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- Creators: Mozart, Wolfgang Amadeus, 1756-1791
Description
On average, our society generates ~0.5 ton of municipal solid waste per person annually. Biomass waste can be gasified to generate synthesis gas (syngas), a gas mixture consisting predominantly of CO, CO2, and H2. Syngas, rich in carbon and electrons, can fuel the metabolism of carboxidotrophs, anaerobic microorganisms that metabolize CO (a toxic pollutant) and produce biofuels (H2, ethanol) and commodity chemicals (acetate and other fatty acids). Despite the attempts for commercialization of syngas fermentation by several companies, the metabolic processes involved in CO and syngas metabolism are not well understood. This dissertation aims to contribute to the understanding of CO and syngas fermentation by uncovering key microorganisms and understanding their metabolism. For this, microbiology and molecular biology techniques were combined with analytical chemistry analyses and deep sequencing techniques. First, environments where CO is commonly detected, including the seafloor, volcanic sand, and sewage sludge, were explored to identify potential carboxidotrophs. Since carboxidotrophs from sludge consumed CO 1000 faster than those in nature, mesophilic sludge was used as inoculum to enrich for CO- and syngas- metabolizing microbes. Two carboxidotrophs were isolated from this culture: an acetate/ethanol-producer 99% phylogenetically similar to Acetobacterium wieringae and a novel H2-producer, Pleomorphomonas carboxidotrophicus sp. nov. Comparison of CO and syngas fermentation by the CO-enriched culture and the isolates suggested mixed-culture syngas fermentation as a better alternative to ferment CO-rich gases. Advantages of mixed cultures included complete consumption of H2 and CO2 (along with CO), flexibility under different syngas compositions, functional redundancy (for acetate production) and high ethanol production after providing a continuous supply of electrons. Lastly, dilute ethanol solutions, typical of syngas fermentation processes, were upgraded to medium-chain fatty acids (MCFA), biofuel precursors, through the continuous addition of CO. In these bioreactors, methanogens were inhibited and Peptostreptococcaceae and Lachnospiraceae spp. most likely partnered with carboxidotrophs for MCFA production. These results reveal novel microorganisms capable of effectively consuming an atmospheric pollutant, shed light on the interplay between syngas components, microbial communities, and metabolites produced, and support mixed-culture syngas fermentation for the production of a wide variety of biofuels and commodity chemicals.
ContributorsEsquivel Elizondo, Sofia Victoria (Author) / Krajmalnik-Brown, Rosa (Thesis advisor) / Rittmann, Bruce E. (Committee member) / Delgado, Anca G. (Committee member) / Torres, Cesar I. (Committee member) / Arizona State University (Publisher)
Created2017
Description
Organic electronics have remained a research topic of great interest over the past few decades, with organic light emitting diodes (OLEDs) emerging as a disruptive technology for lighting and display applications. While OLED performance has improved significantly over the past decade, key issues remain unsolved such as the development of stable and efficient blue devices. In order to further the development of OLEDs and increase their commercial potential, innovative device architectures, novel emissive materials and high-energy hosts are designed and reported.
OLEDs employing step-wide graded-doped emissive layers were designed to improve charge balance and center the exciton formation zone leading to improved device performance. A red OLED with a peak efficiency of 16.9% and an estimated LT97 over 2,000 hours at 1,000 cd/m2 was achieved. Employing a similar structure, a sky-blue OLED was demonstrated with a peak efficiency of 17.4% and estimated LT70 over 1,300 hours at 1,000 cd/m2. Furthermore, the sky-blue OLEDs color was improved to CIE coordinates of (0.15, 0.25) while maintaining an efficiency of 16.9% and estimated LT70 over 600 hours by incorporating a fluorescent sensitizer. These devices represent literature records at the time of publication for efficient and stable platinum phosphorescent OLEDs.
A newly developed class of emitters, metal-assisted delayed-fluorescence (MADF), are demonstrated to achieve higher-energy emission from a relatively low triplet energy. A green MADF device reaches a peak efficiency of 22% with an estimated LT95 over 350 hours at 1,000 cd/m2. Additionally, a blue charge confined OLED of PtON1a-tBu demonstrated a peak efficiency above 20%, CIE coordinated of (0.16, 0.27), and emission onset at 425 nm.
