A method for producing 64 Target shuttle for copper nuclei and method of preparation

Abstract

The application relates to the technical field of medical radionuclide preparation, and discloses a target shuttle for producing Cu radionuclides and a preparation method thereof. 64 The target shuttle and the preparation method are especially suitable for large-scale production of Cu radionuclides based on a domestic 20MeV proton cyclotron. 64 The target shuttle structure integrates gradient target material-directional beam flow-high-efficiency heat dissipation functions, and is matched with an energy partition-time control-impurity pre-control cooperative process, so that high yield and high purity of Cu radionuclides are realized. 64 The target shuttle and the preparation method are especially suitable for large-scale production of Cu radionuclides based on a domestic 20MeV proton cyclotron.

Description

Technical Field

[0001] This invention relates to the field of medical radionuclide preparation technology, and more specifically, to a method for producing... 64 Target shuttles for Cu nuclides and their preparation methods. Background Technology

[0002] 64 Cu, as a typical therapeutic nuclide, also possesses β-properties. + X-ray (PET imaging) and beta - The radiation (targeted therapy) properties have important application value in the fields of neuroendocrine tumors and tumor hypoxia diagnosis. 64 There are three main methods for producing Cu: cyclotron solid target irradiation, cyclotron liquid target irradiation, and reactor neutron activation. The advantages and disadvantages of these three methods are as follows: solid targets offer high specific activity but require chemical separation; liquid targets are simpler to operate but the product contains carrier impurities; and reactor production yields the lowest specific activity but is the least expensive. Currently, regarding... 64 The demand for large-scale supply of Cu nuclides is becoming increasingly urgent, but current production technologies still face the following key challenges: 1. Significant bottleneck in production capacity: Existing technologies mostly employ a single target design, which cannot match the proton energy decay curve, resulting in low utilization of the nuclear reaction cross-section. For example, technologies based on 14.6 MeV accelerators... 64 The actual yield of the Ni(p,n) reaction was only 104 MBq / (μA·h), which is 26% lower than the theoretical value of 142 MBq / (μA·h), making it difficult to meet the needs of large-scale clinical applications.

[0003] 2. Insufficient thermal management efficiency: The proton beam generates a large amount of heat deposition on the de-energizer (e.g., 50μA beam current corresponds to 210W thermal power). Traditional aluminum film de-energizers are prone to failure due to temperature exceeding the melting point (933K), and the complex water-cooling structure increases the difficulty of target shuttle design.

[0004] 3. High difficulty in controlling purity: 68 Zn target irradiation is prone to associated with... 67 Cu impurities require strict control of the energy range; 64 In the preparation of Ni targets, the silver substrate is easily passed through... 64 The (p,n) reaction of Ni@Ag target generates 107 / 109 Radioactive impurities such as Cd increase the purification burden.

[0005] 4. Poor economic efficiency and adaptability: Existing target shuttles are mostly designed for specific energy accelerators and are not compatible with mainstream domestic equipment; the target material recovery process is imperfect, and expensive enrichment is required. 64 Ni / 68 The utilization rate of Zn is less than 70%, which drives up production costs.

[0006] Although domestic enterprises have achieved 64 While mass production of Cu (e.g., Atomic High-Tech's output exceeds 1 Ci) has been achieved, significant room for improvement remains in terms of yield enhancement, thermal management optimization, and impurity control. For example, patent CN112962125B controls the Cu content in the leaching solution to below 0.25 μg / mL through acid treatment of the gold-plated target, addressing the fundamental impurity issue. However, it does not address the synergistic optimization of the target shuttle structure for beam utilization and heat dissipation, nor does it clearly define the target material recovery efficiency and equipment compatibility design. Patent CN120591740A focuses on the homogenization preparation of copper targets, but does not address related aspects. 64 Nuclear reaction characteristics and process adaptability of Cu production.

