Mobility of metals in nickel mine spoil materials     

Sophie Raous  Thierry Becquer  Jérémie Garnier  Éder de Souza Martins  Guillaume Echevarria  Thibault Sterckeman 《Applied Geochemistry》2010

An understanding of the biogeochemical behaviour of metals in mine spoil materials is a prerequisite to rehabilitate Ni mining sites. The objective of this study was to characterize the fate of metals in different Ni ore spoil materials as influenced by hydrological conditions and fertilisation practices. In tropical ultramafic complexes, the different stages of lateritic weathering lead to two types of ores, and therefore, to two spoil types. They are mainly either a clay-rich saprolite, so-called “garnierite”, enriched in phyllosilicates, or a limonitic material, enriched in Fe oxides. Lysimeter columns were designed to monitor leaching waters through both spoil materials. The garnieritic spoil released higher concentrations of Mg (mean = 2.25 mg L⁻¹), Ni (0.39 mg L⁻¹) and Cr (1.19 mg L⁻¹) than the limonitic spoil (Mg = 0.5 mg L⁻¹; Ni = 0.03 mg L⁻¹ and Cr = 0.25 mg L⁻¹). Chromium was mainly in an anionic form in leaching solutions. As exchangeable pools of Cr(VI) in limonite (980 mg kg⁻¹ of KH₂PO₄-extractable Cr) are considerable its release in water may still occur in the case of a pH increase. In mixed spoil, metal concentrations were almost as low as in the limonitic one. The effect of mineral-N fertilisation was a strong release of cations (Ni, Mg) into the leachate. Phosphate amendment did not affect the soil solution composition under experimental conditions.  相似文献   

Rhizosphere and flooding regime as key factors for the mobilisation of arsenic and potentially harmful metals in basic,mining-polluted salt marsh soils     

Antonio María-Cervantes  Héctor M. ConesaMaría Nazaret González-Alcaraz  José Álvarez-Rogel 《Applied Geochemistry》2010

The occurrence of mining areas in the vicinities of salt marshes may affect their ecological functions and facilitate the transfer of pollutants into the food chain. The mobilisation of metals in salt marsh soils is controlled by abiotic (pH, redox potential) and biotic (influence of rhizosphere) factors. The effect of the rhizosphere of two plant species (Sarcocornia fruticosa and Phragmites australis) and different flooding regimes on potentially harmful metals and As mobilisation from salt marsh soil polluted by mining activities were investigated (total concentrations: 536 mg kg⁻¹ As, 37 mg kg⁻¹ Cd, 6746 mg kg⁻¹ Pb, 15,320 mg kg⁻¹ Zn). The results show that the changes in redox conditions (from 300 mV to −100 mV) and pH after flooding and rewetting periods may mobilise the contaminant elements into soil solution (e.g., 100 μg L⁻¹ Cd, 30 μg L⁻¹ Pb, 7 mg L⁻¹ Zn), where they are available for plants or may be leached from the soil. Drying periods generated peaks of concentrations in the soil solution (up to 120 μg L⁻¹ Cd and 50 μg L⁻¹ Pb). The risk assessment of As and metal-polluted salt marshes should take into account flood dynamics in order to prevent metal(loid) mobilisation.  相似文献   

Irrigation produces elevated arsenic in the underlying groundwater of a semi-arid basin in Southwestern Idaho     

Montague W. Busbee  Benjamin D. Kocar  Shawn G. Benner 《Applied Geochemistry》2009

The shallow aquifer beneath the Western Snake River Plain (Idaho, USA) exhibits widespread elevated arsenic concentrations (up to 120 μg L⁻¹). While semi-arid, crop irrigation has increased annual recharge to the aquifer from approximately 1 cm prior to a current rate of >50 cm year⁻¹. The highest aqueous arsenic concentrations are found in proximity to the water table (all values >50 μg L⁻¹ within 50 m) and concentrations decline with depth. Despite strong vertical redox stratification within the aquifer, spatial distribution of aqueous species indicates that redox processes are not primary drivers of arsenic mobilization. Arsenic release and transport occur under oxidizing conditions; groundwater wells containing dissolved arsenic at >50 μg L⁻¹ exhibit elevated concentrations of O₂ (average 4 mg L⁻¹) and NO₃ (average 8 mg L⁻¹) and low concentrations of dissolved Fe (<20 μg L⁻¹). Sequential extractions and spectroscopic analysis of surficial soils and sediments indicate solid phase arsenic is primarily arsenate and is present at elevated concentrations (4–45 mg kg⁻¹, average: 17 mg kg⁻¹) relative to global sedimentary abundances. The highest concentrations of easily mobilized arsenic (up to 7 mg kg⁻¹) are associated with surficial soils and sediments visibly stained with iron oxides. Batch leaching experiments on these materials using irrigation waters produce pore water arsenic concentrations approximating those observed in the shallow aquifer (up to 152 μg L⁻¹). While As:Cl aqueous phase relationships suggest minor evaporative enrichment, this appears to be a relic of the pre-irrigation environment. Collectively, these data indicate that infiltrating irrigation waters leach arsenic from surficial sediments to the underlying aquifer.  相似文献   

