A method for preparing a product based on accelerator irradiation 68 Ge's method

Abstract

The invention discloses a method for preparing the 68 Ge method. The method comprises the following steps: S1, preparing a metal gallium nickel alloy target, and then dissolving it after irradiation; the structure of the metal gallium nickel alloy target is as follows 1) or 2): 1) at least two layers, including a metal base layer and a metal gallium nickel alloy layer; 2) at least three layers, including a metal base layer, a metal protective layer and a metal gallium nickel alloy layer; S2, passing the dissolved solution into a double series chromatographic column for separation and purification, and collecting the 68 Ge solution; S3, the obtained 68 The Ge solution was passed into 68 Ge / 68 In the Ga generator, when 68 After Ge is fully adsorbed, the eluent is used to wash the Ge at preset intervals. 68 Ge / 68 The separation column in the Ga generator is eluted, and the eluted eluent is collected to obtain 68 Ga products. The present invention 68 The separation and purification process of Ge has clear ideas, simple operation, and is easy to realize automated separation and purification, and can obtain high purity and radioactive concentration. 68 Ge.

Description

Technical Field

[0001] The present invention relates to a method for preparing a method based on accelerator irradiation 68 The method of Ge belongs to the technical field of positron tomography. Background Art

[0002] At present, domestic and foreign 68 The production and separation process of Ge is mainly based on solvent extraction, fractionation and chromatography. In the solvent extraction separation process, highly toxic and carcinogenic organic reagents such as carbon tetrachloride and toluene are often used as extractants for extraction and separation. 68 In addition, the solvent extraction was carried out under high acidity conditions, which made 68 Ge is easy to form 68 GeCl4 aerosol, resulting in 68 A large amount of Ge is lost. Another method for separation and purification 68 The process of Ge is fractional distillation, which is mainly based on the 68 GeCl4 (boiling point is 82-84℃) is very volatile and can be heated to 68 Ge is separated from the irradiated target and other impurity nuclides. However, this process produces 68 The Ge recovery rate is low and it is very easy to cause radioactive leakage and pollution.

[0003] Chromatography is the process of separation 68 Common separation methods for Ge, capable of achieving continuous separation 68 Ge operation is very conducive to the design and control of automated separation, and can avoid 68 However, as far as the chromatography separation process is concerned, its separation and purification 68 Ge radioactivity concentration and purity are relatively low, so how to establish a method to obtain high radioactivity concentration and specific activity and compound medical 68 Ge, and can also be mass-produced automatically 68 The chromatography process of Ge is very important. Summary of the invention

[0004] The purpose of the present invention is to provide a method for producing a metal gallium-nickel alloy target for accelerator irradiation. 68 Ge's method, and established a reusable dual-column series separation process of Chelex100 and glucose gel separation column. At the same time, this process was applied to the automated separation system and successfully obtained 68 Ge products; the method of the present invention is simple and easy to implement, the principle of the automation system is simple, easy to operate, and easy to implement 68 Large-scale production of Ge.

[0005] The present invention first provides a 68 The Ge separation automation system includes a liquid collection unit, a conveying unit, a monitoring unit, a pH value control unit, a separation unit, a collection unit and a control unit;

[0006] The liquid taking unit and the collecting unit include several liquid storage containers and liquid conveying pipelines; the conveying unit includes at least one peristaltic pump and four multi-channel switching valves; the monitoring unit includes at least one liquid level sensor; the pH value control unit includes at least one pH value monitor and an injection pump with a switching valve head; the separation unit includes at least two identical or different separation columns; the collecting unit includes several collecting containers and liquid recovery pipelines; the control unit includes a host computer, a programmable logic controller (PLC), control software, and communication protocols, etc.

