Method for separating 176Yb and 177Lu

Abstract

The invention provides a method for separating 176Yb and 177Lu, which comprises the following steps: dissolving a 176Yb target containing 176Yb and 177Lu with acid, and heating and evaporating the target dissolving liquid to dryness; the invention relates to a method for separating 176Yb from 177Lu, comprising the steps of adding a solution comprising a complexing agent capable of complexing at least 176Yb < 3 + > to obtain an electrolyte comprising 176Yb and 177Lu, the electrolyte being electrodeposited to separate 176Yb and 177Lu, the cathode being Hg. According to the method disclosed by the invention, trace 177Lu can be extracted from the gram-scale 176Yb target irradiated by the reactor, the removal effect of Yb is good, and the recovery rate of 177Lu is high.

Description

Technical Field

[0001] The present invention relates to the field of radionuclide separation, and in particular to a separation method. 176 Yb and 177 Lu's method. Background Art

[0002] 177 Lu is an important radioactive therapeutic nuclide. 177 Lu has a half-life of 6.639 days and emits three types of beta particles with energies of 498.3keV (79.3%), 385.4keV (9.1%) and 177.0keV (11.64%). Compared with other therapeutic radionuclides, its particle energy is lower. The released radioactive particles can not only effectively kill tumor cells, but also cause less damage to surrounding healthy tissues. When radiating the lesions, the bone marrow suppression is less severe. It can provide targeted radiotherapy during the treatment process and reduce side effects and complications to patients. 177 Lu can emit gamma rays when it decays, which can be used for imaging and dosimetry analysis. Therefore, single photon emission computed tomography (SPECT) can be used for imaging diagnosis to detect diseases such as cancer and tumors, and to assist in evaluating the location, size, and possible metastasis of tumors.

[0003] at present, 177 Lu is mainly produced through reactors, and there are two methods: direct method and indirect method. 176 Lu(n,γ) 177 Lu reaction preparation, the method produces 177 Lu contains carrier 176 Lu, which has a low specific activity and produces a long half-life (160 days) 177m Lu impurities emit high-energy gamma rays, are highly toxic, and have carriers 177 Lu is mainly used in basic research, bone analgesia and treatment. 176 Yb(n,γ) 177 Yb(β - ) 177 Lu reaction to obtain no-carrier-added (NCA) 177 Lu, prepared by indirect method 177 Lu does not contain 177m Lu impurities have high specific activity and can meet the requirements for the use of peptide radiopharmaceuticals and immunoradiopharmaceuticals. 177 Most Lu-labeled radiopharmaceuticals are carrier-free. 177 Lu, therefore, the carrier-free 177 Lu has wider application prospects.

[0004] pass 176 Yb(n,γ) 177 Yb(β - ) 177 Lu reaction preparation without carrier 177 One of the key technologies of Lu is to convert the constant 176 Yb and trace 177 Lu is separated, while Yb / Lu are both lanthanide elements, their atomic mass, outermost electronic structure and chemical properties are similar. It is difficult to separate them completely by conventional methods, and more efficient methods must be used to achieve effective separation.

[0005] The methods currently used for Yb / Lu separation mainly include solvent extraction, ion exchange chromatography, high performance liquid chromatography (HPLC), electrochemical methods, etc. Solvent extraction can process a large number of samples, and the process is continuous and the selectivity is good, but a lot of radioactive waste liquid is generated during the separation process, and most organic solvents are tissue toxic, requiring subsequent processes to remove the organic solvents. Ion exchange chromatography has good separation effect and is convenient for remote operation, but it requires multi-stage separation, which is time-consuming and generates a large amount of radioactive waste liquid during the separation process. High performance liquid chromatography has good separation effect and short separation time, but it can only process a small amount of samples, and excessive processing volume will lead to reduced separation efficiency.

[0006] China Advanced Research Reactor (CARR) is a high-flux nuclear reactor independently built in my country. The neutron flux of the irradiation channel used for radioisotope production is 2.0E+14n / cm 2 ·s. According to theoretical calculation, the irradiation at the center channel of CARR 176 After 7 days, the Yb target 176 Yb and 177 The mass ratio of Lu is greater than 2000:1. 176 Yb / 177 Lu has a large mass ratio and can be extracted from irradiated 176 Yb target extraction trace 177 Lu is extremely challenging.

