Using streamlines to simulate stochastic reactive transport in heterogeneous aquifers: Kinetic metal release and transport in CO2 impacted drinking water aquifers

A Lagrangian streamline approach that stochastically represents uncertainty in spatial hydraulic conductivity distribution is coupled to kinetic reactive transport in a heterogeneous 3-D domain. This methodology is designed to efficiently account for uncertainties inherent in subsurface reactive transport while maintaining hydro-geochemical processes. A hypothetical CO2 leak from a geological carbon storage site into an overlying aquifer is used to simulate reactive transport where contamination may occur. Uncertainty in subsurface hydraulic conductivity is accounted for using correlated, Gaussian random fields in a Monte Carlo approach. In this approach 100 realizations of each ensemble were simulated with variances of the natural log of hydraulic conductivity (σ2lnK) of 1, 3.61, and 16. Peak ensemble lead concentrations were found at σ2lnK of 3.61, the middle of the variances simulated. σ2lnK within an aquifer was found to influence chemical residence time, which in turn determined the equilibrium state of the plume along the flow path and at the pumping well thus driving geochemical conditions. However, macrodispersion due to heterogeneous flow paths caused lower contaminant concentrations at the pumping well due to dilution with uncontaminated water. Furthermore, a strong link between σ2lnK and the probability of well-capture was found, suggesting that proper characterization of the σ2lnK within an aquifer will help to quantify the impact of uncertainty on risks of groundwater contamination.

[1]  Reed M. Maxwell,et al.  Evaluating effective reaction rates of kinetically driven solutes in large‐scale, statistically anisotropic media: Human health risk implications , 2012 .

[2]  J. M. Shafer,et al.  Assessment of Uncertainty in Time‐Related Capture Zones Using Conditional Simulation of Hydraulic Conductivity , 1991 .

[3]  Rajesh J. Pawar,et al.  The impact of CO2 on shallow groundwater chemistry: observations at a natural analog site and implications for carbon sequestration , 2010 .

[4]  Ci Steefel,et al.  OS3D/GIMRT software for modeling multicomponent-multidimensional reactive transport , 2000 .

[5]  Steven F. Carle,et al.  Analysis of groundwater migration from artificial recharge in a large urban aquifer: A simulation perspective , 1999 .

[6]  P. Kitanidis,et al.  Characterization of mixing and dilution in heterogeneous aquifers by means of local temporal moments , 2000 .

[7]  Yoram Rubin,et al.  The concept of comparative information yield curves and its application to risk‐based site characterization , 2009 .

[8]  A. Lasaga.  Chemical kinetics of water‐rock interactions , 1984 .

[9]  Sookyun Wang,et al.  Dissolution of a mineral phase in potable aquifers due to CO2 releases from deep formations; effect of dissolution kinetics , 2004 .

[10]  R. Jackson,et al.  Potential impacts of leakage from deep CO2 geosequestration on overlying freshwater aquifers. , 2010, Environmental science & technology.

[11]  John Karl Böhlke,et al.  Mixing effects on apparent reaction rates and isotope fractionation during denitrification in a heterogeneous aquifer , 2010 .

[12]  Glenn E. Hammond,et al.  Field‐scale model for the natural attenuation of uranium at the Hanford 300 Area using high‐performance computing , 2010 .

[13]  John L. Wilson,et al.  Efficient and accurate front tracking for two‐dimensional groundwater flow models , 1991 .

[14]  Albert J. Valocchi,et al.  Comparison of continuum and pore-scale models of nutrient biodegradation under transverse mixing conditions , 2007 .

[15]  T. Ginn.  Stochastic-convective transport with nonlinear reactions and mixing: finite streamtube ensemble formulation for multicomponent reaction systems with intra-streamtube dispersion. , 2001, Journal of contaminant hydrology.

[16]  A.F.B. Tompson,et al.  Numerical simulation of solute transport in randomly heterogeneous porous media: Motivation, model development, and application , 1987 .

[17]  Timothy R. Ginn,et al.  Stochastic‐Convective Transport with Nonlinear Reaction: Mathematical Framework , 1995 .

[18]  R. Ababou,et al.  Implementation of the three‐dimensional turning bands random field generator , 1989 .

[19]  A. Lasaga,et al.  Kinetics of geochemical processes , 1981 .

[20]  Martin J. Blunt,et al.  Streamline‐based simulation of carbon dioxide storage in a North Sea aquifer , 2006 .

[21]  Claire Welty,et al.  Revisiting the Cape Cod bacteria injection experiment using a stochastic modeling approach. , 2005, Environmental science & technology.

[22]  P. Aagaard,et al.  Thermodynamic and kinetic constraints on reaction rates among minerals and aqueous solutions; I, Theoretical considerations , 1982 .

[23]  Macrodispersivity and Large-scale Hydrogeologic Variability , 2001 .

