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Frequency Distribution of the Ph of Coal-Mine Drainage in Pennsylvania

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Frequency Distribution of the Ph of Coal-Mine Drainage in Pennsylvania Frequency Distribution of the pH of Coal-Mine Drainage in Pennsylvania By Charles A. Cravotta III, Keith B.C. Brady, Arthur W. Rose, and Joseph B. Douds ABSTRACT The pH of coal-mine drainage in Pennsylvania has a bimodal frequency distribution, with modes at pH 2.5 to 4 (acidic) and pH 6 to 7 (near neutral). Although iron-disulfide and calcareous minerals comprise only a few percent, or less, of the coal-bearing rock, these minerals are highly reactive and are mainly responsible for the bimodal pH distribution. Field and laboratory studies and computer simulations indicate that pH will be driven toward one mode or the other depending on the relative abundance and extent of weathering of pyrite (FeS2; acid-forming) and calcite (CaCO3; acid-neutralizing). The pH values in the - - near-neutral mode result from carbonate buffering (HCO3 /H2CO3 and HCO3 /CaCO3) and imply the presence of calcareous minerals; acid produced by pyrite oxidation is neutralized. The pH values in the acidic mode result from pyrite oxidation and imply a deficiency of calcareous minerals and the absence of carbonate buffering. The oxidation of only a small quantity of pyrite can acidify pure water (0.012 g·L-1 -1 2- FeS2 produces pH~4 and 20 mg·L SO4 ); however, because of the log scale for pH and ion complexation 2- - 3+ 2+ (SO4 /HSO4 and Fe /FeOH ), orders of magnitude greater oxidation is required to produce pH < 3. Laboratory leaching experiments showed that for a specific proportion of FeS2:CaCO3, effluents produced under variably saturated hydrologic conditions, in which oxygen availability and pyrite oxidation were enhanced, had lower pH and greater dissolved solids concentrations than effluents produced under contin- uously saturated conditions, in which oxygen availability and pyrite oxidation were diminished. INTRODUCTION Geochemistry of Coal Mine Drainage In the northern Appalachian Plateau of the Ground water and associated mine discharges eastern United States, drainage from abandoned in the coalfields of Pennsylvania range widely in coal mines affects more than 8,000 km of streams quality from near-neutral, or “alkaline” (alkalinity and associated ground water (Boyer and Sarnoski, > acidity; pH > 6), to strongly acidic (Rose and Cra- 1995). Most affected streams are in Pennsylvania, votta, 1998). The pH of coal-mine drainage in where contaminated mine runoff and mine dis- Pennsylvania has a bimodal frequency distribution charges impair water quality in 45 of 67 counties (Brady and others, 1997, 1998); most samples are (Pennsylvania Department of Environmental Pro- either near neutral (pH 6 to 7) or distinctly acidic tection, 1998). An understanding of factors affect- (pH 2.5 to 4), with few samples having pH 4.5 to 5.5 ing the chemistry of coal-mine drainage is needed (fig.1). The bimodal pH distribution is apparent for for the effective planning and implementation of other regional compilations of water-quality data future mining and remediation of abandoned mine lands. This paper evaluates geochemical and hydro- for coalfields in West Virginia (diPretoro, 1986), logical factors affecting the pH of coal-mine drain- Ohio (Helsel and Hirsch, 1992, p. 61), and Ger- age. Data for ground-water and discharge samples many (Klapper and Schultze, 1995). Whether near and laboratory leaching experiments are presented neutral or acidic, the drainage from most coal mines to explain regional water-quality trends for the has elevated concentrations of dissolved solids, -1 northern Appalachian coalfields. Geochemical sim- ranging from about 200 mg·L to greater than -1 ulations demonstrate the range of effects on pH 10,000 mg·L . In contrast, ground water and spring from different variables, including the amount of water from unmined areas typically are near neutral pyrite oxidized, buffering by carbonate minerals, and are dilute compared to water from mined areas and the formation of secondary minerals. (Brady and others, 1996; Rose and Cravotta, 1998). solution of carbonate, oxide, and aluminosilicate 20 A minerals by acidic water. Near-neutral mine drainage can form from 15 rock that lacks pyrite or can originate as AMD that has been neutralized by reaction with calcareous 10 minerals (Cravotta and others, 1994; Blowes and Ptacek, 1994). In near-neutral mine waters, bicar- - 5 bonate (HCO3 ) is a significant anion along with 2- 2+ SO4 ; concentrations of dissolved calcium (Ca ) and magnesium (Mg2+) generally are elevated rela- FREQUENCY, IN PERCENT (N = 252) FREQUENCY, 0 3+ 3+ 201 23456789 tive to dissolved Fe and Al , which precipitate as B pH increases to above 4 to 5. For example, dissolu- tion of calcite neutralizes acid and can increase the 15 - - 2- pH and alkalinity ([OH ] + [HCO3 ] + 2 [CO3 ]) of mine water: 10 + ↔ 2+ * CaCO3(s) + 2H Ca + H2CO3 (3) 5 * ↔ 2+ - CaCO3(s) + H2CO3 Ca + 2 HCO3 (4) * o where [H2CO3 ] = [CO2 (aq)] + [H2CO3 ] (Stumm FREQUENCY, IN PERCENT (N = 793) FREQUENCY, 0 1 23456789 and Morgan, 1996). However, because