ABSTRACT
Presented here is the first demonstration of supervised discretization to 'declutter' multivariate classification data in chemical sensor applications. The performance of multivariate classification models is often limited by the non-informative chemical variance within each target class; decluttering methods seek to reduce within-class variance while retaining between-class variance. Supervised discretization is shown to declutter classes in a manner that is superior to the state-of-the-art External Parameter Orthogonalization (EPO) by constructing a more parsimonious model with fewer parameters to optimize and is, consequently, less susceptible to overfitting and information loss. The comparison of supervised discretization and EPO is performed on three classification applications: X-ray fluorescence spectra of pine ash where the pine was grown in three distinct soil types, laser induced breakdown spectroscopy of colored artisanal glasses, and laser induced breakdown spectroscopy of exotic hardwood species.
ABSTRACT
Nuclear weapons testing in the atmosphere during the 1950s and 1960s deposited fallout throughout the world, exposing all humans to food and water before the Limited Test Ban Treaty ended large-scale tests. The largest effort to measure in vivo fallout in humans, performed by Washington University (USA), collected over 300,000 deciduous teeth to document a sustained increase in Strontium-90 (Sr-90) during testing and a sharp decline after the test ban. Sr-90 patterns and trends in teeth were consistent with those of bones and milk. Sr-90 is still detectable in about 100,000 of the teeth, which were never tested. Tooth donors were born during atmospheric testing (1946-1965) and thus exposed to fallout in utero and during infancy/childhood, when exposures pose the greatest health risk. Preliminary analysis of global fallout's health risk in the United States indicates recent cancer mortality in several high-fallout areas exceeded that of states with the lowest fallout, peaking for the cohort born in the early 1960s, when fallout was highest. These findings support subsequent measurement of Sr-90 in deciduous teeth of persons who died of diseases such as cancer, along with controls, a novel approach to assessing fallout hazards.
Subject(s)
Neoplasms , Nuclear Weapons , Radioactive Fallout , Infant , United States/epidemiology , Humans , Child , Radioactive Fallout/adverse effects , Tooth, Deciduous , WashingtonABSTRACT
Landscape evolution is driven by tectonics, climate and surface denudation. In New Zealand, tectonics and steep climatic gradients cause a dynamic landscape with intense chemical weathering, rapid soil formation, and high soil losses. In this study, soil, and elemental redistribution along two adjacent hillslopes in East Otago, New Zealand, having different landscape settings (ridge versus valley) are compared to identify soil weathering and erosion dynamics. Fallout radionuclides (239+240Pu) show that over the last ~ 60 years, average soil erosion rates in the valley (~ 260 [t km-2 year-1]) are low compared to the ridge (~ 990 [t km-2 year-1]). The ridge yields up to 26% lower soil weathering intensity than the topographical-protected valley. The lowest soil weathering intensity is found at both hilltop positions, where tors (residual rocks) are present and partially disintegrate. The soil weathering intensity increases with distance from tors, suggesting that tors rejuvenate the chemical weathering signature at the hilltop positions with fresh material. The inversed and decreasing weathering degree with all soil depth indicates that the fresh mineral contribution must be higher at the soil surface than at the bedrock weathering front. Higher erosion rates at the exposed ridge may be partially attributed to wind, consistent with rock abrasion of tors, and low local river sediment yields (56 [t km-2 year-1]). Thus, the East Otago spatial patterns of soil chemistry and erosion are governed by tor degradation and topographic exposure.
Subject(s)
Soil , Weather , New Zealand , RiversABSTRACT
Global nuclear weapon testing and the Chernobyl accident have released large amounts of radionuclides into the environment. However, to date, the spatial patterns of these fallout sources remain poorly constrained. Fallout radionuclides (137Cs, 239Pu, 240Pu) were measured in soil samples (n = 160) collected at flat, undisturbed grasslands in Western Europe in the framework of a harmonised European soil survey. We show that both fallout sources left a specific radionuclide imprint in European soils. Accordingly, we used plutonium to quantify contributions of global versus Chernobyl fallout to 137Cs found in European soils. Spatial prediction models allowed for a first assessment of the global versus Chernobyl fallout pattern across national boundaries. Understanding the magnitude of these fallout sources is crucial not only to establish a baseline in case of future radionuclide fallout but also to define a baseline for geomorphological reconstructions of soil redistribution due to soil erosion processes.
