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- All Subjects: Chemistry
- Genre: Doctoral Dissertation
- Creators: Arizona State University
- Member of: ASU Electronic Theses and Dissertations
Description
Bioanalytes such as protein, cells, and viruses provide vital information but are inherently challenging to measure with selective and sensitive detection. Gradient separation technologies can provide solutions to these challenges by enabling the selective isolation and pre-concentration of bioanalytes for improved detection and monitoring. Some fundamental aspects of two of these techniques, isoelectric focusing and dielectrophoresis, are examined and novel developments are presented. A reproducible and automatable method for coupling capillary isoelectric focusing (cIEF) and matrix assisted laser desorption/ionization mass spectrometry (MALDI-MS) based on syringe pump mobilization is found. Results show high resolution is maintained during mobilization and &beta-lactoglobulin; protein isoforms differing by two amino acids are resolved. Subsequently, the instrumental advantages of this approach are utilized to clarify the microheterogeneity of serum amyloid P component. Comprehensive, quantitative results support a relatively uniform glycoprotein model, contrary to inconsistent and equivocal observations in several gel isoelectric focusing studies. Fundamental studies of MALDI-MS on novel superhydrophobic substrates yield unique insights towards an optimal interface between cIEF and MALDI-MS. Finally, the fundamentals of isoelectric focusing in an open drop are explored. Findings suggest this could be a robust sample preparation technique for droplet-based microfluidic systems. Fundamental advancements in dielectrophoresis are also presented. Microfluidic channels for dielectrophoretic mobility characterization are designed which enable particle standardization, new insights to be deduced, and future devices to be intelligently designed. Dielectrophoretic mobilities are obtained for 1 µm polystyrene particles and red blood cells under select conditions. Employing velocimetry techniques allows models of particle motion to be improved which in turn improves the experimental methodology. Together this work contributes a quantitative framework which improves dielectrophoretic particle separation and analysis.
ContributorsWeiss, Noah Graham (Author) / Hayes, Mark A. (Thesis advisor) / Garcia, Antonio (Committee member) / Ros, Alexandra (Committee member) / Arizona State University (Publisher)
Created2011
Description
Higher education institutions in the state of Arizona have experienced a reduction in government funding due to the economic challenges the state is facing combined with an ongoing national recession. Three higher education institutions studied are located in Phoenix, Arizona. The three higher education institutions are Phoenix College, Arizona State University and The University of Phoenix. An analysis of documents made public by each institution was conducted and high level administrators at each institution were interviewed to learn about revenue streams currently active and planned. The results of this set of analyses were presented to the leadership team of Phoenix College in a three-hour strategic planning and priority setting meeting. The action research study assisted Phoenix College administrators in gaining knowledge about and initiating action plans to increase revenue through entrepreneurial strategies. Increased funding is necessary to offset reductions in state aid and property tax revenues. Implementing entrepreneurial strategies to increase funding can promote self-reliance and flexibility and can mitigate the damage to institutional mission success that is threatened by reductions in traditional funding. The strategic planning and priority setting exercise conducted at Phoenix College produced three immediate outcomes: it informed the community of practice about entrepreneurial strategies to increase funding that are in use by higher education institutions located in greater Phoenix, Arizona; it influenced the community of practice to examine entrepreneurial revenue streams and; it committed the leadership team to pursuing and enlarging three additional revenue streams.
ContributorsKakar, Casandra Gwen (Author) / Clark, Christopher M. (Thesis advisor) / De Los Santos Jr., Alfredo G. (Committee member) / Giovannini, Eugene (Committee member) / Arizona State University (Publisher)
Created2011
Description
The purpose of this study was to analyze the impact of a context-based teaching approach (STS) versus a more traditional textbook approach on the attitudes and achievement of community college chemistry students. In studying attitudes toward chemistry within this study, I used a 30-item Likert scale in order to study the importance of chemistry in students' lives, the importance of chemistry, the difficulty of chemistry, interest in chemistry, and the usefulness of chemistry for their future career. Though the STS approach students had higher attitude post scores, there was no significant difference between the STS and textbook students' attitude post scores. It was noted that females had higher postattitude scores in the STS group, while males had higher postattitude scores in the textbook group. With regard to postachievement, I noted that males had higher scores in both groups. A correlation existed between postattitude and postachievement in the STS classroom. In summary, while an association between attitude and achievement was found in the STS classroom, teaching approach or sex was not found to influence attitudes, while sex was also not found to influence achievement. These results, overall, suggest that attitudes are not expected to change on the basis of either teaching approach or gender, and that techniques other than changing the teaching approach would need to be used in order to improve the attitudes of students. Qualitative analysis of an online discussion activity on Energy revealed that STS students were able to apply aspects of chemistry in decision making related to socioscientific issues. Additional analysis of interview and written responses provided insight regarding attitudes toward chemistry, with respect to topics of applicability of chemistry to life, difficulties with chemistry, teaching approach for chemistry, and the intent for enrolling in additional chemistry courses. In addition, the surveys of female students brought out subcategories with regard to emotional and professional characteristics of a good teacher, under the category of characteristics of teaching approach. With respect to the category of course experience, subcategories of useful knowledge to solve real-life problems and knowledge for future career were revealed. The differences between the control group females and STS group females with respect to these characteristics was striking and threw insight into how teacher behavior and teaching approach shape student attitudes to chemistry in case of female students.
