Method of producing radionuclides

FIELD: chemistry.

SUBSTANCE: invention relates to a method of producing radionuclides. The disclosed method includes irradiating a target medium containing at least a target nuclide material in a neutron radiation zone. Formation of radionuclides is carried out in the target radionuclide material as a result of irradiation, and at least some of the formed radionuclides are extracted from the target nuclide material. The extracted radionuclides are then captured and collected using carbon-based recoil particle capturing material which is free of an empty mesh structure at the crystallographic level.

EFFECT: obtaining radionuclides with high specific activity and soft radiation using the Szilard-Chalmers effect.

16 cl, 4 tbl

 

The technical FIELD

The present invention relates to the production of radionuclides. In particular, the present invention relates to radionuclides obtained in accordance with the effect of the Szilard-Chalmers, and characterized by a high specific activity. Accordingly, the present invention relates to a method for producing such radionuclides, and also covers the radionuclides obtained in this way. The present invention also relates to a device for producing radionuclides.

The LEVEL of TECHNOLOGY

A common cause of complications in the treatment of malignant tumors in patients are metastases of malignant tumors, in particular in the bone. Metastasis is the condition by which malignant cancer spreads from its primary focus in the body, such as breast cancer or prostate cancer, and is localized in another organ, such as bone. Pain and discomfort are common symptoms and side effects of metastases of malignant tumors in the bone, and usually conduct individual therapy or treatment of a malignant tumor in the primary focus is useless, resulting in a malignant tumor often causes the death of the patient. Temporary relief of the pain in the bones, caused by bone metastasis, usually reach oposredstvovanii therapy (RNT), also known as radioisotope therapy (RIT). RNT or RIT provides for the introduction of the radiation source to the target area, such as bone, in which the spread of a malignant tumor, so as to irradiate the target region and to restrain the growth of malignant tumors in this area. This can serve to enhance and Supplement the separate treatment of primary malignant tumors. Especially preferred in the treatment of bone metastasis are the sources of irradiation with slobodianiuk radiation and high specific activity, in order respectively to reduce the impact of radiation on sensitive bone marrow and to provide a high antitumor effect with limited or minimal radiation dose, thereby reducing the effects of irradiation on the rest of the body.

From prior art it is well known that the radionuclides with high specific activity, including metastable nuclides can be obtained by irradiation of a suitable target material containing the material of the target nuclide, neutron radiation so that the bombarding neutrons react with the nuclei of the target material of the target nuclide for the implementation of the nuclear reaction for the absorption of neutrons (n) - gamma-particles (γ), also expressed as (n, γ). Received metastabile radionuclides in the target environment get high recoil energy from γ-radiation and retrieved, or bounce off the original target lattice, that is, the material of the target nuclide. These extracted radionuclides then seize and hold in the environment, or material capture particles of bestowal, which is located in close proximity to the target environment, resulting in separation of the extracted radionuclides from inactive or cold nuclei of the target material of the target nuclide. Thus, there is a concentration or enrichment lessons metastable nuclides relatively cold nuclei in the material capture particles recoil. This process, generally referred to as the effect of the Szilard-Chalmers. Recoil then removed from the material capture particles recoil.

The INVENTION

The purpose of the present invention is to provide a practicable method of producing radionuclides with high specific activity and slobodianiuk radiation radiation using the effect of the Szilard-Chalmers.

Thus, the present invention relates to a method for producing radionuclides, which includes the irradiation area of the irradiation target environment containing at least the material of the target nuclide, neutron radiation, thereby causing the formation of radionuclides in the material of the target nuclide, removing at least some of the formed radionuclides from the material of the target nuclide; and the NAP and collecting the extracted radionuclides material capture particles impact based on carbon where there is no empty lattice structure at the crystallographic level.

The material of the target nuclide can be selected from the group consisting of pure metal and metal joining. In a preferred embodiment of the invention the material of the target nuclide may contain the compound of the metal, including a metal oxide, metal salt or ORGANOMETALLIC compound. The metal material of the target nuclide may in particular be selected from the group of elements-metals of the periodic table of elements, starting with scandium (Sc), atomic number 21 to bismuth (Bi), atomic number 83, and both elements are included, but items-non-metals arsenic (As), selenium (Se), bromine (Br), krypton (Kr), tellurium (Te), iodine (I) and xenon (Xe), therefore, excluded. In a preferred embodiment of the invention, the metal may be tin (Sn). In this case, the material of the target nuclide can therefore generally be selected from elemental tin or metallic tin and tin oxide including tin oxide (II) (SnO) and tin dioxide (IV) (SnO2). The material of the target nuclide may instead be selected from tin salts, including chloride, tin (II) (SnCl2), tin chloride (IV) (SnCl2), sulfate, tin (II) (SnSO4and nitrate of tin (II) (Sn(NO3)2). The material of the target nuclide may instead be optionally selected the C ORGANOMETALLIC compounds of tin, including tetraphenyl tin oxide phthalocyanine tin (IV) phthalocyanine tin (II) and 2,3-naphthalocyanine tin (II).

