EP2104113B1 - Procédé de production de molybdène radioactif - Google Patents

Procédé de production de molybdène radioactif Download PDF

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Publication number
EP2104113B1
EP2104113B1 EP07830597A EP07830597A EP2104113B1 EP 2104113 B1 EP2104113 B1 EP 2104113B1 EP 07830597 A EP07830597 A EP 07830597A EP 07830597 A EP07830597 A EP 07830597A EP 2104113 B1 EP2104113 B1 EP 2104113B1
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Prior art keywords
solution
water
irradiation
generated
hydrogen
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EP07830597A
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German (de)
English (en)
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EP2104113A1 (fr
EP2104113A4 (fr
Inventor
Etsuo Ishitsuka
Katsuyoshi Tatenuma
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Kaken Inc
Japan Atomic Energy Agency
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Kaken Inc
Japan Atomic Energy Agency
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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
    • G21G1/02—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes in nuclear reactors
    • 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
    • G21G1/001—Recovery of specific isotopes from irradiated targets
    • G21G2001/0036—Molybdenum

Definitions

  • the present invention relates to an efficient manufacturing method of radioactive molybdenum 99 Mo which is parent nuclide of radioactive technetium ( 99m Tc) used as the radioactive diagnosis medicine.
  • radioactive technetium ( 99m Tc) used in large quantities around the world to diagnose cancer or disease of internal organs, or to inspect the function of internal organs is 6.0 hours, and it is short. Therefore, radioactive technetium 99m Tc obtained by manufacturing radioactive molybdenum 99 Mo which is the parent nuclide, and extracting from 99 Mo (Half period is 66 hours) manufactured is usually used for the medical diagnosis etc. For mention of irradiation of 98 Mo to produce 99 Mo, see US-A-4 990 787 .
  • neutrons are irradiated to powdered or pelletized molybdenum oxide (MoO 3 ) of a solid state, which is Mo compound of a natural isotope to cause the nuclear reaction of 98 Mo(n, ⁇ ) 99 Mo (Hereinafter, this nuclear reaction is called the (n, ⁇ ) reaction or (n, ⁇ ) method).
  • MoO 3 molybdenum oxide
  • this nuclear reaction is called the (n, ⁇ ) reaction or (n, ⁇ ) method.
  • 99 Mo whose specific radioactivity is very low in comparison with the nuclear fission method in which uranium is used as a raw material is produced.
  • 99 Mo is generally produced by using powdered or pelletized molybdenum oxide (MoO 3 ) of a solid state as a raw material, enclosing the raw material with a closed container, inserting it into a nuclear reactor by using material irradiation equipment of the nuclear reactor, picking up the material irradiation equipment after irradiating neutrons for a fixed period of time (In general, 5-7 days), opening the closed container picked up, and making its contents ( 99 Mo is generated in MoO 3 , and they exist together) react, for instance, with caustic soda or aqueous ammonium, and dissolving them.
  • MoO 3 molybdenum oxide
  • the conventional equipment which irradiates the solid MoO 3 raw material is very expensive, the manufacturing ability is low, and a new container is required every time the (metallic) irradiation container where a MoO 3 raw material is enclosed is irradiated, in addition, because the container itself is made radiation after using (irradiating) and becomes radioactive contamination waste, there is the problem that the radioactive contamination waste increases further according to the increase in an amount of manufacturing of 99 Mo.
  • the above-mentioned problem is solved by manufacturing 99 Mo by changing the state of Mo compound to which neutrons are irradiated in a nuclear reactor from a solid state into a solution state.
  • radioactive molybdenum as set out in claim 1.
  • 99 Mo is obtained by collecting the Mo solution in continuous or batch processing, for instance, by circulating or feeding Mo solution, and generating 99 Mo in the Mo solution by the radioactivation of 98 Mo.
  • the Mo compound containing 98 Mo of the natural isotopic ratio or Mo compound in which 98 Mo is concentrated more than the natural isotopic ratio is dissolved in water, and may be ammonium molybdate.
  • the method further comprises the steps of extracting continuously or periodically hydrogen and oxygen gases generated by the radiolysis of water when neutrons are irradiated to the Mo solution in the nuclear reactor, and purging the hydrogen and oxygen with inert gas to dispose of them.
  • the method may comprise the steps of collecting after reuniting the hydrogen and oxygen with catalyst to return to water, and collecting to remove hydrogen and oxygen obtained by decomposing in radiation the water.
  • the method may employ a fluid pass-through type irradiation capsule installed in a reactor core, and a means for generating and collecting 99 Mo in continuous or batch processing by circulating the Mo solution in the capsule.
  • This method may be carried out in apparatus, which comprises: injection equipment which injects a fixed amount of Mo solution in continuous or batch processing; collecting equipment which collects 99 Mo generated in continuous or batch processing; equipment which extracts and removes hydrogen and oxygen of the gas generated by radiolysis reaction of the water generated in the irradiation capsule; a storage facility in which catalyst which has function to return the hydrogen and oxygen of the extracted gas to water by recombination reaction is filled, circulation equipment of the Mo solution to which a heat exchanger to do cooling in the irradiation capsule is attached; equipment which picks up and collects 99 Mo generated in continuous or batch processing, measuring equipment by which amounts of the generation and the collection of 99 Mo are measured, and a shielding facility to shield the radiation such as gamma rays generated from 99 Mo generated and collected and 99m Tc of the coexisting daughter nuclide.
  • the present invention thus may use an irradiation capsule which is far low-cost compared with the conventional high-cost irradiation equipment. According to the present invention, it is possible to increase the manufacturing ability of 99 Mo and manufacture it in continuous or batch processing.
  • the desired 99 Mo can be manufactured only by installing a fluid pass-through type capsule which can inject and collect solution from the outside and by injecting the solution into it in continuous or batch processing, the radioactive contamination waste generated when manufacturing 99 Mo by using the conventional irradiation equipment is not generated. Moreover, because the Mo solution which contains 99 Mo generated can be shipped only by dispensing and collecting it in a special container like a vial container made of glass without processing after collecting it, the entire process from the stock of raw material to the collection of 99 Mo which is specified substance can be simplified compared with the prior art.
  • the present invention has feature that 99 Mo manufacturing cost is cheaper.
  • the complex operations are accompanied when the raw material is palletized. And The difficulty is attended to the management and the maintenance of the quality, because impurities are apt to be mixed at the pelletizing operation.
  • the Mo solution which is the raw material used in the present invention it is possible to adjust just by dissolving Mo compound to high purity water by maintaining the high purity Mo compound (ammonium molybdate) used. Because impurities can be absorbed and removed just by causing to flow into an aluminum column, et al. even when they are in the Mo solution, it is easy for the Mo solution irradiation method to maintain high quality because the adjustment of the irradiation body raw material is easy, compared with the solid MoO 3 irradiation method.
  • a solid irradiation if the MoO 3 irradiation body is in a powder form, it is necessary to seal up first the irradiation body in a quartz tube, and then enclose in a metallic irradiation container (In general, aluminum family metal). If the MoO 3 irradiation body is in a pelletized form, the sealing up and the enclosing is performed directly in the metallic irradiation container. These irradiation containers become radioactive contamination waste because they are radioactivated by neutron irradiation.
  • a Mo solution irradiation method of the present invention includes only an operation that a constant amount of Mo solution is injected with the pump through piping to an irradiation capsule in continuous or batch processing. An irradiation container is unnecessary. Therefore, the radioactive contamination waste is not generated along with 99 Mo manufacturing.
  • the 99 Mo manufacturing ability by the solid irradiation method in material testing reactor JMTR of Japan Atomic Energy Agency is 220Ci( 99 Mo)/week, for instance, even when existing facility is remodeled. In addition, it is total 570Ci ( 99 Mo)/week even when expanded. Moreover, about 700 million yen to 1.5 billion yen is necessary according to the calculation as those remodeling cost and installation cost.
  • the manufacturing ability of 569Ci( 99 Mo)/week in one system which is almost equal to the solid irradiation method, that is, substantially the same manufacturing ability as the above-mentioned expanded facility in the solid irradiation method can be obtained only by circulating 28% solution of ammonium molybdate to the capsule with the zone of 55 mm in inside diameter ⁇ and 700 mm in height to which neutrons are irradiated (effective content volume 1.66L) at the rate of 277mL/day.
  • the provisional calculation of the installation cost is about 200 million yen a system. Accordingly, the present invention is superior to the conventional method also in 99 Mo manufacturing ability and the installation cost.
  • the conventional solid irradiation method it is manufactured by inserting an irradiation container into a nuclear reactor with material irradiation equipment, picking up after irradiating neutrons for a fixed period of time (generally, for 5 to 7 days), opening the closed container picked up, and making its contents ( 99 Mo is generated in MoO 3 , and they exist together) react, for instance, with alkaline solution such as caustic soda, aqueous ammonium and dissolving them.
  • alkaline solution such as caustic soda, aqueous ammonium and dissolving them.
  • the process to bring into the state which can be shipped as 99 Mo is complex because it is impossible to replace the irradiation body on its way, and it is necessary to open the MoO 3 irradiation body which contains 99 Mo in another facility and dissolve.
  • the Mo solution which contains 99 Mo can be collected only by activating the pump of 99 Mo collection equipment in the Mo solution irradiation method according to the present invention.
  • the Mo solution which contains 99 Mo generated can be shipped only by dispensing and collecting it in a container as it is, the entire process from the stock of raw material to the collection of 99 Mo product can be simplified.
  • radioactive substance according to the present invention which is socially useful can be used to manufacture other radioactive substance.
  • life time of radioactive rhenium ( 88 Re) which can be used to treat cancers is short (The half period of 188 Re is 17.5 hours)
  • radioactive tungsten 188 W which is parent nuclide of 188 Re is manufactured, 188 Re extracted from the 188 W can be used for cancer care.
  • efficiently manufacturing the aimed 188 W becomes possible by irradiating neutrons in a nuclear reactor to W solution in which W compound containing 186 W of the natural isotopic ratio is dissolved in water, or W solution in which 186 W is concentrated more than the natural isotopic ratio is dissolved in water, carrying out two step reaction of 186 W(n, ⁇ ) 187 W ⁇ 187 W(n, ⁇ ) 188 W to produce 188 W in the W solution, and by collecting the W solution in continuous or batch processing. Or it becomes possible by circulating or feeding W solution, radioactivating 186 W to generate 188 W in the W solution, and by collecting the W solution in continuous or batch processing.
  • FIG. 1 is a drawing showing 99 Mo manufacturing apparatus of Mo solution circulating type.
  • FIG. 1 An apparatus for carrying out this invention is shown in FIG. 1 .
  • Capsule4 for solution irradiation is set up in the core 2 of a nuclear reactor (3).
  • This capsule is connected with external Mo solution injection equipment (6, 7, 8) and generation 99 Mo collection container 11 via pipe 9 through which the Mo solution is introduced and pipe 10 through which the Mo solution is collected.
  • Ammonium molybdate solution is adjusted, and stored in a container of Mo solution supplying system 6 beforehand.
  • the Mo solution is injected into the irradiation capsule via pipe 9 by pump 7.
  • the irradiation time of the Mo solution in the capsule by neutrons can be adjusted by injecting the Mo solution in continuous or batch processing. Though time for irradiating neutrons to the Mo solution is needed for 5-7 days, the gas generated by the radiolysis of water and the heat generated by the irradiation of the capsule in the core can be removed by circulating the Mo solution in the capsule by the operation of an external valve and circulating pump 8 into the system to remove hydrogen gas and oxygen gas generated by the radiolysis of water in heat exchanger 13 and extraction gas processing system 14.
  • a constant amount of the Mo solution irradiated by a predetermined amount of neutrons can be collected into 99 Mo collection container 11 to obtain 99 Mo. Because 99 Mo with a high radioactivity is collected into this container 11, it is necessary to cover the radiation such as gamma rays discharged from there with lead etc. and reduce the radiation exposure of workers. It is also possible to automate 99 Mo collection operation because 99 Mo can be collected only by the operation of pumps 8 and 15.
  • the hydrogen gas and the oxygen gas generated by the radiolysis of water of the Mo solution in the capsule whose content volume is 1.66L are respectively 0.18NL and 0.09NL per day, which are few. However, because these gases are in danger of returning to the system, they are removed by extracting in extraction gas processing system 14 when the Mo solution is circulated or collected.
  • These hydrogen and oxygen gases can be discharged outside of the system by purging with inert gas such as nitrogen gas or helium gas for instance, or returned to the Mo solution after returning to the state of water by reuniting the hydrogen and the oxygen by using the catalyst,
  • the Mo solution collected to 99 Mo collection container 11 is transported to 99 Mo dispensation unit 117, and is dispensed in 99 Mo shipping container like a vial.
  • the 99 Mo shipping container is put in the transport container with radiation shield as it is, and shipped as 99 Mo product after packed.
  • the present invention it becomes possible to manufacture efficiently parent nuclide 99 Mo of 99m Tc daily used in large quantities for the medical treatment diagnosis in the world including Japan becomes possible according to the present invention.
  • 99 Mo the most is manufactured by a method of making highly enriched uranium a raw material now.
  • the (n, ⁇ ) method which does not use the uranium as a raw material is going to be used because the conventional nuclear fission method, in which uranium is used as a raw material, has the problem described above.
  • a large amount of 99 Mo is manufactured by using the (n, ⁇ ) method according to the present invention, enormous social contribution becomes possible.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Plasma & Fusion (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Monitoring And Testing Of Nuclear Reactors (AREA)
  • Medicines Containing Antibodies Or Antigens For Use As Internal Diagnostic Agents (AREA)
  • Sampling And Sample Adjustment (AREA)
  • Compositions Of Oxide Ceramics (AREA)

Claims (6)

  1. Procédé de production de molybdène radioactif par irradiation de 98Mo, caractérisé par les étapes de:
    irradier des neutrons dans un réacteur nucléaire à une solution Mo dans laquelle le composé Mo contenant 98Mo du rapport isotopique naturel est dissous dans de l'eau, ou une solution Mo dans laquelle 98Mo est concentrée plus que le rapport isotopique naturel est dissous dans de l'eau, pour produire 99Mo dans la solution Mo par la radioactivation de 98Mo; et
    recueillir la solution Mo pour obtenir 99Mo.
  2. Procédé de production de molybdène radioactif selon la revendication 1, dans lequel ladite solution Mo est recueillie dans un traitement continu ou par lots pour obtenir 99Mo.
  3. Procédé de fabrication de 99Mo selon la revendication 1 ou 2, qui comprend en outre les étapes de:
    extraire continuellement ou périodiquement les gaz d'hydrogène et d'oxygène produits par la radiolyse de l'eau lorsque les neutrons sont irradiés à ladite solution Mo dans le réacteur nucléaire; et
    purger l'hydrogène et l'oxygène avec un gaz inerte pour les mettre au rebut.
  4. Procédé de fabrication de 99Mo selon la revendication 1 ou 2, qui comprend en outre les étapes de:
    extraire continuellement ou périodiquement les gaz d'hydrogène et d'oxygène produits par la radiolyse de l'eau lorsque les neutrons sont irradiés à ladite solution Mo dans le réacteur nucléaire;
    recueillir après la réunion de l'hydrogène et de l'oxygène avec le catalyseur pour le retour à l'eau; et
    recueillir pour retirer l'hydrogène et l'oxygène obtenus par décomposition dans la radiation de l'eau dans laquelle le composé Mo est dissous.
  5. Procédé selon l'une quelconque des revendications 1 à 4, dans lequel la solution Mo est irradiée avec des neutrons dans une capsule d'irradiation du type à fluide traversant (4) installé dans le coeur (2) du réacteur, et des moyens sont prévus pour produire et recueillir 99Mo par un traitement continu ou par lots en amenant la solution Mo à s'écouler dans la capsule.
  6. Procédé selon la revendication 5, exécuté dans l'appareil qui comprend:
    un équipement d'injection (6, 7, 8) qui injecte une quantité fixe de solution Mo lors d'un traitement continu ou par lots;
    recueillir l'équipement (10, 11) qui recueille 99Mo produit lors d'un traitement continu ou par lots;
    retirer l'équipement (14) qui extrait et retire l'hydrogène et l'oxygène du gaz produit par réaction de radiolyse de l'eau produite dans la capsule d'irradiation;
    une installation de stockage dans laquelle le catalyseur, qui a pour fonction de ramener l'hydrogène et l'oxygène du gaz extrait à l'eau par une réaction de recombinaison, est introduit;
    un équipement de circulation de la solution Mo auquel un échangeur de chaleur (13) destiné à provoquer un refroidissement dans la capsule d'irradiation0 est fixé; et
    un équipement de mesure par lequel des quantités de génération et de collecte de 99Mo sont mesurées; et
    une installation de protection pour protéger le rayonnement, comme des rayons gamma produits par 99Mo produits et recueillis et 99mTc du nucléide engendré coexistant.
EP07830597A 2006-10-20 2007-10-19 Procédé de production de molybdène radioactif Not-in-force EP2104113B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2006286159A JP4618732B2 (ja) 2006-10-20 2006-10-20 放射性モリブデンの製造方法と装置
PCT/JP2007/070863 WO2008047946A1 (fr) 2006-10-20 2007-10-19 Procédé de production de molybdène radioactif, appareil prévu à cet effet et molybdène radioactif produit par le procédé

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EP2104113A1 EP2104113A1 (fr) 2009-09-23
EP2104113A4 EP2104113A4 (fr) 2010-09-15
EP2104113B1 true EP2104113B1 (fr) 2012-01-11

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EP (1) EP2104113B1 (fr)
JP (1) JP4618732B2 (fr)
AT (1) ATE541297T1 (fr)
CA (1) CA2666570C (fr)
WO (1) WO2008047946A1 (fr)

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JP2862837B2 (ja) 1996-07-16 1999-03-03 日本原子力研究所 ９９Ｍｏ−９９ｍＴｃジェネレータ用Ｍｏ吸着剤およびその製造方法
US6337055B1 (en) * 2000-01-21 2002-01-08 Tci Incorporated Inorganic sorbent for molybdenum-99 extraction from irradiated uranium solutions and its method of use
JP4994589B2 (ja) * 2004-11-08 2012-08-08 住友重機械工業株式会社 放射性同位元素製造用ターゲット

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9396826B2 (en) * 2010-07-29 2016-07-19 Oregon State University Isotope production target

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CA2666570C (fr) 2011-11-15
WO2008047946A1 (fr) 2008-04-24
JP4618732B2 (ja) 2011-01-26
EP2104113A1 (fr) 2009-09-23
JP2008102078A (ja) 2008-05-01
EP2104113A4 (fr) 2010-09-15
CA2666570A1 (fr) 2008-04-24
ATE541297T1 (de) 2012-01-15

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