US3382152A - Production of high purity radioactive isotopes - Google Patents
Production of high purity radioactive isotopes Download PDFInfo
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- 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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- alumina
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- 230000002285 radioactive effect Effects 0.000 title claims description 36
- 238000004519 manufacturing process Methods 0.000 title description 4
- 239000000463 material Substances 0.000 claims description 35
- 238000000034 method Methods 0.000 claims description 30
- 230000008569 process Effects 0.000 claims description 24
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 19
- 229910052750 molybdenum Inorganic materials 0.000 claims description 19
- 239000011733 molybdenum Substances 0.000 claims description 19
- GKLVYJBZJHMRIY-OUBTZVSYSA-N Technetium-99 Chemical compound [99Tc] GKLVYJBZJHMRIY-OUBTZVSYSA-N 0.000 claims description 14
- 229940056501 technetium 99m Drugs 0.000 claims description 13
- 238000005349 anion exchange Methods 0.000 claims description 12
- 239000002253 acid Substances 0.000 claims description 11
- 230000000694 effects Effects 0.000 claims description 11
- 230000002378 acidificating effect Effects 0.000 claims description 10
- 230000004907 flux Effects 0.000 claims description 10
- 230000001678 irradiating effect Effects 0.000 claims description 8
- 150000001449 anionic compounds Chemical group 0.000 claims description 6
- 229910001412 inorganic anion Inorganic materials 0.000 claims description 6
- 230000005258 radioactive decay Effects 0.000 claims description 6
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 32
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 12
- ZOKXTWBITQBERF-AKLPVKDBSA-N Molybdenum Mo-99 Chemical compound [99Mo] ZOKXTWBITQBERF-AKLPVKDBSA-N 0.000 description 11
- 229950009740 molybdenum mo-99 Drugs 0.000 description 11
- 230000004992 fission Effects 0.000 description 8
- -1 molybdate ions Chemical class 0.000 description 7
- VHUUQVKOLVNVRT-UHFFFAOYSA-N Ammonium hydroxide Chemical compound [NH4+].[OH-] VHUUQVKOLVNVRT-UHFFFAOYSA-N 0.000 description 5
- 239000000908 ammonium hydroxide Substances 0.000 description 5
- 238000010828 elution Methods 0.000 description 4
- 238000005342 ion exchange Methods 0.000 description 4
- 150000002500 ions Chemical class 0.000 description 4
- 230000007246 mechanism Effects 0.000 description 4
- JFALSRSLKYAFGM-OIOBTWANSA-N uranium-235 Chemical compound [235U] JFALSRSLKYAFGM-OIOBTWANSA-N 0.000 description 4
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- APUPEJJSWDHEBO-UHFFFAOYSA-P ammonium molybdate Chemical compound [NH4+].[NH4+].[O-][Mo]([O-])(=O)=O APUPEJJSWDHEBO-UHFFFAOYSA-P 0.000 description 3
- 239000011609 ammonium molybdate Substances 0.000 description 3
- 229940010552 ammonium molybdate Drugs 0.000 description 3
- 235000018660 ammonium molybdate Nutrition 0.000 description 3
- 230000005855 radiation Effects 0.000 description 3
- 239000002901 radioactive waste Substances 0.000 description 3
- 238000000926 separation method Methods 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- 239000013077 target material Substances 0.000 description 3
- PNDPGZBMCMUPRI-HVTJNCQCSA-N 10043-66-0 Chemical compound [131I][131I] PNDPGZBMCMUPRI-HVTJNCQCSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 239000002775 capsule Substances 0.000 description 2
- QXYJCZRRLLQGCR-UHFFFAOYSA-N dioxomolybdenum Chemical compound O=[Mo]=O QXYJCZRRLLQGCR-UHFFFAOYSA-N 0.000 description 2
- MEFBJEMVZONFCJ-UHFFFAOYSA-N molybdate Chemical compound [O-][Mo]([O-])(=O)=O MEFBJEMVZONFCJ-UHFFFAOYSA-N 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- KJTLSVCANCCWHF-NJFSPNSNSA-N ruthenium-103 Chemical compound [103Ru] KJTLSVCANCCWHF-NJFSPNSNSA-N 0.000 description 2
- 239000007787 solid Substances 0.000 description 2
- 229910052713 technetium Inorganic materials 0.000 description 2
- ZNOKGRXACCSDPY-UHFFFAOYSA-N tungsten trioxide Chemical compound O=[W](=O)=O ZNOKGRXACCSDPY-UHFFFAOYSA-N 0.000 description 2
- 238000005406 washing Methods 0.000 description 2
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 description 1
- 241001279686 Allium moly Species 0.000 description 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- CIOAGBVUUVVLOB-NJFSPNSNSA-N Strontium-90 Chemical compound [90Sr] CIOAGBVUUVVLOB-NJFSPNSNSA-N 0.000 description 1
- 229910052776 Thorium Inorganic materials 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 150000001450 anions Chemical class 0.000 description 1
- 230000005255 beta decay Effects 0.000 description 1