[0007] Therefore, an efficient method is needed to 176 Yb separation 177 Lu's method. Summary of the invention

[0008] In view of this, the main purpose of the present invention is to provide a separation 176 Yb and 177 Lu's method, which uses electrochemical methods to generate gram-scale176 Yb separation 177 Lu, the separation efficiency is high, the operation is simple, and less radioactive waste liquid is produced.

[0009] To this end, the present invention provides a separation 176 Yb and 177 Lu's method comprises the following steps:

[0010] Will include 176 Yb and 177 Lu's 176 The Yb target is dissolved with acid, and then the target solution is heated and evaporated to dryness;

[0011] Adding a solution comprising a complexing agent to obtain a solution comprising 176 Yb 3+ and 177 Lu 3+ The electrolyte, wherein the complexing agent is capable of complexing at least 176 Yb 3+ ;

[0012] The electrolyte is subjected to electrodeposition to separate 176 Yb and 177 Lu, where the cathode is Hg.

[0013] In some embodiments, the 176 The Yb target is an irradiated target, wherein 176 Yb and 177 The mass ratio of Lu is less than or equal to 5000:1.

[0014] In some embodiments, the complexing agent is selected from citrate and α-hydroxyisobutyric acid; preferably, the citrate is sodium citrate; more preferably, the solution including the complexing agent is 0.15-0.4 mol / L citrate or 0.3-0.6 mol / L α-hydroxyisobutyric acid.

[0015] In some embodiments, the pH value of the electrolyte is less than or equal to 7, preferably 5.0 to 7.0.

[0016] In some embodiments, the electrodeposition uses a direct current of 8 to 14 V.

[0017] In some embodiments, the anode of the electrolysis is a platinum sheet or a platinum strip.

[0018] In some embodiments, the method further comprises, after the electrodeposition is completed, replacing the cathode Hg, and repeating the electrodeposition.

[0019] In some embodiments, the method further comprises measuring the content of the dissolved solution after the electrodeposition. 177The radioactivity of Lu.

[0020] In some embodiments, the acid is 4-6 mol / L nitric acid or 4-6 mol / L hydrochloric acid.

[0021] The present invention also provides a carrier-free extraction method. 177 Lu's method, comprising the above separation 176 Yb and 177 Lu's method.

[0022] The method of the present invention adopts an electrodeposition method and can extract trace amounts of Yb from a large amount of Yb. 177 Lu, for example, can be found in gram quantities after reactor irradiation 176 Extraction of trace amounts of Yb from the target 177 Lu and Yb have good removal effect. After separation, 176 The removal rate of Yb is 97.6%; 177 The Lu recovery rate is greater than 99.9%, and the recovery rate is high. The device provided by the present invention is simple, low in cost, and the electrodeposition separation process is simple to operate. The separation process is short in time and can reduce 177 The loss of production due to Lu decay makes the process more economical. Less radioactive waste liquid is generated during separation, which can reduce the subsequent radioactive waste liquid treatment costs. BRIEF DESCRIPTION OF THE DRAWINGS

[0023] Figure 1 FIG. 4 is a schematic structural diagram of an electrodeposition device according to an embodiment of the present invention. DETAILED DESCRIPTION

[0024] The following will clearly and completely describe the technical solutions in the embodiments of the present invention in combination with the embodiments of the present invention and the accompanying drawings. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0025] Throughout the specification, unless otherwise specifically stated, the terms used herein should be understood as meanings commonly used in the art. Therefore, unless otherwise defined, all technical and scientific terms used herein have the same meanings as those generally understood by those skilled in the art to which the present invention belongs. In the event of a conflict, the present specification takes precedence.

[0026] It should be noted that, in the embodiments of the present invention, the terms "include", "comprise" or any other variants thereof are intended to cover non-exclusive inclusion, so that a method or device including a series of elements includes not only the elements explicitly stated, but also other elements not explicitly listed, or also includes elements inherent to the implementation of the method or device. In the absence of further restrictions, an element defined by the sentence "includes a ..." does not exclude the existence of other related elements in the method or device including the element.