[24]  Rainer Helmig,et al.  Numerical simulation of biodegradation controlled by transverse mixing , 1999 .

[25]  Glenn E. Hammond,et al.  Elucidating geochemical response of shallow heterogeneous aquifers to CO2 leakage using high-performance computing: Implications for monitoring of CO2 sequestration , 2013 .

[26]  Jim E. Jones,et al.  Newton–Krylov-multigrid solvers for large-scale, highly heterogeneous, variably saturated flow problems , 2001 .

[27]  S. Ashby,et al.  A parallel multigrid preconditioned conjugate gradient algorithm for groundwater flow simulations , 1996 .

[28]  Daniel M. Tartakovsky,et al.  Introduction to the special issue on uncertainty quantification and risk assessment , 2012 .

[29]  S. Gorelick,et al.  Multiple‐Rate Mass Transfer for Modeling Diffusion and Surface Reactions in Media with Pore‐Scale Heterogeneity , 1995 .

[30]  M. Blunt,et al.  Simulating Flow in Heterogeneous Systems Using Streamtubes and Streamlines , 1996 .

[31]  Kate Maher,et al.  The dependence of chemical weathering rates on fluid residence time , 2009 .

[32]  A. Navarre‐Sitchler,et al.  Kinetic metal release from competing processes in aquifers. , 2012, Environmental science & technology.

[33]  Glenn E. Hammond,et al.  Application of Jacobian-free Newton–Krylov with physics-based preconditioning to biogeochemical transport , 2005 .

[34]  O. Cirpka,et al.  How well do mean breakthrough curves predict mixing‐controlled reactive transport? , 2011 .

[35]  Philippe Gouze,et al.  Effective non-local reaction kinetics for transport in physically and chemically heterogeneous media. , 2011, Journal of contaminant hydrology.

[36]  R. Maxwell,et al.  Integrated surface-groundwater flow modeling: A free-surface overland flow boundary condition in a parallel groundwater flow model , 2006 .

[37]  Jan Vanderborght,et al.  Proof of concept of regional scale hydrologic simulations at hydrologic resolution utilizing massively parallel computer resources , 2010 .

[38]  Y. Rubin,et al.  A methodology to integrate site characterization information into groundwater‐driven health risk assessment , 1999 .

[39]  R. Maxwell,et al.  Stochastic environmental risk analysis: an integrated methodology for predicting cancer risk from contaminated groundwater , 1999 .

[40]  V. S. Tripathi,et al.  A critical evaluation of recent developments in hydrogeochemical transport models of reactive multichemical components , 1989 .

[41]  J. Jaime Gómez-Hernández,et al.  Modeling tracer transport at the MADE site: The importance of heterogeneity , 2007 .

[42]  Keith Beven,et al.  Stochastic capture zone delineation within the generalized likelihood uncertainty estimation methodology: Conditioning on head observations , 2001 .

[43]  Martin J. Blunt,et al.  Streamline‐based simulation of solute transport , 1999 .

[44]  Glenn Edward Hammond,et al.  Innovative Methods for Solving Multicomponent Biogeochemical Groundwater Transport on Supercomputers , 2003 .

[45]  Stefan Bachu,et al.  Semianalytical solution for CO2 leakage through an abandoned well. , 2005, Environmental science & technology.

[46]  Christian Lantuéjoul,et al.  TBSIM: A computer program for conditional simulation of three-dimensional Gaussian random fields via the turning bands method , 2006, Comput. Geosci..

[47]  Y. Rubin.  Applied Stochastic Hydrogeology , 2003 .

[48]  P. Lichtner,et al.  Stochastic simulation of uranium migration at the Hanford 300 Area. , 2011, Journal of contaminant hydrology.

[49]  Jean-Raynald de Dreuzy,et al.  Non-Fickian mixing: Temporal evolution of the scalar dissipation rate in heterogeneous porous media , 2010 .

[50]  Carl I. Steefel,et al.  Multidimensional, multicomponent, subsurface reactive transport in nonuniform velocity fields: code verification using an advective reactive streamtube approach , 1998 .

[51]  Martin J. Blunt,et al.  A 3D Field-Scale Streamline-Based Reservoir Simulator , 1997 .

[52]  Glenn E. Hammond,et al.  Subsurface Multiphase Flow and Multicomponent Reactive Transport Modeling using High-Performance Computing , 2007 .

[53]  S. Carroll,et al.  Speciation and fate of trace metals in estuarine sediments under reduced and oxidized conditions, Seaplane Lagoon, Alameda Naval Air Station (USA) , 2002, Geochemical transactions.

[54]  S. Zhang,et al.  Dissolution kinetics of galena in acid NaCl solutions at 25—75 °C , 2004 .

[55]  D. W. Pollock.  Semianalytical Computation of Path Lines for Finite‐Difference Models , 1988 .

[56]  E. Sudicky.  A natural gradient experiment on solute transport in a sand aquifer: Spatial variability of hydraulic conductivity and its role in the dispersion process , 1986 .

