Distribution of <Superscript>137</Superscript>Cs, <Superscript>90</Superscript>Sr, <Superscript>239 + 240</Superscript>Pu, <Superscript>241</Superscript>Am,and <Superscript>244</Superscript>Cm among Components of Organic Matter of Soils in Near Exclusion Zone of the Chernobyl NPP

Distribution of Chernobyl-derived ¹³⁷Cs, ⁹⁰Sr, ^{239 + 240}Pu, ²⁴¹Am, and ²⁴⁴Cm among organic fractions of soddy-podzolic, sandy, soddy-meadow, and peat soils collected from the Chernobyl Exclusion Zone along the North-Western radioactive fallout track was determined. Regardless of the soil type, 80–85% of ¹³⁷Cs is tightly fixed on the mineral fraction of the soil. Depending on the soil type, 50–70% of ⁹⁰Sr and 15– 45% of ²⁴¹Am are associated with fulvic acid fractions. ²⁴¹Am and ²⁴⁴Cu are similarly distributed among the organic acid fractions. In all the soil types studied, ^{239 + 240}Pu is associated essentially with humic acid fractions. Natural ^{230, 232}Th and technogenic ^{239 + 240}Pu are similarly distributed among the organic fractions.__________Translated from Radiokhimiya, Vol. 47, No. 1, 2005, pp. 91–96.Original Russian Text Copyright © 2005 by Odintsov, Pazukhin, Sazhenyuk.     

Transuranium elements in liquid radioactive wastes from the Shelter

The volume activity of ⁹⁰Sr, ¹³⁷Cs, ²³⁸Pu, ^239+240Pu, ²⁴¹Am, and ²⁴⁴Cm in water taken from unorganized water accumulations on lower marks of the Shelter was determined. Separate water accumulations are characterized by their specific radionuclide activity ratios ²³⁸Pu/^239+240Pu, ²⁴¹Am/^239+240Pu, and ²⁴⁴Cm/²⁴¹Am. The activity ratios ²⁴¹Am/^239+240Pu and ²⁴⁴Cm/^239+240Pu in the water accumulations are 5–10 times higher than in the irradiated fuel of the 4th Unit of the Chernobyl NPP and in lava-like fuel-containing materials.     

Determination of the content of radioactive elements in irradiated beryllium

The elemental composition of the material of beryllium blocks of SM reactor reflector in the initial state was determined by inductively coupled plasma atom emission spectrometry (ICP AES). The α-, β-, and Γ-active components of the radiation from Be irradiated to a neutron fluence of 6 × 10²² cm⁻² (E > 0.1 MeV) were determined. Radiochemical analysis revealed the presence in the irradiated Be of ⁶⁰Co, ⁵⁴Mn, ¹³⁷Cs, ¹³⁴Cs, and ⁹⁰Sr. The following α-emitters were revealed: ^238–241Pu, ²⁴¹Am,²⁴³Am, and ²⁴⁴Cm.     

Reduction of radioactive waste volume using selective crystallization processes

Satisfactory combination of small volume of compositions incorporating ¹³⁷Cs, ⁹⁰Sr, and ²⁴⁴Cm with the admissible heat release rate can be attained by crystallization of definite compounds from high-level solutions. The concentrate of cesium isotopes is obtained by their precipitation in the form of phosphoromolybdate and, after additional storage, in the form of CsMgPO₄·6H₂O; the concentrate of Am, Cm, Sr, Ba, and Ln can be obtained using the known but somewhat modified (increased pH of solution) OXAL process. It is appropriate to remove Am and long-lived Cm isotopes from this concentrate also after storage ensuring the decay of ⁹⁰Sr and ²⁴⁴Cm. The remaining rare-earth elements with traces of Am and Cm and stable isotopes of Sr and Ba can be disposed of, e.g., in the form of a mineral-like phosphate.     

Radioactive Contamination of the Neva River-Lake Ladoga Aquatic System

Many-year monitoring data on the ⁹⁰Sr and ¹³⁷Cs levels in water of the Neva River and Lake Ladoga are presented. In 1970-1990, the ⁹⁰Sr level in the Neva River steadily increased. In 1991, a radiological survey was made of the Kit experimental vessel with radioactive wastes in its holds, which was on berthing in the northwesteren part of Lake Ladoga. ⁹⁰Sr, ¹³⁷Cs, and ^239,240Pu were monitored in water and bottom sediments near the Kit vessel berthing after it was towed outside Lake Ladoga. In 2001, the ⁹⁰Sr concentration in water of Lake Ladoga and the Neva River considerably decreased.     

