Influence of small-scale heterogeneities on contaminant transport in fractured crystalline rock

We present a sequence of purely advective transport models that demonstrate the influence of small-scale geometric inhomogeneities on contaminant transport in fractured crystalline rock. Special weight is placed on the role of statistically generated variable fracture apertures. The fracture network geometry and the aperture distribution are based on information from an in situ radionuclide retardation experiment performed at Grimsel test site (Swiss Alps). The obtained breakthrough curves are fitted with the advection dispersion equation and continuous-time random walks (CTRW). CTRW is found to provide superior fits to the late-arrival tailing and is also found to show a good correlation with the velocity distributions obtained from the hydraulic models. The impact of small-scale heterogeneities, both in fracture geometry and aperture, on transport is shown to be considerable.     

Continuous time random walks for non-local radial solute transport

This study formulates and analyzes continuous time random walk (CTRW) models in radial flow geometries for the quantification of non-local solute transport induced by heterogeneous flow distributions and by mobile–immobile mass transfer processes. To this end we derive a general CTRW framework in radial coordinates starting from the random walk equations for radial particle positions and times. The particle density, or solute concentration is governed by a non-local radial advection–dispersion equation (ADE). Unlike in CTRWs for uniform flow scenarios, particle transition times here depend on the radial particle position, which renders the CTRW non-stationary. As a consequence, the memory kernel characterizing the non-local ADE, is radially dependent. Based on this general formulation, we derive radial CTRW implementations that (i) emulate non-local radial transport due to heterogeneous advection, (ii) model multirate mass transfer (MRMT) between mobile and immobile continua, and (iii) quantify both heterogeneous advection in a mobile region and mass transfer between mobile and immobile regions. The expected solute breakthrough behavior is studied using numerical random walk particle tracking simulations. This behavior is analyzed by explicit analytical expressions for the asymptotic solute breakthrough curves. We observe clear power-law tails of the solute breakthrough for broad (power-law) distributions of particle transit times (heterogeneous advection) and particle trapping times (MRMT model). The combined model displays two distinct time regimes. An intermediate regime, in which the solute breakthrough is dominated by the particle transit times in the mobile zones, and a late time regime that is governed by the distribution of particle trapping times in immobile zones. These radial CTRW formulations allow for the identification of heterogeneous advection and mobile-immobile processes as drivers of anomalous transport, under conditions relevant for field tracer tests.     

Chaotic advection at the pore scale: Mechanisms,upscaling and implications for macroscopic transport

The macroscopic spreading and mixing of solute plumes in saturated porous media is ultimately controlled by processes operating at the pore scale. Whilst the conventional picture of pore-scale mechanical dispersion and molecular diffusion leading to persistent hydrodynamic dispersion is well accepted, this paradigm is inherently two-dimensional (2D) in nature and neglects important three-dimensional (3D) phenomena. We discuss how the kinematics of steady 3D flow at the pore scale generate chaotic advection—involving exponential stretching and folding of fluid elements—the mechanisms by which it arises and implications of microscopic chaos for macroscopic dispersion and mixing. Prohibited in steady 2D flow due to topological constraints, these phenomena are ubiquitous due to the topological complexity inherent to all 3D porous media. Consequently 3D porous media flows generate profoundly different fluid deformation and mixing processes to those of 2D flow. The interplay of chaotic advection and broad transit time distributions can be incorporated into a continuous-time random walk (CTRW) framework to predict macroscopic solute mixing and spreading. We show how these results may be generalised to real porous architectures via a CTRW model of fluid deformation, leading to stochastic models of macroscopic dispersion and mixing which both honour the pore-scale kinematics and are directly conditioned on the pore-scale architecture.     