[0027] It should be noted that the terms "first\second\third" involved in the embodiments of the present invention are only used to distinguish similar objects, and do not represent a specific order for the objects. It is understandable that the specific order or sequence of "first\second\third" can be interchanged where permitted. It should be understood that the objects distinguished by "first\second\third" can be interchanged where appropriate, so that the embodiments of the present invention described herein can be implemented in an order other than those illustrated or described herein.

[0028] The electrochemical method is simple to operate and has fast separation, and high purity can be obtained in a short time. 177 Lu, and no large amount of radioactive waste liquid will be produced in the process, so the electrochemical method can be used as an efficient method for carrier-free 177 Separation of Lu. Among the Yb / Lu separation technologies that have been made public, researchers have adopted the sodium amalgam electrodeposition method, which has obvious advantages over extraction methods, ion exchange methods, etc. in separation effect. However, the sodium amalgam electrodeposition method for separating Yb / Lu requires the preparation of sodium amalgam first, and the sodium content of the prepared sodium amalgam needs to be determined. The operation process is complicated, and this process may also produce large errors, affecting the experimental results. In addition, Hg will be exposed to the air during titration, and there may be leakage of Hg vapor, which brings certain safety risks to the operator and the environment.

[0029] In view of this, the present invention provides a separation 176 Yb and 177 Lu's method comprises the following steps:

[0030] Will include 176 Yb and 177 Lu's 176 The Yb target is dissolved with acid, and then the target solution is heated and evaporated to dryness;

[0031] Adding a solution comprising a complexing agent to obtain a solution comprising 176 Yb 3+ and 177 Lu 3+ The electrolyte, wherein the complexing agent is capable of complexing at least 176 Yb 3+ ;

[0032] The electrolyte is subjected to electrodeposition to separate 176 Yb and 177 Lu, where the cathode is Hg.

[0033] The method of the present invention will 176 After the Yb target is completely dissolved with acid, the target solution is evaporated to dryness and then a solution including a complexing agent is added, and then electrodeposition is used to separate 176 Yb and 177 Lu. On the one hand, electrodeposition separation 176 Yb / 177 Lu is obtained by using 176 Yb and 177 The difference in the reduction potential of Lu is achieved. In addition, the complexing agent 176 Yb 3+ Complexation reduction 176 Yb 3+ The reduction potential is more conducive to separation 176 Yb and 177 Lu. On the other hand, the electron configuration of Lu element is [Xe]4f 14 5d 1 6s 2 , can only exist in solutions and compounds in a trivalent form, and the electron configuration of the Yb element is [Xe]4f 14 6s 2 In addition to the trivalent form, it can also exist in a relatively stable divalent form. The divalent form of Yb and metallic Yb have high solubility in mercury (Hg). Therefore, the method of the present invention uses Hg as a cathode for electrolysis to reduce Yb(III) to Yb(II), and then further reduces Yb(II) to metallic Yb, while forming an alloy deposition with the Hg cathode to react with the trivalent Lu in the solution. 3+ Separation is achieved to achieve the purpose of Yb / Lu separation. 177 Lu solution can be further purified using leaching resin or cation exchange resin to ensure 177 Lu is not contaminated by Hg. 177 Lu solution has high purity and can be used for medical applications without carriers 177 Preparation of Lu.

[0034] In the method of the present invention, a large amount of reagents used to dissolve the target are removed by heating and evaporating to concentrate the target solution. 176 Yb and 177 Lu, then add a complexing agent aqueous solution to dissolve the solid obtained after the above evaporation, thereby adjusting the 176 Yb and 177The acidic environment of the Lu solution is conducive to the subsequent electrodeposition treatment.

[0035] In some embodiments, the 176 Yb targets are obtained by irradiation, where 176 Yb and 177 The mass ratio of Lu is less than or equal to 5000:1. In some preferred embodiments, 176 In the Yb target, 176 Yb and 177 The mass ratio of Lu is 2000:1 to 5000:1. When the neutron flux is 2.0E+14n / s·cm 2 1g irradiated under the conditions of 176 Yb target produced 7 to 15 days later 177 The content of Lu is about 0.2mg to 0.4mg. 176 Separation of Yb target 177 Lu, especially from gram quantities 176 Yb target separation micro-scale 177 Lu, achieve micro-level 177 Separation of Lu.

