EP1717819B1 - System for automatically producing radioisotopes - Google Patents
System for automatically producing radioisotopes Download PDFInfo
- Publication number
- EP1717819B1 EP1717819B1 EP05425262A EP05425262A EP1717819B1 EP 1717819 B1 EP1717819 B1 EP 1717819B1 EP 05425262 A EP05425262 A EP 05425262A EP 05425262 A EP05425262 A EP 05425262A EP 1717819 B1 EP1717819 B1 EP 1717819B1
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- EP
- European Patent Office
- Prior art keywords
- unit
- target
- target carrier
- transfer means
- irradiation
- 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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- 238000004070 electrodeposition Methods 0.000 claims abstract description 12
- 239000012535 impurity Substances 0.000 claims abstract description 7
- 238000000034 method Methods 0.000 claims abstract 7
- 230000001678 irradiating effect Effects 0.000 claims abstract 3
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 21
- 229910052751 metal Inorganic materials 0.000 claims description 16
- 239000002184 metal Substances 0.000 claims description 16
- 238000005868 electrolysis reaction Methods 0.000 claims description 12
- 229910052697 platinum Inorganic materials 0.000 claims description 11
- 239000011248 coating agent Substances 0.000 claims description 7
- 238000000576 coating method Methods 0.000 claims description 7
- 238000004090 dissolution Methods 0.000 claims description 7
- 238000005192 partition Methods 0.000 claims description 5
- 230000002285 radioactive effect Effects 0.000 claims description 4
- 229910052741 iridium Inorganic materials 0.000 claims description 3
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 3
- 229910052758 niobium Inorganic materials 0.000 claims description 3
- 239000010955 niobium Substances 0.000 claims description 3
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims description 3
- 239000004411 aluminium Substances 0.000 claims description 2
- 229910052782 aluminium Inorganic materials 0.000 claims description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 2
- 239000000969 carrier Substances 0.000 claims description 2
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052737 gold Inorganic materials 0.000 claims description 2
- 239000010931 gold Substances 0.000 claims description 2
- 229910001220 stainless steel Inorganic materials 0.000 claims description 2
- 239000010935 stainless steel Substances 0.000 claims description 2
- 239000000243 solution Substances 0.000 description 19
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 16
- 239000002253 acid Substances 0.000 description 9
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 8
- 229910052759 nickel Inorganic materials 0.000 description 7
- 238000000746 purification Methods 0.000 description 7
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 4
- 238000004140 cleaning Methods 0.000 description 4
- 239000008367 deionised water Substances 0.000 description 4
- 229910021641 deionized water Inorganic materials 0.000 description 4
- 239000008151 electrolyte solution Substances 0.000 description 4
- 235000019441 ethanol Nutrition 0.000 description 4
- 229910017604 nitric acid Inorganic materials 0.000 description 4
- 239000002904 solvent Substances 0.000 description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 238000002360 preparation method Methods 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 2
- 239000000498 cooling water Substances 0.000 description 2
- 238000000151 deposition Methods 0.000 description 2
- 230000008021 deposition Effects 0.000 description 2
- 239000001307 helium Substances 0.000 description 2
- 229910052734 helium Inorganic materials 0.000 description 2
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 2
- APFVFJFRJDLVQX-FTXFMUIASA-N indium-110 Chemical compound [110In] APFVFJFRJDLVQX-FTXFMUIASA-N 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- JBNOVHJXQSHGRL-UHFFFAOYSA-N 7-amino-4-(trifluoromethyl)coumarin Chemical compound FC(F)(F)C1=CC(=O)OC2=CC(N)=CC=C21 JBNOVHJXQSHGRL-UHFFFAOYSA-N 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- 206010028980 Neoplasm Diseases 0.000 description 1
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 description 1
- 239000004327 boric acid Substances 0.000 description 1
- 239000012876 carrier material Substances 0.000 description 1
- 238000003745 diagnosis Methods 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 238000004255 ion exchange chromatography Methods 0.000 description 1
- 230000004060 metabolic process Effects 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- LGQLOGILCSXPEA-UHFFFAOYSA-L nickel sulfate Chemical compound [Ni+2].[O-]S([O-])(=O)=O LGQLOGILCSXPEA-UHFFFAOYSA-L 0.000 description 1
- 238000002600 positron emission tomography Methods 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000000717 retained effect Effects 0.000 description 1
- 239000000523 sample Substances 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
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
- C25C1/00—Electrolytic production, recovery or refining of metals by electrolysis of solutions
- C25C1/22—Electrolytic production, recovery or refining of metals by electrolysis of solutions of metals not provided for in groups C25C1/02 - C25C1/20
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
- C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
- C25C7/007—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells of cells comprising at least a movable electrode
-
- 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
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
- H05H6/00—Targets for producing nuclear reactions
Definitions
- the present invention relates to a system for automatically producing radioisotopes.
