Cs, Pu concentrations and the Pu/Pu atom ratio in a sediment core from the sub-aqueous delta of Yangtze River estuary

A sediment core collected from the sub-aqueous delta of the Yangtze River estuary was subjected to analyses of ¹³⁷Cs and plutonium (Pu) isotopes. The ¹³⁷Cs was measured using γ-spectrometry at the laboratories at the Nanjing University and Pu isotopes were determined with Accelerator Mass Spectrometry (AMS), measurements made at the Australian National University. The results show considerable structure in the depth concentration profiles of the ¹³⁷Cs and ^239+240Pu. The shape of the vertical ¹³⁷Cs distribution in the sediment core was similar to that of the Pu. The maximum ¹³⁷Cs and ^239+240Pu concentrations were 16.21 ± 0.95 mBq/g and 0.716 ± 0.030 mBq/g, respectively, and appear at same depth. The average ²⁴⁰Pu/²³⁹Pu atom ratio was 0.238 ± 0.007 in the sediment core, slightly higher than the average global fallout value. The changes in the ²⁴⁰Pu/²³⁹Pu atom ratios in the sediment core indicate the presence of at least two different Pu sources, i.e., global fallout and another source, most likely close-in fallout from the Pacific Proving Grounds (PPG) in the Marshall Islands, and suggest the possibility that Pu isotopes are useful as a geochronological tool for coastal sediment studies. The ¹³⁷Cs and ^239+240Pu inventories were estimated to be 7100 ± 1200 Bq/m² and 407 ± 27 Bq/m², respectively. Approximately 40% of the ^239+240Pu inventory originated from the PPG close-in fallout and about 50% has derived from land-origin global fallout transported to the estuary by the river. This study confirms that AMS is a useful tool to measure ²⁴⁰Pu/²³⁹Pu atom ratio and can provide valuable information on sedimentary processes in the coastal environment.     

Geochronology of anthropogenic radionuclides in Ribeira Bay sediments, Rio de Janeiro, Brazil

Ribeira Bay is located approximately 130 km south of the city of Rio de Janeiro and receives discharges of liquid effluent from the Angra dos Reis nuclear power plant (NPP) site, where two pressurized water reactors are located. To test whether the presence of anthropogenic radionuclides in sediments in Ribeira Bay could be correlated to the NPP operations, we sampled seven sediment cores and determined accumulation rates and chronologies. Only one sediment core did not exhibit a superficial mixing layer; this sample was used for dating purposes. Cesium-137 and ²⁰⁷Bi were observed in this sediment profile, but their presence was associated with atmospheric fall-out rather than the nearby NPP. The exponential decay of ²¹⁰Pb concentration with sediment layer depth was verified below a superficial mixing layer for all other sediment cores. Calculated accumulation rates ranged from 1.2 mm y⁻¹ in the inner bay to 6.2 mm y⁻¹ close to its entrance.     

Behavior and analysis of Cesium adsorption on montmorillonite mineral

The adsorption of Cs by montmorillonite and the effects of experimental conditions on adsorption were investigated by using ¹³⁴Cs as a radioactive tracer. Additionally, the Cs-adsorbed and the modified montmorillonite were analyzed by X-ray Diffractometer System (XRD) and Scanning Electron Microscopy (SEM). The results showed that the adsorption of Cs by montmorillonite was efficient in the initial concentration (C₀) of 30 μg/L Cs nitrate solution with 20 g/L montmorillonite at room temperature. In this condition, more than 98% Cs⁺ ions could be adsorbed at pH 8. The adsorption equilibrium was achieved within 5 min and the relationship between the concentration of Cs⁺ in aqueous solutions and adsorption capacities of Cs⁺ can be described by the Langmuir adsorption isotherm. The adsorption rate would decrease when temperature increase from 0 °C to 50 °C or in presence of coexistent K⁺, Na⁺ and Ca²⁺, while modification by (NH₄)₂SO₄, [Ag(NH₃)₂]⁺, [Cu(NH₃)₄]²⁺ or 450 °C could improve the adsorption abilities of montmorillonite for Cs⁺. However, more than 89% of adsorbed Cs⁺ on montmorillonite could be desorbed by 2 mol/L HNO₃ solutions. The XRD and SEM analysis further showed that the structure of the Cs-adsorbed or modified montmorillonite were different from that of the original one.     

