Sequestration of arsenic and molybdenum during the neutralization of uranium mill wastes: Key Lake mill, Saskatchewan, Canada
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The As- and Mo- bearing secondary mineral phases formed during the neutralization of uranium mill wastes were studied for a variety of ore blends including current and future ore sources at the Key Lake milling operation, northern Saskatchewan, Canada. A lab-scale plant model was employed to characterize secondary precipitates obtained during the mill waste neutralization process. Three scenarios of ore blends were processed through the lab-scale plant to produce mill waste solutions for neutralization before combination into final tailings. Slurry samples (n = 12) were collected from the secondary precipitates formed during the neutralization of mill wastes (raffinate) by precipitation with Ca(OH)2 (slaked lime) from pH 1.5 to 10.5. Synchrotron based X-ray absorption spectroscopy of mill and lab-scale plant precipitates showed arsenate adsorbed to ferrihydrite was the dominant As mineral phase regardless of pH or sample blend (53-77%), with fractional contributions from ferric arsenates, and adsorption to aluminum phases (AlOHSO4, As(OH)3 and hydrotalcite). Molybdate adsorbed to ferrihydrite was the dominant Mo mineral phase, regardless of pH or sample blend, with fractional contribution decreasing with increasing pH, and minor contributions from calcium molybdate, ferric molybdate and nickel molybdate. These results were used in geochemical modelling to predict the source terms for these mineral phases in tailings facilities. Sequestration of As and Mo in the model showed solubility was controlled by adsorption to both Fe and Al oxide surfaces as well as by direct precipitation with other dissolved constituents (Ni, Ca and SO4).The models developed pH profiles of mineral phase precipitation to explain the solubility of As, Mo, Fe, Al, Mg and Ni during sequestration from pH 1.5 to 10.5 that were consistent regardless of ore blend used in simulations. Since adsorption of anions to the surface of ferrihydrite has been shown to slow conversion to crystalline forms of Fe oxides (goethite and hematite) and sequestration of arsenate effectively controls As solubility at high pH (pH >10), As-bearing mineral phases are expected to be stable for thousands of years. With adsorption as well as direct precipitation considered, Mo phases though effectively sequestering below pH 8, became unstable and released Mo back into the tailings porewater (pH >10), as predicted by the thermodynamic model. Historical data obtained from as-discharged tailings as well as previously published U mill tailings studies agree with these findings.
DegreeMaster of Science (M.Sc.)
CommitteeKotzer, Tom; Moldovan, Brett J.; Essilfie-Dughan, Joseph
Copyright DateDecember 2015
secondary minerals, uranium milling, x-ray absorption spectroscopy, arsenic, molybdenum, neutralization