ABSTRACT
An important process in the production of drinking water is the recharge of the withdrawn ground water with river water at protected recharge fields. While it is well known that undisturbed soils are efficiently filtering and adsorbing radionuclides, the goal of this study was to investigate their behaviour in an artificial recharge site that may receive rapid and additional input of radionuclides by river water (particularly when draining a catchment including nuclear power plants (NPP)). Soil profiles of recharge sites were drilled and analysed for radionuclides, specifically radiocesium (137Cs), radiostrontium (90Sr) and plutonium (239+240Pu). The distribution of the analysed radionuclides were compared with an uncultivated reference soil outside the recharge site. The main activity of 137Cs was located in the top soil (4.5-7.5 cm) and reached down to a depth of 84 cm and 48 cm for the recharge and the reference site, respectively. The found activities of 239+240Pu originate from the global fallout after 1950. 239+240Pu appeared to be strongly adsorbed onto soil particles. The shape of the depth profile was similar to 137Cs, but also similar between the recharge and the reference site. In contrast, 90Sr showed a uniform distribution over the entire depth of the recharge and reference profiles indicating that 90Sr already entered the gravel zone and the ground water. Elevated inventories of the radionuclides were observed for the recharge site. The soil of the recharge field exhibited a threefold higher activity of 137Cs compared to the reference soil. Also for 239+240Pu higher inventories where observed for the recharge sites (40%). 90Sr behaved differently, showing similar inventories between reference and recharge site. We estimate that 75-89% of the total inventory of 137Cs in the soil at the recharge site (7.000 Bq/m2) originated from the fallout of the Chernobyl accident and from emissions of Swiss NPPs. This estimate is based on the actual activity ratio of 137Cs/239+240Pu of 22 for global fallout. The investigations identified radiostrontium as potential threat to the ground water.
Subject(s)
Cesium Radioisotopes/analysis , Plutonium/analysis , Radiation Monitoring , Soil Pollutants, Radioactive/analysis , Strontium Radioisotopes/analysis , Nuclear Power Plants , SwitzerlandABSTRACT
Measurements of the long-lived radionuclide 236U are an important endeavor, not only in nuclear safeguards work, but also in terms of using this emerging nuclide as a tracer in chemical oceanography, hydrology, and actinide sourcing. Depending on the properties of a sample and its neutron irradiation history, 236U/238U ratios from different sources vary significantly. Therefore, this ratio can be treated as an important fingerprint for radioactive source identification, and in particular, affords a definitive means of discriminating between naturally occurring U and specific types of anthropogenic U. The development of mass spectrometric techniques makes it possible to determine ultra-trace levels of 236U in environmental samples. In this paper, we review the current status of mass spectrometric approaches for determination of 236U in environmental samples. Various sample preparation methods are summarized and compared. The mass spectrometric techniques emphasized herein are thermal ionization mass spectrometry (TIMS), inductively coupled plasma mass spectrometry (ICP-MS) and accelerator mass spectrometry (AMS). The strategies or principles used by each technique for the analysis of 236U are described. The performances of these techniques in terms of abundance sensitivity and detection limit are discussed in detail. To date, AMS exhibits the best capability for ultra-trace determinations of 236U. The levels and behaviors of 236U in various environmental media are summarized and discussed as well. Results suggest that 236U has an important, emerging role as a tracer for geochemical studies.
