Sulphide oxidation, oxygen diffusion and metal mobility in sulphide-bearing mine tailings in Northern Sweden

Abstract: Large quantities of sulphide-bearing mining wastes produced from ore processing are deposited throughout the world. Sulphide oxidation in the wastes may release acidic water with high concentrations of metals to the environment. Remediation strategies are usually site specific, since the physical and chemical properties of the wastes vary. Therefore, sulphide oxidation, oxygen diffusion and metal mobility in unoxidised and oxidised, remediated and unremediated wastes have been studied in the present work. The efficiency of different cover systems on unoxidised tailings from Kristineberg, were studied in pilot-scale test cells (5'5'3 m3)under field conditions. Clayey till, sewage sludge, apatite and Trisoplast were used as sealing layers and unspecified till as a protective cover. In one cell tailings were left uncovered. Unoxidised tailings in the test-cells in the initial stage after deposition showed relatively low sulphur release (600- 800 mg/l)in leachate waters, which probably was an effect of high moisture content in the tailings prior to deposition. Near-neutral pH found in the leachates was an effect of neutralisation by carbonate minerals present and lime (Ca(OH)2) added prior to deposition. Similar sulphur concentrations were found also in the uncovered tailings. The sulphide oxidation rate increased with time in the uncovered tailings, and decreased in the covered. The lowest oxygen concentrations were observed below the cover system with sewage sludge, which was the most effective barriar against oxygen in a short-term perspective. The oxygen fluxes through the clayey till and apatite layers were within the same magnitude and varied between 0.5 and 4 mole/year,m2. The Trisoplast layer seemed to have failed as a barrier against oxygen. Tailings studied at field scale at Laver and Kristineberg had oxidised for more than 50 years. The tailings at Kristineberg have high pyrite content (c.25% and 50%) and those at Laver have low grade of pyrrhotite (2-3%). The Laver tailings are unremediated, while at Kristineberg the tailings were remediated in 1996. The transport of metals in the drainage water at Laver decreased during a study period of 8 years. The transport of dissolved sulphur indicated a declining trend of sulphide oxidation rate in the tailings, which was confirmed by oxygen measurements in the tailings and weathering rate estimations. The decline was considered to be natural as a result of the increased distance that oxygen has to travel to reach unoxidised sulphide grains. The major part of the amounts of metals released by sulphide oxidation were secondarily retained in the tailings, and to a small extent in layers cemented by jarosite and Fe-(oxy)hydroxides. Sequential extraction of these layers showed that metals such as Cu and Pb were mostly associated with crystalline Fe-(oxy)hydroxides. Most important retention mechanism was, however, sorption onto minerals surfaces below the oxidation front. The studied Impoundment 1 at Kristineberg was remediated by two different methods; on one part a dry cover consisting of a sealing layer and a protective cover were applied, and the groundwater table was raised and a single dry cover applied on the other part. When the groundwater table was raised in oxidised tailings, secondarily retained metals such as Fe, Mg, Mn, S and Zn were remobilised resulting in increased concentrations in the groundwater. The concentrations declined with time, due to dilution by inflowing uncontaminated water. Decreased concentrations of Fe, Mg, Mn, S and Zn were observed also in the groundwater below the dry cover as the amount of percolating water decreased. The concentrations of trace elements such as Cd, Co, Cr, Cu, Ni and Pb were almost depleted in the groundwater, since these metals were retained within the tailings by mechanisms such as co-precipitation, precipitation and sorption. Analysis of pyrite grains by LA-ICP-SMS showed that pyrite surfaces were important for retention of As and Cu, in particular, but also for Cd and Zn. This study shows that the physico-chemical conditions expressed by pH and redox potential have a large impact on element mobility’s. For example, As was mobilised as a result of remediation, while the concentrations of most metals decreased in the drainage waters.