Preparation method of high-purity low-acidity 67Cu solution and high-purity low-acidity 67Cu solution

Abstract

The invention relates to a radioisotope preparation method, in particular to a preparation method of a high-purity low-acidity 67Cu solution and the high-purity low-acidity 67Cu solution, and aims to overcome the defects of low purity and too high medium acidity of the 67Cu solution in the prior art. The preparation method comprises the following steps: firstly, dissolving a target material, and then separating by using a CU resin separation column to obtain a 67Cu desorption solution; the preparation method comprises the following steps: preparing 67Cu solution with high purity and low acidity, further removing impurities through a TK201 resin separation column, and carrying out medium conversion to obtain the 67Cu solution with high purity and low acidity, and meanwhile, the invention also provides the 67Cu solution with high purity and low acidity, which is prepared by the method and has the pH value of 1-2.

Description

Technical Field

[0001] The present invention relates to a method for preparing radioactive isotopes, and in particular to a method for preparing a radioactive isotope with high purity and low acidity. 67 Preparation method of Cu solution with high purity and low acidity 67 Cu solution. Background Art

[0002] 67 Cu is a β-radionuclide with a half-life of 61.8h. It emits β-rays with a maximum energy of 577keV and an average energy of 141keV, accompanied by the release of γ-rays of 91, 93 and 185keV. 67 Cu is a medical isotope that is suitable for both radiodiagnosis and in vivo radiotherapy.

[0003] 67 Cu can be 68 Zn(γ,p) 67 Cu, 68 Zn(p,2p) 67 Cu, 70 Zn(p,α) 67 Cu and 70 Zn(d,x) 67 Cu and other reactions, these methods require a large amount of Zn target and can only separate trace amounts of Zn from other radioactive impurities. 67 Cu, and in order to obtain the medical requirements 67 Cu, trace amounts of which must be separated and purified from the irradiated Zn target 67 Cu. Currently, it is difficult to separate trace amounts of Cu from a large amount of Zn target. 67 The methods for removing Cu include anion exchange, coprecipitation, solvent extraction, extraction chromatography, sublimation and electrodeposition.

[0004] Anion exchange can be used to separate Zn and 67 Cu, but to separate trace amounts from large amounts of Zn 67 Cu requires a large separation column to adsorb Zn, the aqueous solution has a slow flow rate, takes a long time, and the obtained 67 Cu desorption solution has large volume and low specific activity, which does not have obvious advantages. 67 It is feasible to separate Cu in the form of CuS, but it needs to be operated in a hot chamber, which makes separation difficult. Sublimation and electrodeposition can remove a large amount of Zn at one time, but 67 There are still milligrams of Zn remaining in Cu, so it is necessary to set up another anion exchange column to remove the residual Zn.

[0005] Solvent extraction is an effective separation method. Dasgupta AK et al. (Dasgupta AK, Mausner L.F. and Srivastava SCA New Separation Procedure For 67 Cu from ProtonIrradiated Zn.Appl.Radiat.Isot.Int.J.Radiat.Appl.Instrum.Part A,1991,42(4):371-376) was separated by 0.01% dithizone-carbon tetrachloride extraction 67 Cu, and then further purified with AG1×8 anion column to remove residual impurities such as Zn, Cr, Mn, Ni, etc., and finally desorbed with 1Mol / L HCl solution 67 Cu.

[0006] Extraction chromatography is a separation technology that combines the high selectivity of solvent extraction with the high efficiency of chromatographic separation. One of the keys to the separation effect of extraction chromatography is the performance of the leaching resin. Dirks C et al. (Dirks C, Scholten B, Happel S, Zulauf A, Bombard A, Jungclas H. Characterization of a Cu selective resin and its application to the production of 64Cu. J Radioanal Nucl Chem, 2010, 286: 671–674) and Ramiz A. Aliev et al. (Ramiz A. Aliev, Sergey S. Belyshev, Alexander A. Kuznetsov, et al. Photonuclear production and radiochemical separation of medically relevant radionuclides: 67 Cu.Journal of Radioanalytical and NuclearChemistry, 2019, 321: 25–132.) The performance of Cu selective resin produced by TrisKem International of France was studied in detail, and the separation of Cu from Zn target solution was established. 67 Cu method: first use a Cu selective resin column to adsorb in a pH = 2 HCl solution medium 67 Cu, then desorbed with 4-7Mol / L HCl solution and collected 67 Cu, get67 The recovery rate of Cu is greater than 95%, and the decontamination coefficients of Zn and Ni are greater than 10 5 .

