WO2011040898A1 - Procédé et appareil pour isoler le radioisotope molybdène 99 - Google Patents

Procédé et appareil pour isoler le radioisotope molybdène 99 Download PDF

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Publication number
WO2011040898A1
WO2011040898A1 PCT/US2009/005410 US2009005410W WO2011040898A1 WO 2011040898 A1 WO2011040898 A1 WO 2011040898A1 US 2009005410 W US2009005410 W US 2009005410W WO 2011040898 A1 WO2011040898 A1 WO 2011040898A1
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Prior art keywords
ions
isotope
primary
source compound
ion source
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Application number
PCT/US2009/005410
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English (en)
Inventor
Suzanne Lapi
Thomas J. Ruth
Dirk W. Becker
John M. D'auria
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Advanced Applied Physics Solutions, Inc.
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Priority to PCT/US2009/005410 priority Critical patent/WO2011040898A1/fr
Priority to CA2776043A priority patent/CA2776043A1/fr
Publication of WO2011040898A1 publication Critical patent/WO2011040898A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D59/00—Separation of different isotopes of the same chemical element
    • B01D59/44—Separation by mass spectrography
    • 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
    • G21G1/04—Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes outside nuclear reactors or particle accelerators
    • G21G1/06—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 neutron irradiation
    • 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
    • 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
    • G21G2001/0042—Technetium

