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A.N. Frumkin Institute of Physical Chemistry and Electrochemistry of the Russian Academy of Sciences
Laboratory of physico-chemical methods of localization of radioactive elements
Publications
160
Citations
408
h-index
9
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Directions of the laboratory's work:
1) Improvement of spent nuclear fuel (SNF) reprocessing processes using oxidation and nitriding operations
2) Creation of new approaches to recycling waste containing plastic, ion-exchange resins, cellulose, toxic organic compounds
3) Development of radioactive iodine localization processes
4) Research in the field of inorganic chemistry of actinides
- X-ray phase analysis
- Differential Scanning Calorimetry (DSC)
- Thermogravimetry (TG)
- IR spectroscopy
- Nuclear spectroscopy
- Low-temperature nitrogen adsorption
- UV spectroscopy
- X-ray diffraction analysis
- X-ray absorption spectroscopy
- Raman spectroscopy
- Various types of inorganic syntheses: hydro (solvo) thermal, sol-gel, solid-phase
Sergey Kulyukhin
Head of Laboratory
Iurii Nevolin
Senior Researcher
Research directions
Improvement of spent nuclear fuel (SNF) reprocessing technologies)
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One of the main tasks of modern radiochemistry is to create a technology for reprocessing spent nuclear fuel for the implementation of a closed nuclear fuel cycle (SNF).
Publications and patents
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Rychagov A.Y., Volfkovich Y.M., Sosenkin V.E., Seliverstov A.F., Kulyukhin S.A., Mamonov V.A., Izmailova M.Y.
Konevnik Y.V., Martynov K.V., Kulyukhin S.A., Zakharova E.V.
The article presents the results of the study of the sorption of 90Sr, 137Cs, 233U, 237Np, 239Pu,and 241Am radionuclides from model groundwater, model leachate of aluminophosphate glass and Na2HPO4 solutions of different concentrations on bentonite clays of Kamalinskoye (Krasnoyarsk Territory), Desyaty Khutor (Republic of Khakassia), and Dinozavrovoye (Republic of Kazakhstan) deposits. We determined that the presence of aluminophosphate glass leachate in the liquid phase reduced the sorption activity of the studied clays towards caesium. The distribution coefficients of strontium depend more on the clay properties than on the liquid phase composition. However, with increasing concentration of phosphate ion, we observed an increase in the strength of sorbed strontium retention by clay. The sorption of uranium, neptunium, plutonium and americium, increased in the presence of components leached from the aluminophosphate glass-like matrix, and the strength of their fixation by clay increased.
Krasavina E.P., Martynov K.V., Arzumanova K.G., Bessonov A.A., Gordeev A.V., Bomchuk A.Y., Zharkova V.O., Kulyukhin S.A.
The extraction of the tricarbonate complex of uranyl [UO2(CO3)3]4– from aqueous solutions on clay powders from kaolin clays of the Kampanovskoye deposit and from bentonite clays of the 10th Khutor and Dinozavrovoe deposits, as well as their mixtures, was investigated. The studies were carried out with clay powders, both untreated and treated with water, 0.5 M Na2CO3 and NaNO3 solutions, and 2 M NaOH solutions. It was shown that the [UO2(CO3)3]4– complex is not sorbed on clay materials from aqueous solutions under static conditions. The filtration of an aqueous solution of [UO2(CO3)3]4– through columns with clay mixtures was established to enable the extraction up to 87% of uranium from the amount passed through the column.
Martynov K.V., Kulemin V.V., Krasavina E.P., Rumer I.A., Kostikova G.V., Kulyukhin S.A.
Phase formation in cast stone matrices (CSMs) fabricated through the interaction of comelted basalt with ZrO2 at 1623 K for 5 h on air was studied. Basalt melted under the above conditions contains two spinels (relict and newly formed), clinopyroxene of the composition Mg0.66Ca0.60Fe0.26Ti0.05Al0.66Si1.80O6, and glass as the major phases. When basalt is comelted with ZrO2, taken in a weight ratio of 1 : 1, CSMs containing zircon (ZrSiO4), glass, and baddeleyite (ZrO2) as the major phases are formed. Zirconium is concentrated mainly in two phases, zircon and baddeleyite. The rate of Zr leaching from the synthesized CSMs into H2O after 28 days is ~1.0 × 10–9 g/(cm2 day).
Martynov K.V., Kulemin V.V., Krasavina E.P., Rumer I.A., Nevolin Y.M., Kulyukhin S.A.
This work examines cast stone matrices (CSM) fabricated by comelting basalt and Sr, Ln (Ce, Nd, Gd) oxides. Matrices containing glass and clinopyroxene as the major phases were established to be resulted from the comelting of basalt with SrO. Strontium partially replaces calcium in clinopyroxene, but mostly enriches the melt in contact with crystallizing clinopyroxene. When this melt cools, glass is formed containing up to 31 wt % SrO. The doping of basalt with oxides of rare earth elements (REE) MxOy: CeO2, Nd2O3, Gd2O3 taken in a weight ratio of 4 : 1 and 2 : 1, results in the formation of CSM, the main permanent phases of which are glass and clinopyroxene. In addition, magnesioferrite can crystallize from a basaltic melt upon cooling, and phases of cerianite CeO2 or britholite Ca(Nd,Gd)4(SiO4)3O can crystallize depending on the basalt/MxOy weight ratio.
Martynov K.V., Kulemin V.V., Krasavina E.P., Rumer I.A., Kostikova G.V., Nevolin Y.M., Kulyukhin S.A.
This work examines cast stone matrices (CSM) fabricated by comelting of basalt with both uranium-bearing perlite (M150 grade) and U3O8 at a temperature of 1623 K in air for 5 h. As a result of comelting of basalt with uranium-free M150 grade perlite, matrices are obtained containing glass and spinel as the major phases. When basalt is comelted with uranium-bearing perlite (M150 grade) CSMs are formed, the major phases of which are two Cr-spinels of different compositions, uranium-bearing glass, and dendritic aluminosilicate crystals. In the case of fusion of basalt and U3O8 taken in the initial weight ratio of 1 : 1, CSM is generated as the major phases containing UO3, CaU3O10, (Al,Cr,Fe)2U2O9, plagioclase, and uranium-bearing glass. The leaching rate of uranium from a basalt melt with uranium-bearing perlite (M150 grade, ~7.2 wt % U) and that of CSM made by comelting of basalt with U3O8, (~42.5 wt % U) after 28 days contact with water at 298 K was investigated.
Kulemin V.V., Kulyukhin S.A.
The possibility of using the polymer sorbent Polysorb-1 for the treatment of nitric acid solutions to remove organophosphorus compounds, including tributyl phosphate (TBP) and hexachlorobutadiene (HCBD), is studied. It is shown that decontamination of nitric acid solutions containing organophosphorus compounds, HCBD, U(VI), and Pu(IV) with Polysorb-1 sorbent under dynamic conditions allows reducing the phosphorus and HCBD content to ~2 mg/dm3 or less and to 0.05 mg/dm3 or less, respectively. In this case, sorption of U(VI) and Pu(IV) does not occur. The procedures of vacuum distillation and overheated steam stripping are described for regeneration of Polysorb-1 sorbent containing TBP and HCBD. The optimal process temperature was chosen to be 170°C.
Kulemin V.V., Kostikova G.V., Kulyukhin S.A.
Sorption of tributyl phosphate (TBP) on a polymer sorbent Polysorb-1 in aqueous solutions and sorption of butylphosphoric acids onto layered Mg-Al double oxides and hydroxides in a 70% solution of TBP in dodecane was studied. It was found that the Polysorb-1 is suitable polymer sorbent to remove TBP in aqueous solutions in the static and dynamic modes, and LDH-Mg-Al-CD-OH is suitable sorbent to remove acidic products of the decomposition and hydrolysis of TBP in TBP solutions in dodecane.
Kulemin V.V., Rumer I.A., Nevolin Y.M., Krasavina E.P., Kulyukhin S.A.
The release of 137Cs into an Ar flow during the reaction of 137CsI and 137CsOH–137Cs2CO3 with molten lead at a temperature of ~852 K was studied. It was determined that during the heating of Pb0 with 137CsI, 137CsOH–137Cs2CO3, and 137CsI–137CsOH–137Cs2CO3 from 2 to 8% of 137Cs can pass into the gas flow. Based on the distribution of 137Cs among the elements of the gas purification system, it was concluded that the chemical and disperse composition of the compounds containing 137Cs in the gas phase is fairly heterogeneous. Volatile 137Cs compounds formed on heating 137CsI, 137CsOH–137Cs2CO3, and 137CsI–137CsOH–137Cs2CO3 with Pb0 in a gas flow at ~852 K can contain both charged aerosols and aerosols without an electric charge.
Volgin M.I., Kulyukhin S.A., Nevolin Y.M.
Oxidation of UO2 and UN by atmospheric oxygen and nitrogen hemioxide, which is a hard-to-localize greenhouse gas, was investigated by thermal analysis. For oxidation, mixtures of N2O–N2 and O2–N2 were used with a 20% volume fraction of the oxidizing agent. For UO2 and UN, the phase composition of the final oxidation product in air and in N2O is the same―U3O8. In both cases, N2O behaves as a milder oxidizing agent compared to atmospheric oxygen. Oxidation of UO2 and UN in an N2O flow starts at a temperature 180 and 70°C higher than in air, respectively. The oxidation of UN in an N2O flow proceeds in three stages. At the first stage, the reaction products are UO2 and U2N3; UO2 is the product of the second stage; and at the third stage U3O8 is produced. No pronounced staging is observed in the UO2 oxidation process. The possibility of utilizing nitrogen hemioxide when it is used in the course of voloxidation (oxidation) of spent nuclear fuel is shown.
Martynov K.V., Kulemin V.V., Kulyukhin S.A.
The work studied the distribution of cesium and strontium in cast stone matrices obtained by co-melting basalt and silica gel (hereinafter SiO2) containing cesium or strontium nitrates at 1623 K during 5 h. The melt cooling rate was ∼2 °C/min. Co-melting basalt and SiO2 containing CsNO3 or Sr(NO3)2 at a basalt/SiO2 initial mass ratio of 5 : 1 produced cast stone matrices, in which the main phases were Cr–Fe spinel and glass. At the same time co-melting basalt and SiO2 containing CsNO3 or Sr(NO3)2 at an initial mass ratio of 2 : 1 yielded matrices which, apart from Cr–Fe spinel and glass, included pollucite, clinopyroxene, and Ti-containing magnetite phases for Cs-containing system, magnetite and olivine phases for Sr-containing system. For Cs-containing system at a basalt/SiO2 initial mass ratio of 5 : 1 the glass phase showed almost an even distribution of cesium, whereas the spinel phase was virtually free of cesium. At a basalt/SiO2 initial mass ratio of 2 : 1 the major amount of cesium was found in the pollucite phase, where it mainly occurred in parts containing SiO2. Some amount of cesium was found in the glass phase. The other crystal phases found in the matrix were virtually free of cesium. For Sr-containing system at a basalt/SiO2 initial mass ratio of 5 : 1 the process yielded two types of glass: one rich in Ca and the other in Sr. Strontium was mainly found in the glass phases. The spinel phase was virtually free of strontium. At a basalt/SiO2 initial mass ratio of 2 : 1 strontium was mainly found in the glass phases. The magnetite, olivine, and Cr–Fe spinel phases were virtually free of strontium.
Kulyukhin S.A., Gordeev A.V., Seliverstov A.F., Kazberova A.Y., Kostikova G.V., Krasavina E.P., Nevolin Y.M.
A new approach to the destructive processing of the cation exchange resin KU-2×8-M (M = Cs, Ni, Cu, Fe, Nd, U) is considered based on the gas phase treatment in a nitrating atmosphere with subsequent chemical treatment of the conversion products. It is shown that exposure of the resin samples in an HNO3(vapour)–air atmosphere at temperatures of 403–443 K for 8 and 24 h followed by dissolution of conversion products in 0.5 M NaOH and ozonation of the resulting solutions allows efficient utilization of the resin.
Gerber E., Krot A., Andreadi K., Averin A.A., Shiryaev A., Trigub A., Sobolev N., Nevolin I.
The synthesis, characterization and thermal stability of uranium hydrazinates xUO3·yN2H4·zH2O – potential precursors for low temperature formation of actinide dioxides – is presented.
Ershov B.G., Komarov V.B., Kulyukhin S.A., Seliverstov A.E., Bondareva V.N.
Treatment of cellulose with ionizing radiation (γ-rays, accelerated electrons) provides the possibility to reduce its molecular weight, change the molecular weight distribution, increase the esterification reactivity and affect other physical and chemical characteristics. The acquired properties, in turn, make it possible to obtain then esters with the desired characteristics. We present the results of studying the effect of γ-irradiation of industrial grades of cellulose on the esterification products, i.e., lacquer colloxylins and xanthogenates. It is found that γ-irradiation at a dose of 3 - 5 kGy prior to mercerization leads to an increase in the reactivity of the polymer in the reaction of xanthogenation by more than 30%. Nitro derivatives corresponding to the technical characteristics (conditional viscosity and nitrogen content) of colloxylins of different grades were obtained by irradiation at a dose of 20 and 30 kGy. It is shown that the stages of prehydrolysis and reduction of nitrocellulose viscosity during its treatment in autoclaves can be excluded when producing colloxylins. It appeared possible to reduce significantly the consumption of carbon disulfide in the technology of xanthocarbon production. The results obtained can be used in developing optimal modes and performance criteria for radiation pretreatment of cellulose of different grades during nitration and xanthogenation proceeding from changes in their physical and chemical properties upon γ-irradiation.
Nevolin I.M., Petrov V.G., Grigoriev M.S., Averin A.A., Shiryaev A.A., Krot A.D., Maslakov K.I., Teterin Y.A., Fedoseev A.M.
This work presents details of the synthesis, properties and structure of a novel neptunium carbonate (NH4)[NpO2CO3], a member of the M[AnO2CO3] (M = K, (NH4), Rb, Cs) class of compounds. Carbonates play an important role in the migration of actinides in the environment, and thus are relevant for handling and disposal of radioactive wastes, including spent nuclear fuel and vitrified raffinates. Knowledge of the crystallographic structure of these compounds is important for models of the environmental migration behavior based on thermodynamic descriptions of such chemical processes. (NH4)[NpO2CO3] crystals were obtained during long-term hydrothermal treatment of Np(VI) in aqueous ammonia at 250 °C. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) show that a single-phase sample containing only Np(V) was obtained. Structural features of (NH4)[NpO2CO3] were elucidated from single crystal X-ray diffraction and confirmed by vibrational spectroscopy. The results obtained are of interest both for fundamental radiochemistry and for applied problems of the nuclear fuel cycle.
Сергей Алексеевич Кулюхин, Андрей Валентинович Гордеев, Елена Петровна Красавина
RU2724893C1,
2020
Сергей Алексеевич Кулюхин, Игорь Андреевич Румер, Владимир Борисович Крапухин, Виктор Александрович Лавриков, Владимир Васильевич Кулемин, Елена Петровна Красавина, Маргарита Петровна Горбачева
RU184350U1,
2018
Алексей Владимирович Сафонов, Варвара Евгеньевна Трегубова, Константин Эдуардович Герман, Сергей Алексеевич Кулюхин, Борис Григорьевич Ершов, Ольга Анатольевна Горбунова
RU2528433C1,
2014
Сергей Алексеевич Кулюхин, Наталья Андреевна Коновалова, Маргарита Петровна Горбачева, Игорь Андреевич Румер, Елена Петровна Красавина, Любовь Владимировна Мизина
RU2497213C1,
2013
Сергей Алексеевич Кулюхин (RU), Сергей Алексеевич Кулюхин, Николай Борисович Михеев (RU), Николай Борисович Михеев, Алла Николаевна Каменска (RU), Алла Николаевна Каменская, Наталь Андреевна Коновалова (RU), Наталья Андреевна Коновалова, Игорь Андреевич Румер (RU), Игорь Андреевич Румер, Любовь Владимировна Мизина (RU), Любовь Владимировна Мизина, Нина Васильевна Танащук (RU), Нина Васильевна Танащук, Елена Петровна Красавина (RU), et. al.
RU2346346C2,
2008
Lab address
Москва, Ленинский проспект, 31, корп. 4
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