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:
-
- 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}
}
Web of Science
Works referenced in this record:
Controls on the geochemistry of rare earth elements in sediments and groundwaters of the Aquia aquifer, Maryland, USA
journal, June 2011
- Willis, Stephanie S.; Johannesson, Karen H.
- Chemical Geology, Vol. 285, Issue 1-4
Impact of Organics and Carbonates on the Oxidation and Precipitation of Iron during Hydraulic Fracturing of Shale
journal, March 2017
- Jew, Adam D.; Dustin, Megan K.; Harrison, Anna L.
- Energy & Fuels, Vol. 31, Issue 4
Shale Kerogen: Hydraulic Fracturing Fluid Interactions and Contaminant Release
journal, August 2018
- Dustin, Megan K.; Bargar, John R.; Jew, Adam D.
- Energy & Fuels, Vol. 32, Issue 9
A Critical Review of the Risks to Water Resources from Unconventional Shale Gas Development and Hydraulic Fracturing in the United States
journal, March 2014
- Vengosh, Avner; Jackson, Robert B.; Warner, Nathaniel
- Environmental Science & Technology, Vol. 48, Issue 15
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976
- Shannon, R. D.
- Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767
Geochemical and Geophysical Changes during Ammonia Gas Treatment of Vadose Zone Sediments for Uranium Remediation
journal, October 2012
- Szecsody, J. E.; Truex, M. J.; Zhong, L.
- Vadose Zone Journal, Vol. 11, Issue 4
Evolution of water chemistry during Marcellus Shale gas development: A case study in West Virginia
journal, September 2015
- Ziemkiewicz, Paul F.; Thomas He, Y.
- Chemosphere, Vol. 134
Characterization and Analysis of Liquid Waste from Marcellus Shale Gas Development
journal, July 2015
- Shih, Jhih-Shyang; Saiers, James E.; Anisfeld, Shimon C.
- Environmental Science & Technology, Vol. 49, Issue 16
Mineralogy and trace element geochemistry of gas shales in the United States: Environmental implications
journal, June 2014
- Chermak, John A.; Schreiber, Madeline E.
- International Journal of Coal Geology, Vol. 126
Concentration and mineralogical residence of elements in rich oil shales of the Green River Formation, Piceance Creek basin, Colorado, and the Uinta Basin, Utah — A preliminary report
journal, January 1976
- Desborough, George A.; Pitman, Janet K.; Huffman, Claude
- Chemical Geology, Vol. 17
Characterization of Marcellus Shale Flowback Water
journal, September 2014
- Abualfaraj, Noura; Gurian, Patrick L.; Olson, Mira S.
- Environmental Engineering Science, Vol. 31, Issue 9
A method for the isolation of kerogen from Green River oil shale
journal, June 1984
- Goklen, Kent E.; Stoecker, Ted J.; Baddour, Raymond F.
- Industrial & Engineering Chemistry Product Research and Development, Vol. 23, Issue 2
Detrital zircons and sediment dispersal in the Appalachian foreland
journal, October 2017
- Thomas, William A.; Gehrels, George E.; Greb, Stephen F.
- Geosphere, Vol. 13, Issue 6
Quantity of flowback and produced waters from unconventional oil and gas exploration
journal, January 2017
- Kondash, Andrew J.; Albright, Elizabeth; Vengosh, Avner
- Science of The Total Environment, Vol. 574
Uranium(IV) adsorption by natural organic matter in anoxic sediments
journal, January 2017
- Bone, Sharon E.; Dynes, James J.; Cliff, John
- Proceedings of the National Academy of Sciences, Vol. 114, Issue 4
Sequential extraction procedure for the speciation of particulate trace metals
journal, June 1979
- Tessier, A.; Campbell, P. G. C.; Bisson, M.
- Analytical Chemistry, Vol. 51, Issue 7
Mercury Speciation by X-ray Absorption Fine Structure Spectroscopy and Sequential Chemical Extractions: A Comparison of Speciation Methods
journal, November 2003
- Kim, Christopher S.; Bloom, Nicolas S.; Rytuba, James J.
- Environmental Science & Technology, Vol. 37, Issue 22
Controls on rare earth element distributions in ancient organic-rich sedimentary sequences: Role of post-depositional diagenesis of phosphorus phases
journal, September 2017
- Yang, Jon; Torres, Marta; McManus, James
- Chemical Geology, Vol. 466
The preparation of uranium-adsorbed silica particles as a reference material for the fission track analysis
journal, June 2005
- Park, Y. J.; Lee, M. H.; Pyo, H. Y.
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 545, Issue 1-2
Trace metal distribution and mobility in drill cuttings and produced waters from Marcellus Shale gas extraction: Uranium, arsenic, barium
journal, September 2015
- Phan, Thai T.; Capo, Rosemary C.; Stewart, Brian W.
- Applied Geochemistry, Vol. 60
Lithofacies and sequence stratigraphy of the Barnett Shale in east-central Fort Worth Basin, Texas
journal, January 2012
- Abouelresh, Mohamed O.; Slatt, Roger M.
- AAPG Bulletin, Vol. 96, Issue 1
Element release and reaction-induced porosity alteration during shale-hydraulic fracturing fluid interactions
journal, July 2017
- Harrison, Anna L.; Jew, Adam D.; Dustin, Megan K.
- Applied Geochemistry, Vol. 82
An EXAFS study of uranium(VI) sorption onto silica gel and ferrihydrite
journal, November 1998
- Reich, T.; Moll, H.; Arnold, T.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 96, Issue 1-3