US3382152A - Production of high purity radioactive isotopes - Google Patents

Production of high purity radioactive isotopes Download PDF

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Publication number
US3382152A
US3382152A US399842A US39984264A US3382152A US 3382152 A US3382152 A US 3382152A US 399842 A US399842 A US 399842A US 39984264 A US39984264 A US 39984264A US 3382152 A US3382152 A US 3382152A
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United States
Prior art keywords
radioactive
molybdenum
alumina
solution
column
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
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US399842A
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English (en)
Inventor
Lieberman Ephraim
Wayne J Gemmill
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Union Carbide Corp
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Union Carbide Corp
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Publication date
Application filed by Union Carbide Corp filed Critical Union Carbide Corp
Priority to US399842A priority Critical patent/US3382152A/en
Priority to GB25433/66A priority patent/GB1131546A/en
Priority to CH850866A priority patent/CH454805A/fr
Priority to DE19661544156 priority patent/DE1544156A1/de
Priority to BE682978D priority patent/BE682978A/xx
Priority to FR66641A priority patent/FR1486542A/fr
Application granted granted Critical
Publication of US3382152A publication Critical patent/US3382152A/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G39/00—Compounds of molybdenum
    • C01G39/003—Preparation involving a liquid-liquid extraction, an adsorption or an ion-exchange
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G39/00—Compounds of molybdenum
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G99/00—Subject matter not provided for in other groups of this subclass
    • C01G99/006—Compounds containing a metal not provided for elsewhere in this subclass, with or without oxygen or hydrogen, and containing two or more other elements

