WO2019203342A1 - Dispositif et procédé de séparation, et système et procédé de séparation et de purification de ri - Google Patents

Dispositif et procédé de séparation, et système et procédé de séparation et de purification de ri Download PDF

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WO2019203342A1
WO2019203342A1 PCT/JP2019/016800 JP2019016800W WO2019203342A1 WO 2019203342 A1 WO2019203342 A1 WO 2019203342A1 JP 2019016800 W JP2019016800 W JP 2019016800W WO 2019203342 A1 WO2019203342 A1 WO 2019203342A1
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solution
separation
metal
purification
electrode
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PCT/JP2019/016800
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English (en)
Japanese (ja)
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勝伸 森
慎一 大平
敬 戸田
由美 須郷
渡辺 茂樹
典子 石岡
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国立大学法人高知大学
国立大学法人 熊本大学
国立研究開発法人量子科学技術研究開発機構
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Priority to JP2020514458A priority Critical patent/JP7288261B2/ja
Publication of WO2019203342A1 publication Critical patent/WO2019203342A1/fr

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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D59/00Separation of different isotopes of the same chemical element
    • B01D59/38Separation by electrochemical methods
    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B15/00Obtaining copper
    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21GCONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G4/00Radioactive sources
    • G21G4/04Radioactive sources other than neutron sources
    • G21G4/06Radioactive sources other than neutron sources characterised by constructional features
    • G21G4/08Radioactive sources other than neutron sources characterised by constructional features specially adapted for medical application

Definitions

  • the present invention relates to a technique for separating and purifying radioisotopes (RI) from metals.
  • positron tomography which is used to diagnose brain function and cancer
  • a compound that is labeled with a radioisotope (RI) that emits positrons to a compound (labeled precursor) that induces the lesion is used.
  • RI radioisotope
  • a radioactive metal having an appropriate half-life such as 64 Cu (half-life of 12.7 hours) (longer than a widely used 18 F (half-life of 110 minutes) or the like) has attracted attention.
  • 64 Cu half-life of 12.7 hours
  • 18 F half-life of 110 minutes
  • Patent Document 1 discloses a general method for producing 64 Cu.
  • FIG. 11 is a flowchart showing a procedure of a general method for producing 64 Cu.
  • 64 Cu is obtained by irradiating a 64 Ni raw material with a proton beam (for example, about 2 hours).
  • the replacement step (S102) After the mixture of 64 Ni and 64 Cu is dissolved by heating, in the replacement step (S102), it takes about 1 hour to repeat evaporation and drying and re-dissolution of the dissolved product.
  • the separation step (S103) it takes about 30 minutes to 1 hour in order to separate 64 Ni and 64 Cu using chromatography in a hydrochloric acid system.
  • the purification step (S104) evaporation to dryness (about 1 hour) for removal of hydrochloric acid and dissolution with ultrapure water are performed, and the separation and purification of 64 Cu is completed. Thereafter, the separated and purified 64 Cu is made into a drug by reacting with a labeling precursor (about 1 to 2 hours) and used for PET diagnosis.
  • the irradiation step when the irradiation step is included, it may take 7 hours or more until a 64 Cu drug is obtained, which is a heavy burden for the medical site.
  • This invention is made in view of the said problem, and makes it a subject to provide the technique which isolate
  • RI can be separated in a very short time by an electrochemical method in which a voltage is applied to a solution containing a metal and its RI.
  • Item 1 A separation device for separating RI from a first solution containing a metal and a radioisotope (RI) converted from the metal, An electrode for applying a predetermined voltage to the first solution; The separation apparatus, wherein the predetermined voltage is a voltage in which an electrodeposition rate of the metal to the electrode and an electrodeposition rate of the RI to the electrode are different.
  • Item 2. Item 2. The separation device according to Item 1, wherein the metal is Ni and the RI is Cu.
  • Item 3. Item 2. The separation apparatus according to Item 1, wherein the metal is Zn and the RI is Cu.
  • the separation apparatus according to any one of Items 1 to 3, further comprising recovery means for dissolving the RI electrodeposited on the electrode in the second solution and recovering the RI from the separation apparatus.
  • Item 5. Item 4. The separation device according to Item 4, A purification device for purifying the RI from the second solution; RI separation and purification system.