ABSTRACT
Fallout radionuclides have been used successfully worldwide as tracers for soil erosion, but relatively few studies exploit the full potential of plutonium (Pu) isotopes. Hence, this study aims to explore the suitability of the plutonium isotopes (239)Pu and (240)Pu as a method to assess soil erosion magnitude by comparison to more established fallout radionuclides such as (137)Cs and (210)Pbex. As test area an erosion affected headwater catchment of the Lake Soyang (South Korea) was selected. All three fallout radionuclides confirmed high erosion rates for agricultural sites (>25tha(-1)yr(-1)). Pu isotopes further allowed determining the origin of the fallout. Both (240)Pu/(239)Pu atomic ratios and (239+240)Pu/(137)Cs activity ratios were close to the global fallout ratio. However, the depth profile of the (239+240)Pu/(137)Cs activity ratios in undisturbed sites showed lower ratios in the top soil increments, which might be due to higher migration rates of (239+240)Pu. The activity ratios further indicated preferential transport of (137)Cs from eroded sites (higher ratio compared to the global fallout) to the depositional sites (smaller ratio). As such the (239+240)Pu/(137)Cs activity ratio offered a new approach to parameterize a particle size correction factor that can be applied when both (137)Cs and (239+240)Pu have the same fallout source. Implementing this particle size correction factor in the conversion of (137)Cs inventories resulted in comparable estimates of soil loss for (137)Cs and (239+240)Pu. The comparison among the different fallout radionuclides highlights the suitability of (239+240)Pu through less preferential transport compared to (137)Cs and the possibility to gain information regarding the origin of the fallout. In conclusion, (239+240)Pu is a promising soil erosion tracer, however, since the behaviour i.e. vertical migration in the soil and lateral transport during water erosion was shown to differ from that of (137)Cs, there is a clear need for a wider agro-environmental testing.
Subject(s)
Plutonium/analysis , Radiation Monitoring/methods , Soil Pollutants/analysis , Soil , Agriculture , Cesium Radioisotopes/analysis , Forestry , Models, Theoretical , Republic of KoreaABSTRACT
Sheet erosion is one of the major threats to alpine soils. To quantify its role and impact in the degradation processes of alpine grasslands, the application of Fallout Radionuclides (FRN) showed very promising results. The specific characteristics of plutonium 239 + 240 (239+240Pu), such as the homogeneous fallout distribution, the long half-life and the cost and time effective measurements make this tracer application for investigating soil degradation in Alpine grasslands more suitable than any other FRN (e.g. 137Cs). However, the conversion of 239+240Pu inventories into soil erosion rates remains a challenge. Currently available conversion models have been developed mainly for 137Cs with later adaptation to other FRN (e.g. Excess 210Pb, and 7Be), each model being defined for specific land use (ploughed and/or unploughed) and processes (erosion or deposition). As such, they may fail in describing correctly the distribution of Pu isotopes in the soil. A new conversion model, MODERN, with an adaptable algorithm to estimate erosion and deposition rates from any FRN inventory changes was recently proposed (Arata et al., 2016). In this complementary contribution, the authors compare the application of MODERN to other available conversion models. The results show a good agreement between soil redistribution rates obtained from MODERN and from the models currently used by the FRN scientific community (i.e. the Inventory Method).
Subject(s)
Models, Chemical , Plutonium/analysis , Radiation Monitoring , Soil Pollutants, Radioactive/analysis , Soil/chemistry , Agriculture , Grassland , Half-LifeABSTRACT
The measurement of fallout radionuclides (FRN) has become one of the most commonly used tools to quantify sediment erosion or depositional processes. The conversion of FRN inventories into soil erosion and deposition rates is done with a variety of models, which suitability is dependent on the selected FRN, soil cultivation (ploughed or unploughed) and movement (erosion or deposition). The authors propose a new conversion model, which can be easily and comprehensively used for different FRN, land uses and soil redistribution processes. The new model MODERN (Modelling Deposition and Erosion rates with RadioNuclides) considers the precise depth distribution of any FRN at the reference site, and allows adapting it for any specific site conditions. MODERN adaptability and performance in converting different FRN inventories is discussed for a theoretical case as well as for two already published case studies i.e. a 137Cs study in an alpine and unploughed area in the Aosta valley (Italy) and a 210Pbex study on a ploughed area located in the Transylvanian Plain (Romania). The tests highlight a highly significant correspondence (i.e. correlation factor of 0.91) between the results of MODERN and the published results of other models currently used by the FRN scientific community (i.e. the Profile Distribution Model and the Mass Balance Model). The development and the cost free accessibility of MODERN (see modern.umweltgeo.unibas.ch) will ensure the promotion of wider application of FRNs for tracing soil erosion and sedimentation.