Definitions

  • the present application relates to the production and extraction of radioisotopes from a source compound.
  • Diagnostic radiopharmaceuticals may include radiolabeled molecules used to provide information about various parts and/or functions of a patient's body (e.g., tumour cells, neuroreceptors, cardiac blood flow).
  • a number of different radioisotopes have been used for these purposes, such as single photon emitters (e.g., 99m Tc, 2 ° i Tl) and positron emitters (e.g., n C, 18 F).
  • 99 mTc is a well-known radioisotope used for various diagnostic procedures. Because the half- life of 99m Tc is only 6.02 h, this radioisotope is typically delivered to the medical practitioner in the form of the parent radioisotope, "Mo, which has a longer half-life of about 65.9 h. The 99m Tc is then obtained from the decay of the parent "Mo.
  • Mo may be produced via an 98 ⁇ ( ⁇ , ⁇ )" ⁇ reaction using neutrons from a nuclear reactor or from a neutron generator.
  • "Mo may be produced via a 235 U(n, fission) reaction.
  • both reactions have their disadvantages.
  • the yield of the "Mo is diluted by the presence of the isotopic contaminant, 98 Mo.
  • the product has a relatively low specific activity (activity/mass) and final total activity.
  • Such a "Mo product is not particularly useful in the commercial context.
  • For a 235 U(n, fission) reaction a relatively large amount of waste products are generated along with the "Mo.
  • a method of isolating a radioisotope for production of a higher specific activity radiopharmaceutical may include vaporizing a source compound containing a plurality of isotopes of an element, wherein the plurality of isotopes include a primary isotope of the element and a desired isotope of the element.
  • the desired isotope may be a parent radioisotope which decays to a daughter radioisotope having diagnostic or therapeutic properties.
  • the vaporized source compound may be ionized to form ions containing the plurality of isotopes.
  • the ions may be separated by mass so as to isolate the ions containing the desired isotope. An electromagnetic approach may be used to achieve the separation.
  • the isolated ions containing the desired isotope may be electrically focused onto a collector.
  • a method of isolating "Mo may include vaporizing a source compound containing isotopes of molybdenum (Mo).
  • the isotopes of Mo may include a primary Mo isotope (e.g., 98 Mo) and "Mo, wherein the "Mo is a nuclear reaction product of the primary Mo isotope.
  • the vaporized source compound may be ionized to form ions containing the isotopes of Mo.
  • An electric field may be generated to extract and accelerate the ions away from the ion source.
  • the electric field may be generated with extraction electrodes (e.g., acceleration electrodes). Additionally, a magnetic field may be generated to draw excess free electrons away from the ions.
  • the ions may be separated by mass using an electro-magnetic separator to isolate the ions containing "Mo.
  • the isolated ions containing "Mo may be collected with a collector.
  • FIG. 1 is an electrical schematic diagram of an ion source according to an example embodiment of the present invention.
  • FIG. 2 is an illustration of a method of producing and isolating "Mo according to an example embodiment of the present invention.
  • FIG. 3 is a graph showing the mass loss of M0O3 due to vaporization as a function of temperature during production of a vapor for entry into an ion source according to an example embodiment of the present invention.
  • FIG. 4 is a plan view, side view, and perspective view of a water-cooled beam stop according to an example embodiment of the present invention.
  • first, second, third, etc. may be used herein to describe various elements, components, regions, layers and/ or sections, these elements, components, regions, layers and/or sections should-.not be limited by these terms. These terms are only used to distinguish one element, component, region, layer or section from another region, layer or section. Thus, a first element, component, region, layer or section discussed below could be termed a second element, component, region, layer or section without departing from the teachings of example embodiments.
  • spatially relative terms e.g., "beneath,” “below,” “lower,” “above,” “upper” and the like, may be used herein for ease of description to describe one element or feature's relationship to another element(s) or feature(s) as illustrated in the figures. It will be understood that the spatially relative terms are intended to encompass different orientations of the device in use or operation in addition to the orientation depicted in the figures. For example, if the device in the figures is turned over, elements described as “below” or “beneath” other elements or features would then be oriented “above” the other elements or features. Thus, the term “below” may encompass both an orientation of above and below.
  • the device may be otherwise oriented (rotated 90 degrees or at other orientations) and the spatially relative descriptors used herein interpreted accordingly.
  • the terminology used herein is for the purpose of describing various embodiments only and is not intended to be limiting of example embodiments. As used herein, the singular forms “a,” “an” and “the” are intended to include the plural forms as well, unless the context clearly indicates otherwise. It will be further understood that the terms “comprises” and/or “comprising,” when used in this specification, specify the presence of stated features, integers, steps, operations, elements, and/or components, but do not preclude the presence or addition of one or more other features, integers, steps, operations, elements, components, and/or groups thereof.
  • Example embodiments are described herein with reference to certain cross- sectional illustrations that may be schematic illustrations of idealized embodiments and/or intermediate structures. As such, variations from the shapes .of the illustrations are to be expected due to, for instance, manufacturing techniques and /or tolerances. Thus, example embodiments should not be construed as limited to the shapes illustrated herein but are to include deviations that result, for example, from manufacturing. For example, an implanted region illustrated as a rectangle will, typically, have rounded or curved features and/or a gradient of implant concentration at its edges rather than a binary change from implanted to non-implanted region.
  • a buried region formed by implantation may result in some implantation in the region between the buried region and the surface through which the implantation takes place.
