Bomb 137Cs in modern honey reveals a regional soil control on pollutant cycling by plants.

137Cs is a long-lived (30-year radioactive half-life) fission product dispersed globally by mid-20th century atmospheric nuclear weapons testing. Here we show that vegetation thousands of kilometers from testing sites continues to cycle 137Cs because it mimics potassium, and consequently, bees magnify this radionuclide in honey. There were no atmospheric weapons tests in the eastern United States, but most honey here has detectable 137Cs at >0.03 Bq kg-1, and in the southeastern U.S., activities can be >500 times higher. By measuring honey, we show regional patterns in the biogeochemical cycling of 137Cs and conclude that plants and animals receive disproportionally high exposure to ionizing radiation from 137Cs in low potassium soils. In several cases, the presence of 137Cs more than doubled the ionizing radiation from gamma and x-rays in the honey, indicating that despite its radioactive half-life, the environmental legacy of regional 137Cs pollution can persist for more than six decades.

Accuracy of methods for reporting inorganic element concentrations and radioactivity in oil and gas wastewaters from the Appalachian Basin, U.S. based on an inter-laboratory comparison.

Accurate and precise analyses of oil and gas (O&G) wastewaters and solids (e.g., sediments and sludge) are important for the regulatory monitoring of O&G development and tracing potential O&G contamination in the environment. In this study, 15 laboratories participated in an inter-laboratory comparison on the chemical characterization of three O&G wastewaters from the Appalachian Basin and four solids impacted by O&G development, with the goal of evaluating the quality of data and the accuracy of measurements for various analytes of concern. Using a variety of different methods, analytes in the wastewaters with high concentrations (i.e., >5 mg L-1) were easily detectable with relatively high accuracy, often within ±10% of the most probable value (MPV). In contrast, often less than 7 of the 15 labs were able to report detectable trace metal(loid) concentrations (i.e., Cr, Ni, Cu, Zn, As, and Pb) with accuracies of approximately ±40%. Despite most labs using inductively coupled plasma mass spectrometry (ICP-MS) with low instrument detection capabilities for trace metal analyses, large dilution factors during sample preparation and low trace metal concentrations in the wastewaters limited the number of quantifiable determinations and likely influenced analytical accuracy. In contrast, all the labs measuring Ra in the wastewaters were able to report detectable concentrations using a variety of methods including gamma spectroscopy and wet chemical approaches following Environmental Protection Agency (EPA) standard methods. However, the reported radium activities were often greater than ±30% different to the MPV possibly due to calibration inconsistencies among labs, radon leakage, or failing to correct for self-attenuation. Reported radium activities in solid materials had less variability (±20% from MPV) but accuracy could likely be improved by using certified radium standards and accounting for self-attenuation that results from matrix interferences or a density difference between the calibration standard and the unknown sample. This inter-laboratory comparison illustrates that numerous methods can be used to measure major cation, minor cation, and anion concentrations in O&G wastewaters with relatively high accuracy while trace metal(loid) and radioactivity analyses in liquids may often be over ±20% different from the MPV.

Forest floor lead, copper and zinc concentrations across the northeastern United States: synthesizing spatial and temporal responses.

Understanding how metal concentrations in soil have responded to reductions of anthropogenic emissions is essential for predicting potential ecosystem impacts and evaluating the effectiveness of pollution control legislation. The objectives of this study were to present new data and synthesize existing literature to document decreases in Pb, Cu, and Zn concentrations in forest soils across the northeastern US. From measurements at 16 sites, we observed that forest floor Pb, Cu, and Zn concentrations have decreased between 1980 and 2011 at an overall mean rate of 1.3 ± 0.5% yr(-1). E-folding times, a concentration exponential decay rate (1/k), for Pb, Cu and Zn at the 16 sites were estimated to be 46 ± 7, 76 ± 20 and 81 ± 19 yr, respectively. Mineral soil concentrations were correlated with forest floor concentrations for Pb, but not for Cu and Zn, suggesting an accumulation in one pool does not strongly influence accumulation in the other. Forest floor Pb, Cu and Zn concentrations from our sites and 17 other studies conducted from 1970-2014 in remote forests across the northeastern US were compiled into pooled data sets. Significant decreasing trends existed for pooled forest floor Pb, Cu, and Zn concentrations. The pooled forest floor Pb e-folding time was determined to be 33 ± 9 yrs, but the explanatory power of pooled Cu and Zn regressions were inadequate for calculating e-folding times (r(2)<0.25). Pooled Pb, Cu, and Zn concentrations in forest floor were multiple-regressed with latitude, longitude, elevation, and year of sampling, cumulatively explaining 55, 38, and 28% of the variation across compiled studies. Our study suggests anthropogenic Pb in the forest floor will continue to decrease, but decreases in forest floor Cu and Zn concentrations may be masked by spatial heterogeneity or are at a new steady state.

Forest Floor Lead Changes from 1980 to 2011 and Subsequent Accumulation in the Mineral Soil across the Northeastern United States.

Quantifying the transport rate of anthropogenic lead (Pb) in forest soils is essential for predicting air pollution impacts on northeastern United States soil quality. In 2011, we resampled the forest floor at 16 sites across the northeastern United States previously sampled in 1980, 1990, and 2002 and also sampled the upper two mineral soil horizons. The mean forest floor Pb concentration decreased from 151 ± 29 mg kg in 1980 to 68 ± 13 mg kg in 2011. However, the mean forest floor Pb amount per unit area remained similar (10 ± 2 kg ha in 1980 and 11 ± 4 kg ha in 2011). Study sites were divided into three geographic regions: western, central, and northern. The modeled forest floor Pb response time (1/) was longer at frigid soil temperature regime sites (61 ± 15 yr) compared with mesic sites (29 ± 4 yr). Mineral soil Pb concentration and amount were approximately four times greater at western and central sites compared with northern sites for both mineral horizons. Furthermore, mean isotope ratios of Pb/Pb (1.201 ± 0.006) and Pb/Pb (2.060 ± 0.021) indicated that Pb in the western and central forest floor and mineral soil was primarily gasoline derived. Our combined analytical approach using long-term forest floor monitoring and stable Pb isotopes suggest that the majority of anthropogenic Pb deposited on soils in the western and central sites has been transported to the mineral soil, whereas it continues to reside in the forest floor at northern sites.