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Metal hydride materials have been intensively studied for hydrogen storage applications. In addition to potential hydrogen economy applications, metal hydrides offer a wide variety of other interesting properties. For example, hydrogen-dominant materials, which are hydrides with the highest hydrogen content for a particular metal/semimetal composition, are predicted to display high-temperature

Metal hydride materials have been intensively studied for hydrogen storage applications. In addition to potential hydrogen economy applications, metal hydrides offer a wide variety of other interesting properties. For example, hydrogen-dominant materials, which are hydrides with the highest hydrogen content for a particular metal/semimetal composition, are predicted to display high-temperature superconductivity. On the other side of the spectrum are hydrides with small amounts of hydrogen (0.1 - 1 at.%) that are investigated as viable magnetic, thermoelectric or semiconducting materials. Research of metal hydride materials is generally important to gain fundamental understanding of metal-hydrogen interactions in materials. Hydrogenation of Zintl phases, which are defined as compounds between an active metal (alkali, alkaline earth, rare earth) and a p-block metal/semimetal, were attempted by a hot sintering method utilizing an autoclave loaded with gaseous hydrogen (< 9 MPa). Hydride formation competes with oxidative decomposition of a Zintl phase. The oxidative decomposition, which leads to a mixture of binary active metal hydride and p-block element, was observed for investigated aluminum (Al) and gallium (Ga) containing Zintl phases. However, a new phase Li2Al was discovered when Zintl phase precursors were synthesized. Using the single crystal x-ray diffraction (SCXRD), the Li2Al was found to crystallize in an orthorhombic unit cell (Cmcm) with the lattice parameters a = 4.6404(8) Å, b = 9.719(2) Å, and c = 4.4764(8) Å. Increased demand for materials with improved properties necessitates the exploration of alternative synthesis methods. Conventional metal hydride synthesis methods, like ball-milling and autoclave technique, are not responding to the demands of finding new materials. A viable alternative synthesis method is the application of high pressure for the preparation of hydrogen-dominant materials. Extreme pressures in the gigapascal ranges can open access to new metal hydrides with novel structures and properties, because of the drastically increased chemical potential of hydrogen. Pressures up to 10 GPa can be easily achieved using the multi-anvil (MA) hydrogenations while maintaining sufficient sample volume for structure and property characterization. Gigapascal MA hydrogenations using ammonia borane (BH3NH3) as an internal hydrogen source were employed in the search for new hydrogen-dominant materials. Ammonia borane has high gravimetric volume of hydrogen, and additionally the thermally activated decomposition at high pressures lead to a complete hydrogen release at reasonably low temperature. These properties make ammonia borane a desired hydrogen source material. The missing member Li2PtH6 of the series of A2PtH6 compounds (A = Na to Cs) was accessed by employing MA technique. As the known heavier analogs, the Li2PtH6 also crystallizes in a cubic K2PtCl6-type structure with a cell edge length of 6.7681(3) Å. Further gigapascal hydrogenations afforded the compounds K2SiH6 and Rb2SiH6 which are isostructural to Li2PtH6. The cubic K2SiH6 and Rb2SiH6 are built from unique hypervalent SiH62- entities with the lattice parameters of 7.8425(9) and 8.1572(4) Å, respectively. Spectroscopic analysis of hexasilicides confirmed the presence of hypervalent bonding. The Si-H stretching frequencies at 1550 cm-1 appeared considerably decreased in comparison with a normal-valent (2e2c) Si-H stretching frequencies in SiH4 at around 2200 cm-1. However, the observed stretching modes in hypervalent hexasilicides were in a reasonable agreement with Ph3SiH2- (1520 cm-1) where the hydrogen has the axial (3e4c bonded) position in the trigoal bipyramidal environment.
ContributorsPuhakainen, Kati (Author) / Häussermann, Ulrich (Thesis advisor) / Seo, Dong (Thesis advisor) / Kouvetakis, John (Committee member) / Wolf, George (Committee member) / Arizona State University (Publisher)
Created2013
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Description

