Radionuclides in soils, 1960–2006: A view from the World Congress of Soil Science
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Fate of radium (Ra) in liquid regeneration brine wastes from water softeners disposed to septic tanks in the New Jersey Coastal Plain was studied. Before treatment, combined Ra ( 226 Ra plus 228 Ra) concentrations (maximum, 1.54 Bq L −1 ) exceeded the 0.185 Bq L −1 Maximum Contaminant Level in 4 of 10 studied domestic-well waters (median pH, 4.90). At the water table downgradient from leachfields, combined Ra concentrations were low (commonly ≤0.019 Bq L −1 ) when pH was >5.3, indicating sequestration; when pH was ≤5.3 (acidic), concentrations were elevated (maximum, 0.985 Bq L −1 – greater than concentrations in corresponding discharged septic-tank effluents (maximum, 0.243 Bq L −1 )), indicating Ra mobilization from leachfield sediments. Confidence in quantification of Ra mass balance was reduced by study design limitations, including synoptic sampling of effluents and ground waters, and large uncertainties associated with analytical methods. The trend of Ra mobilization in acidic environments does match observations from regional water-quality assessments.
Beryllium-7 is a powerful and commonly used tracer for environmental processes such as watershed sediment provenance, soil erosion, fluvial and nearshore sediment cycling, and atmospheric fallout. However, few studies have quantified temporal or spatial variability of 7 Be accumulation from atmospheric fallout, and parameters that would better define the uses and limitations of this geochemical tracer. We investigated the abundance and variability of 7 Be in atmospheric deposition in both rain events and dry periods, and in stream surface-water samples collected over a ten-month interval at sites near northern Monterey Bay (37°N, 122°W) on the central California coast, a region characterized by a rainy winters, dry summers, and small mountainous streams with flashy hydrology. The range of 7 Be activity in rainwater samples from the main sampling site was 1.3–4.4 Bq L −1 , with a mean (±standard deviation) of 2.2 ± 0.9 Bq L −1 , and a volume-weighted average of 2.0 Bq L −1 . The range of wet atmospheric deposition was 18–188 Bq m −2 per rain event, with a mean of 72 ± 53 Bq m −2 . Dry deposition fluxes of 7 Be ranged from less than 0.01 up to 0.45 Bq m −2 d −1 , with an estimated dry season deposition of 7 Bq m −2 month −1 . Annualized 7 Be atmospheric deposition was approximately 1900 Bq m −2 yr −1 , with most deposition via rainwater (>95%) and little via dry deposition. Overall, these activities and deposition fluxes are similar to values found in other coastal locations with comparable latitude and Mediterranean-type climate. Particulate 7 Be values in the surface water of the San Lorenzo River in Santa Cruz, California, ranged from <0.01 Bq g −1 to 0.6 Bq g −1 , with a median activity of 0.26 Bq g −1 . A large storm event in January 2010 characterized by prolonged flooding resulted in the entrainment of 7 Be-depleted sediment, presumably from substantial erosion in the watershed. There were too few particulate 7 Be data over the storm to accurately model a 7 Be load, but the results suggest enhanced watershed export of 7 Be from small, mountainous river systems compared to other watershed types.
The long-lived radionuclide 129 I (half-life: 15.7 × 10 6 yr) is well-known as a useful environmental tracer. At present, the global 129 I in surface water is about 1–2 orders of magnitude higher than pre-1960 levels. Since the 1990s, anthropogenic 129 I produced from industrial nuclear fuels reprocessing plants has been the primary source of 129 I in marine surface waters of the Atlantic and around the globe. Here we present four coral 129 I time series records from: 1) Con Dao and 2) Xisha Islands, the South China Sea, 3) Rabaul, Papua New Guinea and 4) Guam. The Con Dao coral 129 I record features a sudden increase in 129 I in 1959. The Xisha coral shows similar peak values for 129 I as the Con Dao coral, punctuated by distinct low values, likely due to the upwelling in the central South China Sea. The Rabaul coral features much more gradual 129 I increases in the 1970s, similar to a published record from the Solomon Islands. The Guam coral 129 I record contains the largest measured values for any site, with two large peaks, in 1955 and 1959. Nuclear weapons testing was the primary 129 I source in the Western Pacific in the latter part of the 20th Century, notably from testing in the Marshall Islands. The Guam 1955 peak and Con Dao 1959 increases are likely from the 1954 Castle Bravo test, and the Operation Hardtack I test is the most likely source of the 1959 peak observed at Guam. Radiogenic iodine found in coral was carried primarily through surface ocean currents. The coral 129 I time series data provide a broad picture of the surface distribution and depth penetration of 129 I in the Pacific Ocean over the past 60 years.
Understanding iodine concentration, transport, and bioavailability is essential in evaluating iodine's impact to the environment and its effectiveness as an environmental biogeotracer. While iodine and its radionuclides have proven to be important tracers in geologic and biologic studies, little is known about transport of this element to the deep sea and subsequent uptake in deep-sea coral habitats. Results presented here on deep-sea black coral iodine speciation and iodine isotope variability provides key information on iodine behavior in natural and anthropogenic environments, and its geochemical pathway in the Gulf of Mexico. Organo-iodine is the dominant iodine species in the black corals, demonstrating that binding of iodine to organic matter plays an important role in the transport and transfer of iodine to the deep-sea corals. The identification of growth bands captured in high-resolution scanning electron images (SEM) with synchronous peaks in iodine variability suggest that riverine delivery of terrestrial-derived organo-iodine is the most plausible explanation to account for annual periodicity in the deep-sea coral geochemistry. Whereas previous studies have suggested the presence of annual growth rings in deep-sea corals, this present study provides a mechanism to explain the formation of annual growth bands. Furthermore, deep-sea coral ages based on iodine peak counts agree well with those ages derived from radiocarbon ( 14 C) measurements. These results hold promise for developing chronologies independent of 14 C dating, which is an essential component in constraining reservoir ages and using radiocarbon as a tracer of ocean circulation. Furthermore, the presence of enriched 129 I/ 127 I ratios during the most recent period of skeleton growth is linked to nuclear weapons testing during the 1960s. The sensitivity of the coral skeleton to record changes in surface water 129 I composition provides further evidence that iodine composition and isotope variability captured in proteinaceous deep-sea corals is a promising geochronometer as well as an emerging tracer for continental material flux.
Radon (Rnair) was monitored in open air in publicly accessible areas surrounding the Pinenut uranium (U) mine during mining and reclamation activities in 2015–16 to address concerns about mining related effects to areas surrounding Grand Canyon National Park (GCNP) in Arizona, USA. During July 2015, Rnair concentrations associated with the ore storage pile monitoring site were larger than those at the mine vent monitoring site and likely resulted from the relatively large amount of ore stored on site during this period. Higher wind velocities at the ore pile monitoring site generally resulted in lower Rnair concentrations; however, wind velocity did not appear to be an important factor in controlling Rnair concentrations at the mine vent monitoring site. Physical disturbances of the ore pile by heavy equipment did not coincide with elevated Rnair concentrations at the ore storage pile or mine vent monitoring sites. The relative size of the ore storage pile showed a positive trend with the daily mean Rnair concentration measured at the ore pile monitoring site. Principal component analysis (PCA) was applied to the ore pile and mine vent multivariate data sets for simultaneous comparison of all measured variables during 230 days of the study period. A significant positive coefficient for Rnair was associated with a significant negative coefficient for wind speed for principal component (PC) 2ore pile. Significant, positive PC2mine vent coefficients included Rnair, wind direction, and relative ore pile size indicating that Rnair variations at the mine vent monitoring site may be affected by Rn sourced from the ore pile. The ore pile is located about 200 m south of the mine vent Rn monitor with the prevalent wind direction coming from the south. All data generated during the field study and laboratory verification tests were published by Naftz et al. (2018) and are available online at:
Field measurements of Rn-222 fluxes from the tops and bottoms of compacted clay radon barriers were used to calculate effective Rn diffusion coefficients (D Rn ) at four uranium waste disposal sites in the western United States to assess cover performance after more than 20 years of service. Values of D Rn ranged from 7.4 × 10 −7 to 6.0 × 10 −9 m 2 /s, averaging 1.42 × 10 −7 . Water saturation (S W ) from soil cores indicated that there was relatively little control of D Rn by S W , especially at higher moisture levels, in contrast to estimates from most steady-state diffusion models. This is attributed to preferential pathways intrinsic to construction of the barriers or to natural process that have developed over time including desiccation cracks, root channels, and insect burrows in the engineered earthen barriers. A modification to some models in which fast and slow pathway D Rn values are partitioned appears to give a good representation of the data; 4% of the fast pathway was needed to fit the data regression. For locations with high S w and highest D Rn (and fluxes) at each site, the proportion of fast pathway ranged from 1.7% to 34%, but for many locations with lower fluxes, little if any fast pathway was needed.
Problems of underground storage of waste involve geology in its broadest sense, including hydrology, geochemistry, and geophysics. Wastes may be solid, liquid, or gaseous, and they may be chemically toxic or noxious, esthetically offensive, or radioactive. Some wastes require only temporary containment, whereas others must be isolated for indefinitely long periods. The means and locale for emplacement underground depend upon many governing geological factors, including the physical, chemical, hydrological, and hydraulic properties of the host formation. These must be studied relative to the physical, chemical, and thermal properties of the waste and of potential interactions between the waste and the host formation. Thorough knowledge is essential because lack of it may lead to undesirable or disastrous environmental consequences. Escape of waste may contaminate the surface or near-surface environment; it may destroy the usefulness or accessibility of resources such as ground water, petroleum, and minerals. Effective management of underground waste requires adaptation of current technology and development of new technology.
Radioactive hot springs issue from a fault zone in crystalline rock of the Boulder batholith at Alhambra, Jefferson County, in southwestern Montana. The discharge contains high concentrations of radon, and the gross alpha activity and the concentration of adium-226 exceed maximum levels recommended by the Environmental Protection Agency for drinking water. Part of the discharge is diverted for space heating, bathing, and domestic use. The radioactive thermal waters at measured temperatures of about 60°C are of the sodium bicarbonate type and saturated with respect to calcium carbonate. Radium-226 in the rock and on fractured surfaces or coprecipitated with calcium carbonate probably is the principal source of radon that is dissolved in the thermal water and discharged with other gases from some wells and springs. Local surface water and shallow ground water are of the calcium bicarbonate type and exhibit low background activity. The temperature, percent sodium, and radioactivity of mixed waters adjacent to the fault zone increase with depth. Samples from most of the major hot springs in southwestern Montana have been analyzed for gross alpha and beta activity. The high level of radioactivity at Alhambra appears to be related to leaching of radioactive material from siliceous veins by ascending thermal waters and is not a normal characteristic of hot springs issuing from fractured crystalline rock in Montana.
To investigate possible long-range flow paths through the interbedded basalts and sediments of a 200-m-thick unsaturated zone, we applied a chemical tracer to seasonally filled infiltration ponds on the Snake River Plain in Idaho. This site is near the Subsurface Disposal Area for radioactive and other hazardous waste at the Idaho National Engineering and Environmental Laboratory. Within 4 mo, we detected tracer in one of 13 sampled aquifer wells, and in eight of 11 sampled perched-water wells as far as 1.3 km away. These detections show that (i) low-permeability layers in the unsaturated zone divert some flow horizontally, but do not prevent rapid transport to the aquifer; (ii) horizontal convective transport rates within the unsaturated zone may exceed 14 m d −1 , perhaps through essentially saturated basalt fractures, tension cracks, lava tubes, or rubble zones; and (iii) some perched water beneath the Subsurface Disposal Area derives from episodic surface water more than 1 km away. Such rapid and far-reaching flow may be common throughout the Snake River Plain, and possibly occurs in other locations that have a geologically complex unsaturated zone and comparable sources of infiltrating water.
Multiphase, multicomponent numerical models of long-term unsaturated-zone liquid and vapor movement were created for a thick alluvial basin at the Nevada Test Site to predict present-day liquid and vapor fluxes. The numerical models are based on recently developed conceptual models of unsaturated-zone moisture movement in thick alluvium that explain present-day water potential and tracer profiles in terms of major climate and vegetation transitions that have occurred during the past 10 000 yr or more. The numerical models were calibrated using borehole hydrologic and environmental tracer data available from a low-level radioactive waste management site located in a former nuclear weapons testing area. The environmental tracer data used in the model calibration includes tracers that migrate in both the liquid and vapor phases (δD, δ 18 O) and tracers that migrate solely as dissolved solutes (Cl), thus enabling the estimation of some gas-phase as well as liquid-phase transport parameters. Parameter uncertainties and correlations identified during model calibration were used to generate parameter combinations for a set of Monte Carlo simulations to more fully characterize the uncertainty in liquid and vapor fluxes. The calculated background liquid and vapor fluxes decrease as the estimated time since the transition to the present-day arid climate increases. However, on the whole, the estimated fluxes display relatively little variability because correlations among parameters tend to create parameter sets for which changes in some parameters offset the effects of others in the set. Independent estimates on the timing since the climate transition established from packrat midden data were essential for constraining the model calibration results. The study demonstrates the utility of environmental tracer data in developing numerical models of liquid- and gas-phase moisture movement and the importance of considering parameter correlations when using Monte Carlo analysis to characterize the uncertainty in moisture fluxes.
Cost-effective methods are needed to identify the presence and distribution of tritium near radioactive waste disposal and other contaminated sites. The objectives of this study were to (i) develop a simplified sample preparation method for determining tritium contamination in plants and (ii) determine if plant data could be used as an indicator of soil contamination. The method entailed collection and solar distillation of plant water from foliage, followed by filtration and adsorption of scintillation-interfering constituents on a graphite-based solid phase extraction (SPE) column. The method was evaluated using samples of creosote bush [ Larrea tridentata (Sessé & Moc. ex DC.) Coville], an evergreen shrub, near a radioactive disposal area in the Mojave Desert. Laboratory tests showed that a 2-g SPE column was necessary and sufficient for accurate determination of known tritium concentrations in plant water. Comparisons of tritium concentrations in plant water determined with the solar distillation–SPE method and the standard (and more laborious) toluene-extraction method showed no significant difference between methods. Tritium concentrations in plant water and in water vapor of root-zone soil also showed no significant difference between methods. Thus, the solar distillation–SPE method provides a simple and cost-effective way to identify plant and soil contamination. The method is of sufficient accuracy to facilitate collection of plume-scale data and optimize placement of more sophisticated (and costly) monitoring equipment at contaminated sites. Although work to date has focused on one desert plant, the approach may be transferable to other species and environments after site-specific experiments.
Volatile organic compounds (VOCs) are often comingled with low-level radioactive wastes (LLRW), but little is known about subsurface VOC emanations from LLRW landfills. The current study systematically quantified VOCs associated with LLRW over an 11-yr period at the USGS Amargosa Desert Research Site (ADRS) in southwestern Nevada. Unsaturated-zone gas samples of VOCs were collected by adsorption on resin cartridges and analyzed by thermal desorption and GC/MS. Sixty of 87 VOC method analytes were detected in the 110-m-thick unsaturated zone surrounding a LLRW disposal facility. Chlorofluorocarbons (CFCs) were detected in 100% of samples collected. Chlorofluorocarbons are powerful greenhouse gases, deplete stratospheric ozone, and are likely released from LLRW facilities worldwide. Soil-gas samples collected from a depth of 24 m and a horizontal distance 100 m south of the nearest waste-disposal trench contained >60,000 ppbv total VOCs, including >37,000 ppbv CFCs. Extensive sampling in the shallow unsaturated zone (0–2 m deep) identified areas where total VOC concentrations exceeded 5000 ppbv at the 1.5-m depth. Volatile organic compound concentrations exceeded background levels up to 300 m from the facility. Maximum vertical diffusive fluxes of total VOCs were estimated to be 1 g m -2 yr -1 . Volatile organic compound distributions were similar but not identical to those previously determined for tritium and elemental mercury. To our knowledge, this study is the first to characterize the unsaturated zone distribution of VOCs emanating from a LLRW landfill. Our results may help explain anomalous transport of radionuclides at the ADRS and elsewhere.
The US Department of Energy is pursuing Yucca Mountain, Nevada, for the development of a geologic repository for the disposal of spent nuclear fuel and high-level radioactive waste, if the repository is able to meet applicable radiation protection standards established by the US Nuclear Regulatory Commission and the US Environmental Protection Agency (EPA). Effective performance of such a repository would rely on a number of natural and engineered barriers to isolate radioactive waste from the accessible environment. Groundwater beneath Yucca Mountain is the primary medium through which most radionuclides might move away from the potential repository. The saturated zone (SZ) system is expected to act as a natural barrier to this possible movement of radionuclides both by delaying their transport and by reducing their concentration before they reach the accessible environment. Information obtained from Yucca Mountain Site Characterization Project activities is used to estimate groundwater flow rates through the site-scale SZ flow and transport model area and to constrain general conceptual models of groundwater flow in the site-scale area. The site-scale conceptual model is a synthesis of what is known about flow and transport processes at the scale required for total system performance assessment of the site. This knowledge builds on and is consistent with knowledge that has accumulated at the regional scale but is more detailed because more data are available at the site-scale level. The mathematical basis of the site-scale model and the associated numerical approaches are designed to assist in quantifying the uncertainty in the permeability of rocks in the geologic framework model and to represent accurately the flow and transport processes included in the site-scale conceptual model. Confidence in the results of the mathematical model was obtained by comparing calculated to observed hydraulic heads, estimated to measured permeabilities, and lateral flow rates calculated by the site-scale model to those calculated by the regional-scale flow model. In addition, it was confirmed that the flow paths leaving the region of the potential repository are consistent with those inferred from gradients of measured head and those independently inferred from water-chemistry data. The general approach of the site-scale SZ flow and transport model analysis is to calculate unit breakthrough curves for radionuclides at the interface between the SZ and the biosphere using the three-dimensional site-scale SZ flow and transport model. Uncertainties are explicitly incorporated into the site-scale SZ flow and transport abstractions through key parameters and conceptual models. ?? 2002 Elsevier Science B.V. All rights reserved.