[0007] pass 68 Zn(γ,p) 67 Cu, 68 Zn(p,2p) 67 Cu, 70 Zn(p,α) 67 Cu and 70 Zn(d,x) 67 Cu and other reactions 67 The yield of Cu is generally low. For large-scale production, several hundred grams of Zn target must be used. Even if Cu selective resin is used, the decontamination coefficient of Zn is about 10 5 ,final 67 There are also milligrams of Zn in Cu products, which 67 The purity of Cu is not high, and the medium is 4-7Mol / L HCl solution, which has too high acidity, seriously affecting 67 Radiopharmaceutical labeling with Cu and its clinical application in nuclear medicine.

[0008] In summary, the existing 67 There is a separation and purification technology for Cu 67 The purity of Cu solution is low, the acidity of medium is too high, etc., which cannot meet the requirements of nuclear medicine. 67 The Cu solution must have high specific activity, high radiochemical purity and low acidity. Summary of the invention

[0009] The purpose of the present invention is to solve the problems existing in the prior art 67 The purity of Cu solution is not high and the acidity of the medium is too high. 67 Preparation method of Cu solution with high purity and low acidity 67 Cu solution.

[0010] To achieve the above purpose, the technical solution provided by the present invention is as follows:

[0011] A high purity low acidity 67 The preparation method of Cu solution is special in that it comprises the following steps:

[0012] Step 1. Target dissolution

[0013] dissolving the irradiated Zn target to obtain a target dissolving solution;

[0014] Step 2. 67 Cu Separation

[0015] The target material solution was separated using the pre-prepared CU resin separation column to obtain 67 Cu desorption solution;

[0016] 67 The Cu desorption solution is obtained by eluting the CU resin separation column with HCl solution in the concentration range of 5 to 8 Mol / L;

[0017] Step 3. Medium transformation to obtain high purity and low acidity 67 Cu solution

[0018] 3.1. The result from step 2 67 The Cu desorption solution was introduced into the pre-prepared TK201 resin separation column, so that 67 Cu and residual Zn 2+ 、Co 2+ , Ga 2+ 、Ni 2+ Impurities are adsorbed on the separation column;

[0019] The TK201 resin separation column was washed with 1 to 2 column volumes of HCl solution and all of it was discharged; the concentration of the HCl solution was the same as that obtained in step 2. 67 The concentration of HCl solution used in the Cu desorption solution was the same;

[0020] 3.2. Elute the TK201 resin column with HCl solution in the concentration range of 0.5 to 1Mol / L to remove the residual Co 2 + 、Ni 2+ Impurities;

[0021] 3.3. Desorb with 3 to 5 column volumes of HCl solution in the concentration range of 0.01 to 0.02 mol / L 67 Cu gets high purity and low acidity 67 Cu solution, complete the preparation.

[0022] Furthermore, step 2 is specifically as follows:

[0023] 2.1. The target material solution obtained in step 1 is introduced into the pre-prepared CU resin separation column to adsorb 67 Cu, followed by eluting the CU resin separation column with 1 to 2 column volumes of HCl solution in the concentration range of 0.005 to 0.02 Mol / L;

[0024] 2.2. Elute the CU resin column with HCl solution at a concentration of 0.005-0.15Mol / L to remove residual Zn 2+ 、Ni 2+ 、Co 2+ And Ga 2+ Impurities;

[0025] 2.3. Elute the CU resin separation column with 2 to 5 column volumes of HCl solution in the concentration range of 5 to 8 mol / L to desorb 67 Cu, get 67 Cu desorption solution.

[0026] Furthermore, step 2.2 is specifically as follows:

[0027] 2.2.1. Elute the CU resin column with 5 to 10 column volumes of HCl solution in the concentration range of 0.005 to 0.02 mol / L to remove residual Zn 2+ 、Ni 2+ 、Co 2+ Impurities;

[0028] 2.2.2. Elute the CU resin column with 2 to 4 column volumes of HCl solution in the concentration range of 0.1 to 0.15 mol / L to remove residual Ni 2+ , Ga 2+ Impurities.

[0029] Furthermore, step 1 is specifically as follows:

[0030] The irradiated Zn target is transferred to a dissolver, and a mixture of HCl solution and HNO3 solution is added dropwise until the Zn target is completely dissolved, and then evaporated to dryness at 100-140° C., and then HCl solution with a concentration of 0.005-0.02 mol / L is added to dissolve the target solution;

[0031] In the mixture of the HCl solution and the HNO3 solution, the volume ratio of the HCl solution to the HNO3 solution is (49-51):1, the mass concentration of the HCl solution used is greater than 9%, and the mass concentration of the HNO3 solution is greater than 17%.