In recent years, an increase of environmental temperature in urban areas has raised many concerns. These areas are subjected to higher temperature compared to the rural surrounding areas. Modification of land surface and the use of materials such as concrete and/or asphalt are the main factors influencing the surface energy

In recent years, an increase of environmental temperature in urban areas has raised many concerns. These areas are subjected to higher temperature compared to the rural surrounding areas. Modification of land surface and the use of materials such as concrete and/or asphalt are the main factors influencing the surface energy balance and therefore the environmental temperature in the urban areas. Engineered materials have relatively higher solar energy absorption and tend to trap a relatively higher incoming solar radiation. They also possess a higher heat storage capacity that allows them to retain heat during the day and then slowly release it back into the atmosphere as the sun goes down. This phenomenon is known as the Urban Heat Island (UHI) effect and causes an increase in the urban air temperature. Many researchers believe that albedo is the key pavement affecting the urban heat island. However, this research has shown that the problem is more complex and that solar reflectivity may not be the only important factor to evaluate the ability of a pavement to mitigate UHI. The main objective of this study was to analyze and research the influence of pavement materials on the near surface air temperature. In order to accomplish this effort, test sections consisting of Hot Mix Asphalt (HMA), Porous Hot Mix asphalt (PHMA), Portland Cement Concrete (PCC), Pervious Portland Cement Concrete (PPCC), artificial turf, and landscape gravels were constructed in the Phoenix, Arizona area. Air temperature, albedo, wind speed, solar radiation, and wind direction were recorded, analyzed and compared above each pavement material type. The results showed that there was no significant difference in the air temperature at 3-feet and above, regardless of the type of the pavement. Near surface pavement temperatures were also measured and modeled. The results indicated that for the UHI analysis, it is important to consider the interaction between pavement structure, material properties, and environmental factors. Overall, this study demonstrated the complexity of evaluating pavement structures for UHI mitigation; it provided great insight on the effects of material types and properties on surface temperatures and near surface air temperature.

ContributorsPourshams-Manzouri, Tina (Author) / Kaloush, Kamil (Thesis advisor) / Wang, Zhihua (Thesis advisor) / Zapata, Claudia E. (Committee member) / Mamlouk, Michael (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Topological insulators with conducting surface states yet insulating bulk states have generated a lot of interest amongst the physics community due to their varied characteristics and possible applications. Doped topological insulators have presented newer physical states of matter where topological order co&ndashexists; with other physical properties (like magnetic order). The

Topological insulators with conducting surface states yet insulating bulk states have generated a lot of interest amongst the physics community due to their varied characteristics and possible applications. Doped topological insulators have presented newer physical states of matter where topological order co&ndashexists; with other physical properties (like magnetic order). The electronic states of these materials are very intriguing and pose problems and the possible solutions to understanding their unique behaviors. In this work, we use Electron Energy Loss Spectroscopy (EELS) – an analytical TEM tool to study both core&ndashlevel; and valence&ndashlevel; excitations in Bi2Se3 and Cu(doped)Bi2Se3 topological insulators. We use this technique to retrieve information on the valence, bonding nature, co-ordination and lattice site occupancy of the undoped and the doped systems. Using the reference materials Cu(I)Se and Cu(II)Se we try to compare and understand the nature of doping that copper assumes in the lattice. And lastly we utilize the state of the art monochromated Nion UltraSTEM 100 to study electronic/vibrational excitations at a record energy resolution from sub-nm regions in the sample.
ContributorsSubramanian, Ganesh (Author) / Spence, John (Thesis advisor) / Jiang, Nan (Committee member) / Chen, Tingyong (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Vehicle type choice is a significant determinant of fuel consumption and energy sustainability; larger, heavier vehicles consume more fuel, and expel twice as many pollutants, than their smaller, lighter counterparts. Over the course of the past few decades, vehicle type choice has seen a vast shift, due to many households

