EP1464060B1 - Method and device for production of radio-isotopes from a target - Google Patents

Method and device for production of radio-isotopes from a target Download PDF

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Publication number
EP1464060B1
EP1464060B1 EP02806546A EP02806546A EP1464060B1 EP 1464060 B1 EP1464060 B1 EP 1464060B1 EP 02806546 A EP02806546 A EP 02806546A EP 02806546 A EP02806546 A EP 02806546A EP 1464060 B1 EP1464060 B1 EP 1464060B1
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radioisotope
target
precursor
solid
irradiation
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German (de)
French (fr)
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EP1464060A1 (en
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Stéphane Lucas
Ray Bricault
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Ion Beam Applications SA
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Ion Beam Applications SA
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21G—CONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/04—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes outside nuclear reactors or particle accelerators
    • 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

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  • the present invention relates to a method and a device for the production of radioisotopes from a target consisting essentially of an isotope precursor which is irradiated by an accelerated particle beam, the radioisotope once produced being separated from its precursor.
  • a particular application of the present invention relates to the production of palladium 103 from rhodium 103.
  • radioisotopes are by bombardment or irradiation of a target consisting essentially of an isotope precursor using an accelerated particle beam.
  • a nuclear reaction occurs which causes a fraction of the isotope precursor present to be converted to a radioisotope. It should be noted that in most cases the created radioisotope is intimately mixed with the isotope precursor material constituting the target and thus remains in said target.
  • the target is constituted by rhodium, as an isotope precursor, deposited on a copper support.
  • This target is subjected to irradiation with a 14 MeV proton beam for 6 days, which induces a 103 Rh ⁇ 103 Pd reaction and makes it possible to obtain that about 1% of the rhodium 103 is converted into palladium 103.
  • the irradiation is complete, the target is discharged and brought to a shielded enclosure called "hot cell" which is intended to allow the realization of the separation of the isotope of its precursor.
  • the separation procedure described above is used.
  • the target constituted by the copper support and rhodium-palladium mixture in solid form is dissolved with a strong acid solution such as an NH 3 + H 2 SO 4 mixture. This dissolves the copper and keeps rhodium and palladium in the form of precipitates. It is then sufficient to perform at this time a filtration.
  • the separation of palladium from the palladium-rhodium mixture will be obtained by electro-dissolution of the mixture in a hydrochloric acid solution with flow of chlorine to improve the yield (Applied Radiat Isot 38 (2), pp.151-157 (1987).
  • US 5,468,355 discloses in detail a process for producing 13 N oxides comprising a step of bombarding a carbon-based target with a high-energy charged particle beam, so as to generate a layer of 13 N on the surface of the target, then a step of burning the target in the presence of gaseous oxygen so as to extract 13 N oxides from said target.
  • This document also mentions another embodiment for extracting a radio- isotope of a bombarded target, by heating, without combustion of said target.
  • the document thus evokes an embodiment in which a target containing 10 B or 11 B as a precursor is, after bombardment, heated and swept by a gas such as helium to extract the radioisotope 11 C. as much, the document does not detail the implementation of this other form of execution.
  • US 5,987,087 discloses a method for selectively extracting an arsenic-based target, previously irradiated with a charged particle beam, from the selenium-72 radioisotope produced as a result of this irradiation.
  • the target material once irradiated is mixed with a metal reagent, such as stainless steel filings, or aluminum, before undergoing heat treatment.
  • a metal reagent such as stainless steel filings, or aluminum
  • the heat treatment consists in heating in two stages the target once irradiated and then mixed with the metallic reagent.
  • the mixture is heated to a temperature of between 1000 ° C and 1100 ° C.
  • a second heating is carried out at 1300 ° C of the mixture so as to cause the sublimation of selenium-72 which is harvested for example on a cold support.
  • Selenium-72 is then recovered separately.
  • the heat treatment is not done directly on the target but on the target mixed with a metal reagent.
  • the process of this document makes use of a stream of purified inert gas.
  • US Pat. No. 5,987,087 attempts to extract from selenium-72 produced from an arsenic-based target, and the solution it proposes only relate to to a very particular case of precursor / radioisotope.
  • the present invention aims to provide a method and a device for producing radioisotopes which does not have the drawbacks of the state of the art.
  • the present invention aims to provide a solution that reduces the production of radioactive waste.
  • the present invention further aims to provide a method in which the target is not destroyed, and can therefore be reused for a new production of radioisotope.
  • the present invention further aims to provide a radioisotope with a high specific activity.
  • radioisotope and “radioisotope of interest” will be used indifferently to designate the radioisotope that is sought to produce, while the term “precursor” will denote as its name indicates, the element from which one seeks to obtain said radioisotope of interest.
  • the radioisotope of interest is generally obtained by irradiation using a proton beam of a solid target containing the precursor, the radioisotope of interest being produced within of said target, also preferably in solid form.
  • the separation of the radioisotope of interest and the precursor will thus consist of subjecting the solid target to a heat treatment to obtain an effusion reaction, that is to say of thermal separation of the radioisotope of interest.
  • the heat treatment in order to cause the effusion of the radioisotope of interest is therefore carried out in the present invention, directly on the irradiated target, and not on a mixture which would consist of the irradiated target and then mixed with a reagent.
  • a reagent such as stainless steel or aluminum filings, in contrast to the process described in US 5,987,087.
  • the melting temperature of the radioisotope of interest is less than the precursor melting temperature of at least 100 ° C.
  • the precursor therefore remains the pure state that is to say, it can be recovered at the end of the process, without it being necessary for that to perform an additional step of extraction or treatment.
  • said target can be recovered directly without further processing.
  • this feature of the invention allows a certain time saving, while ensuring a better return reuse.
  • the heat treatment used to obtain the effusion of the radioisotope of interest may be any treatment operating by Joule effect.
  • the energy intended for the heat treatment can come from the irradiation by a beam of charged particles such as electrons, by the beam used for the nuclear reaction, by infrared radiation, by laser treatment, by treatment plasma or any other suitable heat treatment.
  • Zn can be zebrased from a Y target by heating the target at a temperature above 900 ° C, from a Zr target's Be by heating the target to a temperature above 1100 ° K, Pd of an Rh target by heating the Rh target to a temperature above 1000 ° C.
  • the effusion velocity of an element also depends on the crystallographic structure of the target. Thus, if during the heating of the target, a recrystallization takes place, there is a decrease in the number of grain boundaries at the crystal and the diffusion of the element can then be done both through the joints and between the joints, which has the effect of affecting the effusion speed of said element.
  • the particle beam can influence the rate of effusion of the radioisotope. Indeed, the effusion rate will be different according to the defects created by this beam within the target, between the surface of the target and the position in the target at which the radioisotope is generated by nuclear reaction. It is thus known that mechanisms referenced in the literature under the abbreviations "RED” (Radiation Enhanced Diffusion) and “RES” (Radiation Enhanced Segregation) and which are linked to the diffusion mechanisms (interstitial, diffusion, ...), or drastically increase the diffusion coefficient, and thus the effusion rate, by creating gaps on the diffusion path, or on the contrary significantly reduce diffusion by creating precipitation sites on the diffusion path.
  • the heat treatment will occur within an effusion chamber separate from the irradiation chamber to obtain said effusion.
  • the collection and condensation step may also be performed within said effusion chamber.
  • this effusion chamber will be provided with means for collecting and condensing said extracted radioisotope.
  • the collection and condensation means may be constituted by a collection substrate such as a ceramic, metal or polymeric support, cold or cooled.
  • a collection substrate such as a ceramic, metal or polymeric support, cold or cooled.
  • this substrate will have low adhesion characteristics.
  • an additional step of separating the radioisotope extracted, collected and condensed on the collection substrate will have to be produce.
  • this separation step may be performed within a separation chamber separate from the effusion chamber.
  • this separation chamber comprises a bath of acid solution in which the collection substrate can be soaked in order to obtain a separation of the radioisotope of said collection substrate. Then, it will be necessary to filter and separate said radioisotope in order to condition it in the desired form.
  • the heat treatment can be carried out directly within the irradiation chamber, for example directly by irradiation with the charged particle beam which has made it possible to transmute the radioisotope.
  • the collection substrate has an interlayer having low adhesion characteristics with the radioisotope.
  • the device according to the invention further comprises means of detaching the radioisotope from said collection substrate.
  • the uncoupling means consist of a separation chamber comprising an acid solution bath in which the collection substrate is placed with the radioisotope.
  • the present invention also relates in particular to the use of said method and device for the production of palladium 103 from rhodium 103.
  • it relates to the reaction 103 Rh 103 Pd by irradiation of a proton beam.
  • metal pairs can of course be envisaged for the implementation of the process (for example the pairs 111 In / 111 Cd , 197 Hg / 197 Au , 95 Tc / 95 Mo , Zn / Y, Be / Zr , Cu / Ni).
  • Figures 1a and 1b schematically describe the various steps of the process for preparing the radioisotope according to a first and a second embodiment of the present invention, respectively.
  • FIGS. 2a and 2b respectively describe the effusion and separation chambers used for carrying out the methods according to the present invention.
  • FIG. 3 describes a second embodiment in which the irradiation and effusion stages can be carried out directly on-line within the irradiation chamber.
  • Figures 4a and 4b schematically describe a particle accelerator that can be used for the implementation of the method.
  • Figure 4a corresponds to a perspective view of this device, while Figure 4b corresponds to a view from above.
  • FIG. 1a schematically describes the various steps of a first embodiment of the method of producing a radioisotope according to the present invention.
  • step A-preparation of the target it is first of all to prepare the target 3 comprising the precursor 1 of the radioisotope 4 (step A-preparation of the target).
  • Rh is deposited on a metal plate 2 which is in this case a copper plate. This is usually done by electrolysis, so as to obtain a deposit of a thickness such that the proton beam used during the irradiation (for example a 14 MeV proton beam) loses at least three quarters of its energy within of the target.
  • other deposition techniques such as evaporation, plasma deposition techniques (DC, radio frequency or microwave) under vacuum or plasma plasma (plasma spraying) can be used.
  • a thickness of 50 microns is sufficient for 14 MeV protons.
  • the target 3 is loaded into a cyclotron and subjected to a proton beam of 14 MeV energy for 6 days (step B-irradiation).
  • the 103 Rh transmutation into 103 Pd occurs at the rate of 0.225 mCi / mAH.
  • a production of 28.8 Ci will be obtained.
  • the amount of 103 Pd (radioisotope 4) harvested corresponds to less than 1% of the initial amount of 103 Rh (precursor 1) present on the target 3.
  • the irradiated target 3 is then discharged and transferred (step C-extraction and transfer) to an effusion chamber 17 as shown in FIG. 2a.
  • This effusion chamber is a shielded enclosure in which effusion is effected (step D).
  • the shedding of a constituent out of an alloy is based on the following physical phenomena.
  • the most volatile component here palladium
  • the volatile component has a lower melting temperature than the other components of the alloy, or a higher partial vaporization pressure for a given temperature.
  • Palladium and rhodium respectively have melting temperatures of 1554.9 ° C and 1964 ° C.
  • the target 3 is heated, for example by means of electric heating, by Joule effect or by induction, of an electron beam, infrared beam, a laser, or a DC plasma or radio-frequency or microwave.
  • the next step then consists in collecting and condensing the palladium 4 extracted from the target 3 on a collection medium 5 (step E) and then separating it and collecting it (step F), for example in the form of PdCl 2 .
  • FIG. 2a describes an effusion chamber 17 used according to the first embodiment of the method of the invention.
  • This is of course a shielded enclosure in which the irradiated target 3 is transferred (step C of FIG. 1a) and which makes it possible to carry out the effusion steps (step D) of the radioisotope 4 out of the target. 3 but also capture and condensation (step E) of said radioisotope 4 extracted.
  • This target 3 is heated preferably under vacuum or in a controlled atmosphere using heat treatment means 18 in order to cause the diffusion of palladium 4 within the target 3 to its surface and its evaporation / sublimation out of it.
  • a temperature of between 800 ° C and 1750 ° C is suitable for causing the shedding of palladium 4 out of the rhodium matrix (target 3).
  • the heat treatment means 18 are in the form of a simple electrical resistance. They must act in a minimum of time and must be very simple to regulate. In addition, they must preserve the target 3 and preserve its integrity to allow its subsequent use for future irradiations.
  • the evacuation and the holding under vacuum of the effusion chamber 17 are provided by a vacuum pump 19.
  • the palladium 4 present in the effusion chamber 17 in gaseous form is captured and condensed (step E of Figure 1a) on a collection medium 5.
  • the collection support 5 is cold or cooled at a temperature below the condensation temperature of palladium 4.
  • Palladium 4 is collected in solid or liquid form.
  • Said substrate 5 is disposed near the target under a protective bell 20.
  • the collection substrate 5 is a cold ceramic or metal support and has poor adhesion. It may for example have a non-adherent interlayer (not shown). For example, soluble polymers or fats can be used to make this interlayer.
  • target 3 After the effusion and collection operation (steps D and E), target 3 still contains substantially the initial amount of rhodium, and it was not affected mechanically or chemically. It can therefore advantageously be reinstalled in the irradiation chamber for a new palladium production campaign (step G).
  • the collection substrate 5 is transferred by means of a transfer system to another enclosure called separation chamber 21 in which the separation step (step F of FIG. 1a) of the radioisotope 4 and the collection substrate 5 is performed.
  • Figure 2b describes such a separation chamber 21 to which the collection substrate is brought.
  • this separation chamber 21 comprises a bath 22 of a solution so as to release 103 Pd (radioisotope 4) into said solution.
  • This separation can be obtained by chemical means, such as dissolution of the interlayer and / or palladium, and / or mechanical means such as stirring.
  • this solution is treated so as to isolate 103 Pd (radioisotope 4) (step F of Figure 1a) which is packaged in small flasks using dose dispensers.
  • the activity of each vial is measured for control, and the product can then be used as a radiochemical product.
  • effusion 17 and separation speakers 21 must be such that they are easily decontaminable, integrable within a shielded enclosure "hot-cell", equipped with a suitable transfer system the target 3, the irradiation chamber 10 to the effusion chamber 17, and the collection substrate 5 of the effusion chamber 17 to the separation chamber 21 and are easy to maintain.
  • the transfer system of the target 3 and the collection substrate 5 must itself be easily removable, for example for verification, and easily decontaminable. It must also be secure.
  • Effusion 17 and separation chamber 21 may be combined into a single enclosure.
  • FIG. 1b schematically describes the various steps of a second embodiment of the process for producing a radioisotope according to the present invention, in which the effusion stage is carried out on-line; ie directly within the irradiation chamber.
  • step A The constitution of the target (step A) is in the same manner as in the first embodiment.
  • a collection substrate 5 is installed in the irradiation chamber. It is therefore not necessary to extract the target 3 to perform the shedding-collection.
  • This device makes it possible to simultaneously perform the irradiation and effusion-collection (steps B, D and E simultaneous).
  • the energy required to heat the target is provided in whole or in part by the accelerated particle beam.
  • the collection substrate 5 is extracted from the irradiation chamber 10.
  • the separation of the deposited palladium (step F) is then carried out in the same manner as in the first embodiment.
  • the target 3 can remain within the irradiation chamber 10.
  • FIG. 3 therefore describes a device that is suitable for implementing the second embodiment of the method of the invention.
  • the irradiation chamber 10 are installed the target 3 as well as the collection substrate 5.
  • a set of vacuum pumps makes it possible to reach gradually the large level of vacuum required within the accelerator.
  • FIG. 24a is a perspective view of this accelerator
  • FIG. 4b is a top view of this same device.
  • the device 7 further comprises a series of auxiliary magnets which correspond to quadrupoles 13 and sextupoles 14 and whose function is to ensure a focusing of the beam.
  • a scanning magnet 16 allows, as its name indicates, to scan the target 3 with the aid of the irradiation beam.
  • the target 3 obtained in the chamber 10 at the end of the beam line of the accelerator 6 charged particles.
  • the accelerator 6 may be constituted by a cyclotron which makes it possible to generate a proton beam having a certain divergence and which is corrected by the presence of the collimators 15.
  • collimators 15 are primarily intended to prevent part of the beam (20%) from striking elements of the beam line and damaging them.
  • these collimators 15 can be removable and themselves coated with a layer of rhodium, so as to take advantage of the beam loss to directly produce 103 Pd (radioisotope 4).
  • the collimators 15 must be able to meet the following requirements: ease of assembly / disassembly and placement in the line, very good cooling of the irradiated surface, ease of transfer to a lead container, ease of disassembly in a hot cell ", Minimum copper substrate mass, minimum rhodium coating surface, reuse for each irradiation of a maximum of components.
  • Target 3 can also be installed directly inside the particle accelerator 6.
  • the target 3 and the collection substrate 5 can be used several times in succession. There is thus an economical process in rhodium, and producing little waste.
  • the target may consist entirely of the isotope precursor, or an alloy comprising this isotope precursor.

