CN116216644A - Low-vacuum-degree high-purity At-211 carbonization production system and production method thereof - Google Patents
Low-vacuum-degree high-purity At-211 carbonization production system and production method thereof Download PDFInfo
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Abstract
The invention discloses a low-vacuum high-purity At-211 carbonization production system and a production method thereof, wherein the system adopts inert gas after drying and filtering to drive gasified At-211 to move, adopts a reducing quartz tube to install a bombarded Bi target, adopts a six-stage variable-temperature cold trap to collect products, and is provided with a tail gas treatment unit and a radiation shielding unit, and the system only needs hundred-Pa-level vacuum degree when in operation, thereby reducing the requirements of the materials of the components of the system; and no target scraping operation is required; the inert gas loaded into the system by the gas control unit can bring gasified At-211 into a product collecting pipe positioned in a time-controllable multistage variable-temperature cold trap for enrichment, and after enrichment is finished, a proper eluent is used for leaching out the high-purity At-211 product, so that the product is small in volume and low in loss, and the system and the method are suitable for various experimental research works based on the At-211.
Description
Technical Field
The invention belongs to the technical field of At-211 production, and particularly relates to a low-vacuum high-purity At-211 carbonization production system and a production method thereof.
Background
At-211 is an alpha nuclide with a half-life of 7.2 hours, emitting on average one alpha particle and 6.3 Auger electrons per decay, and is considered one of the ideal nuclides most suitable for targeted internal radiation therapy; meanwhile, the average alpha ray energy of the At-211 is 6.789MeV, the half-life period is short, and the risk of long-term radiation pollution can be avoided, so that the At-211 is also one of ideal nuclides for researching alpha endogenous radiolysis in the related process of spent fuel treatment; but it must be obtained by means of artificial synthesis.
At present, the At-211 production method is obtained by adopting a separation and purification method, and the separation and purification method comprises a dry method and a wet method. The wet separation yield is stable, the wet separation efficiency is higher than that of the dry separation, nuclides possibly caused by the evaporation of At-211 can be reduced, and the process is fixed, so that the automatic production is facilitated; however, most wet separation is long in time consumption, nuclides decay too much, and valence states of nuclides in different solutions are changeable, so that the mechanism of separation is not thoroughly studied; furthermore, solvent fixation of the product may have an impact on the nuclide labeling and radiolysis systems, so wet separation has potential but still requires further exploration.
The dry separation method has the following obvious advantages: (1) The operation is convenient, the steps of radioactive substance treatment are reduced, and environmental pollution and personnel radiation are avoided as much as possible; (2) Reduced At-211 contact with various chemical agents to avoid unpredictable chemical morphology changes; (3) The At-211 can be rinsed in a relatively small volume and with different media to meet the needs of subsequent radiochemistry; (4) The chemical purity of the separated product is obviously higher than that of a wet product, and the product is more beneficial to the subsequent multi-field application of the At-211.
The dry separation is to scrape the target of the irradiated target piece, collect Bi into a heating pipe, then heat the heating pipe to a temperature above the boiling point of At-211 (337 ℃) to gasify and release Bi, and then sublimate the device into solid by adopting a cooling mode to realize the collection of products. For example, lindegren et al physically delaminate the irradiated bismuth layer and put it into a preheating stepHeating in 650 deg.C distillation tube, condensing and collecting with PEEK capillary tube in-70 deg.C cold trap (ethanol dry ice mixed) with recovery rate of 79+ -3%; this approach of stripping the bismuth layer can be adapted to a small separation device, reducing separation time, but involves the high dose stripping transfer causing unnecessary radiation contamination and radiation exposure to the practitioner. Zalutsky et al distills the irradiated whole target and lets astatine vapor pass through two 0.5mL glass collection tubes holding 0℃with chloroform, directly condensed in the collection tubes for coupling labeling, with a distillation yield of 67.+ -. 16%. Kotaro Nagatsu et al also improved slightly by heating the distillation tube to 500℃in advance and then leaching out the nuclide by capillary condenser tube, and by real-time monitoring of the dosage, the distillation recovery rate was improved to 83.4.+ -. 6.2%. Patent CN107073141B discloses an automated processing platform for producing an astatine-211 (At-211) radiopharmaceutical and patent CN114249301A discloses an elution solution and a method for preparing a radionuclide for targeted nuclide drug, which all bombard a Bi target with an alpha ion beam to produce 209 Bi(α,2n) 211 The reaction At gave At-211 in yields of 85% and 82.+ -. 9%, respectively. Therefore, the carbonization and separation method does not realize solidification, the yield is unstable and is mostly 67-85%, the target scraping operation is tedious and time-consuming, and the nuclide can escape even if a mechanical treatment mode is adopted. Meanwhile, there is almost no consideration of At-211 as a requirement for higher purity in other applications than radiopharmaceutical preparation, and no integration of effective radiation shielding facilities is possible with existing devices.
Disclosure of Invention
The invention aims to provide a low-vacuum high-purity At-211 carbonization production system which can directly heat a bombarded Bi target to gasify and release the At-211 and then cool by adopting a multistage variable-temperature cold trap to obtain a product, so that the enrichment of gasified At-211 in a collecting pipe can be ensured, and the yield and purity of the product are improved.
In order to achieve the above purpose, the invention adopts the following technical scheme:
a low vacuum high purity At-211 dry distillation production system comprises a gas control unit, a gasification separation unit, a product collection unit and a tail gas treatment unit;
the method further realizes the collection of the At-211 products; the device comprises an inert gas storage tank, a gas drying pipe, a one-way regulating valve, an air inlet pressure gauge, a micro gas flow controller and a filter, wherein the inert gas storage tank, the gas drying pipe, the one-way regulating valve, the air inlet pressure gauge and the micro gas flow controller are sequentially connected through pipelines, inert gas is stored in the inert gas storage tank, the inert gas is dried and filtered, the flowing speed of the inert gas is controlled by the micro gas flow controller to enter a gasification separation unit, and gasified At-211 is transferred to a product collecting unit under the flowing of the inert gas;
the gasification separation unit is used for heating and gasifying Bi targets bombarded by ion beams to release At-211 and comprises a tubular furnace, a reducing quartz tube and a quick-release reducing joint, wherein the tubular furnace is used for heating to gasify the At-211 on the Bi targets, the reducing quartz tube is used for installing the Bi targets and is arranged in the tubular furnace, the outlet of the reducing quartz tube is in a conical structure, the conical structure is connected with the product collection unit through the quick-release reducing joint, and heating belts are arranged At the outlet of the reducing quartz tube and on the quick-release reducing joint;
the product collecting unit is used for desublimating gasified At-211 into solid At-211 to collect products, and adopts six-stage variable-temperature cold trap assemblies, each stage of cold trap assembly has the same structure and is connected end to end, the cold trap assembly comprises a cold trap device, a collecting pipe and a leaching device, the collecting pipe is arranged on the cold trap device, the inlet of the collecting pipe is connected with the outlet of the gasification separating unit, and the outlet of the collecting pipe is connected with the leaching device through a three-way valve; the cold trap device reduces the temperature in the collecting pipe, so that the gasified At-211 is sublimated into solid At-211, the solid At-211 is attached to the inner wall of the collecting pipe, and the solid At-211 is leached by the leaching device to obtain a product; the temperature of each six-stage variable temperature cold trap assembly is set as follows: the first-stage cold trap starts to operate in the system preparation stage, and the temperature is-10-0 ℃; the second-stage cold trap starts to operate when the temperature of the tubular furnace reaches 400-450 ℃, and the temperature is minus 20-minus 15 ℃; the third-stage cold trap starts to operate when the temperature of the tube furnace reaches 450-500 ℃ and the temperature is minus 30-minus 25 ℃; the fourth-stage cold trap starts to operate when the temperature of the tubular furnace reaches 500-550 ℃, and the temperature is minus 50-minus 45 ℃; the fifth stage cold trap starts to operate when the temperature of the tube furnace reaches 550-600 ℃ and the temperature is minus 100-minus 60 ℃; the sixth-stage cold trap starts to operate when the temperature of the tubular furnace reaches 650-750 ℃ and is between-250 ℃ and-100 ℃;
the tail gas treatment unit is used for treating the gas after the product collecting unit to prevent the balance At-211 from entering the atmosphere to pollute the environment, and comprises a check valve, a tail gas absorption pipe, a vacuum pressure gauge, a U-shaped active carbon pipe and a vacuum pump, wherein the check valve is arranged on an outlet of a cold trap component of the last stage, the check valve, the tail gas absorption pipe, the vacuum pressure gauge, the U-shaped active carbon pipe and the vacuum pump are sequentially connected through pipelines, and tail gas absorption liquid is filled in the tail gas absorption pipe.
Further, the reducing quartz tube comprises a quartz outer tube, a quartz boat and a quartz target table; the Bi target is arranged on the quartz target table, the quartz target table is arranged in the quartz boat, the quartz boat is arranged in the quartz outer tube, the installed Bi target is level with the center of the quartz outer tube, and the inlet and outlet of the variable-diameter quartz tube are all on the central line.
Further, the collecting pipe adopts a customized glass pipe or a polymer material pipe, the inner diameter of the collecting pipe is less than or equal to 3.175mm, and the single-stage length is 800-1500 mm.
Further, the leaching device comprises a centrifuge tube for storing leaching liquid and a peristaltic pump, wherein an inlet of the peristaltic pump is connected with the centrifuge tube, an outlet of the peristaltic pump is connected with an outlet three-way valve of the collecting tube, and leaching liquid of the peristaltic pump is pumped into the collecting tube in a direction opposite to the air flow direction.
Further, the leaching solution adopts one of high-purity water, methanol, ethanol, methylene dichloride, chloroform, carbon tetrachloride, nitric acid and sodium hydroxide.
Further, the tail gas absorption liquid adopts one of sodium hydroxide, methanol, ultrapure water, dilute nitric acid and an extracting agent.
Further, the invention also comprises a radiation shielding unit for playing a role of radiation shielding, which comprises a box body and a lead glass component, wherein the box body is used for integrally installing a gas control unit, a gasification separation unit, a product collection unit and a tail gas treatment unit, and the lead glass component surrounds and isolates the gasification separation unit.
The invention also provides a low-vacuum high-purity At-211 carbonization production method, which is realized based on the carbonization production system and comprises the following steps:
(1) Bombarding Bi targets: bombarding the Bi target by adopting a CS-30 cyclotron for 4-5 hours, and then standing for 30 minutes, and taking out the Bi target; wherein the alpha beam current parameter of the CS-30 cyclotron is 28MeV, 15-20 mu A;
(2) Preparing a system: the system preparation can be made during Bi target bombardment, firstly, pipeline connection of a production system and the opening condition of valves are detected, and the vacuum degree of the system is set by adopting a vacuum pump of a tail gas treatment unit under the condition of no error, wherein the vacuum degree is-0.4 to-1.2 kPa; then opening the tube furnace to preheat the variable-diameter quartz tube, wherein the preheating temperature is 200-300 ℃; the first stage cold trap device of the product collecting unit starts to work, and the temperature is-10-0 ℃;
(3) And (3) on-system target: taking out the Bi target after standing in the step (1), transferring the Bi target to a gasification separation unit through a lead box, and installing the Bi target on a quartz target table in a reducing quartz tube;
(4) And (3) system setting: the gas control unit controls the flow rate of the inert gas to be 4-20 mL/min and the inert gas enters the system; heating the tube furnace to 700-750 ℃ at a heating rate of 10-50 min/DEG C, preserving heat for 5-10 min, heating to 750-1000 ℃ at the same heating rate, and preserving heat for 5-15 min; the temperature of the heating belt is 200-200 ℃; when the temperature of the tube furnace reaches 400-450 ℃, the temperature of the second-stage cold trap is minus 20-minus 15 ℃; when the temperature of the tube furnace reaches 450-500 ℃, the temperature of the third-stage cold trap is minus 30-minus 25 ℃; when the temperature of the tube furnace reaches 500-550 ℃, the temperature of the fourth-stage cold trap is minus 50-minus 45 ℃; when the temperature of the tube furnace reaches 550-600 ℃, the temperature of the fifth-stage cold trap is minus 100-minus 60 ℃; when the temperature of the tube furnace reaches 650-750 ℃, the temperature of the sixth-stage cold trap is minus 250-minus 100 ℃; the tail gas treatment unit is used for treating the gas output after the sixth-stage cold trap;
(5) And (3) leaching the product: the heating of the tube furnace is completed, the natural cooling is completed to 600-700 ℃, the gas control unit stops working, meanwhile, the leaching device is started, the peristaltic pump pumps the leacheate stored in the centrifuge tube into the collecting tube, and the leacheate brings the At-211 into the product tube to obtain an At-211 product
The invention has the following beneficial effects:
(1) The inert gas is filtered and dried by adopting a dryer and a filter, so that the reaction of moisture, oxygen and the like in the inert gas on the At-211 is avoided to generate products with different valence states, and the chemical purity of the products is further improved; and the gas flow rate of the inert gas carrying system is controlled by the micro gas flow controller, so that the At-211 separated by the gasification separation unit can be ensured to smoothly enter the product collecting unit, and the collecting efficiency of the product collecting unit can be ensured.
(2) The Bi target is installed by adopting the variable-diameter quartz tube, so that the radiation injury of the target scraping action to operators is avoided, the gasified At-211 completely enters the product collecting unit through the variable-diameter outlet, and the product collecting unit is heated by matching with the heating belt, so that the problem of low product yield caused by enrichment of the At-211 At the outlet can be avoided.
(3) The tube furnace heats the variable diameter quartz tube by adopting a preheating and step heating mode, so that the quartz tube is heated uniformly, a Bi target can be completely released, and the yield of products is further improved.
(4) The six-stage variable-temperature cold trap is adopted to enable gasified At-211 to be well sublimated in the collecting pipe, the controllable range of the overall temperature is minus 250-0 ℃, the temperature of each stage of cold trap component is gradually reduced in a decreasing mode, the cold trap components are sequentially arranged in the same air flow direction, and the cold trap temperature is set in cooperation with the heating temperature of the tube furnace, so that the movement of the At-211 to the rear end of the system is effectively prevented, the dosage of absorption liquid and active carbon in the tail gas treatment system is reduced, meanwhile, the rear end of the active carbon is free from enrichment of radioactive substances, and the system is ensured to be free from radioactive substances overflowing the atmosphere; meanwhile, the leaching device can also reduce the volume of the product and ensure the yield.
(5) The tail gas treatment device is adopted to treat the gas after the sixth-stage cold trap, so that the rest At-211 is prevented from entering the atmosphere, radiation is caused to the environment and operators, and meanwhile, the vacuum pump and the pressure gauge can also control the vacuum degree in the system, and the vacuum degree of the system is low and only needs hundred Pa.
(6) The radiation shielding unit is used for shielding the tubular furnace, so that the radiation of the Bi target releasing process to operators can be effectively reduced.
(7) Experiments prove that the At-211 product produced by the system has high purity and wide application range, almost reaches 100 percent of nuclear purity and chemical purity, and is suitable for related researches such as radionuclide targeted therapeutic drug synthesis, alpha radiolysis and the like; the separation effect is good, and the yield can be stabilized between 85 and 95 percent; the cost is low, the operability is high, the safety is high, the high vacuum requirement is not needed, the production cost is greatly reduced, and the operability of equipment is enhanced; the system has the advantages of modularized design, strong system adaptability and simple system structure, and can be applied to dry distillation production of other nuclides.
Drawings
FIG. 1 is a schematic diagram of a production system of the present invention.
FIG. 2 is a schematic diagram of the apparatus of the production system of the present invention.
Fig. 3 is a schematic diagram of the structure of the gas control unit of the present invention.
FIG. 4 is a schematic transverse cross-sectional view of a diameter-variable quartz tube according to the present invention.
Fig. 5 is a schematic longitudinal section of the diameter-variable quartz tube of the present invention.
FIG. 6 is a gamma energy spectrum of At-211 produced by the present invention.
The marks in the figure: 100. a gas control unit; 101. a gas drying tube; 102. a one-way regulating valve; 103. an intake pressure gauge; 104. a micro gas flow controller; 105. a filter; 200. a gasification separation unit; 220. a reducing quartz tube; 221. a quartz outer tube; 222. a quartz boat; 223. a quartz target stage; 230. a quick-release reducer union; 240. a heating belt; 300. a product collection unit; 310. a cold trap device; 320. a collection pipe; 330. a rinsing device; 400. a tail gas treatment unit; 401. a check valve; 402. a tail gas absorption tube; 403. a vacuum pressure gauge; 404. u-shaped active carbon tube; 500. a radiation shielding unit; 600. a system control unit; 700. bi target.
Detailed Description
Example 1
As shown in fig. 1 and 2, the low vacuum high purity At-211 dry distillation production system provided in this embodiment includes a gas control unit 100, a gasification separation unit 200, a product collection unit 300, a tail gas treatment unit 400, and a radiation shielding unit 500.
The gas control unit 100 is used for controlling the gas flow speed and enabling the gasified At-211 to flow along the gas flow direction so as to collect the At-211 product; as shown in FIG. 3, it includes an inert gas storage tank (not shown in FIG. 3), a gas drying pipe 101, a one-way regulating valve 102, an air inlet pressure gauge 103, a trace gas flow controller 104 and a filter 105, wherein the inert gas storage tank, the gas drying pipe 101, the filter 105, the one-way regulating valve 102, the air inlet pressure gauge 103 and the trace gas flow controller 104 are sequentially connected through pipelines, inert gas such as nitrogen is stored in the inert gas storage tank, the inert gas flows in the system through the inert gas, so that the gasified At-211 flows to the next unit, the gas drying pipe 101 is used for drying the inert gas output by the inert gas storage tank, the inert gas is prevented from having moisture, other gases such as oxygen are filtered out after the dried inert gas is filtered by the filter 105, the purity of the inert gas is ensured, the components such as oxygen and the moisture are prevented from oxidizing the At-211 in the gasification separation unit 200, then the air inlet pressure gauge 103 detects the air inlet pressure signal, and the control gas is controlled within a proper pressure range, the pressure is in a low vacuum environment, so that the pressure is-0.4 to-1.2 kPa or the gasified product is prevented from flowing through the gasification separation unit 200, the flow rate is also ensured to be reasonable, and the product collection efficiency is ensured after the gasified by the gas is prevented from flowing through the gasification separation unit 200.
The gas flow rate in this embodiment is controlled to be 4-20 mL/min, and the flow rate is sufficient to ensure that the gasified At-211 in the gasification separation unit 200 performs controllable movement along with the airflow direction, and finally most of the gas enters the product collection unit 300, thereby ensuring stable and efficient separation.
The gasification separation unit 200 is used for heating and gasifying the Bi target 700 bombarded by ion beams to obtain gasified At-211, and comprises a tube furnace, a variable diameter quartz tube 220 and a quick-release reducer union 230, wherein the tube furnace is used for heating and gasifying the At-211 on the Bi target 700, the variable diameter quartz tube 220 is used for installing the Bi target 700 and is arranged in the tube furnace, and as shown in fig. 4, the tube furnace comprises a quartz outer tube 221, a quartz boat 222 and a quartz target table 223; the Bi target 700 is arranged on the quartz target table 223, the quartz target table 223 is arranged in the quartz boat 222, the quartz boat 222 is arranged in the quartz outer tube 221, the matching gap deviation of each component is not more than 1% during production, the quartz tube can relatively fix the Bi target 700, the Bi melted at high temperature is limited at a certain position, and the service life of the quartz outer tube 221 is ensured. The installed Bi target 700 is flush with the center of the quartz outer tube 221, and the inlet and outlet of the variable diameter quartz tube 220 are on the central line, so that the smooth air flow in the system can be ensured, and the gasified At-211 on the Bi target 700 can be smoothly brought into the product collecting unit 300.
