|dc.description.abstract||Water quality degradation is the foremost environmental issue faced by the mining industry. Negative impacts on water quality are commonly associated with unmitigated drainage emanating from sulfide-bearing mine waste deposits. These impacts stem from the liberation of acidity, sulfate, metals (e.g. Fe, Ni, Cu, Zn and Pb), and trace elements (e.g. Co, As, Cd, Sb and Tl) during the oxidation of sulfide minerals. Drainage at operational mines is commonly treated using techniques such as chemical oxidation and acid neutralization, which can succeed in achieving regulatory discharge guidelines. However, active treatment techniques are commonly burdened by high capital and operating costs. The development of passive technologies for treatment of mine drainage, which promote sulfate reduction, metal-sulfide precipitation and alkalinity production, therefore present a cost-effective alternative for managing mine drainage quality. This thesis describes laboratory and field evaluations of techniques for passive in situ treatment of acidic and neutral mine waters.
Laboratory batch experiments evaluated the treatment of acid mine drainage (AMD) with mixtures of organic carbon and zero-valent iron (ZVI) for use in permeable reactive barriers (PRBs). Modest increases in sulfate-reduction rates up to 15 % were achieved by amending organic carbon mixtures with 5 to 10 % (dry wt.) ZVI. Reactive mixtures containing organic carbon supported growth of sulfate-reducing bacteria (SRB) and facilitated removal of Fe, Zn, Cd, Ni, Co and Pb. However, organic carbon was necessary to support SRB growth and sulfate reduction. Removal of Zn, Cd, Ni, Co and Pb in the absence of organic carbon is attributed to sorption and (co)precipitation reactions at the ZVI surface. Scanning electron microscopy (SEM) and X-ray absorption near-edge structure (XANES) spectroscopy confirmed the presence of secondary Fe-sulfides in mixtures containing organic carbon. The dominant reaction product in these mixtures was identified as disordered mackinawite [Fe1+xS]. The addition of ZVI to organic carbon enhanced AMD treatment over the duration of this experiment; however, long-term evaluation is required to identify optimal reactive mixtures.
Field-based investigations into passive management of near-neutral pH tailings pore-water were carried out at the Greens Creek mine, located near Juneau, Alaska, USA. These studies focused on delineation of mechanisms controlling tailings pore-water chemistry, and a evaluation of the effectiveness of organic carbon amendment of tailings for passive in situ management of pore-water quality.
Results demonstrate that sulfide-mineral oxidation and carbonate dissolution are the primary influences on tailings pore-water composition. Pyrite [FeS2] accounted for < 20 to > 35 wt. % of the tailings mineral assemblage, whereas dolomite [CaMg(CO3)2] and calcite [CaCO3] were present at ≤ 30 and 3 wt. %, respectively. The sulfide-mineral assemblage was dominated by pyrite; however, sphalerite [(Zn,Fe)S] and galena [PbS] were commonly observed, and tetrahedrite [(Fe,Zn,Cu,Ag)12Sb4S13], arsenopyrite [FeAsS], and chalcopyrite [CuFeS2] were present in lesser amounts. Geochemical analysis of tailings core samples generally agreed with mineralogical data. The occurrence of Cd, Cr, Co, Mo, Ni, Se, and Tl is attributed to their occurrence as impurities in primary sulfide phases. Most probable number (MPN) populations of neutrophilic sulfur-oxidizing bacteria (nSOB) and SRB were elevated at several locations within the tailings deposit. Near-neutral pH conditions dominated; however, elevated concentrations of dissolved SO4, S2O3, Fe, Zn, As, Sb, and Tl were observed within and below the oxidation zone.
Field-scale experiments conducted over four years evaluated passive in situ treatment of pore-water by amending unoxidized tailings with 5 and 10 vol. % organic carbon. Field-scale cells were constructed to evaluate amendments containing differing mixtures of peat, dried spent brewing grain (SBG), and municipal biosolids (MB). Organic carbon amendment of the tailings supported the development of conditions favorable to sulfate reduction. Decreases in aqueous SO4 concentrations were observed in three cells amended with mixtures of peat, SBG, and MB. Removal of SO4 was generally accompanied by H2S production, enrichment in 34S-SO4, and increased SRB populations. Undersaturation of pore-water with respect to gypsum was observed. Sulfate reduction was sustained for the duration of the experiment in cells amended with 5 vol. % peat + SBG and 10 vol. % peat + SBG + MB. The addition of organic carbon also supported reductive dissolution of Fe(III) (oxy)hydroxides and mobilization of Fe and As. The largest increases in aqueous Fe and As concentrations were observed in cells amended with MB. Subsequent decreases in Fe and As concentrations were observed under sulfate-reducing conditions. Attenuation of Zn, Sb, and Tl accompanied SO4 removal. Mineralogical examination by SEM revealed the presence of secondary Zn-S and Fe-S precipitates on surfaces of organic carbon particles, and carbonate and aluminosilicate grains. This study demonstrates that amendment of tailings with a small and dispersed mass of organic carbon has potential to improve the quality of tailings pore water.||en