Chemical Speciation and Stability of Uranium in Unconventional Shales: Impact of Hydraulic Fracture Fluid
Abstract
Uranium and other radionuclides are prominent in many unconventional oil/gas shales and is a potential contaminant in flowback/produced waters due to the large volumes/types of chemicals injected into the subsurface during stimulation. To understand the stability of U before and after stimulation, a geochemical study of U speciation was carried out on three shales (Marcellus, Green River, and Barnett). Two types of samples for each shale were subjected to sequential chemical extractions: unreacted and shale reacted with synthetic hydraulic fracture fluid. A significant proportion of the total U (20-57%) was released from these three shales after reaction with fracture fluid, indicating that U is readily leachable. The total U released exceeds labile water soluble and exchangeable fractions in unreacted samples, indicating that fluids leach more recalcitrant phases in the shale. Radiographic analysis of unreacted Marcellus shale thin sections shows U associated with detrital quartz and the clay matrix in the shale. Detrital zircon and TiO2 identified by electron microprobe could account for the hotspots. This study shows that significant proportions of U in three shales are mobile upon stimulation. In addition, the extent of mobilization of U depends on the U species in these rocks.
- Authors:
-
[1];
[1];
[1];
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
- Stanford Univ., CA (United States); Ecole Normale Superieure de Paris (France)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Fossil Energy (FE)
- OSTI Identifier:
- 1647335
- Alternate Identifier(s):
- OSTI ID: 1757999
- Grant/Contract Number:
- SC0019165; AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 54; Journal Issue: 12; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; Nuclear fission; inorganic carbon compounds; shale; minerals; extraction
Citation Formats
Jew, Adam D., Besançon, Clémence J., Roycroft, Scott J., Noel, Vincent S., Bargar, John R., and Brown, Jr., Gordon E. Chemical Speciation and Stability of Uranium in Unconventional Shales: Impact of Hydraulic Fracture Fluid. United States: N. p., 2020.
Web. doi:10.1021/acs.est.0c01022.
Jew, Adam D., Besançon, Clémence J., Roycroft, Scott J., Noel, Vincent S., Bargar, John R., & Brown, Jr., Gordon E. Chemical Speciation and Stability of Uranium in Unconventional Shales: Impact of Hydraulic Fracture Fluid. United States. https://doi.org/10.1021/acs.est.0c01022
Jew, Adam D., Besançon, Clémence J., Roycroft, Scott J., Noel, Vincent S., Bargar, John R., and Brown, Jr., Gordon E. Wed .
"Chemical Speciation and Stability of Uranium in Unconventional Shales: Impact of Hydraulic Fracture Fluid". United States. https://doi.org/10.1021/acs.est.0c01022. https://www.osti.gov/servlets/purl/1647335.
@article{osti_1647335,
title = {Chemical Speciation and Stability of Uranium in Unconventional Shales: Impact of Hydraulic Fracture Fluid},
author = {Jew, Adam D. and Besançon, Clémence J. and Roycroft, Scott J. and Noel, Vincent S. and Bargar, John R. and Brown, Jr., Gordon E.},
abstractNote = {Uranium and other radionuclides are prominent in many unconventional oil/gas shales and is a potential contaminant in flowback/produced waters due to the large volumes/types of chemicals injected into the subsurface during stimulation. To understand the stability of U before and after stimulation, a geochemical study of U speciation was carried out on three shales (Marcellus, Green River, and Barnett). Two types of samples for each shale were subjected to sequential chemical extractions: unreacted and shale reacted with synthetic hydraulic fracture fluid. A significant proportion of the total U (20-57%) was released from these three shales after reaction with fracture fluid, indicating that U is readily leachable. The total U released exceeds labile water soluble and exchangeable fractions in unreacted samples, indicating that fluids leach more recalcitrant phases in the shale. Radiographic analysis of unreacted Marcellus shale thin sections shows U associated with detrital quartz and the clay matrix in the shale. Detrital zircon and TiO2 identified by electron microprobe could account for the hotspots. This study shows that significant proportions of U in three shales are mobile upon stimulation. In addition, the extent of mobilization of U depends on the U species in these rocks.},
doi = {10.1021/acs.est.0c01022},
journal = {Environmental Science and Technology},
number = 12,
volume = 54,
place = {United States},
year = {Wed May 13 00:00:00 EDT 2020},
month = {Wed May 13 00:00:00 EDT 2020}
}
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