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- Genre: Doctoral Dissertation
Description
Petroleum contamination is ubiquitous during extraction, transportation, refining, and storage. Contamination damages the soil’s ecosystem function, reduces its aesthetics, and poses a potential threat to human beings. The overall goals of this dissertation are to advance understanding of the mechanisms behind ozonation of petroleum-contaminated soil and to configure an effective integrated bioremediation + ozonation remedial strategy to remove the overall organic carbon. Using a soil column, I conducted batch ozonation experiments for different soils and at different moisture levels. I measured multiple parameters: e.g., total petroleum hydrocarbons (TPH) and dissolved organic carbon (DOC), to build a full understanding of the data that led to the solid conclusions. I first demonstrated the feasibility of using ozone to attack heavy petroleum hydrocarbons in soil settings. I identified the physical and chemical hurdles (e.g., moisture, mass transfer, pH) needed to be overcome to make the integration of chemical oxidation and biodegradation more efficient and defines the mechanisms behind the experimental observations. Next, I completed a total carbon balance, which revealed that multiple components, including soil organic matter (SOM) and non-TPH petroleum, competed for ozone, although TPH was relatively more reactive. Further experiments showed that poor soil mixing and high soil-moisture content hindered mass transfer of ozone to react with the TPH. Finally, I pursued the theme of optimizing the integration of ozonation and biodegradation through a multi-stage strategy. I conducted multi-stages of ozonation and bioremediation for two benchmark soils with distinctly different oils to test if and how much ozonation enhanced biodegradation and vice versa. With pH and moisture optimized for each step, pre-ozonation versus post-ozonation was assessed for TPH removal and mineralization. Multi-cycle treatment was able to achieve the TPH regulatory standard when biodegradation alone could not. Ozonation did not directly enhance the biodegradation rate of TPH; instead, ozone converted TPH into DOC that was biodegraded and mineralized. The major take-home lesson from my studies is that multi-stage ozonation + biodegradation is a useful remediation tool for petroleum contamination in soil.
ContributorsChen, Tengfei (Author) / Rittmann, Bruce E. (Thesis advisor) / Westerhoff, Paul (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Delgado, Anca G (Committee member) / Arizona State University (Publisher)
Created2018
Description
Laterally-loaded short rigid drilled shaft foundations are the primary foundation used within the electric power transmission line industry. Performance of these laterally loaded foundations is dependent on modulus of the subsurface, which is directly measured by the Pressuremeter (PMT). The PMT test provides the lateral shear modulus at intermediate strains, an equivalent elastic modulus for lateral loading, which mimics the reaction of transmission line foundations within the elastic range of motion. The PMT test, however, is expensive to conduct and rarely performed. Correlations of PMT to blow counts and other index properties have been developed but these correlations have high variability and may result in unconservative foundation design. Variability in correlations is due, in part, because difference of the direction of the applied load and strain level between the correlated properties and the PMT. The geophysical shear wave velocity (S-wave velocity) as measured through refraction microtremor (ReMi) methods can be used as a measure of the small strain, shear modulus in the lateral direction. In theory, the intermediate strain modulus of the PMT is proportional to the small strain modulus of S-wave velocity. A correlation between intermediate strain and low strain moduli is developed here, based on geophysical surveys conducted at fourteen previous PMT testing locations throughout the Sonoran Desert of central Arizona. Additionally, seasonal variability in S-wave velocity of unsaturated soils is explored and impacts are identified for the use of the PMT correlation in transmission line foundation design.
ContributorsEvans, Ashley Elizabeth (Author) / Houston, Sandra (Thesis advisor) / Zapata, Claudia (Thesis advisor) / van Paassen, Leon (Committee member) / Arizona State University (Publisher)
Created2018
Description
Enzyme-induced carbonate precipitation (EICP) is a biogeotechnical soil improvement method that involves the precipitation of calcium carbonate via hydrolysis of urea (ureolysis) catalyzed by free urease enzyme in a calcium chloride solution. When this reaction takes place in the pore space of a sand, the precipitated calcium carbonate may bind soil grains together, thereby improving strength. Three studies on EICP are presented in this dissertation. In the first study, chemical equilibrium modeling via PHREEQC is used to develop a method for evaluating urease activity from electrical conductivity (EC) measurements in a closed reactor containing urea and urease. It is shown that a commonly used correlation to estimate urease activity from EC measurements overestimates the initial urea hydrolysis rate (thereby overpredicting the urease activity as well). In the second study, the crystal structure and mechanical properties of calcium carbonate minerals formed by EICP are studied. It is shown that a “modified” precipitate synthesized by the inclusion of nonfat dry milk in the EICP solution is more ductile than a “baseline” precipitate synthesized from an EICP solution without nonfat milk. Additionally, in sands biocemented using the modified EICP solution, precipitation occurs preferentially at the grain contacts. This may contribute to relatively high unconfined compressive strengths at low carbonate contents in some EICP-treated sands. The third study discusses the role of some sand characteristics on the strength following modified EICP treatment. Three batches of Ottawa 20-30 sand from different sources were treated identically using the modified EICP solution. Subsequent testing showed large differences in their unconfined compressive strengths. It is shown that this variation in unconfined compressive strength is due to differences in the surface microtexture and surface mineralogy of the sands.The fundamental studies presented in this dissertation provide a deeper understanding of some aspects of the EICP process.
