EP2146555A1 - Appareil cible pour la production de radio-isotopes - Google Patents

Appareil cible pour la production de radio-isotopes Download PDF

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Publication number
EP2146555A1
EP2146555A1 EP08160763A EP08160763A EP2146555A1 EP 2146555 A1 EP2146555 A1 EP 2146555A1 EP 08160763 A EP08160763 A EP 08160763A EP 08160763 A EP08160763 A EP 08160763A EP 2146555 A1 EP2146555 A1 EP 2146555A1
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EP
European Patent Office
Prior art keywords
chamber
target
target material
cylinder
opening
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Withdrawn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
EP08160763A
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German (de)
English (en)
Inventor
Yves Jongen
Andrea Cambriani
Michel Degeyter
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
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Ion Beam Applications SA
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Filing date
Publication date
Application filed by Ion Beam Applications SA filed Critical Ion Beam Applications SA
Priority to EP08160763A priority Critical patent/EP2146555A1/fr
Priority to PCT/EP2009/059263 priority patent/WO2010007174A1/fr
Publication of EP2146555A1 publication Critical patent/EP2146555A1/fr
Withdrawn legal-status Critical Current

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    • 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 invention relates to a device for use as target for producing a radioisotope, such as 18 F, by irradiating with a beam of particles a target material that includes a precursor of said radioisotope.
  • a radioisotope such as 18 F
  • One of the application of the present invention relates to nuclear medicine, and in particular to positron emission tomography.
  • Positron emission tomography is a precise and non-invasive medical imaging technique.
  • a radiopharmaceutical molecule labeled by a positron-emitting radioisotope, in situ disintegration of which results in the emission of gamma rays is injected into the organism of a patient.
  • These gamma rays are detected and analyzed by an imaging device 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 namely fluorine 18, 2-[ 18 F]-fluoro-2-deoxy-D-glucose (FDG) is the radio-tracer used most often in positron-emission tomography.
  • FDG fluorine 18, 2-[ 18 F]-fluoro-2-deoxy-D-glucose
  • PET performed with 18 F-FDG allows to determine the glucose metabolism of tumors (oncology), myocardium (cardiology) and brain (psychology).
  • the 18 F radioisotope in its anionic form ( l8 F - ) is produced by bombarding a target material, which in the present case consists of 18 O-enriched water (H 2 18 0), with a beam of charged particles, more particularly protons.
  • a target material which in the present case consists of 18 O-enriched water (H 2 18 0)
  • H 2 18 0 18 O-enriched water
  • the cavity in which the target material is placed is sealed by a window, called “irradiation window” which is transparent to the particles of the irradiation beam.
  • irradiation window which is transparent to the particles of the irradiation beam.
  • the beam of particles is advantageously accelerated by an accelerator such as a cyclotron.
  • the power to be dissipated for a 18 MeV proton beam with an intensity of 50 to 150 pA is between 900 W and 2700 W, and this in a volume of 18 O-enriched water of 0.2 to 5 ml, and for irradiation times possibly ranging from a few minutes to a few hours.
  • the irradiation intensities for producing radioisotopes are currently limited to 40 ⁇ A for an irradiated target material volume of 2ml in a silver insert.
  • Current cyclotrons used in nuclear medicine are however theoretically capable of accelerating proton beams with intensities ranging from 80 to 100 ⁇ A, or even higher. The possibilities afforded by current cyclotrons are therefore under-exploited.
  • document BE-A-1011263 discloses an irradiation cell comprising an insert made of silver (Ag) or titanium (Ti), said insert comprising a hollowed-out cavity sealed by a window, in which cavity the target material is placed.
  • the insert is placed in co-operation with a diffuser element which surrounds the outer wall of said cavity so as to form a double-walled jacket allowing the circulation of a refrigerant for cooling said target material.
  • a cavity having a wall as thin as possible is desirable.
  • wall porosity becomes a problem when wall thickness is smaller than 1, 5mm.
  • niobium Nb
  • this material having a thermal conductivity two and a half times higher than titanium (53.7 W/m/K for Nb and 21.9 W/m/K for Ti), though eight times lower than silver (429 W/m/K).
  • Niobium is chemically inert and produces few isotopes of long half-life. Therefore, niobium is a good compromise.
  • niobium is a difficult material to use in an insert of complex design, as it is difficult to machine. A build-up edge may occur on the tools, leading to high tool wear. Eventually, the tool may break.
