Quantification of mineral weathering rates in sulfidic mine tailings under water-saturated conditions

Detta är en avhandling från Stockholm : Institutionen för geologi och geokemi

Sammanfattning: Tailings are a fine-grained waste product produced during the metal recovery process. Tailings consist mostly of different silicates but also sulfides (e.g. pyrite), since 100 % metal recovery is not possible. Freshly processed tailings are deposited in large impoundments. If the mine tailings in the impoundments are exposed to water and oxygen, the sulfides will oxidize and release acidity and metals such as Fe, Cu, Zn, and Pb. The sulfide mineral oxidation reactions are catalyzed by sulfur and iron oxidizing bacteria (principally Acidithiobacillus ferrooxidans) that oxidize ferrous iron to ferric iron, which then oxidizes pyrite. When the leachate produced by this process discharges from the impoundment, it is called acid mine drainage, which may lead to the pollution of adjacent streams and lakes.The intention with this thesis is to investigate and quantify mineral weathering processes and element release rates occurring in water-saturated and soil-covered sulfidic mine tailings. The study was performed in different batch and column experiments in room temperature and in the laboratory. The batch experiments were conducted for ca. three months and investigated: a) microbial and abiotic sulfide oxidation in freshly processed tailings under oxic conditions at pH 2-3 and pH 8, b) microbial oxidation of pure pyrite grains at pH 2-3 under different oxygen concentrations ranging from anoxic to oxic conditions. The column experiments, consisting of unoxidized tailings in water-saturated columns, were conducted for up to three years. In these experiments, an oxygen-saturated solution was continually pumped into the column inlet, and investigated: a) differences in oxidation rates between tailings of two different grain sizes, b) factors affecting element discharge rates, acid neutralization, and sulfide oxidation, c) the effect of ions released in a soil cover on release rates in the tailings.Sulfide oxidation processes within the batch experiments were limited by surface kinetics. The microbial oxidation of pure pyrite at atmospheric conditions produced the most rapid rate, while the microbial oxidation of pure pyrite at anoxic conditions was slower by 1.8 orders of magnitude. Microbial and abiotic oxidation of pyrite in freshly-processed tailings resulted in pyrite oxidation rates that were intermediate between these two extremes. The results from the microbial experiments with pure pyrite indicated a positive correlation between the concentration of dissolved oxygen, ferric iron and bacterial cells (at a total cell concentration > 106 cells/mL and a dissolved oxygen concentration ? 13.2 µM), which implies an interdependence of these factors. The results from these batch experiments support the indirect mechanism for microbial oxidation by the ferric oxidation pathway. Pyrite oxidation rates estimated from the batch experiments may be comparable with oxidation rates in the unsaturated zone and at the groundwater table in a tailings impoundment.Acid neutralization reactions in the column experiments resulted in the release of base cations to the column leachate. Calcite was the most important neutralizing mineral despite that it was only present in minor amounts in the tailings. It was confirmed that acidity forced the calcite dissolution. Element release rates in the column experiments were controlled by the availability of dissolved oxygen, which was a function of the water flow rate into the column. These column experiments also showed that the results are comparable with results from field studies, justifying the use of column experiments to study processes within tailings impoundments.