Material capture particles impact based on carbon may be selected from amorphous carbon allotropic modifications of carbon and mixtures thereof. In particular, the material capture particles of return can be selected from an isotropic amorphous carbon; allotropic modifications of carbon, such as graphite, graphene, carbon nanopen, soot, charcoal, activated carbon and glass carbon; or mixtures thereof. Isotropic amorphous carbon allotropic modifications of carbon, such as presented above, are characterized by the fact that they do not have the so-called empty lattice structure at the crystallographic level, which is easily deformed by radiation when exposed to neutron radiation.

The material of the target nuclide and material capture particle impact can be in the form of fine particles, each of which is generally characterized by an average particle size of not more than approximately 50 nm. In a preferred embodiment of the invention the material of the target nuclide may have a smaller average particle size, essentially, of the order of from approximately 50 nm to approximately 10 μm.

If the material of the target nuclide, and material capture particles recoil nah is incorporated in the form of particles, as described above, the method may include mixing the material of the target nuclide and material capture particles recoil. It should be noted that in this variant of the invention, the material capture particles recoil will also be present in the radiation zone during neutron irradiation, and the target environment, therefore, contains as the material of the target nuclide, and material capture particles recoil. It is expected that the ratio in which the material of the target nuclide and material capture particles of return in this case will be mixed can be determined by standard experiments and optimization. However, typically, the material of the target nuclide and material capture particles recoil can be mixed in the ratio 1:1 by weight.

The irradiation of the target environment may include the placement of the target environment in the path of flow of neutrons from the neutron source. According to one embodiments of the invention, the neutron source may be the reaction products of nuclear fission, which are inside a nuclear reactor. In this case, the method may include placing the target environment in a certain position relative to the nuclear reactor where the neutron flux of fission products is quite intense and has kinetic energy is in the range which is compatible with the desired reaction with the material of the target nuclide. In an alternative embodiment of the invention, the neutron source may be a based on an accelerator neutron source. An example of such a source is a source of fission neutrons (IDNS) at the National laboratory oak ridge, oak ridge, Tennessee, USA.

The method can include the allocation of captured radionuclides from a material capture particles recoil.

In a preferred embodiment of the invention the selection of the captured radionuclides from the material capture particles recoil provides processing of the material capture particles impact the diluted and/or concentrated acid extraction solvent, to obtain, thus, the suspension material capture particle impact, and chemical extraction or leaching captured radionuclides from a material capture particles return to obtain radionuclide enriched extraction solvent. Thus, it is assumed that the material capture particles of return can be processed either dilute acid or concentrated acid, or in an alternative embodiment of the invention as dilute and concentrated acid separately from each other, for example, in the form of two-stage processing.

In cha is in the surrounding area, if the extraction solvent is a dilute acid, separation of the captured radionuclides from the material capture particles recoil may provide for the elution of the captured radionuclides from the material capture particles recoil by dissolving captured radionuclides in dilute acid. The acid may be selected from hydrochloric acid and ascorbic acid. The acid may also be selected from other inorganic or organic acids, including nitric acid, sulfuric acid, forcerenew acid, phosphoric acid, citric acid, oxalic acid, acetic acid and Melkumova acid. It should be noted that the acid may also contain a combination of any two or more of the above acids. In a preferred embodiment of the invention, the acid may be diluted to a concentration of about 0.01 mol/DM3up to 10 mol/DM3typically up to about 0.5 mol/DM3.

The method may include the incubation of a suspension of the material capture particles recoil over a longer period, which preferably does not exceed the half-life obtained radionuclide. It is expected that such incubation of the material capture particles recoil will allow more optimal to allocate captured radionuclides from the material capture the particles impact in the eluate or the filtrate. The term "optimal allocation" refers to getting the desired output captured radionuclides, which is measured on the basis of their gamma activity and is converted into an enrichment factor relative to the total content of tin in the eluate. In an alternative embodiment of the invention, the method may include increasing the speed of elution by choosing the appropriate reaction conditions, such as temperature, acidity and the acid strength, and/or with the use of ultrasonic treatment to facilitate displacement of the captured radionuclides into the suspension. It is expected that such reaction conditions can be determined by standard experiments.

The method may also include maintaining the pH of the suspension material capture particles recoil is low enough to avoid undue hydrolysis of extracted atoms of the radionuclide. Maintaining the pH level may provide selective adding dilute acid to the suspension.

If the extraction solvent contains a concentrated acid, the acid may generally be more aggressive acid than the above acid. Then the method can include dissolving or removing material capture particles impact in these acids. Such is more aggressive acids may include Imperial vodka which is a mixture of 1:3 by volume concentrated nitric acid and hydrochloric acid, chromic acid, hydrofluoric acid, or combinations of these acids.

The method may further include, when the selection of radionuclides from a material capture particles recoil handling of the material capture particles recoil acid extraction solvent, separation or separation of radionuclide enriched extraction solvent from the material capture particles recoil by centrifugation, vortex separation and/or filtration.

In an alternative embodiment of the invention the selection of the captured radionuclides from the material capture particles recoil may provide material handling capture particles recoil alkaline extraction solvent. In a preferred embodiment of the invention, the alkali may be sodium hydroxide. In this case, the radionuclides can usually be extracted in the form of hydroxides of radionuclides metals. In this case, the method may include the selection or separation of the extracted hydroxides of radionuclides metals from the material capture particles recoil usually by centrifugation, vortex separation and/or filtration.

