Seasonal blooms of neutrophilic Betaproteobacterial Fe(II) oxidizers and Chlorobi in iron-rich coal mine drainage sediments.

Waters draining from flooded and abandoned coal mines in the South Wales Coalfield (SWC) are substantial sources of pollution to the environment characterized by circumneutral pH and elevated dissolved iron concentrations (>1 mg L-1). The discharged Fe precipitates to form Fe(III) (oxyhydr)oxides which sustain microbial communities. However, while several studies have investigated the geochemistry of mine drainage in the SWC, less is known about the microbial ecology of the sites presenting a gap in our understanding of biogeochemical cycling and pollutant turnover. This study investigated the biogeochemistry of the Ynysarwed mine adit in the SWC. Samples were collected from nine locations within sediment at the mine entrance from the upper and lower layers three times over one year for geochemical and bacterial 16S rRNA gene sequence analysis. During winter, members of the Betaproteobacteria bloomed in relative abundance (>40%) including the microaerophilic Fe(II)-oxidizing genus Gallionella. A concomitant decrease in Chlorobi-associated bacteria occurred, although by summer the community composition resembled that observed in the previous autumn. Here, we provide the first insights into the microbial ecology and seasonal dynamics of bacterial communities of Fe(III)-rich deposits in the SWC and demonstrate that neutrophilic Fe(II)-oxidizing bacteria are important and dynamic members of these communities.

Linking selective chemical extraction of iron oxyhydroxides to arsenic bioaccessibility in soil.

The relationship between As bioaccessibility using the physiologically based extraction test (PBET) and As extracted by hydroxylamine hydrochloride (HH), targeting the dissolution of amorphous Fe oxyhydroxides, is established in soils from the British Geological Survey Geochemical Baseline Survey of SW England, UK, to represent low As background and high As mineralised/mined soils. The HH-extracted As was of the same order of magnitude as the As extracted in the bioaccessibility test and proved to be a better estimate of bioaccessible As than total As (bioaccessible As - total As: r = 0.955; bioaccessible As - HH-extracted As: r = 0.974; p-values = 0.000). These results provide a means of estimating soil As bioaccessibility on the basis of the HH extraction. Further selective extraction data, using hydrochloride acid that seeks to dissolve both amorphous and crystalline Fe oxyhydroxides, indicates a decrease in the As bioaccessible fraction with the increase of the soil Fe oxyhydroxide crystallinity.

Methodology for the determination of normal background concentrations of contaminants in English soil.

The revised Environmental Protection Act Part 2A contaminated land Statutory Guidance (England and Wales) makes reference to 'normal' levels of contaminants in soil. The British Geological Survey has been commissioned by the United Kingdom Department for Environment, Food and Rural Affairs (Defra) to estimate contaminant levels in soil and to define what is meant by 'normal' for English soil. The Guidance states that 'normal' levels of contaminants are typical and widespread and arise from a combination of both natural and diffuse pollution contributions. Available systematically collected soil data sets for England are explored for inorganic contaminants (As, Cd, Cu, Hg, Ni and Pb) and benzo[a]pyrene (BaP). Spatial variability of contaminants is studied in the context of the underlying parent material, metalliferous mineralisation and associated mining activities, and the built (urban) environment, the latter being indicative of human activities such as industry and transportation. The most significant areas of elevated contaminant concentrations are identified as contaminant domains. Therefore, rather than estimating a single national contaminant range of concentrations, we assign an upper threshold value to contaminant domains. Our representation of this threshold is a Normal Background Concentration (NBC) defined as the upper 95% confidence limit of the 95th percentile for the soil results associated with a particular domain. Concentrations of a contaminant are considered to be typical and widespread for the identified contaminant domain up to (and including) the calculated NBC. A robust statistical methodology for determining NBCs is presented using inspection of data distribution plots and skewness testing, followed by an appropriate data transformation in order to reduce the effects of point source contamination.

Effect of weathering product assemblages on Pb bioaccessibility in mine waste: implications for risk management.

General assessments of orebody types and associated mine wastes with regard to their environmental signature and human health hazards are needed to help in managing present and historical mine waste facilities. Bioaccessibility tests and mineralogical analysis were carried out on mine waste from a systematic sampling of mine sites from the Central Wales orefield, UK. The bioaccessible Pb widely ranged from 270 to 20,300 mg/kg (mean 7,250 mg/kg, median 4,890 mg/kg), and the bioaccessible fraction from 4.53 to >100% (mean 33.2%, median 32.2%), with significant (p=0.001) differences among the mine sites. This implies sensitivity of bioaccessibility to site-specific conditions and suggests caution in the use of models to assess human health impacts generalised on the basis of the mineral deposit type. Mineralogical similarities of the oxidation products of primary galena provided a better control over the observed Pb bioaccessibility range. The higher Pb bioaccessibility (%) was related to samples containing cerussite, irrespective of the presence of other Pb minerals in the mineral assemblage; lower Pb bioaccessibility resulted where anglesite was the main Pb mineral phase and cerussite was absent. A solubility diagram for the various Pb minerals in the waste was derived using PHREEQC model, and the experimental Pb concentrations, measured in the simulated gastric solution, were compared with the equilibrium modelling results. For samples containing cerussite, the model well predicted the soluble Pb concentrations measured in the gastric solution, indicative of the carbonate mineral phase control on the Pb in solution for these samples and little kinetic control on the dissolution of cerussite. On the contrary, most mine waste samples containing dominant anglesite and or plumbojarosite (no cerussite) had lower solution Pb values, falling at or below the anglesite and plumbojarosite solubility equilibrium concentrations, implying kinetic or textural factors hindering the dissolution.

Impact of gut passage and mucus secretion by the earthworm Lumbricus terrestris on mobility and speciation of arsenic in contaminated soil.

Earthworms inhabiting arsenic contaminated soils may accelerate the leaching of As into surface and ground waters. We carried out three experiments to determine the impact of passage of As contaminated soil (1150 mg As kg(-1)) through the gut of the earthworm Lumbricus terrestris on the mobility and speciation of As and the effects of earthworm mucus on As mobility. The concentration of water soluble As in soil increased (from 1.6 to 18 mg kg(-1)) after passage through the earthworm gut. Casts that were aged for 56 days still contained more than nine times greater water soluble As than bulk earthworm inhabited soil. Changes were due to increases in As(V) mobility, with no change in As(III). Dilute mucus extracts reduced As mobility through the formation of As-amino acid-iron oxide ternary complexes. More concentrated mucus extracts increased As mobility. These changes, together with those due to the passage through the gut, were due to increases in pH, phosphate and soluble organic carbon. The mobilisation of As from contaminated soils in the environment by cast production and mucus secretion may allow for accelerated leaching or uptake into biota which is underestimated when bulk soil samples are analysed and the influence of soil biota ignored.

Impact of earthworms on trace element solubility in contaminated mine soils amended with green waste compost.

The common practice of remediating metal contaminated mine soils with compost can reduce metal mobility and promote revegetation, but the effect of introduced or colonising earthworms on metal solubility is largely unknown. We amended soils from an As/Cu (1150 mg As kg(-1) and 362 mg Cu kg(-1)) and Pb/Zn mine (4550 mg Pb kg(-1) and 908 mg Zn kg(-1)) with 0, 5, 10, 15 and 20% compost and then introduced Lumbricus terrestris. Porewater was sampled and soil extracted with water to determine trace element solubility, pH and soluble organic carbon. Compost reduced Cu, Pb and Zn, but increased As solubility. Earthworms decreased water soluble Cu and As but increased Pb and Zn in porewater. The effect of the earthworms decreased with increasing compost amendment. The impact of the compost and the earthworms on metal solubility is explained by their effect on pH and soluble organic carbon and the environmental chemistry of each element.

Impacts of epigeic, anecic and endogeic earthworms on metal and metalloid mobility and availability.

The introduction of earthworms into soils contaminated with metals and metalloids has been suggested to aid restoration practices. Eisenia veneta (epigeic), Lumbricus terrestris (anecic) and Allolobophora chlorotica (endogeic) earthworms were cultivated in columns containing 900 g soil with 1130, 345, 113 and 131 mg kg(-1) of As, Cu, Pb and Zn, respectively, for up to 112 days, in parallel with earthworm-free columns. Leachate was produced by pouring water on the soil surface to saturate the soil and generate downflow. Ryegrass was grown on the top of columns to assess metal uptake into biota. Different ecological groups affected metals in the same way by increasing concentrations and free ion activities in leachate, but anecic L. terrestris had the greatest effect by increasing leachate concentrations of As by 267%, Cu by 393%, Pb by 190%, and Zn by 429% compared to earthworm-free columns. Ryegrass grown in earthworm-bearing soil accumulated more metal and the soil microbial community exhibited greater stress. Results are consistent with earthworm enhanced degradation of organic matter leading to release of organically bound elements. The degradation of organic matter also releases organic acids which decrease the soil pH. The earthworms do not appear to carry out a unique process, but increase the rate of a process that is already occurring. The impact of earthworms on metal mobility and availability should therefore be considered when inoculating earthworms into contaminated soils as new pathways to receptors may be created or the flow of metals and metalloids to receptors may be elevated.

Impact of the earthworm Lumbricus terrestris (L.) on As, Cu, Pb and Zn mobility and speciation in contaminated soils.

To assess the risks that contaminated soils pose to the environment properly a greater understanding of how soil biota influence the mobility of metal(loid)s in soils is required. Lumbricus terrestris L. were incubated in three soils contaminated with As, Cu, Pb and Zn. The concentration and speciation of metal(loid)s in pore waters and the mobility and partitioning in casts were compared with earthworm-free soil. Generally the concentrations of water extractable metal(loid)s in earthworm casts were greater than in earthworm-free soil. The impact of the earthworms on concentration and speciation in pore waters was soil and metal specific and could be explained either by earthworm induced changes in soil pH or soluble organic carbon. The mobilisation of metal(loid)s in the environment by earthworm activity may allow for leaching or uptake into biota.

Bioaccessibility of arsenic in mine waste-contaminated soils: a case study from an abandoned arsenic mine in SW England (UK).

This study characterises the total As concentrations and As bioaccessibility in 109 soils from Devon Great Consols Mine, an abandoned Cu-As mine in Devon, SW England, UK and discusses the soil and mineralogical factors that influence the bioaccessibility of this element. These data provide the basis for developing more accurate exposure estimates for use in human health risk assessments. The median value of the percent bioaccesible As of 15% for these As rich soils contaminated by mining activities indicated that relatively little of the total As is present in a bioaccessible form. Spatial variability of As bioaccesibility in the soils was also recognised throughout the mine site as a function of mineralogy. Multivariate statistical analysis identified a sulphide component responsible for the reduced As bioaccessibility of one cluster of soils. In the larger cluster of acidic mine soils covered by woodland As is mainly hosted in Fe oxyhydroxides whose partial dissolution is responsible for the bioaccessible As fraction. It was highlighted that the degree of Fe oxyhydroxide crystallinity might represent an important factor influencing arsenic bioaccessibility. Mine soils from Devon Great Consols Mine showed overall higher As bioaccessibility (15%) than other mineralised soils not affected by mining activities and background soils within the Tamar Catchment whose percent bioaccessible As median values were 9%.