Influence of freezing on physicochemical forms of natural and technogenic radionuclides in Chernozem soil

Sharp variations of different climatic parameters influence the transport, transfer, and deposition of contaminants in nature. Investigations of the impact of environmental temperature on the fractionation of radionuclides in soil are necessary for adequate assessment of their distribution and bioavailability in case of a nuclear accident. The impact of a sharp decrease of environmental temperature shortly after radioactive contamination on the physicochemical fractionation of natural and technogenic radionuclides in Chernozem soil and its influence on their potential migration ability and bioavailability in case of subsequent warming were evaluated. The soil was contaminated in a laboratory with ²⁴¹Am, ⁶⁰Co, ¹³⁷Cs, ²²⁸Ra, ²³⁴Th, and U and two temperature regimes were used for storage. Changes of the radionuclides association with various soil phases in the first weeks after contamination were studied. Physicochemical forms of ²⁴¹Am, ⁶⁰Co, ²²⁸Ra, ²³⁴Th, and U were determined using two sequential extraction procedures. The ion-exchangeable forms of ¹³⁷Cs were evaluated by single extraction with 1 M NH₄NO₃. The data showed that the freezing, following the radioisotope contamination of the soil, causes an increase of the amount of potentially mobile forms of radiocobalt, radiocesium, radium, and thorium and has an insignificant impact on the fractionation of americium and uranium.     

Chemical speciation of radionuclides migrating in groundwaters

In order to more accurately predict the rates and mechanisms of radionuclide migration from lowlevel waste disposal facilities via groundwater transport, ongoing studies are being conducted at field sites at Chalk River Laboratories to identify and characterize the chemical speciation of mobile, long-lived radionuclides migrating in groundwaters. Large-volume water sampling techniques are being utilized to separate and concentrate radionuclides into particulate, cationic, anionic, and nonionic chemical forms. Most radionuclides are migrating as soluble, anionic species which appear to be predominately organoradionuclide complexes. Laboratory studies utilizing anion exchange chromatography have separated several anionically complexed radionuclides, e.g.,⁶⁰Co and¹⁰⁶Ru, into a number of specific compounds or groups of compounds. Large-volume ultra-filtration experiments have shown that significant fractions of the radionuclides are being transported in these groundwaters in the form of macromolecules having molecular weights ranging from less than 3,000 to 100,000.     

Investigation of the solid phase speciation of90Sr,137Cs,239Pu and241Am in soils determined by extraction and ultra-filtration methods

Bio-availability of radionuclides in soil is influenced by their chemical form and association with different geo-chemical phases. The solid phase speciation of aged⁹⁰Sr,¹³⁷Cs,²³⁹Pu and²⁴¹Am in three common agricultural soil types was investigated using separate extractions with seven reagents. Six of these are commonly used to determine radionuclide association with readily exchangeable forms, carbonates, iron and manganese oxides and organic phases. Trimethyl-chlorosilane was also included because of its ability to extract radionuclide-humate complexes from soil. The extract from this part of the study was subsequently subjected to ultra-filtration to determine the association of radionuclides with different molecular size fractions. The results from this speciation study are discussed in terms of availability for plant uptake.     

Chemical speciation of radionuclides through the microbial process in soils

Environmental factors (nutrients and pH) influence the retention of Sr, Cs, and Ba as analogue of long-lived radionuclides by the microorganism. The effect of pH and concentration of organic nutrients are proved to be significant factors for retention of cations (Sr, Cs and Ba) by the microorganisms inoculated from surface soil. Microorganisms can affect the speciation of Sr, Cs, and Ba in the environment. Concentration of organic nutrients and pH are indicated to be the important environmental factors in the consideration of the migration of the radionuclides through microbial processes in the terrestrial environment.     

