Micron-scale distribution controls metal(loid) release during simulated weathering of a Pennsylvanian coal shale

Singer, David M.; Herndon, Elizabeth; Cole, Kortney; Burkey, Michael; Morisson, Sarah; Cahill, Michael; Bartucci, Matthew A.

doi:10.1016/j.gca.2019.10.034

Micron-scale distribution controls metal(loid) release during simulated weathering of a Pennsylvanian coal shale

Journal Article · Sat Nov 02 00:00:00 EDT 2019 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2019.10.034· OSTI ID:1761688

Singer, David M. ^[1]; ^[2]; Cole, Kortney ^[1]; Burkey, Michael ^[1]; Morisson, Sarah ^[1]; Cahill, Michael ^[1]; Bartucci, Matthew A. ^[3]

Kent State Univ., Kent, OH (United States)
Kent State Univ., Kent, OH (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Thermo Fisher Scientific, Madison, WI (United States)

Coal mine spoil is a long-lasting legacy of historic coal mining operations that continues to impact water quality across Appalachia. Metal(loid) release from abandoned coal mine spoil, which can be a significant source of acid mine drainage (AMD), is dependent on speciation and distribution within the parent coal shale. This work aimed to determine how the micron- and sub-micron scale mineralogy, morphology, and texture of metal(loid)-bearing phases in a coal-shale control the rate and release of metal(loid)s during subsequent weathering through two primary objectives: (1) determine the microscale speciation and distribution of Fe and other metal(loid)s in a parent coal shale, and (2) determine the amount of metal(loid)s released during simulated weathering of shale physically crushed into silt- to sand-sized particles. This work was accomplished through a combination of electron microscopy and synchrotron-based X-ray microprobe analyses. Furthermore, this suite of techniques also provides insight into the geochemical history of the coal shale that could not be determined by bulk techniques. Trace elements were associated with either Fe-sulfides or with other phases that included metal(loid)-sulfides, aluminosilicates, and organic matter. Three distinct pools of Fe-sulfides were present: (i) larger mm-scale grains, with minimal internal fractures; (ii) μm- to mm-scale aggregates of μm-scale crystals forming secondary coatings on the larger mm-scale grains, and (iii) μm- to mm-scale aggregates forming framboidal grains. Fe-sulfide mineralogy was dominated by pyrite with minor contributions of marcasite and a S(-II)-bearing phase. Larger pyrite grains and their secondary coatings contained homogeneous distributions of Fe and Mn as well as other trace metal(loids) including V, Ti, Cr, As, Se, Cu, and Zn. Additionally, the fine-grained pyrite aggregates were strongly enriched in As and Se and contained discrete Cu- and Zn-bearing particles. Clays and organic matter surrounding the sulfide minerals were identified by micro-XRD and FT-IR spectroscopy. Simulated batch weathering of the physically crushed shale resulted in metal(loid) release that varied as function of size fraction and time. Metal(loid) release increased with decreasing particle size from sand-sized to silt-sized fractions. Although small amounts of Fe were released into solution after two days, the bulk of Fe release occurred after 10 days and continued for six months, after which Fe was gradually removed from solution. The weathering trends for Mn, Cu, Zn, and Ni were similar to Fe. In contrast, As and Se were characterized by rapid release into solution followed by removal prior to 10 days. These results indicate that micrometer-scale metal(loid) distribution within Fe sulfides controlled metal(loid) release into solution during simulated weathering of a coal shale. Specifically, elements concentrated in mineral coatings (As, Se) were rapidly mobilized in a short-lived pulse whereas elements associated with the larger grains (Fe, Mn, Cu, Zn, and Ni) exhibited a delayed but prolonged release into solution. The non-concomitant contaminant release indicates that an understanding of the textural relationships in the source material is required to understand weathering trends. This work highlights the importance of non-point sources of AMD, and addressing these sources is a critical step in improving water quality in the region.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; FG02-94ER14466

OSTI ID:: 1761688

Alternate ID(s):: OSTI ID: 1703162
OSTI ID: 1574161

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: 1 Vol. 269; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Data for: Micron-scale distribution controls metal(loid) release during simulated weathering of a Pennsylvanian coal shale Singer, David https://doi.org/10.17632/mrghjdg9mk The current record is supplemented by this dataset	dataset	January 2020
Data for: Micron-scale distribution controls metal(loid) release during simulated weathering of a Pennsylvanian coal shale Singer, David https://doi.org/10.17632/mrghjdg9mk.1 The current record is supplemented by this dataset	dataset	January 2020

Micron-scale distribution controls metal(loid) release during simulated weathering of a Pennsylvanian coal shale

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