ContributorsPerkins, Gita (Author) / Baker, Dale R. (Thesis advisor) / Sloane, Finbarr (Committee member) / Marsh, Josephine P (Committee member) / Arizona State University (Publisher)
Created2011
Description
To sustain world preeminence, 21st century university and college leaders in the United States are redesigning their institutions organizationally and culturally to align with the direction of local and global societies and markets. The New American University enterprise model at Arizona State University has become one of the leading organization and cultural redesigns in United States higher education since its inception in 2002. Yet, sustaining a 21st century model such as this one means every individual in the college or university must understand his or her specific role to further progress the new model forward. Therefore, to advance and sustain a 21st century higher education redesign model at a U.S. college or university, it becomes imperative that every master-level professional who works in the academic/student services field at the institution understand his or her specific role in helping to further progress the new model forward. To this end, there is a need to change the way graduate students in higher education/student affairs masters programs are educated to work in the 21st century institution. This change can prepare new professionals to understand these enterprise models and how to integrate them into their practice in order to meet the needs of the institution, local and global societies and markets. The purpose of this action research study is to highlight one program, the ASU M.Ed. Higher and Postsecondary program, and show how graduates from 2007 - 2011 understand New American University concepts and integrate them into professional practice within higher education. Through use of a quantitative approach, this action research study described how the ASU M.Ed. in Higher and Postsecondary program graduate students' understanding of New American University concepts informs their thinking and practice to lead and respond to changes and challenges facing today's 21st century higher education field.
ContributorsAntonucci, Mark J (Author) / Ewing, Kris M (Thesis advisor) / Denke, Mark (Committee member) / Rund, James (Committee member) / Arizona State University (Publisher)
Created2011
Description
This dissertation reports on an action research study that sought to discover how a new WiFi, tablet computing device, the Apple iPad, affected, enhanced, and impacted student engagement in an English Honors course at Scottsdale Community College. The researcher was also the instructor in the two semester, first-year, college composition sequence (English 101/102) in which all 18 students were provided the new Apple iPad tablet computing device. The researcher described how students adapted the Apple iPads to their academic lives, assessed iPad compatibility with current instructional technology systems, and interviewed participating students to document their beliefs about whether iPad activities enhanced the course. At the conclusion of the college composition sequence, 13 students agreed to participate in focus groups to describe how they made use of the iPad and to report on how the iPad influenced their engagement. Among other findings, students reported that there were compatibility problems with current SCC instructional technology systems, that the iPad increased their efficiency in completing informal educational tasks, but that the iPad was not useful for doing word processing and research. Recommendations for future use of the iPad in this course include reducing the number of iPads accessing the WiFi network at the same time, piloting the use of iPad word processing applications, researching more "mobile-friendly" web sites and documents, and developing innovative assignments that take advantage of iPad capabilities.
