Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Comparison of Electrostatic and Non-Electrostatic Models for U(VI) Sorption on Aquifer Sediments

Abstract

We report that a non-electrostatic generalized composite surface complexation model (SCM) was developed for U(VI) sorption on contaminated F-Area sediments from the U.S. Department of Energy Savannah River Site, South Carolina. The objective of this study was to test if a simpler, semi-empirical, non-electrostatic U(VI) sorption model (NEM) could achieve the same predictive performance as a SCM with electrostatic correction terms in describing U(VI) plume evolution and long-term mobility. One-dimensional reactive transport simulations considering key hydrodynamic processes, Al and Fe minerals, as well as H+ and U surface complexation, with and without electrostatic correction terms, were conducted. The NEM was first calibrated with laboratory batch H+ and U(VI) sorption data on F-Area sediments, and then the surface area of the NEM was adjusted to match field observations of dissolved U(VI). Modeling results indicate that the calibrated NEM was able to perform as well as the previously developed electrostatic model in predicting the long-term evolution of H+ and U(VI) at the site, given the variability of field-site data. The electrostatic and NEM models yield somewhat different results for the time period when basin discharge was active; however, it is not clear which modeling approach may be better to model this earlymore » time period because groundwater quality data during this period were not available. Lastly, a key finding of this study is that the applicability of NEM (and thus robustness of its predictions) to the field system evolves with time and is strongly dependent on the pH range that was used to develop the model.« less

Authors:
 [1];  [1];  [1];  [1];  [1]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM); USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1532288
Alternate Identifier(s):
OSTI ID: 1418695
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Ground Water
Additional Journal Information:
Journal Volume: 56; Journal Issue: 1; Journal ID: ISSN 0017-467X
Publisher:
Wiley - NGWA
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES

Citation Formats

Arora, Bhavna, Davis, James A., Spycher, Nicolas F., Dong, Wenming, and Wainwright, Haruko M. Comparison of Electrostatic and Non-Electrostatic Models for U(VI) Sorption on Aquifer Sediments. United States: N. p., 2017. Web. doi:10.1111/gwat.12551.
Copy to clipboard
Arora, Bhavna, Davis, James A., Spycher, Nicolas F., Dong, Wenming, & Wainwright, Haruko M. Comparison of Electrostatic and Non-Electrostatic Models for U(VI) Sorption on Aquifer Sediments. United States. https://doi.org/10.1111/gwat.12551
Copy to clipboard
Arora, Bhavna, Davis, James A., Spycher, Nicolas F., Dong, Wenming, and Wainwright, Haruko M. Thu . "Comparison of Electrostatic and Non-Electrostatic Models for U(VI) Sorption on Aquifer Sediments". United States. https://doi.org/10.1111/gwat.12551. https://www.osti.gov/servlets/purl/1532288.
Copy to clipboard
@article{osti_1532288,
title = {Comparison of Electrostatic and Non-Electrostatic Models for U(VI) Sorption on Aquifer Sediments},
author = {Arora, Bhavna and Davis, James A. and Spycher, Nicolas F. and Dong, Wenming and Wainwright, Haruko M.},
abstractNote = {We report that a non-electrostatic generalized composite surface complexation model (SCM) was developed for U(VI) sorption on contaminated F-Area sediments from the U.S. Department of Energy Savannah River Site, South Carolina. The objective of this study was to test if a simpler, semi-empirical, non-electrostatic U(VI) sorption model (NEM) could achieve the same predictive performance as a SCM with electrostatic correction terms in describing U(VI) plume evolution and long-term mobility. One-dimensional reactive transport simulations considering key hydrodynamic processes, Al and Fe minerals, as well as H+ and U surface complexation, with and without electrostatic correction terms, were conducted. The NEM was first calibrated with laboratory batch H+ and U(VI) sorption data on F-Area sediments, and then the surface area of the NEM was adjusted to match field observations of dissolved U(VI). Modeling results indicate that the calibrated NEM was able to perform as well as the previously developed electrostatic model in predicting the long-term evolution of H+ and U(VI) at the site, given the variability of field-site data. The electrostatic and NEM models yield somewhat different results for the time period when basin discharge was active; however, it is not clear which modeling approach may be better to model this early time period because groundwater quality data during this period were not available. Lastly, a key finding of this study is that the applicability of NEM (and thus robustness of its predictions) to the field system evolves with time and is strongly dependent on the pH range that was used to develop the model.},
doi = {10.1111/gwat.12551},
journal = {Ground Water},
number = 1,
volume = 56,
place = {United States},
year = {Thu Jul 06 00:00:00 EDT 2017},
month = {Thu Jul 06 00:00:00 EDT 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1111/gwat.12551
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Cation Exchange Capacity of Kaolinite
journal, January 1999

