Associations and mobility of uranium in soils near a depleted uranium （DU） weapons testing site, SW Scotland

Natural uranium has three isotopes, ^238U, ^235U and ^234U, with natural abundances of 99.27 atom %, 0.72% and 0.0055%, respectively. Only ^235U is fissile and the production of nuclear fuel and nuclear weapons involves enrichment of uranium in ^235U. This process also results in separation of ^234U from ^238U, leaving depleted uranium （DU）, with typical ^234U/^238U and ^235U/^238U activity ratios of about 0.19 and 0.013, respectively, as a waste product. The high density, high melting and boiling points and chemical stability of uranium and the availability of DU in relatively pure form mean that DU has many uses, including armour-piercing munitions. Such munitions have been developed in the UK since the 1960s and testing has been carried out by the Ministry of Defence （MoD） at firing ranges such as Dundrennan, SW Scotland and Eskmeals, NW England. The firing of DU munitions can result in the dispersion of DU and its combustion products （oxides） as aerosols or as larger fragments, with the potential for human exposure either directly at the site of detonation or via post-depositional migration in the environment. The aim of this work was to investigate the potential environmental mobility of DU by characterizing the associations of U in soil porewaters with increasing distance from a firing site. To this end, several soil cores located down-wind of the firing site at Dundrennan, near Kirkcudbright, SW Scotland, were collected in May 2006. These were sectioned on-site into 1- or 2-cm depth intervals and porewaters were isolated by centfifugation （10 minutes; 8873 g） on return to the laboratory. Following filtration through 0.2-micron cellulose nitrate filters, the porewaters were analyzed by ICP-QMS （U concentration） and ICP-OES （Fe, Al, Ca, Mg, Mn concentrations）. Sub-samples were also subjected to centrifugal ultrafiltration （100, 30, and 3 kD） and to gel electrophoretic fractionation （agarose; 0.045 M Tris-borate; 20 mA, 30 minutes）. Results showed that U was present at up to 4 μg/L in the soil porewater and that the associations of U varied with sample location and soil depth.     

The acid neutralizing capacity （ANC） of South Africa＇s freshwater ecosystems

Acidification is considered the most important one of the primary chemical stress factors that impact on freshwater ecosystems. In unpolluted freshwater systems, the primary controls on the degree of acidification are factors such as the geological substrate of the catchment area, the presence of organic acids secreted by vegetation in the river system, and equilibrium exchange of carbon dioxide with the atmosphere. Anthropogenic factors that can impact on the degree of acidification of freshwater systems include agricultural, mining and industrial activities, either through direct runoff into river systems or through deposition of atmospheric pollutants from these sources. The capacity factors alkalinity and acidity, which represent the acid- and base-neutralizing capacity （ANC and BCN） of an aqueous system, have been used as more reliable measures of the acidic character of freshwater systems than pH. Unlike pH, ANC and BNC are not affected by parameters such as temperature and pressure. Therefore, ANC has been employed as a predictor of biological status in critical load assessments. Freshwater systems with ANC＇s eq/L isμeq/L are considered sensitive to acidification, ANC=0 μbelow 150 commonly used as the predictor for fish species such as trout in lakes, and an eq/L as more realistic for streams. Acid-neutralizing capacity μANC value of 40 （ANC） can be determined by titration with a strong acid to a preselected equivalence point. Alternatively, it can be calculated as the difference between base cations （[BC]） and strong acid anions （[SAA]）： ANC=[BC]- [SAA]=[Ca^2＋]＋[Mg^2＋]＋[Na^＋]＋[K^＋]-[SO4^2-]-[NO3^-]-[Cl^-] To date, there has been no attempt to establish the ANC of South Africa＇s freshwater ecosystems or variability therein, despite the fact that long-term water quality monitoring data exist for all the parameters needed to calculate it according to the above equations. As a result, the relationship between the acid neutralizing capacity of freshwater ecosystems in South Africa and biodiversity factors, such as fish status, is unknown. Results of the first comprehensive （country-wide scale） evaluation of the acid neutralizing capacity of river systems in South Africa will be presented. Long-term monitoring data obtained from the Department of Water Affairs and Forestry （DWAF） from most of South Africa＇s river systems were used to establish geographic and temporal variabilities in ANC. The results show that the Berg and Breede River systems are most susceptible to acidification, and that geological substrate appears to explain most of the geographic variabilities observed.     

