An apparatus and method for preparing a high specific activity Tb-161 solution

Abstract

This invention discloses an apparatus and method for preparing a high specific activity Tb-161 solution, belonging to the field of radioisotope preparation technology. It includes: a shielded box and a target material processing system, a separation system, a radioactivity detection system, and a control system housed within the shielded box. The separation system is used to adsorb the target material solution, elute it with an organic carboxylic acid eluent, and process the obtained Tb-161-containing eluent to obtain a Tb-161-containing solution. The apparatus for preparing a high specific activity Tb-161 solution provided by this invention separates Tb-161 from irradiated Gd-160-enriched target material using ion chromatography, significantly improving the yield and specific activity of terbium-161 and simplifying the separation process. The constant column temperature during separation greatly reduces waste liquid volume, shortens separation time, and avoids the problem of insufficient terbium-161 specific activity caused by gadolinium tailing.

Description

Technical Field

[0001] This invention relates to the field of radioactive isotope preparation technology, specifically to an apparatus and method for preparing a high specific activity Tb-161 solution. Background Technology

[0002] Terbium-161 possesses suitable decay characteristics, with a half-life of 6.9 days. During decay, it emits beta rays with an average energy of 154 keV, gamma rays with energies of 48.92 keV, 57.19 keV, and 74.57 keV, and a large number of Auger electrons. Due to its relatively low gamma-ray energy, moderate beta-ray energy, and the production of Auger electrons during decay, it is particularly suitable for the treatment of small tumors. Radiolabeled drugs based on terbium-161 have begun clinical trials, with promising results.

[0003] Terbium-161 can be generated by enriching gadolinium-160 through reactor irradiation. However, after irradiation, the gadolinium-160 enriched in the target material and the terbium-161 produced need to be radiochemically separated to obtain terbium-161 that meets the requirements for use. Currently, the production of terbium-161 mainly faces the following problems:

[0004] Separation using lanthanide resins involves a large eluent volume, resulting in high costs for treating radioactive waste and requiring at least two stages for complete separation, leading to lengthy separation times. Since gadolinium is eluted first, gadolinium tailing is unavoidable, reducing the specific activity and yield of terbium-161 in the final product. Furthermore, the lanthanide resin extractant detaches from the matrix during separation, requiring additional processing to treat the detached extractant and maintain separation efficiency, further increasing the complexity of the separation apparatus. Alternatively, a method using lanthanide resins for the first stage of coarse separation followed by ion-exchange chromatography to obtain terbium-161 overcomes the gadolinium tailing problem in the second stage and significantly improves the nuclear purity of terbium-161; however, the first-stage eluent volume remains large. There are also reports of using ion chromatography to directly obtain terbium-161 through a single-stage separation. While this achieves complete separation, the throughput is relatively small, or two consecutive stages of separation are still required for complete separation of gadolinium and terbium. Furthermore, the separation process has a low level of automation, necessitating extensive robotic operations, including target handling, material transfer, and radiochemical separation. Additionally, the eluent is not reused, leading to unnecessary radioactive waste. Moreover, the target dissolution and solution transfer processes involve solution heating steps, posing a high risk of radioactive irradiation. Summary of the Invention

[0005] In view of the above shortcomings, the present invention aims to provide an apparatus and method for preparing a high specific activity Tb-161 solution, so as to achieve remote control, high degree of automation, simple structure and continuous operation of the preparation of a high specific activity Tb-161 solution.

[0006] The technical solution of the present invention to solve the above-mentioned technical problems is as follows:

[0007] This invention provides an apparatus for preparing a high specific activity Tb-161 solution, comprising: a shielded box and a target material processing system, a separation system, a radioactivity detection system and a control system disposed within the shielded box;

[0008] The target material processing system is used to clean and break the target tube, and add a first acid solution to dissolve the irradiated Gd-160 enriched target material to obtain a target material solution.

[0009] The separation system is connected to the target material processing system and is used to adsorb the target material solution and add organic carboxylic acid elution solution for elution. The obtained Tb-161-containing eluent is subjected to system treatment to convert the organic acid in the Tb-161-containing eluent into inorganic acid and reduce the concentration of inorganic acid to obtain a Tb-161-containing solution.

[0010] The radioactivity detection system is connected to the separation system and is used to monitor the changes in the radiation intensity and the corresponding radiation rate of the solution during the separation process.

[0011] The control system controls the operation of the separation system based on the detection results of the radioactivity detection system.

[0012] Furthermore, in the apparatus for preparing the high specific activity Tb-161 solution, the target material processing system includes: a target tube cleaning device, a target material tank, and a filter;

[0013] The target tube cleaning device is connected to the target tank via a pipe. The inlet of the target tank is connected to a first acid tank, and the outlet of the target tank is connected to the filter.

[0014] Furthermore, in the apparatus for preparing the high specific activity Tb-161 solution, the separation system includes: a chromatographic separation column, a target recovery column, a first transfer column, and a second transfer column;

[0015] The chromatographic separation column is connected to the target tube cleaning device via a pipeline;

[0016] The water outlet of the chromatographic separation column is connected to the target recovery column and the first rotating column, respectively. The first rotating column is connected to the second rotating column through a pipeline.

[0017] The inlet of the chromatographic separation column is connected to a first organic carboxylic acid eluent tank and a second organic carboxylic acid eluent tank via pipes.

[0018] Furthermore, in the apparatus for preparing the high specific activity Tb-161 solution, the chromatographic separation column and the first rotating system column are respectively connected to a second acid tank via pipelines, the outlet end of the chromatographic separation column and the first rotating system column are respectively connected to a waste liquid tank via pipelines, and the target recovery column is connected to a liquid to be recovered tank via pipelines.

[0019] Furthermore, in the apparatus for preparing the high specific activity Tb-161 solution, the radioactivity detection system includes a detector using cadmium zinc telluride as a probe.

[0020] This invention also provides a method for preparing a high specific activity Tb-161 solution, comprising:

[0021] After dissolving the irradiated Gd-160 enriched target, the pH was adjusted to 2-5 to obtain a target solution for use as a column loading solution.

[0022] The column feed solution was filtered and then sent into the chromatographic separation column for adsorption. It was eluted with an organic carboxylic acid eluent with a pH of 3-6 to obtain an eluent containing Tb-161.

[0023] The eluent is fed into the first rotating column and eluted with the first hydrochloric acid eluent to convert the organic acid in the eluent into an inorganic acid. The eluent is then fed into the second rotating column to reduce the concentration of inorganic acid in the eluent, thus obtaining a solution containing Tb-161.

[0024] Furthermore, in the method for preparing the high specific activity Tb-161 solution, the organic carboxylic acid eluent includes one or more of acetic acid, citric acid, tartaric acid, α-HIBA, oxalic acid, and lactic acid; the concentration of the organic carboxylic acid eluent is 0.05-0.6 mol / L.

[0025] Furthermore, in the method for preparing the high specific activity Tb-161 solution, the concentration of the first hydrochloric acid eluent is 2-5 mol / L.

[0026] Furthermore, in the method for preparing the high specific activity Tb-161 solution, the column temperature of the chromatographic separation column is 30~50℃, and the elution flow rate of the chromatographic separation column is 8~16 min / BV.

[0027] Furthermore, in the method for preparing the high specific activity Tb-161 solution, the separation material used in the chromatographic separation is a cation exchange resin, the separation material of the first rotating column is a cation exchange resin, and the separation material of the second rotating column is an amide resin.