Stimulating the In Situ Activity of Geobacter Species To Remove Uranium from the Groundwater of a Uranium-Contaminated Aquifer
journal, October 2003

Evaluating the use of “goodness-of-fit” Measures in hydrologic and hydroclimatic model validation
journal, January 1999

  • Legates, David R.; McCabe, Gregory J.
  • Water Resources Research, Vol. 35, Issue 1
  • DOI: 10.1029/1998WR900018

Neptunium(V) Sorption on Montmorillonite: An Experimental and Surface Complexation Modeling Study
journal, January 1998

Sorption phenomena in subsurface systems: Concepts, models and effects on contaminant fate and transport
journal, May 1991

Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments
journal, September 2004

  • Davis, James A.; Meece, David E.; Kohler, Matthias
  • Geochimica et Cosmochimica Acta, Vol. 68, Issue 18
  • DOI: 10.1016/j.gca.2004.03.003

TOUGHREACT Version 2.0: A simulator for subsurface reactive transport under non-isothermal multiphase flow conditions
journal, June 2011

Simulation of reactive transport of uranium(VI) in groundwater with variable chemical conditions: SIMULATION OF REACTIVE TRANSPORT OF URANIUM(VI)
journal, April 2006

  • Curtis, Gary P.; Davis, James A.; Naftz, David L.
  • Water Resources Research, Vol. 42, Issue 4
  • DOI: 10.1029/2005WR003979

Persistent Source Influences on the Trailing Edge of a Groundwater Plume, and Natural Attenuation Timeframes: The F-Area Savannah River Site
journal, March 2012

  • Wan, Jiamin; Tokunaga, Tetsu K.; Dong, Wenming
  • Environmental Science & Technology, Vol. 46, Issue 8
  • DOI: 10.1021/es204265q

Solving iTOUGH2 simulation and optimization problems using the PEST protocol
journal, July 2011

Identifying key controls on the behavior of an acidic-U(VI) plume in the Savannah River Site using reactive transport modeling
journal, August 2013

Mineralogical compositions of aquifer matrix as necessary initial conditions in reactive contaminant transport models
journal, October 2001

Reactive facies: An approach for parameterizing field-scale reactive transport models using geophysical methods: GEOPHYSICS FOR DISTRIBUTING REACTIVE FACIES
journal, October 2012

  • Sassen, Douglas S.; Hubbard, Susan S.; Bea, Sergio A.
  • Water Resources Research, Vol. 48, Issue 10
  • DOI: 10.1029/2011WR011047

Surface Complexation Modeling of U(VI) Adsorption by Aquifer Sediments from a Former Mill Tailings Site at Rifle, Colorado
journal, December 2009

  • Hyun, Sung Pil; Fox, Patricia M.; Davis, James A.
  • Environmental Science & Technology, Vol. 43, Issue 24
  • DOI: 10.1021/es902164n

Competitive sorption of protons and metal cations onto kaolinite: experiments and modeling
journal, February 2005

  • Heidmann, Ilona; Christl, Iso; Leu, Christian
  • Journal of Colloid and Interface Science, Vol. 282, Issue 2
  • DOI: 10.1016/j.jcis.2004.08.019

Comparison of in situ uranium KD values with a laboratory determined surface complexation model
journal, October 2004

Biogeochemical gradients as a framework for understanding waste-site evolution
journal, September 2008

  • Denham, Miles; Vangelas, Karen M.
  • Remediation Journal, Vol. 19, Issue 1
  • DOI: 10.1002/rem.20188

Estimating Escherichia coli loads in streams based on various physical, chemical, and biological factors : Estimating
journal, May 2013

  • Dwivedi, Dipankar; Mohanty, Binayak P.; Lesikar, Bruce J.
  • Water Resources Research, Vol. 49, Issue 5
  • DOI: 10.1002/wrcr.20265

Mineral properties, microbes, transport, and plant-input profiles control vertical distribution and age of soil carbon stocks
journal, April 2017

Environmental Availability of Uranium in an Acidic Plume at the Savannah River Site
journal, January 2007

  • Serkiz, S. M.; Johnson, W. H.; Wile, L. M. Johnson
  • Vadose Zone Journal, Vol. 6, Issue 2
  • DOI: 10.2136/vzj2006.0072

Reactive transport codes for subsurface environmental simulation
journal, September 2014

