Both onsite septic disposal systems and private drinking water wells are commonly utilized in rural areas of Canada. The coexistence of septic systems and drinking water wells has the potential to greatly impact the quality of water obtained in these settings. Human enteric viruses have been recognized as a potential source of groundwater borne disease, although the level of risk they pose and the processes responsible for their transport are poorly understood. As a result of thin overburden, low storage capacity, and high groundwater velocities, fractured rock aquifers are potentially at highest risk to viral contamination. However, only limited research has been conducted to explore this concern. The current study was conducted to investigate both the rate of occurrence of human viruses in fractured rock aquifers and the transport mechanisms acting in these settings. A survey was conducted to identify the prevalence of human enteric viruses in three fractured rock aquifers located across Canada. A total of 61 samples were collected from 28 wells drilled in aquifers in Ontario, Newfoundland, and British Columbia. Molecular PCR techniques were utilized to determine virus presence. Results showed that 37.7% of samples and 58.1% of wells were at some time positive for viruses. Virus presence was found to increase with housing density and viruses were found to travel distances of at least 40 meters. Poor correlation was found between the presence of viruses and traditional bacterial indicators. A field-scale viral infiltration experiment was conducted to investigate viral transport behavior. The bacteriophage ф-X174 and the fluorescent dye Lissamine FF were utilized as viral and solute tracers, respectively. Tracers were applied to an exposed rock outcrop exhibiting fractures with known connection to two nearby wells. Breakthrough was extremely rapid and the colloidal processes of decreased dispersion and slow-release kinetic sorption were identified. This study has provided concrete evidence that viral contamination poses a significant threat to fractured groundwater aquifers in rural areas where onsite septic disposal practices are utilized. The results observed in this study suggest that current set back distances and monitoring techniques may be inadequate to prevent exposure to human viruses. / Thesis (Master, Civil Engineering) -- Queen's University, 2010-11-09 23:07:31.595

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In this thesis a study of the factors affecting virus and virus-sized particle transport in discrete fractured dolomite rocks is presented. Physical and chemical characteristics of two fractured rocks were determined, including fracture aperture distribution, rock matrix porosity, mineral composition, and surface charge. Hydraulic and transport tests were conducted in the fractures with a conservative solute (bromide) and carboxylate-modified latex (CML) microspheres of three sizes (20, 200, and 500 nm in diameter). The earlier arrival of larger microspheres as compared to bromide indicated the effects of pore-size exclusion and preferential flow paths in the fractures. The tailing of the bromide and the smaller microsphere (20 nm) in the breakthrough curves (BTC) indicated the diffusive mass transfer between the mobile water (flowing) and immobile water (stagnant water in the low aperture areas and porous rock matrix). The effects of ionic strength and cation type on the transport of viruses (bacteriophages MS2 and PR772) and virus-sized microspheres (20 and 200 nm) were determined from the transport tests in a fracture at three levels of ionic strength (3, 5, and 12 mM) and composition (containing Na+ and/or Ca2+ ions). Retention of the microspheres and bacteriophages increased with increasing ionic strength. The addition of divalent ions (Ca2+) influenced the retention to a greater extent than monovalent ions (Na+). The effects of the aperture distribution variability, matrix diffusion, and specific discharge on the solute and microsphere transport were determined from the transport tests conducted in two fractures. The higher variability in the aperture distribution contributed to higher solute dispersion, and flow channeling as evident from the breakthrough curves for individual spatially distributed outlets. A three-dimensional model simulation of the bromide transport with varying matrix porosity identified that the porous matrix influenced the solute transport. In the transport tests, retention of the microspheres decreased with increasing specific discharge in both fractures. The results of this research have helped in identifying the important factors and their effects on solute, virus, and virus-sized colloid transport in fractured dolomite rocks, which can be useful in determining the risk of pathogen contamination of water supplies in fractured dolomite rock aquifers.

In this thesis a study of the factors affecting virus and virus-sized particle transport in discrete fractured dolomite rocks is presented. Physical and chemical characteristics of two fractured rocks were determined, including fracture aperture distribution, rock matrix porosity, mineral composition, and surface charge. Hydraulic and transport tests were conducted in the fractures with a conservative solute (bromide) and carboxylate-modified latex (CML) microspheres of three sizes (20, 200, and 500 nm in diameter). The earlier arrival of larger microspheres as compared to bromide indicated the effects of pore-size exclusion and preferential flow paths in the fractures. The tailing of the bromide and the smaller microsphere (20 nm) in the breakthrough curves (BTC) indicated the diffusive mass transfer between the mobile water (flowing) and immobile water (stagnant water in the low aperture areas and porous rock matrix). The effects of ionic strength and cation type on the transport of viruses (bacteriophages MS2 and PR772) and virus-sized microspheres (20 and 200 nm) were determined from the transport tests in a fracture at three levels of ionic strength (3, 5, and 12 mM) and composition (containing Na+ and/or Ca2+ ions). Retention of the microspheres and bacteriophages increased with increasing ionic strength. The addition of divalent ions (Ca2+) influenced the retention to a greater extent than monovalent ions (Na+). The effects of the aperture distribution variability, matrix diffusion, and specific discharge on the solute and microsphere transport were determined from the transport tests conducted in two fractures. The higher variability in the aperture distribution contributed to higher solute dispersion, and flow channeling as evident from the breakthrough curves for individual spatially distributed outlets. A three-dimensional model simulation of the bromide transport with varying matrix porosity identified that the porous matrix influenced the solute transport. In the transport tests, retention of the microspheres decreased with increasing specific discharge in both fractures. The results of this research have helped in identifying the important factors and their effects on solute, virus, and virus-sized colloid transport in fractured dolomite rocks, which can be useful in determining the risk of pathogen contamination of water supplies in fractured dolomite rock aquifers.

[pt] A avaliação do potencial de contaminação de capatações de água, por causa das águas residuais provenientes dos sistemas de tanque séptico, é feita a partir da definição da distância de separação mínima que deve existir entre a captação e o local de infiltração do efluente. A determinação dessa distância define a zona de proteção da captação. Existem três metodologias para definir o tamanho dessa zona de proteção: metodologias baseadas em distâncias fixas e tempos de trânsito, metodologias baseadas na vulnerabilidade e metodologias baseadas no risco de infecção. No caso da Costa Rica, as avaliações são feitas através do uso da metodologia baseada no tempo de trânsito. O tempo de trânsito empregado corresponde ao tempo de sobrevivência dos vírus. Nesta análise determina-se a distância máxima percorrida pelos vírus durante esse tempo, e essa distância define a separação mínima. Esse método considera que o transporte ocorre por percolação vertical saturada através da zona não saturada, e por transporte ao longo da interface água-ar na zona saturada segundo o gradiente natural. Neste trabalho apresenta-se um novo procedimento, baseado no risco de infecção, para a determinação da distância de separação considerando os efeitos da saturação variável e o fraturamento. Este procedimento determina a distância máxima percorrida, a partir do cálculo das concentrações de vírus. A distância de separação mínima corresponde à distância entre a fonte de injeção e o ponto aonde a concentração atinge o valor máximo de concentração permitida. Para o desenvolvimento deste novo procedimento foi implementado um código de programação que inclui: fluxo saturado-não saturado e transporte explícito nos poros e nas fraturas, advecção, dispersão, decaimento, sorção na superfície dos sólidos, sorção nas interfaces água-ar e água-sólido, filtração mecânica e exclusão de poros. Foi realizada uma análise comparativa entre as metodologias acima descritas para três geometrias tipo representativas das condições estratigráficas de algumas áreas do Vale Central da Costa Rica. Os resultados obtidos indicaram que a metodologia normalmente empregada na Costa Rica pode ser inadequada para prever na maioria dos casos a possibilidade de contaminação. / [en] Setback distances of wellhead and catchments from septic tanks are establised by three aproaches: methods based on fixed setback distances or fixed travel times; methods based on vulnerability analysis and methods based on infection risk. In Costa Rica, the determination of setback distances is based on fixed travel times. This approach considers that during and specified travel time all microorganisms will be inactivated, and that the distance traveled during this time defines the minimum safe separation. In this approach a unitary hydraulic gradient and saturated hydraulic conductivity are considered for transport in the unsaturated zone and the natural hydraulic gradient and saturated conductivity for transport in the saturated zone. Only advection is considered as the responsible mechanism for virus transport. A new procedure is presented in this document to define the setback distance. This procedure is based on the infection risk approach. According to this approach the minimum required setback distance is defined as the distance between the injection point and the location where the contaminant reaches a maximum allowable concentration. This procedure was implemented in a computer code that considers variable saturated water flow, fractured-porous media, advection, dispersion, dynamic sorption, inactivation and mechanical filtration. A comparative analysis was performed for three hypothetical geometries using the two approaches described. The results indicate the approach normally used in Costa Rica may no reproduce adequately the possibility of catchments and wellhead contamination.