  • Item 6. A separation method for separating RI from a first solution containing a metal and a radioisotope (RI) converted from the metal, An application step of applying a predetermined voltage to the first solution via an electrode; The separation method, wherein the predetermined voltage is a voltage in which an electrodeposition rate of the metal to the electrode and an electrodeposition rate of the RI to the electrode are different.
  • Item 7. Item 7.
  • Item 7. The separation method according to Item 6, wherein the metal is Zn and the RI is Cu.
  • Item 9. The separation method according to any one of Items 6 to 8, further comprising a recovery step in which the RI electrodeposited on the electrode is dissolved in a second solution and recovered from the separation device.
  • Item 10. Each step of the separation method according to Item 9, A purification step of purifying the RI from the second solution; RI separation and purification method.
  • metal RI can be separated in a short time.
  • Is a graph showing the Zn (II) and electrodeposition rate of Cu (II) dissolved in 100mM solution of HNO 3, the relationship between the applied voltage to the electrode.
  • HNO 3 solution and 10 mM HNO 3 in 100mM is a graph showing the relationship between the recovery rate and the applied voltage at the time of electrodeposition of Cu (II).
  • A) to (c) show the relationship between the extraction rate of Cu (II) in the eluates AA, SC and CA and the applied voltage between the electrodes when a 10 mM HNO 3 solution is used as the acceptor solution. It is a graph to show.
  • (A) to (c) are the extraction ratio of Cu (II) in the eluate AA, SC, CA and the applied voltage between the electrodes when a 10 mM CH 3 CO 2 H solution was used as the acceptor solution. It is a graph which shows the relationship. It is a flowchart which shows the procedure of the manufacturing method of a general 64 Cu. It is a graph which shows the density
  • FIG. 1 is a block diagram showing a schematic configuration of an RI manufacturing system 100 according to this embodiment
  • FIG. 2 is a flowchart showing a procedure of an RI manufacturing method according to this embodiment.
  • the RI manufacturing system 100 includes an irradiation apparatus 10 and an RI separation and purification system 20.
  • the RI separation and purification system 20 includes a separation device 3 and a purification device 4.
  • the irradiation step S ⁇ b> 1 is performed using the irradiation apparatus 10.
  • the irradiation device 10 includes a cyclotron 1 and an irradiation metal 2.
  • the metal 2 for irradiation consists of 64 Ni of a stable stable isotope.
  • the irradiation metal 2 is irradiated from the cyclotron 1 with a proton beam. Thereby, a part of 64 Ni is converted into 64 Cu which is RI by the 64 Ni (p, n) 64 Cu reaction. Thereafter, 64 Ni and 64 Cu mixed in the irradiation metal 2 are dissolved in the first solution.
  • the first solution for example, an aqueous solution containing a strong acid such as HNO 3 or HCl can be used. The first solution is transferred to the RI separation and purification system 20.
  • the separation step S2, the recovery step S3, and the purification step S4 in the RI separation and purification method according to the present embodiment are performed using the RI separation and purification system 20.
  • the separation device 3 includes an electrode for applying a predetermined voltage to the first solution.
  • the predetermined voltage is a voltage in which the electrodeposition rate of 64 Ni to the electrode is different from the electrodeposition rate of 64 Cu to the electrode.
  • FIG. 3 is a schematic cross-sectional view showing an example of the separation device 3.
  • the separation device 3 is composed of a flow column type electrolytic synthesis cell.
  • the separation device 3 includes a working electrode 31 made of carbon fiber and a counter electrode 32 made of platinum wire as electrodes. A voltage is applied to the working electrode 31 via an electrode rod 33 connected to the terminal 34. A voltage is applied to the counter electrode 32 from a terminal 35.
  • the working electrode 31 is filled inside the porous glass tube 36, and the counter electrode 32 is wound around the porous glass tube 36.
  • a reference voltage for keeping the voltage applied to the working electrode 31 and the counter electrode 32 at a constant potential is applied to the terminal 37.
  • the first solution is introduced into the porous glass tube 36 through the introduction pipe 38 and passes through the working electrode 31.
  • the first solution is introduced into the porous glass tube 36 through the introduction pipe 38 and passes through the working electrode 31.
  • the working electrode 31 and the counter electrode 32 by applying a predetermined voltage between the working electrode 31 and the counter electrode 32 via the terminal 34 and the terminal 35, only 64 Cu is electrodeposited on the working electrode 31 by an electrolytic reaction.