Medical radioisotopes in the environment – following the pathway from patient to river sediment

Motivated by the detection of ¹³¹I in river sediment in routine long-term surveillance samples, a systematic short-term study of the wastewater treatment chain was planned and conducted. Inflow, effluent and primary sludge were collected on a daily basis during two weeks at a regional wastewater treatment plant. Samples were investigated by gamma spectroscopy. Four medically used isotopes could be identified (¹³¹I and ^99mTc regularly, ¹⁵³Sm and ¹²³I sporadically). The concentration levels coincide well with literature data for ¹³¹I, and with our own long-term data for ¹³¹I and ^99mTc for the same plant. Cosmogenic ⁷Be activity in primary sludge correlated well with rainfall intensity. Surface sediment was sampled at low tide at both shores of the river, up- and downstream of the plant. ¹³¹I was identified in all samples, with a sharp maximum (about 100 Bq kg⁻¹ d.m.) at the discharge point of the plant and lower levels elsewhere, decreasing monotonically in downstream direction. ⁷Be and ¹³⁷Cs showed the same behaviour, but no peak at the discharge point. Predictions from simple equilibrium models for the transport and sedimentation of ¹³¹I show good agreement with the experimental data and suggest that the wastewater treatment plant is the main source for this isotope.     

Effect of liming on the behaviour of (90)Sr and (137)Cs in a lake ecosystem

Liming of lakes is considered one possible remedial action to reduce the accumulation of radionuclides into fish in the case of a radiological accident. These responses were tested in field conditions in a small acidified lake that was divided into two parts: one limed with CaCO₃ and the other half left as an unlimed control. The transfer of ⁹⁰Sr from water into fish decreased on average by 50% during the first year after liming. However, at the same time the ⁹⁰Sr concentration in water increased, reaching a maximum within 6 months after liming. Approximately 50% more ⁹⁰Sr was detected in water in the limed part of the lake than on control side during the first year. ⁹⁰Sr was most probably released from the sediment as the Ca concentration and pH of the water increased. As a result of these two processes, which counterbalanced each other (increased release of ⁹⁰Sr into water from sediment and decreased transfer of ⁹⁰Sr from water into fish), the ⁹⁰Sr concentration in fish did not notably differ between the limed and control sides of the lake. Liming may only be suitable as a remedial action if carried out immediately after a radiological accident, before significant amounts of radionuclides have been deposited in lake sediments. In the case of ¹³⁷Cs, the effect of liming was less pronounced. ¹³⁷Cs activity concentration in water increased in the first year by 20% and uptake by fish decreased by 20%.     

Intake of ²³⁸U and ²³²Th through the consumption of foodstuffs by tribal populations practicing slash and burn agriculture in an extremely high rainfall area

The concentration of naturally occurring radionuclides ²³²Th, ²³⁸U was determined using Instrumental Neutron Activation Analysis (INAA) in different food groups namely cereals, vegetables, leafy vegetables, roots and tubers cultivated and consumed by tribal population residing around the proposed uranium mine. The study area is a part of rural area K. P. Mawthabah (Domiasiat) in the west Khasi Hills District of Meghalaya, India located in the tropical region of high rainfall that remains steeped in tribal tradition without much outside influence. Agriculture by Jhum (slash and burn) cultivation and animal husbandry are the main occupation of the tribal populations. A total of 89 samples from locally grown food products were analyzed. The concentration of ²³⁸U and ²³²Th in the soil of the study area was found to vary 1.6-15.5 and 2.0-5.0 times respectively to the average mean value observed in India. The estimated daily dietary intake of ²³⁸U and ²³²Th were 2.0 μg d⁻¹ (25 mBq d⁻¹) and 3.4 μg d⁻¹ (14 mBq d⁻¹) is comparable with reported range 0.5-5.0 μg d⁻¹ and 0.15-3.5 μg d⁻¹ respectively for the Asian population.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