Statistical scale-up of 3D particle-tracking simulation for non-Fickian dispersive solute transport modeling

Numerical techniques for subsurface flow and transport modeling are often limited by computational limitations including fine mesh and small time steps to control artificial dispersion. Particle-tracking simulation offers a robust alternative for modeling solute transport in subsurface formations. However, the modeling scale usually differs substantially from the rock measurement scale, and the scale-up of measurements have to be made accounting for the pattern of spatial heterogeneity exhibited at different scales. Therefore, it is important to construct accurate coarse-scale simulations that are capable of capturing the uncertainties in reservoir and transport attributes due to scale-up. A statistical scale-up procedure developed in our previous work is extended by considering the effects of unresolved (residual) heterogeneity below the resolution of the finest modeling scale in 3D. First, a scale-up procedure based on the concept of volume variance is employed to construct realizations of permeability and porosity at the (coarse) transport modeling scale, at which flow or transport simulation is performed. Next, to compute various effective transport parameters, a series of realizations exhibiting detailed heterogeneities at the fine scale, whose domain size is the same as the transport modeling scale, are generated. These realizations are subjected to a hybrid particle-tracking simulation. Probabilistic transition time is considered, borrowing the idea from the continuous time random walk (CTRW) technique to account for any sub-scale heterogeneity at the fine scale level. The approach is validated against analytical solutions and general CTRW formulation. Finally, coarse-scale transport variables (i.e., dispersivities and parameterization of transition time distribution) are calibrated by minimizing the mismatch in effluent history with the equivalent averaged models. Construction of conditional probability distributions of effective parameters is facilitated by integrating the results over the entire suite of realizations. The proposed method is flexible, as it does not invoke any explicit assumption regarding the multivariate distribution of the heterogeneity. In contrast to other hierarchical CTRW formulation for modeling multi-scale heterogeneities, the proposed approach does not impose any length scale requirement regarding sub-grid heterogeneities. In fact, it aims to capture the uncertainty in effective reservoir and transport properties due to the presence of heterogeneity at the intermediate scale, which is larger than the finest resolution of heterogeneity but smaller than the representative elementary volume, but it is often comparable to the transport modeling scale.     

Experiment and Simulation of Non-Reactive Solute Transport in Porous Media

To more accurately predict the migration behavior of pollutants in porous media, we conduct laboratory scale experiments and model simulation. Aniline (AN) is used in one-dimensional soil column experiments designed under various media and hydrodynamic conditions. The advection-dispersion equation (ADE) and the continuous-time random walk (CTRW) were used to simulate the breakthrough curves (BTCs) of the solute transport. The results show that the media and hydrodynamic conditions are two important factors affecting solute transport and are related to the degree of non-Fickian transport. The simulation results show that CTRW can more effectively describe the non-Fickian phenomenon in the solute transport process than ADE. The sensitive parameter in the CTRW simulation process is , which can reflect the degree of non-Fickian diffusion in the solute transport. Understanding the relationship of with velocity and media particle size is conducive to improving the reactive solute transport model. The results of this study provide a theoretical basis for better prediction of pollutant transport in groundwater.     

Modeling contaminant transport in homogeneous porous media with fractional advection-dispersion equation

The newly developed Fractional Advection-Dispersion Equation (FADE), which is FADE was extended and used in this paper for modelling adsorbing contaminant transport by adding an adsorbing term. A parameter estimation method and its corresponding FORTRAN based program named FADEMain were developed on the basis of Nonlinear Least Square Algorithm and the analytical solution for one-dimensional FADE under the conditions of step input and steady state flow. Data sets of adsorbing contaminants Cd and NH4+-N transport in short homogeneous soil columns and conservative solute NaCI transport in a long homogeneous soil column, respectively were used to estimate the transport parameters both by FADEMain and the advection-dispersion equation (ADE) based program CXTFIT2.1. Results indicated that the concentration simulated by FADE agreed well with the measured data. Compared to the ADE model, FADE can provide better simulation for the concentration in the initial lower concentration part and the late higher concentration part of the breakthrough curves for both adsorbing contaminants. The dispersion coefficients for ADE were from 0.13 to 7.06 cm2/min, while the dispersion coefficients for FADE ranged from 0.119 to 3.05 cm1.856/min for NaCI transport in the long homogeneous soil column. We found that the dispersion coefficient of FADE increased with the transport distance, and the relationship between them can be quantified with an exponential function. Less scale-dependent was also found for the dispersion coefficient of FADE with respect to ADE.     

Developing a Lagrangian sediment transport model for open channel flows

A three-dimensional stochastic Lagrangian particle tracking sediment transport model is developed to solve the discrete advection-dispersion equation using a combination of empirical dispersion equations.The performance of three widely-used longitudinal dispersion coefficient equations was examined to select one of them as the primary dispersion equation term in the developed model. Also, a conditional empirical equation was used to consider the effect of vertical dispersion term in top layers n...     

Can a Time Fractional‐Derivative Model Capture Scale‐Dependent Dispersion in Saturated Soils?

Time nonlocal transport models such as the time fractional advection‐dispersion equation (t‐fADE) were proposed to capture well‐documented non‐Fickian dynamics for conservative solutes transport in heterogeneous media, with the underlying assumption that the time nonlocality (which means that the current concentration change is affected by previous concentration load) embedded in the physical models can release the effective dispersion coefficient from scale dependency. This assumption, however, has never been systematically examined using real data. This study fills this historical knowledge gap by capturing non‐Fickian transport (likely due to solute retention) documented in the literature (Huang et al. 1995) and observed in our laboratory from small to intermediate spatial scale using the promising, tempered t‐fADE model. Fitting exercises show that the effective dispersion coefficient in the t‐fADE, although differing subtly from the dispersion coefficient in the standard advection‐dispersion equation, increases nonlinearly with the travel distance (varying from 0.5 to 12 m) for both heterogeneous and macroscopically homogeneous sand columns. Further analysis reveals that, while solute retention in relatively immobile zones can be efficiently captured by the time nonlocal parameters in the t‐fADE, the motion‐independent solute movement in the mobile zone is affected by the spatial evolution of local velocities in the host medium, resulting in a scale‐dependent dispersion coefficient. The same result may be found for the other standard time nonlocal transport models that separate solute retention and jumps (i.e., displacement). Therefore, the t‐fADE with a constant dispersion coefficient cannot capture scale‐dependent dispersion in saturated porous media, challenging the application for stochastic hydrogeology methods in quantifying real‐world, preasymptotic transport. Hence improvements on time nonlocal models using, for example, the novel subordination approach are necessary to incorporate the spatial evolution of local velocities without adding cumbersome parameters.     

Interpretation and nonuniqueness of CTRW transition distributions: Insights from an alternative solute transport formulation

The continuous time random walk (CTRW) has both an elegant mathematical theory and a successful record at modeling solute transport in the subsurface. However, there are some interpretation ambiguities relating to the relationship between the discrete CTRW transition distributions and the underlying continuous movement of solute that have not been addressed in existing literature. These include the exact definition of “transition”, and the extent to which transition probability distributions are unique/quantifiable from data. Here, we present some theoretical results which address these uncertainties in systems with an advective bias. Simultaneously, we present an alternative, reduced parameter CTRW formulation for general advective transport in heterogeneous porous media, which models early- and late-time transport by use of random transition times between sparse, imaginary planes normal to flow. We show that even in the context of this reduced-parameter formulation there is nonuniqueness in the definitions of both transition lengths and waiting time distributions, and that neither may be uniquely determined from experimental data. For practical use of this formulation, we suggest Pareto transition time distributions, leading to a two-degree-of-freedom modeling approach. We then demonstrate the power of this approach in fitting two sets of existing experimental data. While the primary focus is the presentation of new results, the discussion is designed to be pedagogical and to provide a good entry point into practical modeling of solute transport with the CTRW.     

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.     

Effective macroscopic transport parameters between parallel plates with constant concentration boundaries

A macroscopic transport model is developed, following the Taylor shear dispersion analysis procedure, for a 2D laminar shear flow between parallel plates possessing a constant specified concentration. This idealized geometry models flow with contaminant dissolution at pore-scale in a contaminant source zone and flow in a rock fracture with dissolving walls. We upscale a macroscopic transient transport model with effective transport coefficients of mean velocity, macroscopic dispersion, and first-order mass transfer rate. To validate the macroscopic model the mean concentration, covariance, and wall concentration gradient are compared to the results of numerical simulations of the advection–diffusion equation and the Graetz solution. Results indicate that in the presence of local-scale variations and constant concentration boundaries, the upscaled mean velocity and macrodispersion coefficient differ from those of the Taylor–Aris dispersion, and the mass transfer flux described by the first-order mass transfer model is larger than the diffusive mass flux from the constant wall. In addition, the upscaled first-order mass transfer coefficient in the macroscopic model depends only on the plate gap and diffusion coefficient. Therefore, the upscaled first-order mass transfer coefficient is independent of the mean velocity and travel distance, leading to a constant pore-scale Sherwood number of 12. By contrast, the effective Sherwood number determined by the diffusive mass flux is a function of the Peclet number for small Peclet number, and approaches a constant of 10.3 for large Peclet number.     