[0007] The control unit controls the first multi-channel switching valve to rotate to the preset channel to absorb the solution in the liquid storage container of the liquid collection unit; the first multi-channel output end is connected to the peristaltic pump input end, the peristaltic pump output end is connected to the second multi-channel switching valve input end, the second multi-channel switching valve output end is connected to at least two identical or different separation column inlets, and the separation column outlet is connected to the third multi-channel switching valve input end, and the second and third switching valves are freely rotated by the control unit to make them flow through the separation column or not flow through the separation column; the third multi-channel switching valve output end is connected to the fourth multi-channel switching valve input end, and the fourth multi-channel switching valve output end is connected to the collection container of the collection unit, and the fourth multi-channel switching valve is used to introduce the liquid passing through the separation column into the corresponding recovery pipeline and enter 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 to monitor whether the control unit completely extracts the solution; the pH value monitor and the injection pump with a switching valve head in the pH value control unit are used to be connected to the collection container of the collection unit to adjust the pH value of the solution;

[0008] The multi-channel switching valve is at least a six-channel switching valve;

[0009] The liquid in the liquid storage container at least includes a solution of the irradiated metal gallium nickel target, a hydrochloric acid solution, an alkaline solution, a 0.001 mol / L-1.5 mol / L sodium citrate alkaline solution and deionized water;

[0010] Include at least one spare separation column system.

[0011] In the 68 Based on the Ge separation automation system, the present invention provides a method for producing and preparing a metal gallium-nickel alloy target based on accelerator irradiation. 68 The method of Ge comprises the following steps:

[0012] S1, preparing a metal gallium-nickel alloy target, and then dissolving it after irradiation;

[0013] The structure of the metal gallium nickel alloy target is as follows 1) or 2):

[0014] 1) At least two layers, including a metal base layer and a metal gallium-nickel alloy layer;

[0015] 2) at least three layers, including a metal base layer, a metal protective layer and a metal gallium-nickel alloy layer;

[0016] S2, pass the dissolved solution into a double series chromatographic column for separation and purification, and collect 68 Ge solution;

[0017] The dual series chromatographic columns are a Chelex100 separation column and a glucose gel separation column connected in series;

[0018] S3, the obtained 68 The Ge solution was passed into 68 Ge / 68 In the Ga generator, when 68 After Ge is fully adsorbed, the eluent is used to wash the 68 Ge / 68 The separation column in the Ga generator is eluted, and the eluted eluent is collected to obtain 68 Ga products.

[0019] In the above method, in step S1, the material of the metal base layer is Cu or Al, which is a metal with strong electrical and thermal conductivity and high hardness;

[0020] The metal protective layer is made of Au or Pt, has a thickness of at least 5 μm, and is an inert metal with strong electrical and thermal conductivity;

[0021] The Ga content in the metal gallium-nickel alloy layer is not less than 50% by mass and the thickness is greater than 10 mg / cm 2 .

[0022] In the above method, in step S1, the metal gallium-nickel alloy layer is prepared by electroplating;

[0023] The plating solution used can be an acidic solution with an acidity of 0.001-2 mol / L, a temperature of 25-100°C, and a current density of 10-60 mA / cm 2 , the molar concentration ratio of gallium ions to nickel ions is 1 to 10, and the stirring speed is 5 to 500 rpm.

[0024] A proton accelerator is used for irradiation, with an energy of 10 to 70 MeV, a current of 10 to 500 μA, a time of not less than 1 hour, and a cooling time of at least 20 days.

[0025] In the above method, in step S2, a mixed system of an acidic solution and hydrogen peroxide is used for dissolution, wherein the concentration of the acidic solution is greater than 10 mol / L, the concentration of the hydrogen peroxide is 10-30%, and the dissolution temperature is 25-150°C;

[0026] The target solution after dissolution and irradiation is a clear and transparent solution, which contains at least 68 Ge, 68,nat Ga, 56,57,58 Co. 65 Zn, nat Ni and nat Cu et al.

[0027] In the above method, in step S2, the conditions for separation and purification are as follows:

[0028] The solution after dissolving the metal gallium nickel target is adjusted to a pH value of 1.0 to 5.0, and then passed through the Chelex 100 separation column, and eluted with a hydrochloric acid solution with a pH of 1.0 to 5.0, and the eluent is collected; at the same time, 0.6 to 1.5 mol / L sodium citrate solution is added to the eluent, and the pH value is adjusted to 10.0 to 13.0, and then passed through the glucose gel separation column, and 0.001 to 1.5 mol / L sodium citrate solution with a pH of 10.0 to 13.0, an alkaline solution with a pH of 10.0 to 13.0, and deionized water are used to elute in sequence; finally, 0.1 to 2.0 mol / L hydrochloric acid solution is passed through the glucose gel separation column, desorbed and collected 68 Each product.

[0029] 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 Chelex 100 separation column to regenerate it;

[0030] The glucose gel separation column does not need further treatment and can be directly reused.

[0031] In the above method, in step S2, by 68 The Ge separation automation system controls the separation and purification.

[0032] In the above method, in step S3, the 68 Ge / 68 The filling material used in the separation column of the Ga generator is metal oxide or an organic resin with oxide as a matrix (such as pyrogallol resin with silicon dioxide as a matrix, etc.).

[0033] Said 68 Ge / 68The structure of the Ga generator is as follows: the separation column is arranged in the shielding layer; the two ends of the separation column are respectively connected to a liquid inlet hose and a liquid outlet hose, and the liquid inlet hose and the liquid outlet hose are respectively connected to a syringe and a collection bottle through a through-plate joint;

[0034] The syringe is connected to a hose via a Luer connector, and the hose is connected to the through-plate connector. The liquid is delivered to the separation column by squeezing the syringe. 68 The Ga product enters the collecting bottle for collection;

[0035] The shielding layer includes a lead shielding layer and a generator housing.

[0036] In the above method, in step S3, the 68 The Ge solution was passed into the 68 Ge / 68 In the separation column in the Ga generator.

[0037] Can be measured by 68 The radiochemical purity, radionuclear purity and chemical purity of Ga are completed. 68 Ga labeling is used to test 68 Availability of GA.

[0038] The present invention has the following advantages due to the adoption of the above technical solution:

[0039] The present invention 68 The separation and purification process of Ge has clear ideas, simple operation, and is easy to realize automated separation and purification, and can obtain high purity and radioactive concentration. 68 The designed automatic separation and purification system can realize multiple separation columns in series and can be used as a backup separation system, which effectively ensures the reliability and safety of the use of the automatic separation and purification system. 68 Ge / 68 The Ga generator is designed to be simple and easy to operate. 68 Ga has high purity and can be used in the preparation of radioactive drugs. BRIEF DESCRIPTION OF THE DRAWINGS

[0040] Figure 1 yes 68 Schematic diagram of Ge automated separation

[0041] Figure 2 yes 68 General diagram of the connections of the components in the Ga automated separation system.

[0042] Figure 3 The invention is to produce the irradiated metal gallium-nickel alloy target 68 Flowchart of Ge's method.

[0043] Figure 4 is a photograph of a metal gallium-nickel alloy target.

[0044] Figure 5 yes 68 γ spectra before and after Ge separation.

[0045] Figure 6 yes 68 Ge / 68 Ga generator.

[0046] Figure 7 yes 68 Ga product gamma spectrum.

[0047] Figure 8 Thin layer chromatography 68 Radiochemical purity graph of Ga products. DETAILED DESCRIPTION

[0048] Unless otherwise specified, the experimental methods used in the following examples are conventional methods.

[0049] Unless otherwise specified, the materials and reagents used in the following examples can be obtained from commercial sources.

[0050] Example 1: Preparation of irradiated metal gallium-nickel alloy targets 68 Automated Separation System for Ge

[0051] Separation and purification 68 The automated separation system of Ge includes a liquid collection unit, a conveying unit, a monitoring unit, a pH value control unit, a separation unit, a collection unit and a control unit.

[0052] The liquid taking unit and the collecting unit include several liquid storage containers and liquid conveying pipelines; the conveying unit includes at least one peristaltic pump and four multi-channel switching valves; the monitoring unit includes at least one liquid level sensor; the pH value control unit includes at least one pH value monitor and an injection pump with a switching valve head; the separation unit includes at least two identical or different separation columns; the collecting unit includes several collecting containers and liquid recovery pipelines; the control unit includes a host computer, a programmable logic controller (PLC), control software, and communication protocols, etc.