- Radioisotopes have long been produced by cyclotron irradiation for medium- or low-energy (5-30 MeV) medical applications. Radioisotopes have many important industrial and scientific uses, the most important of which is as tracers : by reactions with appropriate nonradioactive precursors, radiodrugs are synthesized and, when administered in the human body, permit diagnosis and therapy monitoring by Positron Emission Tomography (PET), especially in the treatment of tumours. By measuring radiation, it is also possible to follow all the transformations of the element and/or related molecule in chemistry (reaction mechanism research), biology (metabolism genetics research), and, as stated, in medicine for diagnostic and therapeutic purposes.
- PET Positron Emission Tomography
- the only automated passage in known systems for producing radioisotopes is that between the irradiation station and the purifying station, where the desired radioisotope is separated not only from the target carrier material but also from the non-reacting target and any impurities ( W09707122 ).
- the target carrier on which the starting metal isotope is deposited, is dissolved together with the target and subsequently removed from the manufactured radioisotope by means of a purification process.
- the electrodeposition unit and the electrodissolution unit comprise the same electrolytic cell, and the first transfer means and second transfer means coincide.
- first transfer means and second transfer means comprise a conduit connected to a pneumatic system and housing said target carrier in sliding manner.
- Number 1 in Figure 1 indicates as a whole the system for automatically producing radioisotopes according to the present invention.
- System 1 comprises an electrolysis unit 2 for both electrodeposition and electrodissolution; an irradiation unit 3 fixed directly to a cyclotron C; a purifying unit 4; transfer means 5 for transferring the target between electrolysis unit 2 and irradiation unit 3; transfer means 6 for transferring the dissolved target from electrolysis unit 2 to purifying unit 4; and a central control unit 7 for fully controlling operation of system 1.
- System 1 comprises a target carrier 8 ( Figure 2 ) defined by a cylindrical wall 9 having a truncated-cone-shaped end portion 10, and by a partition wall 11 inside and perpendicular to cylindrical wall 9.
- Partition wall 11 and cylindrical wall 9 define two separate cylindrical cavities 12 and 13. More specifically, cylindrical wall 9 thickens inwards at cavity 12; cylindrical wall 9 and partition wall 11 are made of aluminium or stainless steel; and cylindrical cavity 12 is lined with a coating 12a of platinum or niobium or iridium.
- electrolysis unit 2 is supported on a supporting structure 14, which comprises a gripping head 15; four supporting members 16 on which to store four target carriers 8; and a terminal 17 for connecting a conduit 18, as described below.
- Gripping head 15 is connected to a vacuum pump by a fitting 15a, and is moved vertically by a pneumatic cylinder and horizontally by a screw-nut screw system connected to a toothed belt.
- Each supporting member 16 has a target carrier presence sensor.
- Electrolysis unit 2 comprises an electrolytic cell 19; and a heater 20 housed, in use, inside cylindrical cavity 13 of target carrier 8.
- electrolytic cell 19 comprises a delivery tube 21; a return tube 22 defining the dissolved target transfer means 6; a platinum electrode 23 with a corresponding platinum wire 24; a gold or platinum disk electrode 25; and four springs 26 wound about respective assembly screws, and which act on a disk body 27 for disconnecting target carrier 8.
- Heater 20 comprises an electric resistor 28, and a temperature probe 29.
- transfer means 5 for transferring target carrier 8 comprise a conduit 18 connected to a known pneumatic system (not shown for the sake of simplicity) by which the target carrier is pushed or drawn along conduit 18.
- irradiation unit 3 comprises a grip pin 31 housed in use inside cylindrical cavity 13 of target carrier 8; a rotary actuator 32 connected to grip pin 31; a linear actuator 33 also connected to grip pin 31; and a pneumatic cylinder 34 connected to a terminal 35 of conduit 18.
- inside grip pin 31 are formed a central cooling water feed conduit 36 connected to a fitting 37; an intermediate annular cooling water return conduit 38 connected to a fitting 39; and an outer annular conduit 40 connected to a vacuum pump by a fitting 41.
- purification unit 4 comprises an ionic purification column 42, two pumps 43, a reactor 44, and a network of valves and vessels, and is electronically controlled to supply electrolytic cell 19 with the appropriate electrolytic solution containing the isotopes of the metals to be electrodeposited inside cavity 12 of target carrier 8, to supply electrolytic cell 19 with an HNO 3 solution for electrodissolving the irradiated target, to separate the radioisotope from the starting isotope and other radioactive impurities by ion chromatography, and to supply solvents for cleaning electrolytic cell 19, the transfer lines, and the components used to separate the radioisotope.
- a target carrier 8 is picked up by gripping head 15 and placed on heater 20, so that heater 20 is housed inside cylindrical cavity 13 of target carrier 8; and electrolytic cell 19 is then lowered into the Figure 4 position, i.e. in which disk electrode 25 contacts an edge portion of coating 12a of cylindrical cavity 12 of target carrier 8.
- an electrolytic solution from purifying unit 4 and in which the isotope of the metal to be deposited is dissolved, is fed in by delivery tube 21. As the solution flows in, the difference in potential is applied to the electrodes, and the isotope for irradiation is deposited.
