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Title: How long do natural waters “remember” release incidents of Marcellus Shale waters: a first order approximation using reactive transport modeling

Abstract

Natural gas production from the Marcellus Shale formation has significantly changed energy landscape in recent years. Accidental release, including spills, leakage, and seepage of the Marcellus Shale flow back and produced waters can impose risks on natural water resources. With many competing processes during the reactive transport of chemical species, it is not clear what processes are dominant and govern the impacts of accidental release of Marcellus Shale waters (MSW) into natural waters. Here we carry out numerical experiments to explore this largely unexploited aspect using cations from MSW as tracers with a focus on abiotic interactions between cations released from MSW and natural water systems. Reactive transport models were set up using characteristics of natural water systems (aquifers and rivers) in Bradford County, Pennsylvania. Results show that in clay-rich sandstone aquifers, ion exchange plays a key role in determining the maximum concentration and the time scale of released cations in receiving natural waters. In contrast, mineral dissolution and precipitation play a relatively minor role. The relative time scales of recovery τrr, a dimensionless number defined as the ratio of the time needed to return to background concentrations over the residence time of natural waters, vary between 5 and 10more » for Na, Ca, and Mg, and between 10 and 20 for Sr and Ba. In rivers and sand and gravel aquifers with negligible clay, τrr values are close to 1 because cations are flushed out at approximately one residence time. These values can be used as first order estimates of time scales of released MSW in natural water systems. This work emphasizes the importance of clay content and suggests that it is more likely to detect contamination in clay-rich geological formations. As a result, this work highlights the use of reactive transport modeling in understanding natural attenuation, guiding monitoring, and predicting impacts of contamination for risk assessment.« less

Authors:
; ORCiD logo
Publication Date:
Research Org.:
National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1619402
Alternate Identifier(s):
OSTI ID: 1375813
Resource Type:
Published Article
Journal Name:
Geochemical Transactions
Additional Journal Information:
Journal Name: Geochemical Transactions Journal Volume: 17 Journal Issue: 1; Journal ID: ISSN 1467-4866
Publisher:
Springer Science + Business Media
Country of Publication:
United Kingdom
Language:
English
Subject:
58 GEOSCIENCES; Reactive transport modeling; Ion exchange; Marcellus Shale waters; Environmental impacts

Citation Formats

Cai, Zhang, and Li, Li. How long do natural waters “remember” release incidents of Marcellus Shale waters: a first order approximation using reactive transport modeling. United Kingdom: N. p., 2016. Web. doi:10.1186/s12932-016-0038-4.
Cai, Zhang, & Li, Li. How long do natural waters “remember” release incidents of Marcellus Shale waters: a first order approximation using reactive transport modeling. United Kingdom. https://doi.org/10.1186/s12932-016-0038-4
Cai, Zhang, and Li, Li. Tue . "How long do natural waters “remember” release incidents of Marcellus Shale waters: a first order approximation using reactive transport modeling". United Kingdom. https://doi.org/10.1186/s12932-016-0038-4.
@article{osti_1619402,
title = {How long do natural waters “remember” release incidents of Marcellus Shale waters: a first order approximation using reactive transport modeling},
author = {Cai, Zhang and Li, Li},
abstractNote = {Natural gas production from the Marcellus Shale formation has significantly changed energy landscape in recent years. Accidental release, including spills, leakage, and seepage of the Marcellus Shale flow back and produced waters can impose risks on natural water resources. With many competing processes during the reactive transport of chemical species, it is not clear what processes are dominant and govern the impacts of accidental release of Marcellus Shale waters (MSW) into natural waters. Here we carry out numerical experiments to explore this largely unexploited aspect using cations from MSW as tracers with a focus on abiotic interactions between cations released from MSW and natural water systems. Reactive transport models were set up using characteristics of natural water systems (aquifers and rivers) in Bradford County, Pennsylvania. Results show that in clay-rich sandstone aquifers, ion exchange plays a key role in determining the maximum concentration and the time scale of released cations in receiving natural waters. In contrast, mineral dissolution and precipitation play a relatively minor role. The relative time scales of recovery τrr, a dimensionless number defined as the ratio of the time needed to return to background concentrations over the residence time of natural waters, vary between 5 and 10 for Na, Ca, and Mg, and between 10 and 20 for Sr and Ba. In rivers and sand and gravel aquifers with negligible clay, τrr values are close to 1 because cations are flushed out at approximately one residence time. These values can be used as first order estimates of time scales of released MSW in natural water systems. This work emphasizes the importance of clay content and suggests that it is more likely to detect contamination in clay-rich geological formations. As a result, this work highlights the use of reactive transport modeling in understanding natural attenuation, guiding monitoring, and predicting impacts of contamination for risk assessment.},
doi = {10.1186/s12932-016-0038-4},
journal = {Geochemical Transactions},
number = 1,
volume = 17,
place = {United Kingdom},
year = {Tue Dec 13 00:00:00 EST 2016},
month = {Tue Dec 13 00:00:00 EST 2016}
}

Journal Article:
Free Publicly Available Full Text
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https://doi.org/10.1186/s12932-016-0038-4