The concentration and distribution of different mercury species in the water columns and sediment of Aha Lake

In order to find out whether Aha Lake was polluted by the acid mining waste water or not, the concentration and distribution of different mercuryspecies in the water columns and sediment profile collected from Aha Lake were investigated. It was found that discernible seasonal variation of different mercury species in water body were obtained in the Aha Reservoir. With regards to the whole sampling periods, the concentrations of HgP in the Aha Reservoir water body were evidently correlated to the concentrations of total mercury, showing that total mercury was mostly associated with particle mercury. The concentrations of methylmercury in water body were also evidently correlated to the concentrations of dissolved mercury. The dissolved mercury evidently affects the distribution and transportation of methylmercury. However, there is no correlation between methylmercury and total mercury. The dissolved mercury, reactive mercury, dissolved methylmercury levels in the water body of high flow period were much higher than those in low flow period. The distribution, speciation and levels of mercury within the Aha Reservoir water body were governed by several factors, such as the output of river, the release of sediment . Discernible seasonal variation of total mercury and methylmercury in porewater was described during the sampling periods, with the concentrations in high flow period generally higher than those in low flow period. The methylmercury in pore water column was evidently correlated to that of the sediment. The results indicated that highly elevated MeHgD concentrations in the porewater were produced at the depths from 2 to 5 cm in the sediment profile, and decreased sharply with depth. A positive correlation has been found between MeHgD formation and sulfate reducing bacterial activity. These highly elevated concentrations of MeHgD at the intersurface between waters and sediments suggest a favorable methylation condition. Moreover,     

The effect of acid deposition on base cation cycling in a karstic-forested catchment： Evidence from strontium isotopes

Bedrock weathering and atmospheric deposition are the two primary sources of base cations （K^＋, Na^＋, Ca^2＋ and Mg^2＋） to forest ecosystems. Therefore, the key problem is to understand the relative inputs from these two sources and the cycling in the ecosystem. This study focuses on the effects of acid deposition on cation cycling in a small-forested karstic catchment in Guizhou Province. Sr isotope ratios were used as a tracer for understanding the transport process between the different cation pools： rock, soil, surface water, atmospheric deposition and plant. The samples of wet deposition, total deposition, throughfall, surface and ground waters, vegetation, and soil were monthly collected. The exchangeable Sr^2＋ and Ca^2＋ in soil samples were extracted by using 1 M ammonium acetate. The leaf-tissue samples were ashed at 550℃, and the residue was digested in ultrapure HClO4 and HNO3. All water samples were filtrated through 0.45 μm aperture filter paper. Base cation concentrations and Sr isotopic composition were analyzed for all the samples. The results show that acid deposition （average pH 4.9） frequently occurred in the studied region. Cation abundance follows an increasing manner from rainwater, throughfall, to surface water or ground water samples, suggesting that acid deposition at first eiuviates Ca^2＋ , Mg^2＋ and Sr^2＋ from leaf, then the exchangeable cations from soil, and at last cations accumulate in surface water or ground water.     

Attenuation of aqueous metal transport at two natural acid rock drainage occurrences in the Yukon Territory, Canada

Naturally acidic drainage associated with pyritic black shale has been observed in many locations in the Yukon Territory. While not necessarily linked to known mineral deposits, most of these natural acid rock drainage occurrences show elevated dissolved concentrations of trace elements, especially zinc, nickel, copper, cadmium and arsenic. Based on field observations, microbial investigation, chemical analyses and geochemical modeling, the fate and transport of potentially deleterious elements at two natural acid drainage occurrences with slightly different settings are examined. The Macintosh Creek is a small, acidic stream （pH 2.98-3.40）, 2 km long, located in the Macmillan Pass area of east-central Yukon amidst known sedimentary exhalative massive sulfide mineralization but remains undisturbed by exploration activities. Its trace metal content is apparently derived from groundwater discharges, which gave as much as 5.0, 2.5, 0.7, 0.13 and 0.03 mg/L ofZn, Ni, Cu and As, respectively. Interaction and sorption reactions with algal mats, biofilms and iron oxyhydroxides appear to be the dominant mechanisms attenuating aqueous contaminant transport along the stream. Cryogenic precipitation further consolidates the ferricrete formation and reduces the mobility of the sorbed metals. The tributaries of the Engineering Creek along the Dempster Highway in northern Yukon drain through a series of dolomite, phyllite, argillite, limestone, black shale, sandstone and conglomerate with no known concentration of mineralization. In this area, the water chemistry fully reflects the local geology with acidic streams invariably associated with black shale occurrences. Groundwater seeps in the headwaters area of the km-180 Creek completely enclosed in black shale gave pH 3.0 and as much as 148, 39, 2.9 and 9.1 mg/L of Zn, Ni, Cu and As, respectively. Sorption with iron oxyhydroxide and organic matter appear to dominate the attenuation of contaminant transport along the stream. However, once entered into carbonate-dominated terrains, secondary carbonate minerals exercise additional geochemical control on the local water chemistry as a result of neutralization.     

