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- Genre: Doctoral Dissertation
- Resource Type: Text
- Status: Published
Description
Emission of CO2 into the atmosphere has become an increasingly concerning issue as we progress into the 21st century Flue gas from coal-burning power plants accounts for 40% of all carbon dioxide emissions. The key to successful separation and sequestration is to separate CO2 directly from flue gas (10-15% CO2, 70% N2), which can range from a few hundred to as high as 1000°C. Conventional microporous membranes (carbons/silicas/zeolites) are capable of separating CO2 from N2 at low temperatures, but cannot achieve separation above 200°C. To overcome the limitations of microporous membranes, a novel ceramic-carbonate dual-phase membrane for high temperature CO2 separation was proposed. The membrane was synthesized from porous La0.6Sr0.4Co0.8Fe0.2O3-d (LSCF) supports and infiltrated with molten carbonate (Li2CO3/Na2CO3/K2CO3). The CO2 permeation mechanism involves a reaction between CO2 (gas phase) and O= (solid phase) to form CO3=, which is then transported through the molten carbonate (liquid phase) to achieve separation. The effects of membrane thickness, temperature and CO2 partial pressure were studied. Decreasing thickness from 3.0 to 0.375 mm led to higher fluxes at 900°C, ranging from 0.186 to 0.322 mL.min-1.cm-2 respectively. CO2 flux increased with temperature from 700 to 900°C. Activation energy for permeation was similar to that for oxygen ion conduction in LSCF. For partial pressures above 0.05 atm, the membrane exhibited a nearly constant flux. From these observations, it was determined that oxygen ion conductivity limits CO2 permeation and that the equilibrium oxygen vacancy concentration in LSCF is dependent on the partial pressure of CO2 in the gas phase. Finally, the dual-phase membrane was used as a membrane reactor. Separation at high temperatures can produce warm, highly concentrated streams of CO2 that could be used as a chemical feedstock for the synthesis of syngas (H2 + CO). Towards this, three different membrane reactor configurations were examined: 1) blank system, 2) LSCF catalyst and 3) 10% Ni/y-alumina catalyst. Performance increased in the order of blank system < LSCF catalyst < Ni/y-alumina catalyst. Favorable conditions for syngas production were high temperature (850°C), low sweep gas flow rate (10 mL.min-1) and high methane concentration (50%) using the Ni/y-alumina catalyst.
ContributorsAnderson, Matthew Brandon (Author) / Lin, Jerry (Thesis advisor) / Alford, Terry (Committee member) / Rege, Kaushal (Committee member) / Anderson, James (Committee member) / Rivera, Daniel (Committee member) / Arizona State University (Publisher)
Created2011
Description
A relatively simple subset of nanotechnology - nanofluids - can be obtained by adding nanoparticles to conventional base fluids. The promise of these fluids stems from the fact that relatively low particle loadings (typically <1% volume fractions) can significantly change the properties of the base fluid. This research explores how low volume fraction nanofluids, composed of common base-fluids, interact with light energy. Comparative experimentation and modeling reveals that absorbing light volumetrically (i.e. in the depth of the fluid) is fundamentally different from surface-based absorption. Depending on the particle material, size, shape, and volume fraction, a fluid can be changed from being mostly transparent to sunlight (in the case of water, alcohols, oils, and glycols) to being a very efficient volumetric absorber of sunlight. This research also visualizes, under high levels of irradiation, how nanofluids undergo interesting, localized phase change phenomena. For this, images were taken of bubble formation and boiling in aqueous nanofluids heated by a hot wire and by a laser. Infrared thermography was also used to quantify this phenomenon. Overall, though, this research reveals the possibility for novel solar collectors in which the working fluid directly absorbs light energy and undergoes phase change in a single step. Modeling results indicate that these improvements can increase a solar thermal receiver's efficiency by up to 10%.