ContributorsLakshminarayanan, Vinaykrishnan (Author) / Kavazanjian, Jr., Edward (Thesis advisor) / van Paassen, Leon (Committee member) / Khodadadi Tirkolaei, Hamed (Committee member) / Arizona State University (Publisher)
Created2022
Description
Trichloroethene (TCE) and hexavalent chromium (Cr (VI)) are ubiquitous subsurface contaminants affecting the water quality and threatening human health. Microorganisms capable of TCE and Cr (VI) reductions can be explored for bioremediation at contaminated sites. The goal of my dissertation research was to address challenges that decrease the efficiency of bioremediation in the subsurface. Specifically, I investigated strategies to (i) promote improve microbial reductive dechlorination extent through the addition of Fe0 and (ii) Cr (VI) bio-reduction through enrichment of specialized microbial consortia. Fe0 can enhance microbial TCE reduction by inducing anoxic conditions and generating H2 (electron donor). I first evaluated the effect of Fe0 on microbial reduction of TCE (with ClO4– as co-contaminant) using semi-batch soil microcosms. Results showed that high concentration of Fe0 expected during in situ remediation inhibited microbial TCE and ClO4– reduction when added together with Dehalococcoides mccartyi-containing cultures. A low concentration of aged Fe0 enhanced microbial TCE dechlorination to ethene and supported complete microbial ClO4– reduction. I then evaluated a decoupled Fe0 and biostimulation/bioaugmentation treatment approach using soil packed columns with continuous flow of groundwater. I demonstrated that microbial TCE reductive dechlorination to ethene can be benefitted by Fe0 abiotic reactions, when biostimulation and bioaugmentation are performed downstream of Fe0 addition. Furthermore, I showed that ethene production can be sustained in the presence of aerobic groundwater (after Fe0 exhaustion) by the addition of organic substrates. I hypothesized that some lessons learned from TCE Bioremediation can be applied also for other pollutants that can benefit from anaerobic reductions, like Cr (VI). Bioremediation of Cr (VI) has historically relied on biostimulation of native microbial communities, partially due to the lack of knowledge of the benefits of adding enriched consortia of specialized microorganisms (bioaugmentation). To determine the merits of a specialized consortium on bio-reduction of Cr (VI), I first enriched a culture on lactate and Cr (VI). The culture had high abundance of putative Morganella species and showed rapid and sustained Cr (VI) bio-reduction compared to a subculture grown with lactate only (without Morganella). Overall, this dissertation work documents possible strategies for synergistic abiotic and biotic chlorinated ethenes reduction, and highlights that specialized consortia may benefit Cr (VI) bio-reduction.