[0032] Furthermore, in step 1, in the mixture of the HCl solution and the HNO3 solution, the mass concentration of the HCl solution used is greater than or equal to 18%, and the mass concentration of the HNO3 solution is greater than or equal to 34%;

[0033] The amount of 0.005-0.02Mol / L HCl solution added is 2-5mL per gram of Zn;

[0034] In step 2.1, the concentration of the HCl solution used is the same as that thereof.

[0035] Further, in step 1, in the mixture of the HCl solution and the HNO3 solution, the volume ratio of the HCl solution to the HNO3 solution is 50:1, the mass concentration of the HCl solution used is 36%, and the mass concentration of the HNO3 solution is 68%; after evaporation, a 0.01Mol / L HCl solution is added to dissolve the target material solution, and the amount of the HCl solution added is 3mL per gram of Zn;

[0036] In step 2.1, the amount of HCl solution added is 1 column volume;

[0037] In step 2.2.1, the concentration of HCl solution is 0.01Mol / L;

[0038] In step 2.2.2, the concentration of HCl solution is 0.1Mol / L;

[0039] In step 2.3, the amount of HCl solution used is 3 column volumes, and the concentration is 6 Mol / L;

[0040] In step 3.2, the amount of HCl solution used is 3 to 5 column volumes;

[0041] In step 3.3, the amount of HCl solution used is 4 column volumes, and the concentration is 0.01 Mol / L.

[0042] Further, in step 2.1, the CU resin separation column is prepared by the following steps:

[0043] Take an empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, and add it to the separation column. When the height of the CU resin reaches the predetermined height, install the upper filter plate to obtain a CU resin separation column, and balance the CU resin separation column with 10 to 12 column volumes of HCl solution. The concentration of the HCl solution is the same as that used for elution in step 2.1.

[0044] Further, in step 3.1, the TK201 resin separation column is prepared by the following steps:

[0045] Take an empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, and add it to the separation column. When the height of the TK201 resin reaches the predetermined height, install the upper filter plate to obtain a TK201 resin separation column, and balance the TK201 resin separation column with 10 to 12 column volumes of HCl solution. The concentration of the HCl solution is the same as that of the hydrochloric acid solution used for elution in step 3.1.

[0046] Furthermore, in step 3.2, the amount of HCl solution used is 3 column volumes, and the concentration is 0.5 Mol / L.

[0047] At the same time, the present invention also provides a high-purity, low-acidity 67 The Cu solution is special in that it uses a high-purity, low-acidity 67 Preparation method of Cu solution.

[0048] Beneficial effects of the present invention:

[0049] 1. The present invention cleverly combines CU resin and TK201 resin, uses two series-connected separation columns and a specific eluent to separate and purify Zn targets from a large amount of Zn targets. 67 Cu can more effectively remove Zn and other trace impurities, improve 67 The nuclear purity of Cu is high, low acidity and meets the requirements of nuclear medicine applications. 67 Cu solution.

[0050] 2. The present invention utilizes the characteristics of TK201 resin that it can adsorb Zn and Cu at high acidity and adsorb Zn but not Cu at low acidity to separate the high acidity obtained by CU resin separation column. 67 The Cu solution is converted into a low acidity of pH = 1 to 2 67 Cu solution, suitable for labeling of radiopharmaceuticals in downstream industries.

[0051] 3. The present invention reduces 67 Cu solution acidity, and further remove residual Zn and other impurities, to obtain high-purity low-acidity solution that meets the requirements of nuclear medicine applications. 67 Cu solution, and 67 Cu in solution 67 The purity of Cu core reaches over 98%. BRIEF DESCRIPTION OF THE DRAWINGS

[0052] Figure 1 is a flow chart of Embodiment 1 of the present invention;

[0053] Figure 2 This is a gamma energy spectrum of the target material solution before separation in Example 3 of the present invention;

[0054] Figure 3 After separation in Example 3 of the present invention 67 Gamma energy spectrum of Cu solution. DETAILED DESCRIPTION

[0055] Embodiment 1

[0056] The invention discloses a high-purity and low-acidity 67 The Cu solution was prepared by Figure 1 As shown, it specifically includes three steps:

[0057] Step 1: Target dissolution

[0058] The irradiated Zn target was transferred to a dissolver, and a mixture of concentrated HCl solution and concentrated HNO3 solution in a volume ratio of 51:1 was added dropwise until the Zn target was completely dissolved, and then evaporated to dryness at 110°C, and 0.02Mol / L HCl solution was added to dissolve it to obtain a target solution.