- 210000004556 brain Anatomy 0.000 description 1
- GWXLDORMOJMVQZ-OUBTZVSYSA-N cerium-141 Chemical compound [141Ce] GWXLDORMOJMVQZ-OUBTZVSYSA-N 0.000 description 1
- GWXLDORMOJMVQZ-RNFDNDRNSA-N cerium-144 Chemical compound [144Ce] GWXLDORMOJMVQZ-RNFDNDRNSA-N 0.000 description 1
- TVFDJXOCXUVLDH-RNFDNDRNSA-N cesium-137 Chemical compound [137Cs] TVFDJXOCXUVLDH-RNFDNDRNSA-N 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000003745 diagnosis Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 230000008030 elimination Effects 0.000 description 1
- 238000003379 elimination reaction Methods 0.000 description 1
- 239000000284 extract Substances 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 210000004185 liver Anatomy 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 235000010755 mineral Nutrition 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 229910000476 molybdenum oxide Inorganic materials 0.000 description 1
- HOOANQZZUGPTRH-UHFFFAOYSA-N molybdenum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Mo+3].[Mo+3] HOOANQZZUGPTRH-UHFFFAOYSA-N 0.000 description 1
- VLAPMBHFAWRUQP-UHFFFAOYSA-L molybdic acid Chemical compound O[Mo](O)(=O)=O VLAPMBHFAWRUQP-UHFFFAOYSA-L 0.000 description 1
- GUCVJGMIXFAOAE-NJFSPNSNSA-N niobium-95 Chemical compound [95Nb] GUCVJGMIXFAOAE-NJFSPNSNSA-N 0.000 description 1
- 210000000056 organ Anatomy 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- KJTLSVCANCCWHF-BKFZFHPZSA-N ruthenium-106 Chemical compound [106Ru] KJTLSVCANCCWHF-BKFZFHPZSA-N 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 230000002269 spontaneous effect Effects 0.000 description 1
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 description 1
- ZCUFMDLYAMJYST-UHFFFAOYSA-N thorium dioxide Chemical compound O=[Th]=O ZCUFMDLYAMJYST-UHFFFAOYSA-N 0.000 description 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 description 1
- 229910052721 tungsten Inorganic materials 0.000 description 1
- 239000010937 tungsten Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- VWQVUPCCIRVNHF-NJFSPNSNSA-N yttrium-91 Chemical compound [91Y] VWQVUPCCIRVNHF-NJFSPNSNSA-N 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
- QCWXUUIWCKQGHC-RNFDNDRNSA-N zirconium-95 Chemical compound [95Zr] QCWXUUIWCKQGHC-RNFDNDRNSA-N 0.000 description 1
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)
Description
United States Patent 3,382,152 PRODUCTION OF HIGH PURITY RADIOACTIVE ISOTOPES Ephraim Lieberman, Suifern, N.Y., and Wayne J. Gemmill, Milford, Pa., assignors to Union Carbide Corporation, a corporation of New York No Drawing. Filed Sept. 28, 1964, Ser. No. 399,842
' 18 Claims. (Cl. 176-16) 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.
Since the radioisotope sought to be used has such a short half-life, it is common practice to ship the users of the isotope the parent element; in this case M0 The user then extracts the Tc from the Mo as his needs require.
In the past, 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. One is that the M0 has to be separated from the numerous other radioactive fission products of U-235 such as strontium-90, yttrium-91, zirconium-95, niobium-95, ruthenium-103, ruthenium-106, iodine-131, cerium-141, cesium-137, cerium-144, prometh-ium-l47 and many others. Some of these fission products are long lived, and due to their radioactivity are difficult to handle without elaborate shielding.
As a result of separation problems, pure molybdenum-99 and consequently pure Tc cannot be obtained from U-235 fissioning because traces of fission products such as iodine-131 and ruthenium-103 frequently remain in the separated product. In addition, this technique presents radioactive waste disposal problems.
It is an object of this invention to provide a more efficient method of producing radioactive molybdenum from which radioactive technetium may be extracted. It is another object of this invention to produce radioactive molybdenum by a method which avoids the need for separating radioactive fission products and avoids problems relating to disposing of radioactive waste resulting from the fissioning of U-235. It is another object of this invention to prepare high purity technetium-99 which contains no traces of fission products.
It has now been discovered that the aforementioned objects can be achieved by 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.
In order to more fully understand the invention, the following example, which is the preferred embodiment of the invention, is given by way of illustration only and is not intended to limit the scope of this invention.
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.