Landscape variations in stream water SO₄ and δS_SO4 in a boreal stream network     

Louise Björkvald  Reiner Giesler  Christoph Humborg 《Geochimica et cosmochimica acta》2009,73(16):4648-2683

Despite reduced anthropogenic deposition during the last decades, deposition sulphate may still play an important role in the biogeochemical cycles of S and many catchments may act as net sources of S that may remain for several decades. The aim of this study is to elucidate the temporal and spatial dynamics of both SO₄²⁻ and δ³⁴S_SO4 in stream water from catchments with varying percentage of wetland and forest coverage and to determine their relative importance for catchment losses of S. Stream water samples were collected from 15 subcatchments ranging in size from 3 to 6780 ha, in a boreal stream network, northern Sweden. In forested catchments (<2% wetland cover) S-SO₄²⁻ concentrations in stream water averaged 1.7 mg L⁻¹ whereas in wetland dominated catchments (>30% wetland cover) the concentrations averaged 0.3 mg L⁻¹. A significant negative relationship was observed between S-SO₄²⁻ and percentage wetland coverage (r² = 0.77, p < 0.001) and the annual export of stream water SO₄²⁻ and wetland coverage (r² = 0.76, p < 0.001). The percentage forest coverage was on the other hand positively related to stream water SO₄²⁻ concentrations and the annual export of stream water SO₄²⁻ (r² = 0.77 and r² = 0.79, respectively). The annual average δ³⁴S_SO4 value in wetland dominated streams was +7.6‰ and in streams of forested catchments +6.7‰. At spring flood the δ³⁴S_SO4 values decreased in all streams by 1‰ to 5‰. The δ³⁴S_SO4 values in all streams were higher than the δ³⁴S_SO4 value of +4.7‰ in precipitation (snow). The export of S ranged from 0.5 kg S ha⁻¹ yr⁻¹ (wetland headwater stream) to 3.8 kg S ha⁻¹ yr⁻¹ (forested headwater stream). With an average S deposition in open field of 1.3 kg S ha⁻¹ yr⁻¹ (2002-2006) the mass balance results in a net export of S from all catchments, except in catchments with >30% wetland. The high temporal and spatial resolution of this study demonstrates that the reducing environments of wetlands play a key role for the biogeochemistry of S in boreal landscapes and are net sinks of S. Forested areas, on the other hand were net sources of S.  相似文献   

Influence Of Bedrock Geology On Elemental Fluxes In Two Forested Catchments Affected By High Acidic Deposition     

