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EP1429345A1 - Radioisotopen Herstellungsverfahren und -vorrichtung - Google Patents

Radioisotopen Herstellungsverfahren und -vorrichtung Download PDF

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Publication number
EP1429345A1
EP1429345A1 EP02447253A EP02447253A EP1429345A1 EP 1429345 A1 EP1429345 A1 EP 1429345A1 EP 02447253 A EP02447253 A EP 02447253A EP 02447253 A EP02447253 A EP 02447253A EP 1429345 A1 EP1429345 A1 EP 1429345A1
Authority
EP
European Patent Office
Prior art keywords
target material
cavity
irradiation
target
niobium
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.)
Withdrawn
Application number
EP02447253A
Other languages
English (en)
French (fr)
Inventor
Yves Jongen
Jr. Comor J. Comor
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Ion Beam Applications SA
Original Assignee
Ion Beam Applications SA
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Ion Beam Applications SA filed Critical Ion Beam Applications SA
Priority to EP02447253A priority Critical patent/EP1429345A1/de
Priority to AT03782015T priority patent/ATE498183T1/de
Priority to JP2004557684A priority patent/JP4751615B2/ja
Priority to PCT/BE2003/000217 priority patent/WO2004053892A2/en
Priority to CA2502287A priority patent/CA2502287C/en
Priority to US10/537,975 priority patent/US7940881B2/en
Priority to CNB2003801048544A priority patent/CN100419917C/zh
Priority to AU2003289768A priority patent/AU2003289768A1/en
Priority to EP03782015A priority patent/EP1570493B1/de
Priority to DE60336009T priority patent/DE60336009D1/de
Publication of EP1429345A1 publication Critical patent/EP1429345A1/de
Withdrawn legal-status Critical Current

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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
    • G21G1/10—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes outside nuclear reactors or particle accelerators by bombardment with electrically charged particles

