A study of the atmospheric dispersion of a high release of krypton-85 above a complex coastal terrain, comparison with the predictions of Gaussian models (Briggs, Doury, ADMS4)

Atmospheric releases of krypton-85, from the nuclear fuel reprocessing plant at the AREVA NC facility at La Hague (France), were used to test Gaussian models of dispersion. In 2001-2002, the French Institute for Radiological Protection and Nuclear Safety (IRSN) studied the atmospheric dispersion of 15 releases, using krypton-85 as a tracer for plumes emitted from two 100-m-high stacks. Krypton-85 is a chemically inert radionuclide. Krypton-85 air concentration measurements were performed on the ground in the downwind direction, at distances between 0.36 and 3.3 km from the release, by neutral or slightly unstable atmospheric conditions. The standard deviation for the horizontal dispersion of the plume and the Atmospheric Transfer Coefficient (ATC) were determined from these measurements. The experimental results were compared with calculations using first generation (Doury, Briggs) and second generation (ADMS 4.0) Gaussian models. The ADMS 4.0 model was used in two configurations; one takes account of the effect of the built-up area, and the other the effect of the roughness of the surface on the plume dispersion. Only the Briggs model correctly reproduced the measured values for the width of the plume, whereas the ADMS 4.0 model overestimated it and the Doury model underestimated it. The agreement of the models with measured values of the ATC varied according to distance from the release point. For distances less than 2 km from the release point, the ADMS 4.0 model achieved the best agreement between model and measurement; beyond this distance, the best agreement was achieved by the Briggs and Doury models.     

Dynamic modelling of atmospherically-deposited Ni, Cu, Zn, Cd and Pb in Pennine catchments (northern England)

Simulation modelling with CHUM-AM was carried out to investigate the accumulation and release of atmospherically-deposited heavy metals (Ni, Cu, Zn, Cd and Pb) in six moorland catchments, five with organic-rich soils, one with calcareous brown earths, in the Pennine chain of northern England. The model considers two soil layers and a third layer of weathering mineral matter, and operates on a yearly timestep, driven by deposition scenarios covering the period 1400-2010. The principal processes controlling heavy metals are competitive solid-solution partitioning of solutes, chemical interactions in solution, and chemical weathering. Agreement between observed and simulated soil metal pools and surface water concentrations for recent years was generally satisfactory, the results confirming that most contemporary soil metal is from atmospheric pollution. Metals in catchments with organic-rich soils show some mobility, especially under more acid conditions, but the calcareous mineral soils have retained nearly all anthropogenic metal inputs. Complexation by dissolved organic matter and co-transport accounts for up to 80% of the Cu in surface waters.     

One century sedimentary records of polycyclic aromatic hydrocarbons, mercury and trace elements in the Qinghai Lake, Tibetan Plateau

Sediments from a remote lake of northeastern Tibetan Plateau were analyzed for polycyclic aromatic hydrocarbons (PAHs) and trace metals. USEPA priority PAHs, ranged from 11 in 1860 to 279 ng g⁻¹ in 2002, while, the deposition fluxes were in the range of 0.2-11.4 ng cm⁻² yr⁻¹. Similarly, from 1860 to 2002, an increased trend of Hg flux was observed (0.5-3.2 ng cm⁻² yr⁻¹). Remarkable increase of PAHs and Hg concentration began from 1970, nearly the same period of the “Reform and Open” Policy had been embarked (1978) in China. Good correlations were found between concentrations of Pb, Zn, Cd, As, Hg, and PAHs, which suggested the sources of these chemicals in the sediment is analogous, likely from anthroprogenic sources. Based on isomer ratios, PAHs in core were dominantly from the incomplete combustion of coal. Owing to the proximity to dust source area (Qaidam Basin) and the close association between PAHs, Hg, Pb, and particle matters, atmospheric dust-transport and deposition might be the main pathways that pollutants enter into Qinghai Lake.     

Lead-210 and Beryllium-7 fallout rates on the southeastern coast of Brazil

Total ²¹⁰Pb and ⁷Be fallout rates were measured on the coastal region of Niteroi, Brazil. The monthly depositional flux of ²¹⁰Pb and ⁷Be varied by a factor of 26, from 1.7 to 43.3 mBq cm⁻² year⁻¹ and ∼27, from 7.5 to 203.5 mBq cm⁻² year⁻¹, respectively. The relatively large oscillations in the depositional flux of ²¹⁰Pb at this study site were likely due to variations in air mass sources, while the ⁷Be fluctuations may be driven by a combination of weather conditions. Local geology could support the periodic high fluxes of ²¹⁰Pb from continental air masses, as shifting oceanic wind sources were affirmed by the uncorrelated ²¹⁰Pb and ⁷Be fallout activities and ⁷Be/²¹⁰Pb ratios. The ²¹⁰Pb atmospheric deposition was found to be in agreement with local sediment inventories, an important consideration in geochemical studies that estimate sedimentation processes.     

Tritium concentrations in the atmospheric environment at Rokkasho, Japan before the final testing of the spent nuclear fuel reprocessing plant

This study aimed at obtaining background tritium concentrations in precipitation and air at Rokkasho where the first commercial spent nuclear fuel reprocessing plant in Japan has been under construction. Tritium concentration in monthly precipitation during fiscal years 2001-2005 had a seasonal variation pattern which was high in spring and low in summer. The tritium concentration was higher than that observed at Chiba City as a whole. The seasonal peak concentration at Rokkasho was generally higher than that at Chiba City, while the baseline concentrations of both were similar. The reason for the difference may be the effect of air mass from the Asian continent which is considered to have high tritium concentration. Atmospheric tritium was operationally separated into HTO, HT and hydrocarbon (CH₃T) fractions, and the samples collected every 3 d-14 d during fiscal year 2005 were analyzed for these fractions. The HTO concentration as radioactivity in water correlated well with that in the precipitation samples. The HT concentration was the highest among the chemical forms analyzed, followed by the HTO and CH₃T concentrations. The HT and CH₃T concentrations did not have clear seasonal variation patterns. The HT concentration followed the decline previously reported by Mason and Östlund with an apparent half-life of 4.8 y. The apparent and environmental half-lives of CH₃T were estimated as 9.2 y and 36.5 y, respectively, by combining the present data with literature data. The Intergovernmental Panel on Climate Change used the atmospheric lifetime of 12 y for CH₄ to estimate global warming in its 2007 report. The longer environmental half-life of CH₃T suggested its supply from other sources than past nuclear weapon testing in the atmosphere.     

Comparison of airborne and terrestrial gamma spectrometry measurements - evaluation of three areas in southern Sweden

The Geological Survey of Sweden (SGU) has been conducting airborne gamma spectrometry measurements of natural radioactivity in Sweden for more than 40 years. Today, the database covers about 80% of the country’s land surface. This article explores the first step of putting this data into use in radioactive source search at ground level. However, in order to be able to use the airborne background measurements at ground level, SGU data must be validated against terrestrial data. In this work, we compare the SGU data with data measured by a portable backpack system. This is done for three different areas in southern Sweden. The statistical analysis shows that a linear relationship and a positive correlation exist between the air and ground data. However, this linear relationship could be revealed only when the region possessed large enough variations in areal activity. Furthermore, the activity distributions measured show good agreement to those of SGU. We conclude that the SGU database could be used for terrestrial background assessment, given that a linear transfer function is established.     

PCDD/Fs atmospheric deposition fluxes and soil contamination close to a municipal solid waste incinerator

Bulk depositions and surface soil were collected in a suburban area, near the Adriatic Sea, in order to assess the contribution of a municipal solid waste incinerator to the area’s total contamination with polychlorinated dibenzodioxins and polychlorinated dibenzofurans (PCDDs and PCDFs). Samples were collected at two sites, situated in the area most affected by plant emissions (according to the results of the Calpuff air dispersion model), and at an external site, considered as a reference. Results show that the studied area is subject to low contamination, as far as these compounds are concerned. Deposition fluxes range from 14.3 pg m⁻² d⁻¹ to 89.9 pg m⁻² d⁻¹ (0.75 pg-TEQ m⁻² d⁻¹ to 3.73 pg-TEQ m⁻² d⁻¹) and no significant flow differences are observed among the three monitored sites. Total soil concentration amounts to 93.8 ng kg⁻¹ d.w. and 1.35 ng-TEQ kg⁻¹ d.w, on average, and confirms a strong homogeneity in the studied area. Furthermore, from 2006 to 2009, no PCDD/Fs enrichment in the soil was noticed. Comparing the relative congener distributions in environmental samples with those found in stack emissions from the incineration plant, significant differences are observed in the PCDD:PCDF ratio and in the contribution of the most chlorinated congeners. From this study we can conclude that the incineration plant is not the main source of PCDD/Fs in the studied area, which is apparently characterized by a homogeneous and widespread contamination situation, typical of an urban area.     