  • the regions illustrated in the figures are schematic in nature and their shapes are not intended to illustrate the actual shape of a region of a device and are not intended to limit the scope of example embodiments.
  • Example embodiments relate to the production and isolation of an ionic species from a source material.
  • the methods according to example embodiments may be suitable for producing and isolating "Mo (molybdenum-99) radioisotopes.
  • Mo mobdenum-99
  • the higher specific activity of the isolated "Mo material allows for larger quantities of "Mo to be applied to the generator material so as to achieve economies of scale in marketing "Mo/" m Tc generators.
  • the higher specific activity of the isolated “Mo material also leads to a higher production of the desired radioactive decay product from "Mo (e.g., 99m Tc).
  • ⁇ Tc compounds may be utilized in a variety of medical applications.
  • a " m Tc compound may be used in diagnosing various disorders depending upon the molecule to which the " m Tc is attached.
  • a number of such compounds are available and FDA-approved for both cardiology and oncology applications.
  • the present application primarily discusses "Mo, it should be understood that the methods and apparatuses according to example embodiments may also be applied to other radioisotopes so as to facilitate the production of additional higher specific radioactivity materials which may be utilized in a further range of research and /or diagnostic applications.
  • the method may be carried out with a reactor or other neutron source. Although this method may have moderately high yield, separating the desired "Mo isotope from the starting material, 98 Mo, is relatively difficult and is not feasible using chemical separation, thus resulting in products exhibiting relatively low specific radioactivity (activity/mass of molybdenum) .
  • the 100 Mo is converted to "Mo through photon capture.
  • the photons may be produced using an electron accelerator.
  • the method represented by expression (2) does not rely on a source of neutrons.
  • the method represented by expression (2) may have a relatively low yield. Additionally, separating the desired "Mo from the starting material, 100 Mo, is relatively difficult and is not feasible using chemical separation, thus resulting in products exhibiting relatively low specific activity (activity/mass of molybdenum).
  • the methods and apparatuses may involve vaporizing a source compound containing a plurality of isotopes of an element, wherein the plurality of isotopes includes a primary isotope of the element and a desired isotope of the same element.
  • the desired isotope may be a nuclear reaction product of the primary isotope and may constitute a relatively minute portion of the plurality of isotopes.
  • the desired isotope may also be a parent radioisotope which decays to a daughter radioisotope having diagnostic or therapeutic properties.
  • the vaporized source compound may be ionized to form ions containing the plurality of isotopes.
  • the ions may be separated so as to isolate ions containing the desired isotope.
  • the isolated ions containing the desired isotope may be collected with a collector.
  • a target When producing the source compound, a target may be enriched with the primary isotope (e.g., 98 Mo, 100 Mo) so as to increase the amount of the desired isotope (e.g., "Mo) resulting from the reaction.
  • the reaction may be a neutron capture or photon capture reaction.
  • Producing the source compound may be performed with a batch mode approach. Additionally, in view of the disadvantages discussed supra, it may be beneficial to produce the source compound with a process that does not involve irradiating a target containing uranium, particularly one that would involve the fission of uranium.
  • the resulting target material will consist essentially of 98 Mo and "Mo (the desired product).
  • the 98 Mo and "Mo material is ionized in a specially-designed ion source.
  • the “Mo can then be mass separated from the molybdenum (e.g., 98 Mo) starting material so as to facilitate the production of increased specific radioactivity "Mo compounds.
  • Such compounds ultimately provide the diagnostic radioisotope, " m Tc, by virtue of decay.
  • radioisotope production of "Mo in the range of about 100 6-day.
  • an ion source may be employed to ionize and extract the "Mo radioisotopes from the starting material.
  • a number of suitable ion sources may be used, including a Bernas ion source, a Freeman ion source, a Chordis ion source, a Thermal ion source, an ECR ion source, a PIG ion source, a MEWA ion source, or a laser-driven type ion source. Additional information regarding ion source technology may be found, for example, in "The Physics and Technology of Ion Sources, Second, Revised and Extended Edition," edited by Ian G. Brown, WILEY-VCH (2004), the entire contents of which are incorporated herein by reference.
  • FIG. 1 is an electrical schematic diagram of an ion source according to an example embodiment of the present invention.
  • plasma may interact with the radioisotope source compound to produce one or more ionic species (e.g., ⁇ 3 + ).
  • the ionic species may be extracted, accelerated, mass analyzed, and directed toward a beam stop for collection.
  • the beam stop may be water-cooled.
  • this technique may also be applied to other radioisotope source compounds (e.g., oxides, nitrides, halides) that can be vaporized under the appropriate temperature and pressure combination maintained within the ion source chamber.
  • the proper temperature and pressure may be a function of the materials utilized, the power applied, and the configuration of the source chamber and the ancillary equipment (e.g., gas mass flow controllers, valving, control systems, vacuum pumps, cooling assemblies).
  • ancillary equipment e.g., gas mass flow controllers, valving, control systems, vacuum pumps, cooling assemblies.
  • the ion source may be constructed and operated so as to enable the creation and maintenance of the appropriate temperature and pressure conditions within the ion source chamber.
  • the radioisotope source material may be vaporized at a suitable rate without damaging the ion source chamber or generating undesirable levels of byproducts that would interfere with the collection and enrichment of the targeted radioisotope.
  • the ion source may exhibit an efficiency greater than about 70%.
  • the ion source may have single or multiple extraction slits. When the ion source has multiple extraction slits, a plurality of beamlets may be extracted from the multiple slits and converged to form a single beam.
