Redistribution of uranium by physical processes during weathering and implications for radon production

Erosion of the Edale shales of Derbyshire during the Tertiary and Quaternary has resulted in sediment deposits in and on the underlying karstified limestones. Sorting during sedimentation has generated clay-rich sediments which are uranium enriched due to a clay association of uranium in the shales. Radon production in these sediments is at or close to equilibrium with their uranium content, and their fine grain-size ensures efficient radon release. Such sediments are therefore potent local sources of environmental radon.     

Lateral or along-shore distribution of the polychaetous annelids of an intertidal,sandy habitat

The lateral or along-shore distribution of the polychaetous annelids of a subtropical, sandy, intertidal habitat in Florida (USA) was studied on three transects (covering 2.5 km of shoreline), sampled quarterly for 2 years. Although the average species number and density of individuals were not significantly different at specific tidal levels, the species composition was highly variable over time. Composition of density dominants was identical along-shore, and down-shore density distribution of selected species was also identical. Analysis by entire transects rather than by individual stations decreased along-shore heterogeneity by 10 to 15%.     

A preliminary study of the phycological degradation of natural stone masonry

For many years it has been realised that the weathering of stone is not merely determined by physical and chemical factors but also by biological agents. When the stone in question is a historic building or monument, the damage done constitutes an irretrievable loss of our heritage and history. Laboratory studies have commenced in Paisley to study the effect of photoautotrophs on the major sedimentary rock forming minerals, with a view to expanding this work to study the overall effect of these micro-organisms on heritage masonry. Tests were carried out on Albite, Calcite, Dolomite, Orthoclase, Siderite and Quartz, using axenic cultures of the following: Chlorella vulgaris, Chlorococcum tetrasporum, Scenedesmus obliquus, Oocystis marsonii, Stichococcus bacillaris. The rock chips were immersed in either water or bolds basal media and exposed to a mix of the micro-organisms listed above and then tested weekly for their pH, fortnightly for the waters chemical composition using inductively coupled plasma-atomic emission spectrometry (ICP-AES) and visually utilising the universitys SEM facilities. Work so far has revealed biologically mediated etching of minerals, a well-defined pH profile over a period of 90 days, as well as a variety of elemental release patterns for the different minerals.     

Removal of NOM from drinking water: Fenton's and photo-Fenton's processes

The control of disinfection by-products during water treatment is primarily undertaken by reducing the levels of precursor species prior to chlorination. As many waters contain natural organic matter at levels of up to 15 mgl(-1) there is a need for a range of control methods to support conventional coagulation. Two such processes are the Fenton and photo-Fenton's processes and in this paper they are assessed for their potential to remove NOM from organic rich waters. The performance of both processes is shown to be depentent on pH, Fe: H2O2 ratio as well as Fe2+ dose. Under optimum conditions both processes achieved greater than 90% removal of DOC and UV254 absorbance. This removal lead to the trihalomethane formation potential of the water being reduced from 140 to below 10 microgl(-1), well below UK and US standards.     

Hydrochemical and isotopic effects associated with petroleum fuel biodegradation pathways in a chalk aquifer

Hydrochemical data, compound specific carbon isotope analysis and isotopic enrichment trends in dissolved hydrocarbons and residual electron acceptors have been used to deduce BTEX and MTBE degradation pathways in a fractured chalk aquifer. BTEX compounds are mineralised sequentially within specific redox environments, with changes in electron acceptor utilisation being defined by the exhaustion of specific BTEX components. A zone of oxygen and nitrate exhaustion extends approximately 100 m downstream from the plume source, with residual sulphate, toluene, ethylbenzene and xylene. Within this zone complete removal of the TEX components occurs by bacterial sulphate reduction, with sulphur and oxygen isotopic enrichment of residual sulphate (epsilon(s) = -14.4 per thousand to -16.0 per thousand). Towards the plume margins and at greater distance along the plume flow path nitrate concentrations increase with delta15N values of up to +40 per thousand indicating extensive denitrification. Benzene and MTBE persist into the denitrification zone, with carbon isotope enrichment of benzene indicating biodegradation along the flow path. A Rayleigh kinetic isotope enrichment model for 13C-enrichment of residual benzene gives an apparent epsilon value of -0.66 per thousand. MTBE shows no significant isotopic enrichment (delta13C = -29.3 per thousand to -30.7 per thousand) and is isotopically similar to a refinery sample (delta13C = -30.1 per thousand). No significant isotopic variation in dissolved MTBE implies that either the magnitude of any biodegradation-induced isotopic fractionation is small, or that relatively little degradation has taken place in the presence of BTEX hydrocarbons. It is possible, however, that MTBE degradation occurs under aerobic conditions in the absence of BTEX since no groundwater samples were taken with co-existing MTBE and oxygen. Low benzene delta13C values are correlated with high sulphate delta34S, indicating that little benzene degradation has occurred in the sulphate reduction zone. Benzene degradation may be associated with denitrification since increased benzene delta13C is associated with increased delta15N in residual nitrate. Re-supply of electron acceptors by diffusion from the matrix into fractures and dispersive mixing is an important constraint on degradation rates and natural attenuation capacity in this dual-porosity aquifer.     