[57]  Albert J. Valocchi,et al.  A multidimensional streamline-based method to simulate reactive solute transport in heterogeneous porous media , 2010 .

[58]  Y. Rubin.  Transport in heterogeneous porous media: Prediction and uncertainty , 1991 .

[59]  John E. McCray,et al.  A quantitative methodology to assess the risks to human health from CO2 leakage into groundwater , 2010 .

[60]  P. Kitanidis,et al.  Travel‐Time Based Model of Bioremediation Using Circulation Wells , 2001, Ground water.

[61]  M. Goltz,et al.  Application of the method of temporal moments to interpret solute transport with sorption and degradation. , 2003, Journal of contaminant hydrology.

[62]  William L. Bourcier,et al.  Evaluation of the hydrologic source term from underground nuclear tests in Frenchman Flat at the Nevada Test Site: The Cambric test , 1999 .

[63]  S. Carroll,et al.  Rock−Water Interactions Controlling Zinc, Cadmium, and Lead Concentrations in Surface Waters and Sediments, U.S. Tri-State Mining District. 2. Geochemical Interpretation , 1998 .

[64]  Henning Prommer,et al.  Effects of hydrodynamic dispersion on plume lengths for instantaneous bimolecular reactions , 2004 .

[65]  H. Viswanathan,et al.  Comparison of streamtube and three-dimensional models of reactive transport in heterogeneous media , 2004 .

[66]  Peter K. Kitanidis,et al.  The concept of the Dilution Index , 1994 .

[67]  Jens Birkholzer,et al.  On mobilization of lead and arsenic in groundwater in response to CO2 leakage from deep geological storage , 2009 .

[68]  Philip John Binning,et al.  A forward particle tracking Eulerian-Lagrangian localized adjoint method for solution of the contaminant transport equation in three dimensions , 2002 .

[69]  G. Waychunas,et al.  Rock−Water Interactions Controlling Zinc, Cadmium, and Lead Concentrations in Surface Waters and Sediments, U.S. Tri-State Mining District. 1. Molecular Identification Using X-ray Absorption Spectroscopy , 1998 .

[70]  R. Wilkin,et al.  Geochemical impacts to groundwater from geologic carbon sequestration: controls on pH and inorganic carbon concentrations from reaction path and kinetic modeling. , 2010, Environmental science & technology.

[71]  M. Brusseau,et al.  Transport of Co2+ in a Physically and Chemically Heterogeneous Porous Medium , 1993 .

[72]  Martin J. Blunt,et al.  Streamline-based simulation of advective–dispersive solute transport , 2004 .

[73]  Nancy L. Barber,et al.  Estimated use of water in the United States in 2005 , 2009 .

[74]  C. S. Simmons,et al.  Stochastic-Convective Transport with Nonlinear Reaction: Biodegradation With Microbial Growth , 1995 .

[75]  Timothy D. Scheibe,et al.  Mixing‐induced precipitation: Experimental study and multiscale numerical analysis , 2008 .

[76]  S. Carroll,et al.  Metal Speciation and Bioavailability in Contaminated Estuary Sediments, Alameda Naval Air Station, California , 2000 .

[77]  R. Maxwell,et al.  Demonstrating fractal scaling of baseflow residence time distributions using a fully‐coupled groundwater and land surface model , 2008 .

[78]  V. Cvetkovic,et al.  Mass arrival of sorptive solute in heterogeneous porous media. , 1990 .

[79]  Chin-Fu Tsang,et al.  Flow channeling in strongly heterogeneous porous media: A numerical study , 1994 .

[80]  Steven F. Carle,et al.  Contamination, risk, and heterogeneity: on the effectiveness of aquifer remediation , 2008 .

[81]  G. Dagan.  Solute transport in heterogeneous porous formations , 1984, Journal of Fluid Mechanics.

[82]  Reed M. Maxwell,et al.  Streamline-based simulation of virus transport resulting from long term artificial recharge in a heterogeneous aquifer , 2003 .

[83]  Linda M. Abriola,et al.  The influence of field-scale heterogeneity on the surfactant-enhanced remediation of entrapped nonaqueous phase liquids , 2000 .

[84]  D. K. Smith,et al.  On the evaluation of groundwater contamination from underground nuclear tests , 2002 .

[85]  Liange Zheng,et al.  Evaluation of Potential Changes in Groundwater Quality in Response to CO2 Leakage from Deep Geologic Storage , 2010 .

[86]  Yue Hao,et al.  Geochemical detection of carbon dioxide in dilute aquifers , 2009, Geochemical transactions.

[87]  Jesús Carrera,et al.  Coupling of mass transfer and reactive transport for nonlinear reactions in heterogeneous media , 2010 .

[88]  C. Steefel,et al.  A coupled model for transport of multiple chemical species and kinetic precipitation/dissolution rea , 1994 .