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This dissertation combines field data, laboratory experiments, and mathematic models to (1) predict the probability of groundwater arsenic (As) contamination caused by geogenic sources and processes in shallow aquifers of the Mississippi Delta in southern Louisiana, (2) study the role microbes play in controlling As mobilization from sediments to groundwaters, and (3) simulate As mobilization and transport caused by changing redox conditions and groundwater geochemistry along a flow path within the southeastern Chicot aquifer in southern Louisiana. A model based on surface hydrology, soil properties, geology, and sedimentary deposition environments predicts that the Holocene shallow aquifers in southern Louisiana are at high risk of As contamination. Sediment incubation and pore-water chemistry suggest that microbes play a key role in mobilizing As from sediments by reductive dissolution of As-bearing Fe(III) oxides/oxyhydroxides. Finally, groundwater samples were collected along a 10 km flow path in the southeastern Chicot aquifer to determine groundwater geochemical parameters and to simulate reactive transport of Fe and As species along the studied flow path. The model well captures the general trends of Fe(II) and As(III) concentrations along the studied flow path and the close correspondence between Fe(II) and As(III) of the both measured and model predicted As(III) and Fe(II) concentrations support the hypothesis that microbially mediated reductive dissolution of As-bearing Fe(III) oxides/oxyhydroxides is the primary mechanism causing As mobilization from sediments to the shallow reducing groundwaters of the Mississippi Delta in southern Louisiana. / 1 / NINGFANG YANG

This thesis investigated the dissolution of dense non aqueous phase liquids (DNAPL) source zones in the subsurface and the effectiveness of enhanced bioremediation for the treatment of chlorinated ethene DNAPLs, using numerical modeling. For this purpose, an existing multiphase numerical model was extended to include comprehensive models for the processes of dissolution and reaction. The first part of the thesis examined DNAPL dissolution. First, a thermodynamic-based dissolution model was validated using experimental data from two complex heterogeneous DNAPL releases. Model predictions for DNAPL spatial distribution and effluent concentrations agreed well with experimental measurements, without requiring calibration. This is the first successful application of a predictive dissolution model in the literature. Model results showed the important effects of relative permeability and interfacial areas on dissolution rates. Then, the thermodynamic dissolution model was compared to simpler models typically used in the literature. Five Sherwood-Gilland (SG) empirical correlations were evaluated and their limitations were illustrated. A new dissolution model was proposed that combined the predictive ability of the thermodynamic model and the simplicity of SG models, and is applicable for complex source zones. Lastly, the relationship between the DNAPL source architecture and downstream concentrations was investigated, focusing on multistage concentration profiles. A new upscaled model was proposed that is able to capture such complex behavior. In the second part of this thesis the thermodynamic dissolution model was combined with a model for reductive dechlorination of chlorinated ethenes to simulate DNAPL bioremediation. Simulations were conducted for simple DNAPL source zones to investigate the impact of dissolution-related processes on bioremediation effectiveness. Dissolution kinetics and back-partitioning of daughter products in the DNAPL were shown to affect dechlorination. Then, the investigation was extended to DNAPL source zones of complex architectures in heterogeneous domains, illustrating the importance of the source zone architecture for the effectiveness of DNAPL bioremediation. Overall, this thesis presents a comprehensive numerical model that will be an important research tool for evaluating the effectiveness of in-situ bioremediation for DNAPL source zones, and will provide the means for a better understanding and control of the critical factors affecting this technology in the field.