Physicochemical Processes Occurring in Long-Term Storage of Liquid Radioactive Waste in Deep Underground Collector Beds

Interaction under hydrothermal conditions (pressure 3 MPa; temperature 80-170°C; contact time up to 2500 h) of intermediate-level acidic waste with bed rock of the underground repository for liquid radioactive waste is studied. Transformation of rock-forming minerals under these conditions is accompanied by increasing absorption of ¹³⁷Cs, ⁹⁰Sr, ²³⁹Pu, ²⁴¹Am, and ²³⁸U.     

Influence of temperature on the sorption properties of rocks from the Nizhnekansky massif

The kinetics of radionuclide sorption onto finely divided samples of rocks from the Nizhnekansky massif, taken from the level of the planned arrangement of deep radioactive waste repository, was studied, and the times in which the sorption equilibrium was attained at 20 and 90°С were determined. The distribution coefficients of actinides (²³³U, ²³⁹Pu, ²⁴¹Am) and fission products (¹³⁷Cs, ⁹⁰Sr) were determined. Increasing the temperature from 20 to 90°С intensifies the sorption of the radionuclides studied, except cesium for which the sorption slightly decreases.     

Effect of Contact Time of Liquid Radioactive Waste with Bed Rock of Underground Repository on Migration Behavior of 90Sr, 137Cs, 239Pu,and 241Am

Behavior of radionuclides caused by interaction of acidic waste with sandy bedrock in deep underground repositories is studied, including sorption-desorption of ⁹⁰Sr, ¹³⁷Cs, ²³⁹Pu, and ²⁴¹Am. The amount of mobile forms of radionuclides decreases with increasing contact time with bedrock, thus decreasing the migration rate of the radionuclides in the collector bed.     

A Method for Determining the Isotope Composition of U, Pu, Am, and Cm in "Hot" Particles and Spent Nuclear Fuel

A method was proposed for determining the content of ^234-238U, ^238-242Pu, ^241-243Am, and ^242-244Cm in "hot" fuel particles and spent nuclear fuel. The method is based on high-precision measurement of the -activity in the sample and calculation of the relative contributions of individual nuclides or radionuclide groups to the total activity. Partitioning of U, Pu, Am, and Cm was carried out by ion-exchange chromatography. The contents of ²³⁴U, ²³⁶U, ²³⁸U, ²³⁸Pu, ^239+240Pu, ²⁴²Pu, ²⁴¹Am, ^242mAm, ²⁴³Am, ²⁴²Cm, and ²⁴⁴Cm in "hot" particles sampled in the Chernobyl area were reported. The applicability of the method proposed to determining the radionuclide composition of spent nuclear fuel was discussed.     

Procedure for Simultaneous Determination of Uranium and Transuranium Elements in Groundwater and Liquid Radioactive Wastes from the Shelter

An ion-exchange procedure for simultaneous determination of ²³⁴U, ²³⁵U, ²³⁶U, ²³⁸U, ²³⁸Pu, ^{239 + 240}Pu, ²⁴¹Am, and ²⁴⁴Cm in groundwater and liquid radioactive wastes is described. The concentration and separation of U and Pu are performed on AV-17 anion exchanger in the chloride form from 9 M HCl. Am and Cm are separated from rare-earth elements by step-by-step elution from KU-2 cation-exchange resin in the NH ₄ ⁺ form with α-hydroxyisobutyric acid (pH 4.75). Finally, U, Pu, Am, and Cm are determined α-spectrometrically.     

Sorption of long-lived radionuclides onto main types of rocks of the Novaya Zemlya Archipelago

The ability of black carbonaceous siltstones and silt sandstones, lime sandstones, gray limestones, carbon–silicon carbonate schists with pyrite, and other rocks that most widely occur on the Novaya Zemlya Archipelago to sorb ¹³⁷Cs, ⁹⁰Sr, ^239+240Pu, and ²⁴¹Am was studied. The distribution coefficients K _d (cm³ g^–1) are as follows: for ^239+240Pu, 2.7 × 10³–7.7 × 10³; for 241Am, 2.5 × 10³–1.8 × 10⁴; and for ¹³⁷Cs, 1.1 × 10²–2.0 × 10³. Strontium-85(90) it not noticeably sorbed (within the measurement uncertainty) by any of the rocks studied. ^239+240Pu, ²⁴¹Am, and ¹³⁷Cs are strongly sorbed onto the rocks studied and are not noticeably desorbed from them with distilled water. The data obtained are required for predicting the migration of long-lived radionuclides generated by nuclear explosion with surface waters from test sites on the Novaya Zemlya Archipelago.     

