Method of obtaining radioisotope molybdenum-99

FIELD: chemistry.

SUBSTANCE: method of obtaining radioisotope 99Mo includes the irradiation of a target by a beam of neutrons with the following extraction of the target radioisotope, formed as a result of a 98Mo(n,γ)99Mo reaction. As the target applied are nanoparticles of metallic molybdenum or its compounds, insoluble in water, or a water solution of alkali, or water NH4OH solution. Irradiation of the target is carried out in water, or water alkali solution, or water NH4OH solution. The target radioisotope 99Mo is separated in the composition of an anion of water-soluble molybdate(99MoO4)-2 from nanoparticles.

EFFECT: increase of the specific activity of 99Mo radioisotope.

 

Area of technology

The invention relates to a reactor of technology for production of radioisotopes for nuclear medicine.

It is known that one of the most popular diagnostic radioisotopes is currently99mTS. Up to 80% of diagnostic procedures in the world is carried out using99mTC, which is obtained by using99Mo/99mTc isotope generators.

For the parent99Mo applies one of the following methods:

- the selection99Mo from fission fragments of the uranium target;

- radiation-capture method based on the reaction98Mo(n, γ)99Mo;

- cyclotron method based on the reaction100Mo(p, pn)99Mo.

The main quantity of the commodity99Mo in the world today is produced from fission fragments of highly enriched uranium. Radiative capture method and cyclotron method currently have limited application.

Each of these methods has its advantages and disadvantages.

The present invention can be used to improve the radiation-capture method to increase the specific activity of99Mo, allowing its use in standard sorption generators that use today "frag"99Mo.

Background art.

Now for comfort�of specific activity of 99Mo received a radiation-capture method, offers a variety of ways, based on the effect of Szilard-Chalmers. The essence of the effect of Szilard-Chalmers is as follows. As a result of capture of a neutron, the nucleus moves to an excited state. When removing the excitation by the emission of prompt gamma-quantum recoil (in this case99Mo) receives an impulse to break the chemical bonds of atoms and displacement of the resulting radionuclide inside the target material, or release it outside of the structural element of the target (if the characteristic size of the structural element of the target is less than the length of the run of the recoil nucleus in the target material).

The known method of increasing the specific activity of99Mo [Radchenko V. M., Romanov K. V., G. I. Maslakov, V. D. Drawn, Goncharenko Y. D. "a Method for producing radionuclide99Mo". RF patent №2426184, Vol. No. 22, published on 10.08.2011]. As starting material, the authors have proposed the use of a refractory radiation and thermally stable molybdenum compounds in the form of particles smaller than 100 nanometers (nm), irradiation of which is performed by neutron flux densities of more than 1014cm-2with-1within 7÷15 days, and radioisotope99Mo is isolated from the surface layer of the particles by dissolving this layer in acid or alkali.

The main lack�atcom this method is the low specific activity of 99Mo. When dissolved after irradiation of the surface of the layer of nanoscale particles of the target (which, according to the authors, should concentrate the radioisotope99Mo) in a solution together with99Mo goes a large number of target atoms (the authors give the values of 19% and 25%). According to the patent data, the enrichment of99Mo was only 1.5÷1.6 times. The authors present the value of specific activity of99Mo obtained by the specified method at the level of 1 CI/g, which is significantly inferior to the specific activity of shrapnel99Mo (≈105CI/g). When the specific activity of99Mo at 1 CI/g you cannot use the standard99Mo/99mTc-generator sorption type, because you'll need the large column and, accordingly, the size of the generator will also become unacceptably large, resulting in increased weight and size characteristics of radiation protection. In addition, elution99mTc from such a column will need a large flow of eluate, leading to the decrease of the activity concentration of the solution up to the concentration of99mTc.

The known method of increasing the specific activity of99Mo [B. S. Tomar, O. M. Steineback, V. E. Terpstra, P. Bode and H. Th. Wolterbeek ' Studies on production of high specific activity99Mo and90Y by Szilard Chalmers reaction", Radiochim. Acta 98, 499-506 (2010)].

The work investigated the possibility of using�Yu effect of Szilard-Chalmers to increase the specific activity of 99Mo received a radiation-capture method. As targets used ORGANOMETALLIC compound of molybdenum natural isotopic composition (Mo-oxinate). Irradiation was performed at the reactor in a neutron flux of 1012with-1cm-2. The irradiation time varied from 15 minutes to 4 hours. After irradiation of the target was allowed to decay of short-lived isotopes101Mo and101Tc, then was dissolved in dichloromethane, then separated radioisotope99Mo extraction in the aqueous phase. The investigation of the dependence of the output and the enrichment factor (the ratio of specific activity of99Mo after separation from the target material to a specific activity prior to separation) from the pH. Under optimum conditions of separation and irradiation was obtained for the enrichment coefficient equal to ~200.