Definitions

  • the present invention relates to a device and a method intended for the production of radioisotopes such as 18 F, by irradiation using a proton beam of a target material comprising a precursor of said radioisotope.
  • One of the applications of the present invention concerns nuclear medicine.
  • Positron emission tomography is a precise, non-invasive medical imaging technique.
  • a radiopharmaceutical marked with a positron emitting radioisotope is injected into the body of a patient, the disintegration of which in situ leads to the emission of ⁇ radiation.
  • These ⁇ rays are detected by an imaging device and analyzed in order to reconstruct in three dimensions the biodistribution of the injected radioisotope and to obtain its tissue concentration.
  • radiopharmaceuticals synthesized from the radioisotope of interest that is fluorine 18, 2- [ 18 F] fluoro-2-deoxy-D-glucose (FDG)
  • FDG fluoro-2-deoxy-D-glucose
  • an irradiation device which comprises a cavity "hollowed out” in a metal part and intended to receive the target material.
  • the 18 F is generally produced using this production device, by bombardment of a beam of charged particles, and more particularly of protons, on the target material previously disposed in said cavity.
  • This charged particle beam comes from an accelerator such as a cyclotron.
  • the cavity in which the target material is located being closed by a window called “irradiation window" which can be crossed by the protons of the irradiation beam, said protons meet the target material and it is the interaction of said protons with the target material which generates the nuclear reaction intended for the production of the radioisotope of interest.
  • the target material consists of water enriched in 18 O (H 2 18 O).
  • the material target must always produce more radioisotope.
  • This increase in production supposes either to modify the energy of the charged particle beam (protons), and in this case the cross section of the reaction is increased to modify the intensity of said beam, and in this case it is a question of modifying the number of particles accelerated hitting the target material.
  • the power dissipated by the target material irradiated by the boundary particle beam the intensity and / or energy of the particle beam that we can hope to use.
  • the power dissipated by a target material is therefore all the more important as the intensity and / or energy of the particle beam is important.
  • the problem of dissipation of the heat produced by the irradiation of the target material on such a small volume constitutes a major problem to be overcome.
  • the power to be dissipated is between 900 and 1800 watts, for currents of 50 to 100 ⁇ A of protons accelerated to 18 MeV and for irradiation times can range from a few minutes to a few hours.
  • Solutions have been proposed in the state of technique in order to overcome the problem of dissipation of heat by the target material in the cavity within the radioisotope production device.
  • devices have been proposed means for cooling the target material.
  • Belgian patent n ° 1011263 A6 describes an irradiation cell comprising a cavity closed by a window in which the material is placed target, said cavity being surrounded by a double wall allowing the circulation of a refrigerant for cooling said target material, the window being cooled with helium.
  • the present invention aims to provide a device and a method intended for the production of radioisotopes, and in particular 18 F, from a target material irradiated by a beam of charged particles which do not have the drawbacks of the devices and state of the art processes.
  • the present invention aims to provide a device intended for the production of radioisotopes, and in particular of 18 F, and capable of operating with a beam of protons whose current intensity is high, that is to say - say greater than 40 ⁇ A.
  • Another object of the invention is to provide a device which ensures in operation, that is to say during of radioisotope production, heat exchange sufficient with the external environment, so that its temperature mean remains below an average threshold temperature, said average threshold temperature preferably being located around 130 ° C.
  • this device comprises in in addition to internal cooling means to said irradiation cell, said cooling means interns taking the form of a double wall filled with a coolant and which equips said cell irradiation.
  • the external heat exchanger essentially consists of a material chosen from group consisting of silver, titanium, tantalum, niobium and / or palladium.
  • the insert is essentially made of a material selected from the group consisting of Niobium, Niobium / Palladium, silver or titanium.
  • said inlet duct is positioned essentially tangential to said cavity to create a flow vortex therein.
  • Essentially tangential means that the inlet duct forms with the tangent of the cavity assimilated to a sphere, an angle of plus or minus 25 °.
  • said outlet duct is not not located in the same plane, but on the same side as the inlet duct.
  • said cavity is capable of contain a volume of target material between 0.25 and 2.4 mL.
  • said cavity has a diameter less than 25 mm and a minimum depth of 3.5 mm.
  • the device according to the invention is configured to contain as a whole an overall volume of the target material which is less than 20 mL.
  • the various elements of said device are interconnected with each other by pipes (17) having an internal diameter between 0.5 and 2 mm.
  • the device is such that the direction of flow of the target material inside the device can be reversed depending on the layout of the various constituent elements of it.
  • said pipes connecting the different elements of the devices are basically made of a material chosen from the tantalum group, titanium, niobium, palladium, stainless steel and / or money.
