Radium geochemistry in Na-Cl type groundwater in Niigata Prefecture, Japan

Radium isotopes in 23 Na-Cl type groundwater sampled mainly from deep wells in Niigata Prefecture, which is the site of the largest oil- and gas-fields in Japan, were measured along with U isotopes, chemical components and hydrogen and oxygen isotope ratios to elucidate the distribution and behavior of Ra in a brackish environment underground. Also analyzed were U and Th isotopes in 38 rock samples collected from outcrops at 17 locations. Ra-226 concentrations (8.86-1637 mBq kg⁻¹) of groundwater samples roughly correlated with total dissolved solid (TDS) concentrations and other alkaline earth contents. Their ²²⁸Ra/²²⁶Ra activity ratios (0.32-5.2) were similar to or higher than the ²³²Th/²³⁸U activity ratios (0.6-1.7) in the rocks. The most likely transport mechanism of Ra isotopes into groundwater was due to their α-recoil from the solid phase, probably from the water-rock interface where Th isotopes had accumulated, and adsorption/desorption reaction based on the increase in ²²⁶Ra contents with TDS.     

Distribution of uranium isotopes in surface water of the Llobregat river basin (Northeast Spain)

A study is presented on the distribution of ²³⁴U, ²³⁸U, ²³⁵U isotopes in surface water of the Llobregat river basin (Northeast Spain), from 2001 to 2006. Sixty-six superficial water samples were collected at 16 points distributed throughout the Llobregat river basin. Uranium isotopes were measured by alpha spectrometry (PIPS detectors). The test procedure was validated according to the quality requirements of the ISO17025 standard. The activity concentration for the total dissolved uranium ranges from 20 to 261 mBq L⁻¹. The highest concentrations of uranium were detected in an area with formations of sedimentary rock, limestone and lignite. A high degree of radioactive disequilibrium was noted among the uranium isotopes. The ²³⁴U/²³⁸U activity ratio varied between 1.1 and 1.9 and the waters with the lowest uranium activity registered the highest level of ²³⁴U/²³⁸U activity ratio. Correlations between uranium activity in the tested water and chemical and physical characteristics of the aquifer were found.     

Uranium isotopes in Tunisian bottled mineral waters

²³⁴U and ²³⁸U activity concentrations and their relative effective doses have been determined in 10 bottled mineral waters in Tunisia. Alpha spectrometry was used as technique to measure uranium isotopes. The obtained isotopic ratio ²³⁴U/²³⁸U varies between 1.1 and 3 which means that the two isotopes are not in radioactive equilibrium. Measured activity concentration varies between 3.2 and 40 mBq/l for ²³⁴U and between 1.5 and 26.3 mBq/l for ²³⁸U. Effective doses (assuming 2 litres per day of water consumption) coming from this two isotopes are found to vary between 0.16 and 2.02 μSv/a which is lower than the maximum recommended dose level by the WHO.     

Dynamic model for radionuclide uptake in lichen

Samples of atmospheric particulate material and terrestrial plants, including lichens, were collected in New Brunswick, Canada between 1980 and 1983 and analyzed for a wide range of artificial and naturally-occuring radionuclides, including fission products (¹⁴¹Ce, ¹⁴⁴Ce, ¹⁰³Ru, ¹⁰⁶Ru, ⁹⁵Zr and ¹³⁷Cs) derived from the 16 October 1980 Chinese nuclear test. Activity ratios of some of the short-lived fission products in air particulates and lichens are in reasonable agreement with those predicted from fission product yields for nuclear weapons tests, indicating that only minor fractionation occurred for these radionuclides during their transport through air particulate and lichen environmental phases. The ⁷Be inventories measured in a suite of lichen (Cladonia rangiferina) samples were used to calibrate each lichen plant for its collection efficiency for atmospheric particulates and fallout radioactivity.A lichen model has been developed to predict lichen inventories of radioactivity for different lichen growth functions and bio-elimination rates. Assuming that lichen growth results in a linear increase in surface area with time, the experimental results yield biological residence times of 1–2 years for ²¹⁰Pb and Pu and 5–8 years for ¹³⁷Cs. The more efficient retention of ¹³⁷Cs is probably due to its physiological uptake in lichen plants as a proxy for potassium, as evidenced by an observed, inverse relationship between ¹³⁷Cs and ⁴⁰K activities in lichen.     

Global radioxenon emission inventory based on nuclear power reactor reports

Atmospheric radioactivity is monitored for the verification of the Comprehensive Nuclear-Test-Ban Treaty, with xenon isotopes ^131mXe, ¹³³Xe, ^133mXe and ¹³⁵Xe serving as important indicators of nuclear explosions. The treaty-relevant interpretation of atmospheric concentrations of radioxenon is enhanced by quantifying radioxenon emissions released from civilian facilities. This paper presents the first global radioxenon emission inventory for nuclear power plants, based on North American and European emission reports for the years 1995–2005. Estimations were made for all power plant sites for which emission data were unavailable. According to this inventory, a total of 1.3 PBq of radioxenon isotopes are released by nuclear power plants as continuous or pulsed emissions in a generic year.     

A comparison of the particle track and α-spectrometric techniques in excess thorium-230 dating of Eastern Atlantic pelagic sediments

The particle track analysis and α-spectrometric techniques have been applied to a comparative study of excess ²³⁰Th dating of three deep-sea cores from the Eastern Atlantic. Both methods yield similar sediment accumulation rates. Limitations of the α-track phase of the particle track detection process, arising from the non-specific determination of ²³⁰Th and from the mobility of some alpha-emitting daughters, suggest that details of the sedimentation record may fail to be identified. The conventional radiochemical technique, on the other hand, specifically isolates all the radionuclides of interest but at the expense of a more complex experimental procedure and a longer sample processing time. The combined particle track technique (i.e. α and fission track analyses) therefore seems excellently suited to a complementary role in tandem with the α-spectrometric method of ²³⁰Th dating. Uranium determination by the fission track technique is accurate and rapid, showing good agreement with the α-spectrometric method.     

Measuring the radium quartet (Ra, Ra, Ra, Ra) in seawater samples using gamma spectrometry

Radium isotopes are widely used in marine studies (eg. to trace water masses, to quantify mixing processes or to study submarine groundwater discharge). While ²²⁸Ra and ²²⁶Ra are usually measured using gamma spectrometry, short-lived Ra isotopes (²²⁴Ra and ²²³Ra) are usually measured using a Radium Delayed Coincidence Counter (RaDeCC). Here we show that the four radium isotopes can be analyzed using gamma spectrometry. We report ²²⁶Ra, ²²⁸Ra, ²²⁴Ra, ²²³Ra activities measured using low-background gamma spectrometry in standard samples, in water samples collected in the vicinity of our laboratory (La Palme and Vaccarès lagoons, France) but also in seawater samples collected in the plume of the Amazon river, off French Guyana (AMANDES project). The ²²³Ra and ²²⁴Ra activities determined in these samples using gamma spectrometry were compared to the activities determined using RaDeCC. Activities determined using the two techniques are in good agreement. Uncertainties associated with the ²²⁴Ra activities are similar for the two techniques. RaDeCC is more sensitive for the detection of low ²²³Ra activities. Gamma spectrometry thus constitutes an alternate method for the determination of short-lived Ra isotopes.     

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.     

Thorium isotopes in the surface air of the Western North Pacific Ocean

The concentrations and activity ratios of thorium isotopes in maritime airborne particles, collected over the western North Pacific along 137° E during cruises in January 1982 and 1983 and in March 1983, are reported here. The ²³²Th concentration in air is high at mid-latitude, near the Japanese islands and decreases southwards further from land. The ²³²Th concentration ranges from 0·036 to 0·22 μBq m⁻³. The ²³⁰Th/²³²Th activity ratio in the maritime air is almost unity, reflecting the U/Th activity ratio coupled with the crustal abundance. The ²²⁸Th/²³²Th activity ratio ranges from 3 to 69·5 and is, in general, higher than that in air over land. The results indicate the importance of the aeolian flux of the thorium isotopes, especially for ²³²Th and ²²⁸Th, in the geochemical cycle of thorium in the marine environment.     

Global transport rates of Cs and Pu originating from the Nagasaki A-bomb in 1945 as determined from analysis of Canadian Arctic ice cores

Recent advancements in analytical technology make it possible for artificial radionuclides released from nuclear explosions to be detected in Arctic ice core layers. The fission product, ¹³⁷Cs, and the unexpended fission material, ^239+240Pu, originating from the Nagasaki A-bomb of August 1945, were measured by collecting 10 ice cores on the Agassiz ice cap, Ellesmere Island, Canada. The deposition rates were 0·020 mBq cm^-2 for ¹³⁷Cs and 0·0016 mBq cm^-2 for ^239+240Pu, originating from Nagasaki. Assuming the radionuclides, excluding the amount fissioned from the explosion and deposi-ted as local fallout, are deposited evenly throughout the Northern Hemisphere, 67% of the expected amount of ¹³⁷Cs reached the Arctic while 1·1% of ^239+240Pu reached the Arctic. The results suggest that different transport mechanisms exist for various contaminants in the global transport system.     