  • 64 Cu which is RI is separated from the first solution.
  • FIG. 4 is a graph showing the relationship between the electrodeposition rate of Ni (II) and Cu (II) and the voltage applied to the electrode when the first solution is 10 mM HNO 3
  • FIG. is a graph showing the case where the first solution is HNO 3 in 100 mM, and electrodeposition rate of Ni (II) and Cu (II), the relationship between the applied voltage to the electrode.
  • Cu and Ni have different standard oxidation-reduction potentials (Cu + 0.340V, Ni-0.257V)
  • the electrodeposition characteristics with respect to the applied voltage are different from each other.
  • the electrodeposition characteristics with respect to the applied voltage of metal ions are the same among isotopes of the same element. Therefore, the voltage applied to the electrodes, by which the electrodeposition rate of Ni (II) electrodeposition rate and Cu (II) is a different voltage, 64 Cu from the first solution 64 Cu and 64 Ni were dissolved Can be separated.
  • the electrodeposition characteristics with respect to the applied voltage include strong acids such as HNO 3 and HCl as the first solution type when separating Ni (II) from Cu (II) from the viewpoint of separating RI with higher accuracy. It is preferable to use an aqueous solution.
  • the concentration of the first solution is preferably adjusted to 10 to 100 mM.
  • the applied voltage is preferably ⁇ 0.5 to ⁇ 0.1 V, particularly preferably ⁇ 0.4 to ⁇ 0.3 V.
  • the metal electrodeposition rate (%) is (Initial concentration of metal in the first solution introduced from the introduction pipe 38-concentration of metal in the first solution discharged from the discharge pipe 39) / (first concentration introduced from the introduction pipe 38) Initial concentration of metal in solution) x 100 It can be expressed as
  • the recovery step S3 64 Cu electrodeposited on the working electrode 31 is dissolved in the second solution and recovered from the separation device 3.
  • the first solution is taken out from the discharge pipe 39 by a collecting means (not shown), and then the second solution is introduced from the introduction pipe 38.
  • the second solution an aqueous solution containing a strong acid such as HNO 3 or HCl can be used. It is preferable to apply a positive voltage to the working electrode 31 when 64 Cu is dissolved in the second solution. By removing the second solution in which 64 Cu is dissolved from the discharge pipe 39, 64 Cu can be recovered from the separation device 3.
  • 64 Ni is very expensive (about 5,000 yen / mg)
  • 64 Ni dissolved in the first solution taken out from the discharge pipe 39 is reused for the production of 64 Cu. It is preferable to do.
  • the purification device 4 can be constituted by, for example, an electrodialysis purification device (ED).
  • FIG. 6 is a schematic diagram showing an example of the purification apparatus 4 configured by ED.
  • the purification apparatus 4 has a five-layer structure including an anode channel 41, an AA (anion acceptor) channel 42, an SC (introduction channel) 43, a CA (cation acceptor) channel 44, and a cathode channel 45.
  • the cathode channel 45 is provided with an anode 46 and a cathode 47, respectively.
  • the anode channel 41 and the AA channel 42 are separated by a cation exchange membrane F1
  • the CA channel 44 and the cathode channel 45 are separated by an anion exchange membrane F2.
  • the AA channel 42 and the introduction channel 43, and the introduction channel 43 and the CA channel 44 are separated by the regenerated cellulose membrane F3.
  • An isolator is passed through the anode channel 41 and the cathode channel 45.
  • deionized water can be used.
  • An anion acceptor and a cation acceptor are passed through the AA channel 42 and the CA channel 44, respectively.
  • a strong acid such as HNO 3 or a weak acid such as acetic acid (CH 3 CO 2 H) can be used.
  • the second solution is passed through the introduction channel 43.
  • the second solution is an HNO 3 solution in which 64 Cu is dissolved
  • the Cu (II) in the second solution is changed from NO 3 ⁇ .
  • a solvent for example, acetate buffer solution
  • 64 Cu can be purified from the second solution in the purification step S4.
  • the purification device 4 may have a four-layer structure that does not include the AA channel 42. In the case of a four-layer structure, NO 3 ⁇ passes through the introduction channel 43.
  • the 64 Cu is then transferred to the drug synthesizer and reacts with the labeling precursor. Thereby, a high purity Cu label
  • medical agent is obtained.