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Abstract

The process comprises preparing a target (3) from a precursor of the radio-isotope (1) and an optional metal support (2). The target is irradiated in an irradiation chamber by a beam of accelerated particles to induce transmutation of the precursor into the radio-isotope. The target is then heated to provoke effusion of the radio-isotope (4) outside the target in the form of a gas, which is collected and condensed into a solid or liquid.

Description

Objet de l'inventionObject of the invention

La présente invention se rapporte à un procédé et à un dispositif pour la production de radio-isotopes à partir d'une cible essentiellement constituée d'un précurseur d'isotope que l'on irradie par un faisceau de particules accélérées, le radio-isotope une fois produit étant séparé de son précurseur.The present invention relates to a method and a device for the production of radioisotopes from a target consisting essentially of an isotope precursor which is irradiated by an accelerated particle beam, the radioisotope once produced being separated from its precursor.

Une application particulière de la présente invention concerne la production de palladium 103 à partir de rhodium 103.A particular application of the present invention relates to the production of palladium 103 from rhodium 103.

Etat de la techniqueState of the art

La production habituelle de radio-isotopes s'effectue par bombardement ou irradiation d'une cible essentiellement constituée d'un précurseur d'isotope à l'aide d'un faisceau de particules accélérées.The usual production of radioisotopes is by bombardment or irradiation of a target consisting essentially of an isotope precursor using an accelerated particle beam.

