Charles E. Russell

Measuring the specific surface area of natural and manmade glasses: effects of formation process, morphology, and particle size

The specific surface area of natural and manmade solid materials is a key parameter controlling important interfacial processes in natural environments and engineered systems, including dissolution reactions and sorption processes at solid/fluid interfaces. To improve our ability to quantify the release of trace elements trapped in natural glasses, the release of hazardous compounds trapped in manmade glasses, or the release of radionuclides from nuclear melt glass, we measured the specific surface area of natural and manmade glasses as a function of particle size, morphology, and composition. Volcanic ash, volcanic tuff, tektites, obsidian glass, and in situ vitrified rock were analyzed. Specific surface area estimates were obtained using krypton as gas adsorbent and the BET model. The range of surface areas measured exceeded three orders of magnitude. A tektite sample had the highest surface area (1.65 m 2 g 1 ), while one of the samples of in situ vitrified rock had the lowest surface area (0.0016 m 2 g 1 ). The specific surface area of the samples was a function of particle size, decreasing with increasing particle size. Different types of materials, however, showed variable dependence on particle size, and could be assigned to one of three distinct groups: (1) Samples with low surface area dependence on particle size and surface areas approximately two orders of magnitude higher than the surface area of smooth spheres of equivalent size. The specific surface area of these materials was attributed mostly to internal porosity and surface roughness. (2) Samples that showed a trend of decreasing surface area dependence on particle size as the particle size increased. The minimum specific surface area of these materials was between 0.1 and 0.01 m 2 g 1 and was also attributed to internal porosity and surface roughness. (3) Samples whose surface area showed a monotonic decrease with increasing particle size, never reaching an ultimate surface area limit within the particle size range examined. The surface area results were consistent with particle morphology, examined by scanning electron microscopy, and have significant implications for the release of radionuclides and toxic metals in the environment. # 2002 Elsevier Science B.V. All rights reserved.

Comparison of drilling and mining as methods for obtaining microbiological samples from the deep subsurface

Abstract Ashfall tuff samples for microbiological analysis were obtained by mining and drilling within a 400 m deep tunnel system at Rainier Mesa, Nevada Test Site. Comparison of microbiota revealed that bacteria recovered from the core samples were similar to those recovered from the mined samples in abundance, diversity, evenness of distribution, and the numbers of distinct colony types. Cluster analyses based on the characterization of one of each distinct bacterial type from cored and mined samples indicated morphological and physiological similarities between some of the microbiota that were recovered. Drilling fluid microbiota were more abundant, and were distinct from those recovered from cored or mined samples. Storage of both the mined and cored samples for 1 week at 4°C led to the recovery of increased numbers of culturable cells, but with decreased diversity. The presence of bromide tracer indicated penetration of drilling fluids into the cored rock samples, a problem not encountered with mining. However, abundance and diversity values, and isolate characterization indicate that valuable information can be obtained from cored rock samples.

Heterogeneity of deep subsurface microorganisms and correlations to hydrogeological and geochemical parameters

Nineteen samples were obtained from a 21‐m3 section of zeolitized volcanic ash‐fall tuff, 390 m below the surface of Rainier Mesa, Nevada. Rock mined aseptically from the walls of deep subsurface tunnels provided pristine samples for microbiological and geochemical analyses. Microbiological parameters measured on all samples included direct counts and the abundance, diversity, morphology, and metabolic traits of culturable organisms. Physical and chemical parameters measured included ionic and nutrient chemistries, mineralogy, porosity, moisture content, and permeability. The results indicate that the culturable microbiological community size and composition exhibit random spatial variability within the geologically/geochemically homogeneous rock section. The relative abundance of microorganisms testing positive for nitrate reductase demonstrated a spatial trend along the vertical and front‐to‐back axes of the rock section by gradient analysis. The porewater concentration of nitrate correlated with number...

Reconnaissance Estimates of Recharge Based on an Elevation-dependent Chloride Mass-balance Approach