[0036] In some embodiments, the 176 The Yb target is a Yb-176 target with an enrichment of more than 99%. After the Yb-176 target with an enrichment of more than 99% is irradiated in the reactor, in addition to the target 176 Yb and target nuclides 177 Except Lu, there are almost no other impurities, which can greatly reduce the content of 177 Lu solution, reducing the need for further separation of impurities. 176 The Yb target is the target after being irradiated by high flux neutrons in the reactor.

[0037] In some embodiments, 4-6 mol / L nitric acid or 4-6 mol / L hydrochloric acid is used to heat and dissolve the irradiated 176 Yb target. 176 The Yb target is fully dissolved, and the Yb element and the Lu element are converted into trivalent ion form, so as to facilitate subsequent separation by electrodeposition.

[0038] In some embodiments, the heating and evaporation can be performed by a heating method known to those skilled in the art. In the present invention, the target heating and dissolving and the target evaporation can be performed in the same device. For example, in a hot chamber, a target dissolving device is used to heat and dissolve the irradiated Yb target with acid, and the target evaporation is heated to dryness.

[0039] In some embodiments, the complexing agent is selected from citrate and α-hydroxyisobutyric acid. The complexing agent forms a complex with Yb or Lu ions, and due to the different stability constants of the complexes, the reduction potential of the metal ions will change. 176 Yb 3+ Complexation reduces 176 Yb 3+ The reduction potential of 176 Yb 3+ is preferentially reduced and enters the cathode Hg, achieving 176 Yb and 177 In addition, the acid radical ions in the complexing agent can act as a buffer solution in the solution, ensuring the pH stability of the solution and avoiding the hydrolysis of metal ions in the solution, further ensuring 176 Yb 3+ and 177 Lu 3+ In some embodiments, the citrate is sodium citrate.

[0040] In some embodiments, the solution comprising the complexing agent is 0.15-0.4 mol / L citrate or 0.3-0.6 mol / L α-hydroxyisobutyric acid. Too high a concentration of the complexing agent may result in a decrease in the current efficiency during the electrodeposition process, while a low concentration of the complexing agent may have a negative effect on the current efficiency. 176 Yb 3+ The complexing effect is low, which makes 176 Yb 3+ The electrodeposition reduction effect of is relatively poor. By making the concentration of the complexing agent within the above range, it is beneficial to increase the 176 Yb 3+ and 177 Lu 3+ separation efficiency.

[0041] In some embodiments, the pH of the electrolyte is less than or equal to 7, so that the Yb element and the Lu element exist in the solution as trivalent ions, so that the Yb element and the Lu element can be separated by electrodeposition. In some embodiments, the pH of the electrolyte is preferably 5.0-7.0. By making the pH of the electrolyte within the above range, it is beneficial to improve the 176 Yb 3+ and 177 Lu 3+ In the method of the present invention, the added complexing agent can be used as a buffer solution to ensure that the pH of the electrolyte does not change significantly during the electrodeposition process, so there is no need to add acid or alkali to adjust the pH value to ensure that the pH of the electrolyte is stable within a certain range.

[0042] In some embodiments, the pH of the solution can be adjusted using a dilute hydrochloric acid solution or ammonia water. Using the above reagents to adjust the pH can avoid the introduction of new impurity ions into the solution and reduce the occurrence of side reactions during the electrodeposition process, thereby helping to improve 177 Recovery rate of Lu.

[0043] In some embodiments, the anode is a platinum sheet or a platinum bar. The anode is an inert metal, such as Pt metal, to prevent the anode metal material from entering the electrolyte, thereby ensuring that the separated 177 The purity of Lu solution. During the electrodeposition process, 2Cl - +2e - →Cl2 and oxygen evolution reaction, the gas produced by the reaction is discharged into the electrolyte, and the electrodeposition 177 The purity of the Lu solution has little effect.