the rate of pH pyrite oxidation can exceed the rate of calcite disso- Figure 1. Frequency distribution of the pH of coal- lution, particularly where oxygen is abundant, the mine discharges in Pennsylvania. A, Data for 252 pH and alkalinity of mine water will not necessarily coal-mine discharges in the anthracite coalfield increase in the presence of calcite. (source: Growitz and others, 1985); B, Data for 793 surface coal-mine discharges in the Ion complexation, principally the protolysis bituminous coalfield (source: Hellier, 1994). Class of anions and the hydrolysis of cations (Stumm and intervals for pH + 0.25. Morgan, 1996), also can be a significant process that stabilizes, or “buffers,” the pH of mine water. Acidic mine drainage (AMD) is character- For example, pH can be buffered in the near-neutral ized by elevated concentrations of dissolved and range by the protolysis reaction involving bicarbon- 2- particulate iron (Fe) and dissolved sulfate (SO4 ) ate and carbonic acid (pK=6.35; thermodynamic produced by the oxidation of pyrite (FeS2): data from Ball and Nordstrom, 1991): FeS + 3.5 O + H O → Fe2+ + 2 SO 2- + 2 H+ (1) - + ↔ 2 2 2 4 HCO3 + H H2CO3* (5) 2+ → + Fe + 0.25 O2 + 2.5 H2O Fe(OH)3(s) + 2 H (2) Similarly, pH can be buffered in the acidic range by Half the acid (H+) is produced by the oxidation of the protolysis reaction involving sulfate and bisul- pyritic S (reaction 1), and half results from the oxi- fate (pK=2.0) dation and hydrolysis of pyritic Fe (reaction 2). 2- + ↔ - SO4 + H HSO4 , (6) Generally, mines that produce AMD feature inter- connected underground “workings” (voids and rock and by hydrolysis reactions involving ferric ions, rubble) or aboveground “spoil” (rubble and rejected such as the initial hydrolysis step (pK=2.2), coal) where pyrite has been exposed to oxygenated Fe3+ + H O ↔ FeOH2+ + H+.(7) air and water and where the calcareous minerals, 2 calcite (CaCO3) and dolomite (CaMg(CO3)2), are The importance of the above reactions will depend absent or deficient relative to pyrite (Hornberger on the dissolved solute content of the water, the and others, 1990; Brady and others, 1994; Cravotta, nature and abundance of acid-producing and neu- 1994; Rose and Cravotta, 1998; Nordstrom and tralizing materials along flow paths, the sequence Alpers, 1999). Concentrations of manganese and intimacy of contact between the water and these (Mn2+), aluminum (Al3+), and other solutes in materials, as well as the ability of the rock to trans- AMD commonly are elevated due to aggressive dis- mit water and air. Geologic and Hydrologic Framework mining to indicate the potential for AMD formation and to develop a materials handling plan (Brady and Bituminous coal deposits underlie western others, 1994), the quality and movement of water and north-central Pennsylvania, and anthracite within the resultant mine spoil and backfill are dif- deposits underlie east-central and northeastern ficult to predict. Pennsylvania (fig. 2). The mineable coals, mostly of Surface mines and underground mines in the Pennsylvanian Age, are interbedded with shale, silt- bituminous coalfield generally can be categorized stone, sandstone, and occasional limestone (Brady as “updip” or “downdip” depending on the direction and others, 1998). The bituminous coalfield lies that mining proceeded relative to the dip of the coal within the Appalachian Plateaus Physiographic bed. In the past, most bituminous mines were mined Province and is characterized by gently dipping updip so that water would drain freely and pumping strata; nearly horizontal coalbeds commonly crop costs would be minimized. Updip mines also pro- out in the incised stream valleys. The anthracite vided greater access of oxygen to the subsurface, coalfield lies within the adjacent Ridge and Valley however, which facilitates the oxidation of pyrite Physiographic Province, which is characterized by and the formation of AMD (Hornberger, 1985). In complexly deformed strata. Mineable anthracite contrast, downdip mines tend to fill with ground beds are present primarily in steeply folded and water, which requires pumping during active min- fractured synclinal troughs. ing but also reduces the access of oxygen to pyritic rock. Upon mine closure, substantial parts of down- Bituminous Coalfield Anthracite Coalfield dip mines can be permanently inundated thereby minimizing oxygen transport and pyrite oxidation. Hence, the downdip mines generally produce less acidic water than updip mines; however, unless cal- careous strata are present, they may not produce near-neutral water. Most anthracite mines were developed as large underground mine complexes, where shafts and tunnels connected mine workings within multi- ple coalbeds. Because anthracite mines commonly Figure 2. Locations of bituminous and anthracite were developed hundreds of meters below the coalfields in Pennsylvania (modified from regional water table and because of the large size of Pennsylvania Geological Survey, 1964). most underground mine complexes, their discharge volumes (overflows or tunnels) tend to be substan- Coal-bearing rocks in the northern Appala- tially greater than those from surface mines.
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