  • FIG. 2 is an illustration of a method of producing and isolating "Mo according to an example embodiment of the present invention.
  • Mo can be produced from 98 Mo with a 98 ⁇ ( ⁇ , ⁇ ) "Mo reaction.
  • the resulting 98 Mo and "Mo material can then be vaporized, ionized, and mass separated in accordance with the teachings herein to isolate the "Mo.
  • FIG. 3 is a graph showing the mass loss of M0O3 due to vaporization as a function of temperature during production of a vapor for entry into an ion source according to an example embodiment of the present invention.
  • the radioisotope source compound utilized in the ion source may exhibit satisfactory vaporization at temperatures below about 600°C. Additionally, it may be beneficial for the radioisotope source compound to exhibit satisfactory vaporization at temperatures below about 500°C so as to allow for the utilization of a wider range of materials in the construction of the ion source chamber. Furthermore, it may be beneficial for the radioisotope source compound utilized in the ion source to exhibit satisfactory vaporization at pressures below about 1 Torr.
  • the use of an appropriately sized resistor may allow the production of plasma capable of heating the source compound and its vessel to temperatures in excess of about 500°C, thereby volatilizing the source compound (e.g., molybdenum trioxide). Consequently, the source compound may dissociate within the plasma, with the resulting fragments becoming ions (e.g., MoO n + ).
  • the ions may be extracted from the ion source chamber as a beam and implanted on a beam stop.
  • the beam may have an intensity of at least 10 mA (e.g., 30 mA, 100 mA).
  • a. plurality of beamlets may be extracted from the ion source and converged to form a single beam.
  • the beam may be manipulated with a lens system that is configured to minimize space charge effects.
  • Isolating the desired isotope may be a challenge, because the quantity of the desired isotope in the source compound may be relatively sparse.
  • the relative quantity of "Mo to 98 Mo may be in the order of about 1 : 10 4 to 1 : 10 6 .
  • the separation of "Mo from 8 Mo is complicated by the fact that the mass of "Mo and 98 Mo differ by only one neutron.
  • the mass analyzer will need to exhibit a suitable mass resolution factor to achieve an acceptable separation.
  • a mass resolution factor of more than about 1000 may be needed to achieve a suitable separation for the "Mo.
  • FIG. 4 is a plan view, side view, and perspective view of a water-cooled beam stop for an ion source according to an example embodiment of the present invention.
  • the beam stop may be removed and evaluated using gamma spectroscopy to determine the amount of radioactivity implanted in the beam stop.
  • remote processing systems may be used to recover the separated "Mo. Ion source performance analysis indicates that the apparatus illustrated in FIG. 1 may adhere to beam currents of about 50 mA. For instance, 98 MoO n + may constitute a major portion of the beam, while "MoO n + may constitute a minor portion of the beam.
  • the collected ions containing "Mo may be chemically treated to remove unwanted, isobaric species (e.g., "Tc).
  • the treated "Mo may then be converted into a suitable chemical form for medical applications.
  • the primary isotope (e.g., 98 Mo, 100 Mo) recovered from the implant cycle may be reused in a subsequent cycle to produce "Mo.
  • the extraction percentage may be the portion of the desired isotopes released from the source compound vessel (e.g., graphite evaporator cell).
  • the source compound vessel e.g., graphite evaporator cell
  • the majority of the radioactive atoms may be successfully vaporized, ionized, and collected at the target assembly (e.g., beam stop).
  • the target assembly e.g., beam stop
  • various combinations of stable and radioactive atoms, extraction voltages, pressure conditions, slit openings, and lens configurations may provide for further improvements in the extraction percentage.
  • alternative configurations may provide for different heating arrangements.
  • resistance heating and/ or microwave heating may be used in lieu of or in addition to the plasma for vaporizing the source compound.
  • alternative structures e.g., higher voltage filaments
  • the desired species e:g., positive ion radioactive species
  • the source compound may be introduced into the ion source chamber as a vapor.
  • specific radioactivity values in the range of about 30 curies/g to over 1000 curies/g (e.g., 5000 curies/g) may be achieved using the methods and apparatuses according to example embodiments.
  • a BERNAS indirectly heated cathode
  • CHORDIS ion source modified appropriately to achieve the required high intensity extracted ion beams, may be used to separate "Mo from the neutron-irradiated 98 Mo by ionizing M0O3 molecules and implanting them on an appropriate collector element or beam stop.
  • a plasma including an equilibrium of volatile ionized and neutral molybdenum trioxide molecules may be generated in the ionizer volume.
  • An excess of free electrons, formed during the ionization process, may also be present.
  • a relatively weak electric or magnetic field may be established at the "exit" of the ionizer to draw the excess free electrons away from the ions.
  • the electric or magnetic field may be generated with a screening electrode (e.g., deceleration electrode).
  • radioisotope species e.g., 186 Re
  • Additional information may be found in related U.S. Application No. 12/078,409, filed March 31, 2008, the entire contents of which are incorporated herein by reference.
  • Other radionuclides that would benefit from being separated from stable or radioactive isotopes of the same element may include, for instance, 211 At (from 21 °At) and 124 I (from 1 3 I, 1251) .
  • the methods and apparatuses according to example embodiments may be used to isolate a variety of isotopes, thereby facilitating the production of a variety of higher specific activity compounds (e.g., radiopharmaceuticals).
  • higher specific activity compounds e.g., radiopharmaceuticals
  • Those ordinarily skilled in the art will readily appreciate, however, that certain aspects (e.g., type of ion source) may vary depending upon the particular molecule or compound involved.
  • the methods and apparatuses according to example embodiments may be utilized to produce an increased volume of a range of higher specific activity radioisotope materials having a longer shelf life and improved diagnostic effects compared to conventional production and purification techniques.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Medicines Containing Antibodies Or Antigens For Use As Internal Diagnostic Agents (AREA)