Subject(s)
Models, Theoretical , Radiation Monitoring , Soil/chemistry , Cesium Radioisotopes/analysis , Italy , Lead Radioisotopes/analysis , Soil Pollutants, Radioactive/analysisABSTRACT
Two sediment cores were collected in a mangrove forest to construct geochronologies for the previous century using natural and anthropogenic radionuclide tracers. Both sediment cores were dated using (239+240)Pu global fallout signatures as well as (210)Pb, applying both the Constant Initial Concentration (CIC) and the Constant Rate of Supply (CRS) models. The (239+240)Pu and CIC model are interpreted as having comparable sediment accretion rates (SAR) below an apparent mixed region in the upper â¼5 to 10 cm. In contrast, the CRS dating method shows high sediment accretion rates in the uppermost intervals, which is substantially reduced over the lower intervals of the 100-year record. A local anthropogenic nutrient signal is reflected in the high total phosphorus (TP) concentration in younger sediments. The carbon/nitrogen molar ratios and δ(15)N values further support a local anthropogenic nutrient enrichment signal. The origin of these signals is likely the treated sewage discharge to Moreton Bay which began in the early 1970s. While the (239+240)Pu and CIC models can only produce rates averaged over the intervals of interest within the profile, the (210)Pb CRS model identifies elevated rates of sediment accretion, organic carbon (OC), nitrogen (N), and TP burial from 2000 to 2013. From 1920 to 2000, the three dating methods provide similar OC, N and TP burial rates, â¼150, 10 and 2 g m(-2) year(-1), respectively, which are comparable to global averages.
Subject(s)
Carbon/analysis , Geologic Sediments/chemistry , Lead Radioisotopes/analysis , Nitrogen/analysis , Phosphorus/analysis , Plutonium/analysis , Radioactive Fallout/analysis , Bays/analysis , Queensland , Radiometric Dating , WetlandsABSTRACT
Anthropogenic radionuclides have been distributed globally due to nuclear weapons testing, nuclear accidents, nuclear weapons fabrication, and nuclear fuel reprocessing. While the negative consequences of this radioactive contamination are self-evident, the ubiquitous fallout radionuclides (FRNs) distribution form the basis for the use as tracers in ecological studies, namely for soil erosion assessment. Soil erosion is a major threat to mountain ecosystems worldwide. We compare the suitability of the anthropogenic FRNs, 137Cs and 239+240Pu as soil erosion tracers in two alpine valleys of Switzerland (Urseren Valley, Canton Uri, Central Swiss Alps and Val Piora, Ticino, Southern Alps). We sampled reference and potentially erosive sites in transects along both valleys. 137Cs measurements of soil samples were performed with a Li-drifted Germanium detector and 239+240Pu with ICP-MS. Our data indicates a heterogeneous deposition of the 137Cs, since most of the fallout origins from the Chernobyl April/May 1986 accident, when large parts of the European Alps were still snow-covered. In contrast, 239+240Pu fallout originated mainly from 1950s to 1960s atmospheric nuclear weapons tests, resulting in a more homogenous distribution and thus seems to be a more suitable tracer in mountainous grasslands. Soil erosion assessment using 239+240Pu as a tracer pointed to a huge dynamic and high heterogeneity of erosive processes (between sedimentation of 1.9 and 7 t ha(-1) yr(-1) and erosion of 0.2-16.4 t ha(-1) yr(-1) in the Urseren Valley and sedimentation of 0.4-20.3 t ha(-1) yr(-1) and erosion of 0.1-16.4 t ha(-1) yr(-1) at Val Piora). Our study represents a novel and successful application of 239+240Pu as a tracer of soil erosion in a mountain environment.
Subject(s)
Cesium Radioisotopes/analysis , Ecosystem , Plutonium/analysis , Radioactive Fallout/analysis , Soil Pollutants, Radioactive/analysis , Soil/chemistry , Poaceae , Radioactive Hazard Release , Radioactive Tracers , SwitzerlandABSTRACT
The effects of elevated CO2 on ecosystem element stocks are equivocal, in part because cumulative effects of CO2 on element pools are difficult to detect. We conducted a complete above and belowground inventory of non-nitrogen macro- and micronutrient stocks in a subtropical woodland exposed to twice-ambient CO2 concentrations for 11 years. We analyzed a suite of nutrient elements and metals important for nutrient cycling in soils to a depth of ~2 m, in leaves and stems of the dominant oaks, in fine and coarse roots, and in litter. In conjunction with large biomass stimulation, elevated CO2 increased oak stem stocks of Na, Mg, P, K, V, Zn and Mo, and the aboveground pool of K and S. Elevated CO2 increased root pools of most elements, except Zn. CO2-stimulation of plant Ca was larger than the decline in the extractable Ca pool in soils, whereas for other elements, increased plant uptake matched the decline in the extractable pool in soil. We conclude that elevated CO2 caused a net transfer of a subset of nutrients from soil to plants, suggesting that ecosystems with a positive plant growth response under high CO2 will likely cause mobilization of elements from soil pools to plant biomass.