- electrolytic solution is removed, and electrolytic cell 19 and cylindrical cavity 12 are cleaned using deionized water and ethyl alcohol in succession, which are then removed by a stream of helium.
- target carrier 8 is heated and maintained in a stream of gas to dry the deposited metal.
- electrolytic cell 19 is raised, and gripping head 15 removes target carrier 8 and places it either on a supporting member 16, pending irradiation, or directly inside terminal 17, from which it is blown inside conduit 18 by a stream of compressed air.
- Target carrier 8 is fed along conduit 18 to terminal 35 of irradiation unit 3, where the presence of carrier 8 is detected by a sensor.
- target carrier 8 On reaching terminal 35, target carrier 8 is retained by grip pin 31 by virtue of the vacuum produced in outer annular conduit 40. Pneumatic cylinder 34 then lowers terminal 35 and conduit 18, and rotary actuator 32 and linear actuator 33 move grip pin 31 and target carrier 8 into the irradiation position. More specifically, carrier 8 is successively rotated 90° and translated to position cylindrical cavity 12 facing an irradiation opening 45 shown in Figure 5 . Once irradiated, target carrier 8 is replaced inside terminal 35 by linear actuator 33, rotary actuator 32, and pneumatic cylinder 34; at which point, the vacuum holding target carrier 8 on grip pin 31 is cut off, and the vacuum pump connected to conduit 18 is activated to return target carrier 8 to terminal 17.
- the target carrier On reaching terminal 17, the target carrier is picked up by gripping head 15 and placed back on heater 20 as described previously; at which point, electrolytic cell 19 is lowered so that disk electrode 25 contacts the edge portion of coating 12a of cylindrical cavity 12 of target carrier 8. This time, however, unlike the electrodeposition operation described above, a portion of the coating of cylindrical cavity 12 is preferably left exposed to employ its catalyst properties for the electrodissolution reaction.
- an acid solution from purifying unit 4 and comprising nitric or hydrochloric acid, is fed in by delivery tube 21, and target carrier 8 is appropriately heated by resistor 28.
- electrodissolution is performed, by inverting one polarity of the electrodes with respect to electrodeposition, and the resulting solution is sent by a stream of inert gas to purifying unit 4.
- the electrolysis unit is cleaned and dried using deionized water and ethyl alcohol, after which, gripping head 15 can pick up another target carrier 8 and commence another work cycle.
- the acid solution from the electrodissolution operation and therefore containing the starting metal isotope and the radioisotope obtained by irradiation, is transferred to reactor 44 where the nitric acid is evaporated.
- the isotope/radioisotope mixture is redissolved in a hydrochloric acid solution, radioactivity is measured, and the solution is transferred in a stream of helium to ionic purification column 42.
- the starting metal isotope is recovered and used for further deposition.
- a solution of 10 ml of ( 60 Ni, 61 Ni, 64 Ni) comprising nickel sulphate and boric acid is fed into a vessel in purifying unit 4.
- target carrier 8 and electrolytic cell 19 are set up as shown in Figure 4
- the nickel-containing acid solution is circulated, at a temperature of 25° to 50°C, inside cylindrical cavity 12 of target carrier 8 by a closed-circuit system supplied by one of pumps 43.
- the voltage control is activated automatically and turns on the voltage and current supply pre-set to 3V and 20mA.
- the electrodeposition operation lasts an average of 24h, after which, the system is arrested and, once the electrolytic solution circuit is emptied, electrolytic cell 19 and cavity 12 are cleaned using deionized water and ethyl alcohol in succession. Once the cleaning solvents are eliminated, target carrier 8 is heated to 60°C and maintained in a stream of gas for at least 15 minutes to dry the surface of the nickel deposit. The average yield of metal nickel on the bottom of cylindrical cavity 12 corresponds to 50 ⁇ 2% of the initially dissolved nickel. When the above operations are completed, target carrier 8 is transferred automatically along conduit 18 to the irradiation unit, and, after irradiation, is transferred automatically back to electrolysis unit 2.
- electrolytic cell 19 while ensuring disk electrode 25 remains contacting the edge portion of coating 12a, is raised roughly 0.2 mm corresponding to an 88 cm 2 free-platinum surface formed on the lateral wall of cylindrical cavity 12.
- the free-platinum surface acts as a catalyst in dissolving the nickel, which is done using a 5 ml solution of nitric acid 4M contained in a vessel in purifying unit 4.
- the acid solution is circulated for about 10-20 minutes, at a flow rate of 0.5-2 ml/min, inside cylindrical cavity 12 of target carrier 8 heated to a temperature of 25 to 50°C; in which conditions, dissolution of the target is quantitative.
- the acid solution containing the dissolved nickel and the manufactured radioisotope ( 60 Cu, 61 Cu, 64 Cu) is transferred automatically to purifying unit 4, where the manufactured radioisotope ( 60 Cu, 61 Cu, 64 Cu) is separated from the respective starting nickel isotope and any other radioactive and metal impurities.
- a 10 ml solution of cadmium-110 comprising cadmium fluoborate and ammonium fluoborate is fed into a vessel in purifying unit 4 and to electrodeposition unit 2, where target carrier 8 and electrolytic cell 19 are set up as shown in Figure 4 .