Instead, the selection of the captured radionuclides from the material of grip h is STIC recoil may include burning of the material capture particles yield on oxygen.

It should be noted that if the target environment contains a mixture of material capture particles returns and material of the target nuclide, as described above, at least some material of the target nuclide may also be present when selecting the captured radionuclides from the material capture particles impact the way described above, for example, in the suspension material capture particles recoil. Thus, the method may include, if necessary, the separation material capture particles recoil from the material of the target nuclide prior to extraction of radionuclides from a material capture particles recoil. This separation can be achieved through a process of liquid-liquid extraction, usually with the use of organic liquid and water liquids as solvents for liquid-liquid extraction. In a preferred variant of the invention, the organic liquid is selected from tetrabromoethane (TBE) and toluene. Water liquid usually will be a water. At least some material of the target nuclide contained in the suspension material capture particles recoil, can usually be extracted into the aqueous phase. The method may additionally include the immobilization of the aqueous phase containing the material of the target nuclide in order to separate it from containing the second material capture particles impact the organic phase. Typically, immobilization of the aqueous phase can be achieved by adding any suitable natural clay or synthetic filler cracks to a suspension of the material capture particles return for the adsorption of the aqueous phase. The clay may be selected from clays, characterized by a high water-absorbing capacity, which swell under the action of water. It is expected that such clay will be complete, i.e., be immobilized, the aqueous phase before the material of the target nuclide will be able to settle. In a preferred embodiment of the invention, the clay may be selected from montmorillonite clays, such as bentonite clay, CA-bentonite clay, attapulgite, MD-Bentonite and Eccbond-N/Bentonite.

The present invention applies to radionuclides, if they are obtained by implementing the method in accordance with the present invention.

In accordance with another embodiment of the present invention provides a system for producing radionuclides containing

the radiation zone, which placed the target medium containing at least the material of the target nuclide;

the source of neutron radiation, which interacts by means of neutron radiation with the target environment in the exposure zone; and

material capture particles impact based on carbon, is the first to capture radionuclides, which derive from the material of the target nuclide, and material capture particles impact based on carbon there is no empty lattice structure at the crystallographic level.

The material of the target nuclide and material capture particle impact can be the same as described above in this document. The source of neutron radiation may also be as described above in this document.

The present invention will be described in more detail with reference to the following non-limiting examples.

DETAILED description of the INVENTION

In the examples of the tin (Sn) was chosen as the metal for the material of the target nuclide, in particular, due to his preference for treatment of some types of cancer and due to the fact that activated metastable (t) tin - 117 (117mSn) can be easily detected due to its ideal gamma radiation at 160 Kev using a conventional gamma-ray detectors. Thus, in the case of tin high specific activity117mSn obtained by neutron irradiation of the target environment containing tin - 116 (116Sn) in accordance with the following nuclear reaction (n, γ):

116Sn(n,γ)117mSn/mi> (1),

as a result of which the final radioactive nuclei117mSn acquire high energy efficiency from γ-radiation and thus extracts and rebound atom117mSn from the original lattice of the material of the target nuclide.

All reagents were chosen qualification "pure for analysis" (H. D. A.) and were purchased from Merck KGaA, Darmstadt, Germany and Sigma-Aldrich Chemie GmbH, Steinheim, Germany.

EXAMPLE 1

The target environment is selected from combinations of tin oxide with a purity of more than 99% in the form of a powder with an average particle size of the powder is 10 μm, and SnO2in the form of nanopowder as a material of the target nuclide, and carbon with a purity of more than 99% in the form of nanopowder or graphite powder as a material capture particles recoil.

Each of the solutions of ascorbic acid and hydrochloric acid (HCl) was prepared at a concentration of 0.50 mol/DM3for the extraction of the given atoms117mSn from a material capture particles impact based on carbon or graphite after irradiation, i.e., after the reaction (1)116Sn(n,γ)117mSn

The target environment have been prepared in accordance with Table 1, containing a combination of 50 mg (from 0.37 mmol) SnO or 50 mg (0.33 mmol) SnO2mixed with 50 mg nanopowder carbon or graphite powder as a material capture particles recoil.

Received target environment were then sealed in polyethylene capsules. There were prepared two targets from each combination of the material of the target nuclide and material capture particles of return, one must be extracted with a solution of 0.50 mol/DM3HCl, and the second must be extracted with a solution of 0.50 mol/DM3of ascorbic acid.

The target environment were obtained for irradiation in a nuclear reactor of the nuclear research Institute Delft University of technology, Delft, the Netherlands (TU Delft). Then the target environment were irradiated over a period of 10 hours, and were left to cool for a period exceeding five days, in order to allow the samples to cool down or decompose to lower radiation levels for safer handling and reduce false responses from rapidly decaying impurities.