ContributorsTaylor, Robert (Author) / Phelan, Patrick E (Thesis advisor) / Adrian, Ronald (Committee member) / Trimble, Steve (Committee member) / Posner, Jonathan (Committee member) / Maracas, George (Committee member) / Arizona State University (Publisher)
Created2011
Description
Customers today, are active participants in service experiences. They are more informed about product choices, their preferences and tend to actively influence customer and firm related outcomes. However, differences across customers become a significant challenge for firms trying to ensure that all customers have a `delightful' consumption experience. This dissertation studies customers as active participants in service experiences and considers three dimensions of customer participation -- in-role performance; extra-role performance-citizenship and elective behavior; and information sharing -- as its focal dependent variables. This study is grounded in services marketing, customer co-production and motivation literatures. The theoretical model proposes that customer behaviors are goal-directed and different consumers will have different reactions to the service quality because they have different assessments of progress towards their goals and (consequently) different levels of participation during the service experience. Customer role clarity and participation behavior will also influence the service experience and firm outcomes. A multi-step process was adopted to test the conceptual model, beginning with qualitative and quantitative pretests; followed by 2 studies (one cross-sectional and other longitudinal in nature). Results prove that customer participation behaviors are influenced by service quality directly and through the mediated path of progress towards goals. Assessment of progress towards goals directly influences customer participation behaviors cross-sectionally. Service quality from one service interaction influences customer in-role performance and information sharing in subsequent service interactions. Information sharing influences service quality in subsequent service interactions. Role-clarity influences in-role and extra-role performance cross-sectionally and influences these behaviors longitudinally only in the early stages of the customer-firm relationship. Due to multi-collinearity, the moderating effect of customer goals on assessment of progress towards goals could not be tested. The study findings contribute to the understanding of customer participation behaviors in service interactions for both academics and managers. It contributes to the literature by examining consumption during the service interaction; considering customers as active participants; explaining differences in customer participation; integrating a forward-looking component (assessment of progress towards goals) and a retrospective component (perceptions of service quality) to explain customer participation behaviors over time; defining and building measures for customer participation behavior.
ContributorsSaxena, Shruti (Author) / Mokwa, Michael (Thesis advisor) / Bitner, Mary Jo (Committee member) / Bolton, Ruth N (Committee member) / Olsen, Grant D (Committee member) / Arizona State University (Publisher)
Created2010
Description
This research examines the effects of using similar vs. dissimilar models in health messages on message compliance. I find that level of self-awareness moderates the effect of model similarity on message compliance. Across three studies, I demonstrate that when self-awareness is high, a health message that contains a similar model leads to higher compliance than the same message containing a dissimilar model. On the other hand, when self-awareness is low, a health message that contains a similar model leads to lower message compliance than the same message containing a dissimilar model. Additionally, I demonstrate that the increased compliance observed when self-awareness is high and a similar model is used is associated with self-enhancing behavior and increased engagement with the ad, while the decreased compliance observed when self-awareness is low and a similar model is used is associated with disregarding the ad.
ContributorsLoveland, Katherine (Author) / Mandel, Naomi (Thesis advisor) / Miller, Elizabeth G. (Committee member) / Morales, Andrea C. (Committee member) / Smeesters, Dirk (Committee member) / Arizona State University (Publisher)
Created2011
Description
The electrode-electrolyte interface in electrochemical environments involves the understanding of complex processes relevant for all electrochemical applications. Some of these processes include electronic structure, charge storage, charge transfer, solvent dynamics and structure and surface adsorption. In order to engineer electrochemical systems, no matter the function, requires fundamental intuition of all the processes at the interface. The following work presents different systems in which the electrode-electrolyte interface is highly important. The first is a charge storage electrode utilizing percolation theory to develop an electrode architecture producing high capacities. This is followed by Zn deposition in an ionic liquid in which the deposition morphology is highly dependant on the charge transfer and surface adsorption at the interface. Electrode Architecture: A three-dimensional manganese oxide supercapacitor electrode architecture is synthesized by leveraging percolation theory to develop a hierarchically designed tri-continuous percolated network. The three percolated phases include a faradaically-active material, electrically conductive material and pore-former templated void space. The micropores create pathways for ionic conductivity, while the nanoscale electrically conducting phase provides both bulk conductivity and local electron transfer with the electrochemically active phase. Zn Electrodeposition: Zn redox in air and water stable N-ethyl-N-methylmorpholinium bis(trifluoromethanesulfonyl)imide, [C2nmm][NTf2] is presented. Under various conditions, characterization of overpotential, kinetics and diffusion of Zn species and morphological evolution as a function of overpotential and Zn concentration are analyzed. The surface stress evolution during Zn deposition is examined where grain size and texturing play significant rolls in compressive stress generation. Morphological repeatability in the ILs led to a novel study of purity in ionic liquids where it is found that surface adsorption of residual amine and chloride from the organic synthesis affect growth characteristics. The drivers of this work are to understand the processes occurring at the electrode-electrolyte interface and with that knowledge, engineer systems yielding optimal performance. With this in mind, the design of a bulk supercapacitor electrode architecture with excellent composite specific capacitances, as well as develop conditions producing ideal Zn deposition morphologies was completed.