[0053] The control unit of the automated separation system controls the first multi-channel switching valve VA to rotate to the preset channel to extract the solution in the liquid storage container of the liquid collection unit; the output end of the first multi-channel switching valve VA is connected to the input end of the peristaltic pump P1, the output end of the peristaltic pump P is connected to the input end of the second multi-channel switching valve VB, the output end of the second multi-channel switching valve VB is connected to at least two identical or different separation columns C1 and C2 inlets, the outlets of the separation columns C1 and C2 are connected to the input end of the third multi-channel switching valve VC, and the control unit freely rotates VB and VC to make them flow through the separation column or not flow through the separation column; the output end of the third multi-channel switching valve VC is connected to the input end of the fourth multi-channel switching valve VD, the output end of the fourth multi-channel switching valve VD is connected to the collection container of the collection unit, and the fourth multi-channel switching valve VD is used to introduce the liquid passing through the separation column into the corresponding recovery pipeline and enter the collection unit. The liquid level sensor D of the monitoring unit is connected between the first multi-channel switching valve VA and the peristaltic pump P1, and is used to monitor whether the control unit completely extracts the solution. The pH value monitor E with a probe G and the injection pump P2 with a switching valve head in the pH value control unit are used to be connected to the collection container of the collection unit to adjust the pH value of the solution, see Figure 1 shown.

[0054] The separation columns C1 and C2 include at least two identical or different separation columns.

[0055] The VA switching valve is preferably a ten-channel switching valve. The VA0 channel is connected to the peristaltic pump input end, VA1-9 are respectively connected to the liquid reservoirs of the liquid taking units A1-9, and VA10 is connected to the collection unit B1 bottle.

[0056] The VB and VC switching valves are preferably six-channel switching valves. The output end of the peristaltic pump P1 is connected to the VB0 channel, the VB1 channel is directly connected to the VC1 channel, VB5 and 6 are connected to VC5 and 6 respectively through a connecting separation column, and VB2, 3, 4 and VC2, 3, 4 are used as separate standby channels.

[0057] The VD switching valve is preferably a ten-channel switching valve. The VC0 channel is connected to the VD0 channel, and VD1-10 is connected to each liquid storage container of the collection unit B1-10.

[0058] A1-9 is preferably used to hold metal gallium-nickel target solution, hydrochloric acid solution with a pH value of 1 to 5, hydrochloric acid solution with a concentration of 0.5 to 3.0 mol / L, 0.25 mol / L sodium citrate solution, 0.6 to 1.5 mol / L sodium citrate solution (pH 10.0 to 13.0), 0.001 to 0.1 mol / L sodium citrate solution (pH 10.0 to 13.0), alkaline solution with a pH of 10.0 to 13.0, deionized water, and 1 to 5 mol / L sodium hydroxide solution.

[0059] B1 is preferably used to hold 0.6-1.5 mol / L sodium citrate solution, and B2 is preferably used to 68 Ge products, B3 is preferably used to hold radioactive waste liquid, B4 is preferably used to hold non-radioactive waste liquid, and B5-10 are used as spare collection containers.

[0060] Device connection relationship Figure 2 As shown, the multi-channel switching valve, liquid level sensor and peristaltic pump P1 are connected in series by liquid pipelines. The switching valve, peristaltic pump P1, syringe pump P2, liquid level sensor and pH monitor are connected to the PLC communication module through communication cables. Through configuration, the state of the PLC internal output register is established in a one-to-one correspondence with the state of each actuator. The PLC establishes communication with the host computer through the standard TCP / IP protocol, and the communication process is controlled by the host computer software.

[0061] The specific operation process is as follows:

[0062] In the initial state, no command is input, the multi-channel switching valve is in the automatic reset state, and P1 and P2 are in the stop state. Input a command to the upper computer to turn VA to VA8, VB to VB1, VC to VC1, and VD to VD4, so that the liquid pipeline is connected from left to right. Input a command to open P1 and remove the air in the pipeline.

[0063] Will 68 The Ge separation and purification step is entered into the control program and begins execution:

[0064] Step 1: Activate the C1 column, input the command to connect the liquid pipeline according to VA2-VB5-VC5-VD4, open P1 and keep it for a while, activate the column G1, and connect the tail liquid to B4;

[0065] Step 2, activate the C2 column, input the command, first make the liquid pipeline conduction according to VA4-VB1-VC1-VD4, open P1 and keep it for a while, then conduction according to VA4-VB6-VC6-VD4, open P1 and keep it for a while, finally make the liquid pipeline conduction according to VA5-VB6-VC6-VD4, and connect the tail liquid to B4;