Environmental impact of some cement manufacturing plants in Saudi Arabia

This work is concerned with the environmental impact of the cement industry in the west of Saudi Arabia represented in two cement plants and one cement depository. The concentrations of natural and artificial radionuclides in samples of cement (raw materials and end product) and soil, collected from the cement plant and its surrounding area, were measured using γ-ray spectrometer employing a HPGe detector. In addition, the levels of 19 major and trace elements were also determined in these samples using the inductively coupled plasma atomic emission spectroscopy. The concentrations of the ²³⁸U series isotopes in soil samples show a clear radiological impact of the cement industry upon the environment. Possible contamination with Ca and some other elements in soil samples that are rich with the fine grain size was observed. Cluster analysis of soil samples using convenient attributes shows an obvious evidence of the cement industry impact upon the environment. The hidden effect of the cement industry upon the environment was observed when the convenient measured attributes were used in cluster analysis of soil samples.     

Levels and effects of natural radionuclides in soil samples of Garhwal Himalaya

Distribution of natural radionuclide gives significant parameter to assess the presence of gamma radioactivity and its radiological effect in our environment. Natural radionuclides are present in the form of ²²⁶Ra, ²³²Th and ⁴⁰K in soil, rocks, water, air, and building materials. Distribution of natural radionuclides depends on the type of minerals present in the soil and rocks. For this purpose gamma spectrometer is used as tool for finding the concentration of these radionuclides. The activity concentration of naturally occurring radionuclides ²²⁶Ra, ²³²Th and ⁴⁰K in these soil samples were found to vary from of 8 ± 1 Bq/kg to 50 ± 10 Bq/kg with an average 20 Bq/kg, 7 ± 1–88 ± 16 Bq/kg with an Average 26 Bq/kg and 115 ± 18–885 ± 132 Bq/kg with an average 329 Bq/kg, respectively. In this paper, we are presenting the radiological effect due to distribution of natural radionuclide present in soil of Garhwal Himalaya.     

Determination of 241Am in Environmental Samples: A Review

The determination of ²⁴¹Am in the environment is of importance in monitoring its release and assessing its environmental impact and radiological risk. This paper aims to give an overview about the recent developments and the state-of-art analytical methods for ²⁴¹Am determination in environmental samples. Thorough discussions are given in this paper covering a wide range of aspects, including sample pre-treatment and pre-concentration methods, chemical separation techniques, source preparation, radiometric and mass spectrometric measurement techniques, speciation analyses, and tracer applications. The paper focuses on some hyphenated separation methods based on different chromatographic resins, which have been developed to achieve high analytical efficiency and sample throughput for the determination of ²⁴¹Am. The performances of different radiometric and mass spectrometric measurement techniques for ²⁴¹Am are evaluated and compared. Tracer applications of ²⁴¹Am in the environment, including speciation analyses of ²⁴¹Am, and applications in nuclear forensics are also discussed.     

Leaching of uranium,radium and thorium from vertisol soil by ground water

Shallow land burial is routinely used for the disposal of low-level radioactive waste. Natural processes causing leaching of radionuclides can lead to contamination of surrounding ground water and soil by the radionuclides. The comparative leachability of radionuclides U_(nat), ²²⁶Ra, ²²⁸Ra and Th_(nat) from the soil of a radioactive waste disposal site, by ground water was evaluated. The probability of leaching was obtained in the following order Ra (≈77%) > U (≈40%) > Th (≈20%). Observed ratios (OR) were calculated to correlate leachability of radionuclides to that of major cations Ca²⁺ and Mg²⁺. The leaching of the radionuclides was seen to be dependent on Ca²⁺ and SO₄²⁻ leached from the soil. This study provides sitespecific leachability of radionuclides, that can be used as indicator of the tendency for migration or retention in soil. It can play an important role during an unforeseen accident like breach of containment at the waste disposal site leading to contamination of soil and ground water and causing hazard to public via drinking water route.     

Speciation of aluminium fluoride complexes and Al in soils from the vicinity of an aluminium smelter plant by hyphenated High Performance Ion Chromatography Flame Atomic Absorption Spectrometry technique

