Arsenic Geochemistry of Alluvial Sediments and Pore Waters Affected by Mine Tailings along the Belle Fourche and Cheyenne River Floodplains

Abstract

Gold mining operations in the northern Black Hills of South Dakota resulted in the discharge of arsenopyrite-bearing mine tailings into Whitewood Creek from 1876 to 1977. Those tailings were transported further downstream along the Belle Fourche River, the Cheyenne River, and the Missouri River. An estimated 110 million metric tons of tailings remain stored in alluvial deposits of the Belle Fourche and Cheyenne Rivers. Pore-water dialysis samplers were deployed in the channel and backwaters of the Belle Fourche and Cheyenne Rivers to determine temporal and seasonal changes in the geochemistry of groundwater in alluvial sediments. Alluvial sediment adjacent to the dialysis samplers were cored for geochemical analysis. In comparison to US Environmental Protection Agency drinking water standards and reference concentrations of alluvial sediment not containing mine tailings, the Belle Fourche River sites had elevated concentrations of arsenic in pore water (2570 μg/L compared to 10 μg/L) and sediment (1010 ppm compared to < 34 ppm), respectively. Pore water arsenic concentration was affected by dissolution of iron oxyhydroxides under reducing conditions. Sequential extraction of iron and arsenic from sediment cores indicates that substantial quantities of soluble metals were present. Dissolution of arsenic sorbed to alluvial sediment particles appears to be affected by changing groundwater levels that cause shifts in redox conditions. Bioreductive processes did not appear to be a substantial transport pathway but could affect speciation of arsenic, especially at the Cheyenne River sampling sites where microbial activity was determined to be greater than at Belle Fourche sampling sites.

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Acknowledgements

This study was conducted in cooperation with the US Geological Survey, Cheyenne River Sioux Tribe, and the US Army Corps of Engineers, and in collaboration with the South Dakota School of Mines and Technology. Any use of trade, product, or firm names is for descriptive purposes only and does not imply endorsement by the US Government.

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Correspondence to James J. Stone.

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Tables of data used to generate all figures, graphical site sampling locations, sequential chemical extraction results, Biolog average well color development (AWCD) trends and substrate utilization radar plots, and sieve analysis results are provided in Supporting Information.

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Pfeifle, B.D., Stamm, J.F. & Stone, J.J. Arsenic Geochemistry of Alluvial Sediments and Pore Waters Affected by Mine Tailings along the Belle Fourche and Cheyenne River Floodplains. Water Air Soil Pollut 229, 183 (2018). https://doi.org/10.1007/s11270-018-3836-8

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Keywords

  • Mine tailings
  • Arsenic transport
  • Arsenic speciation
  • Sequential extraction
  • Iron dissolution