Accurate prediction of colloid deposition rates in porous media is essential in several applications. These include natural filtration of pathogenic microorganisms such as bacteria, viruses, and protozoa, transport and fate of colloid-associated transport of contaminants, deep bed and river bank filtration for water treatment, fate and transport of engineered nanoparticles released into the environment, and bioremediation of contaminated sites. Colloid transport in porous media is a multi-scale problem, with length scales spanning from the sub-pore scale, where the particle-soil interaction forces control the deposition, up to the Darcy scale, where the macroscopic equations governing particle transport are formulated. Colloid retention at the Darcy scale is due to the lumped effect of processes occurring at the pore scale. This requires the incorporation of the micro-scale physics into macroscopic models for a better understanding of colloid deposition in porous media. That can be achieved through pore-scale modeling and the subsequent upscaling to the Darcy scale. Colloid Filtration Theory (CFT), the most commonly used approach to describe colloid attachment onto the soil grains in the subsurface, is found to accurately predict the deposition rates of micron-sized particles under favorable conditions for deposition. But, CFT has been found to over predict particle deposition rates at low flow velocity conditions, typical of groundwater flow, and for nanoscale particles. Also, CFT is found to be inapplicable at typical environmental conditions, where conditions become unfavorable for deposition, due to factors not considered in CFT such as deposition in the secondary minimum of the interaction energy profile, grain surface roughness, surface charge heterogeneity of grains and colloids, and deposition at grain-to-grain contacts. To the best of our knowledge, mechanistic-based models for predicting colloid deposition rates under unfavorable conditions do not exist. Currently, fitting the colloid breakthrough curve (BTC), obtained from the laboratory column-or field-scale experiments, to the advection-dispersion-deposition model is used to estimate the values of deposition rate coefficients. Because of their small size (less than 100 nm), nanoparticles, a sub-class of colloids, may interact with the porous medium in a different way as compared to the larger colloids, resulting in different retention mechanisms for nanoparticles and micron-sized particles. This emphasizes the need to study nanoparticles separately from larger, micrometer-sized colloids to better understand nanoparticle retention mechanisms. The work reported in this thesis contributes towards developing mathematical models to predict nanoparticle movement in porous media. A comprehensive mechanistic approach is employed by integrating pore-scale processes into Darcy-scale models through pore-network modeling to upscale nanoparticle transport in saturated porous media to the Darcy scale, and to develop correlation equations for the Darcy-scale deposition parameters in terms of various measurable parameters at Darcy scale. Further, a one-dimensional mathematical model to simulate the co-transport of viruses and colloids in partially saturated porous media is developed to understand the relative importance of various interactions on virus transport in porous media. Pore-network modeling offers a valuable upscaling tool to express the macroscopic behavior by accounting for the relevant physics at the underlying pore scale. This is done by idealizing the pore space as an interconnected network of pore elements of different sizes and variably connected to each other, and simulating flow and transport through the network of pores, with the relevant physics implemented on a pore to pore basis (Raoof, 2011). By comparing the results of pore-network modeling with an appropriate mathematical model describing the macro-scale behavior, a relationship between the properties at the macro scale and those at the pore scale can be obtained. A three dimensional multi-directional pore-network model, PoreFlow, developed by Raoof et al. (2010, 2013) is employed in this thesis, which represents the porous medium as an interconnected network of cylindrical pore throats and spherical pore bodies, to upscale nanoparticle transport from pore scale to the Darcy scale. The first step in this procedure is to obtain relationships between adsorbed mass and aqueous mass for a single pore. A mathematical model is developed to simulate nanoparticle transport in a saturated cylindrical pore by solving the full transport equation, considering various processes such as advection, diffusion, hydrodynamic wall effects, and nanoparticle-collector surface interactions. The pore space is divided into three different regions: bulk, diffusion and potential regions, based on the dominant processes acting in each of these regions. In both bulk and diffusion regions, nanoparticle transport is governed by advection and diffusion. However, in the diffusion region, the diffusion is significantly reduced due to hydrodynamic wall effects. Nanoparticle-collector interaction forces dominate the transport in the potential region where deposition occurs. A sensitivity analysis of the model indicates that nanoparticle transport and deposition in a pore is significantly affected by various pore-scale parameters such as the nanoparticle and collector surface potentials, ionic strength of the solution, flow velocity, pore radius, and nanoparticle radius. The model is found to be more sensitive to all parameters under favorable conditions. It is found that the secondary minimum plays an important role in the deposition of small as well as large nanoparticles, and its contribution is found to increase as the favorability of the surface for adsorption decreases. Correlation equations for average deposition rate coefficients of nanoparticles in a saturated cylindrical pore under unfavorable conditions are developed as a function of nine pore-scale parameters: the pore radius, nanoparticle radius, mean flow velocity, solution ionic strength, viscosity, temperature, solution dielectric constant, and nanoparticle and collector surface potentials. Advection-diffusion equations for nanoparticle transport are prescribed for the bulk and diffusion regions, while the interaction between the diffusion and potential regions is included as a boundary condition. This interaction is modeled as a first-order reversible kinetic adsorption. The expressions for the mass transfer rate coefficients between the diffusion and the potential regions are derived in terms of the interaction energy profile between the nanoparticle and the collector. The resulting equations are solved numerically for a range of values of pore-scale parameters. The nanoparticle concentration profile obtained for the cylindrical pore is averaged over a moving averaging volume within the pore in order to get the 1-D concentration field. The latter is fitted to the 1-D advection-dispersion equation with an equilibrium or kinetic adsorption model to determine the values of the average deposition rate coefficients. Pore-scale simulations are performed for three values of Péclet number, Pe = 0.05, 5 and 50. It is found that under unfavorable conditions, the nanoparticle deposition at pore scale is best described by an equilibrium model at low Péclet numbers (Pe = 0.05), and by a kinetic model at high Péclet numbers (Pe = 50). But, at an intermediate Pe (e.g., near Pe = 5), both equilibrium and kinetic models fit the 1-D concentration field. Correlation equations for the pore-averaged nanoparticle deposition rate coefficients under unfavorable conditions are derived by performing a multiple-linear regression analysis between the estimated deposition rate coefficients for a single pore and various pore-scale parameters. The correlation equations, which follow a power law relationship with nine pore-scale parameters, are found to be consistent with the column-scale and pore-scale experimental results, and qualitatively agree with CFT. Nanoparticle transport is upscaled from pore to the Darcy scale in saturated porous media by incorporating the correlations equations for the pore-averaged deposition rate coefficients of nanoparticles in a cylindrical pore into a multi-directional pore-network model, PoreFlow (Raoof et al., 2013). Pore-network model simulations are performed for a range of parameter values, and nanoparticle BTCs are obtained from the pore-network model. Those curves are then modeled using 1-D advection-dispersion equation with a two-site first-order reversible deposition, with terms accounting for both equilibrium and kinetic sorption. Kinetic sorption is found to become important as the favorability of the surface for deposition decreases. Correlation equations for the Darcy¬scale deposition rate coefficients under unfavorable conditions are developed as a function of various measurable Darcy-scale parameters, including: porosity, mean pore throat radius, mean pore water velocity, nanoparticle radius, ionic strength, dielectric constant, viscosity, temperature, and surface potentials on the nanoparticle and grain surface. The correlation equations are found to be consistent with the observed trends from the column experiments available in the literature, and are in agreement with CFT for all parameters, except for the mean pore water velocity and nanoparticle radius. The Darcy-scale correlation equations contain multipliers whose values for a given set of experimental conditions need to be determined by comparing the values of the deposition rate coefficients predicted by the correlation equations against the estimated values of Darcy-scale deposition parameters obtained by fitting the BTCs from column or field experiments with 1-D advection-dispersion-deposition model. They account for the effect of factors not considered in this study, such as the physical and chemical heterogeneity of the grain surface and nanoparticles, flow stagnation points, grain-to-grain contacts, etc. Colloids are abundant in the subsurface and have been observed to interact with a variety of contaminants, including viruses, thereby significantly influencing their transport. A mathematical model is developed to simulate the co-transport of viruses and colloids in partially saturated porous media under steady state flow conditions. The virus attachment to the mobile and immobile colloids is described using a linear reversible kinetic model. It is assumed that colloid transport is not affected by the presence of attached viruses on its surface, and hence, colloid transport is decoupled from virus transport. The governing equations are solved numerically using an alternating three-step operator splitting approach. The model is verified by fitting three sets of experimental data published in the literature: (1) Syngouna and Chrysikopoulos (2013) and (2) Walshe et al. (2010), both on the co-transport of viruses and clay colloids under saturated conditions, and (3) Syngouna and Chrysikopoulos (2015) for the co-transport of viruses and clay colloids under unsaturated conditions. The model results are found to be in good agreement with the observed BTCs under both saturated and unsaturated conditions. Then, the developed model was used to simulate the co-transport of viruses and colloids in porous media under unsaturated conditions, with the aim of understanding the relative importance of various processes on the co-transport of viruses and colloids. The virus retention in porous media in the presence of colloids is greater under unsaturated conditions as compared to the saturated conditions due to: (1) virus attachment to the air-water interface (AWI), and (2) co-deposition of colloids with attached viruses on its surface to the AWI. A sensitivity analysis of the model to various parameters showed that virus attachment to AWI is the most sensitive parameter affecting the BTCs of both free viruses and total mobile viruses, and has a significant effect on all parts of the BTC. The free and the total mobile virus BTCs are mainly influenced by parameters describing virus attachment to the AWI, virus interactions with mobile and immobile colloids, virus attachment to solid-water interface (SWI), and colloid interactions with SWI and AWI. The virus BTC is relatively insensitive to parameters describing the maximum adsorption capacity of the AWI for colloids, inlet colloid concentration, virus detachment rate coefficient from the SWI, maximum adsorption capacity of the AWI for viruses, and inlet virus concentration.