US3468808A - Production of high purity radioactive technetium-99m - Google Patents

Production of high purity radioactive technetium-99m Download PDF

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Publication number
US3468808A
US3468808A US646453A US3468808DA US3468808A US 3468808 A US3468808 A US 3468808A US 646453 A US646453 A US 646453A US 3468808D A US3468808D A US 3468808DA US 3468808 A US3468808 A US 3468808A
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technetium
molybdenum
radioactive
slurry
production
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Expired - Lifetime
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US646453A
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English (en)
Inventor
Hirofumi Arino
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CINTICHEM Inc
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Union Carbide Corp
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Assigned to CINTICHEM, INC. reassignment CINTICHEM, INC. ASSIGNMENT OF ASSIGNORS INTEREST. Assignors: UNION CARBIDE CORPORATION, A CORP. OF NY
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    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22BPRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
    • C22B61/00Obtaining metals not elsewhere provided for in this subclass
    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21GCONVERSION OF CHEMICAL ELEMENTS; RADIOACTIVE SOURCES
    • G21G1/00Arrangements for converting chemical elements by electromagnetic radiation, corpuscular radiation or particle bombardment, e.g. producing radioactive isotopes
    • G21G1/0005Isotope delivery systems

Definitions

  • This invention relates to a novel process for the production of radioactive technetium-99m.
  • this invention relates to a novel process for the production of radioactive technetium-99m in high yields.
  • a further aspect of this invention is directed to a novel process for the production of radioactive technetium-99m which can be obtained in a high degree of purity.
  • technetium- 99m is an extremely useful tool for diagnosis.
  • High purity technetium-99m is used primarily as a radioisotope in a variety of medical research and diagnosis. It is well suited for liver, lung, blood pool and tumor scanning, and is preferred over other radioactive isotopes because of its short half-life which results in reduced exposure of the organs to radiation.
  • technetium-99m can also be employed in industrial applications, such as in the measurement of flow rates, process control, radiometric chemistry, and the like.
  • radioactive molybdenum- 99..Ihe user then extracts the technetium from the molybdenum-99 as his needs require.
  • radioactive technetium-99m has been produced by a variety of methods.
  • M. S. Faddeeva et al., Zhur. Neorg. Khim., 3, 165-166 (1958) has disclosed a process for extracting technetium-99m from 6 N aqueous K CO solutions containing dissolved molybdenum-99* containing material, using methyl ethyl ketone as the extracting medium, followed by washing the ketone solutions with K C aqueous solution.
  • the technetium-99m recovered by this process was not pure, since the product contained detectable K CO and would therefore not be useable for many purposes, such as for medical purposes.
  • molybdenum trioxide is molybdenum trioxide.
  • other compounds it is often necessary to isolate the molybdenum component after irradiation.
  • Illustrative compounds which can be employed as the source of molybdenum-99 include, among others, molybdenum metal, molybdenum nitrate, molybdenum sulfate, organic molybdenum compounds such 'as molybdenum acetylacetonates, and fissionable materials such as uranium-235, uranium- 238, plutonium-239, and the like.
  • Irradiation of compounds to produce molybdenum-99 is a well known technique and can be effected by placing the proper compound in the irradiation zone of a nuclear reactor, particle generator, or neutron isotopic source.
  • the irradiated compound is dissolved in a suitable solvent.
  • a suitable solvent such as sodium hydroxide, ammonium hydroxide, and the like, the techniques to dissolve and isolate a pure molybdenum- 99 solution are well known in the art.
  • molybdenum solution such as aqueous ammonium molybdate is contacted with oxidized zirconium salts.
  • the oxidized zirconium salts are prepared by contacting a compound, such as hydrous zirconium oxide, with an oxidizing agent, in the presence of an acid.
  • Suitable oxidizing agents which can be employed include, among others, bromine water, chlorine water, iodide water, permanganate salts, such as potassium permanganate, chlorate salts, such as potassium chlorate, hydrogen peroxide, organic peroxides, such as benzoyl peroxide and the like.
  • the pH of the contacted solution is adjusted to a range between 2 to 7 and more preferably between 3.5 and 6.0. Normally, it is preferable to heat the solution during pH adjustment and control and to maintain this heat for a duration of approximately twenty minutes to insure adsorption of the molybdenum on the zirconium substrate. Temperature is not necessarily critical and need only be sufiicient to insure complete reaction of the molybdenum and the oxidized zirconium salt. In practice, temperatures greater than 70 C., have been found satisfactory, with the preferred temperature being the boiling point of the slurry.
  • the zirconium substrate containing the molybdenum is then transferred to an appropriate elution system such as a column, or vessel, preferably glass, or other inert material.
  • an appropriate elution system such as a column, or vessel, preferably glass, or other inert material.
  • the supernatant liquid is allowed to drain or removed by filtration or decantation and the substrate washed with isotonic saline.
  • the technetium-99m in the column or vessel which contains 99Mo-99mTc activity can subsequently be isolated, e.g., milked, filtered, centrifuged or the like for technetium-99m as it is formed with an acidic, neutral or basic solution.
  • an acidic, neutral or basic solution e.g., milked, filtered, centrifuged or the like for technetium-99m as it is formed with an acidic, neutral or basic solution.
  • the process of the present invention provides a simple method for the preparation of technetium-99m in a high degree of efficiency.
  • recovery of technetium-99m can be effected with isotonic saline in elficiencies as high as 95% and higher, over a pH range of about 4.0 to about 7.0 without appreciable dissolution of the zirconium substrate or removal of any molybdenum from the zirconium substrate.
  • a further advantage characteristic of the process of this invention is that the substrate and/or the entire elution system can be sterilized, i.e., by autoclaving at the normally prescribed temperatures and pressures.
  • EXAMPLE 1 To 100 grams of Bio-Rad hydrous zirconium oxide (100-200 mesh) was added 100 milliliters of 0.1 MHCl and 10 milliliters of saturated bromine water. The mixture was stirred and allowed to stand for 10 minutes. Thereafter l5 milliliters of 1 M NaOH was added to the slurry. A sufficient volume of this slurry was transferred into a 150' milliliter beaker to provide 1 milliliter of slurry per 57 milligrams of molybdenum. Thereafter the slurry was washed three times with water and four drops of saturated bromine water added.
  • the column was tested for molybdenum break-through 4 by radiometric analysis and no molybdenum-99 was observed. Chemical purity was tested by emission spectroscopy for the major elements of the column substrate, i.e., zirconium, and none was detectable.
  • EXAMPLE 2 A comparison of adsorption-elution characteristics of the column of Example 1 and one prepared in accordance with a recent method, wherein an alumina column is employed the data obtained is set forth in Table I below:
  • radiometric analysis of the eluted technetium-99m indicates that it contains up to percent of the available technetium-99m and the radionuclidic purity is greater than 99.99 percent.
  • the total metal element impurity is less than 1 part per million as determined by emission spectroscopy techniques.
  • the substrate and/or the entire elution system can be sterilized by acceptable autoclave techniques with no reduction in radionuclidic impurity, no increase in the metal element impurities and no reduction in the amount of technetium-99m recoverable.
  • said oxidizing agent is selected from the group consisting of bromine water, chlorine water, iodine Water, potassium permanganate, potgssium chlorate, hydrogen peroxide, and benzoylper- 0x1 e.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Medicines Containing Antibodies Or Antigens For Use As Internal Diagnostic Agents (AREA)
US646453A 1967-06-16 1967-06-16 Production of high purity radioactive technetium-99m Expired - Lifetime US3468808A (en)