[0059] The chemical form of the Zn target is Zn metal or ZnO; the amount of 0.02 Mol / L HCl solution added is 5 mL per gram of Zn.

[0060] Step 2, 67 Cu Separation

[0061] Step 2.1, take a 5mL empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the CU resin reaches a predetermined height, install the upper filter plate to obtain a CU resin separation column;

[0062] Step 2.2, equilibrate the CU resin separation column with 11 column volumes of 0.02 mol / L HCl solution;

[0063] Step 2.3, the target material solution obtained in step 1 is introduced into the CU resin separation column for adsorption 67 Cu, then 2 column volumes of 0.02Mol / L HCl solution were used to elute the CU resin separation column, and the effluent was collected for the recovery and reuse of the Zn target;

[0064] Step 2.4: Elute the CU resin column with 5 column volumes of 0.01Mol / L HCl solution to remove residual Zn 2+ 、Ni 2+ 、Co 2+ etc. impurities;

[0065] Step 2.5: Elute the CU resin column with 4 column volumes of 0.13Mol / L HCl solution to remove residual Ni 2+ , Ga 2+ etc. impurities;

[0066] Step 2.6, desorb with 3 column volumes of 8Mol / L HCl solution 67 Cu, 67 Cu desorption solution.

[0067] Step 3, medium conversion

[0068] Step 3.1, take a 2 mL empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the TK201 resin reaches a predetermined height, install the upper filter plate to obtain a TK201 resin separation column;

[0069] Step 3.2, equilibrate the TK201 resin separation column with 12 column volumes of 8Mol / L HCl solution;

[0070] Step 3.3: Add the result from step 2 67 Cu desorption solution was introduced into TK201 resin separation column, Cu 2+ With residual Zn 2+ 、Co 2+ , Ga 2+ 、Ni 2+ It was adsorbed on the TK201 resin separation column;

[0071] Step 3.4, eluting the TK201 resin separation column with 2 column volumes of 8 Mol / L HCl solution, and draining all 8 Mol / L HCl solution;

[0072] Step 3.5, wash the TK201 resin column with 5 column volumes of 1Mol / L HCl solution to remove Co 2+ 、Ni 2+ Impurities;

[0073] Step 3.6, desorb with 5 column volumes of 0.1Mol / L HCl solution 67 Cu, get 67 Cu solution, while Zn 2+ , Ga 2+ Still adsorbed on the TK201 resin separation column and removed.

[0074] Embodiment 2

[0075] The invention discloses a high-purity and low-acidity 67 The method for preparing a Cu solution specifically comprises the following steps:

[0076] Step 1: Target dissolution

[0077] After irradiation, 100g 68 The Zn metal ingot was transferred to a 500 mL dissolver, and a mixture of concentrated HCl solution and concentrated HNO3 solution with a volume ratio of 50:1 was added dropwise until 68 The Zn metal ingot was completely dissolved, and then evaporated to dryness at 120°C, and then 300 mL of 0.01 Mol / L HCl solution was added to dissolve it, and the target material solution was obtained as the column liquid for later use.

[0078] Step 2, 67 Cu Separation

[0079] Step 2.1, take a 5mL empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the CU resin reaches the 5mL scale line height, install the upper filter plate to obtain a CU resin separation column;

[0080] Step 2.2, equilibrate the CU resin separation column with 50 mL of 0.01 Mol / L HCl solution;

[0081] Step 2.3, the upper column liquid obtained in step 1 is introduced into the CU resin separation column for adsorption 67 Cu, then 5 mL of 0.01 Mol / L HCl solution was used to elute the CU resin separation column, and the effluent was collected for 68 Recycling of Zn targets;

[0082] Step 2.4: Elute the CU resin column with 50 mL of 0.01 Mol / L HCl solution to remove residual Zn 2+ 、Ni 2+ 、Co 2+ etc. impurities;

[0083] Step 2.5: Elute the CU resin column with 10 mL of 0.1 Mol / L HCl solution to remove residual Ni 2+ , Ga 2+ etc. impurities;

[0084] Step 2.6, desorb with 15 mL of 6Mol / L HCl solution 67 Cu, 67 Cu desorption solution.