I1 s'y produit une réaction nucléaire qui fait qu'une fraction du précurseur d'isotope présent est transformée en un radio-isotope. Il convient de noter que dans la plupart des cas, le radio-isotope créé est intimement mêlé au matériau précurseur d'isotope constituant la cible et reste de ce fait dans ladite cible.A nuclear reaction occurs which causes a fraction of the isotope precursor present to be converted to a radioisotope. It should be noted that in most cases the created radioisotope is intimately mixed with the isotope precursor material constituting the target and thus remains in said target.

Il convient également de noter qu'habituellement seuls quelques pour cents du précurseur sont transformés en radio-isotopes exploitables.It should also be noted that usually only a few percent of the precursor is transformed into exploitable radioisotopes.

Plusieurs types de procédés ont été proposés pour séparer le radio-isotope de son précurseur. L'un d'entre eux consiste essentiellement en une séparation chimique selon laquelle on dissout totalement la cible par exemple dans un acide fort. On effectue ensuite une filtration et éventuellement une électro-dissolution du radio-isotope et enfin une précipitation de ce dernier.Several types of processes have been proposed for separating the radioisotope from its precursor. One of them essentially consists of a chemical separation according to which the target is totally dissolved, for example in a strong acid. Then a filtration and possibly an electro-dissolution of the radioisotope and finally a precipitation of the latter.

On peut citer à titre d'exemple de cette méthode de séparation chimique, le couple rhodium palladium 103. La cible est constituée par le rhodium, en tant que précurseur d'isotope, déposé sur un support de cuivre. Cette cible est soumise à une irradiation par un faisceau de protons de 14 MeV pendant 6 jours, ce qui induit une réaction 103 Rh → 103 Pd et permet d'obtenir qu'environ 1% du rhodium 103 soit transformé en palladium 103. Une fois l'irradiation terminée, la cible est déchargée et amenée vers une enceinte blindée appelée "hot cell" qui est destinée à permettre la réalisation de la séparation de l'isotope de son précurseur.By way of example of this method of chemical separation, mention may be made of the rhodium palladium pair 103. The target is constituted by rhodium, as an isotope precursor, deposited on a copper support. This target is subjected to irradiation with a 14 MeV proton beam for 6 days, which induces a 103 Rh → 103 Pd reaction and makes it possible to obtain that about 1% of the rhodium 103 is converted into palladium 103. the irradiation is complete, the target is discharged and brought to a shielded enclosure called "hot cell" which is intended to allow the realization of the separation of the isotope of its precursor.

Afin de séparer le rhodium du palladium, on utilise la procédure de séparation décrite ci-dessus. En particulier, on dissout la cible constituée du support cuivre et de mélange rhodium - palladium sous forme solide avec une solution d'acide fort tel qu'un mélange NH3 + H2SO4. Ceci permet de dissoudre le cuivre et de maintenir le rhodium et le palladium sous forme de précipités. Il suffit alors d'effectuer à ce moment une filtration. La séparation du palladium du mélange palladium - rhodium sera obtenue par électro-dissolution du mélange dans une solution d'acide chlorhydrique avec flux de chlore pour améliorer le rendement (Applied Radiat. Isot. 38(2), pp.151-157 (1987)), suivie par une étape de séparation effectuée par exemple par complexation du palladium à l'aide d'alpha-furil dioxine (AFD) afin d'extraire sélectivement le palladium par la méthode d'extraction liquide-liquide (Radiochim. Radioanal. Lett. 48(1), pp.15-19 (1981)). Une dernière précipitation termine le processus pour isoler le palladium 103 du rhodium 103 et le conditionner sous la forme désirée.In order to separate rhodium from palladium, the separation procedure described above is used. In particular, the target constituted by the copper support and rhodium-palladium mixture in solid form is dissolved with a strong acid solution such as an NH 3 + H 2 SO 4 mixture. This dissolves the copper and keeps rhodium and palladium in the form of precipitates. It is then sufficient to perform at this time a filtration. The separation of palladium from the palladium-rhodium mixture will be obtained by electro-dissolution of the mixture in a hydrochloric acid solution with flow of chlorine to improve the yield (Applied Radiat Isot 38 (2), pp.151-157 (1987). )), followed by a separation step carried out for example by complexing the palladium with using alpha-furil dioxin (AFD) to selectively extract palladium by the liquid-liquid extraction method (Radiochim Radioanal Lett 48 (1), pp.15-19 (1981)). A final precipitation completes the process to isolate palladium 103 from rhodium 103 and package it in the desired form.

Il est également possible de provoquer une dissolution chimique du rhodium 103 en vue de récupérer seulement le palladium 103 au moyen d'une solution de NaAuCl4 (Appl. Radiat. Isot. 48(3), pp.327-331 (1997)) et de séparer le rhodium du palladium en utilisant une solution d'α-benzoinoxime (ABO).It is also possible to cause chemical dissolution of rhodium 103 in order to recover only palladium 103 by means of a solution of NaAuCl 4 (Appl Radiat Isot 48 (3), pp. 327-331 (1997)) and to separate rhodium from palladium using a solution of α-benzoinoxime (ABO).

Cependant, on observe tout d'abord, que quelles que soient les méthodes de séparation utilisées, le rendement maximum jamais atteint décrit dans la littérature se situe aux alentours des 90%.However, it is observed first of all, that whatever the separation methods used, the maximum yield never reached described in the literature is around 90%.

En outre, la mise en oeuvre de telles techniques est complexe et il y a génération d'effluents qui peuvent se révéler dangereux et polluants.In addition, the implementation of such techniques is complex and there is generation of effluents that can be dangerous and polluting.

I1 convient également de noter que malheureusement, ce procédé de séparation détruit totalement la cible, et de ce fait le rhodium, qui est un matériau particulièrement onéreux. Par conséquent, la cible ne pourra être réutilisée pour une prochaine irradiation.It should also be noted that unfortunately this separation process completely destroys the target, and thus rhodium, which is a particularly expensive material. Therefore, the target can not be reused for a next irradiation.

En outre, les solutions acides utilisées pour la séparation seront polluées par des déchets radioactifs et nécessiteront une décontamination, ce qui augmente de manière importante le coût du procédé.In addition, the acid solutions used for separation will be polluted by radioactive waste and will require decontamination, which significantly increases the cost of the process.

Enfin, pour effectuer la dernière précipitation, un entraîneur est nécessaire, par exemple le palladium 102, dont l'utilisation réduit l'activité spécifique du palladium 103.Finally, to carry out the last precipitation, a trainer is necessary, for example palladium 102, the use of which reduces the specific activity of palladium 103.

Le document US 5 468 355 décrit en détail un procédé de production d'oxydes de 13N comprenant une étape de bombardement d'une cible à base de carbone avec un faisceau de particules chargées à haute énergie, de manière à générer une couche de 13N à la surface de la cible, puis une étape de combustion de la cible en présence d'oxygène gazeux de manière à extraire de ladite cible les oxydes de 13N. Ce document mentionne également une autre forme d'exécution pour extraire un radio-isotope d'une cible bombardée, par chauffage, sans combustion de ladite cible. Le document évoque ainsi une forme d'exécution dans laquelle une cible contenant du 10B ou 11B comme précurseur est, après bombardement, chauffée et balayée par un gaz tel que de l'hélium pour en extraire le radio-isotope 11C. Pour autant, le document ne détaille pas la mise en oeuvre de cette autre forme d'exécution.US 5,468,355 discloses in detail a process for producing 13 N oxides comprising a step of bombarding a carbon-based target with a high-energy charged particle beam, so as to generate a layer of 13 N on the surface of the target, then a step of burning the target in the presence of gaseous oxygen so as to extract 13 N oxides from said target. This document also mentions another embodiment for extracting a radio- isotope of a bombarded target, by heating, without combustion of said target. The document thus evokes an embodiment in which a target containing 10 B or 11 B as a precursor is, after bombardment, heated and swept by a gas such as helium to extract the radioisotope 11 C. as much, the document does not detail the implementation of this other form of execution.

