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- All Subjects: Environmental engineering
- Creators: Arizona State University
- Member of: ASU Electronic Theses and Dissertations
Description
The goal of the study was twofold: (i) to investigate the synthesis of hematite-impregnated granular activated carbon (Fe-GAC) by hydrolysis of Fe (III) and (ii) to assess the effectiveness of the fabricated media in removal of arsenic from water. Fe-GAC was synthesized by hydrolysis of Fe(III) salts under two Fe (III) initial dosages (0.5M and 2M) and two hydrolysis periods (24 hrs and 72 hrs). The iron content of the fabricated Fe-GAC media ranged from 0.9% to 4.4% Fe/g of the dry media. Pseudo-equilibrium batch test data at pH = 7.7±0.2 in 1mM NaHCO3 buffered ultrapure water and challenge groundwater representative of the Arizona Mexico border region were fitted to a Freundlich isotherm model. The findings suggested that the arsenic adsorption capacity of the metal (hydr)oxide modified GAC media is primarily controlled by the surface area of the media, while the metal content exhibited lesser effect. The adsorption capacity of the media in the model Mexican groundwater matrix was significantly lower for all adsorbent media. Continuous flow short bed adsorber tests (SBA) demonstrated that the adsorption capacity for arsenic in the challenge groundwater was reduced by a factor of 3 to 4 as a result of the mass transport effects. When compared on metal basis, the iron (hydr)oxide modified media performed comparably well as existing commercial media for treatment of arsenic. On dry mass basis, the fabricated media in this study removed less arsenic than their commercial counterparts because the metal content of the commercial media was significantly higher.
ContributorsJain, Arti (Author) / Hristovski, Kiril (Thesis advisor) / Olson, Larry (Committee member) / Madar, David (Committee member) / Edwards, David (Committee member) / Arizona State University (Publisher)
Created2011
Description
It is estimated that wind induced soil transports more than 500 x 106 metric tons of fugitive dust annually. Soil erosion has negative effects on human health, the productivity of farms, and the quality of surface waters. A variety of different polymer stabilizers are available on the market for fugitive dust control. Most of these polymer stabilizers are expensive synthetic polymer products. Their adverse effects and expense usually limits their use. Biopolymers provide a potential alternative to synthetic polymers. They can provide dust abatement by encapsulating soil particles and creating a binding network throughout the treated area. This research into the effectiveness of biopolymers for fugitive dust control involved three phases. Phase I included proof of concept tests. Phase II included carrying out the tests in a wind tunnel. Phase III consisted of conducting the experiments in the field. Proof of concept tests showed that biopolymers have the potential to reduce soil erosion and fugitive dust transport. Wind tunnel tests on two candidate biopolymers, xanthan and chitosan, showed that there is a proportional relationship between biopolymer application rates and threshold wind velocities. The wind tunnel tests also showed that xanthan gum is more successful in the field than chitosan. The field tests showed that xanthan gum was effective at controlling soil erosion. However, the chitosan field data was inconsistent with the xanthan data and field data on bare soil.
ContributorsAlsanad, Abdullah (Author) / Kavazanjian, Edward (Thesis advisor) / Edwards, David (Committee member) / Zapata, Claudia (Committee member) / Arizona State University (Publisher)
Created2011
Description
Population growth and fresh water depletion challenge drinking water utilities. Surface water quality is impacted significantly by climate variability, human activities, and extreme events like natural disasters. Dissolved organic carbon (DOC) is an important water quality index and the precursor of disinfection by-products (DBPs) that varies with both hydrologic and anthropogenic factors. Granular activated carbon (GAC) is a best available technology for utilities to meet Stage 2 D/DBP rule compliance and to remove contaminants of emerging concern (CECs) (e.g., pharmaceutical, personal care products (PCPs), etc.). Utilities can operate GAC with more efficient and flexible strategies with the understanding of organic occurrence in source water and a model capable predicting DOC occurrence. In this dissertation, it was found that DOC loading significantly correlated with spring runoff and was intensified by dry-duration antecedent to first flush. Dynamic modeling based on reservoir management (e.g., pump-back operation) was established to simulate the DOC transport in the reservoir system. Additionally, summer water recreational activities were found to raise the level of PCPs, especially skin-applied products, in raw waters. GAC was examined in this dissertation for both carbonaceous and emerging nitrogenous DBP (N-DBP) precursors (i.e., dissolved organic nitrogen (DON)) removal. Based on the experimental findings, GAC preferentially removes UV254-absorbing material, and DOC is preferentially removed over DON which may be composed primarily of hydrophilic organic and results in the low affinity for adsorption by GAC. The presence of organic nitrogen can elevate the toxicity of DBPs by forming N-DBPs, and this could be a major drawback for facilities considering installation of a GAC adsorber owing to the poor removal efficiency of DON by GAC. A modeling approach was established for predicting DOC and DON breakthrough during GAC operation. However, installation of GAC adsorber is a burden for utilities with respect to operational and maintenance cost. It is common for utilities to regenerate saturated GAC in order to save the cost of purchasing fresh GAC. The traditional thermal regeneration technology for saturated GAC is an energy intensive process requiring high temperature of incineration. Additionally, small water treatment sites usually ship saturated GAC to specialized facilities for regeneration increasing the already significant carbon footprint of thermal regeneration. An innovative GAC regeneration technique was investigated in this dissertation for the feasibility as on-site water treatment process. Virgin GAC was first saturated by organic contaminant then regenerated in-situ by iron oxide nanocatalysts mixed with hydrogen peroxide. At least 70 % of adsorption capacity of GAC can be regenerated repeatedly for experiments using modeling compound (phenol) or natural organic matter (Suwannee River humic acid). The regeneration efficiency increases with increasing adsorbate concentration. Used-iron nanocatalysts can be recovered repeatedly without significant loss of catalytic ability. This in-situ regeneration technique provides cost and energy efficient solution for water utilities considering GAC installation. Overall, patterns were found for DOC and CEC variations in drinking water sources. Increasing concentrations of bulk (DOC and DON) and/or trace organics challenge GAC operation in utilities that have limited numbers of bed-volume treated before regeneration is required. In-situ regeneration using iron nanocatalysts and hydrogen peroxide provides utilities an alternative energy-efficient operation mode when considering installation of GAC adsorber.
ContributorsChiu, Chao-An (Author) / Westerhoff, Paul (Thesis advisor) / Rittmann, Bruce (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2012
Description
In this work, the vapor transport and aerobic bio-attenuation of compounds from a multi-component petroleum vapor mixture were studied for six idealized lithologies in 1.8-m tall laboratory soil columns. Columns representing different geological settings were prepared using 20-40 mesh sand (medium-grained) and 16-minus mesh crushed granite (fine-grained). The contaminant vapor source was a liquid composed of twelve petroleum hydrocarbons common in weathered gasoline. It was placed in a chamber at the bottom of each column and the vapors diffused upward through the soil to the top where they were swept away with humidified gas. The experiment was conducted in three phases: i) nitrogen sweep gas; ii) air sweep gas; iii) vapor source concentrations decreased by ten times from the original concentrations and under air sweep gas. Oxygen, carbon dioxide and hydrocarbon concentrations were monitored over time. The data allowed determination of times to reach steady conditions, effluent mass emissions and concentration profiles. Times to reach near-steady conditions were consistent with theory and chemical-specific properties. First-order degradation rates were highest for straight-chain alkanes and aromatic hydrocarbons. Normalized effluent mass emissions were lower for lower source concentration and aerobic conditions. At the end of the study, soil core samples were taken every 6 in. Soil moisture content analyses showed that water had redistributed in the soil during the experiment. The soil at the bottom of the columns generally had higher moisture contents than initial values, and soil at the top had lower moisture contents. Profiles of the number of colony forming units of hydrocarbon-utilizing bacteria/g-soil indicated that the highest concentrations of degraders were located at the vertical intervals where maximum degradation activity was suggested by CO2 profiles. Finally, the near-steady conditions of each phase of the study were simulated using a three-dimensional transient numerical model. The model was fit to the Phase I data by adjusting soil properties, and then fit to Phase III data to obtain compound-specific first-order biodegradation rate constants ranging from 0.0 to 5.7x103 d-1.
ContributorsEscobar Melendez, Elsy (Author) / Johnson, Paul C. (Thesis advisor) / Andino, Jean (Committee member) / Forzani, Erica (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Kavazanjian, Edward (Committee member) / Arizona State University (Publisher)
Created2012
Description
Titanium dioxide (TiO2) nanomaterial use is becoming more prevalent as is the likelihood of human exposure and environmental release. The goal of this thesis is to develop analytical techniques to quantify the level of TiO2 in complex matrices to support environmental, health, and safety research of TiO2 nanomaterials. A pharmacokinetic model showed that the inhalation of TiO2 nanomaterials caused the highest amount to be absorbed and distributed throughout the body. Smaller nanomaterials (< 5nm) accumulated in the kidneys before clearance. Nanoparticles of 25 nm diameter accumulated in the liver and spleen and were cleared from the body slower than smaller nanomaterials. A digestion method using nitric acid, hydrofluoric acid, and hydrogen peroxide was found to digest organic materials and TiO2 with a recovery of >80%. The samples were measured by inductively coupled plasma-mass spectrometry (ICP-MS) and the method detection limit was 600 ng of Ti. An intratracheal instillation study of TiO2 nanomaterials in rats found anatase TiO2 nanoparticles in the caudal lung lobe of rats 1 day post instillation at a concentration of 1.2 ug/mg dry tissue, the highest deposition rate of any TiO2 nanomaterial. For all TiO2 nanomaterial morphologies the concentrations in the caudal lobes were significantly higher than those in the cranial lobes. In a study of TiO2 concentration in food products, white colored foods or foods with a hard outer shell had higher concentrations of TiO2. Hostess Powdered Donettes were found to have the highest Ti mass per serving with 200 mg Ti. As much as 3.8% of the total TiO2 mass was able to pass through a 0.45 um indicating that some of the TiO2 is likely nanosized. In a study of TiO2 concentrations in personal care products and paints, the concentration of TiO2 was as high as 117 ug/mg in Benjamin Moore white paint and 70 ug/mg in a Neutrogena sunscreen. Greater than 6% of Ti in one sunscreen was able to pass through a 0.45 um filter. The nanosized TiO2 in food products and personal care products may release as much as 16 mg of nanosized TiO2 per individual per day to wastewater.
ContributorsWeir, Alex Alan (Author) / Westerhoff, Paul K (Thesis advisor) / Hristovski, Kiril (Committee member) / Herckes, Pierre (Committee member) / Arizona State University (Publisher)
Created2011
Description
Intimate coupling of Ti2 photocatalysis and biodegradation (ICPB) offers potential for degrading biorecalcitrant and toxic organic compounds much better than possible with conventional wastewater treatments. This study reports on using a novel sponge-type, Ti2-coated biofilm carrier that shows significant adherence of Ti2 to its exterior and the ability to accumulate biomass in its interior (protected from UV light and free radicals). First, this carrier was tested for ICPB in a continuous-flow photocatalytic circulating-bed biofilm reactor (PCBBR) to mineralize biorecalcitrant organic: 2,4,5-trichlorophenol (TCP). Four mechanisms possibly acting of ICPB were tested separately: TCP adsorption, UV photolysis/photocatalysis, and biodegradation. The carrier exhibited strong TCP adsorption, while photolysis was negligible. Photocatalysis produced TCP-degradation products that could be mineralized and the strong adsorption of TCP to the carrier enhanced biodegradation by relieving toxicity. Validating the ICPB concept, biofilm was protected inside the carriers from UV light and free radicals. ICPB significantly lowered the diversity of the bacterial community, but five genera known to biodegrade chlorinated phenols were markedly enriched. Secondly, decolorization and mineralization of reactive dyes by ICPB were investigated on a refined Ti2-coated biofilm carrier in a PCBBR. Two typical reactive dyes: Reactive Black 5 (RB5) and Reactive Yellow 86 (RY86), showed similar first-order kinetics when being photocatalytically decolorized at low pH (~4-5), which was inhibited at neutral pH in the presence of phosphate or carbonate buffer, presumably due to electrostatic repulsion from negatively charged surface sites on Ti2, radical scavenging by phosphate or carbonate, or both. In the PCBBR, photocatalysis alone with Ti2-coated carriers could remove RB5 and COD by 97% and 47%, respectively. Addition of biofilm inside macroporous carriers maintained a similar RB5 removal efficiency, but COD removal increased to 65%, which is evidence of ICPB despite the low pH. A proposed ICPB pathway for RB5 suggests that a major intermediate, a naphthol derivative, was responsible for most of the residual COD. Finally, three low-temperature sintering methods, called O, D and DN, were compared based on photocatalytic efficiency and Ti2 adherence. The DN method had the best Ti2-coating properties and was a successful carrier for ICPB of RB5 in a PCBBR.
ContributorsLi, Guozheng (Author) / Rittmann, Bruce E. (Thesis advisor) / Halden, Rolf (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2011
Description
The overall goal of this dissertation is to advance understanding of biofilm reduction of oxidized contaminants in water and wastewater. Chapter 1 introduces the fundamentals of biological reduction of three oxidized contaminants (nitrate, perchlorate, and trichloriethene (TCE)) using two biofilm processes (hydrogen-based membrane biofilm reactors (MBfR) and packed-bed heterotrophic reactors (PBHR)), and it identifies the research objectives. Chapters 2 through 6 focus on nitrate removal using the MBfR and PBHR, while chapters 7 through 10 investigate simultaneous reduction of nitrate and another oxidized compound (perchlorate, sulfate, or TCE) in the MBfR. Chapter 11 summarizes the major findings of this research. Chapters 2 and 3 demonstrate nitrate removal in a groundwater and identify the maximum nitrate loadings using a pilot-scale MBfR and a pilot-scale PBHR, respectively. Chapter 4 compares the MBfR and the PBHR for denitrification of the same nitrate-contaminated groundwater. The comparison includes the maximum nitrate loading, the effluent water quality of the denitrification reactors, and the impact of post-treatment on water quality. Chapter 5 theoretically and experimentally demonstrates that the nitrate biomass-carrier surface loading, rather than the traditionally used empty bed contact time or nitrate volumetric loading, is the primary design parameter for heterotrophic denitrification. Chapter 6 constructs a pH-control model to predict pH, alkalinity, and precipitation potential in heterotrophic or hydrogen-based autotrophic denitrification reactors. Chapter 7 develops and uses steady-state permeation tests and a mathematical model to determine the hydrogen-permeation coefficients of three fibers commonly used in the MBfR. The coefficients are then used as inputs for the three models in Chapters 8-10. Chapter 8 develops a multispecies biofilm model for simultaneous reduction of nitrate and perchlorate in the MBfR. The model quantitatively and systematically explains how operating conditions affect nitrate and perchlorate reduction and biomass distribution via four mechanisms. Chapter 9 modifies the nitrate and perchlorate model into a nitrate and sulfate model and uses it to identify operating conditions corresponding to onset of sulfate reduction. Chapter 10 modifies the nitrate and perchlorate model into a nitrate and TCE model and uses it to investigate how operating conditions affect TCE reduction and accumulation of TCE reduction intermediates.
ContributorsTang, Youneng (Author) / Rittmann, Bruce E. (Thesis advisor) / Westerhoff, Paul (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Halden, Rolf (Committee member) / Arizona State University (Publisher)
Created2012
Description
Local municipalities in the Phoenix Metropolitan Area have voiced an interest in purchasing alternate source water with lower DBP precursors. Along the primary source is a hydroelectric dam in which water will be diverted from. This project is an assessment of optimizing the potential blends of source water to a water treatment plant in an effort to enable them to more readily meet DBP regulations. To perform this analysis existing water treatment models were used in conjunction with historic water quality sampling data to predict chemical usage necessary to meet DBP regulations. A retrospective analysis was performed for the summer months of 2007 regarding potential for the WTP to reduce cost through optimizing the source water by an average of 30% over the four-month period, accumulating to overall treatment savings of $154 per MG ($82 per AF).
ContributorsRice, Jacelyn (Author) / Westerhoff, Paul (Thesis advisor) / Fox, Peter (Committee member) / Hristovski, Kiril (Committee member) / Arizona State University (Publisher)
Created2011
Description
Contamination by chlorinated ethenes is widespread in groundwater aquifers, sediment, and soils worldwide. The overarching objectives of my research were to understand how the bacterial genus Dehalococcoides function optimally to carry out reductive dechlorination of chlorinated ethenes in a mixed microbial community and then apply this knowledge to manage dechlorinating communities in the hydrogen-based membrane biofilm reactor (MBfR). The MBfR is used for the biological reduction of oxidized contaminants in water using hydrogen supplied as the electron donor by diffusion through gas-transfer fibers. First, I characterized a new anaerobic dechlorinating community developed in our laboratory, named DehaloR^2, in terms of chlorinated ethene turnover rates and assessed its microbial community composition. I then carried out an experiment to correlate performance and community structure for trichloroethene (TCE)-fed microbial consortia. Fill-and-draw reactors inoculated with DehaloR^2 demonstrated a direct correlation between microbial community function and structure as the TCE-pulsing rate was increased. An electron-balance analysis predicted the community structure based on measured concentrations of products and constant net yields for each microorganism. The predictions corresponded to trends in the community structure based on pyrosequencing and quantitative PCR up to the highest TCE pulsing rate, where deviations to the trend resulted from stress by the chlorinated ethenes. Next, I optimized a method for simultaneous detection of chlorinated ethenes and ethene at or below the Environmental Protection Agency maximum contaminant levels for groundwater using solid phase microextraction in a gas chromatograph with a flame ionization detector. This method is ideal for monitoring biological reductive dechlorination in groundwater, where ethene is the ultimate end product. The major advantage of this method is that it uses a small sample volume of 1 mL, making it ideally suited for bench-scale feasibility studies, such as the MBfR. Last, I developed a reliable start-up and operation strategy for TCE reduction in the MBfR. Successful operation relied on controlling the pH-increase effects of methanogenesis and homoacetogenesis, along with creating hydrogen limitation during start-up to allow dechlorinators to compete against other microorgansims. Methanogens were additionally minimized during continuous flow operation by a limitation in bicarbonate resulting from strong homoacetogenic activity.
ContributorsZiv-El, Michal (Author) / Rittmann, Bruce E. (Thesis advisor) / Krajmalnik-Brown, Rosa (Thesis advisor) / Halden, Rolf U. (Committee member) / Arizona State University (Publisher)
Created2012
Description
Carbon capture and sequestration (CCS) is one of the important mitigation options for climate change. Numerous technologies to capture carbon dioxide (CO2) are in development but currently, capture using amines is the predominant technology. When the flue gas reacts with amines (Monoethanaloamine) the CO2 is absorbed into the solution and forms an intermediate product which then releases CO2 at higher temperature. The high temperature necessary to strip CO2 is provided by steam extracted from the powerplant thus reducing the net output of the powerplant by 25% to 35%. The reduction in electricity output for the same input of coal increases the emissions factor of Nitrogen Oxides, Mercury, Particulate matter, Ammonia, Volatile organic compounds for the same unit of electricity produced. The thesis questions if this tradeoff between CO2 and other emissions is beneficial or not. Three different methodologies, Life Cycle Assessment, Valuation models and cost benefit analysis are used to identify if there is a net benefit to the society on implementation of CCS to a Pulverized coal powerplant. These methodologies include the benefits due to reduction of CO2 and the disbenefits due to the increase of other emissions. The life cycle assessment using ecoindicator'99 methodology shows the CCS is not beneficial under Hierarchical and Egalitarian perspective. The valuation model shows that the inclusion of the other emissions reduces the benefit associated with CCS. For a lower CO2 price the valuation model shows that CCS is detrimental to the environment. The cost benefit analysis shows that a CO2 price of at least $80/tCO2 is required for the cost benefit ratio to be 1. The methodology integrates Montecarlo simulation to characterize the uncertainties associated with the valuation models.
ContributorsSekar, Ashok (Author) / Williams, Eric (Thesis advisor) / Chester, Mikhail (Thesis advisor) / Allenby, Braden (Committee member) / Arizona State University (Publisher)
Created2012