Environmental risk evaluation for radionuclide transport through natural barriers of nuclear waste disposal with multi-scale streamline approaches.

Natural barriers, encompassing stable geological formations that serve as the final bastion against radionuclide transport, are paramount in mitigating the long-term contamination risks associated with the nuclear waste disposal. Therefore, it is important to simulate and predict the processes and spatial-temporal distributions of radionuclide transport within these barriers. However, accurately predicting radionuclide transport on the field scale is challenging due to uncertainties associated with parameter scaling. This study develops an integrated evaluation framework that combines upscaled parameters, streamline transport models, and response surface techniques to systematically assess environmental risk metrics and parameter uncertainties across different scales. Initially, upscaling methods are established to estimate the prior interval of critical transport parameters at the field scale, and streamline models are derived by considering the radionuclides transport with a variety of physicochemical mechanisms and geological characterizations in natural barriers. To assess uncertainty ranges of the risk metrics related to upscaled parameters, uncertainty quantification is performed on the ground of 5000 Monte Carlo simulations. The results indicate that the upscaled dispersivity of fractured media (αLf) has a relatively high sensitivity ranking on release dose for all nuclides, and upscaled matrix sorption coefficient (Kd) of Pu-242 strongly affects breakthrough time and release dose of Pu-242. Facilitated by robust response surface with the lowest R2 of 0.89, it is shown that the release doses of Pu-242 and Pb-210 increase under conditions of low Kd and αLf, respectively. Furthermore, statistical analysis reveals that employing limited laboratory-scale parameters results in narrower confidence intervals for risk metrics, while upscaling methods better account for the highly heterogeneous properties of large-scale field conditions. The developed risk evaluation framework provides valuable insights for utilizing upscaled parameters and modeling radionuclide transport within natural barriers under various scenarios.

Conceptualizing future groundwater models through a ternary framework of multisource data, human expertise, and machine intelligence.

Groundwater models are essential for understanding aquifer systems behavior and effective water resources spatio-temporal distributions, yet they are often hindered by challenges related to model assumptions, parametrization, uncertainty, and computational efficiency. Machine intelligence, especially deep learning, promises a paradigm shift in overcoming these challenges. A critical examination of existing machine-driven methods reveals the inherent limitations, particularly in terms of the interpretability and the ability to generalize findings. To overcome these challenges, we develop a ternary framework that synergizes the valuable insights from multisource data, human expertise, and machine intelligence. This framework capitalizes on the distinct strengths of each element: the value and relevance of multisource data, the innovative capacity of human expertise, and the analytical efficiency of machine intelligence. Our goal is to conceptualize sustainable water management practices and enhance our understanding and predictive capabilities of groundwater systems. Unlike approaches that rely solely on abundant data, our framework emphasizes the quality and strategic use of available data, combined with human intellect and advanced computing, to overcome current limitations and pave the way for more realistic groundwater simulations.

Quantifying the impact of upscaled parameters on radionuclide transport in three-dimensional fracture-matrix systems.

Assessing the long-term safety of geological repositories for high-level radioactive waste is critically dependent on understanding radionuclide transport in multi-scale fractured rocks. This study explores the influence of upscaled parameters on radionuclide movement within a three-dimensional fracture-matrix system using a discrete fracture-matrix (DFM) model. The developed numerical simulation workflow includes creating a random discrete fracture network, meshing of the fractures and matrix, assigning upscaled parameters, and conducting finite element simulations. We simulated the spatiotemporal evolution of radionuclide concentrations in the fractures and matrix over a century, revealing significant spatial heterogeneity driven by a heterogeneous seepage field. Employing geostatistics-based upscaling methods, we predicted the effective ranges of crucial solute transport parameters at the field scale. The matrix diffusion coefficient, matrix distribution coefficient, and longitudinal dispersivity were upscaled by factors of 2.0-3.0, 2.5-4.0, and 10-104, respectively, based on laboratory-scale measurements. Incorporating these upscaled parameters into the DFM model, we analyzed their impact on radionuclide transport. Our findings demonstrate that an upscaled matrix diffusion coefficient and matrix distribution coefficient result in a delayed transport of radionuclides in fractures by enhancing mass transfer between the fractures and rock matrix, while an upscaled longitudinal dispersivity accelerates transport by advancing the positions of concentration peaks. Sensitivity analysis revealed that the matrix distribution coefficient is the most impactful, followed by dispersivity and matrix diffusion coefficient. These insights are important for minimizing parameter uncertainties and enhancing the accuracy of predictions concerning radionuclide transport in multi-scale fractured rocks.

Investigating key drivers of N2O emissions in heterogeneous riparian sediments: Reactive transport modeling and statistical analysis.

Nitrous oxide (N2O) is a potent greenhouse gas that also contributes to ozone depletion. Recent studies have identified river corridors as significant sources of N2O emissions. Surface water-groundwater (hyporheic) interactions along river corridors induce flow and reactive nitrogen transport through riparian sediments, thereby generating N2O. Despite the prevalence of these processes, the controlling influence of physical and geochemical parameters on N2O emissions from coupled aerobic and anaerobic reactive transport processes in heterogeneous riparian sediments is not yet fully understood. This study presents an integrated framework that combines a flow and multi-component reactive transport model (RTM) with an uncertainty quantification and sensitivity analysis tool to determine which physical and geochemical parameters have the greatest impact on N2O emissions from riparian sediments. The framework involves the development of thousands of RTMs, followed by global sensitivity and responsive surface analyses. Results indicate that characterizing the denitrification reaction rate constant and permeability of intermediate-permeability sediments (e.g., sandy gravel) are crucial in describing coupled nitrification-denitrification reactions and the magnitude of N2O emissions. This study provides valuable insights into the factors that influence N2O emissions from riparian sediments and can help in developing strategies to control N2O emissions from river corridors.

Upscaling dispersivity for conservative solute transport in naturally fractured media.

Physical heterogeneities are prevalent features of fracture systems and significantly impact transport processes in aquifers across different spatiotemporal scales. Upscaling solute transport parameter is an effective way of quantifying parameter variability in heterogeneous aquifers including fractured media. This paper develops conceptual models for upscaling conservative transport parameters in fracture media. The focus is on upscaling dispersivity. Lagrangian-based transport model (LBTM) for dispersivity upscaling are derived for the solute transport in two-dimensional fractures surrounded by an impermeable matrix. The LBTM is validated against the random walk particle tracking (RWPT) model, which enables highly efficient and accurate predictions of conservative solute transport. The results show that the derived scale-dependent analytical expressions are in excellent agreement with RWPT model results. In addition, LBTM results are also compared to experimental results from the observed breakthrough curve of a conservative solute transport through a single natural fracture within a granite core. Comparing results from the LBTM and transport experiment shows that LBTM based estimated dispersivity is 10.55% higher than the measured value. Errors introduced by the experiments, the conceptual assumptions in deriving models, and the heterogeneities of fracture apertures not fully sampled by measuring instruments are main factor for such discrepancy. The sensitivity analysis indicates that the longitudinal and transverse dispersivities are positively related to the integral scale and the variance of the log-fracture aperture. The longitudinal dispersivity is strongly contolled by the variance of the log-fracture aperture. The LBTM may be useful for directly predicting solute transports, requiring only the acquisition of fractured geostatistical data. This work provides a better understanding of transport processes in fractured media which ultimately control water quality across scales.

Plutonium reactive transport in fractured granite: Multi-species experiments and simulations.

Plutonium (Pu) in the subsurface environment can transport in different oxidation states as an aqueous solute or as colloidal particles. The transport behavior of Pu is affected by the relative abundances of these species and can be difficult to predict when they simultaneously exist. This study investigates the concurrent transport of Pu intrinsic colloids, Pu(IV)(aq) and Pu(V-VI)(aq) through a combination of controlled experiments and semi-analytical dual-porosity transport modeling. Pu transport experiments were conducted in a fractured granite at high and low flow rates to elucidate sorption processes and their scaling behavior. In the experiments, Pu(IV)(aq) was the least mobile of the Pu species, Pu(V-VI)(aq) had intermediate mobility, and the colloidal Pu, which consisted mainly of precipitated and/or hydrolyzed Pu(IV), was the most mobile. The semi-analytical modeling revealed that the sorption of each Pu species was rate-limited, as the sorption could not be described by assuming local equilibrium in the experiments. The model was able to describe the sorption of the different Pu species that occurring either on fracture surfaces, in the pores of the rock matrix, or simultaneously in both locations. While equally good fits to the data could be achieved using any of these assumptions, a fracture-dominated process was considered to be the most plausible because it provided the most reasonable estimates of sorption rate constants. Importantly, a key result of this work is that the sorption rate constant of all Pu species tends to decrease with increasing time scales, which implies that Pu will tend to be more mobile at longer time scales than observations at shorter time scales suggest. This result has important implications for predicting the environmental impacts of Pu in the safety assessments of geologic repositories for radioactive waste disposal, and we explore potential mechanistic bases for upscaling the sorption rate constants to time and distance scales that cannot be practically evaluated in experiments.