[0085] Step 3, medium conversion

[0086] Step 3.1, take a 2mL empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the TK201 resin reaches the 2mL scale line height, install the upper filter plate to obtain a TK201 resin separation column;

[0087] Step 3.2, equilibrate the TK201 resin separation column with 20 mL of 6Mol / L HCl solution;

[0088] Step 3.3: Add the 67 Cu desorption solution was introduced into TK201 resin separation column, Cu 2+ With residual Zn 2+ 、Co 2 + , Ga 2+ 、Ni 2+It was adsorbed on the TK201 resin separation column;

[0089] Step 3.4, eluting the TK201 resin separation column with 2 mL of 6 Mol / L HCl solution, and discharging all 6 Mol / L HCl solution desorption liquid;

[0090] Step 3.5, wash the TK201 resin column with 8 mL of 0.5 Mol / L HCl solution to remove Co 2+ 、Ni 2+ etc. impurities;

[0091] Step 3.6, desorb with 8 mL of 0.01Mol / L HCl solution 67 Cu, get 67 Cu solution, while Zn 2+ , Ga 2+ Still adsorbed on the TK201 resin separation column and removed.

[0092] Income 67 The Cu solution was tested for quality. 67 The purity of Cu core is 98.5% and the specific activity is 4.1×10 3 Ci / gCu, impurity content is: Zn 1.96μg / mL, Ni 0.87μg / mL, Co 0.64μg / mL, Ga 0.55μg / mL, and the medium is 0.01Mol / L HCl solution.

[0093] Embodiment 3

[0094] The invention discloses a high-purity and low-acidity 67 The method for preparing a Cu solution specifically comprises the following steps:

[0095] Step 1: Target dissolution

[0096] After irradiation, 130 g 68 The ZnO target was transferred to a 500 mL dissolver, and a mixture of concentrated HCl solution and concentrated HNO3 solution with a volume ratio of 50:1 was added dropwise until 68 The ZnO target material was completely dissolved; the solution was then evaporated to dryness at 140°C, and 300 mL of 0.01 Mol / L HCl solution was added to dissolve the target material solution, which was used as the column liquid for standby use. The γ energy spectrum was as follows: Figure 2 shown.

[0097] Step 2, 67 Cu Separation

[0098] Step 2.1, take a 5mL empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the CU resin reaches the 5mL scale line height, install the upper filter plate to obtain a CU resin separation column;

[0099] Step 2.2, equilibrate the CU resin separation column with 50 mL of 0.01 Mol / L HCl solution;

[0100] Step 2.3, the upper column liquid obtained in step 1 is introduced into the CU resin separation column for adsorption 67 Cu, then 5 mL of 0.01 Mol / L HCl solution was used to elute the CU resin separation column, and the effluent was collected for 68 Recycling of Zn targets;

[0101] Step 2.4: Elute the CU resin column with 50 mL of 0.01 Mol / L HCl solution to remove residual Zn 2+ 、Ni 2+ 、Co 2+ etc. impurities;

[0102] Step 2.5: Elute the CU resin column with 10 mL of 0.1 Mol / L HCl solution to remove residual Ni 2+ , Ga 2+ etc. impurities;

[0103] Step 2.6, desorb with 20 mL of 6Mol / L HCl solution 67 Cu, 67 Cu desorption solution.

[0104] Step 3, medium conversion

[0105] Step 3.1, take a 2mL empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the TK201 resin reaches the 2mL scale line height, install the upper filter plate to obtain a TK201 resin separation column;

[0106] Step 3.2, equilibrate the TK201 resin separation column with 20 mL of 6Mol / L HCl solution;

[0107] Step 3.3: Add the 67 Cu desorption solution was introduced into TK201 resin separation column, Cu 2+ With residual Zn 2+ 、Co 2 + , Ga 2+ 、Ni 2+It was adsorbed on the TK201 resin separation column;

[0108] Step 3.4, eluting the TK201 resin separation column with 2 mL of 6 Mol / L HCl solution, and discharging all 6 Mol / L HCl solution desorption liquid;

[0109] Step 3.5, wash the TK201 resin column with 8 mL of 0.5 Mol / L HCl solution to remove Co 2+ 、Ni 2+ etc. impurities;

[0110] Step 3.6, desorb with 8 mL of 0.01Mol / L HCl solution 67 Cu, get 67 Cu solution, while Zn 2+ , Ga 2+ Still adsorbed on the TK201 resin separation column and removed.