[0066] Step 3, C1 column purification 68 Ge, input instructions to make the liquid pipeline conduct according to VA2-VB1-VC1-VD4, and open P1 for a period of time, then make the liquid pipeline conduct according to VA1-VB5-VC5-VD1, open P1 and keep it for a period of time, then make the liquid pipeline conduct according to VA2-VB5-VC5-VD1, perform sample loading operation, and connect the tail liquid to B1. Then make the liquid pipeline perform elution operation according to VA3-VB5-VC5-VD3, and connect the tail liquid to B3;

[0067] Step 4: pH value adjustment: input command, turn on P2, and adjust pH value;

[0068] Step 5, C2 column purification 68 Ge, input instructions, first, make the liquid pipeline conduction according to VA5-VB1-VC1-VD3, open P1 and keep it for a while, and connect the tail liquid to B3; then, make the liquid pipeline conduction according to VA5-VB6-VC6-VD3, open P and keep it for a while, and connect the tail liquid to B3. Then, make the liquid pipeline conduction according to VA10-VB6-VC6-VD3, perform the sample loading operation, and connect the tail liquid to B3. Furthermore, the liquid pipeline is turned on in the order of VA5-VB6-VC6-VD3, and P1 is turned on for a period of time, the liquid pipeline is turned on in the order of VA6-VB6-VC6-VD3, and P1 is turned on for a period of time, the liquid pipeline is turned on in the order of VA7-VB6-VC6-VD3, and P1 is turned on for a period of time, the liquid pipeline is turned on in the order of VA8-VB6-VC6-VD4, and P1 is turned on for a period of time, and the elution operation is performed, and the tail liquid is connected to B3; finally, the liquid pipeline is turned on in the order of VA2-VB6-VC6-VD2, and the elution operation is performed for desorption. 68 Ge, tail liquid is connected to B2;

[0069] Step 6, rebirth of C1 column, input instructions, first make the liquid pipeline conduct according to VA8-VB1-VC1-VD3. Open P1 and keep it for a while, and connect the tail liquid to B3; then make the liquid pipeline conduct according to VA8-VB5-VC5-VD3, open P1 and keep it for a while, make the liquid pipeline conduct according to VA9-VB5-VC5-VD3, and open P1 at the same time and keep it for a while, make the liquid pipeline conduct according to VA8-VB5-VC5-VD3, and open P1 at the same time and keep it for a while, and connect the tail liquid to B3.

[0070] After the above steps are completed, bottles B2, B3 and B4 contain products respectively. 68 Ge products, radioactive waste liquid and non-radioactive waste liquid.

[0071] The redundant channels, redundant pipes and empty bottles of the switching valve are used as backup to ensure the stability and reliability of the entire automated separation system.

[0072] Example 2: Production and preparation based on accelerator irradiation 68 Ga

[0073] Flowchart as Figure 3 shown.

[0074] S1. Preparation and irradiation of metal gallium-nickel alloy target

[0075] In this step, the metal gallium-nickel alloy target is prepared by electrodeposition.

[0076] Metal copper or metal aluminum is selected as the metal base layer, and the thickness can be any thickness and size can be any size. In this embodiment, the preferred metal base layer is a metal copper block with a size of 11×3×0.5mm. The metal base layer is coated with an inert metal by electroplating. In this embodiment, the inert metal is preferably gold with a thickness of 5μm. A mixed solution of GaCl3 and NiCl2 with a molar concentration ratio of 1:10 (pH value is 0.5-3.0) is prepared, and the current density is 10-60mA / cm 2 , electroplating is carried out at a temperature of 25 to 100° C. and a stirring speed of 10 to 500 rpm.

[0077] In this embodiment, the preferred molar concentration ratio is 4, the pH value is 1.5, and the current density is 31 mA / cm 2 , temperature of 50°C and stirring speed of 300 rpm. The prepared metal gallium-nickel alloy target is as follows Figure 4 shown.

[0078] The metal gallium-nickel alloy target is placed at the terminal of the proton accelerator for irradiation. The beam can be at any angle to the target surface, the energy is 10-70 MeV, the flux is 10-500 μA, and the irradiation time is greater than 1 hour. After cooling for a period of time, the irradiated target is dissolved and separated.

[0079] In this embodiment, the preferred angle between the beam and the target surface is 10°, the beam energy is 20 MeV, the flux is 100 μA, and the irradiation time is 10 h.

[0080] S2, 68 Separation and purification of Ge

[0081] S2.1 Target Dissolution

[0082] The irradiated metal gallium nickel alloy target is placed in an acidic and hydrogen peroxide mixed system. The acidic solution can be one of sulfuric acid, nitric acid and hydrochloric acid or a mixed solution with a concentration greater than 10 mol / L, and the concentration of hydrogen peroxide is 10-30%. After complete dissolution, the pH value is adjusted to 1.0-5.0 with an alkaline solution. In this embodiment, the preferred acidic solution is sulfuric acid, the alkaline solution is sodium hydroxide solution, and the pH value is adjusted to 2.0-3.0.

[0083] S2.2 68 Separation and purification of Ge

[0084] First, activate separation column 1 and column 2. Second, pass the target solution into separation column 1, and elute separation column 1 with an acidic solution of pH 3.0, while collecting all the eluent. Figure 5As shown in (above and in the middle), the matrix elements and most of the impurity nuclides are removed. A sodium citrate solution with a concentration of 0.6-1.5 mol / L is added to the collected eluent, and the pH value of the eluent is adjusted to 10.0-13.0, and then passed into the separation column 2, and eluted with a 0.001-1.5 mol / L sodium citrate solution with a pH value of 10.0-13.0, and then eluted with an alkaline solution with a concentration of less than 0.1 mol / L and deionized water. A certain volume of hydrochloric acid solution with a concentration of 0.1-0.001 mol / L is selected for analysis 68 Ge, the final volume is 5~20mL 68 Each product. Figure 5 (Below) is the gamma spectrum obtained after separation column 2. It can be seen that all impurity nuclides are removed. Finally, 5mCi 68 Ge, the recovery rate can reach 70%.

[0085] In this embodiment, the preferred resin for the separation column 1 is Chelex 100 resin. The preferred resin for the separation column 2 in this embodiment is glucose gel resin G25, 68 The preferred volume of Ge product is 10-20 mL.

[0086] S2.3 68 Ge / 68 Ga Generator

[0087] 68 Ge / 68 The Ga generator includes a shielding layer, a syringe, a connecting joint, an inlet and outlet hose, a plate-penetrating joint, a separation column and a collecting bottle, as shown in FIG. Figure 6 shown.

[0088] The shielding layer includes a generator housing 1 and a lead shielding layer 2 with a bracket. The inlet and outlet of the separation column are connected to the inlet and outlet hoses through external threaded straight-through joints 4 and 7 and placed in the lead shielding layer 2 with a bracket. The syringe 13 is connected to the hose through the Luer connector 12, and the hose is connected to the inlet hose of the separation column 5 through the through-plate joint 11. By squeezing the syringe, the solution is transported to the separation column 5. The outlet hose 10 of the separation column 5 is connected to the generator housing through the through-plate joint 8 to transport the waste liquid or 68 The Ga product is transported to a collection bottle 9. The filling material 6 in the separation column is mainly a metal oxide (such as tin oxide, titanium oxide, vanadium oxide, tantalum oxide, etc.) or an organic resin based on a certain oxide (such as a pyrogallol resin based on silicon dioxide, etc.). In this embodiment, the preferred filling material is tin oxide with a particle size of 100 to 300 meshes. The separation column diameter ratio is 10 to 5:1, and preferably 7:1 in this embodiment.

[0089] assembly 68 Ge / 68 The steps of the Ga generator are as follows: 68 The Ge solution is passed into the assembled separation column, and the hydrochloric acid solution of corresponding acidity is selected for elution. The generator is eluted with the hydrochloric acid solution every 4-5 hours to obtain 68 Ga products.

[0090] S2.4 68 Quality inspection of Ga

[0091] pass 68 γ-ray spectrum of Ga( Figure 7 ) It can be seen that no γ energy peaks of other impurity nuclides are found. 68 Ga has a high radionuclear purity of up to 99.9%. Its radiochemical purity is then determined by thin layer chromatography, such as Figure 8 As shown, the radiochemical purity is greater than 99%. 68 The Sn content in Ga products is less than 1ppm, which meets medical standards.

[0092] To verify 68 The availability of Ga will result in 68 The Ga product is further purified and then labeled with DOTATATE and PSMA-617, and the labeling rate can reach more than 92%.

Claims

1. A production method based on accelerator irradiation 68 The method of Ge comprises the following steps: S1, preparing a metal gallium-nickel alloy target, and then dissolving it after irradiation; The structure of the metal gallium nickel alloy target is as follows 1) or 2): 1) At least two layers, including a metal base layer and a metal gallium-nickel alloy layer; 2) At least three layers, including a metal base layer, a metal protective layer and a metal gallium-nickel alloy layer; S2, pass the dissolved solution into a double series chromatographic column for separation and purification, and collect 68 Ge solution; The dual series chromatographic columns at least include a Chelex100 separation column and a glucose gel separation column connected in series; S3, the obtained 68 The Ge solution was passed into 68 Ge / 68 In the Ga generator, when 68 After Ge is fully adsorbed, the eluent is used to wash the 68 Ge / 68 The separation column in the Ga generator is eluted, and the eluted eluent is collected to obtain 68 Each product; The method uses 68 The Ge separation automation system controls the separation and purification process. 68 The Ge separation automation system includes a liquid collection unit, a conveying unit, a monitoring unit, a pH value control unit, a separation unit, a collection unit and a control unit; 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 collection unit; the first multi-channel output end is connected to the peristaltic pump input end, the peristaltic pump output end is connected to the second multi-channel switching valve input end, the second multi-channel switching valve output end is connected to at least two identical or different separation column inlets, the separation column outlet is connected to the third multi-channel switching valve input end, and the second and third switching valves are freely rotated by the control unit to make them flow through the separation column or not flow through the separation column; the third multi-channel switching valve output end is connected to the fourth multi-channel switching valve input end, the fourth multi-channel switching valve output end is connected to the collection container of the collection unit, and the fourth multi-channel switching valve is used to introduce the liquid passing through the separation column into the corresponding recovery pipeline and enter 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 to monitor whether the control unit has completely extracted the solution; The pH value monitor and the injection pump with a switching valve head in the pH value regulating unit are used to be connected to the collection container of the collection unit to adjust the pH value of the solution.

2. The method according to claim 1, characterized in that: In step S1, the material of the metal base layer is Cu or Al; The metal protective layer is made of Au or Pt and has a thickness of at least 5 µm; The metal gallium-nickel alloy layer has a Ga content of not less than 50% and a thickness of more than 10 mg / cm 2 .

3. The method according to claim 1 or 2, characterized in that: In step S1, the metal gallium-nickel alloy layer is prepared by electroplating; Proton accelerator is used for irradiation, with energy of 10~70 MeV, flux of 10~500 µA, and time of not less than 1 h.

4. The method according to claim 1 or 2, characterized in that: In step S2, a mixed system of an acidic solution and hydrogen peroxide is used for dissolution, wherein the concentration of the acidic solution is greater than 10 mol / L, the concentration of the hydrogen peroxide is 10-30%, and the dissolution temperature is 25-150 °C.

5. The method according to claim 1 or 2, characterized in that: In step S2, the conditions for separation and purification are as follows: After the solution after dissolving the metal gallium-nickel alloy target is adjusted to a pH value of 1.0-5.0, it is passed into the Chelex100 separation column, and eluted with a hydrochloric acid solution with a pH value of 1.0-5.0, and the eluent is collected; at the same time, 0.6-1.5 mol / L sodium citrate solution is added to the eluent, and the pH value is adjusted to 10.0-13.0, and then it is passed into the glucose gel separation column, and 0.001-1.5 mol / L sodium citrate solution with a pH value of 10.0-13.0, an alkaline solution with a pH value of 10.0-13.0, and deionized water are used to elute in sequence; finally, 0.1-2.0 mol / L hydrochloric acid solution is passed into the glucose gel separation column, desorbed and collected 68 Each product.

6. The method according to claim 5, characterized in that: 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 it.

7. The method according to claim 1 or 2, characterized in that: In step S3, the 68 Ge / 68 The filling material used in the separation column of the Ga generator is metal oxide or organic resin with oxide as the matrix.

8. The method according to claim 1 or 2, characterized in that: In step S3, the 68 The Ge solution was passed into the 68 Ge / 68 In the separation column in the Ga generator.

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