High triplet energy hosts are required for the realization of stable and efficient deep blue emission. A rigid “M”-type carbazole/fluorene hybrid called mDCzPF and a carbazole/9-silafluorene hybrid called mDCzPSiF are demonstrated to have high triplet energies ET=2.88 eV and 3.03 eV respectively. Both hosts are demonstrated to have reasonable stability and can serve as a template for future material design. The techniques presented here demonstrate alternative approaches for improving the performance of OLED devices and help to bring this technology closer to widespread commercialization.
OLEDs employing step-wide graded-doped emissive layers were designed to improve charge balance and center the exciton formation zone leading to improved device performance. A red OLED with a peak efficiency of 16.9% and an estimated LT97 over 2,000 hours at 1,000 cd/m2 was achieved. Employing a similar structure, a sky-blue OLED was demonstrated with a peak efficiency of 17.4% and estimated LT70 over 1,300 hours at 1,000 cd/m2. Furthermore, the sky-blue OLEDs color was improved to CIE coordinates of (0.15, 0.25) while maintaining an efficiency of 16.9% and estimated LT70 over 600 hours by incorporating a fluorescent sensitizer. These devices represent literature records at the time of publication for efficient and stable platinum phosphorescent OLEDs.
A newly developed class of emitters, metal-assisted delayed-fluorescence (MADF), are demonstrated to achieve higher-energy emission from a relatively low triplet energy. A green MADF device reaches a peak efficiency of 22% with an estimated LT95 over 350 hours at 1,000 cd/m2. Additionally, a blue charge confined OLED of PtON1a-tBu demonstrated a peak efficiency above 20%, CIE coordinated of (0.16, 0.27), and emission onset at 425 nm.
High triplet energy hosts are required for the realization of stable and efficient deep blue emission. A rigid “M”-type carbazole/fluorene hybrid called mDCzPF and a carbazole/9-silafluorene hybrid called mDCzPSiF are demonstrated to have high triplet energies ET=2.88 eV and 3.03 eV respectively. Both hosts are demonstrated to have reasonable stability and can serve as a template for future material design. The techniques presented here demonstrate alternative approaches for improving the performance of OLED devices and help to bring this technology closer to widespread commercialization.
ContributorsKlimes, Kody George (Author) / Li, Jian (Thesis advisor) / Adams, James (Committee member) / Wang, Liping (Committee member) / Arizona State University (Publisher)
Created2019
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
This dissertation critically evaluated methodologies and devices for assessing and protecting the health of human populations, with particular emphasis on groundwater remediation and the use of wastewater-based epidemiology (WBE) to inform population health. A meta-analysis and assessment of laboratory-scale treatability studies for removing chlorinated solvents from groundwater found that sediment microcosms operated as continuous-flow columns are preferable to batch bottles when seeking to emulate with high fidelity the complex conditions prevailing in the subsurface in contaminated aquifers (Chapter 2). Compared to monitoring at the field-scale, use of column microcosms also showed (i) improved chemical speciation, and (ii) qualitative predictability of field parameters (Chapter 3). Monitoring of glucocorticoid hormones in wastewater of a university campus showed (i) elevated stress levels particularly at the start of the semester, (ii) on weekdays relative to weekend days (p = 0.05) (161 ± 42 μg d-1 per person, 122 ± 54 μg d-1 per person; p ≤ 0.05), and (iii) a positive association between levels of stress hormones and nicotine (rs: 0.49) and caffeine (0.63) consumption in this student population (Chapter 4). Also, (i) alcohol consumption determined by WBE was in line with literature estimates for this young sub-population (11.3 ± 7.5 g d-1 per person vs. 10.1 ± 0.8 g d-1 per person), whereas caffeine and nicotine uses were below (114 ± 49 g d-1 per person, 178 ± 19 g d-1 per person; 627 ± 219 g d-1 per person, 927 ± 243 g d-1 per person). The introduction of a novel continuous in situ sampler to WBE brought noted benefits relative to traditional time-integrated sampling, including (i) a higher sample coverage (93% vs. 3%), (ii) an ability to captured short-term analyte pulses (e.g., heroin, fentanyl, norbuprenorphine, and methadone), and (iii) an overall higher mass capture for drugs of abuse like morphine, fentanyl, methamphetamine, amphetamine, and the opioid antagonist metabolite norbuprenorphine (p ≤ 0.01). Methods and devices developed in this work are poised to find applications in the remediation sector and in human health assessments.