Radionuclide transport in multi-scale fractured rocks: A review.

Significant progress has been achieved on radionuclide transport in fractured rocks due to worldwide urgent needs for geological disposal of high-level radioactive waste (HLW). Transport models designed with accurately constrained parameters are a fundamental prerequisite to assess the long-term safety of repositories constructed in deep formations. Focusing on geological disposal systems of HLW, this study comprehensively reviews the behavoir of radionuclides and transport processes in multi-scale fractured rocks. Three issues in transport modeling are emphasized: 1) determining parameters of radionuclide transport models in various scales from laboratory- to field-scale experiments, 2) upscaling physical and chemical parameters across scales, and 3) characterizing fracture structures for radionuclide transport simulations. A broad spectrum of contents is covered relevant to radionuclide transport, including laboratory and field scale experiments, analytical and numerical solutions, parameter upscaling, and conceptual model developments. This paper also discusses the latest progress of radionuclide migration in multi-scale fractured rocks and the most promising development trends in the future. It provides valuable insights into understanding radionuclide transport and long-term safety assessment for HLW geological repository.

Experimental investigations on scale-dependent dispersivity in three-dimensional heterogeneous porous media.

The relationship between the scale-dependent dispersivity and heterogeneous sedimentary structures is investigated through conducting non-reactive tracer experiments in a three-dimensional heterogeneous sand tank. The heterogeneous porous media consists of three sedimentary facies of silty, fine, and medium sands collected from the west of the Songnen Plain, China. Moreover, several corresponding individual facies soil columns were constructed for comparison. A conservative tracer was continuously injected from an upstream source. The effective parameters were estimated by inverse modeling of a one-dimensional transport model. The results show that the scale dependence of the estimated dispersivities was discovered in the individual facies column (with relatively weaker effect) and the heterogeneous porous media (with more significant effect). With increasing transport distances, the dispersivities of the individual facies tend to reach an asymptotic value, while those of the heterogeneous media increase continuously. Furthermore, the results show that a power function can describe the relationship between effective dispersivities and transport distances. The exponent of the function is greater than one for the heterogeneous media, but less than one for the individual facies. The results also indicate that the dispersion plume is macroscopically dominated by the distribution of facies. The heterogeneity of hydraulic conductivity causes the variations of flow velocity, which further enhances the scale dependence of dispersivities. The tracer experiment in heterogeneous media provides the fundamental insight into the understanding of contaminant transport processes.

Dissolution Trapping of Carbon Dioxide in Heterogeneous Aquifers.

The geologic architecture in sedimentary reservoirs affects the behavior of density-driven flow and the dispersion of CO2-rich brine. The spatial organization and connectivity of facies types play an important role. Low-permeability facies may suppress fingering and reduce vertical spreading, but may also increase transverse mixing. This is more pronounced when geologic structures create preferential flow pathways through connected facies types. We perform high-resolution simulations of three-dimensional (3D) heterogeneous formations whose connectivity cannot be represented in two-dimensional models consistent with percolation theory. This work focuses on the importance of 3D facies-based heterogeneity and connectivity on advection-diffusion transport of dissolved CO2. Because the dissolution of CO2 and the subsequent density increase of brine are the driving force for gravitational instabilities, we model the phase behavior with the accurate cubic-plus-association equation-of-state, which accounts for the self-association of polar water molecules and the cross-association between CO2 and water. Our results elucidate how the spatial organization of facies affects the dynamics of CO2 convective mixing. Scaling relations for the evolution of a global dispersion-width provide insights that can be universally applied. The results suggest that the long-term evolution and scaling of dispersion are surprisingly similar for homogeneous and (binary and multiscale) heterogeneous porous media.

Reactive transport in the complex heterogeneous alluvial aquifer of Fortymile Wash, Nevada.