Given the radionuclidesll7mSn were extracted from environment-based carbon or graphite prepared by HCl and ascorbic acid. Each of the respective acid solutions of vildbassen in a volume of 10 ml, accordingly, the irradiated target environments, covered in plastic capsule, which was opened for forming thus the corresponding suspension of the target environment containing the material of the target nuclide and the environment capture, in acid solution. 2 ml sample of each suspension were taken for analysis of total target output or background dissolved irradiated oxides as a reference of the enrichment factor, after which the volume was topped with 2 ml of the appropriate acid solution and left for incubation at room temperature, respectively, during periods of 0.25 hour, 0.5 hour, 1 hour, 5 hours, 48 hours and 7 days.

At appropriate time intervals, as shown below in Table 1, 2 ml samples of the suspension were extracted by filtering through a 0.22 μm filter. Ions117mSn, which were dissolved or washed from the material capture particles results in the acidic solutions were stored in solution, as described above in the present description, and collected in the filtrate, and unreacted or neoteny material of the target nuclide on the basis of stable tin oxide and a material capture particles recoil essentially remained for the filter to be washed back into the capsule through 2 ml of additional solution for additional leaching. Thus, the filtrate soda is shaking concentrate radioactive nuclides 117mSn-enriched compared with any dissolved unreacted tin oxide. Samples taken after seven days of incubation period, as shown below in Table 1 were taken after placing suspensions of materials capture particles recoil in an ultrasonic bath for 1 hour. Within 60 minutes the suspension was again refilled to maintain a constant volume of 10 ml, and stirred by a vortex method in 15 minute intervals.

In a separate set of tests, the target environment were prepared in triplicate to reproduce the results obtained by ultrasonic treatment. They were incubated for 48 hours, samples were taken before and after ultrasonic treatment for 1 hour. The second set of samples was taken on the 7th day of the test. Then activity117mSn in 2 ml of the samples was determined by γ-spectroscopy and restated prior to the termination of exposure to particles. They were analyzed by means of equipment for instrumental neutron activation analysis (INAA) at the Department of radiation, radionuclides and reactors, faculty of applied Sciences Delft University of technology. To determine the specific activity and factors enrich the total concentration of tin was measured by optical emission spectroscopy inductively coupled is lazmi (ECO-COI) at the corresponding tin wavelength, component 189,926 nm.

By implementing the method according to this variant implementation of the present invention were successfully concentrated radionuclides117mSn in environments that capture particles impact on the basis of graphite and amorphous carbon with a receipt for SnO2the enrichment factor 34 (as shown in Table 1) when the specific activity and yield of 2.53 MBq/mmol1and 0.07%, respectively, in the solution of 0.50 mol/DM3HCl. On the other hand, SnO provides a lower specific activity, possibly due to the relatively easy dissolution of unirradiated target SnO applied in an acid environment.

Acid solutions were used to maintain conditions of low pH for the extraction of radionuclides from the environment to capture particles recoil, minimizing the possibility of hydrolysis of ions recoil tin and their eventual deposition, especially for SnO2 (i.e., Sn4+), which would be given to the tin and the target (s) oxide (s) tin are practically inseparable by filtering. Ascorbic acid and HCl are strong reducing agents and minimize the oxidation of dissolved117mSn, which can likewise lead to hydrolysis. Ascorbic acid, which is a weak acid (pH 2), less active than HCl (pH of 0.4). It is considered useful to achieve greater specific activity, as HCl also easily dissolves the unexposed target oxides, the effect is more pronounced for SnO, which is approximately 1000 times more soluble than SnO2in HCl (table 1 vs. Table 2).

Table 1 presents the results of the analyzed samples for extraction with HCl, while in Table 2 below presents the same results for the extraction of ascorbic acid. For SnO2the amount of dissolved tin basically constantly until about 3 days of incubation. However, SnO was less stable and showed a modest increase in dissolved tin over time. As the organic acid, ascorbic acid has an advantage because it allows the particles of carbon or graphite to suspendibility or dispergirujutsja in solution due to the moderate non-polar, hydrophobic effect, thus providing a large surface area for contact with the acid for an effective extraction of the given radioactive substances. In addition, it is reported that ascorbic acid acts as a complexing agent, which can then associate the extracted ions117mSn and keep them in solution, thus minimizing hydrolysis of the tin and providing separation by filtering.

Were performed additional control experiments (table 3) in that the extraction process was repeated with the application of non-irradiated (cold) SnO 2and SnO for HCl and ascorbic acid, to determine the extent to which the acid is dissolved oxides, and the content of dissolved tin was measured by means of ECO-COI. These tests were used to test the reactivity of the oxides of tin with the appropriate acid.

The effectiveness and success of the extraction was controlled by the enrichment factors achieved at each stage of the process. They were calculated as the ratio of the specific activity117mSn samples (each time) and the initial total target output. The initial total value of the target output was 0.11±0,02 MBq/mmol1and 0,10±0,02 MBq/mmol1for SnO2and SnO, respectively. Tables 1 and 2 show the trend of the specific activity (MBq/mmol1) attained at selected intervals (15, 30 and 60 minutes, 5 and 48 hours) and is calculated as the ratio of the measured activity117mSn (MBq/ml1) defined by γ-spectroscopy, and the concentration of tin (mmol/DM3) defined by the ECO-COI. After exposure117mSn is dissolved to provide enrichment factors between 2 and 34.

