Use of AMS in the marine environment

In recent years, the field of AMS has expanded into many areas of science. This paper reviews a variety of applications of AMS in the marine environment, focusing particularly on recent developments and applications. Following a brief summary of the three main isotope techniques used in environmental studies: dating, tracing and source identification, a number of applications are considered. Traditional (14)C-dating is no longer the dominant application of AMS measurements, and together with measurements of (10)Be, (26)Al and (36)Cl, much of the research is now directed towards an understanding of global climate change via studies of oceanic circulation, atmospheric processes and past climates by cosmic ray exposure dating. Profiles of long-lived cosmogenic radionuclides in sediments and ice cores, as a function of depth and, thus, age, provide key information on past solar variability, production rate changes and atmospheric transport and deposition mechanisms. Useful paleoclimatic information may be derived from these archives both because deposition is influenced by climate and because solar activity (which influences production) and solar radiance (which influences climate) are correlated. In recent years, emphasis has been put on the development and application of AMS techniques for the measurement of heavier long-lived isotopes, including (99)Tc, (129)I, (236)U and other actinide isotopes. AMS combines ultra low detection limits and the possibility to analyse isotope ratios that can be difficult with traditional instruments and has been used in a number of applications on the consequences and uses of releases from nuclear energy. Finally, the use AMS in environmental sciences is expected to expand further in the foreseeable future with long-lived cosmogenic radionuclides contributing to a large body of knowledge on processes involving atmosphere, oceans, ice sheets, biosphere, soils and sediments.     

Cosmogenic 22Na as an index of the residence time of water in freshwater basins: a review

The goal of this review is to draw attention to an opportunity for the use of cosmogenic (22)Na for dating young surface and underground waters. After 1961 when a significant quantity of (22)Na was released into the environment as a result of nuclear weapon tests, its concentrations in river waters were greatly increased, and a return to natural (cosmogenic) levels took until the mid-1980s. The studies made during this non-steady-state period showed that the one-box model for freshwater basin correctly describes the experimental data. For the 19 studied basins of Russia, the Baltic States and Japan, a calculation based on this model gave values for the mean residence time of water in the range from 4 to 23 years. Now, only cosmogenic (22)Na is in the environment, and it is the single cosmogenic radionuclide at present, which can serve as a steady-state tracer for dating young waters (up to some decades).     

Distribution of gamma-ray emitting radionuclides in the environment of Burullus Lake: I. Soils and vegetations

The concentrations and distribution of gamma-ray emitting isotopes in Burullus Lake were investigated with the aim of evaluating the environmental radioactivity. Particularly in wetlands, natural properties of the environment can cause the actual inventory to be different from the activity originally deposited. The mean concentrations of (226)Ra, (232)Th and (40)K were 14.3, 15.5 and 224 Bq/kg, respectively, in the coastal soils. On the other hand, soil samples from the islands had mean concentrations of 13.5, 17.4 and 341 Bq/kg for (226)Ra, (232)Th and (40)K, respectively. Samples from coast and islands show evidence of possible transfer and accumulation of the (137)Cs radionuclide. The mean (137)Cs activity concentrations in the soil samples were 1.2 and 15.1 Bq/kg in the coast and islands, respectively. The vertical migration of (137)Cs was studied based on its content in the consequently located three soil layers down to 30 cm depth. The radium equivalent, dose rate in air and annual dose equivalent from the terrestrial natural gamma-radiation were evaluated. The mean activity concentrations of the gamma-ray emitting radionuclides in vegetation were relatively low.     