Persistent organochlorines in beluga whales (Delphinapterus leucas) from the St Lawrence River estuary--I. Concentrations and patterns of specific PCBs, chlorinated pesticides and polychlorinated dibenzo-p-dioxins and dibenzofurans

Blubber samples from beluga whales (Delphinapterus leucas) in the St Lawrence River estuary were analysed for PCB congeners (ortho- and non-ortho-substituted) and other persistent organochlorines as well as chlorinated dibenzo-dioxins/furans (PCDD/Fs). Major individual components (mean concentrations > 1 microg g(-1)) were 4,4'-DDE, -DDD and -DDT, T12 (a toxaphene-related compound), trans-nonachlor, oxychlordane, mirex, HCB, tris(p-chlorophenyl) methane and dieldrin. Concentrations of SigmaPCBs (8.3-412 microg g(-1)), SigmaDDT (3.36-389 microg g(-1)) and mirex (0.18-6.8 microg g(-1)) were particularly elevated relative to other odontocetes in Canadian waters. SigmaDDT, PCBs (as Aroclor), mirex and T12 concentrations were positively correlated with age of adult females (> 10 years) but only weakly, or not significantly, correlated with age of adult males. PCDD/Fs were present at low ng kg(-1) levels and consisted mainly of penta- and hexachlorofurans, and hepta- and octachlorodioxin. CB126 (3,3',4,4',5-PCB) was the most prominent non-ortho-substituted PCB congener in beluga blubber. Total TCDD toxic equivalents averaged 330 ng kg(-1) in females and 1400 ng kg(-1) in males and were dominated by CB126, and the mono-ortho-substituted congeners CB105 and CB118. Biomagnification factors (BMFs) for mirex and SigmaPCB from fish to beluga ranged from 11 to 16, and were similar to BMFs in Arctic animals, indicating that elevated levels in St Lawrence animals are a consequence of relatively high levels of recalcitrant organochlorines in prey of the beluga in the St Lawrence river system.     

Experimental determination of sorption in fractured flow systems

Fracture "skins" are alteration zones on fracture surfaces created by a variety of biological, chemical, and physical processes. Skins increase surface area, where sorption occurs, compared to the unaltered rock matrix. This study examines the sorption of organic solutes on altered fracture surfaces in an experimental fracture-flow apparatus. Fracture skins containing abundant metal oxides, clays, and organic material from the Breathitt Formation (Kentucky, USA) were collected in a manner such that skin surface integrity was maintained. The samples were reassembled in the lab in a flow-through apparatus that simulated approximately 2.7 m of a linear fracture "conduit." A dual-tracer injection scheme was utilized with the sorbing or reactive tracer compared to a non-reactive tracer (chloride) injected simultaneously. Sorption was assessed from the ratio of the first temporal moments of the breakthrough curves and from the loss of reactive tracer mass and evaluated as a function of flow velocity and solute type. The breakthrough curves suggest dual-flow regimes in the fracture with both sorbing and non-sorbing flow fields. Significant sorption occurs for the reactive components, and sorption increased with decreasing flow rate and decreasing compound solubility. Based on moment analysis, however, there was little retardation of the center of solute mass. These data suggest that non-equilibrium sorption processes dominate and that slow desorption and boundary layer diffusion cause extensive tailing in the breakthrough curves.     

BETR North America: a regionally segmented multimedia contaminant fate model for North America

We present the Berkeley-Trent North American contaminant fate model (BETR North America), a regionally segmented multimedia contaminant fate model based on the fugacity concept. The model is built on a framework that links contaminant fate models of individual regions, and is generally applicable to large, spatially heterogeneous areas. The North American environment is modeled as 24 ecological regions, within each region contaminant fate is described using a 7 compartment multimedia fugacity model including a vertically segmented atmosphere, freshwater, freshwater sediment, soil, coastal water and vegetation compartments. Inter-regional transport of contaminants in the atmosphere, freshwater and coastal water is described using a database of hydrological and meteorological data compiled with Geographical Information Systems (GIS) techniques. Steady-state and dynamic solutions to the 168 mass balance equations that make up the linked model for North America are discussed, and an illustrative case study of toxaphene transport from the southern United States to the Great Lakes Basin is presented. Regionally segmented models such as BETR North America can provide a critical link between evaluative models of long-range transport potential and contaminant concentrations observed in remote regions. The continent-scale mass balance calculated by the model provides a sound basis for evaluating long-range transport potential of organic pollutants, and formulation of continent-scale management and regulatory strategies for chemicals.