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Title: Experimental insights into geochemical changes in hydraulically fractured Marcellus Shale

Abstract

Hydraulic fracturing applied to organic-rich shales has significantly increased the recoverable volume of methane available for U.S. energy consumption. Fluid-shale reactions in the reservoir may affect long-term reservoir productivity and waste management needs through changes to fracture mineral composition and produced fluid chemical composition. We performed laboratory experiments with Marcellus Shale and lab-generated hydraulic fracturing fluid at elevated pressures and temperatures to evaluate mineral reactions and the release of trace elements into solution. Results from the experiment containing fracturing chemicals show evidence for clay and carbonate dissolution, secondary clay and anhydrite precipitation, and early-stage (24-48 h) fluid enrichment of certain elements followed by depletion in later stages (i.e. Al, Cd, Co, Cr, Cu, Ni, Sc, Zn). Other elements such as As, Fe, Mn, Sr, and Y increased in concentration and remained elevated throughout the duration of the experiment with fracturing fluid. Geochemical modeling of experimental fluid data indicates primary clay dissolution, and secondary formation of smectites and barite, after reaction with fracturing fluid. Changes in aqueous organic composition were observed, indicating organic additives may be chemically transformed or sequestered by the formation after hydraulic fracturing. The NaCl concentrations in our fluids are similar to measured concentrations in Marcellus Shale producedmore » waters, showing that these experiments are representative of reservoir fluid chemistries and can provide insight on geochemical reactions that occur in the field. These results can be applied towards evaluating the evolution of hydraulically-fractured reservoirs, and towards understanding geochemical processes that control the composition of produced water from unconventional shales.« less

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2];  [3]; ORCiD logo [2]
  1. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States); Univ. of Wyoming, Laramie, WY (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Fossil Energy (FE)
OSTI Identifier:
1412910
Report Number(s):
LA-UR-17-29116
Journal ID: ISSN 0883-2927
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Applied Geochemistry
Additional Journal Information:
Journal Volume: 76; Journal Issue: C; Journal ID: ISSN 0883-2927
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 58 GEOSCIENCES; Earth Sciences; Marcellus shale, hydraulic fracturing, geochemical reactions, barite, organic acids

Citation Formats

Marcon, Virginia, Joseph, Craig, Carter, Kimberly E., Hedges, Sheila W., Lopano, Christina L., Guthrie, George D., and Hakala, J. Alexandra. Experimental insights into geochemical changes in hydraulically fractured Marcellus Shale. United States: N. p., 2016. Web. https://doi.org/10.1016/j.apgeochem.2016.11.005.
Marcon, Virginia, Joseph, Craig, Carter, Kimberly E., Hedges, Sheila W., Lopano, Christina L., Guthrie, George D., & Hakala, J. Alexandra. Experimental insights into geochemical changes in hydraulically fractured Marcellus Shale. United States. https://doi.org/10.1016/j.apgeochem.2016.11.005
Marcon, Virginia, Joseph, Craig, Carter, Kimberly E., Hedges, Sheila W., Lopano, Christina L., Guthrie, George D., and Hakala, J. Alexandra. Wed . "Experimental insights into geochemical changes in hydraulically fractured Marcellus Shale". United States. https://doi.org/10.1016/j.apgeochem.2016.11.005. https://www.osti.gov/servlets/purl/1412910.
@article{osti_1412910,
title = {Experimental insights into geochemical changes in hydraulically fractured Marcellus Shale},
author = {Marcon, Virginia and Joseph, Craig and Carter, Kimberly E. and Hedges, Sheila W. and Lopano, Christina L. and Guthrie, George D. and Hakala, J. Alexandra},
abstractNote = {Hydraulic fracturing applied to organic-rich shales has significantly increased the recoverable volume of methane available for U.S. energy consumption. Fluid-shale reactions in the reservoir may affect long-term reservoir productivity and waste management needs through changes to fracture mineral composition and produced fluid chemical composition. We performed laboratory experiments with Marcellus Shale and lab-generated hydraulic fracturing fluid at elevated pressures and temperatures to evaluate mineral reactions and the release of trace elements into solution. Results from the experiment containing fracturing chemicals show evidence for clay and carbonate dissolution, secondary clay and anhydrite precipitation, and early-stage (24-48 h) fluid enrichment of certain elements followed by depletion in later stages (i.e. Al, Cd, Co, Cr, Cu, Ni, Sc, Zn). Other elements such as As, Fe, Mn, Sr, and Y increased in concentration and remained elevated throughout the duration of the experiment with fracturing fluid. Geochemical modeling of experimental fluid data indicates primary clay dissolution, and secondary formation of smectites and barite, after reaction with fracturing fluid. Changes in aqueous organic composition were observed, indicating organic additives may be chemically transformed or sequestered by the formation after hydraulic fracturing. The NaCl concentrations in our fluids are similar to measured concentrations in Marcellus Shale produced waters, showing that these experiments are representative of reservoir fluid chemistries and can provide insight on geochemical reactions that occur in the field. These results can be applied towards evaluating the evolution of hydraulically-fractured reservoirs, and towards understanding geochemical processes that control the composition of produced water from unconventional shales.},
doi = {10.1016/j.apgeochem.2016.11.005},
journal = {Applied Geochemistry},
number = C,
volume = 76,
place = {United States},
year = {2016},
month = {11}
}

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