Vehicle type choice is a significant determinant of fuel consumption and energy sustainability; larger, heavier vehicles consume more fuel, and expel twice as many pollutants, than their smaller, lighter counterparts. Over the course of the past few decades, vehicle type choice has seen a vast shift, due to many households making more trips in larger vehicles with lower fuel economy. During the 1990s, SUVs were the fastest growing segment of the automotive industry, comprising 7% of the total light vehicle market in 1990, and 25% in 2005. More recently, due to rising oil prices, greater awareness to environmental sensitivity, the desire to reduce dependence on foreign oil, and the availability of new vehicle technologies, many households are considering the use of newer vehicles with better fuel economy, such as hybrids and electric vehicles, over the use of the SUV or low fuel economy vehicles they may already own. The goal of this research is to examine how vehicle miles traveled, fuel consumption and emissions may be reduced through shifts in vehicle type choice behavior. Using the 2009 National Household Travel Survey data it is possible to develop a model to estimate household travel demand and total fuel consumption. If given a vehicle choice shift scenario, using the model it would be possible to calculate the potential fuel consumption savings that would result from such a shift. In this way, it is possible to estimate fuel consumption reductions that would take place under a wide variety of scenarios.
ContributorsChristian, Keith (Author) / Pendyala, Ram M. (Thesis advisor) / Chester, Mikhail (Committee member) / Kaloush, Kamil (Committee member) / Ahn, Soyoung (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Manufacture of building materials requires significant energy, and as demand for these materials continues to increase, the energy requirement will as well. Offsetting this energy use will require increased focus on sustainable building materials. Further, the energy used in building, particularly in heating and air conditioning, accounts for 40 percent

Manufacture of building materials requires significant energy, and as demand for these materials continues to increase, the energy requirement will as well. Offsetting this energy use will require increased focus on sustainable building materials. Further, the energy used in building, particularly in heating and air conditioning, accounts for 40 percent of a buildings energy use. Increasing the efficiency of building materials will reduce energy usage over the life time of the building. Current methods for maintaining the interior environment can be highly inefficient depending on the building materials selected. Materials such as concrete have low thermal efficiency and have a low heat capacity meaning it provides little insulation. Use of phase change materials (PCM) provides the opportunity to increase environmental efficiency of buildings by using the inherent latent heat storage as well as the increased heat capacity. Incorporating PCM into concrete via lightweight aggregates (LWA) by direct addition is seen as a viable option for increasing the thermal storage capabilities of concrete, thereby increasing building energy efficiency. As PCM change phase from solid to liquid, heat is absorbed from the surroundings, decreasing the demand on the air conditioning systems on a hot day or vice versa on a cold day. Further these materials provide an additional insulating capacity above the value of plain concrete. When the temperature drops outside the PCM turns back into a solid and releases the energy stored from the day. PCM is a hydrophobic material and causes reductions in compressive strength when incorporated directly into concrete, as shown in previous studies. A proposed method for mitigating this detrimental effect, while still incorporating PCM into concrete is to encapsulate the PCM in aggregate. This technique would, in theory, allow for the use of phase change materials directly in concrete, increasing the thermal efficiency of buildings, while negating the negative effect on compressive strength of the material.
ContributorsSharma, Breeann (Author) / Neithalath, Narayanan (Thesis advisor) / Mobasher, Barzin (Committee member) / Rajan, Subramaniam D. (Committee member) / Arizona State University (Publisher)
Created2013
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Description
The history of outdoor water use in the Phoenix, Arizona metropolitan area has given rise to a general landscape aesthetic and pattern of residential irrigation that seem in discord with the natural desert environment. While xeric landscaping that incorporates native desert ecology has potential for reducing urban irrigation demand, there