This thesis investigated the dissolution of dense non aqueous phase liquids (DNAPL) source zones in the subsurface and the effectiveness of enhanced bioremediation for the treatment of chlorinated ethene DNAPLs, using numerical modeling. For this purpose, an existing multiphase numerical model was extended to include comprehensive models for the processes of dissolution and reaction. The first part of the thesis examined DNAPL dissolution. First, a thermodynamic-based dissolution model was validated using experimental data from two complex heterogeneous DNAPL releases. Model predictions for DNAPL spatial distribution and effluent concentrations agreed well with experimental measurements, without requiring calibration. This is the first successful application of a predictive dissolution model in the literature. Model results showed the important effects of relative permeability and interfacial areas on dissolution rates. Then, the thermodynamic dissolution model was compared to simpler models typically used in the literature. Five Sherwood-Gilland (SG) empirical correlations were evaluated and their limitations were illustrated. A new dissolution model was proposed that combined the predictive ability of the thermodynamic model and the simplicity of SG models, and is applicable for complex source zones. Lastly, the relationship between the DNAPL source architecture and downstream concentrations was investigated, focusing on multistage concentration profiles. A new upscaled model was proposed that is able to capture such complex behavior. In the second part of this thesis the thermodynamic dissolution model was combined with a model for reductive dechlorination of chlorinated ethenes to simulate DNAPL bioremediation. Simulations were conducted for simple DNAPL source zones to investigate the impact of dissolution-related processes on bioremediation effectiveness. Dissolution kinetics and back-partitioning of daughter products in the DNAPL were shown to affect dechlorination. Then, the investigation was extended to DNAPL source zones of complex architectures in heterogeneous domains, illustrating the importance of the source zone architecture for the effectiveness of DNAPL bioremediation. Overall, this thesis presents a comprehensive numerical model that will be an important research tool for evaluating the effectiveness of in-situ bioremediation for DNAPL source zones, and will provide the means for a better understanding and control of the critical factors affecting this technology in the field.

The overarching objective of this dissertation was to study groundwater resources on global, local, and regional scales. The first objective of this dissertation was to analyze the groundwater nitrate contamination in the Edwards-Trinity and the Southern High-Plains aquifers of Texas. The second was to study groundwater quality in terms of seawater intrusion in the California Coastal Basin, Upper Floridian, and North Atlantic Coastal Plain aquifers. This dissertation also provided a comprehensive overview of the groundwater level in basins at the global scale and further analyzed agricultural activities on groundwater storage in small and large basins. To achieve first objective, Ordinary Least Square (OLS) and Geographically Weighted Regression (GWR) models were used to study the relationship between groundwater nitrate contamination and land use. This dissertation further identified dominant groundwater types using USGS well data and to estimate the extent of seawater intrusion in terms of dominant ions and ocean salinity in the United States coastal aquifers. Finally, groundwater storage anomaly was quantified using Gravity Recovery and Climate Experiment (GRACE) derived variations in total Terrestrial Water Storage (TWS) and the Global Land Data Assimilation System (GLDAS). Land cover data representing a percentage of irrigated lands using groundwater resources was used to study agricultural activities on groundwater storage. Groundwater nitrate contamination was positively associated with cotton production in Southern High-Plains and Edwards-Trinity aquifers. The nitrate concentrations tended to increase as the well-depth decreased in both aquifers. Results showed that the dominant ions in the study area were Na+ and Cl- . The study concluded that Na-Cl and mixed Ca-Mg-Cl were dominant water types in the United States' coastal aquifers. Results also indicated that seawater intrusion is occurring in the US coastal aquifers. Groundwater depletion has increased in southern Asia, western North America, and southwestern Europe due to groundwater withdrawal for agricultural use. However, farming practice is not the main reason for groundwater scarcity in South America, Africa, and Australia.

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Thesis advisor: Rudolph Hon / The application of road de-icers has lead to increasing solute concentrations in surface and ground water across the northern US, Canada, and northern Europe. In a public water supply well field in southeastern Massachusetts, USA, chloride concentrations in ground water from an unconfined aquifer have steadily risen for the past twenty years. The objectives of this study are to understand spatial and temporal trends in road salt concentrations in order to identify contamination sources and fate. To this end, the methods of this project include field and lab work. Water samples were collected from surface, near-surface, and ground water from March 2012 to March 2013. The other major field data are specific conductance measurements from probes located in three piezometers. In the lab, all samples were analyzed for major ions with ion chromatography analysis. Additionally, trace elements were measured by inductively coupled plasma analysis on a subset of samples. The results of these hydrogeochemical procedures showed several important trends. First, the highest concentrations of sodium and chloride from near-surface samples were located near to roadways. Second, ground water samples taken from glacial sediments contained relatively high concentrations throughout the water column, whereas ground water samples from wetlands had high concentrations only near the surface. Third, there was no clear relationship between pH and cation concentrations. Finally, specific conductance data showed strong seasonal trends near to the surface, whereas values taken from deeper in the aquifer were steadily increasing. Based on these results, it is highly probable that road salt application is the dominate contamination source. The pathways of road salt in the watershed include runoff into surface water and infiltration into the vadose zone and ground water. Road salt appears to preferentially travel through glacial features rather than floodplain features. It is possible that sodium from road salt is sorbed to aquifer sediment and displaces other cations. However, the low values of trace metals suggest that cation exchange is not mobilizing heavy metals. Finally, the increasing specific conductance values deep in the aquifer suggest that road salt is retained within the aquifer and concentrations will likely increase in the future if the current road salt application procedures are continued. / Thesis (MS) — Boston College, 2013. / Submitted to: Boston College. Graduate School of Arts and Sciences. / Discipline: Earth and Environmental Sciences.