  • the present invention also relates to a process for manufacturing radioisotopes by through an irradiation cell in which we placed an insert with a window and a cavity containing a target material, characterized in that said target material is recirculated through at least one conduit inlet and at least one outlet pipe from the cavity at y creating a flow vortex and through a heat exchanger heat external to said irradiation cell, by a pump with sufficient flow to cool the material target target, the device being pressurized so as to maintain the target essentially in a liquid state.
  • the direction of circulation of the target material in the device can be reversed from so that the inlet duct becomes the duct of outlet and the outlet duct becomes the duct inlet (4) of the target material.
  • said pump delivers at least 200mL / min for the duration of the irradiation.
  • the present invention relates to also the use of the device and / or the process according to the invention for the manufacture of radioisotopes.
  • Figure 1 shows a plan view of the irradiation cell of the present invention, seen in the direction of arrow X in Figures 2 and 3.
  • Figure 2 shows a section along the A-A shots of the radiation cell.
  • Figure 3 shows a section along the B-B shots of irradiation cell.
  • Figure 4 shows an overall diagram a device for producing radioisotopes comprising the device of the present invention.
  • Figure 5A shows the procedure for filling the device according to the invention.
  • Figure 5B shows the flow diagram for the target during filling
  • Figure 5C shows the routing of the target after irradiation to the FDG module.
  • the device according to the present invention comprises a cell irradiation 1 and which constitutes the mechanical assembly which, during the operation of said device, is subject to irradiation.
  • the irradiation cell 1 comprises an insert 2 which is a metal part in which a volume corresponding to a cavity is “hollowed out”.
  • the insert 2 therefore comprises the cavity 8.
  • This cavity 8 has a configuration such that it can receive the target material from which the device is capable of producing the radioisotope of interest, that is to say the 18 F in this case here.
  • the irradiation cell 1 is also fitted with 5.6 and 6.5 outlet pipes for the delivery or circulation of the target material.
  • the 5.6 inlet / 6.5 outlet ducts allow the arrival / departure of the target material or vice versa, depending on the direction of flow of the target material within the device in operation (reverse arrival and departure).
  • the cavity 8 intended to contain the target material is closed by a window called irradiation window 7.
  • the device is designed to work with a target material in the fluid state, that is to say liquid and / or gaseous.
  • the device also includes external cooling means intended to cool the target material when the device works.
  • these means of external cooling of the target material take the form of an external heat exchanger 15.
  • This external heat exchanger 15 is preferably coupled to a high-flow pump 16, which is preferably a pump specific volumetric.
  • the external heat exchanger 15 / pump 16 assembly is such that when the device operates and is pressurized, this assembly makes it possible to keep the target material in circulation essentially in its initial state, that is to say essentially liquid in the case water enriched in 18 O for the production of 18 F.
  • the configuration of the external means of cooling of target material compared to others elements of the device is such that it allows in operating a circulation speed of said material target high enough to allow an exchange of sufficient heat between said device and the medium outside so that the average internal temperature of the device is located below 130 ° C.
  • the external heat exchanger 15 can be made of silver pipes and other materials resistant to radiation, pressure and ions fluorides.
  • copper is unusable and the Nb seems difficult to machine, the money or titanium therefore being the best compromise.
  • tantalum, niobium or palladium being however possible.
  • the production device comprises advantageously further internal means of cooling intended to cool the target material when the device is working.
  • These internal means of cooling here take the form of a double wall 9 which delimits the irradiation cell 1 and which can contain a refrigerant inside circulation.
  • inserts 2 in the device according to the invention is particularly important. Indeed, depending on the type of insert 2 chosen, undesirable secondary products are likely to be generated by irradiation, during the operation of the device. This can indeed produce radioisotopes disintegrating by emission of energetic ⁇ particle and limiting the repairs on cell 1. It can also give secondary products having an influence on the subsequent synthesis of the radiotracer to be marked by 18 F thus produced.
  • a determining parameter also in the choice of the type of material of the inserts of the device according to the invention is the thermal conductivity of this material. This is how silver is a good conductor, but has the disadvantage that after several irradiations, a contaminating silver oxide formation occurs. Titanium is chemically inert but produces 48 V with a half-life of 16 days. Consequently, in the case of titanium, if there is a break in a target window, its replacement will pose serious problems of exposure to ionizing radiation to the engineers responsible for maintenance.
  • Nb which is two and a half times more conductive than titanium but less than silver. Nb produces few isotopes with a long half-life, an example being 92m Nb (parasitic nuclear reaction 93 Nb (p, d) 92m Nb) whose half-life is around ten days. The overall activation of insert 2, measured after irradiation for production, is however low in comparison with the values measured with a comparable titanium insert.