The main disadvantages of this method are the complexity of the synthesis and destruction of the source material target (ORGANOMETALLIC compounds) under the action of neutrons and gamma rays during irradiation in the reactor, significantly reducing the ratio of enrichment of99Mo. The work data, only 4 hours of exposure to relatively low neutron flux ratio of enrichment of99Mo falls three times. Given the above, there is reason to believe that when irradiated Mo-oxinate in the Techa�their several days (time necessary to produce practically significant activity99Mo) destruction of the target material can negate the potential for increasing the specific activity of99Mo, based on the effect of Szilard-Chalmers.

As a prototype the selected method proposed in [Artyukhov Α.Α., Zagryadskiy V. A., Y. M. Kravets, L. I. Menshikov, Ryzhkov, A. V., Chuvilin, D. Y. "a Method of producing molybdenum-99". RF patent №2490737, from 20.08.2013]. The authors propose to use the target in the form of a structured material composed of nanoparticles of molybdenum or its compounds, surrounded by a buffer in the form of a solid substance, soluble in water or other solvents, and the d (the characteristic size of the nanoparticles) is chosen from the condition λ/d >> 1, where λ is the path length in the material of the nanoparticle recoil atoms99Mo. After irradiation of the target nanoparticles and buffer share one of the known methods, after which the buffer is sent to the radiochemical processing for separation of radioisotope99Mo, nanoparticles and recycled to the reactor core in the new target. Furthermore, in the claims the authors specified the size of the nanoparticles (≤5 nm) and a version of the buffer (NaCl).

The main disadvantages of the prototype are as follows:

1. The task of creating a structured material, comprising innocentis molybdenum or its compounds, surrounded by a buffer in the form of a solid substance, soluble in water or other solvents, it is technologically difficult (in the prototype is not specified how this can be done).

2. The success of enrichment of99Mo (and, accordingly, the value of the specific activity of the resulting99Mo) depend on how efficiently manages to separate the buffer from the nanoparticles of molybdenum, which, in turn, is connected with the choice of a particular buffer. However, in the main part of the formula of the invention, the prototype does not offer unambiguous composition of the buffer and separation from nanoparticles of molybdenum.

3. The proposed in claim 6 of the invention an embodiment of the method involves the localization of "hot" atoms99Mo in NaCl, and the subsequent separation of99Mo nanoparticles from the target by dissolving NaCl in water. However, when you dissolve NaCl in water may cause the formation of insoluble oxides99MoO2and99MoO3that is difficult to separate the nanoparticles from the target.

Disclosure of the invention

The technical result of the proposed method is to increase the specific activity of99Mo received radiation capture method by the reaction98Mo(n, γ)99Mo under irradiation in a nuclear reactor target of natural or enriched in the isotope98Mo molybdenum. In this case, the value of the specific activity�and, achieved by the proposed method, allows to use the obtained99Mo standard sorption generators that use today "frag"99Mo.

To achieve this goal, a method of producing the radioisotope99Mo, including irradiation by the neutron flux of the target, representing the metal nanoparticles of molybdenum or its compounds, followed by separation of the target radioisotope formed in the98Mo(n, γ)99Mo reaction, the compounds use of molybdenum compounds, insoluble in water or aqueous alkali solution, or an aqueous solution of NH4OH, the irradiation of the target is carried out in water or an aqueous alkali solution, or an aqueous solution of NH4OH, and separate99Mo in the composition of the anion of the water-soluble molybdate (99MoO4)-2from nanoparticles.

A method of producing the radioisotope99Mo, based on the effect of Szilard-Chalmers, and includes irradiation in a neutron flux of the target, followed by separation of the target radioisotope resulting from the reaction98Mo(n, γ)99Mo, wherein the target is a metallic nanoparticles of molybdenum or insoluble in water, in aqueous solutions of alkalis and NH4OH molybdenum compounds placed in water or aqueous alkali solution or NH4HE. PR� irradiation as a result of neutron capture target ( 98Mo) formed the nucleus99Mo are initially in the excited state. When de-excitation by emission of prompt gamma-rays part of the recoil atoms (99Mo) receives an impulse sufficient to break chemical bonds and release of nanoparticles into the aquatic environment. At the same time as the movement of nanoparticles inside a "hot" atom loses its outer electron shell, transformed into ion Mo+6. In the aquatic environment ion Mo+6attaches the oxygen atoms, forming poorly soluble in water molybdenum oxide99Of Moo3. As a result of secondary reactions of hydration reaction in an environment with the presence of free hydroxyl ions HE-

99Mo enters the structure of the anion of the water-soluble molybdate. It should be emphasized that during irradiation in the reactor available hydroxyl ions HE-will be present not only in aqueous solutions with the basic properties: aqueous solutions of alkalis and NH4OH, and just in the water due to its radiolysis of neutrons and γ-quanta [V. M. Byakov, F. G. Nichiporov "the Radiolysis of water in nuclear reactors", Moscow, Energoatomizdat, 1990]. In the composition of the molybdate99Mo can be easily separated from water-insoluble nanoparticles, either by filtration of the nanoparticles (with proper filter), or by elution in�s with molybdate (aqueous solution of alkali molybdate, or an aqueous solution of NH4OH with molybdate) and nanoparticles through an anion exchange column or a column with Al2O3. Due to the small size of the nanoparticle columns are not filtered and remain in the eluate.99Mo in the composition of the anion (99MoO4)-2will be sorbed on a column. Assembled with column eluate with nanoparticles can be reused in the new target. After washing the columns with water99Mo in the form (99Of Moo4)-2maybe-eluted them with a concentrated aqueous solution of alkali.