The outlet of the reducing quartz tube 220 is in a conical structure, so that a reducing outlet is realized, the conical structure is connected with the quick-release reducing joint 230, the quick-release reducing joint 230 is reduced again, a pipeline after reducing is thinner, the subsequent product collecting unit 300 is convenient for comprehensively cooling and collecting products, the yield of the products is improved, the gasified At-211 completely enters the product collecting unit 300 along the reducing outlet, a heating belt 240 is arranged At the outlet of the quartz outer tube 221 and on the quick-release reducing joint 230, the temperature At the outlet is controlled by the sensor and the control module, and the enrichment of the products At the joint due to the sudden reduction of the gas path temperature can be effectively prevented, so that the effect of improving the yield is achieved.
The embodiment firstly controls the tube furnace to heat in a step heating mode, can uniformly heat the inside of the variable diameter quartz tube 220, so that the Bi target 700 is completely heated and is fully gasified, specifically, firstly, the temperature is raised to 700-750 ℃ at the heating rate of 10-50 min/DEG C, and the temperature is kept for 5-10 min, so that the center temperature of the tube furnace is uniform; heating the Bi target 700 in the quartz tube At the same heating rate to 750-1000 ℃ and preserving heat for 5-15 min, gasifying the At-211, conveying the gasified At-211 to the product collecting unit 300, and simultaneously controlling the heating belt 240 to heat the outlet of the quartz tube At the heating temperature of 90-260 ℃, wherein the heating belt 240 can avoid the product yield reduction caused by enrichment of the product At the outlet due to sudden temperature drop.
The product collecting unit 300 is configured to desublimate gasified At-211 into solid At-211, and collect the product, as shown in fig. 5, by adopting six-stage variable-temperature cold trap assemblies, each stage of cold trap assemblies has the same structure and is connected end to end, the cold trap assemblies comprise a cold trap device 310, a collecting pipe 320 and a leaching device 330, the collecting pipe 320 is installed in the cold trap device 310, the inlet of the cold trap device is connected with the outlet of the gasification separating unit 200, the cold trap device 310 reduces the temperature in the collecting pipe 320, and further causes the gasified At-211 to desublimate into solid At-211, and is attached to the inner wall of the collecting pipe 320, and is connected with a leaching device 330 At the outlet of the collecting pipe 320 through a three-way valve, the leaching device 330 comprises a centrifuge tube for storing leaching liquid, a peristaltic pump, the inlet of the peristaltic pump is connected with the centrifuge tube, the outlet of the collecting pipe 320 is connected with the outlet of the collecting pipe 320, and the peristaltic pump pumps the leaching liquid into the collecting pipe 320, and the leaching liquid enters the collecting pipe 320 in the direction opposite to the direction of the air flow, and the leaching pipe 320, thereby reducing the volume of the solid At-211 and discharging the solid product.
Specifically, the temperature of the six-stage variable temperature cold trap assembly is set as follows:
the first-stage cold trap starts to operate in the system preparation stage, and the temperature is-10-0 ℃; the second-stage cold trap starts to operate when the temperature of the tubular furnace reaches 400-450 ℃, and the temperature is minus 20-minus 15 ℃; the third-stage cold trap starts to operate when the temperature of the tube furnace reaches 450-500 ℃ and the temperature is minus 30-minus 25 ℃; the fourth-stage cold trap starts to operate when the temperature of the tubular furnace reaches 500-550 ℃, and the temperature is minus 50-minus 45 ℃; the fifth stage cold trap starts to operate when the temperature of the tube furnace reaches 550-600 ℃ and the temperature is minus 100-minus 60 ℃; the sixth-stage cold trap starts to operate when the temperature of the tubular furnace reaches 650-750 ℃ and is between-250 ℃ and-100 ℃.
The time and temperature decreasing control of the cold trap can effectively interfere the airflow velocity in the system, so that the gasified At-211 is well sublimated in the area where the collecting pipe 320 is positioned, if the design is less than 6 stages of cold traps, the setting reference of the front end cold trap is consistent, and the operation temperature and time of the last stage are set to be the same according to the 6 th stage.
The collecting pipe 320 is made of a custom glass pipe or a polymer material pipe, the polymer material is PTFE, FEP, PFA, ETFE, the inner diameter of the collecting pipe 320 is less than or equal to 3.175mm, the single-stage length is 800-1500 mm, and the more the number of stages is, the shorter the length of the single-stage collecting pipe 320 is, and the 2-6 stages are generally set.
The leaching solution adopts one of high-purity water, methanol, ethanol, methylene dichloride, chloroform, carbon tetrachloride, nitric acid and sodium hydroxide, the volume of the product At-211 is controlled within 0.5mL generally, and when the methylene dichloride is taken as the leaching solution, the product can be quickly dried, the loss rate is less than or equal to 2%, and the requirements of the related research work of alpha radiolysis are met.
The tail gas treatment unit 400 is used for treating gas after the product collection unit 300, preventing gasified At-211 from entering the atmosphere to pollute the environment, and comprises a check valve 401, a tail gas absorption device 402, a vacuum pressure gauge 403, a U-shaped active carbon tube 404 and a vacuum pump, wherein the check valve 401 is arranged on an outlet of a cold trap assembly At the last stage, the check valve 401, the tail gas absorption tube 402, the vacuum pressure gauge 403, the U-shaped active carbon tube 404 and the vacuum pump are sequentially connected through pipelines, and the tail gas absorption tube 402 is filled with one tail gas absorption liquid of NaOH, methanol, ultrapure water, dilute nitric acid and an extractant. The tail gas absorption liquid and the U-shaped active carbon tube can effectively prevent radioactive pollution caused by the gasified At-211 entering the atmosphere, and meanwhile, the vacuum pump provides lower negative pressure of-0.4 to-1.2 kPa for the system, so that the gasified At-211 can enter the product collecting unit 300 more quickly, and the purpose of energy saving can be achieved.
The radiation shielding unit 500 is used for radiation shielding, and can effectively reduce radiation exposure to operators, and comprises a box body, wherein the gas control unit 100, the gasification separation unit 200, the product collection unit 300 and the tail gas treatment unit 400 are arranged in the box body, and particularly, a movable lead glass component is arranged in the box body to enclose the gasification separation unit 200, and meanwhile, lead glass is also arranged on a box door of the box body, so that the conditions in the box body can be observed, and the damage of radiation to the operators can be further prevented.
The present embodiment further provides a system control unit 600, configured to adjust the start-up operation between the units, so as to implement collaborative intelligent generation At-211.
Example 2
The embodiment is a generation method based on the low vacuum high purity At-211 production system provided in the embodiment 1, comprising the following steps:
(1) Bombarding a Bi target 700: bombarding the Bi target 700 by adopting a CS-30 cyclotron for 4-5 hours, and then standing for 30 minutes, and taking out the Bi target 700; wherein the alpha beam current parameter of the CS-30 cyclotron is 28MeV, 15-20 mu A;
(2) Preparing a system: when the Bi target 700 is bombarded, a system can be prepared, firstly, pipeline connection of a production system and the opening condition of valves are detected, and the vacuum degree of the system is set by adopting a vacuum pump of the tail gas treatment unit 400 under the condition of no error, wherein the vacuum degree is-0.4 to-1.2 kPa; then opening a tube furnace preheating diameter-reducing quartz tube 220, wherein the preheating temperature is 200-300 ℃; the first stage cold trap device 310 of the product collection unit 300 starts to operate at-10-0 ℃;
(3) And (3) on-system target: taking out the Bi target 700 after standing in the step (1), transferring the Bi target 700 to the gasification separation unit 200 through a lead box, installing the Bi target 700 on a quartz target table 223 in the variable-diameter quartz tube 220, and checking the vacuum degree of the system;
(4) And (3) system setting: the gas control unit 100 controls the flow rate of the inert gas to be 4-20 mL/min and the inert gas enters the system; heating the tube furnace to 700-750 ℃ at a heating rate of 10-50 min/DEG C, preserving heat for 5-10 min, heating to 750-1000 ℃ at the same heating rate, and preserving heat for 5-15 min; the temperature of the heating belt 240 is 90-260 ℃; when the temperature of the tube furnace reaches 400-450 ℃, the temperature of the second-stage cold trap is minus 20-minus 15 ℃; when the temperature of the tube furnace reaches 450-500 ℃, the temperature of the third-stage cold trap is minus 30-minus 25 ℃; when the temperature of the tube furnace reaches 500-550 ℃, the temperature of the fourth-stage cold trap is minus 50-minus 45 ℃; when the temperature of the tube furnace reaches 550-600 ℃, the temperature of the fifth-stage cold trap is minus 100-minus 60 ℃; when the temperature of the tube furnace reaches 650-750 ℃, the temperature of the sixth-stage cold trap is minus 250-minus 100 ℃; the tail gas treatment unit 400 is used for treating the gas output after the sixth-stage cold trap;
(5) And (3) leaching the product: the heating of the tube furnace is completed, the natural cooling is carried out to 600-700 ℃, the gas control unit 100 stops working, meanwhile, the leaching device 330 is started, and a peristaltic pump pumps the leaching liquid in the centrifuge tube into the collecting tube 320; the At-211 in collection tube 320 is then transferred to a product tube to obtain a product.
The production system of example 1 and the production method of example 2 were used to obtain an At-211 product, and the At-211 product was examined.
Wherein the inert gas in the production system adopts nitrogen; the outer diameter of the heating zone of the reducing quartz tube 220 is 45mm; the collecting pipe 320 is made of high silicon glass pipe, the outer diameter is 3mm, the single-stage length is 850mm, and the number of stages is 6; methanol is adopted as the tail gas absorption liquid; the system parameter settings are shown in table 1.
TABLE 1 production System parameter settings
The production site At-211 product A, B, C, D was set according to the above-described production system, and the irradiation conditions of the respective units after the completion of the production were examined as shown in table 2, and the product yields were as shown in table 3.
TABLE 2 Table 2 radiation conditions throughout production System
TABLE 3 product yields
The gamma energy spectrum obtained by the detection of the product by using the high-purity germanium detector is shown in a figure 6, no characteristic peak of At-210 At 1181.39keV and other At-210 is shown in the spectrum, namely the product of the invention does not contain impurity At-210, the existing embodiment contains 2-9ppm of At-210 impurity, and no other irrelevant characteristic peak appears in the spectrum At the same time, which indicates that the purity of the product obtained by the invention is higher. Each peak in the spectrogram is definite in attribution and is a characteristic peak of At-211 or decay daughter thereof, which indicates that the nuclear purity of the product is nearly 100%; the sample after the complete decay of the product is subjected to ICP-MS test, other hetero elements such as Bi, cu and the like are not detected, and the chemical purity of the product is nearly 100%.
The foregoing is merely a preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any modification and substitution based on the technical scheme and the inventive concept provided by the present invention should be covered in the scope of the present invention.
Claims (8)
1. A low vacuum high purity At-211 dry distillation production system is characterized in that: comprises a gas control unit, a gasification separation unit, a product collection unit and a tail gas treatment unit;
the gas control unit is used for controlling the gas flow speed and enabling the gasified At-211 to flow along the gas flow direction so as to collect the At-211 product; the device comprises an inert gas storage tank, a gas drying pipe, a one-way regulating valve, an air inlet pressure gauge, a micro gas flow controller and a filter, wherein the inert gas storage tank, the gas drying pipe, the one-way regulating valve, the air inlet pressure gauge and the micro gas flow controller are sequentially connected through pipelines, inert gas is stored in the inert gas storage tank, the inert gas is dried and filtered, the flowing speed of the inert gas is controlled by the micro gas flow controller to enter a gasification separation unit, and gasified At-211 is transferred to a product collecting unit under the flowing of the inert gas;
the gasification separation unit is used for heating and gasifying Bi targets bombarded by ion beams to release At-211 and comprises a tubular furnace, a reducing quartz tube and a quick-release reducing joint, wherein the tubular furnace is used for heating to gasify the At-211 on the Bi targets, the reducing quartz tube is used for installing the Bi targets and is arranged in the tubular furnace, the outlet of the reducing quartz tube is in a conical structure, the conical structure is connected with the product collection unit through the quick-release reducing joint, and heating belts are arranged At the outlet of the reducing quartz tube and on the quick-release reducing joint;
the product collecting unit is used for desublimating gasified At-211 into solid At-211 to collect products, and adopts six-stage variable-temperature cold trap assemblies, each stage of cold trap assembly has the same structure and is connected end to end, the cold trap assembly comprises a cold trap device, a collecting pipe and a leaching device, the collecting pipe is arranged on the cold trap device, the inlet of the collecting pipe is connected with the outlet of the gasification separating unit, and the outlet of the collecting pipe is connected with the leaching device through a three-way valve; the cold trap device reduces the temperature in the collecting pipe, so that the gasified At-211 is sublimated into solid At-211, the solid At-211 is attached to the inner wall of the collecting pipe, and the solid At-211 is leached by the leaching device to obtain a product; the temperature of each six-stage variable temperature cold trap assembly is set as follows: the first-stage cold trap starts to operate in the system preparation stage, and the temperature is-10-0 ℃; the second-stage cold trap starts to operate when the temperature of the tubular furnace reaches 400-450 ℃, and the temperature is minus 20-minus 15 ℃; the third-stage cold trap starts to operate when the temperature of the tube furnace reaches 450-500 ℃ and the temperature is minus 30-minus 25 ℃; the fourth-stage cold trap starts to operate when the temperature of the tubular furnace reaches 500-550 ℃, and the temperature is minus 50-minus 45 ℃; the fifth stage cold trap starts to operate when the temperature of the tube furnace reaches 550-600 ℃ and the temperature is minus 100-minus 60 ℃; the sixth-stage cold trap starts to operate when the temperature of the tubular furnace reaches 650-750 ℃ and is between-250 ℃ and-100 ℃;
the tail gas treatment unit is used for treating the gas after the product collecting unit to prevent the balance At-211 from entering the atmosphere to pollute the environment, and comprises a check valve, a tail gas absorption pipe, a vacuum pressure gauge, a U-shaped active carbon pipe and a vacuum pump, wherein the check valve is arranged on an outlet of a cold trap component of the last stage, the check valve, the tail gas absorption pipe, the vacuum pressure gauge, the U-shaped active carbon pipe and the vacuum pump are sequentially connected through pipelines, and tail gas absorption liquid is filled in the tail gas absorption pipe.
2. The low vacuum high purity At-211 retort production system according to claim 1, wherein: the reducing quartz tube comprises a quartz outer tube, a quartz boat and a quartz target table; the Bi target is arranged on the quartz target table, the quartz target table is arranged in the quartz boat, the quartz boat is arranged in the quartz outer tube, the installed Bi target is level with the center of the quartz outer tube, and the inlet and outlet of the variable-diameter quartz tube are all on the central line.
3. The low vacuum high purity At-211 retort production system according to claim 1, wherein: the collecting pipe adopts a customized glass pipe or a polymer material pipe, the inner diameter of the collecting pipe is less than or equal to 3.175mm, and the single-stage length is 800-1500 mm.
4. The low vacuum high purity At-211 retort production system according to claim 1, wherein: the leaching device comprises a centrifuge tube for storing leaching liquid and a peristaltic pump, wherein an inlet of the peristaltic pump is connected with the centrifuge tube, an outlet of the peristaltic pump is connected with an outlet of the collecting tube, and the peristaltic pump pumps the leaching liquid into the collecting tube in a direction opposite to the air flow direction.
5. The low vacuum high purity At-211 retort production system according to claim 4, wherein: the leaching solution adopts one of high-purity water, methanol, ethanol, methylene dichloride, chloroform, carbon tetrachloride, hydrochloric acid, nitric acid and sodium hydroxide.
6. The low vacuum high purity At-211 retort production system according to claim 1, wherein: the tail gas absorption liquid adopts one of sodium hydroxide, methanol, ultrapure water, dilute nitric acid and an extracting agent.
7. The low vacuum high purity At-211 retorting production system according to any one of claims 1 to 6, characterized in that: the device also comprises a radiation shielding unit for playing a radiation shielding role, and the device comprises a box body and a lead glass component, wherein the box body is used for integrally installing a gas control unit, a gasification separation unit, a product collection unit and a tail gas treatment unit, and the lead glass component encloses and isolates the gasification separation unit.
8. A method of producing At-211 using the retorting production system as claimed in claim 1, which includes the steps of:
(1) Bombarding Bi targets: bombarding the Bi target by adopting a CS-30 cyclotron for 4-5 hours, and then standing for 30 minutes, and taking out the Bi target; wherein the alpha beam current parameter of the CS-30 cyclotron is 28MeV, 15-20 mu A;
(2) Preparing a system: the system preparation can be made during Bi target bombardment, firstly, pipeline connection of a production system and the opening condition of valves are detected, and the vacuum degree of the system is set by adopting a vacuum pump of a tail gas treatment unit under the condition of no error, wherein the vacuum degree is-0.4 to-1.2 kPa; then opening the tube furnace to preheat the variable-diameter quartz tube, wherein the preheating temperature is 200-300 ℃; the first stage cold trap device of the product collecting unit starts to work, and the temperature is-10-0 ℃;
(3) And (3) on-system target: taking out the Bi target after standing in the step (1), transferring the Bi target to a gasification separation unit through a lead box, and installing the Bi target on a quartz target table in a variable-diameter quartz tube;
(4) And (3) system setting: the gas control unit controls the flow rate of the inert gas to be 4-20 mL/min and the inert gas enters the system; heating the tube furnace to 700-750 ℃ at a heating rate of 10-50 min/DEG C, preserving heat for 5-10 min, heating to 750-1000 ℃ at the same heating rate, and preserving heat for 5-15 min; the temperature of the heating belt is 90-260 ℃; when the temperature of the tube furnace reaches 400-450 ℃, the temperature of the second-stage cold trap is minus 20-minus 15 ℃; when the temperature of the tube furnace reaches 450-500 ℃, the temperature of the third-stage cold trap is minus 30-minus 25 ℃; when the temperature of the tube furnace reaches 500-550 ℃, the temperature of the fourth-stage cold trap is minus 50-minus 45 ℃; when the temperature of the tube furnace reaches 550-600 ℃, the temperature of the fifth-stage cold trap is minus 100-minus 60 ℃; when the temperature of the tube furnace reaches 650-750 ℃, the temperature of the sixth-stage cold trap is minus 250-minus 100 ℃; the tail gas treatment unit is used for treating the gas output after the sixth-stage cold trap;
(5) And (3) leaching the product: the heating of the tube furnace is completed, the natural cooling is carried out to 600-700 ℃, the gas control unit stops working, meanwhile, the leaching device is started, the peristaltic pump pumps the leacheate stored in the centrifuge tube into the collecting tube, and the leacheate brings the At-211 into the product tube to obtain the At-211 product.
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