  • N 2 inserts When N 2 inserts are used, these can be covered with palladium, the latter catalyzing the reaction for the formation of 18 H 2 O from H 2 and 18 O 2 , themselves derived from the 18 H 2 O radiolysis during irradiation.
  • the radioisotope production device is a device for producing 18 F from water enriched in 18 O and a beam of protons.
  • the device can work with proton beams accelerated at understood speeds between 5 and 30 MeV, a current intensity ranging from 1 to 150 ⁇ A with an irradiation time from 1 minute to 10 hours.
  • the device has a system of high speed recirculation of enriched water which includes an advantageously combined external heat exchanger 15 internal cooling means 9 in the cell irradiation, as well as a specific positive displacement pump 16 to generate sufficient flow to maintain enriched water (target material) in the liquid state, i.e. about 200 to 500 ml per minute, the passage (transfer) of enriched water through the heat exchanger external heat 15 and the internal means of cooling to obtain cooling of 70 ° of enriched water.
  • the pump used in the embodiment described is the 120 series, supplied by the company Micropump, Inc. ( http://www.micropump.com ).
  • This pump is a gear pump. Equipped with N21 gears, it is capable of delivering 900 ml / min, under a pressure of 5.6 bar.
  • the device further comprises external means of additional cooling which take the form of a other heat exchanger external to the device and intended to cool the irradiation window 7 with helium.
  • window 7 is in Havar or in niobium and with a thickness between 50 and 200 ⁇ m.
  • the pipes used have a internal diameter between 0.5 and 2 mm. This is here very high speed recirculation which can go up to more than one full circuit tour per second.
  • the recirculation is ensured by a pump 16 which can supply a flow between 0.2 and 0.5 L / min with a gradient of significant pressure.
  • a traffic speed requires careful positioning of the inlet duct 4 and outlet conduit 5 in the cavity containing the target liquid. The goal is to create forced circulation through a vortex in this small volume for avoid the subsistence of "static" areas where the material target would circulate little.
  • the inlet duct 4 of the target material has therefore positioned on the same side as the outlet duct 5 of the target material but on an offset plane. This is fine visible in Figure 1. If the two conduits had been positioned face to face, we would inevitably have created a "static" zone within the cavity 8 containing the target material.
  • the target inlet pipe 4 is positioned tangentially in the direction of rounding of the cavity 8.
  • Target circulation within the circuit 17 and therefore of the cavity 8 can also be reversed by so that the inlet duct becomes the duct of exit.
  • the direction of rotation of the liquid within the device of the present invention is above all determined depending on the pressures generated in the circuit and the different components of it.
  • conduit 5 can be used as input for the filling, and outlet for recirculation.
  • the exit 6 serves as an overflow during filling and is connected to the expansion vessel during irradiation.
  • the valve V5 multi-channel can be placed in two positions. In the first position, it allows filling and in the second, high speed traffic during irradiation and evacuation to the FDG module. this is shown in Figure 5A, 5B and 5C.
  • the V6 valve allows provide helium, argon or nitrogen back pressure for the formation of a working "gas cushion" as an expansion tank. Helium, argon or nitrogen generally allow pressurization of all circuit which is done in particular through valves V1 and V3. Valves V2 and V4 are used for filling of the system.
  • the overall target volume contained in the entire device of the invention must not exceed 20 mL which means that the dead volume of the pump should be reduced as much as possible.
  • the heat exchanger external 15 which also contains a very small volume of target liquid, normally less than 10 mL, and preferably less than 5 mL is generally connected to a secondary cooling system (not shown) to dissipate the heat produced by irradiation of the target liquid in the cell irradiation 1.
  • the irradiation cell 1 is necessarily positioned in the axis of the incident beam.
  • the materials of which it is made must therefore be able to withstand the ionizing radiation. It is however possible to arrange pump 16, external heat exchanger 15 and valve V5 so that they are deported to be at sheltered from this radiation.
  • the inventor was able to design a solution in which these components can be brought protected from ionizing radiation by the back flow of the magnet of the cyclotron, without however the length of the pipes does not exceed 20 cm.
  • the device according to the invention allows to produce radioisotopes from a target material irradiated with a particle beam charged produced by a cyclotron. Thanks to its design, the device according to the invention has the advantage to optimize the use of the irradiation capacities of current cyclotrons. Indeed, while the windows 7 currently do not withstand pressures caused by radiation intensities greater than 45 ⁇ A, the device nevertheless allows to use the maximum intensities available on the cyclotrons currently used in nuclear medicine, i.e. approximately 100 ⁇ A.
  • the device allows to use the maximum capacities of current cyclotrons capable of producing radiation intensities exceeding 100 ⁇ A while controlling the temperature rise.
  • Target remains essentially in the liquid state which allows high speed recirculation without defusing the pump.

