EP2398023A1 - Herstellung von Molybdän-99 - Google Patents

Herstellung von Molybdän-99 Download PDF

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Publication number
EP2398023A1
EP2398023A1 EP10166604A EP10166604A EP2398023A1 EP 2398023 A1 EP2398023 A1 EP 2398023A1 EP 10166604 A EP10166604 A EP 10166604A EP 10166604 A EP10166604 A EP 10166604A EP 2398023 A1 EP2398023 A1 EP 2398023A1
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EP
European Patent Office
Prior art keywords
molybdenum
target
thorium
uranium
production
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Withdrawn
Application number
EP10166604A
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English (en)
French (fr)
Inventor
Kamel Abbas
Jan Kozempel
Uwe Holzwarth
Federica Simonelli
Neil Gibson
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European Union represented by European Commission
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European Union represented by European Commission
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Priority to EP10166604A priority Critical patent/EP2398023A1/de
Publication of EP2398023A1 publication Critical patent/EP2398023A1/de
Withdrawn legal-status Critical Current

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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
    • 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
    • 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 generally relates to a method for the production and the separation of molybdenum-99 (Mo-99).
  • Technetium-99m symbolized Tc-99m
  • molybdenum-99 the daughter product of molybdenum-99, is the most commonly utilized medical radioisotope in the world, used for approximately 20-25 million medical diagnostic procedures annually, comprising some 80% of all diagnostic nuclear medicine procedures.
  • Tc-99m is a metastable nuclear isomer of technetium-99 (Tc-99), which "decays" to Tc-99 by rearrangement of nucleons in its nucleus. It is a short-live gamma ray emitting isotope largely used in radioactive isotope medical tests, for example as a radioactive tracer that medical equipment can detect in the body.
  • the decay process starting from Mo-99 that produces Tc-99m is as follows: Mo - 99 ⁇ Tc - 99 ⁇ m + ⁇ - + v ⁇ e where ⁇ - denotes a beta particle (electron) emitted from the nucleus, and ⁇ e denotes the emitted electron antineutrino.
  • ⁇ - denotes a beta particle (electron) emitted from the nucleus
  • ⁇ e denotes the emitted electron antineutrino.
  • the half-live of this decay is about 66 h.
  • Tc-99m will then undergo an isomeric transition to yield Tc-99 and a monoenergetic gamma emission: Tc - 99 ⁇ m ⁇ Tc - 99 + ⁇ with a half-live of about 6 h.
  • molybdenum-99 have been produced so far in nuclear reactors through the uranium fission process (for example, see US 3799883 ) utilizing highly enriched uranium-235 (HEU) (>90%) and through neutron capture of Mo-98.
  • HEU highly enriched uranium-235
  • the fission process yields Mo-99 with a large array of undesirable fission products that present significant infrastructure, health and security, liability, handling, storage, and waste issues and associated costs, while the neutron capture method produces no nuclear waste, but presents a lower yield and a much smaller specific activity of Mo-99.
  • Table 1 Country City Facility Age of the reactor World supply (%) Power (MW) Canada Rolphton, Ontario NRU Chalk River 52 years 31% 135 The Netherlands Zijpe HFR-Petten 47 years 33% 45 Belgium Mol BR2 47 years 10% 100 France Saclay OSIRIS 42 years 8% 70 South Africa Pelindaba SAFARI 43 years 3% 20 Australia Sydney Opal 2 years 20 Czech republic Rez LWR-15 55 years 10
  • HEU highly enriched U-235
  • WO2006/028620 A2 relates to the production of Mo-99 from Zr-96 through irradiation with (charged) alpha particles, e.g. in a cyclotron or a linear accelerator. This document teaches the irradiation of the zirconium-96 target with alpha particles to yield, via an alpha particle capture/neutron emission process, an irradiated target containing Mo-99.
  • the present invention proposes a method for the production of Mo-99 comprising the steps of
  • the present invention does not start from a target element which is lighter than 99 Mo and which is irradiated with the "missing" or an excess of nucleons to yield the desired element.
  • the present invention provides for an alternative production method of Mo-99.
  • the charged particles are preferably selected from protons, deuterons, alpha or 3 He 2+ particles, but they could also be chosen among heavier charged particles that can be accelerated at the appropriate energy and intensity.
  • the starting materials for the target which are elements usable in the present method are selected from elements which are fissile under charged particle bombardment or combinations of two or more thereof.
  • the expression "elements” also comprises compounds of said elements, such as oxides, nitrides, etc. Furthermore, the elements can be in their natural abundance or enriched.
  • Particularly preferred elements are selected from thorium-232 (Th-232), thorium-229 (Th-229), thorium-230 (Th-230), uranium-238 (U-238), uranium-235 (U-235), uranium-233 (U-233), radium-226 (Ra-226), bismuth (Bi-209), lead (Pb) or any combination thereof, even more preferably from thorium-232 (Th-232), thorium-230 (Th-230), uranium-238 (U-238), radium-226 (Ra-226) or any combination thereof. Still more preferably, the target essentially or totally consists of these preferred or even more preferred elements, either in metal, oxide, nitride form, or any combination thereof.
  • the starting material can be fabricated into various target configurations to enhance the production and recovery of the desired species, such as Mo-99 (or even technetium-99m).
