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- All Subjects: Ozone
- Creators: Delgado, Anca G
- Creators: Civil, Environmental and Sustainable Eng Program
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
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
Terrestrial crude oil spills compromise a soil’s ability to provide ecosystem services by inhibiting plant life and threatening groundwater integrity. Ozone gas, a powerful oxidant, shows promise to aid in soil recovery by degrading petroleum hydrocarbons into more bioavailable and biodegradable chemicals. However, previous research has shown that ozone can change the soil pH and create harmful organic compounds.
The research objective was to determine the short-term ecological toxicity of ozonation byproducts on seed germination of three distinct plant types (radish, lettuce, and grass) compared to untreated and uncontaminated soils. We hypothesize that the reduction of heavy hydrocarbon contamination in soil by ozone application will provide more suitable habitat for the germinating seeds. The effect of ozone treatment on seed germination and seedling quality was measured using ASTM standards for early seedling growth in conjunction with a gradient of potting soil amendments. Ozonation parameters were measured using established methods and include total petroleum hydrocarbons (TPH), dissolved organic carbon (DOC), and pH.
This study demonstrated the TPH levels fall up to 22% with ozonation, suggesting TPH removal is related to the amount of ozone delivered as opposed to the type of crude oil present. The DOC values increase comparably across crude oil types as the ozonation dose increases (from a background level of 0.25 g to 6.2 g/kg dry soil at the highest ozone level), suggesting that DOC production is directly related to the amount of ozone, not crude oil type. While ozonation reduced the mass of heavy hydrocarbons in the soil, it increased the amount of ozonation byproducts in the soil. For the three types of seeds used in the study, these changes in concentrations of TPH and DOC affected the species differently; however, no seed type showed improved germination after ozone treatment. Thus, ozone treatment by itself had a negative impact on germination potential.
Future research should focus on the effects of post-ozonation, long-term bioremediation on eco-toxicity. By helping define the eco-toxicity of ozonation techniques, this research can improve upon previously established ozone techniques for petroleum remediation and provide economic and environmental benefits when used for soil treatment.
The research objective was to determine the short-term ecological toxicity of ozonation byproducts on seed germination of three distinct plant types (radish, lettuce, and grass) compared to untreated and uncontaminated soils. We hypothesize that the reduction of heavy hydrocarbon contamination in soil by ozone application will provide more suitable habitat for the germinating seeds. The effect of ozone treatment on seed germination and seedling quality was measured using ASTM standards for early seedling growth in conjunction with a gradient of potting soil amendments. Ozonation parameters were measured using established methods and include total petroleum hydrocarbons (TPH), dissolved organic carbon (DOC), and pH.
This study demonstrated the TPH levels fall up to 22% with ozonation, suggesting TPH removal is related to the amount of ozone delivered as opposed to the type of crude oil present. The DOC values increase comparably across crude oil types as the ozonation dose increases (from a background level of 0.25 g to 6.2 g/kg dry soil at the highest ozone level), suggesting that DOC production is directly related to the amount of ozone, not crude oil type. While ozonation reduced the mass of heavy hydrocarbons in the soil, it increased the amount of ozonation byproducts in the soil. For the three types of seeds used in the study, these changes in concentrations of TPH and DOC affected the species differently; however, no seed type showed improved germination after ozone treatment. Thus, ozone treatment by itself had a negative impact on germination potential.
Future research should focus on the effects of post-ozonation, long-term bioremediation on eco-toxicity. By helping define the eco-toxicity of ozonation techniques, this research can improve upon previously established ozone techniques for petroleum remediation and provide economic and environmental benefits when used for soil treatment.
ContributorsJanuszewski, Brielle (Author) / Rittmann, Bruce (Thesis director) / Yavuz, Burcu (Committee member) / Civil, Environmental and Sustainable Eng Program (Contributor) / School of International Letters and Cultures (Contributor) / School of Politics and Global Studies (Contributor, Contributor) / School of Life Sciences (Contributor) / Barrett, The Honors College (Contributor)
Created2020-05