[0111] Income 67 The γ spectrum of Cu solution is as follows Figure 3 As shown, after quality inspection, 67 The purity of Cu core is 98.2% and the specific activity is 3.8×10 3 Ci / gCu, impurity content Zn2.25μg / mL, Ni 0.68μg / mL, Co0.75μg / mL, Ga 0.59μg / mL, the medium is 0.01Mol / L HCl solution.

[0112] Embodiment 4

[0113] The invention discloses a high-purity and low-acidity 67 The method for preparing the Cu solution comprises the following three steps:

[0114] Step 1: Target dissolution

[0115] 150g of irradiated 68 Zn metal ingots are distilled to remove most of the 68 Zn (recycling), the remaining less than 100 mg 68 Zn and 67 The Cu product was transferred to a 500 mL dissolver, and a mixture of concentrated HCl solution and concentrated HNO3 solution with a volume ratio of 50:1 was added dropwise until the Cu product contained 100 mL of Cu. 68 Zn and 67 The Cu product was completely dissolved, and then evaporated to dryness at 100°C, and then 0.5 mL of 0.01 Mol / L HCl solution was added to dissolve it and used as the column liquid for later use.

[0116] Step 2, 67Cu separation:

[0117] Step 2.1, take a 2mL empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the CU resin reaches the 2mL scale line height, install the upper filter plate to obtain a CU resin separation column;

[0118] Step 2.2, equilibrate the CU resin separation column with 20 mL of 0.01 Mol / L HCl solution;

[0119] Step 2.3, the upper column liquid obtained in step 1 is introduced into the CU resin separation column for adsorption 67 Cu, then 2 mL of 0.01 Mol / L HCl solution was used to elute the CU resin separation column, and the effluent was collected for 68 Recycling of Zn targets;

[0120] Step 2.4: Elute the CU resin column with 20 mL of 0.01 Mol / L HCl solution to remove residual Zn 2+ 、Ni 2+ 、Co 2+ etc. impurities;

[0121] Step 2.5: Elute the CU resin column with 4 mL of 0.1 Mol / L HCl solution to remove residual Ni 2+ , Ga 2+ etc. impurities;

[0122] Step 2.6, desorb with 8 mL of 6Mol / L HCl solution 67 Cu, 67 Cu desorption solution.

[0123] Step 3, medium transformation:

[0124] Step 3.1, take a 2mL empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the TK201 resin reaches the 2mL scale line height, install the upper filter plate to obtain a TK201 resin separation column;

[0125] Step 3.2, equilibrate the TK201 resin separation column with 20 mL of 6Mol / L HCl solution;

[0126] Step 3.3: Add the 67 Cu desorption solution was introduced into TK201 resin separation column, Cu 2+ With residual Zn 2+ 、Co 2 + , Ga 2+、Ni 2+ It was adsorbed on the TK201 resin separation column;

[0127] Step 3.4, eluting the TK201 resin separation column with 2 mL of 6 Mol / L HCl solution, and discharging all 6 Mol / L HCl solution desorption liquid;

[0128] Step 3.5, wash the TK201 resin column with 8 mL of 0.5 Mol / L HCl solution to remove Co 2+ 、Ni 2+ etc. impurities;

[0129] Step 3.6, desorb with 8 mL of 0.01Mol / L HCl solution 67 Cu, get 67 Cu solution, while Zn 2+ , Ga 2+ Still adsorbed on the TK201 resin separation column and removed.

[0130] Income 67 The Cu solution was tested for quality. 67 The purity of Cu core is 98.8% and the specific activity is 5.4×10 3 Ci / gCu, impurity content Zn 1.27μg / mL, Ni 0.63μg / mL, Co 0.48μg / mL, Ga0.46μg / mL, the medium is 0.01Mol / L HCl solution.

[0131] Embodiment 5

[0132] The invention discloses a high-purity and low-acidity 67 The Cu solution was prepared by Figure 1 As shown, the specific steps include:

[0133] Step 1: Target dissolution

[0134] The irradiated Zn target was transferred to a dissolver, and a mixture of concentrated HCl solution and concentrated HNO3 solution in a volume ratio of 49:1 was added dropwise until the Zn target was completely dissolved, and then evaporated to dryness at 110°C, and 0.005Mol / L HCl solution was added to dissolve it to obtain a target solution.

[0135] The amount of 0.005Mol / L HCl solution added is 4mL per gram of Zn.

[0136] Step 2, 67 Cu Separation

[0137] Step 2.1, take a 5mL empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the CU resin reaches a predetermined height, install the upper filter plate to obtain a CU resin separation column;

[0138] Step 2.2, equilibrate the CU resin separation column with 12 column volumes of 0.005 mol / L HCl solution;

[0139] Step 2.3, the target material solution obtained in step 1 is introduced into the CU resin separation column for adsorption 67 Cu, then eluted the CU resin separation column with 1.5 column volumes of 0.005Mol / L HCl solution, and collected the effluent for recycling of Zn target;

[0140] Step 2.4: Elute the CU resin column with 8 column volumes of 0.015Mol / L HCl solution to remove residual Zn 2+ 、Ni 2+ 、Co 2+ etc. impurities;

[0141] Step 2.5: Elute the CU resin column with 4 column volumes of 0.13Mol / L HCl solution to remove residual Ni 2+ , Ga 2+ etc. impurities;

[0142] Step 2.6, desorb with 5 column volumes of 7Mol / L HCl solution 67 Cu, 67 Cu desorption solution.

[0143] Step 3, medium conversion

[0144] Step 3.1, take a 2 mL empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, add it to the separation column, and when the height of the TK201 resin reaches a predetermined height, install the upper filter plate to obtain a TK201 resin separation column;

[0145] Step 3.2, equilibrate the TK201 resin separation column with 11 column volumes of 7Mol / L HCl solution;

[0146] Step 3.3: Add the result from step 2 67 Cu desorption solution was introduced into TK201 resin separation column, Cu 2+ With residual Zn 2+ 、Co 2+ , Ga 2+ 、Ni 2+ It was adsorbed on the TK201 resin separation column;

[0147] Step 3.4, eluting the TK201 resin separation column with 1.5 column volumes of 8 Mol / L HCl solution, and discharging all 7 Mol / L HCl solution;

[0148] Step 3.5, wash the TK201 resin column with 3 column volumes of 0.8Mol / L HCl solution to remove Co 2+ 、Ni 2 + Impurities;

[0149] Step 3.6, desorb with 3 column volumes of 0.05Mol / L HCl solution 67 Cu, get 67 Cu solution, while Zn 2+ , Ga 2+ Still adsorbed on the TK201 resin separation column and removed.

[0150] Embodiment 6

[0151] The difference between this embodiment and the second embodiment is that:

[0152] In step 2.5, the CU resin separation column was eluted with 3 column volumes of 0.15Mol / L HCl solution; in step 2.6, 2 column volumes of 5Mol / L HCl solution were used for desorption. 67 Cu;

[0153] In step 3.2 and step 3.4, the concentration of the HCl solution used was 5 Mol / L.

[0154] Other contents remain unchanged.

Claims

1. A high purity and low acidity 67 The method for preparing a Cu solution is characterized in that: The following steps are involved: Step 1. Target dissolution dissolving the irradiated Zn target to obtain a target dissolving solution; Step 2. 67 Cu Separation The target material solution was separated using the pre-prepared CU resin separation column to obtain 67 Cu desorption solution; 67 The Cu desorption solution is obtained by eluting the CU resin separation column with HCl solution in the concentration range of 5 to 8 Mol / L; Step 3. Medium transformation to obtain high purity and low acidity 67 Cu solution 3.

1. The result from step 2 67 The Cu desorption solution was introduced into the pre-prepared TK201 resin separation column, so that 67 Cu and residual Zn 2 + 、Co 2+ , Ga 2+ 、Ni 2+ Impurities are adsorbed on the separation column; The TK201 resin separation column was washed with 1 to 2 column volumes of HCl solution and all of it was discharged; the concentration of the HCl solution was the same as that obtained in step 2. 67 The concentration of HCl solution used in the Cu desorption solution was the same; 3.

2. Elute the TK201 resin column with HCl solution in the concentration range of 0.5 to 1Mol / L to remove the residual Co 2+ 、Ni 2+ Impurities; 3.

3. Desorb with 3 to 5 column volumes of HCl solution in the concentration range of 0.01 to 0.02 mol / L 67 Cu gets high purity and low acidity 67 Cu solution, complete the preparation.

2. A high purity low acidity according to claim 1 67 The method for preparing a Cu solution is characterized in that: Step 2 is as follows: 2.

1. The target material solution obtained in step 1 is introduced into the pre-prepared CU resin separation column to adsorb 67 Cu, followed by eluting the CU resin separation column with 1 to 2 column volumes of HCl solution in the concentration range of 0.005 to 0.02 Mol / L; 2.

2. Elute the CU resin column with HCl solution at a concentration of 0.005-0.15Mol / L to remove residual Zn 2+ 、Ni 2+ 、Co 2+ And Ga 2+ Impurities; 2.

3. Elute the CU resin separation column with 2 to 5 column volumes of HCl solution in the concentration range of 5 to 8 mol / L to desorb 67 Cu, get 67 Cu desorption solution.

3. A high purity low acidity according to claim 2 67 The method for preparing a Cu solution is characterized in that: Step 2.2 is as follows: 2.2.

1. Elute the CU resin column with 5 to 10 column volumes of HCl solution in the concentration range of 0.005 to 0.02 mol / L to remove residual Zn 2+ 、Ni 2+ 、Co 2+ Impurities; 2.2.

2. Elute the CU resin column with 2 to 4 column volumes of HCl solution in the concentration range of 0.1 to 0.15 mol / L to remove residual Ni 2+ , Ga 2+ Impurities.

4. A high purity low acidity according to claim 3 67 The method for preparing a Cu solution is characterized in that: Step 1 is as follows: The irradiated Zn target is transferred to a dissolver, and a mixture of HCl solution and HNO3 solution is added dropwise until the Zn target is completely dissolved, and then evaporated to dryness at 100-140° C., and then HCl solution with a concentration of 0.005-0.02 mol / L is added to dissolve the target solution; In the mixture of the HCl solution and the HNO3 solution, the volume ratio of the HCl solution to the HNO3 solution is (49-51):1, the mass concentration of the HCl solution used is greater than 9%, and the mass concentration of the HNO3 solution is greater than 17%.

5. A high purity low acidity according to claim 4 67 The method for preparing a Cu solution is characterized in that: In step 1, in the mixture of the HCl solution and the HNO3 solution, the mass concentration of the HCl solution used is greater than or equal to 18%, and the mass concentration of the HNO3 solution is greater than or equal to 34%; The amount of 0.005-0.02Mol / L HCl solution added is 2-5mL per gram of Zn; In step 2.1, the concentration of the HCl solution used is the same as that thereof.

6. A high purity low acidity according to claim 5 67 The method for preparing a Cu solution is characterized in that: In step 1, in the mixture of the HCl solution and the HNO3 solution, the volume ratio of the HCl solution to the HNO3 solution is 50:1, the mass concentration of the HCl solution used is 36%, and the mass concentration of the HNO3 solution is 68%; after evaporation, a 0.01Mol / L HCl solution is added to dissolve the target material solution, and the amount of the HCl solution added is 3mL per gram of Zn; In step 2.1, the amount of HCl solution added is 1 column volume; In step 2.2.1, the concentration of HCl solution is 0.01Mol / L; In step 2.2.2, the concentration of HCl solution is 0.1Mol / L; In step 2.3, the amount of HCl solution used is 3 column volumes, and the concentration is 6 Mol / L; In step 3.2, the amount of HCl solution used is 3 to 5 column volumes; In step 3.3, the amount of HCl solution used is 4 column volumes, and the concentration is 0.01 Mol / L.

7. A high-purity, low-acidity product according to any one of claims 2 to 6. 67 The method for preparing a Cu solution is characterized in that: In step 2.1, the CU resin separation column is prepared by the following steps: Take an empty separation column, install the lower filter plate, use a dropper to transfer the CU resin soaked in ultrapure water overnight, and add it to the separation column. When the height of the CU resin reaches the predetermined height, install the upper filter plate to obtain a CU resin separation column, and balance the CU resin separation column with 10 to 12 column volumes of HCl solution. The concentration of the HCl solution is the same as that used for elution in step 2.

1.

8. A high purity low acidity according to claim 7 67 The method for preparing a Cu solution is characterized in that: In step 3.1, the TK201 resin separation column is prepared by the following steps: Take an empty separation column, install the lower filter plate, use a dropper to transfer the TK201 resin soaked in ultrapure water overnight, and add it to the separation column. When the height of the TK201 resin reaches the predetermined height, install the upper filter plate to obtain a TK201 resin separation column, and balance the TK201 resin separation column with 10 to 12 column volumes of HCl solution. The concentration of the HCl solution is the same as that of the hydrochloric acid solution used for elution in step 3.

1.

9. A high purity low acidity product according to claim 8 67 The method for preparing a Cu solution is characterized in that: In step 3.2, the amount of HCl solution used is 3 column volumes, and the concentration is 0.5 Mol / L.

10. A high purity and low acidity 67 Cu solution, characterized in that: Using a high-purity, low-acidity 67 Preparation method of Cu solution.

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