EP1883079B1 - Verfahren zur Herstellung von Radioisotopen - Google Patents

Verfahren zur Herstellung von Radioisotopen Download PDF

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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
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Prior art keywords
target
solution
isotope
irradiated
procedure according
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EP06425518A
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English (en)
French (fr)
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EP1883079A1 (de
Inventor
Paolo Bedeschi
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Priority to EP06425518A priority Critical patent/EP1883079B1/de
Priority to AT06425518T priority patent/ATE430983T1/de
Priority to DE602006006667T priority patent/DE602006006667D1/de
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    • 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.

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  • 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)
  • Pharmaceuticals Containing Other Organic And Inorganic Compounds (AREA)
  • Electrolytic Production Of Metals (AREA)

Claims (8)

  1. Verfahren zur Herstellung von Radioisotopen, umfassend als ersten Schritt die Elektroabscheidung eines zu bestrahlenden metallischen Isotop-Targets auf einem Target-Halterungselement, als zweiten Schritt das Bestrahlen des Targets, als dritten Schritt das Auflösen des Targets und als vierten Schritt das Reinigen des Radioisotops von dem anfänglichen metallischen Isotop und von anderen möglichen radioaktiven und metallischen Verunreinigungen; wobei das Verfahren dadurch gekennzeichnet ist, dass der Elektroabscheidungsschritt eine Auflösungsoperation, in welcher das zu bestrahlende Isotop in einer HNO3-Lösung mit einer Konzentration von 0,5 bis 2,5 M gelöst wird, einer pH-Puffer-Operation und einer Rückführoperation, in welcher die oben erhaltene Lösung bei einer Rate von 0,5 bis 3 mL/min innerhalb einer Elektrolysezelle während der Ausgabe von Strom innerhalb der Zelle selbst zirkuliert wird, umfasst, wobei das zu bestrahlende Isotop-Target durch Elektroabscheidung in der Elektrolysezelle während der Rückführoperation gebildet wird.
  2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass während der Auflösungsoperation die Konzentration an HNO3 von 2 bis 2,5 M beträgt.
  3. Verfahren nach Anspruch 1 oder 2, dadurch gekennzeichnet, dass während der Rückführoperation die Lösung bei einer Rate von 1 bis 2 mL/min zirkuliert wird.
  4. Verfahren nach einem der vorangehenden Ansprüche, dadurch gekennzeichnet, dass die pH-Puffer-Operation eine Alkalisierungsoperation darstellt, die angepasst ist, um den pH-Wert auf 5 bis 13,5 zu bringen.
  5. Verfahren nach einem der vorangehenden Ansprüche, dadurch gekennzeichnet, dass der Stromausgang während der Rückführoperation eine Stärke von 40 bis 100 mA und eine Potenzialdifferenz von 2 bis 3 V aufweist.
  6. Verfahren nach einem der vorangehenden Ansprüche, dadurch gekennzeichnet, dass der Elektroauflösungsschritt weiterhin eine Rückführoperation umfasst, in welcher eine HCl-Lösung mit einer Konzentration von 4 bis 6 M bei einer Rate von 3 bis 5 mL/min innerhalb der Elektrolysezelle während der Ausgabe des Stroms, umgekehrt im Hinblick auf die Ausgabe während des Elektroabscheidungsschritts, geführt wird.
  7. Verfahren nach einem der vorangehenden Ansprüche, dadurch gekennzeichnet, dass das zu bestrahlende Metallisotop von der aus 60Ni, 61Ni, 64Ni, 110Cd bestehenden Gruppe umfasst ist.
  8. Verfahren nach einem der vorangehenden Ansprüche, dadurch gekennzeichnet, dass der Reinigungsschritt eine Elutionsoperation in einer Ionenaustauschsäule mittels einer HCl-Lösung mit einem Konzentrationsgradienten umfasst.
EP06425518A 2006-07-24 2006-07-24 Verfahren zur Herstellung von Radioisotopen Active EP1883079B1 (de)

Priority Applications (3)

Application Number Priority Date Filing Date Title
EP06425518A EP1883079B1 (de) 2006-07-24 2006-07-24 Verfahren zur Herstellung von Radioisotopen
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 (de) 2006-07-24 2006-07-24 Verfahren zur Herstellung von Radioisotopen

Publications (2)

Publication Number Publication Date
EP1883079A1 EP1883079A1 (de) 2008-01-30
EP1883079B1 true EP1883079B1 (de) 2009-05-06

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EP06425518A Active EP1883079B1 (de) 2006-07-24 2006-07-24 Verfahren zur Herstellung von Radioisotopen

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EP (1) EP1883079B1 (de)
AT (1) ATE430983T1 (de)
DE (1) DE602006006667D1 (de)

Families Citing this family (2)

* Cited by examiner, † Cited by third party
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的系统及高纯度Ni靶件的制备方法

Family Cites Families (6)

* Cited by examiner, † Cited by third party
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
JP2002530128A (ja) * 1998-11-18 2002-09-17 ラジオバスキュラー、システムズ、リミテッド、ライアビリティ、カンパニー 放射性コーティング溶液、方法および基板
US6157036A (en) * 1998-12-02 2000-12-05 Cedars-Sinai Medical Center System and method for automatically eluting and concentrating a radioisotope

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EP1883079A1 (de) 2008-01-30
DE602006006667D1 (de) 2009-06-18
ATE430983T1 (de) 2009-05-15

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