  • the purity test for the Cu-labeled drug can be performed by high performance liquid chromatography (HPLC) using a reverse phase or size exclusion column.
  • the irradiation step S1 is about 2 hours, which is the same as the irradiation step S101 (FIG. 11) in the prior art, but the separation step S2 and the recovery step S3 are about 5 minutes.
  • the purification step S4 is also about 5 minutes. That is, the time required for the separation steps S2 to S4 is about 10 minutes, and the time can be significantly shortened compared to the time required for the replacement step S102 to the purification step S104 (about 3 hours 30 minutes) in the prior art. . Therefore, in this embodiment, RI can be separated and purified in a short time, and severe time restrictions for handling radiopharmaceuticals can be eliminated.
  • the production amount of RI used for drug synthesis is small, the amount of liquid passing through each channel of the purification apparatus 4 used in the purification step S4 can be small. For this reason, the refining device 4 can be easily downsized, and the refining device 4 according to the present embodiment has a size of about 11 cm long ⁇ 3 cm wide ⁇ 2.5 cm high. Therefore, the scale of the RI separation and purification system 20 can be reduced, and it is possible to contribute to the elimination of spatial restrictions at the medical site.
  • the apparatus used in the substitution process S102 to the purification process S104 of the prior art has a large scale for handling 64 Cu, and loss and reaction due to purification. There was a drop in efficiency.
  • RI can be separated and purified with high efficiency by reducing the system scale according to the amount of 64 Cu produced.
  • the irradiation device 10 and the separation device 3 and the separation device 3 and the purification device 4 are seamlessly connected. Thereby, the irradiation step S1 to the purification step S4 shown in FIG. 2 can be carried out continuously, and RI can be further separated and purified.
  • the metal and RI were 64 Ni and 64 Cu, respectively, but the present invention is not limited to this. Any electrodeposition characteristic (standard oxidation-reduction potential) to the electrode with respect to the voltage applied to the solution can be applied to the present invention as long as the metal is different from RI.
  • the metal is Ni or Zn and the RI is Cu.
  • 63 Cu and 66 Ga standard redox potential -0.529 V
  • 67 Zn standard redox potential -0.763 V
  • 67 Cu and 68 Zn (standard Redox potential -0.763 V) and 67 Cu.
  • 66 Ga is useful for PET diagnosis because it has a half-life of 9.4 hours and emits positrons. Since 67 Cu has a half-life of 61.8 hours and emits ⁇ rays, it is useful for internal therapy of cancer.
  • FIG. 7 is a graph showing the relationship between the electrodeposition rates of Zn (II) and Cu (II) dissolved in a 100 mM HNO 3 solution and the voltage applied to the electrodes. Since Cu and Zn have different standard redox potentials, the electrodeposition characteristics with respect to the applied voltage are different from each other. Therefore, the voltage applied to the electrode is such that the electrodeposition rate of Zn (II) and the electrodeposition rate of Cu (II) are different, so that 67 Cu and 67 Zn or 67 Cu and 68 Zn are dissolved. 67 Cu can be separated from one solution.
  • Example 1 In Example 1, an experiment for separating Cu (II) from a first solution containing Ni (II) and Cu (II) was performed using the separation device 3 according to the above embodiment.
  • the first solution a solution prepared by dissolving 6.0 ⁇ M Ni (II) and 6.0 ⁇ M Cu (II) in a 100 mM HNO 3 solution and a solution dissolved in a 10 mM HNO 3 solution are used. Two were prepared. The first solution was introduced into the porous glass tube 36 through the introduction pipe 38 of the separation device 3. The flow rate of the first solution was 1.0 mL / min. In a state where the first solution was passed through the porous glass tube 36, a voltage was applied between the electrodes 31 and 32, and the first solution was taken out from the discharge pipe 39.
  • FIG. 8 is a graph showing the relationship between the recovery rate of Cu (II) and the applied voltage during electrodeposition when a 100 mM HNO 3 solution and 10 mM HNO 3 are used as the first solution.
  • the recovery rate was very high by setting the applied voltage to ⁇ 0.5 to ⁇ 0.2V.
  • the recovery rate became very high when the applied voltage was -0.5 to -0.3 V.
  • Example 1 general reagents, ie, Ni and Cu of natural composition (hereinafter referred to as natNi and natCu) were used, but the electrodeposition characteristics of dissolved metal ions with respect to the applied voltage are the same between isotopes of the same element. . That is, the electrodeposition characteristics of nat Ni (II) and 64 Ni (II) (mainly nat Ni 2+ and 64 Ni 2+ ) are the same, and nat Cu (II) and 64 Cu (II) (mainly nat Cu 2+ And 64 Cu 2+ ) have the same electrodeposition characteristics. Therefore, it was found that 64 Cu can be separated with high efficiency from the first solution containing 64 Ni and 64 Cu by using the separation device 3.
  • natNi and natCu the electrodeposition characteristics of dissolved metal ions with respect to the applied voltage are the same between isotopes of the same element. . That is, the electrodeposition characteristics of nat Ni (II) and 64 Ni (II) (mainly
  • the recovery rate (%) is (Cu (II) concentration in the second solution discharged from the discharge pipe 39 in the recovery step) / (Cu (II) initial concentration in the first solution introduced from the introduction pipe 38 in the separation step)) ⁇ 100 It is calculated by. Therefore, when Cu (II) is recovered in a concentrated state, the recovery rate exceeds 100%.
  • Example 2 In Example 2, an experiment for purifying Cu from the second solution was performed using the purification apparatus 4 according to the above embodiment.
  • an electrodialysis purification device having a five-layer structure shown in FIG. 6 was used as the purification device 4.
  • Deionized water is passed through the anode channel 41 and the cathode channel 45 as an isolator, and a 10 mM HNO 3 solution or CH 3 CO 2 H solution is passed through the AA channel 42 and the CA channel 44 as an acceptor solution,
  • the second solution was passed through the introduction channel 43.
  • an HNO 3 solution in which 5.0 ⁇ M Cu (II) (mainly in the form of Cu 2+ ) was dissolved was used as the second solution.
  • the extraction rate (%) is (Metal concentration in solution introduced into channel 43 ⁇ metal concentration in solution eluted from each channel 42, 43, 44) / (metal concentration in solution introduced into channel 43) ⁇ 100 It can be expressed as
  • FIGS. 9A to 9C show the extraction rate of Cu (II) in the eluents AA, SC, and CA and the application between the electrodes 46 and 47, respectively, when a 10 mM HNO 3 solution is used as the acceptor solution. It is a graph which shows the relationship with a voltage. In this case, it was found that Cu (II) can be extracted from the eluent CA from the channel 44 with higher efficiency as the applied voltage is increased.
  • 10 (a) to 10 (c) show the extraction ratio of Cu (II) in the eluate AA, SC, CA and the distance between the electrodes 46, 47 when a 10 mM CH 3 CO 2 H solution is used as the acceptor solution. It is a graph which shows the relationship with the applied voltage to. In this case, an extraction rate close to 100% could be achieved by setting the applied voltage to 5 to 10V.
  • Example 2 the concentration of Cu (II) was adjusted in accordance with the lower limit of quantification of the detector (atomic absorption). However, if this concentration is further reduced, it dissolves even in basic, so in a wider range. It is considered that Cu (II) can be purified with an applied voltage.
  • Example 3 In Example 3, an experiment for separating 64 Cu (II) from a first solution containing 57 Ni (II) and 64 Cu (II) was performed using the separation apparatus 3 according to the above embodiment.
  • Example 1 a column type electrolytic synthesis cell (electrolytic synthesis / analysis column type flow cell HX-201) manufactured by Hokuto Denko Co., Ltd. was used as in Example 1.
  • the first solution a solution prepared by dissolving 57 Ni (II) and 64 Cu (II) obtained by proton beam irradiation on nickel oxide in 5 mL of 100 mM HCl solution was prepared.
  • the first solution was introduced into the porous glass tube 36 through the introduction pipe 38 of the separation device 3.
  • a voltage of ⁇ 0.6 V was applied between the electrodes 31 and 32, and the solution was taken out from the discharge pipe 39 in two portions of 2 mL.
  • the second solution was passed through the porous glass tube 36, and the solution was taken out from the discharge pipe 39 in 2 mL portions in two portions. Further, in order to elute 64 Cu electrodeposited on the working electrode 31, the voltage applied between the electrodes 31 and 32 is switched from -0.6V to + 0.6V, and the second solution is put into the porous glass tube 36. While passing through the solution, the solution was taken out from the discharge pipe 39 in two portions of 2 mL. As the second solution, a 100 mM HNO 3 solution was used.
  • FIG. 12 is a graph showing the concentrations of 57 Ni (II) and 64 Cu (II) in the solution taken out from the discharge pipe 39.
  • the horizontal axis indicates the order in which the solutions are removed.
  • 64 Cu (II) of the first solution is electrodeposited on the working electrode 31, so only about 57 Ni (II) is detected in the solution taken out the first to fourth times. It was.
  • the concentration of 57 Ni (II) is low because the ratio of the solution present in the analyzer 3 before introducing the first solution is high. Since the total amount of the first solution introduced into the first solution is 5 mL, the concentration of 57 Ni (II) reaches a maximum with the solution taken out for the second time and then gradually decreases. Was hardly detected in the removed solution.
  • Example 4 In Example 4, an experiment for purifying 64 Cu (II) from the second solution was performed using the purification apparatus 4 according to the above embodiment.
  • the electrodialysis purification apparatus 4 As the purification apparatus 4, the electrodialysis purification apparatus having a five-layer structure shown in FIG. As a pre-process, after deionized water is passed through all the channels 41 to 45, a voltage of 15 V is applied between the electrodes 46 and 47, and then pure water is passed through the anode channel 41 and the cathode channel 45 as an isolator. A 10 mM CH 3 CO 2 H solution was passed as an acceptor solution through the AA channel 42 and the CA channel 44, and a second solution was passed through the introduction channel 43. As the second solution, a 10 mM HCl solution in which 64 Cu (II) was dissolved was used.
  • FIGS. 13A to 13C are graphs showing the extraction rate of 64 Cu (II) in the eluents AA, SC, and CA, respectively.
  • the horizontal axis indicates the order in which the solutions are removed.
  • the eluate CA taken out for the first to third times has an extraction rate of 10 to 20%, which is considered to be due to adsorption of 64 Cu (II) to the CA channel 44.
  • the extraction rate exceeds 100%. This is because H + moves to the CA channel 44 by passing HCl through the introduction channel 43, This is probably because the pH in the CA channel 44 dropped and 64 Cu (II) adsorbed on the CA channel 44 was dissolved.
  • FIG. 14 is a table showing the contents of metal elements other than Ni and Cu after passing through the purification apparatus 4.
  • the unit is mg / L, and “ ⁇ ” indicates that the content is below the detection limit. Further, “ ⁇ 0.001” or “ ⁇ 0.002” indicates that the value is below the lower limit of quantification.
  • Each numerical value shown in FIG. 14 is a level at which there is no problem in clinical practice.
  • the metals shown in FIG. 14 are contained in nickel oxide and air, and are inevitably mixed into the first and second solutions in the manufacturing process of radioactive metals, but these metals are removed by the purifier 4. I found out.

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Abstract

La présente invention vise à séparer un RI métallique en peu de temps. Un dispositif de séparation (3) permettant de séparer un radio-isotope (RI) d'une première solution contenant un métal et le RI, obtenu par transformation du métal, comporte une électrode (31) servant à appliquer une tension prescrite à la première solution, la tension prescrite étant une tension avec laquelle une vitesse d'électrodéposition du métal sur l'électrode (31) est différente de la vitesse d'électrodéposition du RI sur l'électrode (31).
PCT/JP2019/016800 2018-04-19 2019-04-19 Dispositif et procédé de séparation, et système et procédé de séparation et de purification de ri WO2019203342A1 (fr)

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JP5880931B2 (ja) * 2011-11-30 2016-03-09 住友重機械工業株式会社 64Cuの分離精製方法及び64Cuの分離精製装置

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Publication number Priority date Publication date Assignee Title
US11521762B2 (en) 2020-09-03 2022-12-06 Curium Us Llc Purification process for the preparation of non-carrier added copper-64
US11581103B2 (en) 2020-09-03 2023-02-14 Curium Us Llc Purification process for the preparation of non-carrier added copper-64
US11798701B2 (en) 2020-09-03 2023-10-24 Curium Us Llc Purification process for the preparation of non-carrier added copper-64
US11972874B2 (en) 2020-09-03 2024-04-30 Curium Us Llc Purification process for the preparation of non-carrier added copper-64
US11978569B2 (en) 2020-09-03 2024-05-07 Curium Us Llc Purification process for the preparation of non-carrier added copper-64

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