Precipitation scavenging of 7Be and 137Cs radionuclides in air

Atmospheric depositional fluxes of the naturally occurring 7Be of cosmogenic origin and 137Cs from fallout of the Chernobyl accident were measured over a 6-year period (January 1987-December 1992) at Thessaloniki, Greece (40 degrees 38'N, 22 degrees 58'E). Total precipitation accumulation during 1987-1992 varied between 33.7 cm and 65.2 cm, reflecting a relatively dry (precipitation-free) climate. The activity concentrations of 7Be and 137Cs in rainwater depended on the precipitation rate, being higher for low precipitation rates and lesser for high precipitation rates. 137Cs was removed by rain and snow more efficiently than 7Be. Snowfall was more efficient than rainfall in removing the radionuclides from the atmosphere. The annual bulk depositional fluxes of 7Be varied between 477 and 1133 Bq m(-2) y(-1) and this variability was attributed to the amount of precipitation and the variations of the atmospheric concentrations of 7Be. The annual bulk depositional fluxes of 137Cs showed a significant decrease over time from 1987 to 1992, resulting in a removal half-life of 1.33 years. The presence of 137Cs in air, and therefore in rainwater and snow, long after the Chernobyl accident (26 April 1986) was mainly due to the resuspension process. The normalized depositional fluxes of both radionuclides showed maximal values during the spring season where the maximum amount of precipitation occurred. The relatively high positive correlation between 7Be and 137Cs normalized depositional fluxes indicates that the scavenging process of local precipitation controlled the fluxes of both radionuclides. The dry depositional flux of 7Be was less than 9.37% of total (wet and dry) depositional flux. The fraction of dry-to-total depositional flux of 137Cs was much higher than that of 7Be, due to the resuspended soil.     

Anthropogenic radionuclides in the Japan Sea: their distributions and transport processes

The anthropogenic radionuclides, (90)Sr, (137)Cs and (239+240)Pu, were measured in the water column of the Japan Sea/East Sea during 1997-2000. The vertical profiles of radionuclide concentrations showed: exponential decrease with depth for (90)Sr and (137)Cs, and surface minimum/subsurface maximum for (239+240)Pu. These results do not differ substantially from results reported previously. The area-averaged concentrations of radionuclides in the Japan Sea are higher than those found in the Northwest Pacific Ocean below surface layer showing the accumulation of the radionuclides in the deep waters in the Japan Sea. Concerning spatial distributions, the area of high (137)Cs inventory extends from the Japan Basin into the Yamato Basin. It is suggested that wintertime convection of water, occurring mainly in the Japan Basin, causes the radionuclides to sink. The nuclides then advect into the Yamato Basin after detouring around the Yamato Rise.     

The presence of some artificial and natural radionuclides in a Eucalyptus forest in the south of Spain

Long-lived artificial radionuclides (137Cs, 90Sr) were studied in a Eucalyptus plantation located in the south-west of Spain. Radionuclide concentrations were determined in different types of samples corresponding to specific forest components (soil, trees, herbs and litter). Depth profile distributions were obtained in two selected core soils. Two layers were separately measured in three other cores. The concentration factor, defined as the ratio between the mean activity concentration in a component and the mean activity concentration in the soil, was calculated for each component. The biomass of different components was estimated in order to evaluate the total density concentration (Bq/ha) of the artificial radionuclides (137Cs, 90Sr) in the Eucalyptus plantation. The transfer of the radionuclides between the different forest components can be inferred from the results. Additionally, other naturally occurring radionuclides (40K, 226Ra, 228Ra, 228Ac) were determined for comparison. Transport of radionuclides from forest to a nearby pulp mill is also discussed.     

Vertical distribution of radionuclides in soil of a grassland site in Chernobyl exclusion zone

Five soil profiles from a site about 8 km SE of the Chernobyl NPP were investigated for the vertical distribution of radionuclides. The average (137)Cs-inventory at the site is about 2.6 MBq/m(2) (reference date 1 May 1986). Apart from (137)Cs, the following radionuclides have been identified (their activity ratios to (137)Cs in brackets): (134)Cs (0.537), (125)Sb (0.068), (60)Co (0.0022), (154)Eu (0.016), (155)Eu (0.020), (94g)Nb (9.5E-5), (239/240)Pu (0.0088), (238)Pu (0.040), (90)Sr (0.30) and (241)Am (0.011). Apparent vertical migration velocities are between 0.14 and 0.26 cm/a, apparent dispersion coefficients range from 0.02 to 0.13 cm(2)/a. The rankings of the velocities v for different radionuclides are (Sr, Cs, Sb, Co, Pu)< Am < Eu and Sr < (Cs, Nb), for D, the following rankings have been found: (Nb, Sr, Cs) < Am < Eu, Cs相似文献   

Migration ability of radionuclides in soil-vegetation cover of Belarus after Chernobyl accident

This article illustrates the experimental experience achieved in the research of the self-restoration of radioactive-contaminated natural ecosystems. The main directions of studies were: the content and geochemical stability of "hot" particles in radioactive fallout from Chernobyl accident; the physicochemical forms (water-soluble, exchangeable, mobile and fixed) of Cs-137, Sr-90, Pu-239, 240 and Am-241 in the wide varieties of soils; the biological accessibility of radionuclides and their contents in soil pore solutions; and the dynamics and migration parameters of radionuclides vertical redistribution in different landscape conditions.     