ContributorsMohana Rangan, Srivatsan (Author) / Krajmalnik-Brown, Rosa (Thesis advisor) / Delgado, Anca G (Thesis advisor) / Torres, César I (Committee member) / van Paassen, Leon (Committee member) / Arizona State University (Publisher)
Created2022
Description
The world currently faces hundreds of millions of cubic meters of soil contaminated with petroleum crude oil residuals. The application of ozone gas (O3) to contaminated soil is an effective means to oxidize petrogenic compounds and, when used with bioremediation, remove the oxidized byproducts. The overarching goal of this dissertation was to evaluate two areas of potential concern to large-scale O3 deployment: the capacity of O3-treated petroleum contaminated soils to support seed germination before bioremediation and the transport characteristics of O3 in soil columns. A matched study comparing the germination outcomes of radish (Raphanus sativus L.), grass (Lagurus ovatus), and lettuce (Lactuca sativa) in soils contaminated with three crude oils at various O3 total-dose levels showed that radish germination was sensitive to the soluble byproducts of oxidized petroleum (assayed as dissolved organic carbon [DOC]), but not sensitive to the unreacted petroleum (total petroleum hydrocarbon [TPH]). A multivariable logistic regression model based on the radish results showed that adverse germination outcomes varied with the DOC concentration and that DOC ecotoxicity decreased with increasing O3 dose-level and background organic material. The model was used to create a risk management map of conditions that created 10%, 25%, and 50% extra risks of adverse radish germination. Thus, while O3 effectively lowered TPH in soils, the byproducts exhibited ecotoxicity that inhibited radish germination. On the other hand, the sensitivity of radish germination to oxidized petroleum byproducts could be utilized to assess ecological risk. The feasibility of gas transport in the soil matrix is also of paramount concern to field-scale utilization of O3. A matched study comparing TPH removal at three field-relevant loading rates (4, 12, or 36 mgozone/ gsoil/ hr) and various total dose-levels showed an anisotropic pattern along the axial distance favoring the column inlet end. The asymmetry decreased as loading rate decreased and with concurrent improvements in O3-transport distance, O3 utilization, and heat balance. Overall, a low O3 loading rate significantly improved O3 transport and utilization efficiency, while also better distributing reaction-generated heat along the gas flow path for a depth typically utilized in bioremediation field settings.
ContributorsYavuz, Burcu Manolya (Author) / Rittmann, Bruce E (Thesis advisor) / Delgado, Anca G (Committee member) / Westerhoff, Paul (Committee member) / Arizona State University (Publisher)
Created2022
Description
The potential of using bio-geo-chemical processes for applications in geotechnical engineering has been widely explored in order to overcome the limitation of traditional ground improvement techniques. Biomineralization via urea hydrolysis, referred to as Microbial or Enzymatic Induced Carbonate Precipitation (MICP/EICP), has been shown to increase soil strength by stimulating precipitation of calcium carbonate minerals, bonding soil particles and filling the pores. Microbial Induced Desaturation and Precipitation (MIDP) via denitrification has also been studied for its potential to stabilize soils through mineral precipitation, but also through production of biogas, which can mitigate earthquake induced liquefaction by desaturation of the soil. Empirical relationships have been established, which relate the amount of products of these biochemical processes to the engineering properties of treated soils. However, these engineering properties may vary significantly depending on the biomineral and biogas formation mechanism and distribution patterns at pore-scale. This research focused on the pore-scale characterization of biomineral and biogas formations in porous media.
The pore-scale characteristics of calcium carbonate precipitation via EICP and biogenic gas formation via MIDP were explored by visual observation in a transparent porous media using a microfluidic chip. For this purpose, an imaging system was designed and image processing algorithms were developed to analyze the experimental images and detect the nucleation and growth of precipitated minerals and formation and migration mechanisms of gas bubbles within the microfluidic chip. Statistical analysis was performed based on the processed images to assess the evolution of biomineral size distribution, the number of precipitated minerals and the porosity reduction in time. The resulting images from the biomineralization study were used in a numerical simulation to investigate the relation between the mineral distribution, porosity-permeability relationships and process efficiency. By comparing biogenic gas production with abiotic gas production experiments, it was found that the gas formation significantly affects the gas distribution and resulting degree of saturation. The experimental results and image analysis provide insight in the kinetics of the precipitation and gas formation processes and their resulting distribution and related engineering properties.
The pore-scale characteristics of calcium carbonate precipitation via EICP and biogenic gas formation via MIDP were explored by visual observation in a transparent porous media using a microfluidic chip. For this purpose, an imaging system was designed and image processing algorithms were developed to analyze the experimental images and detect the nucleation and growth of precipitated minerals and formation and migration mechanisms of gas bubbles within the microfluidic chip. Statistical analysis was performed based on the processed images to assess the evolution of biomineral size distribution, the number of precipitated minerals and the porosity reduction in time. The resulting images from the biomineralization study were used in a numerical simulation to investigate the relation between the mineral distribution, porosity-permeability relationships and process efficiency. By comparing biogenic gas production with abiotic gas production experiments, it was found that the gas formation significantly affects the gas distribution and resulting degree of saturation. The experimental results and image analysis provide insight in the kinetics of the precipitation and gas formation processes and their resulting distribution and related engineering properties.