In General, both solution, HCl and ascorbic acid, were effective for the extraction of117mSn. However, more reactive tin oxide, SnO, and the solution is a stronger acid, HCl, respectively, seem to give the most output, although their specific activity and enrichment factors are lower. In the SnO2performed better, while the extraction of ascorbic acid proved to be useless, as you can see from undetectable activity117mSn in Table 2. Enrichment factor 34 and the output of 0.07% was achieved in the presence of carbon after treatment of 0.50 mol/DM3HCl (Table 1).

Ultrasonic treatment for 1 hour, after 48 hours and 7 days of incubation, respectively, had no significant effect on the specific activity, and, therefore, the enrichment factor has remained essentially unchanged. As a control observation was made for other isotopes for this study, namely113Sn113mSn125Sn and125mSn, and their enrichment factors were almost the same as the117mSn. This was expected, since they were obtained by the same reaction (n, γ), and especially because the values of energy stimulating their γ-rays were close.

It is assumed that the best extraction environment could be a combination of ascorbic acid and HCl as HCl dissolves better given radioactive substance, while ascorbic acid provides a large surface area of the material capture particles recoil simultaneous to the elektooborudovanie 117mSn, hold it in solution and preventing unwanted hydrolysis and sedimentation. Additional optimization will be necessary to combine and perfect concentration of each component, for example, through the study of composition with the use of potentiometry with a glass electrode. Obviously, the longer the exposure time will also lead to an increase in output and/or enrichment factors.

EXAMPLE 2

In another embodiment of the present invention was investigated the possibility to separate and isolate the material capture particles recoil from oxides before extraction with acid. This was done in order to minimize the presence of "cold" (non-irradiated) tin, which can lower specific activity, as well as to avoid intake of any irradiated, but neotango [117mSn]SnO or [117mSn]SnO2in the acid extract/the filtrate, which may lead to false positive results. One such method involves the initial organic/aqueous liquid-liquid extraction, in which the irradiated material added to the water and tetrabromide (TBA) or toluene, respectively. The choice of organic solvent depends on the preferential orientation of the organic and aqueous phases.

When the Department using TBA and water (the first column under each of the m oxide, Table 4) tin oxides remain suspended in the upper water layer, while the carbon or graphite is distributed in the organic bottom layer. Carbon and graphite are not soluble in the solvents themselves, but the separation is due to differences in the polarity of the environment of capture particles recoil and oxides of tin. The distribution of activity117mSn organic and aqueous phases, as well as utensils (i.e., laboratory glassware and syringes), was measured in the ionization chamber Capintec and the results obtained are presented in Table 4. Although it was required complex manipulation was sufficiently good separation. However, the oxide is typically deposited on the surface of the section water - organic matter, i.e. in the lower part of the water layer at the top, which in the case of an error during phase separation will be extracted from the phase of TBI, as shown in the columns of TBE Table 4.

When toluene was used in place of TBE, organic and aqueous phase were reversed, i.e., the toluene layer was at the top. In this case, the deposition of tin oxide on the bottom (lower part) of the aqueous layer away from the organic phase makes the extraction more efficient (column toluene under each oxide, table 4), effectively minimizing the chance of collecting oxide with graphite or carbon. The Department was good and required less complex manipulations. In addition, the lawsuit emergence of the presence of tin oxide in the organic phase was lower. However, on the surface of the water component watched a thin film of toluene that contained a certain amount of graphite and were difficult to separate.

During testing in accordance with this example of a radioactive substance recoil is not extracted from media capture particles of return, however, they only served as a demonstration of the feasibility of these stages. During the extraction of the used water, not acid or buffer solution, to avoid premature extraction of the ions given117mSn of the media capturing particles of return, which in this case could end up in the aqueous phase. Although the inventors have found a method liquid-liquid extraction bulky and sensitive to deviations, clarification stages can prove that this method is acceptable technological operation.

In addition, although the outputs are not significant (2.2% and 2.6%, respectively), the goal was exceptional achieve a greater ratio of radioactivity (Bq or CI) per unit mass or volume of the nuclide-product. The outputs may eventually be improved by further experiments and optimization.

EXAMPLE 3

In the following example, the possibility of phase separation described in example 2, extended to include immobilization by clay aqueous phase containing the oxide, allowing the organic with the OU to be separated or washed away for further processing and extraction of return 117mSn.

