WO2006114433A2 - Systeme de production automatique de radio-isotopes - Google Patents

Systeme de production automatique de radio-isotopes Download PDF

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Publication number
WO2006114433A2
WO2006114433A2 PCT/EP2006/061853 EP2006061853W WO2006114433A2 WO 2006114433 A2 WO2006114433 A2 WO 2006114433A2 EP 2006061853 W EP2006061853 W EP 2006061853W WO 2006114433 A2 WO2006114433 A2 WO 2006114433A2
Authority
WO
WIPO (PCT)
Prior art keywords
unit
target
target carrier
transfer means
irradiation
Prior art date
Application number
PCT/EP2006/061853
Other languages
English (en)
Other versions
WO2006114433A3 (fr
Inventor
Paolo Bedeschi
Original Assignee
Comecer S.P.A.
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
Priority to US11/919,509 priority Critical patent/US20100025251A1/en
Application filed by Comecer S.P.A. filed Critical Comecer S.P.A.
Priority to CA2606643A priority patent/CA2606643C/fr
Publication of WO2006114433A2 publication Critical patent/WO2006114433A2/fr
Publication of WO2006114433A3 publication Critical patent/WO2006114433A3/fr

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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. BACKGROUND ART
  • 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
  • a system for automatically producing radioisotopes characterized by comprising a target carrier; an electrodeposition unit for electrodepositing a target in said target carrier; an irradiation unit for irradiating said target in said target carrier; first transfer means for transferring the target carrier from the electrodeposition unit to the irradiation unit; an electrodissolution unit for electrodissolving the irradiated target without corroding said target carrier (8) ; second transfer means for transferring the target carrier from the irradiation unit to the electrodissolution unit; a purifying unit for purifying the radioisotope of the non-reacting target and impurities; third transfer means for transferring the electrodissolved irradiated target from the electrodissolution unit to the purifying unit; and a central control unit for controlling the operating
  • the electrodeposition unit and the electrodissolution unit comprise the same electrolytic cell, and the first transfer means and second transfer means coincide.
  • the first transfer means and second transfer means comprise a conduit connected to a pneumatic system and housing said target carrier in sliding manner.
  • 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 2a shows a section of the target carrier according to another embodiment
  • Figure 3 shows a view in perspective of a supporting structure of the electrolysis unit of the Figure 1 system
  • Figure 4 shows a section of the electrolysis unit of the Figure 1 system
  • Figure 4a shows a section of the electrolysis unit according to another embodiment
  • Figure 5 shows a view in perspective of the irradiation unit of the Figure 1 system
  • Figure 6 shows a section of a detail of the Figure 5 irradiation unit
  • Figure 7 shows a front view of the purifying unit of the Figure 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; an irradiation unit 3 fixed directly to a cyclotron C; a purifying unit
  • 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
  • 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.
  • a hole 11a is made in the partition wall 11 to allow a more effective cooling of the coating 12a.
  • 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.
  • electrolytic cell 19 comprises a platinum electrode 23a connected with a platinum tube 24a, in which an electrolytic solution comprising the metal to be deposited is fed.
  • the platinum tubee 24a works as a delivery tube and the tubes 21 e 22 are used to remove the electrolytic solution or to clean the electrolytic cell 19.
  • the four springs 26 and the disk body 27 are absent, and other means (not shown) are used 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 or by the platinum pipe 24a. 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.
  • 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 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.
  • 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 re- dissolved 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.
  • 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 6O 0 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.
  • 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 5O 0 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 .
  • Radioisotope 110 In - 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 3O 0 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.
  • target carrier 8 is heated to 6O 0 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-llO/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. 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.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physics & Mathematics (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Electrochemistry (AREA)
  • Organic Chemistry (AREA)
  • Metallurgy (AREA)
  • Materials Engineering (AREA)
  • Optics & Photonics (AREA)
  • General Engineering & Computer Science (AREA)
  • General Chemical & Material Sciences (AREA)
  • Plasma & Fusion (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Electrolytic Production Of Metals (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Radiation-Therapy Devices (AREA)
  • Medicines Containing Plant Substances (AREA)
  • Preparation Of Compounds By Using Micro-Organisms (AREA)
  • Particle Accelerators (AREA)

Abstract

L'invention concerne un système (1) permettant de produire automatiquement des radio-isotopes, et comprenant un porteur de cibles (8); une unité d'électrodéposition (2) qui permet de déposer une cible dans le porteur de cible; une unité de rayonnement (3) qui irradie la cible dans le porteur de cible (8); un premier dispositif de transport (5, 18) qui transporte le porteur de cible de l'unité d'électrodéposition (2) à l'unité de rayonnement (3); une unité d'électrodissolution (2) qui dissout par électrolyse la cible irradiée; un deuxième dispositif de transport (5, 18) qui transporte le porteur de cible de l'unité de rayonnement (3) à l'unité d'électrodissolution (2); une unité de purification (4) qui purifie le radio-isotope de la cible non réactive et des impuretés; un troisième dispositif de transport (6, 22) qui transporte la cible irradiée dissoute par électrolyse de l'unité d'électrodissolution (2) à l'unité de purification (4); et une unité de commande centrale (7) qui commande les unités d'exploitation et les dispositifs de transport automatisant l'ensemble du processus.
PCT/EP2006/061853 2005-04-27 2006-04-26 Systeme de production automatique de radio-isotopes WO2006114433A2 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
US11/919,509 US20100025251A1 (en) 2005-04-27 2006-04-24 System for automatically producing radioisotopes
CA2606643A CA2606643C (fr) 2005-04-27 2006-04-26 Systeme de production automatique de radio-isotopes