[0028] The present invention has the following beneficial effects:

[0029] The apparatus for preparing high specific activity Tb-161 solution provided by this invention separates Tb-161 from irradiated Gd-160-enriched target material using ion chromatography, significantly improving the yield and specific activity of terbium-161 and simplifying the separation process. Chromatographic separation of gadolinium and terbium is employed, utilizing a uniform particle size distribution of the packing material and a smooth inner surface of the separation column, thus reducing the influence of multipath effects; the column temperature remains constant during separation. This significantly reduces waste liquid volume, shortens separation time, and avoids the problem of insufficient terbium-161 specific activity caused by gadolinium tailing.

[0030] The apparatus for preparing high specific activity Tb-161 solution provided by this invention achieves gadolinium-terbium separation based on ion chromatography. Its packing material has a uniform particle size distribution and a smooth inner surface, thus reducing the influence of multipath effects; the column temperature remains constant during separation. This significantly reduces waste liquid volume, shortens separation time, and avoids the problem of insufficient terbium-161 specific activity caused by gadolinium tailing. The designed eluent recovery system can further reduce the eluent volume.

[0031] The device for preparing high specific activity Tb-161 solution provided by the present invention detects the changes in radiation intensity and corresponding radiation count in the effluent during the entire separation process through an online radioactivity detection system, and transmits the changes to a host computer. The host computer then accurately and promptly switches the separation process based on the detection results, achieving continuous separation and avoiding the manual valve switching operation, thus significantly reducing the radiation exposure time of personnel.

[0032] The apparatus for preparing high specific activity Tb-161 solution provided by this invention has the advantages of using organic carboxylic acid as the eluent in ion chromatography with a low concentration, resulting in a low separation column temperature and allowing the packing material to be reused dozens of times. The packing material used in the separation column has a uniform eccentricity distribution and a smooth inner surface, significantly reducing the influence of multipath effects. This significantly improves separation efficiency and reduces the volume of eluent consumed and the separation time.

[0033] The apparatus for preparing high specific activity Tb-161 solution provided by this invention reduces the acid concentration using a second conversion column with amide resin as the separation material, thus replacing the traditional method of heating and evaporating followed by adding dilute acid; it also replaces the traditional method of dissolving the target material directly with dilute acid instead of dissolving it with concentrated acid, evaporating it to dryness, and then dissolving it with dilute acid. These operations reduce the number of steps and effectively lower the risk of radioactive irradiation.

[0034] The apparatus for preparing high specific activity Tb-161 solution provided by this invention eliminates the need for a high-pressure pump resistant to strong acids, and simultaneously enables pretreatment operations of highly radioactive target materials, such as target tube transfer, cleaning, and dissolution, without requiring complex electrical equipment. The separation process utilizes a separation system connected by multi-port valves, significantly reducing the number of components within the shielded enclosure, including the separation column, pump, and valves, thereby lowering the device failure rate and improving production efficiency. Attached Figure Description

[0035] The accompanying drawings, which are included to provide a further understanding of embodiments of the invention and form part of this application, do not constitute a limitation thereof. In the drawings:

[0036] Figure 1 This is a schematic diagram of the apparatus for preparing the high specific activity Tb-161 solution of the present invention. Figure 1 ;

[0037] Figure 2 This is a schematic diagram of the apparatus for preparing the high specific activity Tb-161 solution of the present invention. Figure 2 .

[0038] The attached diagram shows the markings and corresponding component names:

[0039] In the diagram: 100-Shielding enclosure, 110-Target material processing system, 111-Target tube cleaning device, 112-Target material tank, 113-Filter, 114-First acid tank, 120-Separation system, 121-Chromatographic separation column, 122-Target material recovery column, 123-First transfer system column, 124-Second transfer system column, 125-First organic carboxylic acid eluent tank, 126-Second organic carboxylic acid eluent tank, 127-Second acid tank, 128-Waste liquid tank, 129-Recovery liquid tank, 130-Radioactivity detection system, 140-Control system. Detailed Implementation

[0040] To make the objectives, technical solutions, and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. The components of the embodiments of the present invention described and shown in the accompanying drawings can generally be arranged and designed in various different configurations.