The history of outdoor water use in the Phoenix, Arizona metropolitan area has given rise to a general landscape aesthetic and pattern of residential irrigation that seem in discord with the natural desert environment. While xeric landscaping that incorporates native desert ecology has potential for reducing urban irrigation demand, there are societal and environmental factors that make mesic landscaping, including shade trees and grass lawns, a common choice for residential yards. In either case, there is potential for water savings through irrigation schedules based on fluxes affecting soil moisture in the active plant rooting zone. In this thesis, a point-scale model of soil moisture dynamics was applied to two urban sites in the Phoenix area: one with xeric landscaping, and one with mesic. The model was calibrated to observed soil moisture data from irrigated and non-irrigated sensors, with local daily precipitation and potential evapotranspiration records as model forcing. Simulations were then conducted to investigate effects of irrigation scheduling, plant stress parameters, and precipitation variability on soil moisture dynamics, water balance partitioning, and plant water stress. Results indicated a substantial difference in soil water storage capacity at the two sites, which affected sensitivity to irrigation scenarios. Seasonal variation was critical in avoiding unproductive water losses at the xeric site, and allowed for small water savings at the mesic site by maintaining mild levels of plant stress. The model was also used to determine minimum annual irrigation required to achieve specified levels of plant stress at each site using long-term meteorological records. While the xeric site showed greater potential for water savings, a bimodal schedule consisting of low winter and summer irrigation was identified as a means to conserve water at both sites, with moderate levels of plant water stress. For lower stress levels, potential water savings were found by fixing irrigation depth and seasonally varying the irrigation interval, consistent with municipal recommendations in the Phoenix metropolitan area. These results provide a deeper understanding of the ecohydrologic differences between the two types of landscape treatments, and can assist water and landscape managers in identifying opportunities for water savings in desert urban areas.
ContributorsVolo, Thomas J (Author) / Vivoni, Enrique R (Thesis advisor) / Ruddell, Benjamin L (Committee member) / Wang, Zhihua (Committee member) / Arizona State University (Publisher)
Created2013
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Description
The alkali activation of aluminosilicate materials as binder systems derived from industrial byproducts have been extensively studied due to the advantages they offer in terms enhanced material properties, while increasing sustainability by the reuse of industrial waste and byproducts and reducing the adverse impacts of OPC production. Fly ash and

The alkali activation of aluminosilicate materials as binder systems derived from industrial byproducts have been extensively studied due to the advantages they offer in terms enhanced material properties, while increasing sustainability by the reuse of industrial waste and byproducts and reducing the adverse impacts of OPC production. Fly ash and ground granulated blast furnace slag are commonly used for their content of soluble silica and aluminate species that can undergo dissolution, polymerization with the alkali, condensation on particle surfaces and solidification. The following topics are the focus of this thesis: (i) the use of microwave assisted thermal processing, in addition to heat-curing as a means of alkali activation and (ii) the relative effects of alkali cations (K or Na) in the activator (powder activators) on the mechanical properties and chemical structure of these systems. Unsuitable curing conditions instigate carbonation, which in turn lowers the pH of the system causing significant reductions in the rate of fly ash activation and mechanical strength development. This study explores the effects of sealing the samples during the curing process, which effectively traps the free water in the system, and allows for increased aluminosilicate activation. The use of microwave-curing in lieu of thermal-curing is also studied in order to reduce energy consumption and for its ability to provide fast volumetric heating. Potassium-based powder activators dry blended into the slag binder system is shown to be effective in obtaining very high compressive strengths under moist curing conditions (greater than 70 MPa), whereas sodium-based powder activation is much weaker (around 25 MPa). Compressive strength decreases when fly ash is introduced into the system. Isothermal calorimetry is used to evaluate the early hydration process, and to understand the reaction kinetics of the alkali powder activated systems. A qualitative evidence of the alkali-hydroxide concentration of the paste pore solution through the use of electrical conductivity measurements is also presented, with the results indicating the ion concentration of alkali is more prevalent in the pore solution of potassium-based systems. The use of advanced spectroscopic and thermal analysis techniques to distinguish the influence of studied parameters is also discussed.
ContributorsChowdhury, Ussala (Author) / Neithalath, Narayanan (Thesis advisor) / Rajan, Subramanium D. (Committee member) / Mobasher, Barzin (Committee member) / Arizona State University (Publisher)
Created2013
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Description
Water resource management is becoming increasingly burdened by uncertain and fluctuating conditions resulting from climate change and population growth which place increased demands on already strained resources. Innovative water management schemes are necessary to address the reality of available water supplies. One such approach is the substitution of trade in