The paper presents a new tool for the determination of inorganic speciation forms of aluminium: AlF_n^{(3 − n)+}, and Al³⁺ by means of the HPIC-FAAS. The proposed method has been successfully used for speciation analysis (qualitative and quantitative) of inorganic aluminium forms AlF_n^{(3 − n)+} in soil samples. In order to isolate the most environmentally available fraction, 5 g of the sample was collected and extracted in deionised water (water soluble fraction) for 1 h using a magnetic stirrer. The determinations in a hyphenated technique system were performed for a number of prepared water extracts. Concentration determinations of particular aluminium forms were performed based on model studies and real samples. The separation of Al species with nominal charge of + 1, + 2, and + 3 required a run time of less than 4 min during a single analysis. Based on the analysis of water extracts of soil, it was obtained that aluminium forms elute in the following order: 1PA (first signal) — AlF₂⁺ and/or AlF₄⁻; 2PA (second signal) — AlF²⁺ and/or AlF₃⁰; 3PA (third signal) — Al³⁺. In order to confirm the occurrence of these forms a simulation using the Mineql program was conducted. The details of speciation analysis of aluminium fluoride forms by means of an HPIC-FAAS instrument equipped are presented. Interpretation of the speciation analysis of the water soluble fraction of soil samples is proposed, based on the separation during chromatographic run and calculated data by Mineql.     

The importance of separation chemistry for the determination of radionuclides in environmental samples

Separation chemistry plays an important role when alpha-and beta-emitting natural and artificial radionuclides at low levels must be determined in complex environmental matrices. This paper describes some separation techniques used in radioecology, with special emphasis on extraction chromatography. The very high necessary decontamination factors are pointed out together with the suggested techniques. The following examples are given: (a) determination of⁹⁰Sr in soils in the presence of high concentration of²¹⁰Bi; (b) determination of cosmogenic³²P in sea water and its decontamination from²³⁴Th; (c) determination of⁶³Ni and⁵⁹Ni in liquid effluents; (d) separation techniques used for the speciation of plutonium in sea sediments and (e) plutonium and²⁴¹Am concentration and vertical distribution in mosses.     

Monitoring the environmental contamination of Kara Sea and shallow bays of Novaya Zemlya

The distribution of ¹³⁷Cs and ^239,240Pu in various ecosystems of the Kara Sea as well as speciation of these radionuclides has been studied to assess their potential mobility. In bottom sediment and seawater samples collected in Abrosimov, Tsivolky, Stepovoy, and Sedov Bays and on the coast of Novaya Zemlya, the content of anthropogenic radionuclides ¹³⁷Cs and ^239,240Pu does not exceed the values typical of the offshore zone in the Kara Sea (in sea water: 1.0–3.7 Bq/m³ for ¹³⁷Cs and 50–90 mBq/m³ for ^239,240Pu; in bottom sediments: 0.5–18.3 Bq/kg for ¹³⁷Cs and 4.3–7.3 Bq/kg for ^239,240Pu). The present monitoring study is important for the development of a long-term forecast for the dynamics of environmental contamination in the shallow bays of Novaya Zemlya.     

Depth profiles of long lived radionuclides in Chernobyl soils sampled around 10 years after the accident

Depth profiles of the long-lived radionuclides, ¹³⁷Cs, ⁹⁰Sr, Pu isotopes and ²⁴¹Am were examined in undisturbed sandy, peaty and Podsol soils in the Chernobyl 30 km exclusion zone sampled around 10 years after the accident. Two Podsol soils, which have different radioactive deposition characteristics, have also been examined. Activity ratios of ^239,240Pu/¹³⁷Cs, ⁹⁰Sr/¹³⁷Cs, and ²⁴¹Am/¹³⁷Cs in the 0-1 cm layer of the two Podsol soils differed very much. Speciation of the radionuclides by sequential selective extraction was examined in the soils. Depth profiles of the soils have been analyzed according to the speciation results and soil characteristics.     

The radiation dose and distribution coefficient of 210Po and 210Pb concentrations in aquatic environs of major rivers of coastal Karnataka

The activity of ²¹⁰Po and ²¹⁰Pb was measured in different matrices of aquatic ecosystem of the major rivers of Coastal Karnataka viz, Kali, Sharavathi and Netravathi. The environmental samples such as surface water, suspended particulate matter and sediment have been subjected to analyses. The activity of these two radionuclides were determined by radiochemical separation of ²¹⁰Po and counting the activity using a ZnS(Ag) alpha counter. The activity ratio of ²¹⁰Po and ²¹⁰Pb and correlation between the activity of these radionuclides were studied. From the measured concentration of ²¹⁰Po and ²¹⁰Pb, the internal Committed Effective Dose to the population for the study area was calculated. The distribution coefficient K_d between water, suspended particulate matter and sediments have been calculated to understand the distribution and accumulation of these radionuclides in different matrices of the aquatic environment.