Antlers of Cervus elaphus as biomonitors of ⁹⁰Sr in the environment

Adequate radioprotection of the environment requires the identification of biomonitors sensitive to the variation of its radionuclide content. Due to the chemical similarities between calcium and strontium, calcified tissues of mammals are considered to be good ⁹⁰Sr biomonitors. This work considered Cervus elaphus antlers which, being shed annually, can give information about the importance of radiostrontium contamination in an ecosystem in the time period required for the growth of the antler. The samples were collected at various points of W and SW Spain. The mean value of their ⁹⁰Sr content was (70 ± 43 (S.D.)) Bq/kg d.w., range (16-218) Bq/kg d.w., and the radionuclide was evenly distributed in the different parts of the antler. There was a good correlation between the antlers’ ⁹⁰Sr content and the ⁹⁰Sr deposited in the soil. The antlers’ content of ²²⁶Ra (from the natural uranium series) and the contents of some stable elements (Ca, Mg, Sr, and K) were also determined. The values for these stable elements were practically constant in the analyzed samples, and the concentrations measured decreased in the following order:Ca » Mg > K > Sr » ⁹⁰Sr > ²²⁶Ra     

Recent Cs deposition in sediments of Admiralty Bay, Antarctica

Cesium-137, radium-226 and lead-210 profiles of a 25 cm sediment core give an indication of recent changes in land-ocean interactions at a polar coastal environment (Admiralty Bay, King George Island, Antarctica). The linear sedimentation accumulation rate at the study site calculated from the unsupported ²¹⁰Pb profile was 6.7 mm/year from 1965 to 2005. A 3.5-fold increase in ¹³⁷Cs concentrations was observed in the top layer of this sediment core. This sharp increase seems to indicate a recent redistribution of fallout radionuclides previously deposited on soil, vegetation and snow. These results imply enhanced land-ocean interactions at this site likely as a result of climate change. Because our results are based on a single core, additional investigations are needed to confirm our observations.     

Determination of U, Pu and Am isotopes in Irish Sea sediment by a combination of AMS and radiometric methods

Samples from a marine sediment core from the Irish Sea (54.416 N, 3.563 W) were analyzed for the isotopic composition of uranium, plutonium and americium by a combination of radiometric methods and AMS. The radiochemical procedure consisted of a Pu separation step by anion exchange, subsequent U separation by extraction chromatography using UTEVA^® and finally Am separation with TRU^® Resin.Additionally to radiometric determination of these isotopes by alpha spectrometry, the separated samples were also used for the determination of ²³⁶U/²³⁸U and plutonium isotope ratios by Accelerator Mass Spectrometry (AMS) at the VERA facility.     

Modelling the reworking effects of bioturbation on the incorporation of radionuclides into the sediment column: implications for the fate of particle-reactive radionuclides in Irish Sea sediments

A microcosm laboratory experiment was conducted to determine the impact of biological reworking by the ragworm Nereis diversicolor on the redistribution of particle-bound radionuclides deposited at the sediment-water interface. Over the course of the 40-day experiment, as much as 35% of a ¹³⁷Cs-labelled particulate tracer deposited on the sediment surface was redistributed to depths of up to 11 cm by the polychaete. Three different reworking models were employed to model the profiles and quantify the biodiffusion and biotransport coefficients: a gallery-diffuser model, a continuous sub-surface egestion model and a biodiffusion model. Although the biodiffusion coefficients obtained for each model were quite similar, the continuous sub-surface egestion model provided the best fit to the data. The average biodiffusion coefficient, at 1.8 ± 0.9 cm² y⁻¹, is in good agreement with the values quoted by other workers on the bioturbation effects of this polychaete species. The corresponding value for the biotransport coefficient was found to be 0.9 ± 0.4 cm y⁻¹. The effects of non-local mixing were incorporated in a model to describe the temporal evolution of measured ⁹⁹Tc and ⁶⁰Co radionuclide sediment profiles in the eastern Irish Sea, influenced by radioactive waste discharged from the Sellafield reprocessing plant. Reworking conditions in the sediment column were simulated by considering an upper mixed layer, an exponentially decreasing diffusion coefficient, and appropriate biotransport coefficients to account for non-local mixing. The diffusion coefficients calculated from the ⁹⁹Tc and ⁶⁰Co cores were in the range 2-14 cm² y⁻¹, which are consistent with the values found by other workers in the same marine area, while the biotransport coefficients were similar to those obtained for a variety of macrobenthic organisms in controlled laboratories and field studies.     

Fate of Co at a sludge land application site

Vertical distributions of ⁶⁰Co are determined in soil cores obtained from a 10-ha grassland, where anaerobically digested sludge was applied by surface spraying from 1986 to 1995 on the U.S. Department of Energy's Oak Ridge Reservation. These results, along with historical application records, are used to estimate vertical-migration rates and perform a mass balance. The presence of ⁶⁰Co results solely from the sludge-application process. Soil, vegetation, and surface-water samples were collected. Eleven soil cores were sectioned into 3-cm increments and analyzed by gamma-ray spectrometry. No ⁶⁰Co was detected in the vegetation or water samples. The downward migration rate of ⁶⁰Co in the upper 15 cm of soil ranged from 0.50 to 0.73 cm/yr. About 98%, 0.020 ± 0.011 Bq/cm², of ⁶⁰Co remained in the upper 15 cm of soil, which compared favorably with the expected ⁶⁰Co activity based on historical records of 0.019 ± 0.010 Bq/cm².     

Transfer of Sr into fish in Finnish lakes

The long-term behavior of ⁹⁰Sr was investigated from 1987 to 1997 in fifteen lakes in southern and central Finland following the 1986 Chernobyl accident. Both water and fish samples (perch, pike, vendace) were analyzed. ⁹⁰Sr stays long in the freshwater ecosystem; the observed half-lives during the study period were generally around 10 years in water and even longer in fish. One lake exhibited very different behavior for ⁹⁰Sr, with elevated levels in fish and water and very short observed half-life in fish, less than 2 years. Concentration factors of ⁹⁰Sr in fish (Bqkg⁻¹ f.w. in fish/Bqkg⁻¹ in water) among the studied lakes significantly correlated with both the Ca concentration and electrical conductivity of the water. More ⁹⁰Sr was transferred into fish in lakes with a low electrical conductivity and a low Ca concentration. Among other water parameters evaluated were pH, color, total nitrogen, and phosphorus.     

Bioaccumulation of Ra by plants growing in fresh water ecosystem around the uranium industry at Jaduguda, India

A field study has been conducted to evaluate the ²²⁶Ra bioaccumulation among aquatic plants growing in the stream/river adjoining the uranium mining and ore-processing complex at Jaduguda, India. Two types of plant group have been investigated namely free floating algal species submerged into water and plants rooted in stream & riverbed. The highest ²²⁶Ra activity concentration (9850 Bq kg⁻¹) was found in filamentous algae growing in the residual water of tailings pond. The concentration ratios of ²²⁶Ra in filamentous algae (activity concentration of ²²⁶Ra in plant Bq kg⁻¹ fresh weight/activity concentration of ²²⁶Ra in water Bq l⁻¹) widely varied i.e. from 1.1 × 10³ to 8.6 × 10⁴. Other aquatic plants were also showing wide variability in the ²²⁶Ra activity concentration. The ln-transformed filamentous algae ²²⁶Ra activity concentration was significantly correlated with that of ln-transformed water concentration (r = 0.89, p < 0.001). There was no correlation between the activity concentrations of ²²⁶Ra in stream/riverbed rooted plants and the substrate. For this group, correlation between ²²⁶Ra activity concentration and Mn, Fe, Cu concentration in plants were statistically significant.     