[0007] Therefore, developing a target shuttle and process that balances high yield, high purity, and industrial adaptability is of great practical significance. Summary of the Invention

[0008] The purpose of this invention is to provide a method for production 64 The target shuttle of Cu nuclide and its preparation method are intended to address the above-mentioned issues.

[0009] To achieve the above objectives, the present invention provides the following solution: On the one hand, the present invention provides a method for production 64 The method for preparing Cu nuclide includes the following steps: S1. Target material pretreatment: Prepared by pulse electroplating method 64 Ni target material, nickel plating solution is 0.1 mol / L hydrochloric acid and 50 mg / mL 64 Ni ion mixed solution, positive pulse width 600μs, negative pulse width 30μs, current density 35mA / cm2, electroplating for 1h to form a uniform coating, followed by vacuum annealing. S2, Precision Irradiation Process: During the irradiation process, the beam intensity was maintained at three stages: 20 μA, 50 μA and 80 μA, with each stage lasting 30 minutes. The total irradiation time was 7 hours, and the irradiation was followed by a 2-hour cooling period. S3. Separation, purification, and recovery: The AG1-X8 anion exchange column-TK201 resin column system was used for elution with the following components in sequence: (1) elution with 6 mol / L hydrochloric acid. 64 Ni recovery rate > 85%; (2) Fe / Co impurities were removed with 4 mol / L hydrochloric acid; (3) elution was performed with 0.1 mol / L hydrochloric acid. 64 Cu; eluted 64 Cu is the product.

[0010] Furthermore, in step S1, the vacuum annealing temperature is 300°C and the annealing time is 2 hours.

[0011] Furthermore, in step S2, during the irradiation process, Geant4 simulation is used to ensure that the beam uniformity is >95% and the batch yield fluctuation is ≤5%.

[0012] On the other hand, the present invention also provides a method for generating 64 The target shuttle of Cu nuclide, used in the above preparation method, includes: The beam collimation module has a conical collimator and a graphite energy reduction layer at the inlet. The size is optimized by simulation using SRIM software to precisely control the 20MeV incident proton energy to the range of 10.4-8.7MeV, with an energy dispersion of ≤0.3MeV. The gradient target cavity module adopts a detachable layered structure. The target material bearing surface is equipped with a microgroove structure with a depth of 0.2mm and a spacing of 1mm. A φ2mm pressure balance hole is reserved on the side wall. The high-efficiency heat dissipation module adopts a dual-loop design of spiral water cooling + graphene thermal conductive film. A 0.1mm graphene film is attached to the back of the target material. The thermal conductivity of the thick graphene film is >5000W / (m・K). The water cooling channel has an inner diameter of 3mm and a pitch of 5mm. Through ANSYS simulation verification, the target surface temperature is maintained below 75℃ under 80μA beam current conditions. Impurity isolation components, in 64 An additional 50 mg / cm² of material is added between the Ni target and the silver substrate. 2 The gold-plated transition layer, after being immersed in a mixed solution of hydrochloric acid and hydrogen peroxide at a mass ratio of 5:2 at 80°C, has a Cu content of ≤0.2μg / mL in the secondary leaching solution.

[0013] Furthermore, the target shuttle is made of oxygen-free copper with a thermal conductivity greater than 380 W / (m·K).

[0014] Compared with the prior art, the beneficial effects of the present invention are as follows: 1. Structural-Energy Synergistic Innovation: The combined design of graphite energy reduction layer and gradient target cavity solves the core pain point of low beam energy and target material matching in existing patents, achieving a yield of 110-120 MBq / (μA / h), which is 5.8%-15.4% higher than the actual yield of CN112962125B; 2. Breakthrough in thermal management system: The dual-loop design of graphene thermal conductive film and spiral water cooling improves the heat load capacity by 40% compared with the traditional structure, and can be adapted to 80μA high beam current, solving the thermal failure problem that was not fully addressed in patents such as CN112962125B. 3. Dual optimization of impurities and cost: The gold-plated transition layer reduces metal impurities to below 0.2 μg / mL, the target material recycling rate is >85%, and the cost is reduced by 25% compared with the existing technology, balancing purity and economy; 4. Compatibility with domestic equipment: Custom-designed for 20MeV domestic accelerators, with a target shuttle lifespan of >50 batches and batch-to-batch stability deviation of <3%, filling the gap in existing patents regarding compatibility design with domestic equipment. Attached Figure Description