Water resource management is becoming increasingly burdened by uncertain and fluctuating conditions resulting from climate change and population growth which place increased demands on already strained resources. Innovative water management schemes are necessary to address the reality of available water supplies. One such approach is the substitution of trade in virtual water for the use of local water supplies. This study provides a review of existing work in the use of virtual water and water footprint methods. Virtual water trade has been shown to be a successful method for addressing water scarcity and decreasing overall water consumption by shifting high water consumptive processes to wetter regions. These results however assume that all water resource supplies are equivalent regardless of physical location and they do not tie directly to economic markets. In this study we introduce a new mathematical framework, Embedded Resource Accounting (ERA), which is a synthesis of several different analytical methods presently used to quantify and describe human interactions with the economy and the natural environment. We define the specifics of the ERA framework in a generic context for the analysis of embedded resource trade in a way that links directly with the economics of that trade. Acknowledging the cyclical nature of water and the abundance of actual water resources on Earth, this study addresses fresh water availability within a given region. That is to say, the quantities of fresh water supplies annually available at acceptable quality for anthropogenic uses. The results of this research provide useful tools for water resource managers and policy makers to inform decision making on, (1) reallocation of local available fresh water resources, and (2) strategic supplementation of those resources with outside fresh water resources via the import of virtual water.
ContributorsAdams, Elizabeth Anne (Author) / Ruddell, Benjamin L (Thesis advisor) / Allenby, Braden R. (Thesis advisor) / Seager, Thomas P (Committee member) / Arizona State University (Publisher)
Created2013
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Description
In a laboratory setting, the soil volume change behavior is best represented by using various testing standards on undisturbed or remolded samples. Whenever possible, it is most precise to use undisturbed samples to assess the volume change behavior but in the absence of undisturbed specimens, remodeled samples can be used.

In a laboratory setting, the soil volume change behavior is best represented by using various testing standards on undisturbed or remolded samples. Whenever possible, it is most precise to use undisturbed samples to assess the volume change behavior but in the absence of undisturbed specimens, remodeled samples can be used. If that is the case, the soil is compacted to in-situ density and water content (or matric suction), which should best represent the expansive profile in question. It is standard practice to subject the specimen to a wetting process at a particular net normal stress. Even though currently accepted laboratory testing standard procedures provide insight on how the profile conditions changes with time, these procedures do not assess the long term effects on the soil due to climatic changes. In this experimental study, an assessment and quantification of the effect of multiple wetting/drying cycles on the volume change behavior of two different naturally occurring soils was performed. The changes in wetting and drying cycles were extreme when comparing the swings in matric suction. During the drying cycle, the expansive soil was subjected to extreme conditions, which decreased the moisture content less than the shrinkage limit. Nevertheless, both soils were remolded at five different compacted conditions and loaded to five different net normal stresses. Each sample was subjected to six wetting and drying cycles. During the assessment, it was evident from the results that the swell/collapse strain is highly non-linear at low stress levels. The strain-net normal stress relationship cannot be defined by one single function without transforming the data. Therefore, the dataset needs to be fitted to a bi-modal logarithmic function or to a logarithmic transformation of net normal stress in order to use a third order polynomial fit. It was also determined that the moisture content changes with time are best fit by non-linear functions. For the drying cycle, the radial strain was determined to have a constant rate of change with respect to the axial strain. However, for the wetting cycle, there was not enough radial strain data to develop correlations and therefore, an assumption was made based on 55 different test measurements/observations, for the wetting cycles. In general, it was observed that after each subsequent cycle, higher swelling was exhibited for lower net normal stress values; while higher collapse potential was observed for higher net normal stress values, once the net normal stress was less than/greater than a threshold net normal stress value. Furthermore, the swelling pressure underwent a reduction in all cases. Particularly, the Anthem soil exhibited a reduction in swelling pressure by at least 20 percent after the first wetting/drying cycle; while Colorado soil exhibited a reduction of 50 percent. After about the fourth cycle, the swelling pressure seemed to stabilized to an equilibrium value at which a reduction of 46 percent was observed for the Anthem soil and 68 percent reduction for the Colorado soil. The impact of the initial compacted conditions on heave characteristics was studied. Results indicated that materials compacted at higher densities exhibited greater swell potential. When comparing specimens compacted at the same density but at different moisture content (matric suction), it was observed that specimens compacted at higher suction would exhibit higher swelling potential, when subjected to the same net normal stress. The least amount of swelling strain was observed on specimens compacted at the lowest dry density and the lowest matric suction (higher water content). The results from the laboratory testing were used to develop ultimate heave profiles for both soils. This analysis showed that even though the swell pressure for each soil decreased with cycles, the amount of heave would increase or decrease depending upon the initial compaction condition. When the specimen was compacted at 110% of optimum moisture content and 90% of maximum dry density, it resulted in an ultimate heave reduction of 92 percent for Anthem and 685 percent for Colorado soil. On the other hand, when the soils were compacted at 90% optimum moisture content and 100% of the maximum dry density, Anthem specimens heave 78% more and Colorado specimens heave was reduced by 69%. Based on the results obtained, it is evident that the current methods to estimate heave and swelling pressure do not consider the effect of wetting/drying cycles; and seem to fail capturing the free swell potential of the soil. Recommendations for improvement current methods of practice are provided.
ContributorsRosenbalm, Daniel Curtis (Author) / Zapata, Claudia E (Thesis advisor) / Houston, Sandra L. (Committee member) / Kavazanjian, Edward (Committee member) / Witczak, Mathew W (Committee member) / Arizona State University (Publisher)
Created2013
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Description
The thesis studies new methods to fabricate optoelectronic Ge1-ySny/Si(100) alloys and investigate their photoluminescence (PL) properties for possible applications in Si-based photonics including IR lasers. The work initially investigated the origin of the difference between the PL spectrum of bulk Ge, dominated by indirect gap emission, and the PL spectrum