A finite element solution for the fractional advection–dispersion equation

The fractional advection–dispersion equation (FADE) known as its non-local dispersion, has been proven to be a promising tool to simulate anomalous solute transport in groundwater. We present an unconditionally stable finite element (FEM) approach to solve the one-dimensional FADE based on the Caputo definition of the fractional derivative with considering its singularity at the boundaries. The stability and accuracy of the FEM solution is verified against the analytical solution, and the sensitivity of the FEM solution to the fractional order α and the skewness parameter β is analyzed. We find that the proposed numerical approach converge to the numerical solution of the advection–dispersion equation (ADE) as the fractional order α equals 2. The problem caused by using the first- or third-kind boundary with an integral-order derivative at the inlet is remedied by using the third-kind boundary with a fractional-order derivative there. The problems for concentration estimation at boundaries caused by the singularity of the fractional derivative can be solved by using the concept of transition probability conservation. The FEM solution of this study has smaller numerical dispersion than that of the FD solution by Meerschaert and Tadjeran (J Comput Appl Math 2004). For a given α, the spatial distribution of concentration exhibits a symmetric non-Fickian behavior when β = 0. The spatial distribution of concentration shows a Fickian behavior on the left-hand side of the spatial domain and a notable non-Fickian behavior on the right-hand side of the spatial domain when β = 1, whereas when β = −1 the spatial distribution of concentration is the opposite of that of β = 1. Finally, the numerical approach is applied to simulate the atrazine transport in a saturated soil column and the results indicat that the FEM solution of the FADE could better simulate the atrazine transport process than that of the ADE, especially at the tail of the breakthrough curves.     

Mathematical modeling and practical verification of groundwater and contaminant transport in a chosen natural aquifer

The paper addresses the 2D mathematical equation of conservative contaminant transport in an aquifer for chosen contaminants. The contaminants (chlorides and sulfates) are subject to instantaneous reversible part of sorption process. The term of instantaneous reversible sorption in the presented equation has been described by the non-linear Freundlich adsorption isotherm, widely applied in practice in relation to static processes (for local equilibrium). The numerical solution (using the finite difference method) has been based on the previously calculated values of longitudinal and transverse dispersion coefficients and the non-linear adsorption parameters for the chosen contaminants. Based on this model, the values of chloride and sulfate concentration isolines have been calculated and compared with the measured maximal concentrations in the chosen natural aquifer (installed piezometers). Additionally, the values of chloride concentrations have been calculated taking into account the influence of radioactive decay term, using the numerical value of the firstorder decay rate constant for an adopted theoretical radionuclide.     

Copper dispersion in ephemeral stream sediments

Sediment transport related parameters in ephemeral streams may be used to model and delineate: (1) average dispersion patterns of copper-laden sediments; (2) differences in dispersion of copper in bedload and suspended sediments; and (3) variability in the copper-sediment dispersion patterns. A model that effectively describes dispersion of copper in ephemeral stream sediments in a simple mixing model: where C_r is the resultant concentration beneath the confluence of the main channel with a tributary, C_t is the concentration of metal in sediments of the tributary, C_m is the metal concentration in main channel sediments, and X_m and X_t are the basin areas or sediment yields of the main channel and tributary channel at their confluence. Variability in metal concentrations about values predicted by this model may be due to the different responses of bedload and suspended load to changes in stream hydraulics, the dynamics of bedload transport, the spatial and temporal variability rainfall within the drainage basin, and chemical mobility of the copper.     

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.     