Definitions

  • This invention relates to the production of high .purity radioactive isotopes, particularly molybdenum-99 and technetium-99m.
  • Technetttium-99m which has a half-life of six hours, is produced by the spontaneous radioactive beta decay of molybdenum-99. The latter has a half-life of 67 hours.
  • High purity Tc is used primarily as a radioisotope in medical research and diagnosis. It is well suited for liver and brain scanning, and is preferred over other radioactive isotopes because of its short half-life which results in reduced exposure of the organs to radiation.
  • radioactive molybdenum-99 has been recovered as a fission product formed by the fissioning of uranium-235 in a nuclear reactor.
  • This method of producing M0 has several important shortcomings.
  • Some of these fission products are long lived, and due to their radioactivity are difficult to handle without elaborate shielding.
  • a process which comprises irradiating a molybdenum containing material in the presence of a neutron flux until the desired amount of Mo activity is formed, dissolving the irradiated material (containing M0 in a base, adjusting the pH of the solution to be acidic and above pH 2.5, contacting an inorganic anion exchange material with the pH adjusted solution (thereby loading the molybdenum on the anion exchange material) and then selectively eluting or extracting technetium-99m, formed by the radioactive decay of molybdenum-99, from the loaded anion exchange material with an acid.
  • the present method offers several advantages over prior art methods of preparing technetium-99m.
  • One of these is elimination of the need to separate radioactive molybdenum from other radioactive fission products.
  • Another is a considerable reduction in the radioactive waste disposal problem.
  • a still further advantage of this invention is that a product of high purity is obtained containing no traces of other radioactive fission products.
  • the purity of T0 is of considerable importance because of its medicinal use.
  • EXAMPLE 0.38 gram of M00 were placed in a inch aluminum capsule and sealed. The capsule was irradiated for hours in a neutron flux of 5 x10 n/cm. -sec. The resulting material containing radioactive M0 had an activity of about 135 m-ilicuries. Folio-wing irradiation the M00 was dissolved in approximately 10 ml. of 40 percent NH,OH.
  • the solution of ammonium molybdate was first neutralized to a pH of 7 with 6 M HNO and then acidified to a pH of 3.0 to 3.5 with 1 M HNO Prior to loading the above radioactive solution on an alumina anion-exchange column, the column containing 6 grams of 100 to 200 mesh alumina was washed with water and 0.1 M HNO Effluent from th washing step was acidic (pH 2-6) before the column was loaded.
  • the solution of ammonium molybdate after having its pH adjusted to 3.0 to 3.5 (and which contains M0 was loaded on the alumina column at a flow rate of about l-2 ml. per min. After the column was loaded, it was Washed with about 150 ml. of 0.1 M HCl in order to remove the small quantities of M0 that would subsequently wash through during Tc elution and contaminate the product solution.
  • the loaded column which contained about milicuries of activity can subsequently be eluted or milked repeatedly for Tc as it is formed with 25 ml. portions of 0.1 M HCl solution. This is done by passing the desired volume of 0.1 M HCl through the column and collecting the efiluent.
  • M00 is the preferred target material for the production of M0 other molybdenum containing materials may be used.
  • Such materials include, for example, molybdenum sesquioxide, M0 0 molybdenum dioxide, M00 molybdenum pentoxide, M0 0 hydrated molybdenum oxide (moly blue), Mo -xH O; molybdic acid H MoO and mixtures thereof.
  • Separation of Tc from Mo can be efifected by contacting the M0 (in the form of molybdate ions) with alumina, followed by selective removal of Tc (in the form of the TcO, ion) from the loaded alumina.
  • a column of alumina is preferably used, however, the separation can be made by slurrying the molybdate ion containing solution with finely divided alumina in a container (thereby loading the alumina with molybdate ions), separating the solids from the liquid, for example, by filtration and then removing the T0 from the alumina particles by reslurrying the alumina in an acid and then separating the dissolved Tc" from the unloaded alumina solids.
  • Use of a column is, of course, far simpler and more etficient.
  • the material is referred to in this disclosure as an inorganic anion exchange material, it is to be understood that the materials rather than the mechanism whether ion exchange or adsorption are intended thereby.
  • Alumina is the preferred exchange material.
  • Other materials which are chemically stable in the system, stable to the radiation emitted in the system, and which are able to exchange the molybendum and technetium ions can be used in place of alumina.
  • Such materials include the inorganic refractory oxides of zirconium, thorium, tungsten and silicon. Suitable illustrative materials include Zirconia (ZrO thoria (ThO tungsten trioxide (W and silica (SiO These materials have an affinity for anions when their surfaces have been rendered acidic.
  • Bases other than NH OH may be used to dissolve the irradiated molybdenum containing material, provided they will not interfere with subsequent loading and elution of the inorganic anion-exchange material.
  • Suitable bases include, for example, NaOH and KOH. Ammonium hydroxide is preferred.
  • the solution be acidified and be above pH 2.5 At a pH below 2.5 precipitation results, while at an alkaline pH the molybdate ion will not load properly on the exchange material.
  • the preferred range is pH 3.0 to 3.5. Adjustment of the pH and washing of the exchange material is preferably done with HNO HCl is the preferred acid used for the preferential elution of Tc from the exchange material. ther mineral acids, however, such as HNO may also be used.
  • the amount of radiation to which the molybdenum containing target material is subjected is not critical and both the time and intensity of the neutron flux may be varied considerably from that shown in the preferred embodiment. It is merely necessary that the target material be irradiated until the desired amount of Mo activity is formed. A convenient amount is about 100-300 millicuries of Mo" per loaded column, or about 200-1000 millicuries per gram of irradiated M00 What is claimed is:
  • a process for producing radioactive technetium-99m which comprises the steps of:
  • step (3) (4) contacting an inorganic anion exchange material with the pH adjusted solution of step (3) thereby loading the molybdenum on the exchange material
  • a process for producing radioactive technetium-99m which comprises the steps of:
  • step (3) adjusting the pH of the solution formed in step (2) to be acidic and above pH 2.5,
  • step (2) 8. The process of claim 7 wherein the pH of the solution formed in step (2) is adjusted to be within the range of 3.0 to 3.5.
  • a process for producing radioactive technetium-99m which comprises the steps of:
  • step (3) contacting a column of alumina with the pH adjusted solution of step (2), thereby loading the column with molybdate ions, and
  • a process for producing radioactive technetium- 99rn which comprises the steps of:
  • a process for producing a solution containing radioactive molybdenum-99, from which solution radioactive molybdenum-99 can be loaded onto an inorganic anion exchange material comprises the steps of:
  • step (3) adjusting the pH of the solution formed in step (2) to be acidic and above pH 2.5.
  • a process for producing a solution containing radioactive molybdenum-99, from which solution radioactive molybdenum-99 can be loaded onto alumina comprises the steps of:
  • step (3) adjusting the pH of the solution prepared in step (2) to be within the range of 3.0 to 3.5.
  • a process for producing the combination comprising alumina having loaded thereon radioactive molybdenum-99 which process comprises the steps of:
  • step (2) (3) adjusting the pH of the solution formed in step (2) to be acidic and above pH 2.5, and
  • step (3) (4) loading the pH adjusted solution of step (3) on a column of alumina.
  • a process for producing the combination comprising alumina having loaded thereon radioactive molybdenum-99 which process comprises the steps of (1) irradiating M00 in a neutron flux until the desired amount of M0 activity is formed,
  • step (3) adjusting the pH of the solution prepared in step (2) to be within the range of 3.0 to 3.5, and
  • step (3) (4) loading the pH adjusted solution of step (3) on a column of alumina.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
US399842A 1964-09-28 1964-09-28 Production of high purity radioactive isotopes Expired - Lifetime US3382152A (en)

