Relationship between particle size and radiocesium in fluvial suspended sediment related to the Fukushima Daiichi Nuclear Power Plant accident

We collected fluvial suspended sediments in Fukushima after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident and analyzed the ¹³⁷Cs concentration in bulk and size-fractioned samples to investigate the particle-size-dependent distribution of radiocesium. The ¹³⁷Cs concentration in bulk suspended sediments decreased from August to December 2011, possibly reflecting a decrease of radiocesium concentration in its source materials. Smaller particles had higher radiocesium concentrations, reflecting larger specific surface areas. Silt- and sand-size fractions occupied more than 95 % of the total ¹³⁷Cs in the suspended sediments. The contribution of clay-size fractions, which had the highest ¹³⁷Cs concentration, was quite small because of their low frequency. A line of the data showed that the particle size distribution of radiocesium was essential to evaluate the migration and distribution of radiocesium in river systems where radiocesium is mainly present as particulate form after the FDNPP accident.     

Cs, Am and Pu isotopes as tracers of sedimentation processes in the Curonian Lagoon–Baltic Sea system

¹³⁷Cs, ²⁴¹Am and Pu isotopes were analyzed in seawater, bottom sediments (BS) and suspended particulate matter samples collected in the Baltic Sea during 1997–2011. The particle size distribution and sequential extraction studies were carried out with the aim to better understand the association of radionuclides with particles and their bonding patterns in the BS. δ¹³C_org was applied for identification of sources of organic matter in the studied area. It has been found that massic activities of ¹³⁷Cs in BS varied from 2.1 to 588 Bq/kg. High correlation of ¹³⁷Cs massic activities with total organic carbon (TOC) in BS (r = 0.75) and with clay minerals (r = 0.95) was found. ^239,240Pu massic activities in BS varied from 0.03 to 7.5 Bq/kg. High correlation with TOC was found for ^239,240Pu (R = 0.98) as well as for ²⁴¹Am (r = 0.96). δ¹³C_org in the studied samples ranged from ?22.3 to ?31.8 ‰.     

Local distribution of radioactivity in tree leaves contaminated by fallout of the radionuclides emitted from the Fukushima Daiichi Nuclear Power Plant

We analyzed fresh and dead leaves collected in forests in Fukushima after the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident, using autoradiography. Both fresh and dead leaves of Cryptomeria japonica were contaminated by radionuclides (¹³⁴Cs and ¹³⁷Cs). Contamination of the fresh leaves was possibly attributed to interception of radionuclides by tree canopies, whereas the dead leaves indicated the direct deposition of radionuclides by fallout and/or washout of radionuclides intercepted by tree canopies. Translocation of radiocesium from a contaminated branch to new leaves growing after the FDNPP accident was not clearly observed, although transfer of radiocesium from leaf parts to male flowers occurred. Fallen leaves of Quercus serrata, which started growing after the FDNPP accident, did not show radioactivity, indicating that significant amounts of translocation from other parts to new leaves did not occur. Fallen leaves of Q. serrata collected from a litter showed hot spots originating from direct fallout. Needles of Pinus densiflora were also contaminated by fallout. Leaching with pure water removed soluble fractions of radiocesium and hot particles from the surface of the contaminated leaves, but significant amounts of radioactivity remained. This means that foliar absorption occurred in both fresh and dead leaves. Further leaching experiments using surfactant and acetone could not remove the remaining radiocesium from the leaves. The leaching experiments indicate that radiocesium in the contaminated leaves is strongly fixed in leaf tissues and is not readily released unless leaf tissues are decomposed.     

Accumulation of radiocesium by <Emphasis Type="Italic">Pleurotus citrinopileatus</Emphasis> species of edible mushroom

Pleurotus citrinopileatus, a species of edible mushrooms, is widely accepted food component, especially in Indian subcontinent. The accumulating susceptibility of this edible mushroom species towards long-lived radioisotopes of cesium was studied in controlled laboratory condition using the ¹³⁴Cs (T _1/2 = 2.06 y) radioisotope. It was observed that the experimental mushroom species accumulated ¹³⁴Cs and maximum accumulation took place in the cap portion. The pileus (cap)/stipes (stem) ratio of each ¹³⁴Cs accumulated mushroom sample was determined and found 2.22±0.74. The protein and fat fractions of the experimental mushroom species were extracted separately after accumulation of radiocesium and it was found that most of the radiocesium accumulation occurred in the protein fraction of the mushroom. The mushroom Pleurotus citrinopileatus which is white in color, turned completely black after radiocesium accumulation. The black mushroom so obtained was produced upto fourth generation by tissue culture method without using any radiocesium further. All the successors were found to be black indicating a permanent mutation of the mushroom species.     