ContributorsTualla, Larry Tech (Author) / Clark, Christopher M. (Thesis advisor) / De Los Santos Jr., Alfredo G (Thesis advisor) / Young, Lisa C. (Committee member) / Arizona State University (Publisher)
Created2011
Description
Mechanisms for oxygen reduction are proposed for three distinct cases covering two ionic liquids of fundamentally different archetypes and almost thirty orders of magnitude of proton activity. Proton activity is treated both extrinsically by varying the concentration and intrinsically by selecting proton donors with a wide range of aqueous pKa values. The mechanism of oxygen reduction in ionic liquids is introduced by way of the protic ionic liquid (pIL) triethylammonium triflate (TEATf) which shares some similarities with aqueous acid solutions. Oxygen reduction in TEATf begins as the one electron rate limited step to form superoxide, O2*-, which is then rapidly protonated by the pIL cation forming the perhydroxyl radical, HO2*. The perhydroxyl radical is further reduced to peroxidate (HO2-) and hydrogen peroxide in proportions in accordance with their pKa. The reaction does not proceed beyond this point due to the adsorption of the conjugate base triethylammine interfering with the disproportionation of hydrogen peroxide. This work demonstrates that this mechanism is consistent across Pt, Au, Pd, and Ag electrodes. Two related sets of experiments were performed in the inherently aprotic ionic liquid 1-butyl-2,3-dimethylimidazolium triflate (C4dMImTf). The first involved the titration of acidic species of varying aqueous pKa into the IL while monitoring the extent of oxygen reduction as a function of pKa and potential on Pt and glassy carbon (GC) electrodes. These experiments confirmed the greater propensity of Pt to reduce oxygen by its immediate and abrupt transition from one electron reduction to four electron reduction, while oxygen reduction on GC gradually approaches four electron reduction as the potentials were driven more cathodic. The potential at which oxygen reduction initiates shows general agreement with the Nernst equation and the acid's tabulated aqueous pKa value, however at the extremely acidic end, a small deviation is observed. The second set of experiments in C4dMImTf solicited water as the proton donor for oxygen reduction in an approximation of the aqueous alkaline case. The water content was varied between extremely dry (<0.1 mol% H2O) and saturated (approximately 15.8 mol% H2O}). As the water content increased so too did the extent of oxygen reduction eventually approach two electrons on both Pt and GC. However, additional water led to a linear increase in the Tafel slope under enhanced mass transport conditions up to the point of 10 mol% water. This inhibition of oxygen adsorption is the result of the interaction between superoxide and water and more specifically is proposed to be associated with decomposition of theC4dMIm+ cation by hydroxide at the elevated temperatures required for the experiment. Oxygen reduction on both Pt and GC follows Nernstian behavior as the water content is increased. Separate mechanisms for oxygen reduction on Pt and GC are proposed based on the nature of the Nernstian response in these systems.
ContributorsZeller, Robert August (Author) / Friesen, Cody (Thesis advisor) / Sieradzki, Karl (Committee member) / Buttry, Daniel (Committee member) / Arizona State University (Publisher)
Created2011
Description
A major goal of synthetic biology is to recapitulate emergent properties of life. Despite a significant body of work, a longstanding question that remains to be answered is how such a complex system arose? In this dissertation, synthetic nucleic acid molecules with alternative sugar-phosphate backbones were investigated as potential ancestors of DNA and RNA. Threose nucleic acid (TNA) is capable of forming stable helical structures with complementary strands of itself and RNA. This provides a plausible mechanism for genetic information transfer between TNA and RNA. Therefore TNA has been proposed as a potential RNA progenitor. Using molecular evolution, functional sequences were isolated from a pool of random TNA molecules. This implicates a possible chemical framework capable of crosstalk between TNA and RNA. Further, this shows that heredity and evolution are not limited to the natural genetic system based on ribofuranosyl nucleic acids. Another alternative genetic system, glycerol nucleic acid (GNA) undergoes intrasystem pairing with superior thermalstability compared to that of DNA. Inspired by this property, I demonstrated a minimal nanostructure composed of both left- and right-handed mirro image GNA. This work suggested that GNA could be useful as promising orthogonal material in structural DNA nanotechnology.
ContributorsZhang, Su (Author) / Chaut, John C (Thesis advisor) / Ghirlanda, Giovanna (Committee member) / Yan, Hao (Committee member) / Arizona State University (Publisher)
Created2011
Description
In 2005, the Navajo Sovereignty in Education Act was signed into law by the Navajo Nation. Like the No Child Left Behind Act, this Navajo Nation legislation was as much a policy statement as it was a law. It marked the first time that the Navajo Nation linked sovereignty with education by expressing its intent to control all education within its exterior boundaries. The objective of the law was to create a department of education that would resemble the states of Arizona, New Mexico, and Utah in which the Navajo Nation resides. Through their department of education, the Navajo Nation would operate the educational functions for its populace. This study looked at the implications and impact that perspectives of this law would have on public schools within Arizona from the perspective of five superintendents in Arizona public schools within the Navajo Nation were gained through open-ended interviews. It examined the legal, fiscal, and curricular issues through the prism of sovereignty. Through the process of interviews utilizing a set of guided questions in a semi-structured format, five superintendents in Arizona public schools within the Navajo Nation shared their perspectives. Analysis of the five interviews revealed curriculum, funding, jurisdictional, and fear or mistrust as problems the Navajo Nation will need to overcome if it is to begin full control of all aspects of education within its boundaries. There is a strong need for the Department of Dine' Education to educate public schools with regards to the Navajo Nation Sovereignty in Education Act of 2005. Administrators need more training in tribal governments. Like the constitution, the Navajo Sovereignty in Education Act will be interpreted differently by different people. But, without action, it will be ignored. Within the Act's pages are the hopes of the Navajo Nation and the dreams for our young Navajo students.