     

Certified reference material for radionuclides in seawater IAEA-381 (Irish Sea Water)

A certified reference material (CRM) for radionuclides in seawater, IAEA-381 (Irish Sea Water), is described and the results of certification are presented. The material has been certified for nine radionuclides (⁴⁰K, ⁹⁰Sr, ¹³⁷Cs, ²³⁷Np, ²³⁸Pu, ²³⁹Pu,²⁴⁰Pu, ^239,240Pu and ²⁴¹Am). Information on massic activities with the corresponding 95% confidence intervals are given for eight radionuclides (³H, ¹²⁵Sb, ²³⁴U, ²³⁵U, ²³⁶U, ²³⁸U, ²⁴¹Pu and ²⁴⁴Cm). Less reported radionuclides include ⁶⁰Co, ⁹⁹Tc, and ²⁴²Pu. The CRM may be used for quality assurance/quality control of the analysis of radionuclides in environmental water samples, for the development and validation of analytical methods and for training purposes. The material is available from the IAEA in 5 kg units.     

Influence of plant roots upon the mobility of radionuclides in soil, with respect to location of contamination below the surface

The movement of⁸⁵Sr,¹³⁷Cs,⁵⁴Mn and⁶⁰Co in the 50 cm soil profile was studied with and without the presence of plant roots (triticum aestivum) in order to investigate the influence of roots and depth contamination upon the migration of radionuclides. The water table was maintained manually at 3 cm from the bottom. The physiochemical characteristics (E_h Fe^–2, NH ₄ ⁺ , pH and moisture content) as well as the total and extractable radioactivity were investigated. In the discrete contamination, where the location of contamination varied within the soil profile (0–5, 25–30 or 45–50 cm from the top), the influence of location upon the movement of these radionuclides was also studied. It was found that the changes in the soil physicochemical characteristics influenced the mobility of the four radionuclides. The extractability of⁵⁴Mn and⁶⁰Co was significantly increased in the reducing region of the soil, whereas that of⁸⁵Sr,¹³⁷Cs was not. Plant roots excerted significant effects upon the soil characteristics, via, reducing the E_h pH and moisture content of the soil; increasing the extractability of both⁵⁴Mn and⁶⁰Co from the depth of 35 cm downwards. Radionuclide migration occurred via physicochemical and biological transport. The biological transport via plant roots was of particular importance for¹³⁷Cs. Location of contamination had a significant influence upon the mobility of radionuclides. The migration of radionuclides was in the sequence of contamination in middle>bottom>top. The degree of the influence varied with radionuclides concemed. In the top layer contamination, the rank of the migration from the contamination layers, on the other hand⁵⁴Mn,⁶⁰Co and¹³⁷Cs were more mobile and the movement was:⁸⁵Sr⁵⁴Mn⁶⁰Co>¹³⁷Cs. In the middle and bottom contamination layers, on the other hand,⁵⁴Mn and⁶⁰Co and¹³⁷Cs were more mobile and the movement was⁸⁵Sr⁵⁴Mn⁶⁰Co>¹³⁷Cs. The results provide evidence conceming the soil-root interaction influencing the transfer efficiency of radionuclides from below the soil surface into the human food chain.     

Microstructures and speciation of radionuclides in natural environment studied by advanced spectroscopy and theoretical calculation

The environmental behavior of radionuclides is mainly dependent on their speciation and microstructures at solid particles.The speciation and microstructures of radionuclides at molecular level can be achieved from advanced spectroscopy techniques and theoretical calculations.In this perspective,we give a brief introduction of the advanced X-ray absorption fine structure(XAFS) technique and theoretical calculation in the analysis of the speciation and microstructures of radionuclides in the natural environment,which is crucial to evaluate the physicochemical behavior of radionuclides in the environment.     