Le document US 5 987 087 décrit un procédé pour extraire par traitement thermique sélectivement d'une cible à base d'arsenic, préalablement irradiée par un faisceau de particules chargées, le radio-isotope sélénium-72 produit à la suite de cette irradiation. Dans ce procédé, le matériau cible une fois irradié est mélangé à un réactif métallique, tel que de la limaille d'acier inoxydable, ou d'aluminium, avant de subir un traitement thermique. L'obtention de ce mélange permet d'obtenir une sublimation différenciée de l'arsenic (précurseur) et du sélénium-72 (radio-isotope d'intérêt). Le traitement thermique consiste à chauffer en deux étapes la cible une fois irradiée puis mélangée au réactif métallique. Dans la première étape, on chauffe le mélange à une température comprise entre 1000°C et 1100°C. Dans une seconde étape, on effectue un second chauffage à 1300°C du mélange de manière à provoquer la sublimation du sélénium-72 qui est récolté par exemple sur un support froid. Le sélénium-72 est ensuite récupéré séparément. En d'autres termes, dans ce document, il existe une étape intermédiaire de traitement entre l'irradiation de la cible et l'étape de traitement thermique en vue de séparer le radio-isotope d'intérêt qu'est le sélénium-72. Le traitement thermique ne se fait pas directement sur la cible mais sur la cible mélangée à un réactif métallique. De plus, le procédé de ce document fait usage d'un flux d'un gaz inerte purifié. Par ailleurs, le problème que cherche à résoudre le document US 5 987 087 qui est celui d'extraire du sélénium-72 produit à partir d'une cible à base d'arsenic, et la solution qu'il propose, ne se rapportent qu'à un cas de précurseur/radio-isotope bien particulier.US 5,987,087 discloses a method for selectively extracting an arsenic-based target, previously irradiated with a charged particle beam, from the selenium-72 radioisotope produced as a result of this irradiation. In this process, the target material once irradiated is mixed with a metal reagent, such as stainless steel filings, or aluminum, before undergoing heat treatment. Obtaining this mixture makes it possible to obtain a differentiated sublimation of arsenic (precursor) and selenium-72 (radioisotope of interest). The heat treatment consists in heating in two stages the target once irradiated and then mixed with the metallic reagent. In the first step, the mixture is heated to a temperature of between 1000 ° C and 1100 ° C. In a second step, a second heating is carried out at 1300 ° C of the mixture so as to cause the sublimation of selenium-72 which is harvested for example on a cold support. Selenium-72 is then recovered separately. In other words, in this document, there is an intermediate step of treatment between the irradiation of the target and the heat treatment step in order to separate the radioisotope of interest that is selenium-72. The heat treatment is not done directly on the target but on the target mixed with a metal reagent. In addition, the process of this document makes use of a stream of purified inert gas. Moreover, the problem that US Pat. No. 5,987,087 attempts to extract from selenium-72 produced from an arsenic-based target, and the solution it proposes, only relate to to a very particular case of precursor / radioisotope.

Buts de l'inventionGoals of the invention

La présente invention vise à fournir un procédé et un dispositif de production de radio-isotopes qui ne présente pas les inconvénients de l'état de la technique.The present invention aims to provide a method and a device for producing radioisotopes which does not have the drawbacks of the state of the art.

La présente invention vise à fournir une solution qui permet de réduire la production de déchets radioactifs.The present invention aims to provide a solution that reduces the production of radioactive waste.

La présente invention vise en outre à fournir un procédé dans lequel la cible n'est pas détruite, et peut donc être réutilisée pour une nouvelle production de radio-isotope.The present invention further aims to provide a method in which the target is not destroyed, and can therefore be reused for a new production of radioisotope.

La présente invention vise en outre à permettre d'obtenir un radio-isotope avec une activité spécifique élevée.The present invention further aims to provide a radioisotope with a high specific activity.

Principaux éléments caractéristiques de l'inventionMain characteristic elements of the invention

La présente invention se rapporte à un procédé de production d'un radio-isotope d'intérêt à partir d'une cible comportant un précurseur dudit radio-isotope, à l'aide d'un faisceau de particules accélérées, ledit procédé comprenant les étapes suivantes :

  • préparation d'une cible solide comprenant le précurseur du radio-isotope,
  • irradiation, au sein d'une chambre d'irradiation, de ladite cible solide par un faisceau de particules accélérées, en vue d'induire la transmutation du précurseur en le radio-isotope,
  • chauffage de ladite cible solide en vue de provoquer l'effusion du radio-isotope hors de la cible solide,
  • collecte dudit radio-isotope extrait sous forme gazeuse et condensation dudit radio-isotope sous forme solide ou liquide.
The present invention relates to a method for producing a radioisotope of interest from a target comprising a precursor of said radioisotope, at using an accelerated particle beam, said method comprising the following steps:
  • preparing a solid target comprising the precursor of the radioisotope,
  • irradiating, within an irradiation chamber, said solid target with an accelerated particle beam, in order to induce transmutation of the precursor into the radioisotope,
  • heating said solid target to cause the radioisotope to be released from the solid target,
  • collecting said radioisotope extracted in gaseous form and condensing said radioisotope in solid or liquid form.

On notera que dans la description qui suit, les expressions « radio-isotope » et « radio-isotope d'intérêt » seront indifféremment utilisées pour désigner le radio-isotope que l'on cherche à produire, tandis que le terme « précurseur » désignera, comme son nom l'indique, l'élément à partir duquel on cherche à obtenir ledit radio-isotope d'intérêt.Note that in the following description, the terms "radioisotope" and "radioisotope of interest" will be used indifferently to designate the radioisotope that is sought to produce, while the term "precursor" will denote as its name indicates, the element from which one seeks to obtain said radioisotope of interest.

Dans le procédé selon l'invention, le radio-isotope d'intérêt est généralement obtenu par irradiation à l'aide d'un faisceau de protons d'une cible solide contenant le précurseur, le radio-isotope d'intérêt étant produit au sein de ladite cible, également de préférence sous forme solide.In the process according to the invention, the radioisotope of interest is generally obtained by irradiation using a proton beam of a solid target containing the precursor, the radioisotope of interest being produced within of said target, also preferably in solid form.

La cible, dans la présente invention, comprend donc :

  • avant irradiation : le précurseur, éventuellement lié à un support métallique ;
  • après irradiation: le précurseur, éventuellement lié à un support métallique, et le radio-isotope d'intérêt.
The target in the present invention therefore comprises:
  • before irradiation: the precursor, optionally bonded to a metal support;
  • after irradiation: the precursor, optionally bonded to a metal support, and the radioisotope of interest.

La séparation du radio-isotope d'intérêt et du précurseur consistera donc à soumettre la cible solide à un traitement thermique pour obtenir une réaction d'effusion, c'est-à-dire de séparation thermique du radio-isotope d'intérêt.The separation of the radioisotope of interest and the precursor will thus consist of subjecting the solid target to a heat treatment to obtain an effusion reaction, that is to say of thermal separation of the radioisotope of interest.

Le traitement thermique en vue de provoquer l'effusion du radio-isotope d'intérêt, est donc réalisé dans la présente invention, directement sur la cible irradiée, et non pas sur un mélange qui serait constitué par la cible irradiée puis mélangée à un réactif métallique tel que de la limaille d'acier inoxydable ou d'aluminium, contrairement au procédé décrit dans le document US 5 987 087. En d'autres termes, dans le procédé selon l'invention, il n'est pas nécessaire de soumettre la cible après irradiation à un traitement avant de la chauffer en vue d'extraire le radio-isotope d'intérêt.The heat treatment in order to cause the effusion of the radioisotope of interest is therefore carried out in the present invention, directly on the irradiated target, and not on a mixture which would consist of the irradiated target and then mixed with a reagent. such as stainless steel or aluminum filings, in contrast to the process described in US 5,987,087. In other words, in the process according to the invention, it is not necessary to submit the target after irradiation to a treatment before heating it to extract the radioisotope of interest.

Dans ce but, il doit s'agir de couples précurseur/radio-isotope d'intérêt qui présentent des températures de fusion et d'ébullition relativement différentes l'une de l'autre, de telle sorte que le traitement d'effusion permette d'obtenir une diffusion du radio-isotope au sein même de la cible, son extraction ou échappement par évaporation et sublimation, tandis que le précurseur de la cible reste présent au sein de ladite cible de préférence sous forme solide. On doit donc comprendre que dans la présente invention, la notion d'effusion se réfère à un phénomène physique plus « large » que la sublimation et doit s'entendre comme comprenant le phénomène de sublimation.For this purpose, they must be precursor / radioisotope couples of interest which have relatively different melting and boiling temperatures, so that the effusion treatment allows to obtain a diffusion of the radioisotope within the target itself, its extraction or escape by evaporation and sublimation, while the precursor of the target remains present in said target preferably in solid form. It must therefore be understood that in the present invention the notion of effusion refers to a physical phenomenon that is "wider" than sublimation and must be understood to include the phenomenon of sublimation.

Plus précisément, la température de fusion du radio-isotope d'intérêt est inférieure à la température de fusion du précurseur d'au moins 100 °C.Specifically, the melting temperature of the radioisotope of interest is less than the precursor melting temperature of at least 100 ° C.

Il importe par ailleurs de souligner que, dans la présente invention, le précurseur reste donc à l'état pur c'est-à-dire qu'on peut le récupérer en fin de procédé, sans qu'il soit nécessaire pour cela d'effectuer une étape supplémentaire d'extraction ou de traitement. En d'autres termes, une fois que le radio-isotope a été extrait de la cible, on peut récupérer directement ladite cible sans traitement supplémentaire. Dans le cas où on souhaite par la suite réutiliser ledit précurseur, cette caractéristique de l'invention permet un gain de temps certain, tout en assurant un meilleur rendement de réutilisation.It is also important to emphasize that, in the present invention, the precursor therefore remains the pure state that is to say, it can be recovered at the end of the process, without it being necessary for that to perform an additional step of extraction or treatment. In other words, once the radioisotope has been extracted from the target, said target can be recovered directly without further processing. In the case where it is subsequently desired to reuse said precursor, this feature of the invention allows a certain time saving, while ensuring a better return reuse.

Le traitement thermique mis en oeuvre pour obtenir l'effusion du radio-isotope d'intérêt peut être tout traitement fonctionnant par effet Joule.The heat treatment used to obtain the effusion of the radioisotope of interest may be any treatment operating by Joule effect.