[0044] In some embodiments, the electrodeposition is performed using a DC power supply of 8 to 14 V. 3+ The electroreduction reaction is achieved 176 Yb and 177 For example, the voltage of the DC power supply can be 8V, 9V, 10V, 11V, 12V, 13V, 14V or a value within a range consisting of any two values ​​thereof.

[0045] In some embodiments, the electrodeposition is carried out for 30-60 min. Thus, the trivalent form of Yb in the solution is ensured. 3+ Ions can be completely reduced, increasing 176 The removal rate of Yb increases after electrodeposition. 177 Purity of Lu.

[0046] In some embodiments, during the electrodeposition process, the electrolyte is maintained in the range of 22 to 25°C. When the electrolyte temperature is lower than 20°C, the electrodeposition efficiency is low; and when the electrolyte temperature is greater than 25°C, the volatilization of the toxic substance mercury will be accelerated. Therefore, it is beneficial to maintain the temperature of the electrolyte within the above range, which is beneficial to improve the electrodeposition efficiency and avoid the volatilization of cathode Hg. In the present invention, the electrolyte can be maintained in the range of 22 to 25°C by methods known in the art. Exemplarily, during the electrodeposition process, the electrolyte is maintained in the range of 22 to 25°C by water circulation.

[0047] In some embodiments, the method further comprises, after the electrodeposition is completed, replacing the cathode and repeating the electrodeposition process. By replacing the mercury cathode, a new carrier for dissolving the Yb element reduction product is provided, thereby improving 176 The removal rate of Yb increases the177 After the electrodeposition is completed, the Yb-Hg alloy exists on the surface of the cathode Hg, which leads to a decrease in the electrodeposition reaction rate. By replacing the mercury cathode, the electrodeposition efficiency can be improved, thereby improving 176 Yb and 177 Separation efficiency of Lu.

[0048] In some embodiments, the method further comprises identifying the 177 Lu and measure the content of the dissolved solution after the electrodeposition 177 The radioactivity of Lu and other possible impurities was used to determine the radioactivity of the solution after electrodeposition. 177 The radioactive nuclear purity of Lu and whether the carrier-free Lu that meets the medical requirements is obtained 177 Lu products.

[0049] The separation of the present invention 176 Yb and 177 Lu's method can 176 Yb target 176 Yb and 177 Lu separation, where 176 Yb is enriched in the cathode mercury liquid. 177 Lu is enriched in the electrolyte after electrodeposition.

[0050] Due to enrichment 176 Yb is expensive and needs to be recycled. In the present invention, the enriched Yb deposited in the cathode mercury solution separated by the above method is 176 Yb can be washed multiple times with 6M hydrochloric acid, for example 2-3 times, with sufficient shaking during the washing process to enrich 176 Yb metal reacts with hydrochloric acid to 176 Yb ions are transferred back into the solution, and then treated by precipitation, calcination, etc. to obtain 176 Yb2O3, after three washings 176 The total recovery rate of Yb element is about 90%.

[0051] The present invention also provides a carrier-free extraction method. 177 Lu's method, the method comprising the separation 176 Yb and 177 Lu's method.

[0052] In some embodiments, the separation by electrodeposition 177 Lu is enriched in the electrolyte, which will 177 In some embodiments, the purification is achieved by leaching resin or cation exchange resin. 177 Lu can be used as a medical carrier 177Lu is used for subsequent 177 Preparation and application of Lu drugs.

[0053] Separation of the present invention 176 Yb and 177 In Lu's method, the electrodeposition process can be carried out using an electrodeposition device known in the art, or using an electrodeposition device as described below. By using the electrodeposition device as described below to carry out the electrodeposition step, it is advantageous to simplify the separation 176 Yb and 177 Lu's steps reduce the generation of waste liquid and the consumption of mercury.

[0054] The following will be combined Figure 1 The invention is described in detail for separating 176 Yb and 177 Lu electrodeposition apparatus.