Estimates of Vadose Zone Drainage from a Capped Seepage Basin, F-Area, Savannah River Site
journal, January 2012

  • Tokunaga, Tetsu K.; Wan, Jiamin; Denham, Miles E.
  • Vadose Zone Journal, Vol. 11, Issue 3
  • DOI: 10.2136/vzj2011.0131

A modified Langmuir-Freundlich isotherm model for simulating pH-dependent adsorption effects
journal, March 2012

Bayesian hierarchical approach and geophysical data sets for estimation of reactive facies over plume scales
journal, June 2014

  • Wainwright, Haruko M.; Chen, Jinsong; Sassen, Douglas S.
  • Water Resources Research, Vol. 50, Issue 6
  • DOI: 10.1002/2013WR013842

Role of competing ions in the mobilization of arsenic in groundwater of Bengal Basin: Insight from surface complexation modeling
journal, May 2014

Experimental Investigation and Modeling of Uranium (VI) Transport Under Variable Chemical Conditions
journal, December 1996

  • Kohler, M.; Curtis, G. P.; Kent, D. B.
  • Water Resources Research, Vol. 32, Issue 12
  • DOI: 10.1029/95WR02815

Identifying geochemical hot moments and their controls on a contaminated river floodplain system using wavelet and entropy approaches
journal, November 2016

Surface complexation modeling of Co(II) adsorption on mixtures of hydrous ferric oxide, quartz and kaolinite
journal, July 2009

  • Landry, Christopher J.; Koretsky, Carla M.; Lund, Tracy J.
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 13
  • DOI: 10.1016/j.gca.2009.03.028

Influence of hydrological, biogeochemical and temperature transients on subsurface carbon fluxes in a flood plain environment
journal, February 2016

Comparing Approaches for Simulating the Reactive Transport of U(VI) in Ground Water
journal, February 2009

  • Curtis, Gary P.; Kohler, Matthias; Davis, James A.
  • Mine Water and the Environment, Vol. 28, Issue 2
  • DOI: 10.1007/s10230-009-0064-x

River flow forecasting through conceptual models part I — A discussion of principles
journal, April 1970

Advances in subsurface modeling using the TOUGH suite of simulators
journal, April 2014

Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site
journal, January 2012

  • Dong, Wenming; Tokunaga, Tetsu K.; Davis, James A.
  • Environmental Science & Technology, Vol. 46, Issue 3
  • DOI: 10.1021/es2036256

Modeling the influence of variable pH on the transport of zinc in a contaminated aquifer using semiempirical surface complexation models
journal, December 2000

  • Kent, D. B.; Abrams, R. H.; Davis, J. A.
  • Water Resources Research, Vol. 36, Issue 12
  • DOI: 10.1029/2000WR900244

Surface complexation of U(VI) on goethite (α-FeOOH)
journal, January 2008

  • Sherman, David M.; Peacock, Caroline L.; Hubbard, Christopher G.
  • Geochimica et Cosmochimica Acta, Vol. 72, Issue 2
  • DOI: 10.1016/j.gca.2007.10.023

Application of the Surface Complexation Concept to Complex Mineral Assemblages
journal, October 1998

  • Davis, J. A.; Coston, J. A.; Kent, D. B.
  • Environmental Science & Technology, Vol. 32, Issue 19
  • DOI: 10.1021/es980312q

Theoretical prediction of single-site surface-protonation equilibrium constants for oxides and silicates in water
journal, October 1996

U(VI) Adsorption to Heterogeneous Subsurface Media:  Application of a Surface Complexation Model
journal, March 2002

  • Barnett, Mark O.; Jardine, Philip M.; Brooks, Scott C.
  • Environmental Science & Technology, Vol. 36, Issue 5
  • DOI: 10.1021/es010846i

Facilitated Transport of Contaminant Metals Through an Acidified Aquifer
journal, September 1995

Uranium(VI) sorption on iron oxides in Hanford Site sediment: Application of a surface complexation model
journal, September 2008

Surface complexation modeling of groundwater arsenic mobility: Results of a forced gradient experiment in a Red River flood plain aquifer, Vietnam
journal, December 2012

Effect of Subgrid Heterogeneity on Scaling Geochemical and Biogeochemical Reactions: A Case of U(VI) Desorption
journal, January 2014

  • Liu, Chongxuan; Shang, Jianying; Shan, Huimei
  • Environmental Science & Technology, Vol. 48, Issue 3
  • DOI: 10.1021/es404224j

Ion Exchange in Clays and Other Minerals
journal, January 1959

    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: