Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments

Stoliker, Deborah L.; Liu, Chongxuan; Kent, Douglas B.; Zachara, John M.

doi:10.1002/wrcr.20104

Title: Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments

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Abstract

Rates of contaminant U(VI) release from individual size fractions of a composite sediment from the seasonally saturated lower vadose zone of the Hanford 300-Area were examined in flow-through batch reactors to maintain quasi-constant chemical conditions. Variability in equilibrium adsorption among the various size fractions was determined in static batch reactors and analyzed using the surface complexation modeling approach. The estimated stoichiometric coefficients of U(VI) surface complexation reactions with respect to pH and carbonate concentrations varied with size fractions. This source of variability significantly increased the uncertainty in U(VI) conditional equilibrium constants over that estimated from experimental errors alone. A minimum difference between conditional equilibrium constants was established in order to evaluate statistically significant differences between sediment adsorption properties. A set of equilibrium and kinetic expressions for cation exchange, calcite dissolution, aerobic respiration, and silica dissolution were incorporated in a reaction-rate model to describe the temporal evolution of solute concentrations observed during the flow-through batch experiments. Parameters in the reaction-rate model, calibrated using experimental data for select size fractions, predicted the changes in solute concentrations for the bulk, <2 mm, sediment sample. Kinetic U(VI) desorption was well described using a multi-rate surface complexation model with an assumed lognormal distribution for themore »« less

Authors:: Stoliker, Deborah L.; Liu, Chongxuan; Kent, Douglas B.; Zachara, John M.

Publication Date:: Tue Feb 12 00:00:00 EST 2013

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1082599

Report Number(s):: PNNL-SA-88691
KP1702030

DOE Contract Number:: AC05-76RL01830

Resource Type:: Journal Article

Journal Name:: Water Resources Research, 49(2):1163-1177

Additional Journal Information:: Journal Name: Water Resources Research, 49(2):1163-1177

Country of Publication:: United States

Language:: English

Citation Formats


                    Stoliker, Deborah L., Liu, Chongxuan, Kent, Douglas B., and Zachara, John M. Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments.  United States: N. p., 2013. 
        Web.  doi:10.1002/wrcr.20104.

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                    Stoliker, Deborah L., Liu, Chongxuan, Kent, Douglas B., & Zachara, John M. Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments.  United States.  https://doi.org/10.1002/wrcr.20104

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                    Stoliker, Deborah L., Liu, Chongxuan, Kent, Douglas B., and Zachara, John M. 2013.  
        "Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments".  United States.  https://doi.org/10.1002/wrcr.20104.

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@article{osti_1082599,

  title        = {Characterizing particle-scale equilibrium adsorption and kinetics of uranium(VI) desorption from U-contaminated sediments},

  author       = {Stoliker, Deborah L. and Liu, Chongxuan and Kent, Douglas B. and Zachara, John M.},

  abstractNote = {Rates of contaminant U(VI) release from individual size fractions of a composite sediment from the seasonally saturated lower vadose zone of the Hanford 300-Area were examined in flow-through batch reactors to maintain quasi-constant chemical conditions. Variability in equilibrium adsorption among the various size fractions was determined in static batch reactors and analyzed using the surface complexation modeling approach. The estimated stoichiometric coefficients of U(VI) surface complexation reactions with respect to pH and carbonate concentrations varied with size fractions. This source of variability significantly increased the uncertainty in U(VI) conditional equilibrium constants over that estimated from experimental errors alone. A minimum difference between conditional equilibrium constants was established in order to evaluate statistically significant differences between sediment adsorption properties. A set of equilibrium and kinetic expressions for cation exchange, calcite dissolution, aerobic respiration, and silica dissolution were incorporated in a reaction-rate model to describe the temporal evolution of solute concentrations observed during the flow-through batch experiments. Parameters in the reaction-rate model, calibrated using experimental data for select size fractions, predicted the changes in solute concentrations for the bulk, <2 mm, sediment sample. Kinetic U(VI) desorption was well described using a multi-rate surface complexation model with an assumed lognormal distribution for the rate constants. The estimated mean and standard deviation were the same for all < 2mm size fractions, but differed in the 2-8mm size fraction. Micropore volumes in the varied size fractions were also similar as assessed using t-plots to analyze N2 desorption data. These findings provide further support for the link between microporosity and particle-scale mass transfer rates controlling kinetic U(VI) adsorption/desorption and for the utility of N2 desorption isotherms for characterizing pore networks that influence mass transfer rates.},

  doi          = {10.1002/wrcr.20104},

  url          = {https://www.osti.gov/biblio/1082599},
  journal      = {Water Resources Research, 49(2):1163-1177},
number       = ,

  volume       = ,

  place        = {United States},

  year         = {Tue Feb 12 00:00:00 EST 2013},

  month        = {Tue Feb 12 00:00:00 EST 2013}

}

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