Abstract

Un procédé d'isolement de 99Mo obtenu à l'aide d'une réaction (n,) conformément à des modes de réalisation à titre d'exemples peut comprendre la vaporisation d'un composé source contenant 98Mo et 99Mo. Le composé source vaporisé peut être ionisé pour former des ions contenant 98Mo et 99Mo. Les ions peuvent être séparés pour isoler les ions contenant 99Mo. Les ions isolés contenant 99Mo peuvent être collectés à l'aide d'un collecteur. En conséquence, le 99Mo isolé peut avoir une radioactivité spécifique relativement élevée et, à son tour, peut être utilisé pour produire le radioisotope de diagnostic, 99mTc, par désintégration radioactive.
PCT/US2009/005410 2009-10-01 2009-10-01 Procédé et appareil pour isoler le radioisotope molybdène 99 WO2011040898A1 (fr)

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PCT/US2009/005410 WO2011040898A1 (fr) 2009-10-01 2009-10-01 Procédé et appareil pour isoler le radioisotope molybdène 99
CA2776043A CA2776043A1 (fr) 2009-10-01 2009-10-01 Procede et appareil pour isoler le radioisotope molybdene 99

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20110079108A1 (en) * 2009-10-01 2011-04-07 Suzanne Lapi Method and apparatus for isolating the radioisotope molybdenum-99
JP2015519586A (ja) * 2012-06-15 2015-07-09 デント インターナショナル リサーチ，インコーポレイテッド 元素を変換するための装置及び方法
CN108479394A (zh) * 2018-03-14 2018-09-04 中国科学院近代物理研究所 痕量气体同位素富集系统和方法
CN108977658A (zh) * 2018-08-03 2018-12-11 中国核动力研究设计院 一种Ni-63溶液γ核素去除方法

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3432709A (en) * 1965-10-23 1969-03-11 Atomic Energy Commission Calutron ion source with magnetic field inducing coil within arc chamber
US4035270A (en) * 1975-04-23 1977-07-12 Exxon Research And Engineering Company Isotope separation process
US5784423A (en) * 1995-09-08 1998-07-21 Massachusetts Institute Of Technology Method of producing molybdenum-99
US5802439A (en) * 1997-02-19 1998-09-01 Lockheed Martin Idaho Technologies Company Method for the production of 99m Tc compositions from 99 Mo-containing materials
US20030111948A1 (en) * 1996-03-28 2003-06-19 Retsky Michael W. Method and apparatus for deflecting and focusing a charged particle stream

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3432709A (en) * 1965-10-23 1969-03-11 Atomic Energy Commission Calutron ion source with magnetic field inducing coil within arc chamber
US4035270A (en) * 1975-04-23 1977-07-12 Exxon Research And Engineering Company Isotope separation process
US5784423A (en) * 1995-09-08 1998-07-21 Massachusetts Institute Of Technology Method of producing molybdenum-99
US20030111948A1 (en) * 1996-03-28 2003-06-19 Retsky Michael W. Method and apparatus for deflecting and focusing a charged particle stream
US5802439A (en) * 1997-02-19 1998-09-01 Lockheed Martin Idaho Technologies Company Method for the production of 99m Tc compositions from 99 Mo-containing materials

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20110079108A1 (en) * 2009-10-01 2011-04-07 Suzanne Lapi Method and apparatus for isolating the radioisotope molybdenum-99
US9587292B2 (en) * 2009-10-01 2017-03-07 Advanced Applied Physics Solutions, Inc. Method and apparatus for isolating the radioisotope molybdenum-99
JP2015519586A (ja) * 2012-06-15 2015-07-09 デント インターナショナル リサーチ，インコーポレイテッド 元素を変換するための装置及び方法
CN108479394A (zh) * 2018-03-14 2018-09-04 中国科学院近代物理研究所 痕量气体同位素富集系统和方法
CN108977658A (zh) * 2018-08-03 2018-12-11 中国核动力研究设计院 一种Ni-63溶液γ核素去除方法

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