Utilizing low-cost purple coneflower (Echniacea purpurea) marc for competitive sorption of 152+154Eu(III), 60Co(II) and 134Cs(I) radionuclides.

Echinacea purpurea marc (EPM), a residual of echinacea herb after the extraction process, was used as a natural low-cost sorbent for competitive sorption of 152+154Eu(III), 60Co(II) and 134Cs(I) radionuclides. The EPM was ground to prepare it for use in the sorption process. The variables influencing the sorption process were assessed, including pH, contact time, concentrations of metal ions, and temperature. EPM was characterized by different analytical instruments such as FTIR, SEM, XRD, and DTA/TGA. pH 4.0 was selected as the ideal pH value for competitive sorption of the studied ions. Adsorption kinetics data found that the sorption followed a pseudo-second-order model. The adsorption isotherm data was significantly better suited by the Langmuir isotherms in the case of Eu(III) ions while following Freundlich in the case of Co(II) and Cs(I) ions. Positive ΔHo values confirm the endothermic character of metal ion sorption onto EPM. The loading efficiencies of Eu(III), Co(II), and Cs(I) ions in the EPM column were 66.67%, 9.59%, and 4.81%, respectively. The EPM is a cost-effective and efficient separation of Eu(III) ions more than Cs(I) and Co(II) ions. Therefore, in the future, it will be a starting point for the separation of trivalent elements of lanthanide ions.

A green approach to efficient soil decontamination using supercritical carbon dioxide and ethanol.

As the need for global decommissioning and site remediation of aging and shut-down nuclear power plants continues to grow, it becomes increasingly crucial to efficiently treat contaminated soil while minimizing waste generation. This study explores an innovative soil decontamination approach that utilizes supercritical carbon dioxide (SCCO2) as the primary solvent, along with ethanol as a co-solvent and specific additives, including a chelate ligand (catechol ligand) and a co-ligand (NEt4PFOSA). The advantages of SCCO2, such as its penetration and solubility, coupled with its ability to separate from radioactive waste, are harnessed in this research. The study demonstrates that the combination of SCCO2, ethanol, and additives significantly enhances decontamination efficiency, particularly for cesium (Cs), strontium (Sr), and uranium (U) contamination. Results indicate that decontamination efficiency varies with soil particle size, with smaller particles presenting greater challenges. This study presents a promising eco-friendly soil decontamination technology using SCCO2 containing ethanol and specific additives to efficiently reduce radioactive contamination in soil.

Continuous-wave optically stimulated luminescence properties of Guajillo chilli polyminerals exposed to gamma radiation.

In this investigation, the Continuous-Wave Optically Stimulated Luminescence (CW-OSL) properties of polyminerals extracted from Mexican and Peruvian Guajillo chilli were studied using a source of cesium-137 (Cs-137) gamma radiation. The Guajillo chilli polyminerals were stimulated with blue light for 120 s, and their luminescence was detected in the UV region. The General Order Kinetics (GOK) deconvolution analysis of the CW-OSL curves was carried out using three individual components. The CW-OSL dose response from 10 to 5000 Gy was analysed in Guajillo chilli polyminerals. After different storage periods, the polyminerals show an increase in the CW-OSL intensity. A strong and moderate effect of the sunlight (60 min) and artificial (6 h) light is observed on the CW-OSL response. Therefore, the CW-OSL properties of polyminerals could be used in the identification of Mexican and Peruvian Guajillo chilli exposed to Cs-137 gamma radiation.

MCHP (Monte Carlo + Human Phantom): Platform to facilitate teaching nuclear radiation physics.

Some concepts in nuclear radiation physics are abstract and intellectually demanding. In the present paper, an "MCHP platform" (MCHP was an acronym for Monte Carlo simulations + Human Phantoms) was proposed to provide assistance to the students through visualization. The platform involved Monte Carlo simulations of interactions between ionizing radiations and the Oak Ridge National Laboratory (ORNL) adult male human phantom. As an example to demonstrate the benefits of the proposed MCHP platform, the present paper investigated the variation of the absorbed photon dose per photon from a 137Cs source in three selected organs, namely, brain, spine and thyroid of an adult male for concrete and lead shields with varying thicknesses. The results were interesting but not readily comprehensible without direct visualization. Graphical visualization snapshots as well as video clips of real time interactions between the photons and the human phantom were presented for the involved cases, and the results were explained with the help of such snapshots and video clips. It is envisaged that, if the platform is found useful and effective by the readers, the readers can also propose examples to be gradually added onto this platform in future, with the ultimate goal of enhancing students' understanding and learning the concepts in an undergraduate nuclear radiation physics course or a related course.