Applications Claiming Priority (1)

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US64645367A 1967-06-16 1967-06-16

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US (1) US3468808A (en:Method)
BE (1) BE716569A (en:Method)
DE (1) DE1758118C3 (en:Method)
FR (1) FR1561828A (en:Method)
GB (1) GB1207246A (en:Method)
IL (1) IL29607A (en:Method)
NL (1) NL6804929A (en:Method)
SE (1) SE350954B (en:Method)

Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2207309A1 (de) * 1971-03-02 1972-09-07 Philips Nv Verfahren zur Herstellung eines Radioisotopen erzeugenden Generators mit einem verbesserten Eluierungsgrad und durch dieses Verfahren hergestellter Generator
US4010109A (en) * 1973-07-02 1977-03-01 Kurt Sauerwein Device for marking fluent materials
US4158700A (en) * 1976-03-08 1979-06-19 Karageozian Hampar L Method of producing radioactive technetium-99M
US4206358A (en) * 1977-10-19 1980-06-03 Australian Atomic Energy Commission Technetium-99 generators
US20110206579A1 (en) * 2010-02-19 2011-08-25 Glenn Daniel E Method and apparatus for the extraction and processing of molybdenum-99
CN103650061A (zh) * 2011-07-13 2014-03-19 马林克罗特有限公司 制备Tc-99m的方法
US20160042826A1 (en) * 2014-08-06 2016-02-11 Research Triangle Institute High efficiency neutron capture product production
US9576690B2 (en) 2012-06-15 2017-02-21 Dent International Research, Inc. Apparatus and methods for transmutation of elements
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
CN110325271A (zh) * 2017-02-24 2019-10-11 Bwxt同位素技术集团有限公司 金属-钼酸盐及其制造方法
WO2020005674A3 (en) * 2018-06-20 2020-02-06 BWXT Isotope Technology Group, Inc. SYSTEM AND METHOD FOR EVALUATING ELUTION EFFICIENCY AND RADIOPURITY OF Tc-99m GENERATORS
CN113168929A (zh) * 2019-03-11 2021-07-23 新华锦集团有限公司 99mTc分离提纯系统及99mTc分离提纯方法
CN114121330A (zh) * 2021-11-11 2022-03-01 中国核动力研究设计院 一种钼锝发生器、制备方法及装置