Time pattern of off-site plutonium deposition from rocky flats plant by lake sediment analyses

A sediment core from a lake downwind of the Rocky Flats Plant, where nuclear weapons components are produced, was used to reconstruct a time pattern of off-site plutonium deposition. Core sections were dated by analyses of ¹³⁷Cs, ^239,240Pu, ²³⁸Pu, and ²⁴¹Am fallout from nuclear testing and ²³⁸Pu fallout from a satellite failure. A peak in transuranic concentrations occurred in late 1969 which was attributable to the Plant. This was confirmed by mass isotopic analysis of plutonium isotopes in selected core segments where the global fallout and Plant contributions could be differentiated. The 18 nCi ^239,240Pu per m² from the Plant that had accumulated in the sediment is reasonable when compared to soil analyses.     

Fractionation of plutonium in environmental and bio-shielding concrete samples using dynamic sequential extraction

Fractionation of plutonium isotopes (²³⁸Pu, ^239,240Pu) in environmental samples (i.e. soil and sediment) and bio-shielding concrete from decommissioning of nuclear reactor were carried out by dynamic sequential extraction using an on-line sequential injection (SI) system combined with a specially designed extraction column. Plutonium in the fractions from the sequential extraction was separated by ion exchange chromatography and measured using alpha spectrometry. The analytical results show a higher mobility of plutonium in bio-shielding concrete, which means attention should be paid to the treatment and disposal of nuclear waste from decommissioning.     

Isotope tracing of submarine groundwater discharge offshore Ubatuba, Brazil: results of the IAEA–UNESCO SGD project

Results of groundwater and seawater analyses for radioactive (³H, ²²²Rn, ²²³Ra, ²²⁴Ra, ²²⁶Ra, and ²²⁸Ra) and stable (D and ¹⁸O) isotopes are presented together with in situ spatial mapping and time series ²²²Rn measurements in seawater, direct seepage measurements using manual and automated seepage meters, pore water investigations using different tracers and piezometric techniques, and geoelectric surveys probing the coast. This study represents first time that such a new complex arsenal of radioactive and non-radioactive tracer techniques and geophysical methods have been used for simultaneous submarine groundwater discharge (SGD) investigations. Large fluctuations of SGD fluxes were observed at sites situated only a few meters apart (from 0 cm d⁻¹ to 360 cm d⁻¹; the unit represents cm³/cm²/day), as well as during a few hours (from 0 cm d⁻¹ to 110 cm d⁻¹), strongly depending on the tidal fluctuations. The average SGD flux estimated from continuous ²²²Rn measurements is 17 ± 10 cm d⁻¹. Integrated coastal SGD flux estimated for the Ubatuba coast using radium isotopes is about 7 × 10³ m³ d⁻¹ per km of the coast. The isotopic composition (δD and δ¹⁸O) of submarine waters was characterised by significant variability and heavy isotope enrichment, indicating that the contribution of groundwater in submarine waters varied from a small percentage to 20%. However, this contribution with increasing offshore distance became negligible. Automated seepage meters and time series measurements of ²²²Rn activity concentration showed a negative correlation between the SGD rates and tidal stage. This is likely caused by sea level changes as tidal effects induce variations of hydraulic gradients. The geoelectric probing and piezometric measurements contributed to better understanding of the spatial distribution of different water masses present along the coast. The radium isotope data showed scattered distributions with offshore distance, which imply that seawater in a complex coast with many small bays and islands was influenced by local currents and groundwater/seawater mixing. This has also been confirmed by a relatively short residence time of 1–2 weeks for water within 25 km offshore, as obtained by short-lived radium isotopes. The irregular distribution of SGD seen at Ubatuba is a characteristic of fractured rock aquifers, fed by coastal groundwater and recirculated seawater with small admixtures of groundwater, which is of potential environmental concern and has implications on the management of freshwater resources in the region.     

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.     

Air radionuclide patterns observed at Monaco from the Chernobyl accident

Radionuclide concentrations in air filters taken in Monaco for several weeks after the Chernobyl accident on April 26, 1986 have been carefully examined. Unusual radionuclides such as ¹⁰⁵Ru, ¹¹¹Ag, ¹²⁵Sn and ¹²⁶Sb were identified as being present in small amounts. Nuclides of the more volatile elements I, Te, and Ag peaked 6–24 hours earlier than the average, whereas the refractory elements exhibited a different distribution. Radionuclide concentrations seen in air at Chernobyl compared with those observed at Monaco show that ^134,137Cs was least removed by environmental processes between the two sites and rare earths the most. The second (4–5 May) peak of activity released from the Chernobyl reactor was characterised by a relatively higher content of refractory elements, also observed at Monaco. The different phases of such an accident can thus be observed even at distances approaching 2000 km.     