ContributorsKim, Daehyun (Author) / van Paassen, Leon (Thesis advisor) / Kavazanjian, Edward (Committee member) / Zapata, Claudia (Committee member) / Mahabadi, Nariman (Committee member) / Tao, Junliang (Committee member) / Jang, Jaewon (Committee member) / Arizona State University (Publisher)
Created2019
Description
The Atlantic razor clam burrows underground with effectiveness and efficiency by coordinating shape changings of its shell and foot. Inspired by the burrowing strategy of razor clams, this research is dedicated to developing a self-burrowing technology for active underground explorations by investigating the burrowing mechanism of razor clams from the perspective of soil mechanics. In this study, the razor clam was observed to burrow out of sands simply by extending and contracting its foot periodically. This upward burrowing gait is much simpler than its downward burrowing gait, which also involves opening/closing of the shell and dilation of the foot. The upward burrowing gait inspired the design of a self-burrowing-out soft robot, which drives itself out of sands naturally by extension and contraction through pneumatic inflation and deflation. A simplified analytical model was then proposed and explained the upward burrowing behavior of the robot and razor clams as the asymmetric nature of soil resistances applied on both ends due to the intrinsic stress gradient of sand deposits. To burrow downward, additional symmetry-breaking features are needed for the robot to increase the resistance in the upward burrowing direction and to decrease the resistance in the downward burrowing direction. A potential approach is by incorporating friction anisotropy, which was then experimentally demonstrated to affect the upward burrowing of the soft robot. The downward burrowing gait of razor clams provides another inspiration. By exploring the analogies between the downward burrowing gait and in-situ soil characterization methods, a clam-inspired shape-changing penetrator was designed and penetrated dry granular materials both numerically and experimentally. Results demonstrated that the shell opening not only contributes to forming a penetration anchor by compressing the surrounding particles, but also reduces the foot penetration resistance temporally by creating a stress arch above the foot; the shell closing facilitates the downward burrowing by reducing the friction resistance to the subsequent shell retraction. Findings from this research shed lights on the future design of a clam-inspired self-burrowing robot.
ContributorsHuang, Sichuan (Author) / Tao, Junliang (Thesis advisor) / Kavazanjian, Edward (Committee member) / Marvi, Hamidreza (Committee member) / Zapata, Claudia (Committee member) / van Paassen, Leon (Committee member) / Arizona State University (Publisher)
Created2020
Description
Expansive soils pose considerable geotechnical and structural challenges all over the world. Many cities, towns, transport systems, and structures are built on expansive soils. This study evaluates stabilization of expansive soils using silicate solution extracted from rice husk taking advantage of an agricultural material waste. Rice husk ash production was optimized considering several factors including rinsing solution, rinsing temperature, burning time, and burning temperature. Results indicated that washing the rice husk with HCl (1M) produced an ash with surface area of 320 m2/g and 97% of silicon oxide. Two local soils were treated with sodium silicate solution, silica gel at pH 1.5, and silica gel at pH 4 to evaluate its mechanical properties at curing times of 1 day, 7 days, and 14 days. Results indicated that sodium silicate solution reduced the one-dimensional swell by 48% for Soil A, however, swell for soil B remained about the same. Silica gel at pH 1.5 reduced the one-dimensional swell by 67% for soil A and by 35% for soil B. Silica gel at pH 4 did also reduce the free swell by 40% for soil A and by 35% for soil B. Results also indicated that the swell pressures for all treated soils increased significantly compared to untreated soils. Soils treated with sodium silicate solution showed irregular compaction curves. Silica gel-treated soils showed a reduction in the maximum dry unit weight for both soils but optimum water content decreased for soil A and increased for soil B. Atterberg limits were also reduced for sodium silicate and silica gels-treated soils. Swelling index for bentonite showed a reduction by 53% for all treated bentonites. Soil-water characteristics curves (SWCC) for sodium silicate-treated soils remined almost the same as untreated soils. However, silica gels-treated soils retain more water. Surface area (SSA) decreased for sodium silicate-treated soil but increased for all silica gels-treated soils. It was concluded that curing times did not show additional improvement in most of the experiments, but the results remained about the same as 1-day treatment. The study demonstrated that silicate solution is promising and sustainable technique for stabilization of expansive soils.
Contributorsalharbi, hani (Author) / Zapata, Claudia (Thesis advisor) / Kavazanjian, Edward (Committee member) / van Paassen, Leon (Committee member) / Khodadaditirkolaei, Hamed (Committee member) / Arizona State University (Publisher)
Created2020
Description
Enzyme-induced carbonate precipitation (EICP) is an emerging technology for ground improvement that cements soil with calcium carbonate to increase strength and stiffness. EICP-improved soil can be used to support new facilities or it can be injected under existing facilities to prevent excessive deformation. The limitations for commercial adoption of EICP are the cost and the lack of implementation at field-scale. This research demonstrated two ways to reduce the cost of EICP treatment at field-scale. The first was a modification to the EICP solution such that lower amounts of chemicals are needed to achieve target strengths. The second was to use a simple and inexpensive enzyme extraction method to produce the enzyme at a large-scale. This research also involved a two-stage scale-up process to create EICP biocemented soil columns using a permeation grouting technique. The first stage was at mid-scale where 0.6 m x 0.3 m-diameter EICP biocemented soil columns were created in boxes. This work confirmed that conventional permeation grouting equipment and methods are feasible for EICP soil treatment because the columns were found to have a uniform shape, the injection method was able to deliver the EICP solution to the edges of the treatment zone, and downhole geophysics was effectively used to measure the shear wave velocity of the biocemented soil mass. The field-scale stage was performed in the Test Pit facility at the Center for Bio-mediated and Bio-inspired Geotechnics' Soils Field Laboratory. Seven biocemented soil columns were created with diameters ranging from 0.3-1 m and heights ranging from 1-2.4 m. Effective implementation at this scale was confirmed through monitoring the injection process with embedded moisture sensors, evaluating the in situ strength improvement with downhole geophysics and load testing, and testing of the excavated columns to measure shear wave velocity, dimensions, carbonate content, and strength. Lastly, a hotspot life cycle assessment was performed which identified ways to reduce the environmental impacts of EICP by using alternative sourcing of inputs and extraction of byproducts. Overall, this research project demonstrates that EICP is a viable ground improvement technique by way of successfully producing field-scale biocemented soil columns.
ContributorsMartin, Kimberly Kathryn (Author) / Kavazanjian, Jr., Edward (Thesis advisor) / Zapata, Claudia E. (Committee member) / van Paassen, Leon (Committee member) / Arizona State University (Publisher)
Created2021
Description
Water is a vital resource, and its protection is a priority world-wide. One widespread threat to water quality is contamination by chlorinated solvents. These dry-cleaning and degreasing agents entered the watershed through spills and improper disposal and now are detected in 4% of U.S. aquifers and 4.5-18% of U.S. drinking water sources. The health effects of these contaminants can be severe, as they are associated with damage to the nervous, liver, kidney, and reproductive systems, developmental issues, and possibly cancer. Chlorinated solvents must be removed or transformed to improve water quality and protect human and environmental health. One remedy, bioaugmentation, the subsurface addition of microbial cultures able to transform contaminants, has been implemented successfully at hundreds of sites since the 1990s. Bioaugmentation uses the bacteria Dehalococcoides to transform chlorinated solvents with hydrogen, H2, as the electron donor. At advection limited sites, bioaugmentation can be combined with electrokinetics (EK-Bio) to enhance transport. However, challenges for successful bioremediation remain. In this work I addressed several knowledge gaps surrounding bioaugmentation and EK-Bio. I measured the H2 consuming capacity of soils, detailed the microbial metabolisms driving this demand, and evaluated how these finding relate to reductive dechlorination. I determined which reactions dominated at a contaminated site with mixed geochemistry treated with EK-Bio and compared it to traditional bioaugmentation. Lastly, I assessed the effect of EK-Bio on the microbial community at a field-scale site. Results showed the H2 consuming capacity of soils was greater than that predicted by initial measurements of inorganic electron acceptors and primarily driven by carbon-based microbial metabolisms. Other work demonstrated that, given the benefits of some carbon-based metabolisms to microbial reductive dechlorination, high levels of H2 consumption in soils are not necessarily indicative of hostile conditions for Dehalococcoides. Bench-scale experiments of EK-Bio under mixed geochemical conditions showed EK-Bio out-performed traditional bioaugmentation by facilitating biotic and abiotic transformations. Finally, results of microbial community analysis at a field-scale implementation of EK-Bio showed that while there were significant changes in alpha and beta diversity, the impact of EK-Bio on native microbial communities was minimal.
ContributorsAltizer, Megan Leigh (Author) / Torres, César I (Thesis advisor) / Krajmalnik-Brown, Rosa (Thesis advisor) / Rittmann, Bruce E (Committee member) / Kavazanjian, Edward (Committee member) / Delgado, Anca G (Committee member) / Arizona State University (Publisher)
Created2020