A study on radionuclide association with soil components using a sequential extraction procedure

Measurements performed in 1986–1988 demonstrate that most of the radiocesium isotopes (¹³⁷Cs and¹³⁴Cs) deposited after the Chernobyl accident are still located in the upper soil layers (0–2 cm). The vertical migration appears to be slow, and only a small fraction of the radiocesium has been transferred into the biological cycle. Sequential extraction techniques have been utilized in order to investigate the degree of binding or association between deposited radionuclides (¹³⁷Cs,¹³⁴Cs and⁹⁰Sr) and components in soil. The results indicate that a major fraction of the radiocesium is associated strongly with organic and mineral materials in the litter or upper soil layers: less than 10% is easily leachable. The distribution of¹³⁷Cs throughout the fractions was similar to that determined for naturally occurring stable cesium (¹³³Cs), implying that isotopic exchange had been extensive. For⁹⁰Sr, the results show a relatively high leachable fraction. Therefore, present results indicate that radiocesium should be less mobile, and less available for root uptake, than⁹⁰Sr in soil.     

A laboratory approach for investigations into the potential effectiveness of potassium-based fertilisers in reducing radiocesium transfer from soil to plant

The paper presents a laboratory experimental model based on a simplesoil-plant system used to investigate the potential effectiveness of potassium-basedfertilisers in reducing soil-to-plant transfer of radiocesium. The soil-plantsystem, slightly modified comparing to that described originally in the NEUBAUER'splantlet method, consists in wheat plantlets grown from caryopsis phase onbrown acid soil contaminated with ¹³⁷Cs resulted from Chernobylnuclear accident and treated with potassium salt of 30%. The effectivenessof 30% potassium salt applied to the soil as treatment is discussed in termsof reduction factor for ¹³⁷Cs soil-to-plant transfer coefficientand ¹³⁷Cs ⁺ :K ⁺ ratio in soil and plantlets.     

Experimental investigation of radiocesium sorption on ceramic clay using a batch method

In this study, radiocesium sorption on ceramic clay was investigated as a function of particle size and initial ¹³⁷Cs concentration using a batch method. Ceramic clay samples taken from the Sö?üt(?nisar) clay deposit were composed of kaolinite, dickite and quartz. The equilibrium time and the liquid–solid ratio were determined as 60 min and 250 mL g^?1, respectively. The distribution coefficients (K _d) for variable liquid–solid ratio and the percentage adsorption (P _Ad) were calculated. The values of K _d and P _Ad ranged from 483 to 3165 mL g^?1 and 34–93%, respectively. The K _d and P _Ad values increased with increasing particle size, but decreased with increasing initial concentration. The sorption data were interpreted in terms of a Langmuir isotherm. The results indicated that the Sö?üt(?nhisar) ceramic clay has good sorption capacity for cesium.     

Investigation of radiocesium biokinetics in Manila clam (Ruditapes philippinarum)

This study was carried out to better understand the biokinetics of radiocesium in clams living in sediment. The accumulation and depuration kinetics of ¹³⁴Cs were investigated in the Manila clam (Ruditapes philippinarum) under controlled laboratory conditions. The concentration factor was found to be 3.0 for ¹³⁴Cs in the whole body; however, the concentration factor in the soft part of the clams (12) was significantly higher than those in the whole body and shell (0.80). The depuration kinetics of the radionuclide were described by a two-component exponential model for the whole body. The biological half-lives in the fast and slow components were found to be 0.63 and 22.1 days, respectively. The depuration kinetics for ¹³⁴Cs in the soft parts were described by a single-component exponential model with a resultant the biological half-life of 18.0 days.     

