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The impacts of Sn-W, Ba-Pb-Zn and W-Au-Sb old mine workings on the environment at Central Portugal

Tailings deposited over the Castanheira, a stream which flows through the old Ag–Pb–Zn Terramonte mine area, showed a great potential environmental risk due to sulphide weathering, facilitated by the tailings–water interaction. The high concentrations of Al, Fe, Pb and Zn in the tailings are associated with the exchangeable, reducible and sulphide fractions and suggest sphalerite and pyrite occurrences. Oxidation of pyrite is responsible for the low pH values (3.38–4.89) of the tailings. The water from the Castanheira stream is not suitable for human consumption due to high concentrations of SO4 2−, Mn, Al, Cd, Ni, and Pb. The lowest concentrations of metals and metalloids were detected in downstream stretches of the Castanheira. However, As, Fe and Zn in deeper sediments tend to increase downstream. Significant concentrations of trivalent forms of arsenic were detected in water samples. In downstream stretches of the Castanheira, some free ions (Fe2+, Mn2+ and Zn2+) also predominate and the water is saturated with ferrihydrite, goethite, hematite, lepidocrosite and magnetite.

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The old Senhora das Fontes uranium mine, in central Portugal, consists of quartz veins which penetrated along fracture shear zones at the contact between graphite schist and orthogneiss. The mine was exploited underground until a depth of 90 m and was closed down in 1971. The ores from this mine and two others were treated in the mine area by the heap-leach process which ended in 1982. Seven dumps containing a total of about 33,800 m3 of material and partially covered by natural vegetation were left in the mine area. A remediation process took place from May 2010 to January 2011. The material deposited in dumps was relocated and covered with erosion resisting covers. Surface water and groundwater were collected in the wet season just before the remediation, in the following season at the beginning of the remediation and also after the remediation in the following dry season. Before, at the beginning and after the remediation, surface water and groundwater have an acid-to-alkaline pH, which decreased with the remediation, whereas Eh increased. In general, before the remediation, uranium concentration was up to 83 μg/L in surface water and up to 116 μg/L in groundwater, whereas at the beginning of the remediation it increases up to 183 μg/L and 272 μg/L in the former and the latter, respectively, due to the remobilization of mine dumps and pyrite and chalcopyrite exposures, responsible for the pH decrease. In general, after the remediation, the U concentration decreased significantly in surface water and groundwater at the north part of the mine area, but increased in both, particularly in the latter up to 774 μg/L in the south and southwest parts of this area, attributed to the remobilization of sulphides that caused mobilization of metals and arsenic which migrated to the groundwater flow. Uranium is adsorbed in clay minerals, but also in goethite as indicated by the geochemical modelling. After the remediation, the saturation indices of oxyhydroxides decrease as pH decreases. The remediation also caused decrease in Cd, Co, Cr, Ni, Pb, Zn, Cu, As, Sr and Mn concentrations of surface water and groundwater, particularly in the north part of the mine area, which is supported by the speciation modelling that shows the decrease of most dissolved bivalent species. However, in general, after the remediation, Th, Cd, Al, Li, Pb, Sr and As concentrations increased in groundwater and surface water at south and southwest of the mine area. Before and after the remediation, surface water and groundwater are contaminated in U, Cd, Cr, Al, Mn, Ni, Pb, Cu and As. Remediation caused only some improvement at north of the mine area, because at south and southwest part, after the remediation, the groundwater is more contaminated than before the remediation.

The Pinhal do Souto mine exploited a quartz vein containing uranium minerals, mainly autunite and torbernite. This vein intersects a two-mica granite containing 10 ppm U and uraninite. The mine was exploited underground and produced 93091 kg U3O8 between 1978 and 1989 and was then closed down. Two dumps were left in the mine area and these are partially covered by natural vegetation. Groundwater and surface water have a similar slightly acid-to-alkaline pH. The 2  2 UO is abundant and complexed with 2  3 CO , under neutral to alkaline pH. Metals and arsenic concentrations in the water increase during the dry season due to the evaporation. Uranium concentration in the water increases (up to 104.42 g/l) in the wet season, because secondary uranium minerals are dissolved and uranium is released into the water. Soils tend to retain a higher concentration of several metals, including U (up to 336.79 mg/kg) than stream sediments (up to 35.68 mg/kg), because vermiculite from the former could adsorb it more easily than could kaolinite from the latter. The Fe-oxides precipitate retains the highest concentrations of several metals, including U and Th (up to 485.20 and 1053.12 mg/kg, respectively) and the metalloid As, because it is richer in oxyhydroxides and organic matter than stream sediments and soils. The median concentrations of Fe, As, Cd, Pb, Sb, Th, U, W and Zn in soils from this area are higher than in European soils of the FOREGS data. Waters from dry and wet seasons, stream sediments and soils are contaminated and must not be used. This area was compared with another Portuguese abandoned uranium mine area. The former mine caused a lower environmental impact attributable to it having lower sulfide concentration and mineral alteration than in the latter.

In the abandoned Mortórios uranium mine area there are quartz veins containing wolframite and sulphides and basic rock dykes with torbernite and autunite cutting a porphyritic granite. The basic rock dykes were exploited and produced about 27 t of U3O8, from 1982 to 1988. There are an open pit lake and nine dumps. Surface water and groundwater are contaminated in U, As, Cd, Cr, Cu, Fe, Mn, Ni and Pb. Stream sediments are contaminated in U, As, Th and W, which are adsorbed by smectite, kaolinite and iron- and aluminium- oxy-hydroxides. The maximum U concentrations are of 1268 μg/L in the open pit lake, 100 μg/L in surface water, 103 μg/L in groundwater and 81.5 mg/kg in stream sediments all downstream of the open pit lake and dumps. Further downstream the U concentration in water decreases, due to the high mobility of U (VI), but the U concentration in stream sediments increases. Calcium uranyl carbonate dominates in the open pit lake, but uranyl carbonate complexes dominate in surface water and groundwater. The maximum As concentrations are 56.0 μg/L in the open pit lake, 63.4 μg/L in the surface water and 66.7 μg/L in the groundwater, both downstream of the open pit lake and dumps. The arsenic occurs as As (V). The Mortórios area is compared with two other areas exploited from open pits, all located in the uranium-bearing Beira area of central Portugal. Vale de Abrutiga produced 90 t of U3O8 between 1982 and 1989 and Mondego Sul produced 75 t of U3O8 from 1987 to 1991. The two mines consist of quartz veins containing sulphides, saleeite and meta-saleeite at Vale de Abrutiga and with sulphides, autunite, torbernite, meta-uranocircite and meta-saleeite at Mondego Sul cutting the Schist-graywacke Complex. The mine area of Vale de Abrutiga with the highest exploitation of U3O8 has strongly acidic to slight alkaline water, which is the most contaminated. Mortórios with the lowest exploitation presents a higher contamination of slightly acidic to alkaline water than that of acidic to alkaline water from Mondego Sul, but the former has As (V), whereas the latter has As (III), which is toxic. The stream sediments from Mortórios present the lowest contamination, except for Th that has a higher median value than that from Vale de Abrutiga. Stream sediments from Mondego Sul have higher U, Th, Pb and lower Co, Cr, Cu and Zn median values than those of Vale de Abrutiga.

This work focuses on the study of water–sediment interaction around abandoned uranium mines with open-pit lakes and mine dumps. Nineteen water and eleven stream sediment samples were collected in the abandoned Barrôco D. Frango mine, central Portugal. The trace element distribution was compared with other abandoned uranium mines in Portugal and worldwide. Generally, U, Th, and As contents in the open-pit water are high and similar to those of downstream water, suggesting its influence on aquatic systems. In abandoned mines with small to medium U exploitation, the stream sediments are moderately to heavily contaminated with U, Th and As, being U and As the most important contaminants, confirmed by their partition coefficients. A moderate to considerable potential ecological risk (34–79) was found around the abandoned Barrôco D. Frango mine area, mainly due to As contents in stream sediments. Water and stream sediments from abandoned U mines worldwide have U levels of up to 436 μg/L and 5024 mg/kg, respectively, while those from Barrôco D. Frango have 37.3 μg/L and 189 mg/kg, respectively. However, the longer the distance from the Barrôco D. Frango open-pit lake and mine dump, the higher U, Th and As contents in stream sediments, which is a warning indicator. Cluster heat maps of the water composition from four abandoned uranium mine areas show that Mondego Sul and Barrôco D. Frango mines are the most geochemically similar. Results show that stream sediments should be included in water quality management and future remediation plans of abandoned uranium mines.

The final publication is available at Springer via http://dx.doi.org/10.1007/s10653-017-9945-2

“This is a post-peer-review, pre-copyedit version of an article published in Environmental Geochemistry and Health. The final authenticated version is available online at: http://dx.doi.org/10.1007/s10653-019-00347-x”.