Radiocaesium accumulation capacity of epiphytic lichens and adjacent barks collected at the perimeter boundary site of the Fukushima Dai-ichi Nuclear Power Station.

We investigated the radiocaesium content of nine epiphytic foliose lichens species and the adjacent barks of Zelkova serrata (Ulmaceae, "Japanese elm") and Cerasus sp. (Rosaceae, "Cherry tree") at the boundary of the Fukushima Dai-ichi Nuclear Power Station six years after the accident in 2011. Caesium-137 activities per unit area (the 137Cs-inventory) were determined to compare radiocaesium retentions of lichens (65 specimens) and barks (44 specimens) under the same growth conditions. The 137Cs-inventory of lichens collected from Zelkova serrata and Cerasus sp. were respectively 7.9- and 3.8-times greater than the adjacent barks. Furthermore, we examined the radiocaesium distribution within these samples using autoradiography and on the surfaces with an electron probe micro analyzer (EPMA). Autoradiographic results showed strong local spotting and heterogeneous distributions of radioactivity in both the lichen and bark samples, although the intensities were lower in the barks. The electron microscopy analysis demonstrated that particulates with similar sizes and compositions were distributed on the surfaces of the samples. We therefore concluded that the lichens and barks could capture fine particles, including radiocaesium particles. In addition, radioactivity was distributed more towards the inwards of the lichen samples than the peripheries. This suggests that lichen can retain 137Cs that is chemically immobilised in particulates intracellularly, unlike bark.

Bomb 137Cs in modern honey reveals a regional soil control on pollutant cycling by plants.

137Cs is a long-lived (30-year radioactive half-life) fission product dispersed globally by mid-20th century atmospheric nuclear weapons testing. Here we show that vegetation thousands of kilometers from testing sites continues to cycle 137Cs because it mimics potassium, and consequently, bees magnify this radionuclide in honey. There were no atmospheric weapons tests in the eastern United States, but most honey here has detectable 137Cs at >0.03 Bq kg-1, and in the southeastern U.S., activities can be >500 times higher. By measuring honey, we show regional patterns in the biogeochemical cycling of 137Cs and conclude that plants and animals receive disproportionally high exposure to ionizing radiation from 137Cs in low potassium soils. In several cases, the presence of 137Cs more than doubled the ionizing radiation from gamma and x-rays in the honey, indicating that despite its radioactive half-life, the environmental legacy of regional 137Cs pollution can persist for more than six decades.

Uncertainties in Radiation Doses for a Case-control Study of Thyroid Cancer among Persons Exposed in Childhood to 131 I from Chernobyl Fallout.

Uncertainties in thyroid doses due to I intake were evaluated for 2,239 subjects in a case-control study of thyroid cancer following exposure to Chernobyl fallout during childhood and adolescence carried out in contaminated regions of Belarus and Russia. Using new methodological developments that became available recently, a Monte Carlo simulation procedure was applied to calculate 1,000 alternative vectors of thyroid doses due to I intake for the study population of 2,239 subjects accounting for sources of shared and unshared errors. An overall arithmetic mean of the stochastic thyroid doses in the study was estimated to be 0.43 Gy and median dose of 0.16 Gy. The arithmetic mean and median of deterministic doses estimated previously for 1,615 of 2,239 study subjects were 0.48 Gy and 0.20 Gy, respectively. The geometric standard deviation of individual stochastic doses varied from 1.59 to 3.61 with an arithmetic mean of 1.94 and a geometric mean of 1.89 over all subjects of the study. These multiple sets of thyroid doses were used to update radiation-related thyroid cancer risks in the study population exposed to I after the Chernobyl accident.

Gamma radiation-induced preparation of chitosan-acrylic acid-1-vinyl-2-vinylpyrrolidone/multiwalled carbon nanotubes composite for removal of 152+154Eu, 60Co and 134Cs radionuclides.