On the sensitivity of a marine dispersion model to parameters describing the transfers of radionuclides between the liquid and solid phases

The sensitivity of a marine dispersion model for non-conservative radionuclides, previously developed and validated for the English Channel, to parameters describing the exchanges between the liquid and solid phases (suspended matter and bottom sediments) has been studied using a Monte Carlo method. A probability distribution is assigned to each parameter. They are sampled to obtain a set of model parameters and a model run is carried out. This process is repeated to obtain a distribution of model outputs. Partial correlation coefficients are calculated to assess the relative influence of each parameter on model output. Errors are also assigned to model results. Three situations are studied: an instantaneous release of radionuclides, a continuous release and the case of a contaminated sediment behaving as a long-term source of radionuclides. Calculations have also been carried out for two radionuclides with different geochemical behaviour: (137)Cs and (239,240)Pu. The results indicate that all parameters are relevant, depending on the phase we are interested in obtaining the result and on the source term (instantaneous, continuous or due to sediments). However, parameters that are, in general, more influential are kinetic rates, mixing depth in the sediment and mean radius of suspended and sediment particles. This suggests that including several particle sizes in future radionuclide dispersion models could lead to an improvement in model results. Differences have also been found with respect to the relevance of some parameters depending on the geochemical behaviour of the radionuclide.     

A dynamic model for assessing radiological consequences of routine releases in the Loire river: parameterisation and uncertainty/sensitivity analysis

A dynamic model for assessing the transfer of several radionuclides ((58)Co, (60)Co, (110 m)Ag, (134)Cs, (137)Cs, (54)Mn and (131)I) in a food-chain was applied on the Loire river, where 14 nuclear power plants situated on five different sites operate. The model considers the following potential exposure pathways: (i) transfer of radionuclides through the aquatic food chain and the subsequent internal exposure of humans due to ingestion of contaminated water and/or fish; (ii) use of river water for agricultural purposes (irrigation), transfer of radionuclides through the terrestrial food chain and the subsequent internal exposure of humans due to ingestion of contaminated foodstuffs; (iii) internal exposure due to inhalation of dust originating from resuspension of contaminated soil particles; (iv) external exposure from radionuclides present in the river or deposited on the river sediments or the soil. For each of the parameters introduced in this model, a probability density function, allowing further uncertainty and sensitivity analysis, was proposed. Uncertainty/sensitivity analysis were performed to: (i) compare calculations to empirical data; (ii) determine a confidence interval for the mean annual dose to critical groups; and (iii) identify the parameters responsible for the uncertainty and subsequent research priorities.     

Distribution and mobilization of U, Th and 226Ra in the plant-soil compartments of a mineralized uranium area in south-west Spain

The activity concentrations of natural uranium isotopes (238U and 234U), thorium isotopes (232Th, 230Th and 225Th) and 226Ra were studied in soil and vegetation samples from a disused uranium mine located in the Extremadura region in the south-west of Spain. The results allowed us to characterize radiologically the area close to the installation and one affected zone was clearly manifest as being dependent on the direction of the surface water flow from the mine. The activity concentration mean values (Bq/kg) in this zone were: 10,924, 10,900, 10,075 and 5,289 for 238U, 234U, 230Th and 226Ra, respectively, in soil samples and 1,050, 1,060, 768 and 1,141 for the same radionuclides in plant samples. In an unaffected zone, the activity concentration mean values (Bq/kg) were: 184, 190, 234 and 7251 for 235U, 234U, 230Th and 226Ra, respectively, in soil samples and 28. 29, 31 and 80 in plant samples. The activity concentrations obtained for 232Th and 228Th showed that the influence of the mine was only important for the uranium series radionuclides. The relative radionuclide mobilities were determined from the activity ratios. Correlations between radionuclide activity concentrations and stable element concentrations in the soil samples helped to understand the possible distribution paths for the natural radionuclides.     

