Evaluating Leachability of Residual Solids Generated from Unconventional Shale Gas Production Operations in Marcellus Shale

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Virginia Tech

Hydraulic fracturing operations utilized for shale gas production result in the generation of a large volume of flowback and produced water that contain suspended material, salts, hydrocarbons, metals, chemical additives, and naturally-occurring radioactive material. The water is impounded at drilling sites or treated off-site, resulting in significant generation of residual solids. These are either buried on site or are disposed in lined landfills. The objective of this study was to determine the levels of heavy metals and other elements of concern that will leach from these residual solids when placed in typical disposal environments.

For this purpose, laboratory leaching experiments were employed wherein representative samples were brought into contact with a liquid to determine the constituents that would be leached by the liquid and potentially released into the environment. The samples used included sludge resulting from the physicochemical treatment of process water (TS), sludge solidified with cement kiln dust (SS), raw solids obtained by gravity separation of process water (RS), and drilling mud (DM). The samples were subjected to both single extraction (i.e. Shake Extraction Test, SET) and multiple extraction (i.e. Immersion Test, IT) leaching tests. For the shake extraction test, samples were mixed with a specific amount of leaching solution without renewal over a short time period. In the immersion test, samples were immersed in a specific amount of leaching solution that was periodically renewed over a longer period of time. For both these tests, analyses were performed on the filtered eluate. The tests were performed as per standards with modifications. Distilled de-ionized water, synthetic acid rain (pH ~ 4.2), weak acetic acid (pH ~ 2.88), and synthetic landfill leachate were used as leaching solutions to mimic specific disposal environments.

Alkali metals (Li, K, Na), alkaline earth metals (Ba, Ca, Mg, Sr) and a halide (Br), which are typically associated with Marcellus shale and produced waters, leached at high concentrations from most of the residual solids sample. The SS sample, due to its stabilization with CKD, had a lower extraction efficiency as compared to the unconsolidated TS and RS samples. In EF 2.9 and EF SLL, the leaching took place under acidic conditions, while for EF DDI and EF 4.2, the leaching occurred in alkaline conditions. EF 2.9 and EF SLL were determined to be the most aggressive leaching solutions, causing the maximum solubility of most inorganic elements. Thus, high amounts of most EOCs may leach from these residual solids in MSW landfills disposed under co-disposal conditions. Agitation, pH and composition of the leaching solution were determined to be important variables in evaluating the leaching potential of a sample.

The results of this study should help with the design of further research experiments being undertaken to develop environmentally responsible management/disposal strategies for these residual solids and also prove useful for regulatory authorities in their efforts to develop specific guidelines for the disposal of residuals from shale gas production operations.

hydraulic fracturing, unconventional shale gas production operations, Marcellus shale, residual solids, hydraulic fracturing sludge, produced water treatment by-products, drilling mud, leaching tests, flow around immersion test, shake extraction test