Removal behaviors of 152+154Eu, 60Co, and 134Cs radionuclides onto Chitosan-acrylic acid-1-vinyl-2-vinylpyrrolidone/oxidized multi-walled carbon nanotubes (CTS-AA-VP/o-MWCNTs) composite has been investigated by batch adsorption technique. CTS-AA-VP/o-MWCNTs composite has been synthesized by copolymerization of acrylic acid (AA) and 1-vinyl-2-vinylpyrrolidone (VP) onto the surface of chitosan/oxidized multi-walled carbon nanotubes (CTS/o-MWCNTs) using gamma radiation. SEM, TGA, and FTIR were applied to characterize the morphology, thermal stability, and structure of the composite. The composite shows high removal capacity of 321.77, 369.91, and 456.46 mg/g towards 152+154Eu, 60Co, and 134Cs radionuclides, respectively.

More Efficient Prussian Blue Nanoparticles for an Improved Caesium Decontamination from Aqueous Solutions and Biological Fluids.

Any release of radioactive cesium-137, due to unintentional accidents in nuclear plants, represents a dangerous threat for human health and the environment. Prussian blue has been widely studied and used as an antidote for humans exposed to acute internal contamination by Cs-137, due to its ability to act as a selective adsorption agent and to its negligible toxicity. In the present work, the synthesis protocol has been revisited avoiding the use of organic solvents to obtain Prussian blue nanoparticles with morphological and textural properties, which positively influence its Cs+ binding capacity compared to a commercially available Prussian blue sample. The reduction of the particle size and the increase in the specific surface area and pore volume values compared to the commercial Prussian blue reference led to a more rapid uptake of caesium in simulated enteric fluid solution (+35% after 1 h of contact). Then, after 24 h of contact, both solids were able to remove >98% of the initial Cs+ content. The Prussian blue nanoparticles showed a weak inhibition of the bacterial luminescence in the aqueous phase and no chronic detrimental toxic effects.

Evaluation of a proficiency test of 131I, 134Cs and 137Cs in maize powder.

In 2017, JRC-Geel organised a proficiency test for 120 participants on the massic activity determination of 131I, 134Cs and 137Cs in maize powder. The proficiency test reference material was produced by spiking blank maize powder. The material was characterised for its radioactive content using γ-ray spectrometry. The z scores of the reported massic activity were acceptable in 92% of the results for 131I, and in 94% for both 134Cs and 137Cs. The ζ scores were consistent with the reference value for 66% of the results for 131I, 56% for 134Cs and 68% for 137Cs.

Discovery of Radiocesium-bearing Particles in Masks Worn by Members of the Public in Fukushima in Spring 2013.

To investigate the publics' internal exposure by inhalation of radiocesium from the Fukushima Daiichi nuclear disaster in 2011, we examined the activity of radiocesium and radiocesium-bearing particles adhering to nonwoven fabric masks worn daily by members of the public in spring 2013 and 2014. We found a maximum cumulative Cs activity of 4.58 ± 0.15 Bq in 4 wk of spring 2013, which is 20.8% of the activity measured for the same subject in spring 2012 using the same method. This decrease was faster than the physical decay of radiocesium. Radiocesium was detected in 21 of 722 masks in 2013; three of these included type A radiocesium-bearing particles. The activity ratio of the radiocesium-bearing particles on the mask to the total radiocesium was at most approximately 20%. The two radiocesium sources, radiocesium-bearing particles and fugitive dust, are both insoluble particles. The largest internal dose from inhalation was 7.6 µSv in spring 2013, which is negligible compared to the dose limit recommended for members of the public by the International Commission on Radiological Protection.

Compositional and structural analysis of Fukushima-derived particulates using high-resolution x-ray imaging and synchrotron characterisation techniques.