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.     

99Tc in the sub-arctic food chain Lichen-Reindeer-man

The deposition, migration and annual variations of ⁹⁹Tc fallout in carpets of lichen collected during the period 1956–1981 have been investigated. The transfer of ⁹⁹Tc to reindeer and man has also been studied. Technetium showed a shorter mean residence time than ¹³⁷Cs in the lichen carpet. The activity ratio ⁹⁹Tc/¹³⁷Cs was generally lower than the theoretical fission ratio of 1·43 × 10⁻⁴. The maximum concentration of ⁹⁹Tc in lichens occurred in 1967 (ca. 60 mBq kg⁻¹) but in 1975 higher values were found than would have been predicted from fallout. The average depth integrated concentration of ⁹⁹Tc at 62·3°N, 12·4° E in 1972 was 540 ± 100 mBq m⁻². The studies of reindeer tissues show that technetium has a short mean residence time in the muscle tissues (ca. 5 days) and is not accumulated like ¹³⁷Cs. The committed dose equivalent from ⁹⁹Tc to the local Lapp population engaged in reindeer breeding is negligible.     

Human bones obtained from routine joint replacement surgery as a tool for studies of plutonium, americium and ⁹⁰Sr body-burden in general public

The paper presents a new sampling method for studying in-body radioactive contamination by bone-seeking radionuclides such as ⁹⁰Sr, ^239+240Pu, ²³⁸Pu, ²⁴¹Am and selected gamma-emitters, in human bones. The presented results were obtained for samples retrieved from routine surgeries, namely knee or hip joints replacements with implants, performed on individuals from Southern Poland. This allowed to collect representative sets of general public samples. The applied analytical radiochemical procedure for bone matrix is described in details. Due to low concentrations of ²³⁸Pu the ratio of Pu isotopes which might be used for Pu source identification is obtained only as upper limits other then global fallout (for example Chernobyl) origin of Pu. Calculated concentrations of radioisotopes are comparable to the existing data from post-mortem studies on human bones retrieved from autopsy or exhumations. Human bones removed during knee or hip joint surgery provide a simple and ethical way for obtaining samples for plutonium, americium and ⁹⁰Sr in-body contamination studies in general public.     

Fukushima fallout in Northwest German environmental media

Traces of short- and long-lived fallout isotopes (¹³¹I, ¹³⁴Cs and ¹³⁷Cs) were found in environmental samples collected in Northwest Germany (rain water, river sediment, soil, grass and cow milk) from March to May 2011, following the radioactivity releases after the nuclear accident in Fukushima, Japan. The measured concentrations are consistent with reported concentrations in air, amount of rainfall and expected values applying simple radioecological models. The [¹³⁴Cs]/[¹³⁷Cs] ratio reported for air (about 1) allows for discrimination between “recent” and “old” ¹³⁷Cs. Expected ¹³⁶Cs values fell below the detection limits of the instrumentation, despite large sample masses and long counting times.     

Depth profile of ²³⁶U/²³⁸U in soil samples in La Palma, Canary Islands

The vertical distribution of the ²³⁶U/²³⁸U isotopic ratio was investigated in soil samples from three different locations on La Palma (one of the seven Canary Islands, Spain). Additionally the ²⁴⁰Pu/²³⁹Pu atomic ratio, as it is a well establish tool for the source identification, was determined. The radiochemical procedure consisted of a U separation step by extraction chromatography using UTEVA^® Resin (Eichrom Technologies, Inc.). Afterwards Pu was separated from Th and Np by anion exchange using Dowex 1x2 (Dow Chemical Co.). Furthermore a new chemical procedure with tandem columns to separate Pu and U from the matrix was tested. For the determination of the uranium and plutonium isotopes by alpha spectrometry thin sources were prepared by microprecipitation techniques. Additionally these fractions separated from the soil samples were measured by Accelerator Mass Spectrometry (AMS) to get information on the isotopic ratios ²³⁶U/²³⁸U, ²⁴⁰Pu/²³⁹Pu and ²³⁶U/²³⁹Pu, respectively. The ²³⁶U concentrations [atoms/g] in each surface layer (∼2 cm) were surprisingly high compared to deeper layers where values around two orders of magnitude smaller were found. Since the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated a global fallout signature we assume the same origin as the probable source for ²³⁶U. Our measured ²³⁶U/²³⁹Pu value of around 0.2 is within the expected range for this contamination source.