In these experiments, 5 clay and ordinary household filler cracks were considered as hardening/immobilizing agent, namely: (1) bentonite-MD / 0104 / Environment; (2) CA-bentonite / calcium 100# / 0106 / 1-06-10-12-03; (3) attapulgite; (4) MD-bentonite / 0101; (5) Eccbond-N / bentonite; and (6) filler internal cracks Alcolin (Polyfilla), all purchased from Koppies, Orange province, South Africa (G & W Base &Industrial Minerals, Germiston, 1428, Gauteng, South Africa), and the household filling cracks (Polyfilla) can be purchased at any local hardware store. They, in turn, were carefully added to the two extraction mixtures of example 2, while the aqueous phase was not corresponding saturated clay. Approximately one gram of clay was required in 1 ml of water. All clay and filler cracks, not dispersibility in organic layers; in the case of toluene, they fell immediately freely through it, eventually reacting with water under it. As for TBA, clay remained dispergirovannykh in the upper water layer without penetrating into the organic phase. Clay 1, 4 and 5 acted completely analogous, slowly reacts with water and without sinking into the water layer. Instead, these clays reacted to the edge of the water surface or meniscus. The result is that some amount of unreacted water was kept below clay - out DOS is haemost newly added clay. Clay 2 and 3 reacted more slowly, but they eventually settled in the layer of water and ensure good contact and react with all the water. The same was observed for filling cracks. Stirring the mixture slightly contributed to the settling of the filler cracks. All in all, clay is swollen, but not the filling of cracks. Clay 2 and 3 showed the most relevant characteristics, and are best for use with toluene. Filling cracks were also effective, especially with TBA. However, in the case of clays, the toluene was necessary to decant for 15 minutes after administration of the clay, while the filling of the cracks with toluene, and TBE, it was necessary to leave on the night before the Department, and even then his hardening was only moderate. In all cases with toluene clay and filler cracks kept a certain amount of carbon, as he was settled through toluene. To facilitate sufficient hardening of the filler cracks, thereto was added Na2SO4mass ratio of 1:1, with Na2SO4absorb any excess water, thus contributing to the drying and hardening of the filling of the cracks. However, there has been only modest improvement.

The reverse approach is also possible, i.e., immobilization or curing/encapsulating media capture particles impact with the use of the melt is built paraffin wax, which would replace the organic solvent. However, this would require operation at elevated temperatures to avoid undesirable solidification of the wax.

An alternative means of separation can be achieved by separating the density of dry powders in a shaking device.

It was assumed that once the material capture particles recoil can be successfully separated from the oxides, radioactive substances recoil can be isolated or extracted by leaching with acid, as noted above, or by burning material based on carbon in oxygen to produce a [117mSn]SnO2or [117mSn]SnO and gas of carbon dioxide.

Believed that the specific methods provided in examples 1-3 provide a preferred path for the prospects of production, because of the shape of the applied materials of the target nuclide were flexible and favorable for severe radiation conditions, as well as ease of processing and isolation after irradiation.

Radiolabelled tin II and IV, i.e., [117mSn]-Sn(II) and [117mSn]-Sn(IV), was proposed as promising components of radiopharmaceuticals for the temporary relief of bone pain by RNT. Radionuclide117mSn emits conversion electrons Ave is decay and, reportedly, characterized by short-range approximately from 0.2 mm to 0.3 mm in the tissue that makes117mSn is ideal for the treatment of bone cancer because of exposure to sensitive bone marrow radiation, and, therefore, the radiotoxicity of the117mSn is limited. Its attractiveness as a radiopharmaceutical is additionally enhanced by emitted in approximately 86% of the cases decay gamma radiation at 159 Kev, which makes it also a great radionuclide imaging, for example, for applications intended for tumor localization.

As can be seen from the examples above, if the tin is selected as the preferred target nuclide, oxides SnO and SnO2are the preferred molecular forms of the material of the target nuclide. The applicant has found that the oxides of tin are more resistant to destruction by radiation during prolonged exposure compared with other compounds of tin. Additionally, the applicant was found that these oxides of tin are essentially chemically inert with respect to extraction solvents used in the selection of the captured radionuclides after irradiation. These tin oxides are thermally stable with a melting point of 1080°C and 1127°C that corresponds to the public, that is especially preferable reaction conditions, which are oxides.

Like SnO and SnO2as materials of the target nuclide, the applicant has also found that carbon and graphite as a material capture particles recoil able to withstand the harsh chemical treatment and are inert to dilute the acid. The applicant has found that given the atoms/ions117mSn is characterized by mild/moderately stable relationship with the material capture particles recoil. This characteristic, combined with the stability of carbon and graphite to harsh chemical processing and inertia in dilute acid, allows the atoms/ions to be lirovannye or washed from the material capture particles recoil by dissolving the material capture recoil particles in dilute acid. Carbon and graphite as a material capture particles recoil also resistant to more intense neutron fluxes and large periods of exposure compared to fullerenes With60that can be destroyed by nadalovih neutrons within 2 hours of exposure in an unfiltered stream of neutrons 1014cm-2with-1. Graphite is an allotropic modification of carbon where the carbon atoms are covalently bound in a flat layer from the United Shestopal the different rings. Layers of loosely arranged one above the other and are held together by weak van der Waals forces. On the other hand, amorphous carbon and unlike graphite deprived of the crystal arrangement of the atoms. Without limitation to any theory, it is expected that given the atoms/ions117mSn be included in the lattice of carbon or graphite, from which it can then be removed by chemical and/or physical methods, for example, by burning the carbon material capture particles return oxygen to release enriched tin oxide [117mSn] release gas CO2.