Both the three-dimensional internal structure and elemental distribution of near-field radioactive fallout particulate material released during the March 2011 accident at the Fukushima Daiichi Nuclear Power Plant is analysed using combined high-resolution laboratory and synchrotron radiation x-ray techniques. Results from this study allow for the proposition of the likely formation mechanism of the particles, as well as the potential risks associated with their existence in the environment, and the likely implications for future planned reactor decommissioning. A suite of particles is analyzed from a locality 2 km from the north-western perimeter of the site - north of the primary contaminant plume in an area formerly attributed to being contaminated by fallout from reactor Unit 1. The particles are shown to exhibit significant structural similarities; being amorphous with a textured exterior, and containing inclusions of contrasting compositions, as well as an extensive internal void volume - bimodal in its size distribution. A heterogeneous distribution of the various elemental constituents is observed inside a representative particle, which also exhibited a Fukushima-derived radiocesium (134Cs, 135Cs and 137Cs) signature with negligible natural Cs. We consider the structure and composition of the particle to suggest it formed from materials associated with the reactor Unit 1 building explosion, with debris fragments embedded into the particles surface. Such a high void ratio, comparable to geological pumice, suggests such material formed during a rapid depressurisation and is potentially susceptible to fragmentation through attrition.

Reactor environment during the Fukushima nuclear accident inferred from radiocaesium-bearing microparticles.

Radiocaesium-bearing microparticles (CsMPs), which are substantially silicate glass, were formed inside the damaged reactor and released to the environment by the Fukushima Dai-ichi Nuclear Power Plant accident in March 2011. The present study reports several valuable findings regarding their composition and structure using advanced microanalytical techniques. X-ray absorption near-edge structure of Fe L3-absorption indicated that the oxidation state of the iron dissolved in the glass matrix of the CsMPs was originally nearly divalent, suggesting that the atmosphere in which the CsMPs were formed during the accident was considerably reductive. Another major finding is that sodium, which has not been recognised as a constituent element of CsMPs thus far, is among the major elements in the glass matrix. The atomic percent of Na is higher than that of other alkali elements such as K and Cs. Furthermore, halite (NaCl) was found as an inclusion inside a CsMP. The existence of Na in CsMPs infers that seawater injected for cooling might reach the inside of the reactor before or during the formation of the CsMPs. These results are valuable to infer the environment inside the reactor during the accident and the debris materials to be removed during the decommissioning processes.

Engineered proteoliposome transporter for treatment of cesium contaminated water.

Radioactive cesium (137Cs) released from nuclear power plants and nuclear accidents continues to be a worldwide concern, and its removal from water remains a difficult problem. Here, we present the development of an innovative method to remove Cs+ present at low concentrations in water. To achieve this, a proteoliposome transporter was engineered, composed of a membrane-bound potassium uptake protein, Kup from E. coli, which was reconstituted into a liposome vesicle. Cs+ removal (10-100 µg/L) was demonstrated by incubating the constructed proteoliposome in lab-fortified water, followed by ultracentrifugation to remove captured Cs+. Inductively coupled plasma mass spectrometry (ICP-MS) results from testing water spiked with 100 µg/L Cs+ revealed that adding increasing volumes of proteoliposome solution (containing 0.015-1.2 mg of Kup membrane transporter) resulted in 0.29-12.7% removal in a linear fashion. Proteoliposome addition (containing 0.015-0.3 mg of Kup membrane transporter) to water spiked with 10 µg/L Cs+ resulted in 0.65-3.43% removal, while removal by protein-free liposomes was negligible at 0.03%. These results suggest that Kup transporters inserted into the liposomes are mainly responsible for the removal efficiencies. Consequently, a desired removal efficiency can be achieved by adding a higher volume of constructed proteoliposome and subsequently higher mg of Kup transporter to the contaminated water. This provides new insight on the effectiveness and applicability of proteoliposome transporters, and an alternative and a novel contribution to emerging technologies in removing cesium or other metal contaminants undergoing transmembrane transport.

In vivo removal of radioactive cesium compound using Prussian blue-deposited iron oxide nanoparticles.

Aim: To mitigate the side effects of medical treatment by Prussian blue (PB), a well-known adsorbent for radioactive cesium (Cs), PB-deposited magnetic nanoparticles (MNPs), were prepared and analyzed on the adsorbent capacity for Cs removal. Materials & methods: The PB-deposited MNPs were prepared by photo-deposition method and investigated for their Cs adsorption properties in vitro and in vivo. The distribution of the adsorbents was also evaluated in C57BL/6 mice. Results: PB-deposited MNPs provided an improved adsorbent capacity for Cs removal and reduced toxicity to blood cells compared with those of bulk PB. Conclusion: PB-deposited MNPs could be considered as an alternative of PB-based medicine to reduce the possible hazards caused by high dose of PB intake.

