Stochastic modeling of solute transport in 3-D heterogeneous porous media with random source condition

During probabilistic analysis of flow and transport in porous media, the uncertainty due to spatial heterogeneity of governing parameters are often taken into account. The randomness in the source conditions also play a major role on the stochastic behavior in distribution of the dependent variable. The present paper is focused on studying the effect of both uncertainty in the governing system parameters as well as the input source conditions. Under such circumstances, a method is proposed which combines with stochastic finite element method (SFEM) and is illustrated for probabilistic analysis of concentration distribution in a 3-D heterogeneous porous media under the influence of random source condition. In the first step SFEM used for probabilistic solution due to spatial heterogeneity of governing parameters for a unit source pulse. Further, the results from the unit source pulse case have been used for the analysis of multiple pulse case using the numerical convolution when the source condition is a random process. The source condition is modeled as a discrete release of random amount of masses at fixed intervals of time. The mean and standard deviation of concentration is compared for the deterministic and the stochastic system scenarios as well as for different values of system parameters. The effect of uncertainty of source condition is also demonstrated in terms of mean and standard deviation of concentration at various locations in the domain.     

A generalized transformation approach for simulating steady-state variably-saturated subsurface flow

A numerical method is proposed to accurately and efficiently compute a direct steady-state solution of the nonlinear Richards equation. In the proposed method, the Kirchhoff integral transformation and a complementary transformation are applied to the governing equation in order to separate the nonlinear hyperbolic characteristic from the linear parabolic part. The separation allows the transformed governing equation to be applied to partially- to fully-saturated systems with arbitrary constitutive relations between primary (pressure head) and secondary variables (relative permeability). The transformed governing equation is then discretized with control volume finite difference/finite element approximations, followed by inverse transformation. The approach is compared to analytical and other numerical approaches for variably-saturated flow in 1-D and 3-D domains. The results clearly demonstrate that the approach is not only more computationally efficient but also more accurate than traditional numerical solutions. The approach is also applied to an example flow problem involving a regional-scale variably-saturated heterogeneous system, where the vadose zone is up to 1 km thick. The performance, stability, and effectiveness of the transform approach is exemplified for this complex heterogeneous example, which is typical of many problems encountered in the field. It is shown that computational performance can be enhanced by several orders of magnitude with the described integral transformation approach.     

Application of a data assimilation method via an ensemble Kalman filter to reactive urea hydrolysis transport modeling

With growing importance of water resources in the world, remediations of anthropogenic contaminations due to reactive solute transport become even more important. A good understanding of reactive rate parameters such as kinetic parameters is the key to accurately predicting reactive solute transport processes and designing corresponding remediation schemes. For modeling reactive solute transport, it is very difficult to estimate chemical reaction rate parameters due to complex processes of chemical reactions and limited available data. To find a method to get the reactive rate parameters for the reactive urea hydrolysis transport modeling and obtain more accurate prediction for the chemical concentrations, we developed a data assimilation method based on an ensemble Kalman filter (EnKF) method to calibrate reactive rate parameters for modeling urea hydrolysis transport in a synthetic one-dimensional column at laboratory scale and to update modeling prediction. We applied a constrained EnKF method to pose constraints to the updated reactive rate parameters and the predicted solute concentrations based on their physical meanings after the data assimilation calibration. From the study results we concluded that we could efficiently improve the chemical reactive rate parameters with the data assimilation method via the EnKF, and at the same time we could improve solute concentration prediction. The more data we assimilated, the more accurate the reactive rate parameters and concentration prediction. The filter divergence problem was also solved in this study.     

A multiscale adjoint method to compute sensitivity coefficients for flow in heterogeneous porous media

A multiscale adjoint (MSADJ) method is developed to compute high-resolution sensitivity coefficients for subsurface flow in large-scale heterogeneous geologic formations. In this method, the original fine-scale problem is partitioned into a set of coupled subgrid problems, such that the global adjoint problem can be efficiently solved on a coarse grid. Then, the coarse-scale sensitivities are interpolated to the local fine grid by reconstructing the local variability of the model parameters with the aid of solving embedded adjoint subproblems. The approach employs the multiscale finite-volume (MSFV) formulation to accurately and efficiently solve the highly detailed flow problem. The MSFV method couples a global coarse-scale solution with local fine-scale reconstruction operators, hence yielding model responses that are quite accurate at both scales. The MSADJ method is equally efficient in computing the gradient of the objective function with respect to model parameters. Several examples demonstrate that the approach is accurate and computationally efficient. The accuracy of our multiscale method for inverse problems is twofold: the sensitivity coefficients computed by this approach are more accurate than the traditional finite-difference-based numerical method for computing derivatives, and the calibrated models after history matching honor the available dynamic data on the fine scale. In other words, the multiscale based adjoint scheme can be used to history match fine-scale models quite effectively.     