Hydrogeochemical controls on surface and groundwater chemistry in naturally acidic, porphyry-related mineralized areas, southern Rocky Mountains

In southern Rocky Mountains, catchments characterized by acidic, metalliferous waters that are relatively unaffected by human activity usually occur within areas that have active or historical mining activity. The US Geological Survey has utilized these mineralized but unmined catchments to constrain geochemical processes that control the surface- and ground-water chemistry associated with near surface acid weathering as well as to estimate premining conditions. Study areas include the upper Animas River watershed, Lake City, Mt. Emmons, and Montezuma in Colorado and Questa in New Mexico. Although host-rock lithologies range from Precambrian gneisses to Cretaceous sedimentary units to Tertiary volcanic complexes, mineralization is Tertiary in age and associated with intermediate to felsic composition, porphyritic plutons. Pyrite is ubiquitous. Variability of metal concentrations in water is caused by two main factors： mineralogy and hydrology. Parameters that potentially affect water chemistry include： host-rock lithology, intensity of hydrothermal alteration, sulfide mineralogy and chemistry, gangue mineralogy, length of flow path, precipitation, evaporation, and redox conditions. Springs and headwater streams have pH values as low as 2.5, sulfate up to 3700 mg/L and high dissolved metal concentrations （for example： Al up to 170 mg/L; Fe up to 250 mg/L; Cu up to 3.5 mg/L and Zn up to 14 mg/L）. With the exception of evaporative waters, the lowest pH values and highest Fe and Al concentrations occur in water draining the most intense hydrothermally altered areas consisting of the mineral assemblage quartz-sericite-pyrite. Stream beds tend to be coated with iron floc, and some reaches are underlain by ferricrete. When iron-rich ground water interacts with oxygenated waters in the stream or hyporheic zone, ferrous iron is oxidized to ferric iron, which is less soluble, leading to the precipitation of iron oxyhydroxides.     

Naturally acidic and metalliferous waters at unmined volcanogenic massive sulfide deposits in the Bonnifield mining district, Alaska Range, east-central Alaska

The Bonnifield district hosts 26 tmmined volcanogenic massive sulfide （VMS） occurrences. Environmental geochemical samples of water and stream sediment were collected at several occurrences, concentrating on the two best-exposed and largest deposits, Red Mountain （RM） and Sheep Creek （SC）. Limited samples were also collected at the poorly exposed WTF deposit. The deposits are Late Devonian to Early Mississippian, and are hosted by felsic metavolcanic and carbonaceous schist members of the Totatlanika Schist or Keevy Peak Fm. Spring and stream waters at RM and SC have pH values commonly 〈3.5 （as low as 2.4 at RM and 2.5 at SC）, high conductivity （up to 11000 μS/cm）, and very high （Is to 100s mg/L） dissolved contents of Al, Cd, Co, Cu, Fe, Ni, and Pb. Waters at RM are characterized by extremely high REE contents （summed REE median 3200 μg/L, n=33）. At both RM and SC, pyrite oxidation and dissolution produce low pH waters that interact with and dissolve bedrock minerals, resulting in acidic, metal-laden, naturally degraded streams that are mostly devoid of aquatic life. Ferricrete is common. In contrast, WTF barely produces a surficial environmental footprint, mostly due to topography and relief. RM and SC are well exposed in the areas of relatively high relief, and both exhibit extensive areas of quartz-sericite-pyrite-alteration. While WTF shares many of the same deposit-and alteration characteristics, it is concealed by tundra in a large, nearly flat area. Surface water at WTF is absent and outcrops are sparse. Even though WTF is roughly the same size as Red Mountain （both around 3 million tonnes） and has similar base- and precious-metal grades, the surficial geochemical manifestation of WTF is minimal. However, exposure through mining of the altered, mineralized rock at WTF potentially could initiate the same processes of pyrite oxidation, acid generation, and mineral dissolution that are observed naturally at RM and SC.     

Water chemical behavior at Yangtze （Changjiang） River estuary

Geochemical cycling has received wide attention due to the need to understand the pathways of pollutants through our present environment. In this regard the Yangtze River plays a significant role in putting those pollutants into the East China SeafWorld Oceans. The Yangtze River is of high sedimentation rate and water discharge. The watershed covers variable climate regions from temperate to subtropical and from semiarid to humid. Twenty three （23） sampling locations at the estuary have been selected for understanding the dynamic relationships. The elements （Cl^-, SO4^2-, Na^＋, K^＋, and Ca^2＋） show conservative behavior during mixing of fresh water with saline water whereas Mg^2＋, Mn^2＋ show a non-conservative pattern . The relationships between Na^＋/SO4^2- and Cl^-/SO4^2- molar ratios show a mixing of more than two water sources.     

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