- the acid solution is circulated, at a temperature of 30°C and a flow rate of 0.5-2 ml/min, inside cylindrical cavity 12 by a closed-circuit system fed by one of pumps 43; and, in these conditions, 0.02 A current and 3V voltage are applied for about 4-6h to deposit at least 40mg of cadmium-110.
- the system is cleaned with deionized water and ethyl alcohol, and, once the cleaning solvents are removed, target carrier 8 is heated to 60°C and maintained in a stream of gas for at least 15 minutes to dry the surface of the cadmium-110 deposit.
- target carrier 8 is transferred automatically along conduit 18 to the irradiation unit, and, after irradiation, is transferred automatically back to electrolysis unit 2.
- Electrodissolution is performed using a 4 ml solution of nitric acid 4M contained in a vessel in purifying unit 4.
- the acid solution is circulated for about 2 minutes at a flow rate of 0.5-2 ml/min inside cylindrical cavity 12 of target carrier 8 maintained at ambient temperature; in which conditions, dissolution is quantitative.
- the acid solution containing cadmium-110/indium-110 is transferred automatically to purifying unit 4, where the indium-110 is separated by ionic purification from the cadmium-110 and any other radioactive and metal impurities.
- the system according to the present invention has the advantage of preparing radioisotopes automatically and so ensuring high output levels.
- the system according to the present invention avoids dissolution of the target carrier, with obvious advantages at the purification stage.
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- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
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- Metallurgy (AREA)
- Organic Chemistry (AREA)
- High Energy & Nuclear Physics (AREA)
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- Optics & Photonics (AREA)
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- Spectroscopy & Molecular Physics (AREA)
- Electrolytic Production Of Metals (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
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Abstract
Description
- The present invention relates to a system for automatically producing radioisotopes.
- Radioisotopes have long been produced by cyclotron irradiation for medium- or low-energy (5-30 MeV) medical applications. Radioisotopes have many important industrial and scientific uses, the most important of which is as tracers : by reactions with appropriate nonradioactive precursors, radiodrugs are synthesized and, when administered in the human body, permit diagnosis and therapy monitoring by Positron Emission Tomography (PET), especially in the treatment of tumours. By measuring radiation, it is also possible to follow all the transformations of the element and/or related molecule in chemistry (reaction mechanism research), biology (metabolism genetics research), and, as stated, in medicine for diagnostic and therapeutic purposes.
- The only automated passage in known systems for producing radioisotopes is that between the irradiation station and the purifying station, where the desired radioisotope is separated not only from the target carrier material but also from the non-reacting target and any impurities (
W09707122 - Moreover, in known production systems, once the target has been irradiated, the target carrier, on which the starting metal isotope is deposited, is dissolved together with the target and subsequently removed from the manufactured radioisotope by means of a purification process.
- Such a solution obviously calls for more complex, prolonged purification than that required to simply separate the manufactured radioisotope from the starting isotope.
- It is an object of the present invention to provide a system for automatically producing radioisotopes, and which provides for more efficient production, in terms of output, as compared with known systems.
- According to the present invention, there is provided a system for automatically producing radioisotopes as in claim 1.
- In a preferred embodiment, the electrodeposition unit and the electrodissolution unit comprise the same electrolytic cell, and the first transfer means and second transfer means coincide.
- In a further preferred embodiment, the first transfer means and second transfer means comprise a conduit connected to a pneumatic system and housing said target carrier in sliding manner.
- A non-limiting embodiment of the invention will be described by way of example with reference to the accompanying drawings, in which:
-
Figure 1 shows an overall view of a preferred embodiment of the system for automatically producing radioisotopes according to the present invention; -
Figure 2 shows a section of the target carrier used in the system according to the present invention; -
Figure 3 shows a view in perspective of a supporting structure of the electrolysis unit of theFigure 1 system; -
Figure 4 shows a section of the electrolysis unit of theFigure 1 system; -
Figure 5 shows a view in perspective of the irradiation unit of theFigure 1 system; -
Figure 6 shows a section of a detail of theFigure 5 irradiation unit; -
Figure 7 shows a front view of the purifying unit of theFigure 1 system. - Number 1 in
Figure 1 indicates as a whole the system for automatically producing radioisotopes according to the present invention. - System 1 comprises an
electrolysis unit 2 for both electrodeposition and electrodissolution; anirradiation unit 3 fixed directly to a cyclotron C; a purifyingunit 4; transfer means 5 for transferring the target betweenelectrolysis unit 2 andirradiation unit 3; transfer means 6 for transferring the dissolved target fromelectrolysis unit 2 to purifyingunit 4; and a central control unit 7 for fully controlling operation of system 1. - System 1 comprises a target carrier 8 (
Figure 2 ) defined by acylindrical wall 9 having a truncated-cone-shaped end portion 10, and by apartition wall 11 inside and perpendicular tocylindrical wall 9.Partition wall 11 andcylindrical wall 9 define two separatecylindrical cavities cylindrical wall 9 thickens inwards atcavity 12;cylindrical wall 9 andpartition wall 11 are made of aluminium or stainless steel; andcylindrical cavity 12 is lined with acoating 12a of platinum or niobium or iridium. - As shown in
Figure 3 ,electrolysis unit 2 is supported on a supportingstructure 14, which comprises a grippinghead 15; four supportingmembers 16 on which to store fourtarget carriers 8; and aterminal 17 for connecting aconduit 18, as described below. Grippinghead 15 is connected to a vacuum pump by a fitting 15a, and is moved vertically by a pneumatic cylinder and horizontally by a screw-nut screw system connected to a toothed belt. Each supportingmember 16 has a target carrier presence sensor. -
Electrolysis unit 2 comprises anelectrolytic cell 19; and aheater 20 housed, in use, insidecylindrical cavity 13 oftarget carrier 8. - As shown in
Figure 4 ,electrolytic cell 19 comprises adelivery tube 21; areturn tube 22 defining the dissolved target transfer means 6; aplatinum electrode 23 with acorresponding platinum wire 24; a gold orplatinum disk electrode 25; and foursprings 26 wound about respective assembly screws, and which act on adisk body 27 for disconnectingtarget carrier 8. -
Heater 20 comprises anelectric resistor 28, and atemperature probe 29. - As shown in
Figures 3 and5 , transfer means 5 for transferringtarget carrier 8 comprise aconduit 18 connected to a known pneumatic system (not shown for the sake of simplicity) by which the target carrier is pushed or drawn alongconduit 18. - As shown in
Figure 5 ,irradiation unit 3 comprises agrip pin 31 housed in use insidecylindrical cavity 13 oftarget carrier 8; arotary actuator 32 connected togrip pin 31; alinear actuator 33 also connected togrip pin 31; and apneumatic cylinder 34 connected to aterminal 35 ofconduit 18. - As shown in
Figure 6 , insidegrip pin 31 are formed a central coolingwater feed conduit 36 connected to afitting 37; an intermediate annular coolingwater return conduit 38 connected to afitting 39; and an outerannular conduit 40 connected to a vacuum pump by afitting 41. - As shown in
Figure 7 ,purification unit 4 comprises anionic purification column 42, twopumps 43, areactor 44, and a network of valves and vessels, and is electronically controlled to supplyelectrolytic cell 19 with the appropriate electrolytic solution containing the isotopes of the metals to be electrodeposited insidecavity 12 oftarget carrier 8, to supplyelectrolytic cell 19 with an HNO3 solution for electrodissolving the irradiated target, to separate the radioisotope from the starting isotope and other radioactive impurities by ion chromatography, and to supply solvents for cleaningelectrolytic cell 19, the transfer lines, and the components used to separate the radioisotope. - In actual use, a
target carrier 8 is picked up by grippinghead 15 and placed onheater 20, so thatheater 20 is housed insidecylindrical cavity 13 oftarget carrier 8; andelectrolytic cell 19 is then lowered into theFigure 4 position, i.e. in whichdisk electrode 25 contacts an edge portion ofcoating 12a ofcylindrical cavity 12 oftarget carrier 8. In theFigure 4 condition, an electrolytic solution, from purifyingunit 4 and in which the isotope of the metal to be deposited is dissolved, is fed in bydelivery tube 21. As the solution flows in, the difference in potential is applied to the electrodes, and the isotope for irradiation is deposited. Once deposition is completed, the electrolytic solution is removed, andelectrolytic cell 19 andcylindrical cavity 12 are cleaned using deionized water and ethyl alcohol in succession, which are then removed by a stream of helium. Once the cleaning solvents are removed,target carrier 8 is heated and maintained in a stream of gas to dry the deposited metal. - At this point,
electrolytic cell 19 is raised, and grippinghead 15 removestarget carrier 8 and places it either on a supportingmember 16, pending irradiation, or directly insideterminal 17, from which it is blown insideconduit 18 by a stream of compressed air.Target carrier 8 is fed alongconduit 18 toterminal 35 ofirradiation unit 3, where the presence ofcarrier 8 is detected by a sensor. - On reaching
terminal 35,target carrier 8 is retained bygrip pin 31 by virtue of the vacuum produced in outerannular conduit 40.Pneumatic cylinder 34 then lowersterminal 35 andconduit 18, androtary actuator 32 andlinear actuator 33 movegrip pin 31 andtarget carrier 8 into the irradiation position. More specifically,carrier 8 is successively rotated 90° and translated to positioncylindrical cavity 12 facing anirradiation opening 45 shown inFigure 5 . Once irradiated,target carrier 8 is replaced insideterminal 35 bylinear actuator 33,rotary actuator 32, andpneumatic cylinder 34; at which point, the vacuumholding target carrier 8 ongrip pin 31 is cut off, and the vacuum pump connected toconduit 18 is activated to returntarget carrier 8 toterminal 17. - On reaching
terminal 17, the target carrier is picked up by grippinghead 15 and placed back onheater 20 as described previously; at which point,electrolytic cell 19 is lowered so thatdisk electrode 25 contacts the edge portion ofcoating 12a ofcylindrical cavity 12 oftarget carrier 8. This time, however, unlike the electrodeposition operation described above, a portion of the coating ofcylindrical cavity 12 is preferably left exposed to employ its catalyst properties for the electrodissolution reaction. Once the above situation is established, an acid solution, from purifyingunit 4 and comprising nitric or hydrochloric acid, is fed in bydelivery tube 21, andtarget carrier 8 is appropriately heated byresistor 28. - At this point, electrodissolution is performed, by inverting one polarity of the electrodes with respect to electrodeposition, and the resulting solution is sent by a stream of inert gas to purifying
unit 4. - Once the acid solution is removed from the electrolytic cell, the electrolysis unit is cleaned and dried using deionized water and ethyl alcohol, after which, gripping
head 15 can pick up anothertarget carrier 8 and commence another work cycle. - The acid solution from the electrodissolution operation, and therefore containing the starting metal isotope and the radioisotope obtained by irradiation, is transferred to
reactor 44 where the nitric acid is evaporated. The isotope/radioisotope mixture is redissolved in a hydrochloric acid solution, radioactivity is measured, and the solution is transferred in a stream of helium toionic purification column 42. The starting metal isotope is recovered and used for further deposition. - The preparation of two radioisotopes will now be described in more detail by way of example.
- A solution of 10 ml of (60Ni, 61Ni, 64Ni) comprising nickel sulphate and boric acid is fed into a vessel in purifying
unit 4. Oncetarget carrier 8 andelectrolytic cell 19 are set up as shown inFigure 4 , the nickel-containing acid solution is circulated, at a temperature of 25° to 50°C, insidecylindrical cavity 12 oftarget carrier 8 by a closed-circuit system supplied by one ofpumps 43. When the desired temperature is reached, the voltage control is activated automatically and turns on the voltage and current supply pre-set to 3V and 20mA. The electrodeposition operation lasts an average of 24h, after which, the system is arrested and, once the electrolytic solution circuit is emptied,electrolytic cell 19 andcavity 12 are cleaned using deionized water and ethyl alcohol in succession. Once the cleaning solvents are eliminated,target carrier 8 is heated to 60°C and maintained in a stream of gas for at least 15 minutes to dry the surface of the nickel deposit. The average yield of metal nickel on the bottom ofcylindrical cavity 12 corresponds to 50±2% of the initially dissolved nickel. When the above operations are completed,target carrier 8 is transferred automatically alongconduit 18 to the irradiation unit, and, after irradiation, is transferred automatically back toelectrolysis unit 2. - Once
target carrier 8 andelectrolytic cell 19 are set up as shown inFigure 4 ,electrolytic cell 19, while ensuringdisk electrode 25 remains contacting the edge portion ofcoating 12a, is raised roughly 0.2 mm corresponding to an 88 cm2 free-platinum surface formed on the lateral wall ofcylindrical cavity 12. The free-platinum surface acts as a catalyst in dissolving the nickel, which is done using a 5 ml solution of nitric acid 4M contained in a vessel in purifyingunit 4. The acid solution is circulated for about 10-20 minutes, at a flow rate of 0.5-2 ml/min, insidecylindrical cavity 12 oftarget carrier 8 heated to a temperature of 25 to 50°C; in which conditions, dissolution of the target is quantitative. Once dissolution is completed, the acid solution containing the dissolved nickel and the manufactured radioisotope (60Cu, 61Cu, 64Cu) is transferred automatically topurifying unit 4, where the manufactured radioisotope (60Cu, 61Cu, 64Cu) is separated from the respective starting nickel isotope and any other radioactive and metal impurities. - A 10 ml solution of cadmium-110 comprising cadmium fluoborate and ammonium fluoborate is fed into a vessel in
purifying unit 4 and toelectrodeposition unit 2, wheretarget carrier 8 andelectrolytic cell 19 are set up as shown inFigure 4 . The acid solution is circulated, at a temperature of 30°C and a flow rate of 0.5-2 ml/min, insidecylindrical cavity 12 by a closed-circuit system fed by one ofpumps 43; and, in these conditions, 0.02 A current and 3V voltage are applied for about 4-6h to deposit at least 40mg of cadmium-110. When electrodeposition is completed, the system is cleaned with deionized water and ethyl alcohol, and, once the cleaning solvents are removed,target carrier 8 is heated to 60°C and maintained in a stream of gas for at least 15 minutes to dry the surface of the cadmium-110 deposit. - When the above operations are completed,
target carrier 8 is transferred automatically alongconduit 18 to the irradiation unit, and, after irradiation, is transferred automatically back toelectrolysis unit 2. - Electrodissolution is performed using a 4 ml solution of nitric acid 4M contained in a vessel in
purifying unit 4. The acid solution is circulated for about 2 minutes at a flow rate of 0.5-2 ml/min insidecylindrical cavity 12 oftarget carrier 8 maintained at ambient temperature; in which conditions, dissolution is quantitative. When dissolution is completed, the acid solution containing cadmium-110/indium-110 is transferred automatically topurifying unit 4, where the indium-110 is separated by ionic purification from the cadmium-110 and any other radioactive and metal impurities. - The system according to the present invention has the advantage of preparing radioisotopes automatically and so ensuring high output levels.