Subject(s)
Carbon Dioxide/metabolism , Quercus/metabolism , Soil/chemistry , Biomass , Ecosystem , Metals/chemistry , Metals/metabolism , Phosphorus/chemistry , Phosphorus/metabolism , Plant Leaves/metabolism , Plant Stems/metabolism , Sulfur/chemistry , Sulfur/metabolismABSTRACT
Stratospheric fallout-derived (236)U has been detected by sector field ICPMS at two field locations for which our laboratory possessed available archived samples: A) four soil cores from Washington state (northwestern USA) and B) sediment cores from three small lakes in the Pechora region (Russian Arctic). Four Washington state soil cores exhibit (236)U inventories of 8.1 ± 1.3, 11.1 ± 0.9, 18 ± 2, and 30.2 ± 3.9 Tatoms/m(2); the respective (239)Pu contents are 52.9 ± 3.5, 67 ± 3, 71 ± 2, and 151 ± 2 Tatoms/m(2). A (236)U/(239)Pu atom ratio of 0.19 ± 0.04 (1 SD) has been determined from the Washington state soil cores. The three Pechora region lake cores each exhibit coincident maxima in their (236)U and (239)Pu atom concentration profiles. The (236)U/(238)U atom ratios are controlled by two independent factors; (236)U is from fallout deposition and (238)U concentrations are a property of the geochemical distribution of naturally occurring U. A (236)U/(238)U atom ratio as high as 8.9 × 10(-6) has been observed for acid-leached soils containing Pu solely derived from bomb-test fallout. Accordingly, a non-zero (236)U background from stratospheric fallout must be recognized and taken into account when detectable (236)U is used to infer specific local or regional influences of reactor-irradiated U.
Subject(s)
Plutonium/analysis , Soil Pollutants, Radioactive/analysis , Uranium/analysis , Radiation Monitoring/methods , Washington , Water Pollutants, RadioactiveABSTRACT
The distribution of contaminant elements within ecosystems is an environmental concern because of these elements' potential toxicity to animals and plants and their ability to hinder microbial ecosystem services. As with nutrients, contaminants are cycled within and through ecosystems. Elevated atmospheric CO2 generally increases plant productivity and alters nutrient element cycling, but whether CO2 causes similar effects on the cycling of contaminant elements is unknown. Here we show that 11 years of experimental CO2 enrichment in a sandy soil with low organic matter content causes plants to accumulate contaminants in plant biomass, with declines in the extractable contaminant element pools in surface soils. These results indicate that CO2 alters the distribution of contaminant elements in ecosystems, with plant element accumulation and declining soil availability both likely explained by the CO2 stimulation of plant biomass. Our results highlight the interdependence of element cycles and the importance of taking a broad view of the periodic table when the effects of global environmental change on ecosystem biogeochemistry are considered.