Estimation of the Solubility of Radioactive Aerosol Particles in Biological Liquids

The solubility of the aerosol hot particles, sampled in 1987 in the town of Pripyat, in the simulated lung fluid (SLF) (Gamble or Ringer solution) and in 0.1 M HCl was studied under static conditions. Leaching of radionuclides from the hot particles in the SLF decreases in the order ¹³⁷Cs > ⁹⁰Sr >> ^239+240Pu ²⁴¹Am, and in 0.1 M HCl, in the order ⁹⁰Sr > ²⁴¹Am >> ¹³⁷Cs > ^239+240Pu. The degree of passing into 0.1 M HCl solution for ⁹⁰Sr and ²⁴¹Am was estimated at 3.3-21 and 2.7-17%, respectively. Depending on the particle size, 0.06-2.2% of ²⁴¹Am and 0.2-1.8% of ^239+240Pu passes into the SLF within 28 days.     

Microbiological treatment of oil-containing radioactive waste prior to cementation

Microbiological oxidation of liquid organic radioactive waste (ORW), spent vacuum and transformer oils, is described. The physicochemical properties of oils and their structural-group composition before and after using in the process cycle were studied. Changes in the structural-group composition and physicochemical parameters of oils upon microbiological treatment were determined. The distribution of radionuclides between the organic and aqueous phases upon microbiological treatment was studied by the example of model ORW containing ¹³⁷Cs, ⁹⁰Sr, ²³⁸Pu, and ²⁴¹Am. The compatibility of oils subjected to microbiological treatment with the cement compound intended for ORW disposal was evaluated. The biological step of the radioactive oil processing leads to a decrease in the weight and volume of the organic radioactive waste and increases its amount that can be incorporated into the cement compound (to 30 vol %) without deterioration of the strength characteristics of the cement.     

Diffusion of some critical radionuclides in mineral-like ceramic materials

The diffusion coefficients and activation energy of diffusion of ²²Na, ⁹⁰Sr, ¹⁵²Eu, and ²⁴¹Am radionuclides in zirconolite ceramics prepared by cold crucible induction melting (CCIM), of ²²Na, ⁹⁰Sr, ¹³⁷Cs, ¹⁵²Eu, and ²⁴¹Am in Synroc-C ceramics prepared by hot pressing (HP) and CCIM, and of ²²Na and ¹⁵²Eu in the ceramic from the Lawrence Livermore National Laboratory (the United States), synthesized by cold pressing (CP) and sintering, and also the diffusion mobility of ⁹⁰Sr, ¹³⁷Cs, and ²⁴¹Am in the chromium-containing sphene glass ceramic prepared by CCIM were determined by the method of integral residual activity. In the temperature interval 573–923 K, the ²²Na radionuclide is the most mobile and ²⁴¹Am is the least mobile. The differences between the diffusion coefficients reach 4–5 orders of magnitude. The diffusion coefficients of the examined radionuclides in the ceramic depend both on the preparation procedure (HP, CP, or CCIM) and on the initial charge components when the same procedure is used for preparing the ceramic. Negative values of the activation entropy of the diffusion of ²²Na, ⁹⁰Sr, ¹⁵²Eu, and ²⁴¹Am in ceramics suggest that the mass transfer of radionuclides in them occurs not by the vacancy mechanism but by the interstitial mechanism and, probably, in part along the facilitated migration pathways (grain boundaries, pore surfaces, micro- and macrocracks).     

Role of Suspended Matter and Dissolved Organic Substances in Behavior and Migration of Anthropogenic Radionuclides in River-Sea Aquatic Systems

Distribution of Cs, Sr, and Pu nuclides between suspended matter and the aqueous phase and the features of interaction of these radionuclides with dissolved organic matter are studied, to gain a better insight into the radionuclide behavior in the Ob and Yenisei estuaries and adjacent Kara Sea. For radionuclide speciation, the experimental study included determination of the radionuclide activities in aqueous solutions after filtration and ultrafiltration of large-volume water samples and membrane fractionation of small-volume water samples by passing the solution through a cartridge with filters of regularly decreasing pore size followed by mass-spectrometric determination of elements. In the water-soluble fraction, the ¹³⁷Cs activity increases with increasing salinity, whereas that of ⁹⁰Sr decreases, which can be attributed to the differences in the physicochemical behavior of the radionuclides in solutions and also to the effect of contamination sources. In seawater, suspended material can retain 1-10% of ¹³⁷Cs and ⁹⁰Sr. In the estuarine zones, these values can be 20-40%. More than 50% of ⁹⁰Sr and ^239,240Pu are associated with dissolved organic matter. In saline water this effect is less pronounced.     

Radionuclides in ground waters from observation holes in the Shelter local area

The volume activity of ³H, ⁹⁰Sr, ¹³⁷Cs, ²³⁴U, ²³⁵U, ²³⁸U, ²³⁸Pu, ^239+240Pu, and ²⁴¹Am in ground waters from observation holes 1-G-6-G in the north section of the Shelter local area of the Chernobyl Nuclear Power Plant (CNPP) was measured. The distribution of radionuclides in the suspension fractions of the ground waters was evaluated. The main contribution to the pollution of ground waters with uranium is due to natural uranium isotopes: ^234,235,238U. The activity ratios of ²³⁸Pu, ^239+240Pu, and ²⁴¹Am in ground waters are similar to those in the spent fuel of 4th CNPP block.     