External gamma-ray dose rate and radon concentration in indoor environments covered with Brazilian granites

Health hazard from natural radioactivity in Brazilian granites, covering the walls and floor in a typical dwelling room, was assessed by indirect methods to predict external gamma-ray dose rates and radon concentrations. The gamma-ray dose rate was estimated by a Monte Carlo simulation method and validated by in-situ measurements with a NaI spectrometer. Activity concentrations of ²³²Th, ²²⁶Ra, and ⁴⁰K in an extensive selection of Brazilian commercial granite samples measured by using gamma-ray spectrometry were found to be 4.5-450 Bq kg⁻¹, 4.9-160 Bq kg⁻¹ and 190-2029 Bq kg⁻¹, respectively. The maximum external gamma-ray dose rate from floor and walls covered with the Brazilian granites in the typical dwelling room (5.0 m × 4.0 m area, 2.8 m height) was found to be 120 nGy h⁻¹, which is comparable with the average worldwide exposure to external terrestrial radiation of 80 nGy h⁻¹ due to natural sources, proposed by United Nations Scientific Committee on the Effects of Atomic Radiation. Radon concentrations in the room were also estimated by a simple mass balance equation and exhalation rates calculated from the measured values of ²²⁶Ra concentrations and the material properties. The results showed that the radon concentration in the room ventilated adequately (0.5 h⁻¹) will be lower than 100 Bq m⁻³, value recommended as a reference level by the World Health Organization.     

Cs and K in fruiting bodies of different fungal species collected in a single forest in southern Poland

Fruiting bodies of fungi belonging to more than 70 species were collected within a few thousand square meter area of one forest during 2006 and 2007. The soil profile was collected to check the cumulative deposition of ¹³⁷Cs, which was relatively high, equal to 64 ± 2 kBq/m² (calculated for October 2006). The majority of this activity was in the first 6 cm. Fruitbodies were analyzed for radiocesium and ⁴⁰K by means of gamma-spectrometry. The highest ¹³⁷Cs activity was 54.1 ± 0.7 kBq/kg (dry weight) for a sample of Lactarius helvus collected in 2006. The results for 2006 were higher than those for 2007. In a few cases the traces of short-lived (T_1/2 = 2.06 a) ¹³⁴Cs were still found in samples. The importance of mycorrhizal fungi for radiocesium accumulation is confirmed. The differences in activity among the species are discussed in relation to observations and predictions from previous studies, where the change in relative accumulation between fruiting bodies of different species was at least partially explained by the differences in the depth of the mycelium localization in a litter/soil system. It is concluded that in some cases, such as Boletus edulis and Xerocomus badius, this prediction is fulfilled and therefore this explanation confirmed.     

Fuel particles in the Chernobyl cooling pond: current state and prediction for remediation options

During the coming years, a management and remediation strategy for the Chernobyl cooling pond (CP) will be implemented. Remediation options include a controlled reduction in surface water level of the cooling pond and stabilisation of exposed sediments. In terrestrial soils, fuel particles deposited during the Chernobyl accident have now almost completely disintegrated. However, in the CP sediments the majority of ⁹⁰Sr activity is still in the form of fuel particles. Due to the low dissolved oxygen concentration and high pH, dissolution of fuel particles in the CP sediments is significantly slower than in soils. After the planned cessation of water pumping from the Pripyat River to the Pond, significant areas of sediments will be drained and exposed to the air. This will significantly enhance the dissolution rate and, correspondingly, the mobility and bioavailability of radionuclides will increase with time. The rate of acidification of exposed bottom sediments was predicted on the basis of acidification of similar soils after liming. Using empirical equations relating the fuel particle dissolution rate to soil and sediment pH allowed prediction of fuel particle dissolution and ⁹⁰Sr mobilisation for different remediation scenarios. It is shown that in exposed sediments, fuel particles will be almost completely dissolved in 15–25 years, while in parts of the cooling pond which remain flooded, fuel particle dissolution will take about a century.     