The applicant understands that commercially used technologies for radionuclides, known at the time of filing this application, give radionuclides117mSn, characterized describes the specific activities of up to 25 CI/g1(~88 MBq/mmol1) at the termination of exposure to particles and are available from suppliers such as Curative Technologies Corporation (CTC). The specific activity of this magnitude can be achieved, for example, by irradiation with inelastic scattering of neutrons metal tin enriched to 92% in Sn for approximately 35 days in the reactor SM-3 with high intensity neutron flux at the research Institute of atomic reactors (RIAR), Dimitrovgrad, the ossia, i.e., through the reaction117Sn(n, n')117mSn in alternative embodiments for carrying out the invention117mSn can be obtained by irradiating nodeprofile neutrons using the above-described reaction (n, γ) neutron capture,116Sn(n, γ)117mSn, but the reaction rate in the context of the cross-section of neutron capture for this reaction (0,14 bn) is in General too low for cost-effective obtain117mSn with high specific activity using traditional methods.

In the above reactions (n, γ), however, the end of the kernel get the kinetic recoil energy at the instant of emission of γ-ray in the capture of a neutron, which is much more attainable through normal thermal reactions activation energy (the energy of chemical bonds is usually in the range of 1-5 eV, and the energy of bestowal, the acquired cores thanks to the efficiency, typically greater than 10 MeV), at the same time the atom is chemically converted, resulting in a chemical linkage or the valence of the given atom is reduced to a lower state, as also described earlier in this document. It provides chemical extraction, based on the difference of the binding. In addition, by using the phenomenon of "explosion recoil", whereby a radioactive atom recoil residence permit is or is captured inside the empty lattice of fullerene (C 60or C80), can be obtained from the radiochemical substances without media, for example, metallofullerene, such as177Lu@C60and153Sm@C80where lutetium-177(177Lu) and samarium-153(153Sm) trapped in the lattice With a60and C80-fullerene, respectively. The above is a typical example of a process based on the effect of the Szilard-Chalmers.

Although fullerenes, and for the same reason bacisally as empty lattice structures are ideal as a material capture particles impact in the field of engineering that applies the present invention, the disadvantage of this way is that such carbon structures are able to withstand only the radiation in the flow of pure thermal neutron reactor, and deformed by the destruction of the radiation within 2 hours of exposure nadalovih neutrons.

According to the present invention materials based on carbon, such as amorphous carbon and graphite, in which there is no "empty lattice structure proposed for use as a media capturing particles return to capture the given atoms117mSn from reaction (n, γ)117mSn, since these matrices are based on carbon less prone to destruction by radiation. Thus, specifically addressed the problem of achieving returns117mSn with a high ratio of the activity at relatively low cost and with minimal waste.

Table 1: Total concentration of tin on one extraction pattern defined by the ECO-COI, specific activity117mSn for each sample and the output of the extraction at different values of time of incubation in 0.50 mol DM3HCl for targets containing natural SnO2and SnO

Target environmentTime (h)Activity117mSn (Bq/ml1)Dissolved Sn(µmol/DM3)Odelin. Activity (MBq/mmol1)Enrichment factorOutput (%)
0,25of 6.735,111,32180,05
0,5of 6.494.26 deaths1,53210,05
SnO2/ Carbon18,63,402,5334 0,07
511,75,11to 2.29310,09
4811,8±0,96,2±1,31,9±0,417,5±3,90,061±0,002
7 days7,4±0,74,5±1,31,7±0,3the 15.6±4,50,038±0,004
0,2510,95,961,83220,08
0,513,5for 6.811,98230,09
SnO2/114,77,661,92230,1
Graphite517,47,662,27270,12
4816,0±2,89,1±1,01,8±0,316,5±1,70,09±0,01
7 days9,1±2,34,5±1,02,1±0,820±70,05±0,01
0,253410208000,16219,55
0,52500174000,14214,41
SnO /12070145000,14211,93
Carbon 51650113500,1529,51
483280±25010100±9000,33±0,053,1±0,4the 15.6±0,3
7 days380±1503300±14000,12±0,021,11±0,191,9±0,9
0,253260194000,17221,95
SnO / Graphite0,53010178000,17220,27
12510153000,16216,9
5214013000 0,17214,41
483870±4708400±28000,50±0,164,5±1,816,5±0,3
7 days2900±35020500±13000,14±0,021,24±0,0912,4±0,3

Table 2: concentration of Total tin in one extraction pattern defined by the ECO-COI, specific activity117mSn for each sample and the output of the extraction at different values of time of incubation in a solution of 0.50 mol/DM3ascorbic acid for targets containing natural SnO2and SnO. (Where the results of γ-spectroscopy are below the detection limit of 1.8 Bq per gram of sample), specific activity and enrichment factors cannot be calculated, as shown below (-) in the table).