ContributorsEngstrom, Erika (Author) / Friesen, Cody (Thesis advisor) / Buttry, Daniel (Committee member) / Sieradzki, Karl (Committee member) / Arizona State University (Publisher)
Created2011
Description
The marketing and development of solutions has become an increasingly important concept in both marketing practice and theory. Recent conceptual work has defined solutions as sets of products and services that allow customers to achieve customized outcomes. Although the definition of a solution is becoming clearer, the process through which solution value is generated is still opaque. The purpose of this study was to add clarity to both marketing theory and practice by examining the solution value co-creation process in depth. Service-dominant logic, the relational view, service value co-creation, and theories of organizational learning and knowledge were the basis for this examination. Social capital was also examined to determine how these important relational concepts are involved in solution development. The study was conducted in four separate phases using a multi-method approach of quantitative surveys, qualitative surveys, and depth interviews. A large, multinational educational firm provided the context for the study which included access to their solution sales force and customer base. Quantitative data was collected from 97 key informants across 182 different customer opportunities for both new and existing solution engagements. Qualitative data was also collected from 71 respondents to provide a mixed-method triangulation of how solution value is created. Overall, the study provided strong support to the idea that knowledge sharing between solution providers and their customers plays a pivotal role in the co-creation of solution value.
ContributorsSellman, Collin (Author) / Hutt, Michael (Thesis advisor) / Kumar, Ajith (Committee member) / Walker, Beth (Committee member) / Arizona State University (Publisher)
Created2011
Description
Lipids and free fatty acids (FFA) from cyanobacterium Synechocystis can be used for biofuel (e.g. biodiesel or renewable diesel) production. In order to utilize and scale up this technique, downstream processes including culturing and harvest, cell disruption, and extraction were studied. Several solvents/solvent systems were screened for lipid extraction from Synechocystis. Chloroform + methanol-based Folch and Bligh & Dyer methods were proved to be "gold standard" for small-scale analysis due to their highest lipid recoveries that were confirmed by their penetration of the cell membranes, higher polarity, and stronger interaction with hydrogen bonds. Less toxic solvents, such as methanol and MTBE, or direct transesterification of biomass (without pre-extraction step) gave only slightly lower lipid-extraction yields and can be considered for large-scale application. Sustained exposure to high and low temperature extremes severely lowered the biomass and lipid productivity. Temperature stress also triggered changes of lipid quality such as the degree of unsaturation; thus, it affected the productivities and quality of Synechocystis-derived biofuel. Pulsed electric field (PEF) was evaluated for cell disruption prior to lipid extraction. A treatment intensity > 35 kWh/m3 caused significant damage to the plasma membrane, cell wall, and thylakoid membrane, and it even led to complete disruption of some cells into fragments. Treatment by PEF enhanced the potential for the low-toxicity solvent isopropanol to access lipid molecules during subsequent solvent extraction, leading to lower usage of isopropanol for the same extraction efficiency. Other cell-disruption methods also were tested. Distinct disruption effects to the cell envelope, plasma membrane, and thylakoid membranes were observed that were related to extraction efficiency. Microwave and ultrasound had significant enhancement of lipid extraction. Autoclaving, ultrasound, and French press caused significant release of lipid into the medium, which may increase solvent usage and make medium recycling difficult. Production of excreted FFA by mutant Synechocystis has the potential of reducing the complexity of downstream processing. Major problems, such as FFA precipitation and biodegradation by scavengers, account for FFA loss in operation. Even a low concentration of FFA scavengers could consume FFA at a high rate that outpaced FFA production rate. Potential strategies to overcome FFA loss include high pH, adsorptive resin, and sterilization techniques.