ContributorsRoessel, Karina A (Author) / Appleton, Nicholas (Thesis advisor) / Spencer, Dee Ann (Thesis advisor) / Wauneka, Jacquelyne (Committee member) / Arizona State University (Publisher)
Created2011
Description
Cellular redox phenomena are essential for the life of organisms. Described here is a summary of the synthesis of a number of redox-cycling therapeutic agents. The work centers on the synthesis of antitumor antibiotic bleomycin congeners. In addition, the synthesis of pyridinol analogues of alpha-tocopherol is also described. The bleomycins (BLMs) are a group of glycopeptide antibiotics that have been used clinically to treat several types of cancers. The antitumor activity of BLM is thought to be related to its degradation of DNA, and possibly RNA. Previous studies have indicated that the methylvalerate subunit of bleomycin plays an important role in facilitating DNA cleavage by bleomycin and deglycobleomycin. A series of methylvalerate analogues have been synthesized and incorporated into deglycobleomycin congeners by the use of solid-phase synthesis. All of the deglycobleomycin analogues were found to effect the relaxation of plasmid DNA. Those analogues having aromatic C4-substituents exhibited cleavage efficiency comparable to that of deglycoBLM A5. Some, but not all, of the deglycoBLM analogues were also capable of mediating sequence-selective DNA cleavage. The second project focused on the synthesis of bicyclic pyridinol analogues of alpha-tocopherol. Bicyclic pyridinol antioxidants have recently been reported to suppress the autoxidation of methyl linoleate more effectively than alpha-tocopherol. However, the complexity of the synthetic routes has hampered their further development as therapeutic agents. Described herein is a concise synthesis of two bicyclic pridinol antioxidants and a facile approach to their derivatives with simple alkyl chains attached to the antioxidant core. These analogues were shown to retain biological activity and exhibit tocopherol-like behaviour.
ContributorsCai, Xiaoqing (Author) / Hecht, Sidney M. (Thesis advisor) / Gould, Ian R (Committee member) / Hartnett, Hilairy E (Committee member) / Arizona State University (Publisher)
Created2011
Description
Natural photosynthesis features a complex biophysical/chemical process that requires sunlight to produce energy rich products. It is one of the most important processes responsible for the appearance and sustainability of life on earth. The first part of the thesis focuses on understanding the mechanisms involved in regulation of light harvesting, which is necessary to balance the absorption and utilization of light energy and in that way reduce the effect caused by photooxidative damage. In photosynthesis, carotenoids are responsible not only for collection of light, but also play a major role in protecting the photosynthetic system. To investigate the role of carotenoids in the quenching of the excited state of cyclic tetrapyrroles, two sets of dyads were studied. Both sets of dyads contain zinc phthalocyanine (Pc) covalently attached to carotenoids of varying conjugation lengths. In the first set of dyads, carotenoids were attached to the phthalocyanine via amide linkage. This set of dyads serves as a good model for understanding the molecular "gear-shift" mechanism, where the addition of one double bond can turn the carotenoid from a nonquencher to a very strong quencher of the excited state of a tetrapyrrole. In the second set of dyads, carotenoids were attached to phthalocyanine via a phenyl amino group. Two independent studies were performed on these dyads: femtosecond transient absorption and steady state fluorescence induced by two-photon excitation. In the transient absorption study it was observed that there is an instantaneous population of the carotenoid S1 state after Pc excitation, while two-photon excitation of the optically forbidden carotenoid S1 state shows 1Pc population. Both observations provide a strong indication of the existence of a shared excitonic state between carotenoid and Pc. Similar results were observed in LHC II complexes in plants, supporting the role of such interactions in photosynthetic down regulation. In the second chapter we describe the synthesis of porphyrin dyes functionalized with carboxylate and phosphonate anchoring groups to be used in the construction of photoelectrochemical cells containing a porphyrin-IrO2·nH2O complex immobilized on a TiO2 electrode. The research presented here is a step in the development of high potential porphyrin-metal oxide complexes to be used in the photooxidation of water. The last chapter focuses on developing synthetic strategies for the construction of an artificial antenna system consisting of porphyrin-silver nanoparticle conjugates, linked by DNA of varied length to study the distance dependence of the interaction between nanoparticles and the porphyrin chromophore. Preliminary studies indicate that at the distance of about 7-10 nm between porphyrin and silver nanoparticle is where the porphyrin absorption leading to fluorescence shows maximum enhancement. These new hybrid constructs will be helpful for designing efficient light harvesting systems.
ContributorsPillai, Smitha (Author) / Moore, Ana (Thesis advisor) / Moore, Thomas (Committee member) / Gould, Ian (Committee member) / Arizona State University (Publisher)
Created2011