P. Krám  J. Hruška 《Hydrogeology Journal》1994,2(2):50-58

Water samples have been collected from two forested catchments in the Slavkovsky les Mountains of western Bohemia, in the Czech Republic. The objective of the study was to compare and contrast elemental fluxes in two catchments with similar conditions of climate, topography, vegetation over and acidic atmospheric deposition, but very different bedrock geology. The Lysina catchment is underlain by slow-weathering leucocratic granite. Soils are podzolized brown earths and peaty gleys with small pools of exchangeable basic cations. Both soils and drainage water at Lysina are acidified by atmospheric deposition. Surface runoff was found to be dominated by sulphate and dissolved silica, accompanied by high concentrations of H⁺ (volume weighted pH = 3.87). Stream water also displayed extremely high concentrations of total aluminum (volume-weighted mean 66 7mol.l^у). Inorganic monomeric aluminum was the predominant aluminum fraction present, which contained mainly aquo-Al (Al³⁺ and fluoride complexes. The Pluhuv Bor catchment is characterized by ultramafic serpentinite and, in contrast to Lysina, soil and drainage waters have higher concentration of basic cations. Streamwater chemistry was dominated by magnesium, sulphate and silica. Stream-water at the site was not acidic (volume weighted pH = 7.25). The ratio of output/input of sulphate was similar at both catchments (1.16 for granite site and 1.07 for the serpentinite site). This pattern may be indicative of the conservative behaviour of sulphate in very different soil and bedrock environments under elevated loadings of acidic deposition. Résumé: Des eaux ont été échantillonnées dans deux bassins forestiers du massif de Slavkovsky les, en Bohême occidentale (République Tchèque). Le but de l'étude était de comparer les flux de matière dans les deux bassins, soumis à des conditions identiques de climat, de topographie, de couvert végétal et d'apports atmosphériques acides, mais à une géologie de leur substratum très différente. Le bassin de la Lysina est constitué d'un leucogranite peu altéré. Le couvert pédologique est formé de sols bruns podzolisés et de gleys de tourbières, qui son pauvres en cations de bases échangeables. Les sols et les eaux de drainage de la Lysina sont acidifiés par les apports atmosphériques. L'écoulement de surface est dominé par les sulfates et la silice, associés à de fortes teneurs en H⁺ (pH = 3.87). Les eaux de la rivière présentent en outre des teneurs particulièrement élevées en aluminium total (66 µmol.l^у). L'aluminium domine sous la forme d'un monomère minéral, surtout l'aluminium aqueus (Al³⁺) et des complexes fluorés. Le bassin de la Pluhuv Bor est caractérisé par une serpentinite ultrabasique et, au contraire de la Lysina, par des sols et des eaux de drainage à très fortes teneurs en cations basiques. Les eaux de la rivière sont dominées par le magnésium, les sulfates et la silice. Ces eaux ne sont pas acides (pH = 7.25). Le rapport des flux de sortie et d'entrée de sulfates est identique pour les deux bassins (1.16 pour le bassin granitique; 1.07 pour le bassin de serpentinite). Cette situation parait signifier que les sulfates présentent un comportement conservatif dans des environnements pédologiques et géologiques très différents, sous des apports acides importants.  相似文献   

Dissolution and carbonation of a serpentinite: Inferences from acid attack and high P-T experiments performed in aqueous solutions at variable salinity     

Andrea Orlando  Daniele BorriniLuigi Marini 《Applied Geochemistry》2011,26(8):1569-1583

Dissolution experiments on a serpentinite were performed at 70 °C, 0.1 MPa, in H₂SO₄ solution, in open and closed systems, in order to evaluate the overall dissolution rate of mineral components over different times (4, 9 and 24 h). In addition, the serpentinite powder was reacted with a NaCl-bearing aqueous solution and supercritical CO₂ for 24 h at higher pressures (9-30 MPa) and temperatures (250-300 °C) either in a stirred reactor or in an externally-heated pressure vessel to assess both the dissolution rate of serpentinite minerals and the progress of the carbonation reaction. Results show that, at 0.1 MPa, MgO extraction from serpentinite ranges from 82% to 98% and dissolution rate varies from 8.5 × 10⁻¹⁰ mole m⁻² s⁻¹ to 4.2 × 10⁻⁹ mole m⁻² s⁻¹. Attempts to obtain carbonates from the Mg-rich solutions by increasing their pH failed since Mg- and NH₄- bearing sulfates promptly precipitated. On the other hand, at higher pressures, significant crystallization (5.0-10.4 wt%) of Ca- and Fe-bearing magnesite was accomplished at 30 MPa and 300 °C using 100 g L⁻¹ NaCl aqueous solutions. The corresponding amount of CO₂ sequestered by crystallization of carbonates is 9.4-15.9 mole%. Dissolution rate (from 6.3 × 10⁻¹¹ mole m⁻² s⁻¹ to 1.3 × 10⁻¹⁰ mole m⁻² s⁻¹) is lower than that obtained at 0.1 MPa and 70 °C but it is related to pH values much higher (3.3-4.4) than that (−0.65) calculated for the H₂SO₄ solution.Through a thorough review of previous experimental investigations on the dissolution kinetics of serpentine minerals the authors propose adopting: (i) the log rate [mole m⁻² s⁻¹] value of −12.08 ± 0.16 (1σ), as representative of the neutral dissolution mechanism at 25 °C and (ii) the following relationship for the acidic dissolution mechanism at 25 °C: