Matching Items (9)
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- All Subjects: Environmental sciences
- All Subjects: water treatment
- Genre: Academic theses
- Creators: Fox, Peter
- Creators: Green, Matthew
- Status: Published
Description
The North American Monsoon System (NAMS) contributes ~55% of the annual rainfall in the Chihuahuan Desert during the summer months. Relatively frequent, intense storms during the NAMS increase soil moisture, reduce surface temperature and lead to runoff in ephemeral channels. Quantifying these processes, however, is difficult due to the sparse nature of coordinated observations. In this study, I present results from a field network of rain gauges (n = 5), soil probes (n = 48), channel flumes (n = 4), and meteorological equipment in a small desert shrubland watershed (~0.05 km2) in the Jornada Experimental. Using this high-resolution network, I characterize the temporal and spatial variability of rainfall, soil conditions and channel runoff within the watershed from June 2010 to September 2011, covering two NAMS periods. In addition, CO2, water and energy measurements at an eddy covariance tower quantify seasonal, monthly and event-scale changes in land-atmosphere states and fluxes. Results from this study indicate a strong seasonality in water and energy fluxes, with a reduction in Bowen ratio (B, the ratio of sensible to latent heat fluxes) from winter (B = 14) to summer (B = 3.3). This reduction is tied to shallow soil moisture availability during the summer (s = 0.040 m3/m3) as compared to the winter (s = 0.004 m3/m3). During the NAMS, I analyzed four consecutive rainfall-runoff events to quantify the soil moisture and channel flow responses and how water availability impacted the land-atmosphere fluxes. Spatial hydrologic variations during events occur over distances as short as ~15 m. The field network also allowed comparisons of several approaches to estimate evapotranspiration (ET). I found a more accurate ET estimate (a reduction of mean absolute error by 38%) when using distributed soil moisture data, as compared to a standard water balance approach based on the tower site. In addition, use of spatially-varied soil moisture data yielded a more reasonable relationship between ET and soil moisture, an important parameterization in many hydrologic models. The analyses illustrates the value of high-resolution sampling for quantifying seasonal fluxes in desert shrublands and their improvements in closing the water balance in small watersheds.
ContributorsTempleton, Ryan (Author) / Vivoni, Enrique R (Thesis advisor) / Mays, Larry (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2011
Analysis and modeling of residual compounds in process streams from U.S. wastewater treatment plants
Description
The presence of compounds such as pharmaceuticals and personal care products (PPCPs) in the environment is a cause for concern as they exhibit secondary effects on non-target organisms and are also indicative of incomplete removal by wastewater treatment plants (WWTPs) during water reclamation. Analytical methods and predictive models can help inform on the rates at which these contaminants enter the environment via biosolids use or wastewater effluent release to estimate the risk of adverse effects. The goals of this research project were to integrate the results obtained from the two different methods of risk assessment, (a) in silico modeling and (b) experimental analysis. Using a previously published empirical model, influent and effluent concentration ranges were predicted for 10 sterols and validated with peer-reviewed literature. The in silico risk assessment analysis performed for sterols and hormones in biosolids concluded that hormones possess high leaching potentials and that particularly 17-α-ethinyl estradiol (EE2) can pose significant threat to fathead minnows (P. promelas) via leaching from terrestrial depositions of biosolids. Six mega-composite biosolids samples representative of 94 WWTPs were analyzed for a suite of 120 PPCPs using the extended U.S. EPA Method 1694 protocol. Results indicated the presence of 26 previously unmonitored PPCPs in the samples with estimated annual release rates of 5-15 tons yr-1 via land application of biosolids. A mesocosm sampling analysis that was included in the study concluded that four compounds amitriptyline, paroxetine, propranolol and sertraline warrant further monitoring due to their high release rates from land applied biosolids and their calculated extended half-lives in soils. There is a growing interest in the scientific community towards the development of new analytical protocols for analyzing solid matrices such as biosolids for the presence of PPCPs and other established and emerging contaminants of concern. The two studies presented here are timely and an important addition to the increasing base of scientific articles regarding environmental release of PPCPs and exposure risks associated with biosolids land application. This research study emphasizes the need for coupling experimental results with predictive analytical modeling output in order to more fully assess the risks posed by compounds detected in biosolids.
ContributorsPrakash Chari, Bipin (Author) / Halden, Rolf U. (Thesis advisor) / Westerhoff, Paul (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2012
Description
Granular activated carbon (GAC) is effectively used to remove natural organic matter (NOM) and to assist in the removal of disinfection byproducts (DBPs) and their precursors. However, operation of GAC is cost- and labor-intensive due to frequent media replacement. Optimizing the use of GAC is necessary to ensure treatment efficiency while reducing costs. This dissertation presents four strategies to reduce improve GAC usage while reducing formation of DBPs. The first part of this work adopts Rapid Small Scale Tests (RSSCTs) to evaluate removal of molecular weight fractions of NOM, characterized using size exclusion chromatography (SECDOC). Total trihalomethanes (TTHM), haloacetic acids (HAA5) and haloacetonitriles (HAN) formation were quantified after treatment with GAC. Low MW NOM was removed preferentially in the early bed volumes, up until exhaustion of available adsorption sites. DBP formation potential lowered with DOC removal. Chlorination prior to GAC is investigated in the second part of this work as a strategy to increase removal of NOM and DBP precursors. Results showed lower TTHM formation in the effluent of the GAC treatment when pre-chlorination was adopted, meaning this strategy could help optimize and extend the bed life if GAC filters. The third part of this work investigates in-situ GAC regeneration as an alternative to recover adsorption capacity of field-spent GAC that could potentially offer new modes of operation for water treatment facilities while savng costs with reactivation of spent GAC in an external facility. Field-spent GACs were treated with different oxidant solutions and recovery in adsorption capacity was evaluated for NOM and for two micro pollutants. Recovery of GAC adsorption capacity was not satisfactory for most of conditions evaluated. This indicates that in-situ GAC regeneration could be more effective when the adsorbates are present at high concentrations. Lastly, this work investigates the impact of low molecular weight polyDADMAC on N-nitrosodimethylamine (NDMA) formation. Water treatment facilities rely on polyDADMAC as a coagulant aid to comply with NOM removal and turbidity requirements. Since polymer-derived NDMA precursors are not removed by GAC, it is essential to optimize the use and synthesis of polyDADMAC to reduce NDMA precursors during water treatment.
ContributorsFischer, Natalia (Author) / Westerhoff, Paul (Thesis advisor) / Hristovski, Kiril (Committee member) / Fox, Peter (Committee member) / Arizona State University (Publisher)
Created2017
Description
Safe, readily available, and reliable sources of water are an essential component of any municipality’s infrastructure. Phoenix, Arizona, a southwestern city, has among the highest per capita water use in the United States, making it essential to carefully manage its reservoirs. Generally, municipal water bodies are monitored through field sampling. However, this approach is limited spatially and temporally in addition to being costly. In this study, the application of remotely sensed reflectance data from Landsat 7’s Enhanced Thematic Mapper Plus (ETM+) and Landsat 8’s Operational Land Imager (OLI) along with data generated through field-sampling is used to gain a better understanding of the seasonal development of algal communities and levels of suspended particulates in the three main terminal reservoirs supplying water to the Phoenix metro area: Bartlett Lake, Lake Pleasant, and Saguaro Lake. Algal abundances, particularly the abundance of filamentous cyanobacteria, increased with warmer temperatures in all three reservoirs and reached the highest comparative abundance in Bartlett Lake. Prymnesiophytes (the class of algae to which the toxin-producing golden algae belong) tended to peak between June and August, with one notable peak occurring in Saguaro Lake in August 2017 during which time a fish-kill was observed. In the cooler months algal abundance was comparatively lower in all three lakes, with a more even distribution of abundance across algae classes. In-situ data from March 2017 to March 2018 were compared with algal communities sampled approximately ten years ago in each reservoir to understand any possible long-term changes. The findings show that the algal communities in the reservoirs are relatively stable, particularly those of the filamentous cyanobacteria, chlorophytes, and prymnesiophytes with some notable exceptions, such as the abundance of diatoms, which increased in Bartlett Lake and Lake Pleasant. When in-situ data were compared with Landsat-derived reflectance data, two-band combinations were found to be the best-estimators of chlorophyll-a concentration (as a proxy for algal biomass) and total suspended sediment concentration. The ratio of the reflectance value of the red band and the blue band produced reasonable estimates for the in-situ parameters in Bartlett Lake. The ratio of the reflectance value of the green band and the blue band produced reasonable estimates for the in-situ parameters in Saguaro Lake. However, even the best performing two-band algorithm did not produce any significant correlation between reflectance and in-situ data in Lake Pleasant. Overall, remotely-sensed observations can significantly improve our understanding of the water quality as measured by algae abundance and particulate loading in Arizona Reservoirs, especially when applied over long timescales.
ContributorsRussell, Jazmine Barkley (Author) / Neuer, Susanne (Thesis advisor) / Fox, Peter (Committee member) / Myint, Soe (Committee member) / Arizona State University (Publisher)
Created2018
Description
The large-scale anthropogenic emission of carbon dioxide into the atmosphere leads to many unintended consequences, from rising sea levels to ocean acidification. While a clean energy infrastructure is growing, mid-term strategies that are compatible with the current infrastructure should be developed. Carbon capture and storage in fossil-fuel power plants is one way to avoid our current gigaton-scale emission of carbon dioxide into the atmosphere. However, for this to be possible, separation techniques are necessary to remove the nitrogen from air before combustion or from the flue gas after combustion. Metal-organic frameworks (MOFs) are a relatively new class of porous material that show great promise for adsorptive separation processes. Here, potential mechanisms of O2/N2 separation and CO2/N2 separation are explored.
First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
First, a logical categorization of potential adsorptive separation mechanisms in MOFs is outlined by comparing existing data with previously studied materials. Size-selective adsorptive separation is investigated for both gas systems using molecular simulations. A correlation between size-selective equilibrium adsorptive separation capabilities and pore diameter is established in materials with complex pore distributions. A method of generating mobile extra-framework cations which drastically increase adsorptive selectivity toward nitrogen over oxygen via electrostatic interactions is explored through experiments and simulations. Finally, deposition of redox-active ferrocene molecules into systematically generated defects is shown to be an effective method of increasing selectivity towards oxygen.
ContributorsMcIntyre, Sean (Author) / Mu, Bin (Thesis advisor) / Green, Matthew (Committee member) / Lind, Marylaura (Committee member) / Arizona State University (Publisher)
Created2019
Description
Six high-production-volume neonicotinoids were traced through a municipal wastewater treatment plant (WWTP) and engineered wetland located downstream, in a study motivated by reports on these insecticides posing threats to non-target invertebrate species and potentially playing a role in the global honeybee colony collapse disorder. An array of automated samplers was deployed in a five-day monitoring campaign and resultant flow-weighted samples were analyzed by liquid chromatography tandem mass spectrometry (LC-MS/MS) using the isotope dilution method. Concentrations in WWTP influent and effluent were 54.7 ± 2.9 and 48.6 ± 2.7 ng/L for imidacloprid, respectively, and 3.7 ± 0.3 and 1.8 ± 0.1 ng/L for acetamiprid, respectively. A mass balance over the WWTP showed no (p=0.09, CI = 95%) removal of imidacloprid, and 56 ± 6% aqueous removal of acetamiprid. In the constructed wetland downstream, a lack of removal was noted for both imidacloprid (from 54.4 ± 3.4 ng/L to 49.9 ± 14.6 ng/L) and acetamiprid (from 2.00 ± 0.03 ng/L to 2.30 ± 0.21 ng/L). Clothianidin was detected only inconsistently in the WWTP and wetland (>2 to 288 ng/L; 60% detection frequency), whereas thiamethoxam (<10 ng/L), thiacloprid (<2 ng/L), and dinotefuran (<180 ng/L) were not detected at all. Thus, imidacloprid and acetamiprid were identified as recalcitrant sewage constituents (estimated U.S. WWTP discharge of 1920- 4780 kg/y) that persist during conventional wastewater treatment to enter U.S. surface waters at potentially harmful concentrations.