[0041] Therefore, the following detailed description of the embodiments of the invention provided in the accompanying drawings is not intended to limit the scope of the claimed invention, but merely to illustrate selected embodiments of the invention. All other embodiments obtained by those skilled in the art based on the embodiments of the invention without inventive effort are within the scope of protection of the invention.

[0042] Example 1: Please refer to Figure 1 and Figure 2 The present invention provides an apparatus for preparing a high specific activity Tb-161 solution, comprising: a shielded box 100 and a target material processing system 110, a separation system 120, a radioactivity detection system 130 and a control system 140 disposed within the shielded box 100;

[0043] The target material processing system 110 is used to clean and break the target tube, and add a first acid solution to dissolve the irradiated target material enriched with Gd-160 to obtain a target material solution.

[0044] The separation system 120 is connected to the target material processing system 110 and is used to adsorb the target material solution and add organic carboxylic acid rinsing solution for rinsing. The obtained Tb-161-containing eluent is subjected to a conversion system treatment to convert the organic acid in the Tb-161-containing eluent into inorganic acid and reduce the concentration of inorganic acid to obtain a Tb-161-containing solution.

[0045] The radioactivity detection system 130 is connected to the separation system 120 and is used to monitor the changes in the radiation intensity and the corresponding radiation rate of the solution during the separation process.

[0046] The control system 140 controls the operation of the separation system 120 based on the detection results of the radioactivity detection system 130.

[0047] The apparatus for preparing a high specific activity Tb-161 solution provided by this invention involves cleaning a quartz tube containing the target material using a target tube cleaning device 111. Subsequently, the target tube is crushed in a target material tank 112, and a first acid solution is added to dissolve the target material, obtaining a target material solution for preparing the terbium-161 solution. After sample loading, the chromatographic separation column 121 is eluted with an organic acid (carboxylic acid) and the rotating column is eluted with a high concentration of hydrochloric acid to separate gadolinium and terbium. Then, the hydrochloric acid solution containing a high concentration of terbium-161 is passed through a second rotating column 124 to reduce the hydrochloric acid concentration, obtaining a terbium-161 solution suitable for labeling. During the separation process, the radioactivity detection system 130 performs radioactivity detection on the outlet pipeline of the chromatographic separation column 121, the target material recovery column 122, and the transfer column, allowing operators to understand the gadolinium-terbium separation process in real time. The host computer can automatically perform valve switching and other operations based on the results, or the host computer can be manually controlled to perform related operations.

[0048] In this invention, a radioactive shielding box 100 is used to install and place devices, and provides shielding capability with a lead equivalent thickness of ≥20 mm, reducing the dose of radioactive radiation received by operators. The box has a waste liquid tank for discharging radioactive waste liquid into a waste liquid container 128. A trolley transport track is installed on the back of the box to facilitate material transfer between boxes. Through holes are installed between adjacent boxes for installing solution pipelines, signal or power lines, etc. Specifically, the shielding box 100 has dimensions of 2500 mm wide × 1500 mm deep × 1800 mm high, and is equipped with two articulated robotic arms with a clamping force ≥7 kg. Two lead glass viewing windows, each 500 × 600 mm in size, are installed on the front. It is equipped with one waste disposal chute and one floor drain, each Ф150 mm in size. A trolley transport track is installed on the back. The transport trolley and track are parallel to the back of the box and can stop at the trolley door, thereby achieving the purpose of transporting materials between boxes.

[0049] In this invention, the target material processing system 110 has the functions of target tube cleaning, crushing and target material dissolution. After the target tube is cleaned, the cleaning liquid is transported to the waste liquid tank 128 through the pipeline for collection. The target material is dissolved by crushing the target tube and adding the first acid solution.

[0050] In this invention, the separation system 120 mainly consists of a chromatographic separation column 121, a first rotating column 123, a second rotating column 124, and a target recovery column 122. It employs a simplified pump and valve design, using three pumps to complete the operation of four separation columns through different valve combinations, with only one being a high-pressure constant-flow pump. Valves directly connected to the high-pressure pump and the chromatographic separation column 121 must withstand high pressure, while the remaining valves have less stringent pressure resistance requirements. The chromatographic separation column 121 is made of stainless steel, significantly reducing the cost of the device. In the separation system 120, the separation columns are eluted with organic acid to a strongly acidic cation exchange resin. Simultaneously, the cation exchange resin can also serve as the first rotating column 123 to convert the solution system from organic acid to hydrochloric acid. DGA resin is used to convert the solution system from high inorganic acidity to low inorganic acidity. Specifically, the chromatographic column is Ф50×250 mm in size and made of stainless steel; the target recovery column 122 is Ф20×600 mm in size; and the transfer column is Ф10×60 mm in size, all made of PEEK. The pump operating pressure is not less than 15 MPa.

[0051] In this invention, the radioactive monitoring system employs centralized acquisition across multiple pipelines. Since the intensity of terbium-161 gamma rays is low, probes such as lanthanum bromide cannot be used. Therefore, a detector with zinc cadmium telluride as the probe is employed. Only one probe is used to detect the changes in radioactivity intensity across multiple pipelines. The switching of valves and pumps is controlled by a computer system based on the changes in nuclide composition.

[0052] Furthermore, the target material processing system 110 includes: a target tube cleaning device 111, a target material tank 112, and a filter 113;

[0053] The target tube cleaning device 111 is connected to the target material tank 112 via a pipeline. The inlet of the target material tank 112 is connected to the first acid tank 114, and the outlet of the target material tank 112 is connected to the filter 113. Specifically, the target material dissolution process uses hydrochloric acid with an acidity of 0.05-0.1 mol / L for direct stirring and dissolution, without the need for heating or evaporation before dissolution to prepare the loading solution. The Tb-161 solution flowing out from the first rotating column 123 passes through an amide resin column to achieve a change in acidity from high to low, without the need for evaporation followed by dissolution with dilute acid to achieve the acidity change.

[0054] Furthermore, the separation system 120 includes: a chromatographic separation column 121, a target recovery column 122, a first rotation column 123, and a second rotation column 124;

[0055] The chromatographic separation column 121 is connected to the target tube cleaning device 111 via a pipeline;

[0056] The outlet of the chromatographic separation column 121 is connected to the target recovery column 122 and the first rotating column 123 respectively. The first rotating column 123 is connected to the second rotating column through a pipeline.

[0057] The inlet of the chromatographic column 121 is connected to a first organic carboxylic acid eluent tank 125 and a second organic carboxylic acid eluent tank 126 via pipes. A valve controls the reuse of the eluent from the first organic carboxylic acid eluent tank 125 (excluding the gadolinium and terbium fraction) after passing through the chromatographic column 121 for circulating elution.

[0058] Furthermore, the chromatographic separation column 121 and the first rotating column 123 are respectively connected to a second acid tank 127 via pipelines, the outlet end of the chromatographic separation column 121 and the first rotating column 123 are respectively connected to a waste liquid tank 128 via pipelines, and the target material recovery column 122 is connected to a liquid to be recovered tank 129 via pipelines.

[0059] Furthermore, the radioactive detection system 130 includes a detector using cadmium zinc telluride as a probe. The radioactive detection system 130 is used to detect gadolinium-160 and terbium-161 nuclides. A chromatographic separation column 121 and a target recovery column 122 are included. The effluent pipeline of the rotating column passes through a lead cylindrical base, enabling the detection of nuclide composition in the effluent of all columns using only one detector. The switching of valves and pumps is controlled by a computer system based on changes in nuclide composition.

[0060] The device of the present invention also includes an ammonia tank for adjusting the pH value, which is not shown in the figure.

[0061] The operation procedure of the apparatus for preparing high specific activity Tb-161 solution provided in this embodiment of the invention is as follows:

[0062] Step 1: Using a robotic arm, remove the inner container containing the quartz target tube from the transport trolley. Place the inner container in the target tube cleaning device 111 and add deionized water to the device. After the quartz tube has been soaked, drain the cleaning solution. Using the robotic arm, lift the inner container containing the quartz target tube from the cleaning device 111 and transfer it to the target material tank 112. After the quartz tube transfer is complete, use the robotic arm to operate a hammer to crush and disassemble the quartz target tube in the target material tank 112. Repeat the crushing 5-10 times and then remove the hammer. Then, add dilute hydrochloric acid (0.05-0.1 mol / L) from the first acid tank 114 and stir to dissolve. After complete dissolution, add concentrated ammonia to adjust the pH to 3 to obtain the column loading solution.

[0063] Step 2: After pretreatment, proceed with the column loading operation;

[0064] Step 3: The pretreatment process of chromatographic separation column 121 is then carried out. Column 121 is eluted with an appropriate amount of 0.05 mol / L ammonium chloride. The first transfer column 123 is eluted with a first organic carboxylic acid with a concentration of 0.13 mol / L and pH adjusted to 4.5 by ammonia. The second transfer column is eluted with concentrated hydrochloric acid from the second hydrochloric acid tank. The target recovery column 122 is eluted with an appropriate amount of first organic carboxylic acid with a concentration of 0.13 mol / L and pH adjusted to 4.5 by ammonia. The eluent flows into waste liquid tank 128.

[0065] The liquid in target tank 112 is pumped through filter 113 by a high-pressure pump into chromatographic column 121. Filter 113 is used to prevent glass fragments from damaging the high-pressure pump. The waste liquid after column loading flows into waste liquid tank 128. After column loading, the column is eluted with 0.13 mol / L organic carboxylic acid from the first organic carboxylic acid tank, with the pH adjusted to 4.5 by concentrated ammonia. The elution column temperature is 40°C. At this time, the separation process is switched via computer control based on the changes in radiation intensity and corresponding dose rate detected by the online radioactivity monitoring system.

[0066] When no gadolinium-159 and terbium-161 signals are detected in the eluent from the chromatographic column 121, the eluent flowing out of the chromatographic column 121 can be used for circulating elution of the chromatographic column 121.

[0067] When a terbium-161 signal is detected in the effluent from the chromatographic column 121, the corresponding valve is switched so that the direction of the effluent from the chromatographic column 121 is changed from being used for circulating elution to flowing into the first rotating column 123, and the resulting waste liquid flows into the waste liquid tank 128.

[0068] When the terbium-161 signal disappears in the effluent from column 121, column 123 is eluted with 0.5 mol / L α-HIBA from the first organic carboxylic acid tank, with the pH adjusted to 4.5 by ammonia. The eluent flows into waste tank 128. When the gadolinium-159 signal is detected by the radioactivity monitoring system in the effluent from column 121, the corresponding valve is switched so that the effluent from column 121 flows from waste tank 128 to target recovery column 122. The waste liquid generated after flowing through target recovery column 122 still flows into waste tank 128.

[0069] When the gadolinium-159 signal detected in the effluent of chromatographic column 121 rises rapidly and then falls to a low, flat level, the elution process of chromatographic column 121 is stopped. The transfer operation begins by pumping concentrated hydrochloric acid (2-5 mol / L) from the second hydrochloric acid tank 127 into the first transfer column 123 using a low-pressure pump. The effluent from the first transfer column 123 is then passed into the second transfer column and subsequently flows into the waste tank 128.

[0070] When the effluent from the first rotating column 123 detects the presence of a terbium-161 signal and then it disappears, the rinsing of the first rotating column 123 is stopped. Subsequently, the second rotating column is rinsed with dilute hydrochloric acid (concentration 0.05-0.1 mol / L) from the first acid tank 114 to obtain high specific activity terbium-161 that can be used for labeling.

[0071] Step 4: The concentrated hydrochloric acid (concentration 2-5 mol / L) in the second acid tank 127 is pumped into the target recovery column 122 by a low-pressure pump. The outflow enters the recovery tank 129. After decaying for several months, the target recovery operation can be carried out.

[0072] Example 2: This embodiment of the invention provides a method for preparing a high specific activity Tb-161 solution, based on the apparatus for preparing a high specific activity Tb-161 solution provided in Example 1, comprising:

[0073] Step 1: After dissolving the irradiated enriched Gd-160 target, adjust the pH to 2-5 to obtain a target solution for use as a column loading solution;

[0074] Step 2: After filtering, the column feed solution is sent to the chromatographic separation column for adsorption. It is then eluted with an organic carboxylic acid eluent with a pH of 3-6 to obtain an eluent containing Tb-161.

[0075] Step 3: The eluent is fed into the first rotating column and eluted with the first hydrochloric acid eluent to convert the organic acid in the eluent into an inorganic acid. Then it is fed into the second rotating column and eluted with dilute hydrochloric acid to reduce the concentration of inorganic acid in the eluent, so as to obtain a Tb-161-containing solution that can be used for labeling.

[0076] Further, the organic carboxylic acid elution solution includes one or more of acetic acid, citric acid, tartaric acid, α-HIBA, oxalic acid, and lactic acid; the concentration of the organic carboxylic acid elution solution is 0.05-0.6 mol / L, and can be 0.05 mol / L, 0.1 mol / L, 0.2 mol / L, 0.3 mol / L, 0.4 mol / L, 0.5 mol / L, 0.6 mol / L, etc.

[0077] Furthermore, the concentration of the first hydrochloric acid rinsing solution used is 2-5 mol / L, which can be 2 mol / L, 2.5 mol / L, 3 mol / L, 3.5 mol / L, 4 mol / L, 4.5 mol / L, 5 mol / L, etc.

[0078] Furthermore, the column temperature of the chromatographic separation column is 30~50℃, which can be 30℃, 35℃, 40℃, 45℃, 50℃, etc. It is controlled by the column oven, and the column temperature remains constant throughout the loading and elution process, with a temperature fluctuation of less than ±0.1℃. The preferred column temperature is 40℃. Both the transfer column and the target recovery column are at room temperature. The average particle size of the chromatographic separation column packing material is 5-20μm, with a particle size distribution (d90-d10) / d50 ≤ 1.5. The column height is 250-350 mm, the column diameter is 25-75 mm, and the pressure resistance is ≥10 MPa. The packing material mass and specific column diameter are determined based on the sample loading volume, and the packing material mass must not be less than 1000 times the sample loading volume. The surface roughness of the inner wall of the chromatographic column is less than 0.4 micrometers, and its material is stainless steel.

[0079] The elution flow rate of the chromatographic separation column is 8~16 min / BV, which can be 8 min / BV, 10 min / BV, 12 min / BV, 14 min / BV, or 16 min / BV.

[0080] Furthermore, the separation material used in the chromatographic separation is a cation exchange resin, such as BioAG50W-X8, AMINE*A6, Sykam Resin, etc.; the separation material of the first rotating column is a cation exchange resin, such as BioAG50W-X8, AMINE*A6, Sykam Resin, etc.; and the separation material of the second rotating column is an amide resin.

[0081] The specific embodiments described above further illustrate the purpose, technical solution, and beneficial effects of the present invention. It should be understood that the above description is only a specific embodiment of the present invention and is not intended to limit the scope of protection of the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the scope of protection of the present invention.