The thesis studies new methods to fabricate optoelectronic Ge1-ySny/Si(100) alloys and investigate their photoluminescence (PL) properties for possible applications in Si-based photonics including IR lasers. The work initially investigated the origin of the difference between the PL spectrum of bulk Ge, dominated by indirect gap emission, and the PL spectrum of Ge-on-Si films, dominated by direct gap emission. It was found that the difference is due to the supression of self-absorption effects in Ge films, combined with a deviation from quasi-equilibrium conditions in the conduction band of undoped films. The latter is confirmed by a model suggesting that the deviation is caused by the shorter recombination lifetime in the films relative to bulk Ge. The knowledge acquired from this work was then utilized to study the PL properties of n-type Ge1-ySny/Si (y=0.004-0.04) samples grown via chemical vapor deposition of Ge2H6/SnD4/P(GeH3)3. It was found that the emission intensity (I) of these samples is at least 10x stronger than observed in un-doped counterparts and that the Idir/Iind ratio of direct over indirect gap emission increases for high-Sn contents due to the reduced gamma-L valley separation, as expected. Next the PL investigation was expanded to samples with y=0.05-0.09 grown via a new method using the more reactive Ge3H8 in place of Ge2H6. Optical quality, 1-um thick Ge1-ySny/Si(100) layers were produced using Ge3H10/SnD4 and found to exhibit strong, tunable PL near the threshold of the direct-indirect bandgap crossover. A byproduct of this study was the development of an enhanced process to produce Ge3H8, Ge4H10, and Ge5H12 analogs for application in ultra-low temperature deposition of Group-IV semiconductors. The thesis also studies synthesis routes of an entirely new class of semiconductor compounds and alloys described by Si5-2y(III-V)y (III=Al, V= As, P) comprising of specifically designed diamond-like structures based on a Si parent lattice incorporating isolated III-V units. The common theme of the two thesis topics is the development of new mono-crystalline materials on ubiquitous silicon platforms with the objective of enhancing the optoelectronic performance of Si and Ge semiconductors, potentially leading to the design of next generation optical devices including lasers, detectors and solar cells.
ContributorsGrzybowski, Gordon (Author) / Kouvetakis, John (Thesis advisor) / Chizmeshya, Andrew (Committee member) / Menéndez, Jose (Committee member) / Arizona State University (Publisher)
Created2013