Plutonium isotopes concentration in seawater and bottom sediment off the Pacific coast of Aomori sea area during 1991-2005

A radioactivity survey was launched in 1991 to determine the background levels of ^239+240Pu in the marine environment off a commercial spent nuclear fuel reprocessing plant before full operation of the facility. Particular attention was focused on the ²⁴⁰Pu/²³⁹Pu atom ratio in seawater and bottom sediment to identify the origins of Pu isotopes. The concentration of ^239+240Pu was almost uniform in surface water, decreasing slowly over time. Conversely, the ^239+240Pu concentration varied markedly in the bottom water and was dependent upon the sampling point, with higher concentrations of ^239+240Pu observed in the bottom water sample at sampling points having greater depth. The ²⁴⁰Pu/²³⁹Pu atom ratio in the seawater and sediment samples was higher than that of global fallout Pu, and comparable with the data in the other sea area around Japan which has likely been affected by close-in fallout Pu originating from the Pacific Proving Grounds. The ²⁴⁰Pu/²³⁹Pu atom ratio in bottom sediment samples decreased with sea depth. The land-originated Pu is not considered as the reason of the increasing ^239+240Pu concentration and also decreasing the ²⁴⁰Pu/²³⁹Pu atom ratio with sea depth, and further study is required to clarify it.     

Vertical distributions of (99)Tc and the (99)Tc/(137)Cs activity ratio in the coastal water off Aomori, Japan

Using a sector-field ICP-MS the vertical distributions of the ⁹⁹Tc concentration and ⁹⁹Tc/¹³⁷Cs activity ratio were measured in the coastal waters off Aomori Prefecture, Japan, where a spent-nuclear-fuel reprocessing plant has begun test operation. The ⁹⁹Tc concentrations in surface water ranged from 1.8 to 2.4 mBq/m³, no greater than the estimated background level. Relatively high ⁹⁹Tc/¹³⁷Cs activity ratios (10-12 × 10⁻⁴) would be caused by the inflow of the high-⁹⁹Tc/¹³⁷Cs water mass from the Japan Sea. There is no observable contamination from the reprocessing plant in the investigated area. The ⁹⁹Tc concentration and the ⁹⁹Tc/¹³⁷Cs activity ratio in water column showed gradual decreases with depth. Our results implied that ⁹⁹Tc behaves in a more conservative manner than ¹³⁷Cs in marine environments.     

Pre-concentration of naturally occurring radionuclides and the determination of (212)Pb from fresh waters

A novel technique has been developed for determining the ²¹²Pb activity of fresh waters. This is of interest to environmental monitoring programmes that utilise gross α-activity methods to screen for anthropogenic radionuclides. The contribution from ²¹²Pb varies, and is difficult to experimentally measure due to its relatively short half-life (t_½ = 10.6 h) and low environmental activity (<0.1 Bq l⁻¹). The use of a three-stage technique that encompasses a unique form of pre-concentration, separation and analysis by liquid scintillation counting allows a lower detection limit of 0.006 Bq l⁻¹ with a chemical yield of 92.5 ± 5.6%. The measurement can be obtained within 7 h of sample collection, and is calculated using the radioactive decay of ²¹²Bi. Other naturally occurring radionuclides may also be extracted using the pre-concentration stage of the technique, with efficiencies above 90% at a range of pH values.