- Moreover, by providing for electrodissolution of the irradiated metal, the system according to the present invention avoids dissolution of the target carrier, with obvious advantages at the purification stage.
Claims (13)
- A system (1) for automatically producing radioisotopes comprising a target carrier (8) an electrodeposition unit (2) for electrodepositing a target in said target carrier; an irradiation unit (3) for irradiating said target in said target carrier (8) ; first transfer means (5, 18) for transferring the target carrier from the electrodeposition unit (2) to the irradiation unit (3); a purifying unit (4) for purifying the radioisotope of the non-reacting target and impurities; and a central control unit (7) for controlling the operating units and transfer means to automate the entire process; said system being characterized by comprising an electrodissolution unit (2) able to electrodissolve said target while avoiding dissolution of the target carrier (8); second transfer means (5, 18) for transferring the target carrier from the irradiation unit (3) to the electrodissolution unit (2); third transfer means (6, 22) for transferring the electrodissolved irradiated target from the electrodissolution unit (2) to the purifying unit (4);
- A system as claimed in Claim 1, characterized in that the electrodeposition unit and the electrodissolution unit comprise the same electrolytic cell (2); and in that said first transfer means (5, 18) and said second transfer means (5, 18) coincide.
- A system as claimed in Claim 2, characterized in that said first transfer means (5) and said second transfer means (5) comprise a conduit (18) connected to a pneumatic system and housing said target carrier (8) in sliding manner.
- A system as claimed in any one of the foregoing Claims, characterized in that said target carrier (8) comprises a cylindrical wall (9), and a partition wall (11) inside and perpendicular to the cylindrical wall (9) to define a first (12) and a second (13) cylindrical cavity separate from each other; said first cylindrical cavity (12) housing the target for irradiation.
- A system as claimed in Claim 4, characterized in that said cylindrical wall (9) and said partition wall (11) are made of aluminium or stainless steel; and in that said first cylindrical cavity (12) is lined with a coating (12a) of platinum or niobium or iridium.
- A system as claimed in Claim 5, characterized in that said electrolysis unit comprises an electrolytic cell (19); and a heater (20) which is housed in said second cylindrical cavity (13) of the target carrier (8).
- A system as claimed in Claim 6, characterized in that said electrolytic cell (19) comprises a platinum electrode (23); and a disk electrode (25) made of gold or platinum and which, in use, contacts an edge portion of the coating (12a) of the first cylindrical cavity (12) of the target carrier (8).
- A system as claimed in any one of the foregoing Claims, characterized in that said electrolysis unit (2) is fitted to a supporting structure (14) comprising a pneumatic gripping head (15), and a number of supporting members (16) on which an equal number of target carriers (8) can be stored.
- A system as claimed in any one of the foregoing Claims, characterized in that said irradiation unit (3) comprises a grip pin (31); a rotary.actuator (32) connected to the grip pin (31); and a linear actuator (33) also connected to the grip pin (31).
- A method of producing radioisotopes comprising a first step of electrodepositing a metal isotope for irradiation inside a target carrier (8) lined with platinum or iridium or niobium; a second step of irradiating the deposited metal isotope; and a fourth step of purifying the radioisotope of the starting metal isotope and any other radioactive and metal impurities; said method being characterized by comprising before said fourth step, a third step of electrodissolving the irradiated metal isotope and the formed radioisotope while avoiding dissolution of the target carrier (8).
- A method as claimed in Claim 10, characterized in that said third step comprises the participation of a platinum portion free of surface deposits.
- A method as claimed in Claim 11, characterized in that said platinum portion is part of the lining of said target carrier (8).
- A method as claimed in any one of Claims 10 to 12, characterized in that said metal isotope is included in the group comprising 60Ni, 61Ni, 64Ni and 110Cd.
