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1.
J Environ Radioact ; 243: 106796, 2022 Mar.
Article in English | MEDLINE | ID: mdl-34933215

ABSTRACT

The chemical and isotopic compositions of fallout melt glasses from nuclear tests contain a range of information constraining the physical conditions within the fireball and the mechanisms of fallout formation but historic studies tended to exclude the behavior of stable major and trace elements. Here, we present a large study specifically focused on major and trace element relationships within a population of macroscale fallout samples from a single event. We interpret these data to better constrain how fallout melt glass formation in near surface environments is influenced by that environment and demonstrate how major and trace element abundances can provide useful insights into chemical processes within the fireball. Data confirm that the uranium in the fallout glass population derives from two isotopically distinct endmembers: isotopically enriched uranium (presumably from the weapon), and natural composition uranium that may be a combination of anthropogenic and environmental materials from within the blast zone. The similarity between major and trace element concentrations in fallout and corresponding local soils from the event site confirm the local soils as the most probable source of entrained material into the fireball and the source of carrier material into which the bomb vapor was incorporated. The lack of correlation between major and trace element abundances with size indicates that volatility driven processes, such as condensation from the fireball, do not control the composition of macroscale fallout melt glass. Although the fallout has major and trace element chemical characteristics broadly similar to those of the local, associated soils, some systematic differences are observed between the two populations. Fallout melt glass is depleted in volatile elements such as K, Na, Tl and Pb, consistent with heating to temperatures above ∼1000 °C for 3-10 s. This is supported by the results of laser heating experiments performed on rhyolitic soil at temperatures (1600-2200 °C) and timescales (1-120 s) that are broadly relevant to fallout formation conditions. Relative enrichments of metals such as Cu and Co do not correlate with the abundance of uranium, suggesting that fallout also records input of near field anthropogenic materials. Our observations suggest that major chemical features can be related to processing in the fireball and used to inform the thermal-chemical evolution of the system. Ultimately, these data are consistent with a fallout formation mechanism that involves rapid melting of surface materials to form carrier material melts with minor incorporation of bomb vapor and a degree of volumetric volatile loss due to heating.


Subject(s)
Radiation Monitoring , Trace Elements , Uranium , Environmental Monitoring , Soil , Trace Elements/analysis , Uranium/analysis
2.
Sci Total Environ ; 437: 373-83, 2012 Oct 15.
Article in English | MEDLINE | ID: mdl-22960112

ABSTRACT

Beryllium has been historically machined, handled and stored in facilities at Lawrence Livermore National Laboratory (LLNL) since the 1950s. Additionally, outdoor testing of beryllium-containing components has been performed at LLNL's Site 300 facility. Beryllium levels in local soils and atmospheric particulates have been measured over three decades and are comparable to those found elsewhere in the natural environment. While localized areas of beryllium contamination have been identified, laboratory operations do not appear to have increased the concentration of beryllium in local air or water. Variation in airborne beryllium correlates to local weather patterns, PM10 levels, normal sources (such as resuspension of soil and emissions from coal power stations) but not to LLNL activities. Regional and national atmospheric beryllium levels have decreased since the implementation of the EPA's 1990 Clean-Air-Act. Multi-element analysis of local soil and air samples allowed for the determination of comparative ratios for beryllium with over 50 other metals to distinguish between natural beryllium and process-induced contamination. Ten comparative elemental markers (Al, Cs, Eu, Gd, La, Nd, Pr, Sm, Th and Tl) that were selected to ensure background variations in other metals did not collectively interfere with the determination of beryllium sources in work-place samples at LLNL. Multi-element analysis and comparative evaluation are recommended for all workplace and environmental samples suspected of beryllium contamination. The multi-element analyses of soils and surface dusts were helpful in differentiating between beryllium of environmental origin and beryllium from laboratory operations. Some surfaces can act as "sinks" for particulate matter, including carpet, which retains entrained insoluble material even after liquid based cleaning. At LLNL, most facility carpets had beryllium concentrations at or below the upper tolerance limit determined by sampling facilities with no history of beryllium work. Some facility carpets had beryllium concentrations above the upper tolerance limits but can be attributed to tracking of local soils, while other facilities showed process-induced contamination from adjacent operations. In selected cases, distinctions were made as to the source of beryllium in carpets. Guidance on the determination of facility beryllium sources is given.


Subject(s)
Beryllium/analysis , Particulate Matter/analysis , Soil/analysis , Air Filters/history , Air Pollutants/analysis , Air Pollutants/history , Air Pollutants, Occupational/analysis , Air Pollutants, Occupational/history , Beryllium/history , Environmental Monitoring/history , Floors and Floorcoverings/history , History, 20th Century , History, 21st Century , Metals, Heavy/analysis , Metals, Heavy/history , Particulate Matter/history , Water Pollutants, Chemical/analysis , Water Pollutants, Chemical/history
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