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
EP05425262A EP1717819B1 (fr) 2005-04-27 2005-04-27 Système permettant la production automatique de radioisotopes
EP05425262.2 2005-04-27

Publications (2)

Publication Number Publication Date
WO2006114433A2 true WO2006114433A2 (fr) 2006-11-02
WO2006114433A3 WO2006114433A3 (fr) 2007-02-22

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US (1) US20100025251A1 (fr)
EP (1) EP1717819B1 (fr)
AT (1) ATE517418T1 (fr)
CA (1) CA2606643C (fr)
DK (1) DK1717819T3 (fr)
ES (1) ES2369482T3 (fr)
WO (1) WO2006114433A2 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7781744B2 (en) * 2008-08-21 2010-08-24 Comecer S.P.A. Procedure for the preparation of radioisotopes
JP2020024193A (ja) * 2018-08-06 2020-02-13 イオン ビーム アプリケーションズ ソシエテ アノニムＩｏｎ Ｂｅａｍ Ａｐｐｌｉｃａｔｉｏｎｓ Ｓ．Ａ． ターゲット材料を照射するためのシステム
RU2807899C1 (ru) * 2023-04-06 2023-11-21 Федеральное государственное бюджетное учреждение "Российский научный центр радиологии и хирургических технологий имени академика А.М. Гранова" Министерства здравоохранения Российской Федерации Способ автоматизированного синтеза радиофармпрепаратов на основе полимерных микрочастиц с использованием устройства для его осуществления

Families Citing this family (5)

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Publication number Priority date Publication date Assignee Title
DE102009005893B3 (de) * 2009-01-23 2010-12-02 Forschungszentrum Jülich GmbH Verfahren zur Erzeugung von 11C sowie Targetkörper
JP5322071B2 (ja) * 2010-09-22 2013-10-23 独立行政法人放射線医学総合研究所 加速器による放射性核種の製造方法及び装置
US9991013B2 (en) 2015-06-30 2018-06-05 General Electric Company Production assemblies and removable target assemblies for isotope production
CA3109824A1 (fr) * 2018-08-27 2020-03-05 BWXT Isotope Technology Group, Inc. Systemes d'irradiation de cible pour la production de radio-isotopes
JPWO2020196793A1 (fr) * 2019-03-28 2020-10-01

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GB1369700A (en) * 1970-12-23 1974-10-09 Union Carbide Corp 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
EP0486283A2 (fr) * 1990-11-13 1992-05-20 Uemura, Kazuo Appareil et méthode pour produire et injecter automatiquement du H215O
WO1997007122A2 (fr) * 1995-08-09 1997-02-27 Washington University PRODUCTION DE 64Cu ET AUTRES RADIONUCLEIDES A L'AIDE D'UN ACCELERATEUR DE PARTICULES CHARGEES
WO1999062073A1 (fr) * 1998-05-27 1999-12-02 Battelle Memorial Institute Procede d'injection sequentielle d'echantillons de liquide dans les separations radio-isotopes
WO2000033322A1 (fr) * 1998-12-02 2000-06-08 Cedars-Sinai Medical Center Systeme et procede pour l'elusion et la concentration automatique d'un radio-isotope

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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 (fr) * 2003-09-08 2005-03-09 Ion Beam Applications S.A. Procédé et dispositif pour la dissolution électrolytique d'éléments
WO2006035424A2 (fr) * 2004-09-28 2006-04-06 Soreq Nuclear Research Center Israel Atomic Energy Commission Procede et systeme de production de radio-isotopes et radio-isotopes ainsi produits

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1369700A (en) * 1970-12-23 1974-10-09 Union Carbide Corp 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
EP0486283A2 (fr) * 1990-11-13 1992-05-20 Uemura, Kazuo Appareil et méthode pour produire et injecter automatiquement du H215O
WO1997007122A2 (fr) * 1995-08-09 1997-02-27 Washington University PRODUCTION DE 64Cu ET AUTRES RADIONUCLEIDES A L'AIDE D'UN ACCELERATEUR DE PARTICULES CHARGEES
WO1999062073A1 (fr) * 1998-05-27 1999-12-02 Battelle Memorial Institute Procede d'injection sequentielle d'echantillons de liquide dans les separations radio-isotopes
WO2000033322A1 (fr) * 1998-12-02 2000-06-08 Cedars-Sinai Medical Center Systeme et procede pour l'elusion et la concentration automatique d'un radio-isotope

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7781744B2 (en) * 2008-08-21 2010-08-24 Comecer S.P.A. Procedure for the preparation of radioisotopes
JP2020024193A (ja) * 2018-08-06 2020-02-13 イオン ビーム アプリケーションズ ソシエテ アノニムＩｏｎ Ｂｅａｍ Ａｐｐｌｉｃａｔｉｏｎｓ Ｓ．Ａ． ターゲット材料を照射するためのシステム
RU2807899C1 (ru) * 2023-04-06 2023-11-21 Федеральное государственное бюджетное учреждение "Российский научный центр радиологии и хирургических технологий имени академика А.М. Гранова" Министерства здравоохранения Российской Федерации Способ автоматизированного синтеза радиофармпрепаратов на основе полимерных микрочастиц с использованием устройства для его осуществления

Also Published As

Publication number Publication date
ES2369482T3 (es) 2011-12-01
WO2006114433A3 (fr) 2007-02-22
CA2606643A1 (fr) 2006-11-02
CA2606643C (fr) 2013-09-03
EP1717819A1 (fr) 2006-11-02
DK1717819T3 (da) 2011-11-07
EP1717819B1 (fr) 2011-07-20
ATE517418T1 (de) 2011-08-15
US20100025251A1 (en) 2010-02-04

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