Assessment of radionuclide transfer factors and transfer coefficients near phosphate industrial areas of South Tunisia.

The activity concentrations of naturally occurring and anthropogenic radionuclides in agriculture soils as well as in several food products at four locations within the phosphate area of South Tunisia were investigated. Soil-to-plant transfer factors as well as feed-to-animal products transfer coefficients were determined for the first time for the region. Activity concentrations of 40K, 210Pb, 226Ra, 228Ra and 137Cs in soils of agriculture fields were lower than worldwide average values. The soil-to-plant transfer factors (TFs) for 40K in leafy vegetables were higher than those in fruit vegetables. Soil-to-grass transfer factor (Fv) values were in the following order: 40K > 210Pb > 226Ra. The grass-to-milk transfer coefficient (Fm) values for 40K and 210Pb ranged between 2 × 10-3 and 4 × 10-3(day L-1). The concentration ratios for the animal products (CRmilk-feed, CRmeat-feed and CRegg-feed) varied in the ranges of 2 × 10-2-4 × 10-2 L kg-1, 1 × 10-2-2 × 10-1 (L kg-1) and 5 × 10-2-1 (L kg-1)for 40K, 210Pb and 226Ra, respectively. Transfer parameters determined in the present study were compared with those reported in International Atomic Energy Agency reports and other published values. The absorbed gamma dose rate in air and the external hazard index associated with these natural radionuclides were computed to assess the radiation hazard of radioactivity in this region, and the results indicated that these areas are within set safety limits.

Nano-sized Prussian blue immobilized costless agro-industrial waste for the removal of cesium-137 ions.

For human health and safety, it is of great importance to develop innovative materials with a vast capacity for powerful removal of radioactive ions from aqueous solutions. Prussian blue functionalized sugarcane bagasse (PB-SCB) was successfully prepared for the efficient elimination of radioactive cesium (137Cs) using a nontoxic, environmentally friendly, and costless method. The prepared renewable material was characterized using different techniques to emphasize morphology, functional groups, crystal structure, and the adsorption process. The adsorption of Cs(I) was better fitted to the pseudo-second-order model than pseudo-first-order model which revealed a chemical adsorption mechanism. The experimental isotherm results were best illustrated by the Freundlich model (R2 = 0.98). Besides, the obtained values for the thermodynamic parameters indicating that the adsorption process was endothermic and spontaneous in nature. In addition to demonstrating high adsorption capacity for Cs ion removal (56.7 mg/g at 30 °C), PB-SCB might consider being an efficient and cost-effective adsorbent for the decontamination of cesium, where an estimated cost analysis revealed that the expenditure for the removal of 1000 mg/L cesium from alkaline radioactive wastewater is likely to be US$0.12. Graphical abstract.

Accumulation of natural and anthropogenic radionuclides in body profiles of Bryidae, a subgroup of mosses.

Mosses can be used as biomonitors to monitor radionuclide deposition and heavy metal pollution in cities, forests, and grasslands. The aims of this work were to determine the activity concentrations of natural (210Po, 210Pb or 210Pbex (excess 210Pb is defined as the activity of 210Pb minus the activity of 226Ra), 7Be, 40K, 226Ra, 238U, and 232Th) and anthropogenic radionuclides (137Cs) in moss body profiles and in situ underlying soils of moss samples and to assess/determine the distribution features and accumulation of these radionuclides. Activity concentrations of radionuclides in the samples were measured using a low-background gamma spectrometer and a low-background alpha spectrometer. Consistent with their source, the studied radionuclides in the moss samples and underlying soils were divided according to the principal component analysis (PCA) results into an airborne group (210Po, 210Pb (210Pbex), 7Be, and 137Cs) and a terrestrial group (40K, 238U, 226Ra, and 232Th). The activity concentrations of 210Po and 210Pbex in moss body profiles were mainly concentrated in the stems-rhizoid parts, in which we measured some of the highest 210Po and 210Pbex levels compared to the results in the literature. 7Be mainly accumulated in the leaves-stem parts. Different positive correlations were observed between 210Po and 210Pb and between 7Be and 210Pb, which indicated that the uptake mechanisms of 210Po, 210Pb, and 7Be by moss plants were different, to some extent. 137Cs was detected only in some moss samples, and the fraction of 137Cs in the underlying soils was much lower than that in the moss, suggesting that mosses were protecting the underlying soils from further pollution. Except for 40K, the terrestrial radionuclide (238U, 226Ra, and 232Th) content in mosses was predominantly at low levels, which indicated not only the inability of mosses to use those elements for metabolic purposes but also the rather poor capability of mosses to directly mobilize, absorb, and transport elements (U, Ra, or Th) not dissolved in water.