Carbon isotope signature of dissolved inorganic carbon (DIC) in precipitation and atmospheric CO2

This paper describes results of chemical and isotopic analysis of inorganic carbon species in the atmosphere and precipitation for the calendar year 2008 in Wroc?aw (SW Poland). Atmospheric air samples (collected weekly) and rainwater samples (collected after rain episodes) were analysed for CO₂ and dissolved inorganic carbon (DIC) concentrations and for δ¹³C composition. The values obtained varied in the ranges: atmospheric CO₂: 337-448 ppm; δ¹³C_CO2 from −14.4 to −8.4‰; DIC in precipitation: 0.6-5.5 mg dm⁻³; δ¹³C_DIC from −22.2 to +0.2‰. No statistical correlation was observed between the concentration and δ¹³C value of atmospheric CO₂ and DIC in precipitation. These observations contradict the commonly held assumption that atmospheric CO₂ controls the DIC in precipitation. We infer that DIC is generated in ambient air temperatures, but from other sources than the measured atmospheric CO₂. The calculated isotopic composition of a hypothetical CO₂ source for DIC forming ranges from −31.4 to −11.0‰, showing significant seasonal variations accordingly to changing anthropogenic impact and atmospheric mixing processes.     

Evaluation of surface runoff and road dust as sources of nitrogen using nitrate isotopic composition

Stable nitrogen and oxygen isotope ratios of nitrate (δ¹⁵N-NO₃ and δ¹⁸O-NO₃) have recently been used to identify nitrogen sources in water environments. However, there have been no investigations designed to determine nitrate isotopes in non-point sources in urban areas for evaluating the impact of surface deposits on nitrogen in surface runoff. In this study, we collected rainwater, surface runoff and surface deposits (road dust, roof dust and soil) to evaluate the nitrogen sources in surface runoff using nitrate isotopes. There were no large differences in δ¹⁵N-NO₃ among rainwater (−0.3‰ to 1.5‰), surface runoff (−2.7‰ to 0.4‰), leachates from road dust (−5.8‰ to 6.2‰) and soil (−11.5‰ to 0.6‰). In contrast, the δ¹⁸O-NO₃ in surface runoff (28.5-47.9‰) was lower than that in rainwater (62.7-78.6‰), and higher than that in leachates from road dust (6.1-27.6‰) and soil (−1.1‰ to 6.6‰). δ¹⁸O-NO₃ is a useful indicator for evaluating the NO₃-N sources in surface runoff. Using this indicator, NO₃-N from road dust was estimated to account for more than half of the NO₃-N in surface runoff. This is consistent with a result based on a comparison of their loads per unit surface between rainwater and surface runoff, which also showed that most of the nitrogen in surface runoff was derived from surface deposits.     

The oxidation mechanism of polychlorinated dibenzo-p-dioxins under the atmospheric conditions - A theoretical study

The atmospheric polychlorinated dibenzo-p-dioxins (PCDDs) partition appreciably in the gas phase, where they undergo rapid oxidation. The atmospheric oxidation mechanisms of a few PCDDs, initiated by OH radical, are studied using density functional theory calculations. The oxidations start with OH-addition to the aromatic rings, dominantly at γ-sites, followed by the non-chlorinated β-sites; while additions to the α-sites or chlorinated sites are negligible. For PCDDs with all β-sites being chlorinated, formation of PCDD-γ-OH adducts become virtually the only reaction path. Under the atmospheric conditions, the PCDD-β/γ-OH adducts combine with O₂ slowly at rates <1 s⁻¹. Instead, the PCDD-β-OH adducts will react with O₂ through hydrogen abstraction at rates <50 s⁻¹, forming PCDD-β-ol, and the PCDD-γ-OH adducts will decompose to the substituted phenoxy radicals by fused-ring C-O bond cleavage at rates of 10³ ∼ 10⁵ s⁻¹. The reaction mechanisms of PCDDs are drastically different from the peroxy mechanism for the atmospheric oxidations of benzene and dibenzofuran.