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4280053A (en) * 1977-06-10 1981-07-21 Australian Atomic Energy Commission Technetium-99m generators

Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB896758A (en) * 1959-11-13 1962-05-16 Atomic Energy Authority Uk Improvements in or relating to the separation of technetium from fission product solutions

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB896758A (en) * 1959-11-13 1962-05-16 Atomic Energy Authority Uk Improvements in or relating to the separation of technetium from fission product solutions

Cited By (20)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2207309A1 (de) * 1971-03-02 1972-09-07 Philips Nv Verfahren zur Herstellung eines Radioisotopen erzeugenden Generators mit einem verbesserten Eluierungsgrad und durch dieses Verfahren hergestellter Generator
US4010109A (en) * 1973-07-02 1977-03-01 Kurt Sauerwein Device for marking fluent materials
US4158700A (en) * 1976-03-08 1979-06-19 Karageozian Hampar L Method of producing radioactive technetium-99M
US4206358A (en) * 1977-10-19 1980-06-03 Australian Atomic Energy Commission Technetium-99 generators
US20110206579A1 (en) * 2010-02-19 2011-08-25 Glenn Daniel E Method and apparatus for the extraction and processing of molybdenum-99
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
CN103650061A (zh) * 2011-07-13 2014-03-19 马林克罗特有限公司 制备Tc-99m的方法
US9576690B2 (en) 2012-06-15 2017-02-21 Dent International Research, Inc. Apparatus and methods for transmutation of elements
US9842664B2 (en) 2013-09-26 2017-12-12 Los Alamos National Security, Llc Recovering and recycling uranium used for production of molybdenum-99
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
US20160042826A1 (en) * 2014-08-06 2016-02-11 Research Triangle Institute High efficiency neutron capture product production
CN110325271A (zh) * 2017-02-24 2019-10-11 Bwxt同位素技术集团有限公司 金属-钼酸盐及其制造方法
CN110325271B (zh) * 2017-02-24 2022-11-01 Bwxt同位素技术集团有限公司 金属-钼酸盐及其制造方法
WO2020005674A3 (en) * 2018-06-20 2020-02-06 BWXT Isotope Technology Group, Inc. SYSTEM AND METHOD FOR EVALUATING ELUTION EFFICIENCY AND RADIOPURITY OF Tc-99m GENERATORS
CN112384991A (zh) * 2018-06-20 2021-02-19 Bwxt同位素技术集团有限公司 用于评估锝-99m发生器的洗脱效率和放射性纯度的系统和方法
US11391853B2 (en) 2018-06-20 2022-07-19 BWXT Isotope Technology Group, Inc. System and method for evaluating elution efficiency and radiopurity of tc-99m generators
CN113168929A (zh) * 2019-03-11 2021-07-23 新华锦集团有限公司 99mTc分离提纯系统及99mTc分离提纯方法
CN113168929B (zh) * 2019-03-11 2024-04-19 新华锦集团有限公司 99mTc分离提纯系统及99mTc分离提纯方法
CN114121330A (zh) * 2021-11-11 2022-03-01 中国核动力研究设计院 一种钼锝发生器、制备方法及装置
CN114121330B (zh) * 2021-11-11 2024-05-14 中国核动力研究设计院 一种钼锝发生器、制备方法及装置

Also Published As

Publication number Publication date
IL29607A (en) 1971-10-20
DE1758118A1 (de) 1970-12-23
GB1207246A (en) 1970-09-30
BE716569A (en:Method) 1968-12-16
DE1758118C3 (de) 1974-05-30
FR1561828A (en:Method) 1969-03-28
DE1758118B2 (de) 1973-10-18
SE350954B (en:Method) 1972-11-13
NL6804929A (en:Method) 1968-12-17

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Owner name: CINTICHEM, INC., NEW YORK

Free format text: ASSIGNMENT OF ASSIGNORS INTEREST;ASSIGNOR:UNION CARBIDE CORPORATION, A CORP. OF NY;REEL/FRAME:003951/0224

Effective date: 19810428

Owner name: CINTICHEM, INC., A CORP. OF DE, NEW YORK

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Owner name: CINTICHEM, INC., LONG MEADOW ROAD, P.O. BOX 204, T

Free format text: ASSIGNMENT OF ASSIGNORS INTEREST.;ASSIGNOR:UNION CARBIDE CORPORATION, A CORP. OF NY;REEL/FRAME:003951/0224

Effective date: 19810428