Stability-Indicating HPTLC Method for Analysis of Moclobemide, and Use of the Method to Study Degradation Kinetics

A sensitive, selective, precise, and stability-indicating HPTLC method for analysis of moclobemide in the bulk drug and in formulations has been established and validated. Aluminium TLC plates precoated with silica gel 60 F₂₅₄ were used with benzene–methanol–40% ammonia 7:3:0.1 (v/v) as mobile phase. Densitometric analysis was performed in absorbance mode at 238 nm. Compact bands were obtained for moclobemide (R _F 0.67 ± 0.02; n = 6). The drug was subjected to acidic and alkaline hydrolysis, oxidation, dry heat treatment, and photodegradation. The drug undergoes degradation under acidic, basic, and oxidising conditions. The degradation products were well resolved from the pure drug with significantly different R _F values, so the method can be regarded as stability-indicating. Response to moclobemide was a linear function of amount in the range 50–600 ng per band, with a correlation coefficient, r ², of 0.9967 ± 0.51. LOD and LOQ, determined experimentally, were 10 and 30 ng per band, respectively. Statistical analysis proves the method is repeatable and specific for analysis of moclobemide. The method was used to investigate the kinetics of alkaline degradation. The Arrhenius plot was constructed and the activation energy calculated.     

A preliminary study on 226Ra, 232Th, 40K and 137Cs activity concentrations in vegetables and fruits frequently consumed by inhabitants of Elazığ Region, Turkey

Determining radioactivity levels in foodstuffs is of great importance for the protection of human health. In addition, the literature includes few studies related to this subject in Turkey. In this study, gamma spectroscopic system was used in order to measure ²²⁶Ra, ²³²Th, ⁴⁰K and ¹³⁷Cs activity concentrations in vegetables and fruits produced in Elaz?? Region. The average activity concentrations in vegetables was calculated as 0.64 ± 0.26 Bq kg^?1 for ²²⁶Ra, 0.65 ± 0.14 Bq kg^?1 for ²³²Th, 13.98 ± 1.22 Bq kg^?1 for ⁴⁰K, and 0.54 ± 0.04 Bq kg^?1 for ¹³⁷Cs. The average activity concentrations in fruits were 1.52 ± 0.34, 0.98 ± 0.23, 18.66 ± 1.13 and 0.59 ± 0.16 Bq kg^?1, respectively for ²²⁶Ra, ²³²Th, ⁴⁰K and ¹³⁷Cs. Total committed effective dose value was determined as 20 and 30.55 μSv y^?1, respectively for vegetables and fruits. The findings were compared with previous data reported for Turkey and other regions of the world.     

Radiometric analysis of rock and soil samples of Leepa Valley; Azad Kashmir, Pakistan

In this article, we present results obtained from a radiometric survey that was conducted in the Leepa Valley of Azad Jammu & Kashmir, Pakistan. The purpose of current study is to appraise the radioactivity levels and the associated health hazards due to the terrestrial radionuclide in soil and rock samples. In this regard, 16 soil and 17 rock samples were collected from different locations of the Leepa Valley. After processing the samples, activity concentrations of primordial (²³²Th, ²²⁶Ra and ⁴⁰K) and anthropogenic (¹³⁷Cs) radionuclides were determined using a P-type coaxial high purity germanium detector. From the results obtained the mean activity concentrations of radionuclides ²²⁶Ra, ²³²Th and ⁴⁰K in the soil samples were found to be 31.25 ± 0.46, 44.1 ± 1.07 and 575 ± 8.89 Bq kg^?1 respectively. Whilst, in rock samples ²²⁶Ra, ²³²Th and ⁴⁰K mean activities were found as 28.46 ± 0.45, 48.63 ± 1.12 and 666.7 ± 9.39 Bq kg^?1, respectively. The ¹³⁷Cs concentration level in soil and rock samples is found to be 15.04 ± 0.29 and 5.7 ± 0.16 Bq kg^?1, respectively. The average radium equivalent activity (R _aeq) was found as 143.16 and 142.93 Bq kg^?1 in soil and rock samples, respectively. These findings are less than the recommended safe value of 370 Bq kg^?1 as given in OECD report (1979). The values of external (H _ex) and internal hazard index (H _in) are also less than unity. Mean value of absorbed dose rate was found as 69.78 nGy h^?1 for the soil samples, which is in good agreement with the world wide average value (70 nGy h^?1). Mean value of absorbed dose rate from rock samples was found as 70.01 nGy h^?1. Mean values of the annual effective dose is also lower than the values reported for different other countries of the world.     