Yucca Mountain, Nevada, had been extensively investigated as a potential deep geologic repository for storing high-level nuclear wastes. Previous field investigations of stratified alluvial aquifer downstream of the site revealed that there is a hierarchy of sedimentary facies types. There is a corresponding log conductivity and reactive surface area subpopulations within each facies at each scale of sedimentary architecture. Here we use a Lagrangian-based transport model in order to analyze radionuclide dispersion in the saturated alluvium of Fortymile Wash, Nevada. First, we validate the Lagrangian model using high-resolution flow and reactive transport simulations. Then, we used the validated model to investigate how each scale of sedimentary architecture may affect long-term radionuclide transport at Yucca Mountain. Results show that the reactive solute dispersion developed by the Lagrangian model matches the ensemble average of numerical simulations well. The link between the alluvium spatial variability and reactive solute dispersion at different spatiotemporal scales is demonstrated using the Lagrangian model. The longitudinal dispersivity of the reactive plume can be on the order of hundreds to thousands of meters, and it may not reach its asymptotic value even after 10,000 years of travel time and 2-3 km of travel distance.

Critical Dynamics of Gravito-Convective Mixing in Geological Carbon Sequestration.

When CO2 is injected in saline aquifers, dissolution causes a local increase in brine density that can cause Rayleigh-Taylor-type gravitational instabilities. Depending on the Rayleigh number, density-driven flow may mix dissolved CO2 throughout the aquifer at fast advective time-scales through convective mixing. Heterogeneity can impact density-driven flow to different degrees. Zones with low effective vertical permeability may suppress fingering and reduce vertical spreading, while potentially increasing transverse mixing. In more complex heterogeneity, arising from the spatial organization of sedimentary facies, finger propagation is reduced in low permeability facies, but may be enhanced through more permeable facies. The connectivity of facies is critical in determining the large-scale transport of CO2-rich brine. We perform high-resolution finite element simulations of advection-diffusion transport of CO2 with a focus on facies-based bimodal heterogeneity. Permeability fields are generated by a Markov Chain approach, which represent facies architecture by commonly observed characteristics such as volume fractions. CO2 dissolution and phase behavior are modeled with the cubic-plus-association equation-of-state. Our results show that the organization of high-permeability facies and their connectivity control the dynamics of gravitationally unstable flow. We discover new flow regimes in both homogeneous and heterogeneous media and present quantitative scaling relations for their temporal evolution.

Reactive solute transport in physically and chemically heterogeneous porous media with multimodal reactive mineral facies: the Lagrangian approach.

Physical and chemical heterogeneities have a large impact on reactive transport in porous media. Examples of heterogeneous attributes affecting reactive mass transport are the hydraulic conductivity (K), and the equilibrium sorption distribution coefficient (Kd). This paper uses the Deng et al. (2013) conceptual model for multimodal reactive mineral facies and a Lagrangian-based stochastic theory in order to analyze the reactive solute dispersion in three-dimensional anisotropic heterogeneous porous media with hierarchical organization of reactive minerals. An example based on real field data is used to illustrate the time evolution trends of reactive solute dispersion. The results show that the correlation between the hydraulic conductivity and the equilibrium sorption distribution coefficient does have a significant effect on reactive solute dispersion. The anisotropy ratio does not have a significant effect on reactive solute dispersion. Furthermore, through a sensitivity analysis we investigate the impact of changing the mean, variance, and integral scale of K and Kd on reactive solute dispersion.

The influence of streambed heterogeneity on hyporheic flow in gravelly rivers.

Deposits of open-framework gravel occurring in gravelly streambeds can exert a significant influence on hyporheic flow. The influence was quantified using a numerical model of the hyporheic zone. The model included open-framework gravel stratasets represented with commonly observed characteristics including a volume fraction of about one-third of the streambed sediment, a hydraulic conductivity two orders of magnitude greater than other strata present, and a spatial connectivity forming preferential-flow pathways. The influence of open-framework gravel stratasets on hyporheic flow was much greater than the influence of the channel morphology including meanders, point bars, dunes, and ripples. Seventy percent of the total hyporheic exchange occurred across 30% of the channel boundary at locations of open-framework gravel stratasets. The maximum local interfacial flux rates occurred at these locations, and were orders of magnitude greater than those at other locations. The local flux rates varied by six orders of magnitude over the channel boundary. The composite flow rate through the model with open-framework gravel stratsets was an order of magnitude greater than that through an equivalent but homogeneous model.