Organic soil as a radionuclide sink in a High Arctic environment

Summary The role of organic soil as a sink for radioactive contaminants in a High Arctic environment was studied. Samples were obtained from an area of organic soil located on the Arctic archipelago of Svalbard (79° N) and from a non-organic control site in the same region. Samples were differentiated into organic layers and the underlying material and measured for a suite of anthropogenic and natural radionuclides and for a variety of soil chemistry parameters. Results indicated that the organic components of the soil constitute a sink term for a number of radionuclides. Values for Pu isotopes, ¹³⁷Cs and ²³⁸U were appreciably higher at the study site than at the control site, by up to a factor of 40 for Pu and 20 for ¹³⁷Cs and ²³⁸U. The source of ²³⁸U to the site appeared to be enrichment of this isotope from surface or melt water via adsorption to to either iron hydroxides or organic matter although the situation pertaining to Pu and ¹³⁷Cs remains less clear.     

Actinides and Long-Lived Radionuclides in Tissues of the Japanese Population: Summary of the Past 20-Year Studies

Radioactive fallout constitutes the major source of contamination of the environment with fission products. Our primary interest was in selected fission products, such as ¹³¹I, ⁸⁹Sr, ⁹⁰Sr, and ¹³⁷Cs, and neutron activation products, such as ³H and ¹⁴C. Plutonium-239,240, ²⁴¹Am and ⁹⁰Tc are generated from nuclear tests, and they are important by-products of nuclear industries. Polonium-210, ²¹⁰Pb and ²³²Th, ²³⁰Th and ²²⁸Th occur widely in nature. These radionuclides enter the human body through inhalation and the ingestion through food and water. These nuclides may cause radiation doses to certain organs of the body. Assessment of the resulting health hazards is an essential public health activity, which demands reliable techniques for the assay of the various radionuclides in man and his environment. In this paper, we present the accumulation of radionuclides from man-made sources and primordial radionuclides in various tissues of the Japanese population. The studies were performed at the Department of Public Health, Akita University School of Medicine, during the periods from 1973 to 1995.     

Characterizing phosphorus in environmental and agricultural samples by 31P nuclear magnetic resonance spectroscopy

Phosphorus nuclear magnetic resonance (³¹P-NMR) spectroscopy has advanced our knowledge of organic phosphorus (P) in soils and environmental samples more than any other technique. This paper reviews the use of ³¹P-NMR spectroscopy for soil, water and other environmental samples. The requirements for a successful solid-state or solution ³¹P-NMR experiment are described, including experimental set-up, sample preparation, extractants, experimental conditions, and post-experimental processing. Next, the literature on solid-state and solution ³¹P-NMR spectroscopy in environmental samples is reviewed, including papers on: methods; P transformations; agricultural, forest and natural ecosystem soil studies; humic acid and particle size separations; manure, compost and sludge studies; and water research, including freshwater, estuary and marine studies. Future research needs are also discussed as well as suggestions to improve results, such as increased standardization among research groups.     

Influence of Different Microplastic Forms on pH and Mobility of Cu2+ and Pb2+ in Soil

Microplastics, due to their surface properties, porosity and electrostatic interactions have a high affinity for cations sorption from the aqueous phase. As soil is a complex matrix, interactions between microplastics, soil constituents and heavy metals (HM) may modify the soil microenvironment for heavy metal mobilization/immobilization processes. In order to better understand the problem, three commonly found forms of microplastics in soil (fibers, fragments and microbeads) were mixed with Cu²⁺- or Pb²⁺-contaminated soil and incubated at 22 °C for 180 days. In soil samples pH and the content of water and acid exchangeable species of metals were analyzed. The results of this study showed that the presence of microplastics in HM-contaminated soil affected metal speciation, increasing the amount of easily exchangeable and potentially bioavailable forms of Cu²⁺ or Pb²⁺ in the tested soil. Soil pH also increased, confirming that microplastic particles affect soil properties relevant to the sorption/desorption process of metal cations. Overall, the smallest microplastic particles (≤1 mm), such as fibers or glitter microbeads, had a greater impact on the change in the sorption and desorption conditions of metals in tested soil than larger particles. The findings of our study show that microplastic form, shape and size should be considered as important factors that influence the soil properties and mobility of heavy metals in soil.