Priority Applications (7)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
ES05425262T ES2369482T3 (en) | 2005-04-27 | 2005-04-27 | SYSTEM TO PRODUCE RADIOSOTOPES AUTOMATICALLY. |
AT05425262T ATE517418T1 (en) | 2005-04-27 | 2005-04-27 | SYSTEM FOR AUTOMATICALLY OBTAINING RADIOISOTOPES |
EP05425262A EP1717819B1 (en) | 2005-04-27 | 2005-04-27 | System for automatically producing radioisotopes |
DK05425262.2T DK1717819T3 (en) | 2005-04-27 | 2005-04-27 | System for automatically producing radioisotopes |
US11/919,509 US20100025251A1 (en) | 2005-04-27 | 2006-04-24 | System for automatically producing radioisotopes |
PCT/EP2006/061853 WO2006114433A2 (en) | 2005-04-27 | 2006-04-26 | System for automatically producing radioisotopes |
CA2606643A CA2606643C (en) | 2005-04-27 | 2006-04-26 | System for automatically producing radioisotopes |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
EP05425262A EP1717819B1 (en) | 2005-04-27 | 2005-04-27 | System for automatically producing radioisotopes |
Publications (2)
Publication Number | Publication Date |
---|---|
EP1717819A1 EP1717819A1 (en) | 2006-11-02 |
EP1717819B1 true EP1717819B1 (en) | 2011-07-20 |
Family
ID=35677483
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP05425262A Active EP1717819B1 (en) | 2005-04-27 | 2005-04-27 | System for automatically producing radioisotopes |
Country Status (7)
Country | Link |
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US (1) | US20100025251A1 (en) |
EP (1) | EP1717819B1 (en) |
AT (1) | ATE517418T1 (en) |
CA (1) | CA2606643C (en) |
DK (1) | DK1717819T3 (en) |
ES (1) | ES2369482T3 (en) |
WO (1) | WO2006114433A2 (en) |
Families Citing this family (7)
Publication number | Priority date | Publication date | Assignee | Title |
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US7781744B2 (en) * | 2008-08-21 | 2010-08-24 | Comecer S.P.A. | Procedure for the preparation of radioisotopes |
DE102009005893B3 (en) * | 2009-01-23 | 2010-12-02 | Forschungszentrum Jülich GmbH | Method of generating 11C and target body |
EP2620949A4 (en) * | 2010-09-22 | 2017-06-14 | National Institutes for Quantum and Radiological Science and Technology | Process and device for production of radionuclide using accelerator |
US9991013B2 (en) | 2015-06-30 | 2018-06-05 | General Electric Company | Production assemblies and removable target assemblies for isotope production |
EP3608921B1 (en) | 2018-08-06 | 2020-12-16 | Ion Beam Applications S.A. | Capsule for a target material and system for irradiating said target material |
EP3844784A4 (en) * | 2018-08-27 | 2022-05-18 | BWXT Isotope Technology Group, Inc. | Target irradiation systems for the production of radioisotopes |
WO2020196793A1 (en) * | 2019-03-28 | 2020-10-01 | 住友重機械工業株式会社 | Target irradiation system, and recovery method for radioactive isotope from solid target |
Family Cites Families (10)
Publication number | Priority date | Publication date | Assignee | Title |
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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 |
US5037602A (en) * | 1989-03-14 | 1991-08-06 | Science Applications International Corporation | Radioisotope production facility for use with positron emission tomography |
CA2055297C (en) * | 1990-11-13 | 1996-10-08 | Iwao Kanno | Apparatus and method for producing and automatically injecting h--o |
WO1997007122A2 (en) * | 1995-08-09 | 1997-02-27 | Washington University | PRODUCTION OF 64Cu AND OTHER RADIONUCLIDES USING A CHARGED-PARTICLE ACCELERATOR |
US6153154A (en) * | 1998-05-27 | 2000-11-28 | Battelle Memorial Institute | Method for sequential injection of liquid samples for radioisotope separations |
US6157036A (en) * | 1998-12-02 | 2000-12-05 | Cedars-Sinai Medical Center | System and method for automatically eluting and concentrating a radioisotope |
US6221437B1 (en) * | 1999-04-12 | 2001-04-24 | Reynolds Tech Fabricators, Inc. | Heated workpiece holder for wet plating bath |
US20050006245A1 (en) * | 2003-07-08 | 2005-01-13 | Applied Materials, Inc. | Multiple-step electrodeposition process for direct copper plating on barrier metals |
EP1512774A1 (en) * | 2003-09-08 | 2005-03-09 | Ion Beam Applications S.A. | A method and apparatus for the electrodissolution of elements |
ATE468589T1 (en) * | 2004-09-28 | 2010-06-15 | Soreq Nuclear Res Ct Israel At | METHOD AND SYSTEM FOR PRODUCING RADIOISOTOPES |
-
2005
- 2005-04-27 ES ES05425262T patent/ES2369482T3/en active Active
- 2005-04-27 DK DK05425262.2T patent/DK1717819T3/en active
- 2005-04-27 AT AT05425262T patent/ATE517418T1/en not_active IP Right Cessation
- 2005-04-27 EP EP05425262A patent/EP1717819B1/en active Active
-
2006
- 2006-04-24 US US11/919,509 patent/US20100025251A1/en not_active Abandoned
- 2006-04-26 CA CA2606643A patent/CA2606643C/en active Active
- 2006-04-26 WO PCT/EP2006/061853 patent/WO2006114433A2/en active Application Filing
Also Published As
Publication number | Publication date |
---|---|
ATE517418T1 (en) | 2011-08-15 |
CA2606643A1 (en) | 2006-11-02 |
DK1717819T3 (en) | 2011-11-07 |
ES2369482T3 (en) | 2011-12-01 |
WO2006114433A2 (en) | 2006-11-02 |
EP1717819A1 (en) | 2006-11-02 |
CA2606643C (en) | 2013-09-03 |
US20100025251A1 (en) | 2010-02-04 |
WO2006114433A3 (en) | 2007-02-22 |
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