Extraction equilibrium and thermodynamics of cesium with a new derivative of calix[4]biscrown

A new supermolecular recognition agent named tetra-tert-butyl-calix[4]-bis[(4-methly-1,2-phenylene-crown-6] (TertButylCalixC) was synthesized. Batchwise experiments of extraction of Na(I), K(I), Rb(I), Cs(I), Sr(II), Ba(II), Ru(III) and Fe(III) from aqueous solution with TertButylCalixC/o-nitroanisole were carried out. Effects of HNO₃ concentration, contact time and temperature on the extraction behavior were examined. The equilibrium established within 30 min implied a fast extraction kinetics. The optimal operation temperature was 298 K. Stoichiometry of TertButylCalixC and Cs(I) by electrospray ionization mass spectrometry characterization revealed 1:1 molar ratio. It was observed that the extraction system of TertButylCalixC/o-nitroanisole was effective for selective removal of Cs(I), showing remarkable separation performance.     

Benzene sorption complex of fully dehydrated fully Mn2+-exchanged zeolite Y (FAU) and its single-crystal structure

The single-crystal structure of a benzene sorption complex of fully dehydrated fully Mn²⁺-exchanged zeolite Y, |Mn_37.5(C₆H₆)₂₄|[Si₁₁₇Al₇₅O₃₈₄]-FAU, has been determined by single-crystal synchrotron X-ray diffraction techniques in the cubic space group Fd $ \overline{3} $ m at 100(1) K. A fully dehydrated and fully Mn²⁺-exchanged zeolite Y (|Mn_37.5|[Si₁₁₇Al₇₅O₃₈₄]-FAU, Si/Al = 1.56) was treated with zeolitically dried benzene at 297(1) K for 3 days. The structure was refined using all intensities to the final error indices (using the 544 reflections for which F _o > 4??(F _o)) R ₁ = 0.050 (based on F) and wR ₂ = 0.147 (based on F ²). In this structure, Mn²⁺ ions occupy four crystallographic sites: 13.5 Mn²⁺ ions are at the centers of the double 6-rings; 4 Mn²⁺ ions are in the sodalite cavity opposite to the double 6-rings; the remaining 20 Mn²⁺ ions are found at two non-equivalent threefold axes in the sodalite cavity and supercage with occupancies of 2 and 18, respectively. The 24 benzene molecules are found at two distinct positions within the supercages. Eighteen benzene molecules are found on the threefold axes in the supercages where each interacts facially with one of site-II Mn²⁺ ions (Mn²⁺-benzene center = ca. 2.53 Å). The remaining six benzene molecules lie on the planes of the 12-rings where each is stabilized by multiple weak electrostatic and van der Waals interactions with framework oxygens.     

Radioactivity measurements in epiphytic lichens of Uludağ Mountain in Western Anatolia

Activity concentrations of gross-β, naturally occurring ²²⁶Ra, ²³²Th, ²¹⁰Pb, ⁷Be and anthropogenic ¹³⁷Cs in epiphytic lichens collected from Uluda? Mountain are presented and discussed with the aim of evaluating potential usability of lichens as a biomonitor. The activity concentrations of gross-β, ¹³⁷Cs, ⁴⁰K, ²²⁶Ra, ²³²Th, ²¹⁰Pb and ⁷Be in the lichen samples were found to be in the range of 177–707, 4.05–94.26, 86–211, below detection limit (BDL)—19.2, BDL—14.0, 229–872, and 72.1–220.7 Bq kg^?1 in dry weight, respectively. ¹³⁷Cs content in collected epiphytic lichens was in descending order: Parmelia sulcata > Lobaria pulmonaria > Pseudevernia furfuracea > Usnea filipendula. The best biomonitor for ¹³⁷Cs among the lichen species used in this study was determined as Parmelia sulcata. Pearson’s correlation coefficient was calculated between ¹³⁷Cs and ⁴⁰K activity concentrations using a statistical package program (SPSS ver. 17.0) and a negative correlation value (R = ?0,323, p = 0,222) was obtained. The highest ²²⁶Ra and ²³²Th activity concentrations were found in Bo?azova Yaylas? which has a geological structure including granitic rocks. It was found that ¹³⁷Cs and ⁷Be activity concentrations in species demonstrated an inverse behaviour. The effect of mean annual precipitation and temperature on ⁷Be activity concentration was determined using multi regression analysis. Also, correlations between the ¹³⁷Cs and ⁷Be, and ⁴⁰K and ⁷Be were investigated.     

