Application of non-radioactive germanium and filling method and filling system of germanium-gallium generator

Abstract

The invention discloses application of non-radioactive germanium and a filling method and a filling system of a germanium-gallium generator, particularly relates to the technical field of germanium-gallium generators, and comprises application of the non-radioactive germanium in a filling process of the germanium-gallium generator. The filling process of the germanium-gallium generator comprises the following steps: step a, filling an adsorbent in a filler cylinder; b, preparing column loading liquid of the filler cylinder; the column loading liquid contains non-radioactive germanium and radioactive germanium; and c, flushing the filler cylinder with the upper column liquid, and filling the filler cylinder to obtain the filled germanium-gallium generator filler cylinder and the filling system of the germanium-gallium generator filling process. The invention overcomes the technical problem of low column loading rate of a germanium-gallium generator in the prior art, discloses the application of non-radioactive germanium in the filling process of the germanium-gallium generator, and provides the filling process with high column loading rate and a filling system convenient to operate.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of germanium-gallium generator, in particular to the application of non-radioactive germanium and the filling method and system of germanium-gallium generator. BACKGROUND

[0002] 68 Ga is an ideal diagnostic nuclide, which can be paired with therapeutic nuclides (such as 177 Lu and 225 Ac) to achieve diagnosis and treatment integration. The germanium-gallium generator is a very important source of 68 Ga nuclide, through the parent nucleus in the generator 68 Ge decays into 68 Ga, and the desired 68 Ga nuclide is obtained by hydrochloric acid leaching.

[0003] The germanium-gallium generator is small in size, convenient to transport, and can prepare 68 Ga without large-scale equipment such as accelerators, and is relatively cheap, so that 68 Gz can be produced at any time, and is widely used in hospitals and research units.

[0004] During the production of the germanium-gallium generator, the 68 Ge needs to be filled into the filler column of the germanium-gallium generator, and the 68 Ge activity adsorbed on the filler column is higher than the 68 Ge activity, that is, the column loading rate. The higher the column loading rate, the more 68 Ga is produced when the germanium-gallium generator is leached.

[0005] Excessively low column loading rate will cause technical problems such as difficulty in recycling of 68 Ge, and at the same time, will cause loss of 68 Ge solution. Further, excessively low column loading rate requires more filler to adsorb 68 Ge, and a large amount of filler will make the volume of the germanium-gallium generator larger, since the germanium-gallium generator is composed of lead shielding, the larger volume means that more lead shielding is needed, which eventually leads to exponential growth of the weight of the generator, which is not conducive to actual production and use. Therefore, it is urgent to improve the column loading rate of the germanium-gallium generator. SUMMARY

[0006] The purpose of the present application is to solve the technical problem of low column loading rate of the germanium-gallium generator in the prior art, and the present application provides the following technical solutions:

[0007] Application of non-radioactive germanium in the filling process of the germanium-gallium generator.

[0008] The column loading rate of the radioactive germanium containing non-radioactive germanium is much higher than that of the radioactive germanium without adding non-radioactive germanium in the filling process of the germanium-gallium generator.

[0009] A filling process of a germanium-gallium generator, comprising the following steps:

[0010] Step a: filling the adsorbent in the filling cylinder;

[0011] Step b: preparing the column loading solution of the filling cylinder; the column loading solution contains non-radioactive germanium and radioactive germanium.

[0012] Step c: flushing the filling cylinder with the column loading solution to fill the filling cylinder, and obtaining the filled germanium-gallium generator filling cylinder.

[0013] In an embodiment, the preparation method of the column loading solution of step b comprises the following steps:

[0014] Step b1: directly mixing the non-radioactive germanium solution and the radioactive germanium solution, and diluting to the target concentration to obtain the column loading solution.

[0015] In an embodiment, the preparation method of the column loading solution of step b comprises the following steps:

[0016] Step b2: respectively preparing the non-radioactive germanium solution and the radioactive germanium solution with the target concentration, and dynamically mixing the non-radioactive germanium solution and the radioactive germanium solution.

[0017] Further, in step c, the filling cylinder is flushed with the non-radioactive germanium solution and the radioactive germanium solution prepared in step b1 through the filling system.

[0018] Further, the non-radioactive germanium solution and the radioactive germanium solution flush the filling cylinder simultaneously.

[0019] The content ratio of the non-radioactive germanium, the adsorbent, and the radioactive germanium is (1.8-2.5) μg:500 mg:(1-1.5) mCi.

[0020] Preferably, the content ratio of the non-radioactive germanium, the adsorbent, and the radioactive germanium is 2 μg:500 mg:1 mCi.

[0021] A filling system of a germanium-gallium generator filling process, comprising a filling cylinder, two liquid storage tanks, and a waste liquid tank, the filling cylinder is filled with adsorbent, one of the liquid storage tanks stores non-radioactive germanium solution, the other stores 68 Ge solution; the liquid outlet end of the filling cylinder is communicated with the waste liquid tank through a liquid outlet pipe, and the liquid inlet end is communicated with one channel of a three-way pipe, and the other two channels of the three-way pipe are respectively communicated with the two liquid storage tanks through liquid inlet pipes.

[0022] Each inlet pipe is equipped with a first valve and a peristaltic pump, and the outlet pipe is equipped with a second valve.

[0023] The present invention has the following advantages:

[0024] (1) This invention is the first to propose the use of non-radioactive germanium in the filling process of germanium-gallium generators, and the germanium-gallium generators prepared using non-radioactive germanium have a higher column loading rate than those prepared without using non-radioactive germanium.

[0025] (2) This invention discloses for the first time the preparation steps and methods of filling process for preparing germanium gallium generator using non-radioactive technology.

[0026] (3) This invention discloses for the first time the amount of non-radioactive germanium added in the filling process for preparing germanium-gallium generators. When the content ratio of non-radioactive germanium, adsorbent, and radioactive germanium is (1.8-2.5) μg:500 mg:(1-1.5) mCi, the loading rate of radioactive germanium is high. In particular, when the content ratio of non-radioactive germanium, adsorbent, and radioactive germanium is 2 μg:500 mg:1 mCi, the loading rate of radioactive germanium can reach over 95%, which is 20% higher than the 75% loading rate of the prior art. The high loading rate improves the efficiency of the germanium-gallium generator, thereby reducing the volume of the filler, i.e., reducing the volume of the germanium-gallium generator; at the same time, the increased loading rate reduces the... 68 Reduce the loss of Ge and lower costs.

[0027] (4) This invention discloses for the first time that in the filling process of a germanium-gallium generator, radioactive germanium and non-radioactive germanium are mixed and then rinsed to fill the column. At this time, the column loading rate is the highest and this filling process step is the best.

[0028] (5) The present invention also discloses a filling system adapted to filling germanium gallium generators containing non-radioactive germanium. The filling device has a simple structure, is easy to operate, and has high practicality. Attached Figure Description

[0029] Figure 1 This is a schematic diagram of the filling system of the present invention.

[0030] In the diagram: 1. Packing cylinder, 2. Storage tank, 3. Waste liquid tank, 4. Storage tank, 5. Inlet pipe, 6. First valve, 7. Peristaltic pump, 8. Second valve, 9. Tee. Detailed Implementation

[0031] The technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings of the embodiments of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments.

[0032] Therefore, the following detailed description of the embodiments of the application is not intended to limit the scope of the application as claimed, but merely to represent some embodiments of the application. Based on the embodiments in the application, all other embodiments obtained by those skilled in the art without creative labor are within the scope of protection of the application.

[0033] It should be noted that the embodiments in the application and the features and technical solutions in the embodiments can be combined with each other without conflict.

[0034] It should be noted that: similar reference numerals and letters represent similar items in the following drawings, therefore, once an item is defined in one drawing, it does not need to be further defined and explained in subsequent drawings. In the description of the application, it should be noted that the terms "upper", "lower", and the like indicate the orientation or positional relationship shown in the drawings, or the orientation or positional relationship commonly used when the product of the application is used, or the orientation or positional relationship commonly understood by those skilled in the art, such terms are only for the convenience of describing the application and simplifying the description, and are not intended to indicate or imply that the indicated device or element must have a particular orientation, be constructed and operated in a particular orientation, and therefore cannot be understood as limiting the application. In addition, the terms "first", "second", and the like are only used for differentiation and cannot be understood as indicating or implying relative importance.

[0035] Application of non-radioactive germanium in filling process of germanium-gallium generator.

[0036] In the above filling process of the germanium-gallium generator, the columnation rate of the radioactive germanium containing non-radioactive germanium is much higher than that of the radioactive germanium without adding non-radioactive germanium. It is first proposed to apply non-radioactive germanium in the filling process of the germanium-gallium generator.

[0037] A filling process of a germanium-gallium generator, comprising the following steps:

[0038] Step a: filling the adsorbent in the filling cylinder 1;

[0039] Step b: preparing the columnation liquid of the filling cylinder 1; the columnation liquid contains non-radioactive germanium and radioactive germanium.

[0040] Step c: flushing the filling cylinder 1 with the columnation liquid, filling the filling cylinder 1, and obtaining the filled germanium-gallium generator filling cylinder 1.

[0041] The content ratio of non-radioactive germanium, adsorbent, and radioactive germanium is (1.8-2.5) μg:500 mg:(1-1.5) mCi.

[0042] Preferably, the content ratio of non-radioactive germanium, adsorbent, and radioactive germanium is 2 μg:500 mg:1 mCi.

[0043] The preparation method of the column liquid in step b of the first scheme comprises the following steps:

[0044] Step b1: directly mix the non-radioactive germanium solution and the radioactive germanium solution, and dilute to the target concentration to obtain the column liquid.

[0045] The preparation method of the column liquid in step b of the second scheme comprises the following steps:

[0046] Step b2: prepare the non-radioactive germanium solution and the radioactive germanium solution with the target concentration respectively, and dynamically mix the non-radioactive germanium solution and the radioactive germanium solution. The dynamic mixing refers to mixing the non-radioactive germanium solution and the radioactive germanium solution during the conveying process, and outputting the mixed liquid.

[0047] It should be noted that the non-radioactive germanium solution and the radioactive germanium solution are standard solution purchased in the prior art, and the non-radioactive germanium solution is generally GeCl3 solution or Ge(NO3)3 solution.

[0048] Further, in step c, the non-radioactive germanium solution and the radioactive germanium solution prepared in step b1 are used to flush the packing cylinder 1 through the filling system.

[0049] Further, the non-radioactive germanium solution and the radioactive germanium solution flush the packing cylinder 1 at the same time.

[0050] A filling system of a germanium gallium generator filling process, comprising a packing cylinder 1, two liquid storage tanks 2 and a waste liquid tank 3, the packing cylinder 1 is filled with adsorbent, one of the liquid storage tanks 2 is used to store non-radioactive germanium solution, and the other liquid storage tank 2 is used to store 68 Ge solution; the liquid outlet end of the packing cylinder 1 is communicated with the waste liquid tank 3 through a liquid outlet pipe 4, and the liquid inlet end is communicated with one channel of a three-way pipe, the other two channels of the three-way pipe 9 are respectively communicated with the two liquid storage tanks 2 through liquid inlet pipes 5. A first valve 6 and a peristaltic pump 7 are installed on each liquid inlet pipe 5, and a second valve 8 is installed on the liquid outlet pipe 4. The peristaltic pump 7 is used for liquid inlet, and the first valve 6 and the second valve are respectively used for controlling the opening / closure of the column liquid.

[0051] The above preparation steps and filling system are installed, and the following implementation is carried out, as follows:

[0052] Example 1: in which step b is prepared by the first scheme, and the specific filling steps are as follows:

[0053] Take 0.2 ml of 1 mg / ml standard germanium solution, add to a 100 ml volumetric flask, and then add 0.5 mol / L hydrochloric acid to the volumetric flask to make up to 100 ml, and dilute to obtain 2.0 μg / L of non-radioactive germanium.

[0054] 500.2 mg of adsorbent SnO2 was packed into packing cylinder 1; then 1 mL of non-radioactive germanium with a concentration of 2.0 mg / L and 1 mL of radioactive germanium with a concentration of 1.0 mCi / mL were added. 68 The solution was mixed with Ge to prepare the loading solution; the packing cylinder 1 was rinsed with the loading solution; after all the loading solution had been used for rinsing, the activity of the packing cylinder was measured with an activity meter. 68 Ge activity. The calculated column loading rate was 95.22%.

[0055] Example 2: Step b is prepared using Scheme 2, and the specific filling steps are as follows:

[0056] Take 500.2 mg of SnO2 and fill it into packing cylinder 1; take 1 ml of 2.0 μg / L non-radioactive germanium and put it into one of the storage tanks 2 of the filling system; then take 1 ml of 1.0 mCi / mL radioactive germanium ( 68 Ge) is placed in another storage tank 2 of the filling system; open the second valve, then open the two first valves 6, and simultaneously turn on the two peristaltic pumps 7, all with a flow rate set to 1.5 ml / min; after all the liquid in storage tank 2 has been filled, turn off the two peristaltic pumps 7, then close the two first valves 6, and finally close the second valve to complete the filling; measure the amount of liquid in the filling tank using an activity meter. 68 Ge activity. The calculated column loading rate was 95.83%.

[0057] Example 3: Step b is prepared using Scheme 2, and the specific filling steps are as follows:

[0058] Take 500.2 mg of SnO2 and fill it into packing cylinder 1; take 1 mL of 1.0 mCi / mL germanium ( 68 (Ge) is placed in one of the storage tanks 2 of the filling system; 1 mL of 0.5 mol / L HCl solution is placed in another storage tank 2 of the filling system; the second valve is opened, then the two first valves 6 are opened, and the two peristaltic pumps 7 are turned on simultaneously, with the flow rate set to 1.5 mL / min; after all the liquid in storage tank 2 has been filled, the two peristaltic pumps 7 are turned off, then the two first valves 6 are closed, and finally the second valve is closed, and the filling is completed; the activity of the solution in the filling tank is measured with an activity meter. 68 Ge activity. The calculated loading rate was 77.99%. HCl solution was used as a blank control.

[0059] The specific parameters and results of examples 1-3 are as follows:

[0060]

[0061]

[0062] The above-mentioned embodiments 1-3 can be seen that the column efficiency of the germanium-gallium generator without adding non-radioactive germanium in the eluent is lower than that of the germanium-gallium generator with adding non-radioactive germanium in the eluent, and it can be seen that adding radioactive germanium in the eluent can improve the column efficiency of the germanium-gallium generator. 68 The column efficiency of Ge.

[0063] Embodiment 4: wherein step b is prepared by scheme two, and the specific filling steps are as follows:

[0064] 500.0 mg of the additive SnO2 is filled into the filling cylinder 1; 500.2 mg of the additive SnO2 is filled into the filling cylinder 1; 1 ml of non-radioactive germanium with a concentration of 2.0 μg / L is loaded into one of the liquid storage tanks 2 of the filling system, and 1 mL of radioactive germanium ( 68 Ge) with a concentration of 1.0 mCi / mL is loaded into another liquid storage tank 2 of the filling system; the second valve is opened, and then the first valve 6 of the liquid storage tank 2 storing the non-radioactive germanium and the peristaltic pump 7 are opened, and the flow rate of the peristaltic pump 7 is set to 1.5 ml / min; after the liquid in the liquid storage tank 2 storing the non-radioactive germanium is completely eluted and filling is completed, the first valve 6 of the liquid storage tank 2 storing the non-radioactive germanium and the peristaltic pump 7 are closed, the first valve 6 of the liquid storage tank 2 storing the radioactive germanium ( 68 Ge) and the peristaltic pump 7 are opened, and the flow rate of the peristaltic pump 7 is set to 1.5 ml / min; after the liquid in the liquid storage tank 2 storing the radioactive germanium ( 68 Ge) is completely eluted and filling is completed, the first valve 6 of the liquid storage tank 2 storing the non-radioactive germanium and the peristaltic pump 7 are closed, the second valve is closed, and the filling is completed; the activity of the germanium in the filling cylinder is measured by the activity meter. It is calculated that the column efficiency is 83.22%. 68 Ge).

[0065] Embodiment 5: wherein step b is prepared by scheme two, and the specific filling steps are as follows:

[0066] 500.2 mg of the additive SnO2 is filled into the filling cylinder 1; 1 ml of non-radioactive germanium with a concentration of 2.0 μg / L is loaded into one of the liquid storage tanks 2 of the filling system, and 1 mL of radioactive germanium ( 68 Ge) with a concentration of 1.0 mCi / mL is loaded into another liquid storage tank 2 of the filling system; the second valve is opened, and then the first valve 6 of the liquid storage tank 2 storing the radioactive germanium ( 68 Ge) and the peristaltic pump 7 are opened, and the flow rate of the peristaltic pump 7 is set to 1.5 ml / min; after the liquid in the liquid storage tank 2 storing the radioactive germanium ( 68 Ge) is completely eluted and filling is completed, the first valve 6 of the liquid storage tank 2 storing the non-radioactive germanium and the peristaltic pump 7 are closed, the second valve is closed, and the filling is completed; the activity of the germanium in the filling cylinder is measured by the activity meter. It is calculated that the column efficiency is 83.22%. 68The first valve 6 and the peristaltic pump 7 of the storage tank 2 of the non-radioactive germanium are opened, the first valve 6 and the peristaltic pump 7 of the storage tank 2 of the non-radioactive germanium are opened, and the flow rate of the peristaltic pump 7 is set to 1.5 ml / min; after the liquid elution filling of the storage tank 2 of the non-radioactive germanium is completed, the first valve 6 and the peristaltic pump 7 of the storage tank 2 of the non-radioactive germanium are closed, the second valve is closed, and the filling is completed; the activity of the germanium in the filling barrel is measured by an activity meter 68 The column loading rate of the germanium is 68.89%.