Significant uncertainty is associated with efforts to quantity recharge in arid regions such as southern Nevada. However, accurate estimates of groundwater recharge are necessary to understanding the long-term sustainability of groundwater resources and predictions of groundwater flow rates and directions. Currently, the most widely accepted method for estimating recharge in southern Nevada is the Maxey and Eakin method. This method has been applied to most basins within Nevada and has been independently verified as a reconnaissance-level estimate of recharge through several studies. Recharge estimates derived from the Maxey and Eakin and other recharge methodologies ultimately based upon measures or estimates of groundwater discharge (outflow methods) should be augmented by a tracer-based aquifer-response method. The objective of this study was to improve an existing aquifer-response method that was based on the chloride mass-balance approach. Improvements were designed to incorporate spatial variability within recharge areas (rather than recharge as a lumped parameter), develop a more defendable lower limit of recharge, and differentiate local recharge from recharge emanating as interbasin flux. Seventeen springs, located in the Sheep Range, Spring Mountains, and on the Nevada Test Site were sampled during the course of this study and their discharge was measured. The chloride and bromidemorexa0» concentrations of the springs were determined. Discharge and chloride concentrations from these springs were compared to estimates provided by previously published reports. A literature search yielded previously published estimates of chloride flux to the land surface. {sup 36}Cl/Cl ratios and discharge rates of the three largest springs in the Amargosa Springs discharge area were compiled from various sources. This information was utilized to determine an effective chloride concentration for recharging precipitation and its associated uncertainty via Monte Carlo simulations. Previously developed isohyetal maps were utilized to determine the mean and standard deviation of precipitation within the area. A digital elevation model was obtained to provide elevation information. A geologic model was obtained to provide the spatial distribution of alluvial formations. Both were used to define the lower limit of recharge. In addition, 40 boreholes located in alluvial sediments were drilled and sampled in an attempt to support the argument that the areal distribution of alluvial sediments can be used to define a zone of negligible recharge. The data were compiled in a geographic information system and used in a Monte Carlo analysis to determine recharge occurring within the study area. Results of the analysis yielded estimates of the mean and standard deviation of recharge occurring within the study area (28.168 x 10{sup 6} m{sup 3} yr{sup -1} and 7.008 x 10{sup 6} m{sup 3} yr{sup -1}, and 26.838 x 10{sup 6} m{sup 3} yr{sup -1} and 6.928 x 10{sup 6} m{sup 3} yr{sup -1}) for two sets of simulations using alternate definitions of the lower limit of recharge. A sensitivity analysis determined the recharge estimates were most sensitive to uncertainty associated with the chloride concentration of the spring discharge. The second most sensitive parameter was the uncertainty associated with the mean precipitation within the recharge areas. Comparison of the analysis to previously published estimates of recharge revealed mixed results with the recharge estimates derived during the course of this project generally greater relative to previously published estimates.«xa0less

Sensitivity of Solute Advective Travel Time to Porosities of Hydrogeologic Units

An integral approach is proposed to quantify uncertainty and sensitivity of advective travel time to the effective porosities of hydrogeologic units (HGUs) along groundwater flow paths. The approach is applicable in situations where a groundwater flow model exists, but a full solute transport model is not available. The approach can be used to: (1) determine HGUs whose porosities are influential to the solute advective travel time; and (2) apportion uncertainties of solute advective travel times to the uncertainty contributions from individual HGU porosities. A simple one-dimensional steady-state flow example is used to illustrate the approach. Advective travel times of solutes are obtained based on the one-dimensional steady-state flow results in conjunction with the HGU porosities. The approach can be easily applicable to more complex multi-dimensional cases where advective solute travel time can be calculated based on simulated flow results from groundwater flow models. This approach is particularly valuable for optimizing limited resources when designing field characterization programs for uncertainty reduction by identifying HGUs that contribute most to the estimation uncertainty of advective travel times of solutes.

Fractional dynamics of tracer transport in fractured media from local to regional scales

Tracer transport through fractured media exhibits concurrent direction-dependent super-diffusive spreading along high-permeability fractures and sub-diffusion caused by mass transfer between fractures and the rock matrix. The resultant complex dynamics challenge the applicability of conventional physical models based on Fick’s law. This study proposes a multi-scaling tempered fractional-derivative (TFD) model to explore fractional dynamics for tracer transport in fractured media. Applications show that the TFD model can capture anomalous transport observed in small-scale single fractures, intermediate-scale fractured aquifers, and two-dimensional large-scale discrete fracture networks. Tracer transport in fractured media from local (0.255-meter long) to regional (400-meter long) scales therefore can be quantified by a general fractional-derivative model. Fractional dynamics in fractured media can be scale dependent, owning to 1) the finite length of fractures that constrains the large displacement of tracers, and 2) the increasing mass exchange capacity along the travel path that enhances sub-diffusion.

Evaluation Of Groundwater Pathways And Travel Times From The Nevada Test Site To The Potential Yucca Mountain Repository

Yucca Mountain (YM), Nevada, has been recommended as a deep geological repository for the disposal of spent fuel and high-level radioactive waste. If YM is licensed as a repository by the Nuclear Regulatory Commission, it will be important to identify the potential for radionuclides to migrate from underground nuclear testing areas located on the Nevada Test Site (NTS) to the hydraulically downgradient repository area to ensure that monitoring does not incorrectly attribute repository failure to radionuclides originating from other sources. In this study, we use the Death Valley Regional Flow System (DVRFS) model developed by the U.S. Geological Survey to investigate potential groundwater migration pathways and associated travel times from the NTS to the proposed YM repository area. Using results from the calibrated DVRFS model and the particle tracking post-processing package MODPATH, we modeled three-dimensional groundwater advective pathways in the NTS and YM region. Our study focuses on evaluating the potential for groundwater pathways between the NTS and YM withdrawal area and whether travel times for advective flow along these pathways coincide with the prospective monitoring timeframe at the proposed repository. We include uncertainty in effective porosity, as this is a critical variable in the determination of time for radionuclides morexa0» to travel from the NTS region to the YM withdrawal area. Uncertainty in porosity is quantified through evaluation of existing site data and expert judgment and is incorporated in the model through Monte Carlo simulation. Since porosity information is limited for this region, the uncertainty is quite large and this is reflected in the results as a large range in simulated groundwater travel times. «xa0less

Sensitivity to Formation Porosity of Contaminant Transport from Nevada Test Site to Yucca Mountain

This study quantified the sensitivity of advective contaminant arrival time to the porosity of hydrogeologic units (HGUs) for groundwater transport from the Nevada Test Site (NTS) to the Yucca Mountain (YM) area in the United States. Advective arrival time of contaminants associated with underground nuclear detonations was obtained by using particle tracking on the basis of flow velocities from the Death Valley Regional Groundwater Flow System (DVRFS) model and porosity information for the HGUs along the flowpaths. The objectives were to (1)xa0determine which HGU’s porosity is influential in contaminant advective arrival time from the NTS to the YM, and (2)xa0apportion uncertainties in contaminant advective arrival time to the uncertainty contributions from individual HGU porosity. Over 90% of the uncertainty in advective transport arrival time from the NTS to YM could be described by uncertainties in porosity values of two of the 27 HGUs present in the DVRFS model. The study was significant for optimizing re...

Uncertainty and Sensitivity of Contaminant Travel Times from the Upgradient Nevada Test Site to the Yucca Mountain Area

Yucca Mountain (YM), Nevada, has been proposed by the U.S. Department of Energy as the nation’s first permanent geologic repository for spent nuclear fuel and highlevel radioactive waste. In this study, the potential for groundwater advective pathways from underground nuclear testing areas on the Nevada Test Site (NTS) to intercept the subsurface of the proposed land withdrawal area for the repository is investigated. The timeframe for advective travel and its uncertainty for possible radionuclide movement along these flow pathways is estimated as a result of effective-porosity value uncertainty for the hydrogeologic units (HGUs) along the flow paths. Furthermore, sensitivity analysis is conducted to determine the most influential HGUs on the advective radionuclide travel times from the NTS to the YM area. Groundwater pathways are obtained using the particle tracking package MODPATH and flow results from the Death Valley regional groundwater flow system (DVRFS) model developed by the U.S. Geological Survey (USGS). Effectiveporosity values for HGUs along these pathways are one of several parameters that determine possible radionuclide travel times between the NTS and proposed YM withdrawal areas. Values and uncertainties of HGU porosities are quantified through evaluation of existing site effective-porosity data and expert professional judgment and are incorporated inmorexa0» the model through Monte Carlo simulations to estimate mean travel times and uncertainties. The simulations are based on two steady-state flow scenarios, the pre-pumping (the initial stress period of the DVRFS model), and the 1998 pumping (assuming steady-state conditions resulting from pumping in the last stress period of the DVRFS model) scenarios for the purpose of long-term prediction and monitoring. The pumping scenario accounts for groundwater withdrawal activities in the Amargosa Desert and other areas downgradient of YM. Considering each detonation in a clustered region around Pahute Mesa (in the NTS operational areas 18, 19, 20, and 30) under the water table as a particle, those particles from the saturated zone detonations were tracked forward using MODPATH to identify hydraulically downgradient groundwater discharge zones and to determine the particles from which detonations will intercept the proposed YM withdrawal area. Out of the 71 detonations in the saturated zone, the flowpaths from 23 of the 71 detonations will intercept the proposed YM withdrawal area under the pre-pumping scenario. For the 1998 pumping scenario, the flowpaths from 55 of the 71 detonations will intercept the proposed YM withdrawal area. Three different effective-porosity data sets compiled in support of regional models of groundwater flow and contaminant transport developed for the NTS and the proposed YM repository are used. The results illustrate that mean minimum travel time from underground nuclear testing areas on the NTS to the proposed YM repository area can vary from just over 700 to nearly 700,000 years, depending on the locations of the underground detonations, the pumping scenarios considered, and the effective-porosity value distributions used. Groundwater pumping scenarios are found to significantly impact minimum particle travel time from the NTS to the YM area by altering flowpath geometry. Pumping also attracts many more additional groundwater flowpaths from the NTS to the YM area. The sensitivity analysis further illustrates that for both the pre-pumping and 1998 pumping scenarios, the uncertainties in effective-porosity values for five of the 27 HGUs considered account for well over 90 percent of the effective-porosity-related travel time uncertainties for the flowpaths having the shortest mean travel times to YM.«xa0less

