EP1883079B1 - Procedé destiné à la preparation de radio-isotopes - Google Patents
Procedé destiné à la preparation de radio-isotopes Download PDFInfo
- Publication number
- EP1883079B1 EP1883079B1 EP06425518A EP06425518A EP1883079B1 EP 1883079 B1 EP1883079 B1 EP 1883079B1 EP 06425518 A EP06425518 A EP 06425518A EP 06425518 A EP06425518 A EP 06425518A EP 1883079 B1 EP1883079 B1 EP 1883079B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- target
- solution
- isotope
- irradiated
- procedure according
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 238000000034 method Methods 0.000 title claims abstract description 19
- 238000002360 preparation method Methods 0.000 title claims abstract description 11
- 238000004070 electrodeposition Methods 0.000 claims abstract description 16
- 238000004090 dissolution Methods 0.000 claims abstract description 9
- 230000003139 buffering effect Effects 0.000 claims abstract description 7
- 230000001678 irradiating effect Effects 0.000 claims abstract description 5
- 230000002285 radioactive effect Effects 0.000 claims abstract description 4
- 239000012535 impurity Substances 0.000 claims abstract description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 7
- 229910017604 nitric acid Inorganic materials 0.000 claims description 7
- 238000000746 purification Methods 0.000 claims description 5
- 238000005342 ion exchange Methods 0.000 claims description 4
- 238000010828 elution Methods 0.000 claims description 2
- 239000000243 solution Substances 0.000 description 31
- 239000008367 deionised water Substances 0.000 description 7
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 6
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 4
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 4
- 239000000908 ammonium hydroxide Substances 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- 239000002253 acid Substances 0.000 description 3
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 description 2
- 235000019270 ammonium chloride Nutrition 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 229910052734 helium Inorganic materials 0.000 description 2
- 239000001307 helium Substances 0.000 description 2
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 2
- 238000003756 stirring Methods 0.000 description 2
- 239000005695 Ammonium acetate Substances 0.000 description 1
- USFZMSVCRYTOJT-UHFFFAOYSA-N Ammonium acetate Chemical compound N.CC(O)=O USFZMSVCRYTOJT-UHFFFAOYSA-N 0.000 description 1
- 206010028980 Neoplasm Diseases 0.000 description 1
- 229940043376 ammonium acetate Drugs 0.000 description 1
- 235000019257 ammonium acetate Nutrition 0.000 description 1
- 239000003637 basic solution Substances 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 230000004060 metabolic process Effects 0.000 description 1
- 238000010979 pH adjustment Methods 0.000 description 1
- 238000002600 positron emission tomography Methods 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 239000012217 radiopharmaceutical Substances 0.000 description 1
- 229940121896 radiopharmaceutical Drugs 0.000 description 1
- 230000002799 radiopharmaceutical effect Effects 0.000 description 1
- 230000001225 therapeutic effect Effects 0.000 description 1
- 238000002560 therapeutic procedure Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 238000000844 transformation Methods 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
- G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
- G21G1/04—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes outside nuclear reactors or particle accelerators
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
- G21G4/00—Radioactive sources
- G21G4/04—Radioactive sources other than neutron sources
- G21G4/06—Radioactive sources other than neutron sources characterised by constructional features
- G21G4/08—Radioactive sources other than neutron sources characterised by constructional features specially adapted for medical application
Definitions
- the present invention relates to a procedure for the preparation of radioisotopes.
- Radioisotopes by means of medium or low energy irradiation (5-30 MeV) for medical uses has been know for years. Radioisotopes find several and important industrial and scientific applications. The most important application is their use as tracers: radiopharmaceuticals, whose administration in humans may allow to diagnose and monitor a therapy by means of Positron Emission Tomography (PET), particularly for tumours, are synthesised by means of reactions with appropriate non-radioactive precursors.
- PET Positron Emission Tomography
- By measuring the irradiation it is also possible to follow all the transformations of the element and/or the molecule it is bound to, which is useful in chemistry (study of reaction mechanisms), in biology (study of metabolism genetics) and, as mentioned above, in medicine for diagnostic and therapeutic uses.
- the known systems provide that the target once arranged on the target-holder is placed in the irradiation station and that once the irradiation operation is ended, the target-holder is dissolved with the irradiated target and, subsequently, removed from the radioisotope produced by means of a purification process.
- the object of the present invention is a procedure for the preparation of radioisotopes comprising a first step of electrodepositing a metallic isotope target to be irradiated on a target-holder element, a second step of irradiating said target, a third step of dissolving said target and a fourth step of purifying the radioisotope from the initial metallic isotope and from other possible radioactive and metallic impurities; said procedure being characterised in that said electrodeposition step comprises a dissolution operation in which the isotope to be irradiated is dissolved in a solution of HNO 3 with concentration from 0.5 to 2.5 M, a pH buffering operation, and a recirculation operation, in which the solution obtained above is circulated at a rate from 0.5 to 3 ml/min within an electrolytic cell during the current output within the cell itself; said isotope target to be irradiated being produced by electrodeposition in said electrolytic cell during said recirculation operation.
- the concentration of HNO 3 is from 2 to 2.5 M.
- the solution is circulated at a rate from 1 to 2 ml/min.
- said pH adjustment operation is an alkalisation operation adapted to take the pH to a value from 5 to 13.5.
- the output current during the recirculation operation has an intensity from 40 to 100 mA and a difference of potential from 2 to 3 V.
- the electrodissolution step comprising a further recirculation operation in which a solution of HCl with concentration from 4 to 6M is circulated at a rate from 3 to 5 ml/min within the electrolytic cell during the output of reverse current with respect to that output during the electrodeposition step.
- the metallic isotope to be irradiated is comprised in the group consisting of 60 Ni, 61 Ni, 64 Ni, 110 Cd.
- the purification step comprises an elution operation in an ion-exchange column by means of a concentration gradient solution of HCl.
- the basic solution thus obtained was circulated at a rate of 1.5-2 ml/min through an electrolytic cell in which a 2.3 V current was output at an intensity from 50 to 70 mA. Such conditions were maintained for 7h, with the result that a quantity of 50 mg of 60 Ni was electrodeposited.
- the 60 Cu was purified from the 60 Ni by means of a ion-exchange column.
- the acid solution from the electrodissolution step was transferred to a Bio-Rad AG1-X8 column under helium flow.
- the 60 Ni was eluted with 15 ml of HCl 6M solution and the 60 Cu was eluted with 10 ml of HCl 0.1M solution.
- 100 mg of 110 Cd were dissolved in 0.114 ml of a HNO 3 solution at 69% v:v and 0.114 ml of deionised water at a temperature of 100°C under vigorous stirring.
- 1.552 ml of deionised water were added to the solution thus obtained in order to obtain a final volume of 1.78 ml.
- 1.78 ml of an EDTA solution, 2 ml of a buffering solution of acetic acid/ammonium acetate at pH 4.76, a solution of NaOH at 50% v/v were added to such solution to reach pH 6.5 and deionised water to reach a volume of 10 ml.
- the solution thus obtained was circulated at a rate of 1.5-2 ml/min through an electrolytic cell in which a current of 2.5-2.9 V was output at an intensity from 30 to 70 mA. Such conditions were maintained for a period of 6h, with the result that a quantity of 72 mg of 110 Cd was electrodeposited.
- dissolution was obtained without application of reverse voltage in a time from 3 to 5 minutes.
- the 110 In was purified from the 110 Cd by means of a ion-exchange column.
- the acid solution from the electrodissolution step was transferred to a Bio-Rad AG1-X8 column under helium flow.
- the 110 Cd was eluted with 15 ml of a HCl 4 M solution and the 110 In was eluted with 10 ml of a HCl 0.05M solution.
- This new example shows an alternative method for the preparation of the 110 In.
- Such alternative method differs from what stated above only in that a pH 13.4 buffering solution is used for the electrodeposition step. From the above, it is apparent that only the electrodeposition step will be reported for this specific example.
- 100 mg of 110 Cd were dissolved in 0.114 ml of a HNO 3 solution at 69% v:v and 0.114 ml of deionised water at a temperature of 100°C under strong stirring. 1.552 ml of deionised water were added to the solution thus obtained in order to obtain a final volume of 1.78 ml.
- 1.78 ml of a solution of EDTA, 4 ml of a buffering solution of ammonium hydroxide/ammonium chloride, 0.8 ml of ammonium hydroxide, 5.5 ml of deionised water, 2.44 ml of a NaOH solution at 50% v/v were added to such solution to reach a pH of 13.4.
- the solution thus obtained was circulated at a rate of 1.5-2 ml/min through an electrolytic cell in which a current of 2.5-2.9 V was output at an intensity from 30 to 70 mA. Such conditions were maintained for 6h, with the result that a quantity of 72 mg of 110 Cd was electrodeposited.
- the procedure according to the present invention presents the advantage of not requiring the simultaneous dissolution of the target holder with obvious advantages in terms of time and convenience that this entails, and moreover, allows to perform the electrodeposition step of the target relatively rapidly and in essentially mild current conditions.
- the procedure is perfectly fit to be implemented by means of an automated machine thus drastically reducing the total preparation time of the radioisotopes.
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Electroplating And Plating Baths Therefor (AREA)
- Electrolytic Production Of Metals (AREA)
- Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
Claims (8)
- Procédé de préparation de radio-isotopes comprenant une première étape consistant à électrodéposer une cible d'isotope métallique à irradier sur un élément porte-cible, une deuxième étape consistant à irradier ladite cible, une troisième étape consistant à dissoudre ladite cible et une quatrième étape consistant à purifier le radio-isotope à partir de l'isotope métallique initial et d'autres impuretés radioactives et métalliques éventuelles ; ledit procédé étant caractérisé en ce que ladite étape d'électrodéposition comprend une opération de dissolution dans laquelle l'isotope à irradier est dissous dans une solution de HNO3 de concentration allant de 0,5 à 2,5 M, une opération de tamponnement du pH, et une opération de recirculation, dans laquelle la solution obtenue ci-dessus est mise à circuler à une vitesse de 0,5 à 3 mL/min dans une cellule électrolytique pendant la sortie du courant à l'intérieur de la cellule elle-même ; ladite cible d'isotope à irradier étant produite par électrodéposition dans ladite cellule électrolytique pendant ladite opération de recirculation.
- Procédé selon la revendication 1, caractérisé en ce que dans l'opération de dissolution, la concentration en HNO3 est de 2 à 2,5 M.
- Procédé selon la revendication 1 ou 2,
caractérisé en ce que pendant l'opération de recirculation, la solution est mise à circuler à une vitesse de 1 à 2 mL/min. - Procédé selon l'une quelconque des revendications précédentes, caractérisé en ce que ladite opération de tamponnement du pH est une opération d'alcalinisation adaptée pour amener le pH à une valeur de 5 à 13,5.
- Procédé selon l'une quelconque des revendications précédentes, caractérisé en ce que ladite sortie de courant pendant l'opération de recirculation a une intensité de 40 à 100 mA et une différence de potentiel de 2 à 3 V.
- Procédé selon l'une quelconque des revendications précédentes, caractérisé en ce que l'étape d'électrodissolution comprend une opération de recirculation supplémentaire dans laquelle une solution de HCl de concentration allant de 4 à 6 M est mise à circuler à une vitesse de 3 à 5 mL/min dans la cellule électrolytique pendant la sortie de courant inversée par rapport à la sortie pendant l'étape d'électrodéposition.
- Procédé selon l'une quelconque des revendications précédentes, caractérisé en ce que l'isotope métallique à irradier est compris dans le groupe constitué par 60Ni, 61Ni, 64Ni et 110Cd.
- Procédé selon l'une quelconque des revendications précédentes, caractérisé en ce que l'étape de purification comprend une opération d'élution dans une colonne échangeuse d'ions au moyen d'une solution de HCl à gradient de concentration.
Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP06425518A EP1883079B1 (fr) | 2006-07-24 | 2006-07-24 | Procedé destiné à la preparation de radio-isotopes |
AT06425518T ATE430983T1 (de) | 2006-07-24 | 2006-07-24 | Verfahren zur herstellung von radioisotopen |
DE602006006667T DE602006006667D1 (de) | 2006-07-24 | 2006-07-24 | Verfahren zur Herstellung von Radioisotopen |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP06425518A EP1883079B1 (fr) | 2006-07-24 | 2006-07-24 | Procedé destiné à la preparation de radio-isotopes |
Publications (2)
Publication Number | Publication Date |
---|---|
EP1883079A1 EP1883079A1 (fr) | 2008-01-30 |
EP1883079B1 true EP1883079B1 (fr) | 2009-05-06 |
Family
ID=37606889
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP06425518A Active EP1883079B1 (fr) | 2006-07-24 | 2006-07-24 | Procedé destiné à la preparation de radio-isotopes |
Country Status (3)
Country | Link |
---|---|
EP (1) | EP1883079B1 (fr) |
AT (1) | ATE430983T1 (fr) |
DE (1) | DE602006006667D1 (fr) |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN112614607A (zh) * | 2020-12-02 | 2021-04-06 | 中广核研究院有限公司 | 放射性核素锰-54的制备方法 |
CN113873739A (zh) * | 2021-08-20 | 2021-12-31 | 苏州爱索拓普智能科技有限公司 | 一种基于质子辐照Ni的***及高纯度Ni靶件的制备方法 |
Family Cites Families (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CA935943A (en) * | 1970-12-23 | 1973-10-23 | Union Carbide Corporation | Primary target for the production of fission products in a nuclear reactor and process for preparation |
US4487738A (en) * | 1983-03-21 | 1984-12-11 | The United States Of America As Represented By The United States Department Of Energy | Method of producing 67 Cu |
US5037602A (en) * | 1989-03-14 | 1991-08-06 | Science Applications International Corporation | Radioisotope production facility for use with positron emission tomography |
AU7265096A (en) * | 1995-08-09 | 1997-03-12 | Newton Scientific, Inc. | Production of 64cu and other radionuclides using charged-particle accelerator |
WO2000029501A1 (fr) * | 1998-11-18 | 2000-05-25 | Emory University | Solutions de revetement radioactives, procedes et substrats associes |
US6157036A (en) * | 1998-12-02 | 2000-12-05 | Cedars-Sinai Medical Center | System and method for automatically eluting and concentrating a radioisotope |
-
2006
- 2006-07-24 EP EP06425518A patent/EP1883079B1/fr active Active
- 2006-07-24 DE DE602006006667T patent/DE602006006667D1/de active Active
- 2006-07-24 AT AT06425518T patent/ATE430983T1/de not_active IP Right Cessation
Also Published As
Publication number | Publication date |
---|---|
DE602006006667D1 (de) | 2009-06-18 |
ATE430983T1 (de) | 2009-05-15 |
EP1883079A1 (fr) | 2008-01-30 |
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