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Secondary Sulfate Minerals Associated with Acid Drainage in the Eastern US: Recycling of Metals and Acidity in Surficial Environments

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Secondary Sulfate Minerals Associated with Acid Drainage in the Eastern US: Recycling of Metals and Acidity in Surficial Environments University of Nebraska - Lincoln DigitalCommons@University of Nebraska - Lincoln Geochemistry of Sulfate Minerals: A Tribute to Robert O. Rye US Geological Survey 2005 Secondary sulfate minerals associated with acid drainage in the eastern US: recycling of metals and acidity in surficial environments J.M. Hammarstrom U.S. Geological Survey R.R. Seal II U.S. Geological Survey A.L. Meier U.S. Geological Survey J.M. Kornfeld Dartmouth College Follow this and additional works at: https://digitalcommons.unl.edu/usgsrye Part of the Geochemistry Commons Hammarstrom, J.M.; Seal, R.R. II; Meier, A.L.; and Kornfeld, J.M., "Secondary sulfate minerals associated with acid drainage in the eastern US: recycling of metals and acidity in surficial environments" (2005). Geochemistry of Sulfate Minerals: A Tribute to Robert O. Rye. 2. https://digitalcommons.unl.edu/usgsrye/2 This Article is brought to you for free and open access by the US Geological Survey at DigitalCommons@University of Nebraska - Lincoln. It has been accepted for inclusion in Geochemistry of Sulfate Minerals: A Tribute to Robert O. Rye by an authorized administrator of DigitalCommons@University of Nebraska - Lincoln. Chemical Geology 215 (2005) 407–431 www.elsevier.com/locate/chemgeo Secondary sulfate minerals associated with acid drainage in the eastern US: recycling of metals and acidity in surficial environments J.M. Hammarstroma,*, R.R. Seal IIa, A.L. Meierb, J.M. Kornfeldc aU.S. Geological Survey, 954 National Center, Reston, Virginia 20192, USA bU.S. Geological Survey, 973 Denver Federal Center, Denver, Colorado 80225, USA cDartmouth College, Dartmouth, New Hampshire, USA Accepted 1 June 2004 Abstract Weathering of metal-sulfide minerals produces suites of variably soluble efflorescent sulfate salts at a number of localities in the eastern United States. The salts, which are present on mine wastes, tailings piles, and outcrops, include minerals that incorporate heavy metals in solid solution, primarily the highly soluble members of the melanterite, rozenite, epsomite, halotrichite, and copiapite groups. The minerals were identified by a combination of powder X-ray diffraction (XRD), scanning electron microscopy (SEM), and electron-microprobe. Base-metal salts are rare at these localities, and Cu, Zn, and Co are commonly sequestered as solid solutions within Fe- and Fe–Al sulfate minerals. Salt dissolution affects the surface- water chemistry at abandoned mines that exploited the massive sulfide deposits in the Vermont copper belt, the Mineral district of central Virginia, the Copper Basin (Ducktown) mining district of Tennessee, and where sulfide-bearing metamorphic rocks undisturbed by mining are exposed in Great Smoky Mountains National Park in North Carolina and Tennessee. Dissolution experiments on composite salt samples from three minesites and two outcrops of metamorphic rock showed that, in all cases, the pH of the leachates rapidly declined from 6.9 to b3.7, and specific conductance increased gradually over 24 h. Leachates analyzed after 24-h dissolution experiments indicated that all of the salts provided ready sources of dissolved Al (N30 mg LÀ1), Fe (N47 mg LÀ1), sulfate (N1000 mg LÀ1), and base metals (N1000 mg LÀ1 for minesites, and 2 mg LÀ1 for other sites). Geochemical modeling of surface waters, mine-waste leachates, and salt leachates using PHREEQC software predicted saturation in the observed ochre minerals, but significant concentration by evaporation would be needed to reach saturation in most of the sulfate salts. Periodic surface-water monitoring at Vermont minesites indicated peak annual metal loads during spring runoff. At the Virginia site, where no winter-long snowpack develops, metal loads were highest during summer months when salts were dissolved periodically by rainstorms following sustained evaporation during dry spells. Despite the relatively humid climate of the eastern United States, where precipitation typically exceeds evaporation, salts form intermittently in open * Corresponding author. Tel.: +1 703 648 6165; fax: +1 703 648 6252. E-mail address: [email protected] (J.M. Hammarstrom). 