An EXAFS study for characterizing the time-dependent adsorption of cesium on bentonite.

Bentonite is considered for use as a buffer material in the final disposal repositories of radioactive waste. Long-lived 135Cs with a half-life of 2.3 × 106 years is a key radionuclide in high-level waste, and lots of 137Cs with a half-life of 30.2 years exists in low-level waste. Therefore, the adsorption of Cs on bentonite is a critical issue in evaluating the long-term safety of radioactive waste disposal. In this study, EXAFS techniques were used to characterize the time-dependent process from the beginning of adsorption to equilibrium. From the results of this study, we found changes including to the Cs adsorption sites, the Cs-O distance between Cs and the oxygen atom, and that the adsorption of Cs ions occurred before the reaction reached equilibrium. The fraction of OS complexes when Cs was adsorbed on bentonite can refer to the CN (Cs-O1st)/CN (Cs-O2nd) ratio of coordination numbers, and this study found that the OS complex was the major adsorption species when Cs adsorbed onto bentonite. In addition to the ratio CN (Cs-O1st)/CN (Cs-O2nd) providing information on the adsorption site, we also discussed the change of Cs-O1st and Cs-O2nd bond distances to identify the adsorption sites at different times. Comparing the XRD patterns of montmorillonite and bentonite, we found that the interlayer collapsed after Cs was adsorbed onto montmorillonite, but it expanded after Cs was adsorbed onto bentonite. From the results of EXAFS fitting, we found that the movement of Cs ions was from regular interlayer sites to expanded interlayer sites, which caused the interatomic distance of Cs-O2nd to decrease with an increase in time. It was revealed that the adsorption of Cs on bentonite occurred in two steps. The first step includes the rapid uptake of Cs by attachment to the oxygen atoms of the H2O molecules at the regular interlayer sites, especially for the OS complexes. The second step includes a slower process where dehydrated Cs ions move from the regular interlayer sites to the expanded interlayer sites. In this study, Cs L3-edge EXAFS spectroscopy was conducted for the Cs adsorbed on bentonite to identify the Cs adsorption sites over time, as this is important in evaluating the mobility of Cs in the environment. These results are beneficial in finding the process of Cs adsorption on bentonite, which could be used for the design of the final disposal of spent nuclear fuel.

A new perspective on the 137Cs retention mechanism in surface soils during the early stage after the Fukushima nuclear accident.

The Fukushima Daiichi nuclear power plant accident caused serious radiocesium (137Cs) contamination of the soil in multiple terrestrial ecosystems. Soil is a complex system where minerals, organic matter, and microorganisms interact with each other; therefore, an improved understanding of the interactions of 137Cs with these soil constituents is key to accurately assessing the environmental consequences of the accident. Soil samples were collected from field, orchard, and forest sites in July 2011, separated into three soil fractions with different mineral-organic interaction characteristics using a density fractionation method, and then analyzed for 137Cs content, mineral composition, and organic matter content. The results show that 20-71% of the 137Cs was retained in association with relatively mineral-free, particulate organic matter (POM)-dominant fractions in the orchard and forest surface soil layers. Given the physicochemical and mineralogical properties and the 137Cs extractability of the soils, 137Cs incorporation into the complex structure of POM is likely the main mechanism for 137Cs retention in the surface soil layers. Therefore, our results suggest that a significant fraction of 137Cs is not immediately immobilized by clay minerals and remains potentially mobile and bioavailable in surface layers of organic-rich soils.