Impact of an exceptional Saharan dust outbreak in France: PM10 and artificial radionuclides concentrations in air and in dust deposit

The present study focuses on the exceptional Saharan dust event that affected most of France in February 2004. Activity levels of various artificial radionuclides (⁹⁰Sr, ¹³⁷Cs, uranium, thorium and plutonium isotopes, ²⁴¹Am) were examined. Activity or isotopic ratios are discussed in the context of atmospheric nuclear weapons tests, among them French tests performed in Sahara in the 1960s. The daily evolution of ¹³⁷Cs activity levels in the atmosphere was compared to daily PM₁₀ change. A link between airborne ¹³⁷Cs and PM₁₀, is given. It is estimated that this 2-day event deposited as much ¹³⁷Cs as would be deposited on average over a 10-month period. The amount of deposited ¹³⁷Cs and ^239+240Pu represents respectively about 0.1 and 1% of the activity already present in the soil. Such Saharan dust events correspond to an extreme type of “feeder” process of artificial radionuclides in the atmosphere. Therefore, they contribute to the long term background level of artificial radionuclides kept at trace levels in the atmosphere.     

On the presence of enriched amounts of 235U in hot particles from the terrestrial area affected by the Palomares accident (Spain)

The characterisation by ICP-MS of an isolated Pu-U hot particle originating from the nuclear weapons accident in Palomares (Spain) shows, for the first time, that its uranium content is highly enriched in (235)U. The enrichment has been confirmed by independent analyses of two surface soil samples collected in a heavily contaminated area close to the impact point of one of the bombs. This finding clarifies better the composition of the weapons involved in the accident and is of importance when the inventory of U and Pu in the contaminated area are to be calculated.     

Radium-226 levels and concentration ratios between water, vegetation, and tissues of ruffed grouse (Bonasa umbellus) from a watershed with uranium tailings near Elliot Lake, Canada

Radionuclide levels measured in bone, muscle, kidney and liver tissues, gut contents and diet items of 47 grouse from the Serpent River drainage basin, containing uranium (U) tailings at Elliot Lake, and from control areas in Ontario, showed variation by site and tissue. The mean level of 226radium (Ra) in bones of grouse sampled from Elliot Lake (28.5 mBq g(-1)) was higher than that in bones of birds from a distant control site near Sudbury, Ontario (8.0 mBq g(-1)) but similar to the value in a local control population (28.1 mBq g(-1)). Birds from Mid- and Low-Serpent River basin populations (with 17.1 and 17.7 mBw g(-1), respectively) did not differ from local or distant control populations; muscle, liver and kidney had lower 226Ra concentrations, which did not differ significantly among populations. Levels of 226Ra in the crop contents and intestine did not differ significantly by site and were similar to those of food items consumed by the birds. Stomach content values were higher in birds sampled in Elliot Lake and at the local control site than in those taken at the distant control site; birds sampled downstream from Elliot Lake did not differ from distant controls in this regard. Levels of 232thorium (Th) and 230Th were below detection limits (0.1 microg g(-1) and 5.0 mBq g(-1), respectively) in bone, muscle and liver tissue in two grouse with elevated levels of 226Ra. Other radionuclides were measurable in some tissues: 238U in bone at 0.4 microg g(-1), in muscle to 0.2 microg g(-1), in liver to 1.0 gmg g(-1.), 228Th was found only in muscle (8.0 mBq g(-1)), 210poloniuim (Po) was found in bone, muscle and liver (maxima: 24.0, 7.0, 16.0 mBq g(-1)) with the exception of one muscle sample; 210lead (Pb) was detected in only one liver sample (50.0 mBq g(-1)). Environmental levels fell within ranges previously reported at the sites, or at similar locations elsewhere. Leaves of trembling and largetooth aspen growing in the basin had mean 226Ra levels of 14.8 and 52.7 mBq g(-1) (dry weight) respectively, and fungal material carried up to 215.4 mBq g(-1) (air-dried), with some variation by site. River and lake waters sampled near the U tailings had 118.1 mBq litre(-1) of dissolved 226Ra; at the distant control site the value was 12.1 mBq litre(-1). The concentration ratios (CR) between bone of grouse collected at the Elliot Lake sites and trembling and largetooth aspen leaves were 1.38 and 1.09 (fresh weight basis); from other diet items and to other tissues the values were less than unity. Bone tissue: water ratios, based on dissolved 226Ra levels, ranged to 30.89. People eating grouse from the study area are unlikely to consume radionuclides in excess of limits currently established by Canadian regulatory authorities.     

Colloidal mobilization from soil and transport of uranium in (sub)-surface waters

An analytical methodology was developed to characterize the colloidal distribution of trace elements of interest in environmental waters sampled in a same site and enables the different colloidal distributions from waters to be compared. The purpose was to provide consistent information related to the origin and nature of colloids responsible for the transport of trace element(s). The work was motivated by the observed enhanced mobility of uranium in soil. The colloidal size continuum was investigated by a multi-technique approach involving asymmetric flow field-flow fractionation (AF4) coupled with ultraviolet spectroscopy (UV), multi angle light scattering (MALS), and atomic mass spectrometry (ICPMS). To take into consideration the size and shape variability specific to each sample, the size distributions were established from the gyration radii measured from MALS, also considering the size information from standard nanospheres fractionated by AF4. A new parameter called “shape index” was proposed. It expresses the difference in hydrodynamic behavior between analytes and spherical particles taken as reference. Under AF4 diffusion conditions, it can be considered as an evaluator of the deviation from the sphericity of the fractionated analytes. AF4-UV-MALS-ICPMS enabled the dimensional and chemical characteristics of the colloidal size continuum to be obtained. As a “proof of concept”, the developed methodology was applied at a field scale, in a reference study site. In order to have a “dynamic understanding”, the investigation was based on the joint characterization of colloids from surface waters and soil leachates from static and dynamic processes. In the water samples of the study site, the continuum of gyration radius ranged from a few nanometers up to 200 nm. Colloids containing iron, aluminum, and organic carbon were involved in the uranium transport in the soil column and surface waters. The colloidal uranium concentration in the surface water increased from the upstream location (approximately 13 ng (U) L^?1) to the downstream location (approximately 60 ng (U) L^?1).

     

Using Multimedia Modeling to Expedite Site Characterization

GOAL, SCOPE AND BACKGROUND: This paper uses two case studies of U.S. Department of Energy nuclear weapons complex installations to illustrate the integration of expedited site characterization (ESC) and multimedia modeling in the remedial action decision making process. CONCEPTUAL SITE MODELS, MULTIMEDIA MODELS, AND EXPEDITED SITE CHARACTERIZATION: Conceptual site models outline assumptions about contaminates and the spatial/temporal distribution of potential receptors. Multimedia models simulate contaminant transport and fate through multiple environmental media, estimate potential human exposure via specific exposure pathways, and estimate the risk of cancer and non-cancer health outcomes. ESC relies on using monitoring data to quantify the key components of an initial conceptual site model that is modified iteratively using the multimedia model. CASE STUDIES: Two case studies are presented that used the ESC approach: Los Alamos National Laboratory (LANL) and Pantex. LANL released radionuclides, metals, and organic compounds, into canyons surrounding the facility. The Pantex Plant has past waste management operations which included burning chemical wastes in unlined pits, burying wastes in unlined landfills, and discharging plant wastewaters into on-site surface waters. CONCLUSIONS: The case studies indicate that using multimedia models with the ESC approach can inform assessors about what, where, and how much site characterization data needs to be collected to reduce the uncertainty associated with risk assessment. Lowering the degree of uncertainty reduces the time and cost associated with assessing potential risk and increases the confidence that decision makers have in the assessments performed.     

Mobility of Polychlorinated Aromatic Compounds in Soils Contaminated With Wood-preserving Oil

Greater understanding of the mobility of polychlorinated aromatic compounds in soils is needed to investigate contamination and design suitable remediation strategies for sites contaminated with wood-preserving oil. The objectives of this study were (1) to develop a suitable aqueous batch extraction method for soil containing wood-preservative residues; (2) to determine partition coefficients for the primary contaminants [pentachlorophenol (PCP), polychlorinated dibenzo-p-dloxins (PCDDs), and polychlorinated dibenzofurans (PCDFS)] in oil, soil, and aqueous phases; and (3) to evaluate the potential soil migration of the primary contaminants. In a three-phase oil-soil-water mixture, PCP, PCDDs, and PCDFs were partitioned to the greatest extent in the oil phase. These results suggest that the migration of contaminants can occur in a saturated subsurface soil zone containing an oil phase at a wood-preserving site. In the absence of a free oil phase, PCDDs and PCDFs were highly partitioned onto soil and were considered non-leachable in the aqueous phase. However, PCP was considered highly teachable from contaminated soil containing only an aqueous liquid phase. Results from this study Indicate that removal of any free oil phase present in subsurface soil should have highest priority during the cleanup of contaminated wood-preserving sites.     

Mobility of polychlorinated aromatic compounds in soils contaminated with wood-preserving oil

Greater understanding of the mobility of polychlorinated aromatic compounds in soils is needed to investigate contamination and design suitable remediation strategies for sites contaminated with wood-preserving oil. The objectives of this study were (1) to develop a suitable aqueous batch extraction method for soil containing wood-preservative residues; (2) to determine partition coefficients for the primary contaminants [pentachlorophenol (PCP), polychlorinated dibenzo-p-dioxins (PCDDs), and polychlorinated dibenzofurans (PCDFS)] in oil, soil, and aqueous phases; and (3) to evaluate the potential soil migration of the primary contaminants. In a three-phase oil-soil-water mixture, PCP, PCDDs, and PCDFs were partitioned to the greatest extent in the oil phase. These results suggest that the migration of contaminants can occur in a saturated subsurface soil zone containing an oil phase at a wood-preserving site. In the absence of a free oil phase, PCDDs and PCDFs were highly partitioned onto soil and were considered non-leachable in the aqueous phase. However, PCP was considered highly leachable from contaminated soil containing only an aqueous liquid phase. Results from this study indicate that removal of any free oil phase present in subsurface soil should have highest priority during the cleanup of contaminated wood-preserving sites.     

Influence of pH on pesticide sorption by soil containing wheat residue-derived char

Field burning of crop residues incorporates resulting chars into soil and may thus influence the environmental fate of pesticides in the soil. This study evaluated the influence of pH on the sorption of diuron, bromoxynil, and ametryne by a soil in the presence and absence of a wheat residue-derived char. The sorption was measured at pHs approximately 3.0 and approximately 7.0. Wheat char was found to be a highly effective sorbent for the pesticides, and its presence (1% by weight) in soil contributed >70% to the pesticide sorption (with one exception). The sorption of diuron was not influenced by pH, due to its electroneutrality. Bromoxynil becomes dissociated at high pHs to form anionic species. Its sorption by soil and wheat char was lower at pH approximately 7.0 than at pH approximately 3.0, probably due to reduced partition of the anionic species of bromoxynil into soil organic matter and its weak interaction with the carbon surface of the char. Ametryne in its molecular form at pH approximately 7.0 was sorbed by char-amended soil via partitioning into soil organic matter and interaction with the carbon surface of the char. Protonated ametryne at pH approximately 3.0 was substantially sorbed by soil primarily via electrostatic forces. Sorption of protonated ametryne by wheat char was also significant, likely due not only to the interaction with the carbon surface but also to interactions with hydrated silica and surface functional groups of the char. Sorption of ametryne by char-amended soil at pH approximately 3.0 was thus influenced by both the soil and the char. Environmental conditions may thus significantly influence the sorption and behavior of pesticides in agricultural soils containing crop residue-derived chars.     

Excess plutonium in soil near the Nevada Test Site,USA

Two soil profiles were collected from undisturbed areas near the Nevada Test Site (NTS). The activity of 137Cs in the surface layer of the downwind Queen City Summit profile is three times higher than at the upwind site at Searchlight, NV (41.1+/-0.6 mBq/g vs. 13.0+/-0.4 mBq/g), and the 239,240Pu activity is 100 times greater (51+/-2 mBq/g vs. 0.52+/-0.03 mBq/g). An examination of the literature suggests that the 137Cs/239,240Pu and the 239,240Pu/238Pu activity ratios in soils and sediments from the northern hemisphere, due to fallout from atmospheric atomic weapons testing, have generalized values of 36+/-4 and 30+/-4, respectively (as of 1 July 1995). Deviations from these values may indicate possible contamination by sources other than fallout. Data from the surface soil of the downwind Queen City Summit profile yield a 137Cs/239,240Pu ratio of 0.81+/-0.02 and a 239,240Pu/238Pu ratio of 78+/-6. Clearly, an increase in 239,240Pu relative to 137Cs or 238Pu can account for these observations. There is compelling evidence that this "excess" 239,240Pu came from activities at the NTS during the aboveground testing of nuclear devices, more than likely from safety tests, some 40 years ago, and/or during the interim by the wind-driven resuspension of contaminated surface soil on the NTS and its transport off-site. Moreover, the two concentration profiles show that high percentages of both of these elements are retained for decades in the upper few centimeters of soil in Nevada's desert environment.     

Conceptual and Numerical Modeling of Radionuclide Transport and Retention in Near-Surface Systems

Scenarios of barrier failure and radionuclide release to the near-surface environment are important to consider within performance and safety assessments of repositories for nuclear waste. A geological repository for spent nuclear fuel is planned at Forsmark, Sweden. Conceptual and numerical reactive transport models were developed in order to assess the retention capacity of the Quaternary till and clay deposits for selected radionuclides, in the event of an activity release from the repository. The elements considered were carbon (C), chlorine (Cl), cesium (Cs), iodine (I), molybdenum (Mo), niobium (Nb), nickel (Ni), radium (Ra), selenium (Se), strontium (Sr), technetium (Tc), thorium (Th), and uranium (U). According to the numerical predictions, the repository-derived nuclides that would be most significantly retained are Th, Ni, and Cs, mainly through sorption onto clays, followed by U, C, Sr, and Ra, trapped by sorption and/or incorporation into mineral phases.     

Uptake of radionuclides by vegetation at a High Arctic location

Radionuclide levels in vegetation from a High Arctic location were studied and compared to in situ soil concentrations. Levels of the anthropogenic radionuclide 137Cs and the natural radionuclides 40K, 238U, 226Ra and 232Th are discussed and transfer factor (TF) values and aggregated transfer (Tag) values are calculated for vascular plants. Levels of 137Cs in vegetation generally followed the order mosses > lichen > vascular plants. The uptake of 137Cs in vascular plants showed an inverse relationship with the uptake of 40K, with 137Cs TF and Tag values generally higher than 40K TF and Tag values. 40K activity concentrations in all vegetation showed little correlation to associated soil concentrations, while the uptake of 238U, 226Ra and 232Th by vascular and non-vascular plants was generally low.     

Concentration of tetrachloroethylene in indoor air at a former dry cleaner facility as a function of subsurface contamination: a case study

A field study was performed to evaluate indoor air concentrations and vapor intrusion (VI) of tetrachloroethylene (PCE) and other chlorinated solvents at a commercial retail site in Dallas, TX. The building is approximately 40 yr old and once housed a dry cleaning operation. Results from an initial site characterization were used to select sampling locations for the VI study. The general approach for evaluating VI was to collect time-integrated canister samples for off-site U.S. Environmental Protection Agency Method TO-15 analyses. PCE and other chlorinated solvents were measured in shallow soil gas, subslab soil-gas, indoor air, and ambient air. The subslab soil gas exhibited relatively high values: PCE < or =2,600,000 parts per billion by volume (ppbv) and trichloroethylene < or =170 ppbv. The attenuation factor, the ratio of indoor air and subslab soil-gas concentrations, was unusually low: approximately 5 x 10(-6) based on the maximum subslab soil-gas concentration of PCE and 1.4 x 10(-5) based on average values.     

Leaching behaviour of Cd, Cu, Pb and Zn in surface soils derived from dredged sediments

Leaching of heavy metals from land-disposed dredged sediment spoils is a potential environmental hazard. The leaching behavior of Cd, Cu, Pb and Zn in surface soils sampled from abandoned dredged sediment disposal sites was assessed. Using simple mass-balance calculations, the significance of the leaching test results with respect to metal migration into underlying clean soil was appraised. The potential leachability, defined as the amounts released at constant pH 4, decreased in the order (% of total contents): Zn (58%) approximately equal to Cd (49%)>Cu (5%) approximately equal to Pb (2%). The kinetics of metal release were determined in a cascade shaking test using de-mineralized water acidified to pH 4 (HNO(3)). Metal concentrations in the leachates were low and metal migration was, assuming uniform convective flow, predicted to be of no environmental concern. It is emphasized that any long-term prediction of metal migration is uncertain.     

226Ra and other radionuclides in water, vegetation, and tissues of beavers (Castor canadensis) from a watershed containing U tailings near Elliot Lake, Canada

Radionuclide levels were measured in tissues, gut contents, diet items, and water at site of capture, of adult beavers from the Serpent River drainage basin which contains U tailings at Elliot Lake, Ontario, and from nearby control sites. Levels of (226)Ra in beaver bone, muscle and kidney were highest in animals from locations close to U tailings; liver levels did not vary by site. Environmental (226)Ra levels were within ranges previously reported at these or similar locations elsewhere; levels in beaver gut contents reflected levels in diet items. Concentration ratios exceeded unity only between some vegetation items and beaver bone at the Elliot Lake site and were less than 0.19 between vegetation and other tissues. In two beavers with tissue levels of (226)Ra higher than other sampled, neither (232)Th nor (230)Th were detected in bone, muscle or liver tissues. U-238 was measurable in bone, muscle and liver, (228)Th in bone, (210)Po bone, muscle and liver; and (210)Pb was measurable only in bone. Estimated yearly intakes of radionuclides by people eating beavers were calculated to be below current allowable levels set by the Canadian regulatory authorities.     

Methane balance of a bioreactor landfill in Latin America

This paper presents results from a methane (CH4) gas emission characterization survey conducted at the Loma Los Colorados landfill located 60 km from Santiago, Chile. The landfill receives approximately 1 million metric tons (t) of waste annually, and is equipped with leachate control systems and landfill gas collection systems. The collected leachate is recirculated to enable operation of the landfill as a bioreactor. For this study, conducted between April and July 2000, a total of 232 surface emission measurements were made over the 23-ha surface area of the landfill. The average surface flux rate of CH4 emissions over the landfill surface was 167 g x m(-2) x day(-1), and the total quantity of surface emissions was 13,320 t/yr. These values do not include the contribution made by "hot spots," originating from leachate pools caused by "daylighting" of leachate, that were identified on the landfill surface and had very high CH4 emission rates. Other point sources of CH4 emissions at this landfill include 20 disconnected gas wells that vent directly to the atmosphere. Additionally, there are 13 gas wells connected to an incinerator responsible for destroying 84 t/yr of CH4. The balance also includes CH4 that is being oxidized on the surface of the landfill by meth-anotrophic bacteria. Including all sources, except leachate pool emissions, the emissions were estimated to be 14,584 t/yr CH4. It was estimated that less than 1% of the gas produced by the decomposition of waste was captured by the gas collection system and 38% of CH4 generated was emitted to the atmosphere through the soil cover.     

Environmental Issues—Persistent Problems and Emerging Challenges

Abstract

A field study was performed to evaluate indoor air concentrations and vapor intrusion (VI) of tetrachloroethylene (PCE) and other chlorinated solvents at a commercial retail site in Dallas, TX. The building is approximately 40 yr old and once housed a dry cleaning operation. Results from an initial site characterization were used to select sampling locations for the VI study. The general approach for evaluating VI was to collect time-integrated canister samples for off-site U.S. Environmental Protection Agency Method TO-15 analyses. PCE and other chlorinated solvents were measured in shallow soil gas, subslab soil-gas, indoor air, and ambient air. The subslab soil gas exhibited relatively high values: PCE ≤2,600,000 parts per billion by volume (ppbv) and trichloroethylene ≤170 ppbv. The attenuation factor, the ratio of indoor air and subslab soil-gas concentrations, was unusually low: approximately 5 x 10^-6 based on the maximum subslab soil-gas concentration of PCE and 1.4 x 10^-5 based on average values.     

Characterization of contaminated soil and groundwater surrounding an illegal landfill (S. Giuliano,Venice, Italy) by principal component analysis and kriging

The characterization of a hydrologically complex contaminated site bordering the lagoon of Venice (Italy) was undertaken by investigating soils and groundwaters affected by the chemical contaminants originated by the wastes dumped into an illegal landfill. Statistical tools such as principal components analysis and geostatistical techniques were applied to obtain the spatial distribution of chemical contaminants. Dissolved organic carbon (DOC), SO4(2-) and Cl- were used to trace the migration of the contaminants from the top soil to the underlying groundwaters. The chemical and hydrogeological available information was assembled to obtain the schematic of the conceptual model of the contaminated site capable to support the formulation of major exposure scenarios, which are also provided.     

