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Separation of Molybdenum Isotopes at Supercritical Fluid Extraction with Carbon Dioxide in a Vertical Gradient Field of Temperatures

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Separation of Molybdenum Isotopes at Supercritical Fluid Extraction with Carbon Dioxide in a Vertical Gradient Field of Temperatures Open Journal of Metal, 2020, 10, 1-15 https://www.scirp.org/journal/ojmetal ISSN Online: 2164-277X ISSN Print: 2164-2761 Separation of Molybdenum Isotopes at Supercritical Fluid Extraction with Carbon Dioxide in a Vertical Gradient Field of Temperatures Boris Viktorovich Borts1, Stella Fedorovna Skoromnaya1, Viktor Ivanovich Tkachenко1,2 1NSC Kharkov Institute of Physics and Technology, NAS of Ukraine, Kharkov, Ukraine 2V. N. Karazin Kharkiv National University, Kharkov, Ukraine How to cite this paper: Borts, B.V., Sko- Abstract romnaya, S.F. and Tkachenко, V.I. (2020) Separation of Molybdenum Isotopes at Separation of molybdenum isotope complexes by supercritical fluid extraction Supercritical Fluid Extraction with Carbon (SFE) with carbon dioxide was studied experimentally. The extraction of mo- Dioxide in a Vertical Gradient Field of Temperatures. Open Journal of Metal, 10, lybdenum isotope complexes was carried out in the updated extraction 1-15. chamber (reactor) of the SFE-U installation, which provided an initial pres- https://doi.org/10.4236/ojmetal.2020.101001 sure of P ≤ 20 MPa at constant temperatures of the upper T1 = 35˚C and bot- Received: February 11, 2020 tom T2 = 45˚C flanges. The device, through which the eluent was discharged, Accepted: March 15, 2020 involved a set of four thin tubes of different lengths located inside the reactor. Published: March 18, 2020 The axes of the tubes and the reactor are parallel and the tubes are equally spaced circumferentially inside the reactor. The extract was removed from Copyright © 2020 by author(s) and Scientific Research Publishing Inc. each tube through channels isolated from each other and located in the bot- This work is licensed under the Creative tom flange with cylindrical expansion, in which several layers of filter paper Commons Attribution International were placed. After passing through the filters the extract entered a restrictor License (CC BY 4.0). http://creativecommons.org/licenses/by/4.0/ designed to remove the eluent from the reactor. The initial pressure of carbon Open Access dioxide and the holding time of the extract were specified in the experiments. The level of the eluent sampling was set by the lengths of the tubes depending on the reactor height. A method of producing molybdenum complexes was described. It was experimentally shown that at an initial pressure of 20 MPa and a given holding time a difference from the natural content of Mo isotopes for given heights of extract sampling depending on the reactor height was observed in extracts removed through filters. The ranges of deviation of the content of molybdenum isotopes in extracts from natural one were deter- mined. DOI: 10.4236/ojmetal.2020.101001 Mar. 18, 2020 1 Open Journal of Metal B. V. Borts et al. Keywords Carbon Dioxide, Supercritical Fluids, Extraction, Molybdenum, Isotopes, Separation 1. Introduction In view of various practical applications, there is a problem of separation and extraction of isotopes of chemical elements. A large number of scientific and technical literature is devoted to separation of iotopes of chemical elements. First of all, we should mention the problem of separation of natural uranium isotopes. It is of great practical interest for nuclear fuel production [1]-[7]. Recently, along with the problem of separation of uranium isotopes there is a problem of extraction of isotopes of chemical elements for use in nuclear medicine which deals with application of radionuclide pharmaceuticals in diagnosis and treatment of various diseases [8]. To assess the scale of the global use of radioisotopes we give the information on the United States [9] where about 130 radiodiagnostic methods in vivo and about 60 radiodiagnostic methods in vitro are used, which exceeds the domestic capabilities by several times. The number of radionuclide studies per 1000 people per year in Russia is 7, while in Austria—19, in Japan—25 and in the USA—40. In Ukraine, the number of studies per 1000 people per year is up to 20 [10] and this is only the lower border of the European level (20 - 50). Thus, with a growing number of radionuclide studies by 7% - 14% per year [11] there is a need to increase the production of radioisotope 99m Tc obtained from 99 Mo [12] [13]. The unstable isotope 99 Mo occupies one of the first places in the list of ra- dioisotopes and its use in medical practice is well studied [12]. The isotope 99m Tc 99 Mo β γ produced from as a result of and decay is included in various pharmaceuticals used in medical diagnostics to visualize the human in- ternal organs: thyroid and salivary glands; heart and large vessels; skeleton; brain tumors; genitourinary organs, etc. The start of production