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Cited by: 6 works
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Works referenced in this record:

High Barium Levels in Public Drinking Water and Its Association with Elevated Blood Pressure
journal, January 1981

  • Brenniman, G. R.; Kojola, W. H.; Levy, P. S.
  • Archives of Environmental Health: An International Journal, Vol. 36, Issue 1
  • DOI: 10.1080/00039896.1981.10667602

Simulating river flow velocity on global scale
journal, January 2005


Time behavior of solute transport in heterogeneous media: transition from anomalous to normal transport
journal, February 2004


Investigating Ebullition in a Sand Column Using Dissolved Gas Analysis and Reactive Transport Modeling
journal, September 2006

  • Amos, Richard T.; Mayer, K. Ulrich
  • Environmental Science & Technology, Vol. 40, Issue 17
  • DOI: 10.1021/es0602501

A critical review of data on field-scale dispersion in aquifers
journal, July 1992

  • Gelhar, Lynn W.; Welty, Claire; Rehfeldt, Kenneth R.
  • Water Resources Research, Vol. 28, Issue 7
  • DOI: 10.1029/92WR00607

Effects of barium-induced cardiac contraction on large- and small-vessel intramyocardial blood volume.
journal, January 1991


Impacts of Shale Gas Wastewater Disposal on Water Quality in Western Pennsylvania
journal, September 2013

  • Warner, Nathaniel R.; Christie, Cidney A.; Jackson, Robert B.
  • Environmental Science & Technology, Vol. 47, Issue 20
  • DOI: 10.1021/es402165b

Effect of Hydrofracking Fluid on Colloid Transport in the Unsaturated Zone
journal, June 2014

  • Sang, Wenjing; Stoof, Cathelijne R.; Zhang, Wei
  • Environmental Science & Technology, Vol. 48, Issue 14
  • DOI: 10.1021/es501441e

Effects of physical and geochemical heterogeneities on mineral transformation and biomass accumulation during biostimulation experiments at Rifle, Colorado
journal, March 2010


The Utilization of the Base-Exchange Reaction for the Determination of Activity Coefficients in Mixed Electrolytes
journal, April 1932

  • Vanselow, Albert P.
  • Journal of the American Chemical Society, Vol. 54, Issue 4
  • DOI: 10.1021/ja01343a005

Strontium isotopes in selected streams within the Susquehanna River Basin
journal, October 1976


Chlorite dissolution in the acid ph-range: a combined microscopic and macroscopic approach
journal, April 2003


Impact of Shale Gas Development on Regional Water Quality
journal, May 2013


Magnesite dissolution rates at different spatial scales: The role of mineral spatial distribution and flow velocity
journal, May 2013


Transport of ion-exchanging solutes in groundwater: Chromatographic theory and field simulation
journal, October 1981

  • Valocchi, Albert J.; Street, Robert L.; Roberts, Paul V.
  • Water Resources Research, Vol. 17, Issue 5
  • DOI: 10.1029/WR017i005p01517

Spatial zonation limits magnesite dissolution in porous media
journal, February 2014


Expanding the role of reactive transport models in critical zone processes
journal, February 2017


Basalt weathering across scales
journal, September 2007

  • Navarre-Sitchler, Alexis; Brantley, Susan
  • Earth and Planetary Science Letters, Vol. 261, Issue 1-2
  • DOI: 10.1016/j.epsl.2007.07.010

A surface complex reaction model for the pH-dependence of corundum and kaolinite dissolution rates
journal, November 1988


Adsorption of barium(II) on montmorillonite: an EXAFS study
journal, October 2001

  • Zhang, Peng-Chu; Brady, Pat V.; Arthur, Sara E.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 190, Issue 3
  • DOI: 10.1016/S0927-7757(01)00592-1

Geochemical evaluation of flowback brine from Marcellus gas wells in Pennsylvania, USA
journal, January 2013


Multiple-Rate Mass Transfer for Modeling Diffusion and Surface Reactions in Media with Pore-Scale Heterogeneity
journal, June 1995

  • Haggerty, Roy; Gorelick, Steven M.
  • Water Resources Research, Vol. 31, Issue 10
  • DOI: 10.1029/95WR10583

Solubility and Dissolution Kinetics of Dolomite in Ca-Mg-HCO 3 /CO 3 Solutions at 25°C and 0.1 MPa Carbon Dioxide
journal, November 2000


Upscaling geochemical reaction rates using pore-scale network modeling
journal, September 2006


Upscaling of flow in heterogeneous porous formations: Critical examination and issues of principle
journal, January 2013


Numerical simulation of CO2 disposal by mineral trapping in deep aquifers
journal, June 2004


Assessment of Effluent Contaminants from Three Facilities Discharging Marcellus Shale Wastewater to Surface Waters in Pennsylvania
journal, March 2013

  • Ferrar, Kyle J.; Michanowicz, Drew R.; Christen, Charles L.
  • Environmental Science & Technology, Vol. 47, Issue 7
  • DOI: 10.1021/es301411q

