Sphalerite weathering and controls on Zn and Cd migration in mine waste rock: An integrated study from the molecular scale to the field scale
- Univ. of Waterloo, ON (Canada)
- Univ. of Ottawa, ON (Canada)
- Univ. of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.; Argonne National Lab. (ANL), Argonne, IL (United States)
Degraded water quality and environmental impacts caused by weathering of sulfide-bearing mine wastes are a legacy remaining at many historical mine sites. Release and mobilization of toxic metals (e.g., Zn and Cd) in mine drainage are often associated with weathering of primary sulfide minerals and precipitation and dissolution of secondary minerals. This study aims to couple field-scale measurements of physicochemical parameters with lm-and nm-scale mineralogical characterization to investigate sphalerite weathering and controls on Zn and Cd migration in an uncovered mine waste-rock pile. Elevated concentrations of Zn and Cd, potentially harmful to the receiving environment, were detected in waste-rock pore water and seepage. A suite of analytical techniques, including scanning electron microscopy - energy dispersive X-ray spectroscopy (SEM-EDS), scanning transmission electron microscopy (STEM) with EDS, electron microprobe analysis (EMPA), and synchrotron-based micro X-ray fluorescence (mu-XRF) mapping and micro X-ray absorption near edge structure (mu-XANES) spectroscopy were utilized in a high-resolution investigation of elemental-and secondary-mineral associations with sphalerite grains. EMPA and mu-XRF elemental maps and STEM investigations show depletion of Zn, Fe, S, and Cd, local enrichment of Cu, and distinct dissolution pits at the margins of sphalerite grains. Using mu-XANES, the speciation of solid phases containing Zn, Cu, Fe, and S indicates the dominance of primary sphalerite with microscopic inclusions of chalcopyrite, along with sparse occurrence of secondary Cu-bearing sulfides formed during weathering. These results suggest sphalerite oxidation leads to congruent dissolution without formation of distinct secondary-mineral coatings. Sphalerite weathering significantly contributes to elevated aqueous concentrations of Zn and Cd. Field-scale observations and mineralogical investigations indicate common occurrence of Fe-oxyhydroxides in the waste-rock pile. Seepage chemistry and surface complexation modeling results suggest that pH-dependent variations in reactions on the surfaces of the Fe-oxyhydroxides control aqueous concentrations of Zn and Cd, and the Zn/Cd ratio in the seepage. This work highlights the importance of understanding the mechanisms of sulfide-mineral oxidation and subsequent surface precipitation and adsorption, such that appropriate remediation action can be implemented to limit mobilization of metals to sensitive ecosystems.
- Research Organization:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER); Natural Sciences and Engineering Research Council of Canada (NSERC); National Science Foundation (NSF)
- Grant/Contract Number:
- AC02-06CH11357; FG02-94ER14466; EAR-1634415; 479708-15
- OSTI ID:
- 1881431
- Journal Information:
- Geochimica et Cosmochimica Acta, Vol. 318; ISSN 0016-7037
- Publisher:
- Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement
- Country of Publication:
- United States
- Language:
- English
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