CN114937516A - Production and preparation based on accelerator irradiation 68 Method for Ge - Google Patents

Production and preparation based on accelerator irradiation 68 Method for Ge Download PDF

Info

Publication number
CN114937516A
CN114937516A CN202210561881.9A CN202210561881A CN114937516A CN 114937516 A CN114937516 A CN 114937516A CN 202210561881 A CN202210561881 A CN 202210561881A CN 114937516 A CN114937516 A CN 114937516A
Authority
CN
China
Prior art keywords
solution
separation
metal
nickel alloy
switching valve
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
CN202210561881.9A
Other languages
Chinese (zh)
Inventor
王洁茹
秦芝
高瑞勤
曹石巍
刘宁
黄清钢
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sichuan University
Institute of Modern Physics of CAS
Original Assignee
Sichuan University
Institute of Modern Physics of CAS
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Sichuan University, Institute of Modern Physics of CAS filed Critical Sichuan University
Priority to CN202210561881.9A priority Critical patent/CN114937516A/en
Publication of CN114937516A publication Critical patent/CN114937516A/en
Pending legal-status Critical Current

Links

Images

Classifications

    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/20—Recycling

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Manufacture And Refinement Of Metals (AREA)

Abstract

The invention discloses a production method based on accelerator irradiation 68 A method of Ge. The method comprises the following steps: s1, preparing a metal gallium-nickel alloy target, and then dissolving the metal gallium-nickel alloy target after irradiation; the structure of the metal gallium nickel alloy target is 1) or 2) as follows: 1) at least comprises two layers including a metal substrate layer and a metal gallium nickel alloy layer; 2) at least comprises three layers including a metal substrate layer, a metal protection layer and a metal gallium nickel alloy layer; s2, introducing the dissolved solution into a double-tandem chromatographic column for separation and purification, and collecting the solution containing 68 A solution of Ge; s3, the obtained mixture contains 68 Introduction of Ge solution 68 Ge/ 68 In a Ga generator, when 68 After the Ge is fully adsorbed, eluting with an eluent pair at preset intervals 68 Ge/ 68 Eluting the separation column in the Ga generator, and collecting eluted eluate to obtain 68 Ga products. The invention 68 The separation and purification process of Ge has clear thought, simple operation, easy realization of automatic separation and purification, and high purityOf radioactive concentration 68 Ge。