Uranium Bioreduction Rates across Scales: Biogeochemical Hot Moments and Hot Spots during a Biostimulation Experiment at Rifle, Colorado
journal, August 2014

  • Bao, Chen; Wu, Hongfei; Li, Li
  • Environmental Science & Technology, Vol. 48, Issue 17
  • DOI: 10.1021/es501060d

Mineral Transformation and Biomass Accumulation Associated With Uranium Bioremediation at Rifle, Colorado
journal, July 2009

  • Li, Li; Steefel, Carl I.; Williams, Kenneth H.
  • Environmental Science & Technology, Vol. 43, Issue 14
  • DOI: 10.1021/es900016v

Risks to biodiversity from hydraulic fracturing for natural gas in the Marcellus and Utica shales: Hydraulic fracturing and biodiversity
journal, May 2013

  • Kiviat, Erik
  • Annals of the New York Academy of Sciences, Vol. 1286, Issue 1
  • DOI: 10.1111/nyas.12146

Kinetics of Water-Rock Interaction
book, January 2008


Microbiological and Geochemical Heterogeneity in an In Situ Uranium Bioremediation Field Site
journal, October 2005


The role of magnesite spatial distribution patterns in determining dissolution rates: When do they matter?
journal, April 2015


Solute transport in low-heterogeneity sandboxes: The role of correlation length and permeability variance
journal, October 2014


Illite Spatial Distribution Patterns Dictate Cr(VI) Sorption Macrocapacity and Macrokinetics
journal, January 2015

  • Wang, Li; Li, Li
  • Environmental Science & Technology, Vol. 49, Issue 3
  • DOI: 10.1021/es503230f

Methane contamination of drinking water accompanying gas-well drilling and hydraulic fracturing
journal, May 2011

  • Osborn, S. G.; Vengosh, A.; Warner, N. R.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 20
  • DOI: 10.1073/pnas.1100682108

Geochemical calculations and observations on salt water intrusions, I. A combined geochemical/minxing cell model
journal, October 1987


Shale gas development impacts on surface water quality in Pennsylvania
journal, March 2013

  • Olmstead, S. M.; Muehlenbachs, L. A.; Shih, J. -S.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 13
  • DOI: 10.1073/pnas.1213871110

The effect of time on the weathering of silicate minerals: why do weathering rates differ in the laboratory and field?
journal, December 2003


Adsorption of arsenite and arsenate onto muscovite and biotite mica
journal, May 2007

  • Chakraborty, Sudipta; Wolthers, Mariette; Chatterjee, Debashis
  • Journal of Colloid and Interface Science, Vol. 309, Issue 2
  • DOI: 10.1016/j.jcis.2006.10.014

Ozonation of bromide-containing waters: kinetics of formation of hypobromous acid and bromate
journal, May 1983

  • Haag, Werner R.; Hoigne, Juerg.
  • Environmental Science & Technology, Vol. 17, Issue 5
  • DOI: 10.1021/es00111a004

Should fracking stop?
journal, September 2011

  • Howarth, Robert W.; Ingraffea, Anthony; Engelder, Terry
  • Nature, Vol. 477, Issue 7364
  • DOI: 10.1038/477271a

Evaluation of saline tracer performance during electrical conductivity groundwater monitoring
journal, April 2011


Geochemical and Strontium Isotope Characterization of Produced Waters from Marcellus Shale Natural Gas Extraction
journal, March 2012

  • Chapman, Elizabeth C.; Capo, Rosemary C.; Stewart, Brian W.
  • Environmental Science & Technology, Vol. 46, Issue 6
  • DOI: 10.1021/es204005g

Kinetic Metal Release from Competing Processes in Aquifers
journal, May 2012

  • Bearup, Lindsay A.; Navarre-Sitchler, Alexis K.; Maxwell, Reed M.
  • Environmental Science & Technology, Vol. 46, Issue 12
  • DOI: 10.1021/es203586y

Characterization of complex mineral assemblages: Implications for contaminant transport and environmental remediation
journal, March 1999

  • Bertsch, P. M.; Seaman, J. C.
  • Proceedings of the National Academy of Sciences, Vol. 96, Issue 7
  • DOI: 10.1073/pnas.96.7.3350

A compilation of rate parameters of water-mineral interaction kinetics for application to geochemical modeling
report, January 2004

  • Palandri, James L.; Kharaka, Yousif K.
  • U.S. Geological Survey (USGS)
  • DOI: 10.3133/ofr20041068

Evaluating a groundwater supply contamination incident attributed to Marcellus Shale gas development
journal, May 2015

  • Llewellyn, Garth T.; Dorman, Frank; Westland, J. L.
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 20
  • DOI: 10.1073/pnas.1420279112

Geochemical evidence for possible natural migration of Marcellus Formation brine to shallow aquifers in Pennsylvania
journal, July 2012

  • Warner, Nathaniel R.; Jackson, Robert B.; Darrah, Thomas H.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 30
  • DOI: 10.1073/pnas.1121181109

On mobilization of lead and arsenic in groundwater in response to CO2 leakage from deep geological storage
journal, November 2009