[0015] To more clearly illustrate the technical solutions in the embodiments of the present invention or the prior art, the drawings used in the embodiments will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0016] Figure 1 This is a schematic diagram of the target shuttle provided in an embodiment of the present invention.

[0017] In the diagram, 1 is the top; 2 is the central main body; 21 is the rectangular window; 22 is the internal interlayer of the cylindrical main body; and 3 is the bottom. Detailed Implementation

[0018] 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. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0019] To make the above-mentioned objects, features and advantages of the present invention more apparent and understandable, the present invention will be further described in detail below with reference to the accompanying drawings and specific embodiments.

[0020] Step 1: Target shuttle structure design 1. The target shuttle adopts an integrated architecture of "beam collimation - gradient target cavity - high-efficiency heat dissipation", and the main material is high-temperature resistant oxygen-free copper (thermal conductivity > 380W / (m・K)), specifically including: Beam collimation module: A conical collimator and a graphite degrading layer are installed at the inlet. The dimensions are optimized using SRIM software simulation to precisely control the 20 MeV incident proton energy to the 10.4-8.7 MeV range, with an energy dispersion ≤0.3 MeV. The graphite degrading layer utilizes its high melting point (approximately 4100 K) and low thermal resistance, achieving a contact thermal resistance of 10... -3 m 2• Under K / W conditions, the maximum temperature can be controlled below 625K, solving the overheating failure problem of traditional aluminum film. Compared with the unoptimized beam injection method of CN112962125B, this design improves the utilization rate of the nuclear reaction section by more than 15% through precise energy control.

[0021] Section utilization rate η = actual reaction output Y / theoretical maximum output Y0.

[0022] Wherein, the theoretical maximum output Y0=Φ*N target *σ*t. (t is the irradiation time), the actual reaction yield is inferred from the activity of the activated product.

[0023] 2. Gradient target cavity module: Adopts a detachable layered structure, adaptable to... 64 Ni single-target (12mg / cm) 2 (plating) or 68 The Zn-aluminum buffer layer composite target features a microgroove structure (0.2mm depth, 1mm spacing) on ​​the target material's bearing surface to increase the beam contact area; a φ2mm pressure balance hole is pre-reserved on the sidewall to prevent cavity deformation caused by irradiation heating. Unlike CN120591740A, which only focuses on the homogenization of the target material itself, this module further improves nuclear reaction efficiency through the structural synergy between the target cavity and the target material.

[0024] 3. High-efficiency heat dissipation module: Utilizing a dual-loop design of "spiral water cooling + graphene thermal conductive film," a 0.1mm thick graphene film (thermal conductivity > 5000W / (m・K)) is bonded to the back of the target material. The water cooling channel has an inner diameter of 3mm and a pitch of 5mm, maintaining the target surface temperature below 75℃ under 80μA beam current conditions. Compared to the undefined heat dissipation design of CN112962125B and the conventional heat treatment process of CN120591740A, this system demonstrates a 40% improvement in heat load capacity, supporting higher beam current intensities.

[0025] 4. Impurity isolation component: In 64 An additional 50 mg / cm² of material is added between the Ni target and the silver substrate. 2 After the gold-plated transition layer was treated with hydrochloric acid-hydrogen peroxide (5:2) at 80℃, the Cu content in the secondary leaching solution was ≤0.2μg / mL, which is 20% lower than the upper limit of 0.25μg / mL in CN112962125B (the 20% figure was obtained by a simple percentage comparison between the above 0.2μg / mL and the reported 0.25μg / mL; ICP-MS detected that the Cu content in the secondary leaching solution was ≤0.2μg / mL), while suppressing Cd impurity contamination caused by the activation of the silver substrate (ICP-MS detection).

[0026] Specifically, see Figure 1 As shown, the target shuttle structure of this application includes: Top 1: Beam Collimation Module Area. The top of the target shuttle has a circular end face with a coaxially nested annular opening structure in the center. This opening is the proton beam injection channel, corresponding to the mounting position of the conical collimator and the graphite de-energizing layer. It can precisely control the 20MeV incident proton energy to the 10.4-8.7MeV range. The inclined stepped positioning structure on the outer periphery of the top is used for precise docking and positioning with the accelerator beamline port to ensure coaxial beam injection.

[0027] Central Main Body 2: Core Function Integration Section. The central section of the target shuttle is a straight cylindrical main body, which is the integration area of ​​the gradient target cavity module and the high-efficiency heat dissipation module: the rectangular window 21 on the side of the exterior is used for... 64 Replacement of Ni target material and maintenance of the target cavity; the target cavity is equipped with a microgroove structure target bearing surface with a depth of 0.2mm and a spacing of 1mm at the corresponding position, and the side wall is reserved with a pressure balance hole of φ=2mm to ensure the structural stability of the target cavity during irradiation.

[0028] The cylindrical body has an internal interlayer that integrates a dual-loop high-efficiency heat dissipation module consisting of a spiral water cooling system and a graphene thermal conductive film. A 0.1mm thick graphene thermal conductive film with a thermal conductivity greater than 5000W / (m・K) is bonded to the back of the target material. The inner wall of the cylinder is equipped with a spiral water cooling channel with an inner diameter of 3mm and a pitch of 5mm, which can achieve a heat dissipation effect that keeps the target surface temperature below 75℃ under 80μA beam current conditions.

[0029] Bottom 3: Installation and positioning base section. The bottom of the target shuttle is a stepped base structure with a reduced diameter, used for the coaxial installation and rigid fixation of the entire target shuttle on the accelerator target station. At the same time, this area integrates the inlet and outlet water interfaces of the water cooling circuit, ensuring the fluid connection and stable operation of the dual heat dissipation circuit.

[0030] Step 2: Matching production processes 1. Target material pretreatment: Prepared using pulse electroplating method. 64 Ni target material, nickel plating solution containing 0.1 mol / L hydrochloric acid and 50 mg / mL 64 Ni ion, positive pulse width 600 μs, negative pulse width 30 μs, current density 35 mA / cm² 2 Electroplating for 1 hour forms a uniform coating, increasing the target material utilization rate to over 91%. Vacuum annealing (300℃, 2 hours) is performed after electroplating to eliminate internal stress. Compared to the conventional electroplating and immersion process described in CN112962125B, this pulse electroplating technology increases the target material utilization rate by over 15% (data is obtained by detecting the remaining target material content in the plating solution after electroplating using ICP-MS and then calculating the result), and the batch-to-batch thickness deviation is ≤3% (data is obtained by detecting the batch thickness using TEM and then performing simple calculations).

[0031] 2. Precision Irradiation Process: The beam current intensity adopts a stepped increase strategy (20μA→50μA→80μA), with each stage maintained for 30 minutes; the total irradiation time is 7 hours, followed by a 2-hour cooling period to attenuate short-half-life impurities. Geant4 simulations ensure beam current uniformity >95% and batch yield fluctuation ≤5%. Unlike the unoptimized irradiation parameters in CN112962125B, this strategy achieves [the desired effect] under the same beam current conditions. 64 Cu production increased by 5.8%-15.4% (obtained through multiple irradiation tests using a cyclotron). 64 Cu can be directly displayed on the screen as XX mCi, and the above data can be obtained through calculation.