Eulerian spatial moments for solute transport in three-dimensional heterogeneous,dual-permeability media

A Eulerian analytical method is developed for nonreactive solute transport in heterogeneous, dual-permeability media where the hydraulic conductivities in fracture and matrix domains are both assumed to be stochastic processes. The analytical solution for the mean concentration is given explicitly in Fourier and Laplace transforms. Instead of using the fast fourier transform method to numerically invert the solution to real space (Hu et al., 2002), we apply the general relationship between spatial moments and concentration (Naff, 1990; Hu et al., 1997) to obtain the analytical solutions for the spatial moments up to the second for a pulse input of the solute. Owing to its accuracy and efficiency, the analytical method can be used to check the semi-analytical and Monte Carlo numerical methods before they are applied to more complicated studies. The analytical method can be also used during screening studies to identify the most significant transport parameters for further analysis. In this study, the analytical results have been compared with those obtained from the semi-analytical method (Hu et al., 2002) and the comparison shows that the semi-analytical method is robust. It is clearly shown from the analytical solution that the three factors, local dispersion, conductivity variation in each domain and velocity convection flow difference in the two domains, play different roles on the solute plume spreading in longitudinal and transverse directions. The calculation results also indicate that when the log-conductivity variance in matrix is 10 times less than its counterpart in fractures, it will hardly influence the solute transport, whether the conductivity field is matrix is treated as a homogeneous or random field.     

Analytical Solutions for Water Flow and Solute Transport in the Unsaturated Zone

Analytical solutions for the water flow and solute transport equations in the unsaturated zone are presented. We use the Broadbridge and White nonlinear model to solve the Richards’ equation for vertical flow under a constant infiltration rate. Then we extend the water flow solution and develop an exact parametric solution for the advection-dispersion equation. The method of characteristics is adopted to determine the location of a solute front in the unsaturated zone. The dispersion component is incorporated into the final solution using a singular perturbation method. The formulation of the analytical solutions is simple, and a complete solution is generated without resorting to computationally demanding numerical schemes. Indeed, the simple analytical solutions can be used as tools to verify the accuracy of numerical models of water flow and solute transport. Comparison with a finite-element numerical solution indicates that a good match for the predicted water content is achieved when the mesh grid is one-fourth the capillary length scale of the porous medium. However, when numerically solving the solute transport equation at this level of discretization, numerical dispersion and spatial oscillations were significant.     

A parallel,fully coupled,fully implicit solution to reactive transport in porous media using the preconditioned Jacobian-Free Newton-Krylov Method

Modeling large multicomponent reactive transport systems in porous media is particularly challenging when the governing partial differential algebraic equations (PDAEs) are highly nonlinear and tightly coupled due to complex nonlinear reactions and strong solution-media interactions. Here we present a preconditioned Jacobian-Free Newton-Krylov (JFNK) solution approach to solve the governing PDAEs in a fully coupled and fully implicit manner. A well-known advantage of the JFNK method is that it does not require explicitly computing and storing the Jacobian matrix during Newton nonlinear iterations. Our approach further enhances the JFNK method by utilizing physics-based, block preconditioning and a multigrid algorithm for efficient inversion of the preconditioner. This preconditioning strategy accounts for self- and optionally, cross-coupling between primary variables using diagonal and off-diagonal blocks of an approximate Jacobian, respectively. Numerical results are presented demonstrating the efficiency and massive scalability of the solution strategy for reactive transport problems involving strong solution-mineral interactions and fast kinetics. We found that the physics-based, block preconditioner significantly decreases the number of linear iterations, directly reducing computational cost; and the strongly scalable algebraic multigrid algorithm for approximate inversion of the preconditioner leads to excellent parallel scaling performance.     