  • the solid or liquid target comprising the target nuclide(s) is generally loaded in a target holder adapted for use with the accelerator.
  • the target nuclide(s) is/are in any appropriate form, preferably in metal or oxide form.
  • the charged particle beam is preferably generated using an accelerator, such as in a cyclic and/or linear accelerator, e.g. a biomedical cyclotron.
  • the irradiation energy and target configuration may be selected such that the efficiency or economics of the overall process is optimal.
  • the charged particles in the present method generally need incident energy above 15 MeV all charged particles included.
  • the beam energy of the charged particle beam must be set for a maximum Mo-99 yield production.
  • the Mo-99 production yield is directly proportional to the charged particle beam intensity, so the higher is the intensity of the beam the higher is the production yield of Mo-99. This is to say that accelerators (cyclotrons or linear accelerators) of high beam intensities are necessary for large production of Mo-99.
  • the irradiation can thus be accomplished by inserting the target into any accelerator capable of producing charged particle beams of the desired energy and beam intensity.
  • accelerators of beam intensities in the range 100 ⁇ A-100 mA equipped with suitable target systems able to stand under high beam intensities would be optimum.
  • the method further comprises one or more physical and/or chemical separation step(s) for separating molybdenum-99 from the irradiated target portion to yield Mo-99 and a purified target portion.
  • a "purified target portion" in the present context means a target from which at least a substantial amount of the desired Mo-99 has been removed. Further separation steps may be included if necessary to eliminate possible further impurities or unwanted compounds and elements.
  • the physical and/or chemical separation step(s) are preferably chosen among ion exchange, electrolysis, extraction and sublimation or any combination thereof. Such step may include the oxidation or reduction of Mo-99 or the conversion to a salt form thereof.
  • the purified target portion is recycled in step (a) to produce further Mo-99.
  • Mo-99 compositions produced as described above are preferably used to "generate" Tc-99m.
  • Tc-99m is the result of the decay of Mo-99 as a parent nuclide, which has a half-life of 66h.
  • one embodiment of a method for producing Mo-99 includes the so-called "generation" of Tc-99m by any appropriate method.
  • a chromatographic generator column is charged with an alumina adsorbent.
  • the adsorbent is then equilibrated using a salt solution, such as an ammonium nitrate or saline solution.
  • Mo-99 is loaded on the column, typically at a pH of from about 3 to about 4.
  • Tc-99m is then eluted from the loaded column using a salt solution.
  • the eluted Tc-99m solution may be used without further purification.
  • the Tc-99m solution can be further purified if desired, for example, by loading onto a Tc-99m concentrator column containing an anion-exchange resin known to those of ordinary skill in the art.
  • the concentrator column typically is washed with a small amount of salt solution, followed by a small amount of deionized water.
  • Tc-99m can also be eluted from the column using a reductive solution, such as a solution containing a complexing agent.
  • a further aspect of the invention is the use of the Mo-99 and/or Tc-99m obtained by a method as described above in the preparation of radiopharmaceuticals and/or radiation sources, which contain molybdenum-99 and/or technetium-99m, for use in nuclear medicine or Single photon emission computed tomography (SPECT) applications.
  • SPECT Single photon emission computed tomography
  • Tc-99m Medical uses for Tc-99m are, for example, bone scan, myocardial perfusion imaging (MPI), functional brain imaging, immunoscintigraphy, blood pool labeling, pyrophosphate for heart damage, sulfur colloid for spleen scan, etc.
  • MPI myocardial perfusion imaging
  • functional brain imaging immunoscintigraphy
  • blood pool labeling pyrophosphate for heart damage
  • sulfur colloid for spleen scan etc.
  • the different aspects of the present invention describe the irradiation with charged particles of a target material comprising elements which are heavier than Mo-99, the selective recovery of Mo-99 from the irradiated target material, as well as the fabrication of new or recycled targets from such recovered target material.
  • Such a method can produce sufficient quantities of Mo-99 and thus of Tc-99m for use in the fields on nuclear medicine and/or nuclear chemistry.
  • the above presented method allows to minimize the expenses in relation with preparing molybdenum-99 or technetium-99m.
  • Figure 1 A gamma-ray spectrum of a test irradiation (proton beam on Th-232) performed at the JRC-Cyclotron showing the gamma-ray peaks of the produced Mo-99.
  • the invention proposes the production of Mo-99 by bombarding a heavy material target with accelerated charged particles. Under the bombardment the fission products are produced and Mo-99 is among these products.
  • the steps for the production of Mo-99 may be summarized as follows:
  • FIG. 1 A gamma-ray spectrum of the activated Th-232 showing the gamma-ray peaks of Mo-99 is presented in Figure 1 .
  • the Mo-99 was also identified with its half-life deduced from the measurement of Mo-99 activity at different times during several days after the irradiation test.
  • a significantly higher yield of Mo-99 is expected with charged particle beam of higher energies (>30 MeV).
  • Mo-99 yields of tens of Ci tens of 37 GBq
EP10166604A 2010-06-21 2010-06-21 Herstellung von Molybdän-99 Withdrawn EP2398023A1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP10166604A EP2398023A1 (de) 2010-06-21 2010-06-21 Herstellung von Molybdän-99