ContributorsSadaria, Akash Mahendra (Author) / Halden, Rolf (Thesis advisor) / Fox, Peter (Committee member) / Popat, Sudeep (Committee member) / Arizona State University (Publisher)
Created2015
Description
Water recovery from impaired sources, such as reclaimed wastewater, brackish groundwater, and ocean water, is imperative as freshwater resources are under great pressure. Complete reuse of urine wastewater is also necessary to sustain life on space exploration missions of greater than one year’s duration. Currently, the Water Recovery System (WRS) used on the National Aeronautics and Space Administration (NASA) shuttles recovers only 70% of generated wastewater.1 Current osmotic processes show high capability to increase water recovery from wastewater. However, commercial reverse osmosis (RO) membranes rapidly degrade when exposed to pretreated urine-containing wastewater. Also, non-ionic small molecules substances (i.e., urea) are very poorly rejected by commercial RO membranes.
In this study, an innovative composite membrane that integrates water-selective molecular sieve particles into a liquid-barrier chemically resistant polymer film is synthetized. This plan manipulates distinctive aspects of the two materials used to create the membranes: (1) the innate permeation and selectivity of the molecular sieves, and (2) the decay-resistant, versatile, and mechanical strength of the liquid-barrier polymer support matrix.
To synthesize the membrane, Linde Type A (LTA) zeolite particles are anchored to the porous substrate, producing a single layer of zeolite particles capable of transporting water through the membrane. Thereafter, coating the chemically resistant latex polymer filled the space between zeolites. Finally, excess polymer was etched from the surface to expose the zeolites to the feed solution. The completed membranes were tested in reverse osmosis mode with deionized water, sodium chloride, and rhodamine solutions to determine the suitability for water recovery.
The main distinguishing characteristics of the new membrane design compared with current composite membrane include: (1) the use of an impermeable polymer broadens the range of chemical resistant polymers that can be used as the polymer matrix; (2) the use of zeolite particles with specific pore size insures the high rejection of the neutral molecules since water is transported through the zeolite rather than the polymer; (3) the use of latex dispersions, environmentally friendly water based-solutions, as the polymer matrix shares the qualities of low volatile organic compound, low cost, and non- toxicity.
In this study, an innovative composite membrane that integrates water-selective molecular sieve particles into a liquid-barrier chemically resistant polymer film is synthetized. This plan manipulates distinctive aspects of the two materials used to create the membranes: (1) the innate permeation and selectivity of the molecular sieves, and (2) the decay-resistant, versatile, and mechanical strength of the liquid-barrier polymer support matrix.
To synthesize the membrane, Linde Type A (LTA) zeolite particles are anchored to the porous substrate, producing a single layer of zeolite particles capable of transporting water through the membrane. Thereafter, coating the chemically resistant latex polymer filled the space between zeolites. Finally, excess polymer was etched from the surface to expose the zeolites to the feed solution. The completed membranes were tested in reverse osmosis mode with deionized water, sodium chloride, and rhodamine solutions to determine the suitability for water recovery.
The main distinguishing characteristics of the new membrane design compared with current composite membrane include: (1) the use of an impermeable polymer broadens the range of chemical resistant polymers that can be used as the polymer matrix; (2) the use of zeolite particles with specific pore size insures the high rejection of the neutral molecules since water is transported through the zeolite rather than the polymer; (3) the use of latex dispersions, environmentally friendly water based-solutions, as the polymer matrix shares the qualities of low volatile organic compound, low cost, and non- toxicity.
ContributorsKhosravi, Afsaneh Khosravi (Author) / Lind, Mary Laura (Thesis advisor) / Dai, Lenore (Committee member) / Green, Matthew (Committee member) / Lin, Jerry (Committee member) / Seo, Don (Committee member) / Arizona State University (Publisher)
Created2016
Description
The objective of this research was to predict the persistence of potential future contaminants in indirect potable reuse systems. In order to accurately estimate the fates of future contaminants in indirect potable reuse systems, results describing persistence from EPI Suite were modified to include sorption and oxidation. The target future contaminants studied were the approximately 2000 pharmaceuticals currently undergoing testing by United States Food and Drug Administration (US FDA). Specific organic substances such as analgesics, antibiotics, and pesticides were used to verify the predicted half-lives by comparing with reported values in the literature. During sub-surface transport, an important component of indirect potable reuse systems, the effects of sorption and oxidation are important mechanisms. These mechanisms are not considered by the quantitative structure activity relationship (QSAR) model predictions for half-lives from EPI Suite. Modifying the predictions from EPI Suite to include the effects of sorption and oxidation greatly improved the accuracy of predictions in the sub-surface environment. During validation, the error was reduced by over 50% when the predictions were modified to include sorption and oxidation. Molecular weight (MW) is an important criteria for estimating the persistence of chemicals in the sub-surface environment. EPI Suite predicts that high MW compounds are persistent since the QSAR model assumes steric hindrances will prevent transformations. Therefore, results from EPI Suite can be very misleading for high MW compounds. Persistence was affected by the total number of halogen atoms in chemicals more than the sum of N-heterocyclic aromatics in chemicals. Most contaminants (over 90%) were non-persistent in the sub-surface environment suggesting that the target future drugs do not pose a significant risk to potable reuse systems. Another important finding is that the percentage of compounds produced from the biotechnology industry is increasing rapidly and should dominate the future production of pharmaceuticals. In turn, pharmaceuticals should become less persistent in the future. An evaluation of indirect potable reuse systems that use reverse osmosis (RO) for potential rejection of the target contaminants was performed by statistical analysis. Most target compounds (over 95%) can be removed by RO based on size rejection and other removal mechanisms.
ContributorsLim, Seung (Author) / Fox, Peter (Thesis advisor) / Abbaszadegan, Morteza (Committee member) / Halden, Rolf (Committee member) / Arizona State University (Publisher)
Created2011
Description
Per- and polyfluoroalkyl substances (PFAS) are anthropogenic chemicals used for a wide variety of products and industrial processes, including being an essential class of chemicals in the fabrication of semiconductors. Proven concerns related to bioaccumulation and toxicity across multiple species have resulted in health advisory and regulatory initiatives for PFAS in drinking and wastewaters. Among impacted users of PFAS, the semiconductor industry is in urgent need of technologies to remove PFAS from water. Specifically, they prefer technologies capable of mineralizing PFAS into inorganic fluoride (F-). The goal of this thesis is to compare the effectiveness of photo- versus electrocatalytic treatment in benchtop reactor systems PFAS in industrial wastewater before selecting one technology to investigate comprehensively. First, a model wastewater was developed based upon semiconductor samples to represent water matrices near where PFAS are used and the aggregate Fab effluent, which were then used in batch catalytic experiments. Second, batch experiments with homogenous photocatalysis (UV/SO32-) were found to be more energy-intensive than heterogeneous catalysis using boron-doped diamond (BDD) electrodes, and the latter approach was then studied in-depth.
During electrocatalysis, longer chain PFAS (C8; PFOA & PFOS) were observed to degrade faster than C6 and C4 PFAS. This study is the first to report near-complete defluorination of not only C8- and C6- PFAS, but also C4-PFAS, in model wastewaters using BDD electrocatalysis, and the first to report such degradation in real Fab wastewater effluents. Based upon differences in PFAS degradation rates observed in single-solute systems containing only C4 PFAS versus multi-solute systems including C4, C6, and C8 PFAS, it was concluded that the surfactant properties of the longer-chain PFAS created surface films on the BDD electrode surface which synergistically enhanced removal of shorter-chain PFAS. The results from batch experiments that serve as the basis of this thesis will be used to assess the chemical byproducts and their associated bioaccumulation and toxicity. This thesis was aimed at developing an efficient method for the degradation of perfluoroalkyl substances from industrial process waters at realistic concentrations.
ContributorsNienhauser, Alec Brockway (Author) / Westerhoff, Paul (Thesis advisor) / Garcia-Segura, Sergi (Committee member) / Thomas, Marylaura (Committee member) / Green, Matthew (Committee member) / Arizona State University (Publisher)
Created2021