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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)
  • Particle Accelerators (AREA)
  • Medicines That Contain Protein Lipid Enzymes And Other Medicines (AREA)
  • Preparation Of Compounds By Using Micro-Organisms (AREA)
EP02447253A 2002-12-10 2002-12-10 Radioisotopen Herstellungsverfahren und -vorrichtung Withdrawn EP1429345A1 (de)

Priority Applications (10)

Application Number Priority Date Filing Date Title
EP02447253A EP1429345A1 (de) 2002-12-10 2002-12-10 Radioisotopen Herstellungsverfahren und -vorrichtung
AT03782015T ATE498183T1 (de) 2002-12-10 2003-12-10 Einrichtung und verfahren zur herstellung von radioisotopen
JP2004557684A JP4751615B2 (ja) 2002-12-10 2003-12-10 放射性同位体を製造する装置及び方法
PCT/BE2003/000217 WO2004053892A2 (en) 2002-12-10 2003-12-10 Device and method for producing radioisotopes
CA2502287A CA2502287C (en) 2002-12-10 2003-12-10 Device and method for producing radioisotopes
US10/537,975 US7940881B2 (en) 2002-12-10 2003-12-10 Device and method for producing radioisotopes
CNB2003801048544A CN100419917C (zh) 2002-12-10 2003-12-10 用于制造放射性同位素的装置和方法
AU2003289768A AU2003289768A1 (en) 2002-12-10 2003-12-10 Device and method for producing radioisotopes
EP03782015A EP1570493B1 (de) 2002-12-10 2003-12-10 Einrichtung und verfahren zur herstellung von radioisotopen
DE60336009T DE60336009D1 (de) 2002-12-10 2003-12-10 Einrichtung und verfahren zur herstellung von radioisotopen

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP02447253A EP1429345A1 (de) 2002-12-10 2002-12-10 Radioisotopen Herstellungsverfahren und -vorrichtung

Publications (1)

Publication Number Publication Date
EP1429345A1 true EP1429345A1 (de) 2004-06-16

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EP02447253A Withdrawn EP1429345A1 (de) 2002-12-10 2002-12-10 Radioisotopen Herstellungsverfahren und -vorrichtung
EP03782015A Expired - Lifetime EP1570493B1 (de) 2002-12-10 2003-12-10 Einrichtung und verfahren zur herstellung von radioisotopen

Family Applications After (1)

Application Number Title Priority Date Filing Date
EP03782015A Expired - Lifetime EP1570493B1 (de) 2002-12-10 2003-12-10 Einrichtung und verfahren zur herstellung von radioisotopen

Country Status (9)

Country Link
US (1) US7940881B2 (de)
EP (2) EP1429345A1 (de)
JP (1) JP4751615B2 (de)
CN (1) CN100419917C (de)
AT (1) ATE498183T1 (de)
AU (1) AU2003289768A1 (de)
CA (1) CA2502287C (de)
DE (1) DE60336009D1 (de)
WO (1) WO2004053892A2 (de)

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EP1570493A2 (de) 2005-09-07
CA2502287A1 (en) 2004-06-24
CA2502287C (en) 2011-08-23
EP1570493B1 (de) 2011-02-09
US20060104401A1 (en) 2006-05-18
CN100419917C (zh) 2008-09-17
JP4751615B2 (ja) 2011-08-17
US7940881B2 (en) 2011-05-10
AU2003289768A1 (en) 2004-06-30
JP2006509202A (ja) 2006-03-16
WO2004053892A2 (en) 2004-06-24
DE60336009D1 (de) 2011-03-24
ATE498183T1 (de) 2011-02-15
CN1726563A (zh) 2006-01-25

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