[0067] The specific parameters and results of examples 1, 2, 4 and 5 are as follows:

[0068]

[0069] From the above results, it can be seen that, under the condition that the amounts of the adsorbent, the non-radioactive germanium and the radioactive germanium are consistent, the column loading rates of the germanium are different in different elution filling methods of the filling barrel 1. 68 The column loading rate of the germanium is 68.89%. 68 The column loading rate of the germanium is 68.89%.

[0070] Examples 6-8: The filling process and the filling system of example 2 are used, and the difference lies in that the amounts of the adsorbent, the non-radioactive germanium and the radioactive germanium are different. The specific parameters and results of examples 2 and 6-8 are shown in the following table:

[0071]

[0072]

[0073] From the above table, it can be seen that, when the content ratio of the non-radioactive germanium, the adsorbent and the radioactive germanium is (1.8-2.5) μg: 500 mg: (1-1.5) mCi, 68 The column loading rate of the germanium is 68.89%.

[0074] The above is only a preferred specific embodiment of the present application, but the protection scope of the present application is not limited to this. Any person skilled in the art can make equivalent replacements or changes to the technical solution and the inventive concept of the present application within the technical range disclosed by the present application, which should be covered within the protection scope of the present application.

Claims

1. Application of non-radioactive germanium in the filling process of germanium-gallium generators.

2. A filling process for a germanium gallium generator as claimed in claim 1, characterized in that, Includes the following steps: Step a: Fill the packing tube with adsorbent; Step b: Prepare the top column liquid for the packed tube; the top column liquid contains non-radioactive germanium and radioactive germanium. Step c: Rinse the packing cylinder with the column flux, fill the packing cylinder, and obtain the filled germanium-gallium generator packing cylinder.

3. The germanium-gallium generator filling process according to claim 2, characterized in that, The preparation method of the column loading solution in step b includes the following steps: Step b1: Directly mix the non-radioactive germanium solution and the radioactive germanium solution, dilute to the target concentration, and obtain the column loading solution.

4. The germanium-gallium generator filling process according to claim 2, characterized in that, The preparation method of the column loading solution in step b includes the following steps: Step b2: Prepare non-radioactive germanium solutions and radioactive germanium solutions of the target concentration respectively, and dynamically mix the non-radioactive germanium solutions and radioactive germanium solutions.

5. The germanium-gallium generator filling process according to claim 4, characterized in that, In step c, the packing cylinder is rinsed with the non-radioactive germanium solution prepared in step b1 and the radioactive germanium solution through the filling system.

6. The germanium-gallium generator filling process according to claim 5, characterized in that, The packing cylinder is simultaneously flushed with both non-radioactive germanium solution and radioactive germanium solution.

7. The germanium-gallium generator filling process according to claim 2, characterized in that, The content ratio of non-radioactive germanium, adsorbent, and radioactive germanium is (1.8-2.5) μg: 500 mg: (1-1.5) mCi.

8. The germanium-gallium generator filling process according to claim 7, characterized in that, The content ratio of non-radioactive germanium, adsorbent, and radioactive germanium is 2 μg: 500 mg: 1 mCi.

9. A filling system for any one of the germanium-gallium generator filling processes described in claims 4-6, characterized in that, The device includes a packing cylinder, two storage tanks, and a waste liquid tank. The packing cylinder is filled with adsorbent. One storage tank is used to store a non-radioactive germanium solution, and the other storage tank is used to store a 6Ge solution. The outlet end of the packing cylinder is connected to the waste liquid tank through an outlet pipe, and the inlet end is connected to one channel of a three-way valve. The other two channels of the three-way valve are connected to the two storage tanks respectively through inlet pipes.

10. A filling system as described in claim 9, characterized in that, Each inlet pipe is equipped with a first valve and a peristaltic pump, and the outlet pipe is equipped with a second valve.

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