M. Tech. / Gold (Au) mining in South Africa resulted in vast volumes of hazardous waste being generated. Poor management of most of the tailings dams has resulted in the release of acid mine drainage, which caused stream water and soil contamination with their run-offs. The consequence of mine closure has not only been observed in large-scale land degradation, but also in widespread pollution of surface water and groundwater in the Wonderfonteinspruit Catchment Area (WCA). Thus, clean-up methods must be developed in order to remove heavy metals from contaminated water bodies in this area. The efficacy of algae, zeolite and zeolite functionalized with humic acid in reducing the concentration of the heavy metals iron (Fe3+), zinc (Zn2+), manganese (Mn2+) and nickel (Ni2+) to acceptable levels in WCA was investigated in this study. It is also envisaged that the heavy metals to be removed from contaminated water can be useful in various industries. A sampling exercise was undertaken with the aim of identifying the heavy metals that contaminate the water in the catchment, as well as identify the priority heavy metals for laboratory sorption tests. Batch experiments were conducted to study the adsorption behavior of natural zeolite clinoptilolite and algae Desmodesmus sp. with respect to Fe3+, Mn2+, Ni2+, and Zn2+. The data was analysed using the Langmuir and Freundlich isotherms. Two kinetic models namely, pseudo-first order and pseudo second order were also tested to fit the data. It was found that the concentration of Fe3+, Mn2+, Ni2+ and Zn2+ was 115 mg/L, 121 mg/L, 26.5 mg/L and 6.9 mg/L from the sampled water bodies in the WCA, respectively. The Langmuir isotherm was found to correlate the adsorption of Fe3+, Mn2+, Ni2+, and Zn2+ better, with the adsorption capacity of 11.9 mg/g, 1.2 mg/g, 1.3 mg/g, and 14.7 mg/g, for the functionalized zeolite (FZ), respectively. The algae system gave adsorption capacities of 1.523 mg/g, 144 mg/g and 71.94 mg/g for Fe3+, Mn2+ and Ni2+; respectively. Pseudo second-order equation was found to be the best fit for the adsorption of heavy metals by unfunctionalized zeolite (UFZ) and the algae system. Zeolite functionalization with humic acid increased its uptake ability. The best results for kinetic study was obtained in concentration 120 ppm for Fe3+ and Mn2+, whilst for Ni2+ was at 20 mg/L , which is about the same concentrations found in contaminated water in the WCA (Fe3+ 115 mg/L, Mn2+121 mg/L and Ni2+ 26.5 mg/L).

An alternative on-site wastewater treatment and disposal system (OSWTDS) consisting of a soil infiltrator with low pressure distribution was evaluated in a soil that was unsuitable for a conventional OSWTDS under current Commonwealth of Virginia Sewage Handling and Disposal Regulations, due to a shallow seasonally perched water table and low hydraulic conductivity. The absorption field consisted of two subsystems numbered as 1 and 2 with effluent design loading rates of 5.1 and 10.2 Lpd/m2, respectively (actual loading rates of 2.4 and 4.9 Lpd/m2, respectively). Soil matric potentials compared seasonally for each subsystem and indicated that both provided similar hydraulic performance. Background water quality was generally improved by subsurface movement through the absorption fields. A bacterial tracer was found in shallow (45.7 cm) and deep (213.4 cm) sampling wells within 24 h in the two subsystems (but in low numbers) over both summer and winter sampling periods. A viral tracer was detected within 48 h in both shallow and deep wells, but only in subsystem 2 in the winter. In evaluating denitrification potential, the addition of glucose to soil core samples did increase quantitatively, although not significantly, nitrous oxide production in each subsystem, at each depth, during each season. Overall, the performance of both subsystems was very similar. The soil infiltrator functioned very well, as designed for the site and soil limitations. It appears to be a potential alternative OSWTDS for use in problem soils. / Master of Science