[0032] 3. Separation and purification: A coupling system of "AG1-X8 anion exchange column-TK201 resin column" was used: ① Elution with 6 mol / L hydrochloric acid 64 Ni (recovery rate > 85%); ② Removal of Fe / Co impurities with 4 mol / L hydrochloric acid; ③ Elution with 0.1 mol / L hydrochloric acid. 64 Cu. The purification cycle is approximately 1.5 hours. After decay correction, the recovery rate of the target nuclide reaches 97%, the radiopurity is >99.9%, and the molar activity is >5 GBq / nmol.

[0033] 4. Target Material Recovery: Compared to the target material recovery process not clearly defined in CN112962125B, this process... 64 Ni recovery rate increased by 20% (as detected by ICP-MS, the remaining waste liquid after recovery contained unrecovered components). 64 Ni, compare this data with the content of the liquid before recovery. 64 Compared to Ni, this significantly reduces raw material costs.

[0034] The technical solution of the present invention will be described below with reference to embodiments: 64 Cu nuclide yield: measured using a CRC-55tR radioactivity meter, in MBq / (μA·h), after decay correction; Target surface temperature: The highest temperature under steady-state irradiation was obtained by combining ANSYS finite element simulation with in-situ detection using an infrared thermal imager. Product radioactivity purity: detected using a high-purity germanium gamma spectrometer (HPGe); Metal impurity content: Detected using inductively coupled plasma mass spectrometry (ICP-MS); 64 Ni recovery rate: Ni content in the eluent and undiluted solution was determined by ICP-MS. 64 Ni content, calculate recovery rate; Uniformity of target coating: The coating thickness was detected by transmission electron microscopy (TEM), and the batch-to-batch thickness deviation was calculated.

[0035] Example 1 The target shuttle body is made of oxygen-free copper (measured thermal conductivity 395 W / (m·K)), and it integrates four core modules: Beam collimation module: A conical collimator and a graphite energy reduction layer are set at the inlet. The size is optimized by SRIM software simulation to precisely control the 20MeV incident proton energy to the range of 10.4-8.7MeV, with a measured energy dispersion of 0.25MeV; Gradient target cavity module: adopts a detachable layered structure, with microgrooves (0.2mm depth, 1mm spacing) on ​​the target material bearing surface, and φ2mm pressure balance holes reserved on the side wall; High-efficiency heat dissipation module: It adopts a dual-loop design of spiral water cooling + graphene thermal conductive film, with a 0.1mm thick graphene film (measured thermal conductivity of 5300W / (m・K)) bonded to the back of the target material, and the water cooling channel has an inner diameter of 3mm and a pitch of 5mm. Impurity isolation components: in 64 An additional 50 mg / cm² of material is added between the Ni target and the silver substrate. 2 The gold-plated transition layer is pretreated by immersion in a mixed solution of hydrochloric acid and hydrogen peroxide at 80°C.

[0036] The target material pretreatment was prepared using a pulse electroplating method. 64 Ni target material, nickel plating solution is 0.1 mol / L hydrochloric acid and 50 mg / mL enrichment 64 A mixed solution of Ni ions; electroplating parameters: positive pulse width 600μs, negative pulse width 30μs, current density 35mA / cm². 2 Electroplating for 1 hour yielded a concentration of 12 mg / cm³. 2 A uniform coating is formed; after electroplating, the coating is placed in a vacuum annealing furnace and annealed at 300℃ for 2 hours to eliminate internal stress in the coating.

[0037] Precision irradiation process will prepare the 64 The Ni target was loaded into the target shuttle and connected to a domestically produced 20MeV proton cyclotron accelerator. A stepped current-increasing strategy was adopted: the current was increased in three stages: 20μA, 50μA, and 80μA, with each stage maintained stably for 30 minutes. After the current increase was completed, the irradiation was continued at the rated beam intensity of 80μA, with a total irradiation time of 7 hours. The irradiation process was verified by Geant4 simulation, and the beam uniformity was 96.2%. After the irradiation, the beam was cooled for 2 hours to decay short half-life impurities.

[0038] Separation, purification, and recovery were performed using an AG1-X8 anion exchange column coupled with a TK201 resin column, with the following elution steps: ① Elution with 6 mol / L hydrochloric acid. 64 Ni is recovered, enriched, and recycled; ② 4 mol / L hydrochloric acid is used to remove metallic impurities such as Fe and Co; ③ 0.1 mol / L hydrochloric acid is used for elution.64 Cu, to obtain the final product.

[0039] Test results 64 Cu nuclide yield: 118 MBq / (μA·h); target surface maximum temperature under steady-state 80 μA beam current: 72℃; product radioactivity purity: 99.92%; Cu content in secondary leachate: 0.18 μg / mL; 64 Ni recovery rate 87.2%; purification cycle 1.4h, after decay correction 64 Cu recovery rate was 97.3%, molar activity was 5.6 GBq / nmol; the thickness deviation of the target coating between batches was 2.1%; and no structural deformation or coating peeling was observed after 55 consecutive batches of use of the target shuttle.

[0040] Example 2 The oxygen-free copper target shuttle body was prepared (thermal conductivity 385 W / (m·K)), and the core module parameters were adjusted as follows: Beam collimation module: After optimization of the graphite de-energizing layer, the incident proton energy is tuned to the range of 10.2-8.9 MeV, with an energy dispersion of 0.28 MeV; Gradient target cavity module: The microgroove structure on the target material bearing surface has a depth of 0.18mm and a spacing of 1.1mm; High-efficiency heat dissipation module: graphene film thickness 0.1mm (thermal conductivity 5100W / (m・K)), water cooling channel inner diameter 3.2mm, pitch 4.8mm; Impurity isolation components: Gold-plated transition layer density 50 mg / cm³ 2 The same pretreatment as in Example 1.

[0041] Pretreatment parameters for target material in pulse electroplating: positive pulse width 580μs, negative pulse width 35μs, current density 33mA / cm² 2 Electroplating for 1 hour yielded 11.5 mg / cm³. 2 Coating; vacuum annealing at 300℃ for 2 hours.

[0042] Precision irradiation process with stepped current ramping strategy: 20μA stable for 30min, 50μA stable for 30min, and continuous irradiation at 80μA, with a total irradiation time of 7h; irradiation beam uniformity of 95.7%, followed by 2h cooling.

[0043] The separation, purification, and recovery were carried out using the same dual-column system and elution process as in Example 1.

[0044] Test results 64 Cu nuclide yield: 114 MBq / (μA·h); maximum target surface temperature under steady-state 80 μA beam current: 73℃; product radioactivity purity: 99.91%; Cu content in secondary leachate: 0.19 μg / mL. 64Ni recovery rate was 86.5%; the thickness deviation between batches of target coating was 2.7%; and no abnormalities were found in 52 batches of continuous use of the target shuttle.

[0045] Comparative Example 1 Target fabrication: An oxygen-free copper target is used with gold plating on the surface. It has no graphite energy reduction layer, no graphene thermal conductive film dual-loop heat dissipation, and no gradient target cavity microgroove structure. Target material preparation: prepared using conventional DC electroplating method. 64 Ni target material, without vacuum annealing treatment; Irradiation process: Direct irradiation with a constant beam current of 80μA was used, with a total irradiation time of 7 hours and a stepless current ramping strategy. Separation and purification: Elution was performed using a single AG1-X8 anion exchange column, without TK201 resin column coupling; no clear separation was achieved. 64 Ni recovery process; The remaining experimental environment and raw material specifications are the same as in Example 1.

[0046] Test results 64 Cu nuclide yield: 102 MBq / (μA・h); the highest target surface temperature under steady-state 80 μA beam current was 136℃, with localized peeling of the target coating; product radioactivity purity: 99.2%; Cu content in secondary leaching solution: 0.26 μg / mL. 64 Ni recovery rate was 68.3%; the thickness deviation between batches of target coating was 8.2%; and structural deformation occurred in the target shuttle after 28 consecutive batches of use.

[0047] Comparative Example 2 The target preparation, irradiation process, and separation and purification procedures were completely consistent with those in Example 1. Target pretreatment: prepared using conventional DC electroplating method. 64 Ni target material, electroplating current density 35 mA / cm² 2 Electroplating for 1 hour, without pulse control, and without vacuum annealing after electroplating; The remaining parameters are the same as in Example 1.

[0048] Test results 64 Cu nuclide yield was 103 MBq / (μA・h); the batch-to-batch thickness deviation of the target coating was 7.9%, with pinholes and peeling observed; localized coating detachment occurred during 80 μA beam irradiation, leading to irradiation interruption; 64 Ni recovery rate was 79.4%, and product radioactivity purity was 99.5%.

[0049] Comparative Example 3 The target preparation, target pretreatment, and separation and purification processes are completely consistent with those in Example 1. Irradiation process: Direct irradiation with a constant beam current of 80μA, without the 20μA and 50μA step-up current stabilization stages, with a total irradiation time of 7 hours and a cooling time of 2 hours after irradiation; The remaining parameters are the same as in Example 1.

[0050] Test results 64 Cu nuclide yield was 107 MBq / (μA·h); the sudden increase in beam current caused thermal shock to the target material, and the highest target surface temperature was 94°C under steady-state beam current of 80 μA; the yield fluctuation between batches was 8.7%, which exceeded the control range of ≤5% of this invention; micro-deformation of the target cavity occurred after 36 batches of continuous use of the target shuttle.

[0051] Comparative Example 4 Target shuttle preparation: Only a single spiral water-cooling structure is used, and no graphene thermal conductive film is attached to the back of the target material. The rest of the target shuttle structure and parameters are completely consistent with those in Example 1. The target pretreatment, irradiation process, and separation and purification process are completely consistent with those in Example 1; The remaining parameters are the same as in Example 1.

[0052] The test results showed that the highest target surface temperature under steady-state 80μA beam current was 129℃, which far exceeded the control target of 75℃ in this invention; after continuous irradiation for 4.5h, the coating peeled off due to overheating of the target material, and the irradiation was interrupted. 64 Cu nuclide yield was 92 MBq / (μA・h), and the product radioactivity purity was 99.3%; after 19 consecutive batches of target shuttles, deformation of the water cooling channel occurred.

[0053] Comparative Example 5 Target shuttle preparation: 64 There is no gold plating transition layer between the Ni target and the silver substrate, and the rest of the target structure and parameters are completely consistent with those in Example 1. The target pretreatment, irradiation process, and separation and purification process are completely consistent with those in Example 1; The remaining parameters are the same as in Example 1.

[0054] The test results showed that the Cu content of the secondary leachate was 0.33 μg / mL, with accompanying 107 / 109 Cd radioactive impurities; the product's radioactivity purity was 99.1%, which does not meet the standards for clinical use of medical radionuclides. 64 Cu nuclide yield was 115 MBq / (μA·h), purification cycle was extended to 2.6 h, after decay correction. 64 Cu recovery rate decreased to 89.2%.

[0055] Comparative Example 6 Target shuttle fabrication: A traditional aluminum film energy reducer was used, with a precise energy control design without a graphite energy reduction layer and a conical collimator. The rest of the target shuttle structure and parameters were completely consistent with those in Example 1. The target pretreatment, irradiation process, and separation and purification process are completely consistent with those in Example 1; The remaining parameters are the same as in Example 1.

[0056] The detection results showed that the incident proton energy dispersion was 0.8 MeV, which could not be precisely controlled within the optimal nuclear reaction range of 10.4-8.7 MeV, resulting in a decrease in the utilization rate of the nuclear reaction cross section. 64 Cu nuclide yield was 101 MBq / (μA・h), with 63Cu and 67Cu impurities present. The product radiometric purity was 99.4%. The highest temperature during irradiation of the aluminum film de-energizer was 912 K, close to the melting point of aluminum (933 K). After 12 consecutive batches of use, the de-energizer layer melted and broke.

[0057] Table 1

[0058] The embodiments described above are merely preferred embodiments of the present invention and are not intended to limit the scope of the present invention. Various modifications and improvements made by those skilled in the art to the technical solutions of the present invention without departing from the spirit of the present invention should fall within the protection scope defined by the claims of the present invention.

Claims

1. A device for production 64 The method for preparing Cu nuclide is characterized by, Includes the following steps: S1. Target material pretreatment: Prepared by pulse electroplating method 64 Ni target material, nickel plating solution is 0.1 mol / L hydrochloric acid and 50 mg / mL 64 Ni ion mixed solution, positive pulse width 600μs, negative pulse width 30μs, current density 35mA / cm² 2 Electroplating for 1 hour forms a uniform coating, followed by vacuum annealing. S2, Precision Irradiation Process: During the irradiation process, the beam intensity was maintained at three stages: 20 μA, 50 μA and 80 μA, with each stage lasting 30 minutes. The total irradiation time was 7 hours, and the irradiation was followed by a 2-hour cooling period. S3. Separation, purification, and recovery: The AG1-X8 anion exchange column-TK201 resin column system was used for elution with the following components in sequence: (1) elution with 6 mol / L hydrochloric acid. 64 Ni recovery rate > 85%; (2) Fe / Co impurities were removed with 4 mol / L hydrochloric acid; (3) elution was performed with 0.1 mol / L hydrochloric acid. 64 Cu; eluted 64 Cu is the product.

2. The method for production according to claim 1 64 The method for preparing Cu nuclide is characterized by, In step S1, the vacuum annealing temperature is 300°C and the annealing time is 2 hours.

3. The method for production according to claim 1 64 The method for preparing Cu nuclide is characterized by, In step S2, during the irradiation process, Geant4 simulation is used to ensure that the beam uniformity is >95% and the batch yield fluctuation is ≤5%.

4. A method for generating 64 A target shuttle for Cu nuclides, used in any one of claims 1-3 for the production of 64 The method for preparing Cu nuclide is characterized in that, include: The beam collimation module has a conical collimator and a graphite energy reduction layer at the inlet. The size is optimized by simulation using SRIM software to precisely control the 20MeV incident proton energy to the range of 10.4-8.7MeV, with an energy dispersion of ≤0.3MeV. The gradient target cavity module adopts a detachable layered structure. The target material bearing surface is equipped with a microgroove structure with a depth of 0.2mm and a spacing of 1mm. A φ2mm pressure balance hole is reserved on the side wall. The high-efficiency heat dissipation module adopts a dual-loop design of spiral water cooling and graphene thermal conductive film. A 0.1mm graphene film is attached to the back of the target material. The thermal conductivity of the thick graphene film is >5000W / (m・K). The water cooling channel has an inner diameter of 3mm and a pitch of 5mm. Through ANSYS simulation verification, the target surface temperature is maintained below 75℃ under 80μA beam current conditions. Impurity isolation components, in 64 An additional 50 mg / cm² of material is added between the Ni target and the silver substrate. 2 The gold-plated transition layer, after being immersed in a mixed solution of hydrochloric acid and hydrogen peroxide at a mass ratio of 5:2 at 80°C, has a Cu content of ≤0.2μg / mL in the secondary leaching solution.

5. The method for generating according to claim 4 64 The target shuttle of Cu nuclide, characterized in that... The target shuttle is made of oxygen-free copper with a thermal conductivity greater than 380 W / (m·K).

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