  • the use of electrical discharge machining is not a solution either: the electrodes wear out without shaping the piece to be machined.
  • the insert described in document BE-A-1011263 is of a complex structure, and is difficult to produce in niobium.
  • Tantalum (Ta) is also a material having interesting properties, but, which is, like niobium, difficult to machine. Tantalum has a thermal conductivity (57.5 W/m/K) slightly higher (better) than Niobium.
  • Document WO02101757 is related to an apparatus for producing 18 F-Fluoride, wherein a cylindrical chamber is present, for containing the gaseous or liquid target material which is to be irradiated.
  • the chamber can be made from niobium and comprises an irradiation window on one extremity of the cylinder.
  • the accelerated particle beam is directed following the longitudinal axis of the cylinder and passes trough the irradiation window.
  • the irradiation devices described in US5917874 , US2001/0040223 and US5425063 In the case of gaseous target materials, the chamber length must be long enough to provide an efficient interaction between the accelerated particle beam and the gaseous target molecules.
  • document WO03/099374 describes a target chamber acting as a thermosiphon.
  • the vapor is condensed in the upper part of the cavity target (condenser region CR, 32A) and falls down into the lower part of the said cavity (boiler region, 32B) where is located the beam strike region (34).
  • document US2006/0291607 describes a target that comprises, inside the body cavity (112), an auxiliary cavity where the cooling is improved.
  • This target comprises also two support grid in order to reinforcing the front and rear thin films of the cavity, when the target is irradiated by a high power beam, causing an internal pressure rising.
  • the maximum allowable internal pressure is limited to 40-60 bar, due to the irradiation window foil strength, even if a support grid is used.
  • higher pressures would be desirable for reducing the tunneling effect.
  • Niobium tensile strength being high, it is not easy to produce such a sphere.
  • the authors firstly built two niobium hemispheres with a hydraulic press, and then drilled a hole in their centers. Niobium tubes were electron-beam welded to the holes and then the two hemispheres were electron-beam welded together. Two major disadvantages of the electron-beam welding are:
  • the present invention aims to provide a target apparatus and method for producing a radioisotope of interest, such as 18 F, from a target material irradiated with a beam of accelerated particles, not having the drawbacks of the devices and methods of the prior art.
  • a target apparatus and method that can withstand higher internal pressures than the prior art targets and methods, and therefore a higher production yield of radioisotopes.
  • the present invention relates to a target apparatus for producing a radioisotope of interest from a target material irradiated by a beam of charged accelerated particles having an energy
  • the said target comprising a chamber for containing a target material; a body enclosing said chamber and forming a gap between said chamber and said body adapted for the circulation of a cooling fluid, said body having an opening for leaving a passage for said beam of accelerated particles to said chamber, said opening being provided with a cooling window foil (106) retaining cooling fluid running inside said gap.
  • said chamber is a cylinder, with a thickness higher than 50 ⁇ m, and internal diameter equal or higher than the penetration range of said charged particles in said target material at the energy of said charged particles when penetrating said target material; and the said opening being parallel to the longitudinal axis of the cylinder.
  • said chamber is sealed in the said body by means of crushing seals located in the two cylinder heads of the said body.
  • the surface of the said cooling window foil is parallel to the longitudinal axis of said cylindrical chamber.
  • Said cooling window foil may be clamped between two flanges comprising an opening that fits with the width of the said chamber, the first flange being fixed in a tight manner with seals and screws on the body and the second flange being fixed in a tight manner on the first flange with seals and screws.
  • the target may preferably comprise an insulated conductor inserted in the back of said body in front of the said opening, in order to monitor the fraction of the beam of accelerated particles which passes trough the chamber.
  • the target apparatus may advantageously be pressurized and the upper leg of the filling loop of the chamber may be connected to a pressure transducer in order to monitor the internal pressure of the said chamber.
  • the invention relates to a method for producing an isotope of interest, comprising the steps of:
  • the method may advantageously comprise the step providing an insulated conductor for receiving any part of said charged particle beam traversing said chamber and monitoring the tunnelling effect by measuring the beam current incident on said insulated conductor.
  • the method may be performed using the target apparatus of the invention.
  • Fig. 1 is a cross sectional view of a target apparatus of the present invention.
  • Fig. 2 is a perspective view of a part of the target apparatus of Fig. 1 , comprising a cooling window foil.
  • Fig. 3 is a 3-dimensional exploded perspective view of the target apparatus of Fig. 1 , wherein some O-rings are referenced as 301.
  • Figure 4 is a flow chart of a circuit for use with the target apparatus of the invention.
  • Fig. 1 and fig. 3 are cross sectional and perspective representations respectively of the target apparatus used for the production of isotopes of interest such 18 F.
  • the said target comprises a metallic cylindrical chamber (101), ideally in niobium for its excellent properties of tensile strength and its chemical inertness in corrosives environments.
  • the cylindrical chamber does not comprise any window and the accelerated particle beam must have a sufficient energy to pass trough the wall of the cylindrical chamber and deposit its energy in the target material even if an important part of the energy dissipates in the cylinder wall.
  • a beam of charged particles is directed unto the cylinder, in a direction perpendicular to the cylinder axis.
  • the cylindrical chamber (101) external diameter is selected in order to obtain a high conversion of 18 O enriched water in 18 F. It is known that for a 20MeV energetic proton beam, the range of protons (i.e. the Bragg peak depth) in water is approximately 4.2mm. Thus, for a 20MeV energetic beam entering into the cylinder, the cylinder inner diameter must be of at least 4.2 mm.
  • the cylinder wall thickness must be of 50 ⁇ m for the same external cylinder inner diameter as cited above. A good compromise is to withstand a strong pressure and to not decrease too much the beam energy.
  • the chamber of the present invention makes it possible to utilise high currents and/or energetic particles beam produced for example by a cyclotron.
  • the use of high current and/or high energy beam causes a more important heating of the chamber, thus an efficient cooling system must be employed.
  • That cooling system passes trough the annular gap (107) and comprises an inlet (103) for the arrival of the cooling fluid and an outlet (104) for its evacuation.
  • the resulting pressure inside the cooling system may be of about 4-5 bar, so the conventional sticking of a thin metallic window to separate the vacuum and the cooling fluid is not able to withstand that pressure difference.
  • a cooling window foil (106), advantageously in niobium, is fixed by a system represented on Fig. 2 .
  • the cooling window foil (106) as represented on the fig.2 . is a plane disc, but that form is not a limitation of the present invention.
  • the cooling window foil (106) is clamped between two flanges (211 and 213).
  • the first flange (211) is fixed in a watertight manner with O-rings (212) and screws on the body.
  • the second flange (213) is fixed on the first flange (211) with O-rings (212) and screws.
  • the two flanges comprise an opening (214) that fit with the width of the chamber.
  • the said cylindrical chamber (101) is maintained in the body (102) by O-rings (114) located on the wall of the cylinder heads (113), and sealed in the body (102) with crushing seals (105) which can resist to high temperatures in an order of magnitude of 300°C, even higher and high pressures in an order of magnitude of 300-400 bar, even higher.
  • the said crushing seals are made ideally in Vespel® but that is not a limitation of the present invention.
  • extremities of the cylindrical chamber are not electron beam welded, that welding presenting a weak point for the resistance of the chamber and for the adsorption of fluoride on the asperities created by that welding.
  • the target material for example enriched 18 O water
  • vapour phase water molecules concentration being lower than in the condensed phase, a decreasing of the number of water molecules hit by the particle beam occurs and a higher number of particles pass trough the cylindrical chamber without encountering water molecules.
  • This effect is called tunnelling effect.
  • This tunnelling effect causes an important decreasing of production yield of radioisotopes.
  • the design of the target apparatus described in the present invention permits to the cylindrical chamber (101) to withstand a higher internal pressure than prior art target chambers.
  • the maximal internal pressure allowed is of 275 bar.
  • the cylindrical chamber (101) is not weakened by any welding.
  • high pressurization with an inert gas of an order of magnitude of more than 20 bar is provided inside the cylindrical chamber (101).