Priority Applications (6)

Application Number Priority Date Filing Date Title
US399842A US3382152A (en) 1964-09-28 1964-09-28 Production of high purity radioactive isotopes
GB25433/66A GB1131546A (en) 1964-09-28 1966-06-08 Production of high-purity radioactive isotopes
CH850866A CH454805A (fr) 1964-09-28 1966-06-13 Procédé de préparation du molybdéne-99
DE19661544156 DE1544156A1 (de) 1964-09-28 1966-06-18 Verfahren zur Herstellung von hochreinen radioaktiven Isotopen
BE682978D BE682978A (fr) 1964-09-28 1966-06-22
FR66641A FR1486542A (fr) 1964-09-28 1966-06-23 Production d'isotopes radioactifs d'une haute pureté

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US399842A US3382152A (en) 1964-09-28 1964-09-28 Production of high purity radioactive isotopes
DE19661544156 DE1544156A1 (de) 1964-09-28 1966-06-18 Verfahren zur Herstellung von hochreinen radioaktiven Isotopen

Publications (1)

Publication Number Publication Date
US3382152A true US3382152A (en) 1968-05-07

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US399842A Expired - Lifetime US3382152A (en) 1964-09-28 1964-09-28 Production of high purity radioactive isotopes

Country Status (5)

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US (1) US3382152A (fr)
BE (1) BE682978A (fr)
CH (1) CH454805A (fr)
DE (1) DE1544156A1 (fr)
GB (1) GB1131546A (fr)

Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3466361A (en) * 1968-04-18 1969-09-09 Atomic Energy Commission Technetium-99m labeled chelates
FR2161893A1 (fr) * 1971-09-02 1973-07-13 Mallinckrodt Chemical Works
US3833469A (en) * 1971-08-31 1974-09-03 Atomic Energy Of Australia Process for the production of technetium-99m from neutron irradiated molybdenum trioxide
US4158700A (en) * 1976-03-08 1979-06-19 Karageozian Hampar L Method of producing radioactive technetium-99M
US4701308A (en) * 1984-12-28 1987-10-20 Commissariat A L'energie Atomique Process for the recovery of molybdenum-99 from an irradiated uranium alloy target
US20110206579A1 (en) * 2010-02-19 2011-08-25 Glenn Daniel E Method and apparatus for the extraction and processing of molybdenum-99
US20110272272A1 (en) * 2010-05-10 2011-11-10 Los Alamos National Security, Llc Method of producing molybdenum-99
US20110280357A1 (en) * 2010-05-14 2011-11-17 Stevenson Nigel R Tc-99m PRODUCED BY PROTON IRRADIATION OF A FLUID TARGET SYSTEM
US20120314828A1 (en) * 2010-02-01 2012-12-13 Arnd Baurichter METHOD AND DEVICE FOR PRODUCING 99mTc
JP2013035714A (ja) * 2011-08-08 2013-02-21 Japan Atomic Energy Agency 高濃度かつ高放射能をもつテクネチウム−９９ｍ溶液の製造方法
US8569713B2 (en) 2009-05-13 2013-10-29 Lantheus Medical Imaging, Inc. Radionuclide generator and method of sterilization
US20140234186A1 (en) * 2010-10-07 2014-08-21 Luis A.M.M. Barbosa Extraction Process
US9793023B2 (en) 2013-09-26 2017-10-17 Los Alamos National Security, Llc Recovery of uranium from an irradiated solid target after removal of molybdenum-99 produced from the irradiated target
US9842664B2 (en) 2013-09-26 2017-12-12 Los Alamos National Security, Llc Recovering and recycling uranium used for production of molybdenum-99