A titre d'exemple, l'énergie destinée au traitement thermique peut provenir de l'irradiation par un faisceau de particules chargées telles des électrons , par le faisceau utilisé pour la réaction nucléaire, par rayonnement infrarouge, par un traitement au laser, par traitement plasma ou tout autre traitement thermique adéquat.By way of example, the energy intended for the heat treatment can come from the irradiation by a beam of charged particles such as electrons, by the beam used for the nuclear reaction, by infrared radiation, by laser treatment, by treatment plasma or any other suitable heat treatment.

A titre d'exemple, un chauffage sous vide ou sous atmosphère inerte contrôlée permettra d'obtenir rapidement l'effet d'effusion désiré.For example, heating under vacuum or under controlled inert atmosphere will quickly obtain the desired effusion effect.

On doit donc comprendre que dans la présente invention, on ne fait pas circuler de gaz tel que l'oxygène pendant le traitement thermique que l'on fait subir à la cible irradiée.It is therefore to be understood that in the present invention, no gas such as oxygen is circulated during the heat treatment of the irradiated target.

D'une manière générale, il existe une relation entre la vitesse d'effusion d'un élément contenu dans une cible chauffée et son coefficient de diffusion, dans la mesure un certain nombre de paramètres qui déterminent la vitesse d'effusion influencent également le coefficient de diffusion. Parmi les paramètres déterminant la vitesse d'effusion, on trouve :

  • la température de fusion dudit élément par rapport à la cible;
  • la tension de vapeur de l'élément de l'élément diffusant ;
  • l'énergie d'activation de la diffusion ;
  • la nature de la cible (métal ou céramique, par exemple) ;
  • et la taille de l'élément diffusant, plus précisément son rayon ionique.
In general, there is a relationship between the effusion velocity of an element contained in a heated target and its diffusion coefficient, since a number of parameters which determine the effusion velocity also influence the coefficient. of diffusion. Among the parameters determining the effusion speed, we find:
  • the melting temperature of said element relative to the target;
  • the vapor pressure of the element of the diffusing element;
  • the activation energy of the diffusion;
  • the nature of the target (metal or ceramic, for example);
  • and the size of the scattering element, more precisely its ionic radius.

Ainsi, on peut séparer par effusion du Zn d'une cible d'Y en chauffant la cible à une température supérieure à 900°C, du Be d'une cible de Zr en chauffant la cible à une température supérieure à 1100°K, du Pd d'une cible Rh en chauffant la cible de Rh à une température supérieure à 1000°C.Thus, Zn can be zebrased from a Y target by heating the target at a temperature above 900 ° C, from a Zr target's Be by heating the target to a temperature above 1100 ° K, Pd of an Rh target by heating the Rh target to a temperature above 1000 ° C.

Pour résumer, on constate que la vitesse d'effusion d'un élément (radio-isotope) est d'autant plus importante que son rayon ionique est petit : l'effusion à partir d'une cible de tantale est ainsi deux fois plus rapide pour du berillium que pour du barium. On notera également que la vitesse d'effusion d'un élément croît avec la température selon une loi exponentielle.To summarize, we find that the effusion speed of an element (radioisotope) is all the more important that its ionic radius is small: the effusion from a tantalum target is thus twice as fast for berillium than for barium. It will also be noted that the effusion velocity of an element increases with the temperature according to an exponential law.

La vitesse d'effusion d'un élément (radioisotope) dépend également de la structure cristallographique de la cible. Ainsi, si lors du chauffage de la cible, une recristallisation a lieu, il y a une diminution du nombre de joints de grains au niveau du cristal et la diffusion de l'élément peut alors se faire aussi bien à travers les joints qu'entre les joints, ce qui a pour conséquence d'affecter la vitesse d'effusion dudit élément.The effusion velocity of an element (radioisotope) also depends on the crystallographic structure of the target. Thus, if during the heating of the target, a recrystallization takes place, there is a decrease in the number of grain boundaries at the crystal and the diffusion of the element can then be done both through the joints and between the joints, which has the effect of affecting the effusion speed of said element.

On peut enfin noter que le faisceau de particules peut influencer la vitesse d'effusion du radio-isotope. En effet, la vitesse d'effusion sera différente selon les défauts créés par ce faisceau au sein de la cible, entre la surface de la cible et la position dans la cible au niveau de laquelle le radioisotope est généré par réaction nucléaire. Il est ainsi connu que des mécanismes référencés dans la littérature sous les abréviations « RED » (Radiation Enhanced Diffusion) et « RES » (Radiation Enhanced Segregation) et qui sont liés aux mécanismes de diffusion (intersticielle, diffusion, ...), soit augmentent de façon drastique le coefficient de diffusion, et donc la vitesse d'effusion, par création de mouvements de lacunes sur le chemin de diffusion, ou au contraire réduisent considérablement la diffusion par création de sites de précipitation sur le chemin de diffusion.Finally, it can be noted that the particle beam can influence the rate of effusion of the radioisotope. Indeed, the effusion rate will be different according to the defects created by this beam within the target, between the surface of the target and the position in the target at which the radioisotope is generated by nuclear reaction. It is thus known that mechanisms referenced in the literature under the abbreviations "RED" (Radiation Enhanced Diffusion) and "RES" (Radiation Enhanced Segregation) and which are linked to the diffusion mechanisms (interstitial, diffusion, ...), or drastically increase the diffusion coefficient, and thus the effusion rate, by creating gaps on the diffusion path, or on the contrary significantly reduce diffusion by creating precipitation sites on the diffusion path.

Selon une première forme d'exécution de la présente invention, le traitement thermique se produira au sein d'une enceinte d'effusion distincte de la chambre d'irradiation en vue d'obtenir ladite effusion.According to a first embodiment of the present invention, the heat treatment will occur within an effusion chamber separate from the irradiation chamber to obtain said effusion.

Selon une forme d'exécution encore préférée, l'étape de collecte et de condensation pourra s'effectuer également au sein de ladite enceinte d'effusion.According to a still preferred embodiment, the collection and condensation step may also be performed within said effusion chamber.

Dans ce but, et de manière particulièrement avantageuse, cette enceinte d'effusion sera pourvue de moyens de collecte et de condensation dudit radio-isotope extrait.For this purpose, and particularly advantageously, this effusion chamber will be provided with means for collecting and condensing said extracted radioisotope.

Les moyens de collecte et de condensation peuvent être constitués par un substrat de collection tel un support céramique, métallique ou polymérique, froid ou refroidi. De préférence, ce substrat présentera de faibles caractéristiques d'adhérence.The collection and condensation means may be constituted by a collection substrate such as a ceramic, metal or polymeric support, cold or cooled. Preferably, this substrate will have low adhesion characteristics.

Selon cette forme d'exécution, une étape supplémentaire de séparation du radio-isotope extrait, collecté et condensé sur le substrat de collection devra se produire. Éventuellement, cette étape de séparation pourra être effectuée au sein d'une enceinte de séparation distincte de l'enceinte d'effusion. Avantageusement, cette enceinte de séparation comprend un bain de solution acide dans laquelle on peut tremper le substrat de collection en vue d'obtenir une désolidarisation du radio-isotope dudit substrat de collection. Ensuite, il sera nécessaire de filtrer et séparer ledit radio-isotope en vue de le conditionner sous la forme désirée.According to this embodiment, an additional step of separating the radioisotope extracted, collected and condensed on the collection substrate will have to be produce. Optionally, this separation step may be performed within a separation chamber separate from the effusion chamber. Advantageously, this separation chamber comprises a bath of acid solution in which the collection substrate can be soaked in order to obtain a separation of the radioisotope of said collection substrate. Then, it will be necessary to filter and separate said radioisotope in order to condition it in the desired form.

Selon une autre forme d'exécution, le traitement thermique peut s'effectuer directement au sein de la chambre d'irradiation, par exemple directement par irradiation par le faisceau de particules chargées qui a permis de réaliser la transmutation du radio-isotope.According to another embodiment, the heat treatment can be carried out directly within the irradiation chamber, for example directly by irradiation with the charged particle beam which has made it possible to transmute the radioisotope.

Un autre objet de l'invention concerne un dispositif pour la mise en oeuvre du procédé de production d'un radio-isotope, ledit dispositif comprenant les moyens suivants:

  • des moyens d'irradiation d'une cible solide comportant un précurseur d'isotope en vue d'induire une transmutation du précurseur en le radio-isotope,
  • des moyens de chauffage en vue de provoquer l'effusion du radio-isotope au sein de ladite cible solide,
  • des moyens de collecte et de condensation du radio-isotope extrait.
Another subject of the invention relates to a device for implementing the method for producing a radioisotope, said device comprising the following means:
  • means for irradiating a solid target comprising an isotope precursor in order to induce transmutation of the precursor into the radioisotope,
  • heating means for causing effusion of the radioisotope within said solid target,
  • means for collecting and condensing the extracted radioisotope.

constitués par un substrat de collection froid présents au sein de la chambre d'irradiation enceinte d'éffusion.constituted by a cold collection substrate present within the irradiation chamber irradiation chamber.

De préférence, le substrat de collection présente une inter-couche présentant de faibles caractéristiques d'adhérence avec le radio-isotope.Preferably, the collection substrate has an interlayer having low adhesion characteristics with the radioisotope.

De préférence, le dispositif selon l'invention comprend en outre des moyens de désolidarisation du radio-isotope dudit substrat de collection.Preferably, the device according to the invention further comprises means of detaching the radioisotope from said collection substrate.