Distribution of fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) in soils of Taiwan

Depth profiles and cumulative deposition of four fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) were determined in presumably undisturbed soils in Taiwan. Inventories of these radionuclides in different areas correlate significantly with each other (except 7Be) and with mean annual rainfall, providing a necessary condition for the development of soil erosion studies in Taiwan. However, the data show very large spatial variability between and within landscape units, reflecting the steep topographic and meteorological gradients in the island. Thus, the application of fallout radionuclides to study soil conservation in Taiwan is expected to be a demanding task; it will call for dense sampling even at undisturbed reference sites.     

Occurrence and behaviour of radionuclides in the Moselle River—Part III: Dispersion of radionuclides along the river course

Knowledge about propagation of radionuclides from nuclear power plants (NPPs) along the course of a river is of great interest in radioecological assessments. By use of a model previously applied in the cases of the Rhine and Weser Rivers, the distribution of various radionuclides released into the Moselle from the NPP Cattenom at normal operation is described with ⁵⁸Co, ⁶⁰Co and ^110mAg as tracers. A comparison of field measurements with calculated values revealed that the radionuclide concentrations in suspended matter and nuclide loads calculated from emission rates agreed with the measured data by a factor of less than two on average.Radionuclide concentrations and loads along the river course decrease mainly due to deposition of particulate radioactive matter in high-sedimentation areas and due to dilution with uncontaminated material from tributaries and other sources. The rate constants of both processes were evaluated, and the mean range of suspended radioactive particles in the Moselle was estimated. Moreover, this study showed anew that suspended matter has to be considered as the main carrier by which the radionuclides from NPPs may be transported over long distances.     

Vertical distribution, migration rates, and model comparison of actinium in a semi-arid environment

Vertical soil characterization and migration of radionuclides were investigated at four radioactively contaminated sites on Kirtland Air Force Base (KAFB), New Mexico to determine the vertical downward migration of radionuclides in a semi-arid environment. The surface soils (0-15 cm) were intentionally contaminated with Brazilian sludge (containing (232)Thorium and other radionuclides) approximately 40 years ago, in order to simulate the conditions resulting from a nuclear weapons accident. Site grading consisted of manually raking or machine disking the sludge. The majority of the radioactivity was found in the top 15 cm of soil, with retention ranging from 69 to 88%. Two models, a compartment diffusion model and leach rate model, were evaluated to determine their capabilities and limitations in predicting radionuclide behavior. The migration rates of actinium were calculated with the diffusion compartment and the leach rate models for all sites, and ranged from 0.009 to 0.1 cm/yr increasing with depth. The migration rates calculated with the leach rate models were similar to those using the diffusion compartment model and did not increase with depth (0.045-0.076, 0.0 cm/yr). The research found that the physical and chemical properties governing transport processes of water and solutes in soil provide a valid radionuclide transport model. The evaluation also showed that the physical model has fewer limitations and may be more applicable to this environment.     

Sources of anthropogenic radionuclides in the environment: a review

Studies of radionuclides in the environment have entered a new era with the renaissance of nuclear energy and associated fuel reprocessing, geological disposal of high-level nuclear wastes, and concerns about national security with respect to nuclear non-proliferation. This work presents an overview on sources of anthropogenic radionuclides in the environment, as well as a brief discussion of salient geochemical behavior of important radionuclides. We first discuss the following major anthropogenic sources and current developments that have lead, or could potentially contribute, to the radionuclide contamination of the environment: (1) nuclear weapons program; (2) nuclear weapons testing; (3) nuclear power plants; (4) uranium mining and milling; (5) commercial fuel reprocessing; (6) geological repository of high-level nuclear wastes that include radionuclides might be released in the future, and (7) nuclear accidents. Then, we briefly summarize the inventory of radionuclides ⁹⁹Tc and ¹²⁹I, as well as geochemical behavior for radionuclides ⁹⁹Tc, ¹²⁹I, and ²³⁷Np, because of their complex geochemical behavior, long half-lives, and presumably high mobility in the environment; biogeochemical cycling and environment risk assessment must take into account speciation of these redox-sensitive radionuclides.     