Subject(s)
Air Pollutants/analysis , Carbon Dioxide/analysis , Quercus/drug effects , Soil Pollutants/metabolism , Soil/chemistry , Trace Elements/metabolism , Air Pollutants/metabolism , Air Pollutants/pharmacology , Atmosphere/chemistry , Carbon Cycle , Carbon Dioxide/metabolism , Carbon Dioxide/pharmacology , Plant Leaves/drug effects , Plant Leaves/metabolism , Quercus/growth & development , Quercus/metabolism , Soil Pollutants/analysis , Soil Pollutants/toxicity , Trace Elements/analysis , Trace Elements/toxicityABSTRACT
Childhood uptake of lead from exposure to atmospheric leaded gasoline in the United States has been studied using mainly blood lead levels. Since reliable blood lead techniques were used only after the peak use of leaded gasoline, the prior exposure history is unclear. The well-documented decline in blood lead levels after the mid-1970s could represent the continuation of a historic steady decline in exposure from many sources. Alternatively, the post-1970s decline might represent the declining phase of a unimodal rise and fall corresponding closely to usage of leaded gasoline. To assess these possibilities, lead concentration and 207Pb/206Pb isotope ratios were measured in the enamel of permanent molar teeth formed between 1936 and 1993 in mainly African-American donors who grew up in the Cleveland area. Tooth enamel preserves the lead concentration and isotope ratio that prevails during tooth formation. Historical trends in enamel lead concentration were significantly correlated with surrogates of atmospheric lead exposure: lead in sediments of two dated Lake Erie cores, and lead consumed in gasoline. About two-thirds of the total lead uptake into enamel in this period was attributable to leaded gasoline, and the remainder to other sources (e.g. paint). Enamel 207Pb/206Pb isotope ratios were similar to those of one lake sediment. Multivariate analysis revealed significant correlation in neighborhoods with higher levels of traffic, and including lake sediment data, accounted for 53% of the variation in enamel lead levels. Enamel lead concentration was highly correlated with reported African-American childhood blood levels. The extrapolated peak level of 48microg/dL (range 40 to 63) is associated with clinical and behavioral impairments, which may have implications for adults who were children during the peak gasoline lead exposure. In sum, leaded gasoline emission was the predominant source of lead exposure of African-American Cleveland children during the latter two-thirds of the 20th century.
Subject(s)
Environmental Exposure/analysis , Gasoline , Lead/metabolism , Tooth/metabolism , Child , Dental Enamel/metabolism , Environmental Exposure/statistics & numerical data , Environmental Monitoring , Epidemiological Monitoring , Female , Humans , Isotopes/metabolism , Male , Multivariate Analysis , Ohio/epidemiologyABSTRACT
Sector field inductively coupled plasma mass spectrometry (SF-ICPMS) has been used with analysis of solution samples and laser ablation (LA) of electrodeposited alpha sources to characterize plutonium activities and atom ratios prevalent in the western USA. A large set of surface soils and attic dusts were previously collected from many locations in the states of Nevada, Utah, Arizona, and Colorado; specific samples were analyzed herein to characterize the relative contributions of stratospheric fallout vs. Nevada Test Site (NTS) plutonium. This study illustrates two different ICPMS-based analytical strategies that are successful in fingerprinting Pu in environmental soils and dusts. Two specific datasets have been generated: (1) soils are leached with HNO3-HCl, converted into electrodeposited alpha sources, counted by alpha spectrometry, then re-analyzed using laser ablation SF-ICPMS; (2) samples are completely dissolved by treatment with HNO3-HF-H3BO3, Pu fractions are prepared by extraction chromatography, and analyzed by SF-ICPMS. Optimal laser ablation and ICPMS conditions were determined for the re-analysis of archived alpha spectrometry "planchette" sources. The best ablation results were obtained using a large spot size (200 microm), a defocused beam, full repetition rate (20 Hz) and scan rate (200 microm s(-1)); LA-ICPMS data were collected with a rapid electrostatic sector scanning experiment. Less than 10% of the electroplated surface area is consumed in the LA-ICPMS analysis, which would allow for multiple re-analyses. Excellent agreement was found between (239+240)Pu activities determined by LA-ICPMS vs. activity results obtained by alpha spectrometry for the same samples ten years earlier. LA-ICPMS atom ratios for 240Pu/239Pu and 241Pu/239Pu range from 0.038-0.132 and 0.00034-0.00168, respectively, and plot along a two-component mixing line (241Pu/239Pu = 0.013 [240Pu/239Pu] - 0.0001; r2 = 0.971) with NTS and global fallout end-members. A rapid total dissolution procedure, followed by extraction chromatography and SF-ICPMS solution Pu analysis, generates excellent agreement with certified (239+240)Pu activities for standard reference materials NIST 4350b, NIST 4353, NIST 4357, and IAEA 385. (239+240)Pu activities and atom ratios determined by total dissolution reveal isotopic information in agreement with the LA-ICPMS dataset regarding the ubiquitous mixing of NTS and stratospheric fallout Pu sources in the regional environment. For several specific samples, the total dissolution method reveals that Pu is incompletely recovered by simpler HNO3-HCl leaching procedures, since some of the Pu originating from the NTS is contained in refractory siliceous particles.
Subject(s)
Mass Spectrometry/methods , Plutonium/analysis , Soil/analysis , Plutonium/chemistry , Southwestern United StatesABSTRACT
Lead isotope ratios and lead (Pb) levels were analyzed in 33 individuals from a forgotten cemetery at the Colorado Mental Health Institute at Pueblo, Colorado dating to 1879-1899. Isotopic ratios from healing bone fractures, cortical bone, and tooth dentine provide information about sources of Pb exposures over a range of time that illuminates individual's life histories and migration patterns. Historical records and Pb production data from the 19th century were used to create a database for interpreting Pb exposures for these African, Hispanic and European Americans. The analysis of these individuals suggests that Pb exposure noticeably impacted the mental health of 5-10% of the asylum patients in this frontier population, a high number by standards today, and that differences exist in the three ancestral groups' exposure histories.
Subject(s)
Environmental Exposure/history , Hospitals, Psychiatric , Lead/analysis , Mortuary Practice , Bone and Bones/chemistry , Colorado , History, 19th Century , Humans , Lead Poisoning/epidemiology , Mental Disorders/chemically induced , Tooth/chemistryABSTRACT
Particulate hexavalent chromium [Cr(VI)] compounds are well-established human lung carcinogens. However, their carcinogenic mechanisms are poorly understood as most investigators have used soluble Cr(VI) compounds. Recent work from our laboratory has found that barium chromate (BC) is also cytotoxic and clastogenic. To understand how BC relates to existing data on other particulate Cr(VI) compounds, we compared its cytotoxicity and clastogenicity with lead chromate (LC), which has been used as a prototypical particulate Cr(VI) compound, in WTHBF-6 cells, a near-normal human lung cell line. We found that BC is a more potent cytotoxicant, inducing 67%, 12%, 3%, and 0% relative survival at concentrations of 0.1, 0.5, 1, and 5 microg/cm2, respectively, while LC induced 90%, 71%, 43%, and 15% survival at these same concentrations. We found that BC was also more clastogenic, damaging 22% and 49% of metaphase cells at 0.1 and 0.5 microg/cm2, and causing complete cell cycle arrest at 1 and 5 microg/cm2. By contrast, 0.1, 0.5, and 1.0 microg/cm2 LC damaged 10%, 27%, and 37% of metaphase cells, respectively, and complete cell cycle arrest was not observed until a concentration of 5 microg/cm2 was reached. We found that BC and LC both partially dissolved in complete medium in the presence of cells, producing similar extracellular concentrations. Both compounds were also comparable with respect to particle uptake and the amount of intracellular Cr ions. Considering previous reports showing that lead ions were inactive and that sodium chromate and LC have similar clastogenic potencies, these data suggest that BC genotoxicity may not be solely mediated by Cr ions, but also involve some clastogenic activity of barium ions.
Subject(s)
Barium Compounds/toxicity , Chromates/toxicity , Lead/toxicity , Lung/drug effects , Mutagens/toxicity , Cell Line , Humans , Lung/cytology , Mutagenicity TestsABSTRACT
The (239+240)Pu activity profile is determined for a sediment core collected from 170-m depth at Loch Ness, Scotland. These measurements use magnetic sector inductively coupled plasma mass spectrometry for rapid determination of Pu activities and (240)Pu/(239)Pu atom ratios. A (239+240)Pu detection limit of 0.1 Bq/kg is obtained for 2 g of acid-leached sediment; (242)Pu is used as a spike isotope. The Pu activity profile exhibits a maximum of 42.7+/-0.3 Bq/kg (239+240)Pu in the 9-10-cm depth interval. The position of this maximum coincides with peaks in the (241)Am and (137)Cs activity profiles. These peak activities are ascribed to the 1963/1964 peak fallout from atmospheric testing of nuclear weapons. The (240)Pu/(239)Pu atom ratios are in the range 0.15-0.20, in agreement with the expected range of 0.166-0.194 for Northern Hemisphere fallout, and do not suggest the presence of other contributing sources. This study demonstrates that ICPMS has considerable potential for rapid determination of the chronology of post-1950 sediments, and also for validating (210)Pb dates where chronologies over longer time-scales are needed.