ContributorsSheng, Chieh (Author) / Rittmann, Bruce E. (Thesis advisor) / Westerhoff, Paul (Committee member) / Vermaas, Willem (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
We apply a Bayesian network-based approach for determining the structure of consumers' brand concept maps, and we further extend this approach in order to provide a precise delineation of the set of cognitive variations of that brand concept map structure which can simultaneously coexist within the data. This methodology can operate with nonlinear as well as linear relationships between the variables, and utilizes simple Likert-style marketing survey data as input. In addition, the method can operate without any a priori hypothesized structures or relations among the brand associations in the model. The resulting brand concept map structures delineate directional (as opposed to simply correlational) relations among the brand associations, and differentiates between the predictive and the diagnostic directions within each link. Further, we determine a Bayesian network-based link strength measure, and apply it to a comparison of the strengths of the connections between different semantic categories of brand association descriptors, as well as between different strategically important drivers of brand differentiation. Finally, we apply a precise form of information propagation through the predictive and diagnostic links within the network in order to evaluate the effect of introducing new information to the brand concept network. This overall methodology operates via a factorization of the joint distribution of the brand association variables via conditional independence properties and an application of the causal Markov condition, and as such, it represents an alternative approach to correlation-based structural determination methods. By using conditional independence as a core structural construct, the methods utilized here are especially well- suited for determining and analyzing asymmetric or directional beliefs about brand or product attributes. This methodology builds on the pioneering Brand Concept Mapping approach of Roedder John et al. (2006). Similar to that approach, the Bayesian network-based method derives the specific link-by-link structure among a brand's associations, and also allows for a precise quantitative determination of the likely effects that manipulation of specific brand associations will have upon other strategically important associations within that brand image. In addition, the method's precise informational semantics and specific structural measures allow for a greater understanding of the structure of these brand associations.
ContributorsBrownstein, Steven Alan (Author) / Reingen, Peter (Thesis advisor) / Kumar, Ajith (Committee member) / Mokwa, Michael (Committee member) / Arizona State University (Publisher)
Created2013
Description
Identifying factors associated with service infusion success has become an important issue in theory and practice, as manufacturers turn to services to advance performance. The goals of this dissertation are to identify the key factors associated with service infusion success and develop an integrative framework and associated research propositions to isolate the underlying determinants of successful hybrid solution strategies for business customers. This dissertation is comprised of two phases. The first phase taps into the experience and learning gained by executives from Fortune-100 manufacturing firms who are managing the transition from goods to hybrid offerings for their customers. A discovery-oriented, theory-in-use approach is adopted to glean insights concerning the factors that facilitate and hinder those service transition strategies. Twenty-eight interviews were conducted with key executives, transcripts were analyzed and key themes were identified with special attention directed to the particular capabilities that managers consider crucial for successful service-growth strategies. One such capability centers on the ability of a firm to successfully transfer newly-developed hybrid solutions from one customer engagement to another. Building on this foundation, phase two involves a case study that provides an in-depth examination of the hybrid offering replication process in a business-to-business firm attempting to replicate four strategic hybrid offerings. Emergent themes, based on 13 manager interviews, reveal factors that promote or impede successful hybrid offering transfer. Among the factors that underlie successful hybrid offering transfers across customer engagements are close customer relationships, a clear value proposition embraced by organizational numbers, an accurate forecast of market potential, and collaborative working relationships across units. The findings from the field studies provided a catalyst for a deeper examination of existing literature and formed the building blocks for the conceptual model and several key research propositions related to the successful transfer of hybrid offerings. The model isolates five sets of factors that influence the hybrid offering transfer process, including the characteristics of (1) the source project team, (2) the seeking project team, (3) the hybrid offering, (4) the relationship exchange, and (5) the customer. The conceptualization isolates the critical role that the customer assumes in service infusion strategy implementation.
ContributorsSalas, Jim (Author) / Walker, Beth (Thesis advisor) / Hutt, Michael D. (Thesis advisor) / Park, Sungho (Committee member) / Ulaga, Wolfgang (Committee member) / Arizona State University (Publisher)
Created2013