0009-2541/$ - see front matter. Published by Elsevier B.V. doi:10.1016/j.chemgeo.2004.06.053 408 J.M. Hammarstrom et al. / Chemical Geology 215 (2005) 407–431 areas, persist in protected areas when temperature and relative humidity are appropriate, and contribute to metal loadings and acidity in surface waters upon dissolution, thereby causing short-term perturbations in water quality. Published by Elsevier B.V. Keywords: Sulfate minerals; Mineralogy; Acid rock drainage; Eastern USA 1. Introduction assemblages contribute to acid mine drainage at many coal mines in the eastern US, the base-metal Secondary sulfate minerals play an important role concentrations of minerals and associated waters in acid drainage and metal sequestration in surface typically are lower than those observed at base-metal environments. Efflorescent blooms of hydrated metal mines (Cravotta, 1994; Rose and Cravotta, 1998; salts have long been recognized as products of Cravotta et al., 1999). evaporation of acid-sulfate waters that form from Secondary sulfate minerals associated with acid oxidative weathering of Fe-sulfide and other sulfide drainage in the eastern US include efflorescent salts minerals. Recent emphasis on the environmental and Fe- and Al-hydroxysulfate minerals (Palache et significance of sulfate minerals has spawned a al., 1951; Dagenhart, 1980; Cravotta, 1994; Flohr et renewed interest in these minerals as indicators of al., 1995; Byerly, 1996; Coskren and Lauf, 1996; water quality and as monitors of water–rock Nordstrom and Alpers, 1999; Bigham and Nordstrom, interactions (Alpers et al., 2000). Because of the 2000). Weathering of pyrite [FeS2] and pyrrhotite high solubility of many of the efflorescent sulfate [Fe1ÀxS] provides the primary source of Fe and minerals, climate is an important control on mineral acidity that leads to precipitation of sulfate minerals formation and mobilization of metals. In wet by myriad processes including oxidation, hydrolysis, climates, salts are ephemeral unless they develop and evaporation. A variety of simple hydrated salts in sheltered areas. In arid climates, or during can form, among which those of divalent cations have 2+ 2+ prolonged dry periods in humid climates, thick the general formula M SO4d nH2O, where M=Fe , crusts of salts can form by evaporative processes, Mg, Zn, Ca, and Cu, as well as mixed divalent– where upward migration of water by capillary action trivalent salts. The most common mineral groups that is the dominant process (Olyphant et al., 1991; form efflorescent salts by natural weathering in Dold, 1999). Dissolution of accumulated highly metal-rich environments include: (1) monoclinic soluble sulfate salts during spring snowmelt runoff sulfates of the melanterite group, having the general 2+ or rainstorms can have short-term, catastrophic formula M SO4d 7H2O, where M=Co, Cu, Fe, Mn, effects on metal loadings and on aquatic ecosystems Zn; (2) orthorhombic sulfates of general formula 2+ (Nordstrom, 1977; Dagenhart, 1980; Olyphant et al., M SO4d 7H2O, where M=Mg, Zn, or Ni; (3) 1991; Bayless and Olyphant, 1993; Keith et al., monoclinic sulfates of the hexahydrite group, general 2+ 2001). formula M SO4d 6H2O, where M=Co, Cu, Fe, Mg, More than 100 inactive or abandoned mines and Mn, Ni, Zn; (4) triclinic sulfates of the chalcanthite 2+ prospects associated with massive sulfide deposits group, M SO4d 5H2O, where M=Cu, Fe, Mg, Mn; are documented in the eastern US (Fig. 1). Although (5) monoclinic sulfates of the rozenite group, 2+ most are small, some represent significant, historical M SO4d 4H2O, where M=Co, Cd, Fe, Mg, Mn, Ni, mining districts that were active until about 1960. Zn; (6) monoclinic sulfates of the halotrichite group, 2+ 2+ Some minesites have recently become the focus of AB2(SO4)4d 22H2O, where A=Fe , Mg, Mn , Ni, federal, state, or local remediation activities because Zn; B=Al, Cr3+,Fe3+; and (7) triclinic sulfates of the of the emanation of acid mine drainage. The cycling copiapite group, which includes mixed-valence min- 2+ 3+ of metals and acid by the precipitation and dis- erals of general formula A Fe4 (SO4)6(OH)2d 18– solution of efflorescent salts is an important process 20H2O, wherein A=Ca, Cu, Fe, Mg, Zn, and trivalent at these sites. Although similar sulfate-mineral minerals in the group have the general formula J.M. Hammarstrom et al. / Chemical Geology 215 (2005) 407–431 409 Fig. 1. Study areas. Black dots show locations of inactive mines, prospects, and mineral occurrences classified as massive sulfide-type mineral deposits in the eastern US (McFaul et al., 2000). 3+ 3+ B2/3 Fe4 (SO4)6(OH)2d 20H2O, wherein B=Al, Fe. effectively recycle metals and acidity in surficial Iron hydroxysulfate minerals include the character- environments. istic ochre minerals of acid mine drainage, schwert- In this paper, we describe field occurrences and mannite and jarosite. Secondary Al sulfates typically mineralogical data for sulfate minerals associated are amorphous, although crystalline alunogen and with oxidative weathering of sulfide minerals at felsfba´nyaite (basaluminite) are locally observed. several localities in the eastern US. We also compare Surface accumulations of sulfate minerals form by the effects of sulfate-mineral dissolution on stream evaporation and precipitation within ponded surface metal load as a function of climate. Study areas waters, on wet surfaces, at seeps, in
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