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Application Number Priority Date Filing Date Title
EP10166604A EP2398023A1 (de) 2010-06-21 2010-06-21 Herstellung von Molybdän-99

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EP2398023A1 true EP2398023A1 (de) 2011-12-21

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113178276A (zh) * 2021-04-15 2021-07-27 中国科学院合肥物质科学研究院 一种基于Th-U自持循环的99Mo次临界生产装置及方法

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3799883A (en) 1971-06-30 1974-03-26 Union Carbide Corp Production of high purity fission product molybdenum-99
US5784423A (en) * 1995-09-08 1998-07-21 Massachusetts Institute Of Technology Method of producing molybdenum-99
WO2006028620A2 (en) 2004-08-02 2006-03-16 Battelle Memorial Institute Medical radioisotopes and methods for producing the same

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3799883A (en) 1971-06-30 1974-03-26 Union Carbide Corp Production of high purity fission product molybdenum-99
US5784423A (en) * 1995-09-08 1998-07-21 Massachusetts Institute Of Technology Method of producing molybdenum-99
WO2006028620A2 (en) 2004-08-02 2006-03-16 Battelle Memorial Institute Medical radioisotopes and methods for producing the same

Non-Patent Citations (6)

* Cited by examiner, † Cited by third party
Title
L. H. GEVAERT, R. E. JERVIS, AND H. D. SHARMA: "Cumulative yields in the 14 MeV neutron fission of 232Th and 238U in the symmetric region", CANADIAN JOURNAL OF CHEMISTRY, vol. 48, no. 4, 4 February 1970 (1970-02-04), pages 641 - 651, XP002597161, ISSN: 1480-3291, Retrieved from the Internet <URL:http://article.pubs.nrc-cnrc.gc.ca/RPAS/rpv?hm=HInit&calyLang=eng&journal=cjc&volume=48&afpf=v70-104.pdf> [retrieved on 20100816] *
LAGUNAS-SOLAR, M.C. ; ZENG, N.X. ; MIRSHAD, I. ; CASTANEDA, C.M.: "Cyclotron production of molybdenum-99 via proton-induced uranium-238 fission", TRANSACTIONS OF THE AMERICAN NUCLEAR SOCIETY, vol. 74, 31 December 1996 (1996-12-31), pages 134 - 135, XP002597162, ISSN: 0003-018X *
MANUEL C. LAGUNAS-SOLAR: "Radionuclide production with > 70-MeV proton accelerators: current and future prospects", NUCLEAR INSTRUMENTS AND METHODS IN PHYSICS RESEARCH SECTION B: BEAM INTERACTIONS WITH MATERIALS AND ATOMS, vol. 69, no. 4, 1 July 1992 (1992-07-01), pages 452 - 462, XP002597160 *
W.H. JONES, A. TIMNICK, J.H. PAEHLER, T.H. HANDLEY: "Bombardment Energy and Fission Product Yield Pattern for Protons on Natural Uranium and U-235", PHYSICAL REVIEW, vol. 99, no. 1, 1 July 1955 (1955-07-01), pages 184 - 187, XP002597159 *
YVES JONGEN: "A Cyclotron driven neutronmultiplier for the productionof Mo 99", 29 October 2009 (2009-10-29), Groningen, The Netherlands, XP002597158, Retrieved from the Internet <URL:https://www.kvi.nl/~agorcalc/ECPM2009/Presentations/29_06Jongen.pdf> [retrieved on 20100816] *
Z.I. KOLAR; H.TH. WOLTERBEEK: "MAKING OF FISSION Mo-99 FROM LEU SILICIDE(S): A RADIOCHEMISTS' VIEW", INTERNATIONAL MEETING ON REDUCED ENRICHMENT FOR RESEARCH AND TEST REACTOR, 2004 RERTR, 2004

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113178276A (zh) * 2021-04-15 2021-07-27 中国科学院合肥物质科学研究院 一种基于Th-U自持循环的99Mo次临界生产装置及方法

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