Transuranic and fission product contamination in lake sediments from an alpine wetland, Boréon (France)

Transuranics and fission products have been measured in lake sediment samples, collected in an alpine wetland, to determine their vertical distribution and calculate inventories. The radionuclides considered are 90Sr, 137Cs, 238Pu, 239/240Pu and 241Am. From the results, a better knowledge of radionuclide accumulation mode and behaviour was obtained. In addition, the origins of the individual pollutants could be deduced from activity ratios. Analyses were made on different sediment cores. The sampling sites were chosen to enable future determination of the mass balances of the radiopollutants. As the selected study area is in a recreational area used by urban populations, a rough estimate was made of the mean external dose from 137Cs for comparison with the French regulation.     

Distribution of some natural gamma-emitting radionuclides in the soils of the coastal areas of Nigeria

Studies on the radiation level and the radionuclide distribution of some naturally occurring radioactive materials (NORM) in the soils of the coastal areas of Southern Nigeria were undertaken. The purpose of this study is to provide baseline data for the effective monitoring of unforeseeable radioactive fallout in these areas where a lot of oil exploration activities are going on. The radioactivity concentrations of these naturally occurring radionuclides (specifically (40)K, (238)U and (232)Th) in the soil samples were analyzed using a high-resolution, low-background, hyper-pure coaxial gamma-ray detector (EG&G ORTEC HPGe) coupled to an amplifier and multi-channel analyzer. The activity of (40)K ranges between 111.9 and 444.7 kBq kg(-1) with a median value of 283.28 kBq kg(-1); the activity of (226)Ra (a daughter of (238)U) varies from 23.24 to 43.66 kBq kg(-1) with a median value of 34.54 kBq kg(-1); and that of (232)Th ranges from 6.45 to 12.79 kBq kg(-1) with a median value of 9.17 kBq kg(-1). The mean absorbed dose rate in air due to these NORM is found to be (33.655+/-3.409) nGy h(-1). The correlation analyses showed a positive relationship between the three radionuclides in all the five coastal states.     

The dispersion of 137Cs and 239,240Pu in the Rhone River plume: a numerical model

A numerical three dimensional model to simulate the transport of Cs and Pu by the Rhone River plume has been developed. The model solves the hydrodynamic equations, including baroclinic terms (that account for density variations) and a turbulence model, the suspended matter equations, including several particle classes simultaneously, settling, deposition and erosion of the sediment, and the radionuclide dispersion equations. Exchanges of radionuclides between the liquid and solid phases are described in terms of kinetic transfer coefficients. The dependence of these coefficients with water salinity is explicitly included in the model since it changes from freshwater to seawater values in the model domain. Computed activity levels in water, suspended matter and bed sediments are, in general, in agreement with measurements in the area. The model can also give a wide amount of information, as distribution coefficients for total suspended matter and sediments and for each particle class, fractions of radionuclides fixed to solid particles, and vertical profiles of radionuclides and distribution coefficients.     

Radionuclides deposition over Antarctica

A detailed and comprehensive map of the distribution patterns for both natural and artificial radionuclides over Antarctica has been established. This work integrates the results of several decades of international programs focusing on the analysis of natural and artificial radionuclides in snow and ice cores from this polar region. The mean value (37+/-20 Bq m(-2)) of (241)Pu total deposition over 28 stations is determined from the gamma emissions of its daughter (241)Am, presenting a long half-life (432.7 yrs). Detailed profiles and distributions of (241)Pu in ice cores make it possible to clearly distinguish between the atmospheric thermonuclear tests of the fifties and sixties. Strong relationships are also found between radionuclide data ((137)Cs with respect to (241)Pu and (210)Pb with respect to (137)Cs), make it possible to estimate the total deposition or natural fluxes of these radionuclides. Total deposition of (137)Cs over Antarctica is estimated at 760 TBq, based on results from the 90-180 degrees East sector. Given the irregular distribution of sampling sites, more ice cores and snow samples must be analyzed in other sectors of Antarctica to check the validity of this figure.