  • a gas inlet connection (108) is located at the upper cylinder head (113) for performing high pressurization of the cylindrical chamber (101).
  • a conductor (110) isolated by an insulator (303, fig. 3 ) is inserted in the back of the body (102) and opposite to the cooling window foil (106).
  • the protons In case of tunnelling, the protons have sufficient energy to hit the insulated conductor (110).
  • the corresponding measured current, the tunnelling current is an estimate of the magnitude of the tunnelling phenomenon and of the exact conditions when it sets on.
  • a pressure transducer (402, Fig. 4 ) is connected to the upper part of the cylindrical chamber (101).
  • thermocouples (403) inserted via two ports, in the upper (111) and lower (112) region of the cylindrical chamber.
  • the lower thermocouple tip is at least 6 mm under the beam strike region, whereas the upper thermocouple tip is 6 mm above the beam strike region.
  • the two thermocouples are submerged in the target material.
  • the successive steps for the production of radioisotopes are:
  • a double three-way valve actuated by compressed air for example the commercial Rheodyne valve model 7030 (401, Fig 4 ), makes possible the target loading and unloading procedures.
  • the three-position actuator that makes the valve rotate into position is designed and manufactured by the applicant.
  • the actuators rotates the valve into positions (with an angle of either +30°, 0° or -30°), by supplying 24 V DC pulse to one solenoid 5/2-way valve.
  • the position is maintained when power is interrupted.
  • the system operation is shown on fig. 4 .
  • the valve body is made in stainless steel while the rotor seals are made in PEEK.
  • the maximum allowable pressure is 483 bar.
  • the valve is located inside the irradiation vault, close to the target.
  • the liquid is then delivered to the cylindrical chamber (101) through the rheodyne valve (401).
  • the syringe mechanism is located inside the irradiation vault as close as possible to the target.
  • port B to port A When port B to port A is open the liquid is loaded inside the chamber by an inlet (109, Fig1 ) and port E to port D is open, to evacuate the overflow liquid in an overflow reservoir (409) advantageously located inside the irradiation vault as close as possible to the chamber, in order to minimise the loop volume.
  • the chamber is connected to a loop for the unloading of the products and for the pressurization of the chamber.
  • the loop comprises a bottle of helium outside the vault connected to a pressure regulator connected to two lines.
  • a first line is connected to the chamber via a valve V1, in order to provide the over pressure into the chamber before irradiation and while all the ports are closed.
  • the second line is connected to the rheodyne valve via a valve V2 in order, after irradiation, to push the produced radioisotopes solution, from the chamber to the lab dispensing (408), while port B to C and port E to F are open.
  • Typical experiments were performed on a target apparatus comprising a cylindrical chamber having the following dimensions: 100 mm length, 10 mm cylinder outer diameter, 0.4 mm cylinder wall thickness.
  • Deionised water flowed at 19 ml/min in a 1 mm annular gap between the cylinder chamber (101) and the body (102).
  • the cooling window was made of a 50 ⁇ m thick niobium foil clamped into two flanges fixed on an aluminum body. It is assumed that the minimal distance between the plane cooling window foil and the cylindrical chamber is of 700 ⁇ m.
  • the window surface seen by the beam was of 6mm X 26mm.
  • the total volume of the cylindrical chamber is approximately 6.65ml and the target was filled up to 6 ml.
  • a cylinder chamber may be designed by first setting the cylinder wall thickness (t). Knowing the cooling window foil thickness, the water thickness between the cooling window foil and the cylinder, and setting the cylinder wall thickness, it is possible to calculate theoretically the energy of the beam entering the cylindrical chamber. Knowing this, it is possible to calculate the range of protons in water, which can be assimilated to a minimal inner diameter (d min ) of the cylindrical chamber. One can obtain a maximal internal pressure (P max ) for a thickness combined with the corresponding minimal inner diameter. Some non-limitative examples are shown in table 3 for an accelerated proton beam of 30MeV.
  • Table 3 t beam Energy inside the chamber proton range d min P max ( ⁇ m) (MeV) (mm) (mm) (bar) 300 25 6,2 6,2 305 400 24 5,8 5,8 426 500 23 5,4 5,4 560 700 20 4,2 4,2 943
  • Others designs of the target comprising a cylindrical chamber with a thinner thickness suitable for irradiation with 18MeV protons may be constructed according to the same way, in order to withstand a needed pressure to suppress or reduce the tunnelling and in order to have a sufficient beam energy entering inside the chamber.
  • Some non-limitative examples are shown in table 4 for an accelerated proton beam of 18MeV.

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  • Physics & Mathematics (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Optics & Photonics (AREA)
  • Engineering & Computer Science (AREA)
  • Plasma & Fusion (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Particle Accelerators (AREA)
EP08160763A 2008-07-18 2008-07-18 Appareil cible pour la production de radio-isotopes Withdrawn EP2146555A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP08160763A EP2146555A1 (fr) 2008-07-18 2008-07-18 Appareil cible pour la production de radio-isotopes
PCT/EP2009/059263 WO2010007174A1 (fr) 2008-07-18 2009-07-17 Appareil-cible pour la production de radio-isotopes

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Cited By (7)

* Cited by examiner, † Cited by third party
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WO2011133281A1 (fr) * 2010-04-19 2011-10-27 General Electric Company Cible à auto-blindage pour systèmes de production d'isotopes
EP2581914A1 (fr) * 2011-10-10 2013-04-17 Ion Beam Applications S.A. Procédé et installation pour la production d'un radioisotope
CN103222009A (zh) * 2010-09-08 2013-07-24 雷迪诺华公司 正电子发射器辐射系统
CN104206027A (zh) * 2012-03-30 2014-12-10 通用电气公司 用于同位素产生系统的靶窗
US10354771B2 (en) 2016-11-10 2019-07-16 General Electric Company Isotope production system having a target assembly with a graphene target sheet
US10595392B2 (en) 2016-06-17 2020-03-17 General Electric Company Target assembly and isotope production system having a grid section
WO2023183281A1 (fr) * 2022-03-21 2023-09-28 Potentalpha Nükleer Tip Biyoteknoloji Klinik Araştirma Ve Danişmanlik Limited Şirket Procédé et appareil de production d'isotope d'actinium 225

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CN102946686B (zh) * 2012-11-19 2015-07-01 北京大学 一种基于等离子体窗无窗密封的液态金属散裂中子靶装置
US10714225B2 (en) 2018-03-07 2020-07-14 PN Labs, Inc. Scalable continuous-wave ion linac PET radioisotope system
US11315700B2 (en) 2019-05-09 2022-04-26 Strangis Radiopharmacy Consulting and Technology Method and apparatus for production of radiometals and other radioisotopes using a particle accelerator

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US5425063A (en) 1993-04-05 1995-06-13 Associated Universities, Inc. Method for selective recovery of PET-usable quantities of [18 F] fluoride and [13 N] nitrate/nitrite from a single irradiation of low-enriched [18 O] water
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US5917874A (en) 1998-01-20 1999-06-29 Brookhaven Science Associates Accelerator target
WO1999063550A1 (fr) * 1998-06-02 1999-12-09 European Community (Ec) Procede de production d'actinium-225 par irradiation de radium-226 au moyen de protons
US20010040223A1 (en) 1998-09-02 2001-11-15 Ichiro Fujiwara Positron source, method of preparing the same, and automated system for supplying the same
WO2002101757A2 (fr) 2001-06-13 2002-12-19 The University Of Alberta, The University Of British Columbia, Carleton University, Simon Fraser University And The University Of Victoria Appareil et procede de generation de 18f-fluorure au moyen de faisceaux ioniques
WO2003099374A2 (fr) 2002-05-21 2003-12-04 Duke University Cibles en lot et procede de production de radionucleides
US20060291607A1 (en) 2005-06-21 2006-12-28 Hong Bong H Target apparatus

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WO2002101757A2 (fr) 2001-06-13 2002-12-19 The University Of Alberta, The University Of British Columbia, Carleton University, Simon Fraser University And The University Of Victoria Appareil et procede de generation de 18f-fluorure au moyen de faisceaux ioniques
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Cited By (17)

* Cited by examiner, † Cited by third party
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WO2011133281A1 (fr) * 2010-04-19 2011-10-27 General Electric Company Cible à auto-blindage pour systèmes de production d'isotopes
US9693443B2 (en) 2010-04-19 2017-06-27 General Electric Company Self-shielding target for isotope production systems
CN103222009B (zh) * 2010-09-08 2016-06-08 雷迪诺华公司 正电子发射器辐射系统
CN103222009A (zh) * 2010-09-08 2013-07-24 雷迪诺华公司 正电子发射器辐射系统
CN104011803A (zh) * 2011-10-10 2014-08-27 离子束应用股份有限公司 制备放射性同位素的方法和设备
JP2014529089A (ja) * 2011-10-10 2014-10-30 イオン・ビーム・アプリケーションズ・エス・アー 放射性同位体を生成するための方法及び装置
US20140376677A1 (en) * 2011-10-10 2014-12-25 Ion Beam Applications S. A. Process And Installation For Producing Radioisotopes
WO2013064342A1 (fr) * 2011-10-10 2013-05-10 Ion Beam Applications S.A. Procédé et installation pour la production d'un radioisotope
EP2581914A1 (fr) * 2011-10-10 2013-04-17 Ion Beam Applications S.A. Procédé et installation pour la production d'un radioisotope
US9941027B2 (en) * 2011-10-10 2018-04-10 Ion Beam Applications S.A. Process and installation for producing radioisotopes
CN104206027A (zh) * 2012-03-30 2014-12-10 通用电气公司 用于同位素产生系统的靶窗
US9894746B2 (en) 2012-03-30 2018-02-13 General Electric Company Target windows for isotope systems
CN104206027B (zh) * 2012-03-30 2020-04-21 通用电气公司 用于同位素产生系统的靶窗
US10595392B2 (en) 2016-06-17 2020-03-17 General Electric Company Target assembly and isotope production system having a grid section
US10354771B2 (en) 2016-11-10 2019-07-16 General Electric Company Isotope production system having a target assembly with a graphene target sheet
WO2023183281A1 (fr) * 2022-03-21 2023-09-28 Potentalpha Nükleer Tip Biyoteknoloji Klinik Araştirma Ve Danişmanlik Limited Şirket Procédé et appareil de production d'isotope d'actinium 225
US12232245B2 (en) 2022-03-21 2025-02-18 Ali A Abbasi Method and apparatus for production of actinium 225 isotope

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