Development of RWHet to Simulate Contaminant Transport in Fractured Porous Media

Accurate simulation of matrix diffusion in regional-scale dual-porosity and dual-permeability media is a critical issue for the DOE Underground Test Area (UGTA) program, given the prevalence of fractured geologic media on the Nevada National Security Site (NNSS). Contaminant transport through regional-scale fractured media is typically quantified by particle-tracking based Lagrangian solvers through the inclusion of dual-domain mass transfer algorithms that probabilistically determine particle transfer between fractures and unfractured matrix blocks. UGTA applications include a wide variety of fracture aperture and spacing, effective diffusion coefficients ranging four orders of magnitude, and extreme end member retardation values. This report incorporates the current dual-domain mass transfer algorithms into the well-known particle tracking code RWHet [LaBolle, 2006], and then tests and evaluates the updated code. We also develop and test a direct numerical simulation (DNS) approach to replace the classical transfer probability method in characterizing particle dynamics across the fracture/matrix interface. The final goal of this work is to implement the algorithm identified as most efficient and effective into RWHet, so that an accurate and computationally efficient software suite can be built for dual-porosity/dual-permeability applications. RWHet is a mature Lagrangian transport simulator with a substantial user-base that has undergone significant development and model validation.morexa0» In this report, we also substantially tested the capability of RWHet in simulating passive and reactive tracer transport through regional-scale, heterogeneous media. Four dual-domain mass transfer methodologies were considered in this work. We first developed the empirical transfer probability approach proposed by Liu et al. [2000], and coded it into RWHet. The particle transfer probability from one continuum to the other is proportional to the ratio of the mass entering the other continuum to the mass in the current continuum. Numerical examples show that this method is limited to certain ranges of parameters, due to an intrinsic assumption of an equilibrium concentration profile in the matrix blocks in building the transfer probability. Subsequently, this method fails in describing mass transfer for parameter combinations that violate this assumption, including small diffusion coefficients (i.e., the free-water molecular diffusion coefficient 1×10-11 meter2/second), relatively large fracture spacings (such as meter), and/or relatively large matrix retardation coefficients (i.e., ). These “outliers” in parameter range are common in UGTA applications. To address the above limitations, we then developed a Direct Numerical Simulation (DNS)-Reflective method. The novel DNS-Reflective method can directly track the particle dynamics across the fracture/matrix interface using a random walk, without any empirical assumptions. This advantage should make the DNS-Reflective method feasible for a wide range of parameters. Numerical tests of the DNS-Reflective, however, show that the method is computationally very demanding, since the time step must be very small to resolve particle transfer between fractures and matrix blocks. To improve the computational efficiency of the DNS approach, we then adopted Roubinet et al.’s method [2009], which uses first passage time distributions to simulate dual-domain mass transfer. The DNS-Roubinet method was found to be computationally more efficient than the DNS-Reflective method. It matches the analytical solution for the whole range of major parameters (including diffusion coefficient and fracture aperture values that are considered “outliers” for Liu et al.’s transfer probability method [2000]) for a single fracture system. The DNS-Roubinet method, however, has its own disadvantage: for a parallel fracture system, the truncation of the first passage time distribution creates apparent errors when the fracture spacing is small, and thus it tends to erroneously predict breakthrough curves (BTCs) for the parallel fracture system. Finally, we adopted the transient range approach proposed by Pan and Bodvarsson [2002] in RWHet. In this method, particle transfer between fractures and matrix blocks can be resolved without using very small time steps. It does not use any truncation of the first passage time distribution for particles. Hence it does not have the limitation identified above for the DNS-Reflective method and the DNS-Roubinet method. Numerical results were checked against analytical solutions, and also compared to DCPTV2.0 [Pan, 2002]. This version of RWHet (called RWHet-Pan&Bodvarsson in this report) can accurately capture contaminant transport in fractured porous media for a full range of parameters without any practical or theoretical limitations.«xa0less