Nonlocal transport models for capturing solute transport in one-dimensional sand columns: Model review,applicability, limitations and improvement

Modelling pollutant transport in water is one of the core tasks of computational hydrology, and various physical models including especially the widely used nonlocal transport models have been developed and applied in the last three decades. No studies, however, have been conducted to systematically assess the applicability, limitations and improvement of these nonlocal transport models. To fill this knowledge gap, this study reviewed, tested and improved the state-of-the-art nonlocal transport models, including their physical background, mathematical formula and especially the capability to quantify conservative tracers moving in one-dimensional sand columns, which represents perhaps the simplest real-world application. Applications showed that, surprisingly, neither the popular time-nonlocal transport models (including the multi-rate mass transfer model, the continuous time random walk framework and the time fractional advection-dispersion equation), nor the spatiotemporally nonlocal transport model (ST-fADE) can accurately fit passive tracers moving through a 15-m-long heterogeneous sand column documented in literature, if a constant dispersion coefficient or dispersivity is used. This is because pollutant transport in heterogeneous media can be scale-dependent (represented by a dispersion coefficient or dispersivity increasing with spatiotemporal scales), non-Fickian (where plume variance increases nonlinearly in time) and/or pre-asymptotic (with transition between non-Fickian and Fickian transport). These different properties cannot be simultaneously and accurately modelled by any of the transport models reviewed by this study. To bypass this limitation, five possible corrections were proposed, and two of them were tested successfully, including a time fractional and space Hausdorff fractal model which minimizes the scale-dependency of the dispersion coefficient in the non-Euclidean space, and a two-region time fractional advection-dispersion equation which accounts for the spatial mixing of solute particles from different mobile domains. Therefore, more efforts are still needed to accurately model transport in non-ideal porous media, and the five model corrections proposed by this study may shed light on these indispensable modelling efforts.     

Effects of rate-limited mass transfer on water sampling with partially penetrating wells

Nonequilibrium concentration type curves are numerically developed and sensitivity analyses are performed to examine the relationships between effluent concentrations in partially penetrating monitoring/extraction wells, the vertical plume shape, and the mass transfer characteristics of the aquifer. The governing two-dimensional, axisymmetric nonequilibrium solute transport equation is solved in three stages using an operator-splitting approach. In the first two stages, the advection and dispersion terms are solved with the Eulerian-Lagrangian method, based on the backward method of characteristics for advection and the standard implicit Galerkin finite element method for dispersion. In the third step, the first-order, immobile-mobile domain mass transfer term is computed analytically for both two-site and lognormally distributed, multirate models. Effluent concentration variations with time and contour plots of the pore water concentration distribution in the aquifer are compared for a wide range of field- and laboratory-measured mass transfer rates, various plume shapes, and relevant physical/chemical parameter values, including pumping rate, vertical anisotropy ratio, retardation factor, and porosity. The simulation results show that rate-limited mass transfer can have a significant impact on sample and aquifer pore water concentrations during three-dimensional transport to a partially penetrating well. An alternative dimensionless form of the nonequilibrium solute transport equation is derived to illustrate the key parameter groupings that quantify rate-limited sorption effects and show the relative importance of individual parameters. A hypothetical field application example demonstrates the fitting of dimensional type curves to discrete-interval sampling data in order to evaluate the mass transfer characteristics of an aquifer and shows how type curve superposition can be used to model complex plume shapes.     

基于MATLAB工具箱的地震预测模型

地震分析和预测对未来地震趋势有一定预见性。本文建立了基于MATLAB工具箱的地震预测模型,通过建模、局限性分析,认为多元线性和非线性回归方法不适合地震预测,基于BP神经网络的方法在地震预报中有一定应用价值。     

Relaxation and reversibility of extended Taylor dispersion from a Markovian–Lagrangian point of view

Taylor dispersion in a two-dimensional (2D) stratified velocity field describes a transition, called relaxation, from convective behaviour for short times, towards Fickian behaviour for large times and is partially reversible upon reversal of the flow direction. In 2D the physics are assumed to be governed by the unidirectional convection diffusion equation (2D uCDE). The approximate height-averaged 1D Generalised Telegraph Equation (GTE) catches an essential part of the longitudinal spreading. Contrary to the 1D Fickian approach, it explicitly accounts for the transient reversible nature [Camacho J. Purely global model for Taylor dispersion. Phys Rev E 1993/2;48(1); Berentsen CWJ, Verlaan ML, van Kruijsdijk CPJW. Upscaling and reversibility of Taylor dispersion in heterogeneous porous media. Phys Rev E 2005;71:046308].