[0055] The electrodeposition device of the present invention comprises:

[0056] An electrodeposition tank (1), the electrodeposition tank (1) is sealed and used to contain an electrolyte;

[0057] A power source (2), including a positive electrode and a negative electrode;

[0058] a cathode (3), one end of which is connected to the negative electrode of the power source (1), the cathode being Hg and located below the electrodeposition tank (1); when the electrodeposition tank contains an electrolyte, one end of the cathode is in contact with the electrolyte;

[0059] an anode (4), one end of the anode (4) being connected to the positive electrode of the power source (1), and the other end of the anode (4) being located in the electrodeposition tank (1), and when the electrodeposition tank contains an electrolyte, one end of the anode is in contact with the electrolyte;

[0060] In the electrodeposition device, one end of the cathode (3) and the anode (4) are connected to a power source (2) through a wire, and the other end is in contact with the solution in the electrolytic cell, thereby forming a conductive loop to achieve an electrodeposition reaction.

[0061] In one embodiment, the electrodeposition tank is sealed by a detachable sealing cover (5). By sealing the electrodeposition tank, mercury can be prevented from volatilizing into the air. In some embodiments, the detachable sealing cover is made of polytetrafluoroethylene material. The detachable sealing cover can be used to easily open the electrodeposition tank and add the electrolyte or cathode liquid into the electrodeposition device from above the electrodeposition tank.

[0062] In some embodiments, the anode (4) is selected from a platinum sheet or a platinum bar.

[0063] In one embodiment, the cathode (4) is connected to a conductive wire via a platinum wire electrode (8), and further connected to the negative electrode of the power source (2).

[0064] In one embodiment, the electrodeposition device further comprises a cathode liquid outlet plug (6) and a cathode outlet (7), wherein the cathode outlet (7) is located below the cathode (3) and is connected via the cathode liquid outlet plug (6), and the cathode liquid outlet plug (6) is used to control the opening and closing of the cathode outlet (7). When the cathode liquid outlet plug (6) is opened, the cathode outlet (7) is opened and the cathode liquid is discharged from the cathode outlet.

[0065] In some embodiments, the electrodeposition device further comprises a circulating cooling system (9), the circulating cooling system (9) surrounds the electrodeposition tank and is used to provide a constant temperature for the solution. The circulating cooling system (9) comprises a circulating cooling water inlet (10) and a circulating cooling water outlet (11). The circulating cooling water enters through the circulating cooling water inlet (10), flows through the cavity surrounding the electrodeposition tank, and then flows out from the circulating cooling water outlet (11). The cooling water in the circulating cooling system (9) can be circulated by means known in the art, for example, the circulating flow of the cooling water can be achieved by a circulating pump.

[0066] In some embodiments, the electrodeposition device further comprises a gas filling system, wherein the gas filling system connects the inside of the electrodeposition tank with the external environment through a pipeline. The gas filling system comprises a gas inlet (12) and a gas outlet (13), and the gas enters the sealed electrodeposition tank (1) through the gas inlet (12) and is discharged to the outside of the device through the gas outlet (13). An inert gas, such as argon, is introduced into the electrodeposition device through the gas filling system to play a stirring role, and the gas does not participate in the reaction.

[0067] Through the above-mentioned electrodeposition device, Yb in the electrolyte 3+ Reduction reaction occurs at the cathode to obtain divalent Yb 2+ and / or metallic Yb, and dissolved in the cathode mercury, the solution 177 Lu does not undergo electrochemical reaction and is insoluble in mercury, and thus remains in the solution in the electrolytic cell in the form of trivalent ions. After the electrodeposition reaction is completed, the cathode mercury in which the Yb element is dissolved can be conveniently removed from the cathode outlet, thereby removing the Yb element from the electrolyte. The separation of the present invention is carried out by the electrodeposition device of the present invention. 176 Yb and 177 Lu's method is simple to operate and time-saving, produces less radioactive waste liquid during the separation process, and has a Yb removal rate of up to 97.6%. 177 The recovery rate of Lu was greater than 99.9%.

[0068] The following describes the embodiments of the present invention in detail through specific examples. It should be understood that these examples are only exemplary and cannot be used as a limitation on the scope of the present invention.

[0069] Example

[0070] In the following examples, since radioactive targets are strictly controlled, in order to verify the feasibility of the method of the present invention, a self-prepared target dissolution simulation solution containing Yb and Lu elements was used to implement the method of the present invention.

[0071] Example 1

[0072] Weigh appropriate amounts of YbCl3 and LuCl3 and dissolve them in 500 mL of deionized water to prepare a simulated solution with a Yb concentration of 2 g / L and a Lu concentration of 1 mg / L (the mass ratio of Yb to Lu in the simulated solution is 2000:1). Take 20 mL of the Yb / Lu simulated solution and add 0.5 mCi 177 Lu is used as a tracer. Weigh an appropriate amount of sodium citrate and add it to the above mixed solution to make the concentration of sodium citrate 0.15 mol / L. After shaking and dissolving, use NH3·H2O or HCl solution to adjust the pH to 5. Take 10 mL of Hg and add it to Figure 1 In the electrodeposition device shown, 20 mL of Yb / Lu mixed solution was added, a platinum electrode was inserted, Hg was used as the cathode, the platinum electrode was used as the anode, and the solution temperature was maintained at 25°C with circulating cooling water. Electrolysis was performed for 30 minutes with 14 V DC. After the first electrodeposition, Hg was released from the lower end, the sealing cover was opened, new Hg was added from the top of the electrodeposition tank, and the second electrodeposition was performed under the same conditions.

[0073] After the two electrodepositions were completed, a certain volume of the 177 Lu solution, using high purity germanium gamma spectrometer to measure the solution 177 Lu radioactivity, Yb in electrolyte before and after separation measured by ICP-MS 3+ The removal rate and concentration of Yb element are calculated using the following formula: 177 Recovery rate of Lu.

[0074] Yb removal rate = [(Yb in electrolyte before separation 3+ Content of Yb in the electrolyte after separation 3+ Content of Yb in electrolyte before separation 3+ Content] × 100%.

[0075] 177 Lu recovery rate = (Lu in electrolyte after separation 177 Radioactivity of Lu in electrolyte before separation 177 radioactivity)×100%.

[0076] The test results are shown in Table 1. The results show that 92.0% of Yb in the solution can be removed under this condition. 177 There is almost no loss of Lu and the recovery rate is greater than 99.99%.

[0077] Embodiments 2 to 4

[0078] The separation of Yb / Lu was carried out in a similar manner to Example 1, except that the concentration of the complexing agent sodium citrate was adjusted with reference to the parameters shown in Table 1. 177 The test results of Lu recovery are shown in Table 1.

[0079] Example 5

[0080] Weigh appropriate amounts of YbCl3 and LuCl3 and dissolve them in 500 mL of deionized water to prepare a simulated solution with a Yb element concentration of 2 g / L and a Lu element concentration of 1 mg / L (the mass ratio of Yb to Lu in the simulated solution is 2000:1). Take 20 mL of the Yb / Lu simulated solution and add 0.5 mCi 177 Lu is used as a tracer. Weigh an appropriate amount of α-hydroxyisobutyric acid and add it to the above mixed solution to make the concentration of α-hydroxyisobutyric acid 0.3 mol / L. After shaking and dissolving, use NH3·H2O or HCl solution to adjust the pH to 5. Take 10 mL of Hg and add it to Figure 1 In the electrodeposition device shown, 20 mL of Yb / Lu mixed solution was added, a platinum electrode was inserted, Hg was used as the cathode, the platinum electrode was used as the anode, and the solution temperature was maintained at 25°C with circulating cooling water. Electrolysis was performed for 30 minutes with 14 V DC. After the first electrolysis, Hg was released from the lower end, the sealing cover was opened, new Hg was added from the top of the electrodeposition tank, and the second electrodeposition was performed under the same conditions.

[0081] After the two electrodepositions, a high-purity germanium γ spectrometer was used to measure the concentration of 177 The activity of Lu was measured by ICP-MS in the electrolyte before and after separation of Yb 3+ The test results are shown in Table 1. The results show that 97.6% of Yb in the solution can be removed under this condition. 177 The Lu recovery rate is greater than 99.99%.

[0082] Embodiment 6-8

[0083] The separation of Yb / Lu was carried out in a similar manner to that of Example 5, except that the concentration of the complexing agent α-hydroxyisobutyric acid was adjusted with reference to the parameters shown in Table 1. 177 The test results of Lu recovery are shown in Table 1.

[0084] Comparative Example 1

[0085] Weigh appropriate amounts of YbCl3 and LuCl3 and dissolve them in 500 mL of deionized water to prepare a simulated solution with a Yb element concentration of 2 g / L and a Lu element concentration of 1 mg / L (the mass ratio of Yb to Lu in the simulated solution is 2000:1). Take 20 mL of the Yb / Lu simulated solution and add 0.5 mCi 177 Lu is used as a tracer. After shaking and dissolving, adjust the pH to 5 using NH3·H2O or HCl solution. Take 10 mL of Hg and add it to Figure 1 In the electrodeposition device shown, 20 mL of Yb / Lu mixed solution was added, a platinum electrode was inserted, Hg was used as the cathode, the platinum electrode was used as the anode, and the solution temperature was maintained at 25°C with circulating cooling water. Electrolysis was performed for 30 minutes with 14 V DC. After the first electrolysis, Hg was released from the lower end, the sealing cover was opened, new Hg was added from the top of the electrodeposition tank, and the second electrodeposition was performed under the same conditions.

[0086] After the two electrodepositions, a high-purity germanium γ spectrometer was used to measure the concentration of 177 The activity of Lu was measured by ICP-MS in the electrolyte before and after separation of Yb 3+ The test results are shown in Table 1. The results show that 72.1% of Yb in the solution can be removed under this condition, but 177 The recovery rate of Lu was only 23.6%. Under this condition, the loss of Yb and Lu was mainly due to the change of pH value of the solution during electrolysis, which led to ion hydrolysis and finally formed precipitation.

[0087] Table 1

[0088]

[0089]

[0090] “-” in the table means not added.

[0091] From the test results shown in Table 1, it can be seen that 176 Yb and 177 In the separation process of Lu, adding complexing agent can effectively improve 177 The recovery rate of Lu is high, and it has a high Yb removal rate, which can realize the separation of Yb and Lu elements.

[0092] The above description is only a preferred embodiment of the present invention, and does not limit the patent scope of the present invention. All equivalent structural changes made by using the contents of the present invention specification and drawings under the inventive concept of the present invention, or directly / indirectly applied in other related technical fields are included in the patent protection scope of the present invention.

Claims

1. A separation 176 Yb and 177 Lu's method, characterized in that The following steps are involved: Will include 176 Yb and 177 Lu's 176 The Yb target is dissolved with acid, and then the target solution is heated and evaporated to dryness; Adding a solution comprising a complexing agent to obtain a solution comprising 176 Yb 3+ and 177 Lu 3+ The electrolyte, wherein the complexing agent is capable of complexing at least 176 Yb 3+ ; The electrolyte is subjected to electrodeposition to separate 176 Yb and 177 Lu, where the cathode is Hg.

2. The method according to claim 1, wherein: Said 176 The Yb target is an irradiated target, wherein 176 Yb and 177 The mass ratio of Lu is less than or equal to 5000:

1.

3. The method according to claim 1 or 2, wherein: The complexing agent is selected from citrate and α-hydroxyisobutyric acid; preferably, the citrate is sodium citrate; more preferably, the solution including the complexing agent is 0.15-0.4 mol / L citrate or 0.3-0.6 mol / L α-hydroxyisobutyric acid.

4. The method according to claim 1 or 2, wherein: The pH value of the electrolyte is less than or equal to 7, preferably 5.0 to 7.

0.

5. The method according to claim 1 or 2, wherein: The electrodeposition adopts 8-14V direct current.

6. The method according to claim 1 or 2, wherein: The anode of the electrolysis is a platinum sheet or a platinum strip.

7. The method according to claim 1 or 2, wherein: The method further includes, after the electrodeposition is completed, replacing the cathode Hg and repeating the electrodeposition.

8. The method according to claim 1, wherein: The method further comprises measuring the 177 The radioactivity of Lu.

9. The method according to claim 1, wherein: The acid is 4-6 mol / L nitric acid or 4-6 mol / L hydrochloric acid.

10. An extraction without carrier 177 Lu's method, comprising the separation of any one of claims 1-9 176 Yb and 177 Lu's method.

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