Numerous variations of the preferred embodiment described above may be practiced, as will be apparent to those skilled in the art, without departing from the basic concepts of the present invention. Thus, while 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 exact nature of the exchange mechanism by which the molybdenum is loaded on alumina and by which the T0 is eluted is not entirely certain. While not wishing to be limited to any theory, it is believed to be an ion exchange mechanism whereby molybdate ions are loaded on the acidified alumina column in exchange for OH ions. Upon elution, the To is removed from the column as pertechnate, TcO ions in exchange for C1 ions. However, the ion exchange reaction appears to be limited to a surface phenomena, and it is therefore possible that the mechanism is actually a surface adsorption phenomena. It is most likely a combination of both ion exchange and adsorption. Thus, While 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, however, 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.
Following dissolution of the irradiated molybdenum containing material it is essential that 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:
1. A process for producing radioactive technetium-99m which comprises the steps of:
(l) irradiating a base-soluble molybdenum containing material in a neutron flux until the desired amount of M0 activity is formed,
(2) dissolving the irradiated molybdenum containing material, containing the radioactive M0, in a base,
(3) adjusting the pH of the solution prepared in step (2) to be acidic and above pH 2.5,
(4) contacting an inorganic anion exchange material with the pH adjusted solution of step (3) thereby loading the molybdenum on the exchange material, and
(5) extracting technetium-99m, formed by the radioactive decay of M0 from the loaded anion exchange material with an acid.
2. The process of claim 1 wherein the inorganic anion exchange material is alumina.
3. The process of claim 2 wherein the base used to dissolve the irradiated material is ammonium hydroxide.
4. The process of claim 2 wherein the pH of the solution prepared in step (2) is adjusted to be within the range of 3.0 to 3.5.
5. The process of claim 2 wherein the particle size of the alumina is 100 to 200 mesh.
6. The process of claim 2 wherein the acid used for extracting the technetium-99m from the loaded alumina is hydrochloric acid.
7. A process for producing radioactive technetium-99m which comprises the steps of:
(1) irradiating M00 in a neutron flux until the desired amount of M0 activity is formed,
(2) dissolving the irradiated M00 containing radioactive Mo in ammonium hydroxide,
(3) adjusting the pH of the solution formed in step (2) to be acidic and above pH 2.5,
(4) contacting a column of alumina with the pH adjusted solution of step (3) thereby loading the alumina With molybdate ions, and
(5) eluting technetium-99m, formed by the radioactive decay of M0 from the loaded alumina column with hydrochloric acid.
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.
9. A process for producing radioactive technetium-99m which comprises the steps of:
(1) providing a solution of ammonium molybdate in which at least some of the molybdenum is radioactive 99 (2) adjusting the pH of the solution to be acidic and above pH 2.5,
(3) contacting a column of alumina with the pH adjusted solution of step (2), thereby loading the column with molybdate ions, and
(4) eluting technetium-99m, formed by the radioactive decay of M0 from the loaded alumina column with an acid.
10. The process of claim 9 wherein the pH of the solution is adjusted to be within the range of 3.0 to 3.5.
11. The process of claim 9 wherein the acid used for eluting the loaded alumina column is hydrochloric acid.
12. A process for producing radioactive technetium- 99rn which comprises the steps of:
(1) providing a solution containing molybdate ions, which is acidic, has a pH above 2.5, and in which at least some of the molybdenum is radioactive M0 (2) loading a column of alumina with the solution of step 1) and (3) eluting technetium-99m, formed by the radioactive decay of M0 from the loaded alumina column with an acid.
13. The process of claim 12 wherein the pH of the solution is adjusted to be within the range of 3.0 to 3.5.
14. The process of claim 12 wherein the acid used for eluting the loaded alumina column is hydrochloric acid.
15. 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, which process comprises the steps of:
(l) irradiating M00 in a neutron flux until the desired amount of Mo activity is formed,
(2) dissolving the irradiated M00 containing radioactive Mo in a base, and
(3) adjusting the pH of the solution formed in step (2) to be acidic and above pH 2.5.
16. A process for producing a solution containing radioactive molybdenum-99, from which solution radioactive molybdenum-99 can be loaded onto alumina, which process comprises the steps of:
(l) irradiating M00 in a neutron flux until the desired amount of Mo activity is formed,
(2) dissolving the irradiated M00 containing radioactive M0 in ammonium hydroxide and,
(3) adjusting the pH of the solution prepared in step (2) to be within the range of 3.0 to 3.5.
17. 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 Mo activity is formed,
(2) dissolving the irradiated M00 containing radioactive M0 in a base,
5 (3) adjusting the pH of the solution formed in step (2) to be acidic and above pH 2.5, and
(4) loading the pH adjusted solution of step (3) on a column of alumina.
18. 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,
(2) dissolving the irradiated MoO containing radioactive M0 in ammonium hydroxide,
(3) adjusting the pH of the solution prepared in step (2) to be within the range of 3.0 to 3.5, and
(4) loading the pH adjusted solution of step (3) on a column of alumina.
References Cited O 1 CARL D. QUARF'ORTH, Primary Examiner.
L. DEWAY'NE RUTLEDGE, Examiner.
H. E. BEHREND, Assistant Examiner.
Claims (1)
1. A PROCESS FOR PRODUCING RADIOACTIVE TECHNETIUM-99M WHICH COMPRISES THE STEPS OF: (1) IRRADIATING A BASE-SOLUBLE MOLYBDENUM CONTAINING MATERIAL IN A NEUTRON FLUX UNTIL THE DESIRED AMOUNT OF MO99 ACTIVITY IS FORMED, (2) DISSOLVING THE IRRADIATED MOLYBDENUM CONTAINING MATERIAL, CONTAINING THE RADIOACTIVE MO99, IN A BASE, (3) ADJUSTING THE PH OF THE SOLUTION PREPARED IN STEP (2) TO BE ACIDIC AND ABOVE PH 2.5, (4) CONTACTING AN INORGANIC ANION EXCHANGE MATERIAL WITH THE PH ADJUSTED SOLUTION OF STEP (3) THEREBY LOADING THE MOLYBDENUM ON THE EXCHANGE MATERIAL, AND (5) EXTRACTING TECHNETIUM-99M, FORMED BY THE RADIOACTIVE DECAY OF MO99, FROM THE LOADED ANION EXCHANGE MATERIAL WITH AN ACID.
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 (en) | 1964-09-28 | 1966-06-13 | Process for preparing molybdenum-99 |
| DE19661544156 DE1544156A1 (en) | 1964-09-28 | 1966-06-18 | Process for the production of high-purity radioactive isotopes |
| BE682978D BE682978A (en) | 1964-09-28 | 1966-06-22 | |
| FR66641A FR1486542A (en) | 1964-09-28 | 1966-06-23 | Production of high purity radioactive isotopes |
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 (en) | 1964-09-28 | 1966-06-18 | Process for the production of high-purity radioactive isotopes |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| US3382152A true US3382152A (en) | 1968-05-07 |
Family
ID=25752849
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US399842A Expired - Lifetime US3382152A (en) | 1964-09-28 | 1964-09-28 | Production of high purity radioactive isotopes |
Country Status (5)
| Country | Link |
|---|---|
| US (1) | US3382152A (en) |
| BE (1) | BE682978A (en) |
| CH (1) | CH454805A (en) |
| DE (1) | DE1544156A1 (en) |
| GB (1) | GB1131546A (en) |
Cited By (14)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3466361A (en) * | 1968-04-18 | 1969-09-09 | Atomic Energy Commission | Technetium-99m labeled chelates |
| FR2161893A1 (en) * | 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 (en) * | 2011-08-08 | 2013-02-21 | Japan Atomic Energy Agency | Method for producing technetium-99m solution having high concentration and high radioactivity |
| 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)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| FR2046951B1 (en) * | 1969-06-20 | 1974-09-06 | Union Carbide Corp | |
| NL165321C (en) * | 1971-03-02 | 1981-03-16 | Byk Mallinckrodt Cil Bv | METHOD FOR THE MANUFACTURE OF A RADIO ISOTOPE GENERATOR GENERATOR. |
| DE2610948C3 (en) * | 1976-03-16 | 1980-01-10 | Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe | Process for the extraction of molybdenum -99 from a matrix containing fissile substances and fission products irradiated with neutrons |
| DE2610947C3 (en) * | 1976-03-16 | 1980-01-10 | Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe | Process for the extraction of molybdenum-99 from a matrix containing fissile substances and fission products irradiated with neutrons |
| 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 |
-
1964
- 1964-09-28 US US399842A patent/US3382152A/en not_active Expired - Lifetime
-
1966
- 1966-06-08 GB GB25433/66A patent/GB1131546A/en not_active Expired
- 1966-06-13 CH CH850866A patent/CH454805A/en unknown
- 1966-06-18 DE DE19661544156 patent/DE1544156A1/en active Pending
- 1966-06-22 BE BE682978D patent/BE682978A/xx unknown
Non-Patent Citations (1)
| Title |
|---|
| None * |
Cited By (20)
| 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 (en) * | 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 (en) * | 2011-08-08 | 2013-02-21 | Japan Atomic Energy Agency | Method for producing technetium-99m solution having high concentration and high radioactivity |
| 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 (en) | 1966-12-22 |
| DE1544156A1 (en) | 1970-06-04 |
| GB1131546A (en) | 1968-10-23 |
| CH454805A (en) | 1968-04-30 |
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