De manière avantageuse, les moyens de désolidarisation sont constitués par une enceinte de séparation comprenant un bain de solution acide dans laquelle est disposé le substrat de collection avec le radio-isotope.Advantageously, the uncoupling means consist of a separation chamber comprising an acid solution bath in which the collection substrate is placed with the radioisotope.

La présente invention se rapporte également en particulier à l'utilisation dudit procédé et dudit dispositif pour la production de palladium 103 à partir de rhodium 103. En d'autres termes, elle concerne la réaction 103Rh

Figure imgb0001
103Pd par irradiation d'un faisceau de protons.The present invention also relates in particular to the use of said method and device for the production of palladium 103 from rhodium 103. In other words, it relates to the reaction 103 Rh
Figure imgb0001
103 Pd by irradiation of a proton beam.

D'autres exemples de couples de métaux peuvent être bien entendu envisagés pour la mise en oeuvre du procédé (par exemple les couples 111In/111Cd, 197Hg/197Au, 95Tc/95Mo, Zn/Y, Be/Zr, Cu/Ni).Other examples of metal pairs can of course be envisaged for the implementation of the process (for example the pairs 111 In / 111 Cd , 197 Hg / 197 Au , 95 Tc / 95 Mo , Zn / Y, Be / Zr , Cu / Ni).

Brève description des figuresBrief description of the figures

Les figure 1a et 1b décrivent de manière schématique les diverses étapes du procédé de préparation du radio-isotope selon une première et une seconde forme d'exécution de la présente invention, respectivement.Figures 1a and 1b schematically describe the various steps of the process for preparing the radioisotope according to a first and a second embodiment of the present invention, respectively.

Les figures 2a et 2b décrivent respectivement les enceintes d'effusion et de séparation utilisées pour la mise en oeuvre des procédés selon la présente invention.FIGS. 2a and 2b respectively describe the effusion and separation chambers used for carrying out the methods according to the present invention.

La figure 3 décrit une seconde forme d'exécution dans laquelle les étapes d'irradiation et d'effusion peuvent être effectuées directement on-line au sein de la chambre d'irradiation.FIG. 3 describes a second embodiment in which the irradiation and effusion stages can be carried out directly on-line within the irradiation chamber.

Les figures 4a et 4b décrivent de manière schématique un accélérateur de particules qui peut être utilisé pour la mise en oeuvre du procédé. La figure 4a correspond à une vue en perspective de ce dispositif, tandis que la figure 4b correspond à une vue de dessus.Figures 4a and 4b schematically describe a particle accelerator that can be used for the implementation of the method. Figure 4a corresponds to a perspective view of this device, while Figure 4b corresponds to a view from above.

Description de plusieurs formes d'exécution préférées de l'inventionDescription of several preferred embodiments of the invention

La figure la décrit de manière schématique les diverses étapes d'une première forme d'exécution du procédé de production d'un radio-isotope selon la présente invention. On se réfère à la préparation du radio-isotope 103Pd, référencé 4, à partir d'une cible 3 comportant du rhodium 103Rh, précurseur d'isotope, référencé 1, par irradiation par un faisceau de protons.Figure 1a schematically describes the various steps of a first embodiment of the method of producing a radioisotope according to the present invention. Reference is made to the preparation of the radioisotope 103 Pd, referenced 4, from a target 3 comprising Rhodium 103 Rh, an isotope precursor, referenced 1, by irradiation with a proton beam.

Au départ, il s'agit tout d'abord de préparer la cible 3 comportant le précurseur 1 du radio-isotope 4 (étape A-préparation de la cible). Pour ce faire, on effectue un dépôt de Rh sur une plaque métallique 2 qui est dans le présent cas une plaque en cuivre. Ceci se fait habituellement par électrolyse, de manière à obtenir un dépôt d'une épaisseur telle que le faisceau de protons utilisé pendant l'irradiation (par exemple un faisceau de protons de 14 MeV) perde au moins les trois quarts de son énergie au sein de la cible. Cependant, d'autres techniques de dépôts comme l'évaporation, les techniques de dépôts par plasma (courant continu (DC), radiofréquence ou micro-ondes) sous vide ou plasma atmosphérique (plasma spraying) peuvent être utilisées.Initially, it is first of all to prepare the target 3 comprising the precursor 1 of the radioisotope 4 (step A-preparation of the target). To do this, Rh is deposited on a metal plate 2 which is in this case a copper plate. This is usually done by electrolysis, so as to obtain a deposit of a thickness such that the proton beam used during the irradiation (for example a 14 MeV proton beam) loses at least three quarters of its energy within of the target. However, other deposition techniques such as evaporation, plasma deposition techniques (DC, radio frequency or microwave) under vacuum or plasma plasma (plasma spraying) can be used.

Dans le cas d'une cible 3 inclinée à 10 ° par rapport à la direction du faisceau, une épaisseur de 50 µm suffit pour des protons de 14 MeV.In the case of a target 3 inclined at 10 ° relative to the direction of the beam, a thickness of 50 microns is sufficient for 14 MeV protons.

Une fois la cible 3 réalisée, celle-ci est chargée dans un cyclotron et soumise à un faisceau de protons d'une énergie de 14 MeV pendant 6 jours (étape B-irradiation). La transmutation du 103Rh en 103Pd s'effectue au taux de 0,225 mCi/mAH. Au terme de 144 heures, on obtiendra, pour un courant de 1 mA continu, et en tenant compte de la décroissance, une production de 28,8 Ci.Once the target 3 is made, it is loaded into a cyclotron and subjected to a proton beam of 14 MeV energy for 6 days (step B-irradiation). The 103 Rh transmutation into 103 Pd occurs at the rate of 0.225 mCi / mAH. At the end of 144 hours, for a current of 1 mA continuous, and taking into account the decay, a production of 28.8 Ci will be obtained.

Il convient de noter que la quantité de 103Pd (radio-isotope 4) récoltée correspond à moins de 1 % de la quantité initiale de 103Rh (précurseur 1) présente sur la cible 3.It should be noted that the amount of 103 Pd (radioisotope 4) harvested corresponds to less than 1% of the initial amount of 103 Rh (precursor 1) present on the target 3.

Dans cette première forme d'exécution de l'invention, il convient de maintenir la température de la cible 3 à tout moment inférieure à la température d'effusion du palladium au sein du rhodium. S'il n'en était pas ainsi, le palladium sortirait de la cible, et se condenserait sur les parois environnantes.In this first embodiment of the invention, it is necessary to maintain the temperature of the target 3 at any time below the effusion temperature of the palladium within the rhodium. If it were not so, the palladium would come out of the target and condense on the surrounding walls.

La cible 3 irradiée est alors déchargée et transférée (étape C-extraction et transfert) vers une enceinte d'effusion 17 telle que représentée à la fig. 2a. Cette enceinte d'effusion est une enceinte blindée dans laquelle est effectuée l'effusion (étape D).The irradiated target 3 is then discharged and transferred (step C-extraction and transfer) to an effusion chamber 17 as shown in FIG. 2a. This effusion chamber is a shielded enclosure in which effusion is effected (step D).

L'effusion d'un constituant hors d'un alliage (en dehors de cet alliage) est basée sur les phénomènes physiques suivants. Le constituant le plus volatil (ici le palladium) passe en phase gazeuse, à partir de la surface, ce qui entraîne une différence de concentration en constituant volatil entre la surface et l'intérieur de la cible. Un flux de diffusion du constituant volatil, de l'intérieur de la cible, vers la surface, prend alors naissance. L'évaporation du constituant volatil se poursuit, et réduit la concentration en constituant volatil au sein de la cible. Finalement, la vapeur du constituant volatil est condensée et recueillie sur une surface froide.The shedding of a constituent out of an alloy (apart from this alloy) is based on the following physical phenomena. The most volatile component (here palladium) passes into the gas phase, from the surface, resulting in a difference in concentration of volatile component between the surface and the interior of the target. A diffusion flux of the volatile component, from the inside of the target, towards the surface, then takes birth. Evaporation of the volatile component continues, and reduces the volatile component concentration within the target. Finally, the vapor of the volatile component is condensed and collected on a cold surface.

On notera qu'il est nécessaire que le constituant volatil ait une température de fusion inférieure à celle des autres constituants de l'alliage, ou une pression partielle de vaporisation supérieure pour une température donnée. Le palladium et le rhodium ont respectivement des températures de fusion de 1554.9°C et 1964°C.Note that it is necessary that the volatile component has a lower melting temperature than the other components of the alloy, or a higher partial vaporization pressure for a given temperature. Palladium and rhodium respectively have melting temperatures of 1554.9 ° C and 1964 ° C.

Au sein de l'enceinte d'effusion 17, on chauffe la cible 3 par exemple au moyen d'un chauffage électrique, par effet Joule ou par induction, d'un faisceau d'électrons, d'infrarouges, d'un laser, ou d'un plasma DC ou radio-fréquence ou micro-onde.Within the effusion chamber 17, the target 3 is heated, for example by means of electric heating, by Joule effect or by induction, of an electron beam, infrared beam, a laser, or a DC plasma or radio-frequency or microwave.

L'étape suivante consiste ensuite à collecter et condenser le palladium 4 extrait de la cible 3 sur un support de collection 5 (étape E) pour ensuite le séparer et le recueillir (étape F), par exemple sous forme de PdCl2 .The next step then consists in collecting and condensing the palladium 4 extracted from the target 3 on a collection medium 5 (step E) and then separating it and collecting it (step F), for example in the form of PdCl 2 .

La figure 2a décrit une enceinte d'effusion 17 utilisée selon la première forme d'exécution du procédé de l'invention. Il s'agit bien sûr d'une enceinte blindée dans laquelle la cible 3 irradiée est transférée (étape C de la figure 1a) et qui permet de réaliser les étapes d'effusion (étape D) du radio-isotope 4 hors de la cible 3 mais également de captation et condensation (étape E) dudit radio-isotope 4 extrait.FIG. 2a describes an effusion chamber 17 used according to the first embodiment of the method of the invention. This is of course a shielded enclosure in which the irradiated target 3 is transferred (step C of FIG. 1a) and which makes it possible to carry out the effusion steps (step D) of the radioisotope 4 out of the target. 3 but also capture and condensation (step E) of said radioisotope 4 extracted.

Cette cible 3 est chauffée de préférence sous vide ou sous atmosphère contrôlée à l'aide de moyens de traitement thermique 18 en vue de provoquer la diffusion du palladium 4 au sein de la cible 3 jusqu'à sa surface et son évaporation / sublimation hors de celle-ci. Une température comprise entre 800°C et 1750°C convient pour provoquer l'effusion du palladium 4 hors de la matrice de rhodium (cible 3).This target 3 is heated preferably under vacuum or in a controlled atmosphere using heat treatment means 18 in order to cause the diffusion of palladium 4 within the target 3 to its surface and its evaporation / sublimation out of it. A temperature of between 800 ° C and 1750 ° C is suitable for causing the shedding of palladium 4 out of the rhodium matrix (target 3).

Avantageusement, les moyens de traitement thermique 18 se présentent sous la forme d'une simple résistance électrique. Ils doivent agir en un minimum de temps et doivent être très simples à réguler. En outre, ils doivent permettre de préserver la cible 3 et d'en sauver l'intégrité afin de permettre son utilisation ultérieure pour de prochaines irradiations.Advantageously, the heat treatment means 18 are in the form of a simple electrical resistance. They must act in a minimum of time and must be very simple to regulate. In addition, they must preserve the target 3 and preserve its integrity to allow its subsequent use for future irradiations.

La mise sous vide et le maintien sous vide de l'enceinte d'effusion 17 sont assurés par une pompe à vide 19.The evacuation and the holding under vacuum of the effusion chamber 17 are provided by a vacuum pump 19.

Le palladium 4 présent au sein de la l'enceinte d'effusion 17 sous forme gazeuse est capté et condensé (étape E de la figure 1a) sur un support 5 de collection. Le support de collection 5 est froid ou refroidi, à une température inférieure à la température de condensation du palladium 4. Le palladium 4 est recueilli sous forme solide ou liquide.The palladium 4 present in the effusion chamber 17 in gaseous form is captured and condensed (step E of Figure 1a) on a collection medium 5. The collection support 5 is cold or cooled at a temperature below the condensation temperature of palladium 4. Palladium 4 is collected in solid or liquid form.

Ledit substrat 5 est disposé à proximité de la cible sous une cloche de protection 20.Said substrate 5 is disposed near the target under a protective bell 20.

De manière particulièrement avantageuse, le substrat de collection 5 est un support froid en céramique ou en métal et il présente une mauvaise adhérence. Il peut par exemple présenter une intercouche non adhérente (non représentée). A titre d'exemple, des polymères solubles ou des graisses peuvent être utilisés pour réaliser cette intercouche.Particularly advantageously, the collection substrate 5 is a cold ceramic or metal support and has poor adhesion. It may for example have a non-adherent interlayer (not shown). For example, soluble polymers or fats can be used to make this interlayer.

A l'issue de l'opération d'effusion et de collecte (étapes D et E), la cible 3 contient encore pratiquement la quantité initiale de rhodium, et elle n'a pas été affectée mécaniquement ou chimiquement. Elle peut donc avantageusement être réinstallée dans la chambre d'irradiation, pour une nouvelle campagne de production de palladium (étape G).After the effusion and collection operation (steps D and E), target 3 still contains substantially the initial amount of rhodium, and it was not affected mechanically or chemically. It can therefore advantageously be reinstalled in the irradiation chamber for a new palladium production campaign (step G).

Ensuite, le substrat 5 de collection est transféré à l'aide d'un système de transfert vers une autre enceinte appelée enceinte de séparation 21 dans laquelle l'étape de séparation (étape F de la figure 1a) du radio-isotope 4 et du substrat de collection 5 est effectuée. La figure 2b décrit une telle enceinte de séparation 21 vers laquelle le substrat de collection est amené.Then, the collection substrate 5 is transferred by means of a transfer system to another enclosure called separation chamber 21 in which the separation step (step F of FIG. 1a) of the radioisotope 4 and the collection substrate 5 is performed. Figure 2b describes such a separation chamber 21 to which the collection substrate is brought.

De manière avantageuse, cette enceinte de séparation 21 comprend un bain 22 d'une solution de manière à libérer le 103Pd (radio-isotope 4) dans ladite solution. Cette séparation peut être obtenue par des moyens chimiques, tels qu'une dissolution de l'intercouche et/ou du palladium, et/ou des moyens mécaniques tels qu'une agitation.Advantageously, this separation chamber 21 comprises a bath 22 of a solution so as to release 103 Pd (radioisotope 4) into said solution. This separation can be obtained by chemical means, such as dissolution of the interlayer and / or palladium, and / or mechanical means such as stirring.

Ensuite, cette solution est traitée de manière à isoler le 103Pd (radio-isotope 4) (étape F de la figure 1a) qui est conditionné dans de petites fioles à l'aide de distributeurs de doses (« doses dispenser »). L'activité de chaque fiole est mesurée pour contrôle, et le produit peut ensuite être utilisé en tant que produit radio-chimique.Then, this solution is treated so as to isolate 103 Pd (radioisotope 4) (step F of Figure 1a) which is packaged in small flasks using dose dispensers. The activity of each vial is measured for control, and the product can then be used as a radiochemical product.

Il convient de noter que les différents éléments des enceintes d'effusion 17 et de séparation 21 doivent être tels qu'ils soient facilement décontaminables, intégrables au sein d'une enceinte blindée "hot-cell", équipés d'un système de transfert adéquat de la cible 3, de la chambre d'irradiation 10 vers l'enceinte d'effusion 17, et du substrat de collection 5 de l'enceinte d'effusion 17 vers l'enceinte de séparation 21 et soient faciles d'entretien.It should be noted that the different elements of effusion 17 and separation speakers 21 must be such that they are easily decontaminable, integrable within a shielded enclosure "hot-cell", equipped with a suitable transfer system the target 3, the irradiation chamber 10 to the effusion chamber 17, and the collection substrate 5 of the effusion chamber 17 to the separation chamber 21 and are easy to maintain.

Le système de transfert de la cible 3 et du substrat de collection 5 doit être lui-même facilement démontable, par exemple en vue d'une vérification, et facilement décontaminable. Il doit en outre être sécurisé.The transfer system of the target 3 and the collection substrate 5 must itself be easily removable, for example for verification, and easily decontaminable. It must also be secure.

L'enceinte d'effusion 17 et de séparation 21 peuvent être combinées en une seule et unique enceinte.Effusion 17 and separation chamber 21 may be combined into a single enclosure.

La figure 1b décrit de manière schématique les diverses étapes d'une seconde forme d'exécution du procédé de production d'un radio-isotope selon la présente invention, dans laquelle l'étape d'effusion est réalisée on-line, c'est-à-dire directement au sein de la chambre d'irradiation.FIG. 1b schematically describes the various steps of a second embodiment of the process for producing a radioisotope according to the present invention, in which the effusion stage is carried out on-line; ie directly within the irradiation chamber.

La constitution de la cible (étape A) se fait de la même manière que dans la première forme de réalisation. Comme montré à la figure 3, un substrat de collection 5 est installé dans la chambre d'irradiation. Il n'est donc pas nécessaire d'extraire la cible 3 pour procéder à l'effusion-collecte. Ce dispositif permet de réaliser simultanément l'irradiation et l'effusion-collecte (étapes B, D et E simultanées). L'énergie nécessaire pour chauffer la cible est apportée en tout ou en partie par le faisceau de particules accélérées. A l'issue de l'irradiation, le substrat de collection 5 est extrait de la chambre d'irradiation 10. La séparation du palladium déposé (étape F) est ensuite réalisée de la même manière que dans la première forme de réalisation. La cible 3 peut rester au sein de la chambre d'irradiation 10.The constitution of the target (step A) is in the same manner as in the first embodiment. As shown in FIG. 3, a collection substrate 5 is installed in the irradiation chamber. It is therefore not necessary to extract the target 3 to perform the shedding-collection. This device makes it possible to simultaneously perform the irradiation and effusion-collection (steps B, D and E simultaneous). The energy required to heat the target is provided in whole or in part by the accelerated particle beam. At the end of the irradiation, the collection substrate 5 is extracted from the irradiation chamber 10. The separation of the deposited palladium (step F) is then carried out in the same manner as in the first embodiment. The target 3 can remain within the irradiation chamber 10.