Speciation of artificial radionuclides 60Co, 137Cs, 152Eu, and 241Am in bottom sediments of the Yenisei river

The speciation of artificial radionuclides ⁶⁰Co, ¹³⁷Cs, ¹⁵²Eu, and ²⁴¹Am in surface layers of bottom sediments of the Yenisei river, collected within the near zone of impact of the Mining and Chemical Combine (Rosatom), was studied. In these samples the radionuclides ⁶⁰Co, ¹⁵²Eu, and ²⁴¹Am are mainly associated with fractions of humic and fulvic acids. The fraction of ¹⁵²Eu associated with nonsilicate iron is approximately 92%. The migration capability of radionuclides collected near the Atamanovo settlement decreases in the order ¹⁵²Eu > ²⁴¹Am > ⁶⁰Co > ¹³⁷Cs. For samples collected near Bol’shoi Balchug settlement, this order is as follows: ¹⁵²Eu ≈ ²⁴¹Am > ⁶⁰Co > ¹³⁷Cs. The presence of radionuclide-bearing micro-particles in bottom sediments considerably complicates the distribution of radionuclides, in particular, of ²⁴¹Am and ¹³⁷Cs, among migration forms.     

Preparation, Properties, and Application of Modified Mikoton Sorbents

To improve the performance of chitin-containing Mikoton-Ch sorbent, it was modified with K2Cu[Fe(CN)6] or Fe2O3. The sorbents modified with a mixture of these agents were also prepared. The modifying agents are strongly fixed on the Mikoton surface. The techniques for preparing the modified Mikoton are described. The sorption of Cs, Sr, Pu, and Am on modified Mikoton sorbents was studied in relation to the modifier content. Mikoton modified with K2Cu[Fe(CN)6] efficiently sorbs ¹³⁷Cs with the distribution factor K _d of up to 10⁴ ml/g but exhibits low sorption power for Sr, Pu, and Am. Mikoton modified with Fe3O4 is a ferromagnetic material. This sorbent exhibits increased sorption power for Pu and Am (K _d = 10⁴-10⁵ ml/g) but poorly sorbs ¹³⁷Cs. The feasibility of practical application of different kinds of modified Mikoton sorbents is demonstrated.     

Radioactive Fallout and Accumulated Level of Soil Surface Contamination with 90Sr and 137Cs around St. Petersburg in 1954-1999

Systematic data on radioactive atmospheric fallout in 1954-1999 and accumulated levels of contamination of the soil-vegetable cover with ⁹⁰Sr and ¹³⁷Cs around St. Petersburg, estimated on 1998, are presented. Comparative analysis is made of these data and directly obtained data on the vertical distribution of these radionuclides in the surface horizon (0-25 cm) of soddy-podzolic sandy loam soil: the levels of surface contamination with ^90Sr and ¹³⁷Cs were found to be 580±90 and 6500±600 Bq m^-2 on 1998. Before April 28, 1986 the ⁹⁰Sr and ¹³⁷Cs radioactivity in the investigated region corresponded to the global level. After Chernobyl accident the contamination levels with ⁹⁰Sr and ¹³⁷Cs increased, respectively, from 1200 to 1280 (by 6.3%) and from 2400 to 7050 Bq m^-2 (by a factor of 2.9). The ⁹⁰Sr and ¹³⁷Cs vertical distributions throughout the soil profile are considerably different: ¹³⁷Cs is practically totally fixed in the surface horizon, its activity being exponentially declining; whereas the stock of ⁹⁰Sr in horizons 0-10 and 0-25 cm represents only 22 and 59% of the integral accumulated inventory of ⁹⁰Sr in the soil (990 Bq m^{- 2}). The activity ratio of ¹³⁷Cs to ⁹⁰Sr in the atmospheric fallout in 1963-1985 was 1.85±0.42, and in river water in the same period, ca. 0.18, suggesting higher mobility in the soil of ⁹⁰Sr as compared to ¹³⁷Cs, and, therefore, higher rate of self-cleaning of the surface soil horizon with respect to ⁹⁰Sr.     

Radionuclide composition of fragments of lava-like fuel-containing materials from the CNPP fourth unit

Samples of fuel-containing materials taken inside the CNPP Fourth Unit were analyzed by γ- and α-ray spectrometry. The isotope ratios for Cs, Eu, Pu, Am, and Cm were measured, and the fuel burn-up in the samples was determined. Inconsistencies in theoretical estimations on the production of all the radionuclides over ²⁴¹Am were revealed. The burn-up values determined from data on the Cs isotopes systematically differ from those determined from data on the other radionuclides. The causes of these facts are discussed.