Time (h)Activity117mSn (Bq/ml1)Dissolved Sn(µmol/DM3) Specific Activity (MBq/mmol1)Enrichment factorOutput (%)
0,25<1,81,85---
0,5<1,81,58---
SnO2/1<1,81,48---
Carbon5<1,81,21---
483,7±1,33,1±0,31.2±0.611±70,019±0.010
7 days3,0±0,7 2,4±0,41,14±0,1010±40,015±0,008
0,25<1,81,58
0,5<1,81,67---
Sn2O /1<1,81,67-
Graphite5<1,81,39-
483,9±0,73,1±0,51,27±0,1414±40,03±0,01
7 days4,1±1,92,72±0,14 1,54±0,2022,2±0,80,035±0,030
0,25<1,85,38---
0,5<1,86,30---
SnO /1<1,87,88---
Carbon54,8232,40,1550,09
48580±805400±900to 0.108±0,0080,99±0,212,6±0,3
7 days2170±19020000±900to 0.108±0,0059,7±2,5
0,251,8227,6of 0.06610,02
0,52,1921,00,1120,02
SnO / Graphite12,8321,70,1330,03
5is 3.0823,60,1330,03
48530±4002900±5000,17±0,111,9±1,22,3±1,2
7 days1770±9017400±700is 0.102±0,0031,19±0,289±3

Table is 3: Dissolution SnO 2and SnO in solutions of 0.50 mol/DM3HCl or 0.50 mol/DM3ascorbic acid up to 3 days at ambient temperature

The tin oxideSolutionTime (hours)Dissolved Sn
(0.50 mol/DM3)(µmol/DM3)
SnO2HCl0,253,40
0,52,55
14,25
5for 6.81
487,66
3 days16,2
SnO2Ascorbic acid 0,252,69
0,52,50
12,32
52,32
482,13
3 days2,32
SnOHCl0,258380
0,521010
120700
518780
4817230
3 days11060
SnOAscorbic acid0,256,02
0,59,45
113,2
5of 17.5
4819,3
3 days21,3

Table 4: Percentage (%) activity117mSn present in the organic and aqueous phases, with the subsequent technology of liquid-liquid extraction to separate the oxides of tin from the media material capture particles impact based on carbon, carbon or graphite

The liquid phaseSnOSnO2
TBA TolueneTBAToluene
Water34,1of 97.822,993,9
Rastvoritel57,62,250,62,6
Laboratory glassware8,226,53,5

1. The method of producing radionuclides, including
the irradiation area of the irradiation target environment containing at least the material of the target nuclide, neutron radiation, thereby causing the formation of radionuclides in the material of the target nuclide, removing at least some of the formed radionuclides from the material of the target nuclide; and
capturing and collecting the extracted radionuclides material capture particles impact based on carbon, in which there is no empty lattice structure at the crystallographic level.

2. The method according to p. 1, in which the material of the target nuclide selected from the group consisting of pure metal and metal joining.

3. The method according to p. 2, in which the metal material of the target nuclide selected from the gr is PPI elements-metals of the periodic table of elements, starting with scandium atomic number 21 to bismuth with atomic number 83, and both elements are included, except for the items-non-metals: arsenic, selenium, bromine, krypton, tellurium, iodine and xenon.

4. The method according to p. 3, in which the metal material of the target nuclide is a tin.

5. The method according to p. 1, in which the material capture recoil particles selected from amorphous carbon allotropic modifications of carbon and mixtures thereof.

6. The method according to p. 1, in which as the material of the target nuclide, and material capture recoil particles are in the form of fine particles, each of which has an average particle size of not more than 50 nm.

7. The method according to p. 6, comprising mixing the material of the target nuclide and material capture particles recoil, and the target environment, therefore, contains as the material of the target nuclide, and material capture particles recoil.

8. The method according to p. 1, in which the irradiation target environment provides the location of the target environment in the path of flow of neutrons from the neutron source.

9. The method according to p. 1, including the selection of the captured radionuclides from the material capture particles recoil by processing the material capture particles impact the diluted and/or concentrated acidic extraction solvent, to obtain, thus, the suspension material capture particle impact, and chemical extraction or imyanya captured radionuclides from a material capture particles return to obtain radionuclide enriched extraction solvent.

10. The method according to p. 9, comprising incubating a suspension of the material capture particles of return during the period that does not exceed the half-life captured radionuclides.

11. The method according to p. 9, including the selection or separation of radionuclide enriched extraction solvent from the material capture particles recoil by centrifugation, vortex separation and/or filtration.

12. The method according to p. 1, including the selection of the captured radionuclides from the material capture particles recoil by processing the material capture particles recoil alkaline extraction solvent.

13. The method according to p. 1, including the selection of the captured radionuclides from the material capture particles recoil by burning material capture particles yield on oxygen.

14. The method according to p. 9, including if the target environment contains a mixture of material capture particles returns and material of the target nuclide, the separation material capture particles recoil from the material of the target nuclide prior to extraction of radionuclides from a material capture particles recoil.

15. The method according to p. 14, in which the separation material capture particles recoil from the material of the target nuclide is realized by means of liquid-liquid extraction using water and liquid organic liquids as solvents for liquid-liquid ek the traction.

16. For radionuclides, including
the radiation zone, which placed the target medium containing at least the material of the target nuclide;
the source of neutron radiation that interacts with the target environment in the zone of irradiation by neutron radiation; and
material capture particles impact based on carbon, located with the ability to capture radionuclides extracted from the material of the target nuclide, and material capture particles impact based on carbon there is no empty lattice structure at the crystallographic level.



 

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