially connected end to end; the first-stage separation column is filled with phosphate extraction resin, and the second-stage separation column is filled with DGA resin;
the liquid inlet of each stage of separation column is connected with an inorganic acid leaching solution storage tank, and the liquid outlet of each stage of separation column is respectively connected with a waste liquid tank and a lutetium-177 solution collecting bottle; and
the radioactivity detection device is connected with the liquid outlet pipeline of each stage of separation column and is used for detecting the radioactivity intensity of the liquid outlet of each stage of separation column.
2. The carrier-free lutetium-177 solution preparation system of claim 1, wherein said number of radioactive shielding boxes is at least 2, said target processing device and said ytterbium lutetium separation device are respectively disposed in different ones of said radioactive shielding boxes, said target processing device and said ytterbium lutetium separation device being in communication via a pump tube.
3. The carrier-free lutetium-177 solution preparation system of claim 1, wherein said target material processing device comprises: the quartz tube cleaning tank is used for cleaning a quartz tube filled with target materials; the target material treatment tank is used for smashing and disintegrating a quartz tube filled with target materials, heating and dissolving the target materials, and obtaining lutetium-177 feed liquid;
preferably, the target processing device further comprises a steam condensing sleeve connected to the target processing device for collecting and heating to dissolve to generate acid steam.
4. The carrier-free lutetium-177 solution preparation system of claim 1, further comprising a transport cart disposed at a back of the radiation-shielding box.
5. The carrier-free lutetium-177 solution preparation system of claim 1, wherein said mineral acid leaching solution storage tank is at least 4 in number;
preferably, the number of the inorganic acid leaching solution storage tanks is 4, and the inorganic acid leaching solution storage tanks respectively store 0.05 to 0.1mol/L HCl and 0.05 to 0.1mol/L HNO 3 、1.0～2.0mol/L HNO 3 、3.0～5.0mol/L HNO 3 ；
Preferably, 1.0 to 2.0mol/L HNO is stored 3 The temperature of the leacheate in (2) is from room temperature to 80 ℃.
6. The unsupported lutetium-177 solution preparation system of claim 1, wherein the size of the second stage separation column in the separation unit is smaller than the size of the first stage separation column;
preferably, the size of the separation column is determined by the required mass of the ytterbium-176 target material to be separated, and the mass of the resin filled in the separation column is not less than 200% of the required adsorption capacity for ytterbium-176 separation;
preferably, the ytterbium lutetium separation device at least comprises three separation units, and the sizes of the separation columns in the separation units are sequentially reduced;
preferably, the ytterbium lutetium separation device comprises three separation units, and the sizes of the separation columns in the ytterbium lutetium separation device are as follows: phi 30 multiplied by 1000mm and phi 30 multiplied by 150mm; phi 30 x 500mm and phi 20 x 100mm; phi 10 multiplied by 500mm and phi 10 multiplied by 40mm;
preferably, each stage of separation column is respectively connected with a plunger pump for conveying liquid, and the flow rate of the plunger pump is 0-200 mL/min;
preferably, the ytterbium lutetium separating device is made of PP or PEEK nonmetallic materials.
7. A method of a carrier-free lutetium-177 solution preparation system, comprising:
conveying the irradiated quartz tube filled with the target material into a radioactive shielding box, cleaning, decomposing, heating and dissolving the target material to obtain lutetium-177 feed liquid;
adopts HNO of 0.05 to 0.1mol/L 3 Eluting a first-stage separation column in the separation unit by 3.0-5.0 mol/L HNO 3 Eluting a second separation column in the separation unit to complete pretreatment of the separation column;
loading lutetium-177 feed liquid into a first-stage separation column in a separation unit, and adopting 1.0-2.0 mol/L HNO with the temperature of 40-50 DEG C 3 Eluting, conveying effluent liquid to a waste liquid tank for collection, and monitoring the change of the radioactivity intensity in the eluting process;
when the radioactivity intensity is 'low to high to low to high', 3.0-5.0 mol/L HNO is used instead 3 Eluting the first-stage separation column, conveying effluent to a second-stage separation column in a separation unit, and monitoring the change of the radioactivity intensity in the eluting process;
the radioactive intensity is rapidly increased and rapidly reduced, and 3.0-5.0 mol/L HNO of the first-stage separation column is stopped when the decrease is slow 3 Leaching, adopting HNO with the concentration of 0.05-0.1 mol/L 3 Eluting the second-stage separation column by 1-3 times of column volume, then delivering the effluent to a waste liquid tank for collection, eluting the second-stage separation column in the separation unit by adopting 0.05-0.1 mol/L HCl, delivering the effluent to the first-stage separation column in the next separation unit, and simultaneously monitoring the change of the radioactivity intensity in the eluting process;
the radioactive intensity is rapidly increased and rapidly reduced, and when the reduction is slow, the radioactive intensity stops 0.05 to 0.1mol/L HNO of the second-stage separation column in the separation unit 3 Leaching;
and the next separation unit is sequentially leached according to the previous steps, and the separation process is repeated for a plurality of times, so as to finish ytterbium lutetium separation.
8. The method for preparing a solution of lutetium-177 without a carrier as claimed in claim 7, wherein the step of heating the dissolved target is: adding 1-4 mol/L hydrochloric acid or nitric acid solution, heating to 80-100 ℃ to dissolve target material.
9. The method for preparing carrier-free lutetium-177 solution as claimed in claim 7, wherein after separation of ytterbium and lutetium is completed, 0.05-0.1 mol/L HNO is adopted 3 Eluting a first-stage separation column in the separation unit by 3.0-5.0 mol/L HNO 3 The second stage separation column in the separation unit is rinsed.
10. The method for preparing a solution of lutetium-177 without carrier as claimed in claim 7, wherein the next separation unit is repeatedly washed twice in sequence.
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