Finite-element analysis of the transport of water and solutes in title-drained soils

The finite-element method based on a Galerkin technique was used to formulate the problem of simulating the two-dimensional (cross-sectional) transient movement of water and solute in saturated or partially saturated nonuniform porous media. The numerical model utilizes linear triangular elements. Nonreactive, as well as reactive solutes whose behaviour can be described by a distribution coefficient or first-order reaction term were considered. The flow portion of the model was tested by comparison of the model results with experimental and finite-difference results for transient flow in an unsaturated sand column and the solute transport portion of the model was tested by comparison with analytical solution results. The model was applied to a hypothetical case involving movement of water and solutes in tile-drained soils. The simulation results showed the development of distinct solute leaching patterns in the soil as drainage proceeded. Although applied to a tile drainage problem in this study, the model should be equally useful in the study of a wide range of two-dimensional water and solute migration problems.     

Mass-conservative finite volume methods on 2-D unstructured grids for the Richards’ equation

The solution to the 2-D time-dependent unsaturated flow equation is numerically approximated by a second-order accurate cell-centered finite-volume discretization on unstructured grids. The approximation method is based on a vertex-centered Least Squares linear reconstruction of the solution gradients at mesh edges.A Taylor series development in time of the water content dependent variable in a finite-difference framework guarantees that the proposed finite volume method is mass conservative. A Picard iterative scheme solves at each time step the resulting non-linear algebraic problem. The performance of the method is assessed on five different test cases and implementing four distinct soil constitutive relationships. The first test case deals with a column infiltration problem. It shows the capability of providing a mass-conservative behavior. The second test case verifies the numerical approximation by comparison with an analytical mixed saturated–unsaturated solution. In this case, the water drains from a fully saturated portion of a 1-D column. The third and fourth test cases illustrate the performance of the approximation scheme on sharp soil heterogeneities on 1-D and 2-D multi-layered infiltration problems. The 2-D case shows the passage of an abrupt infiltration front across a curved interface between two layers. Finally, the fifth test case compares the numerical results with an analytical solution that is developed for a 2-D heterogeneous soil with a source term representing plant roots. This last test case illustrates the formal second-order accuracy of the method in the numerical approximation of the pressure head.     

一维溶质运移源(汇)项系数反演的迭代正则化算法

对于多孔介质中发生物理化学反应的溶质运移现象,可以用带有非线性源（汇）项作用的一维对流弥散-反应扩散方程来描述,但方程中反映溶质吸附/解吸附能力的源(汇)项系数往往是未知的. 本文讨论了基于出流端浓度观测数据的源项系数反演问题. 根据Tikhonov正则化和矩阵的奇异值分解系统,建立了一种离散的迭代正则化算法,给出了算法实现步骤.数值模拟结果表明该算法不仅精度高,而且对于数据的随机扰动具有稳定性.最后应用建立的算法反演计算了一个具体的土柱试验源项系数,数值结果也表明文中所构造算法的有效性.     

Probability density functions for advective–reactive transport in radial flow

We study transport of a reactive solute in a chemically heterogeneous porous medium whose chemical properties are uncertain. The dissolved substance undergoes a heterogeneous chemical reaction with a solid phase in the presence of advection caused by extraction/injection from a point source. We present semi-analytical solutions for the probability density function of the solute concentration, which allows us to quantify predictive uncertainty associated with uncertain reaction rate constants for both linear and nonlinear reactions. This enables one to compute probabilities of rare events, which are required for quantitative risk analyses.     

Development and application of a coupled-process parameter inversion model based on the maximum likelihood estimation method

The coupled flow-mass transport inverse problem is formulated using the maximum likelihood estimation concept. An evolutionary computational algorithm, the genetic algorithm, is applied to search for a global or near-global solution. The resulting inverse model allows for flow and transport parameter estimation, based on inversion of spatial and temporal distributions of head and concentration measurements. Numerical experiments using a subset of the three-dimensional tracer tests conducted at the Columbus, Mississippi site are presented to test the model's ability to identify a wide range of parameters and parametrization schemes. The results indicate that the model can be applied to identify zoned parameters of hydraulic conductivity, geostatistical parameters of the hydraulic conductivity field, angle of hydraulic conductivity anisotropy, solute hydrodynamic dispersivity, and sorption parameters. The identification criterion, or objective function residual, is shown to decrease significantly as the complexity of the hydraulic conductivity parametrization is increased. Predictive modeling using the estimated parameters indicated that the geostatistical hydraulic conductivity distribution scheme produced good agreement between simulated and observed heads and concentrations. The genetic algorithm, while providing apparently robust solutions, is found to be considerably less efficient computationally than a quasi-Newton algorithm.     

Positive solution of two-dimensional solute transport in heterogeneous aquifers

The transport of contaminants in aquifers is usually represented by a convection-dispersion equation. There are several well-known problems of oscillation and artificial dispersion that affect the numerical solution of this equation. For example, several studies have shown that standard treatment of the cross-dispersion terms always leads to a negative concentration. It is also well known that the numerical solution of the convective term is affected by spurious oscillations or substantial numerical dispersion. These difficulties are especially significant for solute transport in nonuniform flow in heterogeneous aquifers. For the case of coupled reactive-transport models, even small negative concentration values can become amplified through nonlinear reaction source/sink terms and thus result in physically erroneous and unstable results. This paper includes a brief discussion about how nonpositive concentrations arise from numerical solution of the convection and cross-dispersion terms. We demonstrate the effectiveness of directional splitting with one-dimensional flux limiters for the convection term. Also, a new numerical scheme for the dispersion term that preserves positivity is presented. The results of the proposed convection scheme and the solution given by the new method to compute dispersion are compared with standard numerical methods as used in MT3DMS.     

Smooth Particle Hydrodynamics with nonlinear Moving-Least-Squares WENO reconstruction to model anisotropic dispersion in porous media

Most numerical schemes applied to solve the advection–diffusion equation are affected by numerical diffusion. Moreover, unphysical results, such as oscillations and negative concentrations, may emerge when an anisotropic dispersion tensor is used, which induces even more severe errors in the solution of multispecies reactive transport. To cope with this long standing problem we propose a modified version of the standard Smoothed Particle Hydrodynamics (SPH) method based on a Moving-Least-Squares-Weighted-Essentially-Non-Oscillatory (MLS-WENO) reconstruction of concentrations. This scheme formulation (called MWSPH) approximates the diffusive fluxes with a Rusanov-type Riemann solver based on high order WENO scheme. We compare the standard SPH with the MWSPH for different a few test cases, considering both homogeneous and heterogeneous flow fields and different anisotropic ratios of the dispersion tensor. We show that, MWSPH is stable and accurate and that it reduces the occurrence of negative concentrations compared to standard SPH. When negative concentrations are observed, their absolute values are several orders of magnitude smaller compared to standard SPH. In addition, MWSPH limits spurious oscillations in the numerical solution more effectively than classical SPH. Convergence analysis shows that MWSPH is computationally more demanding than SPH, but with the payoff a more accurate solution, which in addition is less sensitive to particles position. The latter property simplifies the time consuming and often user dependent procedure to define the initial dislocation of the particles.     

Solution of the nonlinear transport equation using modified Picard iteration

The transport and fate of reactive chemicals in groundwater is governed by equations which are often difficult to solve due to the nonlinear relationship between the solute concentrations for the liquid and solid phases. The nonlinearity may cause mass balance errors during the numerical simulation in addition to numerical errors for linear transport system. We have generalized the modified Picard iteration algorithm of Celia et al.⁵ for unsaturated flow to solve the nonlinear transport equation. Written in a ‘mixed-form’ formulation, the total solute concentration is expanded in a Taylor series with respect to the solution concentration to linearize the transport equation, which is then solved with a conventional finite element method. Numerical results of this mixed-form algorithm are compared with those obtained with the concentration-based scheme using conventional Picard iteration. In general, the new solver resulted in negligible mass balance errors (< ∥10⁻⁸∥%) and required less computational time than the conventional iteration scheme for the test examples, including transport involving highly nonlinear adsorption under steady-state as well as transient flow conditions. In contrast, mass balance errors resulting from the conventional Picard iteration method were higher than 10% for some highly nonlinear problems. Application of the modified Picard iteration scheme to solve the nonlinear transport equation may greatly reduce the mass balance errors and increase computational efficiency.     

Transport in chemically and mechanically heterogeneous porous media. I: Theoretical development of region-averaged equations for slightly compressible single-phase flow

Transport processes in heterogeneous porous media are often treated in terms of one-equation models. Such treatment assumes that the velocity, pressure, temperature, and concentration can be represented in terms of a single large-scale averaged quantity in regions having significantly different mechanical, thermal, and chemical properties. In this paper we explore the process of single-phase flow in a two-region model of heterogeneous porous media. The region-averaged equations are developed for the case of a slightly compressible flow which is an accurate representation for a certain class of liquid-phase flows. The analysis leads to a pair of transport equations for the region averaged pressures that are coupled through a classic exchange term, in addition to being coupled by a diffusive cross effect. The domain of validity of the theory has been identified in terms of a series of length and timescale constraints.In Part II the theory is tested, in the absence of adjustable parameters, by comparison with numerical experiments for transient, slightly compressible flow in both stratified and nodular models of heterogeneous porous media. Good agreement between theory and experiment is obtained for nodular and stratified systems, and effective transport coefficients for a wide range of conditions are presented on the basis of solutions of the three closure problems that appear in the theory. Part III of this paper deals with the principle of large-scale mechanical equilibrium and the region-averaged form of Darcy's law. This form is necessary for the development and solution of the region-averaged solute transport equations that are presented in Part IV. Finally, in Part V we present results for the dispersion tensors and the exchange coefficient associated with the two-region model of solute transport with adsorption.     

A quasi three-dimensional model for flow and transport in unsaturated and saturated zones: 1. Implementation of the quasi two-dimensional case

A quasi three-dimensional (QUASI 3-D) model is presented for simulating the subsurface water flow and solute transport in the unsaturated and in the saturated zones of soil. The model is based on the assumptions of vertical flow in the unsaturated zone and essentially horizontal groundwater flow. The 1-D Richards equation for the unsaturated zone is coupled at the phreatic surface with the 2-D flow equation for the saturated zone. The latter was obtained by averaging 3-D flow equation in the saturated zone over the aquifer thickness. Unlike the Boussinesq equation for a leaky-phreatic aquifer, the developed model does not contain a storage term with specific yield and a source term for natural replenishment. Instead it includes a water flux term at the phreatic surface through which the Richards equation is linked with the groundwater flow equation. The vertical water flux in the saturated zone is evaluated on the basis of the fluid mass balance equation while the horizontal fluxes, in that equation, are prescribed by Darcy law. A 3-D transport equation is used to simulate the solute migration. A numerical algorithm to solve the problem for the general quasi 3-D case was developed. The developed methodology was exemplified for the quasi 2-D cross-sectional case (QUASI2D). Simulations for three synthetic problems demonstrate good agreement between the results obtained by QUASI2D and two fully 2-D flow and transport codes (SUTRA and 2DSOIL). Yet, simulations with the QUASI2D code were several times faster than those by the SUTRA and the 2DSOIL codes.     

Parameter estimation in nonlinear environmental problems

Popular parameter estimation methods, including least squares, maximum likelihood, and maximum a posteriori (MAP), solve an optimization problem to obtain a central value (or best estimate) followed by an approximate evaluation of the spread (or covariance matrix). A different approach is the Monte Carlo (MC) method, and particularly Markov chain Monte Carlo (MCMC) methods, which allow sampling from the posterior distribution of the parameters. Though available for years, MC methods have only recently drawn wide attention as practical ways for solving challenging high-dimensional parameter estimation problems. They have a broader scope of applications than conventional methods and can be used to derive the full posterior pdf but can be computationally very intensive. This paper compares a number of different methods and presents improvements using as case study a nonlinear DNAPL source dissolution and solute transport model. This depth-integrated semi-analytical model approximates dissolution from the DNAPL source zone using nonlinear empirical equations with partially known parameters. It then calculates the DNAPL plume concentration in the aquifer by solving the advection-dispersion equation with a flux boundary. The comparison is among the classical MAP and some versions of computer-intensive Monte Carlo methods, including the Metropolis–Hastings (MH) method and the adaptive direction sampling (ADS) method.     

MODFLOW/MT3DMS-based simulation of variable-density ground water flow and transport

This paper presents an approach for coupling MODFLOW and MT3DMS for the simulation of variable-density ground water flow. MODFLOW routines were modified to solve a variable-density form of the ground water flow equation in which the density terms are calculated using an equation of state and the simulated MT3DMS solute concentrations. Changes to the MODFLOW and MT3DMS input files were kept to a minimum, and thus existing data files and data files created with most pre- and postprocessors can be used directly with the SEAWAT code. The approach was tested by simulating the Henry problem and two of the saltpool laboratory experiments (low- and high-density cases). For the Henry problem, the simulated results compared well with the steady-state semianalytic solution and also the transient isochlor movement as simulated by a finite-element model. For the saltpool problem, the simulated breakthrough curves compared better with the laboratory measurements for the low-density case than for the high-density case but showed good agreement with the measured salinity isosurfaces for both cases. Results from the test cases presented here indicate that the MODFLOW/MT3DMS approach provides accurate solutions for problems involving variable-density ground water flow and solute transport.