An example of carrying out the invention

Powder natural metallic molybdenum isotopic composition in an amount of 50 mg with a particle size of predominantly 10÷40 nm) was mixed with 0.1 M aqueous solution of NH4OH and was placed in a quartz ampoule with a diameter of 8 mm and length 80 mm. the Ampoule was hermetically welded and was irradiated in a research reactor IR-8 in a neutron flux of 1.5·1013with-1cm-2within approximately 4 hours to achieve the integral flux of ~2·1017with-1cm-2. After removal from the reactor and three days of exposure, a measurement of the activity of the target. Then, the ampoule was opened, removed the irradiated mixture of nano-particles of molybdenum with 0.1 M aqueous solution of NH4OH, to content added ~30 ml of 0.1 M aqueous solution of NH4OH, stirred and received �Sveti nanosized particles of molybdenum in 0.1 M aqueous solution of NH 4OH was suirable through an anion exchange column with Dowex-1 (200-400 mesh Cl-form) with flow rate of ~1 ml/min, collecting the eluate nanoparticles of molybdenum and the ions on the column (99Of Moo4)-2. The column was washed with water and making sure that the flush has no activity99Mo, suirable column with99Mo 5 M aqueous NaOH. Then measured the activity of99Mo in the eluate. Withstood the eluate for about two months, reducing the activity to background values, and measured therein the content of Mo by atomic emission spectrometry with inductively coupled plasma (ICP-AES). The ratio of enrichment of99Mo (the ratio of the specific activity of99Mo in the eluate to a specific activity of99Mo in irradiated targets to highlight99Mo) amounted to the value of 2.3·102. Because the mechanisms of formation of soluble in the aqueous environment of molybdates (99Mo in the composition of the anion) for water, aqueous solution of NH4OH, or aqueous solutions of alkalis the same (see (1)) and are determined by the presence of free hydroxyl ions HE-the enrichment factors for99Mo under irradiation of the same nanoparticles of molybdenum in water, aqueous solution of NH4OH, or aqueous solutions of alkalis will not practically differ from each other.

Evaluate the possibility of using99Mo obtained by the proposed method, the standard Sorb�ion generators, working today on "shrapnel"99Mo. As an example of such a generator can be considered a generator, developed at the Institute of physical chemistry. Karpov (branch in Obninsk). The sorption parameters specified column of the generator are: the length of the sorbent from Al2O3in column 56 mm, diameter 4 mm, weight 2 g, Respectively, equal to the volume of the sorbent 0.703 cm3and the bulk density of Al2O3equal to 2 g/0.703 cm3=2.845 g/cm3. It is known that in normal mode the generator has activity99Mo about 1 Curie and about 90% of activity is located on a 1 cm length of the column. One centimeter of length of the column corresponds to 0.3573 g of Al2Ο3. The sorption capacity of Al2Ο3according to, for example, [R. E. Boyd Molybdenum-99:are technetium-99m Generator. // Radiochimica Acta 30 / Akademische Verlagsgesellschaft. - Wiesbaden, 1982, p.123-145], can be 20÷80 mg of molybdenum per gram of Al2O3. For definiteness valuation used in the calculation of the lower value of the sorption capacity of 20 mg Mo/g of Al2O3. Then on the column length of 1 cm can be adsorbed 7.146 mg Mo. According to the prototype in 1 g of molybdenum metal of natural isotopic composition for 7 days of irradiation in a neutron flux of 2·1014cm-2with-1you can easily gain 1 Curie99Mo. Taking into account the enrichment coefficient, equal to 2.3·102specific sup> 99Mo obtained by the proposed method, can be 2.3·102×1 Curie/gram Mo=230 Curie/gram99Mo. Specified specific activity allows to adsorb for 1 cm column activity99Mo is equal to: 7.146 mg Mo×230×10-3curies/mg Mo=1.64 Curie that is 1.64 times that of regular activity99Mo in the generator. The use of highly enriched98Mo is a natural molybdenum target will raise the specific activity approximately 4 times. Thus, the obtained in this way99Mo can be used in standard sorption generators, providing them with regular operation.

A method of producing the radioisotope99Mo, including irradiation by the neutron flux of the target, representing the metal nanoparticles of molybdenum or its compounds, followed by separation of the target radioisotope formed in the98Mo(n,γ)99Mo reaction, characterized in that as compounds of molybdenum are used compounds, insoluble in water or aqueous alkali solution, or an aqueous solution of NH4OH, the irradiation of the target is carried out in water or an aqueous alkali solution, or an aqueous solution of NH4OH, and separate99Mo in the composition of the anion of the water-soluble molybdate (99MoO4)-2from nanoparticles.



 

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