Claims

1. An apparatus for the preparation of a high specific activity Tb-161 solution, characterized in that, include: The shielding enclosure (100) includes a target material processing system (110), a separation system (120), a radioactivity detection system (130), and a control system (140) installed inside the shielding enclosure (100). The target material processing system (110) is used to clean and break the target tube, and add a first acid solution to dissolve the irradiated Gd-160 enriched target material to obtain a target material solution. The separation system (120) is connected to the target material processing system (110) for adsorbing the target material solution and adding organic carboxylic acid rinsing solution for rinsing. The obtained Tb-161-containing eluent is subjected to system treatment to convert the organic acid in the Tb-161-containing eluent into inorganic acid and reduce the concentration of inorganic acid to obtain a Tb-161-containing solution. The radioactive detection system (130) is connected to the separation system (120) and is used to monitor the changes in the radiation intensity and the corresponding radiation rate of the solution during the separation process. The control system (140) controls the operation of the separation system (120) based on the detection results of the radioactivity detection system (130); The target material processing system (110) includes: a target tube cleaning device (111), a target material tank (112), and a filter (113). The target tube cleaning device (111) is connected to the target material tank (112) through a pipe. The inlet of the target material tank (112) is connected to the first acid tank (114), and the outlet of the target material tank (112) is connected to the filter (113). The separation system (120) includes: a chromatographic separation column (121), a target recovery column (122), a first rotating column (123), and a second rotating column (124); The chromatographic separation column (121) is connected to the target tube cleaning device (111) via a pipeline; The outlet of the chromatographic separation column (121) is connected to the target recovery column (122) and the first rotating column (123), respectively. The first rotating column (123) is connected to the second rotating column (124) through a pipeline. The inlet of the chromatographic column (121) is connected to the first organic carboxylic acid eluent tank (125) and the second organic carboxylic acid eluent tank (126) respectively via pipes.

2. The apparatus for preparing a high specific activity Tb-161 solution according to claim 1, characterized in that, The chromatographic separation column (121) and the first rotating column (123) are respectively connected to a second acid tank (127) through pipes. The outlet end of the chromatographic separation column (121) and the first rotating column (123) are respectively connected to a waste liquid tank (128) through pipes. The target material recovery column (122) is connected to a liquid tank (129) to be recovered through pipes.

3. The apparatus for preparing a high specific activity Tb-161 solution according to claim 1, characterized in that, The radioactive detection system (130) includes a detector using cadmium zinc telluride as a probe.

4. A method for preparing a high specific activity Tb-161 solution using an apparatus according to any one of claims 1-3, characterized in that, include: After dissolving the irradiated Gd-160 enriched target, the pH was adjusted to 2-5 to obtain a target solution for use as a column loading solution. The column feed solution was filtered and then sent into the chromatographic separation column for adsorption. It was eluted with an organic carboxylic acid eluent with a pH of 3-6 to obtain an eluent containing Tb-161. The eluent is fed into the first rotating column and eluted with the first hydrochloric acid eluent to convert the organic acid in the eluent into an inorganic acid. The eluent is then fed into the second rotating column to reduce the concentration of inorganic acid in the eluent, thus obtaining a solution containing Tb-161.

5. The method for preparing a high specific activity Tb-161 solution according to claim 4, characterized in that, The organic carboxylic acid rinsing solution includes one or more of the following: acetic acid, citric acid, tartaric acid, α-HIBA, oxalic acid, and lactic acid; the concentration of the organic carboxylic acid rinsing solution is 0.05-0.6 mol / L.

6. The method for preparing a high specific activity Tb-161 solution according to claim 4, characterized in that, The concentration of the first hydrochloric acid rinsing solution used was 2-5 mol / L.

7. The method for preparing a high specific activity Tb-161 solution according to claim 4, characterized in that, The column temperature of the chromatographic separation column is 30~50℃, and the elution flow rate of the chromatographic separation column is 8~16 min / BV.

8. The method for preparing a high specific activity Tb-161 solution according to claim 4, characterized in that, The separation material used in the chromatographic separation is cation exchange resin. The separation material of the first rotating column is cation exchange resin, and the separation material of the second rotating column is amide resin.

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