Families Citing this family (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
NL7008953A (fr) * 1969-06-20 1970-12-22
NL165321C (nl) * 1971-03-02 1981-03-16 Byk Mallinckrodt Cil Bv Werkwijze voor de vervaardiging van een radio-isotopen producerende generator.
DE2610948C3 (de) * 1976-03-16 1980-01-10 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur Gewinnung von Molybdän -99 aus mit Neutronen bestrahlter, spaltbare Stoffe und Spaltprodukte enthaltender Matrix
DE2610947C3 (de) * 1976-03-16 1980-01-10 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur Gewinnung von Molybdän-99 aus mit Neutronen bestrahlter, spaltbare Stoffe und Spaltprodukte enthaltender Matrix
US4280053A (en) * 1977-06-10 1981-07-21 Australian Atomic Energy Commission Technetium-99m generators
US20180244535A1 (en) 2017-02-24 2018-08-30 BWXT Isotope Technology Group, Inc. Titanium-molybdate and method for making the same

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None *

Cited By (20)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3466361A (en) * 1968-04-18 1969-09-09 Atomic Energy Commission Technetium-99m labeled chelates
US3833469A (en) * 1971-08-31 1974-09-03 Atomic Energy Of Australia Process for the production of technetium-99m from neutron irradiated molybdenum trioxide
FR2161893A1 (fr) * 1971-09-02 1973-07-13 Mallinckrodt Chemical Works
US4158700A (en) * 1976-03-08 1979-06-19 Karageozian Hampar L Method of producing radioactive technetium-99M
US4701308A (en) * 1984-12-28 1987-10-20 Commissariat A L'energie Atomique Process for the recovery of molybdenum-99 from an irradiated uranium alloy target
US8822950B2 (en) 2009-05-13 2014-09-02 Lantheus Medical Imaging, Inc. Radionuclide generator and method of sterilization
US8569713B2 (en) 2009-05-13 2013-10-29 Lantheus Medical Imaging, Inc. Radionuclide generator and method of sterilization
US9576692B2 (en) * 2010-02-01 2017-02-21 Siemens Aktiengesellschaft Method and device for producing 99mTc
US20120314828A1 (en) * 2010-02-01 2012-12-13 Arnd Baurichter METHOD AND DEVICE FOR PRODUCING 99mTc
US8449850B2 (en) * 2010-02-19 2013-05-28 Babcock & Wilcox Technical Services Group, Inc. Method and apparatus for the extraction and processing of molybdenum-99
US20110206579A1 (en) * 2010-02-19 2011-08-25 Glenn Daniel E Method and apparatus for the extraction and processing of molybdenum-99
US8450629B2 (en) * 2010-05-10 2013-05-28 Los Alamos National Security, Llc Method of producing molybdenum-99
US20110272272A1 (en) * 2010-05-10 2011-11-10 Los Alamos National Security, Llc Method of producing molybdenum-99
US20110280357A1 (en) * 2010-05-14 2011-11-17 Stevenson Nigel R Tc-99m PRODUCED BY PROTON IRRADIATION OF A FLUID TARGET SYSTEM
US9336916B2 (en) * 2010-05-14 2016-05-10 Tcnet, Llc Tc-99m produced by proton irradiation of a fluid target system
US20140234186A1 (en) * 2010-10-07 2014-08-21 Luis A.M.M. Barbosa Extraction Process
US9991012B2 (en) * 2010-10-07 2018-06-05 Mallinckrodt Nuclear Medicine Llc Extraction process
JP2013035714A (ja) * 2011-08-08 2013-02-21 Japan Atomic Energy Agency 高濃度かつ高放射能をもつテクネチウム−９９ｍ溶液の製造方法
US9793023B2 (en) 2013-09-26 2017-10-17 Los Alamos National Security, Llc Recovery of uranium from an irradiated solid target after removal of molybdenum-99 produced from the irradiated target
US9842664B2 (en) 2013-09-26 2017-12-12 Los Alamos National Security, Llc Recovering and recycling uranium used for production of molybdenum-99

Also Published As

Publication number Publication date
BE682978A (fr) 1966-12-22
DE1544156A1 (de) 1970-06-04
CH454805A (fr) 1968-04-30
GB1131546A (en) 1968-10-23

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