ContributorsDriver, Erin Michelle (Author) / Halden, Rolf (Thesis advisor) / Conroy-Ben, Otakuye (Committee member) / Kavazanjian, Edward (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Arizona State University (Publisher)
Created2018
Description
Widespread use of chlorinated solvents for commercial and industrial purposes makes co-occurring contamination by 1,1,1-trichloroethane (TCA), trichloroethene (TCE), and 1,4-dioxane (1,4-D) a serious problem for groundwater. TCE and TCA often are treated by reductive dechlorination, while 1,4-D resists reductive treatment. Aerobic bacteria are able to oxidize 1,4-D, but the biological oxidation of 1,4-D could be inhibited TCA, TCE, and their reductive transformation products. To overcome the challenges from co-occurring contamination, I propose a two-stage synergistic system. First, anaerobic reduction of the chlorinated hydrocarbons takes place in a H2-based hollow-fiber “X-film” (biofilm or catalyst-coated film) reactor (MXfR), where “X-film” can be a “bio-film” (MBfR) or an abiotic “palladium-film” (MPfR). Then, aerobic removal of 1,4-D and other organic compounds takes place in an O2-based MBfR. For the reductive part, I tested reductive bio-dechlorination of TCA and TCE simultaneously in an MBfR. I found that the community of anaerobic bacteria can rapidly reduce TCE to cis-dichloroethene (cis-DCE), but further reductions of cis-DCE to vinyl chloride (VC) and VC to ethene were inhibited by TCA. Also, it took months to grow a strong biofilm that could reduce TCA and TCE. Another problem with reductive dechlorination in the MBfR is that mono-chloroethane (MCA) was not reduced to ethane. In contrast, a film of palladium nano-particles (PdNPs), i.e., an MPfR, could the simultaneous reductions of TCA and TCE to mainly ethane, with only small amounts of intermediates: 1,1-dichloroethane (DCA) (~3% of total influent TCA and TCE) and MCA (~1%) in continuous operation. For aerobic oxidation, I enriched an ethanotrophic culture that could oxidize 1,4-D with ethane as the primary electron donor. An O2-based MBfR, inoculated with the enriched ethanotrophic culture, achieved over 99% 1,4-D removal with ethane as the primary electron donor in continuous operation. Finally, I evaluated two-stage treatment with a H2-based MPfR followed by an O2-MBfR. The two-stage system gave complete removal of TCA, TCE, and 1,4-D in continuous operation.
ContributorsLuo, Yihao (Author) / Rittmann, Bruce E. (Committee member) / Krajmalnik-Brown, Rosa (Committee member) / Zhou, Chen (Committee member) / Arizona State University (Publisher)
Created2018
Description
As the prevalence and awareness of Autism Spectrum Disorder (ASD) increases, so does the variety of treatment options for primary symptoms (social interaction, communication, behavior) and secondary symptoms (anxiety, hyperactivity, GI problems, and insomnia). Various treatments, from Adderall to Citalopram to Flax Seed Oil promise relief for these symptoms. However, very little research has actually been done on some of these treatments. Additionally, the research that has been done fails to compare these treatments against one another in terms of symptom relief. The Autism Treatment Effectiveness Survey, written by Dr. James Adams, director of the Autism/Asperger's Research Program at ASU, and graduate student/program coordinator Devon Coleman, aims to fill this gap. The survey numerically rates medications based on benefit and adverse effects, in addition to naming specific symptoms that are impacted by the treatments. However, the survey itself was retrospective in nature and requires further evidence to support its claims. Therefore, the purpose of this research paper is to evaluate evidence related to the results of the survey. After the performing an extensive literature review of over 70 different treatments, it appears that the findings of the Autism Treatment Effectiveness Survey are generally well supported. There were a few minor discrepancies regarding the primary benefitted symptom, but there was not enough of a conflict to discount the information from the survey. As research is still ongoing, conclusions cannot yet be drawn for Nutritional Supplements, although the current data looks promising.