Investigation into the crystal structure of bis(pyridine)-bis(trichloroacetato) copper(II) and its electrophotochemical properties

A novel chained Cu(II) complex was synthesized from trichloroacetato copper(II) and pyridine in ethanol solvent, and characterized by elemental analysis and infrared (IR) spectroscopy. The special crystal structure of the Cu(II) complex was determined by X-ray single-crystal diffraction. The results indicate that a chained structure of the Cu(II) complex formed through intermolecular hydrogen bonds. Cu(CCl₃COO)₂(C₅H₅N)₂(H₂O) was monoclinic, with unit cell P21/c and cell parameters as follows: a = 14.389(3) Å, b = 7.1911(14) Å, c = 23.107(8) Å, V = 2,257.5(10) Å³, Z = 4, M _r = 564.51, D _c = 1.661 mg/m³, T = 293(2) K, F(000) = 1,124, μ(Mo K_α) = 1.704 mm^?1, R = 0.0984, and ωR = 0.2791. The electrochemical behavior of the Cu(II) complex on a glassy carbon working electrode determined by cyclic voltammetry showed the electrochemical activity of the title compound at 0.2 to ?0.3 V (versus SCE) in NH₃–NH₄Cl buffer solution (pH 9.2), and the redox peak current of the complex had a good linear relationship with the square root of the scan rate in the range 0.02–0.2 V/s.     

Biomonitoring of 137Cs fall-out in Kudankulam coastal waters, Gulf of Mannar, India

Concentration of fall-out ¹³⁷Cs activity was monitored for a period of 3 years in coastline surface, near-shore surface and bottom waters of Kudankulam coast where a mega nuclear power station is being set up. Activity of ¹³⁷Cs was estimated by HPGe gamma spectrometry after chemical processing with AMP (ammonium molybdophosphate). The total ¹³⁷Cs concentration ranged from 1.2 to 1.6 mBq/L in coastline surface waters and between 0.75 and 1.4 mBq/L in near-shore surface and bottom waters. The data set followed a log-normal distribution. An insignificant relationship between ¹³⁷Cs and salinity, temperature and pH was noted. No yearly variation and no variation between surface and bottom waters were observed (p > 0.05) in the concentration of ¹³⁷Cs. The ¹³⁷Cs activity between seasons was found to be significantly different (p < 0.05).     

Dietary intakes of radioactive cesium for Ukrainians

Daily intakes of ¹³⁴Cs and ¹³⁷Cs in Ukrainians were estimated in relation to the health effects on habitants after the Chernobyl accident. Two hundred and sixty-eight diet samples were collected from 25 oblasts (regions) using a duplicate portion method. For Ukrainians, the range and median daily intakes of ¹³⁷Cs were 0.53–571 and 8.8 Bq per person, respectively. Intakes of ¹³⁴Cs were also detected in highly ¹³⁷Cs contaminated areas. Daily intakes of ¹³⁴Cs were in the range of not detected to 3.6 Bq per person. Using the highest radiocesium intakes, annual effective doses for ¹³⁴Cs and ¹³⁷Cs were estimated to be 2.5·10⁻² and 2.7 mSv, respectively.     

Crystal structure and <Superscript>121,123</Superscript>Sb NQR parameters of ammonium tridecafluorotetraantimonate(III) NH<Subscript>4</Subscript>Sb<Subscript>4</Subscript>F<Subscript>13</Subscript>

(NH₄)Sb₄F₁₃ crystals (I) are synthesized and their crystal structure (tetragonal crystal system: a = 9.6431(2) Å, c = 6.5503(2) Å, V = 609.11(3) ų, Z = 2, d _calc = 4.100 g/cm³, F(000) = 664, space group I4?) is determined. The main structural units of I are tetranuclear anionic [Sb₄F₁₃]^? complexes and [NH₄]⁺ cations. The anionic complexes are built of four SbF₃ groups linked together by tetrahedral bridging fluorine atom. At room temperature the (NH₄)Sb₄F₁₃ crystals are isostructural to previously studied МSb₄F₁₃ (М = K, Rb, Cs, and Tl). The study of ^121,123Sb NQR spectra of compound I is performed in a range of 77-370 K, which shows that when the temperature decreases (<250 K) the substance exhibits piezoelectric properties, as do other compounds of this group, but with a violation of their isostructurality.     

An electron-diffraction study of the molecular structure of gaseous perbromyl fluoride and calculation of its force field and vibrational amplitudes

The molecular structure of FBrO₃ has been studied by gas-phase electron diffraction. Least-squares refinements of the molecular geometry using fixed spectroscopic amplitudes revealed two geometrical minima. Initially, the amplitudes employed were derived from diagonal force fields obtained by spectroscopic least-squares refinements to fit observed and calculated wave numbers; for each geometry there are two spectroscopic minima. In the lowest geometrical minimum the wave number agreement is poor, however, the introduction of the ∠OBrO/∠FBrO interaction force constant removed the discrepancies; the resulting force field is F(Br-O) = 6.92 ± 0.02 mdyn Å^?1F(Br-F) = 3.22 ± 0.03 mdyn Å^?1, F(∠OBrO) = 1.06 ± 0.02 mdyn Å, F(∠FBrO) = 0.81 ± 0.03 mdyn Å, F(∠OBrO/∠FBrO) = ?0.19 ± 0.02 mdyn Å. In the corresponding geometrical minimum r_g(Br-O) = 1.582 ± 0.001 Å, r_g(Br-F) = 1.708 ± 0.003 Å, r_α(∠OBrO) = 114.9 ± 0.3°, r_α(∠FBrO) = 103.3 ± 0.3°. Perpendicular amplitude correction coefficients, calculated for each force field employed, were used throughout to relate the interatomic distances through the r_α-structure. The geometries of the r_α^o- and r_e-structures are estimated.     

Distribution of cesium-137 in tree crop products collected from residence islands impacted by the U.S. nuclear test program in the northern Marshall Islands

The Marshall Islands Program at the Lawrence Livermore National Laboratory has completed a series of radiological surveys at Bikini, Rongelap, Utrōk, and Enewetak Atolls in the Marshall Islands designed to take a representative sample of food supplies with emphasis on determining ¹³⁷Cs activity concentrations in common food plants. Coconuts (Cocos nucifera L.) are the most common and abundant food plant, and provided a common sample type to characterize the level and variability of activity concentrations of ¹³⁷Cs in plant foods collected from different islands and atolls. Other dominant food types included Pandanus (Pandanus spp.) and breadfruit (Actocarpus spp.). In general, the activity concentration of ¹³⁷Cs in food plants was found to decrease significantly between the main residence islands on Bikini, Rongelap, Utrōk, and Enewetak Atolls. The mean activity concentration of ¹³⁷Cs measured in drinking coconut meat and juice was 0.72 (95 % CI 0.68–0.77) and 0.34 (95 % CI 0.30–0.38) Bq g^?1, respectively, on Bikini Island; 0.019 (95 % CI 0.017–0.021) and 0.027 (95 % CI 0.023–0.031) Bq g^?1, respectively, on Rongelap Island; 0.010 (95 % CI 0.007–0.013) and 0.007 (95 % CI 0.004–0.009) Bq g^?1, respectively, on Utrōk Island; and 0.002 (95 % CI 0.0013–0.0024) and 0.002 (95 % CI 0.001–0.0025) Bq g^?1, respectively, on Enewetak Island. High levels of variability are reported across all islands. These results will be used to improve the accuracy and reliability of predictive dose assessments, help characterize levels of uncertainty and variability in activity concentrations of fallout radionuclides in plant foods, and allow atoll communities to make informed decisions about resettlement and possible options for cleanup and rehabilitation of islands and atolls.