Comparison of parameter sensitivities between a laboratory and field‐scale model of uranium transport in a dual domain, distributed rate reactive system

[1] A laboratory-derived conceptual and numerical model for U(VI) transport at the Hanford 300A site, Washington, USA, was applied to a range of field-scale scenarios of different geochemical complexity to identify the importance of individual processes in controlling the fate of U(VI), as well as to elucidate the characteristic differences between well-defined laboratory and the more complex field-scale conditions. Therefore, a rigorous sensitivity analysis was carried out for the various simulation scenarios. The underlying conceptual and numerical model, originally developed from column experiment data, includes distributed rate surface complexation kinetics of U(VI), aqueous speciation, and physical nonequilibrium transport processes. The field scenarios accounted additionally for highly transient groundwater flow and variable geochemical conditions driven by frequent water level changes of the nearby Columbia River. The results of the sensitivity analysis showed not only similarities but also important differences in parameter sensitivities between the laboratory and field-scale models. It was found that the actual degree of sorption disequilibrium, actual concentration of sorbed U(VI), and the sorption extent (i.e., theoretical concentration of sorbed U(VI) at equilibrium) are the major controls for the magnitude of the calculated parameter sensitivities. These internal model variables depended mainly on (1) the groundwater flow conditions, i.e., the relatively long phases of limited groundwater movement in the field scale (intercepted by short peak flow events) and the long sustained flow phases in the column experiment (intercepted by relatively short stop flow events), and (2) the sampling location in the field-scale model, i.e., plume fringe versus plume center.

[1]  S W Wang,et al.  Simulating bioremediation of uranium-contaminated aquifers; uncertainty assessment of model parameters. , 2003, Journal of contaminant hydrology.

[2]  John M. Zachara,et al.  Scale‐dependent desorption of uranium from contaminated subsurface sediments , 2008 .

[3]  James A. Davis,et al.  Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments , 2004 .

[4]  Ming Ye,et al.  Combined Estimation of Hydrogeologic Conceptual Model, Parameter, and Scenario Uncertainty with Application to Uranium Transport at the Hanford Site 300 Area , 2006 .

[5]  Wassana Yantasee,et al.  Microscopic reactive diffusion of uranium in the contaminated sediments at Hanford, United States , 2006 .

[6]  D. A. Barry,et al.  Modelling of physical and reactive processes during biodegradation of a hydrocarbon plume under transient groundwater flow conditions. , 2002, Journal of contaminant hydrology.

[7]  J. M. Zachara,et al.  Chemical contaminants on DOE lands and selection of contaminant mixtures for subsurface science research , 1992 .

[8]  A. Valocchi,et al.  Calculation of reaction parameter sensitivity coefficients in multicomponent subsurface transport models , 2000 .

[9]  Matthias Kohler,et al.  Experimental Investigation and Modeling of Uranium (VI) Transport Under Variable Chemical Conditions , 1996 .

[10]  R Kahnt,et al.  Modelling the closure-related geochemical evolution of groundwater at a former uranium mine. , 2001, Journal of contaminant hydrology.

[11]  Arlen W. Harbaugh,et al.  MODFLOW-2000, The U.S. Geological Survey Modular Ground-Water Model - User Guide to Modularization Concepts and the Ground-Water Flow Process , 2000 .

[12]  Paul P. Wang,et al.  MT3DMS: A Modular Three-Dimensional Multispecies Transport Model for Simulation of Advection, Dispersion, and Chemical Reactions of Contaminants in Groundwater Systems; Documentation and User's Guide , 1999 .

[13]  Christopher F. Brown,et al.  Limited Field Investigation Report for Uranium Contamination in the 300 Area, 300-FF-5 Operable Unit, Hanford Site, Washington , 2007 .

[14]  Vijay S. Tripathi,et al.  Coupled reaction/transport modeling of a chemical barrier for controlling uranium(VI) contamination in groundwater , 1995 .

[15]  Sean Andrew McKenna,et al.  Tracer tests in a fractured dolomite: 2. Analysis of mass transfer in single‐well injection‐withdrawal tests , 1999 .

[16]  James A. Davis,et al.  Simulation of reactive transport of uranium(VI) in groundwater with variable chemical conditions , 2006 .

[17]  J. Zachara,et al.  Kinetics of uranium(VI) desorption from contaminated sediments: effect of geochemical conditions and model evaluation. , 2009, Environmental science & technology.

[18]  C. Zheng,et al.  Natural Attenuation of BTEX Compounds: Model Development and Field‐Scale Application , 1999, Ground water.

[19]  Hans Wanner,et al.  Chemical thermodynamics of uranium , 1992 .

[20]  Mary C Hill,et al.  Parameter and observation importance in modelling virus transport in saturated porous media-investigations in a homogenous system. , 2005, Journal of contaminant hydrology.

[21]  A. Valocchi,et al.  Evaluating the sensitivity of a subsurface multicomponent reactive transport model with respect to transport and reaction parameters. , 2001, Journal of contaminant hydrology.

[22]  S. Brooks,et al.  Adsorption and Transport of Uranium(VI) in Subsurface Media , 2000 .

[23]  James A. Davis,et al.  Uranium(VI) Release from Contaminated Vadose Zone Sediments: Estimation of Potential Contributions from Dissolution and Desorption , 2007 .

[24]  E. Roden,et al.  Reactive transport of uranium(VI) and phosphate in a goethite-coated sand column: an experimental study. , 2007, Chemosphere.

[25]  H. Prommer,et al.  Modeling of carbon cycling and biogeochemical changes during injection and recovery of reclaimed water at Bolivar, South Australia , 2005 .

[26]  D. Read,et al.  Uranium migration through intact sandstone cores , 1993 .

[27]  Henning Prommer,et al.  A field‐scale reactive transport model for U(VI) migration influenced by coupled multirate mass transfer and surface complexation reactions , 2010 .

[28]  C. Zhu,et al.  Mineralogical compositions of aquifer matrix as necessary initial conditions in reactive contaminant transport models. , 2001, Journal of contaminant hydrology.

[29]  Scott C Brooks,et al.  U(VI) adsorption to heterogeneous subsurface media: application of a surface complexation model. , 2002, Environmental science & technology.

[30]  Henning Prommer,et al.  Fringe-controlled natural attenuation of phenoxy acids in a landfill plume: integration of field-scale processes by reactive transport modeling. , 2006, Environmental science & technology.

[31]  J. Gaudet,et al.  Reactive transport of uranyl in a goethite column: an experimental and modelling study , 1998 .

[32]  M. Vanclooster,et al.  Parameter uncertainty in the mobile-immobile solute transport model , 1997 .

[33]  D. L. Parkhurst,et al.  User's guide to PHREEQC (Version 2)-a computer program for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations , 1999 .

[34]  D. A. Barry,et al.  MODFLOW/MT3DMS‐Based Reactive Multicomponent Transport Modeling , 2003, Ground water.

[35]  F. Hu,et al.  Multi-component reactive transport modeling of natural attenuation of an acid groundwater plume at a uranium mill tailings site. , 2001, Journal of contaminant hydrology.

[36]  Mary C Hill,et al.  Numerical methods for improving sensitivity analysis and parameter estimation of virus transport simulated using sorptive-reactive processes. , 2005, Journal of contaminant hydrology.

[37]  Brian J. Wagner,et al.  Experimental design for estimating parameters of rate‐limited mass transfer: Analysis of stream tracer studies , 1997 .

[38]  Chongxuan Liu,et al.  Kinetic desorption and sorption of U(VI) during reactive transport in a contaminated Hanford sediment. , 2005, Environmental science & technology.

[39]  Steven B. Yabusaki,et al.  Building conceptual models of field‐scale uranium reactive transport in a dynamic vadose zone‐aquifer‐river system , 2008 .