ContributorsAnderson, Amy Lynn (Author) / Adams, James (Thesis director) / Coleman, Devon (Committee member) / School of Nutrition and Health Promotion (Contributor) / W.P. Carey School of Business (Contributor) / Barrett, The Honors College (Contributor)
Created2018-05
Description
The vastly growing field of supercomputing is in dire need of a new measurement system to optimize JMRAM (Josephson junction magnetoresistive random access memory) devices. To effectively measure these devices, an ultra-low-noise, low cost cryogenic dipping probe with a dynamic voltage range is required. This dipping probe has been designed by ASU with <100 nVp-p noise, <10 nV offsets, 10 pV to 16 mV voltage range, and negligible thermoelectric drift. There is currently no other research group or company that can currently match both these low noise levels and wide voltage range. Two different dipping probes can be created with these specifications: one for high-use applications and one for low-use applications. The only difference between these probes is the outer shell; the high-use application probe has a shell made of G-10 fiberglass for a higher price, and the low-use application probe has a shell made of AISI 310 steel for a lower price. Both types of probes can be assembled in less than 8 hours for less than $2,500, requiring only soldering expertise. The low cost and short time to create these probes makes wide profit margins possible. The market for these cryogenic dipping probes is currently untapped, as most research groups and companies that use these probes build their own, which allows for rapid business growth. These potential consumers can be easily reached by marketing these probes at superconducting conferences. After several years of selling >50 probes, mass production can easily become possible by hiring several technicians, and still maintaining wide profit margins.
ContributorsHudson, Brooke Ashley (Author) / Adams, James (Thesis director) / Anwar, Shahriar (Committee member) / Materials Science and Engineering Program (Contributor) / W. P. Carey School of Business (Contributor) / Barrett, The Honors College (Contributor)
Created2016-05
Description
The goal of the paper was to examine the fatigue mechanisms of polymers and silicone based elastomers. The mechanisms of fatigue due to crazing: the alignment of polymer chains to the stress axis, and shear banding: the localized orientation of the polymer by the shear stresses from two planes, were discussed in depth in this paper. Crazing only occurs in tensile stress, is initiated on the surface of the material, and only occurs in brittle polymers. Crazing also accounts for a 40-60% decrease in density, causing localized weakening of the material and a concentration in stress. This is due to a decrease in effective cross sectional area. The mechanism behind discontinuous growth bands was also discussed to be the cause of cyclic crazing. Shear banding only occurs in ductile polymers and can result in the failure of polymers via necking. Furthermore, the high fatigue resistance of silicone elastomers was discussed in this paper. This conclusion was made because of the lack of fatigue mechanisms (crazing, discontinuous growth bands, and shears banding) in the observed elastomer's microstructure after the samples had undergone fatigue tests. This was done through an analysis of room temperature vulcanized silicone adhesives, a heat-curing silicone elastomer, and a self-curing transparent silicone rubber. Fatigue of room temperature vulcanized silicon was observed, however this was reasoned to be the failure of the adhesion of the elastomer to the steel substrate instead of the microstructure itself. Additionally, the significance of fatigue in real world applications was discussed using SouthWest Airlines Flight 812 as an example.
ContributorsWong, Christopher Stanley (Author) / Adams, James (Thesis director) / Krause, Stephen (Committee member) / Anwar, Shahriar (Committee member) / Materials Science and Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2016-05
Description
Vitamins and minerals are, by definition, essential substances that are necessary for good health, and needed by every cell and organ to function appropriately. A deficiency of any one vitamin or mineral can be very serious. Although a very healthy diet rich in vegetables, fruits, and protein can provide sufficient amounts of most vitamins and minerals, many people do not consume an adequate diet. During pregnancy, there is an increased need for vitamins and minerals to promote a healthy pregnancy and a healthy baby. Prenatal supplements are intended to supplement a normal diet to ensure that adequate amounts of vitamins and minerals are consumed. The US Food and Drug Administration (FDA) has established Recommended Dietary Allowances for total vitamin/mineral intake from food and supplements, but they have not established recommendations for prenatal supplements. Therefore, there is a very wide variation in the content and quality of prenatal supplements. Many prenatal supplements contain only minimal levels of some vitamins and few or no minerals, in order to minimize cost and the number of pills. This results in insufficient vitamin/mineral supplementation for many women, and hence does not fully protect them or their children from pregnancy complications and health problems. Therefore, we have created our own set of recommendations for prenatal supplements. Our recommendations are based primarily on four sources: 1) FDA's Recommended Daily Allowances for pregnant women, which are estimated to meet the needs of 97.5% of healthy pregnant women. 2) FDA's Tolerable Upper Limit, which is the maximum amount of vitamins/minerals that can be safely consumed without any risk of health problems. 3) National Health and Nutrition Examination Survey (NHANES), which evaluates the average intake of vitamins and minerals by women ages 20-40 years in the US 4) Research studies on vitamin/mineral deficiencies or vitamin/mineral supplementation during pregnancy, and the effect on pregnancy, birth, and child health problems. In summary, the RDA establishes minimum recommended levels of vitamin/mineral intake from all sources, and the NHANES establishes the average intake from foods. The difference is what needs to be consumed in a supplement, on average. However, since people vary greatly in the quality of their diet, and since most vitamins and minerals have a high Tolerable Upper Limit, we generally recommend more than the difference between the RDA and the average NHANES. Vitamins generally have a larger Tolerable Upper Limit than do minerals. So, we recommend that prenatal vitamin/mineral supplements contain 100% of the RDA for most vitamins, and about 50% of the RDA for most minerals. However, based on additional research studies described below, in some cases we vary our recommendations from those averages.
ContributorsSorenson, Jacob (Author) / Adams, James (Thesis director) / Pollard, Elena (Committee member) / College of Integrative Sciences and Arts (Contributor) / Barrett, The Honors College (Contributor)
Created2017-05
Description
The purpose of this honors project is to analyze the difference between different powder separation techniques, and their suitability for my capstone project – ‘Effect of Powder Reuse on DMLS (Direct Metal Laser Sintering) Product Integrity’. Due to the nature of my capstone project, my group needs to characterize foreign contaminants in IN 718 (Ni-based superalloy) powder with a mean diameter around 40um. In order to clearly analyze the contaminants and recycle useful IN 718 powders, powder separation is favorable since the filtered samples will be much easier to characterize rather than inspect all the powders at once under microscope. By conducting literature review, I found that powder separation is commonly used in Geology, and Chemistry department. To screen which combination of techniques could be the best for my project, I have consulted several research specialists, obtained adequate knowledge about powder separation. Accordingly, I will summarize the pros and cons of each method with regard the specific project that I am working on, and further explore the impacts of each method under economical, societal, and environmental considerations. Several powder separation techniques will be discussed in details in the following sections, including water elutriation, settling column, magnetic separation and centrifugation. In addition to these methods, sieving, water tabling and panning will be briefly introduced. After detailed comparison, I found that water elutriation is the most efficient way to purity IN718 powder for reuse purpose, and recovery rate is as high as 70%, which could result in a significant reduction in the manufacturing cost for Honeywell since currently Honeywell only use virgin powders to build parts, and 90% of the leftover powders are discarded.
ContributorsLuo, Zheyu (Author) / Adams, James (Thesis director) / Tasooji, Amaneh (Committee member) / Materials Science and Engineering Program (Contributor) / School of Sustainability (Contributor) / Barrett, The Honors College (Contributor)
Created2016-05