Description

Based on acceleratorIrradiation production preparation 68 Method for Ge
Technical Field
The invention relates to a production method based on accelerator irradiation 68 A Ge method, belonging to the technical field of positron tomography.
Background
At present, at home and abroad 68 The production and separation process of Ge mainly includes solvent extraction, fractional distillation and chromatographic separation. In the solvent extraction separation process, organic reagents with high toxicity and carcinogenicity, such as carbon tetrachloride, toluene and the like, are commonly used as extracting agents for extraction separation 68 And Ge. Furthermore, the solvent extraction is carried out under conditions of high acidity, so that 68 Easy formation of Ge 68 GeCl 4 Aerosol, cause of 68 A large loss of Ge. The other is used for separation and purification 68 The Ge process is a fractional distillation process based mainly on acidic solutions 68 GeCl 4 (the boiling point is 82-84 ℃) and is very volatile, and the heating mode is utilized to heat the mixture 68 Ge is separated from the irradiated target and other impurity species. But produced by this process 68 The recovery rate of Ge is low, and radioactive leakage is easy to cause, and pollution is brought.
The chromatographic separation process is separation 68 The common separation method of Ge can realize continuous separation 68 The operation of Ge is very favorable for the design and control of automatic separation, and simultaneously, the operation can be avoided 68 A large loss of Ge. However, in the case of chromatographic processes, they are purified separately 68 The Ge radioactivity concentration and purity are relatively low, therefore, how to establish a compound medical use capable of obtaining high radioactivity concentration and specific activity 68 Ge, and can be automatically produced in large scale 68 The process of chromatography of Ge is very important.
Disclosure of Invention
The invention aims to provide production of a metal gallium-nickel alloy target irradiated by an accelerator 68 Ge method, and establishes a dual-chromatographic-column series separation process with Chelex100 and glucose gel separation columns and capable of being recycled, and meanwhile, the process is applied to automationSeparation system, successfully obtained 68 A Ge product; the method is simple and easy to implement, the principle of the automatic system is simple, the operation is convenient, and the realization is easy 68 And (5) large-scale production of Ge.
The invention firstly provides 68 The automatic Ge separation system comprises a liquid taking unit, a conveying unit, a monitoring unit, a pH value regulating and controlling unit, a separating unit, a collecting unit and a control unit;
the liquid taking unit and the collecting unit comprise a plurality of liquid storage containers and liquid conveying pipelines; the conveying unit comprises at least one peristaltic pump and four multi-channel switching valves; the monitoring unit comprises at least one liquid level sensor; the pH value regulating and controlling unit comprises at least one pH value monitor and an injection pump with a switching valve head; the separation unit at least comprises two identical or different separation columns; the collecting unit comprises a plurality of collecting containers and a liquid recovery pipeline; the control unit comprises an upper computer, a Programmable Logic Controller (PLC), control software, a communication protocol and the like;
the control unit controls the first multi-channel switching valve to rotate to a preset channel to absorb the solution in the liquid storage container of the liquid taking unit; the output end of the first multi-channel is connected with the input end of a peristaltic pump, the output end of the peristaltic pump is connected with the input end of a second multi-channel switching valve, the output end of the second multi-channel switching valve is connected with the inlets of at least two same or different separation columns, the outlets of the separation columns are connected with the input end of a third multi-channel switching valve, and the second and third switching valves are freely rotated by the control unit to be in two states of flowing through the separation columns or not flowing through the separation columns; the output end of the third multi-channel switching valve is connected with the input end of a fourth multi-channel switching valve, the output end of the fourth multi-channel switching valve is connected with the collection container of the collection unit, and the fourth multi-channel switching valve is used for introducing the liquid passing through the separation column into the corresponding recovery pipeline and entering the collection unit; the liquid level sensor of the monitoring unit is connected between the first multi-channel switching valve and the peristaltic pump and is used for monitoring whether the control unit completely extracts the solution; the pH value monitor and the injection pump with the switching valve head in the pH value regulating and controlling unit are connected to a collecting container of the collecting unit and used for regulating the pH value of the solution;
the multi-channel switching valve is at least a six-channel switching valve;
the liquid of the liquid storage container at least comprises solution of irradiated metal gallium nickel target, hydrochloric acid solution, alkaline solution, 0.001-1.5 mol/L sodium citrate alkaline solution and deionized water;
at least comprises a spare separation column system.
In the above-mentioned 68 Based on an automatic Ge separation system, the invention provides a method for producing and preparing a metallic gallium-nickel alloy target based on accelerator irradiation 68 A method of Ge comprising the steps of:
s1, preparing a metal gallium-nickel alloy target, and then dissolving the metal gallium-nickel alloy target after irradiation;
the structure of the metal gallium nickel alloy target is 1) or 2) as follows:
1) at least comprises two layers including a metal substrate layer and a metal gallium nickel alloy layer;
2) at least comprises three layers including a metal substrate layer, a metal protective layer and a metal gallium-nickel alloy layer;
s2, introducing the dissolved solution into a double-tandem chromatographic column for separation and purification, and collecting the solution containing 68 A solution of Ge;
the double tandem chromatographic columns are a Chelex100 separation column and a glucose gel separation column which are connected in series;
s3, the obtained mixture contains 68 Introduction of Ge solution 68 Ge/ 68 In a Ga generator, when 68 After the Ge is fully adsorbed, the leaching solution is used for leaching the Ge at preset time intervals 68 Ge/ 68 Eluting the separation column in the Ga generator, and collecting eluted eluate to obtain 68 And (4) Ga products.
In the above method, in step S1, the material of the metal first underlayer is Cu or Al, and the metal first underlayer is a metal having high electrical conductivity, thermal conductivity, and hardness;
the metal protective layer is made of Au or Pt, has the thickness of at least 5 mu m, and is made of inert metal with strong electric and thermal conductivity;
in the metal gallium-nickel alloy layer, the Ga mass content is not less than 50%, and the thickness is more than 10mg/cm 2 。
In the above method, in step S1, the metal gallium-nickel alloy layer is prepared by an electroplating method;
the plating solution can be an acidic solution, the acidity is 0.001-2 mol/L, the temperature is 25-100 ℃, and the current density is 10-60 mA/cm 2 The molar concentration ratio of the gallium ions to the nickel ions is 1-10, and the stirring speed is 5-500 rpm.
And (3) irradiating by using a proton accelerator, wherein the energy is 10-70 MeV, the flow intensity is 10-500 muA, the time is not less than 1h, and the cooling time is at least 20 days.
In the method, in the step S2, a mixed system of an acidic solution and hydrogen peroxide is adopted for dissolving, wherein the concentration of the acidic solution is more than 10mol/L, the concentration of the hydrogen peroxide is 10-30%, and the dissolving temperature is 25-150 ℃;
the target solution after dissolving and irradiation is a clear and transparent solution, and the solution at least contains 68 Ge、 68,nat Ga、 56,57,58 Co、 65 Zn、 nat Ni and nat cu, and the like.
In the above method, in step S2, the separation and purification conditions are as follows:
adjusting the pH value of the solution obtained after the metal gallium nickel target is dissolved to 1.0-5.0, introducing the solution into the Chelex100 separation column, leaching the solution by adopting a hydrochloric acid solution with the pH value of 1.0-5.0, and collecting leacheate; simultaneously adding 0.6-1.5mol/L sodium citrate solution into the leacheate, adjusting the pH value to 10.0-13.0, introducing the glucose gel separation column, and leaching by adopting 0.001-1.5 mol/L, pH of 10.0-13.0 sodium citrate solution, 10.0-13.0 alkaline solution and deionized water in sequence; finally, introducing 0.1-2.0 mol/L hydrochloric acid solution into the glucose gel separation column, desorbing and collecting 68 And (4) Ge product.
In the above method, in step S2, after the separation and purification, hydrochloric acid, deionized water, sodium hydroxide, and deionized water are sequentially introduced into the Chelex100 separation column to regenerate the separation column;
the glucose gel separation column can be directly recycled without further treatment.
In the above method, in step S2, the method is implemented by 68 And the Ge separation automation system controls the separation and purification.
In the above method, in step S3, the method is 68 Ge/ 68 The packing material used for the separation column in the Ga generator is a metal oxide or an oxide-based organic resin (e.g., a silica-based phloroglucinol resin, etc.).
The described 68 Ge/ 68 The structure of the Ga generator is as follows: the separation column is arranged in the shielding layer; two ends of the separation column are respectively connected with a liquid inlet hose and a liquid outlet hose, and the liquid inlet hose and the liquid outlet hose are respectively connected with an injector and a collection bottle through a plate penetrating joint;
the injector is connected with a hose through a luer connector, the hose is connected with the plate penetrating connector, the injector is extruded to convey liquid into the separation column, and the liquid passes through the separation column and then is delivered to the separation column 68 The Ga product enters the collecting bottle to be collected;
the shielding layer comprises a lead shielding layer and a generator shell.
In the above method, in step S3, the method includes 68 Adjusting the acidity (0.5-2.0 mol/L) of Ge solution, and introducing into the solution 68 Ge/ 68 In the separation column in a Ga generator.
Can be determined by 68 The radiochemical purity, radionuclide purity and chemical purity of Ga are finished, 68 labelling of Ga for inspection 68 Availability of Ga.
Due to the adoption of the technical scheme, the invention has the following advantages:
the invention 68 The separation and purification process of Ge has clear thought, simple operation, easy realization of automatic separation and purification and high purity and radioactive concentration 68 And Ge. The designed automatic separation and purification system can realize the series connection of a plurality of separation columns and can be used as a standby separation system, thereby effectively ensuring the use reliability and safety of the automatic separation and purification system. 68 Ge/ 68 The Ga generator has simple design and easy operationObtained by 68 The Ga has high purity and can be applied to the preparation of radiopharmaceuticals.
Drawings
FIG. 1 is 68 Schematic diagram of Ge automatic separation
FIG. 2 is 68 And (4) connecting all parts in the Ga automatic separation system.
FIG. 3 shows the production of irradiated metal gallium-nickel alloy target according to the present invention 68 Flow chart of Ge method.
Fig. 4 is a photograph of a metallic gallium-nickel alloy target.
FIG. 5 is 68 Gamma spectra before and after Ge separation.
FIG. 6 is a drawing 68 Ge/ 68 A Ga generator.
FIG. 7 is 68 And a gamma spectrum of the Ga product.
FIG. 8 is a thin layer chromatography assay 68 Radiochemical purity of Ga products.
Detailed Description
The experimental procedures used in the following examples are all conventional procedures unless otherwise specified.
Materials, reagents and the like used in the following examples are commercially available unless otherwise specified.
Example 1 production of irradiated metallic gallium-nickel alloy targets 68 Automatic separation system of Ge
Separating and purifying 68 The automatic Ge separation system comprises a liquid taking unit, a conveying unit, a monitoring unit, a pH value regulating and controlling unit, a separation unit, a collection unit and a control unit.
The liquid taking unit and the collecting unit comprise a plurality of liquid storage containers and liquid conveying pipelines; the conveying unit comprises at least one peristaltic pump and four multi-channel switching valves; the monitoring unit comprises at least one liquid level sensor; the pH value regulating and controlling unit comprises at least one pH value monitor and an injection pump with a switching valve head; the separation unit at least comprises two identical or different separation columns; the collecting unit comprises a plurality of collecting containers and a liquid recovery pipeline; the control unit comprises an upper computer, a Programmable Logic Controller (PLC), control software, a communication protocol and the like;
the control unit of the automatic separation system controls the first multi-channel switching valve VA to rotate to a solution in a solution storage container of the preset channel extraction solution taking unit; the output end of a VA (vertical alignment) multi-channel switching valve is connected with the input end of a peristaltic pump P1, the output end of the peristaltic pump P is connected with the input end of a VB (visual alignment) multi-channel switching valve, the output end of the VB multi-channel switching valve is connected with inlets of at least two identical or different separation columns C1 and C2, outlets of the separation columns C1 and C2 are connected with the input end of a VC (visual alignment) multi-channel switching valve, and the VB and the VC are freely rotated by a control unit to be in two states of flowing through the separation columns or not flowing through the separation columns; the output end of the third multi-channel switching valve VC is connected with the input end of a fourth multi-channel switching valve VD, the output end of the fourth multi-channel switching valve VD is connected with a collecting container of the collecting unit, and the fourth multi-channel switching valve VD is used for introducing the liquid passing through the separation column into a corresponding recovery pipeline and entering the collecting unit. A level sensor D of the monitoring unit is connected between the first multi-channel switching valve VA and the peristaltic pump P1 for monitoring whether the control unit is completely extracting solution. A pH monitor E with probe G in the pH control unit and a syringe pump P2 with a switching valve head are used in connection with the collection container of the collection unit for adjusting the pH of the solution, see fig. 1.
The separation columns C1 and C2 include at least two identical or different separation columns.
The VA switching valve is preferably a ten-channel switching valve. The VA0 channel is connected with the input end of the peristaltic pump, the VA1-9 is respectively connected with each liquid storage device of the liquid taking unit A1-9, and the VA10 is connected with a bottle of the collecting unit B1.
The VB and VC switching valves are preferably six-channel switching valves. The output end of the peristaltic pump P1 is connected with a VB0 channel, a VB1 channel is directly communicated with a VC1 channel, VB5 and VB6 are respectively communicated with VC5 and VC6 through connecting separation columns, and VB2, 3 and 4 and VC2, 3 and 4 are used as separated standby channels.
The VD switching valve is preferably a ten-channel switching valve. The VC0 channel is communicated with the VD0 channel, and the VD1-10 is connected with each liquid storage container of the collection unit B1-10.
A1-9 is preferably used for containing metal gallium-nickel target solution, hydrochloric acid solution with pH value of 1-5, hydrochloric acid solution with concentration of 0.5-3.0 mol/L, sodium citrate solution with concentration of 0.25mol/L, sodium citrate solution with concentration of 0.6-1.5mol/L (pH 10.0-13.0), sodium citrate solution with concentration of 0.001-0.1 mol/L (pH 10.0-13.0), alkaline solution with pH value of 10.0-13.0, deionized water and sodium hydroxide solution with concentration of 1-5 mol/L.
B1 is preferably used for containing 0.6-1.5mol/L sodium citrate solution, and B2 is preferably used for containing 68 The Ge product, B3, is preferably used to hold radioactive waste, and B4 is preferably used to hold non-radioactive waste. B5-10 is used as a spare collection container.
The connection relation of the equipment is shown in figure 2, a multi-channel switching valve, a liquid level sensor and a peristaltic pump P1 are connected in series through a liquid pipeline, the switching valve, the peristaltic pump P1, an injection pump P2, the liquid level sensor and a pH monitor are connected with a PLC communication module through communication cables, the one-to-one correspondence relation is established between the state of an internal output register of the PLC and the state of each execution element through configuration, the PLC is communicated with an upper computer through a standard TCP/IP protocol, and the communication process is controlled by upper computer software.
The specific operation process is as follows:
in the initial state, no command is input, the multi-channel switching valve is in the automatic reset state, and the P1 and the P2 are in the stop state. And (3) inputting a command to the upper computer, so that VA is converted to VA8 position, VB is converted to VB1 position, VC is converted to VC1, and VD is converted to VD4, and the liquid pipeline is communicated from left to right. The input command opens P1 to remove air from the line.
Will be provided with 68 Inputting a control program in the Ge separation and purification step, and starting to execute:
step 1, activating a C1 column, inputting a command, enabling a liquid pipeline to be conducted according to VA2-VB5-VC5-VD4, starting P1 and keeping for a period of time, activating a column G1, and connecting tail liquid into B4;
step 2, activating a C2 column, inputting a command, firstly enabling a liquid pipeline to be conducted according to VA4-VB1-VC1-VD4, starting P1 and keeping for a period of time, then conducting according to VA4-VB6-VC6-VD4, starting P1 and keeping for a period of time, finally enabling the liquid pipeline to be conducted according to VA5-VB6-VC6-VD4, and connecting tail liquid into B4;
step 3, C1 column purification 68 Ge, inputting a command to make the liquid pipeline be conducted according to VA2-VB1-VC1-VD4, and opening P1 to keep a sectionAnd after time, the liquid pipeline is conducted according to VA1-VB5-VC5-VD1, P1 is started and kept for a period of time, the liquid pipeline is conducted according to VA2-VB5-VC5-VD1, sample loading operation is carried out, and tail liquid is accessed into B1. Then the liquid pipeline is leached according to VA3-VB5-VC5-VD3, and tail liquid is accessed to B3;
step 4, adjusting the pH value, inputting an instruction, starting P2, and adjusting the pH value;
step 5, C2 column purification 68 Ge, inputting a command, firstly enabling a liquid pipeline to be conducted according to VA5-VB1-VC1-VD3, starting P1 and keeping for a period of time, and connecting tail liquid into B3; then, the liquid pipeline is conducted according to VA5-VB6-VC6-VD3, P is started and kept for a period of time, and tail liquid is connected into B3. Then, the liquid pipeline is conducted according to VA10-VB6-VC6-VD3, the sample loading operation is carried out, and tail liquid is connected into B3. Thirdly, enabling the liquid pipeline to be communicated according to VA5-VB6-VC6-VD3 in sequence, simultaneously starting P1 and keeping for a period of time, enabling the liquid pipeline to be communicated according to VA6-VB6-VC6-VD3, simultaneously starting P1 and keeping for a period of time, enabling the liquid pipeline to be communicated according to VA7-VB6-VC6-VD3, simultaneously starting P1 and keeping for a period of time, enabling the liquid pipeline to be communicated according to VA8-VB6-VC6-VD4, simultaneously starting P1 and keeping for a period of time, carrying out leaching operation, and enabling tail liquid to be connected into B3; finally, the liquid pipeline is conducted according to VA2-VB6-VC6-VD2 to carry out elution operation and desorption 68 Ge, tail liquid is accessed into B2;
step 6, regenerating the C1 column, inputting a command, firstly enabling the liquid pipeline to be conducted according to VA8-VB1-VC1-VD3, starting P1 and keeping for a period of time, and connecting tail liquid into B3; and then the liquid pipeline is conducted according to VA8-VB5-VC5-VD3, P1 is started and kept for a period of time, the liquid pipeline is kept for a period of time according to VA9-VB5-VC5-VD3, and simultaneously P1 is started and kept for a period of time, the liquid pipeline is kept for a period of time according to VA8-VB5-VC5-VD3, and simultaneously P1 is started and kept for a period of time, and tail liquid is connected to B3.
After the above steps are completed, bottles B2, B3 and B4 are filled with products respectively 68 Ge products, radioactive spent liquors and non-radioactive spent liquors.
Redundant channels, redundant pipelines and empty bottles of the switching valve are used for standby, and the stability and the reliability of the whole automatic separation system are guaranteed.
Example 2 baseIn accelerator irradiation production 68 Ga
The flow chart is shown in fig. 3.
S1, preparation and irradiation of metal gallium-nickel alloy target
The metal gallium nickel alloy target in the step is prepared by an electrodeposition method.
The metal copper or the metal aluminum is selected as the metal base layer, the thickness can be any, and the size can be any, and in the embodiment, the metal base layer is preferably a metal copper block with the size of 11 × 3 × 0.5 mm. The metal substrate layer is wrapped by an inert metal through an electroplating method, and the inert metal in the implementation is preferably gold and has the thickness of 5 μm. Preparing a mixture with a molar concentration ratio of 1: GaCl of 10 3 And NiCl 2 The pH value of the mixed solution is 0.5-3.0, and the current density is 10-60 mA/cm 2 Electroplating is carried out at a temperature of 25 to 100 ℃ and a stirring speed of 10 to 500 rpm.
In this example, it is preferable that the molar concentration ratio is 4, the pH value is 1.5, and the current density is 31mA/cm 2 The temperature was 50 ℃ and the stirring speed was 300 rpm. The metallic gallium-nickel alloy target prepared is shown in fig. 4.
The metal gallium-nickel alloy target is placed at the terminal of a proton accelerator for irradiation, the beam current and the target surface can form any angle, the energy is 10-70 MeV, the flow intensity is 10-500 muA, and the irradiation time is longer than 1 h. And cooling the irradiated target for a period of time, and dissolving and separating.
In the embodiment, the angle between the beam and the target surface is preferably 10 degrees, the beam energy is 20MeV, the flow intensity is 100 muA, and the irradiation time is 10 h.
S2、 68 Separation and purification of Ge
S2.1 dissolution of target
Placing the irradiated metal gallium-nickel alloy target in a mixed system of acidity and hydrogen peroxide, wherein the acidic solution can be one or a mixed solution of sulfuric acid, nitric acid and hydrochloric acid, the concentration of the acidic solution is more than 10mol/L, and the concentration of the hydrogen peroxide is 10-30%. After complete dissolution, the pH value is adjusted to 1.0-5.0 by using an alkaline solution. In the embodiment, the preferable acidic solution is sulfuric acid, the preferable alkaline solution is sodium hydroxide solution, and the pH value is adjusted to be 2.0-3.0.
S2.2 68 Separation and purification of Ge
First, the first and second separation columns are activated. Secondly, the target dissolved solution is introduced into the first separation column, and the first separation column is eluted with an acidic solution having a pH of 3.0 while collecting all eluates. A separation column as shown in fig. 5 (top and middle) before and after separation, the matrix elements and most of the impurity species are removed. Adding a sodium citrate solution with the concentration of 0.6-1.5mol/L into the collected leacheate, adjusting the pH value of the leacheate to 10.0-13.0, introducing the leacheate into a second separation column, leaching the leacheate by using a sodium citrate solution with the pH value of 10.0-13.0 and the concentration of 0.001-1.5 mol/L, and leaching the leacheate by using an alkaline solution with the concentration of less than 0.1mol/L and deionized water. Selecting a hydrochloric acid solution with a certain volume concentration of 0.1-0.001 mol/L for analysis 68 Ge, the final volume of 5-20 mL 68 And (4) Ge product. Fig. 5 (bottom) is a gamma energy spectrum obtained by the second separation column, and it can be seen that all impurity species are removed. Finally, 5mCi is obtained 68 The recovery rate of Ge can reach 70%.
The packed resin of the first separation column in this embodiment is preferably a Chelex100 resin. The preferred resin for the second separation column in this embodiment is glucose gel resin G25, 68 the preferred volume of the Ge product is 10-20 mL.
S2.3 68 Ge/ 68 Ga generator
68 Ge/ 68 The Ga generator comprises a shielding layer, a syringe, a connecting joint, a liquid inlet and outlet hose, a plate penetrating joint, a separation column and a collecting bottle, and is particularly shown in figure 6.
The shielding comprises a generator housing 1 and a lead shielding 2 with a holder. Wherein, the inlet and outlet of the separation column are connected with a liquid inlet and outlet hose through external thread straight-through connectors 4 and 7 and are arranged in the lead shielding layer 2 with a bracket. The syringe 13 is connected with a hose through a luer connector 12, the hose is connected with a liquid inlet hose of the separation column 5 through a plate penetrating connector 11, and the solution is conveyed into the separation column 5 through the squeezing syringe. The liquid outlet hose 10 of the separation column 5 is communicated with the generator shell through a plate penetrating joint 8 to assemble the waste liquid or the waste liquid of the generator 68 The Ga product is transported to a collection bottle 9. Wherein the packing material 6 in the separation column is mainlyIn order to use a metal oxide (e.g., tin oxide, titanium oxide, vanadium oxide, tantalum oxide, etc.) or an organic resin based on an oxide (e.g., a silicon dioxide-based phloroglucinol resin, etc.), a preferred filler in the present embodiment is tin oxide having a particle size of 100 to 300 mesh. Wherein, the ratio of the separation column diameter is 10-5: 1, and the ratio is preferably 7:1 in the embodiment.
Assembly 68 Ge/ 68 The steps of the Ga generator are as follows: will adjust the acidity 68 Introducing the Ge solution into the installed separation column, selecting hydrochloric acid solution with corresponding acidity for washing, and washing the generator with hydrochloric acid solution about every 4-5h to obtain the Ge-containing solution 68 Ga products.
S2.4 68 Quality control of Ga
By passing 68 As can be seen from the gamma energy spectrum of Ga (fig. 7), no gamma energy peak of other impurity species was found, 68 ga has high radioactive nuclear purity, which can reach 99.9%. The radiochemical purity was then determined by thin layer chromatography, as shown in FIG. 8, with radiochemical purity greater than 99%. Determined by ICP-OES, wherein 68 The Ga product contains Sn less than 1ppm and meets the medical standard.
To verify 68 Availability of Ga, will be 68 The Ga product is further purified and then is marked with DOTATATE and PSMA-617, and the marking rate can reach more than 92%.

Claims (10)

1. A kind of 68 The automatic Ge separation system comprises a liquid taking unit, a conveying unit, a monitoring unit, a pH value regulating and controlling unit, a separating unit, a collecting unit and a control unit;
the control unit controls the first multi-channel switching valve to rotate to a preset channel to suck the solution in the liquid storage container of the liquid taking unit; the output end of the first multi-channel is connected with the input end of a peristaltic pump, the output end of the peristaltic pump is connected with the input end of a second multi-channel switching valve, the output end of the second multi-channel switching valve is connected with the inlets of at least two same or different separation columns, the outlets of the separation columns are connected with the input end of a third multi-channel switching valve, and the second and third switching valves are freely rotated by the control unit to be in two states of flowing through the separation columns or not flowing through the separation columns; the output end of the third multi-channel switching valve is connected with the input end of a fourth multi-channel switching valve, the output end of the fourth multi-channel switching valve is connected with the collection container of the collection unit, and the fourth multi-channel switching valve is used for introducing the liquid passing through the separation column into the corresponding recovery pipeline and entering the collection unit. A liquid level sensor of the monitoring unit is connected between the first multi-channel switching valve and the peristaltic pump and used for monitoring whether the control unit completely extracts the solution; and a pH value monitor and a syringe pump with a switching valve head in the pH value regulating and controlling unit are connected in a collecting container of the collecting unit and used for regulating the pH value of the solution.
2. Production and preparation of metallic gallium-nickel alloy target based on accelerator irradiation 68 Method of Ga comprising the steps of:
s1, preparing a metal gallium nickel alloy target, and then dissolving the metal gallium nickel alloy target after irradiation;
the structure of the metal gallium nickel alloy target is 1) or 2) as follows:
1) at least comprises two layers including a metal substrate layer and a metal gallium nickel alloy layer;
2) at least comprises three layers including a metal substrate layer, a metal protective layer and a metal gallium-nickel alloy layer;
s2, introducing the dissolved solution into a double-tandem chromatographic column for separation and purification, and collecting the solution containing 68 A solution of Ge;
the double tandem chromatographic columns at least comprise a Chelex100 separation column and a glucose gel separation column which are connected in series;
s3, the obtained mixture contains 68 Introduction of Ge solution 68 Ge/ 68 In a Ga generator, when 68 After the Ge is fully adsorbed, the leaching solution is used for leaching the Ge at preset time intervals 68 Ge/ 68 Leaching the separation column in the Ga generator, and collecting leached leacheate to obtain 68 Ga products.
3. The method of claim 2, wherein: in step S1, the material of the metal first substrate layer is Cu or Al;
the metal protective layer is made of Au or Pt and has the thickness of at least 5 mu m;
in the metal gallium-nickel alloy layer, the Ga mass content is not less than 50%, and the thickness is more than 10mg/cm 2 。
4. A method according to claim 2 or 3, characterized in that: in step S1, preparing the metal gallium-nickel alloy layer by an electroplating method;
and (3) irradiating by using a proton accelerator, wherein the energy is 10-70 MeV, the flow intensity is 10-500 muA, and the time is not less than 1 h.
5. The method according to any one of claims 2-4, wherein: in the step S2, a mixed system of an acidic solution and hydrogen peroxide is adopted for dissolution, wherein the concentration of the acidic solution is greater than 10mol/L, the concentration of the hydrogen peroxide is 10-30%, and the dissolution temperature is 25-150 ℃.
6. The method according to any one of claims 2-5, wherein: in step S2, the separation and purification conditions are as follows:
adjusting the pH value of the solution obtained after the metal gallium nickel target is dissolved to 1.0-5.0, introducing the solution into the Chelex100 separation column, leaching the solution by adopting a hydrochloric acid solution with the pH value of 1.0-5.0, and collecting leacheate; simultaneously adding 0.6-1.5mol/L sodium citrate solution into the leacheate, adjusting the pH value to 10.0-13.0, introducing the glucose gel separation column, and leaching by adopting 0.001-1.5 mol/L, pH of 10.0-13.0 sodium citrate solution, 10.0-13.0 alkaline solution and deionized water in sequence; finally, introducing 0.1-2.0 mol/L hydrochloric acid solution into the glucose gel separation column, desorbing and collecting 68 And (4) Ge product.
7. The method of claim 6, wherein: in step S2, after the separation and purification, hydrochloric acid, deionized water, sodium hydroxide, and deionized water are sequentially introduced into the Chelex100 separation column to regenerate the column.
8. The method according to any one of claims 2-7, wherein: in step S2, the method according to claim 1 68 And the Ge separation automation system controls the separation and purification.
9. The method according to any one of claims 2-8, wherein: in step S3, the 68 Ge/ 68 The packing material adopted by the separation column in the Ga generator is metal oxide or organic resin taking oxide as matrix.
10. The method according to any one of claims 2-9, wherein: in step S3, the product contains 68 The solution of Ge is introduced into the reactor after the acidity is adjusted 68 Ge/ 68 In the separation column in a Ga generator.
CN202210561881.9A 2022-05-23 2022-05-23 Production and preparation based on accelerator irradiation 68 Method for Ge Pending CN114937516A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202210561881.9A CN114937516A (en) 2022-05-23 2022-05-23 Production and preparation based on accelerator irradiation 68 Method for Ge

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202210561881.9A CN114937516A (en) 2022-05-23 2022-05-23 Production and preparation based on accelerator irradiation 68 Method for Ge

Publications (1)

Publication Number Publication Date
CN114937516A true CN114937516A (en) 2022-08-23

Family

ID=82864063

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202210561881.9A Pending CN114937516A (en) 2022-05-23 2022-05-23 Production and preparation based on accelerator irradiation 68 Method for Ge

Country Status (1)

Country Link
CN (1) CN114937516A (en)

Similar Documents

Publication Publication Date Title
EP1820197B1 (en) Method and device for isolating a chemically and radiochemically cleaned 68ga-radio nuclide and for marking a marking precursor with the 68ga-radio nuclide
US5596611A (en) Medical isotope production reactor
CN100551497C (en) Technology with boron resin ion-exchange chromatography Separation of boron isotopes
US20040164025A1 (en) Method and apparatus for separating ions of metallic elements in aqueous solution
CN111485123B (en) Separation from large-amount and low-specific-activity Mo solution99mTc device and method
CN103263849B (en) The fast separating process of activation products gallium in a kind of fission product
CN114732918A (en) Production equipment of liquid composition and preparation method and application thereof
CN114937516A (en) Production and preparation based on accelerator irradiation 68 Method for Ge
CN101451188A (en) Method for separating and purifying cobalt solution by extraction chromatography
CA2764086A1 (en) A system for automatically separating 99mtc-radionuclide from low-medium specific activity 99mo and a process for the same
US3745119A (en) Production of high purity molybdenum using silver coated carbon as adsorbent
CN109437343B (en) Preparation method of sodium pertechnetate solution
CN112473369B (en) For separating 68 System and method of Ge
US8647595B2 (en) Method for separating radioactive copper using chelating-ion exchange resin
CN216062117U (en) Automatic separation system for radioactive nuclide
CN111068482B (en) Extraction from dissolved irradiation uranium target tail gas131I device
CN112853100B (en) Metal cation extraction device, system, method and application thereof
CN108977659B (en) Method for separating plutonium, palladium, silver, cadmium, tin and antimony
CN112973445A (en) Automatic processing device for separating Ac-225 and operation method thereof
CN213611415U (en) Ion replacement and compound purification device
US20210407699A1 (en) System and method for producing molybdenum 99
RU2091878C1 (en) Rhenium generator production process
CN220026628U (en) Radionuclide Ga-68 separation and purification system
CN115094251B (en) Method for separating molybdenum-99 as radioactive fission product
CN104357687B (en) A kind of high abundance93the preparation method of Zr

Legal Events

Date Code Title Description
PB01 Publication
PB01 Publication
SE01 Entry into force of request for substantive examination
SE01 Entry into force of request for substantive examination