La figure 3 décrit donc un dispositif approprié à la mise en oeuvre de la seconde forme d'exécution du procédé de l'invention. Dans la chambre d'irradiation 10 sont installés la cible 3 ainsi que le substrat de collection 5. Un ensemble de pompes à vides permet d'atteindre de proche en proche le niveau de vide important requis au sein de l'accélérateur.FIG. 3 therefore describes a device that is suitable for implementing the second embodiment of the method of the invention. In the irradiation chamber 10 are installed the target 3 as well as the collection substrate 5. A set of vacuum pumps makes it possible to reach gradually the large level of vacuum required within the accelerator.

Les figures 4a et 4b décrivent de manière schématique un accélérateur de particules qui peut être utilisé pour la mise en oeuvre du procédé. Plus précisément, la figure 24a est une vue en perspective de cet accélérateur, tandis que la figure 4b est une vue de dessus de ce même dispositif.Figures 4a and 4b schematically describe a particle accelerator that can be used for the implementation of the method. More precisely, FIG. 24a is a perspective view of this accelerator, while FIG. 4b is a top view of this same device.

Comme illustré sur ces figures, l'accélérateur de particules 7 comprend :

  • une source capable de générer un faisceau de particules,
  • l'accélérateur 6 lui-même,
  • un circuit 9 d'acheminement du faisceau,
  • un aimant de déviation 11 qui permet de diriger le faisceau de particules soit vers un système de pompage 12 destiné à contrôler la qualité des paramètres du faisceau, soit vers une enceinte blindée 10 constituant la chambre d'irradiation placée en bout de ligne.
As illustrated in these figures, the particle accelerator 7 comprises:
  • a source capable of generating a particle beam,
  • the accelerator 6 itself,
  • a beam routing circuit 9,
  • a deflection magnet 11 which makes it possible to direct the beam of particles either towards a pumping system 12 intended to control the quality of the parameters of the beam, or towards a shielded enclosure 10 constituting the irradiation chamber placed at the end of the line.

Entre l'accélérateur 6 et l'aimant de déviation 11, le dispositif 7 comprend en outre une série d'aimants auxiliaires qui correspondent à des quadrupôles 13 et à des sextupôles 14 et qui ont pour fonction d'assurer une focalisation du faisceau.Between the accelerator 6 and the deflection magnet 11, the device 7 further comprises a series of auxiliary magnets which correspond to quadrupoles 13 and sextupoles 14 and whose function is to ensure a focusing of the beam.

On notera également que juste à la sortie de l'accélérateur 6 se trouvent des collimateurs 15.Note also that just at the exit of the accelerator 6 are collimators 15.

Par ailleurs un aimant de balayage 16 permet, comme son nom l'indique, de balayer la cible 3 à l'aide du faisceau d'irradiation.Moreover, a scanning magnet 16 allows, as its name indicates, to scan the target 3 with the aid of the irradiation beam.

De manière classique, on dispose la cible 3 obtenue dans la chambre 10 en bout de ligne de faisceau de l'accélérateur 6 de particules chargées. De manière avantageuse, l'accélérateur 6 peut être constitué par un cyclotron qui permet de générer un faisceau de protons présentant une certaine divergence et qui est corrigé par la présence des collimateurs 15.Conventionally, the target 3 obtained in the chamber 10 at the end of the beam line of the accelerator 6 charged particles. Advantageously, the accelerator 6 may be constituted by a cyclotron which makes it possible to generate a proton beam having a certain divergence and which is corrected by the presence of the collimators 15.

Ces collimateurs 15 ont essentiellement pour but d'empêcher qu'une partie du faisceau (20%) ne frappe des éléments de la ligne du faisceau et ne les endommage. Avantageusement, ces collimateurs 15 peuvent être amovibles et eux-mêmes revêtus d'une couche de rhodium, de manière à profiter de la perte de faisceau pour produire directement du 103Pd (radio-isotope 4).These collimators 15 are primarily intended to prevent part of the beam (20%) from striking elements of the beam line and damaging them. Advantageously, these collimators 15 can be removable and themselves coated with a layer of rhodium, so as to take advantage of the beam loss to directly produce 103 Pd (radioisotope 4).

Dans ce but, les collimateurs 15 doivent pouvoir répondre aux exigences suivantes: facilité de montage / démontage et placement dans la ligne, très bon refroidissement de la surface irradiée, facilité de transfert vers un container en plomb, facilité de démontage dans une « hot cell », masse de substrat en cuivre minimale, surface à recouvrir en rhodium minimale, réutilisation pour chaque irradiation d'un maximum de composants.For this purpose, the collimators 15 must be able to meet the following requirements: ease of assembly / disassembly and placement in the line, very good cooling of the irradiated surface, ease of transfer to a lead container, ease of disassembly in a hot cell ", Minimum copper substrate mass, minimum rhodium coating surface, reuse for each irradiation of a maximum of components.

La cible 3 peut également être installée directement à l'intérieur de l'accélérateur de particules 6.Target 3 can also be installed directly inside the particle accelerator 6.

Tant dans la première que dans la seconde forme de réalisation de l'invention, la cible 3 et le substrat de collection 5 peuvent être utilisés plusieurs fois successivement. On dispose ainsi d'un procédé économique en rhodium, et produisant peu de déchets.In both the first and the second embodiment of the invention, the target 3 and the collection substrate 5 can be used several times in succession. There is thus an economical process in rhodium, and producing little waste.

L'invention ne doit pas être considérée comme limitée aux exemples de réalisation préférés décrits ci-dessus. En particulier, la cible peut être constituée entièrement en le précurseur d'isotope, ou en un alliage comprenant ce précurseur d'isotope.The invention is not to be considered as limited to the preferred exemplary embodiments described above. In particular, the target may consist entirely of the isotope precursor, or an alloy comprising this isotope precursor.

Claims (14)

  1. Method for producing by means of a beam of accelerated particles, a radioisotope (4) from a target (3) comprising a precursor (1) of said radioisotope (4), said method comprising the following steps:
    - preparing a solid target (3) comprising the precursor (1) of the radioisotope (4),
    - irradiating within an irradiation chamber (10), said solid target (3) with a beam of accelerated particles, in order to induce transmutation of the precursor (1) into the radioisotope (4),
    - heating said solid target (3) in order to cause the efflux of the radioisotope (4) from the solid target (3),
    - collecting said radioisotope (4) extracted as a gas and condensing said radioisotope (4) into a solid or liquid.
  2. Method according to claim 1, characterized in that condensation of the radio-isotope (4) as a liquid or solid is achieved by contact of the radio-isotope (4) as a gas with adequate solid means, the radio-isotope (4) being separated from said medium in a subsequent step.
  3. Method according to claim 2, characterized in that it further comprises a step for conditioning said radioisotope (4) produced as a suitable liquid or solid.
  4. Method according to any of claims 1 to 3, characterized in that heating is achieved by the Joule effect, a treatment by a beam of charged particles such as electrons, by infrared radiation, by laser treatment, by plasma treatment.
  5. Method according to claim 4, characterized in that the heating is carried out in vacuo or under a controlled inert atmosphere.
  6. Method according to any of the preceding claims, characterized in that the heating is carried out within a shielded efflux enclosure (17) located outside the irradiation chamber (10).
  7. Method according to claim 6, characterized in that the collection and condensation step is carried out within said efflux enclosure (17).
  8. Method according to any of claims 1 to 5, characterized in that the irradiation, heating and collection and condensation steps for the extracted radioisotope are carried out on-line within the irradiation chamber (10).
  9. Method according to any of the preceding claims, characterized in that, at the end of the heating step, the target (3) is again used for a new irradiation step.
  10. Device for applying the method for producing a radioisotope (4) according to any of the preceding claims, from a target which remains solid, said device comprising the following means:
    - means (6,7,8,9,10) for irradiating a solid target (3) comprising an isotope precursor (1) in order to induce transmutation of the precursor (1) into the radioisotope (4),
    - heating means in order to cause the efflux of the radioisotope (4) within said solid target,
    - means for collecting and condensing the extracted radioisotope, formed by a cold collecting substrate (5) present within the irradiation chamber/efflux enclosure.
  11. Device according to claim 10, characterized in that the collecting substrate (5) has an interlayer having low characteristics for adhering to the radioisotope (4).
  12. Device according to claim 11, characterized in that it further comprises means for releasing the radioisotope from said collection substrate.
  13. Device according to claim 12, characterized in that the releasing means are formed by a separation enclosure (21) comprising an acid solution bath (22) in which the collecting substrate (5) with the radioisotope (4) is positioned.
  14. Use of the method according to any of claims 1 to 9 or of the device according to any of claims 10 to 13 for producing palladium 103 from rhodium 103.
EP02806546A 2001-12-21 2002-12-23 Method and device for production of radio-isotopes from a target Expired - Lifetime EP1464060B1 (en)

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PCT/BE2002/000198 WO2003063181A1 (en) 2001-12-21 2002-12-23 Method and device for production of radio-isotopes from a target
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DE60220316D1 (en) 2007-07-05
ATE363126T1 (en) 2007-06-15
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WO2003063181A1 (en) 2003-07-31
DE60220316T2 (en) 2008-01-17
EP1321948A1 (en) 2003-06-25

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