Noninvasive characterization of the Trecate (Italy) crude-oil contaminated site: links between contamination and geophysical signals

The characterization of contaminated sites can benefit from the supplementation of direct investigations with a set of less invasive and more extensive measurements. A combination of geophysical methods and direct push techniques for contaminated land characterization has been proposed within the EU FP7 project ModelPROBE and the affiliated project SoilCAM. In this paper, we present results of the investigations conducted at the Trecate field site (NW Italy), which was affected in 1994 by crude oil contamination. The less invasive investigations include ground-penetrating radar (GPR), electrical resistivity tomography (ERT), and electromagnetic induction (EMI) surveys, together with direct push sampling and soil electrical conductivity (EC) logs. Many of the geophysical measurements were conducted in time-lapse mode in order to separate static and dynamic signals, the latter being linked to strong seasonal changes in water table elevations. The main challenge was to extract significant geophysical signals linked to contamination from the mix of geological and hydrological signals present at the site. The most significant aspects of this characterization are: (a) the geometrical link between the distribution of contamination and the site’s heterogeneity, with particular regard to the presence of less permeable layers, as evidenced by the extensive surface geophysical measurements; and (b) the link between contamination and specific geophysical signals, particularly evident from cross-hole measurements. The extensive work conducted at the Trecate site shows how a combination of direct (e.g., chemical) and indirect (e.g., geophysical) investigations can lead to a comprehensive and solid understanding of a contaminated site’s mechanisms.     

A review of the Texas,USA San Jacinto Superfund site and the deposition of polychlorinated dibenzo-p-dioxins and dibenzofurans in the San Jacinto River and Houston Ship Channel

The San Jacinto River (SJR) waste pits that lie just under the 1–10 overpass in eastern Harris County east of Houston, Texas, USA, were created in the 1960s as dumping grounds for paper mill waste. The deposition of this waste led to accumulation of highly toxic polychlorinated dibenzo-p-dioxins and dibenzofurans (PCCDDs/PCDFs) over the course of several decades. After abandonment, the waste material eventually became submerged under the waters of the SJR, resulting in widespread environmental contamination that currently constitutes a significant health concern for eastern Harris County communities. The original waste pits were rediscovered in 2005, and the San Jacinto waste site is now a designated EPA superfund site. The objective of this review then is to discuss the history and current state of containment around the San Jacinto waste pits and analyze spatial and temporal trends in the PCDD/PCDF deposition through the SJR system from the data available. We will discuss the current exposure and health risks represented by the Superfund site and the SJR system itself, as well as the discovery of liver, kidney, brain (glioma), and retinoblastoma cancer clusters in eastern Harris County across multiple census tracts that border the Superfund site. We will also cover the two primary management options, containment versus removal of the waste from the Superfund and provide recommendations for increased monitoring of existing concentrations of polychlorinated waste in the SJR and its nearby associated communities.     

Accumulation history of radionuclides in the lichen Stereocaulon vesuvianum from Mt. Vesuvius (south Italy)

The fruticose lichen Stereocaulon vesuvianum, growing on the slopes of Mt. Vesuvius (south Italy), was used as a biomonitor of 134Cs, 137Cs, 103Ru and 106Ru derived from the April 26 1986 Chernobyl nuclear reactor accident. Samples were taken at five different quotes (370, 490, 580, 780 and 960 m a.s.l.) and four successive dates (October 1986, December 1986, October 1987 and May 1999). At the first sampling, the concentrations (as Bq kg(-1) dry weight) ranged between 460 and 1020 for 134Cs, 1330 and 2500 for 137Cs, 90 and 200 for 103Ru and 360 and 710 for 106Ru, values generally lower in respect to those measured in soil and higher plants. Of the total 137Cs measured only 14% was due to 1950s and 1960s nuclear weapons tests fallout. Highest average activities of all nuclides were observed at the quote of 960 m and significant correlation (0.7相似文献