and organizing the application of 99m Tc isotope in Ukraine are relevant objectives due to the large number of cancers compared to world standards. [14]. Therefore, the isotope 99m Tc is an extremely necessary means for detecting cancer at an early stage. Along with traditional methods for producing the isotope 99m Tc in Ukraine [13], there is an alternative method based on new physical principles. The basis of this method is the recently developed technology for producing molybdenum complexes and its isotope complexes by supercritical fluid extraction with car- bon dioxide (SFE-СО2) [15] [16]. In this technology, molybdenum was extracted with tributyl phosphate from nitric acid solutions [15] [16]. It shows a rather low efficiency of molybdenum extraction due to its low solubility in dilute nitric ac- DOI: 10.4236/ojmetal.2020.101001 2 Open Journal of Metal B. V. Borts et al. id, as well as due to availability of molybdenum in nitric acid solutions in the form of molybdenum acids of various compositions. In [17], the redistribution of the isotopic composition of natural uranium 235U in natural in supercritical carbon dioxide (SC-CO2) experimentally is investi- gated. A diagram and description of the principle work of the experimental se- tup reactor are shown. A method for sample preparation of samples of granite, containing natural uranium, and the order of extraction are described. The con- 235 clusion that the spatial redistribution of isotopes U in SC-CO2 based on the analysis of gamma spectra of extracts is made. It is shown that for certain para- 235 meters of SC-CO2 the concentration of the isotope U is distributed unevenly in the reactor height: its maximum is near the heated lower flange and decreases with approaching to the top, the colder the flange of the reactor. The separation 235 factor U isotope in SC-CO2 could be a value near 1.2 is concluded. In [18], the models and analytical solutions extraction of 235U and 238U iso- topes complexes in the presence of microdroplets of water in the homogeneous temperature field or in the heated from bellow layer of the SC-CO2 are sug- gested. A homogeneous temperature field shows that the effectiveness of SFE with carbon dioxide complexes of uranium isotopes reaches a maximum at the limit of water solubility in SC-CO2. Theoretical calculations have shown that the maximum concentration of 235U isotope complexes in the heated from below SC-CO2 layer reaches 1.2% and observed near the heated bottom of layer. The order of the fulfillment of the SFE with carbon dioxide, in which the concentra- tion of the 235U isotope complexes is higher than the natural value, is described. In [19], the extraction of molybdenum acetylacetonate and its isotopes by the SFE-СО2 method was studied. The type of modifier, the time of fluid holding and the pressure in the reactor for the most efficient extraction of molybdenum and its isotopes were determined. A series of experiments for extraction of mo- lybdenum isotope complexes in the updated SFE-U installation at a constant pressure value of P = 20 MPa and at constant temperatures of the bottom T2 = 45˚C and upper T1 = 35˚C reactor flanges was carried out. In the experiments, the extract holding time and the height level of eluent sampling from the reactor were changed. The effect of deviation of the content of Mo isotopes from nat- ural one in the eluent depending on the temperature gradient, holding time and height sampling was described. In this paper, we continued the study of the extraction of molybdenum acety- lacetonate and its isotopes by the SFE-СО2 method with a new extract sampling device allowing us to obtain test samples differentially according to the reactor height. 2. The Idea, Materials and Updated Reactor for Extraction of Molybdenum Isotopes The idea of the experiments is to establish the fact of an uneven distribution of molybdenum isotopes in a vertical gradient temperature field at SFE-СО2 which DOI: 10.4236/ojmetal.2020.101001 3 Open Journal of Metal B. V. Borts et al. is set in the reactor after holding the fluid for 0.5 hours. Materials. Molybdenum acid (LRW) was used as the original source of mo- lybdenum. The extraction solution was obtained in a Soxhlet apparatus using 100 ml of acetylacetone (CP) and 10 g of molybdenum acid powder. Molybde- num acid powder was poured into a filter paper bag and placed in a glass sleeve. The sleeve was located in the center of the apparatus. After 20 cycles of Soxhlet apparatus operation, the upper vessel was completely filled with distilled acety- lacetone and the extract remaining in the lower flask was extracted for further experiments. The concentration of molybdenum solution in acetylacetone ob- tained for SFE-СО2 was about 25 mg/ml. Reactor for Extraction of Molybdenum Isotopes The experiments on study of SFE-СО2 of complexes of molybdenum isotopes were carried out on a laboratory facility for supercritical fluid extraction SFE-U in which, unlike [17], another type of device was used for extract removing.
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